Characteristics of regional aerosols: Southern Arizona and eastern Pacific Ocean

NASA Astrophysics Data System (ADS)

Prabhakar, Gouri

Atmospheric aerosols impact the quality of our life in many direct and indirect ways. Inhalation of aerosols can have harmful effects on human health. Aerosols also have climatic impacts by absorbing or scattering solar radiation, or more indirectly through their interactions with clouds. Despite a better understanding of several relevant aerosol properties and processes in the past years, they remain the largest uncertainty in the estimate of global radiative forcing. The uncertainties arise because although aerosols are ubiquitous in the Earth's atmosphere they are highly variable in space, time and their physicochemical properties. This makes in-situ measurements of aerosols vital in our effort towards reducing uncertainties in the estimate of global radiative forcing due to aerosols. This study is an effort to characterize atmospheric aerosols at a regional scale, in southern Arizona and eastern Pacific Ocean, based on ground and airborne observations of aerosols. Metals and metalloids in particles with aerodynamic diameter (Dp) smaller than 2.5 μm are found to be ubiquitous in southern Arizona. The major sources of the elements considered in the study are identified to be crustal dust, smelting/mining activities and fuel combustion. The spatial and temporal variability in the mass concentrations of these elements depend both on the source strength and meteorological conditions. Aircraft measurements of aerosol and cloud properties collected during various field campaigns over the eastern Pacific Ocean are used to study the sources of nitrate in stratocumulus cloud water and the relevant processes. The major sources of nitrate in cloud water in the region are emissions from ships and wildfires. Different pathways for nitrate to enter cloud water and the role of meteorology in these processes are examined. Observations of microphysical properties of ambient aerosols in ship plumes are examined. The study shows that there is an enhancement in the number concentration of giant cloud condensation nuclei (Dp > 2 microm) in ship plumes relative to the unperturbed background regions over the ocean.

Perspective: Aerosol microphysics: From molecules to the chemical physics of aerosols

NASA Astrophysics Data System (ADS)

Bzdek, Bryan R.; Reid, Jonathan P.

2017-12-01

Aerosols are found in a wide diversity of contexts and applications, including the atmosphere, pharmaceutics, and industry. Aerosols are dispersions of particles in a gas, and the coupling of the two phases results in highly dynamic systems where chemical and physical properties like size, composition, phase, and refractive index change rapidly in response to environmental perturbations. Aerosol particles span a wide range of sizes from 1 nm to tens of micrometres or from small molecular clusters that may more closely resemble gas phase molecules to large particles that can have similar qualities to bulk materials. However, even large particles with finite volumes exhibit distinct properties from the bulk condensed phase, due in part to their higher surface-to-volume ratio and their ability to easily access supersaturated solute states inaccessible in the bulk. Aerosols represent a major challenge for study because of the facile coupling between the particle and gas, the small amounts of sample available for analysis, and the sheer breadth of operative processes. Time scales of aerosol processes can be as short as nanoseconds or as long as years. Despite their very different impacts and applications, fundamental chemical physics processes serve as a common theme that underpins our understanding of aerosols. This perspective article discusses challenges in the study of aerosols and highlights recent chemical physics advancements that have enabled improved understanding of these complex systems.

Interactive coupling of regional climate and sulfate aerosol models over eastern Asia

NASA Astrophysics Data System (ADS)

Qian, Yun; Giorgi, Filippo

1999-03-01

The NCAR regional climate model (RegCM) is interactively coupled to a simple radiatively active sulfate aerosol model over eastern Asia. Both direct and indirect aerosol effects are represented. The coupled model system is tested for two simulation periods, November 1994 and July 1995, with aerosol sources representative of present-day anthropogenic sulfur emissions. The model sensitivity to the intensity of the aerosol source is also studied. The main conclusions from our work are as follows: (1) The aerosol distribution and cycling processes show substantial regional spatial variability, and temporal variability varying on a range of scales, from the diurnal scale of boundary layer and cumulus cloud evolution to the 3-10 day scale of synoptic scale events and the interseasonal scale of general circulation features; (2) both direct and indirect aerosol forcings have regional effects on surface climate; (3) the regional climate response to the aerosol forcing is highly nonlinear, especially during the summer, due to the interactions with cloud and precipitation processes; (4) in our simulations the role of the aerosol indirect effects is dominant over that of direct effects; (5) aerosol-induced feedback processes can affect the aerosol burdens at the subregional scale. This work constitutes the first step in a long term research project aimed at coupling a hierarchy of chemistry/aerosol models to the RegCM over the eastern Asia region.

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

NASA Astrophysics Data System (ADS)

Fan, Tianyi; Liu, Xiaohong; Ma, Po-Lun; Zhang, Qiang; Li, Zhanqing; Jiang, Yiquan; Zhang, Fang; Zhao, Chuanfeng; Yang, Xin; Wu, Fang; Wang, Yuying

2018-02-01

Global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results are compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22-28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at the surface, and in the atmosphere to be -5.02, -18.47, and 13.45 W m-2, respectively, over eastern China, which are enhanced by -0.91, -3.48, and 2.57 W m-2 compared with the AR5 emission. The differences of ADREs by using MEIC and AR5 emissions are larger than the decadal changes of the modeled ADREs, indicating the uncertainty of the emission inventories. This study highlights the importance of improving both the emission and aerosol secondary production processes in modeling the atmospheric aerosols and their radiative effects. Yet, if the estimations of MEIC emissions in trace gases do not suffer similar biases to those in the AOD, our findings will help affirm a fundamental error in the conversion from precursor gases to secondary aerosols as hinted in other recent studies following different approaches.

Coupling Spectral-bin Cloud Microphysics with the MOSAIC Aerosol Model in WRF-Chem: Methodology and Results for Marine Stratocumulus Clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Wenhua; Fan, Jiwen; Easter, Richard C.

Aerosol-cloud interaction processes can be represented more physically with bin cloud microphysics relative to bulk microphysical parameterizations. However, due to computational power limitations in the past, bin cloud microphysics was often run with very simple aerosol treatments. The purpose of this study is to represent better aerosol-cloud interaction processes in the Chemistry version of Weather Research and Forecast model (WRF-Chem) at convection-permitting scales by coupling spectral-bin cloud microphysics (SBM) with the MOSAIC sectional aerosol model. A flexible interface is built that exchanges cloud and aerosol information between them. The interface contains a new bin aerosol activation approach, which replaces themore » treatments in the original SBM. It also includes the modified aerosol resuspension and in-cloud wet removal processes with the droplet loss tendencies and precipitation fluxes from SBM. The newly coupled system is evaluated for two marine stratocumulus cases over the Southeast Pacific Ocean with either a simplified aerosol setup or full-chemistry. We compare the aerosol activation process in the newly-coupled SBM-MOSAIC against the SBM simulation without chemistry using a simplified aerosol setup, and the results show consistent activation rates. A longer time simulation reinforces that aerosol resuspension through cloud drop evaporation plays an important role in replenishing aerosols and impacts cloud and precipitation in marine stratocumulus clouds. Evaluation of the coupled SBM-MOSAIC with full-chemistry using aircraft measurements suggests that the new model works realistically for the marine stratocumulus clouds, and improves the simulation of cloud microphysical properties compared to a simulation using MOSAIC coupled with the Morrison two-moment microphysics.« less

Coupling spectral-bin cloud microphysics with the MOSAIC aerosol model in WRF-Chem: Methodology and results for marine stratocumulus clouds

NASA Astrophysics Data System (ADS)

Gao, Wenhua; Fan, Jiwen; Easter, R. C.; Yang, Qing; Zhao, Chun; Ghan, Steven J.

2016-09-01

Aerosol-cloud interaction processes can be represented more physically with bin cloud microphysics relative to bulk microphysical parameterizations. However, due to computational power limitations in the past, bin cloud microphysics was often run with very simple aerosol treatments. The purpose of this study is to represent better aerosol-cloud interaction processes in the Chemistry version of Weather Research and Forecast model (WRF-Chem) at convection-permitting scales by coupling spectral-bin cloud microphysics (SBM) with the MOSAIC sectional aerosol model. A flexible interface is built that exchanges cloud and aerosol information between them. The interface contains a new bin aerosol activation approach, which replaces the treatments in the original SBM. It also includes the modified aerosol resuspension and in-cloud wet removal processes with the droplet loss tendencies and precipitation fluxes from SBM. The newly coupled system is evaluated for two marine stratocumulus cases over the Southeast Pacific Ocean with either a simplified aerosol setup or full-chemistry. We compare the aerosol activation process in the newly coupled SBM-MOSAIC against the SBM simulation without chemistry using a simplified aerosol setup, and the results show consistent activation rates. A longer time simulation reinforces that aerosol resuspension through cloud drop evaporation plays an important role in replenishing aerosols and impacts cloud and precipitation in marine stratocumulus clouds. Evaluation of the coupled SBM-MOSAIC with full-chemistry using aircraft measurements suggests that the new model works realistically for the marine stratocumulus clouds, and improves the simulation of cloud microphysical properties compared to a simulation using MOSAIC coupled with the Morrison two-moment microphysics.

Unveiling aerosol-cloud interactions - Part 2: Minimising the effects of aerosol swelling and wet scavenging in ECHAM6-HAM2 for comparison to satellite data

NASA Astrophysics Data System (ADS)

Neubauer, David; Christensen, Matthew W.; Poulsen, Caroline A.; Lohmann, Ulrike

2017-11-01

Aerosol-cloud interactions (ACIs) are uncertain and the estimates of the ACI effective radiative forcing (ERFaci) magnitude show a large variability. Within the Aerosol_cci project the susceptibility of cloud properties to changes in aerosol properties is derived from the high-resolution AATSR (Advanced Along-Track Scanning Radiometer) data set using the Cloud-Aerosol Pairing Algorithm (CAPA) (as described in our companion paper) and compared to susceptibilities from the global aerosol climate model ECHAM6-HAM2 and MODIS-CERES (Moderate Resolution Imaging Spectroradiometer - Clouds and the Earth's Radiant Energy System) data. For ECHAM6-HAM2 the dry aerosol is analysed to mimic the effect of CAPA. Furthermore the analysis is done for different environmental regimes. The aerosol-liquid water path relationship in ECHAM6-HAM2 is systematically stronger than in AATSR-CAPA data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM2 the strength of the susceptibilities of liquid water path, cloud droplet number concentration and cloud albedo as well as ERFaci agree much better with those of AATSR-CAPA or MODIS-CERES. When comparing satellite-derived to model-derived susceptibilities, this study finds it more appropriate to use dry aerosol in the computation of model susceptibilities. We further find that the statistical relationships inferred from different satellite sensors (AATSR-CAPA vs. MODIS-CERES) as well as from ECHAM6-HAM2 are not always of the same sign for the tested environmental conditions. In particular the susceptibility of the liquid water path is negative in non-raining scenes for MODIS-CERES but positive for AATSR-CAPA and ECHAM6-HAM2. Feedback processes like cloud-top entrainment that are missing or not well represented in the model are therefore not well constrained by satellite observations. In addition to aerosol swelling, wet scavenging and aerosol processing have an impact on liquid water path, cloud albedo and cloud droplet number susceptibilities. Aerosol processing leads to negative liquid water path susceptibilities to changes in aerosol index (AI) in ECHAM6-HAM2, likely due to aerosol-size changes by aerosol processing. Our results indicate that for statistical analysis of aerosol-cloud interactions the unwanted effects of aerosol swelling, wet scavenging and aerosol processing need to be minimised when computing susceptibilities of cloud variables to changes in aerosol.

Utilization of AERONET polarimetric measurements for improving retrieval of aerosol microphysics: GSFC, Beijing and Dakar data analysis

NASA Astrophysics Data System (ADS)

Fedarenka, Anton; Dubovik, Oleg; Goloub, Philippe; Li, Zhengqiang; Lapyonok, Tatyana; Litvinov, Pavel; Barel, Luc; Gonzalez, Louis; Podvin, Thierry; Crozel, Didier

2016-08-01

The study presents the efforts on including the polarimetric data to the routine inversion of the radiometric ground-based measurements for characterization of the atmospheric aerosols and analysis of the obtained advantages in retrieval results. First, to operationally process the large amount of polarimetric data the data preparation tool was developed. The AERONET inversion code adapted for inversion of both intensity and polarization measurements was used for processing. Second, in order to estimate the effect from utilization of polarimetric information on aerosol retrieval results, both synthetic data and the real measurements were processed using developed routine and analyzed. The sensitivity study has been carried out using simulated data based on three main aerosol models: desert dust, urban industrial and urban clean aerosols. The test investigated the effects of utilization of polarization data in the presence of random noise, bias in measurements of optical thickness and angular pointing shift. The results demonstrate the advantage of polarization data utilization in the cases of aerosols with pronounced concentration of fine particles. Further, the extended set of AERONET observations was processed. The data for three sites have been used: GSFC, USA (clean urban aerosol dominated by fine particles), Beijing, China (polluted industrial aerosol characterized by pronounced mixture of both fine and coarse modes) and Dakar, Senegal (desert dust dominated by coarse particles). The results revealed considerable advantage of polarimetric data applying for characterizing fine mode dominated aerosols including industrial pollution (Beijing). The use of polarization corrects particle size distribution by decreasing overestimated fine mode and increasing the coarse mode. It also increases underestimated real part of the refractive index and improves the retrieval of the fraction of spherical particles due to high sensitivity of polarization to particle shape. Overall, the study demonstrates a substantial value of polarimetric data for improving aerosol characterization.

Modeling Atmospheric Aerosols in WRF/Chem

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yang; Hu, X.-M.; Howell, G.

2005-06-01

In this study, three aerosol modules are tested and compared. The first module is the Modal Aerosol Dynamics Model for Europe (MADE) with the secondary organic aerosol model (SORGAM) (referred to as MADE/SORGAM). The second module is the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC). The third module is the Model of Aerosol Dynamics, Reaction, Ionization and Dissolution (MADRID). The three modules differ in terms of size representation used, chemical species treated, assumptions and numerical algorithms used. Table 1 compares the major processes among the three aerosol modules.

Using satellites and global models to investigate aerosol-cloud interactions

NASA Astrophysics Data System (ADS)

Gryspeerdt, E.; Quaas, J.; Goren, T.; Sourdeval, O.; Mülmenstädt, J.

2017-12-01

Aerosols are known to impact liquid cloud properties, through both microphysical and radiative processes. Increasing the number concentration of aerosol particles can increase the cloud droplet number concentration (CDNC). Through impacts on precipitation processes, this increase in CDNC may also be able to impact the cloud fraction (CF) and the cloud liquid water path (LWP). Several studies have looked into the effect of aerosols on the CDNC, but as the albedo of a cloudy scene depends much more strongly on LWP and CF, an aerosol influence on these properties could generate a significant radiative forcing. While the impact of aerosols on cloud properties can be seen in case studies involving shiptracks and volcanoes, producing a global estimate of these effects remains challenging due to the confounding effect of local meteorology. For example, relative humidity significantly impacts the aerosol optical depth (AOD), a common satellite proxy for CCN, as well as being a strong control on cloud properties. This can generate relationships between AOD and cloud properties, even when there is no impact of aerosol-cloud interactions. In this work, we look at how aerosol-cloud interactions can be distinguished from the effect of local meteorology in satellite studies. With a combination global climate models and multiple sources of satellite data, we show that the choice of appropriate mediating variables and case studies can be used to develop constraints on the aerosol impact on CF and LWP. This will lead to improved representations of clouds in global climate models and help to reduce the uncertainty in the global impact of anthropogenic aerosols on cloud properties.

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

NASA Astrophysics Data System (ADS)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

Satellite observations and EMAC model calculations of sulfate aerosols from Kilauea: a study of aerosol formation, processing, and loss

NASA Astrophysics Data System (ADS)

Penning de Vries, Marloes; Beirle, Steffen; Brühl, Christoph; Dörner, Steffen; Pozzer, Andrea; Wagner, Thomas

2016-04-01

The currently most active volcano on Earth is Mount Kilauea on Hawaii, as it has been in a state of continuous eruption since 1983. The opening of a new vent in March 2008 caused half a year of strongly increased SO2 emissions, which in turn led to the formation of a sulfate plume with an extent of at least two thousand kilometers. The plume could be clearly identified from satellite measurements from March to November, 2008. The steady trade winds in the region and the lack of interfering sources allowed us to determine the life time of SO2 from Kilauea using only satellite-based measurements (no a priori or model information). The current investigation focuses on sulfate aerosols: their formation, processing and subsequent loss. Using space-based aerosol measurements by MODIS, we study the evolution of aerosol optical depth, which first increases as a function of distance from the volcano due to aerosol formation from SO2 oxidation, and subsequently decreases as aerosols are deposited to the surface. The outcome is compared to results from calculations using the EMAC (ECHAM/MESSy Atmospheric Chemistry) model to test the state of understanding of the sulfate aerosol life cycle. For this comparison, a particular focus is on the role of clouds and wet removal processes.

Extending 'Deep Blue' aerosol retrieval coverage to cases of absorbing aerosols above clouds: sensitivity analysis and first case studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sayer, Andrew M.; Hsu, C.; Bettenhausen, Corey

Cases of absorbing aerosols above clouds (AAC), such as smoke or mineral dust, are omitted from most routinely-processed space-based aerosol optical depth (AOD) data products, including those from the Moderate Resolution Imaging Spectroradiometer (MODIS). This study presents a sensitivity analysis and preliminary algorithm to retrieve above-cloud AOD and liquid cloud optical depth (COD) for AAC cases from MODIS or similar

Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Fast, J. D.; Takigawa, M.

2014-09-01

Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimations of aerosol direct and indirect effects. In this study, we develop an aerosol module, designated the Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can explicitly represent these parameters by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 μm to resolve both aerosol sizes (12 bins) and BC mixing states (10 bins) for a total of 120 bins. The particles with diameters between 1 and 40 nm are resolved using additional eight size bins to calculate NPF. The ATRAS module is implemented in the WRF-Chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging, and SOA processes over East Asia during the spring of 2009. The BC absorption enhancement by coating materials is about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement is estimated to be 10-20% over northern East Asia and 20-35% over southern East Asia. A clear north-south contrast is also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increases CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increases CCN concentrations at lower supersaturations (larger particles) over southern East Asia. The application of ATRAS in East Asia also shows that the impact of each process on each optical and radiative parameter depends strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA processes under different meteorological conditions and emissions.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

NASA Astrophysics Data System (ADS)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-01-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number concentration.

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice

NASA Astrophysics Data System (ADS)

Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

2015-10-01

The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of cloud and aerosol over the Southern Ocean.

SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

NASA Technical Reports Server (NTRS)

Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

2008-01-01

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

Aerosol-Phase Production of Nitrogen-Containing Oligomers After Uptake of Methylglyoxal and Cloud Processing

NASA Astrophysics Data System (ADS)

De Haan, D. O.; Riva, M.; Surratt, J. D.; Cazaunau, M.; Doussin, J. F.

2016-12-01

Minimal organic aerosol forms when aerosol particles are exposed to gas-phase methylglyoxal, but condensed phase laboratory studies of aerosol chemistry have suggested that methylglyoxal is a significant source of oligomerized aerosol material. In this study, various types of seed particles were exposed to gaseous methylglyoxal and then cloud-processed in the CESAM chamber. The gas phase was continuously probed by high-resolution PTR-MS during the experiments, and the particle phase WSOC was chemically characterized by high-resolution UPLC/ESI-DAD-QTOFMS. Uptake of methylglyoxal to dry particles caused optical rather than size changes, along with the release of imine products to the gas phase. High RH and cloud processing released some particle-bound methylglyoxal back to the gas phase but triggered an uptake of imine products. Analysis of the particle phase identified N-containing aldol condensation products derived from methylglyoxal, imine (produced from methylglyoxal and amine reactions), acetaldehyde (produced by methylglyoxal photolysis) and hydroxyacetone (produced by methylglyoxal disproportionation) monomers.

Preliminary results of the aerosol optical depth retrieval in Johor, Malaysia

NASA Astrophysics Data System (ADS)

Lim, H. Q.; Kanniah, K. D.; Lau, A. M. S.

2014-02-01

Monitoring of atmospheric aerosols over the urban area is important as tremendous amounts of pollutants are released by industrial activities and heavy traffic flow. Air quality monitoring by satellite observation provides better spatial coverage, however, detailed aerosol properties retrieval remains a challenge. This is due to the limitation of aerosol retrieval algorithm on high reflectance (bright surface) areas. The aim of this study is to retrieve aerosol optical depth over urban areas of Iskandar Malaysia; the main southern development zone in Johor state, using Moderate Resolution Imaging Spectroradiometer (MODIS) 500 m resolution data. One of the important steps is the aerosol optical depth retrieval is to characterise different types of aerosols in the study area. This information will be used to construct a Look Up Table containing the simulated aerosol reflectance and corresponding aerosol optical depth. Thus, in this study we have characterised different aerosol types in the study area using Aerosol Robotic Network (AERONET) data. These data were processed using cluster analysis and the preliminary results show that the area is consisting of coastal urban (65%), polluted urban (27.5%), dust particles (6%) and heavy pollution (1.5%) aerosols.

Aerosol processing in stratiform clouds in ECHAM6-HAM

NASA Astrophysics Data System (ADS)

Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

2013-04-01

Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the chemical components as well as 5 tracers for aerosol particles in ice crystals. This allows simulations of aerosol processing in warm, mixed-phase (e.g. through the Bergeron-Findeisen process) and ice clouds. The fixed scavenging ratios used for wet deposition in clouds in standard HAM are replaced by an explicit treatment of collision of cloud droplets/ice crystals with interstitial aerosol particles. Nucleation scavenging of aerosol particles by acting as cloud condensation nuclei or ice nuclei, freezing and evaporation of cloud droplets and melting and sublimation of ice crystals are treated explicitly. In extension to previous studies, aerosol particles from evaporating precipitation are released to modes which correspond to their size. Cloud processing of aerosol particles changes their size distribution and hence influences cloud droplet and ice crystal number concentrations as well as precipitation rate, which in turn affects aerosol concentrations. Results will be presented at the conference. Hoose et al., JGR, 2008a, doi: 10.1029/2007JD009251 Hoose et al., ACP, 2008b, doi: 10.5194/acp-8-6939-2008 Stevens et al., 2013, submitted Stier et al., ACP, 2005, doi: 10.5194/acp-5-1125-2005

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Tianyi; Liu, Xiaohong; Ma, Po -Lun

Here, global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results aremore » compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22–28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at the surface, and in the atmosphere to be –5.02, –18.47, and 13.45 W m –2, respectively, over eastern China, which are enhanced by –0.91, –3.48, and 2.57 W m –2 compared with the AR5 emission. The differences of ADREs by using MEIC and AR5 emissions are larger than the decadal changes of the modeled ADREs, indicating the uncertainty of the emission inventories. This study highlights the importance of improving both the emission and aerosol secondary production processes in modeling the atmospheric aerosols and their radiative effects. Yet, if the estimations of MEIC emissions in trace gases do not suffer similar biases to those in the AOD, our findings will help affirm a fundamental error in the conversion from precursor gases to secondary aerosols as hinted in other recent studies following different approaches.« less

Emission or atmospheric processes? An attempt to attribute the source of large bias of aerosols in eastern China simulated by global climate models

DOE PAGES

Fan, Tianyi; Liu, Xiaohong; Ma, Po -Lun; ...

2018-02-01

Here, global climate models often underestimate aerosol loadings in China, and these biases can have significant implications for anthropogenic aerosol radiative forcing and climate effects. The biases may be caused by either the emission inventory or the treatment of aerosol processes in the models, or both, but so far no consensus has been reached. In this study, a relatively new emission inventory based on energy statistics and technology, Multi-resolution Emission Inventory for China (MEIC), is used to drive the Community Atmosphere Model version 5 (CAM5) to evaluate aerosol distribution and radiative effects against observations in China. The model results aremore » compared with the model simulations with the widely used Intergovernmental Panel on Climate Change Fifth Assessment Report (IPCC AR5) emission inventory. We find that the new MEIC emission improves the aerosol optical depth (AOD) simulations in eastern China and explains 22–28 % of the AOD low bias simulated with the AR5 emission. However, AOD is still biased low in eastern China. Seasonal variation of the MEIC emission leads to a better agreement with the observed seasonal variation of primary aerosols than the AR5 emission, but the concentrations are still underestimated. This implies that the atmospheric loadings of primary aerosols are closely related to the emission, which may still be underestimated over eastern China. In contrast, the seasonal variations of secondary aerosols depend more on aerosol processes (e.g., gas- and aqueous-phase production from precursor gases) that are associated with meteorological conditions and to a lesser extent on the emission. It indicates that the emissions of precursor gases for the secondary aerosols alone cannot explain the low bias in the model. Aerosol secondary production processes in CAM5 should also be revisited. The simulation using MEIC estimates the annual-average aerosol direct radiative effects (ADREs) at the top of the atmosphere (TOA), at the surface, and in the atmosphere to be –5.02, –18.47, and 13.45 W m –2, respectively, over eastern China, which are enhanced by –0.91, –3.48, and 2.57 W m –2 compared with the AR5 emission. The differences of ADREs by using MEIC and AR5 emissions are larger than the decadal changes of the modeled ADREs, indicating the uncertainty of the emission inventories. This study highlights the importance of improving both the emission and aerosol secondary production processes in modeling the atmospheric aerosols and their radiative effects. Yet, if the estimations of MEIC emissions in trace gases do not suffer similar biases to those in the AOD, our findings will help affirm a fundamental error in the conversion from precursor gases to secondary aerosols as hinted in other recent studies following different approaches.« less

During air cool process aerosol absorption detection with photothermal interferometry

NASA Astrophysics Data System (ADS)

Li, Baosheng; Xu, Limei; Huang, Junling; Ma, Fei; Wang, Yicheng; Li, Zhengqiang

2014-11-01

This paper studies the basic principle of laser photothermal interferometry method of aerosol particles absorption coefficient. The photothermal interferometry method with higher accuracy and lower uncertainty can directly measure the absorption coefficient of atmospheric aerosols and not be affected by scattered light. With Jones matrix expression, the math expression of a special polarization interferometer is described. This paper using folded Jamin interferometer, which overcomes the influence of vibration on measuring system. Interference come from light polarization beam with two orthogonal and then combine to one beam, finally aerosol absorption induced refractive index changes can be gotten with four beam of phase orthogonal light. These kinds of styles really improve the stability of system and resolution of the system. Four-channel detections interact with interference fringes, to reduce the light intensity `zero drift' effect on the system. In the laboratory, this device typical aerosol absorption index, it shows that the result completely agrees with actual value. After heated by laser, cool process of air also show the process of aerosol absorption. This kind of instrument will be used to monitor ambient aerosol absorption and suspended particulate matter chemical component. Keywords: Aerosol absorption coefficient; Photothermal interferometry; Suspended particulate matter.

Aerosol particle shrinkage event phenomenology in a South European suburban area during 2009-2015

NASA Astrophysics Data System (ADS)

Alonso-Blanco, E.; Gómez-Moreno, F. J.; Núñez, L.; Pujadas, M.; Cusack, M.; Artíñano, B.

2017-07-01

A high number of aerosol particle shrinkage cases (70) have been identified and analyzed from an extensive and representative database of aerosol size distributions obtained between 2009 and 2015 at an urban background site in Madrid (Spain). A descriptive classification based on the process from which the shrinkage began is proposed according which shrinkage events were divided into three groups: (1) NPF + shrinkage (NPF + S) events, (2) aerosol particle growth process + shrinkage (G + S) events, and (3) pure shrinkage (S) events. The largest number of shrinkages corresponded to the S-type followed by NPF + S, while the G + S events were the least frequent group recorded. Duration of shrinkages varied widely from 0.75 to 8.5 h and SR from -1.0 to -11.1 nm h-1. These processes typically occurred in the afternoon, around 18:00 UTC, caused by two situations: i) a wind speed increase usually associated with a change in the wind direction (over 60% of the observations) and ii) the reduction of photochemical activity at the end of the day. All shrinkages were detected during the warm period, mainly between May and August, when local meteorological conditions (high solar irradiance and temperature and low relative humidity), atmospheric processes (high photochemical activity) and availability of aerosol-forming precursors were favorable for their development. As a consequence of these processes, the particles concentration corresponding to the Aitken mode decreased into the nucleation mode. The accumulation mode did not undergo significant changes during these processes. In some cases, a dilution of the particulate content in the ambient air was observed. This work, goes further than others works dealing with aerosol particles shrinkages, as it incorporates as a main novelty a classification methodology for studying these processes. Moreover, compared to other studies, it is supported by a high and representative number of observations. Thus, this study contributes to get a better understanding of this type of atmospheric aerosol transformations and its features.

Impacts of aerosol pollutant mitigation on lowland rice yields in China

NASA Astrophysics Data System (ADS)

Zhang, Tianyi; Li, Tao; Yue, Xu; Yang, Xiaoguang

2017-10-01

Aerosol pollution in China is significantly altering radiative transfer processes and is thereby potentially affecting rice photosynthesis and yields. However, the response of rice photosynthesis to aerosol-induced radiative perturbations is still not well understood. Here, we employ a process-based modelling approach to simulate changes in incoming radiation (RAD) and the diffuse radiation fraction (DF) with aerosol mitigation in China and their associated impacts on rice yields. Aerosol reduction has the positive effect of increasing RAD and the negative effect of decreasing DF on rice photosynthesis and yields. In rice production areas where the average RAD during the growing season is lower than 250 W m-2, aerosol reduction is beneficial for higher rice yields, whereas in areas with RAD>250 W m-2, aerosol mitigation causes yield declines due to the associated reduction in the DF, which decreases the light use efficiency. As a net effect, rice yields were estimated to significantly increase by 0.8%-2.6% with aerosol concentrations reductions from 20 to 100%, which is lower than the estimates obtained in earlier studies that only considered the effects of RAD. This finding suggests that both RAD and DF are important processes influencing rice yields and should be incorporated into future assessments of agricultural responses to variations in aerosol-induced radiation under climate change.

A sensitivity analysis of volcanic aerosol dispersion in the stratosphere. [Mt. Fuego, Guatemala eruptions

NASA Technical Reports Server (NTRS)

Butler, C. F.

1979-01-01

A computer sensitivity analysis was performed to determine the uncertainties involved in the calculation of volcanic aerosol dispersion in the stratosphere using a 2 dimensional model. The Fuego volcanic event of 1974 was used. Aerosol dispersion processes that were included are: transport, sedimentation, gas phase sulfur chemistry, and aerosol growth. Calculated uncertainties are established from variations in the stratospheric aerosol layer decay times at 37 latitude for each dispersion process. Model profiles are also compared with lidar measurements. Results of the computer study are quite sensitive (factor of 2) to the assumed volcanic aerosol source function and the large variations in the parameterized transport between 15 and 20 km at subtropical latitudes. Sedimentation effects are uncertain by up to a factor of 1.5 because of the lack of aerosol size distribution data. The aerosol chemistry and growth, assuming that the stated mechanisms are correct, are essentially complete in several months after the eruption and cannot explain the differences between measured and modeled results.

Meeting Review: Airborne Aerosol Inlet Workshop

NASA Technical Reports Server (NTRS)

Baumgardner, Darrel; Huebert, Barry; Wilson, Chuck

1991-01-01

Proceedings from the Airborne Aerosol Inlet Workshop are presented. The two central topics of discussion were the role of aerosols in atmospheric processes and the difficulties in characterizing aerosols. The following topics were discussed during the working sessions: airborne observations to date; identification of inlet design issues; inlet modeling needs and directions; objectives for aircraft experiments; and future laboratory and wind tunnel studies.

Application of remote sensing techniques to study aerosol water vapour uptake in a real atmosphere

NASA Astrophysics Data System (ADS)

Fernández, A. J.; Molero, F.; Becerril-Valle, M.; Coz, E.; Salvador, P.; Artíñano, B.; Pujadas, M.

2018-04-01

In this work, a study of several observations of aerosol water uptake in a real (non-controlled) atmosphere, registered by remote sensing techniques, are presented. In particular, three events were identified within the Atmospheric Boundary Layer (ABL) and other two events were detected in the free troposphere (beyond the top of the ABL). Then, aerosol optical properties were measured at different relative humidity (RH) conditions by means of a multi-wavelength (MW) Raman lidar located at CIEMAT (Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, Research Centre for Energy, Environment and Technology) facilities in Madrid (Spain). Additionally, aerosol optical and microphysical properties provided by automatic sun and sky scanning spectral radiometers (CIMEL CE-318) and a meteorological analysis complement the study. However, a detailed analysis only could be carried out for the cases observed within the ABL since well-mixed atmospheric layers are required to properly characterize these processes. This characterization of aerosol water uptake is based on the curve described by the backscatter coefficient at 532 nm as a function of RH which allows deriving the enhancement factor. Thus, the Hänel parameterization is utilized, and the results obtained are in the range of values reported in previous studies, which shows the suitability of this approach to study such hygroscopic processes. Furthermore, the anti-correlated pattern observed on backscatter-related Ångström exponent (532/355 nm) and RH indicates plausible signs of aerosol hygroscopic growth. According to the meteorological analysis performed, we attribute such hygroscopic behaviour to marine aerosols which are advected from the Atlantic Ocean to the low troposphere in Madrid. We have also observed an interesting response of aerosols to RH at certain levels which it is suggested to be due to a hysteresis process. The events registered in the free troposphere, which deal with volcano and wild fire plumes transported at higher altitudes, indicate that these processes can take place in the free troposphere, where the climate relevance can be rather different considering the role of aerosol as cloud condensation nuclei.

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign.

PubMed

Collier, Sonya; Zhou, Shan; Onasch, Timothy B; Jaffe, Daniel A; Kleinman, Lawrence; Sedlacek, Arthur J; Briggs, Nicole L; Hee, Jonathan; Fortner, Edward; Shilling, John E; Worsnop, Douglas; Yokelson, Robert J; Parworth, Caroline; Ge, Xinlei; Xu, Jianzhong; Butterfield, Zachary; Chand, Duli; Dubey, Manvendra K; Pekour, Mikhail S; Springston, Stephen; Zhang, Qi

2016-08-16

Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (∼2700 m a.s.l.) as well as near their sources using an aircraft. The regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), an index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (∼1 h old) and emissions sampled after atmospheric transport (6-45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate.

Is there an aerosol signature of aqueous processing?

NASA Astrophysics Data System (ADS)

Ervens, B.; Sorooshian, A.

2017-12-01

The formation of aerosol mass in cloud water has been recognized as a substantial source of atmospheric aerosol mass. While sulfate formation can be relatively well constrained, the formation of secondary organic aerosol mass in the aqueous phase (aqSOA) is much more complex due to the multitude of precursors and variety in chemical processes. Aqueous phase processing adds aerosol mass to the droplet mode, which is formed due to mass addition to activated particles in clouds. In addition, it has been shown that aqSOA mass has specific characteristics in terms of oxidation state and hygroscopicity that might help to distinguish it from other SOA sources. Many models do not include detailed chemical mechanisms of sulfate and aqSOA formation and also lack details on the mass distribution of newly formed mass. Mass addition inside and outside clouds modifies different parts of an aerosol population and consequently affects predictions of properties and lifetime of particles. Using a combination of field data analysis and model studies for a variety of air masses, we will show which chemical and physical aerosol properties can be used, in order to identify an `aqueous phase signature' in processed aerosol populations. We will discuss differences in this signature in clean (e.g., background), moderately polluted (e.g., urban) and highly polluted (e.g., biomass burning) air masses and suggest air-mass-specific chemical and/or physical properties that will help to quantify the aqueous-phase derived aerosol mass.

Understanding the impact of saharan dust aerosols on tropical cyclones

NASA Astrophysics Data System (ADS)

Naeger, Aaron

Genesis of Tropical Cyclones (TCs) in the main development region for Atlantic hurricanes is tied to convection initiated by African easterly waves (AEWs) during Northern hemisphere summer and fall seasons. The main development region is also impacted by dust aerosols transported from the Sahara. It has been hypothesized that dust aerosols can modulate the development of TCs through aerosol-radiation and aerosol-cloud interaction processes. In this study, we investigate the impact of dust aerosols on TC development using the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). We first develop a technique to constrain the WRF-Chem model with a realistic three-dimensional spatial distribution of dust aerosols. The horizontal distribution of dust is specified using the Moderate Resolution Imaging Spectroradiometer (MODIS) derived aerosol products and output from the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. The vertical distribution of dust is constrained using the Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). We validate our technique through in situ aircraft measurements where both showed aerosol number concentrations from 20-30 cm-3 in the atmosphere for Saharan dust moving over the eastern Atlantic Ocean. Then, we use the satellite data constraint technique to nudge the WRF-Chem aerosol fields throughout the simulation of TC Florence developing over the eastern Atlantic Ocean during September 2006. Three different experiments are conducted where the aerosol-radiation and aerosol-cloud interaction processes are either activated or deactivated in the model while all other model options are identical between the experiments. By comparing the model experiment results, the impact of the aerosol interaction processes on TC development can be understood. The results indicate that dust aerosols can delay or prevent the development of a TC as the minimum sea level pressure of TC Florence was 13 hPa higher when the aerosols interactions were activated as opposed to deactivated in the model.

Modeling and measurements of urban aerosol processes on the neighborhood scale in Rotterdam, Oslo and Helsinki

NASA Astrophysics Data System (ADS)

Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lützenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq

2016-04-01

This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1 h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64 %. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, the model predicts that condensational growth contributes to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes predicts the change in particle number concentrations between roadside and urban background within 10 % of that predicted by the fully size-resolved MAFOR model.

On the validity of the Poisson assumption in sampling nanometer-sized aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Damit, Brian E; Wu, Dr. Chang-Yu; Cheng, Mengdawn

2014-01-01

A Poisson process is traditionally believed to apply to the sampling of aerosols. For a constant aerosol concentration, it is assumed that a Poisson process describes the fluctuation in the measured concentration because aerosols are stochastically distributed in space. Recent studies, however, have shown that sampling of micrometer-sized aerosols has non-Poissonian behavior with positive correlations. The validity of the Poisson assumption for nanometer-sized aerosols has not been examined and thus was tested in this study. Its validity was tested for four particle sizes - 10 nm, 25 nm, 50 nm and 100 nm - by sampling from indoor air withmore » a DMA- CPC setup to obtain a time series of particle counts. Five metrics were calculated from the data: pair-correlation function (PCF), time-averaged PCF, coefficient of variation, probability of measuring a concentration at least 25% greater than average, and posterior distributions from Bayesian inference. To identify departures from Poissonian behavior, these metrics were also calculated for 1,000 computer-generated Poisson time series with the same mean as the experimental data. For nearly all comparisons, the experimental data fell within the range of 80% of the Poisson-simulation values. Essentially, the metrics for the experimental data were indistinguishable from a simulated Poisson process. The greater influence of Brownian motion for nanometer-sized aerosols may explain the Poissonian behavior observed for smaller aerosols. Although the Poisson assumption was found to be valid in this study, it must be carefully applied as the results here do not definitively prove applicability in all sampling situations.« less

Combined observational and modeling efforts of aerosol-cloud-precipitation interactions over Southeast Asia

NASA Astrophysics Data System (ADS)

Loftus, Adrian; Tsay, Si-Chee; Nguyen, Xuan Anh

2016-04-01

Low-level stratocumulus (Sc) clouds cover more of the Earth's surface than any other cloud type rendering them critical for Earth's energy balance, primarily via reflection of solar radiation, as well as their role in the global hydrological cycle. Stratocumuli are particularly sensitive to changes in aerosol loading on both microphysical and macrophysical scales, yet the complex feedbacks involved in aerosol-cloud-precipitation interactions remain poorly understood. Moreover, research on these clouds has largely been confined to marine environments, with far fewer studies over land where major sources of anthropogenic aerosols exist. The aerosol burden over Southeast Asia (SEA) in boreal spring, attributed to biomass burning (BB), exhibits highly consistent spatiotemporal distribution patterns, with major variability due to changes in aerosol loading mediated by processes ranging from large-scale climate factors to diurnal meteorological events. Downwind from source regions, the transported BB aerosols often overlap with low-level Sc cloud decks associated with the development of the region's pre-monsoon system, providing a unique, natural laboratory for further exploring their complex micro- and macro-scale relationships. Compared to other locations worldwide, studies of springtime biomass-burning aerosols and the predominately Sc cloud systems over SEA and their ensuing interactions are underrepresented in scientific literature. Measurements of aerosol and cloud properties, whether ground-based or from satellites, generally lack information on microphysical processes; thus cloud-resolving models are often employed to simulate the underlying physical processes in aerosol-cloud-precipitation interactions. The Goddard Cumulus Ensemble (GCE) cloud model has recently been enhanced with a triple-moment (3M) bulk microphysics scheme as well as the Regional Atmospheric Modeling System (RAMS) version 6 aerosol module. Because the aerosol burden not only affects cloud droplet size and number concentration, but also the spectral width of the cloud droplet size distribution, the 3M scheme is well suited to simulate aerosol-cloud-precipitation interactions within a three-dimensional regional cloud model. Moreover, the additional variability predicted on the hydrometeor distributions provides beneficial input for forward models to link the simulated microphysical processes with observations as well as to assess both ground-based and satellite retrieval methods. In this presentation, we provide an overview of the 7 South East Asian Studies / Biomass-burning Aerosols and Stratocumulus Environment: Lifecycles and Interactions Experiment (7-SEAS/BASELInE) operations during the spring of 2013. Preliminary analyses of pre-monsoon Sc system lifecycles observed during the first-ever deployment of a ground-based cloud radar to northern Vietnam will be also be presented. Initial results from GCE model simulations of these Sc using double-moment and the new 3M bulk microphysics schemes under various aerosol loadings will be used to showcase the 3M scheme as well as provide insight into how the impact of aerosols on cloud and precipitation processes in stratocumulus over land may manifest themselves in simulated remote-sensing signals. Applications and future work involving ongoing 7-SEAS campaigns aimed at improving our understanding of aerosol-cloud-precipitation interactions of will also be discussed.

Atmo-metabolomics: a new measurement approach for investigating aerosol composition and ecosystem functioning.

NASA Astrophysics Data System (ADS)

Rivas-Ubach, A.; Liu, Y.; Sardans, J.; Tfaily, M. M.; Kim, Y. M.; Bourrianne, E.; Paša-Tolić, L.; Penuelas, J.; Guenther, A. B.

2016-12-01

Aerosols play crucial roles in the processes controlling the composition of the atmosphere and the functioning of ecosystems. Gaining a deeper understanding of the chemical composition of aerosols is one of the major challenges for atmospheric and climate scientists and is beginning to be recognized as important for ecological research. Better comprehension of aerosol chemistry can potentially provide valuable information on atmospheric processes such as oxidation of organics and the production of cloud condensation nuclei as well as provide an approximation of the general status of an ecosystem through the measurement of certain stress biomarkers. In this study, we describe an efficient aerosol sampling method, the metabolite extraction and the analytical procedures for the chemical characterization of aerosols, namely, the atmo-metabolome. We used mass spectrometry (MS) coupled to liquid chromatography (LC-MS), gas chromatography (GC-MS) and Fourier transform ion cyclotron resonance (FT-ICR-MS) to characterize the atmo-metabolome of two marked seasons; spring and summer. Our sampling and extraction methods demonstrated to be suitable for aerosol chemical characterization with any of the analytical platforms used in this study. The atmo-metabolome between spring and summer showed overall statistically differences. We identified several metabolites that can be attributed to pollen and other plant-related aerosols. Spring aerosols exhibit higher concentrations of metabolites linked to higher plant activity while summer samples had higher concentrations of metabolites that may reflect certain oxidative stresses in primary producers. Moreover, the elemental composition of aerosols showed clear different between seasons. Summer aerosols were generally higher in molecular weight and with higher O/C ratios, indicating higher oxidation levels and condensation of compounds relative to spring. Our method represents an advanced approach for characterizing the composition of aerosols that will benefit scientists attempting to understand complex atmospheric processes and the ecosystem status across a whole ecoregion.

Process evaluation of sea salt aerosol concentrations at remote marine locations

NASA Astrophysics Data System (ADS)

Struthers, H.; Ekman, A. M.; Nilsson, E. D.

2011-12-01

Sea salt, an important natural aerosol, is generated by bubbles bursting at the surface of the ocean. Sea salt aerosol contributes significantly to the global aerosol burden and radiative budget and are a significant source of cloud condensation nuclei in remote marine areas (Monahan et al., 1986). Consequently, changes in marine aerosol abundance is expected to impact on climate forcing. Estimates of the atmospheric burden of sea salt aerosol mass derived from chemical transport and global climate models vary greatly both in the global total and the spatial distribution (Texor et al. 2006). This large uncertainty in the sea salt aerosol distribution in turn contributes to the large uncertainty in the current estimates of anthropogenic aerosol climate forcing (IPCC, 2007). To correctly attribute anthropogenic climate change and to veraciously project future climate, natural aerosols including sea salt must be understood and accurately modelled. In addition, the physical processes that determine the sea salt aerosol concentration are susceptible to modification due to climate change (Carslaw et al., 2010) which means there is the potential for feedbacks within the climate/aerosol system. Given the large uncertainties in sea salt aerosol modelling, there is an urgent need to evaluate the process description of sea salt aerosols in global models. An extremely valuable source of data for model evaluation is the long term measurements of PM10 sea salt aerosol mass available from a number of remote marine observation sites around the globe (including the GAW network). Sea salt aerosol concentrations at remote marine locations depend strongly on the surface exchange (emission and deposition) as well as entrainment or detrainment to the free troposphere. This suggests that the key parameters to consider in any analysis include the sea surface water temperature, wind speed, precipitation rate and the atmospheric stability. In this study, the sea salt aerosol observations are analysed to quantify the key sensitivities of the processes connecting the physical drivers of sea salt aerosol to the mass tendency. The analysis employs a semi-empirical model based on the time-tendency of the aerosol mass. This approach of focusing on the time-tendency of the sea salt aerosol concentration provides a framework for the process evaluation of sea salt aerosol concentrations in global models. The same analysis methodology can be applied to output from global models. A process of comparing the sensitivity parameters derived from observations and models will reveal model inadequacies and thus guide model improvements. Carslaw, K. S., Boucher, O., Spracklen, D. V., Mann G. W., Rae, J. G. L, Woodward, S., Kulmala, M. (2010). Atmos. Chem. Phys., 10, 1701-1737 IPCC (2007). Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, Solomon, S., D. Monahan, E. C., Spiel, D. E., Davidson, K. L. (1986) Oceanic Whitecaps ed. Monahan E. C. & MacNiochaill, D. Reidel, Norwell, Mass. Texor, C., et al. (2006) Atmos. Chem. Phys., 6, 1777-1813.

Impact of Asian Aerosols on Precipitation Over California: An Observational and Model Based Approach

NASA Technical Reports Server (NTRS)

Naeger, Aaron R.; Molthan, Andrew L.; Zavodsky, Bradley T.; Creamean, Jessie M.

2015-01-01

Dust and pollution emissions from Asia are often transported across the Pacific Ocean to over the western United States. Therefore, it is essential to fully understand the impact of these aerosols on clouds and precipitation forming over the eastern Pacific and western United States, especially during atmospheric river events that account for up to half of California's annual precipitation and can lead to widespread flooding. In order for numerical modeling simulations to accurately represent the present and future regional climate of the western United States, we must account for the aerosol-cloud-precipitation interactions associated with Asian dust and pollution aerosols. Therefore, we have constructed a detailed study utilizing multi-sensor satellite observations, NOAA-led field campaign measurements, and targeted numerical modeling studies where Asian aerosols interacted with cloud and precipitation processes over the western United States. In particular, we utilize aerosol optical depth retrievals from the NASA Moderate Resolution Imaging Spectroradiometer (MODIS), NOAA Geostationary Operational Environmental Satellite (GOES-11), and Japan Meteorological Agency (JMA) Multi-functional Transport Satellite (MTSAT) to effectively detect and monitor the trans-Pacific transport of Asian dust and pollution. The aerosol optical depth (AOD) retrievals are used in assimilating the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) in order to provide the model with an accurate representation of the aerosol spatial distribution across the Pacific. We conduct WRF-Chem model simulations of several cold-season atmospheric river events that interacted with Asian aerosols and brought significant precipitation over California during February-March 2011 when the NOAA CalWater field campaign was ongoing. The CalWater field campaign consisted of aircraft and surface measurements of aerosol and precipitation processes that help extensively validate our WRF-Chem model simulations. After validating the capability of the WRF-Chem in realistically simulating the aerosol-cloud precipitation interactions, we conduct sensitivity studies where the AOD is doubled to diagnose whether an increasing concentration of Asian aerosols over the western United States will lead to further impacts on the cloud and precipitation processes over California. We also perform sensitivity studies where the aerosols will be partitioned into dust-only and pollution-only in order to separate the impacts of the differing Asian aerosol species. The results of our WRF-Chem model simulations aim to show that the trans-Pacific transport of Asian aerosols influence the precipitation associated with atmospheric river events that can ultimately impact the regional climate of the western United States. 1 University

Host Model Uncertainty in Aerosol Radiative Effects: the AeroCom Prescribed Experiment and Beyond

NASA Astrophysics Data System (ADS)

Stier, Philip; Schutgens, Nick; Bian, Huisheng; Boucher, Olivier; Chin, Mian; Ghan, Steven; Huneeus, Nicolas; Kinne, Stefan; Lin, Guangxing; Myhre, Gunnar; Penner, Joyce; Randles, Cynthia; Samset, Bjorn; Schulz, Michael; Yu, Hongbin; Zhou, Cheng; Bellouin, Nicolas; Ma, Xiaoyan; Yu, Fangqun; Takemura, Toshihiko

2013-04-01

Anthropogenic and natural aerosol radiative effects are recognized to affect global and regional climate. Multi-model "diversity" in estimates of the aerosol radiative effect is often perceived as a measure of the uncertainty in modelling aerosol itself. However, current aerosol models vary considerably in model components relevant for the calculation of aerosol radiative forcings and feedbacks and the associated "host-model uncertainties" are generally convoluted with the actual uncertainty in aerosol modelling. In the AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in eleven participating models. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention. However, uncertainties in aerosol radiative effects also include short-term and long-term feedback processes that will be systematically explored in future intercomparison studies. Here we will present an overview of the proposals for discussion and results from early scoping studies.

Contribution of Primary and Secondary Sources to Organic Aerosol and PM2.5 at SEARCH Network Sites

EPA Science Inventory

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. La...

Microphysical processing of aerosol particles in orographic clouds

NASA Astrophysics Data System (ADS)

Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number concentration.

Building America Case Study: Apartment Compartmentalization with an Aerosol-Based Sealing Process - Queens, NY; Technology Solutions for New and Existing Homes, Energy Efficiency & Renewable Energy (EERE)

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

2015-07-01

Air sealing of building enclosures is a difficult and time-consuming process. Current methods in new construction require laborers to physically locate small and sometimes large holes in multiple assemblies and then manually seal each of them. The innovation demonstrated under this research study was the automated air sealing and compartmentalization of buildings through the use of an aerosolized sealant, developed by the Western Cooling Efficiency Center at University of California Davis.CARB sought to demonstrate this new technology application in a multifamily building in Queens, NY. The effectiveness of the sealing process was evaluated by three methods: air leakage testing ofmore » overall apartment before and after sealing, point-source testing of individual leaks, and pressure measurements in the walls of the target apartment during sealing. Aerosolized sealing was successful by several measures in this study. Many individual leaks that are labor-intensive to address separately were well sealed by the aerosol particles. In addition, many diffuse leaks that are difficult to identify and treat were also sealed. The aerosol-based sealing process resulted in an average reduction of 71% in air leakage across three apartments and an average apartment airtightness of 0.08 CFM50/SF of enclosure area.« less

Impacts of aerosol mitigation on Chinese rice photosynthesis: An integrated modeling approach

NASA Astrophysics Data System (ADS)

Zhang, T.; Li, T.; Yue, X.; Yang, X.

2017-12-01

Aerosol pollution in China is significantly altering radiative transfer processes and is thereby potentially affecting rice photosynthesis. However, the response of rice photosynthesis to aerosol-induced radiative perturbations is still not well understood. Here, we employ an integrated process-based modeling approach to simulate changes in incoming radiation (RAD) and the diffuse radiation fraction (DF) with aerosol mitigation in China and their associated impacts on rice yields. Aerosol reduction has the positive effect of increasing RAD and the negative effect of decreasing DF on rice photosynthesis and yields. In rice production areas where the average RAD during the growing season is lower than 250 W m-2, aerosol reduction is beneficial for higher rice yields, whereas in areas with RAD>250 W m-2, aerosol mitigation causes yield declines due to the associated reduction in the DF, which decreases the light use efficiency. This response pattern and threshold are similar with observations, even through more data are needed in future investigation. As a net effect, rice yields were estimated to significantly increase by 0.8-2.6% with aerosol concentrations reductions from 20 to 100%, which is lower than the estimates obtained in earlier studies that only considered the effects of RAD. This finding suggests that both RAD and DF are important processes influencing rice yields and should be incorporated into future assessments of agricultural responses to variations in aerosol-induced radiation under climate change.

Field and Laboratory Studies of Atmospheric Organic Aerosol

NASA Astrophysics Data System (ADS)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of these conditions to all measurements conducted during E-PEACE demonstrated that a large fraction of cloud droplet (72%) and dry aerosol mass (12%) sampled in the California coastal study region was heavily or moderately influenced by ship emissions. Another study investigated the chemical and physical evolution of a controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed of oxidized organic compounds contributed nearly an order of magnitude more cloud condensation nuclei (CCN) than less oxidized particles formed under cloudy conditions. The processing time necessary for particles to become CCN active was short ( 4 hr). Laboratory chamber experiments were also conducted to evaluate particle-phase processes influencing aerosol phase and composition. In one study, ammonium sulfate seed was coated with a layer of secondary organic aerosol (SOA) from toluene oxidation followed by a layer of SOA from α-pinene oxidation. The system exhibited different evaporative properties than ammonium sulfate seed initially coated with α-pinene SOA followed by a layer of toluene SOA. This behavior is consistent with a shell-and-core model and suggests limited mixing among different SOA types. Another study investigated the reactive uptake of isoprene epoxy diols (IEPOX) onto non-acidified aerosol. It was demonstrated that particle acidity has limited influence on organic aerosol formation onto ammonium sulfate seed, and that the chemical system is limited by the availability of nucleophiles such as sulfate. Flow tube experiments were conducted to examine the role of iron in the reactive uptake and chemical oxidation of glycolaldehyde. Aerosol particles doped with iron and hydrogen peroxide were mixed with gas-phase glycolaldehyde and photochemically aged in a custom-built flow reactor. Compared to particles free of iron, iron-doped aerosols significantly enhanced the oxygen to carbon (O/C) ratio of accumulated organic mass. The primary oxidation mechanism is suggested to be a combination of Fenton and photo-Fenton reactions which enhance particle-phase OH radical concentrations.

422nd Brookhaven Lecture. Aerosols, Clouds and Climate: From Micro to Micro

ScienceCinema

Yangang Liu

2018-01-05

As scientists who study aerosols, clouds, and precipitation know, particles in the atmosphere interact with one another and affect the Earth's climate through a myriad of complex processes. Learn more about this topic from Yangang Liu as he presents "Aerosols, Clouds, and Climate: From Micro to Macro."

The application of chemical and isotopic tracers to characterize aerosol sources and processing in marine air

NASA Astrophysics Data System (ADS)

Turekian, Vaughan Charles

2000-12-01

Aerosol production, transport, chemical and physical evolution and deposition impact the environment by influencing radiation budgets, altering the composition of the atmosphere, and delivering nutrients to marine and terrestrial ecosystems. The objective of this research was to combine high-resolution chemical measurements with stable isotopic analysis in order to characterize the sources and processing of carbon, nitrogen and sulfur bearing compounds, associated with sized aerosols on Bermuda, during spring. Chemical tracers combined with forward and backward trajectories demonstrated the transport of biomass burning products from North America to Bermuda. The size distributions of NH4+ from 1998 differed from those during spring, 1997, a year without the large-scale burning. These results suggest that transport of biomass burning products altered the pH of the aerosols. Marine and continentally derived carbon was associated with all aerosol size fractions. Supermicron radius sea- salt aerosol was enriched in marine derived carbon by 2 orders of magnitude compared to bulk surface seawater. Enrichments of oxalate relative to methanesulfonic acid (MSA) in supermicron radius aerosol suggested in situ formation of oxalate within the sea-salt solution, or direct injection from the organic rich surface microlayer. Compound specific isotope analysis of oxalic acid, indicated a marine source for all aerosol size fractions, indicating formation from in the gas phase for the submicron radius aerosol. Stable sulfur isotopes indicated that the biogenic non- sea-salt (nss) SO42-/MSA ratio varied with aerosol size indicating that MSA may not be a conservative tracer of biogenic nss SO4 2- in bulk aerosol sampling. The calculated biogenic nss SO 42-/MSA based on stable isotopes and sized aerosol sampling, was 3 times lower than previous estimates for Bermuda. Stable nitrogen isotope values for submicron and supermicron aerosol where significantly different, consistent with their different chemical compositions. Results suggested that HNO3 incorporation into supermicron aerosol was essentially unidirectional whereas submicron aerosol was both a source and a sink for NH3(g). Variable aerosol liquid water content over the relatively longer atmospheric lifetimes of submicron aerosol may lead to multiple NH3 phase changes. This study was the first to combine sized aerosol sampling, high-resolution chemical analysis and multiple stable isotopes to characterize both the sources and the processing of aerosols in marine air. The results of this study, therefore, provide crucial information for source apportionment of environmentally important atmospheric species in continentally impacted, marine air.

Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsui, H.; Koike, Makoto; Kondo, Yutaka

2014-09-30

Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we developed an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 µm to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particlesmore » with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module was implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials was about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement was estimated to be 10 – 20% over northern East Asia and 20 – 35% over southern East Asia. A clear north-south contrast was also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increased CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increased CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also showed that the impact of each process on each optical and radiative parameter depended strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA processes under different meteorological conditions and emissions.« less

Anthropogenic and Biogenic Emissions, and their Contributions to Summertime Haze in the Southeast U.S.: Results from the NOAA SENEX Study in 2013

NASA Astrophysics Data System (ADS)

De Gouw, J. A.

2015-12-01

The NOAA Southeast Nexus of Air Quality and Climate Change (SENEX) study was focused on biogenic and anthropogenic emissions in the Southeast United States, their interactions to form oxidants and aerosol, and the implications of these processes for air quality and climate. For SENEX, the NOAA WP-3D research aircraft was deployed out of a regional airport in Smyrna, Tennessee during June and July of 2013. The aircraft carried an extensive suite of instruments to characterize the gas- and aerosol-phase composition of the atmosphere, as well as the climate-relevant properties of the aerosol. The SENEX study was performed in close collaboration with several other studies in the framework of the Southeast Atmosphere Study. Some highlights of the measurements will be presented with a particular focus on the processes by which anthropogenic and biogenic emissions interact to form secondary species including aerosol. The FLEXPART Lagrangian transport model was found to be a useful tool to quantify the relative contribution from anthropogenic and biogenic emissions to different trace species in the sampled air masses. Observations in power plant plumes provided constraints on the dependence of hydroxyl radical concentrations on nitrogen oxides (NOx). Oxidation rates were higher at enhanced concentrations of NOx, leading to faster production of products from biogenic volatile organic compounds (VOCs) in polluted conditions. Organic aerosol was formed from isoprene downwind from one power plant that had relatively high sulfur emissions. Nighttime flights were conducted to constrain organic aerosol formation from the reaction between biogenic VOCs and nitrate radicals. The volume of aerosol water depends on aerosol composition (e.g. sulfate versus organics), which has been proposed as a link between anthropogenic emissions and products of aqueous-phase chemistry. Vertical profiles of aerosol volume and composition provided evidence for aqueous-phase formation of sulfate aerosol, but formation of organic aerosol was not significant within the uncertainties of the analysis.

Global CALIPSO Observations of Aerosol Changes Near Clouds

NASA Technical Reports Server (NTRS)

Varnai, Tamas; Marshak, Alexander

2011-01-01

Several recent studies have found that clouds are surrounded by a transition zone of rapidly changing aerosol optical properties and particle size. Characterizing this transition zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects, and also for improving satellite retrievals of aerosol properties. This letter presents a statistical analysis of a monthlong global data set of Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations over oceans. The results show that the transition zone is ubiquitous over all oceans and extends up to 15 km away from clouds. They also show that near-cloud enhancements in backscatter and particle size are strongest at low altitudes, slightly below the top of the nearest clouds. Also, the enhancements are similar near illuminated and shadowy cloud sides, which confirms that the asymmetry of Moderate Resolution Imaging Spectroradiometer reflectances found in an earlier study comes from 3-D radiative processes and not from differences in aerosol properties. Finally, the effects of CALIPSO aerosol detection and cloud identification uncertainties are discussed. The findings underline the importance of accounting for the transition zone to avoid potential biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.

Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (~2700 m a.s.l.) as well as near their sources using an aircraft. In addition, the regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), anmore » index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (~1 h old) and emissions sampled after atmospheric transport (6–45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. In conclusion, these results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate.« less

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign

DOE PAGES

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.; ...

2016-07-11

Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (~2700 m a.s.l.) as well as near their sources using an aircraft. In addition, the regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), anmore » index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (~1 h old) and emissions sampled after atmospheric transport (6–45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. In conclusion, these results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate.« less

Aerosol studies with Listeria innocua and Listeria monocytogenes.

PubMed

Zhang, Guodong; Ma, Li; Oyarzabal, Omar A; Doyle, Michael P

2007-08-01

Aerosol studies of Listeria monocytogenes in food processing plants have been limited by lack of a suitable surrogate microorganism. The objective of this study was to investigate the potential of using green fluorescent protein-labeled strains of Listeria innocua as a surrogate for L. monocytogenes for aerosol studies. These studies were conducted in a laboratory bioaerosol chamber and a pilot food-processing facility. Four strains of L. innocua and five strains of L. monocytogenes were used. In the laboratory chamber study, Listeria cells were released into the environment at two different cell numbers and under two airflow conditions. Trypticase soy agar (TSA) plates and oven-roasted breasts of chicken and turkey were placed in the chamber to monitor Listeria cell numbers deposited from aerosols. A similar experimental design was used in the pilot plant study; however, only L. innocua was used. Results showed that L. monocytogenes and L. innocua survived equally well on chicken and turkey breast meats and TSA plates. No-fan and continuous fan applications, which affected airflow, had no significant effect on settling rates of aerosolized L. monocytogenes and L. innocua in the bioaerosol chamber or L. innocua in the pilot plant study. Listeriae cell numbers in the air decreased rapidly during the first 1.5 h following release, with few to no listeriae detected in the air at 3 h. Aerosol particles with diameters of 1 and 2 microM correlated directly with the number of Listeria cells in the aerosol but not with particles that were 0.3, 0.5, and 5 microM in diameter. Results indicate that L. innocua can be used as a surrogate for L. monocytogenes in an aerosol study.

Impact of Aerosols on Convective Clouds and Precipitation

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong; Li, Xiaowen

2012-01-01

Aerosols are a critical.factor in the atmospheric hydrological cycle and radiation budget. As a major agent for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosols have a major impact on the dynamics, microphysics, and electrification properties of continental mixed-phase convective clouds. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing a significant source of cloud condensation nuclei (CCN). Such pollution . effects on precipitation potentially have enormous climatic consequences both in terms of feedbacks involving the land surface via rainfall as well as the surface energy budget and changes in latent heat input to the atmosphere. Basically, aerosol concentrations can influence cloud droplet size distributions, the warm-rain process, the cold-rain process, cloud-top heights, the depth of the mixed-phase region, and the occurrence of lightning. Recently, many cloud resolution models (CRMs) have been used to examine the role of aerosols on mixed-phase convective clouds. These modeling studies have many differences in terms of model configuration (two- or three-dimensional), domain size, grid spacing (150-3000 m), microphysics (two-moment bulk, simple or sophisticated spectral-bin), turbulence (1st or 1.5 order turbulent kinetic energy (TKE)), radiation, lateral boundary conditions (i.e., closed, radiative open or cyclic), cases (isolated convection, tropical or midlatitude squall lines) and model integration time (e.g., 2.5 to 48 hours). Among these modeling studies, the most striking difference is that cumulative precipitation can either increase or decrease in response to higher concentrations of CCN. In this presentation, we review past efforts and summarize our current understanding of the effect of aerosols on convective precipitation processes. Specifically, this paper addresses the following topics: observational evidence of the effect of aerosols on precipitation processes, and results from (CRM) simulations. Note that this presentation is mainly based on a recent paper published in Geophy. Rev. (Tao et al. 2012).

Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi

NASA Astrophysics Data System (ADS)

Kumar, Sudhanshu

2012-07-01

{Identifying Metals as Marker for Waste Burning Aerosol Particles in New Delhi } Tracing of aerosol sources is an important task helpful for making control strategy, and for climate change study. However, it is a difficult job as aerosols have several sources, involve in complex atmospheric processing, degradation and removal processes. Several approaches have been used for this task, e.g., models, which are based on the input of chemical species; stable- and radio-isotope compositions of certain species; chemical markers in which trace metals are the better options because they persist in atmosphere until the life of a particle. For example, K and Hg are used for biomass and coal burning tracings, respectively. Open waste burning has recently been believed to be a considerable source of aerosols in several mega cities in India and China. To better understand this source contribution in New Delhi aerosols, we have conducted aerosol sampling at a landfill site (Okhla), and in proximity (within 1 km distance) of this site. Aerosol filter samples were acid digested in microwave digestion system and analyzed using inductively coupled plasma -- high resolution mass spectrometry (ICP-HRMS) for getting metal signatures in particles. The metals, e.g., Sn, Sb and As those are found almost negligible in remote aerosols, are maximized in these waste burning aerosols. Sample collected in other location of New Delhi also shows the considerable presence of these metals in particles. Preliminary studies of isotopic ratios of these metals suggested that these metals, especially Sn can be used as marker for tracing the open waste burning sources of aerosols in New Delhi.

Ambient Observations of the Soot Aging Process during the SHARP Intensive Field Campaign

NASA Astrophysics Data System (ADS)

Reed, C.; Collins, D. R.; Khalizov, A. F.; Zheng, J.; Zhang, R.

2009-12-01

Soot aerosols affect climate both directly through absorption of solar radiation and indirectly by potentially serving as cloud condensation nuclei. Among the sources of uncertainty surrounding the effects of soot aerosol on the environment is the lack of scientific insight into the soot aging process, in which soot particles develop a coating of secondary species such as sulfates, ammonium, nitrate, and organics. Such processes may alter the behavior of soot by modifying particle morphology over time leading to changes in chemical, physical and scattering properties of the aerosol. However, it is often difficult to quantify such processes in the ambient environment due to the complex composition and spatial and temporal variability of the atmospheric aerosol. In order to better understand the effects of the environment on soot particles, it is desirable to study the processes responsible for their transformation in the ambient air without influence from variability in source region and history prior to sampling. To achieve this, the overall soot aging process in the ambient environment was physically isolated utilizing environmental chambers. Chamber measurements were conducted on the Moody Tower at the University of Houston using The Ambient Aerosol Chamber for Evolution Studies (AACES) during the SHARP campaign. AACES is a roughly cubical chamber constructed of a rigid acrylic outer shell, which transmits UV radiation both in the UV-B and UV-A ranges. FEP Teflon lines the inside of the chamber on all sides and the top, while expanded-PTFE (ePTFE) Teflon is used on the bottom of the chamber. The fibrous structure of the ePTFE acts as a barrier to particulates, while allowing gas molecules to move virtually unimpeded from the surrounding air into the chamber, creating an environment inside the chamber that is initially free of particles and continuously mimics the local ambient air. In order to study the effects of the soot aging process, a non-premixed propane flame was used to generate a polydisperse fresh soot aerosol. Then, using a differential mobility analyzer, a monodisperse, uncharged soot aerosol was injected into the environmental chamber. Observations of particle concentration, size, hygroscopicity, effective density, and light extinction and scattering properties were carried out over time using a tandem differential mobility analyzer system, an aerosol particle mass analyzer, a nephelometer and a cavity ringdown spectrometer. Results from preliminary analysis of the data collected during the campaign will be presented.

Evaluating WRF-Chem multi-scale model in simulating aerosol radiative properties over the tropics – A case study over India

DOE Office of Scientific and Technical Information (OSTI.GOV)

Seethala, C.; Pandithurai, G.; Fast, Jerome D.

We utilized WRF-Chem multi-scale model to simulate the regional distribution of aerosols, optical properties and its effect on radiation over India for a winter month. The model is evaluated using measurements obtained from upper-air soundings, AERONET sun photometers, various satellite instruments, and pyranometers operated by the Indian Meteorological Department. The simulated downward shortwave flux was overestimated when the effect of aerosols on radiation and clouds was neglected. Downward shortwave radiation from a simulation that included aerosol-radiation interaction processes was 5 to 25 Wm{sup -2} closer to the observations, while a simulation that included aerosol-cloud interaction processes were another 1 tomore » 20 Wm{sup -2} closer to the observations. For the few observations available, the model usually underestimated particulate concentration. This is likely due to turbulent mixing, transport errors and the lack of secondary organic aerosol treatment in the model. The model efficiently captured the broad regional hotspots such as high aerosol optical depth over Indo-Gangetic basin as well as the northwestern and southern part of India. The regional distribution of aerosol optical depth compares well with AVHRR aerosol optical depth and the TOMS aerosol index. The magnitude and wavelength-dependence of simulated aerosol optical depth was also similar to the AERONET observations across India. Differences in surface shortwave radiation between simulations that included and neglected aerosol-radiation interactions were as high as -25 Wm{sup -2}, while differences in surface shortwave radiation between simulations that included and neglect aerosol-radiation-cloud interactions were as high as -30 Wm{sup -2}. The spatial variations of these differences were also compared with AVHRR observation. This study suggests that the model is able to qualitatively simulate the impact of aerosols on radiation over India; however, additional measurements of particulate mass and composition are needed to fully evaluate whether the aerosol precursor emissions are adequate when simulating radiative forcing in the region.« less

A 3-D Model Study of Aerosol Composition and Radiative Forcing in the Asian-Pacific Region

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Torres, Omar; Zhao, Xuepeng; Einaudi, Franco (Technical Monitor)

2000-01-01

The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model will be used in analyzing the aerosol data in the ACE-Asia program. Our objectives are (1) to understand the physical, chemical, and optical properties of aerosol and the processes that control these properties over the Asian-Pacific region, (2) to determine the aerosol radiative forcing over the Asian-Pacific region, and (3) to investigate the interaction between aerosol and tropospheric chemistry. We will present the GOCART aerosol simulations of sulfate, dust, carbonaceous, and sea salt concentrations, their optical thicknesses, and their radiative effects. We will also show the comparisons of model results with data taken from previous field campaigns, ground-based sun photometer measurements, and satellite observations. Finally, we will present our plan for the ACE-Asia study.

2-Hydroxyterpenylic acid: An oxygenated marker compound for a-pinene secondary organic aerosol in ambient fine aerosol

EPA Science Inventory

An oxygenated MW 188 compound is commonly observed in substantial abundance in atmospheric aerosol samples and was proposed in previous studies as an α-pinene-related marker compound that is associated with aging processes. Owing to difficulties in producing this compound in suff...

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

NASA Technical Reports Server (NTRS)

Mazurek, Monica A.; Cofer, Wesley R., III; Levine, Joel S.

1991-01-01

During the boreal forest burn studied, the ambient concentrations for the particle carbon smoke aerosol are highest for the full-fire burn conditions and vary significantly throughout the burn. Collection strategies must accordingly define ranges in the smoke aerosol concentrations produced. While the highest elemental C concentrations are observed during full-fire conditions, the great majority of smoke aerosol particles are in the form of organic C particles irrespective of fire temperature. The formation of organic C light-scattering particles was a significant process in the burn studied.

Final Report: Process Models of the Equilibrium Size & State of Organic/Inorganic Aerosols for the Development of Large Scale Atmospheric Models & the Analysis of Field Data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wexler, Anthony Stein; Clegg, Simon Leslie

2013-10-26

Our work addressed the following elements of the Call for Proposals: (i) “to improve the theoretical representation of aerosol processes studied in ASP laboratory or field studies”, (ii) “to enhance the incorporation of aerosol process information into modules suitable for large-scale or global atmospheric models”, and (iii) “provide systematic experimental validation of process model predictions ... using data from targeted laboratory and field experiments”. Achievements to the end of 2012 are described in four previous reports, and include: new models of densities and surface tensions of pure (single solute) and mixed aqueous solutions of typical aerosol composition under all atmosphericmore » conditions (0 to 100% RH and T > 150 K); inclusion of these models into the widely used Extended Aerosol Inorganics model (E-AIM, http://www.aim.env.uea.ac.uk/aim/aim.php); the addition of vapor pressure calculators for organic compounds to the E-AIM website; the ability of include user-defined organic compounds and/or lumped surrogates in gas/aerosol partitioning calculations; the development of new equations to represent the properties of soluble aerosols over the entire concentration range (using methods based upon adsorption isotherms, and derived using statistical mechanics), including systems at close to zero RH. These results are described in publications 1-6 at the end of this report, and on the “News” page of the E-AIM website (http://www.aim.env.uea.ac.uk/aim/info/news.html). During 2012 and 2013 we have collaborated in a combined observation and lab-based study of the water uptake of the organic component of atmospheric aerosols (PI Gannet Hallar, of the Desert Research Institute). The aerosol samples were analyzed using several complementary techniques (GC/MS, FT-ICR MS, and ion chromatography) to produce a very complete organic “speciation” including both polar and non-polar compounds. Hygroscopic growth factors of the samples were measured, and we have just completed comparisons of the data with our process model predictions based upon the inorganic and organic composition of the samples.« less

Effect of Heterogeneous Chemical Reactions on the Köhler Activation of Aqueous Organic Aerosols.

PubMed

Djikaev, Yuri S; Ruckenstein, Eli

2018-05-03

We study some thermodynamic aspects of the activation of aqueous organic aerosols into cloud droplets considering the aerosols to consist of liquid solution of water and hydrophilic and hydrophobic organic compounds, taking into account the presence of reactive species in the air. The hydrophobic (surfactant) organic molecules on the surface of such an aerosol can be processed by chemical reactions with some atmospheric species; this affects the hygroscopicity of the aerosol and hence its ability to become a cloud droplet either via nucleation or via Köhler activation. The most probable pathway of such processing involves atmospheric hydroxyl radicals that abstract hydrogen atoms from hydrophobic organic molecules located on the aerosol surface (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). These two reactions play a crucial role in the enhancement of the Köhler activation of the aerosol and its evolution into a cloud droplet. Taking them and a third reaction (next in the multistep chain of relevant heterogeneous reactions) into account, one can derive an explicit expression for the free energy of formation of a four-component aqueous droplet on a ternary aqueous organic aerosol as a function of four independent variables of state of a droplet. The results of numerical calculations suggest that the formation of cloud droplets on such (aqueous hydrophilic/hydrophobic organic) aerosols is most likely to occur as a Köhler activation-like process rather than via nucleation. The model allows one to determine the threshold parameters of the system necessary for the Köhler activation of such aerosols, which are predicted to be very sensitive to the equilibrium constant of the chain of three heterogeneous reactions involved in the chemical aging of aerosols.

Seasonality of Forcing by Carbonaceous Aerosols

NASA Astrophysics Data System (ADS)

Habib, G.; Bond, T.; Rasch, P. J.; Coleman, D.

2006-12-01

Aerosols can influence the energy balance of Earth-Atmosphere system with profound effect on regional climate. Atmospheric processes, such as convection, scavenging, wet and dry deposition, govern the lifetime and location of aerosol; emissions affect its quantity and location. Both affect climate forcing. Here we investigate the effect of seasonality in emissions and atmospheric processes on radiative forcing by carbonaceous aerosols, focusing on aerosol from fossil fuel and biofuel. Because aerosol lifetime is seasonal, ignoring the seasonality of sources such as residential biofuel may introduce a bias in aerosol burden and therefore in predicted climate forcing. We present a global emission inventory of carbonaceous aerosols with seasonality, and simulate atmospheric concentrations using the Community Atmosphere Model (CAM). We discuss where and when the seasonality of emissions and atmospheric processes has strong effects on atmospheric burden, lifetime, climate forcing and aerosol optical depth (AOD). Previous work has shown that aerosol forcing is higher in summer than in winter, and has identified the importance of aerosol above cloud in determining black carbon forcing. We show that predicted cloud height is a very important factor in determining normalized radiative forcing (forcing per mass), especially in summer. This can affect the average summer radiative forcing by nearly 50%. Removal by cloud droplets is the dominant atmospheric cleansing mechanism for carbonaceous aerosols. We demonstrate the modeled seasonality of removal processes and compare the importance of scavenging by warm and cold clouds. Both types of clouds contribute significantly to aerosol removal. We estimate uncertainty in direct radiative forcing due to scavenging by tagging the aerosol which has experienced cloud interactions. Finally, seasonal variations offer an opportunity to assess modeled processes when a single process dominates variability. We identify regions where aerosol burden is most sensitive to convection and scavenging in warm and cold clouds, and compare seasonally modeled AOD with that retrieved by the Moderate Resolution Imaging Spectroradiometer (MODIS).

The Southeast Atmosphere Studies (SAS): coordinated investigation and discovery to answer critical questions about fundamental atmospheric processes

EPA Science Inventory

The Southeast Atmosphere Studies (SAS), encompassing the Southern Oxidant and Aerosol Study (SOAS), the Southeast Nexus of Air Quality and Climate (SENEX) study, the Nitrogen, Oxidants, Mercury and Aerosols: Distributions, Sources and Sinks (NOMADSS) study deployed in the field f...

Cloud and Radiation Mission with Active and Passive Sensing from the Space Station

NASA Technical Reports Server (NTRS)

Spinhirne, James D.

1998-01-01

A cloud and aerosol radiative forcing and physical process study involving active laser and radar profiling with a combination of passive radiometric sounders and imagers would use the space station as an observation platform. The objectives are to observe the full three dimensional cloud and aerosol structure and the associated physical parameters leading to a complete measurement of radiation forcing processes. The instruments would include specialized radar and lidar for cloud and aerosol profiling, visible, infrared and microwave imaging radiometers with comprehensive channels for cloud and aerosol observation and specialized sounders. The low altitude,. available power and servicing capability of the space station are significant advantages for the active sensors and multiple passive instruments.

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

NASA Astrophysics Data System (ADS)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

a Study on the Physical and Chemical Properties of Stratospheric Aerosols.

NASA Astrophysics Data System (ADS)

Tabazadeh, Azadeh

The physical and chemical properties of stratospheric aerosols under background and perturbed conditions are discussed. First, a multi-component aerosol physical chemistry model was developed to study the composition and reactivity of stratospheric aerosols. The compositions are predicted from an equilibrium assumption between the condensed-and gas-phases, and they are calculated as a function of ambient temperature, relative humidity, and the total mass of nitric acid and sulfuric acid present per unit volume of air. The water and solute activity parameters in the aerosol model are derived from various laboratory sources, and the set of equilibrium equations are solved using a unique numerical scheme. The aerosol model is applied to study the formation of nitric acid-containing aerosols in the stratosphere. Also, the equilibrium compositions are used to estimate the extent of aqueous phase processing of chlorine species in the aerosol solutions. This processing can contribute to the depletion of the stratospheric ozone layer, especially after major volcanic eruptions where sulfate aerosols are more abundant. Second, a surface chemistry model was constructed that includes Langmuir trace-gas adsorption and desorption, Brunauer, Emmett and Teller adsorption of water vapor, surface poisoning, solvation and diffusion of molecules on the surface, chemical activation and reaction of adsorbates, and product desorption or reaction. This model is used to study the effects of relative humidity and other physical parameters on the efficiency of heterogeneous chemical processes which occur on the surfaces of solid polar stratospheric clouds. These heterogeneous chemical processes are responsible for the formation of the "ozone hole", can contribute to global ozone depletion, and may have tropospheric significance. Finally, a fluid dynamics and thermodynamics model of volcanic eruption columns was used to develop a scheme for predicting the extent of HCl removal from volcanic plumes. If most of the volcanically emitted chlorine stays in the upper atmosphere, the chlorine concentration in the stratosphere could increase by a factor of 2 to 10, leading to severe global ozone depletions. However, model results indicate that HCl is efficiently scavenged from volcanic plumes by supercooled water droplets, which form as the plume lofts and cools. HCl dissolution in these drops, followed by rainout, prevents substantial injections of chlorine into the stratosphere.

