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.

A Global, Decadal, Quantitative Record of Absorbing Aerosols above Cloud Using OMI's Near-UV Observations

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2016-12-01

Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes of the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regions of the world. Contrary to the known cooling effects of these aerosols in cloud-free scenario over dark surface, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing (warming) at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud directly depends on the aerosol loading, microphysical and optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of above-cloud aerosol optical depth (ACAOD) of absorbing aerosols retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. Physically based on the strong `color ratio' effect in the near-UV caused by the spectral absorption of aerosols above cloud, the algorithm, formally named as OMACA, retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. Here, we present the algorithm architecture and results from an 11-year global record (2005-2015) including global climatology of frequency of occurrence and ACAOD. The theoretical uncertainty analysis and planned validation activities using measurements from upcoming field campaigns are also discussed.

Sensitivity of multiangle photo-polarimetry to absorbing aerosol vertical layering and properties: Quantifying measurement uncertainties for ACE requirements

NASA Astrophysics Data System (ADS)

Kalashnikova, O. V.; Garay, M. J.; Davis, A. B.; Natraj, V.; Diner, D. J.; Tanelli, S.; Martonchik, J. V.; JPl Team

2011-12-01

The impact of tropospheric aerosols on climate can vary greatly based upon relatively small variations in aerosol properties, such as composition, shape and size distributions, as well as vertical layering. Multi-angle polarimetric measurements have been advocated in recent years as an additional tool to better understand and retrieve the aerosol properties needed for improved predictions of aerosol radiative forcing on climate. The central concern of this work is the assessment of the effects of absorbing aerosol properties under measurement uncertainties achievable for future generation multi-angle, polarimetric imaging instruments under ACE mission requirements. As guidelines, the on-orbit performance of MISR for multi-angle intensity measurements and the reported polarization sensitivities of a MSPI prototype were adopted. In particular, we will focus on sensitivities to absorbing aerosol layering and observation-constrained refractive indices (resulting in various single scattering albedos (SSA)) of both spherical and non-spherical absorbing aerosol types. We conducted modeling experiments to determine how the measured Stokes vector elements are affected in UV-NIR range by the vertical distribution, mixing and layering of smoke and dust aerosols, and aerosol SSA under the assumption of a black and polarizing ocean surfaces. We use a vector successive-orders-of-scattering (SOS) and VLIDORT transfer codes that show excellent agreement. Based on our sensitivity studies we will demonstrate advantages and disadvantages of wavelength selection in UV-NIR range to access absorbing aerosol properties. Polarized UV channels do not show particular advantage for absorbing aerosol property characterization due to dominating molecular signal. Polarimetric SSA sensitivity is small, however needed to be considered in the future polarimetric retrievals under ACE-defined uncertainty.

Measurement-based estimates of direct radiative effects of absorbing aerosols above clouds

NASA Astrophysics Data System (ADS)

Feng, Nan; Christopher, Sundar A.

2015-07-01

The elevated layers of absorbing smoke aerosols from western African (e.g., Gabon and Congo) biomass burning activities have been frequently observed above low-level stratocumulus clouds off the African coast, which presents an excellent natural laboratory for studying the effects of aerosols above clouds (AAC) on regional energy balance in tropical and subtropical environments. Using spatially and temporally collocated Moderate Resolution Imaging Spectroradiometer, Ozone Monitoring Instrument (OMI), and Clouds and the Earth's Radiant Energy System data sets, the top-of-atmosphere shortwave aerosol direct shortwave radiative effects (ARE) of absorbing aerosols above low-level water clouds in the southeast Atlantic Ocean was examined in this study. The regional averaged instantaneous ARE has been estimated to be 36.7 ± 20.5 Wm-2 (regional mean ± standard deviation) along with a mean positive OMI Aerosol Index at 1.3 in August 2006 based on multisensors measurements. The highest magnitude of instantaneous ARE can even reach 138.2 Wm-2. We assess that the 660 nm cloud optical depth (COD) values of 8-12 is the critical value above (below) which aerosol absorption (scattering) effect dominates and further produces positive (negative) ARE values. The results further show that ARE values are more sensitive to aerosols above lower COD values than cases for higher COD values. This is among the first studies to provide quantitative estimates of shortwave ARE due to AAC events from an observational perspective.

Radiative effects of absorbing aerosols over northeastern India: Observations and model simulations

NASA Astrophysics Data System (ADS)

Gogoi, Mukunda M.; Babu, S. Suresh; Moorthy, K. Krishna; Bhuyan, Pradip Kumar; Pathak, Binita; Subba, Tamanna; Chutia, Lakhima; Kundu, Shyam Sundar; Bharali, Chandrakala; Borgohain, Arup; Guha, Anirban; De, Barin Kumar; Singh, Brajamani; Chin, Mian

2017-01-01

Multiyear measurements of spectral properties of aerosol absorption are examined over four geographically distinct locations of northeastern India. Results indicated significant spatiotemporal variation in aerosol absorption coefficients (σabs) with highest values in winter and lowest in monsoon. The western parts of the region, close to the outflow of Indo-Gangetic Plains, showed higher values of σabs and black carbon (BC) concentration—mostly associated with fossil fuel combustion. But, the eastern parts showed higher contributions from biomass-burning aerosols, as much as 20-25% to the total aerosol absorption, conspicuously during premonsoon season. This is attributed to a large number of burning activities over the Southeast Asian region, as depicted from Moderate Resolution Imaging Spectroradiometer fire count maps, whose spatial extent and magnitude peaks during March/April. The nearly consistent high values of aerosol index (AI) and layer height from Ozone Monitoring Instrument indicate the presence of absorbing aerosols in the upper atmosphere. The observed seasonality has been captured fairly well by Goddard Chemistry Aerosol Radiation and Transport (GOCART) as well as Weather Research and Forecasting-Chemistry (WRF-Chem) model simulations. The ratio of column-integrated optical depths due to particulate organic matter and BC from GOCART showed good coincidence with satellite-based observations, indicating the increased vertical dispersion of absorbing aerosols, probably by the additional local convection due to higher fire radiative power caused by the intense biomass-burning activities. In the WRF-Chem though underperformed by different magnitude in winter, the values are closer or overestimated near the burnt areas. Atmospheric forcing due to BC was highest ( 30 Wm-2) over the western part associated with the fossil fuel combustion.

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

Light-absorbing aerosol properties retrieved from the sunphotometer observation over the Yangtze River Delta, China.

PubMed

Wang, Jing; Niu, Shengjie; Xu, Dan

2018-02-10

In this study, aerosol optical depth (AOD) and extinction Ångström exponent (EAE) are derived from ground-based sunphotometer observations between 2007 and 2014 at urban sites of Nanjing over the Yangtze River Delta. In addition, the present study aims to investigate aerosol light-absorbing properties such as single-scattering albedo (SSA), absorption Ångström exponent (AAE), and the aerosol-absorbing optical depth (AAOD). The retrieval of aerosol properties is compared with AERONET inversion products. The results demonstrate that the retrieved AOD has a good agreement with the AERONET Level 1.5 data, with the root mean square error being 0.068, 0.065, and 0.026 for total, fine mode, and coarse mode at 440 nm, respectively. The SSA values indicate similar accuracies in the results, which are about 0.003, -0.009, -0.008, and 0.010 different from AERONET at 440, 670, 870, and 1020 nm, respectively. The occurrence frequency of background level AOD (AOD<0.10) at 440 nm in this region is limited (1%). Monthly mean AOD, SSA, the effective radius (R eff ), and the volume concentration at 440 nm were 0.6-1.3, 0.85-0.92, 0.24-0.40 μm, and 0.18-0.28  μm 3  μm -2 , respectively. The mean value of AAOD at 440 nm (AAOD 440 ) was the highest in both summer (0.095±0.041) and autumn (0.094±0.042), but was the lowest in winter (0.079±0.036). It was also noted that SSA was found to be higher during summer (0.89±0.05). The spectral variation of SSA was observed to be strongly wavelength-dependent during all seasons. The seasonal mean AAE440-870 is the highest in winter (0.86±0.41) and lowest in spring (0.49±0.29). In winter, the cumulative frequency for AAE between 1.0 and 1.2 was about 87%. The peak in the AAE distribution was close to 1.0, indicating that the aerosol column was dominated by urban-industrial aerosols and absorption species other than black carbon. Analysis of the relationship between EAE and SSA showed that the aerosol populations could be

Effects of Absorbing Aerosols on Accelerated Melting of Snowpack in the Tibetan-Himalayas Region

NASA Technical Reports Server (NTRS)

Lau, William K. M.

2011-01-01

The impacts of absorbing aerosol on melting of snowpack in the Hindu-Kush-Tibetan-Himalayas (HKTH) region are studied using NASA satellite and GEOS-5 GCM. Results from GCM experiments shows that a 8-10% in the rate of melting of snowpack over the western Himalayas and Tibetan Plateau can be attributed to the aerosol elevated-heat-pump (EHP) feedback effect (Lau et al. 2008), initiated by the absorption of solar radiation by absorbing aerosols accumulated over the Indo-Gangetic Plain and Himalayas foothills. On the other hand, deposition of black carbon on snow surface was estimated to give rise to a reduction in snow surface albedo of 2 - 5%, and an increased annual runoff of 9-24%. From case studies using satellite observations and re-analysis data, we find consistent signals of possible impacts of dust and black carbon aerosol in blackening snow surface, in accelerating spring melting of snowpack in the HKHT, and consequentially in influencing shifts in long-term Asian summer monsoon rainfall pattern.

Assessment of capabilities of multiangle imaging photo-polarimetry for atmospheric correction in presence of absorbing aerosols

NASA Astrophysics Data System (ADS)

Kalashnikova, O. V.; Garay, M. J.; Xu, F.; Seidel, F. C.; Diner, D. J.

2015-12-01

Satellite remote sensing of ocean color is a critical tool for assessing the productivity of marine ecosystems and monitoring changes resulting from climatic or environmental influences. Yet water-leaving radiance comprises less than 10% of the signal measured from space, making correction for absorption and scattering by the intervening atmosphere imperative. Traditional ocean color retrieval algorithms utilize a standard set of aerosol models and the assumption of negligible water-leaving radiance in the near-infrared. Modern improvements have been developed to handle absorbing aerosols such as urban particulates in coastal areas and transported desert dust over the open ocean, where ocean fertilization can impact biological productivity at the base of the marine food chain. Even so, imperfect knowledge of the absorbing aerosol optical properties or their height distribution results in well-documented sources of error. In the UV, the problem of UV-enhanced absorption and nonsphericity of certain aerosol types are amplified due to the increased Rayleigh and aerosol optical depth, especially at off-nadir view angles. Multi-angle spectro-polarimetric measurements have been advocated as an additional tool to better understand and retrieve the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of the work to be described is the assessment of the effects of absorbing aerosol properties on water leaving radiance measurement uncertainty by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. The phase matrices for the spherical smoke particles were calculated using a standard

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.

Formation of light absorbing organo-nitrogen species from evaporation of droplets containing glyoxal and ammonium sulfate.

PubMed

Lee, Alex K Y; Zhao, Ran; Li, Richard; Liggio, John; Li, Shao-Meng; Abbatt, Jonathan P D

2013-11-19

In the atmosphere, volatile organic compounds such as glyoxal can partition into aqueous droplets containing significant levels of inorganic salts. Upon droplet evaporation, both the organics and inorganic ions become highly concentrated, accelerating reactions between them. To demonstrate this process, we investigated the formation of organo-nitrogen and light absorbing materials in evaporating droplets containing glyoxal and different ammonium salts including (NH4)2SO4, NH4NO3, and NH4Cl. Our results demonstrate that evaporating glyoxal-(NH4)2SO4 droplets produce light absorbing species on a time scale of seconds, which is orders of magnitude faster than observed in bulk solutions. Using aerosol mass spectrometry, we show that particle-phase organics with high N:C ratios were formed when ammonium salts were used, and that the presence of sulfate ions promoted this chemistry. Since sulfate can also significantly enhance the Henry's law partitioning of glyoxal, our results highlight the atmospheric importance of such inorganic-organic interactions in aqueous phase aerosol chemistry.

Absorbing Aerosols Above Cloud: Detection, Quantitative Retrieval, and Radiative Forcing from Satellite-based Passive Sensors

NASA Astrophysics Data System (ADS)

Jethva, H.; Torres, O.; Remer, L. A.; Bhartia, P. K.

2012-12-01

Light absorbing particles such as carbonaceous aerosols generated from biomass burning activities and windblown dust particles can exert a net warming effect on climate; the strength of which depends on the absorption capacity of the particles and brightness of the underlying reflecting background. When advected over low-level bright clouds, these aerosols absorb the cloud reflected radiation from ultra-violet (UV) to shortwave-IR (SWIR) and makes cloud scene darker-a phenomenon commonly known as "cloud darkening". The apparent "darkening" effect can be seen by eyes in satellite images as well as quantitatively in the spectral reflectance measurements made by space borne sensors over regions where light absorbing carbonaceous and dust aerosols overlay low-level cloud decks. Theoretical radiative transfer simulations support the observational evidence, and further reveal that the strength of the cloud darkening and its spectral signature (or color ratio) between measurements at two wavelengths are a bi-function of aerosol and cloud optical thickness (AOT and COT); both are measures of the total amount of light extinction caused by aerosols and cloud, respectively. Here, we developed a retrieval technique, named as the "color ratio method" that uses the satellite measurements at two channels, one at shorter wavelength in the visible and one at longer wavelength in the shortwave-IR for the simultaneous retrieval of AOT and COT. The present technique requires assumptions on the aerosol single-scattering albedo and aerosol-cloud separation which are supplemented by the Aerosol Robotic Network (AERONET) and space borne CALIOP lidar measurements. The retrieval technique has been tested making use of the near-UV and visible reflectance observations made by the Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) for distinct above-cloud smoke and dust aerosol events observed seasonally over the southeast and tropical Atlantic Ocean

Spatio-temporal distribution of absorbing and non-absorbing aerosols derived from Aura-OMI Aerosol Index over Greece

NASA Astrophysics Data System (ADS)

Kaskaoutis, D. G.; Nastos, P. T.; Kosmopoulos, P. G.; Kambezidis, H. D.; Kharol, S. K.; Badarinath, K. V. S.

2009-04-01

The Aerosol Index (AI) observations derived from the Ozone Monitoring Instrument (OMI) on board the Dutch-Finnish Aura satellite are analyzed over Greece covering the whole period of the OMI available data, from September 2004 to August 2008. The objective of this study was to analyze the spatial, seasonal and inter-annual variability of AI over Greece, detected by OMI during 2004-2008, with an evaluation of potential contributing factors, including precipitation and long-range transport (Sahara dust and European pollution). The AI data cover the whole Greek territory (34o-42oN, 20o-28oE) with a spatial resolution of 0.25o x 0.25o (13 km x 24 km at nadir). The results show significant spatial and temporal variability of the seasonal and monthly mean AI, with higher values at the southern parts and lower values over northern Greece. On the other hand, the AI values do not show significant differences between the western and eastern parts and, therefore, the longitude-averaged AI values can be utilized to reveal the strong south-to-north gradient. This gradient significantly changes from season to season being more intense in spring and summer, while it is minimized in winter. Another significant remark is the dominance of negative AI values over northern Greece in the summer months, indicating the presence of non-UV absorbing aerosols, such as sulfate and sea-salt particles. The great geographical extent of the negative AI values in the summer months is indicative of long-range transport of such aerosols. In contrast, the high positive AI values over south Greece, mainly in spring, clearly reveal the UV-absorbing nature of desert-dust particles affecting the area during Saharan dust events. Synoptically, the spatial distribution in OMI-AI values was related to the Saharan dust events mainly over southern Greece and to the trans-boundary-pollution transport, consisting mainly of sulfate particles, in northern Greece. The annual variation of spatial-averaged AI values

Spatio-temporal interaction between absorbing aerosols and temperature: Correlation and causality based approach

NASA Astrophysics Data System (ADS)

Dave, P.; Bhushan, M.; Venkataraman, C.

2016-12-01

Indian subcontinent, in particular, the Indo-gangetic plain (IGP) has witnessed large temperature anomalies (Ratnam et al., 2016) along with high emission of absorbing aerosols (AA) (Gazala, et al., 2005). The anomalous high temperature observed over this region may bear a relationship with high AA emissions. Different studies have been conducted to understand AA and temperature relationships (Turco et al., 1983; Hansen et al., 1997, 2005; Seinfeld 2008; Ramanathan et al. 2010b; Ban-Weiss et al., 2012). It was found that when the AA was injected in the lower- mid troposphere the surface air temperature increases while injection of AA at higher troposphere-lower stratosphere surface temperature decreases. These studies used simulation based results to establish link between AA and temperature (Hansen et al., 1997, 2005; Ban-Weiss et al., 2012). The current work focuses on identifying the causal influence of AA on temperature using observational and re-analysis data over Indian subcontinent using cross correlation (CCs) and Granger causality (GC) (Granger, 1969). Aerosol index (AI) from TOMS-OMI was used as index for AA while ERA-interim reanalysis data was used for temperature at varying altitude. Period of study was March-April-May-June (MAMJ) for years 1979-2015. CCs were calculated for all the atmospheric layers. In each layer nearby and distant pixels (>500 kms) with high CCs were identified using clustering technique. It was found that that AI and Temperature shows statistically significant cross-correlations for co-located and distant pixels and more prominently over IGP. The CCs fades away with higher altitudes. CCs analysis was followed by GC analysis to identify the lag over which AI can influence the Temperature. GC also supported the findings of CCs analysis. It is an early attempt to link persisting large temperature anomalies with absorbing aerosols and may help in identifying the role of absorbing aerosol in causing heat waves.

A multi-satellite analysis of the direct radiative effects of absorbing aerosols above clouds

NASA Astrophysics Data System (ADS)

Chang, Y. Y.; Christopher, S. A.

2015-12-01

Radiative effects of absorbing aerosols above liquid water clouds in the southeast Atlantic as a function of fire sources are investigated using A-Train data coupled with the Visible Infrared Imaging Radiometer Suite (VIIRS) onboard Suomi National Polar-orbiting Partnership (Suomi NPP). Both the VIIRS Active Fire product and the Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) Thermal Anomalies product (MYD14) are used to identify the biomass burning fire origin in southern Africa. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) are used to assess the aerosol type, aerosol altitude, and cloud altitude. We use back trajectory information, wind data, and the Fire Locating and Modeling of Burning Emissions (FLAMBE) product to infer the transportation of aerosols from the fire source to the CALIOP swath in the southeast Atlantic during austral winter.

Role of absorbing aerosols on hot extremes in India in a GCM

NASA Astrophysics Data System (ADS)

Mondal, A.; Sah, N.; Venkataraman, C.; Patil, N.

2017-12-01

Temperature extremes and heat waves in North-Central India during the summer months of March through June are known for causing significant impact in terms of human health, productivity and mortality. While greenhouse gas-induced global warming is generally believed to intensify the magnitude and frequency of such extremes, aerosols are usually associated with an overall cooling, by virtue of their dominant radiation scattering nature, in most world regions. Recently, large-scale atmospheric conditions leading to heat wave and extreme temperature conditions have been analysed for the North-Central Indian region. However, the role of absorbing aerosols, including black carbon and dust, is still not well understood, in mediating hot extremes in the region. In this study, we use 30-year simulations from a chemistry-coupled atmosphere-only General Circulation Model (GCM), ECHAM6-HAM2, forced with evolving aerosol emissions in an interactive aerosol module, along with observed sea surface temperatures, to examine large-scale and mesoscale conditions during hot extremes in India. The model is first validated with observed gridded temperature and reanalysis data, and is found to represent observed variations in temperature in the North-Central region and concurrent large-scale atmospheric conditions during high temperature extremes realistically. During these extreme events, changes in near surface properties include a reduction in single scattering albedo and enhancement in short-wave solar heating rate, compared to climatological conditions. This is accompanied by positive anomalies of black carbon and dust aerosol optical depths. We conclude that the large-scale atmospheric conditions such as the presence of anticyclones and clear skies, conducive to heat waves and high temperature extremes, are exacerbated by absorbing aerosols in North-Central India. Future air quality regulations are expected to reduce sulfate particles and their masking of GHG warming. It is

Remote sensing of soot carbon - Part 1: Distinguishing different absorbing aerosol species

NASA Astrophysics Data System (ADS)

Schuster, G. L.; Dubovik, O.; Arola, A.