Review of Aerosol–Cloud Interactions: Mechanisms, Significance, and Challenges

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Wang, Yuan; Rosenfeld, Daniel

2016-11-01

Over the past decade, the number of studies that investigate aerosol-cloud interactions has increased considerably. Although tremendous progress has been made to improve our understanding of basic physical mechanisms of aerosol-cloud interactions and reduce their uncertainties in climate forcing, we are still in poor understanding of (1) some of the mechanisms that interact with each other over multiple spatial and temporal scales, (2) the feedback between microphysical and dynamical processes and between local-scale processes and large-scale circulations, and (3) the significance of cloud-aerosol interactions on weather systems as well as regional and global climate. This review focuses on recent theoreticalmore » studies and important mechanisms on aerosol-cloud interactions, and discusses the significances of aerosol impacts on raditative forcing and precipitation extremes associated with different cloud systems. Despite significant understanding has been gained about aerosol impacts on the main cloud types, there are still many unknowns especially associated with various deep convective systems. Therefore, large efforts are needed to escalate our understanding. Future directions should focus on obtaining concurrent measurements of aerosol properties, cloud microphysical and dynamic properties over a range of temporal and spatial scales collected over typical climate regimes and closure studies, as well as improving understanding and parameterizations of cloud microphysics such as ice nucleation, mixed-phase properties, and hydrometeor size and fall speed« less

Identification and Mitigation of Generated Solid By-Products during Advanced Electrode Materials Processing

DOE PAGES

Tsai, Candace S. J.; Dysart, Arthur D.; Beltz, Jay H.; ...

2015-12-30

A scalable, solid-state elevated temperature process was developed to produce high capacity carbonaceous electrode materials for energy storage devices via decomposition of starch-based precursor in an inert atmosphere. The fabricated carbon-based architectures are useful as an excellent electrode material for lithium-ion, sodium-ion and lithium-sulfur batteries. This article focuses on the study and analysis of the formed nanometer-sized byproducts during the lab-scale production of carbonaceous electrode materials in the process design phase. The complete material production process was studied by operation, namely during heating, holding the reaction at elevated temperature, followed by cooling. The unknown downstream particles in the process exhaustmore » were collected and characterized via aerosol and liquid suspensions, and they were quantified using direct-reading instruments for number and mass concentrations. The airborne emissions were collected on polycarbonate filters and TEM grids using the Tsai diffusion sampler (TDS) for characterization and further analysis. Released byproduct aerosols collected in a deionized (DI) water trap were analyzed using a Nanosight real time nanoparticle characterization system and the aerosols emitted post water suspension were collected and characterized. Individual particles in the nanometer size range were found in exhaust aerosols, however, crystal structured aggregates were formed on the sampling substrate after a long-term sampling of emitted exhaust. After characterizing the released aerosol byproducts, methods were also identified to mitigate possible human and environmental exposures upon the industrial implementation of such a process.« less

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Collier, Sonya; Zhou, Shan; Onasch, Timothy B.

Abstract Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, wildfire emissions in the Pacific Northwest region of the United States were characterized using real-time measurements near their sources using an aircraft, and farther downwind from a fixed ground site located at the Mt. Bachelor Observatory (~ 2700 m a.s.l.). The characteristics of aerosol emissions were found to depend strongly on the modified combustion efficiency (MCE), a qualitative index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereasmore » the carbon oxidation state of organic aerosol increased with MCE. The relationships between the aerosol properties and MCE were consistent between fresher emissions (~1 hour old) and emissions sampled after atmospheric transport (6 - 45 hours), suggesting that organic aerosol mass loading and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of regionally transported wildfire emissions and their impacts on regional air quality and global climate.« less

Contrasting influences of aerosols on cloud properties during deficient and abundant monsoon years

PubMed Central

Patil, Nitin; Dave, Prashant; Venkataraman, Chandra

2017-01-01

Direct aerosol radiative forcing facilitates the onset of Indian monsoon rainfall, based on synoptic scale fast responses acting over timescales of days to a month. Here, we examine relationships between aerosols and coincident clouds over the Indian subcontinent, using observational data from 2000 to 2009, from the core monsoon region. Season mean and daily timescales were considered. The correlation analyses of cloud properties with aerosol optical depth revealed that deficient monsoon years were characterized by more frequent and larger decreases in cloud drop size and ice water path, but increases in cloud top pressure, with increases in aerosol abundance. The opposite was observed during abundant monsoon years. The correlations of greater aerosol abundance, with smaller cloud drop size, lower evidence of ice processes and shallower cloud height, during deficient rainfall years, imply cloud inhibition; while those with larger cloud drop size, greater ice processes and a greater cloud vertical extent, during abundant rainfall years, suggest cloud invigoration. The study establishes that continental aerosols over India alter cloud properties in diametrically opposite ways during contrasting monsoon years. The mechanisms underlying these effects need further analysis. PMID:28337991

Contrasting influences of aerosols on cloud properties during deficient and abundant monsoon years.

PubMed

Patil, Nitin; Dave, Prashant; Venkataraman, Chandra

2017-03-24

Direct aerosol radiative forcing facilitates the onset of Indian monsoon rainfall, based on synoptic scale fast responses acting over timescales of days to a month. Here, we examine relationships between aerosols and coincident clouds over the Indian subcontinent, using observational data from 2000 to 2009, from the core monsoon region. Season mean and daily timescales were considered. The correlation analyses of cloud properties with aerosol optical depth revealed that deficient monsoon years were characterized by more frequent and larger decreases in cloud drop size and ice water path, but increases in cloud top pressure, with increases in aerosol abundance. The opposite was observed during abundant monsoon years. The correlations of greater aerosol abundance, with smaller cloud drop size, lower evidence of ice processes and shallower cloud height, during deficient rainfall years, imply cloud inhibition; while those with larger cloud drop size, greater ice processes and a greater cloud vertical extent, during abundant rainfall years, suggest cloud invigoration. The study establishes that continental aerosols over India alter cloud properties in diametrically opposite ways during contrasting monsoon years. The mechanisms underlying these effects need further analysis.

New capabilities for characterizing smoke and dust aerosol over land using MODIS

NASA Astrophysics Data System (ADS)

Levy, R. C.; Remer, L. A.

2006-12-01

Smoke and dust aerosol have different chemical, optical and physical properties and both types affect many processes within the climate system. As earth's surface and atmosphere are continuously altered by natural and anthropogenic processes, the emission and presumably the effects of these aerosols are also changing. Thus it is necessary to observe and characterize aerosols on a global and climatic scale. While MODIS has been reporting characteristics of smoke and dust aerosol over land and ocean since shortly after Terra launch, the uncertainties in the over-land retrieval have been larger than expected. To better characterize different aerosol types closer to their source regions with greater accuracy, we have developed a new operational algorithm for retrieving aerosol properties over dark land surfaces from MODIS-observed visible (VIS) and infrared (IR) reflectance. Like earlier versions, this algorithm estimates the total loading (aerosol optical depth-τ) and relative weighting of fine (non-dust) and coarse (dust) -dominated aerosol to the total τ (fine weighting-η) over dark land surfaces. However, the fundamental mathematics and major assumptions have been overhauled. The new algorithm performs simultaneous multi-channel inversion that includes information about coarse aerosol in the IR channels, while assuming a fine-tuned relationship between VIS and IR surface reflectances, that is itself a function of scattering angle and vegetation condition. Finally, the suite of expected aerosol optical models described by the lookup table have been revised to closer resemble the AERONET climatology, including for smoke and dust aerosol. Beginning in April 2006, this algorithm has been used for forward processing and backward re- processing of the entire MODIS dataset observed from both Terra and Aqua. "Collection 5" products were completed for Aqua reprocessing by July 2006 and should be complete for Terra by December 2006. In this study, we used the complete Aqua dataset (July 2002-Aug 2006) and two years of Terra (2005-Aug 2006) data to evaluate the products in regions known to be dominated by smoke and/or dust. We compared with sunphotometer data at selected AERONET sites and found improved τ retrievals,within prescribed accuracy.

Cloud Condensation Nuclei in Cumulus Humilis - Selected Case Study During the CHAPS Campaign

NASA Astrophysics Data System (ADS)

Yu, X.; Berg, L. K.; Berkowitz, C. M.; Alexander, M. L.; Lee, Y.; Laskin, A.; Ogren, J. A.; Andrews, B.

2009-12-01

The Cumulus Humilis Aerosol Processing Study (CHAPS) provided a unique opportunity to study aerosol and cloud processing. Clouds play an active role in the processing and cycling of atmospheric constituents. Gases and particles can partition to cloud droplets by absorption and condensation as well as activation and pact scavenging. The Department of Energy (DOE) G-1 aircraft was used as one of the main platforms in CHAPS. Flight tracks were designed and implemented to characterize freshly emitted aerosols on cloud top and cloud base as well as with cloud, i.e., cumulus humilis (or fair-weather cumulus), in the vicinity of Oklahoma City. Measurements of interstitial aerosols and residuals of activated condensation cloud nuclei were conducted simultaneously. The interstitial aerosols were determined downstream of an isokinetic inlet; and the activated particles downstream of a counter-flow virtual impactor (CVI). The sampling line to the Aerodyne Aerosol Mass Spectrometer was switched between the isokinetic inlet and the CVI to allow characterization of interstitial particles out of clouds in contrast to particles activated in clouds. Trace gases including ozone, carbon monoxide, sulfur dioxide, and a series of volatile organic compounds (VOCs) were also measured as were key meteorological state parameters including liquid water content, cloud drop size, and dew point temperature were measured. This work will focus on studying CCN properties in cumulus humilis. Several approaches will be taken. The first is single particle analysis of particles collected by the Time-Resolved Aerosol Sampler (TRAC) by SEM/TEM coupled with EDX. We will specifically look into differences in particle properties such as chemical composition and morphology between activated and interstitial ones. The second analysis will link in situ measurements with the snap shots observations by TRAC. For instance, by looking into the characteristic m/z obtained by AMS vs. CO or isoprene, one can gain more insight into the role of primary and secondary organic aerosols in CCNs and background aerosols. Combined with observations of cloud properties, an improved picture of CCN activation in cumulus humilis can be made.

AN INITIAL ASSESSMENT OF THE CLIMATE IMPACT OF SECONDARY ORGANIC AEROSOLS

NASA Astrophysics Data System (ADS)

O'Donnell, D.; Feichter, J.

2009-12-01

Atmospheric aerosols influence the Earth’s climate by absorbing and scattering solar radiation (the direct effect) and by altering the properties of clouds (indirect effects). Measurements have shown that a substantial fraction of the tropospheric aerosol burden consists of organic compounds. Hundreds of different organic species have been identified. While progress has been made in the understanding of the role of certain aerosol types in the climate system, that of organic aerosols remains poorly understood and the climate influences resulting from their presence poorly constrained. Organic aerosols are emitted directly from the surface (primary organic aerosols, POA) and are also formed in the atmosphere from gaseous precursors by oxidation reactions (secondary organic aerosols, SOA). Both biogenic and anthropogenic precursors have been identified. Biogenic emissions of aerosol precursors are known to be climate-dependent. Thus, a bi-directional dependency exists between the biosphere and the atmosphere, whereby aerosols of biogenic origin influence the climate system, which in turn affects biogenic aerosol precursor production. This study builds upon the global aerosol-climate model ECHAM5/HAM and adds techniques to model SOA as well as the necessary global emission inventories. Emission of biogenic precursors is calculated online. Formation of SOA is modeled by the well-known two-product model of SOA formation. SOA is subject to the same aerosol microphysics and sink processes as other modeled species (sulphate, black carbon, primary organic carbon, sea salt and dust). The aerosol radiative effects are calculated on a size resolved basis, and the aerosol scheme is coupled to the model cloud microphysics, permitting estimation of both direct and indirect aerosol effects. The following results will be discussed: (i) Estimation of the direct and indirect effects of biogenic and anthropogenic SOA, (ii) Estimation of the sign and magnitude of the biospheric feedback (through biogenic aerosol precursor emission) on the climate system, and (iii) Identification of physical processes and aerosol physical properties that need further experimental investigation in order to improve our understanding of the climate impact of SOA

Maritime Aerosol Network (MAN) as a Component of AERONET

NASA Technical Reports Server (NTRS)

Smirnov, A.; Holben, B. N.; Slutsker, I.; Giles, D. M.; McClain, C. R.; Eck, T. F.; Sakerin, S. M.; Macke, A.; Croot, P.; Zibordi, G.;

Introducing Convective Cloud Microphysics to a Deep Convection Parameterization Facilitating Aerosol Indirect Effects

NASA Astrophysics Data System (ADS)

Alapaty, K.; Zhang, G. J.; Song, X.; Kain, J. S.; Herwehe, J. A.

2012-12-01

Short lived pollutants such as aerosols play an important role in modulating not only the radiative balance but also cloud microphysical properties and precipitation rates. In the past, to understand the interactions of aerosols with clouds, several cloud-resolving modeling studies were conducted. These studies indicated that in the presence of anthropogenic aerosols, single-phase deep convection precipitation is reduced or suppressed. On the other hand, anthropogenic aerosol pollution led to enhanced precipitation for mixed-phase deep convective clouds. To date, there have not been many efforts to incorporate such aerosol indirect effects (AIE) in mesoscale models or global models that use parameterization schemes for deep convection. Thus, the objective of this work is to implement a diagnostic cloud microphysical scheme directly into a deep convection parameterization facilitating aerosol indirect effects in the WRF-CMAQ integrated modeling systems. Major research issues addressed in this study are: What is the sensitivity of a deep convection scheme to cloud microphysical processes represented by a bulk double-moment scheme? How close are the simulated cloud water paths as compared to observations? Does increased aerosol pollution lead to increased precipitation for mixed-phase clouds? These research questions are addressed by performing several WRF simulations using the Kain-Fritsch convection parameterization and a diagnostic cloud microphysical scheme. In the first set of simulations (control simulations) the WRF model is used to simulate two scenarios of deep convection over the continental U.S. during two summer periods at 36 km grid resolution. In the second set, these simulations are repeated after incorporating a diagnostic cloud microphysical scheme to study the impacts of inclusion of cloud microphysical processes. Finally, in the third set, aerosol concentrations simulated by the CMAQ modeling system are supplied to the embedded cloud microphysical scheme to study impacts of aerosol concentrations on precipitation and radiation fields. Observations available from the ARM microbase data, the SURFRAD network, GOES imagery, and other reanalysis and measurements will be used to analyze the impacts of a cloud microphysical scheme and aerosol concentrations on parameterized convection.

Secondary Organic Aerosol Formation in the Captive Aerosol Growth and Evolution (CAGE) Chambers during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL

NASA Astrophysics Data System (ADS)

Leong, Y.; Karakurt Cevik, B.; Hernandez, C.; Griffin, R. J.; Taylor, N.; Matus, J.; Collins, D. R.

2013-12-01

Secondary organic aerosol (SOA) represents a large portion of sub-micron particulate matter on a global scale. The composition of SOA and its formation processes are heavily influenced by anthropogenic and biogenic activity. Volatile organic compounds (VOCs) that are emitted naturally from forests or from human activity serve as precursors to SOA formation. Biogenic SOA (BSOA) is formed from biogenic VOCs and is prevalent in forested regions like the Southeastern United States. The formation and enhancement of BSOA under anthropogenic influences such as nitrogen oxides (NOx), sulfur dioxide (SO2), and oxygen radicals are still not well understood. The lack of information on anthropogenic BSOA enhancement and the reversibility of SOA formation could explain the underprediction of SOA in current models. To address some of these gaps in knowledge, this study was conducted as part of the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL during the summer of 2013. SOA growth experiments were conducted in two Captive Aerosol Growth and Evolution (CAGE) outdoor chambers located at the SEARCH site. Ambient trace gas concentrations were maintained in these chambers using semi-permeable gas-exchange membranes, while studying the growth of injected monodisperse seed aerosol. The control chamber was operated under ambient conditions; the relative humidity and oxidant and NOx levels were perturbed in the second chamber. This design allows experiments to capture the natural BSOA formation processes in the southeastern atmosphere and to study the influence of anthropogenic activity on aerosol chemistry. Chamber experiments were periodically monitored with physical and chemical instrumentation including a scanning mobility particle sizer (SMPS), a cloud condensation nuclei counter (CCNC), a humidified tandem differential mobility analyzer (H-TDMA), and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The CAGE experiments focused on SOA reversibility and the sensitivity of SOA reactions to oxidant or NOx enhancement and aerosol liquid water content. Available ambient trace gas concentrations include VOCs, NOx, SO2, ozone, peroxyaxyl nitrates, and ammonia. Chamber data will also be compared to ambient aerosol measurements collected by the instruments mentioned above as well as those from other research groups.

Organic and inorganic markers and stable C-, N-isotopic compositions of tropical coastal aerosols from megacity Mumbai: sources of organic aerosols and atmospheric processing

NASA Astrophysics Data System (ADS)

Aggarwal, S. G.; Kawamura, K.; Umarji, G. S.; Tachibana, E.; Patil, R. S.; Gupta, P. K.

2012-08-01

To better understand the sources of PM10 samples from Mumbai, India, aerosol chemical compositions, i.e. total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4‰, also suggest that biofuel/biomass burning is the dominant source in both summer and winter seasons. Aerosol mass concentrations of major species increased 3-4 times in winter compared to summer, indicating an enhanced emission from these sources in winter season. Photochemical production tracers, C2 diacid and nssSO42- do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for day- (0.37 ± 0.06 (0.28 ± 0.04)) and nighttime (0.38 ± 0.07 (0.28 ± 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant rather the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from -27.0 to -25.4‰ with slightly lower average (-26.5 ± 0.3‰) in summer than in winter (-25.9 ± 0.3‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the increment in δ13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in the summer aerosols.

Impacts of Aerosol-Monsoon Interaction on Rainfall and Circulation over Northern India and the Himalaya Foothills

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, Kyu-Myong; Shi, Jainn-Jong; Matsui, T.; Chin, M.; Tan, Qian; Peters-Lidard, C.; Tao, W. K.

2016-01-01

The boreal summer of 2008 was unusual for the Indian monsoon, featuring exceptional heavy loading of dust aerosols over the Arabian Sea and northern-central India, near normal all- India rainfall, but excessive heavy rain, causing disastrous flooding in the Northern Indian Himalaya Foothills (NIHF) regions, accompanied by persistent drought conditions in central and southern India. Using NASA Unified-physics Weather Research Forecast (NUWRF) model with fully interactive aerosol physics and dynamics, we carried out three sets of 7-day ensemble model forecast experiments: 1) control with no aerosol, 2) aerosol radiative effect only and 3) aerosol radiative and aerosol-cloud-microphysics effects, to study the impacts of aerosol monsoon interactions on monsoon variability over the NIHF during the summer of 2008. Results show that aerosol-radiation interaction (ARI), i.e., dust aerosol transport, and dynamical feedback processes induced by aerosol-radiative heating, plays a key role in altering the large scale monsoon circulation system, reflected by an increased north-south tropospheric temperature gradient, a northward shift of heavy monsoon rainfall, advancing the monsoon onset by 1-5 days over the HF, consistent with the EHP hypothesis (Lau et al. 2006). Additionally, we found that dust aerosols, via the semi-direct effect, increase atmospheric stability, and cause the dissipation of a developing monsoon onset cyclone over northeastern India northern Bay of Bengal. Eventually, in a matter of several days, ARI transforms the developing monsoon cyclone into mesoscale convective cells along the HF slopes. Aerosol-Cloud-microphysics Interaction (ACI) further enhances the ARI effect in invigorating the deep convection cells and speeding up the transformation processes. Results indicate that even in short-term (up to weekly) numerical forecasting of monsoon circulation and rainfall, effects of aerosol-monsoon interaction can be substantial and cannot be ignored.

Influence of Atmospheric Processes on the Solubility and Composition of Iron in Saharan Dust

NASA Astrophysics Data System (ADS)

Ingall, E. D.; Longo, A.; Feng, Y.; Lai, B.; Landing, W. M.; Shelley, R.; Nenes, A.; Mihalopoulos, N.; Violaki, K.

2016-12-01

Iron is a key micronutrient that is vital for all organisms. The supply of bioavailable, soluble iron controls primary productivity in approximately 30% of the world's oceans. The significant contribution of atmospheric aerosols to the bioavailable iron budget in vast ocean regions, underscores the need to understand the controls and transformations of aerosol iron solubility during atmospheric transport. The Sahara Desert contains the largest and most active sources of aerosol dust globally and can be a key source of nutrients to the Mediterranean Sea, much of the North Atlantic Ocean, and even as far as the Gulf of Mexico. Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated aerosol iron in Mediterranean samples. In Atlantic samples, iron(II & III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation state became more reduced, and aerosol acidity increased. Atmospheric processing, including acidic reactions and photo-reduction, likely influence the form of iron minerals and the oxidation state in Saharan dust aerosols and contribute to increases in aerosol iron solubility. Overall, these findings suggest that a combination of factors affects aerosol iron solubility during long-distance atmospheric transport and emphasize the need to consider reductive mechanisms as well as proton-induced solubilization of aerosol iron in modeling studies.

Effect of temperature tuning on the aerosol acoustic aggregation process.

PubMed

Qiao, Zhenghui; Dong, Wei; Huang, Yaji; Naso, Vincenzo

2018-05-01

Diesel exhaust aerosols (DEAs) can absorb and accumulate toxic metal particulates and bacteria suspended in the atmospheric environment, which impact human health and the environment. The use of acoustic standing waves (ASWs) to aggregate DEA is currently considered to be an efficient particle removal method; however, study of the effect of different temperatures on the acoustic aggregation process is scarce. To explore the method and technology to regulate and optimize the aerosol aggregation process through temperature tuning, an acoustic apparatus integrated with a temperature regulation function was constructed. Using this apparatus, the effect of different characteristic temperatures (CTs) on the aerosol aggregation process was investigated experimentally in the ASW environment. Under constant conditions of acoustic frequency 1.286kHz, voltage amplitude 17V and input electric power 16.7W, the study concentrated on temperature effects on the aggregation process in the CT range of 58-72°C. The DEA opacity was used. The results demonstrate that the aggregation process is quite sensitive to the CT, and that the optimal DEA aggregation can be achieved at 66°C. The aggregated particles of 68.17μm are composed of small nanoparticles of 13.34-62.15nm. At CTs higher and lower than 66°C, the apparatus in non-resonance mode reduces the DEA aggregation level. For other instruments, the method for obtaining the optimum temperature for acoustic agglomeration is universal. This preliminary demonstration shows that the use of acoustic technology to regulate the aerosol aggregation process through tuning the operating temperature is feasible and convenient. Copyright © 2017. Published by Elsevier B.V.

Analysis of reversibility and reaction products of glyoxal uptake onto ammonium sulfate aerosol

NASA Astrophysics Data System (ADS)

Galloway, M. M.; Chhabra, P. S.; Chan, A. W.; Surratt, J. D.; Kwan, A. J.; Wennberg, P. O.; Flagan, R. C.; Seinfeld, J. H.; Keutsch, F. N.

2009-04-01

Glyoxal, the smallest alpha-dicarbonyl, is an oxidation product of both biogenic and anthropogenic volatile organic compounds (Fu et al. JGR 113, D15303, 2008). Despite its low molecular weight, its role in secondary organic aerosol (SOA) formation has gained interest and a recent study suggested that it accounts for more than 15% of SOA in Mexico City (Volkamer et al. GRL 34, L19807, 2007). Despite numerous previous studies, questions remain regarding the processes controlling glyoxal uptake onto aerosol, including the role of acid catalysis, degree of reversibility, and identity of aerosol phase reaction products. We present results of chamber aerosol studies (Galloway et al. ACPD 8, 20799, 2008) and laboratory studies of bulk samples aimed at improving the understanding of these processes, in particular formation of oligomers and organosulfates of glyoxal, as well as the formation of imidazoles (carbon-nitrogen containing heterocyclic aromatic compounds) under dark and irradiated conditions. The relevance of these classes of reaction products extends beyond glyoxal, as evidence of oligomers and organosulfates other than those of glyoxal have been found in ambient aerosol (Surratt et al. JPCA 112, 8345, 2008; Denkenberger et al. Environ. Sci. Technol. 41, 5439, 2007). Experiments in which a chamber air mass was diluted after equilibration of glyoxal uptake onto ammonium sulfate seed aerosol (relative humidity 60% and glyoxal mixing ratios of 25-200 ppbv) shows that under these conditions uptake is reversible. The most important condensed phase products are hydrated oligomers of glyoxal, which are also formed reversibly under these conditions. Our studies show that organosulfates were not formed under dark conditions for neutral or acidified aerosol; similarly, Minerath et al. have recently shown that formation of a different class of organosulfates (alkyl sulfates) also proceeds very slowly even under acidic conditions (Environ. Sci. Technol. 42, 4410, 2008). The masses assigned to sulfate esters in previous work (Liggio et al. Environ. Sci. Technol. 39, 1532, 2005) via low resolution AMS studies were assigned as glyoxal oligomers in our study via high resolution AMS spectra. However, organosulfates were identified under irradiated conditions, and we present attempts to identify the specific species via comparison with lab synthesized organosulfates. The influence of irradiation on organosulfate formation is still under investigation. Under irradiated conditions we see clear evidence for active oxidative photochemistry. The aerosol phase becomes increasingly oxidized and oxidation products, such as organic acids, similar to those observed in studies using bulk samples by Carlton et al. (Atmos. Environ. 41, 7588, 2007) are formed. Overall uptake is reduced under our experimental conditions, likely due to increasing temperature and decreasing relative humidity. We also report observation of imidazoles (carbon-nitrogen containing aromatic heterocycles) resulting from reaction of glyoxal with the nitrogen component of the ammonium sulfate seed aerosol. The imidazoles form irreversibly under dark and irradiated conditions, in ammonium sulfate and acidified ammonium sulfate (pH~1) aerosol. The molecular framework of imidazoles is very stable as a result of the aromaticity. The primary imidazole product, which has a low vapor pressure estimated at 0.0014 Torr, is predicted to be present as a (protonated) cation, owing to its basicity (pKB = 7). It is thus likely not a candidate for repartitioning to the gas phase. Evidence for participation of ammonium in reactions with glyoxal using bulk samples has recently been reported by Noziere et al. (JPCA 113, 231, 2008; ACPD 9, 1, 2009). This study reveals the complex chemistry occurring within ammonium sulfate seed aerosol even for systems with greatly reduced complexity compared to atmospheric aerosol. The results increase our understanding of the contribution of glyoxal to SOA formation processes. More specifically, these results provide valuable insights into important aerosol processes, such as organosulfate and oligomer formation, as well as the formation of aromatic nitrogen containing heterocycles from reaction of a carbonyl with ammonium sulfate aerosol.

Case Studies of the Vertical Structure of the Direct Shortwave Aerosol Radiative Forcing During TARFOX

NASA Technical Reports Server (NTRS)

Redemann, J.; Turco, R. P.; Liou, K. N.; Hobbs, P. V.; Hartley, W. S.; Bergstrom, R. W.; Browell, E. V.; Russell, P. B.

2000-01-01

The vertical structure of aerosol-induced radiative flux changes in the Earth's troposphere affects local heating rates and thereby convective processes, the formation and lifetime of clouds, and hence the distribution of chemical constituents. We present observationally based estimates of the vertical structure of direct shortwave aerosol radiative forcing for two case studies from the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) which took place on the U.S. east coast in July 1996. The aerosol radiative forcings are computed using the Fu-Liou broadband radiative transfer model. The aerosol optical properties used in the radiative transfer simulations are calculated from independent vertically resolved estimates of the complex aerosol indices of refraction in two to three distinct vertical layers, using profiles of in situ particle size distributions measured aboard the University of Washington research aircraft. Aerosol single-scattering albedos at 450 nm thus determined range from 0.9 to 0.985, while the asymmetry factor varies from 0.6 to 0.8. The instantaneous shortwave aerosol radiative forcings derived from the optical properties of the aerosols are of the order of -36 Wm(exp -2) at the top of the atmosphere and about -56 Wm(exp -2) at the surface for both case studies.

Studying of welding aerosol using laser granulometry

NASA Astrophysics Data System (ADS)

Kirichenko, K. Y.; Gridasov, A. V.; Drozd, V. A.; Golokhvast, K. S.

2016-11-01

The paper presents results of a study of the size of the particles that arise during the welding process using laser granulometry method. It is shown that the welding aerosol - extremely dangerous for human and animal health and the source of nano- and micro-sized particles.

Effect of operation conditions of the drop-on-demand aerosol generator on aerosol characteristics: Pseudo-cinematographic and plasma mass spectrometric studies

NASA Astrophysics Data System (ADS)

Orlandini v. Niessen, Jan O.; Krone, Karin M.; Bings, Nicolas H.

2014-02-01

The recently presented drop-on-demand (DOD) aerosol generator overcomes some of the drawbacks of pneumatic nebulization, as its aerosol is no longer generated by gas-liquid interaction. In the current study, an advanced imaging technique is presented, based on a CCD camera equipped with magnifying telecentric optics to allow for fast, automated and precise aerosol characterization as well as fundamental studies on the droplet generation processes by means of pseudo-cinematography. The DOD aerosol generator is thoroughly characterized regarding its droplet size distribution, which shows few distinct populations rather than a continuous distribution. Other important figures, such as the Sauter diameter (D3,2) of 22 μm and the span of 0.4 were also determined. Additionally, the influence of the electrical operation conditions of the dosing device on the aerosol generation process is described. The number and volume of the generated droplets were found to be very reproducible and user-variable, e.g. from 17 to 27 μm (D3,2), within a span of 0.07-0.89. The performances of different setups of the DOD as liquid sample introduction system in ICP-MS are correlated to the respective achievable aerosol characteristics and are also compared to the performance of a state-of-the-art μ-flow nebulizer (EnyaMist). The DOD system allowed for improved sensitivity, but slightly elevated signal noise and overall comparable limits of detection. The results are critically discussed and future directions are outlined.

A study of photochemical againg of ambient air using Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions

NASA Astrophysics Data System (ADS)

Lee, T.; Son, J.; Kim, J.; Kim, S.; Sung, K.; Park, G.; Link, M.; Park, T.; Kim, K.; Kang, S.; Ban, J.; Kim, D. S.

2016-12-01

Recent research proposed that Secondary Aerosol (SA) is important class of predicting future climate change scenarios, health effect, and a general air quality. However, there has been lack of studies to investigate SA formation all over the world. This study tried to focus on understanding potential secondary aerosol formation and its local impact by the photochemical aging of inorganic and organic aerosols in the ambient air using the Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions. PAM chamber manufactured by Aerodyne make an oxidizing environment that simulates oxidation processes on timescales of 12-15 hrs in the atmosphere. Chemical compositions of ambient aerosol and aerosol that was aged in the PAM chamber were alternately measured every 2-minutes using the High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS). HR-ToF-AMS provides non-refractory aerosol mass concentrations including nitrate, sulfate, hydrocarbon-like and oxygenated organic aerosol in real time. This study includes a residence area of mixture of sources, a forest site of dominant source of biogenic VOCs, an underground parking lot of dominant vehicle emission, and laboratory experiment of vehicle emissions under different fuels and speeds using the chassis dynamometer. As a result, it was revealed that gasoline and LPG vehicle relatively made more potential SA than diesel vehicle.

Comparison of C5 and C6 Aqua-MODIS Dark Target Aerosol Validation

NASA Technical Reports Server (NTRS)

Munchak, Leigh A.; Levy, Robert C.; Mattoo, Shana

2014-01-01

We compare C5 and C6 validation to compare the C6 10 km aerosol product against the well validated and trusted aerosol product on global and regional scales. Only the 10 km aerosol product is evaluated in this study, validation of the new C6 3 km aerosol product still needs to be performed. Not all of the time series has processed yet for C5 or C6, and the years processed for the 2 products is not exactly the same (this work is preliminary!). To reduce the impact of outlier observations, MODIS is spatially averaged within 27.5 km of the AERONET site, and AERONET is temporatally averaged within 30 minutes of the MODIS overpass time. Only high quality (QA = 3 over land, QA greater than 0 over ocean) pixels are included in the mean.

Effects of Aerosol Pollution on Clouds over Megacities

NASA Astrophysics Data System (ADS)

Sechrist, B.; Jacobson, M. Z.

2013-12-01

The correlation between aerosol optical depth (AOD) and cloud properties - principally cloud fraction and cloud optical depth (COD) - is examined using satellite retrievals from the MODIS satellites over Los Angeles and Beijing. Ten Hoeve et al. (2011, Atmos. Chem. Phys, 11(7), 3021-3036) used satellite data to examine the impact of aerosols on warm clouds around Rondonia, Brazil, during the biomass burning season. They found that the COD-AOD relationship exhibits a 'boomerang' shape in which COD initially increases with increasing AOD but then decreases as AOD continues to increase beyond some critical level. This result is thought to reflect the balance between the microphysical and radiative components of a cloud's response to aerosols. The microphysical process dominates at low AOD, while the radiative process dominates at high AOD. This study is analogous to Ten Hoeve et al., but for aerosols derived primarily from fossil fuel combustion rather than biomass burning. Preliminary results will be presented.

Energy-based and process-based constraints on aerosol-climate interaction

NASA Astrophysics Data System (ADS)

Suzuki, K.; Sato, Y.; Takemura, T.; Michibata, T.; Goto, D.; Oikawa, E.

2017-12-01

Recent advance in both satellite observations and global modeling provides us with a novel opportunity to investigate the long-standing aerosol-climate interaction issue at a fundamental process level, particularly with a combined use of them. In this presentation, we will highlight our recent progress in understanding the aerosol-cloud-precipitation interaction and its implication for global climate with a synergistic use of a state-of-the-art global climate model (MIROC), a global cloud-resolving model (NICAM) and recent satellite observations (A-Train). In particular, we explore two different aspects of the aerosol-climate interaction issue, i.e. (i) the global energy balance perspective with its modulation due to aerosols and (ii) the process-level characteristics of the aerosol-induced perturbations to cloud and precipitation. For the former, climate model simulations are used to quantify how components of global energy budget are modulated by the aerosol forcing. The moist processes are shown to be a critical pathway that links the forcing efficacy and the hydrologic sensitivity arising from aerosol perturbations. Effects of scattering (e.g. sulfate) and absorbing (e.g. black carbon) aerosols are compared in this context to highlight their distinctively different impacts on climate and hydrologic cycle. The aerosol-induced modulation of moist processes is also investigated in the context of the second aspect above to facilitate recent arguments on possible overestimates of the aerosol-cloud interaction in climate models. Our recent simulations with NICAM are shown to highlight how diverse responses of cloud to aerosol perturbation, which have been failed to represent in traditional climate models, are reproduced by the high-resolution global model with sophisticated cloud microphysics. We will discuss implications of these findings for a linkage between the two aspects above to aid advance process-based understandings of the aerosol-climate interaction and also to mitigate a "dichotomy" recently found by the authors between the two aspects in the context of the climate projection.

Enviro-HIRLAM Applicability for Black Carbon Studies in Arctic

NASA Astrophysics Data System (ADS)

Nuterman, Roman; Mahura, Alexander; Baklanov, Alexander; Kurganskiy, Alexander; Amstrup, Bjarne; Kaas, Eigil

2015-04-01

One of the main aims of the Nordic CarboNord project ("Impact of black carbon on air quality and climate in Northern Europe and Arctic") is focused on providing new information on distribution and effects of black carbon in Northern Europe and Arctic. It can be done through assessing robustness of model predictions of long-range black carbon distribution and its relation to climate change and forcing. In our study, the online integrated meteorology-chemistry/aerosols model - Enviro-HIRLAM (Environment - HIgh Resolution Limited Area Model) - is used. This study, at first, is focused on adaptation (model setup, domain for the Northern Hemisphere and Arctic region, emissions, boundary conditions, refining aerosols microphysics and chemistry, cloud-aerosol interaction processes) of Enviro-HIRLAM model and selection of most unfavorable weather and air pollution episodes for the Arctic region. Simulations of interactions between black carbon and meteorological processes in northern conditions for selected episodes will be performed (at DMI's supercomputer HPC CRAY-XT5), and then long-term simulations at regional scale for selected winter vs. summer months. Modelling results will be compared on a diurnal cycle and monthly basis against observations for key meteorological parameters (such as air temperature, wind speed, relative humidity, and precipitation) as well as aerosol concentration. Finally, evaluation of black carbon atmospheric transport, dispersion, and deposition patterns at different spatio-temporal scales; physical-chemical processes and transformations of black carbon containing aerosols; and interactions and effects between black carbon and meteorological processes in Arctic weather conditions will be done.

Scanning vertical distributions of typical aerosols along the Yangtze River using elastic lidar.

PubMed

Fan, Shidong; Liu, Cheng; Xie, Zhouqing; Dong, Yunsheng; Hu, Qihou; Fan, Guangqiang; Chen, Zhengyi; Zhang, Tianshu; Duan, Jingbo; Zhang, Pengfei; Liu, Jianguo

2018-07-01

In recent years, China has experienced heavy air pollution, especially haze caused by particulate matter (PM). The compositions, horizontal distributions, transport, and chemical formation mechanisms of PM and its precursors have been widely investigated in China based on near-ground measurements. However, the understanding of the distributions and physical and chemical processes of PM in the vertical direction remains limited. In this study, an elastic lidar was employed to investigate the vertical profiles of aerosols along the Yangtze River during the Yangtze River Campaign of winter 2015. Some typical aerosols were identified and some events were analyzed in three cases. Dust aerosols can be transported from the Gobi Desert to the Yangtze River basin across a long distance at both low and high altitudes in early December. The transport route was perpendicular to the ship track, suggesting that the dust aerosols may have affected a large area. Moreover, during transport, some dust was also affected by the areas below its transport route since some anthropogenic pollutants were mixed with the dust and changed some of its optical properties. Biomass-burning aerosols covering a distant range along the Yangtze River were identified. This result directly shows the impact areas of biomass-burning aerosols in some agricultural fields. Some directly emitted aerosol plumes were observed, and direct effects of such plumes were limited both temporally and spatially. In addition, an aerosol plume with very low linear depolarization ratios, probably formed through secondary processes, was also observed. These results can help us better understand aerosols in large spatial scales in China and can be useful to regional haze studies. Copyright © 2018. Published by Elsevier B.V.

A satellite view of aerosols in the climate system

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Tanre, Didier; Boucher, Olivier

2002-01-01

Anthropogenic aerosols are intricately linked to the climate system and to the hydrologic cycle. The net effect of aerosols is to cool the climate system by reflecting sunlight. Depending on their composition, aerosols can also absorb sunlight in the atmosphere, further cooling the surface but warming the atmosphere in the process. These effects of aerosols on the temperature profile, along with the role of aerosols as cloud condensation nuclei, impact the hydrologic cycle, through changes in cloud cover, cloud properties and precipitation. Unravelling these feedbacks is particularly difficult because aerosols take a multitude of shapes and forms, ranging from desert dust to urban pollution, and because aerosol concentrations vary strongly over time and space. To accurately study aerosol distribution and composition therefore requires continuous observations from satellites, networks of ground-based instruments and dedicated field experiments. Increases in aerosol concentration and changes in their composition, driven by industrialization and an expanding population, may adversely affect the Earth's climate and water supply.

Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO 3 − aerosol during the 2013 Southern Oxidant and Aerosol Study

DOE PAGES

Allen, H. M.; Draper, D. C.; Ayres, B. R.; ...

2015-09-25

Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO 3 −) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na + and Ca 2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms bymore » multiphase reactions of HNO 3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH 4NO 3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. In addition, calculation of the rate of the heterogeneous uptake of HNO 3 on mineral aerosol supports the conclusion that aerosol NO 3 − is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO 3 − and HNO 3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas–aerosol phase partitioning.« less

Aerosol-halogen interaction: Change of physico-chemical properties of SOA by naturally released halogen species

NASA Astrophysics Data System (ADS)

Ofner, J.; Balzer, N.; Buxmann, J.; Grothe, H.; Krüger, H.; Platt, U.; Schmitt-Kopplin, P.; Zetzsch, C.

2011-12-01

Reactive halogen species are released by various sources like photo-activated sea-salt aerosol or salt pans and salt lakes. These heterogeneous release mechanisms have been overlooked so far, although their potential of interaction with organic aerosols like Secondary Organic Aerosol (SOA), Biomass Burning Organic Aerosol (BBOA) or Atmospheric Humic LIke Substances (HULIS) is completely unknown. Such reactions can constitute sources of gaseous organo-halogen compounds or halogenated organic particles in the atmospheric boundary layer. To study the interaction of organic aerosols with reactive halogen species (RHS), SOA was produced from α-pinene, catechol and guaiacol using an aerosol smog-chamber. The model SOAs were characterized in detail using a variety of physico-chemical methods (Ofner et al., 2011). Those aerosols were exposed to molecular halogens in the presence of UV/VIS irradiation and to halogens, released from simulated natural halogen sources like salt pans, in order to study the complex aerosol-halogen interaction. The heterogeneous reaction of RHS with those model aerosols leads to different gaseous species like CO2, CO and small reactive/toxic molecules like phosgene (COCl2). Hydrogen containing groups on the aerosol particles are destroyed to form HCl or HBr, and a significant formation of C-Br bonds could be verified in the particle phase. Carbonyl containing functional groups of the aerosol are strongly affected by the halogenation process. While changes of functional groups and gaseous species were visible using FTIR spectroscopy, optical properties were studied using Diffuse Reflectance UV/VIS spectroscopy. Overall, the optical properties of the processed organic aerosols are significantly changed. While chlorine causes a "bleaching" of the aerosol particles, bromine shifts the maximum of UV/VIS absorption to the red end of the UV/VIS spectrum. Further physico-chemical changes were recognized according to the aerosol size-distributions or the averaged carbon oxidation state (OSc). The heterogeneous reaction of SOA with molecular halogens released from the simulated salt-pan at different simulated environmental conditions leads to changes of several physico-chemical features of the aerosol. However, the halogen release mechanisms are also affected by the presence of organic aerosols. One order of magnitude less BrO was detected by an active Differential Optical Absorption Spectroscopy (DOAS) instrument in the presence of SOA compared to experiments without SOA. This work was supported by the German Research Foundation within the HALOPROC project. Ofner, J., Krüger, H.-U., Grothe, H., Schmitt-Kopplin, P., Whitmore, K., and Zetzsch, C. (2011), Atmos. Chem. Phys., 11, 1-15.

Narrowing the Gap in Quantification of Aerosol-Cloud Radiative Effects

NASA Astrophysics Data System (ADS)

Feingold, G.; McComiskey, A. C.; Yamaguchi, T.; Kazil, J.; Johnson, J. S.; Carslaw, K. S.

2016-12-01

Despite large advances in our understanding of aerosol and cloud processes over the past years, uncertainty in the aerosol-cloud radiative effect/forcing is still of major concern. In this talk we will advocate a methodology for quantifying the aerosol-cloud radiative effect that considers the primacy of fundamental cloud properties such as cloud amount and albedo alongside the need for process level understanding of aerosol-cloud interactions. We will present a framework for quantifying the aerosol-cloud radiative effect, regime-by-regime, through process-based modelling and observations at the large eddy scale. We will argue that understanding the co-variability between meteorological and aerosol drivers of the radiative properties of the cloud system may be as important an endeavour as attempting to untangle these drivers.

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combinationmore » of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol mass and number with knowledge of particle properties such as volatility and viscosity are crucial for improving understanding of non-linear SOA-related processes. For example, useful insights can be attained by combining bottom-up information related to the molecular speciation of gas- and particle-phase precursors with top-down insights on size evolution dynamics of SOA. Continuing efforts are also needed to rank the most influential processes affecting SOA lifecycle, so that these processes can be accurately represented in atmospheric chemistry-climate models.« less

Modelling absorbing aerosol with ECHAM-HAM: Insights from regional studies

NASA Astrophysics Data System (ADS)

Tegen, Ina; Heinold, Bernd; Schepanski, Kerstin; Banks, Jamie; Kubin, Anne; Schacht, Jacob

2017-04-01

Quantifying distributions and properties of absorbing aerosol is a basis for investigations of interactions of aerosol particles with radiation and climate. While evaluations of aerosol models by field measurements can be particularly successful at the regional scale, such results need to be put into a global context for climate studies. We present an overview over studies performed at the Leibniz Institute for Tropospheric Research aiming at constraining the properties of mineral dust and soot aerosol in the global aerosol model ECHAM6-HAM2 based on different regional studies. An example is the impact of different sources for dust transported to central Asia, which is influenced, by far-range transport of dust from Arabia and the Sahara together with dust from local sources. Dust types from these different source regions were investigated in the context of the CADEX project and are expected to have different optical properties. For Saharan dust, satellite retrievals from MSG SEVIRI are used to constrain Saharan dust sources and optical properties. In the Arctic region, on one hand dust aerosol is simulated in the framework of the PalMod project. On the other hand aerosol measurements that will be taken during the DFG-funded (AC)3 field campaigns will be used to evaluate the simulated transport pathways of soot aerosol from European, North American and Asian sources, as well as the parameterization of soot ageing processes in ECHAM6-HAM2. Ultimately, results from these studies will improve the representation of aerosol absorption in the global model.

Aerosol indirect effects on summer precipitation in a regional climate model for the Euro-Mediterranean region

NASA Astrophysics Data System (ADS)

Da Silva, Nicolas; Mailler, Sylvain; Drobinski, Philippe

2018-03-01

Aerosols affect atmospheric dynamics through their direct and semi-direct effects as well as through their effects on cloud microphysics (indirect effects). The present study investigates the indirect effects of aerosols on summer precipitation in the Euro-Mediterranean region, which is located at the crossroads of air masses carrying both natural and anthropogenic aerosols. While it is difficult to disentangle the indirect effects of aerosols from the direct and semi-direct effects in reality, a numerical sensitivity experiment is carried out using the Weather Research and Forecasting (WRF) model, which allows us to isolate indirect effects, all other effects being equal. The Mediterranean hydrological cycle has often been studied using regional climate model (RCM) simulations with parameterized convection, which is the approach we adopt in the present study. For this purpose, the Thompson aerosol-aware microphysics scheme is used in a pair of simulations run at 50 km resolution with extremely high and low aerosol concentrations. An additional pair of simulations has been performed at a convection-permitting resolution (3.3 km) to examine these effects without the use of parameterized convection. While the reduced radiative flux due to the direct effects of the aerosols is already known to reduce precipitation amounts, there is still no general agreement on the sign and magnitude of the aerosol indirect forcing effect on precipitation, with various processes competing with each other. Although some processes tend to enhance precipitation amounts, some others tend to reduce them. In these simulations, increased aerosol loads lead to weaker precipitation in the parameterized (low-resolution) configuration. The fact that a similar result is obtained for a selected area in the convection-permitting (high-resolution) configuration allows for physical interpretations. By examining the key variables in the model outputs, we propose a causal chain that links the aerosol effects on microphysics to their simulated effect on precipitation, essentially through reduction of the radiative heating of the surface and corresponding reductions of surface temperature, resulting in increased atmospheric stability in the presence of high aerosol loads.

A study on the relationship between mass concentrations, chemistry and number size distribution of urban fine aerosols in Milan, Barcelona and London

NASA Astrophysics Data System (ADS)

Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R.; Tardivo, R.; Scarnato, B.; Gemelli, V.

2007-05-01

A physicochemical characterization, including aerosol number size distribution, chemical composition and mass concentrations, of the urban fine aerosol captured in MILAN, BARCELONA and LONDON is presented in this article. The objective is to obtain a comprehensive picture of the microphysical processes involved in aerosol dynamics during the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) the link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of >100 nm particles N>100 (nm) ("accumulation mode particles") which only account for <20% of the total number concentration N of fine aerosols; but do not correlate with the number of <100 nm particles ("ultrafine particles"), which accounts for >80% of fine particles number concentration. Organic matter and black-carbon are the only aerosol components showing a significant correlation with the ultrafine particles, attributed to vehicles exhausts emissions; whereas ammonium-nitrate, ammonium-sulphate and also organic matter and black-carbon correlate with N>100 (nm) and attributed to condensation mechanisms, other particle growth processes and some primary emissions. Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100 (nm) concentrations exhibit correlated day-to-day variations, which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the observation that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow large enough to produce significant number concentrations of N>100 (nm) ("accumulation mode particles"). In contrast, because the low contribution of ultrafine particles to the fine aerosol mass concentrations, high "ultrafine particles N<100(nm) events" frequently occurs under low PM2.5 conditions. The results of this study demonstrate that vehicles exhausts emissions are strongly involved in this ultrafine particles aerosol pollution.

Near-Real-Time Detection and Monitoring of Dust Events by Satellite (SeaWIFS, MODIS, and TOMS)

NASA Technical Reports Server (NTRS)

Hsu, N. Christina; Tsay, Si-Chee; Herman, Jay R.; Kaufman, Yoram

2002-01-01

Over the last few years satellites have given us increasingly detailed information on the size, location, and duration of dust events around the world. These data not only provide valuable feedback to the modelling community as to the fidelity of their aerosol models but are also finding increasing use in near real-time applications. In particular, the ability to locate and track the development of aerosol dust clouds on a near real-time basis is being used by scientists and government to provide warning of air pollution episodes over major urban area. This ability has also become a crucial component of recent coordinated campaigns to study the characteristics of tropospheric aerosols such as dust and their effect on climate. One such recent campaign was ACE-Asia, which was designed to obtain the comprehensive set of ground, aircraft, and satellite data necessary to provide a detailed understanding of atmospheric aerosol particles over the Asian-Pacific region. As part of ACE-Asia, we developed a near real-time data processing and access system to provide satellite data from the polar-orbiting instruments Earth Probe TOMS (in the form of absorbing aerosol index) and SeaWiFS (in the form of aerosol optical thickness, AOT, and Angstrom exponent). The results were available via web access. The location and movement information provided by these data were used both in support of the day-to-day flight planning of ACE-Asia and as input into aerosol transport models. While near real-time SeaWiFS data processing can be performed using either the normal global data product or data obtained via direct broadcast to receiving stations close to the area of interest, near real-time MODIS processing of data to provide aerosol retrievals is currently only available using its direct broadcast capability. In this paper, we will briefly discuss the algorithms used to generate these data. The retrieved aerosol optical thickness and Angstrom exponent from SeaWiFS will be compared with those obtained from various AERONET sites over the Asian-Pacific region. The TOMS aerosol index will also be compared with AERONET aerosol optical thickness over different aerosol conditions, and comparisons between the MODIS and SeaWiFS data will also be presented. Finally, we will discuss the climate implication of our studies using the combined satellite and AERONET observations.

Photoacoustic measurements of photokinetics in single optically trapped aerosol droplets

NASA Astrophysics Data System (ADS)

Covert, Paul; Cremer, Johannes; Signorell, Ruth; Thaler, Klemens; Haisch, Christoph

2017-04-01

It is well established that interaction of light with atmospheric aerosols has a large impact on the Earth's climate. However, uncertainties in the magnitude of this impact remain large, due in part to broad distributions of aerosol size, composition, and chemical reactivity. In this context, photoacoustic spectroscopy is commonly used to measure light absorption by aerosols. Here, we present photoacoustic measurements of single, optically-trapped nanodroplets to reveal droplet size-depencies of photochemical and physical processes. Theoretical considerations have pointed to a size-dependence in the magnitude and phase of the photoacoustic response from aerosol droplets. This dependence is thought to originate from heat transfer processes that are slow compared to the acoustic excitation frequency. In the case of a model aerosol, our measurements of single particle absorption cross-section versus droplet size confirm these theoretical predictions. In a related study, using the same model aerosol, we also demonstrate a droplet size-dependence of photochemical reaction rates [1]. Within sub-micron sized particles, photolysis rates were observed to be an order of magnitude greater than those observed in larger droplets. [1] J. W. Cremer, K. M. Thaler, C. Haisch, and R. Signorell. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics. Nat. Commun., 7:10941, 2016.

The Sectional Stratospheric Sulfate Aerosol module (S3A-v1) within the LMDZ general circulation model: description and evaluation against stratospheric aerosol observations

NASA Astrophysics Data System (ADS)

Kleinschmitt, Christoph; Boucher, Olivier; Bekki, Slimane; Lott, François; Platt, Ulrich

2017-09-01

Stratospheric aerosols play an important role in the climate system by affecting the Earth's radiative budget as well as atmospheric chemistry, and the capabilities to simulate them interactively within global models are continuously improving. It is important to represent accurately both aerosol microphysical and atmospheric dynamical processes because together they affect the size distribution and the residence time of the aerosol particles in the stratosphere. The newly developed LMDZ-S3A model presented in this article uses a sectional approach for sulfate particles in the stratosphere and includes the relevant microphysical processes. It allows full interaction between aerosol radiative effects (e.g. radiative heating) and atmospheric dynamics, including e.g. an internally generated quasi-biennial oscillation (QBO) in the stratosphere. Sulfur chemistry is semi-prescribed via climatological lifetimes. LMDZ-S3A reasonably reproduces aerosol observations in periods of low (background) and high (volcanic) stratospheric sulfate loading, but tends to overestimate the number of small particles and to underestimate the number of large particles. Thus, it may serve as a tool to study the climate impacts of volcanic eruptions, as well as the deliberate anthropogenic injection of aerosols into the stratosphere, which has been proposed as a method of geoengineering to abate global warming.

Incorporating radioactive decay into charging and coagulation of multicomponent radioactive aerosols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, Yong-ha; Yiacoumi, Sotira; Nenes, Athanasios

Compositional changes by the decay of radionuclides in radioactive aerosols can influence their charging state, coagulation frequency and size distribution throughout their atmospheric lifetime. The importance of such effects is unknown as they have not been considered in microphysical and global radioactivity transport studies to date. Here, we explore the effects of compositional changes on the charging efficiency and coagulation rates of aerosols using a set of kinetic equations that couple all relevant processes (decay, charging and coagulation) and their evolution over time. Compared to a coupled aggregation-tracer model for the prediction of the radioactive composition of particulates undergoing coagulation,more » our kinetic approach can provide similar results using much less central processing unit time. Altogether with other considerations, our approach is computational efficient enough to allow implementation in 3D atmospheric transport models. The decay of radionuclides and the production of decay products within radioactive aerosols may significantly affect the aerosol charging rates, and either hinder or promote the coagulation of multicomponent radioactive aerosols. Our results suggest that radiological phenomena occurring within radioactive aerosols, as well as subsequent effects on aerosol microphysics, should be considered in regional and global models to more accurately predict radioactivity transport in the atmosphere in case of a nuclear plant accident.« less

Incorporating radioactive decay into charging and coagulation of multicomponent radioactive aerosols

DOE PAGES

Kim, Yong-ha; Yiacoumi, Sotira; Nenes, Athanasios; ...

2017-09-29

Compositional changes by the decay of radionuclides in radioactive aerosols can influence their charging state, coagulation frequency and size distribution throughout their atmospheric lifetime. The importance of such effects is unknown as they have not been considered in microphysical and global radioactivity transport studies to date. Here, we explore the effects of compositional changes on the charging efficiency and coagulation rates of aerosols using a set of kinetic equations that couple all relevant processes (decay, charging and coagulation) and their evolution over time. Compared to a coupled aggregation-tracer model for the prediction of the radioactive composition of particulates undergoing coagulation,more » our kinetic approach can provide similar results using much less central processing unit time. Altogether with other considerations, our approach is computational efficient enough to allow implementation in 3D atmospheric transport models. The decay of radionuclides and the production of decay products within radioactive aerosols may significantly affect the aerosol charging rates, and either hinder or promote the coagulation of multicomponent radioactive aerosols. Our results suggest that radiological phenomena occurring within radioactive aerosols, as well as subsequent effects on aerosol microphysics, should be considered in regional and global models to more accurately predict radioactivity transport in the atmosphere in case of a nuclear plant accident.« less

Trend analysis of the aerosol optical depth from fusion of MISR and MODIS retrievals over China

NASA Astrophysics Data System (ADS)

Guo, Jing; Gu, Xingfa; Yu, Tao; Cheng, Tianhai; Chen, Hao

2014-03-01

Atmospheric aerosol plays an important role in the climate change though direct and indirect processes. In order to evaluate the effects of aerosols on climate, it is necessary to have a research on their spatial and temporal distributions. Satellite aerosol remote sensing is a developing technology that may provide good temporal sampling and superior spatial coverage to study aerosols. The Moderate Resolution Imaging Spectroradiometer (MODIS) and Multi-angle Imaging Spectroradiometer (MISR) have provided aerosol observations since 2000, with large coverage and high accuracy. However, due to the complex surface, cloud contamination, and aerosol models used in the retrieving process, the uncertainties still exist in current satellite aerosol products. There are several observed differences in comparing the MISR and MODIS AOD data with the AERONET AOD. Combing multiple sensors could reduce uncertainties and improve observational accuracy. The validation results reveal that a better agreement between fusion AOD and AERONET AOD. The results confirm that the fusion AOD values are more accurate than single sensor. We have researched the trend analysis of the aerosol properties over China based on nine-year (2002-2010) fusion data. Compared with trend analysis in Jingjintang and Yangtze River Delta, the accuracy has increased by 5% and 3%, respectively. It is obvious that the increasing trend of the AOD occurred in Yangtze River Delta, where human activities may be the main source of the increasing AOD.

Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

NASA Astrophysics Data System (ADS)

Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

2017-12-01

The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Zhanqing; Lau, W. K. -M.; Ramanathan, V.

Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. Themore » atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.« less

Airborne measurements of multi-wavelength aerosol optical depth and cloud-transmitted radiances in the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES)

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Johnson, R. R.; LeBlanc, S. E.; Chang, C. S.; Redemann, J.

2016-12-01

We report on our recent airborne measurements of multi-wavelength aerosol optical depth and cloud-transmitted radiances over the North Atlantic. We ran the Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) in November 2015 and the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) in May and June 2016, both aboard the NASA C-130 aircraft. These sunphotometers provide measurements of overlying cirrus and aerosol optical depths of up to about 0.5 and constrain ecosystem and aerosol retrievals from the accompanying nadir-viewing remote sensing instruments. In addition, 4STAR measures hyperspectral transmitted light, which enables the retrieval of cloud optical depth, effective radius, and thermodynamic phase from below cloud. Our measurements contribute to the science objectives of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES), an interdisciplinary investigation resolving key processes controlling marine ecosystems and aerosols that are essential to our understanding of Earth system function and future change.

Impacts of different aerosol climatologies on the European climate during the last decades

NASA Astrophysics Data System (ADS)

Schultze, Markus; Rockel, Burkhardt

2015-04-01

As summarized in the 5th Assessment Report of the IPCC, the effects of aerosols on the Earth's energy budget are one of the largest uncertainties in a changing climate. Despite a better understanding of aerosol processes since the previous report, it remains unclear to which degree of complexity these processes need to be represented within the climate models to consider their effects in a sufficient manner. Within the nonhydrostatic regional climate model COSMO-CLM, the aerosol climatology of Tanre from 1984 is widely used to simulate the direct effect of aerosols on radiative processes. Apart from a very low spatial resolution and a missing temporal variability, this climatology is dominated by high values of Aerosol Optical Depth (AOD) over Northern Africa, caused by an overestimation of Saharan dust. To investigate the impacts of different aerosol distributions on the European climate, the Tanre aerosol climatology is replaced by the more realistic climatologies of Tegen from 1997 and AEROCOM from 2006 with constant annual cycles of AOD. In addition a control simulation without any aerosol feedbacks was performed. The simulations cover a period of 30 years from 1980 to 2010. In parts of the regions surveyed, we found a near surface cooling, which is strongly linked to AOD, and a broad mid-troposphere warming for all simulations in comparison to the control simulation. A decrease in convective precipitation is mainly caused by stabilization of stratification and by less evapotranspiration resulting from surface cooling. The horizontal differing mid-troposphere warming induces a drop in surface pressure and therefore leads to changes in circulation patterns which are still under investigation. The largest impacts of direct and semi direct aerosol effects was found in summer season. As next step, pre-calculated transient aerosol data will be used to compile an up-to-date aerosol climatology including temporal changes. One main focus of the study will be to investigate whether a decrease in anthropogenic aerosol load in Europe during the last decades enhances the GHG induced near surface warming.

Aerosol and monsoon climate interactions over Asia

NASA Astrophysics Data System (ADS)

Li, Zhanqing; Lau, W. K.-M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S.-S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

2016-12-01

The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcing of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.

Effect of dust and anthropogenic aerosols on columnar aerosol optical properties over Darjeeling (2200 m asl), eastern Himalayas, India.

PubMed

Chatterjee, Abhijit; Ghosh, Sanjay K; Adak, Anandamay; Singh, Ajay K; Devara, Panuganti C S; Raha, Sibaji

2012-01-01

The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca(2+)) during pre-monsoon (Apr-May) which was higher by 162% than its annual mean whereas during winter (Dec-Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO(4)(2-) and black carbon) were higher (76% for black carbon and 96% for fine mode SO(4)(2-)) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas.

Separating Real and Apparent Effects of Cloud, Humidity, and Dynamics on Aerosol Optical Thickness near Cloud Edges

NASA Technical Reports Server (NTRS)

Jeong, Myeong-Jae; Li, Zhanqing

2010-01-01

Aerosol optical thickness (AOT) is one of aerosol parameters that can be measured on a routine basis with reasonable accuracy from Sun-photometric observations at the surface. However, AOT-derived near clouds is fraught with various real effects and artifacts, posing a big challenge for studying aerosol and cloud interactions. Recently, several studies have reported correlations between AOT and cloud cover, pointing to potential cloud contamination and the aerosol humidification effect; however, not many quantitative assessments have been made. In this study, various potential causes of apparent correlations are investigated in order to separate the real effects from the artifacts, using well-maintained observations from the Aerosol Robotic Network, Total Sky Imager, airborne nephelometer, etc., over the Southern Great Plains site operated by the U.S. Department of Energy's Atmospheric Radiation Measurement Program. It was found that aerosol humidification effects can explain about one fourth of the correlation between the cloud cover and AOT. New particle genesis, cloud-processed particles, atmospheric dynamics, and aerosol indirect effects are likely to be contributing to as much as the remaining three fourth of the relationship between cloud cover and AOT.

An overview of mesoscale aerosol processes, comparisons, and validation studies from DRAGON networks

NASA Astrophysics Data System (ADS)

Holben, Brent N.; Kim, Jhoon; Sano, Itaru; Mukai, Sonoyo; Eck, Thomas F.; Giles, David M.; Schafer, Joel S.; Sinyuk, Aliaksandr; Slutsker, Ilya; Smirnov, Alexander; Sorokin, Mikhail; Anderson, Bruce E.; Che, Huizheng; Choi, Myungje; Crawford, James H.; Ferrare, Richard A.; Garay, Michael J.; Jeong, Ukkyo; Kim, Mijin; Kim, Woogyung; Knox, Nichola; Li, Zhengqiang; Lim, Hwee S.; Liu, Yang; Maring, Hal; Nakata, Makiko; Pickering, Kenneth E.; Piketh, Stuart; Redemann, Jens; Reid, Jeffrey S.; Salinas, Santo; Seo, Sora; Tan, Fuyi; Tripathi, Sachchida N.; Toon, Owen B.; Xiao, Qingyang

2018-01-01

Over the past 24 years, the AErosol RObotic NETwork (AERONET) program has provided highly accurate remote-sensing characterization of aerosol optical and physical properties for an increasingly extensive geographic distribution including all continents and many oceanic island and coastal sites. The measurements and retrievals from the AERONET global network have addressed satellite and model validation needs very well, but there have been challenges in making comparisons to similar parameters from in situ surface and airborne measurements. Additionally, with improved spatial and temporal satellite remote sensing of aerosols, there is a need for higher spatial-resolution ground-based remote-sensing networks. An effort to address these needs resulted in a number of field campaign networks called Distributed Regional Aerosol Gridded Observation Networks (DRAGONs) that were designed to provide a database for in situ and remote-sensing comparison and analysis of local to mesoscale variability in aerosol properties. This paper describes the DRAGON deployments that will continue to contribute to the growing body of research related to meso- and microscale aerosol features and processes. The research presented in this special issue illustrates the diversity of topics that has resulted from the application of data from these networks.

In Situ Single Particle Measurement of Atmospheric Aging of Carbonaceous Aerosols During CARES

NASA Astrophysics Data System (ADS)

Cahill, J. F.; Suski, K.; Hubbe, J.; Shilling, J.; Zaveri, R. A.; Springston, S. R.; Prather, K. A.

2011-12-01

Atmospheric aging of aerosols through photochemistry, heterogeneous reactions and aqueous processing can change their physical and chemical properties, impacting their gas uptake, radiative forcing, and activation of cloud nuclei. Understanding the timescale and magnitude of this aging process is essential for accurate aerosol-climate modeling and predictions. An aircraft aerosol time-of-flight mass spectrometer (A-ATOFMS) measured single particle mixing state during the Carbonaceous Aerosols and Radiative Effects Study (CARES) in the summer of 2010 over Sacramento, CA. On 6/23/10, flights in the morning and afternoon performed pseudo-Lagrangian sampling of the Sacramento urban plume. Carbonaceous particles from these flights were classified into 'aged' and 'fresh' classes based on their mixing state, with aged particles having more secondary species, such as nitrate and sulfate. In the morning flight, a clear decreasing trend in the ratio of fresh/aged particle types was seen as the flight progressed, whereas in the afternoon flight, the ratio was essentially constant. These data show that in the morning carbonaceous aerosols can become heavily oxidized in a few hours. Further analysis of particle mixing state and the timescale of carbonaceous aerosol aging will be presented

Microphysical processes affecting stratospheric aerosol particles

NASA Technical Reports Server (NTRS)

Hamill, P.; Toon, O. B.; Kiang, C. S.

1977-01-01

Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

A Compact Airborne High Spectral Resolution Lidar for Observations of Aerosol and Cloud Optical Properties

NASA Technical Reports Server (NTRS)

Hostetler, Chris A.; Hair, John W.; Cook, Anthony L.

2002-01-01

We are in the process of developing a nadir-viewing, aircraft-based high spectral resolution lidar (HSRL) at NASA Langley Research Center. The system is designed to measure backscatter and extinction of aerosols and tenuous clouds. The primary uses of the instrument will be to validate spaceborne aerosol and cloud observations, carry out regional process studies, and assess the predictions of chemical transport models. In this paper, we provide an overview of the instrument design and present the results of simulations showing the instrument's capability to accurately measure extinction and extinction-to-backscatter ratio.

Primary and secondary aerosols in Beijing in winter: sources, variations and processes

NASA Astrophysics Data System (ADS)

Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

2016-07-01

Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size distributions, oxidation states of OA and evolutionary processes of secondary aerosols.

Aerosol ionic components at Mt. Heng in central southern China: abundances, size distribution, and impacts of long-range transport.

PubMed

Gao, Xiaomei; Xue, Likun; Wang, Xinfeng; Wang, Tao; Yuan, Chao; Gao, Rui; Zhou, Yang; Nie, Wei; Zhang, Qingzhu; Wang, Wenxing

2012-09-01

Water-soluble ions in PM(2.5) were continuously measured, along with the measurements of many other species and collection of size-resolved aerosol samples, at the summit of Mt. Heng in the spring of 2009, to understand the sources of aerosols in rural central southern China. The mean concentrations of SO(4)(2-), NH(4)(+) and NO(3)(-) in PM(2.5) were 8.02, 2.94 and 1.47 μg/m(3), indicating a moderate aerosol pollution level at Mt. Heng. Water-soluble ions composed approximately 40% of the PM(2.5) mass on average. PM(2.5) was weakly acidic with about 66% of the samples being acidic. SO(4)(2-), NO(3)(-) and NH(4)(+) exhibited similar diurnal patterns with a broad afternoon maximum. SO(4)(2-) and NH(4)(+) were mainly present in the fine aerosols with a peak in the droplet mode of 0.56-1 μm, suggesting the important role of cloud processing in the formation of aerosol sulfate. NO(3)(-) was largely distributed in the coarse particles with a predominant peak in the size-bin of 3.2-5.6 μm. Long-distance transport of processed air masses, dust aerosols, and cloud/fog processes were the major factors determining the variations of fine aerosol at Mt. Heng. The results at Mt. Heng were compared with those obtained from our previous study at Mt. Tai in north China. The comparison revealed large differences in the aerosol characteristics and processes between southern and northern China. Backward trajectories indicated extensive transport of anthropogenic pollution from the coastal regions of eastern/northern China and the Pearl River Delta (PRD) to Mt. Heng in spring, highlighting the need for regionally coordinated control measures for the secondary pollutants. Copyright © 2012 Elsevier B.V. All rights reserved.

Enhancement of PM2.5 Concentrations by Aerosol-Meteorology Interactions Over China

NASA Astrophysics Data System (ADS)

Zhang, Xin; Zhang, Qiang; Hong, Chaopeng; Zheng, Yixuan; Geng, Guannan; Tong, Dan; Zhang, Yuxuan; Zhang, Xiaoye

2018-01-01

Aerosol-meteorology interactions can change surface aerosol concentrations via different mechanisms such as altering radiation budget or cloud microphysics. However, few studies investigated the impacts of different mechanisms on temporal and spatial distribution of PM2.5 concentrations over China. Here we used the fully coupled Weather Research and Forecasting model with online chemistry (WRF-Chem) to quantify the enhancement of PM2.5 concentrations by aerosol-meteorology feedback in China in 2014 for different seasons and separate the relative impacts of aerosol radiation interactions (ARIs) and aerosol-cloud interactions (ACIs). We found that ARIs and ACIs could increase population-weighted annual mean PM2.5 concentration over China by 4.0 μg/m3 and 1.6 μg/m3, respectively. We found that ARIs play a dominant role in aerosol-meteorology interactions in winter, while the enhancement of PM2.5 concentration by ARIs and ACIs is comparable in other three seasons. ARIs reduced the wintertime monthly mean wind speed and planetary boundary layer (PBL) height by up to 0.1 m/s and 160 m, respectively, but increased the relative humidity by up to 4%, leading to accumulation of pollutants within PBL. Also, ARIs reduced dry deposition velocity of aerosols by up to 20%, resulting in an increase in PM2.5 lifetime and concentrations. ARIs can increase wintertime monthly mean surface PM2.5 concentration by a maximum of 30 μg/m3 in Sichuan Basin. ACIs can also increase PM2.5 concentration with more significant impacts in wet seasons via reduced wet scavenging and enhanced in-cloud chemistry. Dominant processes in PM2.5 enhancement are also clarified in different seasons. Results show that physical process is more important than chemical processes in winter in ARIs, while chemical process of secondary inorganic aerosols production may be crucial in wet seasons via ACIs.

Marine CCN Activation: A Battle Between Primary and Secondary Sources

NASA Astrophysics Data System (ADS)

Fossum, K. N.; Ovadnevaite, J.; Ceburnis, D.; Preissler, J.; O'Dowd, C. D. D.

2017-12-01

Low-altitude marine clouds are cooling components of the Earth's radiative budget, and the direct measurements of the properties of these cloud forming particles, called cloud condensation nuclei (CCN), helps modellers reconstruct aerosol-to-cloud droplet processes, improving climate predictions. In this study, CCN are directly measured (CCNC commercially available from Droplet Measurement Technologies, Inc.), resolving activation efficiency at varying supersaturated conditions. Previous studies show that sub-micron sea salt particulates activate competitively, reducing the cloud peak supersaturation and inhibiting the activation of sulphate particulates into cloud droplets, making chemical composition an important component in determining cloud droplet number concentration (CDNC). This effect and the sea salt numbers needed to induce it have not been previously studied long-term in the natural environment. As part of this work, data was analysed from a two month marine research ship campaign during the Antarctic Austral summer, in 2015. Ambient aerosol in the Scotia Sea region was sampled continuously, and through the use of multiple aerosol in-situ instruments, this study shows that CCN number in both the open ocean and ice-pack influenced air masses are largely proportionate to secondary aerosol. However, open ocean air masses show a significant primary aerosol influence which changes the aerosol characteristics. Higher sea salt mass concentrations in the open ocean lead to better CCN activation efficiencies. Coupled with high wind speeds and sea surface turbulence, open ocean air masses show a repression of the CDNC number compared with the theoretical values that should be expected with the sub-cloud aerosol number concentration. This is not seen in the ice-pack air masses. Work is ongoing, looking into a long-term North Atlantic marine aerosol data set, but it would appear that chemical composition plays a large role in aerosol to cloud droplet processes, and can initially restrict CDNC when sea salt is abundant and updraft velocities are relatively low.

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Qi

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routinemore » measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from this research into data products and formulations that may be directly used to inform, improve, and evaluate regional and global models. In addition, we will continue our current very active collaborations with several modeling groups to enhance the use and interpretation of our data products. Overall, this research will contribute new data to improve quantification of the aerosol’s effects on climate and thus the achievement of ASR’s science goal of – “improving the fidelity and predictive capability of global climate models”.« less

Impacts of Aerosol Direct Effects on the South Asian climate: Assessment of Radiative Feedback Processes Using Model Simulations and Satellite/surface Measurements

NASA Astrophysics Data System (ADS)

Wang, S.; Gautam, R.; Lau, W. K.; Tsay, S.; Sun, W.; Kim, K.; Chern, J.; Colarco, P. R.; Hsu, N. C.; Lin, N.

2011-12-01

Current assessment of aerosol radiative effect is hindered by our incomplete knowledge of aerosol optical properties, especially absorption, and our current inability to quantify physical and microphysical processes. In this research, we investigate direct aerosol radiative effect over heavy aerosol loading areas (e.g., Indo-Gangetic Plains, South/East Asia) and its feedbacks on the South Asian climate during the pre-monsoon season (March-June) using the Purdue Regional Climate Model (PRCM) with prescribed aerosol data derived by the NASA Goddard Earth Observing System Model (GEOS-5). Our modeling domain covers South and East Asia (60-140E and 0-50N) with spatial resolutions of 45 km in horizontal and 28 layers in vertical. The model is integrated from 15 February to 30 June 2008 continuously without nudging (i.e., only forced by initial/boundary conditions). Two numerical experiments are conducted with and without the aerosol-radiation effects. Both simulations are successful in reproducing the synoptic patterns on seasonal-to-interannual time scales and capturing a pre-monsoon feature of the northward rainfall propagation over Indian region in early June which shown in Tropical Rainfall Measuring Mission (TRMM) observation. Preliminary result suggests aerosol-radiation interactions mainly alter surface-atmosphere energetics and further result in an adjustment of the vertical temperature distribution in lower atmosphere (below 700 hPa). The modifications of temperature and associated rainfall and circulation feedbacks on the regional climate will be discussed in the presentation. In addition to modeling study, we will also present the most recent results on aerosol properties, regional aerosol absorption, and radiative forcing estimation based on NASA's operational satellite and ground-based remote sensing. Observational results show spatial gradients in aerosol loading and solar absorption accounting over Indo-Gangetic Plains during the pre-monsoon season. The direct radiative forcing of aerosols at surface to be -19-23 Wm-2 (12-15 % of the surface solar insolation) over NW India is estimated using an observational approach. A comparison of aerosol radiative forcing between numerical simulation and observational estimate will be presented. Overall, this work will demonstrate the aerosol direct effects from both modeling and observation perspectives, and further to assess the physical processes underlying the aerosol radiative feedbacks and possible impacts on the large-scale South Asian monsoon system.

Applying super-droplets as a compact representation of warm-rain microphysics for aerosol-cloud-aerosol interactions

NASA Astrophysics Data System (ADS)

Arabas, S.; Jaruga, A.; Pawlowska, H.; Grabowski, W. W.

2012-12-01

Clouds may influence aerosol characteristics of their environment. The relevant processes include wet deposition (rainout or washout) and cloud condensation nuclei (CCN) recycling through evaporation of cloud droplets and drizzle drops. Recycled CCN physicochemical properties may be altered if the evaporated droplets go through collisional growth or irreversible chemical reactions (e.g. SO2 oxidation). The key challenge of representing these processes in a numerical cloud model stems from the need to track properties of activated CCN throughout the cloud lifecycle. Lack of such "memory" characterises the so-called bulk, multi-moment as well as bin representations of cloud microphysics. In this study we apply the particle-based scheme of Shima et al. 2009. Each modelled particle (aka super-droplet) is a numerical proxy for a multiplicity of real-world CCN, cloud, drizzle or rain particles of the same size, nucleus type,and position. Tracking cloud nucleus properties is an inherent feature of the particle-based frameworks, making them suitable for studying aerosol-cloud-aerosol interactions. The super-droplet scheme is furthermore characterized by linear scalability in the number of computational particles, and no numerical diffusion in the condensational and in the Monte-Carlo type collisional growth schemes. The presentation will focus on processing of aerosol by a drizzling stratocumulus deck. The simulations are carried out using a 2D kinematic framework and a VOCALS experiment inspired set-up (see http://www.rap.ucar.edu/~gthompsn/workshop2012/case1/).

Assessing the impact of aerosol-atmosphere interactions in convection-permitting regional climate simulations: the Rolf medicane in 2011

NASA Astrophysics Data System (ADS)

José Gómez-Navarro, Juan; María López-Romero, José; Palacios-Peña, Laura; Montávez, Juan Pedro; Jiménez-Guerrero, Pedro

2017-04-01

A critical challenge for assessing regional climate change projections relies on improving the estimate of atmospheric aerosol impact on clouds and reducing the uncertainty associated with the use of parameterizations. In this sense, the horizontal grid spacing implemented in state-of-the-art regional climate simulations is typically 10-25 kilometers, meaning that very important processes such as convective precipitation are smaller than a grid box, and therefore need to be parameterized. This causes large uncertainties, as closure assumptions and a number of parameters have to be established by model tuning. Convection is a physical process that may be strongly conditioned by atmospheric aerosols, although the solution of aerosol-cloud interactions in warm convective clouds remains nowadays a very important scientific challenge, rendering parametrization of these complex processes an important bottleneck that is responsible from a great part of the uncertainty in current climate change projections. Therefore, the explicit simulation of convective processes might improve the quality and reliability of the simulations of the aerosol-cloud interactions in a wide range of atmospheric phenomena. Particularly over the Mediterranean, the role of aerosol particles is very important, being this a crossroad that fuels the mixing of particles from different sources (sea-salt, biomass burning, anthropogenic, Saharan dust, etc). Still, the role of aerosols in extreme events in this area such as medicanes has been barely addressed. This work aims at assessing the role of aerosol-atmosphere interaction in medicanes with the help of the regional chemistry/climate on-line coupled model WRF-CHEM run at a convection-permitting resolution. The analysis is exemplary based on the "Rolf" medicane (6-8 November 2011). Using this case study as reference, four sets of simulations are run with two spatial resolutions: one at a convection-permitting configuration of 4 km, and other at the lower resolution of 12 km, in whose case the convection has to be parameterized. Each configuration is used to produce two simulations, including and not including aerosol-radiation-cloud interactions. The comparison of the simulated output at different scales allows to evaluate the impact of sub-grid scale mixing of precursors on aerosol production. By focusing on these processes at different resolutions, the differences between convection-permitting models running at resolutions of 4 km to 12 km can be explored. Preliminary results indicate that the inclusion of aerosol effects may indeed impact the severity of this simulated medicane, especially sea salt aerosols, and leads to important spatial shifts and differences in intensity of surface precipitation.