2016-02-01

We describe a method of using the Aerosol Robotic Network (AERONET) size distributions and complex refractive indices to retrieve the relative proportion of carbonaceous aerosols and free iron minerals (hematite and goethite). We assume that soot carbon has a spectrally flat refractive index and enhanced imaginary indices at the 440 nm wavelength are caused by brown carbon or hematite. Carbonaceous aerosols can be separated from dust in imaginary refractive index space because 95 % of biomass burning aerosols have imaginary indices greater than 0.0042 at the 675-1020 nm wavelengths, and 95 % of dust has imaginary refractive indices of less than 0.0042 at those wavelengths. However, mixtures of these two types of particles can not be unambiguously partitioned on the basis of optical properties alone, so we also separate these particles by size. Regional and seasonal results are consistent with expectations. Monthly climatologies of fine mode soot carbon are less than 1.0 % by volume for West Africa and the Middle East, but the southern African and South American biomass burning sites have peak values of 3.0 and 1.7 %. Monthly averaged fine mode brown carbon volume fractions have a peak value of 5.8 % for West Africa, 2.1 % for the Middle East, 3.7 % for southern Africa, and 5.7 % for South America. Monthly climatologies of free iron volume fractions show little seasonal variability, and range from about 1.1 to 1.7 % for coarse mode aerosols in all four study regions. Finally, our sensitivity study indicates that the soot carbon retrieval is not sensitive to the component refractive indices or densities assumed for carbonaceous and free iron aerosols, and the retrieval differs by only 15.4 % when these parameters are altered from our chosen baseline values. The total uncertainty of retrieving soot carbon mass is ˜ 50 % (when uncertainty in the AERONET product and mixing state is included in the analysis).

Optical properties and aging of light-absorbing secondary organic aerosol

DOE PAGES

Liu, Jiumeng; Lin, Peng; Laskin, Alexander; ...

2016-10-14

The light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various volatile organic carbon (VOC) precursors, NO x concentrations, photolysis time, and relative humidity (RH) on the lightmore » absorption of selected secondary organic aerosols (SOA). Light absorption of chamber-generated SOA samples, especially aromatic SOA, was found to increase with NO x concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficient (MAC) value is observed from toluene SOA products formed under high-NO x conditions at moderate RH, in which nitro-aromatics were previously identified as the major light-absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organic nitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible (Vis) and ultraviolet (UV) light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.« less

Optical Properties and Aging of Light Absorbing Secondary Organic Aerosol

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

Liu, Jiumeng; Lin, Peng; Laskin, Alexander

2016-10-14

The light-absorbing organic aerosol (OA), commonly referred to as “brown carbon (BrC)”, has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various VOC precursors, NOx concentrations, photolysis time and relative humidity (RH) on the lightmore » absorption of selected secondary organic aerosols (SOA). Light absorption of chamber generated SOA samples, especially aromatic SOA, was found to increase with NOx concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficients (MAC) value is observed from toluene SOA products formed under high NOx conditions at moderate RH, in which nitro-aromatics were previously identified as the major light absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organonitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible and UV light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed-SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.« less

Atmospheric correction of SeaWiFS ocean color imagery in the presence of absorbing aerosols off the Indian coast using a neuro-variational method

NASA Astrophysics Data System (ADS)

Brajard, J.; Moulin, C.; Thiria, S.

2008-10-01

This paper presents a comparison of the atmospheric correction accuracy between the standard sea-viewing wide field-of-view sensor (SeaWiFS) algorithm and the NeuroVaria algorithm for the ocean off the Indian coast in March 1999. NeuroVaria is a general method developed to retrieve aerosol optical properties and water-leaving reflectances for all types of aerosols, including absorbing ones. It has been applied to SeaWiFS images of March 1999, during an episode of transport of absorbing aerosols coming from pollutant sources in India. Water-leaving reflectances and aerosol optical thickness estimated by the two methods were extracted along a transect across the aerosol plume for three days. The comparison showed that NeuroVaria allows the retrieval of oceanic properties in the presence of absorbing aerosols with a better spatial and temporal stability than the standard SeaWiFS algorithm. NeuroVaria was then applied to the available SeaWiFS images over a two-week period. NeuroVaria algorithm retrieves ocean products for a larger number of pixels than the standard one and eliminates most of the discontinuities and artifacts associated with the standard algorithm in presence of absorbing aerosols.

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.

Anomalies of the Asian Monsoon Induced by Aerosol Forcings

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, M. K.

2004-01-01

Impacts of aerosols on the Asian summer monsoon are studied using the NASA finite volume General Circulation Model (fvGCM), with radiative forcing derived from three-dimensional distributions of five aerosol species i.e., black carbon, organic carbon, soil dust, and sea salt from the Goddard Chemistry Aerosol Radiation and Transport Model (GOCART). Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in & early onset of the Indian summer monsoon. Absorbing aerosols also I i enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface' temperature cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.

Light-absorbing Aerosol Properties in the Kathmandu Valley during SusKat-ABC Field Campaign

NASA Astrophysics Data System (ADS)

Kim, S.; Yoon, S.; Kim, J.; Cho, C.; Jung, J.

2013-12-01

Light-absorbing aerosols, such as black carbon (BC), are major contributors to the atmospheric heating and the reduction of solar radiation reaching at the earth's surface. In this study, we investigate light-absorption and scattering properties of aerosols (i.e., BC mass concentration, aerosol solar-absorption/scattering efficiency) in the Kathmandu valley during Sustainable atmosphere for the Kathmandu valley (SusKat)-ABC campaign, from December 2012 to February 2013. Kathmandu City is among the most polluted cities in the world. However, there are only few past studies that provide basic understanding of air pollution in the Kathmandu Valley, which is not sufficient for designing effective mitigation measures (e.g., technological, financial, regulatory, legal and political measures, planning strategies). A distinct diurnal variation of BC mass concentration with two high peaks observed during wintertime dry monsoon period. BC mass concentration was found to be maximum around 09:00 and 20:00 local standard time (LST). Increased cars and cooking activities including substantial burning of wood and other biomass in the morning and in the evening contributed to high BC concentration. Low BC concentrations during the daytime can be explain by reduced vehicular movement and cooking activities. Also, the developmements of the boundary layer height and mountain-valley winds in the Kathmandu Valley paly a crucial role in the temproal variation of BC mass concentrations. Detailed radiative effects of light-absorbing aerosols will be presented.

Carbonaceous Aerosol Removal During Precipitation Events: Climate Implications

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Bridges, G. L.; Marchany-Rivera, A.; Begum, M.

2009-12-01

Atmospheric aerosols and their links to clouds are one of the main focus areas of the Department of Energy’s Atmospheric Systems Research, due to the fact that aerosols and clouds constitute the major uncertainties in radiative forcing that need to be reduced for more accurate modeling of climate, particularly regional climate. The impact of absorbing aerosols on radiative balance of the atmosphere will depend on their atmospheric lifetimes as well as their UV-visible absorption profiles. Aerosol lifetimes depend on the aerosols ability to take up water and grow to sufficient size to be either removed by gravitational settling or to act as cloud condensation nuclei and be removed by precipitation scavenging. The investigation of uv-visible absorbing aerosols is underway using a seven-channel aethalometer to evaluate the change in aerosol optical absorption during precipitation events. Angstrom absorption exponents (AAEs) are determined before, during, and after rain events to examine the impact on the aerosol absorption profiles anticipated by removal of the water soluble short-wave absorbing species (i.e. HULIS) that can be produced by photochemical oxidation of biogenic emissions (isoprene, monoterpenes, sesquiterpenes). Aerosol absorption data are presented from observations made at the University of Arkansas at Little Rock and other sites, which clearly show that a significant amount of absorbing carbon is not removed during rain events, and that the organic matter removed is likely secondary organics produced from biogenic precursors. The dissolved organic carbon measured in precipitation samples along with determinations of natural radionuclide tracers are also used to help examine the extent of carbonaceous aerosol removal by precipitation. The data are discussed in terms of the potential impacts of anthropogenic enhancement of aerosol absorption by secondary organic aerosols adding to atmospheric heating and changes in atmospheric dynamics. The potential

Impacts of solar-absorbing aerosol layers on the transition of stratocumulus to trade cumulus clouds

NASA Astrophysics Data System (ADS)

Zhou, Xiaoli; Ackerman, Andrew S.; Fridlind, Ann M.; Wood, Robert; Kollias, Pavlos

2017-10-01

The effects of an initially overlying layer of solar-absorbing aerosol on the transition of stratocumulus to trade cumulus clouds are examined using large-eddy simulations. For lightly drizzling cloud the transition is generally hastened, resulting mainly from increased cloud droplet number concentration (Nc) induced by entrained aerosol. The increased Nc slows sedimentation of cloud droplets and shortens their relaxation time for diffusional growth, both of which accelerate entrainment of overlying air and thereby stratocumulus breakup. However, the decrease in albedo from cloud breakup is more than offset by redistributing cloud water over a greater number of droplets, such that the diurnal-average shortwave forcing at the top of the atmosphere is negative. The negative radiative forcing is enhanced by sizable longwave contributions, which result from the greater cloud breakup and a reduced boundary layer height associated with aerosol heating. A perturbation of moisture instead of aerosol aloft leads to a greater liquid water path and a more gradual transition. Adding absorbing aerosol to that atmosphere results in substantial reductions in liquid water path (LWP) and cloud cover that lead to positive shortwave and negative longwave forcings on average canceling each other. Only for heavily drizzling clouds is the breakup delayed, as inhibition of precipitation overcomes cloud water loss from enhanced entrainment. Considering these simulations as an imperfect proxy for biomass burning plumes influencing Namibian stratocumulus, we expect regional indirect plus semi-direct forcings to be substantially negative to negligible at the top of the atmosphere, with its magnitude sensitive to background and perturbation properties.

Impacts of Solar-Absorbing Aerosol Layers on the Transition of Stratocumulus to Trade Cumulus Clouds

NASA Technical Reports Server (NTRS)

Zhou, Xiaoli; Ackerman, Andrew S.; Fridlind, Ann M.; Wood, Robert; Kollias, Pavlos

2017-01-01

The effects of an initially overlying layer of solar-absorbing aerosol on the transition of stratocumulus to trade cumulus clouds are examined using large-eddy simulations. For lightly drizzling cloud the transition is generally hastened, resulting mainly from increased cloud droplet number concentration (Nc) induced by entrained aerosol. The increased Nc slows sedimentation of cloud droplets and shortens their relaxation time for diffusional growth, both of which accelerate entrainment of overlying air and thereby stratocumulus breakup. However, the decrease in albedo from cloud breakup is more than offset by redistributing cloud water over a greater number of droplets, such that the diurnal-average shortwave forcing at the top of the atmosphere is negative. The negative radiative forcing is enhanced by sizable longwave contributions, which result from the greater cloud breakup and a reduced boundary layer height associated with aerosol heating. A perturbation of moisture instead of aerosol aloft leads to a greater liquid water path and a more gradual transition. Adding absorbing aerosol to that atmosphere results in substantial reductions in liquid water path (LWP) and cloud cover that lead to positive short-wave and negative longwave forcings on average canceling each other. Only for heavily drizzling clouds is the breakup delayed, as inhibition of precipitation overcomes cloud water loss from enhanced entrainment. Considering these simulations as an imperfect proxy for biomass burning plumes influencing Namibian stratocumulus, we expect regional indirect plus semi-direct forcings to be substantially negative to negligible at the top of the atmosphere, with its magnitude sensitive to background and perturbation properties.

Heating Rate of Light Absorbing Aerosols: Time-Resolved Measurements, the Role of Clouds, and Source Identification.

PubMed

Ferrero, Luca; Močnik, Griša; Cogliati, Sergio; Gregorič, Asta; Colombo, Roberto; Bolzacchini, Ezio

2018-03-20

Light absorbing aerosols (LAA) absorb sunlight and heat the atmosphere. This work presents a novel methodology to experimentally quantify the heating rate (HR) induced by LAA into an atmospheric layer. Multiwavelength aerosol absorption measurements were coupled with spectral measurements of the direct, diffuse and surface reflected radiation to obtain highly time-resolved measurements of HR apportioned in the context of LAA species (black carbon, BC; brown carbon, BrC; dust), sources (fossil fuel, FF; biomass burning, BB), and as a function of cloudiness. One year of continuous and time-resolved measurements (5 min) of HR were performed in the Po Valley. We experimentally determined (1) the seasonal behavior of HR (winter 1.83 ± 0.02 K day -1 ; summer 1.04 ± 0.01 K day -1 ); (2) the daily cycle of HR (asymmetric, with higher values in the morning than in the afternoon); (3) the HR in different sky conditions (from 1.75 ± 0.03 K day -1 in clear sky to 0.43 ± 0.01 K day -1 in complete overcast); (4) the apportionment to different sources: HR FF (0.74 ± 0.01 K day -1 ) and HR BB (0.46 ± 0.01 K day -1 ); and (4) the HR of BrC (HR BrC : 0.15 ± 0.01 K day -1 , 12.5 ± 0.6% of the total) and that of BC (HR BC : 1.05 ± 0.02 K day -1 ; 87.5 ± 0.6% of the total).

The Impact of Atmospheric Aerosols on the Fraction of absorbed Photosynthetically Active Radiation

NASA Astrophysics Data System (ADS)

Veroustraete, Frank

2010-05-01

Aerosol pollution attracts a growing interest from atmospheric scientists with regard to their impact on health, the global climate and vegetation stress. A hypothesis, less investigated, is whether atmospheric aerosol interactions in the solar radiation field affect the amount of radiation absorbed by vegetation canopies and hence terrestrial vegetation productivity. Typically, aerosols affect vegetation canopy radiation absorption efficiency by altering the physical characteristics of solar radiation incoming on for example a forest canopy. It has been illustrated, that increasing mixing ratio's of atmospheric particulate matter lead to a higher fraction of diffuse sunlight as opposed to direct sunlight. It can be demonstrated, based on the application of atmospheric (MODTRAN) and leaf/canopy radiative transfer (LIBERTY/SPRINT) models, that radiation absorption efficiency in the PAR band of Picea like forests increases with increasing levels of diffuse radiation. It can be documented - on a theoretical basis - as well, that increasing aerosol loads in the atmosphere, induce and increased canopy PAR absorption efficiency. In this paper it is suggested, that atmospheric aerosols have to be taken into account when estimating vegetation gross primary productivity (GPP). The results suggest that Northern hemisphere vegetation CO2 uptake magnitude may increase with increasing atmospheric aerosol loads. Many climate impact scenario's related to vegetation productivity estimates, do not take this phenomenon into account. Boldly speaking, the results suggest a larger sink function for terrestrial vegetation than generally accepted. Keywords: Aerosols, vegetation, fAPAR, CO2 uptake, diffuse radiation.

Impacts of solar-absorbing aerosol layers on the transition of stratocumulus to trade cumulus clouds

DOE PAGES

Zhou, Xiaoli; Ackerman, Andrew S.; Fridlind, Ann M.; ...

2017-10-26

Here, the effects of an initially overlying layer of solar-absorbing aerosol on the transition of stratocumulus to trade cumulus clouds are examined using large-eddy simulations. For lightly drizzling cloud the transition is generally hastened, resulting mainly from increased cloud droplet number concentration ( N c) induced by entrained aerosol. The increased N c slows sedimentation of cloud droplets and shortens their relaxation time for diffusional growth, both of which accelerate entrainment of overlying air and thereby stratocumulus breakup. However, the decrease in albedo from cloud breakup is more than offset by redistributing cloud water over a greater number of droplets,more » such that the diurnal-average shortwave forcing at the top of the atmosphere is negative. The negative radiative forcing is enhanced by sizable longwave contributions, which result from the greater cloud breakup and a reduced boundary layer height associated with aerosol heating. A perturbation of moisture instead of aerosol aloft leads to a greater liquid water path and a more gradual transition. Adding absorbing aerosol to that atmosphere results in substantial reductions in liquid water path (LWP) and cloud cover that lead to positive shortwave and negative longwave forcings on average canceling each other. Only for heavily drizzling clouds is the breakup delayed, as inhibition of precipitation overcomes cloud water loss from enhanced entrainment. Considering these simulations as an imperfect proxy for biomass burning plumes influencing Namibian stratocumulus, we expect regional indirect plus semi-direct forcings to be substantially negative to negligible at the top of the atmosphere, with its magnitude sensitive to background and perturbation properties.« less

Impacts of solar-absorbing aerosol layers on the transition of stratocumulus to trade cumulus clouds

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

Zhou, Xiaoli; Ackerman, Andrew S.; Fridlind, Ann M.

Here, the effects of an initially overlying layer of solar-absorbing aerosol on the transition of stratocumulus to trade cumulus clouds are examined using large-eddy simulations. For lightly drizzling cloud the transition is generally hastened, resulting mainly from increased cloud droplet number concentration ( N c) induced by entrained aerosol. The increased N c slows sedimentation of cloud droplets and shortens their relaxation time for diffusional growth, both of which accelerate entrainment of overlying air and thereby stratocumulus breakup. However, the decrease in albedo from cloud breakup is more than offset by redistributing cloud water over a greater number of droplets,more » such that the diurnal-average shortwave forcing at the top of the atmosphere is negative. The negative radiative forcing is enhanced by sizable longwave contributions, which result from the greater cloud breakup and a reduced boundary layer height associated with aerosol heating. A perturbation of moisture instead of aerosol aloft leads to a greater liquid water path and a more gradual transition. Adding absorbing aerosol to that atmosphere results in substantial reductions in liquid water path (LWP) and cloud cover that lead to positive shortwave and negative longwave forcings on average canceling each other. Only for heavily drizzling clouds is the breakup delayed, as inhibition of precipitation overcomes cloud water loss from enhanced entrainment. Considering these simulations as an imperfect proxy for biomass burning plumes influencing Namibian stratocumulus, we expect regional indirect plus semi-direct forcings to be substantially negative to negligible at the top of the atmosphere, with its magnitude sensitive to background and perturbation properties.« less

Fourier transform infrared analysis of aerosol formed in the photooxidation of 1-octene

NASA Astrophysics Data System (ADS)

Palen, Edward J.; Allen, David T.; Pandis, Spyros N.; Paulson, Suzanne; Seinfeld, John H.; Flagan, Richard C.

The chemical composition of aerosol generated in the photooxidation of 1-octene was examined using infrared microscopy interfaced with a low pressure impactor. The low pressure impactor segregated the aerosol into eight size fractions and deposited the aerosol onto ZnSe impaction substrates. The ZnSe surfaces were transparent in the mid-infrared region and therefore allowed direct analysis of the aerosol, with no extraction, using infrared microscopy. Infrared spectra of the size segregated aerosol showed strong absorbances due to ketone, alcohol, carboxylic acid and organonitrate functional groups. Absorbance features were relatively independent of particle size, with the exception of the carboxylic acid absorbances, which were found only in the largest aerosol size fractions. Molar loadings for each of the groups were estimated, based on model compound calibration standards. The molar loadings indicate that most aerosol species are multifunctional, with an average of one ketone group per molecule, an alcohol group in two of every three molecules and an organonitrate group in one of every three molecules.