Indirect estimation of absorption properties for fine aerosol particles using AATSR observations: a case study of wildfires in Russia in 2010

NASA Astrophysics Data System (ADS)

Rodriguez, E.; Kolmonen, P.; Virtanen, T. H.; Sogacheva, L.; Sundstrom, A.-M.; de Leeuw, G.

2015-08-01

The Advanced Along-Track Scanning Radiometer (AATSR) on board the ENVISAT satellite is used to study aerosol properties. The retrieval of aerosol properties from satellite data is based on the optimized fit of simulated and measured reflectances at the top of the atmosphere (TOA). The simulations are made using a radiative transfer model with a variety of representative aerosol properties. The retrieval process utilizes a combination of four aerosol components, each of which is defined by their (lognormal) size distribution and a complex refractive index: a weakly and a strongly absorbing fine-mode component, coarse mode sea salt aerosol and coarse mode desert dust aerosol). These components are externally mixed to provide the aerosol model which in turn is used to calculate the aerosol optical depth (AOD). In the AATSR aerosol retrieval algorithm, the mixing of these components is decided by minimizing the error function given by the sum of the differences between measured and calculated path radiances at 3-4 wavelengths, where the path radiances are varied by varying the aerosol component mixing ratios. The continuous variation of the fine-mode components allows for the continuous variation of the fine-mode aerosol absorption. Assuming that the correct aerosol model (i.e. the correct mixing fractions of the four components) is selected during the retrieval process, also other aerosol properties could be computed such as the single scattering albedo (SSA). Implications of this assumption regarding the ratio of the weakly/strongly absorbing fine-mode fraction are investigated in this paper by evaluating the validity of the SSA thus obtained. The SSA is indirectly estimated for aerosol plumes with moderate-to-high AOD resulting from wildfires in Russia in the summer of 2010. Together with the AOD, the SSA provides the aerosol absorbing optical depth (AAOD). The results are compared with AERONET data, i.e. AOD level 2.0 and SSA and AAOD inversion products. The RMSE (root mean square error) is 0.03 for SSA and 0.02 for AAOD lower than 0.05. The SSA is further evaluated by comparison with the SSA retrieved from the Ozone Monitoring Instrument (OMI). The SSA retrieved from both instruments show similar features, with generally lower AATSR-estimated SSA values over areas affected by wildfires.

Analysis of aerosol-cloud-precipitation interactions based on MODIS data

NASA Astrophysics Data System (ADS)

Cheng, Feng; Zhang, Jiahua; He, Junliang; Zha, Yong; Li, Qiannan; Li, Yunmei

2017-01-01

Aerosols exert an indirect impact on climate change via its impact on clouds by altering its radiative and optical properties which, in turn, changes the process of precipitation. Over recent years how to study the indirect climate effect of aerosols has become an important research topic. In this study we attempted to understand the complex mutual interactions among aerosols, clouds and precipitation through analysis of the spatial correlation between aerosol optical depth (AOD), cloud effective radius (CER) and precipitation during 2000-2012 in central-eastern China that has one of the highest concentrations of aerosols globally. With the assistance of moderate resolution imaging spectroradiometer (MODIS)-derived aerosol and cloud product data, this analysis focuses on regional differentiation and seasonal variation of the correlation in which in situ observed precipitation was incorporated. On the basis of the achieved results, we proposed four patterns depicting the mutual interactions between aerosols, clouds and precipitation. They characterize the indirect effects of aerosols on the regional scale. These effects can be summarized as complex seasonal variations and north-south regional differentiation over the study area. The relationship between AOD and CER is predominated mostly by the first indirect effect (the negative correlation between AOD and CER) in the north of the study area in the winter and spring seasons, and over the entire study area in the summer season. The relationship between CER and precipitation is dominated chiefly by the second indirect effect (the positive correlation between CER and precipitation) in the northern area in summer and over the entire study area in autumn. It must be noted that aerosols are not the factor affecting clouds and rainfall singularly. It is the joint effect of aerosols with other factors such as atmospheric dynamics that governs the variation in clouds and rainfall.

Stratospheric Heterogeneous Chemistry and Microphysics: Model Development, Validation and Applications

NASA Technical Reports Server (NTRS)

Turco, Richard P.

1996-01-01

The objectives of this project are to: define the chemical and physical processes leading to stratospheric ozone change that involve polar stratospheric clouds (PSCS) and the reactions occurring on the surfaces of PSC particles; study the formation processes, and the physical and chemical properties of PSCS, that are relevant to atmospheric chemistry and to the interpretation of field measurements taken during polar stratosphere missions; develop quantitative models describing PSC microphysics and heterogeneous chemical processes; assimilate laboratory and field data into these models; and calculate the extent of chemical processing on PSCs and the impact of specific microphysical processes on polar composition and ozone depletion. During the course of the project, a new coupled microphysics/physical-chemistry/ photochemistry model for stratospheric sulfate aerosols and nitric acid and ice PSCs was developed and applied to analyze data collected during NASA's Arctic Airborne Stratospheric Expedition-II (AASE-II) and other missions. In this model, detailed treatments of multicomponent sulfate aerosol physical chemistry, sulfate aerosol microphysics, polar stratospheric cloud microphysics, PSC ice surface chemistry, as well as homogeneous gas-phase chemistry were included for the first time. In recent studies focusing on AASE measurements, the PSC model was used to analyze specific measurements from an aircraft deployment of an aerosol impactor, FSSP, and NO(y) detector. The calculated results are in excellent agreement with observations for particle volumes as well as NO(y) concentrations, thus confirming the importance of supercooled sulfate/nitrate droplets in PSC formation. The same model has been applied to perform a statistical study of PSC properties in the Northern Hemisphere using several hundred high-latitude air parcel trajectories obtained from Goddard. The rates of ozone depletion along trajectories with different meteorological histories are presently being systematically evaluated to identify the principal relationships between ozone loss and aerosol state. Under this project, we formulated a detailed quantitative model that predicts the multicomponent composition of sulfate aerosols under stratospheric conditions, including sulfuric, nitric, hydrochloric, hydrofluoric and hydrobromic acids. This work defined for the first time the behavior of liquid ternary-system type-1b PSCS. The model also allows the compositions and reactivities of sulfate aerosols to be calculated over the entire range of environmental conditions encountered in the stratosphere (and has been incorporated into a trajectory/microphysics model-see above). Important conclusions that derived from this work over the last few years include the following: the HNO3 content of liquid-state aerosols dominate PSCs below about 195 K; the freezing of nitric acid ice from sulfate aerosol solutions is likely to occur within a few degrees K of the water vapor frost point; the uptake and reactions of HCl in liquid aerosols is a critical component of PSC heterogeneous chemistry. In a related application of this work, the inefficiency of chlorine injection into the stratosphere during major volcanic eruptions was explained on the basis of nucleation of sulfuric acid aerosols in rising volcanic plumes leading to the formation of supercooled water droplets on these aerosols, which efficiently scavenges HCl via precipitation.

An in-depth investigation of the life cycle of sulfate from the Kilauea volcano using satellite observations and EMAC model calculations

NASA Astrophysics Data System (ADS)

Penning de Vries, Marloes; Beirle, Steffen; Brühl, Christoph; Hörmann, Christoph; Wagner, Thomas

2015-04-01

The Kilauea volcano (Hawaii), currently perhaps the most active volcano on Earth, has been continuously erupting since the beginning of 1983. A pronounced degassing phase in March-November 2008 caused the formation of an extensive SO2 plume, which in turn led to the formation of sulfate aerosols. The steady trade winds and lack of interfering sources previously allowed us to determine the life time of SO2 using only satellite-based measurements (no a priori or model information). The current investigation is focused on improving our understanding of the processes contributing to sulfate aerosol formation, processing, and loss. We use space-based aerosol measurements by MODIS, MISR, and CALIOP to characterize the aerosols (amount, size, altitude) and study the evolution of aerosol optical depth as a function of distance from the volcano to determine formation and loss rates. The outcome is compared to results from calculations using the EMAC (ECHAM/MESSy Atmospheric Chemistry) model to test the state of understanding of the sulfate aerosol life cycle.

Scattering and Absorption of E&M radiation by small particles-applications to study impact of biomass aerosols on climate

NASA Astrophysics Data System (ADS)

Bililign, Solomon; Singh, Sujeeta; Fiddler, Marc; Smith, Damon

2015-03-01

The phenomena of scattering, absorption, and emission of light and other electromagnetic radiation by small particles are central to many science and engineering disciplines. Absorption of solar radiation by black carbon aerosols has a significant impact on the atmospheric energy distribution and hydrologic processes. By intercepting incoming solar radiation before it reaches the surface, aerosols heat the atmosphere and, in turn, cool the surface. The magnitude of the atmospheric forcing induced by anthropogenic absorbing aerosols, mainly black carbon (BC) emitted from biomass burning and combustion processes has been suggested to be comparable to the atmospheric forcing by all greenhouse gases (GHGs). Despite the global abundance of biomass burning for cooking, forests clearing for agriculture and wild fires, the optical properties of these aerosols have not been characterized at wide range of wavelengths. Our laboratory uses a combination of Cavity ring down spectroscopy and integrating nephelometry to measure optical properties of (extinction, absorption and scattering coefficients) of biomass aerosols. Preliminary results will be presented. Supported by the Department of Defense under Grant #W911NF-11-1-0188.

Reconciling the aerosol-liquid water path relationship in the ECHAM6-HAM GCM and the Aerosol_cci/Cloud_cci (A)ATSR dataset by minimizing the effect of aerosol swelling

NASA Astrophysics Data System (ADS)

Neubauer, D.; Christensen, M.; Lohmann, U.; Poulsen, C. A.

2016-12-01

Studies using present day variability to assess statistical relationships between aerosol and cloud properties find different strengths of these relationships between satellite data and general circulation model (GCM) data. This discrepancy can be explained by structural uncertainties due to differences in the analysis/observational scale and the process scale or spurious relationships between aerosol and cloud properties. Such spurious relationships are the growth of aerosol particles in the humid environment surrounding clouds, misclassification of partly cloudy satellite pixels as cloud free pixels, brightening of aerosol particles by sunlight reflected at cloud edges, or effects of clouds on aerosol like processing of aerosol particles in clouds by nucleation or impact scavenging and subsequent growth by heterogeneous chemistry and release by cloud droplet evaporation or wet scavenging of aerosol particles. To minimize the effects of spatial aggregation and spurious relationships we apply a new nearest neighbour approach to high resolution (A)ATSR datasets from the Aerosol_cci and Cloud_cci projects of the Climate Change Initiative (CCI) programme of ESA. For the ECHAM6-HAM GCM we quantify the impact of using dry aerosol (without aerosol water) in the analysis to mimic the effect of the nearest neighbour approach. The aerosol-liquid water path relationship in ECHAM6-HAM is systematically stronger than in (A)ATSR data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM the strength of the aerosol-liquid water path relationship agrees much better with the ones of (A)ATSR or MODIS. We further find that while the observed relationships of different satellite sensors ((A)ATSR vs. MODIS) are not always consistent for tested environmental conditions the relationships in ECHAM6-HAM are missing a strong dependence on environmental conditions which is critical for bridging the gap between satellite and model estimates of aerosol indirect forcing.

Toward Investigating Optically Trapped Organic Aerosols with CARS Microspectroscopy

NASA Astrophysics Data System (ADS)

Voss, L. F.

2009-12-01

The Intergovernmental Panel on Climate Change notes the huge uncertainty in the effect that atmospheric aerosols play in determining overall global temperature, specifically in their ability to nucleate clouds. To better understand aerosol chemistry, the novel coupling of gradient force optical trapping with broad bandwidth coherent anti-Stokes Raman scattering (CARS) spectroscopy is being developed to study single particles suspended in air. Building on successful designs employed separately for the techniques, this hybrid technology will be used to explain how the oxidation of organic compounds changes the chemical and physical properties of aerosols. By trapping the particles, an individual aerosol can be studied for up to several days. Using a broad bandwidth pulse for one of the incident beams will result in a Raman vibrational spectrum from every laser pulse. Combined with signal enhancement due to resonance and coherence of nonlinear CARS spectroscopy, this technique will allow for acquisition of data on the millisecond time scale, facilitating the study of dynamic processes. This will provide insights on how aerosols react with and absorb species from the gas phase. These experiments will increase understanding of aerosol oxidation and growth mechanisms and the effects that aerosols have on our atmosphere and climate. Progress in efforts developing this novel technique to study model systems is presented.

The performance of Yonsei CArbon Retrieval (YCAR) algorithm with improved aerosol information using GOSAT measurements over East Asia

NASA Astrophysics Data System (ADS)

Jung, Y.; Kim, J.; Kim, W.; Boesch, H.; Yoshida, Y.; Cho, C.; Lee, H.; Goo, T. Y.

2016-12-01

The Greenhouse Gases Observing SATellite (GOSAT) is the first satellite dedicated to measure atmospheric CO2 concentrations from space that can able to improve our knowledge about carbon cycle. Several studies have performed to develop the CO2 retrieval algorithms using GOSAT measurements, but limitations in spatial coverage and uncertainties due to aerosols and thin cirrus clouds are still remained as a problem for monitoring CO2 concentration globally. In this study, we develop the Yonsei CArbon Retrieval (YCAR) algorithm based on optimal estimation method to retrieve the column-averaged dry-air mole fraction of carbon dioxide (XCO2) with optimized a priori CO2 profiles and aerosol models over East Asia. In previous studies, the aerosol optical properties (AOP) and the aerosol top height used to cause significant errors in retrieved XCO2 up to 2.5 ppm. Since this bias comes from a rough assumption of aerosol information in the forward model used in CO2 retrieval process, the YCAR algorithm improves the process to take into account AOPs as well as aerosol vertical distribution; total AOD and the fine mode fraction (FMF) are obtained from the ground-based measurements closely located, and other parameters are obtained from a priori information. Comparing to ground-based XCO2 measurements, the YCAR XCO2 product has a bias of 0.59±0.48 ppm and 2.16±0.87 ppm at Saga and Tsukuba sites, respectively, showing lower biases and higher correlations rather than the GOSAT standard products. These results reveal that considering better aerosol information can improve the accuracy of CO2 retrieval algorithm and provide more useful XCO2 information with reduced uncertainties.

Modeling of growth, evaporation and sedimentation effects on transmission of visible and IR laser beams in artificial fogs

NASA Technical Reports Server (NTRS)

Yue, G. K.; Deepak, A.

1980-01-01

The dense polydisperse aerosol particles in a quiet chamber may spontaneously go through different microphysical processes including gravitational sedimentation, thermal coagulation, and growth or evaporation. In an earlier paper, we presented the results of a parametric study of the combined and separate effects of thermal coagulation and sedimentation on the time dependence of extinction of four visible and IR laser beams traversing an aerosol medium. As a continuation of this series of studies, the separate and combined effects of growth or evaporation and gravitational sedimentation on the time dependence of extinction of the same four visible and IR laser beams traversing in artificial fogs will be reported in this paper. The method of numerically modeling the change of water droplet size distribution with time due to growth/evaporation and the cutoff of larger aerosols due to gravitational sedimentation is described in detail. Factors governing the relative importance of these two processes are discussed. Results of this study show that the relative humidity or ambient temperature is a crucial parameter in determining the optical depth of the water droplet and aerosol media undergoing microphysical processes.

Organic and inorganic markers and stable C-, N-isotopic compositions of tropical coastal aerosols from megacity Mumbai: sources of organic aerosols and atmospheric processing

NASA Astrophysics Data System (ADS)

Aggarwal, S. G.; Kawamura, K.; Umarji, G. S.; Tachibana, E.; Patil, R. S.; Gupta, P. K.

2013-05-01

To better understand the sources of PM10 samples in Mumbai, India, aerosol chemical composition, i.e., total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4‰, also suggests that biofuel/biomass burning is a predominate source in both the summer and winter seasons. Aerosol mass concentrations of major species increased 3-4 times in winter compared to summer, indicating enhanced emission from these sources in the winter season. Photochemical production tracers, C2 diacid and nssSO42-, do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for daytime (0.37 ± 0.06 (0.28 ± 0.04)) and nighttime (0.38 ± 0.07 (0.28 ± 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant and the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from -27.0 to -25.4‰, with slightly lower average (-26.5 ± 0.3‰) in summer than in winter (-25.9 ± 0.3‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the relative increment in 13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in summer aerosols. However, these conclusions are based on the analysis of a limited number of samples (n=25) and more information on this topic may be needed from other similar coastal sites in future.

Aerosol-radiation-cloud interactions in the South-East Atlantic: first results from the ORACLES-2016 deployment and plans for future activities

NASA Astrophysics Data System (ADS)

Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; Abel, S.

2016-12-01

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for regional and global climate change predictions. Our understanding of aerosol-cloud interactions in the SE Atlantic is severely limited. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We describe first results from various synergistic, international research activities aimed at studying aerosol-cloud interactions in the region: NASA's airborne ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) deployment in August/September of 2016, the DoE's LASIC (Layered Atlantic Smoke Interactions with Clouds) deployment of the ARM Mobile Facility to Ascension Island (June 2016 - October 2017), the ground-based components of CNRS' AEROCLO-sA (Aerosols Clouds and Fog over the west coast of southern Africa), and ongoing regional-scale integrative, process-oriented science efforts as part of SEALS-sA (Sea Earth Atmosphere Linkages Study in southern Africa). We expect to describe experimental setups as well as showcase initial aerosol and cloud property distributions. Furthermore, we discuss the implementation of future activities in these programs in coordination with the UK Met Office's CLARIFY (CLoud-Aerosol-Radiation Interactions and Forcing) experiment in 2017.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidovits, Paul

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign andmore » much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in 17 manuscripts published in refereed journals.« less

Development of the aerosol generation system for simulating the dry deposition behavior of radioaerosol emitted by the accident of FDNPP

NASA Astrophysics Data System (ADS)

Zhang, Z.

2015-12-01

A large amount of radioactivity was discharged by the accident of FDNPP. The long half-life radionuclide, 137Cs was transported through the atmosphere mainly as the aerosol form and deposited to the forests in Fukushima prefecture. After the dry deposition of the 137Cs, the foliar uptake process would occur. To evaluate environmental transfer of radionuclides, the dry deposition and following foliar uptake is very important. There are some pioneering studies for radionuclide foliar uptake with attaching the solution containing stable target element on the leaf, however, cesium oxide aerosols were used for these deposition study [1]. In the FDNPP case, 137Cs was transported in sulfate aerosol form [2], so the oxide aerosol behaviors could not represent the actual deposition behavior in this accident. For evaluation of whole behavior of 137Cs in vegetation system, fundamental data for deposition and uptake process of sulfate aerosol was desired. In this study, we developed aerosol generation system for simulating the dry deposition and the foliar uptake behaviors of aerosol in the different chemical constitutions. In this system, the method of aerosol generation based on the spray drying. Solution contained 137Cs was send to a nozzle by a syringe pump and spraying with a high speed air flow. The sprayed mist was generated in a chamber in the relatively high temperature. The solution in the mist was dried quickly, and micro size solid aerosols consisting 137Cs were generated. The aerosols were suctioned by an ejector and transported inside a tube by the dry air flow, then were directly blown onto the leaves. The experimental condition, such as the size of chamber, chamber temperature, solution flow rate, air flow rate and so on, were optimized. In the deposition experiment, the aerosols on leaves were observed by a SEM/EDX system and the deposition amount was evaluated by measuring the stable Cs remaining on leaf. In the presentation, we will discuss the detail results of aerosol deposition behavior using the developed system. [1]C.Madoz-Escande, et al., Journal of Environmental Radioactivity, 73 pp49-71, (2004) [2] N. Kaneyasu, et al.,Environmental Science & Technology, 2012, 46 (11), pp 5720-5726

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds

PubMed Central

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H.; Rudich, Yinon

2013-01-01

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges. PMID:24297908

Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

PubMed

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

2013-12-17

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

Aircraft- and ground-based assessment of the CCN-AOD relationship and implications on model analysis of ACI and underlying aerosol processes

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Lathem, T. L.; Redemann, J.; Jefferson, A.; Wood, R.

2014-12-01

Contrary to common assumptions in satellite-based modeling of aerosol-cloud interactions, ∂logCCN/∂logAOD is less than unity, i.e., the number concentration of cloud condensation nuclei (CCN) less than doubles as aerosol optical depth (AOD) doubles. This can be explained by omnipresent aerosol processes. Condensation, coagulation and cloud processing, for example, generally make particles scatter more light while hardly increasing their number. This paper reports on the relationship in local air masses between CCN concentration, aerosol size distribution and light extinction observed from aircraft and the ground at diverse locations. The CCN-to-local-extinction relationship, when averaged over ~1 km distance and sorted by the wavelength dependence of extinction, varies approximately by a factor of 2, reflecting the variability in aerosol intensive properties. This, together with retrieval uncertainties and the variability in aerosol spatio-temporal distribution and hygroscopic growth, challenges satellite-based CCN estimates. However, the large differences in estimated CCN may correspond to a considerably lower uncertainty in cloud drop number concentration (CDNC), given the sublinear response of CDNC to CCN. Overall, our findings from airborne and ground-based observations call for model-based reexamination of aerosol-cloud interactions and underlying aerosol processes.

Recent advances in understanding secondary organic aerosols: implications for global climate forcing

NASA Astrophysics Data System (ADS)

Shrivastava, Manish

2017-04-01

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the 'climate sensitivity'). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, often represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This presentation is based on a US Department of Energy Atmospheric Systems Research sponsored workshop, which highlighted key SOA processes overlooked in climate models that could greatly affect climate forcing estimates. We will highlight the importance of processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. We also highlight some of the recently discovered important processes that involve interactions between natural biogenic emissions and anthropogenic emissions such as effects of sulfur and NOx emissions on SOA. We will present examples of integrated model-measurement studies that relate the observed evolution of organic aerosol mass and number with knowledge of particle properties such as volatility and viscosity. We will also highlight the importance of continuing efforts to rank the most influential SOA processes that affect climate forcing, but are often missing in climate models. Ultimately, gas- and particle-phase chemistry processes that capture the dynamic evolution of number and mass concentrations of SOA particles need to be accurately and efficiently represented in regional and global atmospheric chemistry-climate models.

The effect of aerosol-derived changes in the warm phase on the properties of deep convective clouds

NASA Astrophysics Data System (ADS)

Chen, Qian; Koren, Ilan; Altaratz, Orit; Heiblum, Reuven; Dagan, Guy

2017-04-01

The aerosol impact on deep convective clouds starts in an increased number of cloud droplets in higher aerosol loading environment. This change drives many others, like enhanced condensational growth, delay in collision-coalescence and others. Since the warm processes serve as the initial and boundary conditions for the mixed and cold-phase processes in deep clouds, it is highly important to understand the aerosol effect on them. The weather research and forecasting model (WRF) with spectral bin microphysics was used to study a deep convective system over the Marshall Islands, during the Kwajalein Experiment (KWAJEX). Three simulations were conducted with aerosol concentrations of 100, 500 and 2000 cm-3, to reflect clean, semipolluted, and polluted conditions. The results of the clean run agreed well with the radar profiles and rain rate observations. The more polluted simulations resulted in larger total cloud mass, larger upper level cloud fraction and rain rates. There was an increased mass both below and above the zero temperature level. It indicates of more efficient growth processes both below and above the zero level. In addition the polluted runs showed an increased upward transport (across the zero level) of liquid water due to both stronger updrafts and larger droplet mobility. In this work we discuss the transport of cloud mass crossing the zero temperature level (in both directions) in order to gain a process level understanding of how aerosol effects on the warm processes affect the macro- and micro-properties of deep convective clouds.

The climate impacts of absorbing aerosols on and within the Arctic

NASA Astrophysics Data System (ADS)

Rasch, P.; Wang, H.; Ma, P.; Fast, J. D.; Wang, M.; Easter, R. C.; Liu, X.; Qian, Y.; Flanner, M. G.; Ghan, S.; Singh, B.

2011-12-01

Absorbing aerosols are receiving increasing attention as forcing agents in the climate system. By scattering and absorbing light they can reduce planetary albedo, particularly over bright surfaces (clouds, snow and ice). They also act as cloud condensation and/or ice nuclei, influencing the brightness, lifetime and precipitation properties of clouds. Atmospheric stability and primary circulation features respond to the changing vertical and horizontal patterns of heating, cooling, and surface fluxes produced by the aerosols, clouds and surface properties. These changes in meteorology have further impacts on aerosols and clouds producing a complex interplay between transport, forcings, and feedbacks involving absorbing aerosols and climate. The complexity of the processes and the interactions between them make it very challenging to represent aerosols realistically in large scale (global and regional) climate models. Simulations of important features of aerosols still contain easily identifiable biases. I will describe our efforts to identify the processes responsible for some of those biases and the deficiencies in model formulations that impede progress in treating aerosols and understanding their role in polar climate. I plan to summarize some studies performed with the NCAR CESM (global) and WRF-Chem (regional) Community models that examine the simulation sensitivity to treatments of physics, chemistry, and meteorology. Some of these simulations were allowed to evolve freely; others were strongly constrained to agree with observed meteorological fields. We have also altered the formulation of a number of the processes in the model to improve fidelity in the aerosol distributions. The parameterizations used in our global model have also been transferred to the regional model, allowing comparisons to be made between the simpler formulations used in the global model with more elaborate and costly formulations available in the regional model. The regional model can be run at higher resolution in order to explore the resolution dependence of the parameterizations and make comparisons to field experiments more straightforward. Aerosols sources have also been tagged by sector and geographic region to help in attribution and interpretation. The many variations mentioned here help in understanding how aerosols reach the arctic and how they produce changes in radiative forcing and Arctic climate. I will provide a brief overview of these studies, with more detail available in presentations submitted to this session and elsewhere.

Consistency of Global Modis Aerosol Optical Depths over Ocean on Terra and Aqua Ceres SSF Datasets

NASA Technical Reports Server (NTRS)

Ignatov, Alexander; Minnis, Patrick; Miller, Walter F.; Wielicki, Bruce A.; Remer, Lorraine

2006-01-01

Aerosol retrievals over ocean from the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard Terra and Aqua platforms are available from the Clouds and the Earth's Radiant Energy System (CERES) Single Scanner Footprint (SSF) datasets generated at NASA Langley Research Center (LaRC). Two aerosol products are reported side-by-side. The primary M product is generated by sub-setting and remapping the multi-spectral (0.47-2.1 micrometer) MODIS produced oceanic aerosol (MOD04/MYD04 for Terra/Aqua) onto CERES footprints. M*D04 processing uses cloud screening and aerosol algorithms developed by the MODIS science team. The secondary AVHRR-like A product is generated in only two MODIS bands 1 and 6 (on Aqua, bands 1 and 7). The A processing uses the CERES cloud screening algorithm, and NOAA/NESDIS glint identification, and single-channel aerosol retrieval algorithms. The M and A products have been documented elsewhere and preliminarily compared using 2 weeks of global Terra CERES SSF Edition 1A data in which the M product was based on MOD04 collection 3. In this study, the comparisons between the M and A aerosol optical depths (AOD) in MODIS band 1 (0.64 micrometers), tau(sub 1M) and tau(sub 1A) are re-examined using 9 days of global CERES SSF Terra Edition 2A and Aqua Edition 1B data from 13 - 21 October 2002, and extended to include cross-platform comparisons. The M and A products on the new CERES SSF release are generated using the same aerosol algorithms as before, but with different preprocessing and sampling procedures, lending themselves to a simple sensitivity check to non-aerosol factors. Both tau(sub 1M) and tau(sub 1A) generally compare well across platforms. However, the M product shows some differences, which increase with ambient cloud amount and towards the solar side of the orbit. Three types of comparisons conducted in this study - cross-platform, cross-product, and cross-release confirm the previously made observation that the major area for improvement in the current aerosol processing lies in a more formalized and standardized sampling (and most importantly, cloud screening) whereas optimization of the aerosol algorithm is deemed to be an important yet less critical element.

Impacts of aerosol-monsoon interaction on rainfall and circulation over Northern India and the Himalaya Foothills

NASA Astrophysics Data System (ADS)

Lau, William K. M.; Kim, Kyu-Myong; Shi, Jainn-Jong; Matsui, T.; Chin, M.; Tan, Qian; Peters-Lidard, C.; Tao, W. K.

2017-09-01

The boreal summer of 2008 was unusual for the Indian monsoon, featuring exceptional heavy loading of dust aerosols over the Arabian Sea and northern-central India, near normal all-India rainfall, but excessive heavy rain, causing disastrous flooding in the Northern Indian Himalaya Foothills (NIHF) regions, accompanied by persistent drought conditions in central and southern India. Using the NASA Unified-physics Weather Research Forecast (NUWRF) model with fully interactive aerosol physics and dynamics, we carried out three sets of 7-day ensemble model forecast experiments: (1) control with no aerosol, (2) aerosol radiative effect only and (3) aerosol radiative and aerosol-cloud-microphysics effects, to study the impacts of aerosol-monsoon interactions on monsoon variability over the NIHF during the summer of 2008. Results show that aerosol-radiation interaction (ARI), i.e., dust aerosol transport, and dynamical feedback processes induced by aerosol-radiative heating, plays a key role in altering the large-scale monsoon circulation system, reflected by an increased north-south tropospheric temperature gradient, a northward shift of heavy monsoon rainfall, advancing the monsoon onset by 1-5 days over the HF, consistent with the EHP hypothesis (Lau et al. in Clim Dyn 26(7-8):855-864, 2006). Additionally, we found that dust aerosols, via the semi-direct effect, increase atmospheric stability, and cause the dissipation of a developing monsoon onset cyclone over northeastern India/northern Bay of Bengal. Eventually, in a matter of several days, ARI transforms the developing monsoon cyclone into meso-scale convective cells along the HF slopes. Aerosol-Cloud-microphysics Interaction (ACI) further enhances the ARI effect in invigorating the deep convection cells and speeding up the transformation processes. Results indicate that even in short-term (up to weekly) numerical forecasting of monsoon circulation and rainfall, effects of aerosol-monsoon interaction can be substantial and cannot be ignored.

Satellite Remote Sensing and Mesoscale Modeling of Biomass Burning Aerosols over the Southeast Asian Maritime Continent: Climatic Implications of Smokes on Regional Energy Balance, Cloud Formations and Precipitations

NASA Astrophysics Data System (ADS)

Feng, N.

2015-12-01

The influences of anthropogenic aerosols have been suggested as an important reason for climate changes over Southeast Asia (SE Asia, 10°S~20°N and 90°E~135°E). Accurate observations and modelling of aerosols effects on the weather and climate patterns is crucial for a better understanding and mitigation of anthropogenic climate change. This study uses NASA satellite observations along with online-coupled Weather Research and Forecasting model with Chemistry (WRF-Chem) to evaluate aerosols impacts on climate over SE Asia. We assess the direct and semi-direct radiative effects of smoke particles over this region during September, 2009 when a significant El Niño event caused the highest biomass burning activity during the last 15 years. Quantification efforts are made to assess how changes of radiative and non radiative parameters (sensible and latent heat) due to smoke aerosols would affect regional climate process such as precipitations, clouds and planetary boundary layer process. Comparison of model simulations for the current land cover conditions against surface meteorological observations and satellite observations of precipitations and cloudiness show satisfactory performance of the model over our study area. In order to quantitatively validate the model results, several experiments will be performed to test the aerosols radiative feedback under different radiation schemes and with/without considering aerosol effects explicitly in the model. Relevant ground-based data (e.g. AERONET), along with aerosol vertical profile data from CALIPSO, will also be applied.

Aerosol Indirect Effect on Warm Clouds over Eastern China Using Combined CALIOP and MODIS Observations

NASA Astrophysics Data System (ADS)

Guo, Jianping; Wang, Fu; Huang, Jingfeng; Li, Xiaowen

2015-04-01

Aerosol, one of key components of the climate system, is highly variable, both temporally and spatially. It often exerts great influences on the cloud-precipitation chain processes by serving as CCN/IN, altering cloud microphysics and its life cycle. Yet, the aerosol indirect effect on clouds remains largely unknown, because the initial changes in clouds due to aerosols may be enhanced or dampened by such feedback processes as modified cloud dynamics, or evaporation of the smaller droplets due to the competition for water vapor. In this study, we attempted to quantify the aerosol effects on warm cloud over eastern China, based on near-simultaneous retrievals from MODIS/AQUA, CALIOP/CALIPSO and CPR/CLOUDSAT during the period 2006 to 2010. The seasonality of aerosol from ground-based PM10 is quite different from that estimated from MODIS AOD. This result is corroborated by lower level profile of aerosol occurrence frequency from CALIOP, indicating the significant role CALIOP could play in aerosol-cloud interaction. The combined use of CALIOP and CPR facilitate the process to exactly determine the (vertical) position of warm cloud relative to aerosol, out of six scenarios in terms of aerosol-cloud mixing status in terms of aerosol-cloud mixing status, which shows as follows: AO (Aerosol only), CO (Cloud only), SASC (Single aerosol-single cloud), SADC (single aerosol-double cloud), DASC (double aerosol-single cloud), and others. Results shows that about 54% of all the cases belong to mixed status, among all the collocated aerosol-cloud cases. Under mixed condition, a boomerang shape is observed, i.e., reduced cloud droplet radius (CDR) is associated with increasing aerosol at moderate aerosol pollution (AOD<0.4), becoming saturated at AOD of 0.5, followed by an increase in CDR with aerosol. In contrast, there is no such boomerang shape found for (aerosol-cloud) separated cases. We categorize dataset into warm-season and cold-season subsets to figure out how the boomerang shape varies with season. For moderate aerosol loading (AOD<0.4), the effect on the droplet size for the "Mixed" cases is greater during cold season (denoted by a large slope), as compared with that during warm season. It is likely associated with an increase in the emission of light absorbing aerosol like smoke (black carbon), mainly caused by coal-fired heating during the cold season in China. As expected, the sensitivity of CDR to AOD is much weaker for "Separated" cases, irrespective of warm or cold seasons, indicating no real aerosol indirect effect occurring in this case. In contrast, for heavy aerosol loading (AOD>0.4), an increasing CDR with AOD can be seen in "Mixed" scenario during the warm season. Conversely, a closer look at the responses of CDR during the cold season shows that CDR decreases with AOD, although the strength is not much large. Therefore, we argue that cloud droplet size decreases with aerosol loading during cold season, irrespective of moderate or heavy atmospheric pollution. Finally, we discuss the possible factors that may influence the aerosol indirect effects on warm clouds investigated here. For instance, aerosol-cloud interaction conundrum might be affected by aerosol humidification, which is the case for MODIS AOD during warm seasons. But this issue can be partly overcome by categorizing dataset into warm-season and cold-season subsets, representing different ambient humidity condition in the atmosphere. The different boomerang shapes observed during various seasons, particularly after transition zone due to droplet saturation effect, have great implications for climate forcing by aerosol in eastern China.

13C and 15N fractionation of CH4/N2 mixtures during photochemical aerosol formation: Relevance to Titan

NASA Astrophysics Data System (ADS)

Sebree, Joshua A.; Stern, Jennifer C.; Mandt, Kathleen E.; Domagal-Goldman, Shawn D.; Trainer, Melissa G.

2016-05-01

The ratios of the stable isotopes that comprise each chemical species in Titan's atmosphere provide critical information towards understanding the processes taking place within its modern and ancient atmosphere. Several stable isotope pairs, including 12C/13C and 14N/15N, have been measured in situ or probed spectroscopically by Cassini-borne instruments, space telescopes, or through ground-based observations. Current attempts to model the observed isotope ratios incorporate fractionation resulting from atmospheric diffusion, hydrodynamic escape, and primary photochemical processes. However, the effect of a potentially critical pathway for isotopic fractionation - organic aerosol formation and subsequent deposition onto the surface of Titan - has not been considered due to insufficient data regarding fractionation during aerosol formation. To better understand the nature of this process, we have conducted a laboratory study to measure the isotopic fractionation associated with the formation of Titan aerosol analogs, commonly referred to as 'tholins', via far-UV irradiation of several methane (CH4) and dinitrogen (N2) mixtures. Analysis of the δ13C and δ15N isotopic signatures of the photochemical aerosol products using an isotope ratio mass spectrometer (IRMS) show that fractionation direction and magnitude are dependent on the initial bulk composition of the gas mixture. In general, the aerosols showed enrichment in 13C and 14N, and the observed fractionation trends can provide insight into the chemical mechanisms controlling photochemical aerosol formation.

Aerosol and CCN over the Southern Ocean: Sources, Sinks and Processes

NASA Astrophysics Data System (ADS)

Clarke, A. D.; Freitag, S.; Howell, S. G.; Snider, J. R.; Kazil, J.; Feingold, G.; McNaughton, C. S.; Brekhovskikh, V.; Kapustin, V.; Campos, T. L.; Shank, L.

2013-12-01

Aerosol able to activate as cloud condensation nuclei (CCN) in marine stratus play an important role in cloud properties and processes. The 2008 VOCALS experiment (http://www.eol.ucar.edu/projects/vocals/) explored the aerosol cloud system over the South East Pacific (SEP). There, marine boundary layer (MBL) air from the Southern Ocean is directed north parallel to the South American coast and exposed to continental emissions. During this transport the initial clean MBL aerosol is modified in response to production, processing, entrainment, mixing, and removal. Here we discuss how the aerosol, the CCN and the clouds over the SEP are coupled by these processes. VOCALS data along 20S indicated cleanest air offshore and west of about 78W. However, some of the cleanest air (lowest CO concentrations) over the SEP were present in pockets of open cells (POC's). This suggests POC's are favored in places where remnants of Southern Ocean MBL air experienced the least mixing with higher CO sources during transport, either coastal or via entrainment of free troposphere air. Entrainment from the free troposphere (FT) was found to be an important source of marine boundary layer (MBL) aerosol in both near-shore and off-shore regions while direct advection of continental aerosol tended to influence aerosol and CCN closer to the coast. Entrainment from the FT included diverse sources from South America as well as long range transport from the western Pacific. Entrainment of FT aerosol can resupply the MBL with CCN and this process appears greatly enhanced when patchy 'rivers' of pollution lie directly above the inversion. This process was evident both offshore and near the coast. Production of CCN from sea spray aerosol (SSA) were found to increase with wind speed but atmospheric concentrations did not generally increase in the higher wind offshore regions because these regions had greater drizzle removal that compensated for increased production. Generally SSA larger than 60 nm were effective as marine cloud CCN but were only about 20% of the total. Elevated organic aerosol was usually associated with biomass burning sources and a natural marine organic aerosol source was weak. Although nucleation in clean scavenged air layers near the top of the boundary layer were observed under certain conditions, the resulting small aerosol sizes did not appear to provide an effective source of CCN sizes compared to other processes.

Uncertainty associated with convective wet removal of entrained aerosols in a global climate model

NASA Astrophysics Data System (ADS)

Croft, B.; Pierce, J. R.; Martin, R. V.; Hoose, C.; Lohmann, U.

2012-11-01

The uncertainties associated with the wet removal of aerosols entrained above convective cloud bases are investigated in a global aerosol-climate model (ECHAM5-HAM) under a set of limiting assumptions for the wet removal of the entrained aerosols. The limiting assumptions for the wet removal of entrained aerosols are negligible scavenging and vigorous scavenging (either through activation, with size-dependent impaction scavenging, or with the prescribed fractions of the standard model). To facilitate this process-based study, an explicit representation of cloud-droplet-borne and ice-crystal-borne aerosol mass and number, for the purpose of wet removal, is introduced into the ECHAM5-HAM model. This replaces and is compared with the prescribed cloud-droplet-borne and ice-crystal-borne aerosol fraction scavenging scheme of the standard model. A 20% to 35% uncertainty in simulated global, annual mean aerosol mass burdens and optical depth (AOD) is attributed to different assumptions for the wet removal of aerosols entrained above convective cloud bases. Assumptions about the removal of aerosols entrained above convective cloud bases control modeled upper tropospheric aerosol concentrations by as much as one order of magnitude. Simulated aerosols entrained above convective cloud bases contribute 20% to 50% of modeled global, annual mean aerosol mass convective wet deposition (about 5% to 10% of the total dry and wet deposition), depending on the aerosol species, when including wet scavenging of those entrained aerosols (either by activation, size-dependent impaction, or with the prescribed fraction scheme). Among the simulations, the prescribed fraction and size-dependent impaction schemes yield the largest global, annual mean aerosol mass convective wet deposition (by about two-fold). However, the prescribed fraction scheme has more vigorous convective mixed-phase wet removal (by two to five-fold relative to the size-dependent impaction scheme) since nearly all entrained accumulation and coarse mode aerosols are assumed to be cloud-droplet borne or ice-crystal borne, and evaporation due to the Bergeron-Findeisen process is neglected. The simulated convective wet scavenging of entrained accumulation and coarse mode aerosols has feedbacks on new particle formation and the number of Aitken mode aerosols, which control stratiform and convective cloud droplet number concentrations and yield precipitation changes in the ECHAM5-HAM model. However, the geographic distribution of aerosol annual mean convective wet deposition change in the model is driven by changes to the assumptions regarding the scavenging of aerosols entrained above cloud bases rather than by precipitation changes, except for sea salt deposition in the tropics. Uncertainty in the seasonal, regional cycles of AOD due to assumptions about entrained aerosol wet scavenging is similar in magnitude to the estimated error in the AOD retrievals. The uncertainty in aerosol concentrations, burdens, and AOD attributed to different assumptions for the wet scavenging of aerosols entrained above convective cloud bases in a global model motivates the ongoing need to better understand and model the activation and impaction processes that aerosols undergo after entrainment into convective updrafts.

Long-range Transport of Aerosol at a Mountain Site in the Western Mediterranean Basin

NASA Astrophysics Data System (ADS)

Roberts, Greg; Corrigan, Craig; Ritchie, John; Pont, Véronique; Claeys, Marine; Sciare, Jean; Dulac, François

2016-04-01

The Mediterranean Region has been identified as sensitive to changes in the hydrological cycle, which could affect the water resources for millions of people by the turn of the century. However, prior to recent observations, most climate models have not accounted for the impacts of aerosol in this region. Past airborne studies have shown that aerosol sources from Europe and Africa are often transported throughout the lower troposphere; yet, because of their complex vertical distribution, it is a challenge to capture the variability and quantify the contribution of these sources to the radiative budget and precipitation processes. The PAEROS ChArMEx Mountain Experiment (PACMEx) complemented the regional activities by collecting aerosol data from atop a mountain on the island of Corsica, France in order to assess boundary layer / free troposphere atmospheric processes. In June/July 2013, PACMEx instruments were deployed at 2000 m.asl near the center of Corsica, France to complement ground-based aerosol observations at 550 m.asl on the northern peninsula, as well as airborne measurements. Comparisons between the peninsula site and the mountain site show similar general trends in aerosol properties; yet, differences in aerosol properties reveal the myriad transport mechanisms over the Mediterranean Basin. Using aerosol physicochemical data coupled with back trajectory analysis, different sources have been identified including Saharan dust transport, residual dust mixed with sea salt, anthropogenic emissions from Western Europe, and a period of biomass burning from Eastern Europe. Each period exhibits distinct signatures in the aerosol related to transport processes above and below the boundary layer. In addition, the total aerosol concentrations at the mountain site revealed a strong diurnal cycling the between the atmospheric boundary layer and the free troposphere, which is typical of mountain-top observations. PACMEx was funded by the National Science Foundation (NSF) as a cooperative collaboration with French research agencies (INSU-MISTRALS, ANR-ADRIMED, and Météo France).

Sources and Transport of Aerosol above the Boundary Layer over the Mediterranean Basin

NASA Astrophysics Data System (ADS)

Roberts, Greg; Corrigan, Craig; Ritchie, John; Pont, Veronique; Claeys, Marine; Sciare, Jean; Mallet, Marc; Dulac, François; Mihalopoulos, Nikos

2015-04-01

The Mediterranean Region has been identified as sensitive to changes in the hydrological cycle, which could affect the water resources for millions of people by the turn of the century. However, prior to recent observations, most climate models have not accounted for the impacts of aerosol in this region. Past airborne studies have shown that aerosol sources from Europe and Africa are often transported throughout the lower troposphere; yet, because of their complex vertical distribution, it is a challenge to capture the variability and quantify the contribution of these sources to the radiative budget and precipitation processes. The PAEROS ChArMEx Mountain Experiment (PACMEx) complemented the regional activities by collecting aerosol data from atop a mountain on the island of Corsica, France in order to assess boundary layer / free troposphere atmospheric processes. In June/July 2013, PACMEx instruments were deployed at 2000 m.asl near the center of Corsica, France to complement ground-based aerosol observations at 550 m.asl on the northern peninsula, as well as airborne measurements. Comparisons between the peninsula site and the mountain site show similar general trends in aerosol properties; yet, differences in aerosol properties reveal the myriad transport mechanisms over the Mediterranean Basin. Using aerosol physicochemical data coupled with back trajectory analysis, different sources have been identified including Saharan dust transport, residual dust mixed with sea salt, anthropogenic emissions from Western Europe, and a period of biomass burning from Eastern Europe. Each period exhibits distinct signatures in the aerosol related to transport processes above and below the boundary layer. In addition, the total aerosol concentrations at the mountain site revealed a strong diurnal cycling the between the atmospheric boundary layer and the free troposphere, which is typical of mountain-top observations. PACMEx was funded by the National Science Foundation (NSF) as a cooperative collaboration with French research agencies (INSU-MISTRALS, ANR-ADRIMED, and Météo France).

The effect of smoke, dust, and pollution aerosol on shallow cloud development over the Atlantic Ocean

PubMed Central

Kaufman, Yoram J.; Koren, Ilan; Remer, Lorraine A.; Rosenfeld, Daniel; Rudich, Yinon

2005-01-01

Clouds developing in a polluted environment tend to have more numerous but smaller droplets. This property may lead to suppression of precipitation and longer cloud lifetime. Absorption of incoming solar radiation by aerosols, however, can reduce the cloud cover. The net aerosol effect on clouds is currently the largest uncertainty in evaluating climate forcing. Using large statistics of 1-km resolution MODIS (Moderate Resolution Imaging Spectroradiometer) satellite data, we study the aerosol effect on shallow water clouds, separately in four regions of the Atlantic Ocean, for June through August 2002: marine aerosol (30°S–20°S), smoke (20°S–5°N), mineral dust (5°N–25°N), and pollution aerosols (30°N– 60°N). All four aerosol types affect the cloud droplet size. We also find that the coverage of shallow clouds increases in all of the cases by 0.2–0.4 from clean to polluted, smoky, or dusty conditions. Covariability analysis with meteorological parameters associates most of this change to aerosol, for each of the four regions and 3 months studied. In our opinion, there is low probability that the net aerosol effect can be explained by coincidental, unresolved, changes in meteorological conditions that also accumulate aerosol, or errors in the data, although further in situ measurements and model developments are needed to fully understand the processes. The radiative effect at the top of the atmosphere incurred by the aerosol effect on the shallow clouds and solar radiation is –11 ± 3 W/m2 for the 3 months studied; 2/3 of it is due to the aerosol-induced cloud changes, and 1/3 is due to aerosol direct radiative effect. PMID:16076949

Impact of fog processing on water soluble organic aerosols.

NASA Astrophysics Data System (ADS)

Tripathi, S. N.; Chakraborty, A.; Gupta, T.

2017-12-01

Fog is a natural meteorological phenomenon that occurs all around the world, and contains a substantial quantity of liquid water. Fog is generally seen as a natural cleansing agent but can also form secondary organic aerosols (SOA) via aqueous processing of ambient organics. Few field studies have reported elevated O/C ratio and SOA mass during or after fog events. However, mechanism behind aqueous SOA formation and its contribution to total organic aerosols (OA) still remains unclear. In this study we have tried to explore the impact of fog/aqueous processing on the characteristics of water soluble organic aerosols (WSOC), which to our knowledge has not been studied before. To assess this, both online (using HR-ToF-AMS) and offline (using a medium volume PM2.5 sampler and quartz filter) aerosol sampling were carried out at Kanpur, India from 15 December 2014 - 10 February 2015. Further, offline analysis of the aqueous extracts of the collected filters were carried out by AMS to characterize the water soluble OA (WSOA). Several (17) fog events occurred during the campaign and high concentrations of OA (151 ± 68 µg/m3) and WSOA (47 ± 19 µg/m3) were observed. WSOA/OA ratios were similar during fog (0.36 ± 0.14) and nofog (0.34 ± 0.15) periods. WSOA concentrations were also similar (slightly higher) during foggy (49 ± 18 µg/m3) and non-foggy periods (46 ± 20 µg/m3), in spite of fog scavenging. However, WSOA was more oxidized during foggy period (average O/C = 0.81) than non foggy periods (average O/C = 0.70). Like WSOA, OA was also more oxidized during foggy periods (average O/C = 0.64) than non foggy periods (average O/C = 0.53). During fog, WSOA to WIOA (water insoluble OA) ratios were higher (0.65 ± 0.16) compared to non foggy periods (0.56 ± 0.15). These observations clearly showed that WSOA become more dominant and processed during fog events, possibly due to the presence of fog droplets. This study highlights that fog processing of soluble organics can affect the overall chemical characteristics of the entire aerosol population.

Multiple stable oxygen isotopic studies of atmospheric sulfate: A new quantitative way to understand sulfate formation processes in the atmosphere

NASA Astrophysics Data System (ADS)

Lee, Charles Chi-Woo

2000-11-01

Sulfate is an important trace species in the Earth's atmosphere because of its roles in numerous atmospheric processes. In addition to its inherent light-scattering properties, sulfate can serve as cloud condensation nucleus (CCN), affecting cloud formation as well as microphysical properties of clouds. Consequently, atmospheric sulfate species influence the global radiative energy balance. Sulfate is known to increase acidity of rainwater with negative consequences in both natural and urban environments. In addition, aerosol sulfate (<=2.5 μm) is respirable and poses a threat to human health as a potential carrier of toxic pollutants through the respiratory tract. Despite intense investigative effort, uncertainty regarding the relative significance of gas and aqueous phase oxidation pathways still remains. Acquisition of such information is important because the lifetime and transport of S(IV) species and sulfate aerosols are influenced by the oxidative pathways. In addition, sulfate formation processes affect the aerosol size distribution, which ultimately influences radiative properties of atmospheric aerosols. Therefore, the budgetary information of the sulfur cycle, as well as the radiative effects of sulfate on global climate variation, can be attained from better quantitative understanding of in situ sulfate formation processes in the atmosphere. Multiple stable oxygen isotopic studies of atmospheric sulfate are presented as a new tool to better comprehend the atmospheric sulfate formation processes. Coupled with isotopic studies, 35S radioactivity measurements have been utilized to assess contribution of sulfate from high altitude air masses. Atmospheric sulfate (aerosols and rainwater) samples have been collected from diverse environments. Laboratory experiments of gas and aqueous phase S(IV) oxidation by various oxidants, as well as biomass burning experiments, have also been conducted. The main isotopic results from these studies are as follows: (1)Atmospheric (aerosol and rainwater) sulfate has a mass independent oxygen isotopic composition; (2)Aqueous phase S(IV) oxidation by atmospheric ozone and hydrogen peroxide are the source of the mass independent anomaly in atmospheric sulfate; (3)The mass independent oxygen isotopic anomaly appears to enhance with increasing altitude, suggesting a stratospheric contribution; (4)Primary sulfate from biomass burning has a mass dependent oxygen isotopic composition.

Photoacoustic absorption spectroscopy of single optically trapped aerosol droplets

NASA Astrophysics Data System (ADS)

Covert, Paul A.; Cremer, Johannes W.; Signorell, Ruth

2017-08-01

Photoacoustics have been widely used for the study of aerosol optical properties. To date, these studies have been performed on particle ensembles, with minimal ability to control for particle size. Here, we present our singleparticle photoacoustic spectrometer. The sensitivity and stability of the instrument is discussed, along with results from two experiments that illustrate the unique capabilities of this instrument. In the first experiment, we present a measurement of the particle size-dependence of the photoacoustic response. Our results confirm previous models of aerosol photoacoustics that had yet to be experimentally tested. The second set of results reveals a size-dependence of photochemical processes within aerosols that results from the nanofocusing of light within individual droplets.

Optical extinction of highly porous aerosol following atmospheric freeze drying

NASA Astrophysics Data System (ADS)

Adler, Gabriela; Haspel, Carynelisa; Moise, Tamar; Rudich, Yinon

2014-06-01

Porous glassy particles are a potentially significant but unexplored component of atmospheric aerosol that can form by aerosol processing through the ice phase of high convective clouds. The optical properties of porous glassy aerosols formed from a freeze-dry cycle simulating freezing and sublimation of ice particles were measured using a cavity ring down aerosol spectrometer (CRD-AS) at 532 nm and 355 nm wavelength. The measured extinction efficiency was significantly reduced for porous organic and mixed organic-ammonium sulfate particles as compared to the extinction efficiency of the homogeneous aerosol of the same composition prior to the freeze-drying process. A number of theoretical approaches for modeling the optical extinction of porous aerosols were explored. These include effective medium approximations, extended effective medium approximations, multilayer concentric sphere models, Rayleigh-Debye-Gans theory, and the discrete dipole approximation. Though such approaches are commonly used to describe porous particles in astrophysical and atmospheric contexts, in the current study, these approaches predicted an even lower extinction than the measured one. Rather, the best representation of the measured extinction was obtained with an effective refractive index retrieved from a fit to Mie scattering theory assuming spherical particles with a fixed void content. The single-scattering albedo of the porous glassy aerosols was derived using this effective refractive index and was found to be lower than that of the corresponding homogeneous aerosol, indicating stronger relative absorption at the wavelengths measured. The reduced extinction and increased absorption may be of significance in assessing direct, indirect, and semidirect forcing in regions where porous aerosols are expected to be prevalent.

Aerosol and Cloud Interaction Observed From High Spectral Resolution Lidar Data

NASA Technical Reports Server (NTRS)

Su, Wenying; Schuster, Gregory L.; Loeb, Norman G.; Rogers, Raymond R.; Ferrare, Richard A.; Hostetler, Chris A.; Hair, Johnathan W.; Obland, Michael D.

2008-01-01

Recent studies utilizing satellite retrievals have shown a strong correlation between aerosol optical depth (AOD) and cloud cover. However, these retrievals from passive sensors are subject to many limitations, including cloud adjacency (or 3D) effects, possible cloud contamination, uncertainty in the AOD retrieval. Some of these limitations do not exist in High Spectral Resolution Lidar (HSRL) observations; for instance, HSRL observations are not a ected by cloud adjacency effects, are less prone to cloud contamination, and offer accurate aerosol property measurements (backscatter coefficient, extinction coefficient, lidar ratio, backscatter Angstrom exponent,and aerosol optical depth) at a neospatial resolution (less than 100 m) in the vicinity of clouds. Hence, the HSRL provides an important dataset for studying aerosol and cloud interaction. In this study, we statistically analyze aircraft-based HSRL profiles according to their distance from the nearest cloud, assuring that all profile comparisons are subject to the same large-scale meteorological conditions. Our results indicate that AODs from HSRL are about 17% higher in the proximity of clouds (approximately 100 m) than far away from clouds (4.5 km), which is much smaller than the reported cloud 3D effect on AOD retrievals. The backscatter and extinction coefficients also systematically increase in the vicinity of clouds, which can be explained by aerosol swelling in the high relative humidity (RH) environment and/or aerosol growth through in cloud processing (albeit not conclusively). On the other hand, we do not observe a systematic trend in lidar ratio; we hypothesize that this is caused by the opposite effects of aerosol swelling and aerosol in-cloud processing on the lidar ratio. Finally, the observed backscatter Angstrom exponent (BAE) does not show a consistent trend because of the complicated relationship between BAE and RH. We demonstrate that BAE should not be used as a surrogate for Angstrom exponent, especially at high RH.

Puerto Rico - 2002 : field studies to resolve aerosol processes.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gaffney, J. S.; Marley, N. A.; Ravelo, R.

1999-10-05

A number of questions remain concerning homogeneous aerosol formation by natural organics interacting with anthropogenic pollutants. For example, chlorine has been proposed as a potential oxidant in the troposphere because of its very high reactivity with a wide range of organics (Finlayson-Pitts, 1993). Indeed, sea salt aerosol in the presence of ozone has been shown to produce chlorine atoms in heterogeneous photochemical reactions under laboratory conditions. Whether chlorine can initiate oxidation of natural organics such as monoterpene hydrocarbons and can generate homogeneous nucleation or condensable material that contributes to aerosol loadings needs to be assessed. The nighttime reactions of ozonemore » and nitrate radical can also result in monoterpene reactions that contribute to aerosol mass. We are currently planning field studies in Puerto Rico to assess these aerosol issues and other atmospheric chemistry questions. Puerto Rico has a number of key features that make it very attractive for a field study of this sort. The principal feature is the island's very regular meteorology and its position in the Caribbean Sea relative to the easterly trade winds. This meteorology and the island's rectangular shape (100 x 35 miles) make it highly suitable for simplification of boundary layer conditions. In addition, the long stretch between Puerto Rico and the nearest pollution sources in Africa and southern Europe make the incoming background air relatively clean and constant. Furthermore, Puerto Rico has approximately 3.5 million people with a very well defined source region and a central area of rain forest vegetation. These features make Puerto Rico an ideal locale for assessing aerosol processes. The following sections describe specific areas of atmospheric chemistry that can be explored during the proposed field study.« less

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

NASA Astrophysics Data System (ADS)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

A Systematic Evaluation of the Extent of Photochemical Processing in Different Types of Secondary Organic Aerosols in the Aqueous Phase

NASA Astrophysics Data System (ADS)

Romonosky, D.; Lee, H.; Epstein, S. A.; Nizkorodov, S.; Laskin, J.; Laskin, A.

2013-12-01

A significant fraction of atmospheric organic compounds are predominantly found in condensed phases, such as organic phase in aerosol particles or aqueous phase in cloud droplets. The oxidation of VOCs followed by the condensation of products into particles was thought to be the main mechanism of organic aerosol (OA) formation. However, in the last several years, scientists have realized that a large fraction, if not the majority of organic particles, is produced through cloud and fog photochemical processes. Many of these organic compounds are photolabile, and can degrade through direct photolysis or indirect photooxidation processes on time scales that are comparable to the typical lifetimes of droplets (hours) and particles (days). We previously reported that compounds in secondary organic aerosol (SOA) from ozonolysis of d-limonene efficiently photodegrade in both organic (Walser et al., 2007) and aqueous phases (Bateman et al., 2011). Significant photolysis was also observed in an aqueous extract of SOA from high-NOx photooxidation of isoprene (Nguyen et al., 2012). More recent experiments studying the response to irradiation of complex aqueous mixtures (as opposed to solutions of isolated compounds) found surprising resilience to photodegradation in aqueous extracts of SOA prepared by photooxidation of alpha-pinene (Romonosky et al., unpublished). We present a systematic investigation of the extent of photochemical processing in different types of SOA from various biogenic and anthropogenic precursors. Chamber- or flowtube-generated SOA is collected on an inert substrate, extracted in a methanol/water solution (70:30), photolyzed in the aqueous solution, and the extent of change in the molecular level composition of the material is assessed with high-resolution mass spectrometry (HR-MS). The outcome of this study will be improved understanding of the role of condensed-phase photochemistry in chemical aging of aerosol particles and cloud droplets. Bateman et al. Photolytic processing of secondary organic aerosols dissolved in cloud droplets. Phys. Chem. Chem. Phys. 2011, 13, 12199. Nguyen et al. Direct aqueous photochemistry of isoprene high-NOx secondary organic aerosol. Phys. Chem. Chem. Phys. 2012, 14, 9702. Walser et al. Photochemical aging of secondary organic aerosol particles generated from the oxidation of d-limonene. J. Phys. Chem. A 2007, 111, 1907.

Overview of the aerosol measurements in the UTLS during the POSIDON campaign

NASA Astrophysics Data System (ADS)

Gao, R. S.; Liu, S.; Thornberry, T. D.; Rollins, A. W.; Yu, P.; Woods, S.; Bui, T. V.

2017-12-01

The tropical tropopause layer (TTL) is the main gateway for transport of aerosols from the troposphere to the stratosphere. Studies of aerosol properties in the TTL, however, are very limited. During the NASA Pacific Oxidants, Sulfur, Ice, Dehydration, and cONvection (POSIDON) Experiment in Guam in October 2016, we measured aerosol size distributions onboard the NASA WB-57F high altitude research aircraft up to 19 km. Multiple aerosol vertical profiles showed a robust enhancement of aerosols as a function of altitude between 15 and 19 km, with the aerosol number and mass concentrations of 10 cm-3 and 0.1 µg m-3, respectively, for particles in the size range of 140-3000 nm at 17 km altitude. Simulation using a global sectional aerosol model coupled with the Community Earth System Model generally agreed with aerosol observations, suggesting that the aerosol enhancement was likely due to in-situ particle formation and growth. Concurrent SO2 measurement showed that conversion of SO2 to sulfuric acid alone cannot explain the enhanced aerosol layer at TTL, indicating that other precursors or formation pathways exist for efficient aerosol formation. Using the measured mass concentration and an average vertical air velocity, the aerosol mass flux at the tropopause has been estimated. In addition, we investigated the potential aerosol removal processes and found no evidence for aerosol scavenging by ice.

Secondary organic aerosol formation through cloud processing of aromatic VOCs

NASA Astrophysics Data System (ADS)

Herckes, P.; Hutchings, J. W.; Ervens, B.

2010-12-01

Field observations have shown substantial concentrations (20-5,500 ng L-1) of aromatic volatile organic compounds (VOC) in cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric laboratory conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction rates decreased with increasing organic carbon content. Kinetic data derived from these experiments were used as input to a multiphase box model in order to evaluate the secondary organic aerosol (SOA) mass formation potential of cloud processing of BTEX. Model results will be presented that quantify the SOA amounts from these aqueous phase pathways. The efficiency of this multiphase SOA source will be compared to SOA yields from the same aromatics as treated in traditional SOA models that are restricted to gas phase oxidation and subsequent condensation on particles.

Influence of atmospheric processes on the solubility and composition of iron in Saharan dust

DOE PAGES

Longo, Amelia F.; Feng, Yan; Lai, Barry; ...

2016-06-10

Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation statemore » became more reduced, and aerosol acidity increased. As a result, atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.« less

Influence of Atmospheric Processes on the Solubility and Composition of Iron in Saharan Dust.

PubMed

Longo, Amelia F; Feng, Yan; Lai, Barry; Landing, William M; Shelley, Rachel U; Nenes, Athanasios; Mihalopoulos, Nikolaos; Violaki, Kalliopi; Ingall, Ellery D

2016-07-05

Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation state became more reduced, and aerosol acidity increased. Atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.

Aerosol Synthesis of N and N-S Doped and Crumpled Graphene Nanostructures.

PubMed

Carraro, Francesco; Cattelan, Mattia; Favaro, Marco; Calvillo, Laura

2018-06-06

Chemically modified graphene⁻based materials (CMG) are currently attracting a vast interest in their application in different fields. In particular, heteroatom-doped graphenes have revealed great potentialities in the field of electrocatalysis as substitutes of fuel cell noble metal⁻based catalysts. In this work, we investigate an innovative process for doping graphene nanostructures. We optimize a novel synthetic route based on aerosol preparation, which allows the simultaneous doping, crumpling, and reduction of graphene oxide (GO). Starting from aqueous solutions containing GO and the dopant precursors, we synthesize N- and N,S-dual-doped 3D graphene nanostructures (N-cGO and N,S-cGO). In the aerosol process, every aerosol droplet can be considered as a microreactor where dopant precursors undergo thermal decomposition and react with the GO flakes. Simultaneously, thanks to the relatively high temperature, GO undergoes crumpling and partial reduction. Using a combination of spectroscopic and microscopic characterization techniques, we investigate the morphology of the obtained materials and the chemical nature of the dopants within the crumpled graphene sheets. This study highlights the versatility of the aerosol process for the design of new CMG materials with tailored electrocatalytic properties.

Onsite aerosol measurements for various engineered nanomaterials at industrial manufacturing plants

NASA Astrophysics Data System (ADS)

Ogura, I.; Sakurai, H.; Gamo, M.

2011-07-01

Evaluation of the health impact of and control over exposure to airborne engineered nanomaterials (ENMs) requires information, inter alia, the magnitude of environmental release during various industrial processes, as well as the size distribution and morphology of the airborne ENM particles. In this study, we performed onsite aerosol measurements for various ENMs at industrial manufacturing plants. The industrial processes investigated were the collection of SiC from synthesis reactors, synthesis and bagging of LiFePO4, and bagging of ZnO. Real-time aerosol monitoring using condensation particle counters, optical particle counters, and an electrical low-pressure impactor revealed frequent increases in the number concentrations of submicron- and micron-sized aerosol particles, but few increases in the number concentrations of nanoparticles. In the SEM observations, a large number of submicron- and micron-sized agglomerated ENM particles were observed.

Measurements of Gases and Aerosols during 2010Cal-Mex

NASA Astrophysics Data System (ADS)

Zheng, J.; Zhang, R.; Molina, L.

2012-04-01

The major goal of the collaborative Cal-Mex 2010 research project is to assess the sources and processing of emissions along the California-Mexico border region and their effects on regional air quality and climate in order to provide scientific information to decision makers of both nations when addressing these two inter-related issues. During the Cal-Mex 2010 field study, the TAMU teams have collected extensive data sets from Tijuana/San Diego border, including volatile organic compounds (VOCs), gaseous sulfuric acid (H2SO4) and a suite set of physical and chemical parameters of aerosols. This comprehensive data set requires additional effort to process and analyze the measurements of gases and aerosols during Cal-Mex 2010. In this talk, preliminary data analysis of gases and aerosols will be presented, including VOCs and particle mixing states, morphology, and effective densities.

Temporal and spatial variation of morphological descriptors for atmospheric aerosols collected in Mexico City

NASA Astrophysics Data System (ADS)

China, S.; Mazzoleni, C.; Dubey, M. K.; Chakrabarty, R. K.; Moosmuller, H.; Onasch, T. B.; Herndon, S. C.

2010-12-01

We present an analysis of morphological characteristics of atmospheric aerosol collected during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign that took place in Mexico City in March 2006. The sampler was installed on the Aerodyne mobile laboratory. The aerosol samples were collected on nuclepore clear polycarbonate filters mounted in Costar pop-top membrane holders. More than one hundred filters were collected at different ground sites with different atmospheric and geographical characteristics (urban, sub-urban, mountain-top, industrial, etc.) over a month period. Selected subsets of these filters were analyzed for aerosol morphology using a scanning electron microscope and image analysis techniques. In this study we investigate spatial and temporal variations of aerosol shape descriptors, morphological parameters, and fractal dimension. We also compare the morphological results with other aerosol measurements such as aerosol optical properties(scattering and absorption) and size distribution data. Atmospheric aerosols have different morphological characteristics depending on many parameters such as emission sources, atmospheric formation pathways, aging processes, and aerosol mixing state. The aerosol morphology influences aerosol chemical and mechanical interactions with the environment, physical properties, and radiative effects. In this study, ambient aerosol particles have been classified in different shape groups as spherical, irregularly shaped, and fractal-like aggregates. Different morphological parameters such as aspect ratio, roundness, feret diameter, etc. have been estimated for irregular shaped and spherical particles and for different kinds of soot particles including fresh soot, collapsed and coated soot. Fractal geometry and image processing have been used to obtain morphological characteristics of different soot particles. The number of monomers constituting each aggregate and their diameters were measured and used to estimate an ensemble three-dimensional (3-d) fractal dimension. One-dimensional (1-d) and two-dimensional (2-d) fractal geometries have been measured using a power-law scaling relationship between 1-d and 2-d properties of projected images. Temporal variations in fractal dimension of soot-like aggregates have been observed at the mountaintop site and spatial variation of fractal dimension and other morphological descriptors of different shaped particles have been investigated for the different ground sites.

Source apportionment of particulate organic matter using infrared spectra at multiple IMPROVE sites

NASA Astrophysics Data System (ADS)

Kuzmiakova, A.; Dillner, A. M.; Takahama, S.

2016-12-01

As organic aerosol is a dominant contributor to air pollution and radiative forcing in many regions in the United States, characterizing its composition and apportioning the organic mass to its major sources provides insight into atmospheric processes and guidance for decreasing its abundance. National networks, such as Interagency Monitoring of Protected Visual Environment (IMPROVE), provide multi-site and multi-year particulate matter samples useful for evaluating sources over all four seasons. To this end, our study focuses on apportioning the particulate organic matter (OM) to specific anthropogenic and biological processes from year-long infrared aerosol measurements collected at six IMPROVE sites (five national park sites and one urban site) during 2011. Pooling these organic aerosol samples into one dataset, we apply factor and cluster analyses to extract four chemical factors (two dominated by processed emissions, one dominated by hydroxyl groups, and one by hydrocarbons) and ascribe each factor to a specific source depending on the site and season. We also present a method to characterize measurement uncertainty in infrared instrumental analysis and investigate sensitivity analysis in generated factors. In Phoenix (the urban site) we find the majority (80-95%) of the OM consisted of anthropogenic activities, such as traffic emissions, fossil fuel combustion (both all year long), and residential wood burning (fall to winter). Mineral dust emissions accounted for the rest of OM (5-20%). At the National Park sites the OM concentration was lower on average and consisted of marine and dust aerosols, summertime biomass burning and biogenic aerosols, processed fossil fuel combustion, and emissions from ships and oil refineries. Our study highlights the potential for further site-specific or multi-year aerosol characterization in the context of a long-term atmospheric sampling program to quantify sources of organic particles impacting air quality, aid in policy-making, and assess which (trans)formation mechanisms proposed in laboratory studies are consistent with observations.

Consistency of two global MODIS aerosol products over ocean on Terra and Aqua CERES SSF datasets

NASA Astrophysics Data System (ADS)

Ignatov, Alexander; Minnis, Patrick; Wielicki, Bruce; Loeb, Norman G.; Remer, Lorraine A.; Kaufman, Yoram J.; Miller, Walter F.; Sun-Mack, Sunny; Laszlo, Istvan; Geier, Erika B.

2004-12-01

MODIS aerosol retrievals over ocean from Terra and Aqua platforms are available from the Clouds and the Earth's Radiant Energy System (CERES) Single Scanner Footprint (SSF) datasets generated at NASA Langley Research Center (LaRC). Two aerosol products are reported side by side. The primary M product is generated by subsetting and remapping the multi-spectral (0.44 - 2.1 μm) MOD04 aerosols onto CERES footprints. MOD04 processing uses cloud screening and aerosol algorithms developed by the MODIS science team. The secondary (AVHRR-like) A product is generated in only two MODIS bands: 1 and 6 on Terra, and ` and 7 on Aqua. The A processing uses NASA/LaRC cloud-screening and NOAA/NESDIS single channel aerosol algorthm. The M and A products have been documented elsewhere and preliminarily compared using two weeks of global Terra CERES SSF (Edition 1A) data in December 2000 and June 2001. In this study, the M and A aerosol optical depths (AOD) in MODIS band 1 and (0.64 μm), τ1M and τ1A, are further checked for cross-platform consistency using 9 days of global Terra CERES SSF (Edition 2A) and Aqua CERES SSF (Edition 1A) data from 13 - 21 October 2002.

Microspectroscopic Analysis of Anthropogenic- and Biogenic-Influenced Aerosol Particles during the SOAS Field Campaign

NASA Astrophysics Data System (ADS)

Ault, A. P.; Bondy, A. L.; Nhliziyo, M. V.; Bertman, S. B.; Pratt, K.; Shepson, P. B.

2013-12-01

During the summer, the southeastern United States experiences a cooling haze due to the interaction of anthropogenic and biogenic aerosol sources. An objective of the summer 2013 Southern Oxidant and Aerosol Study (SOAS) was to improve our understanding of how trace gases and aerosols are contributing to this relative cooling through light scattering and absorption. To improve understanding of biogenic-anthropogenic interactions through secondary organic aerosol (SOA) formation on primary aerosol cores requires detailed physicochemical characterization of the particles after uptake and processing. Our measurements focus on single particle analysis of aerosols in the accumulation mode (300-1000 nm) collected using a multi orifice uniform deposition impactor (MOUDI) at the Centreville, Alabama SEARCH site. Particles were characterized using an array of microscopic and spectroscopic techniques, including: scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray analysis (EDX), and Raman microspectroscopy. These analyses provide detailed information on particle size, morphology, elemental composition, and functional groups. This information is combined with mapping capabilities to explore individual particle spatial patterns and how that impacts structural characteristics. The improved understanding will be used to explore how sources and processing (such as SOA coating of soot) change particle structure (i.e. core shell) and how the altered optical properties impact air quality/climate effects on a regional scale.

SeReNA Project: studying aerosol interactions with cloud microphysics in the Amazon Basin

NASA Astrophysics Data System (ADS)

Correia, A. L.; Catandi, P. B.; Frigeri, F. F.; Ferreira, W. C.; Martins, J.; Artaxo, P.

2012-12-01

Cloud microphysics and its interaction with aerosols is a key atmospheric process for weather and climate. Interactions between clouds and aerosols can impact Earth's radiative balance, its hydrological and energetic cycles, and are responsible for a large fraction of the uncertainty in climatic models. On a planetary scale, the Amazon Basin is one of the most significant land sources of moisture and latent heat energy. Moreover, every year this region undergoes mearked seasonal shifts in its atmospheric state, transitioning from clean to heavily polluted conditions due to the occurrence of seasonal biomass burning fires, that emit large amounts of smoke to the atmosphere. These conditions make the Amazon Basin a special place to study aerosol-cloud interactions. The SeReNA Project ("Remote sensing of clouds and their interaction with aerosols", from the acronym in Portuguese, @SerenaProject on Twitter) is an ongoing effort to experimentally investigate the impact of aerosols upon cloud microphysics in Amazonia. Vertical profiles of droplet effective radius of water and ice particles, in single convective clouds, can be derived from measurements of the emerging radiation on cloud sides. Aerosol optical depth, cloud top properties, and meteorological parameters retrieved from satellites will be correlated with microphysical properties derived for single clouds. Maps of cloud brightness temperature will allow building temperature vs. effective radius profiles for hydrometeors in single clouds. Figure 1 shows an example extracted from Martins et al. (2011), illustrating a proof-of-concept for the kind of result expected within the framework for the SeReNA Project. The results to be obtained will help foster the quantitative knowledge about interactions between aerosols and clouds in a microphysical level. These interactions are a fundamental process in the context of global climatic changes, they are key to understanding basic processes within clouds and how aerosols can influence them. Reference: Martins et al. (2011) ACP, v.11, p.9485-9501. Available at: http://bit.ly/martinspaper Figure 1. Brightness temperature (left panel) and thermodynamic phase (right) of hydrometeors in the convective cloud shown in the middle panel. Extracted from Martins et al. (2011).

Combined ground-based and satellite remote sensing of atmospheric aerosol and Earth surface in the Antarctic

NASA Astrophysics Data System (ADS)

Chaikovsky, Anatoli; Korol, Michail; Malinka, A.; Zege, E.; Katsev, I.; Prikhach, A.; Denisov, S.; Dick, V.; Goloub, P.; Blarel, L.; Chaikovskaya, L.; Lapyonok, A.; Podvin, T.; Denishchik-Nelubina, N.; Fedarenka, A.; Svidinsky, V.

2016-01-01

The paper presents lecture materials given at the Nineteenth International Conference and School on Quantum Electronics "Laser Physics and Applications" (19th ICSQE) in 2016, Sozopol, Bulgaria and contains the results of the 10-year research of Belarusian Antarctic expeditions to study the atmospheric aerosol and Earth surface in Antarctica. The works focus on the studying variability and trends of aerosol, cloud and snow characteristics in the Antarctic and the links of these processes with the long range transport of atmospheric pollutants and climate changes.

Simulation of the Aerosol-Atmosphere Interaction in the Dead Sea Area with COSMO-ART

NASA Astrophysics Data System (ADS)

Vogel, Bernhard; Bangert, Max; Kottmeier, Christoph; Rieger, Daniel; Schad, Tobias; Vogel, Heike

2014-05-01

The Dead Sea is a unique environment located in the Dead Sea Rift Valley. The fault system of the Dead Sea Rift Valley marks the political borders between Israel, Jordan, and Palestine. The Dead Sea region and the ambient Eastern Mediterranean coastal zone provide a natural laboratory for studying atmospheric processes ranging from the smallest scale of cloud processes to regional weather and climate. The virtual institute DESERVE is designed as a cross-disciplinary and cooperative international project of the Helmholtz Centers KIT, GFZ, and UFZ with well-established partners in Israel, Jordan and Palestine. One main focus of one of the work packages is the role of aerosols in modifying clouds and precipitation and in developing the Dead Sea haze layer as one of the most intriguing questions. The haze influences visibility, solar radiation, and evaporation and may even affect economy and health. We applied the online coupled model system COSMO-ART, which is able to treat the feedback processes between aerosol, radiation, and cloud formation, for a case study above the Dead Sea and adjacent regions. Natural aerosol like mineral dust and sea salt as well as anthropogenic primary and secondary aerosol is taken into account. Some of the observed features like the vertical double structure of the haze layer are already covered by the simulation. We found that absorbing aerosol like mineral dust causes a temperature increase in parts of the model domain. In other areas a decrease in temperature due to cirrus clouds modified by elevated dust layers is simulated.

Interaction of Burning Metal Particles

NASA Technical Reports Server (NTRS)

Dreizin, Edward L.; Berman, Charles H.; Hoffmann, Vern K.

1999-01-01

Physical characteristics of the combustion of metal particle groups have been addressed in this research. The combustion behavior and interaction effects of multiple metal particles has been studied using a microgravity environment, which presents a unique opportunity to create an "aerosol" consisting of relatively large particles, i.e., 50-300 m diameter. Combustion behavior of such an aerosol could be examined using methods adopted from well-developed single particle combustion research. The experiment included fluidizing relatively large (order of 100 m diameter) uniform metal particles under microgravity and igniting such an "aerosol" using a hot wire igniter. The flame propagation and details of individual particle combustion and particle interaction have been studied using a high speed movie and video-imaging with cameras coupled with microscope lenses to resolve individual particles. Interference filters were used to separate characteristic metal and metal oxide radiation bands from the thermal black body radiation. Recorded flame images were digitized and various image processing techniques including flame position tracking, color separation, and pixel by pixel image comparison were employed to understand the processes occurring in the burning aerosol. The development of individual particle flames, merging or separation, and extinguishment as well as induced particle motion have been analyzed to identify the mechanisms governing these processes. Size distribution, morphology, and elemental compositions of combustion products were characterized and used to link the observed in this project aerosol combustion phenomena with the recently expanded mechanism of single metal particle combustion.

Pulmonary aerosol delivery and the importance of growth dynamics.

PubMed

Haddrell, Allen E; Lewis, David; Church, Tanya; Vehring, Reinhard; Murnane, Darragh; Reid, Jonathan P

2017-12-01

Aerosols are dynamic systems, responding to variations in the surrounding environmental conditions by changing in size, composition and phase. Although, widely used in inhalation therapies, details of the processes occurring on aerosol generation and during inhalation have received little attention. Instead, research has focused on improvements to the formulation of the drug prior to aerosolization and the resulting clinical efficacy of the treatment. Here, we highlight the processes that occur during aerosol generation and inhalation, affecting aerosol disposition when deposited and, potentially, impacting total and regional doses. In particular, we examine the response of aerosol particles to the humid environment of the respiratory tract, considering both the capacity of particles to grow by absorbing moisture and the timescale for condensation to occur. [Formula: see text].