Composition and spectral characteristics of ambient aerosol at Mauna Loa Observatory

NASA Technical Reports Server (NTRS)

Johnson, Stanley A.; Kumar, Romesh

1991-01-01

The spectral and the chemical characteristics of ambient aerosol at Mauna Loa Observatory (Hawaii) were determined in aerosol particles continuously sampled during an 8-day period in August 1986. During this period, the chemical species in the ambient aerosol varied considerably. During the major fraction of the sampling period, the aerosol was acidic due to predominance of (NH4)3H(SO4)2, NH4HSO4, or H2SO4. Aerosol samples showed much higher absorbance at 9.1 microns than at 10.6 microns. Moreover, changes in chemical composition from the neutral (NH4)2SO4 aerosol to more acidic sulphate forms were accompanied by substantial changes in the samples' absorbance at 9.1 microns (with lesser changes in the 10.6-micron absorptions).

Light-Absorbing Aerosol during NASA GRIP: Overview of Observations in the Free Troposphere and Associated with Tropical Storm Systems

NASA Astrophysics Data System (ADS)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C. A.; Craig, L.; Dhaniyala, S.; Dibb, J. E.; Hudgins, C. H.; Ismail, S.; Latham, T.; Nenes, A.; Thornhill, K. L.; Winstead, E.; Anderson, B. E.

2010-12-01

Aerosols play a significant role in regulating Earth’s climate. Absorbing aerosols typically constitute a small fraction of ambient particle mass but can contribute significantly to direct and indirect climate forcing depending on size, mixing state, concentration, chemical composition, and vertical and spatial distribution. Aerosols may also significantly affect tropical storm/hurricane dynamics through direct light absorption and activation as cloud nuclei. An extensive suite of instrumentation measuring aerosol chemical, physical, and optical properties was deployed aboard the NASA DC-8 to characterize aerosol during the NASA GRIP (Genesis and Rapid Intensification Processes; August-September 2010) mission. The majority of flight time was spent at high altitude (greater than 9 km) and thus much of the sampling was done in the free troposphere, including extensive sampling in the vicinity of tropical storm systems and more diffuse cirrus clouds. With operations based in Fort Lauderdale, FL and St. Croix, U.S. Virgin Islands, a large geographic region was sampled including much of the Gulf of Mexico and tropical Atlantic Ocean. Observations are reported for light-absorbing carbon aerosol (mainly black carbon, BC) primarily using a single particle soot photometer (SP2). The SP2 employs single-particle laser-induced incandescence to provide a mass-specific measurement not subject to scattering interference that is optimal for the low concentration environments like those encountered during GRIP. BC mass concentrations, 100-500 nm size distributions, and mixing state (i.e. coating thickness of scattering material) are presented. Total and sub-micron aerosol absorption coefficients (principally from BC and dust aerosol) are reported using a particle soot absorption photometer (PSAP) along with comparisons with calculated absorption coefficients derived from SP2 observations in various conditions. In addition, dust aerosol is specifically identified using optical and

In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of absorbing and non-absorbing organic coatings on spectral light absorption

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Lewis, K.; Moosmüller, H.

2009-10-01

Hundreds of wildfires in Northern California were sparked by lightning during the summer of 2008, resulting in downwind smoke for the months of June and July. Comparisons are reported for aerosol optics measurements in Reno, Nevada made during the very smoky month of July and the relatively clean month of August. Photoacoustic instruments equipped with integrating nephelometers were used to measure aerosol light scattering and absorption coefficients at wavelengths of 405 nm and 870 nm, revealing a strong variation of aerosol light absorption with wavelength. Insight on fuels burned is gleaned from comparison of Ångström exponents of absorption (AEA) versus single scattering albedo (SSA) of the ambient measurements with laboratory biomass smoke measurements for many fuels. Measurements during the month of August, which were largely unaffected by fire smoke, exhibit surprisingly low AEA for aerosol light absorption when the SSA is highest, again likely as a consequence of the underappreciated wavelength dependence of aerosol light absorption by particles coated with non-absorbing organic and inorganic matter. Coated sphere calculations were used to show that AEA as large as 1.6 are possible for wood smoke even with non-absorbing organic coatings on black carbon cores, suggesting care be exercised when diagnosing AEA.

Nitrogen-Containing, Light-Absorbing Oligomers Produced in Aerosol Particles Exposed to Methylglyoxal, Photolysis, and Cloud Cycling.

PubMed

De Haan, David O; Tapavicza, Enrico; Riva, Matthieu; Cui, Tianqu; Surratt, Jason D; Smith, Adam C; Jordan, Mary-Caitlin; Nilakantan, Shiva; Almodovar, Marisol; Stewart, Tiffany N; de Loera, Alexia; De Haan, Audrey C; Cazaunau, Mathieu; Gratien, Aline; Pangui, Edouard; Doussin, Jean-François

2018-04-03

Aqueous methylglyoxal chemistry has often been implicated as an important source of oligomers in atmospheric aerosol. Here we report on chemical analysis of brown carbon aerosol particles collected from cloud cycling/photolysis chamber experiments, where gaseous methylglyoxal and methylamine interacted with glycine, ammonium, or methylammonium sulfate seed particles. Eighteen N-containing oligomers were identified in the particulate phase by liquid chromatography/diode array detection/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry. Chemical formulas were determined and, for 6 major oligomer products, MS 2 fragmentation spectra were used to propose tentative structures and mechanisms. Electronic absorption spectra were calculated for six tentative product structures by an ab initio second order algebraic-diagrammatic-construction/density functional theory approach. For five structures, matching calculated and measured absorption spectra suggest that they are dominant light-absorbing species at their chromatographic retention times. Detected oligomers incorporated methylglyoxal and amines, as expected, but also pyruvic acid, hydroxyacetone, and significant quantities of acetaldehyde. The finding that ∼80% (by mass) of detected oligomers contained acetaldehyde, a methylglyoxal photolysis product, suggests that daytime methylglyoxal oligomer formation is dominated by radical addition mechanisms involving CH 3 CO*. These mechanisms are evidently responsible for enhanced browning observed during photolytic cloud events.

The role of anthropogenic species in Biogenic aerosol formation

EPA Science Inventory

Isoprene is a widely recognized source of organic aerosol in the southeastern United States. Models have traditionally represented isoprene-derived aerosol as semivolatile species formed from the initial isoprene + OH reaction. Recent laboratory and field studies indicate later g...

Estimating the Direct Radiative Effect of Absorbing Aerosols Overlying Marine Boundary Layer Clouds in the Southeast Atlantic Using MODIS and CALIOP

NASA Technical Reports Server (NTRS)

Meyer, Kerry; Platnick, Steven; Oreopoulos, Lazaros; Lee, Dongmin

2013-01-01

Absorbing aerosols such as smoke strongly absorb solar radiation, particularly at ultraviolet and visible/near-infrared (VIS/NIR) wavelengths, and their presence above clouds can have considerable implications. It has been previously shown that they have a positive (i.e., warming) direct aerosol radiative effect (DARE) when overlying bright clouds. Additionally, they can cause biased passive instrument satellite retrievals in techniques that rely on VIS/NIR wavelengths for inferring the cloud optical thickness (COT) and effective radius (re) of underlying clouds, which can in turn yield biased above-cloud DARE estimates. Here we investigate Moderate Resolution Imaging Spectroradiometer (MODIS) cloud optical property retrieval biases due to overlying absorbing aerosols observed by Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and examine the impact of these biases on above-cloud DARE estimates. The investigation focuses on a region in the southeast Atlantic Ocean during August and September (2006-2011), where smoke from biomass burning in southern Africa overlies persistent marine boundary layer stratocumulus clouds. Adjusting for above-cloud aerosol attenuation yields increases in the regional mean liquid COT (averaged over all ocean-only liquid clouds) by roughly 6%; mean re increases by roughly 2.6%, almost exclusively due to the COT adjustment in the non-orthogonal retrieval space. It is found that these two biases lead to an underestimate of DARE. For liquid cloud Aqua MODIS pixels with CALIOP-observed above-cloud smoke, the regional mean above-cloud radiative forcing efficiency (DARE per unit aerosol optical depth (AOD)) at time of observation (near local noon for Aqua overpass) increases from 50.9Wm(sup-2)AOD(sup-1) to 65.1Wm(sup-2)AOD(sup -1) when using bias-adjusted instead of nonadjusted MODIS cloud retrievals.

Vertical Profiles of Light-Absorbing Aerosol: A Combination of In-situ and AERONET Observations during NASA DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C.; Crumeyrolle, S.; Giles, D. M.; Holben, B. N.; Hudgins, C.; Martin, R.; Moore, R.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.

2014-12-01

Understanding the vertical profile of atmospheric aerosols plays a vital role in utilizing spaceborne, column-integrated satellite observations. The properties and distribution of light-absorbing aerosol are particularly uncertain despite significant air quality and climate ramifications. Advanced retrieval algorithms are able to derive complex aerosol properties (e.g., wavelength-dependent absorption coefficient and single scattering albedo) from remote-sensing measurements, but quantitative relationships to surface conditions remain a challenge. Highly systematic atmospheric profiling during four unique deployments for the NASA DISCOVER-AQ project (Baltimore, MD, 2011; San Joaquin Valley, CA, 2013; Houston, TX, 2013; Denver, CO, 2014) allow statistical assessment of spatial, temporal, and source-related variability for light-absorbing aerosol properties in these distinct regions. In-situ sampling in conjunction with a dense network of AERONET sensors also allows evaluation of the sensitivity, limitations, and advantages of remote-sensing data products over a wide range of conditions. In-situ aerosol and gas-phase observations were made during DISCOVER-AQ aboard the NASA P-3B aircraft. Aerosol absorption coefficients were measured by a Particle Soot Absorption Photometer (PSAP). Approximately 200 profiles for each of the four deployments were obtained, from the surface (25-300m altitude) to 5 km, and are used to calculate absorption aerosol optical depths (AAODs). These are quantitatively compared to AAOD derived from AERONET Level 1.5 retrievals to 1) explore discrepancies between measurements, 2) quantify the fraction of AAOD that exists directly at the surface and is often missed by airborne sampling, and 3) evaluate the potential for deriving ground-level black carbon (BC) concentrations for air quality prediction. Aerosol size distributions are used to assess absorption contributions from mineral dust, both at the surface and aloft. SP2 (Single Particle Soot

Advantages of measuring the Q Stokes parameter in addition to the total radiance I in the detection of absorbing aerosols

NASA Astrophysics Data System (ADS)

Stamnes, Snorre; Fan, Yongzhen; Chen, Nan; Li, Wei; Tanikawa, Tomonori; Lin, Zhenyi; Liu, Xu; Burton, Sharon; Omar, Ali; Stamnes, Jakob J.; Cairns, Brian; Stamnes, Knut

2018-05-01

A simple but novel study was conducted to investigate whether an imager-type spectroradiometer instrument like MODIS, currently flying on board the Aqua and Terra satellites, or MERIS, which flew on board Envisat, could detect absorbing aerosols if they could measure the Q Stokes parameter in addition to the total radiance I, that is if they could also measure the linear polarization of the light. Accurate radiative transfer calculations were used to train a fast neural network forward model, which together with a simple statistical optimal estimation scheme was used to retrieve three aerosol parameters: aerosol optical depth at 869 nm, optical depth fraction of fine mode (absorbing) aerosols at 869 nm, and aerosol vertical location. The aerosols were assumed to be bimodal, each with a lognormal size distribution, located either between 0 and 2 km or between 2 and 4 km in the Earth's atmosphere. From simulated data with 3% random Gaussian measurement noise added for each Stokes parameter, it was found that by itself the total radiance I at the nine MODIS VIS channels was generally insufficient to accurately retrieve all three aerosol parameters (˜ 15% to 37% successful), but that together with the Q Stokes component it was possible to retrieve values of aerosol optical depth at 869 nm to ± 0.03, single-scattering albedo at 869 nm to ± 0.04, and vertical location in ˜ 65% of the cases. This proof-of-concept retrieval algorithm uses neural networks to overcome the computational burdens of using vector radiative transfer to accurately simulate top-of-atmosphere (TOA) total and polarized radiances, enabling optimal estimation techniques to exploit information from multiple channels. Therefore such an algorithm could, in concept, be readily implemented for operational retrieval of aerosol and ocean products from moderate or hyperspectral spectroradiometers.

Aqueous aerosol SOA formation: impact on aerosol physical properties.

PubMed

Woo, Joseph L; Kim, Derek D; Schwier, Allison N; Li, Ruizhi; McNeill, V Faye

2013-01-01

Organic chemistry in aerosol water has recently been recognized as a potentially important source of secondary organic aerosol (SOA) material. This SOA material may be surface-active, therefore potentially affecting aerosol heterogeneous activity, ice nucleation, and CCN activity. Aqueous aerosol chemistry has also been shown to be a potential source of light-absorbing products ("brown carbon"). We present results on the formation of secondary organic aerosol material in aerosol water and the associated changes in aerosol physical properties from GAMMA (Gas-Aerosol Model for Mechanism Analysis), a photochemical box model with coupled gas and detailed aqueous aerosol chemistry. The detailed aerosol composition output from GAMMA was coupled with two recently developed modules for predicting a) aerosol surface tension and b) the UV-Vis absorption spectrum of the aerosol, based on our previous laboratory observations. The simulation results suggest that the formation of oligomers and organic acids in bulk aerosol water is unlikely to perturb aerosol surface tension significantly. Isoprene-derived organosulfates are formed in high concentrations in acidic aerosols under low-NO(x) conditions, but more experimental data are needed before the potential impact of these species on aerosol surface tension may be evaluated. Adsorption of surfactants from the gas phase may further suppress aerosol surface tension. Light absorption by aqueous aerosol SOA material is driven by dark glyoxal chemistry and is highest under high-NO(x) conditions, at high relative humidity, in the early morning hours. The wavelength dependence of the predicted absorption spectra is comparable to field observations and the predicted mass absorption efficiencies suggest that aqueous aerosol chemistry can be a significant source of aerosol brown carbon under urban conditions.

Absorbing and scattering aerosols over the source region of biomass burning emissions: Implications in the assessment of optical and radiative properties

NASA Astrophysics Data System (ADS)

Singh, Atinderpal; Srivastava, Rohit; Rastogi, Neeraj; Singh, Darshan

2016-02-01

The current study focuses on the assessment of model simulated optical and radiative properties of aerosols incorporating the measured chemical composition of aerosol samples collected at Patiala during October, 2011-February, 2012. Monthly average mass concentration of PM2.5, elemental carbon (EC), primary organic carbon (POC), water-soluble (WS) and insoluble (INS) aerosols ranged from 120 to 192, 6.2 to 7.2, 20 to 39, 59 to 111 and 35 to 90 μg m-3, respectively. Mass concentration of different components of aerosols was further used for the assessment of optical properties derived from Optical Properties of Aerosols and Clouds (OPAC) model simulations. Microtops based measured aerosol optical depth (AOD500) ranged from 0.47 to 0.62 showing maximum value during November and December, and minimum during February. Ångström exponent (α380-870) remained high (>0.90) throughout the study period except in February (0.74), suggesting predominance of fine mode particles over the study region. The observed ratio of scattering to absorbing aerosols was incorporated in OPAC model simulations and single scattering albedo (SSA at 500 nm) so obtained ranged between 0.80 and 0.92 with relatively low values during the period of extensive biomass burning. In the present study, SBDART based estimated values of aerosol radiative forcing (ARF) at the surface (SRF) and top of the atmosphere (TOA) ranged from -31 to -66 Wm-2 and -2 to -18 W m-2 respectively. The atmospheric ARF, ranged between + 18 and + 58 Wm-2 resulting in the atmospheric heating rate between 0.5 and 1.6 K day-1. These results signify the role of scattering and absorbing aerosols in affecting the magnitude of aerosol forcing.

Glyoxal-methylglyoxal cross-reactions in secondary organic aerosol formation.

PubMed

Schwier, Allison N; Sareen, Neha; Mitroo, Dhruv; Shapiro, Erica L; McNeill, V Faye

2010-08-15

Glyoxal (G) and methylglyoxal (MG) are potentially important secondary organic aerosol (SOA) precursors. Previous studies of SOA formation by G and MG have focused on either species separately; however, G and MG typically coexist in the atmosphere. We studied the formation of secondary organic material in aqueous aerosol mimic mixtures containing G and MG with ammonium sulfate. We characterized the formation of light-absorbing products using UV-vis spectrophotometry. We found that absorption at 280 nm can be described well using models for the formation of light-absorbing products by G and MG in parallel. Pendant drop tensiometry measurements showed that surface tension depression by G and MG in these solutions can be modeled as a linear combination of the effects of G and MG alone. Product species were identified using chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol CIMS). Peaks consistent with G-MG cross-reaction products were observed, accounting for a significant fraction of detected product mass, but most peaks could be attributed to self-reaction. We conclude that cross-reactions contribute to SOA mass from uptake of G and MG, but they are not required to accurately model the effects of this process on aerosol surface tension or light absorption.

Tar balls are processed, weakly absorbing, primary aerosol particles formed downwind of boreal forest fires

NASA Astrophysics Data System (ADS)

Sedlacek, A. J., III; Buseck, P. R.; Adachi, K.; Kleinman, L. I.; Onasch, T. B.; Springston, S. R.

2017-12-01

Biomass burning is a major source of light-absorbing black and brown carbonaceous aerosols Brown carbon is a poorly characterized mixture that includes tar balls (TBs), a type of carbonaceous particle unique to biomass burning. Here we describe the first atmospheric observations of the formation and evolution of TBs Aerosol particles were collected on TEM grids during individual aircraft transects at varying downwind distances from the Colockum Tarp wildland fire. The TEM images show primary particles transforming from viscous, impact-deformed particles to spherical TBs. The number fraction of TBs in the wildfire smoke plume increased from less than 5% in samples collected close to the emission source to greater than 40% after 3 hours of aging, with little change in downwind TB diameters. The TB mass fraction increased from 2% near the fire to 23±9% downwind. Single-scatter albedo determined from scattering and absorption measurements increased slightly with downwind distance. Mie calculations show this observation is consistent with weak light absorbance by TBs (m=1.56 - 0.02i) but not consistent with order-of-magnitude stronger absorption observed in different settings. The field-derived TB mass fractions reported here indicate that this particle type should be accounted for in biomass-burn emission inventories.