Study of particulate matter from Primary/Secondary Marine Aerosol and anthropogenic sources collected by a self-made passive sampler for the evaluation of the dry deposition impact on built heritage.

PubMed

Morillas, Héctor; Maguregui, Maite; García-Florentino, Cristina; Marcaida, Iker; Madariaga, Juan Manuel

2016-04-15

Dry deposition is one of the most dangerous processes that can take place in the environment where the compounds that are suspended in the atmosphere can react directly on different surrounding materials, promoting decay processes. Usually this process is related with industrial/urban fog and/or marine aerosol in the coastal areas. Particularly, marine aerosol transports different types of salts which can be deposited on building materials and by dry deposition promotes different decay pathways. A new analytical methodology based on the combined use of Raman Spectroscopy and SEM-EDS (point-by-point and imaging) was applied. For that purpose, firstly evaporated seawater (presence of Primary Marine Aerosol (PMA)) was analyzed. After that, using a self-made passive sampler (SMPS), different suspended particles coming from marine aerosol (transformed particles in the atmosphere (Secondary Marine Aerosol (SMA)) and metallic airborne particulate matter coming from anthropogenic sources, were analyzed. Finally in order to observe if SMA and metallic particles identified in the SMPS can be deposited on a building, sandstone samples from La Galea Fortress (Getxo, north of Spain) located in front of the sea and in the place where the passive sampler was mounted were analyzed. Copyright © 2016 Elsevier B.V. All rights reserved.

Effect of Dust and Anthropogenic Aerosols on Columnar Aerosol Optical Properties over Darjeeling (2200 m asl), Eastern Himalayas, India

PubMed Central

Chatterjee, Abhijit; Ghosh, Sanjay K.; Adak, Anandamay; Singh, Ajay K.; Devara, Panuganti C. S.; Raha, Sibaji

2012-01-01

Background The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. Methodology/Principal Findings An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca2+) during pre-monsoon (Apr – May) which was higher by 162% than its annual mean whereas during winter (Dec – Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO4 2− and black carbon) were higher (76% for black carbon and 96% for fine mode SO4 2−) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. Conclusion/Significance The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas. PMID:22792264

Seasonality of Aerosols the Southeastern United States

NASA Astrophysics Data System (ADS)

Ford, B. J.; Heald, C. L.

2012-12-01

Previous studies have suggested that increases in atmospheric aerosols of biogenic origin may have caused regional cooling over the southeastern United States in recent decades. Understanding the sources and behaviors of these aerosols is important for determining their role in a changing climate and managing their air quality impacts. In this study, we investigate the strong seasonality in aerosol optical depth (AOD) observed by MODIS, MISR, and CALIOP instruments over the southeastern United States and show that this is not simulated by a chemical transport model (GEOS-Chem). However, the model does reproduce surface PM 2.5 concentrations in the region as reported by the IMPROVE and Southeastern Aerosol Research and Characterization (SEARCH) networks, as well as the muted seasonality of these concentrations. In addition, these surface measurements show that organic aerosol makes up a small fraction of total PM 2.5 and has relatively little seasonality, which calls into question the importance of biogenic aerosol as a driver for climate change in the region. Sounding profiles and ground observations of relative humidity suggest that the magnitude of seasonality in AOD cannot be explained by seasonal differences in the hygroscopic growth of aerosols. CALIOP measurements of the vertical profile of aerosol extinction confirm that the likely reconciliation of the differences in seasonality between the surface PM 2.5 and AOD observations is the formation of aerosol aloft, a process not captured by the model. These findings provide initial insights for the Southern Oxidant and Aerosol Study (SOAS) campaign in 2013 which aims to investigate the anthropogenic influence on biogenic aerosol formation in the Southeastern US and elucidate the impact on regional climate and air quality.

Stratospheric Aerosol--Observations, Processes, and Impact on Climate

NASA Technical Reports Server (NTRS)

Kresmer, Stefanie; Thomason, Larry W.; von Hobe, Marc; Hermann, Markus; Deshler, Terry; Timmreck, Claudia; Toohey, Matthew; Stenke, Andrea; Schwarz, Joshua P.; Weigel, Ralf;

Isotopic mass independent signature of black crusts: a proxy for atmospheric aerosols formation in the Paris area (France).

NASA Astrophysics Data System (ADS)

Genot, Isabelle; Martin, Erwan; Yang, David Au; De Rafelis, Marc; Cartigny, Pierre; Wing, Boswell; Le Gendre, Erwann; Bekki, Slimane

2016-04-01

In view of the negative forcing of the sulfate aerosols on climate, a more accurate understanding of the formation of these particles is crucial. Indeed, despite the knowledge of their effects, uncertainties remain regarding the formation of sulfate aerosols, particularly the oxidation processes of S-bearing gases. Since the discovery of oxygen and sulfur mass independent fractionation (O- and S-MIF) processes on Earth, the sulfate isotopic composition became essential to investigate the atmospheric composition evolution and its consequences on the climate and the biosphere. Large amount of S-bearing compounds (SO2 mainly) is released into the atmosphere by anthropogenic and natural sources. Their oxidation in the atmosphere generates sulfate aerosols, H2SO4, which precipitate on the earth surface mainly as acid rain. One consequence of this precipitation is the formation of black crust on buildings made of carbonate stones. Indeed the chemical alteration of CaCO3 by H2SO4 leads to gypsum (CaSO4·2H2O) concretions on building walls. Associated to other particles, gypsum forms black-crusts. Therefore, black crusts acts as 'sulfate aerosol traps', meaning that their isotopic composition reveals the composition and thus the source and formation processes of sulfate aerosols in the atmosphere in a specific region. In this study we collected 37 black crusts on a 300km NW-SE profile centered on Paris (France). In our samples, sulfate represent 40wt.% and other particles 60wt.% of the black crusts. After sulfate extraction from each samples we measured their O- and S-isotopes composition. Variations of about 10‰ in δ18O and δ34S are observed and both O-MIF (Δ17O from 0 to 1.4‰) and S-MIF (Δ33S from 0 to -0.3‰) compositions have been measured. In regards to these compositions we can discuss the source and formation (oxidation pathways) of the sulfate aerosols in troposphere above the Paris region that covers urban, rural and coastal environments. Furthermore, this study shows for the first time O- and S-MIF signature in black crusts. Finally, we demonstrate that black crusts can be considered as a good 'sulfate aerosols traps', which can be widely used to study the sulfate aerosol formation, fate and sink in the troposphere.

Seasonal dependence of aerosol processing in urban Philadelphia

NASA Astrophysics Data System (ADS)

Avery, A. M.; Waring, M. S.; DeCarlo, P. F.

2017-12-01

Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower temperatures. Aerosol compositional differences in winter and summer indicate Philadelphia resident's aerosol exposures vary significantly with season.

Comprehensive modeling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition

NASA Astrophysics Data System (ADS)

Gallimore, P. J.; Griffiths, P. T.; Pope, F. D.; Reid, J. P.; Kalberer, M.

2017-04-01

The chemical composition of organic aerosols profoundly influences their atmospheric properties, but a detailed understanding of heterogeneous and in-particle reactivity is lacking. We present here a combined experimental and modeling study of the ozonolysis of oleic acid particles. An online mass spectrometry (MS) method, Extractive Electrospray Ionization (EESI), is used to follow the composition of the aerosol at a molecular level in real time; relative changes in the concentrations of both reactants and products are determined during aerosol aging. The results show evidence for multiple non-first-order reactions involving stabilized Criegee intermediates, including the formation of secondary ozonides and other oligomers. Offline liquid chromatography MS is used to confirm the online MS assignment of the monomeric and dimeric products. We explain the observed EESI-MS chemical composition changes, and chemical and physical data from previous studies, using a process-based aerosol chemistry simulation, the Pretty Good Aerosol Model (PG-AM). In particular, we extend previous studies of reactant loss by demonstrating success in reproducing the time dependence of product formation and the evolving particle size. This advance requires a comprehensive chemical scheme coupled to the partitioning of semivolatile products; relevant reaction and evaporation parameters have been refined using our new measurements in combination with PG-AM.

Quantifying the effect of organic aerosol aging and intermediate-volatility emissions on regional-scale aerosol pollution in China

PubMed Central

Zhao, Bin; Wang, Shuxiao; Donahue, Neil M.; Jathar, Shantanu H.; Huang, Xiaofeng; Wu, Wenjing; Hao, Jiming; Robinson, Allen L.

2016-01-01

Secondary organic aerosol (SOA) is one of the least understood constituents of fine particles; current widely-used models cannot predict its loadings or oxidation state. Recent laboratory experiments demonstrated the importance of several new processes, including aging of SOA from traditional precursors, aging of primary organic aerosol (POA), and photo-oxidation of intermediate volatility organic compounds (IVOCs). However, evaluating the effect of these processes in the real atmosphere is challenging. Most models used in previous studies are over-simplified and some key reaction trajectories are not captured, and model parameters are usually phenomenological and lack experimental constraints. Here we comprehensively assess the effect of organic aerosol (OA) aging and intermediate-volatility emissions on regional-scale OA pollution with a state-of-the-art model framework and experimentally constrained parameters. We find that OA aging and intermediate-volatility emissions together increase OA and SOA concentrations in Eastern China by about 40% and a factor of 10, respectively, thereby improving model-measurement agreement significantly. POA and IVOCs both constitute over 40% of OA concentrations, and IVOCs constitute over half of SOA concentrations; this differs significantly from previous apportionment of SOA sources. This study facilitates an improved estimate of aerosol-induced climate and health impacts, and implies a shift from current fine-particle control policies. PMID:27350423

Evidence of Aerosols as a Media for Rapid Daytime HONO Production over China

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Zhen; Wang, Yuhang; Costabile, Francesa

Current knowledge of daytime HONO sources remains incomplete. A large missing daytime HONO source has been found in many places around the world, including polluted regions in China. Conventional understanding and recent studies attributed this missing source mainly to ground surface processes or gas-phase chemistry, while assuming aerosols to be an insignificant media for HONO production. We analyze in situ observations of HONO and its precursors at an urban site in Beijing, China, and report an apparent dependence of the missing HONO source strength on aerosol surface area and solar ultraviolet radiation. Based on extensive correlation analysis and process-modeling, wemore » propose that the rapid daytime HONO production in Beijing can be explained by enhanced hydrolytic disproportionation of NO2 on aqueous aerosol surfaces due to catalysis by dicarboxylic acid anions. The combination of high abundance of NO2, aromatic hydrocarbons, and aerosols over broad regions in China likely leads to elevated HONO levels, rapid OH production, and enhanced oxidizing capacity on a regional basis. Our findings call for attention to aerosols as a media for daytime heterogeneous HONO production in polluted regions like Beijing. This study also highlights the complex and uncertain heterogeneous chemistry in China, which merits future efforts of reconciling regional modeling and laboratory experiments, in order to understand and mitigate the regional particulate and O3 pollutions over China.« less

A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects

NASA Technical Reports Server (NTRS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-01-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

A global modeling study on carbonaceous aerosol microphysical characteristics and radiative effects

NASA Astrophysics Data System (ADS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-08-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.

Desiccation by Foliar Deposition of Hygroscopic Aerosols may link Air Pollution to Forest Decline and Tree Mortality associated with Global-Change-Type Drought

NASA Astrophysics Data System (ADS)

Burkhardt, J.; Grantz, D. A.; Hunsche, M.; Pariyar, S.; Sutton, M. A.; Zinsmeister, D.

2016-12-01

Leaf surfaces are a major sink for atmospheric aerosol deposition. Plants benefit from aerosol associated nutrients and are able to increase deposition by leaf surface micromorphology. Recent studies have shown that deposited hygroscopic aerosols can also influence plant water relations. This might be an important issue even for remote forest ecosystems, given the strong anthropogenic influence on aerosol production and efficient atmospheric transport. We study processes of aerosol deposition to plant surfaces and their impact on water relations and drought tolerance, both for experimental particle amendment and for aerosol exclusion in filtered air (FA). FA plants experience an environment with < 10% concentration of hygroscopic aerosols compared to ambient air (AA), but no difference in trace gases. Increasing particle concentration leads to decreasing water use efficiency and increasing minimum epidermal conductance (gmin; a measure of uncontrolled water loss inversely related to drought tolerance). After particle amendment, anisohydric beech seedlings increased transpiration and maintained photosynthesis, while isohydric pine seedlings maintained transpiration and tended to reduce photosynthesis. FA seedlings of pine, oak, and fir showed lower gmin than corresponding AA seedlings. The results support the concept of hydraulic activation of stomata (HAS) and an associated wick action caused by leaf surface particles. Concentrated salt solutions formed by hygroscopicity even in unsaturated air may create a thin liquid film that penetrates the stomatal pore, allowing evaporation of liquid water at the leaf surface. Increased gmin suggests the significance of this process under ambient conditions. The direct impact of air pollution on plant drought tolerance is poorly integrated in current scenarios of forest decline and tree mortality, but might represent an important component.

The Aerosol/Cloud/Ecosystems Mission (ACE)

NASA Technical Reports Server (NTRS)

Schoeberl, Mark

2008-01-01

The goals and measurement strategy of the Aerosol/Cloud/Ecosystems Mission (ACE) are described. ACE will help to answer fundamental science questions associated with aerosols, clouds, air quality and global ocean ecosystems. Specifically, the goals of ACE are: 1) to quantify aerosol-cloud interactions and to assess the impact of aerosols on the hydrological cycle and 2) determine Ocean Carbon Cycling and other ocean biological processes. It is expected that ACE will: narrow the uncertainty in aerosol-cloud-precipitation interaction and quantify the role of aerosols in climate change; measure the ocean ecosystem changes and precisely quantify ocean carbon uptake; and, improve air quality forecasting by determining the height and type of aerosols being transported long distances. Overviews are provided of the aerosol-cloud community measurement strategy, aerosol and cloud observations over South Asia, and ocean biology research goals. Instruments used in the measurement strategy of the ACE mission are also highlighted, including: multi-beam lidar, multiwavelength high spectra resolution lidar, the ocean color instrument (ORCA)--a spectroradiometer for ocean remote sensing, dual frequency cloud radar and high- and low-frequency micron-wave radiometer. Future steps for the ACE mission include refining measurement requirements and carrying out additional instrument and payload studies.

An Overview of the Tropospheric Aerosol Radiative Forcing Observational Experiment

NASA Technical Reports Server (NTRS)

Russell, P. B.; Chan, K. Roland (Technical Monitor)

1997-01-01

Aerosol effects on atmospheric radiation are a leading source of uncertainty in predicting future climate. As a result, the International Global Atmospheric Chemistry Program has established a Focus on Atmospheric Aerosols (IGAC/FAA) and endorsed a series of aerosol field campaigns. TARFOX, the second in the IGAC/FAA series, was designed to reduce this uncertainty by measuring aerosol properties and effects in the US eastern seaboard, where one of the world's major plumes of industrial haze moves from the continent over the Atlantic Ocean. TARFOX's objectives are to: 1. Make simultaneous measurements of: (a) aerosol effects on radiation fields, and (b) the chemical, physical, and optical properties of the aerosols causing those effects. 2. Perform a variety of closure studies by using overdetermined data sets to test the mutual consistency of measurements and calculations of a wide range of aerosol properties and effects. 3. Use the results of the closure studies to assess and reduce uncertainties in estimates of aerosol radiative forcing, as well as to guide future field programs. An important subset of the closure studies is tests and improvements of algorithms used to derive aerosol properties and radiative effects from satellite measurements. The TARFOX Intensive Field Period (IFP) was conducted July 10-31, 1996. It included coordinated measurements from four satellites (GOES-8, NOAA-14, ERS-2, LANDSAT), four aircraft (ER-2, C-130, C-131, and a modified Cessna), land sites, and ships. A variety of aerosol conditions was sampled, ranging from relatively clean behind frontal passages to moderately polluted with aerosol optical depths exceeding 0.5 at mid-visible wavelengths. The latter conditions included separate incidents of enhancements caused primarily by anthropogenic sources and another incident of enhancement apparently influenced by recent fog processing. Spatial gradients of aerosol optical thickness were sampled to aid in isolating aerosol effects from other radiative effects and to more tightly constrain closure tests, including those of satellite retrievals. This talk gives an overview of TARFOX goals, rationale, methods, and initial key findings.

Aerosol processing: a wind of innovation in the field of advanced heterogeneous catalysts.

PubMed

Debecker, Damien P; Le Bras, Solène; Boissière, Cédric; Chaumonnot, Alexandra; Sanchez, Clément

2018-06-05

Aerosol processing is long known and implemented industrially to obtain various types of divided materials and nanomaterials. The atomisation of a liquid solution or suspension produces a mist of aerosol droplets which can then be transformed via a diversity of processes including spray-drying, spray pyrolysis, flame spray pyrolysis, thermal decomposition, micronisation, gas atomisation, etc. The attractive technical features of these aerosol processes make them highly interesting for the continuous, large scale, and tailored production of heterogeneous catalysts. Indeed, during aerosol processing, each liquid droplet undergoes well-controlled physical and chemical transformations, allowing for example to dry and aggregate pre-existing solid particles or to synthesise new micro- or nanoparticles from mixtures of molecular or colloidal precursors. In the last two decades, more advanced reactive aerosol processes have emerged as innovative means to synthesise tailored-made nanomaterials with tunable surface properties, textures, compositions, etc. In particular, the "aerosol-assisted sol-gel" process (AASG) has demonstrated tremendous potential for the preparation of high-performance heterogeneous catalysts. The method is mainly based on the low-cost, scalable, and environmentally benign sol-gel chemistry process, often coupled with the evaporation-induced self-assembly (EISA) concept. It allows producing micronic or submicronic, inorganic or hybrid organic-inorganic particles bearing tuneable and calibrated porous structures at different scales. In addition, pre-formed nanoparticles can be easily incorporated or formed in a "one-pot" bottom-up approach within the porous inorganic or hybrid spheres produced by such spray drying method. Thus, multifunctional catalysts with tailored catalytic activities can be prepared in a relatively simple way. This account is an overview of aerosol processed heterogeneous catalysts which demonstrated interesting performance in various relevant chemical reactions like isomerisation, hydrogenation, olefin metathesis, pollutant total oxidation, selective oxidation, CO2 methanation, etc. A short survey of patents and industrial applications is also presented. Our objective is to demonstrate the tremendous possibilities offered by the coupling between bottom up synthesis routes and these aerosol processing technologies which will most probably represent a major route of innovation in the mushrooming field of catalyst preparation research.

Applications of Sunphotometry to Aerosol Extinction and Surface Anisotropy

NASA Technical Reports Server (NTRS)

Tsay, S. C.; Holben, B. N.; Privette, J. L.

2005-01-01

Support cost-sharing of a newly developed sunphotometer in field deployment for aerosol studies. This is a cost-sharing research to deploy a newly developed sun-sky-surface photometer for studying aerosol extinction and surface anisotropy at the ARM SGP, TWP, and NSA-AAO CART sites and in many field campaigns. Atmospheric aerosols affect the radiative energy balance of the Earth, both directly by perturbing the incoming/outgoing radiation fields and indirectly by influencing the properties/processes of clouds and reactive greenhouse gases. The surface bidirectional reflectance distribution function (BRDF) also plays a crucial role in the radiative energy balance, since the BRDF is required to determine (1) the spectral and spectrally-averaged surface albedo, and (2) the top-of-the-atmosphere (TOA) angular distribution of radiance field. Therefore, the CART sites provide an excellent, albeit unique, opportunity to collect long-term climatic data in characterizing aerosol properties and various types of surface anisotropy.

Precipitation effects on aerosol concentration in the background EMEP station of Zarra (Valencia), Spain

NASA Astrophysics Data System (ADS)

Calvo, Ana Isabel; San Martín, Isabel; Castro, Amaya; Alonso-Blanco, Elisabeth; Alves, Célia; Duarte, Márcio; Fernández-González, Sergio; Fraile, Roberto

2014-05-01

Aerosols and precipitation are closely related, presenting a bidirectional influence and constituting an important source of uncertainties on climate change studies. However, they are usually studied independently and in general are only linked to one another for the development or validation of cloud models. The primary and secondary pollutants may be removed by wet and dry deposition. Wet deposition, including in-cloud and below-cloud scavenging processes, can efficiently remove atmospheric aerosols and it is considered a critical process for determining aerosol concentrations in the atmosphere. In this study, aerosols and precipitation data from a background Spanish EMEP (Cooperative Programme for the Monitoring and Evaluation of Long Range Transmission of Air Pollutants in Europe) station located in Zarra, Valencia (Spain) were analyzed (1° 06' W and 39° 05' N, 885 m asl). The effect of precipitation on aerosol concentration was studied and the correlation between the intensity of precipitation and scavenging effect was investigated. In order to evaluate the effects of precipitation on different aerosol size ranges three different aerosol fractions were studied: PM10, PM10-2.5 and PM2.5. In order to eliminate the influence of the air mass changes, only the days in which the air mass of the precipitation day and the previous day had the same origin were considered. Thus, from a total of 3586 rainy days registered from March 2001 to December 2010, 34 precipitation days satisfied this condition and were analyzed. During the period of study, daily precipitation ranged between 0.2 and 28.8 mm, with a mean value of 4 mm. Regarding the origin of the air masses, those from west were dominant at the three height levels investigated (500, 1500 and 3000 m). In order to obtain additional information, aerosol and precipitation chemical composition were also studied in relation to the days of precipitation and the previous days. Furthermore, in order to identify the type of weather associated with each particular synoptic situation, a Circulation Weather Type (CWT) classification was applied. Acknowledgment: This work has been funded by the Spanish Ministry of Science and Innovation (Grant TEC2010-19241-C02-01). S. Fernández-González acknowledges the grant from the "Programa de Formación de Profesorado Universitario (FPU)" awarded by the Spanish Ministry of Education.

Time-resolved distributions of bulk parameters, diacids, ketoacids and α-dicarbonyls and stable carbon and nitrogen isotope ratios of TC and TN in tropical Indian aerosols: Influence of land/sea breeze and secondary processes

NASA Astrophysics Data System (ADS)

Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.

2015-02-01

To better understand the photochemical production and diurnal distributions of organic and inorganic aerosols in the tropical coastal Indian atmosphere, the aerosol (TSP) samples were collected every 3 h during 30-31 January, 14-15 February and 28-29 May 2007 from Chennai and studied for total carbon (TC) and nitrogen (TN) and their stable isotope ratios (δ13CTC and δ15NTN), carbonaceous components, inorganic ions, diacids, ketoacids and α-dicarbonyls. Time-resolved distributions of bulk parameters, inorganic ions, and diacids and related compounds, except for few species, did not show any clear diurnal trend but showed peaks at 6-9 h during all the study periods, except for the peak at 15-18 h on 28 May. SO42-, C2 - C6 diacids, ketoacids and α-dicarbonyls in February and on 29 May showed a diurnal trend. δ13CTC and δ15NTN stayed relatively constant during the study periods but showed 13C depletion (in January) and 15 N enrichment when TC and TN peaked. Based on these results together with air mass trajectories, we found that the diurnal distributions of Chennai aerosols are mainly influenced by land/sea breeze and the aged (photochemically processed) air masses, although in situ photochemical production and nighttime chemistry of secondary aerosol species, particularly C2-C4 diacids and SO42-, are significant. The characteristics of seasonal variations of carbonaceous components, and diacids and related compounds and comparisons of δ13CTC and δ15NTN of Chennai aerosols with the isotopic signatures of the point sources inferred that biofuel/biomass burning in South and Southeast Asia are the major sources of aerosols (TSP).

Cloud processing of organic compounds: Secondary organic aerosol and nitrosamine formation

NASA Astrophysics Data System (ADS)

Hutchings, James W., III

Cloud processing of atmospheric organic compounds has been investigated through field studies, laboratory experiments, and numerical modeling. Observational cloud chemistry studies were performed in northern Arizona and fog studies in central Pennsylvania. At both locations, the cloud and fogs showed low acidity due to neutralization by soil dust components (Arizona) and ammonia (Pennsylvania). The field observations showed substantial concentrations (20-5500 ng•L -1) of volatile organic compounds (VOC) in the cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase with half lives of approximately three hours. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction kinetics decreased with increasing organic carbon content, resulting in half lives of approximately 7 hours. The secondary organic aerosol (SUA) mass formation potential of cloud processing of BTEX was evaluated. SOA mass formation by cloud processing of BTEX, while strongly dependent on the atmospheric conditions, could contribute up to 9% of the ambient atmospheric aerosol mass, although typically ˜1% appears realistic. Field observations also showed the occurrence of N-nitrosodimethylamine (NDMA), a potent carcinogen, in fogs and clouds (100-340 ng•L -1). Laboratory studies were conducted to investigate the formation of NDMA from nitrous acid and dimethylamine in the homogeneous aqueous phase within cloud droplets. While NDMA was produced in the cloud droplets, the low yields (<1%) observed could not explain observational concentrations. Therefore heterogeneous or gaseous formation of NDMA with partitioning to droplet must be the source of aqueous NDMA. Box-model calculations tended to demonstrate a predominance of a gas phase formation mechanism followed by partitioning into the cloud droplets. The calculations were consistent with field measurements of gaseous and aqueous NDMA concentrations. Measurements and model calculations showed that while NDMA is eventually photolyzed, it might persist in the atmosphere for hours.

Comprehensive chemical comparison of fuel composition and aerosol particles emitted from a ship diesel engine by gas chromatography atmospheric pressure chemical ionisation ultra-high resolution mass spectrometry with improved data processing routines.

PubMed

Rüger, Christopher P; Schwemer, Theo; Sklorz, Martin; O'Connor, Peter B; Barrow, Mark P; Zimmermann, Ralf

2017-02-01

The analysis of petrochemical materials and particulate matter originating from combustion sources remains a challenging task for instrumental analytical techniques. A detailed chemical characterisation is essential for addressing health and environmental effects. Sophisticated instrumentation, such as mass spectrometry coupled with chromatographic separation, is capable of a comprehensive characterisation, but needs advanced data processing methods. In this study, we present an improved data processing routine for the mass chromatogram obtained from gas chromatography hyphenated to atmospheric pressure chemical ionisation and ultra high resolution mass spectrometry. The focus of the investigation was the primary combustion aerosol samples, i.e. particulate matter extracts, as well as the corresponding fossil fuels fed to the engine. We demonstrate that utilisation of the entire transient and chromatographic information results in advantages including minimisation of ionisation artefacts and a reliable peak assignment. A comprehensive comparison of the aerosol and the feed fuel was performed by applying intensity weighted average values, compound class distribution and principle component analysis. Certain differences between the aerosol generated with the two feed fuels, diesel fuel and heavy fuel oil, as well as between the aerosol and the feed were revealed. For the aerosol from heavy fuel oil, oxidised species from the CHN and CHS class precursors of the feed were predominant, whereas the CHO x class is predominant in the combustion aerosol from light fuel oil. Furthermore, the complexity of the aerosol increases significantly compared to the feed and incorporating a higher chemical space. Coupling of atmospheric pressure chemical ionisation to gas chromatography was found to be a useful additional approach for characterisation of a combustion aerosol, especially with an automated utilisation of the information from the ultra-high resolution mass spectrometer and the chromatographic separation.

Assessing regional scale predictions of aerosols, marine stratocumulus, and their interactions during VOCALS-REx using WRF-Chem

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang Q.; Lee Y.; Gustafson Jr., W. I.

2011-12-02

This study assesses the ability of the recent chemistry version (v3.3) of the Weather Research and Forecasting (WRF-Chem) model to simulate boundary layer structure, aerosols, stratocumulus clouds, and energy fluxes over the Southeast Pacific Ocean. Measurements from the VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) and satellite retrievals (i.e., products from the MODerate resolution Imaging Spectroradiometer (MODIS), Clouds and Earth's Radiant Energy System (CERES), and GOES-10) are used for this assessment. The Morrison double-moment microphysics scheme is newly coupled with interactive aerosols in the model. The 31-day (15 October-16 November 2008) WRF-Chem simulation with aerosol-cloud interactions (AERO hereafter) is also comparedmore » to a simulation (MET hereafter) with fixed cloud droplet number concentrations in the microphysics scheme and simplified cloud and aerosol treatments in the radiation scheme. The well-simulated aerosol quantities (aerosol number, mass composition and optical properties), and the inclusion of full aerosol-cloud couplings lead to significant improvements in many features of the simulated stratocumulus clouds: cloud optical properties and microphysical properties such as cloud top effective radius, cloud water path, and cloud optical thickness. In addition to accounting for the aerosol direct and semi-direct effects, these improvements feed back to the simulation of boundary-layer characteristics and energy budgets. Particularly, inclusion of interactive aerosols in AERO strengthens the temperature and humidity gradients within the capping inversion layer and lowers the marine boundary layer (MBL) depth by 130 m from that of the MET simulation. These differences are associated with weaker entrainment and stronger mean subsidence at the top of the MBL in AERO. Mean top-of-atmosphere outgoing shortwave fluxes, surface latent heat, and surface downwelling longwave fluxes are in better agreement with observations in AERO, compared to the MET simulation. Nevertheless, biases in some of the simulated meteorological quantities (e.g., MBL temperature and humidity) and aerosol quantities (e.g., underestimations of accumulation mode aerosol number) might affect simulated stratocumulus and energy fluxes over the Southeastern Pacific, and require further investigation. The well-simulated timing and outflow patterns of polluted and clean episodes demonstrate the model's ability to capture daily/synoptic scale variations of aerosol and cloud properties, and suggest that the model is suitable for studying atmospheric processes associated with pollution outflow over the ocean. The overall performance of the regional model in simulating mesoscale clouds and boundary layer properties is encouraging and suggests that reproducing gradients of aerosol and cloud droplet concentrations and coupling cloud-aerosol-radiation processes are important when simulating marine stratocumulus over the Southeast Pacific.« less

Rapid Measurements of Aerosol Size Distribution and Hygroscopic Growth via Image Processing with a Fast Integrated Mobility Spectrometer (FIMS)

NASA Astrophysics Data System (ADS)

Wang, Y.; Pinterich, T.; Spielman, S. R.; Hering, S. V.; Wang, J.

2017-12-01

Aerosol size distribution and hygroscopicity are among key parameters in determining the impact of atmospheric aerosols on global radiation and climate change. In situ submicron aerosol size distribution measurements commonly involve a scanning mobility particle sizer (SMPS). The SMPS scanning time is in the scale of minutes, which is often too slow to capture the variation of aerosol size distribution, such as for aerosols formed via nucleation processes or measurements onboard research aircraft. To solve this problem, a Fast Integrated Mobility Spectrometer (FIMS) based on image processing was developed for rapid measurements of aerosol size distributions from 10 to 500 nm. The FIMS consists of a parallel plate classifier, a condenser, and a CCD detector array. Inside the classifier an electric field separates charged aerosols based on electrical mobilities. Upon exiting the classifier, the aerosols pass through a three stage growth channel (Pinterich et al. 2017; Spielman et al. 2017), where aerosols as small as 7 nm are enlarged to above 1 μm through water or heptanol condensation. Finally, the grown aerosols are illuminated by a laser sheet and imaged onto a CCD array. The images provide both aerosol concentration and position, which directly relate to the aerosol size distribution. By this simultaneous measurement of aerosols with different sizes, the FIMS provides aerosol size spectra nearly 100 times faster than the SMPS. Recent deployment onboard research aircraft demonstrated that the FIMS is capable of measuring aerosol size distributions in 1s (Figure), thereby offering a great advantage in applications requiring high time resolution (Wang et al. 2016). In addition, the coupling of the FIMS with other conventional aerosol instruments provides orders of magnitude more rapid characterization of aerosol optical and microphysical properties. For example, the combination of a differential mobility analyzer, a relative humidity control unit, and a FIMS was used to measure aerosol hygroscopic growth. Such a system reduced the time of measuring the hygroscopic properties of submicron aerosols (six sizes) to less than three minutes in total, with an error within 1%. Pinterich et al. (2017) Aerosol Sci. Technol. accepted Spielman et al. (2017) Aerosol Sci. Technol. accepted Wang et al. (2016) Nature 539:416-419

Impacts of Saharan Dust on the Atmospheric Radiative Balance in the Caribbean during SALTRACE 2013

NASA Astrophysics Data System (ADS)

Sauer, D. N.; Weinzierl, B.; Gross, S.; Minikin, A.; Freudenthaler, V.; Gasteiger, J.; Mayer, B. C.

2013-12-01

Direct and indirect aerosol radiative effects represent one of the largest uncertainties in the modeling of the climate system. To better quantify the effects of aerosols on the Earth's radiative balance and understand important physical effects on small scales such as the influence of aerosols on clouds, detailed measurements of aerosol properties are needed to build a globally representative data set. Mineral dust is among the most abundant aerosols and the Sahara Desert constitutes its largest source. During frequent dust outbreaks thick elevated aerosol layers are formed and transported over large distances -often across the Atlantic Ocean into the Caribbean. The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in June/July 2013 continues the SAMUM field experiments conducted in 2006 and 2008. It aims to study the long-range transport of Saharan mineral dust, the properties of aged mineral dust aerosol, and its impact on radiative quantities and cloud processes. The experiment led to an extensive data set on dust layers from Senegal to the Caribbean using airborne in-situ and remote sensing measurements, complemented with ground-based remote sensing and in-situ measurements on sites in Barbados and Puerto Rico as well as satellite remote sensing data. The airborne data were obtained with an extensive aerosol payload aboard the DLR-operated Falcon 20E research aircraft. The measurements cover the entire size range of atmospheric aerosol with a combination of cabin-operated and wing-mounted instruments. In addition, particle properties such as absorption coefficients and volatility are measured. A nadir-looking 2-μm Doppler-lidar system aboard the aircraft was used for wind measurements and served as a path finder for the selection of representative aerosol in-situ levels. In the Caribbean the dust usually arrives in several layers with distinct properties: the mostly undisturbed pure dust layer in altitudes up to 4-5 km, a transition layer where mixing and cloud processing has occurred, and a lower layer with a significant contribution from marine boundary layer aerosol. Here we present a case study of the direct radiative effects of Saharan dust layers found over Barbados using airborne in-situ and ground-based lidar observations. Using the radiative transfer package libRadtran we estimate the direct radiative forcing and radiative heating rate profiles inside the tropospheric column over Barbados. To deduce aerosol optical properties for the radiative transfer model, particle size distributions, aerosol refractive indices, and shape distributions are obtained from in-situ data. Coinciding lidar observations are used to deduce the vertical extent and structure of the different aerosol layers. To study the effect of aerosol aging on the radiative balance we compare the model results from in-situ data obtained in Barbados with results based on data from Senegal and the Cape Verde region and from the SAMUM field experiments, which characterized the dust properties near the source.

Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Brook, J.; Chang, R. Y.-W.; Evans, G. J.; Hayden, K.; Jeong, C.-H.; Li, S.-M.; Liggio, J.; Liu, P. S. K.; McGuire, M.; Mihele, C.; Sjostedt, S.; Vlasenko, A.; Abbatt, J. P. D.

2010-10-01

As part of the BAQS-Met 2007 field campaign, Aerodyne time-of-flight aerosol mass spectrometers (ToF-AMS) were deployed at two sites in southwestern Ontario from 17 June to 11 July, 2007. One instrument was located at Harrow, ON, a rural, agriculture-dominated area approximately 40 km southeast of the Detroit/Windsor/Windsor urban area and 5 km north of Lake Erie. The second instrument was located at Bear Creek, ON, a rural site approximately 70 km northeast of the Harrow site and 50 km east of Detroit/Windsor. Positive matrix factorization analysis of the combined organic mass spectral dataset yields factors related to secondary organic aerosol (SOA), direct emissions, and uptake processes. This is the first application of PMF to simultaneous AMS measurements at different sites, an approach which allows for self-consistent, direct comparison of the datasets. Case studies are utilized to investigate processing of SOA from (1) fresh emissions from Detroit/Windsor and (2) regional aerosol during periods of inter-site flow. A strong correlation is observed between SOA/excess CO and photochemical age as represented by the NOx/NOy ratio for Detroit/Windsor outflow. Although this correlation is not evident for more aged air, measurements at the two sites during inter-site transport nevertheless show evidence of continued atmospheric processing by SOA production.

A Miniaturized Nickel Oxide Thermistor via Aerosol Jet Technology.

PubMed

Wang, Chia; Hong, Guan-Yi; Li, Kuan-Ming; Young, Hong-Tsu

2017-11-12

In this study, a miniaturized thermistor sensor was produced using the Aerosol Jet printing process for temperature sensing applications. A nickel oxide nanoparticle ink with a large temperature coefficient of resistance was fabricated. The thermistor was printed with a circular NiO thin film in between the two parallel silver conductive tracks on a cutting tool insert. The printed thermistor, which has an adjustable dimension with a submillimeter scale, operates over a range of 30-250 °C sensitively (B value of ~4310 K) without hysteretic effects. Moreover, the thermistor may be printed on a 3D surface through the Aerosol Jet printing process, which has increased capability for wide temperature-sensing applications.

A Miniaturized Nickel Oxide Thermistor via Aerosol Jet Technology

PubMed Central

Wang, Chia; Hong, Guan-Yi; Li, Kuan-Ming; Young, Hong-Tsu

2017-01-01

In this study, a miniaturized thermistor sensor was produced using the Aerosol Jet printing process for temperature sensing applications. A nickel oxide nanoparticle ink with a large temperature coefficient of resistance was fabricated. The thermistor was printed with a circular NiO thin film in between the two parallel silver conductive tracks on a cutting tool insert. The printed thermistor, which has an adjustable dimension with a submillimeter scale, operates over a range of 30–250 °C sensitively (B value of ~4310 K) without hysteretic effects. Moreover, the thermistor may be printed on a 3D surface through the Aerosol Jet printing process, which has increased capability for wide temperature-sensing applications. PMID:29137148

Overview of TANGENT (Tandem Aerosol Nucleation and Growth ENvironment Tube) 2017 IOP Study

NASA Astrophysics Data System (ADS)

Tiszenkel, L.

2017-12-01

New particle formation consists of two steps: nucleation and growth of nucleated particles. However, most laboratory studies have been conducted under conditions where these two processes are convoluted together, thereby hampering the detailed understanding of the effect of chemical species and atmospheric conditions on two processes. The objective of the Tandem Aerosol Nucleation and Growth ENvironment Tube (TANGENT) laboratory study is to investigate aerosol nucleation and growth properties independently by separating these two processes in two different flow tubes. This research is a collaboration between the University of Alabama in Huntsville and the University of Delaware. In this poster we will present the experimental setup of TANGENT and summarize the key results from the first IOP (intense observation period) experiments undertaken during Summer 2017. Nucleation takes place in a temperature- and RH-controlled fast flow reactor (FT-1) where sulfuric acid forms from OH radicals and sulfur dioxide. Sulfuric acid and impurity base compounds are detected with chemical ionization mass spectrometers (CIMS). Particle sizes and number concentrations of newly nucleated particles are measured with a scanning mobility particle sizer (SMPS) and particle size magnifier (PSM), providing concentrations of particles between 1-100 nm. The nucleation particles are transferred directly to the growth tube (FT-2) where oxidants and biogenic organic precursors are added to grow nucleated nanoparticles. Sizes of particles after growth are analyzed with an additional SMPS and elemental chemical composition of 50 nm and above particles detected with a nano-aerosol mass spectrometer (NAMS). TANGENT provides the unique ability to conduct experiments that can monitor and control reactant concentrations, aerosol size and aerosol chemical composition during nucleation and growth. Experiments during this first IOP study have elucidated the effects of sulfur dioxide, particle size, relative humidity, temperature, oxidants and biogenic organics on nanoparticle formation and growth. In another 3 companion posters, we will discuss findings of these results in detail.

The Role of Aerosols on Precipitation Processes: Cloud Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Li, X.; Matsui, T.

2012-01-01

Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region, the sub-tropics (Florida) and midlatitudes using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CeN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for these cases. It is shown that since the low (CN case produces fewer droplets, larger sizes develop due to greater condensational and collection growth, leading to a broader size spectrum in comparison to the high CCN case. Sensitivity tests were performed to identify the impact of ice processes, radiation and large-scale influence on cloud-aerosol interactive processes, especially regarding surface rainfall amounts and characteristics (i.e., heavy or convective versus light or stratiform types). In addition, an inert tracer was included to follow the vertical redistribution of aerosols by cloud processes. We will also give a brief review from observational evidence on the role of aerosol on precipitation processes.

DOE Office of Scientific and Technical Information (OSTI.GOV)

None, None

This 3-year project has studied how aerosol pollution influences glaciated clouds. The tool applied has been an 'aerosol-cloud model'. It is a type of Cloud-System Resolving Model (CSRM) modified to include 2-moment bulk microphysics and 7 aerosol species, as described by Phillips et al. (2009, 2013). The study has been done by, first, improving the model and then performing sensitivity studies with validated simulations of a couple of observed cases from ARM. These are namely the Tropical Warm Pool International Cloud Experiment (TWP-ICE) over the tropical west Pacific and the Cloud and Land Surface Interaction Campaign (CLASIC) over Oklahoma. Duringmore » the project, sensitivity tests with the model showed that in continental clouds, extra liquid aerosols (soluble aerosol material) from pollution inhibited warm rain processes for precipitation production. This promoted homogeneous freezing of cloud droplets and aerosols. Mass and number concentrations of cloud-ice particles were boosted. The mean sizes of cloud-ice particles were reduced by the pollution. Hence, the lifetime of glaciated clouds, especially ice-only clouds, was augmented due to inhibition of sedimentation and ice-ice aggregation. Latent heat released from extra homogeneous freezing invigorated convective updrafts, and raised their maximum cloud-tops, when aerosol pollution was included. In the particular cases simulated in the project, the aerosol indirect effect of glaciated clouds was twice than of (warm) water clouds. This was because glaciated clouds are higher in the troposphere than water clouds and have the first interaction with incoming solar radiation. Ice-only clouds caused solar cooling by becoming more extensive as a result of aerosol pollution. This 'lifetime indirect effect' of ice-only clouds was due to higher numbers of homogeneously nucleated ice crystals causing a reduction in their mean size, slowing the ice-crystal process of snow production and slowing sedimentation. In addition to the known indirect effects (glaciation, riming and thermodynamic), new indirect effects were discovered and quantified due to responses of sedimentation, aggregation and coalescence in glaciated clouds to changing aerosol conditions. In summary, the change in horizontal extent of the glaciated clouds ('lifetime indirect effects'), especially of ice-only clouds, was seen to be of higher importance in regulating aerosol indirect effects than changes in cloud properties ('cloud albedo indirect effects').« less

Fog and Cloud Induced Aerosol Modification Observed by AERONET

NASA Technical Reports Server (NTRS)

Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M. A.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Platnick, S. E.; Arnold, G. T.;

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

NASA Astrophysics Data System (ADS)

Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

2016-02-01

Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of cloud and aerosol over the Southern Ocean.

Minimum aerosol layer detection sensitivities and their subsequent impacts on aerosol optical thickness retrievals in CALIPSO level 2 data products

NASA Astrophysics Data System (ADS)

Toth, Travis D.; Campbell, James R.; Reid, Jeffrey S.; Tackett, Jason L.; Vaughan, Mark A.; Zhang, Jianglong; Marquis, Jared W.

2018-01-01

Due to instrument sensitivities and algorithm detection limits, level 2 (L2) Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) 532 nm aerosol extinction profile retrievals are often populated with retrieval fill values (RFVs), which indicate the absence of detectable levels of aerosol within the profile. In this study, using 4 years (2007-2008 and 2010-2011) of CALIOP version 3 L2 aerosol data, the occurrence frequency of daytime CALIOP profiles containing all RFVs (all-RFV profiles) is studied. In the CALIOP data products, the aerosol optical thickness (AOT) of any all-RFV profile is reported as being zero, which may introduce a bias in CALIOP-based AOT climatologies. For this study, we derive revised estimates of AOT for all-RFV profiles using collocated Moderate Resolution Imaging Spectroradiometer (MODIS) Dark Target (DT) and, where available, AErosol RObotic NEtwork (AERONET) data. Globally, all-RFV profiles comprise roughly 71 % of all daytime CALIOP L2 aerosol profiles (i.e., including completely attenuated profiles), accounting for nearly half (45 %) of all daytime cloud-free L2 aerosol profiles. The mean collocated MODIS DT (AERONET) 550 nm AOT is found to be near 0.06 (0.08) for CALIOP all-RFV profiles. We further estimate a global mean aerosol extinction profile, a so-called noise floor, for CALIOP all-RFV profiles. The global mean CALIOP AOT is then recomputed by replacing RFV values with the derived noise-floor values for both all-RFV and non-all-RFV profiles. This process yields an improvement in the agreement of CALIOP and MODIS over-ocean AOT.

Explicit Cloud Nucleation from Arbitrary Mixtures of Aerosol Types and Sizes Using an Ultra-Efficient In-Line Aerosol Bin Model in High-Resolution Simulations of Hurricanes

NASA Astrophysics Data System (ADS)

Walko, R. L.; Ashby, T.; Cotton, W. R.

2017-12-01

The fundamental role of atmospheric aerosols in the process of cloud droplet nucleation is well known, and there is ample evidence that the concentration, size, and chemistry of aerosols can strongly influence microphysical, thermodynamic, and ultimately dynamic properties and evolution of clouds and convective systems. With the increasing availability of observation- and model-based environmental representations of different types of anthropogenic and natural aerosols, there is increasing need for models to be able to represent which aerosols nucleate and which do not in supersaturated conditions. However, this is a very complex process that involves competition for water vapor between multiple aerosol species (chemistries) and different aerosol sizes within each species. Attempts have been made to parameterize the nucleation properties of mixtures of different aerosol species, but it is very difficult or impossible to represent all possible mixtures that may occur in practice. As part of a modeling study of the impact of anthropogenic and natural aerosols on hurricanes, we developed an ultra-efficient aerosol bin model to represent nucleation in a high-resolution atmospheric model that explicitly represents cloud- and subcloud-scale vertical motion. The bin model is activated at any time and location in a simulation where supersaturation occurs and is potentially capable of activating new cloud droplets. The bins are populated from the aerosol species that are present at the given time and location and by multiple sizes from each aerosol species according to a characteristic size distribution, and the chemistry of each species is represented by its absorption or adsorption characteristics. The bin model is integrated in time increments that are smaller than that of the atmospheric model in order to temporally resolve the peak supersaturation, which determines the total nucleated number. Even though on the order of 100 bins are typically utilized, this leads only to a 10 or 20% increase in overall computational cost due to the efficiency of the bin model. This method is highly versatile in that it automatically accommodates any possible number and mixture of different aerosol species. Applications of this model to simulations of Typhoon Nuri will be presented.

Modeling aerosol suspension from soils and oceans as sources of micropollutants to air.

PubMed

Qureshi, Asif; MacLeod, Matthew; Hungerbühler, Konrad

2009-10-01

Soil and marine aerosol suspension are two physical mass transfer processes that are not usually included in models describing fate and transport of environmental pollutants. Here, we review the literature on soil and marine aerosol suspension and estimate aerosol suspension mass transfer velocities for inclusion in multimedia models, as a global average and on a 1 x 1 scale. The yearly, global average mass transfer velocity for soil aerosol suspension is estimated to be 6 x 10(-10)mh(-1), approximately an order of magnitude smaller than marine aerosol suspension, which is estimated to be 8 x 10(-9)mh(-1). Monthly averages of these velocities can be as high as 10(-7)mh(-1) and 10(-5)mh(-1) for soil and marine aerosol suspension, respectively, depending on location. We use a unit-world multimedia model to analyze the relevance of these two suspension processes as a mechanism that enhances long-range atmospheric transport of pollutants. This is done by monitoring a metric of long-range transport potential, phi-one thousand (phi1000), that denotes the fraction of modeled emissions to air, water or soil in a source region that reaches a distance of 1000 km in air. We find that when the yearly, globally averaged mass transfer velocity is used, marine aerosol suspension increases phi1000 only fractionally for both emissions to air and water. However, enrichment of substances in marine aerosols, or speciation between ionic and neutral forms in ocean water may increase the influence of this surface-to-air transfer process. Soil aerosol suspension can be the dominant process for soil-to-air transfer in an emission-to-soil scenario for certain substances that have a high affinity to soil. When a suspension mass transfer velocity near the maximum limit is used, soil suspension remains important if the emissions are made to soil, and marine aerosol suspension becomes important regardless of if emissions are made to air or water compartments. We recommend that multimedia models designed to assess the environmental fate and long-range transport behavior of substances with a range of chemical properties include both aerosol suspension processes, using the mass transfer velocities estimated here.

Sensitivity of nephelometric method for the investigation of condensation processes in submicron aerosol

NASA Astrophysics Data System (ADS)

Panchenko, Mikhail V.; Sviridenkov, Mikhail A.; Terpugova, Svetlana A.

2004-02-01

The possiblities to study the aerosol transformation with the artificial change fo the relative humidity, using the data of polarization and nephelometer measurements are discussed. It is shown that the set of parameters, measured by FAN nephelometer enable to retrieve the aerosol size distribution at different stages of humidification in the size range from 0.07 to 0.6-0.8 μm. The uncertainty in the estimation of the refractive index is within 0.02.

Substantial convection and precipitation enhancements by ultrafine aerosol particles

NASA Astrophysics Data System (ADS)

Fan, Jiwen; Rosenfeld, Daniel; Zhang, Yuwei; Giangrande, Scott E.; Li, Zhanqing; Machado, Luiz A. T.; Martin, Scot T.; Yang, Yan; Wang, Jian; Artaxo, Paulo; Barbosa, Henrique M. J.; Braga, Ramon C.; Comstock, Jennifer M.; Feng, Zhe; Gao, Wenhua; Gomes, Helber B.; Mei, Fan; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; de Souza, Rodrigo A. F.

2018-01-01

Ultrafine aerosol particles (smaller than 50 nanometers in diameter) have been thought to be too small to affect cloud formation. Fan et al. show that this is not the case. They studied the effect of urban pollution transported into the otherwise nearly pristine atmosphere of the Amazon. Condensational growth of water droplets around the tiny particles releases latent heat, thereby intensifying atmospheric convection. Thus, anthropogenic ultrafine aerosol particles may exert a more important influence on cloud formation processes than previously believed.

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dzepina, K.; Mazzoleni, C.; Fialho, P.

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.« less

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

DOE PAGES

Dzepina, K.; Mazzoleni, C.; Fialho, P.; ...

2015-05-05

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.« less

Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume

NASA Astrophysics Data System (ADS)

Dzepina, K.; Mazzoleni, C.; Fialho, P.; China, S.; Zhang, B.; Owen, R. C.; Helmig, D.; Hueber, J.; Kumar, S.; Perlinger, J. A.; Kramer, L. J.; Dziobak, M. P.; Ampadu, M. T.; Olsen, S.; Wuebbles, D. J.; Mazzoleni, L. R.

2015-05-01

Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m-3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100-1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.

Org Areo Boreal Forest Sources, compositions and properties of newly formed and regional organic aerosol in a boreal forest during the Biogenic Aerosol: Effects on Clouds and Climate Campaign

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thornton, Joel A

The major goals of this project were to make unique measurements, as part of the DOE sponsored Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign, of the volatility and molecular composition of organic aerosol, as well as gas-phase concentrations of oxygenated organic compounds that interact and affect organic aerosol. In addition, we aimed to conduct a similar set of measurements as part of a collaborative set of environmental simulation chamber experiments at PNNL, the aim of which was to simulate the atmospheric oxidation of key biogenic volatile organic compounds (BVOC) and study the associated formation and evolution of secondarymore » organic aerosol (SOA). The target BVOC were a set of monoterpenes, isoprene, and related intermediates such as IEPOX. The ultimate goal of such measurements are to develop a more detailed mechanistic understanding of the sensitivity of SOA mass formation and lifetime to precursor and environmental conditions. Molecular composition and direct volatility measurements provide robust tracers of chemical processing and properties. As such, meeting these goals will allow for stronger constraints on the types of processes and their fundamental descriptions needed to simulate aerosol particle number and size, and cloud nucleating ability in regional and global earth system models.« less

Parameterizations of Cloud Microphysics and Indirect Aerosol Effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tao, Wei-Kuo

1. OVERVIEW Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e.,more » Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al., 2000]. Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 1999]. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005]. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and summertime convection over a mid-latitude continent with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. The impact of atmospheric aerosol concentration on cloud and precipitation will be investigated. 2. MODEL DESCRIPTION AND CASE STUDIES 2.1 GCE MODEL The model used in this study is the 2D version of the GCE model. Modeled flow is anelastic. Second- or higher-order advection schemes can produce negative values in the solution. Thus, a Multi-dimensional Positive Definite Advection Transport Algorithm (MPDATA) has been implemented into the model. All scalar variables (potential temperature, water vapor, turbulent coefficient and all five hydrometeor classes) use forward time differencing and the MPDATA for advection. Dynamic variables, u, v and w, use a second-order accurate advection scheme and a leapfrog time integration (kinetic energy semi-conserving method). Short-wave (solar) and long-wave radiation as well as a subgrid-scale TKE turbulence scheme are also included in the model. Details of the model can be found in Tao and Simpson (1993) and Tao et al. (2003). 2.2 Microphysics (Bin Model) The formulation of the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (cloud droplets and raindrops), and six types of ice particles: pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail. Each type is described by a special size distribution function containing 33 categories (bins). Atmospheric aerosols are also described using number density size-distribution functions (containing 33 bins). Droplet nucleation (activation) is derived from the analytical calculation of super-saturation, which is used to determine the sizes of aerosol particles to be activated and the corresponding sizes of nucleated droplets. Primary nucleation of each type of ice crystal takes place within certain temperature ranges. A detailed description of these explicitly parameterized processes can be found in Khain and Sednev (1996) and Khain et al. (1999, 2001). 2.3 Case Studies Three cases, a tropical oceanic squall system observed during TOGA COARE (Tropical Ocean and Global Atmosphere Coupled Ocean-Atmosphere Response Experiment, which occurred over the Pacific Ocean warm pool from November 1992 to February 1993), a midlatitude continental squall system observed during PRESTORM (Preliminary Regional Experiment for STORM-Central, which occurred in Kansas and Oklahoma during May-June 1985), and mid-afternoon convection observed during CRYSTAL-FACE (Cirrus Regional Study of Tropical Anvils and Cirrus Layers – Florida Area Cumulus Experiment, which occurred in Florida during July 2002), will be used to examine the impact of aerosols on deep, precipitating systems. 3. SUMMARY of RESULTS • For all three cases, higher CCN produces smaller cloud droplets and a narrower spectrum. Dirty conditions delay rain formation, increase latent heat release above the freezing level, and enhance vertical velocities at higher altitude for all cases. Stronger updrafts, deeper mixed-phase regions, and more ice particles are simulated with higher CCN in good agreement with observations. • In all cases, rain reaches the ground early with lower CCN. Rain suppression is also evident in all three cases with high CCN in good agreement with observations (Rosenfeld, 1999, 2000 and others). Rain suppression, however, only occurs during the first hour of simulation. This result suggests that microphysical processes dominate the impact of aerosols on precipitation in the early stage of precipitation development. • During the mature stage of the simulations, the effect of increasing aerosol concentration ranges from rain suppression in the PRESTORM case to little effect on surface rainfall in the CRYSTAL-FACE case to rain enhancement in the TOGA COARE case. • The model results suggest that evaporative cooling is a key process in determining whether higher CCN reduces or enhances precipitation. Cold pool strength can be enhanced by stronger evaporation. When cold pool interacts with the near surface wind shear, the low-level convergence can be stronger, facilitating secondary cloud formation and more vigorous precipitation processes. Evaporative cooling is more than two times stronger at low levels with higher CCN for the TOGA COARE case during the early stages of precipitation development. However, evaporative cooling is slightly stronger at lower levels with lower CCN for the PRESTORM case. The early formation of rain in the clean environment could allow for the formation of an earlier and stronger cold pool compared to a dirty environment. PRESTORM has a very dry environment and both large and small rain droplets can evaporate. Consequently, the cold pool is relatively weaker, and the system is relatively less intense with higher CCN. • Sensitivity tests are conducted to determine the impact of ice processes on aerosol-precipitation interaction. The results suggested that ice processes are crucial for suppressing precipitation due to high CCN for the PRESTORM case. More and smaller ice particles are generated in the dirty case and transported to the trailing stratiform region. This reduces the heavy convective rain and contributes to the weakening of the cold pool. Warm rain processes dominate the TOGA COARE case. Therefore, ice processes only play a secondary role in terms of aerosol-precipitation interaction. • Two of the three cloud systems presented in this paper formed a line structure (squall system). A 2D simulation, therefore, gives a good approximation to such a line of convective clouds. Since the real atmosphere is 3D, further 3D cloud-resolving simulations are needed to address aerosol-precipitation interactions. 4. REFERENCES Tao, W.-K., X. Li, A. Khain, T. Matsui, S. Lang, and J. Simpson, 2007: The role of atmospheric aerosol concentration on deep convective precipitation: Cloud-resolving model simulations. J. Geophy. Res., 112, D24S18, doi:10.1029/2007JD008728. All other references can be found in above paper. 5. Acknowledgements The GCE model is mainly supported by the NASA Headquarters Atmospheric Dynamics and Thermodynamics Program and the NASA Tropical Rainfall Measuring Mission (TRMM). The research was also supported by the Office of Science (BER), U. S. Department of Energy/Atmospheric Radiation Measurement (DOE/ARM) Interagency. The authors acknowledge NASA Goddard Space Flight Center for computer time used in this research.« less

Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

NASA Astrophysics Data System (ADS)

Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

2014-12-01

Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the observed features.

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-03-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range of temporal variability, enabling the elucidation of the determinants of aerosol chemical composition, including source emissions, chemical processing, and transport, at the Canada-US border. This paper presents the first study to characterize the coupled influences of these determinants on temporal variability in aerosol chemical composition using single particle-type-based receptor modelling.

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

NASA Astrophysics Data System (ADS)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range of temporal variability, enabling the elucidation of the determinants of aerosol chemical composition, including source emissions, chemical processing, and transport, at the Canada-US border. This paper presents the first study to elucidate the coupled influences of these determinants on temporal variability in aerosol chemical composition using single particle-type-based receptor modelling.

Sugars in Antarctic aerosol

NASA Astrophysics Data System (ADS)

Barbaro, Elena; Kirchgeorg, Torben; Zangrando, Roberta; Vecchiato, Marco; Piazza, Rossano; Barbante, Carlo; Gambaro, Andrea

2015-10-01

The processes and transformations occurring in the Antarctic aerosol during atmospheric transport were described using selected sugars as source tracers. Monosaccharides (arabinose, fructose, galactose, glucose, mannose, ribose, xylose), disaccharides (sucrose, lactose, maltose, lactulose), alcohol-sugars (erythritol, mannitol, ribitol, sorbitol, xylitol, maltitol, galactitol) and anhydrosugars (levoglucosan, mannosan and galactosan) were measured in the Antarctic aerosol collected during four different sampling campaigns. For quantification, a sensitive high-pressure anion exchange chromatography was coupled with a single quadrupole mass spectrometer. The method was validated, showing good accuracy and low method quantification limits. This study describes the first determination of sugars in the Antarctic aerosol. The total mean concentration of sugars in the aerosol collected at the ;Mario Zucchelli; coastal station was 140 pg m-3; as for the aerosol collected over the Antarctic plateau during two consecutive sampling campaigns, the concentration amounted to 440 and 438 pg m-3. The study of particle-size distribution allowed us to identify the natural emission from spores or from sea-spray as the main sources of sugars in the coastal area. The enrichment of sugars in the fine fraction of the aerosol collected on the Antarctic plateau is due to the degradation of particles during long-range atmospheric transport. The composition of sugars in the coarse fraction was also investigated in the aerosol collected during the oceanographic cruise.

Application of computational fluid mechanics to atmospheric pollution problems

NASA Technical Reports Server (NTRS)

Hung, R. J.; Liaw, G. S.; Smith, R. E.

1986-01-01

One of the most noticeable effects of air pollution on the properties of the atmosphere is the reduction in visibility. This paper reports the results of investigations of the fluid dynamical and microphysical processes involved in the formation of advection fog on aerosols from combustion-related pollutants, as condensation nuclei. The effects of a polydisperse aerosol distribution, on the condensation/nucleation processes which cause the reduction in visibility are studied. This study demonstrates how computational fluid mechanics and heat transfer modeling can be applied to simulate the life cycle of the atmosphereic pollution problems.

Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

NASA Astrophysics Data System (ADS)

Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

2016-10-01

Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

Mesoscale modeling of smoke radiative feedback over the Sahel region

NASA Astrophysics Data System (ADS)

Yang, Z.; Wang, J.; Ichoku, C. M.; Ellison, L.; Zhang, F.; Yue, Y.

2013-12-01

This study employs satellite observations and a fully-coupled meteorology-chemistry-aerosol model, Weather Research and Forecasting model with Chemistry (WRF-Chem) to study the smoke radative feedback on surface energy budget, boundary layer processes, and atmospheric lapse rate in February 2008 over the Sahel region. The smoke emission inventories we use come from various sources, including but not limited to the Fire Locating and Modeling of Burning Emissions (FLAMBE) developed by NRL and the Fire Energetic and Emissions Research (FEER) developed by NASA GSFC. Model performance is evaluated using numerous satellite and ground-based datasets: MODIS true color images, ground-based Aerosol Optical Depth (AOD) measurements from AERONET, MODIS AOD retrievals, and Cloud-Aerosol Lidar data with Orthogonal Polarization (CALIOP) atmospheric backscattering and extinction products. Specification of smoke injection height of 650 m in WRF-Chem yields aerosol vertical profiles that are most consistent with CALIOP observations of aerosol layer height. Statistically, 5% of the CALIPSO valid measurements of aerosols in February 2008 show aerosol layers either above the clouds or between the clouds, reinforcing the importance of the aerosol vertical distribution for quantifying aerosol impact on climate in the Sahel region. The results further show that the smoke radiative feedbacks are sensitive to assumptions of black carbon and organic carbon ratio in the particle emission inventory. Also investigated is the smoke semi-direct effect as a function of cloud fraction.

Zonal Aerosol Direct and Indirect Radiative Forcing using Combined CALIOP, CERES, CloudSat, and CERES Data

NASA Astrophysics Data System (ADS)

Miller, W. F.; Kato, S.; Rose, F. G.; Sun-Mack, S.

2009-12-01

Under the NASA Energy and Water Cycle System (NEWS) program, cloud and aerosol properties derived from CALIPSO, CloudSat, and MODIS data then matched to the CERES footprint are used for irradiance profile computations. Irradiance profiles are included in the publicly available product, CCCM. In addition to the MODIS and CALIPSO generated aerosol, aerosol optical thickness is calculated over ocean by processing MODIS radiance through the Stowe-Ignatov algorithm. The CERES cloud mask and properties algorithm are use with MODIS radiance to provide additional cloud information to accompany the actively sensed data. The passively sensed data is the only input to the standard CERES radiative flux products. The combined information is used as input to the NASA Langley Fu-Liou radiative transfer model to determine vertical profiles and Top of Atmosphere shortwave and longwave flux for pristine, all-sky, and aerosol conditions for the special data product. In this study, the three sources of aerosol optical thickness will be compared directly and their influence on the calculated and measured TOA fluxes. Earlier studies indicate that the largest uncertainty in estimating direct aerosol forcing using aerosol optical thickness derived from passive sensors is caused by cloud contamination. With collocated CALIPSO data, we are able to estimate frequency of occurrence of cloud contamination, effect on the aerosol optical thickness and direct radiative effect estimates.

Dust and biological aerosols from the Sahara and Asia influence precipitation in the western U.S.

PubMed

Creamean, Jessie M; Suski, Kaitlyn J; Rosenfeld, Daniel; Cazorla, Alberto; DeMott, Paul J; Sullivan, Ryan C; White, Allen B; Ralph, F Martin; Minnis, Patrick; Comstock, Jennifer M; Tomlinson, Jason M; Prather, Kimberly A

2013-03-29

Winter storms in California's Sierra Nevada increase seasonal snowpack and provide critical water resources and hydropower for the state. Thus, the mechanisms influencing precipitation in this region have been the subject of research for decades. Previous studies suggest Asian dust enhances cloud ice and precipitation, whereas few studies consider biological aerosols as an important global source of ice nuclei (IN). Here, we show that dust and biological aerosols transported from as far as the Sahara were present in glaciated high-altitude clouds coincident with elevated IN concentrations and ice-induced precipitation. This study presents the first direct cloud and precipitation measurements showing that Saharan and Asian dust and biological aerosols probably serve as IN and play an important role in orographic precipitation processes over the western United States.

Vacuum FTIR Observation on the Dynamic Hygroscopicity of Aerosols under Pulsed Relative Humidity.

PubMed

Leng, Chun-Bo; Pang, Shu-Feng; Zhang, Yun; Cai, Chen; Liu, Yong; Zhang, Yun-Hong

2015-08-04

A novel approach based on a combination of a pulse RH controlling system and a rapid scan vacuum FTIR spectrometer (PRHCS-RSVFTIR) was utilized to investigate dynamic hygroscopicity of two atmospheric aerosols: ammonium sulfate ((NH4)2SO4) and magnesium sulfate (MgSO4). In this approach, rapid-scan infrared spectra of water vapor and aerosols were obtained to determine relative humidity (RH) in sample cell and hygroscopic property of aerosols with a subsecond time resolution. Heterogeneous nucleation rates of (NH4)2SO4 were, for the first time, measured under low RH conditions (<35% RH). In addition, studies of MgSO4 aerosols revealed that water mass transport may be limited by different processes depending on RH values (surface limited at 40% < RH < 52% and bulk phase limited at RH < 40%). Furthermore, we are also the first to report water diffusion constants in micron size MgSO4 aerosols at very low RH values. Our results have shown that the PRHCS-RSVFTIR is well-suited for determination of hygroscopicity of atmospheric aerosols and water transport and nucleation kinetics of liquid aerosols.

Aerosol-Cloud Interactions and Cloud Microphysical Properties in the Asir Region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Kucera, P. A.; Axisa, D.; Burger, R. P.; Li, R.; Collins, D. R.; Freney, E. J.; Buseck, P. R.

2009-12-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region, located adjacent to the Red Sea in the southwest region of Saudi Arabia. Ground measurements of aerosol size distributions, hygroscopic growth factors, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were observed in the Asir region in August 2009. The presentation will include a summary of the analysis and results with a focus on aerosol-cloud interactions and cloud microphysical properties observed during the convective season in the Asir region.

Process to make core-shell structured nanoparticles

DOEpatents

Luhrs, Claudia; Phillips, Jonathan; Richard, Monique N

2014-01-07

Disclosed is a process for making a composite material that contains core-shell structured nanoparticles. The process includes providing a precursor in the form of a powder a liquid and/or a vapor of a liquid that contains a core material and a shell material, and suspending the precursor in an aerosol gas to produce an aerosol containing the precursor. In addition, the process includes providing a plasma that has a hot zone and passing the aerosol through the hot zone of the plasma. As the aerosol passes through the hot zone of the plasma, at least part of the core material and at least part of the shell material in the aerosol is vaporized. Vapor that contains the core material and the shell material that has been vaporized is removed from the hot zone of the plasma and allowed to condense into core-shell structured nanoparticles.

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

DOE PAGES

Wang, Jian; Krejci, Radovan; Giangrande, Scott; ...

2016-10-24

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall

NASA Astrophysics Data System (ADS)

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M. J.; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E.; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L.; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A. F.; Springston, Stephen R.; Tomlinson, Jason M.; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N.; Kulmala, Markku; Machado, Luiz A. T.; Artaxo, Paulo; Andreae, Meinrat O.; Petäjä, Tuukka; Martin, Scot T.

2016-11-01

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall.

PubMed

Wang, Jian; Krejci, Radovan; Giangrande, Scott; Kuang, Chongai; Barbosa, Henrique M J; Brito, Joel; Carbone, Samara; Chi, Xuguang; Comstock, Jennifer; Ditas, Florian; Lavric, Jost; Manninen, Hanna E; Mei, Fan; Moran-Zuloaga, Daniel; Pöhlker, Christopher; Pöhlker, Mira L; Saturno, Jorge; Schmid, Beat; Souza, Rodrigo A F; Springston, Stephen R; Tomlinson, Jason M; Toto, Tami; Walter, David; Wimmer, Daniela; Smith, James N; Kulmala, Markku; Machado, Luiz A T; Artaxo, Paulo; Andreae, Meinrat O; Petäjä, Tuukka; Martin, Scot T

2016-11-17

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.

Advantages and Challenges in using Multi-Sensor Data for Studying Aerosols from Space

NASA Astrophysics Data System (ADS)

Leptoukh, Gregory

We are living now in the golden era of numerous sensors measuring aerosols from space, e.g., MODIS, MISR, MERIS, OMI, POLDER, etc. Data from multiple sensors provide a more complete coverage of physical phenomena than data from a single sensor. These sensors are rather different from each other, are sensitive to various parts of the atmosphere, use different aerosol models and treat surface differently when retrieving aerosols. However, they complement each other thus providing more information about spatial, vertical and temporal distribution of aerosols. In addition to differences in instrumentation, retrieval algorithms and calibration, there are quite substantial differences in processing algorithms from Level 0 up to Level 3 and 4. Some of these differences in processing steps, at times not well documented and not widely known by users, can lead to quite significant differences in final products. Without documenting all the steps leading to the final product, data users will not trust the data and/or may use data incorrectly. Data by themselves without quality assessment and provenance are not sufficient to make accurate scientific conclusions. In this paper we provide examples of striking differences between aerosol optical depth data from MODIS, MISR, and MERIS that can be attributed to differences in a certain threshold, aggregation methods, and the dataday definition. We talk about challenges in developing processing provenance. Also, we address issues of harmonization of data, quality and provenance that is needed to guide the multi-sensor data usage and avoid apples-to-oranges comparison and fusion.

Giant aerosol observations with cloud radar: methodology and effects

NASA Astrophysics Data System (ADS)

Guma Claramunt, Pilar; Madonna, Fabio; Amodeo, Aldo; Bauer-Pfundstein, Matthias; Papagiannopoulos, Nikolaos; Pappalardo, Gelsomina

2017-04-01

Giant aerosol particles can act as Giant Cloud Condensation Nuclei (GCCN), and determine the droplet concentration at the cloud formation, the clouds albedo and lifetime, and the precipitation formation. In addition, depending on their composition, they can also act as IN. It is not yet clear if they can also expedite rain processes. The main techniques used nowadays in measuring aerosols, which are lidar and sun photometer, cannot retrieve aerosol microphysical properties for particles bigger than a few microns, which means that they do not account for giant aerosols. Therefore, the distribution and impact in the atmosphere and climate of these particles is not well known and the aerosol transport models largely underestimate them. Recent studies have demonstrated that cloud radars are able to detect ultragiant volcanic aerosols also at a large distance from the source. In this study, an innovative methodology for the observation of giant aerosols using the millimeter wavelength radar has been developed and applied to 6 years of measurements carried out at CNR-IMAA Atmospheric Observatory (CIAO), in Potenza, South Italy, finding more than 40 giant aerosol events per year and a good agreement with the aerosol climatologic data. Besides, the effects of giant aerosols in the local and regional meteorology have been studied by correlating several atmospheric variables in the time period following the observation of giant particles. The meteorological situation has been assessed through the data classification into cases characterized by different pressure vertical velocities at the upper atmosphere (400 hPa), Giant aerosols are correlated to lower values of the Cloud Optical Depth (COD) in presence of stable or unstable atmospheric conditions while higher values are found for an intermediate stability. The giant aerosols effects on the Liquid Water Path (LWP) are closely linked to those in the Aerosol Optical Thickness (AOD). The highest increases in the LWP occurs together with the increases of AOD. Finally, the effects of giant aerosols on precipitation at a regional scale have been studied. The observation of giant aerosols can be correlated to an enhancement of the accumulated precipitation, which is quite relevant in the first 12 hours after their observation, as well as of the maximum rain rate in presence of the unstable atmospheric conditions. The increase in the maximum rain rate is instead more remarkable in correlation with stable atmospheric conditions and mainly during the first 6 hours after their observations.

Regional Simulations of Stratospheric Lofting of Smoke Plumes

NASA Astrophysics Data System (ADS)

Stenchikov, G. L.; Fromm, M.; Robock, A.

2006-12-01

The lifetime and spatial distribution of sooty aerosols from multiple fires that would cause major climate impact were debated in studies of climatic and environmental consequences of a nuclear war in the 1980s. The Kuwait oil fires in 1991 did not show a cumulative effect of multiple smoke plumes on large-scale circulation systems and smoke was mainly dispersed in the middle troposphere. However, recent observations show that smoke from large forest fires can be directly injected into the lower stratosphere by strong pyro-convective storms. Smoke plumes in the upper troposphere can be partially mixed into the lower stratosphere because of the same heating and lofting effect that was simulated in large-scale nuclear winter simulations with interactive aerosols. However nuclear winter simulations were conducted using climate models with grid spacing of more than 100 km, which do not account for the fine-scale dynamic processes. Therefore in this study we conduct fine-scale regional simulations of the aerosol plume using the Regional Atmospheric Modeling System (RAMS) mesoscale model which was modified to account for radiatively interactive tracers. To resolve fine-scale dynamic processes we use horizontal grid spacing of 25 km and 60 vertical layers, and initiate simulations with the NCEP reanalysis fields. We find that dense aerosol layers could be lofted from 1 to a few km per day, but this critically depends on the optical depth of aerosol layer, single scatter albedo, and how fast the plume is being diluted. Kuwaiti plumes from different small-area fires reached only 5-6 km altitude and were probably diffused and diluted in the lower and middle troposphere. A plume of 100 km spatial scale initially developed in the upper troposphere tends to penetrate into the stratosphere. Short-term cloud resolving simulations of such a plume show that aerosol heating intensifies small-scale motions that tend to mix smoke polluted air into the lower stratosphere. Regional simulations allow us to more accurately estimate the rate of lifting and spreading of aerosol clouds. But they do not reveal any dynamic processes that could prevent heating and lofting of absorbing aerosols.

Global Survey of Submicron Aerosol Acidity (pH)

NASA Astrophysics Data System (ADS)

Nault, B.; Day, D. A.; Campuzano Jost, P.; Hu, W.; Schroder, J. C.; Bian, H.; Chin, M.; Clegg, S. L.; Colarco, P. R.; Dibb, J. E.; Kim, M. J.; Kodros, J.; Marais, E. A.; Pierce, J. R.; Scheuer, E. M.; Wennberg, P. O.; Jimenez, J. L.

2017-12-01

Aerosol acidity (H+, often expressed as "pH" defined in various ways) is an important property that influences uptake and partitioning of gases, and homogeneous and surface aqueous reactions of key inorganic and organic compounds. As there is currently no rapid method to measure ambient aerosol acidity, a thermodynamic model, constrained by both inorganic aerosol species (e.g., NH4, NO3, SO4, Cl) and at least one inorganic gas (HNO3, NH3, or HCl), are currently understood to lead to the most reliable estimates of aerosol acidity. In this study, we calculated submicron (less than PM1) aerosol pH from the NASA ATom, "pole-to-pole," flights that covers both the Pacific and Atlantic ocean basins. The E-AIM thermodynamic model was used with measurements by an Aerodyne high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) of inorganic aerosol species, along with inorganic gas measurements from other mass spectrometers and ion chromatography. We compare the results with those for the NASA KORUS-AQ, SEAC4RS, DC3, and ARCTAS campaigns, as well as several ground-based campaigns and recently-published studies. This provides an opportunity to compare the aerosol acidity in urban, rural, and remote regions, by season, and between the boundary layer and free troposphere. In addition, we compare the submicron aerosol acidity from these various localities with results from global models, such as GEOS-Chem, in order to investigate the ability of the global models to simulate aerosol acidity, and the processes it affects, such as nitrate, ammonium, and MSA partitioning.

Retrieval of Absorbing Aerosols Above Clouds retrieval over the South East Atlantic Ocean from MSG/SEVIRI

NASA Astrophysics Data System (ADS)

Peers, F.; Haywood, J. M.; Francis, P. N.; Meyer, K.; Platnick, S. E.

2017-12-01

Over the South East Atlantic Ocean, biomass burning aerosols from Southern Africa are frequently observed above clouds during fire season. However, the quantification of their interactions with both radiations and clouds remains uncertain because of a lack of information on aerosol properties and on their interaction process. In the last decade, methods have been developed to retrieve aerosol optical properties above clouds from satellite measurements, especially over the South East Atlantic Ocean. Most of these methods have been applied to polar orbiting instruments which prevent the analysis of aerosols and clouds at a sub-daily scale. With its wide spatial coverage and its high temporal resolution, the geostationary instrument SEVIRI, on board the MSG platform, offers a unique opportunity to monitor aerosols in this region and to evaluate their impact on clouds and their radiative effects. In this study, we will investigate the possibility of retrieving simultaneously aerosol and cloud properties (i.e. aerosol and cloud optical thicknesses and cloud droplet effective radius) when aerosols are located above clouds. The retrieved properties will then be compared with the ones obtained from MODIS [Meyer et al., 2015] as well as observations from the CLARIFY-2017 field campaign.

Simulating the phase partitioning of NH3, HNO3, and HCl with size-resolved particles over northern Colorado in winter

EPA Science Inventory

Numerical modeling of inorganic aerosol processes is useful in air quality management, but comprehensive evaluation of modeled aerosol processes is rarely possible due to the lack of comprehensive datasets. During the Nitrogen, Aerosol Composition, and Halogens on a Tall Tower (N...

Interaction of Burning Metal Particles

NASA Technical Reports Server (NTRS)

Dreizin, Edward L.; Berman, Charles H.; Hoffmann, Vern K.

1999-01-01

Physical characteristics of the combustion of metal particle groups have been addressed in this research. The combustion behavior and interaction effects of multiple metal particles has been studied using a microgravity environment, which presents a unique opportunity to create an "aerosol" consisting of relatively large particles, i.e., 50-300 micrometer diameter. Combustion behavior of such an aerosol could be examined using methods adopted from well-developed single particle combustion research. The experiment included fluidizing relatively large (order of 100 micrometer diameter) uniform metal particles under microgravity and igniting such an "aerosol" using a hot wire igniter. The flame propagation and details of individual particle combustion and particle interaction have been studied using a high speed movie and video-imaging with cameras coupled with microscope lenses to resolve individual particles. Interference filters were used to separate characteristic metal and metal oxide radiation bands form the thermal black body radiation. Recorded flame images were digitized and employed to understand the processes occurring in the burning aerosol. The development of individual particle flames, merging or separation, and extinguishing as well as induced particle motion have been analyzed to identify the mechanisms governing these processes. Size distribution, morphology, and elemental compositions of combustion products were characterized and used to link the observed in this project aerosol combustion phenomena with the recently expanded mechanism of single metal particle combustion.

Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

NASA Astrophysics Data System (ADS)

Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

2017-06-01

Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

New Photosensitized Processes at Aerosol and Ocean Surfaces

NASA Astrophysics Data System (ADS)

Rossignol, S.; Aregahegn, K. Z.; Ciuraru, R.; Bernard, F.; Tinel, L.; Fine, L.; George, C.

2014-12-01

From a few years now, there is a growing body of evidence that photoinduced processes could be of great importance for the tropospheric chemistry. Here, we would like to present two additional outcomes of this new area of research, firstly the photosensitized direct VOC uptake by aerosols and, secondly, the photoinduced chemical formation of unsaturated VOC from marine microlayer proxy. It was recently shown that the chemistry of glyoxal toward ammonium ions into droplets and wet aerosols leads to the formation of light-absorbing compounds. Among them, we found that imidazole-2-carboxaldehyde (IC) acts as a photosensitizer and is able to initiate the growth of organic aerosols via the uptake of VOC, such as limonene. Given its potential importance, the mechanism of this photoinduced uptake was investigated thanks to aerosol flow tube experiments and UPLC-ESI-HRMS analysis. Results reveal hydrogen abstraction on the VOC molecule by the triplet state of IC leading to the VOC oxidation without any traditional oxidant. As well as aerosol, the sea-surface microlayer, known to be enriched in light-absorbing organics, is largely impacted by photochemical processes. Recent studies have pointed out for example the role of photosentitized processes in the loss of NO2 and ozone at water surfaces containing photoactive compounds such as chlorophyll. In order to go further, we worked from sea-surface microlayer proxy containing humic acids as photoactive material and organic acids as surfactants. Beside oxidation processes, we monitored by high resolution PTR-MS the release in the gas phase of unsaturated compounds, including C5 dienes (isoprene ?). A strong correlation between the measured surface tension and the C5 diene concentration in the gas phase was evidenced, clearly pointing toward an interfacial process. This contribution will highlight the similarities between both systems and will attempt to present a general chemical scheme for photosensitized chemistry at interfaces.

Influence of aqueous chemistry on the chemical composition of fog water and interstitial aerosol in Fresno

NASA Astrophysics Data System (ADS)

Kim, Hwajin; Ge, Xinlei; Collier, Sonya; Xu, Jianzhong; Sun, Yele; Wang, Youliang; Herckes, Pierre; Zhang, Qi

2015-04-01

A measurement study was conducted in the Central Valley (Fresno) of California in January 2010, during which radiation fog events were frequently observed. Fog plays important roles in atmospheric chemistry by scavenging aerosol particles and trace gases and serving as a medium for various aqueous-phase reactions. Understanding the effects of fog on the microphysical and chemical processing of aerosol particles requires detailed information on their chemical composition. In this study, we characterized the chemical composition of fog water and interstitial aerosol particles to study the effects of fog processing on aerosol properties. Fog water samples were collected during the 2010 Fresno campaigns with a Caltech Active Strand Cloud water Collector (CASCC) while interstitial submicron aerosols were characterized in real time with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a scanning Mobility Particle Sizer (SMPS). The fog water samples were later analyzed using the HR-ToF-AMS, ion chromatography, and a total carbon analyzer. The chemical composition and characteristics of interstitial particles during the fog events were compared to those of dissolved inorganic and organic matter in fog waters. Compared to interstitial aerosols, fog water is composed of a higher fraction of ammonium nitrate and oxygenated organics, due to aqueous formation of secondary aerosol species as well as enhanced gas-to-particle partitioning of water soluble species under water rich conditions. Sulfate is formed most efficiently in fog water although its contribution to total dissolved mass is relatively low. The HR-ToF-AMS mass spectra of organic matter in fog water (FOM) are very similar to that of oxygenated organic aerosols (OOA) derived from positive matrix factorization (PMF) of the HR-ToF-AMS spectra of ambient aerosol (r2 = 0.96), but FOM appears to contain a large fraction of acidic functional groups than OOA. FOM is also enriched of organic nitrogen compounds, with an average N/C ratio ~3.8 times that of OOA. Most strikingly is the enhancement of the CxHyN2+ family ions in FOM spectra, indicating the presence of imidazole compounds, which commonly result from the aqueous phase reactions of tropospheric aldehyde such as glyoxal, formaldehyde or acetaldehyde with amino compounds. The results of this study demonstrate that aqueous phase reactions in fog water lead to the formation of some oxidized and nitrogen-containing compounds. Details and the environmental implications of results will be discussed.

A study on the relationship between mass concentrations, chemistry and number size distribution of urban fine aerosols in Milan, Barcelona and London

NASA Astrophysics Data System (ADS)

Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R. M.; Tardivo, R.; Scarnato, B.; Gianelle, V.

2007-01-01

A physicochemical characterization of the urban fine aerosol (aerosol number size distribution, chemical composition and mass concentrations) in Milan, Barcelona and London is presented in this article. The objective is to obtain a comprehensive picture on the involvement of the microphysical processes of the aerosol dynamic in the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of particles >100 nm (which only accounts for <20% of the total number concentration N of fine aerosols) and do not correlate with the number of particles <100 nm ("ultrafine particles", which accounts for >80% of fine particles). Organic matter (OM) and black-carbon (BC) are the only aerosol components showing a significant correlation with ultrafine particles (attributed to vehicles emissions), whereas ammonium-nitrate, ammonium-sulphate and also OM and BC correlate with N>100(nm) (attributed to gas-to-particle transformation mechanisms and some primary emissions). Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100(nm) concentrations, exhibit correlated day-to-day variations which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the fact that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow enough to produce significant concentrations of N>100(nm). In contrast, because the low contribution of ultrafine particles to the fine aerosol mass concentrations, high "ultrafine particles N<100(nm) events" frequently occurs under low PM2.5 conditions. The data of this study point that vehicles emissions are strongly involved in this ultrafine particles aerosol pollution (for example, the "morning-rush-hours to nocturnal-background" concentrations ratio is 1.5-2.5 for "particles 10-100 nm" and <1.5 for both "particle >100 nm and PM2.5").

Influence of aerosols on surface reaching spectral irradiance and introduction to a new technique for estimating aerosol radiative forcing from spectral flux measurements

NASA Astrophysics Data System (ADS)

Rao, R. R.

2015-12-01

Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. In this study we look into the approach where ground based spectral radiation flux measurements along with an RT model is used to estimate radiative forcing. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and 3nm resolution for around 54 clear-sky days during which AOD range was around 0.1 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. All the measurements were made in the campus of Indian Institute of Science which is in the heart of Bangalore city. The primary study involved in understanding the sensitivity of spectral flux to change in the mass concentration of individual aerosol species (Optical properties of Aerosols and Clouds -OPAC classified aerosol species) using the SBDART RT model. This made us clearly distinguish the region of influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves an iterative process where the mixture of aerosol species are changed in OPAC model and RT model is run as long as the mixture which mimics the measured spectral flux within 2-3% deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model aerosol radiative forcing is estimated. The new method is limited to clear sky scenes and its accuracy to derive an optically equivalent aerosol mixture reduces when diffuse component of flux increases. Our analysis also showed that direct component of spectral flux is more sensitive to different aerosol species than total spectral flux which was also supported by our observed data.

Development studies towards an 11-year global gridded aerosol optical thickness reanalysis for climate and applied applications

NASA Astrophysics Data System (ADS)

Lynch, P.; Reid, J. S.; Westphal, D. L.; Zhang, J.; Hogan, T. F.; Hyer, E. J.; Curtis, C. A.; Hegg, D. A.; Shi, Y.; Campbell, J. R.; Rubin, J. I.; Sessions, W. R.; Turk, F. J.; Walker, A. L.

2015-12-01

While standalone satellite and model aerosol products see wide utilization, there is a significant need in numerous climate and applied applications for a fused product on a regular grid. Aerosol data assimilation is an operational reality at numerous centers, and like meteorological reanalyses, aerosol reanalyses will see significant use in the near future. Here we present a standardized 2003-2013 global 1° × 1° and 6 hourly modal aerosol optical thickness (AOT) reanalysis product. This dataset can be applied to basic and applied earth system science studies of significant aerosol events, aerosol impacts on numerical weather prediction, and electro-optical propagation and sensor performance, among other uses. This paper describes the science of how to develop and score an aerosol reanalysis product. This reanalysis utilizes a modified Navy Aerosol Analysis and Prediction System (NAAPS) at its core and assimilates quality controlled retrievals of AOT from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Multi-angle Imaging SpectroRadiometer (MISR) on Terra. The aerosol source functions, including dust and smoke, were regionally tuned to obtain the best match between the model fine and coarse mode AOTs and the Aerosol Robotic Network (AERONET) AOTs. Other model processes, including deposition, were tuned to minimize the AOT difference between the model and satellite AOT. Aerosol wet deposition in the tropics is driven with satellite retrieved precipitation, rather than the model field. The final reanalyzed fine and coarse mode AOT at 550 nm is shown to have good agreement with AERONET observations, with global mean root mean square error around 0.1 for both fine and coarse mode AOTs. This paper includes a discussion of issues particular to aerosol reanalyses that make them distinct from standard meteorological reanalyses, considerations for extending such a reanalysis outside of the NASA A-Train era, and examples of how the aerosol reanalysis can be applied or fused with other model or remote sensing products. Finally, the reanalysis is evaluated in comparison with other available studies of aerosol trends, and the implications of this comparison are discussed.

Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) Science Plan

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Jian; Dong, Xiquan; Wood, Robert

With their extensive coverage, low clouds greatly impact global climate. Presently, low clouds are poorly represented in global climate models (GCMs), and the response of low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The poor representations of low clouds in GCMs are in part due to inadequate observations of their microphysical and macrophysical structures, radiative effects, and the associated aerosol distribution and budget in regions where the aerosol impact is the greatest. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary-layer (MBL) clouds,more » whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. Boundary-layer aerosol in the ENA region is influenced by a variety of sources, leading to strong variations in cloud condensation nuclei (CCN) concentration and aerosol optical properties. Recently a permanent ENA site was established by the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility on Graciosa Island in the Azores, providing invaluable information on MBL aerosol and low clouds. At the same time, the vertical structures and horizontal variabilities of aerosol, trace gases, cloud, drizzle, and atmospheric thermodynamics are critically needed for understanding and quantifying the budget of MBL aerosol, the radiative properties, precipitation efficiency, and lifecycle of MBL clouds, and the cloud response to aerosol perturbations. Much of this data can be obtained only through aircraft-based measurements. In addition, the interconnected aerosol and cloud processes are best investigated by a study involving simultaneous in situ aerosol, cloud, and thermodynamics measurements. Furthermore, in situ measurements are also necessary for validating and improving ground-based retrieval algorithms at the ENA site. This project is motivated by the need for comprehensive in situ characterizations of boundary-layer structure, and associated vertical distributions and horizontal variabilities of low clouds and aerosol over the Azores. ARM Aerial Facility (AAF) Gulfstream-1 (G-1) aircraft will be deployed at the ENA site during two intensive operational periods (IOPs) of early summer (June to July) of 2017 and winter (January to February) of 2018, respectively. Deployments during both seasons allow for examination of key aerosol and cloud processes under a variety of representative meteorological and cloud conditions. The science themes for the deployments include: 1) Budget of MBL CCN and its seasonal variation; 2) Effects of aerosol on cloud and precipitation; 3) Cloud microphysical and macrophysical structures, and entrainment mixing; 4) Advancing retrievals of turbulence, cloud, and drizzle; and 5) Model evaluation and processes studies. A key advantage of the deployments is the strong synergy between the measurements onboard the G-1 and the routine measurements at the ENA site, including state-of-the-art profiling and scanning radars. The 3D cloud structures provided by the scanning radars will put the detailed in situ measurements into mesoscale and cloud lifecycle contexts. On the other hand, high quality in situ measurements will enable validation and improvements of ground-based retrieval algorithms at the ENA site, leading to high-quality and statistically robust data sets from the routine measurements. The deployments, combined with the routine measurements at the ENA site, will have a long lasting impact on the research and modeling of low clouds and aerosols in the remote marine environment.« less

Dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls in fine aerosols over central Alaska: Implications for sources and atmospheric processes

NASA Astrophysics Data System (ADS)

Deshmukh, Dhananjay K.; Mozammel Haque, Md.; Kawamura, Kimitaka; Kim, Yongwon

2018-04-01

The presence of water-soluble dicarboxylic acids in atmospheric aerosols has a significant influence on the regional radiative forcing through direct aerosol effect and cloud formation process. Fine aerosol (PM2.5) samples collected in central Alaska (Fairbanks: 64.51°N and 147.51°W) during summer of 2009 were measured for water-soluble diacids (C2-C12), oxoacids (C2-C9) and α-dicarbonyls (C2-C3) as well as elemental carbon (EC), organic carbon (OC) and water-soluble OC (WSOC) to assess their sources and formation processes. We found the predominance of oxalic acid (C2) followed by malonic (C3) and succinic acid (C4) in Alaskan aerosols. Higher C3/C4 diacid ratios (ave. 1.2) in Alaskan aerosols than those reported for fresh aerosols emitted from fossil fuel combustion (ave. 0.35) and biomass burning (0.51-0.66) suggest that organic aerosols in central Alaska were photochemically processed. The relatively high correlations of major diacids and related compounds with levoglucosan (r = 0.80-0.99) than those with 2-methylglyceric acid (r = 0.59-0.98) suggest that they were significantly produced from biomass burning emission. Strong correlations of C2 with normal-chain saturated diacids (C3-C9: r = 0.80-0.98), glyoxylic acid (ωC2: r = 0.95) and methylglyoxal (MeGly: r = 0.88), together with strong correlations of solar radiation with ratio of C2 to C2-C12 diacids (r = 0.83), ωC2 (r = 0.80) and MeGly (r = 0.82) suggest that oxalic acid in PM2.5 aerosol was produced by the photooxidation of higher homologous diacids, glyoxylic acid and methylglyoxal in the atmosphere of central Alaska. These results reveal that photochemical processing of organic precursors mainly produced from biomass burning control the water-soluble organic chemical composition of fine aerosols in central Alaska.

Characterization of ice nucleating particles during continuous springtime measurements in Prudhoe Bay: an Arctic oilfield location

NASA Astrophysics Data System (ADS)

Creamean, J.; Spada, N. J.; Kirpes, R.; Pratt, K.

2017-12-01

Aerosols that serve as ice nucleating particles (INPs) have the potential to modulate cloud microphysical properties. INPs can thus subsequently impact cloud radiative forcing in addition to modification of precipitation formation processes. In regions such as the Arctic, aerosol-cloud interactions are severely understudied yet have significant implications for surface radiation reaching the sea ice and snow surfaces. Further, uncertainties in model representations of heterogeneous ice nucleation are a significant hindrance to simulating Arctic mixed-phase cloud processes. Characterizing a combination of aerosol chemical, physical, and ice nucleating properties is pertinent to evaluating of the role of aerosols in altering Arctic cloud microphysics. We present preliminary results from an aerosol sampling campaign called INPOP (Ice Nucleating Particles at Oliktok Point), which took place at a U.S. Department of Energy's Atmospheric Radiation Measurement (DOE ARM) facility on the North Slope of Alaska. Three time- and size-resolved aerosol samplers were deployed from 1 Mar to 31 May 2017 and were co-located with routine measurements of aerosol number, size, chemical, and radiative property measurements conducted by DOE ARM at their Aerosol Observing System (AOS). Offline analysis of samples collected at a daily time resolution included composition and morphology via single-particle analysis and drop freezing measurements for INP concentrations, while analysis of 12-hourly samples included mass, optical, and elemental composition. We deliberate the possible influences on the aerosol and INP population from the Prudhoe Bay oilfield resource extraction and daily operations in addition to what may be local background or long-range transported aerosol. To our knowledge our results represent some of the first INP characterization measurements in an Arctic oilfield location and can be used as a benchmark for future INP characterization studies in Arctic locations impacted by local resource extraction pollution. Ultimately, these results can be used to evaluate the impacts of oil exploration activities on Arctic cloud aerosol composition and possible linkages to Arctic cloud ice formation.

Detailed Chemical Characterization of Unresolved Complex Mixtures (UCM) inAtmospheric Organics: Insights into Emission Sources, Atmospheric Processing andSecondary Organic Aerosol Formation

EPA Science Inventory

Recent studies suggest that semivolatile organic compounds (SVOCs) are important precursors to secondary organic aerosol (SOA) in urban atmospheres. However, knowledge of the chemical composition of SVOCs is limited by current analytical techniques, which are typically unable to...

Stratospheric aerosols and precursor gases

NASA Technical Reports Server (NTRS)

1982-01-01

Measurements were made of the aerosol size, height and geographical distribution, their composition and optical properties, and their temporal variation with season and following large volcanic eruptions. Sulfur-bearing gases were measured in situ in the stratosphere, and studied of the chemical and physical processes which control gas-to-particle conversion were carried out in the laboratory.

Aerosol composition and its sources at the King Sejong Station, Antarctic peninsula

NASA Astrophysics Data System (ADS)

Mishra, Vinit K.; Kim, Ki-Hyun; Hong, Sungmin; Lee, Khanghyun

The annual cycles of major metals and ions in suspended particulate matters (SPM) have been investigated at a costal site of the Antarctic Peninsula in order to elucidate temporal variations as well as major source processes responsible for their formation. The measurements had been performed from January 2000 to December 2001 at the Korean Antarctic research station, 'King Sejong' (62°13' S, 58°47' W). The observed time series of important aerosol components showed clear seasonal variation patterns, while the mean elemental concentrations (e.g., 1875 (Al), 10.3 (Ba), 0.3 (Bi), 1.3 (Cd), 1.7 pg m -3 (Co)) were generally compatible with those reported previously. The presence of high EF values with respect to both mean crustal and seawater composition (such as Bi, Cd, Cr, Cu, Ni, V, and Zn), however, suggests a possibly important role of anthropogenic processes in this remote site. In contrast, the concentrations of ionic species were not clearly distinguishable from those of other Antarctic sites; but the consideration of ionic mass balance between cations and anions pointed out the uniqueness of their source/sink processes in the study area. The major source processes of those aerosol components were also investigated using a series of statistical analyses. The overall results of our study indicated the dominance of several processes (or sources) such as sea-salt emission, secondary aerosol formation, and anthropogenic pollution from both local and distant sources.

Atmospheric System Research Marine Low Clouds Workshop Report, January 27-29,2016

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jensen, M.; Wang, J.; Wood, R.

Marine low clouds are a major determinant of the Earth?s albedo and are a major source of uncertainty in how the climate responds to changing greenhouse gas levels and anthropogenic aerosol. Marine low clouds are particularly difficult to simulate accurately in climate models, and their remote locations present a significant observational challenge. A complex set of interacting controlling processes determine the coverage, condensate loading, and microphysical and radiative properties of marine low clouds. Marine low clouds are sensitive to atmospheric aerosol in several ways. Interactions at microphysical scales involve changes in the concentration of cloud droplets and precipitation, which inducemore » cloud dynamical impacts including changes in entrainment and mesoscale organization. Marine low clouds are also impacted by atmospheric heating changes due to absorbing aerosols. The response of marine low clouds to aerosol perturbations depends strongly upon the unperturbed aerosol-cloud state, which necessitates greater understanding of processes controlling the budget of aerosol in the marine boundary layer. Entrainment and precipitation mediate the response of low clouds to aerosols but these processes also play leading roles in controlling the aerosol budget. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Climate Research Facility and Atmospheric System Research (ASR) program are making major recent investments in observational data sets from fixed and mobile sites dominated by marine low clouds. This report provides specific action items for how these measurements can be used together with process modeling to make progress on understanding and quantifying the key cloud and aerosol controlling processes in the next 5-10 years. Measurements of aerosol composition and its variation with particle size are needed to advance a quantitative, process-level understanding of marine boundary-layer aerosol budget. Quantitative precipitation estimates that combine radar and lidar measurements are becoming available, and these could be used to test process models, quantify precipitation responses to aerosol, and constrain climate models. Models and observations can be used to constrain how clouds respond dynamically to changing precipitation. New measurements of turbulence from ground-based remote sensing could be used to attempt to relate entrainment to the vertical and horizontal structure of turbulence in the boundary layer. Cloud-top entrainment plays a major role in modulating how low clouds respond to both aerosols and to greenhouse gases, so investment in promising new observational estimates would be beneficial. Precipitation formation and radiative cooling both help marine low clouds to organize on the mesoscale. More work is needed to develop metrics to characterize mesoscale organization, to elucidate mechanisms that determine the type and spatial scale of mesoscale cellular convection, and to understand the role of mesoscale structures in the stratocumulus-to-cumulus transition.« less

Global aerosol effects on convective clouds

NASA Astrophysics Data System (ADS)

Wagner, Till; Stier, Philip

2013-04-01

Atmospheric aerosols affect cloud properties, and thereby the radiation balance of the planet and the water cycle. The influence of aerosols on clouds is dominated by increase of cloud droplet and ice crystal numbers (CDNC/ICNC) due to enhanced aerosols acting as cloud condensation and ice nuclei. In deep convective clouds this increase in CDNC/ICNC is hypothesised to increase precipitation because of cloud invigoration through enhanced freezing and associated increased latent heat release caused by delayed warm rain formation. Satellite studies robustly show an increase of cloud top height (CTH) and precipitation with increasing aerosol optical depth (AOD, as proxy for aerosol amount). To represent aerosol effects and study their influence on convective clouds in the global climate aerosol model ECHAM-HAM, we substitute the standard convection parameterisation, which uses one mean convective cloud for each grid column, with the convective cloud field model (CCFM), which simulates a spectrum of convective clouds, each with distinct values of radius, mixing ratios, vertical velocity, height and en/detrainment. Aerosol activation and droplet nucleation in convective updrafts at cloud base is the primary driver for microphysical aerosol effects. To produce realistic estimates for vertical velocity at cloud base we use an entraining dry parcel sub cloud model which is triggered by perturbations of sensible and latent heat at the surface. Aerosol activation at cloud base is modelled with a mechanistic, Köhler theory based, scheme, which couples the aerosols to the convective microphysics. Comparison of relationships between CTH and AOD, and precipitation and AOD produced by this novel model and satellite based estimates show general agreement. Through model experiments and analysis of the model cloud processes we are able to investigate the main drivers for the relationship between CTH / precipitation and AOD.

Aerosol properties and their impacts on surface CCN at the ARM Southern Great Plains site during the 2011 Midlatitude Continental Convective Clouds Experiment

NASA Astrophysics Data System (ADS)

Logan, Timothy; Dong, Xiquan; Xi, Baike

2018-02-01

Aerosol particles are of particular importance because of their impacts on cloud development and precipitation processes over land and ocean. Aerosol properties as well as meteorological observations from the Department of Energy Atmospheric Radiation Measurement (ARM) platform situated in the Southern Great Plains (SGP) are utilized in this study to illustrate the dependence of continental cloud condensation nuclei (CCN) number concentration ( N CCN) on aerosol type and transport pathways. ARM-SGP observations from the 2011 Midlatitude Continental Convective Clouds Experiment field campaign are presented in this study and compared with our previous work during the 2009-10 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer field campaign over the current ARM Eastern North Atlantic site. Northerly winds over the SGP reflect clean, continental conditions with aerosol scattering coefficient ( σ sp) values less than 20 Mm-1 and N CCN values less than 100 cm-3. However, southerly winds over the SGP are responsible for the observed moderate to high correlation ( R) among aerosol loading ( σ sp < 60 Mm-1) and N CCN, carbonaceous chemical species (biomass burning smoke), and precipitable water vapor. This suggests a common transport mechanism for smoke aerosols and moisture via the Gulf of Mexico, indicating a strong dependence on air mass type. NASA MERRA-2 reanalysis aerosol and chemical data are moderately to highly correlated with surface ARM-SGP data, suggesting that this facility can represent surface aerosol conditions in the SGP, especially during strong aerosol loading events that transport via the Gulf of Mexico. Future long-term investigations will help to understand the seasonal influences of air masses on aerosol, CCN, and cloud properties over land in comparison to over ocean.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Jian; Krejci, Radovan; Giangrande, Scott

The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- andmore » ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. Lastly, this rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.« less

Observations of Dust Using the NASA Geoscience Laser Altimeter System (GLAS): New New Measurements of Aerosol Vertical Distribution From Space

NASA Technical Reports Server (NTRS)

Welton, Ellsworth; Spinhirne, James D.; Palm, Steven P.; Hlavka, Dennis; Hart, William

2003-01-01

On January 12, 2003 NASA launched the first satellite-based lidar, the Geoscience Laser -Altimeter System (GLAS), onboard the ICESat spacecraft. The GLAS atmospheric measurements introduce a fundamentally new and important tool for understanding the atmosphere and climate. In the past, aerosols have only been studied from space using images gathered by passive sensors. Analysis of this passive data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth's climate. However, these images do not show the aerosol's vertical distribution. As a result, a key piece of information has been missing. The measurements now obtained by GLAS will provide information on the vertical distribution of aerosols and clouds, and improve our ability to study their transport processes and aerosol-cloud interactions. Here we show an overview of GLAS, provide an update of its current status, and present initial observations of dust profiles. In particular, a strategy of characterizing the height profile of dust plumes over source regions will be presented.

Principles in Remote Sensing of Aerosol from MODIS Over Land and Ocean

NASA Technical Reports Server (NTRS)

Remer, L. A.; Kaufman, Y. J.; Tanre, D.; Chu, D. A.

1999-01-01

The well-calibrated spectral radiances measured by MODIS will be processed to retrieve daily aerosol properties that include optical thickness and mass loading over land and optical thickness, the mean particle size of the dominant mode and the ratio between aerosol modes over ocean. In addition, after launch, aerosol single scattering albedo will be calculated as an experimental product. The retrieval process over land is based on a dark target method that identifies appropriate targets in the mid-IR channels and uses an empirical relationship found between the mid-ER and the visible channels to estimate surface reflectance in the visible from the mid-HZ reflectance measured by satellite. The method employs new aerosol models for industrial, smoke and dust aerosol. The process for retrieving aerosol over the ocean makes use of the wide spectral band from 0.55-2.13 microns and a look-up table constructed from combinations of five accumulation modes and five coarse modes. Both the over land and over ocean algorithms have been validated with satellite and airborne radiance measurements. We estimate that MODIS will be able to measure aerosol optical thickness (t) to within 0.05 +/- 0.2t over land and to within 0.05 +/- 0.05t over ocean. Much of the earth's surface is located far from aerosol sources and experience very low aerosol optical thickness. Will the accuracy expected from MODIS retrievals be sufficient to measure the global aerosol direct and indirect forcing? We are attempting to answer this question using global model results and cloud climatology.

pH Variance in Aerosols Undergoing Liquid-Liquid Phase Separation

NASA Astrophysics Data System (ADS)

Eddingsaas, N. C.; Dallemagne, M.; Huang, X.

2014-12-01

The water content of aerosols is largely governed by relative humidity (RH). As the relative humidity decreases, and thus the water content of aerosols, a number of processes occur including the shrinking of aerosols, the increase in concentration of components, and potentially the formation of liquid liquid phase separation (llps) due to the salting out of inorganic salts. The most ubiquitous salt in atmospheric aerosols is ammonium sulfate which results in many aerosols to be at least mildly acidic. However, during llps, the pH of the different phases is not necessarily the same. Many reactions that take place within atmospheric aerosols are acid catalyzed so a better understanding of the pH of the individual phases as well as the interface between the phases is important to understanding aerosol processing and aging. Through the use of pH sensitive dyes and confocal microscopy we have directly measured the pH of micron sized model aerosols during high RH where the aerosols are in a single phase, at intermediate while the aerosols are in llps, and low RH where the aerosols consist of one liquid phase and one solid phase. We will discuss the variation in RH during these different phase states in the presence and absence of excess sulfuric acid. We will also discuss how this variation in pH affects aging of aerosols.

Effects of aerosol formulation to amino acids and fatty acids contents in Haruan extract.

PubMed

Febriyenti; Bai-Baie, Saringat Bin; Laila, Lia

2012-01-01

Haruan (Channa striatus) extract was formulated to aerosol for wound and burn treatment. Haruan extract is containing amino acids and fatty acids that important for wound healing process. The purpose of this study is to observe the effect of formulation and other excipients in the formula to amino acids and fatty acids content in Haruan extract before and after formulated into aerosol. Precolumn derivatization with 6-aminoquinolyl-N-hydroxysuccinimidyl carbamate (AQC) method is used for amino acids analysis. Fatty acids in Haruan extract were esterified using transesterification method to form FAMEs before analyzed using GC. Boron trifluoride-methanol reagent is used for transesterification. Tyrosine and methionine concentrations were different after formulated. The concentrations were decrease. There are six fatty acids have amount that significantly different after formulated into concentrate and aerosol. Contents of these fatty acids were increase. Generally, fatty acids which had content increased after formulated were the long-chain fatty acids. This might be happen because of chain extension process. Saponification and decarboxylation would give the chain extended product. Therefore contents of long-chain fatty acids were increase. Generally, the aerosol formulation did not affect the amino acids concentrations in Haruan extract while some long-chain fatty acids concentrations were increase after formulated into concentrate and aerosol.

Aerosols implicated as a prime driver of twentieth-century North Atlantic climate variability.

PubMed

Booth, Ben B B; Dunstone, Nick J; Halloran, Paul R; Andrews, Timothy; Bellouin, Nicolas

2012-04-04

Systematic climate shifts have been linked to multidecadal variability in observed sea surface temperatures in the North Atlantic Ocean. These links are extensive, influencing a range of climate processes such as hurricane activity and African Sahel and Amazonian droughts. The variability is distinct from historical global-mean temperature changes and is commonly attributed to natural ocean oscillations. A number of studies have provided evidence that aerosols can influence long-term changes in sea surface temperatures, but climate models have so far failed to reproduce these interactions and the role of aerosols in decadal variability remains unclear. Here we use a state-of-the-art Earth system climate model to show that aerosol emissions and periods of volcanic activity explain 76 per cent of the simulated multidecadal variance in detrended 1860-2005 North Atlantic sea surface temperatures. After 1950, simulated variability is within observational estimates; our estimates for 1910-1940 capture twice the warming of previous generation models but do not explain the entire observed trend. Other processes, such as ocean circulation, may also have contributed to variability in the early twentieth century. Mechanistically, we find that inclusion of aerosol-cloud microphysical effects, which were included in few previous multimodel ensembles, dominates the magnitude (80 per cent) and the spatial pattern of the total surface aerosol forcing in the North Atlantic. Our findings suggest that anthropogenic aerosol emissions influenced a range of societally important historical climate events such as peaks in hurricane activity and Sahel drought. Decadal-scale model predictions of regional Atlantic climate will probably be improved by incorporating aerosol-cloud microphysical interactions and estimates of future concentrations of aerosols, emissions of which are directly addressable by policy actions.

A Novel Tool for Simulating Aerosol-cloud Interactions with a Sectional Model Implemented to a Large-Eddy Simulator

NASA Astrophysics Data System (ADS)

Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Maalick, Z.; Korhonen, H.; Liqing, H.

2015-12-01

A new cloud-resolving model setup for studying aerosol-cloud interactions, with a special emphasis on partitioning and wet deposition of semi-volatile aerosol species, is presented. The model is based on modified versions of two well-established model components: the Large-Eddy Simulator (LES) UCLALES, and the sectional aerosol model SALSA, previously employed in the ECHAM climate model family. Implementation of the UCLALES-SALSA is described in detail. As the basis for this work, SALSA has been extended to include a sectional representation of the size distributions of cloud droplets and precipitation. Microphysical processes operating on clouds and precipitation have also been added. Given our main motivation, the cloud droplet size bins are defined according to the dry particle diameter. The droplet wet diameter is solved dynamically through condensation equations, but represents an average droplet diameter inside each size bin. This approach allows for accurate tracking of the aerosol properties inside clouds, but minimizes the computational cost. Since the actual cloud droplet diameter is not fully resolved inside the size bins, processes such as precipitation formation rely on parameterizations. For realistic growth of drizzle drops to rain, which is critical for the aerosol wet deposition, the precipitation size bins are defined according to the actual drop size. With these additions, the implementation of the SALSA model replaces most of the microphysical and thermodynamical components within the LES. The cloud properties and aerosol-cloud interactions simulated by the model are analysed and evaluated against detailed cloud microphysical boxmodel results and in-situ aerosol-cloud interaction observations from the Puijo measurement station in Kuopio, Finland. The ability of the model to reproduce the impacts of wet deposition on the aerosol population is demonstrated.

Electronic cigarette solutions and resultant aerosol profiles.

PubMed

Herrington, Jason S; Myers, Colton

2015-10-30

Electronic cigarettes (e-cigarettes) are growing in popularity exponentially. Despite their ever-growing acceptance, their aerosol has not been fully characterized. The current study focused on evaluating e-cigarette solutions and their resultant aerosol for potential differences. A simple sampling device was developed to draw e-cigarette aerosol into a multi-sorbent thermal desorption (TD) tube, which was then thermally extracted and analyzed via a gas chromatography (GC) mass spectrometry (GC-MS) method. This novel application provided detectable levels of over one hundred fifteen volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) from a single 40mL puff. The aerosol profiles from four commercially available e-cigarettes were compared to their respective solution profiles with the same GC-MS method. Solution profiles produced upwards of sixty four unidentified and identified (some only tentatively) constituents and aerosol profiles produced upwards of eighty two compounds. Results demonstrated distinct analyte profiles between liquid and aerosol samples. Most notably, formaldehyde, acetaldehyde, acrolein, and siloxanes were found in the aerosol profiles; however, these compounds were never present in the solutions. These results implicate the aerosolization process in the formation of compounds not found in solutions; have potential implications for human health; and stress the need for an emphasis on electronic cigarette aerosol testing. Copyright © 2015 The Authors. Published by Elsevier B.V. All rights reserved.

Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

DOE PAGES

Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.; ...

2016-09-09

During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmosphericmore » aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O:C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ~50 % RH in the sampling inlets. Furthermore, while the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.« less

Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.

During the summer 2013 Southern Aerosol and Oxidant Study (SOAS) field campaign in a rural site in the southeastern United States, the effect of hygroscopicity and composition on the phase state of atmospheric aerosol particles dominated by the organic fraction was studied. The analysis is based on hygroscopicity measurements by a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA), physical phase state investigations by an Aerosol Bounce Instrument (ABI) and composition measurements using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). To study the effect of atmospheric aging on these properties, an OH-radical oxidation flow reactor (OFR) was used to simulate longer atmosphericmore » aging times of up to 3 weeks. Hygroscopicity and bounce behavior of the particles had a clear relationship showing higher bounce at elevated relative humidity (RH) values for less hygroscopic particles, which agrees well with earlier laboratory studies. Additional OH oxidation of the aerosol particles in the OFR increased the O:C and the hygroscopicity resulting in liquefying of the particles at lower RH values. At the highest OH exposures, the inorganic fraction starts to dominate the bounce process due to production of inorganics and concurrent loss of organics in the OFR. Our results indicate that at typical ambient RH and temperature, organic-dominated particles stay mostly liquid in the atmospheric conditions in the southeastern US, but they often turn semisolid when dried below ~50 % RH in the sampling inlets. Furthermore, while the liquid phase state suggests solution behavior and equilibrium partitioning for the SOA particles in ambient air, the possible phase change in the drying process highlights the importance of thoroughly considered sampling techniques of SOA particles.« less

Advancing Littoral Zone Aerosol Prediction via Holistic Studies in Regime-Dependent Flows: August 3-9, 2016 Middle East Dust Event

NASA Astrophysics Data System (ADS)

Solbrig, J. E.; Miller, S. D.; van den Heever, S. C.; Kreidenweis, S. M.; Oo, M. M.; Zupanski, M.; Zhang, J.; Wang, J.; Holz, R.; Albers, S. C.; Grasso, L. D.; Kliewer, A.; Bukowski, J.; Park, J.; Saleeby, S. M.; Wu, T. C.

2017-12-01

Coastal regions represent a complex environment for meteorological processes, their effect on aerosol distributions, and the resulting impacts of those aerosols. These regions are rife with discontinuities that make dynamical processes difficult to predict and confound optical retrieval algorithms with highly variable and poorly characterized backgrounds. Local dynamics can be complicated by interactions between maritime and continental airmasses and the presence of coastal terrain. Additionally, coastal shallow water and high-turbidity produce backgrounds with high water leaving radiance which biases results from remote sensing retrievals. Here we present the highlights of the first two years of work from a Multi-disciplinary University Research Initiative entitled Holistic Analysis of Aerosol in Littoral Environments (HAALE-MURI) with specific focus on a dust event that occurred during the period of August 3-9 2016. During this period, two large dust plumes were observed advecting across the Arabian Peninsula. The first, embedded in a dry airmass, moved across the peninsula from north-west to south-east. This plume eventually stalls as it encounters a moist airmass, likely driven by the sea breeze. Embedded in the moist airmass is a second dust plume lofted from Oman, which then advects northwards over the Persian Gulf. This case presents significant challenges for forecasting, remote sensing, and data assimilation due to a complex meteorological environment and variable coastal bright-water backgrounds. The project team, who endeavor to advance our fundamental understanding of the factors that govern aerosol distribution, optical properties, and microphysical properties in the coastal regions, have focused on this case as our first in-depth case study. We demonstrate new retrieval techniques during both day and night including retrievals over bright coastal waters, a novel approach to in-line data assimilation of aerosol properties including AOT, and the results of model sensitivity studies. We take a holistic approach to better understanding aerosol processes in a coupled system as opposed to stand-alone analyses that fail to account for the myriad of covariances that exist in any real-world scenario.

Two-Column Aerosol Project (TCAP) Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berg, Larry K

This study included the deployment of the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Mobile Facility (AMF), ARM Mobile Aerosol Observing System (MAOS) and the ARM Aerial Facility (AAF). The study was a collaborative effort involving scientists from DOE national laboratories, NOAA, NASA, and universities. The AAF and MAOS were deployed for two approximately month-long Intensive Operational Periods (IOPs) conducted in June 2012 and February 2013. Seasonal differences in the aerosol chemical and optical properties observed using the AMF, AAF, and MAOS are presented in this report. The total mass loading of aerosol is found tomore » be much greater in the summer than in the winter, with the difference associated with greater amounts of organic aerosol. The mass fraction of organic aerosol is much reduced in the winter, when sulfate is the dominant aerosol type. Surprisingly, very little sea-salt aerosol was observed in the summer. In contrast, much more sea salt aerosol was observed in the winter. The mass loading of black carbon is nearly the same in both seasons. These differences lead to a relative increase in the aerosol light absorption in the winter and an associated decrease in observed single-scattering albedo. Measurements of aerosol mixing state were made using a single-particle mass spectrometer, which showed that the majority of the summertime aerosol consisted of organic compounds mixed with various amounts of sulfate. A number of other findings are also summarized in the report, including: impact of aerosol layers aloft on the column aerosol optical depth; documentation of the aerosol properties at the AMF; differences in the aerosol properties associated with both columns, which are not systematic but reflect the complicated meteorological and chemical processes that impact aerosol as it is advected away from North America; and new instruments and data-processing techniques for measuring both aerosol and cloud properties that were deployed for the first time during the TCAP. Key lessons learned during TCAP include the need for closer coordination between the AMF, MAOS, and the AAF so that all AMF instruments can be online and functioning during the AAF IOPs. Based on experiences from TCAP, it is also important for instrument mentors, or other relevant individuals, to review data on a regular basis to ensure that data quality remains high during the entire deployment. TCAP was marked by two important meteorological events including the passage of Hurricane Sandy at the end of October 2012 and the occurrence of one of the largest New England blizzards in recorded history. During Sandy the AMF received some, generally minor, damage and was largely functional a short time after the storm. The blizzard led to extensive power outages on Cape Cod and a multi-day interruption of measurements by the AMF, MAOS, and AAF. In each case, however, the ARM Facilities were returned to service and functioning as soon as was reasonably possible.« less

Weathering of Olivine during Interaction of Sulfate Aerosols with Mars Soil under Current Climate Conditions

NASA Astrophysics Data System (ADS)

Niles, P. B.; Golden, D. C.; Michalski, J. R.; Ming, D. W.

2017-12-01

Sulfur concentrations in the Mars soils are elevated above 1 wt% in nearly every location visited by landed spacecraft. This observation was first made by the Viking landers, and has been confirmed by subsequent missions. The wide distribution of sulfur in martian soils has been attributed to volcanic degassing, formation of sulfate aerosols, and later incorporation into martian soils during gravitational sedimentation. However, later discoveries of more concentrated sulfur bearing sediments by the Opportunity rover has led some to believe that sulfates may instead be a product of evaporation and aeolian redistribution. One question that has not been addressed is whether the modern surface conditions are too cold for weathering of volcanic materials by sulfate aerosols. We suggest here that mixtures of atmospheric aerosols, ice, and dust have the potential for creating small films of cryo-concentrated acidic solutions that may represent an important unexamined environment for understanding weathering processes on Mars. Laboratory experiments were conducted to simulate weathering of olivine under Mars-like conditions. The weathering rates measured in this study suggest that fine grained olivine on Mars would weather into sulfate minerals in short time periods if they are exposed to H2SO4 aerosols at temperatures at or above -40°C. In this system, the strength of the acidic solution is maximized through eutectic freezing in an environment where the silicate minerals are extremely fine grained and have high surface areas. This provides an ideal environment for olivine weathering despite the very low temperatures. The likelihood of substantial sulfur-rich volcanism on Mars and creation of abundant sulfate aerosols suggests that this process would have been important during formation of martian soils and sediments. Future work modeling sulfur release rates during volcanic eruptions and aerosol distribution over the surface will help understand how well this process could concentrate sulfate minerals in nearby surface materials or whether this process would simply result in widespread globally distributed sulfur materials.

Modeling the feedback between aerosol and boundary layer processes: a case study in Beijing, China.

PubMed

Miao, Yucong; Liu, Shuhua; Zheng, Yijia; Wang, Shu

2016-02-01

Rapid development has led to frequent haze in Beijing. With mountains and sea surrounding Beijing, the pollution is found to be influenced by the mountain-plain breeze and sea-land breeze in complex ways. Meanwhile, the presence of aerosols may affect the surface energy balance and impact these boundary layer (BL) processes. The effects of BL processes on aerosol pollution and the feedback between aerosol and BL processes are not yet clearly understood. Thus, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to investigate the possible effects and feedbacks during a haze episode on 23 September 2011. Influenced by the onshore prevailing wind, sea-breeze, and upslope breeze, about 45% of surface particulate matter (PM)2.5 in Beijing are found to be contributed by its neighbor cities through regional transport. In the afternoon, the development of upslope breeze suppresses the growth of BL in Beijing by imposing a relatively low thermal stable layer above the BL, which exacerbates the pollution. Two kinds of feedback during the daytime are revealed as follows: (1) as the aerosols absorb and scatter the solar radiation, the surface net radiation and sensible heat flux are decreased, while BL temperature is increased, resulting in a more stable and shallower BL, which leads to a higher surface PM2.5 concentration in the morning and (2) in the afternoon, as the presence of aerosols increases the BL temperature over plains, the upslope breeze is weakened, and the boundary layer height (BLH) over Beijing is heightened, resulting in the decrease of the surface PM2.5 concentration there.

Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

NASA Astrophysics Data System (ADS)

Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

2015-01-01

To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic aerosols (BA), for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2) and malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment, except for ω-oxooctanoic acid (ωC8) that showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids dominates their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

Laboratory photochemical processing of aqueous aerosols: formation and degradation of dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls

NASA Astrophysics Data System (ADS)

Pavuluri, C. M.; Kawamura, K.; Mihalopoulos, N.; Swaminathan, T.

2015-07-01

To better understand the photochemical processing of dicarboxylic acids and related polar compounds, we conducted batch UV irradiation experiments on two types of aerosol samples collected from India, which represent anthropogenic (AA) and biogenic (BA) aerosols, for time periods of 0.5 to 120 h. The irradiated samples were analyzed for molecular compositions of diacids, oxoacids and α-dicarbonyls. The results show that photochemical degradation of oxalic (C2), malonic (C3) and other C8-C12 diacids overwhelmed their production in aqueous aerosols, whereas succinic acid (C4) and C5-C7 diacids showed a significant increase (ca. 10 times) during the course of irradiation experiments. The photochemical formation of oxoacids and α-dicarbonyls overwhelmed their degradation during the early stages of experiment except for ω-oxooctanoic acid (ωC8), which showed a similar pattern to that of C4. We also found a gradual decrease in the relative abundance of C2 to total diacids and an increase in the relative abundance of C4 during prolonged experiment. Based on the changes in concentrations and mass ratios of selected species with the irradiation time, we hypothesize that iron-catalyzed photolysis of C2 and C3 diacids controls their concentrations in Fe-rich atmospheric waters, whereas photochemical formation of C4 diacid (via ωC8) is enhanced with photochemical processing of aqueous aerosols in the atmosphere. This study demonstrates that the ambient aerosols contain abundant precursors that produce diacids, oxoacids and α-dicarbonyls, although some species such as oxalic acid decompose extensively during an early stage of photochemical processing.

Organic Aerosol Formation Photoenhanced by the Formation of Secondary Photo-sensitizers in ageing Aerosols

NASA Astrophysics Data System (ADS)

Aregahegn, Kifle; Nozière, Barbara; George, Christian

2013-04-01

Humankind is facing a changing environment possibly due to anthropogenic stress on the atmosphere. In this context, aerosols play a key role by affecting the radiative climate forcing, hydrological cycle, and by their adverse effect on health. The role of organic compounds in these processes is however still poorly understood because of their massive chemical complexity and numerous transformations. This is particularly true for Secondary Organic Aerosol (SOA), which are produced in the atmosphere by organic gases. Traditionally, the driving forces for SOA growth is believed to be the partitioning onto aerosol seeds of condensable gases, either emitted primarily or resulting from the gas phase oxidation of organic gases. However, even the most up-to-date models based on such mechanisms can not account for the SOA mass observed in the atmosphere, suggesting the existence of other, yet unknown formation processes. The present study shows experimental evidence that particulate phase chemistry produces photo-sensitizers that lead to photo-induced formation and growth of secondary organic aerosol in the near UV and the presence of volatile organic compounds (VOC) such as terpenes. By means of an aerosol flow tube reactor equipped with Scanning Mobility Particle Sizer (SMPS) having Kr-85 source aerosol neutralizer, Differential Mobility Analyser (DMA) and Condensation Particle Sizer (CPC), we identified that traces of the aerosol phase product of glyoxal chemistry as is explained in Gallway et al., and Yu et al., namely imidazole-2-carboxaldehyde (IC) is a strong photo-sensitizer when irradiated by near-UV in the presence of volatile organic compounds such as terpenes. Furthermore, the influence of pH, type and concentration of VOCs, composition of seed particles, relative humidity and irradiation intensity on particle growth were studied. This novel photo-sensitizer contributed to more than 30% of SOA growth in 19min irradiation time in the presence of terpenes in the system and has linear relationship with the irradiation intensity. These results demonstrate that, upon ageing, organic aerosols can produce photo-sensitizers which auto-photo-catalyses their SOA growth.

A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berg, L. K.; Shrivastava, M.; Easter, R. C.

A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is anticipated that they will be included in a future public release of WRF-Chem.« less

A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

DOE PAGES

Berg, L. K.; Shrivastava, M.; Easter, R. C.; ...

2015-02-24

A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is anticipated that they will be included in a future public release of WRF-Chem.« less

The Impact of Aerosol Sources and Aging on CCN Formation in the Houston-Galveston-Gulf of Mexico Region

NASA Astrophysics Data System (ADS)

Quinn, P.; Bates, T.; Coffman, D.; Covert, D.

2007-12-01

The impact of anthropogenic aerosol on cloud properties, cloud lifetime, and precipitation processes is one of the largest uncertainties in our current understanding of climate change. Aerosols affect cloud properties by serving as cloud condensation nuclei (CCN) thereby leading to the formation of cloud droplets. The process of cloud drop activation is a function of both the size and chemistry of the aerosol particles which, in turn, depend on the source of the aerosol and transformations that occur downwind. In situ field measurements that can lead to an improved understanding of the process of cloud drop formation and simplifying parameterizations for improving the accuracy of climate models are highly desirable. During the Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources, aging, chemistry, and size in the activation of particles to form cloud droplets. Here, we use the correlation between variability in critical diameter for activation (determined empirically from measured CCN concentrations and the number size distribution) and aerosol composition to quantify the impact of composition on particle activation. Variability in aerosol composition is parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA) for particle diameters less than 200 nm (vacuum aerodynamic). The HOA mass fraction in this size range is lowest for marine aerosol and higher for aerosol impacted by anthropogenic emissions. Combining all data collected at 0.44 percent supersaturation (SS) reveals that composition (defined in this way) explains 40 percent of the variance in the critical diameter. As expected, the dependence of activation on composition is strongest at lower SS. At the same time, correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during GoMACCS, composition plays a dominant role in determining the fraction of particles that are activated to form cloud droplets. Using Kohler theory, we estimate the error that results in calculated CCN concentrations if the organic fraction of the aerosol is neglected (i.e., a fully soluble composition of ammonium sulfate is assumed) for the range of organic mass fractions and mean diameters observed during GoMACCS. We then relate this error to the source and age of the aerosol. At 0.22 and 0.44 percent SS, the error is considerable for anthropogenic aerosol sampled near the source region as this aerosol has, on average, a high POM mass fraction and smaller particle mean diameter. The error is lower for more aged aerosol as it has a lower POM mass fraction and larger mean particle diameter. Hence, the percent error in calculated CCN concentration is expected to be larger for younger, organic- rich aerosol and smaller for aged, sulfate rich aerosol and for marine aerosol. We extend this analysis to continental and marine data sets recently reported by Dusek et al. [Science, 312, 1375, 2006] and Hudson [Geophys. Res., Lett., 34, L08801, 2007].

The Cloud Ice Mountain Experiment (CIME) 1998: experiment overview and modelling of the microphysical processes during the seeding by isentropic gas expansion

NASA Astrophysics Data System (ADS)

Wobrock, Wolfram; Flossmann, Andrea I.; Monier, Marie; Pichon, Jean-Marc; Cortez, Laurent; Fournol, Jean-François; Schwarzenböck, Alfons; Mertes, Stephan; Heintzenberg, Jost; Laj, Paolo; Orsi, Giordano; Ricci, Loretta; Fuzzi, Sandro; Brink, Harry Ten; Jongejan, Piet; Otjes, René

The second field campaign of the Cloud Ice Mountain Experiment (CIME) project took place in February 1998 on the mountain Puy de Dôme in the centre of France. The content of residual aerosol particles, of H 2O 2 and NH 3 in cloud droplets was evaluated by evaporating the drops larger than 5 μm in a Counterflow Virtual Impactor (CVI) and by measuring the residual particle concentration and the released gas content. The same trace species were studied behind a round jet impactor for the complementary interstitial aerosol particles smaller than 5 μm diameter. In a second step of experiments, the ambient supercooled cloud was converted to a mixed phase cloud by seeding the cloud with ice particles by the gas release from pressurised gas bottles. A comparison between the physical and chemical characteristics of liquid drops and ice particles allows a study of the fate of the trace constituents during the presence of ice crystals in the cloud. In the present paper, an overview is given of the CIME 98 experiment and the instrumentation deployed. The meteorological situation during the experiment was analysed with the help of a cloud scale model. The microphysics processes and the behaviour of the scavenged aerosol particles before and during seeding are analysed with the detailed microphysical model ExMix. The simulation results agreed well with the observations and confirmed the assumption that the Bergeron-Findeisen process was dominating during seeding and was influencing the partitioning of aerosol particles between drops and ice crystals. The results of the CIME 98 experiment give an insight on microphysical changes, redistribution of aerosol particles and cloud chemistry during the Bergeron-Findeisen process when acting also in natural clouds.

A single-step aerosol process for in-situ surface modification of nanoparticles: Preparation of stable aqueous nanoparticle suspensions.

PubMed

Sapra, Mahak; Pawar, Amol Ashok; Venkataraman, Chandra

2016-02-15

Surface modification of nanoparticles during aerosol or gas-phase synthesis, followed by direct transfer into liquid media can be used to produce stable water-dispersed nanoparticle suspensions. This work investigates a single-step, aerosol process for in-situ surface-modification of nanoparticles. Previous studies have used a two-step sublimation-condensation mechanism following droplet drying, for surface modification, while the present process uses a liquid precursor containing two solutes, a matrix lipid and a surface modifying agent. A precursor solution in chloroform, of stearic acid lipid, with 4 %w/w of surface-active, physiological molecules [1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC), 1,2-dipalmitoyl-sn-glycero-3-phospho-(1'-rac-glycerol)-sodium salt (DPPG) or 1,2-dipalmitoyl-sn-glycero-3-phosphoethanolamine-N-[methoxy (polyethylene glycol) 2000]-ammonium salt (DPPE-PEG)] was processed in an aerosol reactor at a low gas temperatures. The surface modified nanoparticles were characterized for morphology, surface composition and suspension properties. Spherical, surface-modified lipid nanoparticles with median mobility diameters in the range of 105-150nm and unimodal size distributions were obtained. Fourier transform infra-red spectroscopy (FTIR) measurements confirmed the presence of surface-active molecules on external surfaces of modified lipid nanoparticles. Surface modified nanoparticles exhibited improved suspension stability, compared to that of pure lipid nanoparticles for a period of 30days. Lowest aggregation was observed in DPPE-PEG modified nanoparticles from combined electrostatic and steric effects. The study provides a single-step aerosol method for in-situ surface modification of nanoparticles, using minimal amounts of surface active agents, to make stable, aqueous nanoparticle suspensions. Copyright © 2015 Elsevier Inc. All rights reserved.

Bounding the heterogeneous gas uptake on aerosols and ground using resistance model

NASA Astrophysics Data System (ADS)

Su, H.; Li, M.; Cheng, Y.

2017-12-01

Heterogeneous uptake on aerosols and ground are potential important atmospheric sinks for gases. Different schemes have been used to characterize the dry deposition and heterogeneous aerosol gas uptake, although they share similar characteristics. In this work, we propose a unified resistance model to compare the uptake flux on both ground and aerosols, to identify the dominate heterogeneous process within the planetary boundary layer (PBL). The Gamma(eq) is introduced to represent the reactive uptake coefficient on aerosols when these two processes are equally important. It's shown that Gamma(eq) is proportional to the dry deposition velocity, inversely proportional to aerosol surface area concentration. Under typical regional background condition, Gamma(eq) vary from 1x10-5 to 4x10-4 with gas species, land-use type and season, which indicates that aerosol gas uptake should be included in atmospheric models when uptake coefficient higher than 10-5. We address the importance of heterogeneous gas uptake on aerosols over ground especially for ozone uptake on liquid organic aerosols and for marine PBL atmosphere.

Evaluation of liquid aerosol transport through porous media

NASA Astrophysics Data System (ADS)

Hall, R.; Murdoch, L.; Falta, R.; Looney, B.; Riha, B.

2016-07-01

Application of remediation methods in contaminated vadose zones has been hindered by an inability to effectively distribute liquid- or solid-phase amendments. Injection as aerosols in a carrier gas could be a viable method for achieving useful distributions of amendments in unsaturated materials. The objectives of this work were to characterize radial transport of aerosols in unsaturated porous media, and to develop capabilities for predicting results of aerosol injection scenarios at the field-scale. Transport processes were investigated by conducting lab-scale injection experiments with radial flow geometry, and predictive capabilities were obtained by developing and validating a numerical model for simulating coupled aerosol transport, deposition, and multi-phase flow in porous media. Soybean oil was transported more than 2 m through sand by injecting it as micron-scale aerosol droplets. Oil saturation in the sand increased with time to a maximum of 0.25, and decreased with radial distance in the experiments. The numerical analysis predicted the distribution of oil saturation with only minor calibration. The results indicated that evolution of oil saturation was controlled by aerosol deposition and subsequent flow of the liquid oil, and simulation requires including these two coupled processes. The calibrated model was used to evaluate field applications. The results suggest that amendments can be delivered to the vadose zone as aerosols, and that gas injection rate and aerosol particle size will be important controls on the process.

Evolution of Asian aerosols during transpacific transport in INTEX-B

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dunlea, E. J.; DeCarlo, Peter; Aiken, Allison

2009-10-01

Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B 5 (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to 10 be a robust tracer formore » air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). 15 Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, 20 the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of SOA mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary 25 organic aerosol formation in the free troposphere.« less

Marine Aerosols and Clouds.

PubMed

Brooks, Sarah D; Thornton, Daniel C O

2018-01-03

The role of marine bioaerosols in cloud formation and climate is currently so uncertain that even the sign of the climate forcing is unclear. Marine aerosols form through direct emissions and through the conversion of gas-phase emissions to aerosols in the atmosphere. The composition and size of aerosols determine how effective they are in catalyzing the formation of water droplets and ice crystals in clouds by acting as cloud condensation nuclei and ice nucleating particles, respectively. Marine organic aerosols may be sourced both from recent regional phytoplankton blooms that add labile organic matter to the surface ocean and from long-term global processes, such as the upwelling of old refractory dissolved organic matter from the deep ocean. Understanding the formation of marine aerosols and their propensity to catalyze cloud formation processes are challenges that must be addressed given the major uncertainties associated with aerosols in climate models.

Aerosol Emissions from Fuse-Deposition Modeling 3D Printers in a Chamber and in Real Indoor Environments.

PubMed

Vance, Marina E; Pegues, Valerie; Van Montfrans, Schuyler; Leng, Weinan; Marr, Linsey C

2017-09-05

Three-dimensional (3D) printers are known to emit aerosols, but questions remain about their composition and the fundamental processes driving emissions. The objective of this work was to characterize the aerosol emissions from the operation of a fuse-deposition modeling 3D printer. We modeled the time- and size-resolved emissions of submicrometer aerosols from the printer in a chamber study, gained insight into the chemical composition of emitted aerosols using Raman spectroscopy, and measured the potential for exposure to the aerosols generated by 3D printers under real-use conditions in a variety of indoor environments. The average aerosol emission rates ranged from ∼10 8 to ∼10 11 particles min -1 , and the rates varied over the course of a print job. Acrylonitrile butadiene styrene (ABS) filaments generated the largest number of aerosols, and wood-infused polylactic acid (PLA) filaments generated the smallest amount. The emission factors ranged from 6 × 10 8 to 6 × 10 11 per gram of printed part, depending on the type of filament used. For ABS, the Raman spectra of the filament and the printed part were indistinguishable, while the aerosol spectra lacked important peaks corresponding to styrene and acrylonitrile, which are both present in ABS. This observation suggests that aerosols are not a result of volatilization and subsequent nucleation of ABS or direct release of ABS aerosols.

Ice nucleating particle concentration during a combustion aerosol event

NASA Astrophysics Data System (ADS)

Adams, Mike; O'Sullivan, Daniel; Porter, Grace; Sanchez-Marroquin, Alberto; Tarn, Mark; Harrison, Alex; McQuaid, Jim; Murray, Benjamin

2017-04-01

The formation of ice in supercooled clouds is important for cloud radiative properties, their lifetime and the formation of precipitation. Cloud water droplets can supercool to below -33oC, but in the presence of Ice Nucleating Particles (INPs) freezing can be initiated at much higher temperatures. The concentration of atmospheric aerosols that are active as INPs depends on a number of factors, such as temperature and aerosol composition and concentration. However, our knowledge of which aerosol types serve as INPs is limited. For example, there has been much discussion over whether aerosol from combustion processes are important as INP. This is significant because combustion aerosol have increased in concentration dramatically since pre-industrial times and therefore have the potential to exert a significant anthropogenic impact on clouds and climate. In this study we made measurements of INP concentrations in Leeds over a specific combustion aerosol event in order to test if there was a correlation between INP concentrations and combustion aerosol. The combustion aerosol event was on the 5th November which is a major bonfire and firework event celebrated throughout the UK. During the event we observed a factor of five increase in aerosol and a factor of 10 increase in black carbon, but observed no significant increase in INP concentration. This implies that black carbon and combustion aerosol did not compete with the background INP during this event.

Dissolved organic matter in sea spray: a transfer study from marine surface water to aerosols

NASA Astrophysics Data System (ADS)

Schmitt-Kopplin, P.; Liger-Belair, G.; Koch, B. P.; Flerus, R.; Kattner, G.; Harir, M.; Kanawati, B.; Lucio, M.; Tziotis, D.; Hertkorn, N.; Gebefügi, I.

2012-04-01

Atmospheric aerosols impose direct and indirect effects on the climate system, for example, by absorption of radiation in relation to cloud droplets size, on chemical and organic composition and cloud dynamics. The first step in the formation of Organic primary aerosols, i.e. the transfer of dissolved organic matter from the marine surface into the atmosphere, was studied. We present a molecular level description of this phenomenon using the high resolution analytical tools of Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and nuclear magnetic resonance spectroscopy (NMR). Our experiments confirm the chemoselective transfer of natural organic molecules, especially of aliphatic compounds from the surface water into the atmosphere via bubble bursting processes. Transfer from marine surface water to the atmosphere involves a chemical gradient governed by the physicochemical properties of the involved molecules when comparing elemental compositions and differentiating CHO, CHNO, CHOS and CHNOS bearing compounds. Typical chemical fingerprints of compounds enriched in the aerosol phase were CHO and CHOS molecular series, smaller molecules of higher aliphaticity and lower oxygen content, and typical surfactants. A non-targeted metabolomics analysis demonstrated that many of these molecules corresponded to homologous series of oxo-, hydroxy-, methoxy-, branched fatty acids and mono-, di- and tricarboxylic acids as well as monoterpenes and sugars. These surface active biomolecules were preferentially transferred from surface water into the atmosphere via bubble bursting processes to form a significant fraction of primary organic aerosols. This way of sea spray production leaves a selective biological signature of the surface water in the corresponding aerosol that may be transported into higher altitudes up to the lower atmosphere, thus contributing to the formation of secondary organic aerosol on a global scale or transported laterally with possible deposition in the context of global biogeocycling.

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Technical Reports Server (NTRS)

Zaveri, R. A.; Shaw, W. J.; Cahill, J. F.; Cairns, Brian; Cappa, C. D.; Ottaviani, Matteo; Cziczo, D. J.; Ferrare, Richard A.; Alexander, M. L.; Alexandrov, Mikhail Dmitrievic;

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Ferrare, R. A.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Erickson, M. H.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kassianov, E. I.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Kubátová, A.; Langford, A. O.; Laskin, A.; Laulainen, N.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Suski, K.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Worsnop, D. R.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

2012-08-01

Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data analyses and focused modeling efforts that will facilitate the integration of new knowledge into improved representations of key aerosol processes and properties in climate models.

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Zaveri, R. A.; Shaw, W. J.; Cziczo, D. J.; Schmid, B.; Alexander, M. L.; Alexandrov, M.; Alvarez, R. J.; Arnott, W. P.; Atkinson, D. B.; Baidar, S.; Banta, R. M.; Barnard, J. C.; Beranek, J.; Berg, L. K.; Brechtel, F.; Brewer, W. A.; Cahill, J. F.; Cairns, B.; Cappa, C. D.; Chand, D.; China, S.; Comstock, J. M.; Dubey, M. K.; Easter, R. C.; Fast, J. D.; Floerchinger, C.; Flowers, B. A.; Fortner, E.; Gaffney, J. S.; Gilles, M. K.; Gorkowski, K.; Gustafson, W. I.; Gyawali, M.; Hair, J.; Hardesty, R. M.; Harworth, J. W.; Herndon, S.; Hiranuma, N.; Hostetler, C.; Hubbe, J. M.; Jayne, J. T.; Jeong, H.; Jobson, B. T.; Kleinman, L. I.; Kluzek, C.; Knighton, B.; Kolesar, K. R.; Kuang, C.; Langford, A. O.; Laskin, A.; Marchbanks, R. D.; Mazzoleni, C.; Mei, F.; Moffet, R. C.; Nelson, D.; Obland, M. D.; Oetjen, H.; Onasch, T. B.; Ortega, I.; Ottaviani, M.; Pekour, M.; Prather, K. A.; Radney, J. G.; Rogers, R. R.; Sandberg, S. P.; Sedlacek, A.; Senff, C. J.; Senum, G.; Setyan, A.; Shilling, J. E.; Shrivastava, M.; Song, C.; Springston, S. R.; Subramanian, R.; Tomlinson, J.; Volkamer, R.; Wallace, H. W.; Wang, J.; Weickmann, A. M.; Yu, X.-Y.; Zelenyuk, A.; Zhang, Q.

2012-01-01

Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data analyses and focused modeling efforts that will facilitate the integration of new knowledge into improved representations of key aerosol processes in climate models.

Long-term Aerosol Lidar Measurements At CNR-IMAA

NASA Astrophysics Data System (ADS)

Mona, L.; Amodeo, A.; D'Amico, G.; Pandolfi, M.; Pappalardo, G.

2006-12-01

Actual estimations of the aerosol effect on the radiation budget are affected by a large uncertainties mainly due to the high inhomogeneity and variability of atmospheric aerosol, in terms of concentration, shape, size distribution, refractive index and vertical distribution. Long-term measurements of vertical profiles of aerosol optical properties are needed to reduce these uncertainties. At CNR-IMAA (40° 36'N, 15° 44' E, 760 m above sea level), a lidar system for aerosol study is operative since May 2000 in the framework of EARLINET (European Aerosol Research Lidar Network). Until August 2005, it provided independent measurements of aerosol extinction and backscatter at 355 nm and aerosol backscatter profiles at 532 nm. After an upgrade of the system, it provides independent measurements of aerosol extinction and backscatter profiles at 355 and 532 nm, and of aerosol backscatter profiles at 1064 nm and depolarization ratio at 532 nm. For these measurements, lidar ratio at 355 and 532 nm and Angstrom exponent profiles at 355/532 nm are also obtained. Starting on May 2000, systematic measurements are performed three times per week according to the EARLINET schedule and further measurements are performed in order to investigate particular events, like dust intrusions, volcanic eruptions and forest fires. A climatological study has been carried out in terms of the seasonal behavior of the PBL height and of the aerosol optical properties calculated inside the PBL itself. In the free troposphere, an high occurrences of Saharan dust intrusions (about 1 day of Saharan dust intrusion every 10 days) has been observed at CNR-IMAA because of the short distance from the Sahara region. During 6 years of observations, very peculiar cases of volcanic aerosol emitted by Etna volcano and aerosol released by large forest fires burning occurred in Alaska and Canada have been observed in the free troposphere at our site. Particular attention is devoted to lidar ratio both for the PBL and the free troposphere region, in order to study influences of aerosol modification/transportation processes on its values and its variability. ACKNOWLEDGMENTS The financial support of this work by the European Commission under grant RICA-025991 is gratefully acknowledged.

Investigation of the evolution of atmospheric particles with integration of the stochastic particle-resolved model partmc-mosaic and atmospheric measurements

NASA Astrophysics Data System (ADS)

Tian, Jian

With the recently-developed particle-resolved model PartMC-MOSAIC, the mixing state and other physico-chemical properties of individual aerosol particles can be tracked as the particles undergo aerosol aging processes. However, existing PartMC-MOSAIC applications have mainly been based on idealized scenarios, and a link to real atmospheric measurement has not yet been established. In this thesis, we extend the capability of PartMC-MOSAIC and apply the model framework to three distinct scenarios with different environmental conditions to investigate the physical and chemical aging of aerosols in those environments. The first study is to investigate the evolution of particle mixing state and cloud condensation nuclei (CCN) activation properties in a ship plume. Comparisons of our results with observations from the QUANTIFY Study in 2007 in the English channel and the Gulf of Biscay showed that the model was able to reproduce the observed evolution of total number concentration and the vanishing of the nucleation mode consisting of sulfate particles. Further process analysis revealed that during the first hour after emission, dilution reduced the total number concentration by four orders of magnitude, while coagulation reduced it by an additional order of magnitude. Neglecting coagulation resulted in an overprediction of more than one order of magnitude in the number concentration of particles smaller than 40 nm at a plume age of 100 s. Coagulation also significantly altered the mixing state of the particles, leading to a continuum of internal mixtures of sulfate and black carbon. The impact of condensation on CCN concentrations depended on the supersaturation threshold at which CCN activity was evaluated. Nucleation was observed to have a limited impact on the CCN concentration in the ship plume we studied, but was sensitive to formation rates of secondary aerosol. For the second study we adapted PartMC to represent the aerosol evolution in an aerosol chamber, with the intention to use the model as a tool to interpret and guide chamber experiments in the future. We added chamber-specific processes to our model formulation such as wall loss due to particle diffusion and sedimentation, and dilution effects due to sampling. We also implemented a treatment of fractal particles to account for the morphology of agglomerates and its impact on aerosol dynamics. We verified the model with published results of self-similar size distributions, and validated the model using experimental data from an aerosol chamber. To this end we developed a fitting optimization approach to determine the best-estimate values for the wall loss parameters based on minimizing the l2-norm of the model errors of the number distribution. Obtaining the best fit required taking into account the non-spherical structure of the particle agglomerates. Our third study focuses on the implementation of volatility basis set (VBS) framework in PartMC-MOSAIC to investigate the chemical aging of organic aerosols in the atmosphere. The updated PartMC-MOSAIC model framework was used to simulate the evolution of aerosols in air trajectories initialized from CARES field campaign conducted in California in June 2010. The simulation results were compared with aircraft measurement data during the campaign. PartMC-MOSAIC was able to produce gas and aerosol concentrations at similar levels compared to the observation data. Moreover, the simulation with VBS enabled produced consistently more secondary organic aerosols (SOA). The investigation of particle mixing state revealed that the impact of VBS framework on particle mixing state is sensitive to the daylight exposure time. (Abstract shortened by ProQuest.).

Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Hansen, Kristen J.

An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain different source and process components, and to examine concentration changes in groups of variables with respect to time of day and meteorological conditions. Seven orthogonal groups of variables resulted from the statistical analysis; the groups serve as molecular markers for different biologic and anthropogenic emission sources. In addition, the results of the statistical analysis were used to investigate how several emission source contributions vary with respect to local atmospheric dynamics. Field studies were conducted in the urban environment in and around Boulder, CO. to characterize the dynamics, chemistry, and emission sources which affect the composition and concentration of different size-fractions of aerosol particles in the Boulder air mass. Relationships between different size fractions of particles and some gas-phase pollutants were elucidated. These field studies included an investigation of seasonal variations in the organic content and concentration of aerosol particles, and how these characteristics are related to local meteorology and to the concentration of some gas-phase pollutants. The elemental and organic composition of aerosol particles was investigated according to particle size in preliminary studies of size-differentiated samples of aerosol particles. In order to aid in future studies of urban aerosol particles, samples were collected at a forest fire near Boulder. Molecular markers specific to wood burning processes will be useful indicators of residential wood burning activities in future field studies.

Maritime Aerosol Network as a Component of AERONET - First Results and Comparison with Global Aerosol Models and Satellite Retrievals

NASA Technical Reports Server (NTRS)

Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.;

Maritime Aerosol Network as a component of AERONET - first results and comparison with global aerosol models and satellite retrievals

NASA Astrophysics Data System (ADS)

Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.; Smyth, T. J.; Zielinski, T.; Zibordi, G.; Goes, J. I.; Harvey, M. J.; Quinn, P. K.; Nelson, N. B.; Radionov, V. F.; Duarte, C. M.; Losno, R.; Sciare, J.; Voss, K. J.; Kinne, S.; Nalli, N. R.; Joseph, E.; Krishna Moorthy, K.; Covert, D. S.; Gulev, S. K.; Milinevsky, G.; Larouche, P.; Belanger, S.; Horne, E.; Chin, M.; Remer, L. A.; Kahn, R. A.; Reid, J. S.; Schulz, M.; Heald, C. L.; Zhang, J.; Lapina, K.; Kleidman, R. G.; Griesfeller, J.; Gaitley, B. J.; Tan, Q.; Diehl, T. L.

2011-01-01

The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurements areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.

Maritime aerosol network as a component of AERONET - first results and comparison with global aerosol models and satellite retrievals

NASA Astrophysics Data System (ADS)

Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.; Smyth, T. J.; Zielinski, T.; Zibordi, G.; Goes, J. I.; Harvey, M. J.; Quinn, P. K.; Nelson, N. B.; Radionov, V. F.; Duarte, C. M.; Losno, R.; Sciare, J.; Voss, K. J.; Kinne, S.; Nalli, N. R.; Joseph, E.; Krishna Moorthy, K.; Covert, D. S.; Gulev, S. K.; Milinevsky, G.; Larouche, P.; Belanger, S.; Horne, E.; Chin, M.; Remer, L. A.; Kahn, R. A.; Reid, J. S.; Schulz, M.; Heald, C. L.; Zhang, J.; Lapina, K.; Kleidman, R. G.; Griesfeller, J.; Gaitley, B. J.; Tan, Q.; Diehl, T. L.

2011-03-01

The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.

Scanning Transmission X-ray Microscopy: Applications in Atmospheric Aerosol Research

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moffet, Ryan C.; Tivanski, Alexei V.; Gilles, Mary K.

Scanning transmission x-ray microscopy (STXM) combines x-ray microscopy and near edge x-ray absorption fine structure spectroscopy (NEXAFS). This combination provides spatially resolved bonding and oxidation state information. While there are reviews relevant to STXM/NEXAFS applications in other environmental fields (and magnetic materials) this chapter focuses on atmospheric aerosols. It provides an introduction to this technique in a manner approachable to non-experts. It begins with relevant background information on synchrotron radiation sources and a description of NEXAFS spectroscopy. The bulk of the chapter provides a survey of STXM/NEXAFS aerosol studies and is organized according to the type of aerosol investigated. Themore » purpose is to illustrate the current range and recent growth of scientific investigations employing STXM-NEXAFS to probe atmospheric aerosol morphology, surface coatings, mixing states, and atmospheric processing.« less

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen

Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate modelsmore » typically do not comprehensively include all important processes. Our review summarizes some of the important developments during the past decade in understanding SOA formation. We also highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.« less

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

DOE PAGES

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen; ...

2017-06-15

Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate modelsmore » typically do not comprehensively include all important processes. Our review summarizes some of the important developments during the past decade in understanding SOA formation. We also highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.« less

Observations of fluorescent aerosol-cloud interactions in the free troposphere at the Sphinx high Alpine research station, Jungfraujoch

NASA Astrophysics Data System (ADS)

Crawford, I.; Lloyd, G.; Bower, K. N.; Connolly, P. J.; Flynn, M. J.; Kaye, P. H.; Choularton, T. W.; Gallagher, M. W.

2015-09-01

The fluorescent nature of aerosol at a high Alpine site was studied using a wide-band integrated bioaerosol (WIBS-4) single particle multi-channel ultra violet-light induced fluorescence (UV-LIF) spectrometer. This was supported by comprehensive cloud microphysics and meteorological measurements with the aims of cataloguing concentrations of bio-fluorescent aerosols at this high altitude site and also investigating possible influences of UV-fluorescent particle types on cloud-aerosol processes. Analysis of background free tropospheric air masses, using a total aerosol inlet, showed there to be a minor but statistically insignificant increase in the fluorescent aerosol fraction during in-cloud cases compared to out of cloud cases. The size dependence of the fluorescent aerosol fraction showed the larger aerosol to be more likely to be fluorescent with 80 % of 10 μm particles being fluorescent. Whilst the fluorescent particles were in the minority (NFl/NAll = 0.27±0.19), a new hierarchical agglomerative cluster analysis approach, Crawford et al. (2015) revealed the majority of the fluorescent aerosol were likely to be representative of fluorescent mineral dust. A minor episodic contribution from a cluster likely to be representative of primary biological aerosol particles (PBAP) was also observed with a wintertime baseline concentration of 0.1±0.4 L-1. Given the low concentration of this cluster and the typically low ice active fraction of studied PBAP (e.g. pseudomonas syringae) we suggest that the contribution to the observed ice crystal concentration at this location is not significant during the wintertime.

Aerosol Size and Chemical Composition in the Canadian High Arctic

NASA Astrophysics Data System (ADS)

Chang, R. Y. W.; Hayes, P. L.; Leaitch, W. R.; Croft, B.; O'Neill, N. T.; Fogal, P.; Drummond, J. R.; Sloan, J. J.

2015-12-01

Arctic aerosol have a strong annual cycle, with winter months dominated by long range transport from lower latitudes resulting in high mass loadings. Conversely, local emissions are more prominent in the summer months because of the decreased influence of transported aerosol, allowing us to regularly observe both transported and local aerosol. This study will present observations of aerosol chemical composition and particle number size distribution collected at the Polar Environment Artic Research Laboratory and the Alert Global Atmospheric Watch Observatory at Eureka (80N, 86W) and Alert (82N, 62W), Nunavut, respectively. Summer time observations of the number size distribution reveal a persistent mode of particles centered between 30-50 nm, with occasional bursts of smaller particles. The non-refractory aerosol chemical composition, measured by the Canadian Network for the Detection of Atmospheric Change quadrupole aerosol mass spectrometer, is primarily organic, with contributions from both aged and fresher organic aerosol. Factor analysis will be conducted to better understand these sources. The site at Eureka is more susceptible to long range transport since it is at the top of a mountain ridge (610 m above sea level) and will be compared to the site at Alert on an elevated plain (200 m above sea level). This will allow us to determine the relative contributions from processes and sources at the sites at different elevations. Comparisons with aerosol optical depth and GEOS-Chem model output will also be presented to put these surface measurements into context with the overlying and regional atmosphere. Results from this study contribute to our knowledge of aerosol in the high Arctic.

An overview of the CATS level 1 processing algorithms and data products

NASA Astrophysics Data System (ADS)

Yorks, J. E.; McGill, M. J.; Palm, S. P.; Hlavka, D. L.; Selmer, P. A.; Nowottnick, E. P.; Vaughan, M. A.; Rodier, S. D.; Hart, W. D.

2016-05-01

The Cloud-Aerosol Transport System (CATS) is an elastic backscatter lidar that was launched on 10 January 2015 to the International Space Station (ISS). CATS provides both space-based technology demonstrations for future Earth Science missions and operational science measurements. This paper outlines the CATS Level 1 data products and processing algorithms. Initial results and validation data demonstrate the ability to accurately detect optically thin atmospheric layers with 1064 nm nighttime backscatter as low as 5.0E-5 km-1 sr-1. This sensitivity, along with the orbital characteristics of the ISS, enables the use of CATS data for cloud and aerosol climate studies. The near-real-time downlinking and processing of CATS data are unprecedented capabilities and provide data that have applications such as forecasting of volcanic plume transport for aviation safety and aerosol vertical structure that will improve air quality health alerts globally.

Cloud microphysics modification with an online coupled COSMO-MUSCAT regional model

NASA Astrophysics Data System (ADS)

Sudhakar, D.; Quaas, J.; Wolke, R.; Stoll, J.; Muehlbauer, A. D.; Tegen, I.

2015-12-01

Abstract: The quantification of clouds, aerosols, and aerosol-cloud interactions in models, continues to be a challenge (IPCC, 2013). In this scenario two-moment bulk microphysical scheme is used to understand the aerosol-cloud interactions in the regional model COSMO (Consortium for Small Scale Modeling). The two-moment scheme in COSMO has been especially designed to represent aerosol effects on the microphysics of mixed-phase clouds (Seifert et al., 2006). To improve the model predictability, the radiation scheme has been coupled with two-moment microphysical scheme. Further, the cloud microphysics parameterization has been modified via coupling COSMO with MUSCAT (MultiScale Chemistry Aerosol Transport model, Wolke et al., 2004). In this study, we will be discussing the initial result from the online-coupled COSMO-MUSCAT model system with modified two-moment parameterization scheme along with COSP (CFMIP Observational Simulator Package) satellite simulator. This online coupled model system aims to improve the sub-grid scale process in the regional weather prediction scenario. The constant aerosol concentration used in the Seifert and Beheng, (2006) parameterizations in COSMO model has been replaced by aerosol concentration derived from MUSCAT model. The cloud microphysical process from the modified two-moment scheme is compared with stand-alone COSMO model. To validate the robustness of the model simulation, the coupled model system is integrated with COSP satellite simulator (Muhlbauer et al., 2012). Further, the simulations are compared with MODIS (Moderate Resolution Imaging Spectroradiometer) and ISCCP (International Satellite Cloud Climatology Project) satellite products.