A climatology of fine absorbing biomass burning, urban and industrial aerosols detected from satellites

NASA Astrophysics Data System (ADS)

Kalaitzi, Nikoleta; Hatzianastassiou, Nikos; Gkikas, Antonis; Papadimas, Christos D.; Torres, Omar; Mihalopoulos, Nikos

2017-04-01

Natural biomass burning (BB) along with anthropogenic urban and industrial aerosol particles, altogether labeled here as BU aerosols, contain black and brown carbon which both absorb strongly the solar radiation. Thus, BU aerosols warm significantly the atmosphere also causing adjustments to cloud properties, which traditionally are known as cloud indirect and semi-direct effects. Given the role of the effects of BU aerosols for contemporary and future climate change, and the uncertainty associated with BU, both ascertained by the latest IPCC reports, there is an urgent need for improving our knowledge on the spatial and temporal variability of BU aerosols all over the globe. Over the last few decades, thanks to the rapid development of satellite observational techniques and retrieval algorithms it is now possible to detect BU aerosols based on satellite measurements. However, care must be taken in order to ensure the ability to distinguish BU from other aerosol types usually co-existing in the Earth's atmosphere. In the present study, an algorithm is presented, based on a synergy of different satellite measurements, aiming to identify and quantify BU aerosols over the entire globe and during multiple years. The objective is to build a satellite-based climatology of BU aerosols intended for use for various purposes. The produced regime, namely the spatial and temporal variability of BU aerosols, emphasizes the BU frequency of occurrence and their intensity, in terms of aerosol optical depth (AOD). The algorithm is using the following aerosol optical properties describing the size and atmospheric loading of BU aerosols: (i) spectral AOD, (ii) Ångström Exponent (AE), (iii) Fine Fraction (FF) and (iv) Aerosol Index (AI). The relevant data are taken from Collection 006 MODIS-Aqua, except for AI which is taken from OMI-Aura. The identification of BU aerosols by the algorithm is based on a specific thresholding technique, with AI≥1.5, AE≥1.2 and FF≥0.6 threshold

Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

NASA Technical Reports Server (NTRS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Dickerson, R. R.; Thompson, A. M.; Slutsker, I.; Li, Z.; Tripathi, S. N.; Singh, R. P.;

An Accurate Analytic Approximation for Light Scattering by Non-absorbing Spherical Aerosol Particles

NASA Astrophysics Data System (ADS)

Lewis, E. R.

2017-12-01

The scattering of light by particles in the atmosphere is a ubiquitous and important phenomenon, with applications to numerous fields of science and technology. The problem of scattering of electromagnetic radiation by a uniform spherical particle can be solved by the method of Mie and Debye as a series of terms depending on the size parameter, x=2πr/λ, and the complex index of refraction, m. However, this solution does not provide insight into the dependence of the scattering on the radius of the particle, the wavelength, or the index of refraction, or how the scattering varies with relative humidity. Van de Hulst demonstrated that the scattering efficiency (the scattering cross section divided by the geometric cross section) of a non-absorbing sphere, over a wide range of particle sizes of atmospheric importance, depends not on x and m separately, but on the quantity 2x(m-1); this is the basis for the anomalous diffraction approximation. Here an analytic approximation for the scattering efficiency of a non-absorbing spherical particle is presented in terms of this new quantity that is accurate over a wide range of particle sizes of atmospheric importance and which readily displays the dependences of the scattering efficiency on particle radius, index of refraction, and wavelength. For an aerosol for which the particle size distribution is parameterized as a gamma function, this approximation also yields analytical results for the scattering coefficient and for the Ångström exponent, with the dependences of scattering properties on wavelength and index of refraction clearly displayed. This approximation provides insight into the dependence of light scattering properties on factors such as relative humidity, readily enables conversion of scattering from one index of refraction to another, and demonstrates the conditions under which the aerosol index (the product of the aerosol optical depth and the Ångström exponent) is a useful proxy for the number of cloud

Modeling investigation of light-absorbing aerosols in the Amazon Basin during the wet season

NASA Astrophysics Data System (ADS)

Wang, Qiaoqiao; Saturno, Jorge; Chi, Xuguang; Walter, David; Lavric, Jost; Moran-Zuloaga, Daniel; Ditas, Florian; Pöhlker, Christopher; Brito, Joel; Carbone, Samara; Artaxo, Paulo; Andreae, Meinrat

2017-04-01

We use a global chemical transport model (GEOS-Chem) to interpret observed light-absorbing aerosols in Amazonia during the wet season. Observed aerosol properties, including black carbon (BC) concentration and light absorption, at the Amazon Tall Tower Observatory (ATTO) site in the central Amazon have relatively low background levels but frequently show high peaks during the study period of January-April 2014. With daily temporal resolution for open fire emissions and modified aerosol optical properties, our model successfully captures the observed variation in fine/coarse aerosol and BC concentrations as well as aerosol light absorption and its wavelength dependence over the Amazon Basin. The source attribution in the model indicates the important influence of open fire on the observed variances of aerosol concentrations and absorption, mainly from regional sources (northern South America) and from northern Africa. The contribution of open fires from these two regions is comparable, with the latter becoming more important in the late wet season. The analysis of correlation and enhancement ratios of BC versus CO suggests transport times of < 3 days for regional fires and 11 days for African plumes arriving at ATTO during the wet season. The model performance of long-range transport of African plumes is also evaluated with observations from AERONET, MODIS, and CALIOP. Simulated absorption aerosol optical depth (AAOD) averaged over the wet season is lower than 0.0015 over the central Amazon, including the ATTO site. We find that more than 50% of total absorption at 550 nm is from BC, except for the northeastern Amazon and the Guianas, where the influence of dust becomes significant (up to 35 %). The brown carbon contribution is generally between 20 and 30 %. The distribution of absorption Ångström exponents (AAE) suggests more influence from fossil fuel combustion in the southern part of the basin (AAE 1) but more open fire and dust influence in the northern part

Simultaneous Retrieval of Effective Refractive Index and Density from Size Distribution and Light Scattering Data: Weakly-Absorbing Aerosol

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

Kassianov, Evgueni I.; Barnard, James C.; Pekour, Mikhail S.

2014-10-01

We propose here a novel approach for retrieving in parallel the effective density and real refractive index of weakly absorbing aerosol from optical and size distribution measurements. Here we define “weakly absorbing” as aerosol single-scattering albedos that exceed 0.95 at 0.5 um.The required optical measurements are the scattering coefficient and the hemispheric backscatter fraction, obtained in this work from an integrating nephelometer. The required size spectra come from a Scanning Mobility Particle Sizer and an Aerodynamic Particle Sizer. The performance of this approach is first evaluated using a sensitivity study with synthetically generated but measurement-related inputs. The sensitivity study revealsmore » that the proposed approach is robust to random noise; additionally the uncertainties of the retrieval are almost linearly proportional to the measurement errors, and these uncertainties are smaller for the real refractive index than for the effective density. Next, actual measurements are used to evaluate our approach. These measurements include the optical, microphysical, and chemical properties of weakly absorbing aerosol which are representative of a variety of coastal summertime conditions observed during the Two-Column Aerosol Project (TCAP; http://campaign.arm.gov/tcap/). The evaluation includes calculating the root mean square error (RMSE) between the aerosol characteristics retrieved by our approach, and the same quantities calculated using the conventional volume mixing rule for chemical constituents. For dry conditions (defined in this work as relative humidity less than 55%) and sub-micron particles, a very good (RMSE~3%) and reasonable (RMSE~28%) agreement is obtained for the retrieved real refractive index (1.49±0.02) and effective density (1.68±0.21), respectively. Our approach permits discrimination between the retrieved aerosol characteristics of sub-micron and sub-10micron particles. The evaluation results also reveal that the

Estimation of columnar concentrations of absorbing and scattering fine mode aerosol components using AERONET data

NASA Astrophysics Data System (ADS)

Choi, Yongjoo; Ghim, Young Sung

2016-11-01

Columnar concentrations of absorbing and scattering components of fine mode aerosols were estimated using Aerosol Robotic Network (AERONET) data for a site downwind of Seoul. The study period was between March 2012 and April 2013 including the period of the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-Asia campaign in March to May 2012. The Maxwell Garnett mixing rule was assumed for insoluble components embedded in a host solution, while the volume average mixing rule was assumed for the aqueous solution of soluble components. During the DRAGON-Asia campaign the surface concentrations of major components of fine particles were measured. The columnar mass fractions of black carbon (BC), organic carbon (OC), mineral dust (MD), and ammonium sulfate (AS) were 1.5, 5.9, 6.6, and 52%, respectively, which were comparable to the mass fractions measured at the surface for BC, OC, and secondary inorganic aerosols at 2.3, 18, and 55%. The vertical distributions of BC and AS were investigated by employing the concept of a column height. While the column height for BC was similar to the planetary boundary layer (PBL) height, that for AS was 4.4 times higher than the PBL height and increased with air temperature from March to May. The monthly variations of the columnar mass concentrations during the study period were generally well explained in term of meteorology and emission characteristics. However, certain variations of MD were different from those typically observed primarily because only fine mode aerosols were considered.

Synergy of Satellite-Surface Observations for Studying the Properties of Absorbing Aerosols in Asia

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee

2010-01-01

Through interaction with clouds and alteration of the Earth's radiation budget, atmospheric aerosols significantly influence our weather and climate. Monsoon rainfalls, for example, sustain the livelihood of more than half of the world's population. Thus, understanding the mechanism that drives the water cycle and freshwater distribution is high-lighted as one of the major near-term goals in NASA's Earth Science Enterprise Strategy. Every cloud droplet/ice-crystal that serves as an essential element in portraying water cycle and distributing freshwater contains atmospheric aerosols at its core. In addition, the spatial and temporal variability of atmospheric aerosol properties is complex due to their dynamic nature. In fact, the predictability of the tropical climate system is much reduced during the boreal spring, which is associated with the peak season of biomass burning activities and regional/long-range transport of dust aerosols. Therefore, to accurately assess the impact of absorbing aerosols on regional-to-global climate requires not only modeling efforts but also continuous observations from satellites, aircraft, networks of ground-based instruments and dedicated field experiments. Since 1997 NASA has been successfully launching a series of satellites the Earth Observing System - to intensively study, and gain a better understanding of, the Earth as an integrated system. Through participation in many satellite remote-sensing/retrieval and validation projects over the years, we have gradually developed and refined the SMART (Surface-sensing Measurements for Atmospheric Radiative Transfer) and COMMIT (Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile observatories, a suite of surface remote sensing and in-situ instruments that proved to be vital in providing high temporal measurements, which complement the satellite observations. In this talk, we will present SMART-COMMIT which has played key roles, serving as network or supersite

Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

NASA Astrophysics Data System (ADS)

Marley, N. A.; Marchany-Rivera, A.; Kelley, K. L.; Mangu, A.; Gaffney, J. S.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (<0.1micron) were also collected at site T0 and T1 (Universidad Technologica de Tecamac, State of Mexico) from 5 am to 5 pm (day) and from 5 pm to 5 am (night) during the month of March 2006. Samples were collected on quartz fiber filters with high volume impactor samplers. Continuous absorption spectra of these aerosol samples have been obtained in the laboratory from 280 to 900nm with the use of an integrating sphere coupled to a UV spectrometer (Beckman DU with a Labsphere accessory). The integrating sphere allows the detector to collect and spatially integrate the total radiant flux reflected from the sample and therefore allows for the measurement of absorption on highly reflective or diffusely scattering samples. These continuous spectra have also been used to obtain the

Two chemically distinct light-absorbing pools of urban organic aerosols: A comprehensive multidimensional analysis of trends.