Effects of Convective Transport on the Budget of Amazonian Aerosol under Background Conditions

NASA Astrophysics Data System (ADS)

Wang, J.; Krejci, R.; Giangrande, S. E.; Kuang, C.; Barbosa, H. M.; Brito, J.; Carbone, S.; Chi, X.; Comstock, J. M.; Ditas, F.; Lavric, J. V.; Manninen, H. E.; Mei, F.; Moran, D.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Schmid, B.; Souza, R. A. F. D.; Springston, S. R.; Tomlinson, J. M.; Toto, T.; Walter, D.; Wimmer, D.; Smith, J. N.; Machado, L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.

2016-12-01

Aerosol particles can strongly influence the radiative properties of clouds, and they represent one of the largest uncertainties in computer simulations of climate change. The large uncertainty is in large part due to a poor understanding of processes under natural conditions, which serves as the baseline to measure change against. Understanding the processes under natural conditions is critical for a reliable assessment and quantification of ongoing and future climate change. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions. Here we examine the aerosol number and CCN budget under background conditions in the Amazon basin using data collected during the Observations and Modeling of the Green Ocean Amazon (GoAmazon 2014/5) campaign, which took place from January 2014 to December 2015 near Manaus, Brazil. The aerosol size spectrum was observed at the Amazon Tall Tower Observatory (ATTO), 150 km upwind of Manaus, and its variation with convection and precipitation during the wet season is presented. Air masses arriving at the ATTO during the wet season are typically brought by the northeasterly trade winds and travel across at least 1000 km of undeveloped tropical rainforest, therefore are generally clean. Also shown are vertical profiles of aerosol observed onboard the DOE Gulfstream-1 research aircraft. The impact of convective transport on the budget of boundary layer aerosol and CCN under the background conditions is discussed.

Changes in Stratiform Clouds of Mesoscale Convective Complex Introduced by Dust Aerosols

NASA Technical Reports Server (NTRS)

Lin, B.; Min, Q.-L.; Li, R.

2010-01-01

Aerosols influence the earth s climate through direct, indirect, and semi-direct effects. There are large uncertainties in quantifying these effects due to limited measurements and observations of aerosol-cloud-precipitation interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate because of its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust aerosol loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective complex (MCC). A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed MCCs under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially over stratiform areas.

Laboratory Experiments and Modeling for Interpreting Field Studies of Secondary Organic Aerosol Formation Using an Oxidation Flow Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jimenez, Jose-Luis

2016-02-01

This grant was originally funded for deployment of a suite of aerosol instrumentation by our group in collaboration with other research groups and DOE/ARM to the Ganges Valley in India (GVAX) to study aerosols sources and processing. Much of the first year of this grant was focused on preparations for GVAX. That campaign was cancelled due to political reasons and with the consultation with our program manager, the research of this grant was refocused to study the applications of oxidation flow reactors (OFRs) for investigating secondary organic aerosol (SOA) formation and organic aerosol (OA) processing in the field and laboratorymore » through a series of laboratory and modeling studies. We developed a gas-phase photochemical model of an OFR which was used to 1) explore the sensitivities of key output variables (e.g., OH exposure, O 3, HO 2/OH) to controlling factors (e.g., water vapor, external reactivity, UV irradiation), 2) develop simplified OH exposure estimation equations, 3) investigate under what conditions non-OH chemistry may be important, and 4) help guide design of future experiments to avoid conditions with undesired chemistry for a wide range of conditions applicable to the ambient, laboratory, and source studies. Uncertainties in the model were quantified and modeled OH exposure was compared to tracer decay measurements of OH exposure in the lab and field. Laboratory studies using OFRs were conducted to explore aerosol yields and composition from anthropogenic and biogenic VOC as well as crude oil evaporates. Various aspects of the modeling and laboratory results and tools were applied to interpretation of ambient and source measurements using OFR. Additionally, novel measurement methods were used to study gas/particle partitioning. The research conducted was highly successful and details of the key results are summarized in this report through narrative text, figures, and a complete list of publications acknowledging this grant.« less

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Future Suborbital Activities to Address Knowledge Gaps in Satellite and Model Assessments

NASA Technical Reports Server (NTRS)

Redemann, Jens; Wood, R.; Zuidema, P.; Haywood, J.; Piketh, S.; Formenti, P.; L'Ecuyer, T.; Kacenelenbogen, M.; Segal-Rosenheimer, M.; Shinozuka, Y.;

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Future Suborbital Activities to Address Knowledge Gaps in Satellite and Model Assessments

NASA Astrophysics Data System (ADS)

Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; L'Ecuyer, T. S.; Kacenelenbogen, M. S.; Segal-Rosenhaimer, M.; Shinozuka, Y.; LeBlanc, S. E.; Vaughan, M. A.; Schmidt, S.; Flynn, C. J.; Song, S.; Schmid, B.; Luna, B.; Abel, S.

2015-12-01

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. Our understanding of aerosol-cloud interactions in the SE Atlantic is hindered both by the lack of knowledge on aerosol and cloud properties, as well as the lack of knowledge about detailed physical processes involved. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling. Recent efforts to make full use of A-Train aerosol sensor synergies will be highlighted. We describe planned field campaigns in the region to address the existing knowledge gaps. Specifically, we describe the scientific objectives and implementation of the five synergistic, international research activities aimed at providing some of the key aerosol and cloud properties and a process-level understanding of aerosol-cloud interactions over the SE Atlantic: NASA's ORACLES, the UK Met Office's CLARIFY-2016, the DoE's LASIC, NSF's ONFIRE, and CNRS' AEROCLO-SA.

Processes Controlling the Seasonal Cycle of Arctic Aerosol Number and Size Distributions

NASA Astrophysics Data System (ADS)

Wentworth, G.; Croft, B.; Martin, R.; Leaitch, W. R.; Tunved, P.; Breider, T. J.; D'Andrea, S.; Pierce, J. R.; Murphy, J. G.; Kodros, J.; Abbatt, J.

2015-12-01

Measurements at high-Arctic sites show a strong seasonal cycle in aerosol number and size. The number of aerosols with diameters larger than 20 nm exhibits a maximum in late spring associated with a dominant accumulation mode, and a second maximum in the summer associated with a dominant Aitken mode. Seasonal-mean aerosol effective diameter ranges from about 160 nm in summer to 250 nm in winter. This study interprets these seasonal cycles with the GEOS-Chem-TOMAS global aerosol microphysics model. We find improved agreement with in situ measurements (SMPS) of aerosol size at both Alert, Nunavut, and Mt. Zeppelin, Svalbard following model developments: 1) increase the efficiency of wet scavenging in the Arctic summer and 2) represent coagulation between interstitial aerosols and aerosols activated to form cloud droplets. Our simulations indicate that the dominant summer-time Aitken mode is associated with increased efficiency of wet removal, which limits the number of larger aerosols and promotes local new-aerosol formation. We also find an important role of interstitial coagulation in clouds in the Arctic, which limits the number of Aitken-mode aerosols in the non-summer seasons when direct wet removal of these aerosols is inefficient. The summertime Arctic atmosphere is particularly pristine and strongly influenced by natural regional emissions which have poorly understood climate impacts. Especially influenced are the climatic roles of atmospheric particles and clouds. Here we present evidence that ammonia (NH3) emissions from migratory-seabird guano (dung) are the primary contributor to summertime free ammonia levels recently measured in the Canadian Arctic atmosphere. These findings suggest that ammonia from seabird guano is a key factor contributing to bursts of new-particle formation, which are observed every summer in the near-surface atmosphere at Alert, Canada. Chemical transport model simulations show that these newly formed particles can grow by vapour condensation to diameters sufficiently large to influence Arctic cloud properties and lead to a pan-Arctic cooling over -0.1 W m-2 with local cooling exceeding -1 W m-2 near some bird colonies. These coupled ecological-chemical processes may be susceptible to Arctic warming and industrialization.

Chemical, physical, and optical evolution of biomass burning aerosols: a case study

NASA Astrophysics Data System (ADS)

Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

2011-02-01

In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

Possible indicators of long-range transport for aerosol emitted from various source regions in Northeast Asia

NASA Astrophysics Data System (ADS)

Park, S.; Kim, C.

2013-12-01

Air pollutant is affected by both long-range transboundary processes and local air pollution emission. Therefore it is important to identify the origin of air pollutant, for example, by classifying air pollutants into long-range transport (LRT) dominant process and local emission dominant (LED) cases. This study proposed several chemical and physical indicators of LRT process of aerosol concentrations observed at Korean peninsula. In order to identify the source regions and to estimate the contributions of both LRT and LED, we performed Lagrangian particle dispersion model(FLEXPART) and selected high pollution days over the three source regions in China inland and one Korea peninsula defined in this study; LRT-I to III and LED case. Next, we investigated the chemical and physical characteristics of LRT process of aerosol, and contrasted to those in the LED case over the Northeast Asia. We examined the difference of both modeled features simulated by CMAQ and as well measured aerosol optical properties of satellite-based sensor MODIS and AERONET data. Modeling study showed that the most effective indicator is the sulfur conversion ratios such as SO42-/(SO2+ SO42-) and SO42-/ SO2 for high sulfate condition. The ratio of N-containing species such as NOx (or NOy) to CO were the next best alternative indicators. In the meteorological fields, the results showed that pressure pattern and streamline flow are similar on a case by case basis. For observational physical features, we obtained the spatial distributions of the mean AOD, fine mode fraction (FMF), angstrom exponent (AE) by taking the average of MODIS aerosol products for the each analysis period. The highest AOD was found over the industrialized coastal region regardless of cases. AERONET data showed that aerosol size distribution showed significantly higher concentration of fine-mode particle in LED cases in comparison with that of LRT groups, suggesting that the amplitude fine modes of LRT relative to LED could be a possible LRT indicator. We expressed the ratio of both fine- and coarse-mode amplitudes according to the various source regions for LRT and LED process at receptor of Korean peninsula. Other characteristics of simulated and observational features of physical properties were also discussed here.

Experimental investigation of aerosol composition and growth rates

NASA Astrophysics Data System (ADS)

Wimmer, Daniela; Winkler, Paul; Kulmala, Markku; Petäjä, Tuukka

2017-04-01

Atmospheric aerosol particles have relevant influence on human lives. Human health is affected, as by breathing in the aerosol particles, they deposit in the lungs causing various health problems. Also they interfere indirectly and directly with sunlight, which affects the climate on Earth. Primary aerosol particles originate for example from anthropogenic sources, such as Diesel cars or natural sources such as dessert dust. Secondary aerosol particles are formed via condensation of low volatile gas phase compounds. First, small clusters consisting of a few gas molecules only are formed, which can then grow to bigger aerosol particles. These then form seeds for cloud droplets. The chemical composition of the cloud particles determines whether the cloud absorbs or scatters sunlight more. Intensive experimental and theoretical work has been put into understanding the details of the initial processes leading to the natural formation of these secondary aerosol particles. According to modelling studies, aerosol particles formed via the nucleation process are responsible for about 50% of the global cloud condensation nuclei concentration. With currently used methods, the chemical composition of small molecular clusters (up to 2nm in diameter) can be resolved. Also standard methods to determine aerosol particle composition at sizes >10 nm are available. Within this project, the aerosol particle composition in the 2-4 nm size range will be investigated experimentally. The setup will consist of a combination of an electrical method that allows determine the electrical mobility of the particles which then can be converted to a diameter. By letting the charged particles travel through a changing electrical field, they travel at different speeds according to their mobility. That allows to particles with certain mobilities, which then can be converted to a diameter. After the size selection, the particles are counted by means of optical detection. Condensation particle counters (CPCs) grow the particles internally, after which they are detected optically. By changing the condensing liquid, depending on the aerosol particle composition, they are activated differently. By combining the electrical size selection with CPCs with different liquids, information about particle composition can be determined. The project includes laboratory studies and field measurements in different locations (one rural site and two urban sites). I wish to acknowledge the Austrian Science Fund (FWF; Grant No J3951 - N36).

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated organic aerosol (OOA) factors: a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). The MO-OOA dominated during the pre-monsoon period, whereas LO-OOA dominated during monsoon. The sensitivity of air mass transport during pre-monsoon with synoptic process was also evaluated with a 3-D chemical transport model.

Large Contribution of Coarse Mode to Aerosol Microphysical and Optical Properties: Evidence from Ground-Based Observations of a Transpacific Dust Outbreak at a High-Elevation North American Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kassianov, E.; Pekour, M.; Flynn, C.

Our work is motivated by previous studies of the long-range trans-Atlantic transport of Saharan dust and the observed quasi-static nature of coarse mode aerosol with a volume median diameter (VMD) of approximately 3.5 µm. We examine coarse mode contributions from the trans-Pacific transport of Asian dust to North American aerosol microphysical and optical properties using a dataset collected at the high-elevation, mountain-top Storm Peak Laboratory (SPL, 3.22 km above sea level [ASL]) and the nearby Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF, 2.76 km ASL). Data collected during the SPL Cloud Property Validation Experiment (STORMVEX, March 2011) are complemented bymore » quasi-global high-resolution model simulations coupled with aerosol chemistry. We identify dust event associated mostly with Asian plume (about 70% of dust mass) where the coarse mode with moderate (~4 µm) VMD is distinct and contributes substantially to aerosol microphysical (up to 70% for total volume) and optical (up to 45% for total scattering and aerosol optical depth) properties. Our results, when compared with previous Saharan dust studies, suggest a fairly invariant behavior of coarse mode dust aerosols. If confirmed in additional studies, this invariant behavior may simplify considerably model parameterizations for complex and size-dependent processes associated with dust transport and removal.« less

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

The Asian Tropopause Aerosol Layer: Balloon-Borne Measurements, Satellite Observations and Modeling Approaches

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Natarajan, M.; Deshler, Terry; Liu, H.; Wegner, T.; Baker, N.; Gadhavi, H.; Jayaraman, A.; Pandit, A.;

Indirect and semi-direct aerosol campaign: The impact of Arctic aerosols on clouds

DOE PAGES

McFarquhar, Greg M.; Ghan, Steven; Verlinde, Johannes; ...

2011-02-01

A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the boundary layer in the vicinity of Barrow, Alaska, was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's primary aim was to examine the effects of aerosols, including those generated by Asian wildfires, on clouds that contain both liquid and ice. ISDAC utilized the Atmospheric Radiation Measurement Pro- gram's permanent observational facilities at Barrow and specially deployed instruments measuring aerosol, ice fog, precipitation, and radiation. The National Research Council of Canada Convair-580 flew 27 sorties and collected data using an unprecedented 41more » stateof- the-art cloud and aerosol instruments for more than 100 h on 12 different days. Aerosol compositions, including fresh and processed sea salt, biomassburning particles, organics, and sulfates mixed with organics, varied between flights. Observations in a dense arctic haze on 19 April and above, within, and below the single-layer stratocumulus on 8 and 26 April are enabling a process-oriented understanding of how aerosols affect arctic clouds. Inhomogeneities in reflectivity, a close coupling of upward and downward Doppler motion, and a nearly constant ice profile in the single-layer stratocumulus suggests that vertical mixing is responsible for its longevity observed during ISDAC. Data acquired in cirrus on flights between Barrow and Fairbanks, Alaska, are improving the understanding of the performance of cloud probes in ice. Furthermore, ISDAC data will improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and determine the extent to which surface measurements can provide retrievals of aerosols, clouds, precipitation, and radiative heating.« less

Optical and Chemical Characterization of Aerosols Produced from Cooked Meats

NASA Astrophysics Data System (ADS)

Niedziela, R. F.; Foreman, E.; Blanc, L. E.

2011-12-01

Cooking processes can release a variety compounds into the air immediately above a cooking surface. The distribution of compounds will largely depend on the type of food that is being processed and the temperatures at which the food is prepared. High temperatures release compounds from foods like meats and carry them away from the preparation surface into cooler regions where condensation into particles can occur. Aerosols formed in this manner can impact air quality, particularly in urban areas where the amount of food preparation is high. Reported here are the results of laboratory experiments designed to optically and chemically characterize aerosols derived from cooking several types of meats including ground beef, salmon, chicken, and pork both in an inert atmosphere and in synthetic air. The laboratory-generated aerosols are studied using a laminar flow cell that is configured to accommodate simultaneous optical characterization in the mid-infrared and collection of particles for subsequent chemical analysis by gas chromatography. Preliminary optical results in the visible and ultra-violet will also be presented.

Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

NASA Astrophysics Data System (ADS)

Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

2018-04-01

In the frame of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), we analyse the budget of primary aerosols and secondary inorganic aerosols over the Mediterranean Basin during the years 2012 and 2013. To do this, we use two year-long numerical simulations with the chemistry-transport model MOCAGE validated against satellite- and ground-based measurements. The budget is presented on an annual and a monthly basis on a domain covering 29 to 47° N latitude and 10° W to 38° E longitude. The years 2012 and 2013 show similar seasonal variations. The desert dust is the main contributor to the annual aerosol burden in the Mediterranean region with a peak in spring, and sea salt being the second most important contributor. The secondary inorganic aerosols, taken as a whole, contribute a similar level to sea salt. The results show that all of the considered aerosol types, except for sea salt aerosols, experience net export out of our Mediterranean Basin model domain, and thus this area should be considered as a source region for aerosols globally. Our study showed that 11 % of the desert dust, 22.8 to 39.5 % of the carbonaceous aerosols, 35 % of the sulfate and 9 % of the ammonium emitted or produced into the study domain are exported. The main sources of variability for aerosols between 2012 and 2013 are weather-related variations, acting on emissions processes, and the episodic import of aerosols from North American fires. In order to assess the importance of the anthropogenic emissions of the marine and the coastal areas which are central for the economy of the Mediterranean Basin, we made a sensitivity test simulation. This simulation is similar to the reference simulation but with the removal of the international shipping emissions and the anthropogenic emissions over a 50 km wide band inland along the coast. We showed that around 30 % of the emissions of carbonaceous aerosols and 35 to 60 % of the exported carbonaceous aerosols originates from the marine and coastal areas. The formation of 23, 27 and 27 %, respectively of, ammonium, nitrate and sulfate aerosols is due to the emissions within the marine and coastal area.

Quantification of model uncertainty in aerosol optical thickness retrieval from Ozone Monitoring Instrument (OMI) measurements

NASA Astrophysics Data System (ADS)

Määttä, A.; Laine, M.; Tamminen, J.; Veefkind, J. P.

2013-09-01

We study uncertainty quantification in remote sensing of aerosols in the atmosphere with top of the atmosphere reflectance measurements from the nadir-viewing Ozone Monitoring Instrument (OMI). Focus is on the uncertainty in aerosol model selection of pre-calculated aerosol models and on the statistical modelling of the model inadequacies. The aim is to apply statistical methodologies that improve the uncertainty estimates of the aerosol optical thickness (AOT) retrieval by propagating model selection and model error related uncertainties more realistically. We utilise Bayesian model selection and model averaging methods for the model selection problem and use Gaussian processes to model the smooth systematic discrepancies from the modelled to observed reflectance. The systematic model error is learned from an ensemble of operational retrievals. The operational OMI multi-wavelength aerosol retrieval algorithm OMAERO is used for cloud free, over land pixels of the OMI instrument with the additional Bayesian model selection and model discrepancy techniques. The method is demonstrated with four examples with different aerosol properties: weakly absorbing aerosols, forest fires over Greece and Russia, and Sahara dessert dust. The presented statistical methodology is general; it is not restricted to this particular satellite retrieval application.

Cloud Condensation Nuclei Prediction Error from Application of Kohler Theory: Importance for the Aerosol Indirect Effect

NASA Technical Reports Server (NTRS)

Sotiropoulou, Rafaella-Eleni P.; Nenes, Athanasios; Adams, Peter J.; Seinfeld, John H.

2007-01-01

In situ observations of aerosol and cloud condensation nuclei (CCN) and the GISS GCM Model II' with an online aerosol simulation and explicit aerosol-cloud interactions are used to quantify the uncertainty in radiative forcing and autoconversion rate from application of Kohler theory. Simulations suggest that application of Koehler theory introduces a 10-20% uncertainty in global average indirect forcing and 2-11% uncertainty in autoconversion. Regionally, the uncertainty in indirect forcing ranges between 10-20%, and 5-50% for autoconversion. These results are insensitive to the range of updraft velocity and water vapor uptake coefficient considered. This study suggests that Koehler theory (as implemented in climate models) is not a significant source of uncertainty for aerosol indirect forcing but can be substantial for assessments of aerosol effects on the hydrological cycle in climatically sensitive regions of the globe. This implies that improvements in the representation of GCM subgrid processes and aerosol size distribution will mostly benefit indirect forcing assessments. Predictions of autoconversion, by nature, will be subject to considerable uncertainty; its reduction may require explicit representation of size-resolved aerosol composition and mixing state.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gaffney, Jeffrey

This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

NASA Astrophysics Data System (ADS)

Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-07-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms.Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (M{O/Y}D04). The M{O/Y}D04 product is of course normally produced from M{O/Y}D021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a M{O/Y}D021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source.We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

NASA Technical Reports Server (NTRS)

Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-01-01

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Assessment of aerosol optics, microphysics, and transport process of biomass-burning haze over northern SE Asia: 7-SEAS AERONET observations

NASA Astrophysics Data System (ADS)

Wang, S.; Giles, D. M.; Eck, T. F.; Lin, N.; Tsay, S.; Holben, B. N.

2013-12-01

Initiated in 2007, the Seven South East Asian Studies (7-SEAS) is aimed to facilitate an interdisciplinary research on the aerosol environment in SE Asia (SEA) as a whole, promote international collaboration, and further enhance scientific understanding of the impact of biomass burning on clouds, atmospheric radiation, hydrological cycle, and region climates. One of the key measurements proposed in the 7-SEAS is the NASA/AERONET (AErosol RObotic NETwork) observation, which provides helpful information on columnar aerosol optical properties and allows us consistently to examine biomass-burning aerosols across northern SEA from ground-based remote-sensing point of view. In this presentation, we will focus on the two 7-SEAS field deployments, i.e. the 2012 Son La Experiment and the 2013 BASELInE (Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles and Interactions Experiment). We analyze the daytime variation of aerosol by using consistent measurements from 15 of AERONET sites over Indochina, the South China Sea, and Taiwan. Spatiotemporal characteristics of aerosol optical properties (e.g., aerosol optical depth (AOD), fine/coarse mode AOD, single-scattering albedo, asymmetry factor) will be discussed. Strong diurnal variation of aerosol optical properties was observed to be attributed to planetary boundary layer (PBL) dynamics. A comparison between aerosol loading (i.e. AOD) and surface PM2.5 concentration will be presented. Our results demonstrate that smoke aerosols emitted from agriculture burning that under certain meteorological conditions can degrade regional air quality 3000 km from the source region, with additional implications for aerosol radiative forcing and regional climate change over northern SE Asia.

Comparisons of spectral aerosol single scattering albedo in Seoul, South Korea

NASA Astrophysics Data System (ADS)

Mok, Jungbin; Krotkov, Nickolay A.; Torres, Omar; Jethva, Hiren; Li, Zhanqing; Kim, Jhoon; Koo, Ja-Ho; Go, Sujung; Irie, Hitoshi; Labow, Gordon; Eck, Thomas F.; Holben, Brent N.; Herman, Jay; Loughman, Robert P.; Spinei, Elena; Lee, Seoung Soo; Khatri, Pradeep; Campanelli, Monica

2018-04-01

Quantifying aerosol absorption at ultraviolet (UV) wavelengths is important for monitoring air pollution and aerosol amounts using current (e.g., Aura/OMI) and future (e.g., TROPOMI, TEMPO, GEMS, and Sentinel-4) satellite measurements. Measurements of column average atmospheric aerosol single scattering albedo (SSA) are performed on the ground by the NASA AERONET in the visible (VIS) and near-infrared (NIR) wavelengths and in the UV-VIS-NIR by the SKYNET networks. Previous comparison studies have focused on VIS and NIR wavelengths due to the lack of co-incident measurements of aerosol and gaseous absorption properties in the UV. This study compares the SKYNET-retrieved SSA in the UV with the SSA derived from a combination of AERONET, MFRSR, and Pandora (AMP) retrievals in Seoul, South Korea, in spring and summer 2016. The results show that the spectrally invariant surface albedo assumed in the SKYNET SSA retrievals leads to underestimated SSA compared to AMP values at near UV wavelengths. Re-processed SKYNET inversions using spectrally varying surface albedo, consistent with the AERONET retrieval improve agreement with AMP SSA. The combined AMP inversions allow for separating aerosol and gaseous (NO2 and O3) absorption and provide aerosol retrievals from the shortest UVB (305 nm) through VIS to NIR wavelengths (870 nm).

A prototype single-port device for pressurized intraperitoneal aerosol chemotherapy. Technical feasibility and local drug distribution.

PubMed

Seitenfus, Rafael; Ferreira, Paulo Roberto Walter; Santos, Gabriel Oliveira Dos; Alves, Rafael José Vargas; Kalil, Antonio Nocchi; Barros, Eduardo Dipp de; Glehen, Olivier; Casagrande, Thaís Andrade Costa; Bonin, Eduardo Aimoré; Silva Junior, Edison Martins da

2017-12-01

To evaluate the technical feasibility and homogeneity of drug distribution of pressurized intraperitoneal aerosol chemotherapy (PIPAC) based on a novel process of intraperitoneal drug application (multidirectional aerosolization). This was an in vivo experimental study in pigs. A single-port device was manufactured at the smallest diameter possible for multidirectional aerosolization of the chemotherapeutic drug under positive intraperitoneal pressure. Four domestic pigs were used in the study, one control animal that received multidirectional microjets of 9 mL/sec for 30 min and three animals that received multidirectional aerosolization (pig 02: 9 mL/sec for 30 min; pigs 03 and 04: 3 mL/sec for 15 min). Aerosolized silver nitrate solution was applied for anatomopathological evaluation of intraperitoneal drug distribution. Injection time was able to maintain the pneumoperitoneum pressure below 20 mmHg. The rate of moderate silver nitrate staining was 45.4% for pig 01, 36.3% for pig 02, 36.3% for pig 03, and 72.7% for pig 04. Intra-abdominal drug distribution had a broad pattern, especially in animals exposed to the drug for 30 min. Our sample of only four animals was not large enough to demonstrate an association between aerosolization and a higher silver nitrate concentration in the stained abdominal regions.

Aerosol impacts on deep convective storms in the tropics: A combination of modeling and observations

NASA Astrophysics Data System (ADS)

Storer, Rachel Lynn

It is widely accepted that increasing the number of aerosols available to act as cloud condensation nuclei (CCN) will have significant effects on cloud properties, both microphysical and dynamical. This work focuses on the impacts of aerosols on deep convective clouds (DCCs), which experience more complicated responses than warm clouds due to their strong dynamical forcing and the presence of ice processes. Several previous studies have seen that DCCs may be invigorated by increasing aerosols, though this is not the case in all scenarios. The precipitation response to increased aerosol concentrations is also mixed. Often precipitation is thought to decrease due to a less efficient warm rain process in polluted clouds, yet convective invigoration would lead to an overall increase in surface precipitation. In this work, modeling and observations are both used in order to enhance our understanding regarding the effects of aerosols on DCCs. Specifically, the area investigated is the tropical East Atlantic, where dust from the coast of Africa frequently is available to interact with convective storms over the ocean. The first study investigates the effects of aerosols on tropical DCCs through the use of numerical modeling. A series of large-scale, two-dimensional cloud-resolving model simulations was completed, differing only in the concentration of aerosols available to act as CCN. Polluted simulations contained more deep convective clouds, wider storms, higher cloud tops and more convective precipitation across the entire domain. Differences in the warm cloud microphysical processes were largely consistent with aerosol indirect theory, and the average precipitation produced in each DCC column decreased with increasing aerosol concentration. A detailed microphysical budget analysis showed that the reduction in collision and coalescence largely dominated the trend in surface precipitation; however the production of rain through the melting of ice, though it also decreased, became more important as the aerosol concentration increased. The DCCs in polluted simulations contained more frequent, stronger updrafts and downdrafts, but the average updraft speed decreased with increasing aerosols in DCCs above 6 km. An examination of the buoyancy term of the vertical velocity equation demonstrates that the drag associated with condensate loading is an important factor in determining the average updraft strength. The largest contributions to latent heating in DCCs were cloud nucleation and vapor deposition onto water and ice, but changes in latent heating were, on average, an order of magnitude smaller than those in the condensate loading term. It is suggested that the average updraft is largely influenced by condensate loading in the more extensive stratiform regions of the polluted storms, while invigoration in the convective core leads to stronger updrafts and higher cloud tops. The goal of the second study was to examine observational data for evidence that would support the findings of the modeling work. In order to do this, four years of CloudSat data were analyzed over a region of the East Atlantic, chosen for the similarity (in meteorology and the presence of aerosols) to the modeling study. The satellite data were combined with information about aerosols taken from the output of a global transport model, and only those profiles fitting the definition of deep convective clouds were analyzed. Overall, the cloud center of gravity, cloud top, rain top, and ice water path were all found to increase with increased aerosol loading. These findings are in agreement with what was found in the modeling work, and are suggestive of convective invigoration with increased aerosols. In order to separate environmental effects from that due to aerosols, the data were sorted by environmental convective available potential energy (CAPE) and lower tropospheric static stability (LTSS). The aerosol effects were found to be largely independent of the environment. A simple statistical test suggests that the difference between the cleanest and most polluted clouds sampled are significant, lending credence to the hypothesis of convective invigoration. This is the first time evidence of deep convective invigoration has been demonstrated within a large region and over a long time period, and it is quite promising that there are many similarities between the modeling and observational results.

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

NASA Astrophysics Data System (ADS)

Lee, H.-H.; Chen, S.-H.; Kleeman, M. J.; Zhang, H.; DeNero, S. P.; Joe, D. K.

2015-11-01

The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-dimensional chemical variable (X, Z, Y, Size Bins, Source Types, Species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and longwave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into CCN at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

Sources, Sinks, and Transatlantic Transport of North African Dust Aerosol: A Multimodel Analysis and Comparison With Remote Sensing Data

NASA Technical Reports Server (NTRS)

Kim, Dongchul; Chin, Mian; Yu, Hongbin; Diehl, Thomas; Tan, Qian; Kahn, Ralph A.; Tsigaridis, Kostas; Bauer, Susanne E.; Takemura, Toshihiko; Pozzoli, Luca;

Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

PubMed

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

Physico-chemical properties of aerosols in Sao Paulo, Brazil and mechanisms of secondary organic aerosol formation.

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Ferreira de Brito, Joel; Varanda Rizzo, Luciana; Luiza Godoy, Maria; Godoy, Jose Marcus

2013-04-01

Megacities emissions are increasingly becoming a global issue, where emissions from the transportation sector play an increasingly important role. Sao Paulo is a megacity with a population of about 18 million people, 7 million cars and large-scale industrial emissions. As a result of the vehicular and industrial emissions, the air quality in Sao Paulo is bellow WMO standards for aerosol particles and ozone. Many uncertainties are found on gas- and particulate matter vehicular emission factors and their following atmospheric processes, e.g. secondary organic aerosol formation. Due to the uniqueness of the vehicular fuel in Brazil, largely based on ethanol use, such characterization currently holds further uncertainties. To improve the understanding of the role of this unique emission characteristics, we are running a source apportionment study in Sao Paulo focused on the mechanisms of organic aerosol formation. One of the goals of this study is a quantitative aerosol source apportionment focused on vehicular emissions, including ethanol and gasohol (both fuels used by light-duty vehicles). This study comprises four sampling sites with continuous measurements for one year, where trace elements and organic aerosol are being measured for PM2.5 and PM10 along with real-time NOx, O3, PM10 and CO measurements. Aerosol optical properties and size distribution are being measured on a rotation basis between sampling stations. Furthermore, a Proton-Transfer-Reaction Mass Spectrometer (PTR-MS) and an Aerosol Chemical Speciation Monitor (ACSM) are used to measure in real time VOCs and aerosol composition, respectively. Trace elements were measured using XRF and OC/EC analysis was determined with a Sunset OC/EC instrument. A TSI Nephelometer with 3 wavelengths measure light scattering and a MAAP measure black carbon. Results show aerosol number concentrations ranging between 10,000 and 35,000 cm-3, mostly concentrated in the nucleation and Aitken modes, with a peak in size at 80-120 nm. Average mass concentrations were measured at 11.5 ug/m3 and 30.7 ug/m3 for fine and coarse mode, respectively. The elemental analysis shows that Fe, Si and Al dominate the coarse mode indicating strong contribution from soil dust resuspension whereas sulfur dominates the fine mode (0.8 micrograms/m3). Scattering coefficients typically range between 20 and 150 Mm-1 at 637 nm, and absorption varied between 10 to 60 Mm-1 at 637 nm, respectively, both of them peaking at 7:00 local time, the morning rush hour. The corresponding single scattering albedo varies between 0.50 and 0.80, indicating a significant contribution of primary soot particles to the aerosol population. Organic aerosol accounts for 70% of the aerosol mass, with nitrates accounting for 11.7%, ammonia 8.4%, sulfate 8.2% and chlorine 1.6% pf PM1 measured by AMS techniques. Most of the organic aerosol were oxygenated. Several new particle formation events were observed, with a clear increase in organic aerosol and VOCs amounts associated with new particle formation. The study allows the characterization of a unique fueled fleet emissions and its impact on atmospheric chemistry, particle formation and other atmospheric dynamic processes. This work was funded by Petrobras S/A

Impact of Aerosols on Convective Clouds and Precipitation

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong

2011-01-01

Aerosols are a critical factor in the atmospheric hydrological cycle and radiation budget. As a major reason for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosol effects on clouds could further extend to precipitation, both through the formation of cloud particles and by exerting persistent radiative forcing on the climate system that disturbs dynamics. However, the various mechanisms behind these effects, in particular the ones connected to precipitation, are not yet well understood. The atmospheric and climate communities have long been working to gain a better grasp of these critical effects and hence to reduce the significant uncertainties in climate prediction resulting from such a lack of adequate knowledge. The central theme of this paper is to review past efforts and summarize our current understanding of the effect of aerosols on precipitation processes from theoretical analysis of microphysics, observational evidence, and a range of numerical model simulations. In addition, the discrepancy between results simulated by models, as well as that between simulations and observations will be presented. Specifically, this paper will address the following topics: (1) fundamental theories of aerosol effects on microphysics and precipitation processes, (2) observational evidence of the effect of aerosols on precipitation processes, (3) signatures of the aerosol impact on precipitation from large-scale analyses, (4) results from cloud-resolving model simulations, and (5) results from large-scale numerical model simulations. Finally, several future research directions on aerosol - precipitation interactions are suggested.

Impact of Aerosols on Convective Clouds and Precipitation

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Chen, Jen-Ping; Li, Zhanqing; Wang, Chien; Zhang, Chidong

2012-01-01

Aerosols are a critical factor in the atmospheric hydrological cycle and radiation budget. As a major agent for clouds to form and a significant attenuator of solar radiation, aerosols affect climate in several ways. Current research suggests that aerosol effects on clouds could further extend to precipitation, both through the formation of cloud particles and by exerting persistent radiative forcing on the climate system that disturbs dynamics. However, the various mechanisms behind these effects, in particular the ones connected to precipitation, are not yet well understood. The atmospheric and climate communities have long been working to gain a better grasp of these critical effects and hence to reduce the significant uncertainties in climate prediction resulting from such a lack of adequate knowledge. Here we review past efforts and summarize our current understanding of the effect of aerosols on convective precipitation processes from theoretical analysis of microphysics, observational evidence, and a range of numerical model simulations. In addition, the discrepancy between results simulated by models, as well as that between simulations and observations, are presented. Specifically, this paper addresses the following topics: (1) fundamental theories of aerosol effects on microphysics and precipitation processes, (2) observational evidence of the effect of aerosols on precipitation processes, (3) signatures of the aerosol impact on precipitation from largescale analyses, (4) results from cloud-resolving model simulations, and (5) results from large-scale numerical model simulations. Finally, several future research directions for gaining a better understanding of aerosol--cloud-precipitation interactions are suggested.

Cloud Condensation Nuclei Activity of Aerosols during GoAmazon 2014/15 Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, J.; Martin, S. T.; Kleinman, L.

2016-03-01

Aerosol indirect effects, which represent the impact of aerosols on climate through influencing the properties of clouds, remain one of the main uncertainties in climate predictions (Stocker et al. 2013). Reducing this large uncertainty requires both improved understanding and representation of aerosol properties and processes in climate models, including the cloud activation properties of aerosols. The Atmospheric System Research (ASR) science program plan of January 2010 states that: “A key requirement for simulating aerosol-cloud interactions is the ability to calculate cloud condensation nuclei and ice nuclei (CCN and IN, respectively) concentrations as a function of supersaturation from the chemical andmore » microphysical properties of the aerosol.” The Observations and Modeling of the Green Ocean Amazon (GoAmazon 2014/15) study seeks to understand how aerosol and cloud life cycles are influenced by pollutant outflow from a tropical megacity (Manaus)—in particular, the differences in cloud-aerosol-precipitation interactions between polluted and pristine conditions. One key question of GoAmazon2014/5 is: “What is the influence of the Manaus pollution plume on the cloud condensation nuclei (CCN) activities of the aerosol particles and the secondary organic material in the particles?” To address this question, we measured size-resolved CCN spectra, a critical measurement for GoAmazon2014/5.« less

Radiative Importance of Aerosol-Cloud Interaction

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee

1999-01-01

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.

The generation of diesel exhaust particle aerosols from a bulk source in an aerodynamic size range similar to atmospheric particles

PubMed Central

Cooney, Daniel J; Hickey, Anthony J

2008-01-01

The influence of diesel exhaust particles (DEP) on the lungs and heart is currently a topic of great interest in inhalation toxicology. Epidemiological data and animal studies have implicated airborne particulate matter and DEP in increased morbidity and mortality due to a number of cardiopulmonary diseases including asthma, chronic obstructive pulmonary disorder, and lung cancer. The pathogeneses of these diseases are being studied using animal models and cell culture techniques. Real-time exposures to freshly combusted diesel fuel are complex and require significant infrastructure including engine operations, dilution air, and monitoring and control of gases. A method of generating DEP aerosols from a bulk source in an aerodynamic size range similar to atmospheric DEP would be a desirable and useful alternative. Metered dose inhaler technology was adopted to generate aerosols from suspensions of DEP in the propellant hydrofluoroalkane 134a. Inertial impaction data indicated that the particle size distributions of the generated aerosols were trimodal, with count median aerodynamic diameters less than 100 nm. Scanning electron microscopy of deposited particles showed tightly aggregated particles, as would be expected from an evaporative process. Chemical analysis indicated that there were no major changes in the mass proportion of 2 specific aromatic hydrocarbons (benzo[a]pyrene and benzo[k]fluoranthene) in the particles resulting from the aerosolization process. PMID:19337412

Evaluation of a new microphysical aerosol module in the ECMWF Integrated Forecasting System

NASA Astrophysics Data System (ADS)

Woodhouse, Matthew; Mann, Graham; Carslaw, Ken; Morcrette, Jean-Jacques; Schulz, Michael; Kinne, Stefan; Boucher, Olivier

2013-04-01

The Monitoring Atmospheric Composition and Climate II (MACC-II) project will provide a system for monitoring and predicting atmospheric composition. As part of the first phase of MACC, the GLOMAP-mode microphysical aerosol scheme (Mann et al., 2010, GMD) was incorporated within the ECMWF Integrated Forecasting System (IFS). The two-moment modal GLOMAP-mode scheme includes new particle formation, condensation, coagulation, cloud-processing, and wet and dry deposition. GLOMAP-mode is already incorporated as a module within the TOMCAT chemistry transport model and within the UK Met Office HadGEM3 general circulation model. The microphysical, process-based GLOMAP-mode scheme allows an improved representation of aerosol size and composition and can simulate aerosol evolution in the troposphere and stratosphere. The new aerosol forecasting and re-analysis system (known as IFS-GLOMAP) will also provide improved boundary conditions for regional air quality forecasts, and will benefit from assimilation of observed aerosol optical depths in near real time. Presented here is an evaluation of the performance of the IFS-GLOMAP system in comparison to in situ aerosol mass and number measurements, and remotely-sensed aerosol optical depth measurements. Future development will provide a fully-coupled chemistry-aerosol scheme, and the capability to resolve nitrate aerosol.

Assessing Impact of Aerosol Intercontinental Transport on Regional Air Quality and Climate: What Satellites Can Help

NASA Technical Reports Server (NTRS)

Yu, Hongbin

2011-01-01

Mounting evidence for intercontinental transport of aerosols suggests that aerosols from a region could significantly affect climate and air quality in downwind regions and continents. Current assessment of these impacts for the most part has been based on global model simulations that show large variability. The aerosol intercontinental transport and its influence on air quality and climate involve many processes at local, regional, and intercontinental scales. There is a pressing need to establish modeling systems that bridge the wide range of scales. The modeling systems need to be evaluated and constrained by observations, including satellite measurements. Columnar loadings of dust and combustion aerosols can be derived from the MODIS and MISR measurements of total aerosol optical depth and particle size and shape information. Characteristic transport heights of dust and combustion aerosols can be determined from the CALIPSO lidar and AIRS measurements. CALIPSO liar and OMI UV technique also have a unique capability of detecting aerosols above clouds, which could offer some insights into aerosol lofting processes and the importance of above-cloud transport pathway. In this presentation, I will discuss our efforts of integrating these satellite measurements and models to assess the significance of intercontinental transport of dust and combustion aerosols on regional air quality and climate.

Lidar-Radiometer Inversion Code (LIRIC) for the Retrieval of Vertical Aerosol Properties from Combined Lidar Radiometer Data: Development and Distribution in EARLINET

NASA Technical Reports Server (NTRS)

Chaikovsky, A.; Dubovik, O.; Holben, Brent N.; Bril, A.; Goloub, P.; Tanre, D.; Pappalardo, G.; Wandinger, U.; Chaikovskaya, L.; Denisov, S.;

Downscaling Aerosols and the Impact of Neglected Subgrid Processes on Direct Aerosol Radiative Forcing for a Representative Global Climate Model Grid Spacing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gustafson, William I.; Qian, Yun; Fast, Jerome D.

2011-07-13

Recent improvements to many global climate models include detailed, prognostic aerosol calculations intended to better reproduce the observed climate. However, the trace gas and aerosol fields are treated at the grid-cell scale with no attempt to account for sub-grid impacts on the aerosol fields. This paper begins to quantify the error introduced by the neglected sub-grid variability for the shortwave aerosol radiative forcing for a representative climate model grid spacing of 75 km. An analysis of the value added in downscaling aerosol fields is also presented to give context to the WRF-Chem simulations used for the sub-grid analysis. We foundmore » that 1) the impact of neglected sub-grid variability on the aerosol radiative forcing is strongest in regions of complex topography and complicated flow patterns, and 2) scale-induced differences in emissions contribute strongly to the impact of neglected sub-grid processes on the aerosol radiative forcing. The two of these effects together, when simulated at 75 km vs. 3 km in WRF-Chem, result in an average daytime mean bias of over 30% error in top-of-atmosphere shortwave aerosol radiative forcing for a large percentage of central Mexico during the MILAGRO field campaign.« less

Spatial and temporal variations of aerosols around Beijing in summer 2006: 2. Local and column aerosol optical properties

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Fast, J. D.; PöSchl, U.; Garland, R. M.; Andreae, M. O.; Wiedensohler, A.; Sugimoto, N.; Zhu, T.

2010-11-01

Model calculations were conducted using the Weather Research and Forecasting model coupled with chemistry (WRF-chem) for the region around Beijing, China, in the summer of 2006, when the CAREBeijing-2006 intensive campaign was conducted. In this paper, we interpret aerosol optical properties in terms of aerosol mass concentrations and their chemical compositions by linking model calculations with measurements. The model calculations generally captured the observed variability of various surface and column aerosol optical parameters in and around Beijing. At the surface, the spatial and temporal variations of aerosol absorption and scattering coefficients corresponded well to those of elemental carbon and sulfate mass concentrations, respectively, and were controlled by local-scale (<100 km and <24 hours) and regional-scale (<500 km and <3 days) emissions, respectively. The contribution of secondary aerosols and their water uptake increased with altitude within the planetary boundary layer. This variation led to a considerable increase in column aerosol optical depth and was responsible for the differences in regional and temporal variations between surface and column aerosol optical properties around Beijing. These processes are expected to be common in other megacity regions as well. Model calculations, however, underestimated or overestimated the absolute levels of aerosol optical properties in and around Beijing by up to 60%. Sensitivity studies showed that these discrepancies were mostly due to the uncertainties in aerosol mixing state and aerosol density (affecting mass extinction efficiency) in the model calculations. Good agreement with measurements is achieved when these aerosol properties are accurately predicted or assumed; however, significant bias can result when these properties are inadequately treated, even if total aerosol mass concentrations are reproduced well in the model calculations.

10 CFR 32.26 - Gas and aerosol detectors containing byproduct material: Requirements for license to manufacture...

Code of Federal Regulations, 2014 CFR

2014-01-01

... 10 Energy 1 2014-01-01 2014-01-01 false Gas and aerosol detectors containing byproduct material... CONTAINING BYPRODUCT MATERIAL Exempt Concentrations and Items § 32.26 Gas and aerosol detectors containing... application for a specific license to manufacture, process, or produce gas and aerosol detectors containing...

10 CFR 32.26 - Gas and aerosol detectors containing byproduct material: Requirements for license to manufacture...

Code of Federal Regulations, 2013 CFR

2013-01-01

... 10 Energy 1 2013-01-01 2013-01-01 false Gas and aerosol detectors containing byproduct material... CONTAINING BYPRODUCT MATERIAL Exempt Concentrations and Items § 32.26 Gas and aerosol detectors containing... application for a specific license to manufacture, process, or produce gas and aerosol detectors containing...

Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: an AQMEII-2 perspective

EPA Science Inventory

The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model in...

Enviro-HIRLAM/ HARMONIE Studies in ECMWF HPC EnviroAerosols Project

NASA Astrophysics Data System (ADS)

Hansen Sass, Bent; Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander; Palamarchuk, Julia; Ivanov, Serguei; Pagh Nielsen, Kristian; Penenko, Alexey; Edvardsson, Nellie; Stysiak, Aleksander Andrzej; Bostanbekov, Kairat; Amstrup, Bjarne; Yang, Xiaohua; Ruban, Igor; Bergen Jensen, Marina; Penenko, Vladimir; Nurseitov, Daniyar; Zakarin, Edige

2017-04-01

The EnviroAerosols on ECMWF HPC project (2015-2017) "Enviro-HIRLAM/ HARMONIE model research and development for online integrated meteorology-chemistry-aerosols feedbacks and interactions in weather and atmospheric composition forecasting" is aimed at analysis of importance of the meteorology-chemistry/aerosols interactions and to provide a way for development of efficient techniques for on-line coupling of numerical weather prediction and atmospheric chemical transport via process-oriented parameterizations and feedback algorithms, which will improve both the numerical weather prediction and atmospheric composition forecasts. Two main application areas of the on-line integrated modelling are considered: (i) improved numerical weather prediction with short-term feedbacks of aerosols and chemistry on formation and development of meteorological variables, and (ii) improved atmospheric composition forecasting with on-line integrated meteorological forecast and two-way feedbacks between aerosols/chemistry and meteorology. During 2015-2016 several research projects were realized. At first, the study on "On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies" focused on assessment of scenarios with accidental and continuous emissions of sulphur dioxide for case studies for Atyrau (Kazakhstan) near the northern part of the Caspian Sea and metallurgical enterprises on the Kola Peninsula (Russia), with GIS integration of modelling results into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system. At second, the studies on "The sensitivity of precipitation simulations to the soot aerosol presence" & "The precipitation forecast sensitivity to data assimilation on a very high resolution domain" focused on sensitivity and changes in precipitation life-cycle under black carbon polluted conditions over Scandinavia. At third, studies on "Aerosol effects over China investigated with a high resolution convection permitting weather model" & "Meteorological and chemical urban scale modelling for Shanghai metropolitan area" with focus on aerosol effects and influence of urban areas in China at regional-subregional-urban scales. At fourth, study on "Direct variational data assimilation algorithm for atmospheric chemistry data with transport and transformation model" with focus on testing chemical data assimilation algorithm of in situ concentration measurements on real data scenario. At firth, study on "Aerosol influence on High Resolution NWP HARMONIE Operational Forecasts" with focus on impact of sea salt aerosols on numerical weather prediction during low precipitation events. And finally, study on "Impact of regional afforestation on climatic conditions in metropolitan areas: case study of Copenhagen" with focus on impact of forest and land-cover change on formation and development of temperature regimes in the Copenhagen metropolitan area of Denmark. Selected results and findings will be presented and discussed.

Local and regional components of aerosol in a heavily trafficked street canyon in central London derived from PMF and cluster analysis of single-particle ATOFMS spectra.

PubMed

Giorio, Chiara; Tapparo, Andrea; Dall'Osto, Manuel; Beddows, David C S; Esser-Gietl, Johanna K; Healy, Robert M; Harrison, Roy M

2015-03-17

Positive matrix factorization (PMF) has been applied to single particle ATOFMS spectra collected on a six lane heavily trafficked road in central London (Marylebone Road), which well represents an urban street canyon. PMF analysis successfully extracted 11 factors from mass spectra of about 700,000 particles as a complement to information on particle types (from K-means cluster analysis). The factors were associated with specific sources and represent the contribution of different traffic related components (i.e., lubricating oils, fresh elemental carbon, organonitrogen and aromatic compounds), secondary aerosol locally produced (i.e., nitrate, oxidized organic aerosol and oxidized organonitrogen compounds), urban background together with regional transport (aged elemental carbon and ammonium) and fresh sea spray. An important result from this study is the evidence that rapid chemical processes occur in the street canyon with production of secondary particles from road traffic emissions. These locally generated particles, together with aging processes, dramatically affected aerosol composition producing internally mixed particles. These processes may become important with stagnant air conditions and in countries where gasoline vehicles are predominant and need to be considered when quantifying the impact of traffic emissions.

Contrasting aerosol refractive index and hygroscopicity in the inflow and outflow of deep convective storms: Analysis of airborne data from DC3

NASA Astrophysics Data System (ADS)

Sorooshian, Armin; Shingler, T.; Crosbie, E.; Barth, M. C.; Homeyer, C. R.; Campuzano-Jost, P.; Day, D. A.; Jimenez, J. L.; Thornhill, K. L.; Ziemba, L. D.; Blake, D. R.; Fried, A.

2017-04-01

We examine three case studies during the Deep Convective Clouds and Chemistry (DC3) field experiment when storm inflow and outflow air were sampled for aerosol subsaturated hygroscopicity and the real part of refractive index (n) with a Differential Aerosol Sizing and Hygroscopicity Probe (DASH-SP) on the NASA DC-8. Relative to inflow aerosol particles, outflow particles were more hygroscopic (by 0.03 based on the estimated κ parameter) in one of the three storms examined. Two of three "control" flights with no storm convection reveal higher κ values, albeit by only 0.02, at high altitude (> 8 km) versus < 4 km. Entrainment modeling shows that measured κ values in the outflow of the three storm flights are higher than predicted values (by 0.03-0.11) based on knowledge of κ values from the inflow and clear air adjacent to the storms. This suggests that other process(es) contributed to hygroscopicity enhancements such as secondary aerosol formation via aqueous-phase chemistry. Values of n were higher in the outflow of two of the three storm flights, reaching as high as 1.54. More statistically significant differences were observed in control flights (no storms) where n decreased from 1.50-1.52 (< 4 km) to 1.49-1.50 (> 8 km). Chemical data show that enhanced hygroscopicity was coincident with lower organic mass fractions, higher sulfate mass fractions, and higher O:C ratios of organic aerosol. Refractive index did not correlate as well with available chemical data. Deep convection is shown to alter aerosol radiative properties, which has implications for aerosol effects on climate.

Intercomparison and Evaluation of Global Aerosol Microphysical Properties Among Aerocom Models of a Range of Complexity

NASA Technical Reports Server (NTRS)

Mann, G. W.; Carslaw, K. S.; Reddington, C. L.; Pringle, K. J.; Schulz, M.; Asmi, A.; Spracklen, D. V.; Ridley, D. A.; Woodhouse, M. T.; Lee, L. A.;

Occurrence of pristine aerosol environments on a polluted planet.

PubMed

Hamilton, Douglas S; Lee, Lindsay A; Pringle, Kirsty J; Reddington, Carly L; Spracklen, Dominick V; Carslaw, Kenneth S

2014-12-30

Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol-cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present--day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions-the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty.

Aerosol radiative forcing from GEO satellite data over land surfaces

NASA Astrophysics Data System (ADS)

Costa, Maria J.; Silva, Ana M.

2005-10-01

Aerosols direct and indirect effects on the Earth's climate are widely recognized but have yet to be adequately quantified. Difficulties arise due to the very high spatial and temporal variability of aerosols, which is a major cause of uncertainties in radiative forcing studies. The effective monitoring of the global aerosol distribution is only made possible by satellite monitoring and this is the reason why the interest in aerosol observations from satellite passive radiometers is steadily increasing. From the point of view of the study of land surfaces, the atmosphere with its constituents represents an obscurant whose effects should be as much as possible eliminated, being this process sometimes referred to as atmospheric correction. In absence of clouds and using spectral intervals where gas absorption can be avoided to a great extent, only the aerosol effect remains to be corrected. The monitoring of the aerosol particles present in the atmosphere is then crucial to succeed in doing an accurate atmospheric correction, otherwise the surface properties may be inadequately characterised. However, the atmospheric correction over land surfaces turns out to be a difficult task since surface reflection competes with the atmospheric component of the signal. On the other hand, a single mean pre-established aerosol characterisation would not be sufficient for this purpose due to very high spatial and temporal variability of aerosols and their unpredictability, especially what concerns particulary intense "events" such as biomass burning and forest fires, desert dust episodes and volcanic eruptions. In this context, an operational methodology has been developed at the University of Evora - Evora Geophysics Centre (CGE), in the framework of the Satellite Application Facility for Land Surface Analysis - Land SAF, to derive an Aerosol Product from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) data, flying on the Geostationary (GEO) satellite system Meteosat-8. The aerosol characterization obtained is used to calculate the fluxes and estimate the aerosol radiative forcing at the top of the atmosphere. The methodology along with the results of the aerosol properties and radiative forcing using SEVIRI images is presented. The aerosol optical thickness results are compared with ground-based measurements from the Aerosol Robotic NETwork (AERONET), to assess the accuracy of the methodology presented.

An 11-year global gridded aerosol optical thickness reanalysis (v1.0) for atmospheric and climate sciences

NASA Astrophysics Data System (ADS)

Lynch, Peng; Reid, Jeffrey S.; Westphal, Douglas L.; Zhang, Jianglong; Hogan, Timothy F.; Hyer, Edward J.; Curtis, Cynthia A.; Hegg, Dean A.; Shi, Yingxi; Campbell, James R.; Rubin, Juli I.; Sessions, Walter R.; Turk, F. Joseph; Walker, Annette L.

2016-04-01

While stand alone satellite and model aerosol products see wide utilization, there is a significant need in numerous atmospheric and climate applications for a fused product on a regular grid. Aerosol data assimilation is an operational reality at numerous centers, and like meteorological reanalyses, aerosol reanalyses will see significant use in the near future. Here we present a standardized 2003-2013 global 1 × 1° and 6-hourly modal aerosol optical thickness (AOT) reanalysis product. This data set can be applied to basic and applied Earth system science studies of significant aerosol events, aerosol impacts on numerical weather prediction, and electro-optical propagation and sensor performance, among other uses. This paper describes the science of how to develop and score an aerosol reanalysis product. This reanalysis utilizes a modified Navy Aerosol Analysis and Prediction System (NAAPS) at its core and assimilates quality controlled retrievals of AOT from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Multi-angle Imaging SpectroRadiometer (MISR) on Terra. The aerosol source functions, including dust and smoke, were regionally tuned to obtain the best match between the model fine- and coarse-mode AOTs and the Aerosol Robotic Network (AERONET) AOTs. Other model processes, including deposition, were tuned to minimize the AOT difference between the model and satellite AOT. Aerosol wet deposition in the tropics is driven with satellite-retrieved precipitation, rather than the model field. The final reanalyzed fine- and coarse-mode AOT at 550 nm is shown to have good agreement with AERONET observations, with global mean root mean square error around 0.1 for both fine- and coarse-mode AOTs. This paper includes a discussion of issues particular to aerosol reanalyses that make them distinct from standard meteorological reanalyses, considerations for extending such a reanalysis outside of the NASA A-Train era, and examples of how the aerosol reanalysis can be applied or fused with other model or remote sensing products. Finally, the reanalysis is evaluated in comparison with other available studies of aerosol trends, and the implications of this comparison are discussed.

Evaluation of biomass burning aerosols in the HadGEM3 climate model with observations from the SAMBBA field campaign

NASA Astrophysics Data System (ADS)

Johnson, Ben T.; Haywood, James M.; Langridge, Justin M.; Darbyshire, Eoghan; Morgan, William T.; Szpek, Kate; Brooke, Jennifer K.; Marenco, Franco; Coe, Hugh; Artaxo, Paulo; Longo, Karla M.; Mulcahy, Jane P.; Mann, Graham W.; Dalvi, Mohit; Bellouin, Nicolas

2016-11-01

We present observations of biomass burning aerosol from the South American Biomass Burning Analysis (SAMBBA) and other measurement campaigns, and use these to evaluate the representation of biomass burning aerosol properties and processes in a state-of-the-art climate model. The evaluation includes detailed comparisons with aircraft and ground data, along with remote sensing observations from MODIS and AERONET. We demonstrate several improvements to aerosol properties following the implementation of the Global Model for Aerosol Processes (GLOMAP-mode) modal aerosol scheme in the HadGEM3 climate model. This predicts the particle size distribution, composition, and optical properties, giving increased accuracy in the representation of aerosol properties and physical-chemical processes over the Coupled Large-scale Aerosol Scheme for Simulations in Climate Models (CLASSIC) bulk aerosol scheme previously used in HadGEM2. Although both models give similar regional distributions of carbonaceous aerosol mass and aerosol optical depth (AOD), GLOMAP-mode is better able to capture the observed size distribution, single scattering albedo, and Ångström exponent across different tropical biomass burning source regions. Both aerosol schemes overestimate the uptake of water compared to recent observations, CLASSIC more so than GLOMAP-mode, leading to a likely overestimation of aerosol scattering, AOD, and single scattering albedo at high relative humidity. Observed aerosol vertical distributions were well captured when biomass burning aerosol emissions were injected uniformly from the surface to 3 km. Finally, good agreement between observed and modelled AOD was gained only after scaling up GFED3 emissions by a factor of 1.6 for CLASSIC and 2.0 for GLOMAP-mode. We attribute this difference in scaling factor mainly to different assumptions for the water uptake and growth of aerosol mass during ageing via oxidation and condensation of organics. We also note that similar agreement with observed AOD could have been achieved with lower scaling factors if the ratio of organic carbon to primary organic matter was increased in the models toward the upper range of observed values. Improved knowledge from measurements is required to reduce uncertainties in emission ratios for black carbon and organic carbon, and the ratio of organic carbon to primary organic matter for primary emissions from biomass burning.

The Role of Atmospheric Aerosol Concentration on Deep Convective Precipitation: Cloud-Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

2010-01-01

Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds NRC [2001]." The aerosol effect on Clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path and the "semi-direct" effect on cloud coverage. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect, is even more complex, especially for mixed-phase convective clouds. In this paper, a cloud-resolving model (CRM) with detailed spectral-bin microphysics was used to examine the effect of aerosols on three different deep convective cloud systems that developed in different geographic locations: South Florida, Oklahoma and the Central Pacific, In all three cases, rain reaches the ground earlier for the low CCN (clean) case. Rain suppression is also evident in all three cases with high CCN (dirty) case. However, this suppression only occurs during the first hour of the simulations. During the mature stages of the simulations, the effects of increasing aerosol concentration range from rain suppression in the Oklahoma case, to almost no effect in the Florida case, to rain enhancement in the Pacific case. These results show the complexity of aerosol interactions with convection. The model results suggest that evaporative cooling is a key process in determining whether high CCN reduces or enhances precipitation. Stronger evaporative cooling can produce a stronger cold pool and thus stronger low-level convergence through interactions with the low-level wind shear. Consequently, precipitation processes can be more vigorous. For example,, the evaporative cooling is more than two times stronger in the lower troposphere with high CCN for the Pacific case. Sensitivity tests also suggest that ice processes are crucial for suppressing precipitation in the Oklahoma case with high CCN.

Arctic “ozone hole” in a cold volcanic stratosphere

PubMed Central

Tabazadeh, A.; Drdla, K.; Schoeberl, M. R.; Hamill, P.; Toon, O. B.

2002-01-01

Optical depth records indicate that volcanic aerosols from major eruptions often produce clouds that have greater surface area than typical Arctic polar stratospheric clouds (PSCs). A trajectory cloud–chemistry model is used to study how volcanic aerosols could affect springtime Arctic ozone loss processes, such as chlorine activation and denitrification, in a cold winter within the current range of natural variability. Several studies indicate that severe denitrification can increase Arctic ozone loss by up to 30%. We show large PSC particles that cause denitrification in a nonvolcanic stratosphere cannot efficiently form in a volcanic environment. However, volcanic aerosols, when present at low altitudes, where Arctic PSCs cannot form, can extend the vertical range of chemical ozone loss in the lower stratosphere. Chemical processing on volcanic aerosols over a 10-km altitude range could increase the current levels of springtime column ozone loss by up to 70% independent of denitrification. Climate models predict that the lower stratosphere is cooling as a result of greenhouse gas built-up in the troposphere. The magnitude of column ozone loss calculated here for the 1999–2000 Arctic winter, in an assumed volcanic state, is similar to that projected for a colder future nonvolcanic stratosphere in the 2010 decade. PMID:11854461

A one-dimensional sectional model to simulate multicomponent aerosol dynamics in the marine boundary layer 2. Model application

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fitzgerald, James W.; Hoppel, William A.; Frick, Glendon M.

1998-07-01

The dynamics of aerosols in the marine boundary layer (MBL) are simulated with the marine boundary layer aerosol model (MARBLES), a one-dimensional, multicomponent sectional aerosol model [{ital Fitzgerald} {ital et al.}, this issue; {ital Gelbard} {ital et al.}, this issue]. First, to illustrate how the various aerosol processes influence the particle size distribution, the model was run with one or two processes operating on the same initial size distribution. Because of current interest in the effects of cloud processing of aerosols and exchange of aerosols with the free troposphere (FT) on marine aerosol size distributions, these two processes are examinedmore » in considerable detail. The simulations show that the effect of cloud processing (characteristic double-peaked size distribution) in the upper part of the MBL is manifested at the surface on a timescale that is much faster than changes due to exchange with the FT, assuming a typical exchange velocity of 0.6 cmthinsps{sup {minus}1}. The model predicts that the FT can be a significant source of particles for the MBL in the size range of the cloud-processing minimum, between the unactivated interstitial particles and the cloud condensation nuclei (CCN) which have grown as a result of conversion of dissolved SO{sub 2} to sulfate in cloud droplets. The model was also used to simulate the evolution of the aerosol size distribution in an air mass advecting from the east coast of the United States out over the ocean for up to 10 days. The modification of a continental aerosol size distribution to one that is remote marine in character occurs on a timescale of 6{endash}8 days. Nucleation was not observed in the base case 10-day advection simulation which assumed rather typical meteorological conditions. However, significant nucleation was predicted under a more favorable (albeit, atypical) combination of conditions which included significant precipitation scavenging (5 mmthinsph{sup {minus}1} of rain for 12 hours), colder temperatures by 10thinsp{degree}C (283 K at the surface decreasing to 278 K at 1000 m) and a high DMS flux (40 {mu}molthinspm{sup {minus}2}thinspd{sup {minus}1}). In a test of model self initialization, long-term (8{endash}10 days) predictions of marine aerosol size distributions were found to be essentially independent of initial conditions. {copyright} 1998 American Geophysical Union« less

A Study of Extreme Events in Subseasonal Forecasts Made by a High Resolution Version of the NCEP Climate Forecast System

NASA Astrophysics Data System (ADS)

Saha, S.; Vandendool, H. M.; Johansson, A.; Vintzileos, A.; Pan, H.; Thiaw, C.

2005-05-01

Actual estimations of the aerosol effect on the radiation budget are affected by a large uncertainties mainly due to the high inhomogeneity and variability of atmospheric aerosol, in terms of concentration, shape, size distribution, refractive index and vertical distribution. Long-term measurements of vertical profiles of aerosol optical properties are needed to reduce these uncertainties. At CNR-IMAA (40° 36'N, 15° 44' E, 760 m above sea level), a lidar system for aerosol study is operative since May 2000 in the framework of EARLINET (European Aerosol Research Lidar Network). Until August 2005, it provided independent measurements of aerosol extinction and backscatter at 355 nm and aerosol backscatter profiles at 532 nm. After an upgrade of the system, it provides independent measurements of aerosol extinction and backscatter profiles at 355 and 532 nm, and of aerosol backscatter profiles at 1064 nm and depolarization ratio at 532 nm. For these measurements, lidar ratio at 355 and 532 nm and Angstrom exponent profiles at 355/532 nm are also obtained. Starting on May 2000, systematic measurements are performed three times per week according to the EARLINET schedule and further measurements are performed in order to investigate particular events, like dust intrusions, volcanic eruptions and forest fires. A climatological study has been carried out in terms of the seasonal behavior of the PBL height and of the aerosol optical properties calculated inside the PBL itself. In the free troposphere, an high occurrences of Saharan dust intrusions (about 1 day of Saharan dust intrusion every 10 days) has been observed at CNR-IMAA because of the short distance from the Sahara region. During 6 years of observations, very peculiar cases of volcanic aerosol emitted by Etna volcano and aerosol released by large forest fires burning occurred in Alaska and Canada have been observed in the free troposphere at our site. Particular attention is devoted to lidar ratio both for the PBL and the free troposphere region, in order to study influences of aerosol modification/transportation processes on its values and its variability. ACKNOWLEDGMENTS The financial support of this work by the European Commission under grant RICA-025991 is gratefully acknowledged.

A global modeling study on carbonaceous aerosol microphysical characteristics and radiative forcing

NASA Astrophysics Data System (ADS)

Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.

2010-02-01

Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Assuming that sulfates, nitrates and secondary organics form a coating around a black carbon core, rather than forming a uniformly mixed particle, changes the overall net aerosol radiative forcing from negative to positive. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Black carbon absorption is amplified by sulfate and nitrate coatings, but even more strongly by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative forcing when sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to climate benefits.

The great Indian haze revisited: aerosol distribution effects on microphysical and optical properties of warm clouds over peninsular India

NASA Astrophysics Data System (ADS)

Ghanti, R.; Ghosh, S.

2010-03-01

The Indian subcontinent is undergoing a phase of rapid urbanisation. Inevitable fallout of this process is a concomitant increase in air pollution much of which can be attributed to the infamous great Indian haze phenomena. One observes that the aerosol size distributions vary considerably along the Bay of Bengal (BOB), Arabian Sea (AS) and the Indian Ocean (IO), although, the dynamical attributes are very similar, particularly over the BOB and the AS during this season. Unlike major European studies (e.g. Aerosol Characterization Experiment-2, Ghosh et al., 2005), there are no cloud microphysical modelling studies to complement these observational results for the Indian sub-continent. Ours is the first modelling study over this important region where a time-tested model (O'Dowd et al., 1999a; Ghosh et al., 2007; Rap et al., 2009) is used to obtain cloud microphysical and optical properties from observed aerosol size distributions. Un-activated aerosol particles and very small cloud droplets have to be treated specially to account for non-ideal effects-our model does this effectively yielding realistic estimate of cloud droplet number concentrations (Nc). Empirical relationships linking aerosol concentration to (Nc) yield a disproportionately higher Nc suggesting that such empirical formulations should be used with caution. Our modelling study reveals that the cloud's microphysical and optical properties are very similar along the AS and the BOB despite them having disparate dry aerosol spectral distributions. This is non-intuitive, as one would expect changes in microphysical development with widely different aerosol distributions. There is some increase in cloud droplet numbers with increased haze concentrations but much less than a simple proportion would indicate.

Evaluating aerosol influence on cloud models using in-situ measurements during the INUPIAQ campaign

NASA Astrophysics Data System (ADS)

Farrington, R.; Connolly, P.; Choularton, T.; Bower, K.; Lloyd, G.; Flynn, M.; Crosier, J.; Field, P.

2014-12-01

At temperatures between -35°C and 0°C, the presence of insoluble aerosols acting as ice nuclei (IN) initiate the nucleation of ice under atmospheric conditions. Previous field and laboratory campaigns have suggested that mineral dust present in the atmosphere act as IN at temperatures around -20°C (e.g. Sassen et al. 2003), however the cause of ice nucleation at temperatures of around -5°C is less certain. Coupled with the limited representation of aerosol and cloud processes in large-scale weather and climate models, the need for improved in-situ measurements of aerosol properties and cloud micro-physical processes to drive the improvement of aerosol-clouds processes in models is evident. As part of the Ice NUcleation Process Investigation and Quantification (INUPIAQ) project, two field campaigns were conducted in early 2013 and early 2014. Both campaigns included measurements of cloud micro-physical properties at the summit of Jungfraujoch in Switzerland (3580m asl). Using data from the 2013 campaign and modelling simulations from the Weather Research and Forecasting model (WRF), an upwind site, located at Schilthorn (2970m asl), was determined for measuring aerosol properties out of cloud during the 2014 campaign. Further measurements of the cloud and aerosols properties were taken remotely using a doppler LiDAR located at Kleine Scheidegg (2061m asl). The aim of this project is to determine whether detailed aerosol information is important to determining cloud and precipitation properties downwind. To this end WRF was run using the aerosol number concentrations and size distributions measured at the Schilthorn site to compare modelled ice number concentrations with measurements taken at Jungfraujoch using state of the science cloud ice probes, including the Three-View Cloud Particle Imager (3V-CPI) and the Cloud Aerosol Spectrometer with Depolarization (CAS-DPOL), with the results of the comparison presented and discussed at this meeting. ReferencesSassen, K., et al, 2003: Saharan dust storms and indirect aerosol effects on clouds: Crystal-face results. Geophys. Res. Lett., 30(12), 1633-1636.

COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thornton, Joel A.; Worsnop, Douglas

2016-09-22

This project was part of a collaborative campaign, including the participation of scientists from seven research groups as part of the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London to study wintertime sources of urban particulate matter. The UW contribution by PI Thornton’s group was to make the first deployment of a chemical ionization mass spectrometer instrument (MOVI-CI-ToFMS) to measure both particle and gas phase organic acids. The new instrument ran nearly continuously during the ClearfLo WINTER IOP at the Detlingmore » site, producing a first-ever data set of molecular composition information that can be used for source apportionment and process studies. The UW group published a paper in Environmental Science and Technology and contributed to another (Bohnenstengel et al BAMS 2015) detailing a direct molecular connection between biomass/biofuel burning particles and aerosol light absorption. The ES&T paper (Mohr, et al ES&T 2013) has received 42 citations in just 3 years indicative of its significant impact on the field. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal.« less

Connections Between Stratospheric Pollution and the Asian Summer Monsoon

NASA Technical Reports Server (NTRS)

Bauer, Susanne E.; Tsigaridis, Konstas

2015-01-01

The Asian Monsoon leads to rapid vertical transport of gases and aerosols into the upper troposphere. Some of the pollution might be transported above cloud levels, which will allow it to spread globally and possibly at some occasions reach into the stratosphere. In this study we will use the GISS climate model to investigate the interactions between pollution and convective transport as well as secondary aerosol formation. Pollution resulting from anthropogenic activity as well as from natural sources such as small and large volcanic eruptions, dust storms and forest fires will be quantified. This modeling study will be accompanied by satellite observations from space that monitor aerosol optical thickness (AOT), and absorption AOT (AAOT) in two and three dimensions. Our goal is a better process level understanding of the evolution of natural and anthropogenic aerosol plumes in conjunction with the Asian Monsoon. Hence, we aim to explain their large-scale expansion, which eventually determines their impacts on climate.

Connections between Pollution and the Asian Monsoon Circulation

NASA Astrophysics Data System (ADS)

Bauer, S.

2015-12-01

The Asian Monsoon leads to rapid vertical transport of gases and aerosols into the upper troposphere. Some of the pollution might be transported above cloud levels, which will allow it to spread globally and possibly at some occasions reach into the stratosphere. In this study we will use the GISS climate model to investigate the interactions between pollution and convective transport as well as secondary aerosol formation. Pollution resulting from anthropogenic activity as well as from natural sources such as small and large volcanic eruptions, dust storms and forest fires will be quantified. This modeling study will be accompanied by satellite observations from space that monitor aerosol optical thickness (AOT), and absorption AOT (AAOT) in two and three dimensions. Our goal is a better process level understanding of the evolution of natural and anthropogenic aerosol plumes in conjunction with the Asian Monsoon. Hence, we aim to explain their large-scale expansion, which eventually determines their impacts on climate.

New Satellite Project Aerosol-UA: Remote Sensing of Aerosols in the Terrestrial Atmosphere

NASA Technical Reports Server (NTRS)

Milinevsky, G.; Yatskiv, Ya.; Degtyaryov, O.; Syniavskyi, I.; Mishchenko, Michael I.; Rosenbush, V.; Ivanov, Yu.; Makarov, A.; Bovchaliuk, A.; Danylevsky, V.;

Simplified aerosol modeling for variational data assimilation

NASA Astrophysics Data System (ADS)

Huneeus, N.; Boucher, O.; Chevallier, F.

2009-11-01

We have developed a simplified aerosol model together with its tangent linear and adjoint versions for the ultimate aim of optimizing global aerosol and aerosol precursor emission using variational data assimilation. The model was derived from the general circulation model LMDz; it groups together the 24 aerosol species simulated in LMDz into 4 species, namely gaseous precursors, fine mode aerosols, coarse mode desert dust and coarse mode sea salt. The emissions have been kept as in the original model. Modifications, however, were introduced in the computation of aerosol optical depth and in the processes of sedimentation, dry and wet deposition and sulphur chemistry to ensure consistency with the new set of species and their composition. The simplified model successfully manages to reproduce the main features of the aerosol distribution in LMDz. The largest differences in aerosol load are observed for fine mode aerosols and gaseous precursors. Differences between the original and simplified models are mainly associated to the new deposition and sedimentation velocities consistent with the definition of species in the simplified model and the simplification of the sulphur chemistry. Furthermore, simulated aerosol optical depth remains within the variability of monthly AERONET observations for all aerosol types and all sites throughout most of the year. Largest differences are observed over sites with strong desert dust influence. In terms of the daily aerosol variability, the model is less able to reproduce the observed variability from the AERONET data with larger discrepancies in stations affected by industrial aerosols. The simplified model however, closely follows the daily simulation from LMDz. Sensitivity analyses with the tangent linear version show that the simplified sulphur chemistry is the dominant process responsible for the strong non-linearity of the model.

Chemical Processing of Organics within Clouds: Pilot Study at Whiteface Mountain in Upstate NY

NASA Astrophysics Data System (ADS)

Lance, S.; Carlton, A. G.; Barth, M. C.; Schwab, J. J.; Minder, J. R.; Freedman, J. M.; Zhang, J.; Brandt, R. E.; Casson, P.; Brewer, M.; Orlowski, D.; Christiansen, A.

2017-12-01

Aqueous chemical processing within cloud and fog water has been identified as a key process in the formation of secondary organic aerosol (SOA) mass, which is found abundantly throughout the troposphere. Yet, significant uncertainty remains regarding the organic chemical reactions taking place within clouds and the conditions under which those reactions occur. Routine longterm measurements from the Whiteface Mountain (WFM) Research Observatory in upstate NY provide a unique and broad view of regional air quality relevant to the formation of particulate matter within clouds, largely due to the fact that the summit of WFM is within non-precipitating clouds 30-50% in summertime and the site is undisturbed by local sources. An NSF-funded Cloud Chemistry Workshop in Sept 2016 brought together key researchers at WFM to lay out the most pertinent scientific questions relevant to heterogeneous chemistry occurring within fogs and clouds and to discuss preliminary model intercomparisons. The workshop culminated in a plan to coordinate chemical analyses of cloud water samples focused on chemical constituents thought to be most relevant for SOA formation. Workshop participants also recommended that a pilot study be conducted at WFM to better characterize the meteorological conditions, airflow patterns and clouds intercepting the site, in preparation for future intensive field operations focused on the chemical processing of organics within clouds. This presentation will highlight the experimental design and preliminary observations from the pilot study taking place at WFM in August 2017. Upwind below-cloud measurements of aerosol CCN activation efficiency, size distribution and chemical composition will be compared with similar measurements made at the summit. Under certain conditions, we anticipate that aerosols measured at the summit between cloud events will be representative of cloud droplet residuals recently detrained from the frequent shallow cumulus intercepting the summit. Wind LIDAR and radiosonde observations will be used to link the below-cloud and summit observations. These pre- and post- `cloud processed' aerosols will also be compared with the chemical composition of cloud water samples to evaluate changes to the organic partitioning in the aqueous and aerosol phases.

Small molecules as tracers in atmospheric secondary organic aerosol

NASA Astrophysics Data System (ADS)

Yu, Ge

Secondary organic aerosol (SOA), formed from in-air oxidation of volatile organic compounds, greatly affects human health and climate. Although substantial research has been devoted to SOA formation and evolution, the modeled and lab-generated SOA are still low in mass and degree of oxidation compared to ambient measurements. In order to compensate for these discrepancies, the aqueous processing pathway has been brought to attention. The atmospheric waters serve as aqueous reaction media for dissolved organics to undergo further oxidation, oligomerization, or other functionalization reactions, which decreases the vapor pressure while increasing the oxidation state of carbon atoms. Field evidence for aqueous processing requires the identification of tracer products such as organosulfates. We synthesized the standards for two organosulfates, glycolic acid sulfate and lactic acid sulfate, in order to measure their aerosol-state concentration from five distinct locations via filter samples. The water-extracted filter samples were analyzed by LC-MS. Lactic acid sulfate and glycolic acid sulfate were detected in urban locations in the United States, Mexico City, and Pakistan with varied concentrations, indicating their potential as tracers. We studied the aqueous processing reaction between glyoxal and nitrogen-containing species such as ammonium and amines exclusively by NMR spectrometry. The reaction products formic acid and several imidazoles along with the quantified kinetics were reported. The brown carbon generated from these reactions were quantified optically by UV-Vis spectroscopy. The organic-phase reaction between oxygen molecule and alkenes photosensitized by alpha-dicarbonyls were studied in the same manner. We observed the fast kinetics transferring alkenes to epoxides under simulated sunlight. Statistical estimations indicate a very effective conversion of aerosol-phase alkenes to epoxides, potentially forming organosulfates in a deliquescence event and increasing aerosol mass. Finally, we built a containerless apparatus to study aqueous processing reactions using an acoustic levitator paired with a mass spectrometer. The levitator is capable of trapping droplets with the size of 80-500 mum in diameter for over eight hours. The apparatus is also capable of drying and wetting the droplet in a controllable manner. We performed am example reaction between glyoxal and ammonium sulfate using this instrument, and showed that it could qualitatively monitor aqueous processing reactions.

North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Roberts, G.; Mauger, G.; Hadley, O.; Ramanathan, V.

2006-07-01

Measurements of aerosol and cloud properties in the Eastern Pacific Ocean were taken during an airborne experiment on the University of Wyoming's King Air during April 2004 as part of the Cloud Indirect Forcing Experiment (CIFEX). We observed a wide variety of aerosols, including those of long-range transport from Asia, clean marine boundary layer, and North American emissions. These aerosols, classified by their size distribution and history, were found in stratified layers between 500 to 7500 m above sea level and thicknesses from 100 to 3000 m. A comparison of the aerosol size distributions to measurements of cloud condensation nuclei (CCN) provides insight to the CCN activity of the different aerosol types. The overall ratio of measured to predicted CCN concentration (NCCN) is 0.56 ± 0.41 with a relationship of NCCN,measured = NCCN,predicted0.846±0.002 for 23 research flights and 1884 comparisons. Such a relationship does not accurately describe a CCN closure; however, it is consistent with our measurements that high CCN concentrations are more influenced by anthropogenic sources, which are less CCN active. While other CCN closures have obtained results closer to the expected 1:1 relationship, the different aerosol types (and presumably differences in aerosol chemistry) are responsible for the discrepancy. The measured NCCN at 0.3% supersaturation (Sc) ranged from 20 cm-3 (pristine) to 350 cm-3 (anthropogenic) with an average of 106 ± 54 cm-3 over the experiment. The inferred supersaturation in the clouds sampled during this experiment is ˜0.3%. CCN concentrations of cloud-processed aerosol were well predicted using an ammonium sulfate approximation for Sc ≤ 0.4%. Predicted NCCN for other aerosol types (i.e., Asian and North American aerosols) were high compared to measured values indicating a less CCN active aerosol. This study highlights the importance of chemical effects on CCN measurements and introduces a CCN activation index as a method of classifying the efficiency of an aerosol to serve as CCN relative to an ammonium sulfate particle. This index ranged from close to unity for cloud processed aerosols to as low as 0.31 for aged aerosols transported from Asia. We also compare the performance of two CCN instruments (static thermal diffusion chamber and streamwise continuous flow chamber) on a 45 minute level leg where we observe an aged layer and a nucleation event. More than 50% of the aged aerosol served as CCN at 0.2% Sc, primarily owing to their large size, while CCN concentrations during the nucleation event were close to 0 cm-3. CCN concentrations from both instruments agreed within instrument errors; however, the continuous flow chamber effectively captured the rapid transition in aerosol properties.

Variability in optical properties of atmospheric aerosols and their frequency distribution over a mega city "New Delhi," India.

PubMed

Tiwari, S; Tiwari, Suresh; Hopke, P K; Attri, S D; Soni, V K; Singh, Abhay Kumar

2016-05-01

The role of atmospheric aerosols in climate and climate change is one of the largest uncertainties in understanding the present climate and in capability to predict future climate change. Due to this, the study of optical properties of atmospheric aerosols over a mega city "New Delhi" which is highly polluted and populated were conducted for two years long to see the aerosol loading and its seasonal variability using sun/sky radiometer data. Relatively higher mean aerosol optical depth (AOD) (0.90 ± 0.38) at 500 nm and associated Angstrom exponent (AE) (0.82 ± 0.35) for a pair of wavelength 400-870 nm is observed during the study period indicating highly turbid atmosphere throughout the year. Maximum AOD value is observed in the months of June and November while minimum is in transition months March and September. Apart from this, highest value of AOD (AE) value is observed in the post-monsoon [1.00 ± 0.42 (1.02 ± 0.16)] season followed by the winter [0.95 ± 0.36 (1.02 ± 0.20)] attributed to significance contribution of urban as well as biomass/crop residue burning aerosol which is further confirmed by aerosol type discrimination based on AOD vs AE. During the pre-monsoon season, mostly dust and mixed types aerosols are dominated. AODs value at shorter wavelength observed maximum in June and November while at longer wavelength maximum AOD is observed in June only. For the better understanding of seasonal aerosol modification process, the aerosol curvature effect is studied which show a strong seasonal dependency under a high turbid atmosphere, which are mainly associated with various emission sources. Five days air mass back trajectories were computed. They suggest different patterns of particle transport during the different seasons. Results suggest that mixtures of aerosols are present in the urban environment, which affect the regional air quality as well as climate. The present study will be very much useful to the modeler for validation of satellite data with observed data during estimation of radiative effect.

A13K-0336: Airborne Multi-Wavelength High Spectral Resolution Lidar for Process Studies and Assessment of Future Satellite Remote Sensing Concepts

NASA Technical Reports Server (NTRS)

Hostetler, Chris A.; Ferrare, Rich A.; Hair, Johnathan W.; Cook, Anthony L.; Harper, David B.; Mack, Terry L.; Hare, Richard J.; Cleckner, Craig S.; Rogers, Raymond R.; Muller, Detlef;

Aerosol Classification from High Spectral Resolution Lidar Measurements

NASA Astrophysics Data System (ADS)

Burton, S. P.; Hair, J. W.; Ferrare, R. A.; Hostetler, C. A.; Kahnert, M.; Vaughan, M. A.; Cook, A. L.; Harper, D. B.; Berkoff, T.; Seaman, S. T.; Collins, J. E., Jr.; Fenn, M. A.; Rogers, R. R.

2015-12-01

The NASA Langley airborne High Spectral Resolution Lidars, HSRL-1 and HSRL-2, have acquired large datasets of vertically resolved aerosol extinction, backscatter, and depolarization during >30 airborne field missions since 2006. The lidar measurements of aerosol intensive parameters like lidar ratio and color ratio embed information about intrinsic aerosol properties, and are combined to qualitatively classify HSRL aerosol measurements into aerosol types. Knowledge of aerosol type is important for assessing aerosol radiative forcing, and can provide useful information for source attribution studies. However, atmospheric aerosol is frequently not a single pure type, but instead is a mixture, which affects the optical and radiative properties of the aerosol. We show that aerosol intensive parameters measured by lidar can be understood using mixing rules for cases of external mixing. Beyond coarse classification and mixing between classes, variations in the lidar aerosol intensive parameters provide additional insight into aerosol processes and composition. This is illustrated by depolarization measurements at three wavelengths, 355 nm, 532 nm, and 1064 nm, made by HSRL-2. Particle depolarization ratio is an indicator of non-spherical particles. Three cases each have a significantly different spectral dependence of the depolarization ratio, related to the size of the depolarizing particles. For two dust cases, large non-spherical particles account for the depolarization of the lidar light. The spectral dependence reflects the size distribution of these particles and reveals differences in the transport histories of the two plumes. For a smoke case, the depolarization is inferred to be due to the presence of small coated soot aggregates. Interestingly, the depolarization at 355 nm is similar for this smoke case compared to the dust cases, having potential implications for the upcoming EarthCARE satellite, which will measure particle depolarization ratio only at 355 nm.

The Effect of Central American Smoke Aerosols on the Air Quality and Climate over the Southeastern United States: First Results from RAMS-AROMA

NASA Astrophysics Data System (ADS)

Wang, J.; Christopher, S. A.; Nair, U. S.; Reid, J.; Prins, E. M.; Szykman, J.

2004-12-01

Observation shows that smoke aerosols from biomass burning activities in Central America can be transported to the Southeastern United States (SEUS). In this study, the Regional Atmospheric Modeling System - Assimilation and Radiation Online Modeling of Aerosols (RAMS-AROMA) is used to investigate the effect of transported smoke aerosols on climate and air quality over the SEUS. AROMA is an aerosol transport model with capabilities of online integration of aerosol radiation effects and online assimilation of satellite-derived aerosol and emission products. It is assembled within the RAMS, so two-way interactions between aerosol fields and other meteorology fields are achieved simultaneously during each model time step. RAMS-AROMA is a unique tool that can be used to examine the aerosol radiative impacts on the surface energy budget and atmospheric heating rate and to investigate how atmospheric thermal and dynamical processes respond to such impacts and consequently affect the aerosol distribution (so called feedbacks). First results regarding air quality effects and radiative forcing of transported smoke aerosols will be presented from RAMS-AROMA based on assimilation of smoke emission products from the Fire Locating and Modeling of Burning Emissions (FLAMBE) project and aerosol optical thickness data derived from the MODIS instrument on the Terra and Aqua satellites. Comparisons with PM2.5 data collected from the EPA observation network and the aerosol optical thickness data from the DOE Atmosphere Radiation Measurements in the Southern Great Plains (ARM SGP) showed that RAMS-AROMA can predict the timing and spatial distribution of smoke events very well, with an accuracy useful for air quality forecasts. The smoke radiative effects on the surface temperature and atmospheric heating rate as well as their feedbacks will also be discussed.

GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

NASA Technical Reports Server (NTRS)

Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

2001-01-01

We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W m(exp -2) in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

Long term atmospheric aerosol characterization in the Amazon Basin

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

GCM Simulations of the Aerosol Indirect Effect: Sensitivity to Cloud Parameterization and Aerosol Burden

NASA Technical Reports Server (NTRS)

Menon, Surabi; DelGenio, Anthony D.; Koch, Dorothy; Tselioudis, George; Hansen, James E. (Technical Monitor)

2001-01-01

We describe the coupling of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) to an online sulfur chemistry model and source models for organic matter and sea-salt that is used to estimate the aerosol indirect effect. The cloud droplet number concentration is diagnosed empirically from field experiment datasets over land and ocean that observe droplet number and all three aerosol types simultaneously; corrections are made for implied variations in cloud turbulence levels. The resulting cloud droplet number is used to calculate variations in droplet effective radius, which in turn allows us to predict aerosol effects on cloud optical thickness and microphysical process rates. We calculate the aerosol indirect effect by differencing the top-of-the-atmosphere net cloud radiative forcing for simulations with present-day vs. pre-industrial emissions. Both the first (radiative) and second (microphysical) indirect effects are explored. We test the sensitivity of our results to cloud parameterization assumptions that control the vertical distribution of cloud occurrence, the autoconversion rate, and the aerosol scavenging rate, each of which feeds back significantly on the model aerosol burden. The global mean aerosol indirect effect for all three aerosol types ranges from -1.55 to -4.36 W/sq m in our simulations. The results are quite sensitive to the pre-industrial background aerosol burden, with low pre-industrial burdens giving strong indirect effects, and to a lesser extent to the anthropogenic aerosol burden, with large burdens giving somewhat larger indirect effects. Because of this dependence on the background aerosol, model diagnostics such as albedo-particle size correlations and column cloud susceptibility, for which satellite validation products are available, are not good predictors of the resulting indirect effect.

Nano- and Microparticles in Welding Aerosol: Granulometric Analysis

NASA Astrophysics Data System (ADS)

Kirichenko, K. Yu.; Drozd, V. A.; Chaika, V. V.; Gridasov, A. V.; Kholodov, A. S.; Golokhvast, K. S.

The paper presents the first results of the study of the size of particles appearing in the welding process by means of laser granulometry. It is shown that welding aerosol is the source of nano-and micro-sized particles extremely dangerous for human and animal health. Particle size distribution in the microrange was from 1 to 10 μm and up to 100%. It is shown that in 9 cases out of 28 with the use of various welding modes, welding rods and components the emission of aerosol with nano-sized particles (from 45.5% to 99.4%) is observed.

Insight into Chemistry on Cloud/Aerosol Water Surfaces.

PubMed

Zhong, Jie; Kumar, Manoj; Francisco, Joseph S; Zeng, Xiao Cheng

2018-05-15

Cloud/aerosol water surfaces exert significant influence over atmospheric chemical processes. Atmospheric processes at the water surface are observed to follow mechanisms that are quite different from those in the gas phase. This Account summarizes our recent findings of new reaction pathways on the water surface. We have studied these surface reactions using Born-Oppenheimer molecular dynamics simulations. These studies provide useful information on the reaction time scale, the underlying mechanism of surface reactions, and the dynamic behavior of the product formed on the aqueous surface. According to these studies, the aerosol water surfaces confine the atmospheric species into a specific orientation depending on the hydrophilicity of atmospheric species or the hydrogen-bonding interactions between atmospheric species and interfacial water. As a result, atmospheric species are activated toward a particular reaction on the aerosol water surface. For example, the simplest Criegee intermediate (CH 2 OO) exhibits high reactivity toward the interfacial water and hydrogen sulfide, with the reaction times being a few picoseconds, 2-3 orders of magnitude faster than that in the gas phase. The presence of interfacial water molecules induces proton-transfer-based stepwise pathways for these reactions, which are not possible in the gas phase. The strong hydrophobicity of methyl substituents in larger Criegee intermediates (>C1), such as CH 3 CHOO and (CH 3 ) 2 COO, blocks the formation of the necessary prereaction complexes for the Criegee-water reaction to occur at the water droplet surface, which lowers their proton-transfer ability and hampers the reaction. The aerosol water surface provides a solvent medium for acids (e.g., HNO 3 and HCOOH) to participate in reactions via mechanisms that are different from those in the gas and bulk aqueous phases. For example, the anti-CH 3 CHOO-HNO 3 reaction in the gas phase follows a direct reaction between anti-CH 3 CHOO and HNO 3 , whereas on a water surface, the HNO 3 -mediated stepwise hydration of anti-CH 3 CHOO is dominantly observed. The high surface/volume ratio of interfacial water molecules at the aerosol water surface can significantly lower the energy barriers for the proton transfer reactions in the atmosphere. Such catalysis by the aerosol water surface is shown to cause the barrier-less formation of ammonium bisulfate from hydrated NH 3 and SO 3 molecules rather than from the reaction of H 2 SO 4 with NH 3 . Finally, an aerosol water droplet is a polar solvent, which would favorably interact with high polarity substrates. This can accelerate interconversion of different conformers (e.g., anti and syn) of atmospheric species, such as glyoxal, depending on their polarity. The results discussed here enable an improved understanding of atmospheric processes on the aerosol water surface.

Connecting Aerosol Size Distributions at Three Arctic Stations

NASA Astrophysics Data System (ADS)

Freud, E.; Krejci, R.; Tunved, P.; Barrie, L. A.

2015-12-01

Aerosols play an important role in Earth's energy balance mainly through interactions with solar radiation and cloud processes. There is a distinct annual cycle of arctic aerosols, with greatest mass concentrations in the spring and lowest in summer due to effective wet removal processes - allowing for new particles formation events to take place. Little is known about the spatial extent of these events as no previous studies have directly compared and linked aerosol measurements from different arctic stations during the same times. Although the arctic stations are hardly affected by local pollution, it is normally assumed that their aerosol measurements are indicative of a rather large area. It is, however, not clear if that assumption holds all the time, and how large may that area be. In this study, three different datasets of aerosol size distributions from Mt. Zeppelin in Svalbard, Station Nord in northern Greenland and Alert in the Canadian arctic, are analyzed for the measurement period of 2012-2013. All stations are 500 to 1000 km from each other, and the travel time from one station to the other is typically between 2 to 5 days. The meteorological parameters along the calculated trajectories are analyzed in order to estimate their role in the modification of the aerosol size distribution while the air is traveling from one field station to another. In addition, the exposure of the sampled air to open waters vs. frozen sea is assessed, due to the different fluxes of heat, moisture, gases and particles, that are expected to affect the aerosol size distribution. The results show that the general characteristics of the aerosol size distributions and their annual variation are not very different in all three stations, with Alert and Station Nord being more similar. This is more pronounced when looking into the cases for which the trajectory calculations indicated that the air traveled from one of the latter stations to the other. The probable causes for the measurements at Mt. Zeppelin to stand out are the greater exposure to ice-free water all year round. In addition, the air sampled at Mt. Zeppelin is sometimes decoupled from the air at sea level. This results in a greater potential contribution of long-range transport to the aerosols that are measured there, compared to the other low-altitude stations.

Detection of Remarkably Low Isotopic Ratio of Iron in Anthropogenic Aerosols and Evaluation of its Contribution to the Surface Ocean

NASA Astrophysics Data System (ADS)

Kurisu, M.; Iizuka, T.; Sakata, K.; Uematsu, M.; Takahashi, Y.

2015-12-01

It has been reported that phytoplankton growth in the High Nutrient-Low Chlorophyll (HNLC) regions is limited by dissolved iron (DFe) concentration (e.g., Martin and Fitzwater, 1988). Aerosol is known as one of the dominant sources of DFe to the ocean and classified into two origins such as anthropogenic and natural. A series of recent studies showed that Fe in anthropogenic aerosols is more soluble than that in natural aerosols (Takahashi et al., 2013) and has lower isotopic ratio (Mead et al., 2013). However, the difference between Fe isotopic ratio　(δ56Fe: [(56Fe/54Fe)sample/(56Fe/54Fe)IRMM-14]-1) of two origins reported in Mead et al. (2013) is not so large compared with the standard deviation. Therefore, the aim of this study is to determine Fe species and δ56Fe in anthropogenic aerosols more accurately and to evaluate its contribution to the ocean surface. Iron species were determined by X-ray absorption fine structure (XAFS) analysis, while δ56Fe in size-fractionated aerosols were measured by MC-ICP-MS (NEPTUNE Plus) after chemical separation using anion exchange resin. Dominant Fe species in the samples were, ferrihydrite, hematite, and biotite. It was also revealed that coarse particles contained a larger amount of biotite and that fine particles contained a larger amount of hematite, which suggested that anthropogenic aerosols were emitted during combustion processes. In addition, results of Fe isotopic ratio analysis suggested that δ56Fe of coarse particles were around +0.25‰, whereas that of fine particles were -0.5 ˜ -2‰, which was lower than the δ56Fe in anthropogenic aerosol by Mead et al. (2013). The size-fractionated sampling made it possible to determine the δ56Fe in anthropogenic aerosol. Soluble component in fine particles extracted by simulated rain water also showed much lower δ56Fe (δ56Fe = -3.9±0.12‰), suggesting that anthropogenic Fe has much lower isotopic ratio. The remarkably low δ56Fe may be caused by the anthropogenic combustion process. The δ56Fe in anthropogenic aerosols measured here is important to model the budget of iron in the surface ocean.

Aerosolization Characteristics of Dry Powder Inhaler Formulations for the Excipient Enhanced Growth (EEG) Application: Effect of Spray Drying Process Conditions on Aerosol Performance

PubMed Central

Son, Yoen-Ju; Longest, P. Worth; Hindle, Michael

2013-01-01

The aim of this study was to develop a spray dried submicrometer powder formulation suitable for the excipient enhanced growth (EEG) application. Combination particles were prepared using the Buchi Nano spray dryer B-90. A number of spray drying and formulation variables were investigated with the aims of producing dry powder formulations that were readily dispersed upon aerosolization and maximizing the fraction of submicrometer particles. Albuterol sulfate, mannitol, L-leucine, and poloxamer 188 were selected as a model drug, hygroscopic excipient, dispersibility enhancer and surfactant, respectively. Formulations were assessed by scanning electron microscopy and aerosol performance following aerosolization using an Aerolizer® dry powder inhaler (DPI). In vitro drug deposition was studied using a realistic mouth-throat (MT) model. Based on the in vitro aerosolization results, the best performing submicrometer powder formulation consisted of albuterol sulfate, mannitol, L-leucine and poloxamer 188 in a ratio of 30:48:20:2, containing 0.5% solids in a water:ethanol (80:20% v/v) solution which was spray dried at 70 °C. The submicrometer particle fraction (FPF1μm/ED) of this final formulation was 28.3% with more than 80% of the capsule contents being emitted during aerosolization. This formulation also showed 4.1% MT deposition. The developed combination formulation delivered a powder aerosol developed for the EEG application with high dispersion efficiency and low MT deposition from a convenient DPI device platform. PMID:23313343

Three Dimensional Modeling Analysis of the Transpacific Transport of Aerosols During PACDEX

NASA Astrophysics Data System (ADS)

Carmichael, G. R.; Adhikary, B.; Hatch, C.; Kulkarni, S.; Moen, J.; Mena, M.

2007-12-01

Mineral dust and aerosols emitted from Asia are known to traverse long distances across the Pacific Ocean and can reach North America within a few days. A pilot field study, the PACific Dust Experiment (PACDEX), was carried out in April and May of 2007, during the peak East Asian dust emission season. The NSF/NCAR-HIAPER (High Performance Instrumented Airborne Platform for Environmental Research) platform allowed for sampling the evolution of mineral aerosol/pollution plumes and their physical and chemical characteristics as they traverse the Pacific Ocean and interact with the Pacific cloud systems en route to North America in both the upper and lower troposphere. A comprehensive 3-dimensional regional-scale model developed at The University of Iowa (Sulfur Transport dEposition Model, STEM) has been used for the analysis of aerosol interactions to help define key measurement strategies during the mission and to help interpret observations from the HIAPER platform. In this study we will present model aerosol distribution inter-comparison with cloud fields and aircraft observations. Model analysis provides further insight into cloud/pollution/dust interactions as East Asian emissions transit the Pacific Ocean en route to North America. Trajectory analysis and emission markers are used to help understand the air mass history and aerosol aging processes of the aerosols sampled by the HIAPER platform. Estimates of the fluxes of aerosol dust, BC and sulfate due to transpacific transport will also be presented.

Comparisons of Spectral Aerosol Single Scattering Albedo in Seoul, South Korea

NASA Technical Reports Server (NTRS)

Mok, Jungbin; Krotkov, Nickolay A.; Torres, Omar; Jethva, Hiren; Loughman, Robert P.; Spinei, Elena; Campanelli, Monica; Li, Zhanqing; Go, Sujung; Labow, Gordon;

Secondary Organic Aerosol Formation from Glyoxal: photochemical versus dark uptake and reversible versus irreversible SOA formation

NASA Astrophysics Data System (ADS)

Waxman, E.; Slowik, J. G.; Kampf, C. J.; Timkovsky, J.; Noziere, B.; Praplan, A. P.; Pfaffenberger, L.; Holzinger, R.; Hoffmann, T.; Dommen, J.; Prevot, A. S.; Baltensperger, U.; Volkamer, R.

2011-12-01

Glyoxal forms secondary organic aerosol (SOA) by partitioning to the aerosol aqueous phase according to Henry's law. The subsequent processing by heterogeneous and multiphase reactions shifts the partitioning towards aerosols. Currently it is not well understood whether these reactions result in reversible or irreversible SOA formation, and what parameters influence the rate limiting step of multiphase processing. We conducted a series of simulation chamber experiments at PSI in April and May 2011 to investigate processing under dark conditions, UV and/or visible light irradiated conditions, and in the presence and absence of OH radicals. Experiments used ammonium sulfate or ammonium sulfate/fulvic acid mixtures as seed aerosols, and were conducted between 50% and 85% relative humidity at approximately constant RH over the course of any given experiment. Glyoxal was produced photochemically from acetylene, using HONO photolysis as the OH radical source. Gas-phase glyoxal was measured by the CU LED-Cavity Enhanced-DOAS. The Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS) and Ion Chromatography Mass Spectrometer (IC-MS) monitored both gas and aerosol-phase organic reaction products. Particle composition was monitored by High-Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-ToF-AMS), and HPLC-ESI MS/MS and LC-MS analysis of filter samples.

Secondary Organic Aerosol Formation from Glyoxal: photochemical versus dark uptake and reversible versus irreversible SOA formation

NASA Astrophysics Data System (ADS)

Waxman, E.; Slowik, J.; Kampf, C.; Timkovsky, J.; Noziere, B.; Praplan, A.; Pffafenberger, L.; Holzinger, R.; Hoffmann, T.; Dommen, J.; Prevot, A.; Baltensperger, U.; Volkamer, R.

2012-04-01

Glyoxal forms secondary organic aerosol (SOA) by partitioning to the aerosol aqueous phase according to Henry's law. The subsequent processing by heterogeneous and multiphase reactions shifts the partitioning towards aerosols. Currently it is not well understood whether these reactions result in reversible or irreversible SOA formation, and what parameters influence the rate limiting step of multiphase processing. We conducted a series of simulation chamber experiments at PSI in April and May 2011 to investigate processing under dark conditions, UV and/or visible light irradiated conditions, and in the presence and absence of OH radicals. Experiments used ammonium sulfate or ammonium sulfate/fulvic acid mixtures as seed aerosols, and were conducted between 50% and 85% relative humidity at approximately constant RH over the course of any given experiment. Glyoxal was produced photochemically from acetylene, using HONO photolysis as the OH radical source. Gas-phase glyoxal was measured by the CU LED-Cavity Enhanced-DOAS. The Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS) and Ion Chromatography Mass Spectrometer (IC-MS) monitored both gas and aerosol-phase organic reaction products. Particle composition was monitored by High-Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-ToF-AMS), and HPLC-ESI MS/MS and LC-MS analysis of filter samples.

Theoretical and global scale model studies of the atmospheric sulfur/aerosol system

NASA Technical Reports Server (NTRS)

Kasibhatla, Prasad

1996-01-01

The primary focus during the third-phase of our on-going multi-year research effort has been on 3 activities. These are: (1) a global-scale model study of the anthropogenic component of the tropospheric sulfur cycle; (2) process-scale model studies of the factors influencing the distribution of aerosols in the remote marine atmosphere; and (3) an investigation of the mechanism of the OH-initiated oxidation of DMS in the remote marine boundary layer. In this paper, we describe in more detail our research activities in each of these areas. A major portion of our activities during the fourth and final phase of this project will involve the preparation and submission of manuscripts describing the results from our model studies of marine boundary-layer aerosols and DMS-oxidation mechanisms.

Semi-continuous measurement and characteristics of water-soluble organic carbon and ions of PM2.5 aerosol with PILS-TOC-IC in Baengnyeong Island

NASA Astrophysics Data System (ADS)

Kang, S.; Kim, K.; Park, G.; Ban, J.; Park, D.; Bae, M. S.; Shin, H. J.; Lee, M.; Seo, Y.; Choi, J.; Jung, D.; Seo, S.; Lee, T.; Kim, D. S.

2016-12-01

Aerosols have an important effect from scattering and absorbing the solar energy and indirectly by acting as cloud condensation nuclei and also some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. In various experimental results were showed that organic compounds have an important fraction from 10 to 70% of the total aerosol mass. Organic carbon contains water-soluble organic carbon (WSOC) and water insoluble organic carbon. WSOC are involved in the most unknown liquid-phase chemistry of wet aerosol and clouds. It is also worked as cloud condensation nuclei (CCN). Formation of secondary organic aerosol by chemical reaction of hydrocarbon compounds is a source of main pollution of WSOC compounds. Study of pollution source of WSOC is important method for creation process of secondary organic aerosol that completely has not studied.Analysis of WSOC is important and need to real-time measurement system for definition of chemical cause and sources. In this study, Particle-into-liquid sampler (PILS) coupled with total organic carbon (TOC) analyser and ion chromatography (PILS-TOC-IC), was used for semi-continuous measurement of WSOC and ionic compounds of PM2.5 during April-June 2016 at Baengnyeong Island Atmospheric Research Center, operated by the Korea National Institute of Environmental Research (NIER). PILS-TOC-IC can provide chemical information about real-time changes from ions composition and concentrations of WSOC and ionic compounds.

Aerosol modelling and validation during ESCOMPTE 2001

NASA Astrophysics Data System (ADS)

Cousin, F.; Liousse, C.; Cachier, H.; Bessagnet, B.; Guillaume, B.; Rosset, R.

The ESCOMPTE 2001 programme (Atmospheric Research. 69(3-4) (2004) 241) has resulted in an exhaustive set of dynamical, radiative, gas and aerosol observations (surface and aircraft measurements). A previous paper (Atmospheric Research. (2004) in press) has dealt with dynamics and gas-phase chemistry. The present paper is an extension to aerosol formation, transport and evolution. To account for important loadings of primary and secondary aerosols and their transformation processes in the ESCOMPTE domain, the ORISAM aerosol module (Atmospheric Environment. 35 (2001) 4751) was implemented on-line in the air-quality Meso-NH-C model. Additional developments have been introduced in ORganic and Inorganic Spectral Aerosol Module (ORISAM) to improve the comparison between simulations and experimental surface and aircraft field data. This paper discusses this comparison for a simulation performed during one selected day, 24 June 2001, during the Intensive Observation Period IOP2b. Our work relies on BC and OCp emission inventories specifically developed for ESCOMPTE. This study confirms the need for a fine resolution aerosol inventory with spectral chemical speciation. BC levels are satisfactorily reproduced, thus validating our emission inventory and its processing through Meso-NH-C. However, comparisons for reactive species generally denote an underestimation of concentrations. Organic aerosol levels are rather well simulated though with a trend to underestimation in the afternoon. Inorganic aerosol species are underestimated for several reasons, some of them have been identified. For sulphates, primary emissions were introduced. Improvement was obtained too for modelled nitrate and ammonium levels after introducing heterogeneous chemistry. However, no modelling of terrigeneous particles is probably a major cause for nitrates and ammonium underestimations. Particle numbers and size distributions are well reproduced, but only in the submicrometer range. Our work points out to the need of introducing coarse dust particles to further improve the simulation of PM-10 concentrations and more accurate modelling of gas-particle interactions.

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

DOE PAGES

Zhou, Shan; Collier, Sonya; Xu, Jianzhong; ...

2016-05-19

Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m –3 with 64% of the mass being organic. Organic aerosol (OA) atmore » BNL was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhou, Shan; Collier, Sonya; Xu, Jianzhong

Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m –3 with 64% of the mass being organic. Organic aerosol (OA) atmore » BNL was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

Understanding aerosol-cloud interactions in the development of orographic cumulus congestus during IPHEx

NASA Astrophysics Data System (ADS)

Barros, A. P.; Duan, Y.

2017-12-01

A new cloud parcel model (CPM) including activation, condensation, collision-coalescence, and lateral entrainment processes is presented here to investigate aerosol-cloud interactions (ACI) in cumulus development prior to rainfall onset. The CPM was employed along with ground based radar and surface aerosol measurements to predict the vertical structure of cloud formation at early stages and evaluated against airborne observations of cloud microphysics and thermodynamic conditions during the Integrated Precipitation and Hydrology Experiment (IPHEx) over the Southern Appalachian Mountains. Further, the CPM was applied to explore the space of ACI physical parameters controlling cumulus congestus growth not available from measurements, and to examine how variations in aerosol properties and microphysical processes influence the evolution and thermodynamic state of clouds over complex terrain via sensitivity analysis. Modeling results indicate that simulated spectra with a low value of condensation coefficient (0.01) are in good agreement with IPHEx aircraft observations around the same altitude. This is in contrast with high values reported in previous studies assuming adiabatic conditions. Entrainment is shown to govern the vertical development of clouds and the change of droplet numbers with height, and the sensitivity analysis suggests that there is a trade-off between entrainment strength and condensation process. Simulated CDNC also exhibits high sensitivity to variations in initial aerosol concentration at cloud base, but weak sensitivity to aerosol hygroscopicity. Exploratory multiple-parcel simulations capture realistic time-scales of vertical development of cumulus congestus (deeper clouds and faster droplet growth). These findings provide new insights into determinant factors of mid-day cumulus congestus formation that can explain a large fraction of warm season rainfall in mountainous regions.

Remote sensing of atmospheric aerosol and ocean color for the COMS/GOCI

NASA Astrophysics Data System (ADS)

Lee, Kwon-Ho; Kim, Young J.; Kim, Gwan C.; Wong, Man S.; Ahn, Yu H.

2010-10-01

The Geostationary Ocean Color Imager (GOCI) on board the Communication Ocean Meteorological Satellite (COMS) requires accurate atmospheric correction for the purpose of qualified ocean remote sensing. Since its eight bands are affected by atmospheric constituents such as gases, molecules and atmospheric aerosols, understanding of aerosolradiation interactions is needed. Aerosol optical properties based on sun-photometer measurements are used to analysis aerosol optical thickness (AOT) under various aerosol type and loadings. It is found that the choice of aerosol type makes little different in AOT retrieval for AOT<0.2. These results will be useful for aerosol retrieval of COMS/GOCI data processing.

Predicting the Mineral Composition of Dust Aerosols. Part 2; Model Evaluation and Identification of Key Processes with Observations

NASA Technical Reports Server (NTRS)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

VUV photodynamics of free tholins nanoparticles investigated by imaging Angle-Resolved Photoemission with the Synchrotron Radiation

NASA Astrophysics Data System (ADS)

Tigrine, Sarah; Nahon, Laurent; Carrasco, Nathalie; Garcia-Macias, Gustavo

2016-06-01

Thanks to the Cassini Huygens mission, it is now established that the aerosols appear from an altitude of 1,000 km in Titan's atmosphere. Once they are formed and through their descent towards the surface, those grains will still interact with persistent UV/VUV radiations, at different energies, that can reach lower atmospheric layers. This interaction has some impact, for example on the radiative transfer or on the ionization yield of the atmospheric compounds. Models are a good way to study those processes, but the lack of data on the refractive index or the absolute absorption/ionization cross subsections of the aerosols can be an obstacle. In order to shed some light and quantify those processes, we ionize analogs of aerosols produced with the PAMPRE experiment (LATMOS) on the SAPHIRS platform from the DESIRS VUV beamline at the synchrotron SOLEIL, equipped with an aerodynamic lens. The aerosols are injected directly under vacuum as isolated free nanoparticles and do not need to take the form of a film deposited on a substrate. The generated photoelectrons are then collected with a Velocity Map Imaging detector and their energetic and angular signatures are analyzed using the ARPES method (Angle-Resolved PhotoElectron Spectroscopy). Both the nanoparticles size distribution and the incident wavelength determine the parameters governing the photoemission process (intra-particles electron mean free path, photon penetration depth) as revealed by the angular distribution of the photoelectron showing in same cases a marked forward/backward asymmetry with respect to the photon axis. Those parameters may provide us with information on the optical behavior of the aerosols. In addition we can extract the ionization potential in direct connection with the absorption cross subsections of the aerosol, from which altitude dependent photodynamics can be unraveled. We will present here the experiments performed, at different VUV energies, on Titan's aerosol analogs with the ARPES method and show how the first results can have implications regarding Titan's atmosphere overall optical characteristics.

Predicting the mineral composition of dust aerosols – Part 2: Model evaluation and identification of key processes with observations

DOE PAGES

Perlwitz, J. P.; Perez Garcia-Pando, C.; Miller, R. L.

2015-10-21

A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second methodmore » approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. In conclusion, the importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.« less

Experimental Characterization of Radiation Forcing due to Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Sreenivas, K. R.; Singh, D. K.; Ponnulakshmi, V. K.; Subramanian, G.

2011-11-01

Micro-meteorological processes in the nocturnal atmospheric boundary layer (NBL) including the formation of radiation-fog and the development of inversion layers are controlled by heat transfer and the vertical temperature distribution close to the ground. In a recent study, it has been shown that the temperature profile close to the ground in stably-stratified, NBL is controlled by the radiative forcing due to suspended aerosols. Estimating aerosol forcing is also important in geo-engineering applications to evaluate the use of aerosols to mitigate greenhouse effects. Modeling capability in the above scenarios is limited by our knowledge of this forcing. Here, the design of an experimental setup is presented which can be used for evaluating the IR-radiation forcing on aerosols under either Rayleigh-Benard condition or under conditions corresponding to the NBL. We present results indicating the effect of surface emissivities of the top and bottom boundaries and the aerosol concentration on the temperature profiles. In order to understand the observed enhancement of the convection-threshold, we have determined the conduction-radiation time constant of an aerosol laden air layer. Our results help to explain observed temperature profiles in the NBL, the apparent stability of such profiles and indicate the need to account for the effect of aerosols in climatic/weather models.

Aerosol Daytime Variations over North and South America Derived from Multiyear AERONET Measurements

NASA Technical Reports Server (NTRS)

Zhang, Yan; Yu, Hongbin; Eck, Tom F.; Smirnov, Alexander; Chin, Mian; Remer, Lorraine A.; Bian, Huisheng; Tan, Qian; Levy, Roberrt; Holben, Brent N.

2012-01-01

This study analyzes the daytime variation of aerosol with seasonal distinction by using multi-year measurements from 54 of the Aerosol Robotic Network (AERONET) sites over North America, South America, and islands in surrounding oceans. The analysis shows a wide range of daily variability of aerosol optical depth (AOO) and Angstrom exponent depending on location and season. Possible reasons for daytime variations are given. The largest AOO daytime variation range at 440 nm, up to 75%, occurs in Mexico City, with maximum AOO in the afternoon. Large AOO daily variations are also observed in the polluted mid-Atlantic U.S. and U.S. West Coast with maximum AOO occurring in the afternoon in the mid-Atlantic U.S., but in the morning in the West Coast. In South American sites during the biomass burning season (August to October), maximum AOO generally occurs in the afternoon. But the daytime variation becomes smaller when sites are influenced more by long-range transported smoke than by local burning. Islands show minimum AOO in the morning and maximum AOO in the afternoon. The diverse patterns of aerosol daytime variation suggest that geostationary satellite measurements would be invaluable for characterizing aerosol temporal variations on regional and continental scales. In particular, simultaneous measurements of aerosols and aerosol precursors from a geostationary satellite would greatly aid in understanding the evolution of aerosol as determined by emissions, chemical transformations, and transport processes.

Continuous dry dispersion of multi-walled carbon nanotubes to aerosols with high concentrations of individual fibers

NASA Astrophysics Data System (ADS)

Simonow, Barbara Katrin; Wenzlaff, Daniela; Meyer-Plath, Asmus; Dziurowitz, Nico; Thim, Carmen; Thiel, Jana; Jandy, Mikolaj; Plitzko, Sabine

2018-06-01

The assessment of the toxicity of airborne nanofibers is an important task. It relies on toxicological inhalation studies and validated exposure measurement techniques. Both require nanofiber-containing aerosols of known morphological composition and controlled fraction of individual fibers. Here, a dry powder dispersion method is presented that operates with mixtures of nanofibers and microscale beads. Aerosolization experiments of mixtures of multi-walled carbon nanotubes (MWCNTs) and glass beads that were continuously fed into a Venturi nozzle enabled high generation rates of aerosols composed of individual and agglomerate nanofiber structures. The aerosol process achieved good stability over more than 2 h with respect to concentration and aerodynamic size distribution. Its operation duration is limited only by the reservoir volume of the cyclone used to separate the beads from the aerosol. The aerosol concentration can be controlled by changing the mass ratio of MWCNTs and glass beads or by adapting the mass feed rate to the nozzle. For two agglomerated MWCNT materials, aerosol concentrations ranged from 1700 to 64,000 nano-objects per cm3. Comprehensive scanning electron microscope analysis of filter samples was performed to categorize and determine the morphological composition of the aerosol, its fiber content as well as fiber length and diameter distributions. High fractions of individual fibers of up to 34% were obtained, which shows the setup to be capable of dispersing also highly tangled MWCNT agglomerates effectively.

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.: URBAN INFLUENCE ON RURAL AEROSOL

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhou, Shan; Collier, Sonya; Xu, Jianzhong

2016-05-19

Continuous real-time measurements of atmospheric aerosol with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the DOE Aerosol Life Cycle Intensive Operational Period (ALC-IOP) campaign.

The Regional Environmental Impacts of Atmospheric Aerosols over Egypt

NASA Astrophysics Data System (ADS)

Zakey, Ashraf; Ibrahim, Alaa

2015-04-01

Identifying the origin (natural versus anthropogenic) and the dynamics of aerosols over Egypt at varying temporal and spatial scales provide valuable knowledge on the regional climate impacts of aerosols and their ultimate connections to the Earth's regional climate system at the MENA region. At regional scale, Egypt is exposed to air pollution with levels exceeding typical air-quality standards. This is particularly true for the Nile Delta region, being at the crossroads of different aerosol species originating from local urban-industrial and biomass-burning activities, regional dust sources, and European pollution from the north. The Environmental Climate Model (EnvClimA) is used to investigate both of the biogenic and anthropogenic aerosols over Egypt. The dominant natural aerosols over Egypt are due to the sand and dust storms, which frequently occur during the transitional seasons (spring and autumn). In winter, the maximum frequency reaches 2 to 3 per day in the north, which decreases gradually southward with a frequency of 0.5-1 per day. Monitoring one of the most basic aerosol parameters, the aerosol optical depth (AOD), is a main experimental and modeling task in aerosol studies. We used the aerosol optical depth to quantify the amount and variability of aerosol loading in the atmospheric column over a certain areas. The aerosols optical depth from the model is higher in spring season due to the impacts of dust activity over Egypt as results of the westerly wind, which carries more dust particles from the Libyan Desert. The model result shows that the mass load of fine aerosols has a longer life-time than the coarse aerosols. In autumn season, the modelled aerosol optical depth tends to increase due to the biomass burning in the delta of Egypt. Natural aerosol from the model tends to scatter the solar radiation while most of the anthropogenic aerosols tend to absorb the longwave solar radiation. The overall results indicate that the AOD is lowest in winter due to airborne particles washed out by rain events. Conversely, the AOD increases in summer because particle accumulation is favored by the absence of precipitation during this season. Moreover, in summer, photochemical processes in the atmosphere lead to slight increases in the values of aerosol optical characteristics, despite lower wind speeds [hence less wind-blown dust] relative to other seasons. This study has been conducted under the PEER 2-239 research project titled "the Impact of Biogenic and Anthropogenic Atmospheric Aerosols to Climate in Egypt". Project website: CleanAirEgypt.org

Radiative Effects of Carbonaceous and Inorganic Aerosols over California during CalNex and CARES: Observations versus Model Predictions

NASA Astrophysics Data System (ADS)

Vinoj, V.; Fast, J. D.; Liu, Y.

2012-12-01

Aerosols have been identified to be a major contributor to the uncertainty in understanding the present climate. Most of this uncertainty arises due to the lack of knowledge of their micro-physical and chemical properties as well as how to adequately represent their spatial and temporal distributions. Increased process level understanding can be achieved through carefully designed field campaigns and experiments. These measurements can be used to elucidate the aerosol properties, mixing, transport and transformation within the atmosphere and also to validate and improve models that include meteorology-aerosol-chemistry interactions. In the present study, the WRF-Chem model is used to simulate the evolution of carbonaceous and inorganic aerosols and their impact on radiation during May and June of 2010 over California when two field campaigns took place: the California Nexus Experiment (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES). We merged CalNex and CARES data along with data from operational networks such as, California Air Resources Board (CARB's) air quality monitoring network, the Interagency Monitoring of Protected Visual Environments (IMPROVE) network, the AErosol RObotic NETwork (AERONET), and satellites into a common dataset for the Aerosol Modeling Test bed. The resulting combined dataset is used to rigorously evaluate the model simulation of aerosol mass, size distribution, composition, and optical properties needed to understand uncertainties that could affect regional variations in aerosol radiative forcing. The model reproduced many of the diurnal, multi-day, and spatial variations of aerosols as seen in the measurements. However, regionally the performance varied with reasonably good agreement with observations around Los Angeles and Sacramento and poor agreement with observations in the vicinity of Bakersfield (although predictions aloft were much better). Some aerosol species (sulfate and nitrate) were better represented than others (organic matter, black carbon) at many locations. The model also reproduced the observed transport of sea-salt by intrusions of marine air from the Bay Area to Sacramento. The vertical distribution of aerosols was simulated reasonably as evidenced from comparison with observed profiles from the High Spectral Resolution Lidar (HSRL) on the NASA B-200 aircraft, although the values in the boundary layer were too high at times. Consistent with the bias in aerosol mass, the simulated column aerosol optical depths at the AERONET and field campaign sites were often too high. Comparisons between observed and predicted aerosol optical depth and single scattering albedo will be presented. Using aerosol observations as a constraint, we will present the radiative effect of simulated aerosols and its sensitivity to the uncertainties in predicted aerosol properties.

How well do satellite observations and models capture diurnal variation in aerosols over the Korean Peninsula?

NASA Astrophysics Data System (ADS)

Hyer, E. J.; Xian, P.; Campbell, J. R.

2016-12-01

Aerosol sources, sinks, and transport processes have important variations over the diurnal cycle. Advances in geostationary satellite observation have made it possible to retrieve aerosol properties over a larger fraction of the diurnal cycle in many areas. However, the conditions for retrieval of aerosol from space also have systematic diurnal variation, which must be considered when interpreting satellite data. We used surface PM2.5 observations from the Korean National Institute for Environmental Research, together with the dense network of AERONET sun photometers deployed in Korea for the KORUS-AQ mission in spring 2016, to examine diurnal variations in aerosol conditions and quantify the effect of systematic diurnal processes on daily integrated aerosol quantities of forcing and PM2.5 24-hour exposure. Time-resolved observations of aerosols from in situ data were compared to polar and geostationary satellite observations to evaluate these questions: 1) How well is diurnal variation observed in situ captured by satellite products? 2) Do the satellite products show evidence of systematic biases related to diurnally varying observing conditions? 3) What is the implication of diurnal variation for aerosol forcing estimates based on observations near solar noon? The diurnal variation diagnosed from observations was also compared to the output of the Navy Aerosol Analysis and Prediction System (NAAPS), to examine the ability of this model to capture aerosol diurnal variation. Finally, we discuss the implications of the observed diurnal variation for assimilation of aerosol observations into forecast models.

Use of high-volume outdoor smog chamber photo-reactors for studying physical and chemical atmospheric aerosol formation and composition

NASA Astrophysics Data System (ADS)

Borrás, E.; Ródenas, M.; Vera, T.; Muñoz, A.

2015-12-01

The atmospheric particulate matter has a large impact on climate, biosphere behaviour and human health. Its study is complex because of large number of species are present at low concentrations and the continuous time evolution, being not easily separable from meteorology, and transport processes. Closed systems have been proposed by isolating specific reactions, pollutants or products and controlling the oxidizing environment. High volume simulation chambers, such as EUropean PHOtoREactor (EUPHORE), are an essential tool used to simulate atmospheric photochemical reactions. This communication describes the last results about the reactivity of prominent atmospheric pollutants and the subsequent particulate matter formation. Specific experiments focused on organic aerosols have been developed at the EUPHORE photo-reactor. The use of on-line instrumentation, supported by off-line techniques, has provided well-defined reaction profiles, physical properties, and up to 300 different species are determined in particulate matter. The application fields include the degradation of anthropogenic and biogenic pollutants, and pesticides under several atmospheric conditions, studying their contribution on the formation of secondary organic aerosols (SOA). The studies performed at the EUPHORE have improved the mechanistic studies of atmospheric degradation processes and the knowledge about the chemical and physical properties of atmospheric particulate matter formed during these processes.

Regional trends in the fractional solubility of Fe and other metals from North Atlantic aerosols (GEOTRACES cruises GA01 and GA03) following a two-stage leach

NASA Astrophysics Data System (ADS)

Shelley, Rachel U.; Landing, William M.; Ussher, Simon J.; Planquette, Helene; Sarthou, Geraldine

2018-04-01

The fractional solubility of aerosol-derived trace elements deposited to the ocean surface is a key parameter of many marine biogeochemical models. Despite this, it is currently poorly constrained, in part due to the complex interplay between the various processes that govern the solubilisation of aerosol trace elements. In this study, we used a sequential two-stage leach to investigate the regional variability in fractional solubility of a suite of aerosol trace elements (Al, Ti, Fe, Mn, Co, Ni, Cu, Zn, Cd, and Pb) from samples collected during three GEOTRACES cruises to the North Atlantic Ocean (GA01, GA03-2010, and GA03-2011). We present aerosol trace element solubility data from two sequential leaches that provide a solubility window, covering a conservative lower limit to an upper limit, the maximum potentially soluble fraction, and discuss why this upper limit of solubility could be used as a proxy for the bioavailable fraction in some regions. Regardless of the leaching solution used in this study (mild versus strong leach), the most heavily loaded samples generally had the lowest solubility. However, there were exceptions. Manganese fractional solubility was relatively uniform across the full range of atmospheric loading (32 ± 13 and 49 ± 13 % for ultra high-purity water and 25 % acetic acid leaches, respectively). This is consistent with other marine aerosol studies. Zinc and Cd fractional solubility also appeared to be independent of atmospheric loading. Although the average fractional solubilities of Zn and Cd (37 ± 28 and 55 ± 30 % for Zn and 39 ± 23 and 58 ± 26 % for Cd, for ultra high-purity water and 25 % acetic acid leaches, respectively) were similar to Mn, the range was greater, with several samples being 100 % soluble after the second leach. Finally, as the objective of this study was to investigate the regional variability in TE solubility, the samples were grouped according to air mass back trajectories (AMBTs). However, we conclude that AMBTs are not sufficiently discriminating to identify the aerosol sources or the potential effects of atmospheric processing on the physicochemical composition and solubility of the aerosols.

The Effect of Aerosols on Pluto's C2 Hydrocarbon Chemistry

NASA Astrophysics Data System (ADS)

Luspay-Kuti, Adrienn; Mandt, Kathleen; Jessup, Kandis-Lea; Hue, Vincent; Kammer, Joshua; Filwett, Rachael; Hamel, Mark

2017-10-01

On July 14, 2015 the New Horizons spacecraft flew through the Pluto system, providing critical details about Pluto’s atmosphere. The vertical profiles of N2 and CH4, C2H2, C2H4, and C2H6 derived from New Horizons Alice transmission data allow the more accurate modeling of Pluto’s atmosphere than in the pre-New Horizons era, and help better understand the physical and photochemical processes in Pluto’s atmosphere. All the measured C2 hydrocarbon densities showed an unexpected inversion between ~100 and 400 km, which suggests that processes other than chemistry play an important role in shaping their vertical profiles. We present here a state-of-the-art Pluto Ion-Neutral-Photochemistry (Pluto INP) model that includes the condensation onto and incorporation into aerosol particles, and evaluate the dominant production and loss processes of C2 hydrocarbons with a special emphasis on the role of aerosol interaction. We found that in order to reproduce the C2 profiles measured by New Horizons, they must stick to and be permanently removed by aerosols - a process different from condensation. We determined through empirical fits to the New Horizons data that the sticking efficiency of C2 hydrocarbons and the stickiness of the aerosol particles are inversely related to the available aerosol surface area, which has been inferred from observation to increase as altitude decreases. This counterintuitive relationship between sticking efficiency and available aerosol surfaces indicates that similarly to Titan, Pluto’s aerosols must harden and become less sticky as they age. Such hardening with ageing is both necessary and sufficient to explain the vertical profiles of C2 hydrocarbons in Pluto’s atmosphere.

How much of the global aerosol optical depth is found in the boundary layer and free troposphere?

NASA Astrophysics Data System (ADS)

Bourgeois, Quentin; Ekman, Annica M. L.; Renard, Jean-Baptiste; Krejci, Radovan; Devasthale, Abhay; Bender, Frida A.-M.; Riipinen, Ilona; Berthet, Gwenaël; Tackett, Jason L.

2018-06-01

The global aerosol extinction from the CALIOP space lidar was used to compute aerosol optical depth (AOD) over a 9-year period (2007-2015) and partitioned between the boundary layer (BL) and the free troposphere (FT) using BL heights obtained from the ERA-Interim archive. The results show that the vertical distribution of AOD does not follow the diurnal cycle of the BL but remains similar between day and night highlighting the presence of a residual layer during night. The BL and FT contribute 69 and 31 %, respectively, to the global tropospheric AOD during daytime in line with observations obtained in Aire sur l'Adour (France) using the Light Optical Aerosol Counter (LOAC) instrument. The FT AOD contribution is larger in the tropics than at mid-latitudes which indicates that convective transport largely controls the vertical profile of aerosols. Over oceans, the FT AOD contribution is mainly governed by long-range transport of aerosols from emission sources located within neighboring continents. According to the CALIOP aerosol classification, dust and smoke particles are the main aerosol types transported into the FT. Overall, the study shows that the fraction of AOD in the FT - and thus potentially located above low-level clouds - is substantial and deserves more attention when evaluating the radiative effect of aerosols in climate models. More generally, the results have implications for processes determining the overall budgets, sources, sinks and transport of aerosol particles and their description in atmospheric models.

A Pure Marine Aerosol Model, for Use in Remote Sensing Applications

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Smirnov, A.; Hsu, N. C.; Holben, B. N.

2011-01-01

Retrievals of aerosol optical depth (AOD) and related parameters from satellite measurements typically involve prescribed models of aerosol size and composition, and are therefore dependent on how well these models are able to represent the radiative behaviour of real aerosols, This study uses aerosol volume size distributions retrieved from Sun-photometer measurements at 11 Aerosol Robotic Network (AERONET) island sites, spread throughout the world's oceans, as a basis to define such a model for unpolluted maritime aerosols. Size distributions are observed to be bimodal and approximately lognormal, although the coarse mode is skewed with a long tail on the low-radius end, The relationship of AOD and size distribution parameters to meteorological conditions is also examined, As wind speed increases, so do coarse-mode volume and radius, The AOD and Angstrom exponent (alpha) show linear relationships with wind speed, although there is considerable scatter in all these relationships, limiting their predictive power. Links between aerosol properties and near-surface relative humidity, columnar water vapor, and sea surface temperature are also explored. A recommended bimodal maritime model, which is able to reconstruct the AERONET AOD with accuracy of order 0.01-0.02, is presented for use in aerosol remote sensing applications. This accuracy holds at most sites and for wavelengths between 340 nm and 1020 nm. Calculated lidar ratios are also provided, and differ significantly from those currently used in Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) processing.

Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

NASA Astrophysics Data System (ADS)

Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

2015-05-01

A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

Investigation of Atmospheric Aerosol properties by Atomic Force Microscopy

NASA Astrophysics Data System (ADS)

Sevalia, Barry; Joseph, Kelli; Gasseller, Morewell

The effects of aerosols on the atmosphere, climate, and public health are among the central topics in current environmental research. Aerosol particles scatter and absorb solar and terrestrial radiation, they are involved in the formation of clouds and precipitation as cloud condensation and ice nuclei, and they affect the abundance and distribution of atmospheric trace gases by chemical reactions and other multiphase processes. Moreover, airborne particles play an important role in the spreading of biological organisms, reproductive materials, and pathogens and they can cause or enhance respiratory, cardiovascular, infectious, and allergic diseases. In this study we use two distinct methods to characterize atmospheric aerosol particles. With the AFM, we use analytical and interpretative techniques to deduce fundamental physical properties of the aerosol particles such as particle sizes and morphology. The microscopy techniques are then compared and complemented with optical techniques that employ hand held sun photometers to measure aerosol optical thickness (AOT) of the atmosphere. The chemical nature of the aerosols is investigated by exposing the samples to a stream of ozone gas and then reimage them. Using this approach, we are only able to classify particles as organic, gr Maryam Foroozesh, Ph.D. Chair, Division of Mathematical and Physical Sciences Head, Department of Chemistry.

Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

NASA Astrophysics Data System (ADS)

Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

2011-12-01

Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

Development and Initial Testing of a Multi-Sensor Platform for Cloud-Aerosol Interactions in the Lower Troposphere

NASA Astrophysics Data System (ADS)

Nehrir, A. R.; Hoffman, D. S.; Repasky, K. S.; Todt, B.; Sharpe, T.; Half Red, C.; Carlsten, J. L.

2009-12-01

Coupled atmospheric components of the lower troposphere including aerosols and water vapor have a large affect on the chemical processes that drive the earth’s complex climate system. Aerosols can affect the earth’s global radiation budget directly by absorbing or reflecting incoming solar radiation, and indirectly by changing the microphysical properties of clouds by serving as cloud condensation nuclei (CCN). An increase in CCN results in higher cloud droplet concentration which has been shown to suppress drizzle formation and lead to more reflective clouds. The changes in the cloud microphysical structure due to the interaction of aerosols and water vapor result in more incoming solar radiation being reflected back into space, leading to a net negative radiative forcing in the global radiation budget. The uncertainty in this radiative forcing reflects the uncertainty in the understanding of the aerosol indirect effect and its role in the climate system. To better understand the aerosol direct and indirect effects, lidar measurements of aerosol properties and water vapor distributions can provide important information to enhance our understanding of the role of aerosols in the climate system. The LIDAR group at Montana State University has initiated a program to simultaneously study aerosols, water vapor, and cloud formation with high spatial and temporal resolution using both active and passive sensors. Aerosol distributions and radiative properties are currently being studied with a two-color LIDAR system at 1064 and 532 nm. In addition, a three color, high spectral resolution LIDAR system at 1064,532, and 355 nm has also been developed and is starting to take initial data. Daytime and nighttime boundary layer water vapor number density profiles are also currently being studied with an external cavity diode oscillator/diode amplifier based micro-pulsed differential absorption lidar (DIAL) instrument at the 830 nm water vapor absorption band. Cloud formation studies are being conducted by a simultaneous, spatially correlated digital sky imaging camera system where aerosol loading and water vapor distributions are monitored as a function of lateral distance to clouds. Furthermore, a commercially purchased sun/sky scanning solar radiometer (CIMEL 318) as part of the NASA run AERONET program is also being used to study aerosol loading and radiative transfer through the atmosphere. A brief description of these instruments will be presented as well as initial simultaneous results showing correlated data between lower tropospheric aerosols and boundary layer water vapor distributions over extended periods if time.

Physico-chemical characterization of Mediterranean background aerosol at the Capogranitola observatory (Sicily)

NASA Astrophysics Data System (ADS)

Rinaldi, Matteo; Gilardoni, Stefania; Paglione, Marco; Sandrini, Silvia; Decesari, Stefano; Zanca, Nicola; Marinoni, Angela; Cristofanelli, Paolo; Bonasoni, Paolo; Ielpo, Piera; Fossum, Kirsten; Gobbi, Gian Paolo; Facchini, Maria Cristina

2017-04-01

The Mediterranean basin is characterized by elevated aerosol amounts and co-existence of different aerosol types, both natural and anthropogenic, while it is one of the most climatically sensitive areas. Therefore, it offers ideal conditions for studying aerosol processes and aerosol-climate interactions. An intensive aerosol physico-chemical characterization campaign was held at the Environmental-Climatic Observatory at Capo Granitola (Sicily; 37.5753° N, 12.6595° E) during April 2016, under the framework of the project Air-Sea Lab. The Observatory is located at the coast-line, facing the Strait of Sicily, and is part of the national I-AMICA network (http://www.i-amica.it/i-amica/?lang=en). Sub-micrometer aerosol chemical composition was measured by high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS), for the first time at Capogranitola. Sea-salt concentration was estimated from AMS measurements following Ovadnevaite et al. (2012). For a complete mass closure of the submicron aerosol, black carbon (BC) concentration was derived from multiangle absorption photometer (MAAP) measurements. Positive matrix factorization was deployed to investigate organic aerosol (OA) sources at the site. Aerosol chemical composition confirms that Capogranitola is a representative background site, with generally low contribution of BC and nitrate and highly oxidized OA. In particular, aerosol sampled in the marine sector (130-310°) is less affected by local sources and it is likely representative of the central Mediterranean background. Aerosol in background conditions is dominated by sulfate and OA (37% and 31%), followed by ammonium (12%), sea-salt (10%), BC (6%) and nitrate (3%). The average reconstructed sub-micrometer aerosol mass in background conditions is 3.7±2.3 μg m-3. OA source apportionment shows a minor contribution from primary sources, with hydrocarbon-like OA (HOA), from fossil fuel combustion, contributing for 3% and biomass burning OA (BBOA) for 2%. Oxidized OA (OOA) dominates the rest of OA mass. In particular, OOA1 and OOA2 (70% in total, OM:OC ˜ 2.5) represent the result of prolonged atmospheric processing of OA, while OOA3 (25%, OM:OC ˜ 2.0) clearly represents fresher inputs of OOA from land. Investigation of HOA and BC time trends suggests that HOA in background conditions may be strongly contributed by ship traffic more than by land sources. The representativity of the background aerosol collected at Capogranitola will be discussed by comparing with measurements performed in parallel at the other I-AMICA southern Italy coastal stations and with those acquired in a subsequent cruise (May-June 2016) around the Italian Peninsula. Aerosol climate relevant properties, in relation with chemical composition, will be also presented and discussed. Ovadnevaite J. et al. (2012), J. Geophys. Res., 117, D16201.

Aerosol-cloud interactions in mixed-phase convective clouds - Part 1: Aerosol perturbations

NASA Astrophysics Data System (ADS)

Miltenberger, Annette K.; Field, Paul R.; Hill, Adrian A.; Rosenberg, Phil; Shipway, Ben J.; Wilkinson, Jonathan M.; Scovell, Robert; Blyth, Alan M.

2018-03-01

Changes induced by perturbed aerosol conditions in moderately deep mixed-phase convective clouds (cloud top height ˜ 5 km) developing along sea-breeze convergence lines are investigated with high-resolution numerical model simulations. The simulations utilise the newly developed Cloud-AeroSol Interacting Microphysics (CASIM) module for the Unified Model (UM), which allows for the representation of the two-way interaction between cloud and aerosol fields. Simulations are evaluated against observations collected during the COnvective Precipitation Experiment (COPE) field campaign over the southwestern peninsula of the UK in 2013. The simulations compare favourably with observed thermodynamic profiles, cloud base cloud droplet number concentrations (CDNC), cloud depth, and radar reflectivity statistics. Including the modification of aerosol fields by cloud microphysical processes improves the correspondence with observed CDNC values and spatial variability, but reduces the agreement with observations for average cloud size and cloud top height. Accumulated precipitation is suppressed for higher-aerosol conditions before clouds become organised along the sea-breeze convergence lines. Changes in precipitation are smaller in simulations with aerosol processing. The precipitation suppression is due to less efficient precipitation production by warm-phase microphysics, consistent with parcel model predictions. In contrast, after convective cells organise along the sea-breeze convergence zone, accumulated precipitation increases with aerosol concentrations. Condensate production increases with the aerosol concentrations due to higher vertical velocities in the convective cores and higher cloud top heights. However, for the highest-aerosol scenarios, no further increase in the condensate production occurs, as clouds grow into an upper-level stable layer. In these cases, the reduced precipitation efficiency (PE) dominates the precipitation response and no further precipitation enhancement occurs. Previous studies of deep convective clouds have related larger vertical velocities under high-aerosol conditions to enhanced latent heating from freezing. In the presented simulations changes in latent heating above the 0°C are negligible, but latent heating from condensation increases with aerosol concentrations. It is hypothesised that this increase is related to changes in the cloud field structure reducing the mixing of environmental air into the convective core. The precipitation response of the deeper mixed-phase clouds along well-established convergence lines can be the opposite of predictions from parcel models. This occurs when clouds interact with a pre-existing thermodynamic environment and cloud field structural changes occur that are not captured by simple parcel model approaches.

Day-night differences in the composition and sources of carbonaceous aerosol at a polluted regional background site in the Netherlands

NASA Astrophysics Data System (ADS)

Dusek, Ulrike; Broekema, Elise; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro

2017-04-01

The origin of carbonaceous aerosol differs during day- and night-time, because emissions from major sources such as traffic, biomass combustion, and secondary organic aerosol formation show a distinct diurnal pattern. Moreover, photochemical processing and evaporation of semi-volatile organic compounds are enhanced during day-time, due to the availability of sunlight and higher temperatures. Assessing day-night differences in sources and chemical composition can give an indication of the importance of local/regional carbon sources and processing, since day-night differences should be averaged out during long-range transport. If local sources dominate, one could expect a strong diurnal variation in the source profile, but if long-range transport dominates the diurnal variation would be much weaker. In this study we measure the isotopic (14C and 13C) and detailed chemical composition of the organic fraction of the aerosol on high volume PM2.5 filter samples that were collected separately during day and night time. Radiocarbon (14C) measurements are used to estimate three main aerosol sources of organic and elemental carbon (OC and EC): Fossil fuel combustion (ff), biomass combustion (bb), and biogenic sources (bio). The detailed chemical and stable isotopic composition are measured at different desorption temperatures from the filter, which separates the more and less refractory organic compounds. The composition of the organic aerosol is measured using an thermal-desporption Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) method (Holzinger et al, 2010) and the stable isotopic composition is measured using a thermal desorption IRMS method (Dusek et al., 2013). Source apportionment results using 14C show that the contribution of fossil fuel combustion to EC and OC is higher during day-time than during night-time. This is valid for all seasons. During night-time biomass combustion plays a bigger role as a source of carbonaceous aerosol. Even in the summer, when biomass combustion is a small source, its relative contribution increases between 19:00 and 07:00. However, the diurnal changes in source contributions are relatively moderate (e.g., the biomass burning contribution to TC increased from 31% to 43% for the winter sample with the most distinct day-night difference.) This highlights the importance of long-range transport as a source of the carbonaceous aerosol in this region. First results from chemical composition measurements on four of the samples show that the concentration of less refractory organic carbon (desorption temperature up to 200 °C) increases at night-time much more strongly than the concentration of the more refractory carbon. Similarly, the concentration of small organic compounds with m/z < 100 also increases more strongly than heavier compounds. This indicates partitioning of semi-volatile OC as a possible additional night-time source. The chemical composition will be studied in more detail, focusing on diurnal changes in O/C ratios, individual compounds and compound classes, such as hydrocarbons or organic acids. Dusek, U., Meusinger, C., Oyama, B., Ramon, W., de Wilde, P., Holzinger, R., and Röckmann, T.: A thermal desorption system for measuring δ 13 C ratios on organic aerosol, Journal of aerosol science, 66, 72-82, 2013. Holzinger, R., Williams, J., Herrmann, F., Lelieveld, J., Donahue, N., Röckmann, T., 2010. Aerosol analysis using a Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS): a new approach to study processing of organic aerosols. Atmospheric chemistry and physics 10, 2257-2267.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petäjä, T

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. Themore » formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.« less

Collection of Viable Aerosolized Influenza Virus and Other Respiratory Viruses in a Student Health Care Center through Water-Based Condensation Growth

PubMed Central

Pan, Maohua; Bonny, Tania S.; Loeb, Julia; Jiang, Xiao; Eiguren-Fernandez, Arantzazu; Hering, Susanne; Fan, Z. Hugh; Wu, Chang-Yu

2017-01-01

ABSTRACT The dynamics and significance of aerosol transmission of respiratory viruses are still controversial, for the major reasons that virus aerosols are inefficiently collected by commonly used air samplers and that the collected viruses are inactivated by the collection method. Without knowledge of virus viability, infection risk analyses lack accuracy. This pilot study was performed to (i) determine whether infectious (viable) respiratory viruses in aerosols could be collected from air in a real world environment by the viable virus aerosol sampler (VIVAS), (ii) compare and contrast the efficacy of the standard bioaerosol sampler, the BioSampler, with that of the VIVAS for the collection of airborne viruses in a real world environment, and (iii) gain insights for the use of the VIVAS for respiratory virus sampling. The VIVAS operates via a water vapor condensation process to enlarge aerosolized virus particles to facilitate their capture. A variety of viable human respiratory viruses, including influenza A H1N1 and H3N2 viruses and influenza B viruses, were collected by the VIVAS located at least 2 m from seated patients, during a late-onset 2016 influenza virus outbreak. Whereas the BioSampler when operated following our optimized parameters also collected virus aerosols, it was nevertheless overall less successful based on a lower frequency of virus isolation in most cases. This side-by-side comparison highlights some limitations of past studies based on impingement-based sampling, which may have generated false-negative results due to either poor collection efficiency and/or virus inactivation due to the collection process. IMPORTANCE The significance of virus aerosols in the natural transmission of respiratory diseases has been a contentious issue, primarily because it is difficult to collect or sample virus aerosols using currently available air sampling devices. We tested a new air sampler based on water vapor condensation for efficient sampling of viable airborne respiratory viruses in a student health care center as a model of a real world environment. The new sampler outperformed the industry standard device (the SKC BioSampler) in the collection of natural virus aerosols and in maintaining virus viability. These results using the VIVAS indicate that respiratory virus aerosols are more prevalent and potentially pose a greater inhalation biohazard than previously thought. The VIVAS thus appears to be a useful apparatus for microbiology air quality tests related to the detection of viable airborne viruses. PMID:29034325

Accelerated simulation of stochastic particle removal processes in particle-resolved aerosol models

DOE Office of Scientific and Technical Information (OSTI.GOV)

Curtis, J.H.; Michelotti, M.D.; Riemer, N.

2016-10-01

Stochastic particle-resolved methods have proven useful for simulating multi-dimensional systems such as composition-resolved aerosol size distributions. While particle-resolved methods have substantial benefits for highly detailed simulations, these techniques suffer from high computational cost, motivating efforts to improve their algorithmic efficiency. Here we formulate an algorithm for accelerating particle removal processes by aggregating particles of similar size into bins. We present the Binned Algorithm for particle removal processes and analyze its performance with application to the atmospherically relevant process of aerosol dry deposition. We show that the Binned Algorithm can dramatically improve the efficiency of particle removals, particularly for low removalmore » rates, and that computational cost is reduced without introducing additional error. In simulations of aerosol particle removal by dry deposition in atmospherically relevant conditions, we demonstrate about 50-times increase in algorithm efficiency.« less

Aircraft measurements to characterize polluted winter boundary layers: Overview of twin otter flights during the Utah Winter Fine Particulate Matter Study

NASA Astrophysics Data System (ADS)

Brown, S. S.; Baasandorj, M.; Franchin, A.; Middlebrook, A. M.; Goldberger, L.; Thornton, J. A.; Dube, W. P.; McDuffie, E. E.; Womack, C.; Fibiger, D. L.; Moravek, A.; Clark, J. C.; Murphy, J. G.; Mitchell, R.

2017-12-01

Winter air pollution is a significant public health concern. In many regions of the U.S., Europe and Asia, wintertime particulate matter concentrations exceed national and / or international air quality standards. Winter air pollution also represents a scientific challenge because these events occur during stagnation events in shallow, vertically stratified boundary layers whose composition is difficult to probe from surface level measurements. Chemical processes responsible for the conversion of primary emissions to secondary pollutants such as ammonium nitrate aerosol vary with height above ground level. Sources of oxidants are poorly understood and may result from both local chemical production and mixing between shallow inversion layers and background air. During the Utah Winter Fine Particulate Study (UWFPS) in January - February 2017, the NOAA twin otter executed 23 research flights with a payload designed to characterize the formation of ammonium nitrate aerosol in three mountain valleys of northern Utah (Salt Lake, Cache, and Utah). These valleys are subject to periodic episodes of winter aerosol pollution well in excess of U.S. national ambient air quality standards. This presentation will describe the measurement strategy of the twin otter flights to address the specific features of aerosol pollution within winter boundary layer of this region. This strategy is relevant to understanding the broader issue of winter air pollution in other regions and potentially to the design of future studies. The presentation will summarize findings from UWFPS related to boundary layer structure, emissions and chemical processes responsible for ammonium nitrate aerosol in this region.

Spherical agglomerates of pure drug nanoparticles for improved pulmonary delivery in dry powder inhalers

NASA Astrophysics Data System (ADS)

Hu, Jun; Dong, Yuancai; Pastorin, Giorgia; Ng, Wai Kiong; Tan, Reginald B. H.

2013-04-01

The aim of this study was to produce micron-sized spherical agglomerates of pure drug nanoparticles to achieve improved aerosol performance in dry powder inhalers (DPIs). Sodium cromoglicate was chosen as the model drug. Pure drug nanoparticles were prepared through a bottom-up particle formation process, liquid antisolvent precipitation, and then rapidly agglomerated into porous spherical microparticles by immediate (on-line) spray drying. Nonporous spherical drug microparticles with similar geometric size distribution were prepared by conventional spray drying of the aqueous drug solution, which together with the mechanically micronized drug particles were used as the control samples. The three samples were characterized by field emission scanning electron microscopy, laser diffraction, Brunauer-Emmett-Teller analysis, density measurement, powder X-ray diffraction, and in vitro aerosol deposition measurement with a multistage liquid impinger. It was found that drug nanoparticles with a diameter of 100 nm were precipitated and agglomerated into highly porous spherical microparticles with a volume median diameter ( D 50 %) of 2.25 ± 0.08 μm and a specific surface area of 158.63 ± 3.27 m2/g. In vitro aerosol deposition studies showed the fine particle fraction of such spherical agglomerates of drug nanoparticles was increased by more than 50 % in comparison with the control samples, demonstrating significant improvements in aerosol performance. The results of this study indicated the potential of the combined particle engineering process of liquid antisolvent precipitation followed by immediate (on-line) spray drying in the development of novel DPI drug products with improved aerosol performance.

Field Trial of an Aerosol-Based Enclosure Sealing Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harrington, Curtis; Springer, David

2015-09-01

This report presents the results from several demonstrations of a new method for sealing building envelope air leaks using an aerosol sealing process developed by the Western Cooling Efficiency Center at UC Davis. The process involves pressurizing a building while applying an aerosol sealant to the interior. As air escapes through leaks in the building envelope, the aerosol particles are transported to the leaks where they collect and form a seal that blocks the leak. Standard blower door technology is used to facilitate the building pressurization, which allows the installer to track the sealing progress during the installation and automaticallymore » verify the final building tightness. Each aerosol envelope sealing installation was performed after drywall was installed and taped, and the process did not appear to interrupt the construction schedule or interfere with other trades working in the homes. The labor needed to physically seal bulk air leaks in typical construction will not be replaced by this technology.« less

Clear-sky remote sensing in the vicinity of clouds: what can be learned about aerosol changes?

NASA Astrophysics Data System (ADS)

Marshak, Alexander; Varnai, Tamas; Wen, Guoyong

2010-05-01

Studies on aerosol direct and indirect effects require a precise separation of cloud-free and cloudy air. However, separation between cloud-free and cloudy areas from remotely-sensed measurements is ambiguous. The transition zone in the regions around clouds often stretches out tens of km, which are neither precisely clear nor precisely cloudy. We study the transition zone between cloud-free and cloudy air using MODerate-resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) measurements. Both instruments show enhanced clear-sky reflectance (MODIS) and clear-sky backscatterer (CALIPSO) near clouds. Analyzing a large dataset of MODIS observations we examine the effect of three-dimensional (3D) radiative interactions between clouds and cloud-free areas, also known as a cloud adjacency effect. Comparing with CALIPSO clear-sky backscatterer measurements, we show that the cloud adjacency effect may be responsible for a large portion of the enhanced clear sky reflectance observed by MODIS. While aerosol particles are responsible for a large part of the near-cloud enhancements in CALIPSO observations, misidentified or undetected cloud particles are also likely to contribute. As a result, both the nature of these particles (cloud vs. aerosol) and the processes creating them need to be clarified using a quantitative assessment of remote sensing limitations in particle detection and identification. The width and ubiquity of the transition zone near clouds imply that studies of aerosol-cloud interactions and aerosol direct radiative effects need to account for aerosol changes near clouds. Not accounted, these changes can cause systematic biases toward smaller aerosol radiative forcing. On the other hand, including aerosol products near clouds despite their uncertainties may overestimate aerosol radiative forcing. Therefore, there is an urgent need for developing methods that can assess and account for remote sensing challenges and thus allow for including the transition zone into the study. We describe a simple model that estimates the cloud-induced enhanced reflectances of cloud-free areas in the vicinity of clouds. The model assumes that the enhancement is due entirely to Rayleigh scattering and is therefore bigger at shorter wavelengths, thus creating a so-called apparent "bluing" of aerosols in remote sensing retrievals.

Imaging aerosol viscosity

NASA Astrophysics Data System (ADS)

Pope, Francis; Athanasiadis, Thanos; Botchway, Stan; Davdison, Nicholas; Fitzgerald, Clare; Gallimore, Peter; Hosny, Neveen; Kalberer, Markus; Kuimova, Marina; Vysniauskas, Aurimas; Ward, Andy

2017-04-01

Organic aerosol particles play major roles in atmospheric chemistry, climate, and public health. Aerosol particle viscosity is important since it can determine the ability of chemical species such as oxidants, organics or water to diffuse into the particle bulk. Recent measurements indicate that OA may be present in highly viscous states; however, diffusion rates of small molecules such as water appear not to be limited by these high viscosities. We have developed a technique for measuring viscosity that allows for the imaging of aerosol viscosity in micron sized aerosols through use of fluorescence lifetime imaging of viscosity sensitive dyes which are also known as 'molecular rotors'. These rotors can be introduced into laboratory generated aerosol by adding minute quantities of the rotor to aerosol precursor prior to aerosolization. Real world aerosols can also be studied by doping them in situ with the rotors. The doping is achieved through generation of ultrafine aerosol particles that contain the rotors; the ultrafine aerosol particles deliver the rotors to the aerosol of interest via impaction and coagulation. This work has been conducted both on aerosols deposited on microscope coverslips and on particles that are levitated in their true aerosol phase through the use of a bespoke optical trap developed at the Central Laser Facility. The technique allows for the direct observation of kinetic barriers caused by high viscosity and low diffusivity in aerosol particles. The technique is non-destructive thereby allowing for multiple experiments to be carried out on the same sample. It can dynamically quantify and track viscosity changes during atmospherically relevant processes such oxidation and hygroscopic growth (1). This presentation will focus on the oxidation of aerosol particles composed of unsaturated and saturated organic species. It will discuss how the type of oxidant, oxidation rate and the composition of the oxidized products affect the time dependent aerosol viscosity. (1) Hosny, N. A., C. Fitzgerald, A. Vysniauskas, T. Athanasiadis, T. Berkemeier, N. Uygur, U. Pöschl, M. Shiraiwa, M. Kalberer, F.D. Pope and M.K. Kuimova (2016) 'Direct imaging of changes in aerosol particle viscosity upon hydration and chemical aging'. Chemical Science, 17, 32194-32203. http://dx.doi.org/doi:10.1039/C5SC02959G

Characterisation of aerosol combustible mixtures generated using condensation process

NASA Astrophysics Data System (ADS)

Saat, Aminuddin; Dutta, Nilabza; Wahid, Mazlan A.

2012-06-01

An accidental release of a liquid flammable substance might be formed as an aerosol (droplet and vapour mixture). This phenomenon might be due to high pressure sprays, pressurised liquid leaks and through condensation when hot vapour is rapidly cooled. Such phenomena require a fundamental investigation of mixture characterisation prior to any subsequent process such as evaporation and combustion. This paper describes characterisation study of droplet and vapour mixtures generated in a fan stirred vessel using condensation technique. Aerosol of isooctane mixtures were generated by expansion from initially a premixed gaseous fuel-air mixture. The distribution of droplets within the mixture was characterised using laser diagnostics. Nearly monosized droplet clouds were generated and the droplet diameter was defined as a function of expansion time. The effect of changes in pressure, temperature, fuel-air fraction and expansion ratio on droplet diameter was evaluated. It is shown that aerosol generation by expansion was influenced by the initial pressure and temperature, equivalence ratio and expansion rates. All these parameters affected the onset of condensation which in turn affected the variation in droplet diameter.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chitra Sivaraman, PNNL

Cloud droplet number concentration is an important factor in understanding aerosol-cloud interactions. As aerosol concentration increases, it is expected that droplet number concentration (Nd) will increase and droplet size will decrease, for a given liquid water path. This will greatly affect cloud albedo as smaller droplets reflect more shortwave radiation; however, the magnitude and variability of these processes under different environmental conditions is still uncertain.McComiskey et al. (2009) have implemented a method, based onBoers and Mitchell (1994), for calculating Nd from ground-based remote sensing measurements of optical depth and liquid water path. They show that the magnitude of the aerosol-cloudmore » interactions (ACI) varies with a range of factors, including the relative value of the cloud liquid water path (LWP), the aerosol size distribution, and the cloud updraft velocity. Estimates of Nd under a range of cloud types and conditions and at a variety of sites are needed to further quantify the impacts of aerosol cloud interactions. In order to provide data sets for studying aerosol-cloud interactions, the McComiskey et al. (2009) method was implemented as the Droplet Number Concentration (NDROP) value-added product (VAP).« less

SOA formation by biogenic and carbonyl compounds: data evaluation and application.

PubMed

Ervens, Barbara; Kreidenweis, Sonia M

2007-06-01

The organic fraction of atmospheric aerosols affects the physical and chemical properties of the particles and their role in the climate system. Current models greatly underpredict secondary organic aerosol (SOA) mass. Based on a compilation of literature studies that address SOA formation, we discuss different parameters that affect the SOA formation efficiency of biogenic compounds (alpha-pinene, isoprene) and aliphatic aldehydes (glyoxal, hexanal, octanal, hexadienal). Applying a simple model, we find that the estimated SOA mass after one week of aerosol processing under typical atmospheric conditions is increased by a few microg m(-3) (low NO(x) conditions). Acid-catalyzed reactions can create > 50% more SOA mass than processes under neutral conditions; however, other parameters such as the concentration ratio of organics/NO(x), relative humidity, and absorbing mass are more significant. The assumption of irreversible SOA formation not limited by equilibrium in the particle phase or by depletion of the precursor leads to unrealistically high SOA masses for some of the assumptions we made (surface vs volume controlled processes).

Integrating biomass, sulphate and sea-salt aerosol responses into a microphysical chemical parcel model: implications for climate studies.

PubMed

Ghosh, S; Smith, M H; Rap, A

2007-11-15

Aerosols are known to influence significantly the radiative budget of the Earth. Although the direct effect (whereby aerosols scatter and absorb solar and thermal infrared radiation) has a large perturbing influence on the radiation budget, the indirect effect (whereby aerosols modify the microphysical and hence the radiative properties and amounts of clouds) poses a greater challenge to climate modellers. This is because aerosols undergo chemical and physical changes while in the atmosphere, notably within clouds, and are removed largely by precipitation. The way in which aerosols are processed by clouds depends on the type, abundance and the mixing state of the aerosols concerned. A parametrization with sulphate and sea-salt aerosol has been successfully integrated within the Hadley Centre general circulation model (GCM). The results of this combined parametrization indicate a significantly reduced role, compared with previous estimates, for sulphate aerosol in cloud droplet nucleation and, consequently, in indirect radiative forcing. However, in this bicomponent system, the cloud droplet number concentration, N(d) (a crucial parameter that is used in GCMs for radiative transfer calculations), is a smoothly varying function of the sulphate aerosol loading. Apart from sea-salt and sulphate aerosol particles, biomass aerosol particles are also present widely in the troposphere. We find that biomass smoke can significantly perturb the activation and growth of both sulphate and sea-salt particles. For a fixed salt loading, N(d) increases linearly with modest increases in sulphate and smoke masses, but significant nonlinearities are observed at higher non-sea-salt mass loadings. This non-intuitive N(d) variation poses a fresh challenge to climate modellers.

Sensitivity of Homogeneous Ice Nucleation to Aerosol Perturbations and Its Implications for Aerosol Indirect Effects Through Cirrus Clouds

NASA Astrophysics Data System (ADS)

Liu, X.; Shi, X.

2018-02-01

The magnitude and sign of anthropogenic aerosol impacts on cirrus clouds through ice nucleation are still very uncertain. In this study, aerosol sensitivity (ηα), defined as the sensitivity of the number concentration (Ni) of ice crystals formed from homogeneous ice nucleation to aerosol number concentration (Na), is examined based on simulations from a cloud parcel model. The model represents the fundamental process of ice crystal formation that results from homogeneous nucleation. We find that the geometric dispersion (σ) of the aerosol size distribution used in the model is a key factor for ηα. For a monodisperse size distribution, ηα is close to zero in vertical updrafts (V < 50 cm s-1) typical of cirrus clouds. However, ηα increases to 0.1-0.3 (i.e., Ni increases by a factor of 1.3-2.0 for a tenfold increase in Na) if aerosol particles follow lognormal size distributions with a σ of 1.6-2.3 in the upper troposphere. By varying the input aerosol and environmental parameters, our model reproduces a large range of ηα values derived from homogeneous ice nucleation parameterizations widely used in global climate models (GCMs). The differences in ηα from these parameterizations can translate into a range of anthropogenic aerosol longwave indirect forcings through cirrus clouds from 0.05 to 0.36 W m-2 with a GCM. Our study suggests that a larger ηα (0.1-0.3) is more plausible and the homogeneous nucleation parameterizations should include a realistic aerosol size distribution to accurately quantify anthropogenic aerosol indirect effects.

Use of Field Observations for Understanding Controls of Polar Low Cloud Microphysical Properties

NASA Astrophysics Data System (ADS)

McFarquhar, G. M.

2016-12-01

Although arctic clouds have a net warming effect on the Arctic surface, their radiative effect is sensitive to cloud microphysical properties, namely the sizes, phases and shapes of cloud particles. Such cloud properties are influenced by the numbers, compositions and sizes of aerosols, meteorological conditions, and surface characteristics. Uncertainty in representing cloud-aerosol interactions in varying environmental conditions and associated feedbacks is a major cause in our lack of understanding of why the Arctic is warming faster than the rest of the Earth. Here, the understanding of cloud-aerosol interactions gained from past arctic field experiments is reviewed. Such studies have characterized the structure of single-layer mixed phase clouds that are ubiquitous in the Arctic and investigated different aerosol indirect effect mechanisms acting in these clouds. But, it is still unknown what controls the amount of supercooled water in arctic clouds (especially in complex frequently occurring multi-layer clouds), how probability distributions of cloud properties and radiative heating and their subsequent impact on temperature profiles and underlying snow and sea ice cover vary with aerosol loading and composition in different surface and meteorological conditions, how the composition and concentration of arctic aerosols and cloud microphysical properties vary annually and interannually, and how cloud-aerosol-radiative interactions can be better represented in models with varying temporal and spatial scales. These needs can be addressed in two ways. First, there is a need for comprehensive and routine aircraft, UAV and tethered balloon measurements in the presence of ground, air or space-based remote sensors over a variety of surface and meteorological conditions. Second, planned observational campaigns (the Measurements of Aerosols Radiation and Clouds over the Southern Oceans MARCUS and the Southern Oceans Cloud Radiation Transport Experimental Study SOCRATES) should provide cloud, aerosol, radiative and precipitation observations over the pristine and continually cloudy Southern Oceans that are remote from natural and continental anthropogenic aerosol sources should provide a process-oriented understanding of cloud-aerosol interactions in liquid and ice clouds.

Aerosolization of cyanobacterial cells across ecosystem boundaries in the McMurdo Dry Valleys, Antarctica

NASA Astrophysics Data System (ADS)

Trout-Haney, J.; Heindel, R. C.; Virginia, R. A.

2017-12-01

Cyanobacteria play a major ecological role in polar freshwaters, occurring predominately as small single cells in the water column, i.e., picocyanobacteria, or large multicellular colonies and mats that reside on the lake bottom. Cyanobacteria are also present in terrestrial polar habitats, including within soils, soil crusts, rocks, and glacial ice. Despite their predominance in polar ecosystems, the extent to which cyanobacteria move between terrestrial and aquatic landscape units remains poorly understood. In polar deserts such as the McMurdo Dry Valleys, aeolian processes influence terrestrial landscape morphology and drive the transport of sediments and other particles. Water surfaces can also act as a source of aerosolized particles, such as the production of sea spray aerosols through wave breaking in marine environments. However, aerosolization from freshwater bodies has been far less studied, especially in polar regions. We conducted a field-study to examine the transport of aerosolized cyanobacterial cells from ponds and soils in the McMurdo Dry Valleys. We used highly portable aerosol collection devices fitted with GF/F filters combusted at 500°C (0.3 µm) to collect small particles, such as picocyanobacteria (0.2 - 2 µm), from near-shore water and adjacent soil. We used epifluorescence microscopy to quantify aerosolized cells, with excitation filters for chlorophyll a (435 nm) and phycobilin pigments (572 nm), to distinguish cyanobacterial cells. We detected aerosolized picocyanobacterial cells from all ponds and soils sampled, indicating that these cells may be quite mobile and transported across ecosystem boundaries. We observed cyanobacterial cells individually, clustered, and associated with other organic material, suggesting multiple modes of cell transport. Further, we investigated the potential for aerosolization of toxin-producing cyanobacterial taxa (or unbound cyanotoxins), and the ecological and ecosystem-scale implications of aerosolization on cyanobacterial transport, cyanotoxin exposure, and nutrient cycling. Our results highlight the role of aerosolization in transporting cyanobacterial cells and suggest that even in extreme polar deserts, biological connectivity exists between aquatic and terrestrial habitats.

Spatial and temporal distributions of aerosol concentrations and depositions in Asia during the year 2010.

PubMed

Park, Soon-Ung; Lee, In-Hye; Joo, Seung Jin

2016-01-15

Aerosol Modeling System (AMS) that is consisted of the Asian Dust Aerosol Model2 (ADAM2) and the Community Multi-scale Air Quality (CMAQ) modeling system has been employed to document the spatial distributions of the monthly and the annual averaged concentration of both the Asian dust (AD) aerosol and the anthropogenic aerosol (AA), and their total depositions in the Asian region for the year 2010. It is found that the annual mean surface aerosol (PM10) concentrations in the Asian region affect in a wide region as a complex mixture of AA and AD aerosols; they are predominated by the AD aerosol in the AD source region of northern China and Mongolia with a maximum concentration exceeding 300 μg m(-3); AAs are predominated in the high pollutant emission regions of southern and eastern China and northern India with a maximum concentration exceeding 110 μg m(-3); while the mixture of AA and AD aerosols is dominated in the downwind regions extending from the Yellow Sea to the Northwest Pacific Ocean. It is also found that the annual total deposition of aerosols in the model domain is found to be 485 Tg (372 Tg by AD aerosol and 113 Tg by AA), of which 66% (319 Tg) is contributed by the dry deposition (305 Tg by AD aerosol and 14 Tg by AA) and 34% (166 Tg) by the wet deposition (66 Tg by AD aerosol and 100 Tg by AA), suggesting about 77% of the annual total deposition being contributed by the AD aerosol mainly through the dry deposition process and 24% of it by AA through the wet deposition process. The monthly mean aerosol concentration and the monthly total deposition show a significant seasonal variation with high in winter and spring, and low in summer. Copyright © 2015 Elsevier B.V. All rights reserved.

Tying Biological Activity to Changes in Sea Spray Aerosol Chemical Composition via Single Particle Analyses

NASA Astrophysics Data System (ADS)

Sultana, C. M.; Lee, C.; Collins, D. B.; Axson, J. L.; Laskina, O.; Grandquist, J. R.; Grassian, V. H.; Prather, K. A.

2014-12-01

In remote marine environments, sea spray aerosols (SSA) often represent the greatest aerosol burden, thus having significant impacts on direct radiative interactions and cloud processes. Previous studies have shown that SSA is a complex mixture of inorganic salts and an array of dissolved and particulate organic components. Enrichment of SSA organic content is often correlated to seawater chlorophyll concentrations, a measure of oceanic biological activity. As the physical and chemical properties of aerosols control their radiative effects, recent studies conducted by the Center for Aerosol Impacts on Climate and the Environment have endeavored to further elucidate the ties between marine biological activity and primary SSA chemical composition using highly time resolved single particle analyses. A series of experiments performed in the recently developed Marine Aerosol Reference Tank evaluated the effect of changing marine microbial populations on SSA chemical composition, which was monitored via an aerosol time-of-flight mass spectrometer and a variety of offline spectroscopic and microscopic techniques. Each experiment was initiated using unfiltered and untreated seawater, thus maintaining a high level of biogeochemical complexity. This study is the first of its kind to capture daily changes in the primary SSA mixing state over the growth and death of a natural phytoplankton bloom. Increases in organic aerosol types (0.4-3 μm), internally and externally mixed with sea salt, could not be correlated to chlorophyll concentrations. Maximum production of these populations occurred two to four days after the in vivo chlorophyll fluorescence peaked in intensity. This work is in contrast to the current paradigm of correlating SSA organic content to seawater chlorophyll concentration.

The NASA-AMES Research Center Stratospheric Aerosol Model. 1. Physical Processes and Computational Analogs

NASA Technical Reports Server (NTRS)

Turco, R. P.; Hamill, P.; Toon, O. B.; Whitten, R. C.; Kiang, C. S.

1979-01-01

A time-dependent one-dimensional model of the stratospheric sulfate aerosol layer is presented. In constructing the model, a wide range of basic physical and chemical processes are incorporated in order to avoid predetermining or biasing the model predictions. The simulation, which extends from the surface to an altitude of 58 km, includes the troposphere as a source of gases and condensation nuclei and as a sink for aerosol droplets. The size distribution of aerosol particles is resolved into 25 categories with particle radii increasing geometrically from 0.01 to 2.56 microns such that particle volume doubles between categories.

The role of semi-volatile organic compounds in the mesoscale evolution of biomass burning aerosol: a modeling case study of the 2010 mega-fire event in Russia

NASA Astrophysics Data System (ADS)

Konovalov, I. B.; Beekmann, M.; Berezin, E. V.; Petetin, H.; Mielonen, T.; Kuznetsova, I. N.; Andreae, M. O.

2015-12-01

Chemistry transport models (CTMs) are an indispensable tool for studying and predicting atmospheric and climate effects associated with carbonaceous aerosol from open biomass burning (BB); this type of aerosol is known to contribute significantly to both global radiative forcing and to episodes of air pollution in regions affected by wildfires. Improving model performance requires systematic comparison of simulation results with measurements of BB aerosol and elucidation of possible reasons for discrepancies between them, which, by default, are frequently attributed in the literature to uncertainties in emission data. Based on published laboratory data on the atmospheric evolution of BB aerosol and using the volatility basis set (VBS) framework for organic aerosol modeling, we examined the importance of taking gas-particle partitioning and oxidation of semi-volatile organic compounds (SVOCs) into account in simulations of the mesoscale evolution of smoke plumes from intense wildfires that occurred in western Russia in 2010. Biomass burning emissions of primary aerosol components were constrained with PM10 and CO data from the air pollution monitoring network in the Moscow region. The results of the simulations performed with the CHIMERE CTM were evaluated by considering, in particular, the ratio of smoke-related enhancements in PM10 and CO concentrations (ΔPM10 and ΔCO) measured in Finland (in the city of Kuopio), nearly 1000 km downstream of the fire emission sources. It is found that while the simulations based on a "conventional" approach to BB aerosol modeling (disregarding oxidation of SVOCs and assuming organic aerosol material to be non-volatile) strongly underestimated values of ΔPM10/ΔCO observed in Kuopio (by a factor of 2), employing the "advanced" representation of atmospheric processing of organic aerosol material resulted in bringing the simulations to a much closer agreement with the ground measurements. Furthermore, taking gas-particle partitioning and oxidation of SVOCs into account is found to result in a major improvement of the agreement of simulations and satellite measurements of aerosol optical depth, as well as in considerable changes in predicted aerosol composition and top-down BB aerosol emission estimates derived from AOD measurements.

Simple aerosol correction technique based on the spectral relationships of the aerosol multiple-scattering reflectances for atmospheric correction over the oceans.

PubMed

Ahn, Jae-Hyun; Park, Young-Je; Kim, Wonkook; Lee, Boram

2016-12-26

An estimation of the aerosol multiple-scattering reflectance is an important part of the atmospheric correction procedure in satellite ocean color data processing. Most commonly, the utilization of two near-infrared (NIR) bands to estimate the aerosol optical properties has been adopted for the estimation of the effects of aerosols. Previously, the operational Geostationary Color Ocean Imager (GOCI) atmospheric correction scheme relies on a single-scattering reflectance ratio (SSE), which was developed for the processing of the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) data to determine the appropriate aerosol models and their aerosol optical thicknesses. The scheme computes reflectance contributions (weighting factor) of candidate aerosol models in a single scattering domain then spectrally extrapolates the single-scattering aerosol reflectance from NIR to visible (VIS) bands using the SSE. However, it directly applies the weight value to all wavelengths in a multiple-scattering domain although the multiple-scattering aerosol reflectance has a non-linear relationship with the single-scattering reflectance and inter-band relationship of multiple scattering aerosol reflectances is non-linear. To avoid these issues, we propose an alternative scheme for estimating the aerosol reflectance that uses the spectral relationships in the aerosol multiple-scattering reflectance between different wavelengths (called SRAMS). The process directly calculates the multiple-scattering reflectance contributions in NIR with no residual errors for selected aerosol models. Then it spectrally extrapolates the reflectance contribution from NIR to visible bands for each selected model using the SRAMS. To assess the performance of the algorithm regarding the errors in the water reflectance at the surface or remote-sensing reflectance retrieval, we compared the SRAMS atmospheric correction results with the SSE atmospheric correction using both simulations and in situ match-ups with the GOCI data. From simulations, the mean errors for bands from 412 to 555 nm were 5.2% for the SRAMS scheme and 11.5% for SSE scheme in case-I waters. From in situ match-ups, 16.5% for the SRAMS scheme and 17.6% scheme for the SSE scheme in both case-I and case-II waters. Although we applied the SRAMS algorithm to the GOCI, it can be applied to other ocean color sensors which have two NIR wavelengths.

Retrieval of tropospheric aerosol properties over land from visible and near-infrared spectral reflectance: Application over Maryland

NASA Astrophysics Data System (ADS)

Levy, Robert Carroll

Aerosols are major components of the Earth's global climate system, affecting the radiation budget and cloud processes of the atmosphere. When located near the surface, high concentrations lead to lowered visibility, increased health problems and generally reduced quality of life for the human population. Over the United States mid-Atlantic region, aerosol pollution is a problem mainly during the summer. Satellites, such as the MODerate Imaging Spectrometer (MODIS), from their vantage point above the atmosphere, provide unprecedented coverage of global and regional aerosols over land. During MODIS' eight-year operation, exhaustive data validation and analyses have shown how the algorithm should be improved. This dissertation describes the development of the 'second-generation' operational algorithm for retrieval of global tropospheric aerosol properties over dark land surfaces, from MODIS-observed spectral reflectance. New understanding about global aerosol properties, land surface reflectance characteristics, and radiative transfer properties were learned in the process. This new operational algorithm performs a simultaneous inversion of reflectance in two visible channels (0.47 and 0.66 mum) and one shortwave infrared channel (2.12 mum), thereby having increased sensitivity to coarse aerosol. Inversion of the three channels retrieves the aerosol optical depth (tau) at 0.55 mum, the percentage of non-dust (fine model) aerosol (eta) and the surface reflectance. This algorithm is applied globally, and retrieves tau that is highly correlated (y = 0.02 + 1.0x, R=0.9) with ground-based sunphotometer measurements. The new algorithm estimates the global, over-land, long-term averaged tau ˜ 0.21, a 25% reduction from previous MODIS estimates. This leads to reducing estimates of global, non-desert, over-land aerosol direct radiative effect (all aerosols) by 1.7 W·m-2 (0.5 W·m-2 over the entire globe), which significantly impacts assessment of aerosol direct radiative forcing (contribution from anthropogenic aerosols only). Over the U.S. mid-Atlantic region, validated retrievals of tau (an integrated column property) can help to estimate surface PM2.5 concentration, a monitored criteria air quality property. The 3-dimensional aerosol loading in the region is characterized using aircraft measurements and the Community Multi-scale Air Quality Model (CMAQ) model, leading to some convergence of observed quantities and modeled processes.

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing

NASA Astrophysics Data System (ADS)

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen; Goldstein, Allen H.; Guenther, Alex B.; Jimenez, Jose L.; Kuang, Chongai; Laskin, Alexander; Martin, Scot T.; Ng, Nga Lee; Petaja, Tuukka; Pierce, Jeffrey R.; Rasch, Philip J.; Roldin, Pontus; Seinfeld, John H.; Shilling, John; Smith, James N.; Thornton, Joel A.; Volkamer, Rainer; Wang, Jian; Worsnop, Douglas R.; Zaveri, Rahul A.; Zelenyuk, Alla; Zhang, Qi

2017-06-01

Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.

Biomass Burning Observation Project (BBOP) Final Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kleinman, LI; Sedlacek, A. J.

2016-01-01

The Biomass Burning Observation Project (BBOP) was conducted to obtain a better understanding of how aerosols generated from biomass fires affect the atmosphere and climate. It is estimated that 40% of carbonaceous aerosol produced originates from biomass burning—enough to affect regional and global climate. Several biomass-burning studies have focused on tropical climates; however, few campaigns have been conducted within the United States, where millions of acres are burned each year, trending to higher values and greater climate impacts because of droughts in the West. Using the Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF), the BBOP deployed the Gulfstream-1 (G-1) aircraftmore » over smoke plumes from active wildfire and agricultural burns to help identify the impact of these events and how impacts evolve with time. BBOP was one of very few studies that targeted the near-field time evolution of aerosols and aimed to obtain a process-level understanding of the large changes that occur within a few hours of atmospheric processing.« less

Quantification of Semi-Volatile gas-phase Organic Compounds (SVOCs) & Organic Aerosol species and the role of SVOCs in Secondary Organic Aerosol formation

NASA Astrophysics Data System (ADS)

Khan, M. H.; Holzinger, R.

2013-12-01

A Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS) with different sampling systems (multi-stage denuder for gas phase and impact on a collector for aerosol phase) has been deployed in summer 2013 during the Southern Oxidant and Aerosol Study (SOAS) at the SEARCH ground site, Centreville, Alabama for in-situ gas phase and aerosol measurements on an hourly time resolution. A bunch of DB-1 column (0.53 mm x 5.0 μm) is used in the denuder for capturing the bulk of SVOCs and a collection-thermal-desorption (CTD) cell is used for collecting aerosol particles. Several hundreds semivolatile organic compounds (SVOCs) in gas phase and aerosol phases have been detected. The high mass resolution capabilities of ~5000, low detection limit (<0.05 pptv for gas species, <0.01 ng m-3 for aerosol species) and good physical and chemical characterization of SVOCs with the TD-PTR-MS allows constraining both, the quantity and the chemical composition. The SEARCH site was highly impacted by Biogenic Volatile Organic Compounds (BVOCs) and occasionally influenced by anthropogenic pollution. BVOCs and their oxidation products are capable of partitioning into the particle phase, so their simultaneous quantification in both phases has been used to determine the gas/particle-phase partitioning. Our results show the expected diurnal variation based on the changes of air temperature for many species. The results from this study give valuable insights into sources and processing of Secondary Organic Aerosols (SOAs) that can be used to improve parameterization algorithms in regional and global climate models.

Low-Temperature Alkaline pH Hydrolysis of Oxygen-Free Titan Tholins: Carbonates' Impact.

PubMed

Brassé, Coralie; Buch, Arnaud; Coll, Patrice; Raulin, François

2017-01-01

Titan, the largest moon of Saturn, is one of the key planetary objects in the field of exobiology. Its dense, nitrogen-rich atmosphere is the site of important organic chemistry. This paper focuses on the organic aerosols produced in Titan's atmosphere that play an important role in atmospheric and surface processes and in organic chemistry as it applies to exobiological interests. To produce reliable laboratory analogues of these aerosols, we developed, tested, and optimized a device for the synthesis of clean tholins. The potential chemical evolution of Titan aerosols at Titan's surface has been studied, in particular, the possible interaction between aerosols and putative ammonia-water cryomagma. Modeling of the formation of Saturn's atmosphere has permitted the characterization of a composition of salts in the subsurface ocean and cryolava. From this new and original chemical composition, a laboratory study of several hydrolyses of tholins was carried out. The results obtained show the formation of many organic compounds, among them, species identified only in the presence of salts. In addition, a list of potential precursors of these compounds was established, which could provide a database for research of the chemical composition of tholins and/or aerosols of Titan. Key Words: Titan tholins-Titan aerosols-Hydrolysis-Carbonates-Titan's surface. Astrobiology 17, 8-26.

Production of inhalation phage powders using spray freeze drying and spray drying techniques for treatment of respiratory infections

PubMed Central

Leung, Sharon S.Y.; Parumasivam, Thaigarajan; Gao, Fiona G.; Carrigy, Nicholas B.; Vehring, Reinhard; Finlay, Warren H.; Morales, Sandra; Britton, Warwick J; Kutter, Elizabeth; Chan, Hak-Kim

2016-01-01

Purpose The potential of aerosol phage therapy for treating lung infections has been demonstrated in animal models and clinical studies. This work compared the performance of two dry powder formation techniques, spray freeze drying (SFD) and spray drying (SD), in producing inhalable phage powders. Method A Pseudomonas podoviridae phage, PEV2, was incorporated into multi-component formulation systems consisting of trehalose, mannitol and L-leucine (F1 = 60:20:20 and F2 = 40:40:20). The phage titer loss after the SFD and SD processes and in vitro aerosol performance of the produced powders were assessed. Results A significant titer loss (~ 2 log) was noted for droplet generation using an ultrasonic nozzle employed in the SFD method, but the conventional two-fluid nozzle used in the SD method was less destructive for the phage (~0.75 log loss). The phage were more vulnerable during the evaporative drying process (~0.75 log further loss) compared with the freeze drying step, which caused negligible phage loss. In vitro aerosol performance showed that the SFD powders (~80% phage recovery) provided better phage protection than the SD powders (~20% phage recovery) during the aerosolization process. Despite this, higher total lung doses were obtained for the SD formulations (SD-F1 = 13.1 ± 1.7 × 104 pfu and SD-F2 = 11.0 ± 1.4 × 104 pfu) than from their counterpart SFD formulations (SFD-F1 = 8.3 ± 1.8 × 104 pfu and SFD-F2 = 2.1 ± 0.3 × 104 pfu). Conclusion Overall, the SD method caused less phage reduction during the powder formation process and the resulted powders achieved better aerosol performance for PEV2. PMID:26928668

Investigation of aerosol indirect effects on simulated flash-flood heavy rainfall over Korea

NASA Astrophysics Data System (ADS)

Lim, Kyo-Sun Sunny; Hong, Song-You

2012-11-01

This study investigates aerosol indirect effects on the development of heavy rainfall near Seoul, South Korea, on 12 July 2006, focusing on precipitation amount. The impact of the aerosol concentration on simulated precipitation is evaluated by varying the initial cloud condensation nuclei (CCN) number concentration in the Weather Research and Forecasting (WRF) Double-Moment 6-class (WDM6) microphysics scheme. The simulations are performed under clean, semi-polluted, and polluted conditions. Detailed analysis of the physical processes that are responsible for surface precipitation, including moisture and cloud microphysical budgets shows enhanced ice-phase processes to be the primary driver of increased surface precipitation under the semi-polluted condition. Under the polluted condition, suppressed auto-conversion and the enhanced evaporation of rain cause surface precipitation to decrease. To investigate the role of environmental conditions on precipitation response under different aerosol number concentrations, a set of sensitivity experiments are conducted with a 5 % decrease in relative humidity at the initial time, relative to the base simulations. Results show ice-phase processes having small sensitivity to CCN number concentration, compared with the base simulations. Surface precipitation responds differently to CCN number concentration under the lower humidity initial condition, being greatest under the clean condition, followed by the semi-polluted and polluted conditions.

Laboratory and field based evaluation of chromatography ...

EPA Pesticide Factsheets

The Monitor for AeRosols and GAses in ambient air (MARGA) is an on-line ion-chromatography-based instrument designed for speciation of the inorganic gas and aerosol ammonium-nitrate-sulfate system. Previous work to characterize the performance of the MARGA has been primarily based on field comparison to other measurement methods to evaluate accuracy. While such studies are useful, the underlying reasons for disagreement among methods are not always clear. This study examines aspects of MARGA accuracy and precision specifically related to automated chromatography analysis. Using laboratory standards, analytical accuracy, precision, and method detection limits derived from the MARGA chromatography software are compared to an alternative software package (Chromeleon, Thermo Scientific Dionex). Field measurements are used to further evaluate instrument performance, including the MARGA’s use of an internal LiBr standard to control accuracy. Using gas/aerosol ratios and aerosol neutralization state as a case study, the impact of chromatography on measurement error is assessed. The new generation of on-line chromatography-based gas and particle measurement systems have many advantages, including simultaneous analysis of multiple pollutants. The Monitor for Aerosols and Gases in Ambient Air (MARGA) is such an instrument that is used in North America, Europe, and Asia for atmospheric process studies as well as routine monitoring. While the instrument has been evaluat

Study on Dicarboxylic Acids in Aerosol Samples with Capillary Electrophoresis

PubMed Central

Adler, Heidi; Sirén, Heli

2014-01-01

The research was performed to study the simultaneous detection of a homologous series of α, ω-dicarboxylic acids (C2–C10), oxalic, malonic, succinic, glutaric, adipic, pimelic, suberic, azelaic, and sebacic acids, with capillary electrophoresis using indirect UV detection. Good separation efficiency in 2,6-pyridinedicarboxylic acid as background electrolyte modified with myristyl trimethyl ammonium bromide was obtained. The dicarboxylic acids were ionised and separated within five minutes. For the study, authentic samples were collected onto dry cellulose membrane filters of a cascade impactor (12 stages) from outdoor spring aerosols in an urban area. Hot water and ultrasonication extraction methods were used to isolate the acids from membrane filters. Due to the low concentrations of acids in the aerosols, the extracts were concentrated with solid-phase extraction (SPE) before determination. The enrichment of the carboxylic acids was between 86 and 134% with sample pretreatment followed by 100-time increase by preparation of the sample to 50 μL. Inaccuracy was optimised for all the sample processing steps. The aerosols contained dicarboxylic acids C2–C10. Then, mostly they contained C2, C5, and C10. Only one sample contained succinic acid. In the study, the concentrations of the acids in aerosols were lower than 10 ng/m3. PMID:24729915

Assessment of Aerosol Distributions from GEOS-5 Using the CALIPSO Feature Mask

NASA Technical Reports Server (NTRS)

Welton, Ellsworth

2010-01-01

A-train sensors such as MODIS, MISR, and CALIPSO are used to determine aerosol properties, and in the process a means of estimating aerosol type (e.g. smoke vs. dust). Correct classification of aerosol type is important for climate assessment, air quality applications, and for comparisons and analysis with aerosol transport models. The Aerosols-Clouds-Ecosystems (ACE) satellite mission proposed in the NRC Decadal Survey describes a next generation aerosol and cloud suite similar to the current A-train, including a lidar. The future ACE lidar must be able to determine aerosol type effectively in conjunction with modeling activities to achieve ACE objectives. Here we examine the current capabilities of CALIPSO and the NASA Goddard Earth Observing System general circulation model and data assimilation system (GEOS-5), to place future ACE needs in context. The CALIPSO level 2 feature mask includes vertical profiles of aerosol layers classified by type. GEOS-5 provides global 3D aerosol mass for sulfate, sea salt, dust, and black and organic carbon. A GEOS aerosol scene classification algorithm has been developed to provide estimates of aerosol mixtures and extinction profiles along the CALIPSO orbit track. In previous work, initial comparisons between GEOS-5 derived aerosol mixtures and CALIPSO derived aerosol types were presented for July 2007. In general, the results showed that model and lidar derived aerosol types did not agree well in the boundary layer. Agreement was poor over Europe, where CALIPSO indicated the presence of dust and pollution mixtures yet GEOS-5 was dominated by pollution with little dust. Over the ocean in the tropics, the model appeared to contain less sea salt than detected by CALIPSO, yet at high latitudes the situation was reserved. Agreement between CALIPSO and GEOS-5, aerosol types improved above the boundary layer, primarily in dust and smoke dominated regions. At higher altitudes (> 5 km), the model contained aerosol layers not detected by CALIPSO. Here we present new results for a full year study using the new Version 3 CALIPSO data and most recent GEOS-5 model results.

Mass spectrometric airborne measurements of submicron aerosol and cloud residual composition in tropic deep convection during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

Schulz, Christiane; Schneider, Johannes; Mertes, Stephan; Kästner, Udo; Weinzierl, Bernadett; Sauer, Daniel; Fütterer, Daniel; Walser, Adrian; Borrmann, Stephan

2015-04-01

Airborne measurements of submicron aerosol and cloud particles were conducted in the region of Manaus (Amazonas, Brazil) during the ACRIDICON-CHUVA campaign in September 2014. ACRIDICON-CHUVA aimed at the investigation of convective cloud systems in order to get a better understanding and quantification of aerosol-cloud-interactions and radiative effects of convective clouds. For that, data from airborne measurements within convective cloud systems are combined with satellite and ground-based data. We used a C-ToF-AMS (Compact-Time-of-Flight-Aerosol-Mass-Spectrometer) to obtain information on aerosol composition and vertical profiles of different aerosol species, like organics, sulphate, nitrate, ammonium and chloride. The instrument was operated behind two different inlets: The HASI (HALO Aerosol Submicrometer Inlet) samples aerosol particles, whereas the CVI (Counterflow Virtual Impactor) samples cloud droplets and ice particles during in-cloud measurements, such that cloud residual particles can be analyzed. Differences in aerosol composition inside and outside of clouds and cloud properties over forested or deforested region were investigated. Additionally, the in- and outflow of convective clouds was sampled on dedicated cloud missions in order to study the evolution of the clouds and the processing of aerosol particles. First results show high organic aerosol mass concentrations (typically 15 μg/m3 and during one flight up to 25 μg/m3). Although high amounts of organic aerosol in tropic air over rainforest regions were expected, such high mass concentrations were not anticipated. Next to that, high sulphate aerosol mass concentrations (about 4 μg/m3) were measured at low altitudes (up to 5 km). During some flights organic and nitrate aerosol was observed with higher mass concentrations at high altitudes (10-12 km) than at lower altitudes, indicating redistribution of boundary layer particles by convection. The cloud residuals measured during in-cloud sampling through the CVI contained mainly organic material and, to a lesser extent, nitrate.

Extending "Deep Blue" aerosol retrieval coverage to cases of absorbing aerosols above clouds: Sensitivity analysis and first case studies

NASA Astrophysics Data System (ADS)

Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.; Lee, J.; Redemann, J.; Schmid, B.; Shinozuka, Y.

2016-05-01

Cases of absorbing aerosols above clouds (AACs), such as smoke or mineral dust, are omitted from most routinely processed space-based aerosol optical depth (AOD) data products, including those from the Moderate Resolution Imaging Spectroradiometer (MODIS). This study presents a sensitivity analysis and preliminary algorithm to retrieve above-cloud AOD and liquid cloud optical depth (COD) for AAC cases from MODIS or similar sensors, for incorporation into a future version of the "Deep Blue" AOD data product. Detailed retrieval simulations suggest that these sensors should be able to determine AAC AOD with a typical level of uncertainty ˜25-50% (with lower uncertainties for more strongly absorbing aerosol types) and COD with an uncertainty ˜10-20%, if an appropriate aerosol optical model is known beforehand. Errors are larger, particularly if the aerosols are only weakly absorbing, if the aerosol optical properties are not known, and the appropriate model to use must also be retrieved. Actual retrieval errors are also compared to uncertainty envelopes obtained through the optimal estimation (OE) technique; OE-based uncertainties are found to be generally reasonable for COD but larger than actual retrieval errors for AOD, due in part to difficulties in quantifying the degree of spectral correlation of forward model error. The algorithm is also applied to two MODIS scenes (one smoke and one dust) for which near-coincident NASA Ames Airborne Tracking Sun photometer (AATS) data were available to use as a ground truth AOD data source, and found to be in good agreement, demonstrating the validity of the technique with real observations.

Evaluating WRF-Chem aerosol indirect effects in Southeast Pacific marine stratocumulus during VOCALS-REx

DOE Office of Scientific and Technical Information (OSTI.GOV)

Saide, Pablo; Spak, S. N.; Carmichael, Gregory

2012-03-30

We evaluate a regional-scale simulation with the WRF-Chem model for the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx), which sampled the Southeast Pacific's persistent stratocumulus deck. Evaluation of VOCALS-REx ship-based and aircraft observations focuses on analyzing how aerosol loading affects marine boundary layer (MBL) dynamics and cloud microphysics. We compare local time series and campaign averaged longitudinal gradients, and highlight differences in model simulations with (W) and without wet (NW) deposition processes. The higher aerosol loadings in the NW case produce considerable changes in MBL dynamics and cloud microphysics, in accordance with the established conceptualmore » model of aerosol indirect effects. These include increase in cloud albedo, increase in MBL and cloud heights, drizzle suppression, increase in liquid water content, and increase in cloud lifetime. Moreover, better statistical representation of aerosol mass and number concentration improves model fidelity in reproducing observed spatial and temporal variability in cloud properties, including top and base height, droplet concentration, water content, rain rate, optical depth (COD) and liquid water path (LWP). Together, these help to quantify confidence in WRF-Chem's modeled aerosol-cloud interactions, while identifying structural and parametric uncertainties including: irreversibility in rain wet removal; overestimation of marine DMS and sea salt emissions and accelerated aqueous sulfate conversion. Our findings suggest that WRF-Chem simulates marine cloud-aerosol interactions at a level sufficient for applications in forecasting weather and air quality and studying aerosol climate forcing, including the reliability required for policy analysis and geo-engineering applications.« less

Impacts of Cross-Platform Vicarious Calibration on the Deep Blue Aerosol Retrievals for Moderate Resolution Imaging Spectroradiometer Aboard Terra

NASA Technical Reports Server (NTRS)

Jeong, Myeong-Jae; Hsu, N. Christina; Kwiatkowska, Ewa J.; Franz, Bryan A.; Meister, Gerhard; Salustro, Clare E.

2012-01-01

The retrieval of aerosol properties from spaceborne sensors requires highly accurate and precise radiometric measurements, thus placing stringent requirements on sensor calibration and characterization. For the Terra/Moderate Resolution Imaging Spedroradiometer (MODIS), the characteristics of the detectors of certain bands, particularly band 8 [(B8); 412 nm], have changed significantly over time, leading to increased calibration uncertainty. In this paper, we explore a possibility of utilizing a cross-calibration method developed for characterizing the Terral MODIS detectors in the ocean bands by the National Aeronautics and Space Administration Ocean Biology Processing Group to improve aerosol retrieval over bright land surfaces. We found that the Terra/MODIS B8 reflectance corrected using the cross calibration method resulted in significant improvements for the retrieved aerosol optical thickness when compared with that from the Multi-angle Imaging Spectroradiometer, Aqua/MODIS, and the Aerosol Robotic Network. The method reported in this paper is implemented for the operational processing of the Terra/MODIS Deep Blue aerosol products.

Lidar Measurements of Ozone, Aerosols, and Clouds Observed in the Tropics Near Central America During TC4-Costa Rica

NASA Astrophysics Data System (ADS)

Hair, J. W.; Browell, E.; Butler, C.; Fenn, M.; Notari, A.; Simpson, S.; Ismail, S.; Avery, M.

2007-12-01

Large-scale measurements of ozone and aerosol distributions were made from the NASA DC-8 aircraft during the TC4 (Tropical Composition, Cloud, and Climate Coupling) field experiment conducted from June 28 - August 10, 2007 based in San Jose, Costa Rica. Remote measurements were made with an airborne lidar to provide ozone and multiple-wavelength aerosol and cloud backscatter profiles from near the surface to above the tropopause along the flight track. Aerosol depolarization measurements were also made for the detection of nonspherical aerosols, such as mineral dust, biomass burning, and recent emissions from South American volcanoes. Long-range transport of Saharan dust with depolarizing aerosols was frequently observed in the lower troposphere both over the Caribbean Sea and Pacific Ocean and within the marine boundary layer. In addition, visible and sub-visible cirrus clouds were observed with the multi-wavelength backscatter and depolarization measurements. Initial distributions of ozone, aerosol, and cloud are presented which will be used to interpret large-scale atmospheric processes. In situ measurements of ozone and aerosols made onboard the DC-8 will be compared to the remote lidar measurements. This paper provides a first look at the characteristics of ozone, aerosol, and cloud distributions that were encountered during this field experiment and provide a unique dataset that will be further related through satellite data, backward trajectories, and chemical transport models (CTM) to sources and sinks of ozone, aerosols, and clouds and to dynamical, chemical, and radiative processes.

Biogenic Aerosols—Effects on Clouds and Climate (BAECC) Final Campaign Summary

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petäjä, T; Moisseev, D; Sinclair, V

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the Northern latitudes throughout the United States, Canada, Russia, and Scandinavia, are, of all biomes, among the most active areas of atmospheric aerosol formation. Themore » formation of aerosol particles and their growth to cloud condensation nuclei sizes in these areas are associated with biogenic volatile organic emissions (BVOC) from vegetation and soil.« less

Effect of ethanol as a co-solvent on the aerosol performance and stability of spray-dried lysozyme.

PubMed

Ji, Shuying; Thulstrup, Peter Waaben; Mu, Huiling; Hansen, Steen Honoré; van de Weert, Marco; Rantanen, Jukka; Yang, Mingshi

2016-11-20

In the spray drying process, organic solvents can be added to facilitate drying, accommodate certain functional excipients, and modify the final particle characteristics. In this study, lysozyme was used as a model pharmaceutical protein to study the effect of ethanol as a co-solvent on the stability and aerosol performance of spray-dried protein. Lysozyme was dissolved in solutions with various ratios of ethanol and water, and subsequently spray-dried. A change from spherical particles into wrinkled and folded particles was observed upon increasing the ratio of ethanol in the feed. The aerosol performance of the spray-dried lysozyme from ethanol-water solution was improved compared to that from pure water. The conformation of lysozyme in the ethanol-water solution and spray dried powder was altered, but the native structure of lysozyme was restored upon reconstitution in water after the spray drying process. The enzymatic activities of the spray-dried lysozyme showed no significant impact of ethanol; however, the lysozyme enzymatic activity was ca. 25% lower compared to the starting material. In conclusion, the addition of ethanol as a co-solvent in the spray drying feed for lysozyme did not compromise the conformation of the protein after drying, while it improved the inhaled aerosol performance. Copyright © 2016 Elsevier B.V. All rights reserved.

A miniature Marine Aerosol Reference Tank (miniMART) as a compact breaking wave analogue

NASA Astrophysics Data System (ADS)

Stokes, M. Dale; Deane, Grant; Collins, Douglas B.; Cappa, Christopher; Bertram, Timothy; Dommer, Abigail; Schill, Steven; Forestieri, Sara; Survilo, Mathew

2016-09-01

In order to understand the processes governing the production of marine aerosols, repeatable, controlled methods for their generation are required. A new system, the miniature Marine Aerosol Reference Tank (miniMART), has been designed after the success of the original MART system, to approximate a small oceanic spilling breaker by producing an evolving bubble plume and surface foam patch. The smaller tank utilizes an intermittently plunging jet of water produced by a rotating water wheel, into an approximately 6 L reservoir to simulate bubble plume and foam formation and generate aerosols. This system produces bubble plumes characteristic of small whitecaps without the large external pump inherent in the original MART design. Without the pump it is possible to easily culture delicate planktonic and microbial communities in the bulk water during experiments while continuously producing aerosols for study. However, due to the reduced volume and smaller plunging jet, the absolute numbers of particles generated are approximately an order of magnitude less than in the original MART design.

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

NASA Astrophysics Data System (ADS)

Pfrang, C.; Shiraiwa, M.; Pöschl, U.

2011-04-01

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles representative of atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant time scales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

NASA Astrophysics Data System (ADS)

Pfrang, C.; Shiraiwa, M.; Pöschl, U.

2011-07-01

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

UV–Vis Light-induced Aging of Titan’s Haze and Ice

NASA Astrophysics Data System (ADS)

Couturier-Tamburelli, Isabelle; Piétri, Nathalie; Le Letty, Vincent; Chiavassa, Thierry; Gudipati, Murthy

2018-01-01

The study of the photochemical aging of aerosols is an important tool for understanding Titan’s stratosphere/troposphere composition and evolution, particularly the haze. Laboratory simulations of the photoreactivity of the haze aerosol analogs provide insight into the photochemical evolution of Titan’s atmosphere at and below the haze layers. Here we use experimental simulations to investigate the evolution of the laboratory analogs of these organic aerosols under ultraviolet (UV)–visible (Vis) photons, which make it through the haze layers during their sedimentation process. We present experimental results for the aging of Titan’s aerosol analogs obtained from two dominant nitrogen-containing organics, HC3N and HCN, under simulated Titan atmospheric conditions (photons and temperature). We report that volatile nitriles condensed on haze particles could be incorporated through photochemistry and provide one such sink mechanism for nitrile compounds. We provide laboratory evidence that the organic aerosols could photochemically evolve during their sedimentation through Titan’s atmosphere.

Taxon-specific aerosolization of bacteria and viruses in an experimental ocean-atmosphere mesocosm.

PubMed

Michaud, Jennifer M; Thompson, Luke R; Kaul, Drishti; Espinoza, Josh L; Richter, R Alexander; Xu, Zhenjiang Zech; Lee, Christopher; Pham, Kevin M; Beall, Charlotte M; Malfatti, Francesca; Azam, Farooq; Knight, Rob; Burkart, Michael D; Dupont, Christopher L; Prather, Kimberly A

2018-05-22

Ocean-derived, airborne microbes play important roles in Earth's climate system and human health, yet little is known about factors controlling their transfer from the ocean to the atmosphere. Here, we study microbiomes of isolated sea spray aerosol (SSA) collected in a unique ocean-atmosphere facility and demonstrate taxon-specific aerosolization of bacteria and viruses. These trends are conserved within taxonomic orders and classes, and temporal variation in aerosolization is similarly shared by related taxa. We observe enhanced transfer into SSA of Actinobacteria, certain Gammaproteobacteria, and lipid-enveloped viruses; conversely, Flavobacteriia, some Alphaproteobacteria, and Caudovirales are generally under-represented in SSA. Viruses do not transfer to SSA as efficiently as bacteria. The enrichment of mycolic acid-coated Corynebacteriales and lipid-enveloped viruses (inferred from genomic comparisons) suggests that hydrophobic properties increase transport to the sea surface and SSA. Our results identify taxa relevant to atmospheric processes and a framework to further elucidate aerosolization mechanisms influencing microbial and viral transport pathways.

Aerosol measurements in the winter/spring Antarctic stratosphere. I - Correlative measurements with ozone. II - Impact on polar stratospheric cloud theories

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.; Harder, J. W.

1988-01-01

Aerosol measurements collected from August 25-November 3, 1986 at McMurdo Station using balloon-borne optical particle counters are examined in order to study the relationship between aerosol and ozone distribution and the formation of polar stratospheric clouds (PSCs). Ozone, aerosol, and condensation nuclei profiles, and pressure, temperature, and humidity measurements are analyzed. It is observed that the height of the stratospheric sulfate layer decreases over the period of measurement suggesting that upwelling in the votex is not important in the zone depletion process. Three theories on PSC formation are described, and the effects of the aerosol measurements on the theories are considered. The three theories are: (1) the original theory of water vapor pressure over a solution of H2SO4 of Steele et al. (1983) and Hamill and Mc Master (1984); (2) the nitric acid theory of PSCs of Toon et al. (1986) and Hamill et al. (1986); and (3) the quasi-cirrus cloud theory of Heymsfield (1986).

Model analysis of secondary organic aerosol formation by glyoxal in laboratory studies: the case for photoenhanced chemistry.

PubMed

Sumner, Andrew J; Woo, Joseph L; McNeill, V Faye

2014-10-21

The reactive uptake of glyoxal by atmospheric aerosols is believed to be a significant source of secondary organic aerosol (SOA). Several recent laboratory studies have been performed with the goal of characterizing this process, but questions remain regarding the effects of photochemistry on SOA growth. We applied GAMMA (McNeill et al. Environ. Sci. Technol. 2012, 46, 8075-8081), a photochemical box model with coupled gas-phase and detailed aqueous aerosol-phase chemistry, to simulate aerosol chamber studies of SOA formation by the uptake of glyoxal by wet aerosol under dark and irradiated conditions (Kroll et al. J. Geophys. Res. 2005, 110 (D23), 1-10; Volkamer et al. Atmos. Chem. Phys. 2009, 9, 1907-1928; Galloway et al. Atmos. Chem. Phys. 2009, 9, 3331- 306 3345 and Geophys. Res. Lett. 2011, 38, L17811). We find close agreement between simulated SOA growth and the results of experiments conducted under dark conditions using values of the effective Henry's Law constant of 1.3-5.5 × 10(7) M atm(-1). While irradiated conditions led to the production of some organic acids, organosulfates, and other oxidation products via well-established photochemical mechanisms, these additional product species contribute negligible aerosol mass compared to the dark uptake of glyoxal. Simulated results for irradiated experiments therefore fell short of the reported SOA mass yield by up to 92%. This suggests a significant light-dependent SOA formation mechanism that is not currently accounted for by known bulk photochemistry, consistent with recent laboratory observations of SOA production via photosensitizer chemistry.

Aerosol Indirect Effects on Cirrus Clouds in Global Aerosol-Climate Models

NASA Astrophysics Data System (ADS)

Liu, X.; Zhang, K.; Wang, Y.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Zhou, C.; Penner, J.; Barahona, D.; Shi, X.

2015-12-01

Cirrus clouds play an important role in regulating the Earth's radiative budget and water vapor distribution in the upper troposphere. Aerosols can act as solution droplets or ice nuclei that promote ice nucleation in cirrus clouds. Anthropogenic emissions from fossil fuel and biomass burning activities have substantially perturbed and enhanced concentrations of aerosol particles in the atmosphere. Global aerosol-climate models (GCMs) have now been used to quantify the radiative forcing and effects of aerosols on cirrus clouds (IPCC AR5). However, the estimate uncertainty is very large due to the different representation of ice cloud formation and evolution processes in GCMs. In addition, large discrepancies have been found between model simulations in terms of the spatial distribution of ice-nucleating aerosols, relative humidity, and temperature fluctuations, which contribute to different estimates of the aerosol indirect effect through cirrus clouds. In this presentation, four GCMs with the start-of-the art representations of cloud microphysics and aerosol-cloud interactions are used to estimate the aerosol indirect effects on cirrus clouds and to identify the causes of the discrepancies. The estimated global and annual mean anthropogenic aerosol indirect effect through cirrus clouds ranges from 0.1 W m-2 to 0.3 W m-2 in terms of the top-of-the-atmosphere (TOA) net radiation flux, and 0.5-0.6 W m-2 for the TOA longwave flux. Despite the good agreement on global mean, large discrepancies are found at the regional scale. The physics behind the aerosol indirect effect is dramatically different. Our analysis suggests that burden of ice-nucleating aerosols in the upper troposphere, ice nucleation frequency, and relative role of ice formation processes (i.e., homogeneous versus heterogeneous nucleation) play key roles in determining the characteristics of the simulated aerosol indirect effects. In addition to the indirect effect estimate, we also use field campaign measurements and satellite retrievals to evaluate the simulated micro- and macro- physical properties of ice clouds in the four GCMs.

Summer and winter time heterogeneity in aerosol single scattering albedo over the northwestern Atlantic Ocean during the TCAP field campaign: Relationship to chemical composition and mixing state

NASA Astrophysics Data System (ADS)

Berg, L. K.; Chand, D.; Fast, J. D.; Zelenyuk, A.; Wilson, J. M.; Sedlacek, A. J., III; Tomlinson, J. M.; Hubbe, J. M.; Comstock, J. M.; Mei, F.; Kassianov, E.; Schmid, B.

2015-12-01

Aerosol play crucial role in earth's radiative budget by scattering and absorbing solar radiation. The impact of aerosol on radiation budget depend on several factors including single scattering albedo (SSA), composition, and the growth processes, like coating or mixing. We describe findings relevant to optical properties of aerosol characterized over the Cape Cod and nearby northwest Atlantic Ocean during the Two Column Aerosol Project (TCAP) during the summer (July 2012) and winter (February 2013) campaigns. The average single scattering albedo (SSA) shows distinctly different vertical profiles during the summer and winter periods. During the summer study period, the average SSA is greater than 0.95 near surface, it increases to 0.97 until an altitude of 2.5 km, and then decreases to 0.94 at top of the column near 4 km. In contrast, during the winter study period the average SSA is less than 0.93 and decreases with height reaching an average value of 0.87 near the top of the column. The large difference in summer and winter time SSA is linked to the presence of biomass burning (BB) aerosol rather than black carbon or soot in both seasons. In our study, the BB on average is factor of two higher in free troposphere (FT) during summer and more than a factor of two higher in the boundary layer during winter. Single particle analysis indicates that the average profiles of refractory black carbon (rBC) mass are similar in both seasons. The average rBC size are similar at all altitudes sampled (0-4 km) in summer time but different during winter time. In addition, the particles sampled in the summertime FT appear to be more aged than those seen during winter. The observed large heterogeneity in SSA and its links to the particle coating and composition highlights the importance of aging and mixing processes of aerosol in this region and represents a challenge for both regional and global scale models.

Wavelet and adaptive methods for time dependent problems and applications in aerosol dynamics

NASA Astrophysics Data System (ADS)

Guo, Qiang

Time dependent partial differential equations (PDEs) are widely used as mathematical models of environmental problems. Aerosols are now clearly identified as an important factor in many environmental aspects of climate and radiative forcing processes, as well as in the health effects of air quality. The mathematical models for the aerosol dynamics with respect to size distribution are nonlinear partial differential and integral equations, which describe processes of condensation, coagulation and deposition. Simulating the general aerosol dynamic equations on time, particle size and space exhibits serious difficulties because the size dimension ranges from a few nanometer to several micrometer while the spatial dimension is usually described with kilometers. Therefore, it is an important and challenging task to develop efficient techniques for solving time dependent dynamic equations. In this thesis, we develop and analyze efficient wavelet and adaptive methods for the time dependent dynamic equations on particle size and further apply them to the spatial aerosol dynamic systems. Wavelet Galerkin method is proposed to solve the aerosol dynamic equations on time and particle size due to the fact that aerosol distribution changes strongly along size direction and the wavelet technique can solve it very efficiently. Daubechies' wavelets are considered in the study due to the fact that they possess useful properties like orthogonality, compact support, exact representation of polynomials to a certain degree. Another problem encountered in the solution of the aerosol dynamic equations results from the hyperbolic form due to the condensation growth term. We propose a new characteristic-based fully adaptive multiresolution numerical scheme for solving the aerosol dynamic equation, which combines the attractive advantages of adaptive multiresolution technique and the characteristics method. On the aspect of theoretical analysis, the global existence and uniqueness of solutions of continuous time wavelet numerical methods for the nonlinear aerosol dynamics are proved by using Schauder's fixed point theorem and the variational technique. Optimal error estimates are derived for both continuous and discrete time wavelet Galerkin schemes. We further derive reliable and efficient a posteriori error estimate which is based on stable multiresolution wavelet bases and an adaptive space-time algorithm for efficient solution of linear parabolic differential equations. The adaptive space refinement strategies based on the locality of corresponding multiresolution processes are proved to converge. At last, we develop efficient numerical methods by combining the wavelet methods proposed in previous parts and the splitting technique to solve the spatial aerosol dynamic equations. Wavelet methods along the particle size direction and the upstream finite difference method along the spatial direction are alternately used in each time interval. Numerical experiments are taken to show the effectiveness of our developed methods.

The validation of the Yonsei CArbon Retrieval algorithm with improved aerosol information using GOSAT measurements

NASA Astrophysics Data System (ADS)

Jung, Yeonjin; Kim, Jhoon; Kim, Woogyung; Boesch, Hartmut; Goo, Tae-Young; Cho, Chunho

2017-04-01

Although several CO2 retrieval algorithms have been developed to improve our understanding about carbon cycle, limitations in spatial coverage and uncertainties due to aerosols and thin cirrus clouds are still remained as a problem for monitoring CO2 concentration globally. Based on an optimal estimation method, the Yonsei CArbon Retrieval (YCAR) algorithm was developed to retrieve the column-averaged dry-air mole fraction of carbon dioxide (XCO2) using the Greenhouse Gases Observing SATellite (GOSAT) measurements with optimized a priori CO2 profiles and aerosol models over East Asia. In previous studies, the aerosol optical properties (AOP) are the most important factors in CO2 retrievals since AOPs are assumed as fixed parameters during retrieval process, resulting in significant XCO2 retrieval error up to 2.5 ppm. In this study, to reduce these errors caused by inaccurate aerosol optical information, the YCAR algorithm improved with taking into account aerosol optical properties as well as aerosol vertical distribution simultaneously. The CO2 retrievals with two difference aerosol approaches have been analyzed using the GOSAT spectra and have been evaluated throughout the comparison with collocated ground-based observations at several Total Carbon Column Observing Network (TCCON) sites. The improved YCAR algorithm has biases of 0.59±0.48 ppm and 2.16±0.87 ppm at Saga and Tsukuba sites, respectively, with smaller biases and higher correlation coefficients compared to the GOSAT operational algorithm. In addition, the XCO2 retrievals will be validated at other TCCON sites and error analysis will be evaluated. These results reveal that considering better aerosol information can improve the accuracy of CO2 retrieval algorithm and provide more useful XCO2 information with reduced uncertainties. This study would be expected to provide useful information in estimating carbon sources and sinks.

Aerosol and Cloud Microphysical Properties in the Asir region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Axisa, Duncan; Kucera, Paul; Burger, Roelof; Li, Runjun; Collins, Don; Freney, Evelyn; Posada, Rafael; Buseck, Peter

2010-05-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region of Saudi Arabia as part of a Precipitation Enhancement Feasibility Study. Ground measurements of aerosol size distributions, hygroscopic growth factor, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were done in the Asir region of Saudi Arabia in August 2009. Research aircraft operations focused primarily on conducting measurements in clouds that are targeted for cloud top-seeding, on their microphysical characterization, especially the preconditions necessary for precipitation; understanding the evolution of droplet coalescence, supercooled liquid water, cloud ice and precipitation hydrometeors is necessary if advances are to be made in the study of cloud modification by cloud seeding. Non-precipitating mixed-phase clouds less than 3km in diameter that developed on top of the stable inversion were characterized by flying at the convective cloud top just above the inversion. Aerosol measurements were also done during the climb to cloud base height. The presentation will include a summary of the analysis and results with a focus on the unique features of the Asir region in producing convective clouds, characterization of the aerosol prior to convective development and the microphysical properties of convective clouds in the Asir region of Saudi Arabia.

Impact of Transpacific Aerosol on Air Quality over the United States: A Perspective from Aerosol-Cloud-Radiation Interactions

NASA Technical Reports Server (NTRS)

Tao, Zhining; Yu, Hongbin; Chin, Mian

2015-01-01

Observations have well established that aerosols from various sources in Asia, Europe, and Africa can travel across the Pacific and reach the contiguous United States (U.S.) at least on episodic bases throughout a year, with a maximum import in spring. The imported aerosol not only can serve as an additional source to regional air pollution (e.g., direct input), but also can influence regional air quality through the aerosol-cloud-radiation (ACR) interactions that change local and regional meteorology. This study assessed impacts of the transpacific aerosol on air quality, focusing on surface ozone and PM2.5, over the U.S. using the NASA Unified Weather Research Forecast model. Based on the results of 3- month (April to June of 2010) simulations, the impact of direct input (as an additional source) of transpacific aerosol caused an increase of surface PM2.5 concentration by approximately 1.5 micro-g/cu m over the west coast and about 0.5 micro-g/cu m over the east coast of the U.S. By influencing key meteorological processes through the ACR interactions, the transpacific aerosol exerted a significant effect on both surface PM2.5 (+/-6 micro-g/cu m3) and ozone (+/-12 ppbv) over the central and eastern U.S. This suggests that the transpacific transport of aerosol could either improve or deteriorate local air quality and complicate local effort toward the compliance with the U.S. National Ambient Air Quality Standards.

A one-dimensional sectional aerosol model integrated with mesoscale meteorological data to study marine boundary layer aerosol dynamics

NASA Astrophysics Data System (ADS)

Caffrey, Peter F.; Hoppel, William A.; Shi, Jainn J.

2006-12-01

The dynamics of aerosols in the marine boundary layer are simulated with a one-dimensional, multicomponent, sectional aerosol model using vertical profiles of turbulence, relative humidity, temperature, vertical velocity, cloud cover, and precipitation provided by 3-D mesoscale meteorological model output. The Naval Research Laboratory's (NRL) sectional aerosol model MARBLES (Fitzgerald et al., 1998a) was adapted to use hourly meteorological input taken from NRL's Coupled Ocean-Atmosphere Prediction System (COAMPS). COAMPS-generated turbulent mixing coefficients and large-scale vertical velocities determine vertical exchange within the marine boundary layer and exchange with the free troposphere. Air mass back trajectories were used to define the air column history along which the meteorology was retrieved for use with the aerosol model. Details on the integration of these models are described here, as well as a description of improvements made to the aerosol model, including transport by large-scale vertical motions (such as subsidence and lifting), a revised sea-salt aerosol source function, and separate tracking of sulfate mass from each of the five sources (free tropospheric, nucleated, condensed from gas phase oxidation products, cloud-processed, and produced from heterogeneous oxidation of S(IV) on sea-salt aerosol). Results from modeling air masses arriving at Oahu, Hawaii, are presented, and the relative contribution of free-tropospheric sulfate particles versus sea-salt aerosol from the surface to CCN concentrations is discussed. Limitations and benefits of the method are presented, as are sensitivity analyses of the effect of large-scale vertical motions versus turbulent mixing.

Vacuum FTIR study on the hygroscopicity of magnesium acetate aerosols

NASA Astrophysics Data System (ADS)

Wang, Na; Cai, Chen; He, Xiang; Pang, Shu-Feng; Zhang, Yun-Hong

2018-03-01

Hygroscopicity and volatility of secondary organic aerosol (SOA) are two important properties, which determine the composition, concentration, size, phase state of SOA and thus chemical and optical properties for SOA. In this work, magnesium acetate (Mg(Ac)2) aerosol was used as a simple SOA model in order to reveal relationship between hygroscopicity and volatility. A novel approach was set up based on a combination of a vacuum FTIR spectrometer and a home-made relative humidity (RH) controlling system. The striking advantage of this approach was that the RH and the compositions of aerosols could be obtained from a same IR spectrum, which guaranteed the synchronism between RH and spectral features on a sub-second scale. At the constant RH of 90% and 80% for 3000 s, the water content within Mg(Ac)2 aerosol particles decreased about 19.0% and 9.4% while there were 13.4% and 6.0% of acetate loss. This was attributed to a cooperation between volatile of acetic acid and Mg2 + hydrolysis in Mg(Ac)2 aerosols, which greatly suppressed the hygroscopicity of Mg(Ac)2 aerosols. When the RH changed with pulsed mode between 70% and 90%, hygroscopicity relaxation was observed for Mg(Ac)2 aerosols. Diffuse coefficient of water in the relaxation process was estimated to be 5 × 10- 12 m2·s- 1 for the Mg(Ac)2 aerosols. Combining the IR spectra analysis, the decrease in the diffuse coefficient of water was due to the formation of magnesium hydroxide accompanying acetic acid evaporation in the aerosols.

Broadband Measurement of Aerosol Extinction in the Visible Range

NASA Astrophysics Data System (ADS)

He, Quanfu; Bluvshtein, Nir; Segev, Lior; Flores, Michel; Rudich, Yinon; Washenfelder, Rebecca; Brown, Steven

2017-04-01

Atmospheric aerosols influence the Earth's radiative budget directly by scattering and absorbing incoming solar radiation. Aerosol direct forcing remains one of the largest uncertainties in quantifying the role that aerosols play in the Earth's radiative budget. The optical properties of aerosols vary as a function of wavelength, but few measurements reported the wavelength dependence of aerosol extinction cross section and complex refractive indices, particularly in the blue and visible spectral range. There is also currently a large gap in our knowledge of how the optical properties evolve as a function of atmospheric aging in the visible spectrum. In this study, we constructed a new and novel laboratory instrument to measure aerosol extinction as a function of wavelength, using cavity enhanced spectroscopy with a white light source. This broadband cavity enhanced spectroscopy (BBCES) covers the 395-700 nm spectral region using a broadband light source and a grating spectrometer with charge-coupled device detector (CCD). We evaluated this BBCES by measuring extinction cross section for aerosols that are pure scattering, slightly absorbing and strongly absorbing atomized from standard materials. We also retrieved the refractive indices from the measured extinction cross sections. Secondary organic aerosols from biogenic and anthropogenic precursors were "aged" to differential time scales (1 to 10 days) in an Oxidation Flow Reactor (OFR) under the combined influence of OH, O3 and UV light. The new BBCES was used to online measure the extinction cross sections of the SOA. This talk will provide a comprehensive understanding of aerosol optical properties alerting during aging process in the 395 - 700 nm spectrum.

Occurrence of pristine aerosol environments on a polluted planet

PubMed Central

Hamilton, Douglas S.; Lee, Lindsay A.; Pringle, Kirsty J.; Reddington, Carly L.; Spracklen, Dominick V.; Carslaw, Kenneth S.

2014-01-01

Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol−cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present-day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions—the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty. PMID:25512511

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

NASA Astrophysics Data System (ADS)

Lee, Hsiang-He; Chen, Shu-Hua; Kleeman, Michael J.; Zhang, Hongliang; DeNero, Steven P.; Joe, David K.

2016-07-01

The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN) at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

Formation of Oxidized Organic Aerosol (OOA) through Fog Processing in the Po Valley

NASA Astrophysics Data System (ADS)

Gilardoni, S.; Paglione, M.; Rinaldi, M.; Giulianelli, L.; Massoli, P.; Hillamo, R. E.; Carbone, S.; Lanconelli, C.; Laaksonen, A. J.; Russell, L. M.; Poluzzi, V.; Fuzzi, S.; Facchini, C.

2014-12-01

Aqueous phase chemistry might be responsible for the formation of a significant fraction of the organic aerosol (OA) observed in the atmosphere, and could explain some of the discrepancies between OA concentration and properties predicted by models and observed in the environment. Aerosol - fog interaction and its effect on submicron aerosol properties were investigated in the Po Valley (northern Italy) during fall 2011, in the framework of the Supersite project (ARPA Emilia Romagna). Composition and physical properties of submicron aerosol were measured online by a High Resolution- Time of Flight - Aerosol Mass Spectrometer (HR-TOF-AMS), a Soot Photometer - Aerosol Mass Spectrometer (SP-AMS), and a Tandem Differential Mobility Particle Sizer (TDMPS). Organic functional group analysis was performed off-line by Hydrogen - Nuclear Magnetic Resonance (H-NMR) spectrometry and by Fourier Transform Infrared (FTIR) spectrometry. Aerosol absorption, scattering, and total extinction were measured simultaneously with a Particle Soot Absorption Photometer (PSAP), a Nephelometer, and a Cavity Attenuated Phase Shift Spectrometer particle extinction monitor (CAPS PMex), respectively. Water-soluble organic carbon in fog-water was characterized off-line by HR-TOF-AMS. Fourteen distinct fog events were observed. Fog dissipation left behind an aerosol enriched in particles larger than 400 nm, typical of fog and cloud processing, and dominated by secondary species, including ammonium nitrate, ammonium sulfate and oxidized OA (OOA). Source apportionment of OA allowed us to identify OOA as the difference between total OA and primary OA (hydrocarbon like OA and biomass burning OA). The formation of OOA through fog processing is proved by the correlation of OOA concentration with hydroxyl methyl sulfonate signal and by the similarity of OOA spectra with organic mass spectra obtained by re-aerosolization of fog water samples. The oxygen to carbon ratio and the hydrogen to carbon ratio of this OOA fraction was about 0.6 and 1.3, respectively. Organic functional group analysis showed that OOA observed after fog dissipation was characterized by organic-sulfur and organic-nitrogen species.

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

2005-01-01

Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds, Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

Chemistry and Composition of Atmospheric Aerosol Particles

NASA Astrophysics Data System (ADS)

Kolb, Charles E.; Worsnop, Douglas R.

2012-05-01

For more than two decades a cadre of physical chemists has focused on understanding the formation processes, chemical composition, and chemical kinetics of atmospheric aerosol particles and droplets with diameters ranging from a few nanometers to ˜10,000 nm. They have adapted or invented a range of fundamental experimental and theoretical tools to investigate the thermochemistry, mass transport, and chemical kinetics of processes occurring at nanoscale gas-liquid and gas-solid interfaces for a wide range of nonideal, real-world substances. State-of-the-art laboratory methods devised to study molecular spectroscopy, chemical kinetics, and molecular dynamics also have been incorporated into field measurement instruments that are deployed routinely on research aircraft, ships, and mobile laboratories as well as at field sites from megacities to the most remote jungle, desert, and polar locations. These instruments can now provide real-time, size-resolved aerosol particle physical property and chemical composition data anywhere in Earth's troposphere and lower stratosphere.

Extending MODIS Deep Blue Aerosol Retrieval Coverage to Cases of Absorbing Aerosols Above Clouds: First Results

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Hsu, N. C.; Bettenhausen, C.; Lee, J.; Redemann, J.; Shinozuka, Y.; Schmid, B.

2015-01-01

Absorbing smoke or mineral dust aerosols above clouds (AAC) are a frequent occurrence in certain regions and seasons. Operational aerosol retrievals from sensors like MODIS omit AAC because they are designed to work only over cloud-free scenes. However, AAC can in principle be quantified by these sensors in some situations (e.g. Jethva et al., 2013; Meyer et al., 2013). We present a summary of some analyses of the potential of MODIS-like instruments for this purpose, along with two case studies using airborne observations from the Ames Airborne Tracking Sunphotometer (AATS; http://geo.arc.nasa.gov/sgg/AATS-website/) as a validation data source for a preliminary AAC algorithm applied to MODIS measurements. AAC retrievals will eventually be added to the MODIS Deep Blue (Hsu et al., 2013) processing chain.

Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

NASA Astrophysics Data System (ADS)

Phillips, B.; Dawson, K. W.; Royalty, T. M.; Reed, R. E.; Petters, M.; Meskhidze, N.

2015-12-01

Atmospheric aerosols play a central role in many environmental processes by influencing the Earth's radiative balance, tropospheric chemistry, clouds, biogeochemical cycles, and visibility as well as adversely impacting human health. Based on their origin, atmospheric aerosols can be defined as anthropogenic or natural. Recent studies have shown that a large fraction of uncertainty in the radiative effects of anthropogenic aerosols is related to uncertainty in natural—background—aerosols. Marine aerosols are of particular interest due to the abundance of oceans covering the Earth's surface. Despite their importance, limited information is currently available for size- and composition-resolved marine aerosol emission fluxes. Our group has designed and built an instrument for measuring the size- and hygroscopicity-resolved sea spray aerosol fluxes. The instrument was first deployed during spring 2015 at the end of the 560 m pier of the US Army Corps of Engineers' Field Research Facility in Duck, NC. Measurements include 200 nm-sized diameter growth factor (hygroscopicity) distributions, sea spray particle flux measurements, and total sub-micron sized aerosol concentration. Ancillary ocean data includes salinity, pH, sea surface temperature, dissolved oxygen content, and relative fluorescence (proxy for [Chl-a]). Hygroscopicity distribution measurements show two broad peaks, one indicative of organics and sulfates and another suggestive of sea salt. The fraction of 200 nm-sized salt particles having hygroscopicity similar to that of sea-spray aerosol contributes up to ~24% of the distribution on days with high-speed onshore winds and up to ~3% on calm days with winds blowing from the continent. However, the total concentration of sea-spray-like particles originating from offshore versus onshore winds was relatively similar. Changes in the relative contribution of sea-salt to number concentration were caused by a concomitant changes in total aerosol concentration, indicating a local source.

Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

PubMed

Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

2014-04-01

The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions. © 2013 SETAC.

Profiling Transboundary Aerosols over Taiwan and Assessing Their Radiative Effects

NASA Technical Reports Server (NTRS)

Wang, Sheng-Hsiang; Lin, Neng-Huei; Chou, Ming-Dah; Tsay, Si-Chee; Welton, Ellsworth J.; Hsu, N. Christina; Giles, David M.; Liu, Gin-Rong; Holben, Brent N.

2010-01-01

A synergistic process was developed to study the vertical distributions of aerosol optical properties and their effects on solar heating using data retrieved from ground-based radiation measurements and radiative transfer simulations. Continuous MPLNET and AERONET observations were made at a rural site in northern Taiwan from 2005 to 2007. The aerosol vertical extinction profiles retrieved from ground-based lidar measurements were categorized into near-surface, mixed, and two-layer transport types, representing 76% of all cases. Fine-mode (Angstrom exponent, alpha, approx.1.4) and moderate-absorbing aerosols (columnar single-scattering albedo approx.0.93, asymmetry factor approx.0.73 at 440 nm wavelength) dominated in this region. The column-integrated aerosol optical thickness at 500 nm (tau(sub 500nm)) ranges from 0.1 to 0.6 for the near-surface transport type, but can be doubled in the presence of upper-layer aerosol transport. We utilize aerosol radiative efficiency (ARE; the impact on solar radiation per unit change of tau(sub 500nm)) to quantify the radiative effects due to different vertical distributions of aerosols. Our results show that the ARE at the top-of-atmosphere (-23 W/ sq m) is weakly sensitive to aerosol vertical distributions confined in the lower troposphere. On the other hand, values of the ARE at the surface are -44.3, -40.6 and -39.7 W/sq m 38 for near-surface, mixed, and two-layer transport types, respectively. Further analyses show that the impact of aerosols on the vertical profile of solar heating is larger for the near-surface transport type than that of two-layer transport type. The impacts of aerosol on the surface radiation and the solar heating profiles have implications for the stability and convection in the lower troposphere.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Longo, Amelia F.; Feng, Yan; Lai, Barry

Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation statemore » became more reduced, and aerosol acidity increased. As a result, atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.« less

Algorithms for radiative transfer simulations for aerosol retrieval

NASA Astrophysics Data System (ADS)

Mukai, Sonoyo; Sano, Itaru; Nakata, Makiko

2012-11-01

Aerosol retrieval work from satellite data, i.e. aerosol remote sensing, is divided into three parts as: satellite data analysis, aerosol modeling and multiple light scattering calculation in the atmosphere model which is called radiative transfer simulation. The aerosol model is compiled from the accumulated measurements during more than ten years provided with the world wide aerosol monitoring network (AERONET). The radiative transfer simulations take Rayleigh scattering by molecules and Mie scattering by aerosols in the atmosphere, and reflection by the Earth surface into account. Thus the aerosol properties are estimated by comparing satellite measurements with the numerical values of radiation simulations in the Earth-atmosphere-surface model. It is reasonable to consider that the precise simulation of multiple light-scattering processes is necessary, and needs a long computational time especially in an optically thick atmosphere model. Therefore efficient algorithms for radiative transfer problems are indispensable to retrieve aerosols from space.

CATS Aerosol Typing and Future Directions

NASA Technical Reports Server (NTRS)

McGill, Matt; Yorks, John; Scott, Stan; Palm, Stephen; Hlavka, Dennis; Hart, William; Nowottnick, Ed; Selmer, Patrick; Kupchock, Andrew; Midzak, Natalie;

Development of a Sampler for Total Aerosol Deposition in the Human Respiratory Tract

PubMed Central

Koehler, Kirsten A.; Clark, Phillip; Volckens, John

2009-01-01

Studies that seek to associate reduced human health with exposure to occupational and environmental aerosols are often hampered by limitations in the exposure assessment process. One limitation involves the measured exposure metric itself. Current methods for personal exposure assessment are designed to estimate the aspiration of aerosol into the human body. Since a large proportion of inhaled aerosol is subsequently exhaled, a portion of the aspirated aerosol will not contribute to the dose. This leads to variable exposure misclassification (for heterogenous exposures) and increased uncertainty in health effect associations. Alternatively, a metric for respiratory deposition would provide a more physiologically relevant estimate of risk. To address this challenge, we have developed a method to estimate the deposition of aerosol in the human respiratory tract using a sampler engineered from polyurethane foam. Using a semi-empirical model based on inertial, gravitational, and diffusional particle deposition, a foam was engineered to mimic aerosol total deposition in the human respiratory tract. The sampler is comprised of commercially available foam with fiber diameter = 49.5 μm (equivalent to industry standard 100 PPI foam) of 8 cm thickness operating at a face velocity of 1.3 m s−1. Additionally, the foam sampler yields a relatively low-pressure drop, independent of aerosol loading, providing uniform particle collection efficiency over time. PMID:19638392

Retrieve Aerosol Concentration Based On Surface Model and Distribution of Concentration of PM2.5 ——A Case Study of Beijing

NASA Astrophysics Data System (ADS)

Cui, H.

2017-12-01

As China's economy continues to grow, urbanization continues to advance, along with growth in all areas to pollutant emissions in the air industry, air quality also continued to deteriorate. Aerosol concentrations as a measure of air quality of the most important part of are more and more people's attention. Traditional monitoring stations measuring aerosol concentration method is accurate, but time-consuming and can't be done simultaneously measure a large area, can only rely on data from several monitoring sites to predict the concentration of the panorama. Remote Sensing Technology retrieves aerosol concentrations being by virtue of their efficient, fast advantages gradually into sight. In this paper, by the method of surface model to start with the physical processes of atmospheric transport, innovative aerosol concentration coefficient proposed to replace the traditional aerosol concentrations, pushed to a set of retrieval of aerosol concentration coefficient method, enabling fast and efficient Get accurate air pollution target area. At the same paper also monitoring data for PM2.5 in Beijing were analyzed from different angles, from the perspective of the data summarized in Beijing PM2.5 concentration of time, space, geographical distribution and concentration of PM2.5 and explored the relationship between aerosol concentration coefficient and concentration of PM2.5.

An Overview of Regional Experiments on Biomass Burning Aerosols and Related Pollutants in Southeast Asia: From BASE-ASIA and the Dongsha Experiment to 7-SEAS

NASA Technical Reports Server (NTRS)

Lin, Neng-Huei; Tsay, Si-Chee; Maring, Hal B.; Yen, Ming-Cheng; Sheu, Guey-Rong; Wang, Sheng-Hsiang; Chi, Kai Hsien; Chuang, Ming-Tung; Ou-Yang, Chang-Feng; Fu, Joshua S.;

Aerosol Production and Growth in the Upper Troposphere over the Amazon Forest Observed during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Machado, L.; Mertes, S.; Pöhlker, C.; Pöhlker, M. L.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Wang, J.; Weinzierl, B.; Wendisch, M.

2016-12-01

Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with aerosol number concentrations after normalization to STP often exceeding those in the boundary layer (BL) by one or two orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO. The campaign took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were consistently observed on all flights, using several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were depleted in aerosol particles, whereas dramatically enhanced small (<90 nm diameter) aerosol number concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. We also found elevated concentrations of larger (>90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest that aerosol production takes place in the UT from volatile material brought up by deep convection, which is converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new particle formation has not been observed. We propose that this may have been the dominant process supplying secondary aerosols in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

Clear-sky remote sensing in the vicinity of clouds: what we learned from MODIS and CALIPSO

NASA Astrophysics Data System (ADS)

Marshak, Alexander; Varnai, Tamas; Wen, Guoyong; Cahalan, Robert

Studies on aerosol direct and indirect effects require a precise separation of cloud-free and cloudy air. However, separation between cloud-free and cloudy areas from remotely-sensed measurements is ambiguous. The transition zone in the regions around clouds often stretches out tens of km, which are neither precisely clear nor precisely cloudy. We study the transition zone between cloud-free and cloudy air using MODerate-resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) measurements. Both instruments show enhanced clear-sky reflectance (MODIS) and clear-sky backscatterer (CALIPSO) near clouds. Analyzing a large dataset of MODIS observations we examine the effect of three-dimensional (3D) radiative interactions between clouds and cloud-free areas, also known as a cloud adjacency effect. Comparing with CALIPSO clear-sky backscatterer measurements, we show that the cloud adjacency effect may be responsible for a large portion of the enhanced clear sky reflectance observed by MODIS. While aerosol particles are responsible for a large part of the near-cloud enhancements in CALIPSO observations, misidentified or undetected cloud particles are also likely to contribute. As a result, both the nature of these particles (cloud vs. aerosol) and the processes creating them need to be clarified using a quantitative assessment of remote sensing limitations in particle detection and identification. The width and ubiquity of the transition zone near clouds imply that studies of aerosol-cloud interactions and aerosol direct radiative effects need to account for aerosol changes near clouds. Not accounted, these changes can cause systematic biases toward smaller aerosol radiative forcing. On the other hand, including aerosol products near clouds despite their uncertainties may overestimate aerosol radiative forcing. Therefore, there is an urgent need for developing methods that can assess and account for remote sensing challenges and thus allow for including the transition zone into the study. We describe a simple model that estimates the cloud-induced enhanced reflectances of cloud-free areas in the vicinity of clouds. The model assumes that the enhancement is due entirely to Rayleigh scattering and is therefore bigger at shorter wavelengths, thus creating a so-called apparent "bluing" of aerosols in remote sensing retrievals.