PubMed

Paula, Andreia S; Matos, João T V; Duarte, Regina M B O; Duarte, Armando C

2016-02-01

The chemical and light-absorption dynamics of organic aerosols (OAs), a master variable in the atmosphere, have yet to be resolved. This study uses a comprehensive multidimensional analysis approach for exploiting simultaneously the compositional changes over a molecular size continuum and associated light-absorption (ultraviolet absorbance and fluorescence) properties of two chemically distinct pools of urban OAs chromophores. Up to 45% of aerosol organic carbon (OC) is soluble in water and consists of a complex mixture of fluorescent and UV-absorbing constituents, with diverse relative abundances, hydrophobic, and molecular weight (Mw) characteristics between warm and cold periods. In contrast, the refractory alkaline-soluble OC pool (up to 18%) is represented along a similar Mw and light-absorption continuum throughout the different seasons. Results suggest that these alkaline-soluble chromophores may actually originate from primary OAs sources in the urban site. This work shows that the comprehensive multidimensional analysis method is a powerful and complementary tool for the characterization of OAs fractions. The great diversity in the chemical composition and optical properties of OAs chromophores, including both water-soluble and alkaline-soluble OC, may be an important contribution to explain the contrasting photo-reactivity and atmospheric behavior of OAs. Copyright © 2015 Elsevier Ltd. All rights reserved.

Influences of external vs. core-shell mixing on aerosol optical properties at various relative humidities.

PubMed

Ramachandran, S; Srivastava, Rohit

2013-05-01

Aerosol optical properties of external and core-shell mixtures of aerosol species present in the atmosphere are calculated in this study for different relative humidities. Core-shell Mie calculations are performed using the values of radii, refractive indices and densities of aerosol species that act as core and shell, and the core-shell radius ratio. The single scattering albedo (SSA) is higher when the absorbing species (black carbon, BC) is the core, while for a sulfate core SSA does not vary significantly as the BC in the shell dominates the absorption. Absorption gets enhanced in core-shell mixing of absorbing and scattering aerosols when compared to their external mixture. Thus, SSA is significantly lower for a core-shell mixture than their external mixture. SSA is more sensitive to core-shell ratio than mode radius when BC is the core. The extinction coefficient, SSA and asymmetry parameter are higher for external mixing when compared to BC (core)-water soluble aerosol (shell), and water soluble aerosol (core)-BC (shell) mixtures in the relative humidity range of 0 to 90%. Spectral SSA exhibits the behaviour of the species which acts as a shell in core-shell mixing. The asymmetry parameter for an external mixture of water soluble aerosol and BC is higher than BC (core)-water soluble aerosol (shell) mixing and increases as function of relative humidity. The asymmetry parameter for the water soluble aerosol (core)-BC (shell) is independent of relative humidity as BC is hydrophobic. The asymmetry parameter of the core-shell mixture decreases when BC aerosols are involved in mixing, as the asymmetry parameter of BC is lower. Aerosol optical depth (AOD) of core-shell mixtures increases at a higher rate when the relative humidity exceeds 70% in continental clean and urban aerosol models, whereas AOD remains the same when the relative humidity exceeds 50% in maritime aerosol models. The SSA for continental aerosols varies for core-shell mixing of water soluble

Global Aerosol Optical Models and Lookup Tables for the New MODIS Aerosol Retrieval over Land

NASA Technical Reports Server (NTRS)

Levy, Robert C.; Remer, Loraine A.; Dubovik, Oleg

2007-01-01

Since 2000, MODIS has been deriving aerosol properties over land from MODIS observed spectral reflectance, by matching the observed reflectance with that simulated for selected aerosol optical models, aerosol loadings, wavelengths and geometrical conditions (that are contained in a lookup table or 'LUT'). Validation exercises have showed that MODIS tends to under-predict aerosol optical depth (tau) in cases of large tau (tau greater than 1.0), signaling errors in the assumed aerosol optical properties. Using the climatology of almucantur retrievals from the hundreds of global AERONET sunphotometer sites, we found that three spherical-derived models (describing fine-sized dominated aerosol), and one spheroid-derived model (describing coarse-sized dominated aerosol, presumably dust) generally described the range of observed global aerosol properties. The fine dominated models were separated mainly by their single scattering albedo (omega(sub 0)), ranging from non-absorbing aerosol (omega(sub 0) approx. 0.95) in developed urban/industrial regions, to neutrally absorbing aerosol (omega(sub 0) approx.90) in forest fire burning and developing industrial regions, to absorbing aerosol (omega(sub 0) approx. 0.85) in regions of savanna/grassland burning. We determined the dominant model type in each region and season, to create a 1 deg. x 1 deg. grid of assumed aerosol type. We used vector radiative transfer code to create a new LUT, simulating the four aerosol models, in four MODIS channels. Independent AERONET observations of spectral tau agree with the new models, indicating that the new models are suitable for use by the MODIS aerosol retrieval.

Light absorbing material (soot) in rainwater and in aerosol particles in the Maldives

NASA Astrophysics Data System (ADS)

Granat, L.; EngströM, J. E.; Praveen, S.; Rodhe, H.

2010-08-01

Simultaneous measurements of soot (absorbing material at 528 nm) and inorganic ions in aerosol and precipitation at the Maldives Climate Observatory Hanimaadhoo during the period May 2005 to February 2007 have made it possible to calculate the washout ratio (WR) of these components as a measure of how efficiently they are scavenged by precipitation. On the basis of air trajectories the data have been separated into days with polluted air arriving from the Indian subcontinent in a northeasterly sector during winter and clean monsoon days with southerly flow from the Indian Ocean. The average soot concentration was a factor of 10 higher in the former situations. Despite considerable scatter for individual days, a systematic pattern emerged when the WR for the different components were compared with each other. During the monsoon season the WR for soot was similar to that of sulfate and other fine mode aerosol components, indicating that soot containing particles in these situations were efficient as cloud condensation nuclei. The origin of the light absorbing material during the monsoon season is unclear. During the polluted winter days, on the other hand, the WR for soot was three times smaller than that of sulfate. This indicates that, even after a travel time of several days, the soot containing particles from India have retained much of their hydrophobic property. The low WR and the infrequent rain during this season probably contribute to extending the atmospheric lifetime of soot well beyond several days. Surprisingly high concentrations of non-sea-salt calcium were measured during the monsoon season, substantially higher than during the winter season. The origin of these high values could be long-range transport from the Australian or African continents. Another possibility might be exopolymer gels derived from the ocean surface microlayer.

Estimate of the Impact of Absorbing Aerosol Over Cloud on the MODIS Retrievals of Cloud Optical Thickness and Effective Radius Using Two Independent Retrievals of Liquid Water Path

NASA Technical Reports Server (NTRS)

Wilcox, Eric M.; Harshvardhan; Platnick, Steven

2009-01-01

Two independent satellite retrievals of cloud liquid water path (LWP) from the NASA Aqua satellite are used to diagnose the impact of absorbing biomass burning aerosol overlaying boundary-layer marine water clouds on the Moderate Resolution Imaging Spectrometer (MODIS) retrievals of cloud optical thickness (tau) and cloud droplet effective radius (r(sub e)). In the MODIS retrieval over oceans, cloud reflectance in the 0.86-micrometer and 2.13-micrometer bands is used to simultaneously retrieve tau and r(sub e). A low bias in the MODIS tau retrieval may result from reductions in the 0.86-micrometer reflectance, which is only very weakly absorbed by clouds, owing to absorption by aerosols in cases where biomass burning aerosols occur above water clouds. MODIS LWP, derived from the product of the retrieved tau and r(sub e), is compared with LWP ocean retrievals from the Advanced Microwave Scanning Radiometer-EOS (AMSR-E), determined from cloud microwave emission that is transparent to aerosols. For the coastal Atlantic southern African region investigated in this study, a systematic difference between AMSR-E and MODIS LWP retrievals is found for stratocumulus clouds over three biomass burning months in 2005 and 2006 that is consistent with above-cloud absorbing aerosols. Biomass burning aerosol is detected using the ultraviolet aerosol index from the Ozone Monitoring Instrument (OMI) on the Aura satellite. The LWP difference (AMSR-E minus MODIS) increases both with increasing tau and increasing OMI aerosol index. During the biomass burning season the mean LWP difference is 14 g per square meters, which is within the 15-20 g per square meter range of estimated uncertainties in instantaneous LWP retrievals. For samples with only low amounts of overlaying smoke (OMI AI less than or equal to 1) the difference is 9.4, suggesting that the impact of smoke aerosols on the mean MODIS LWP is 5.6 g per square meter. Only for scenes with OMI aerosol index greater than 2 does the

Impacts of snow darkening by absorbing aerosols on South Asian monsoon

NASA Astrophysics Data System (ADS)

Kim, K. M.; Lau, W. K. M.; Kim, M. K.; Sang, J.; Yasunari, T. J.; Koster, R. D.

2016-12-01

Seasonal heating over the Tibetan Plateau is a main driver of the onset of the South Asian Monsoon. Aerosols can play an important role in pre- and early monsoon seasonal heating process over the Tibetan Plateau by increasing atmospheric heating in the northern India, and by heating of the surface of the Tibetan Plateau and Himalayan slopes, via reduction of albedo of the snow surface through surface deposition - the so call snow-darkening effect (SDE). To examine the impact of SDE on weather and climate during late spring and early summer, two sets of NASA/GEOS-5 model simulations with and without SDE are conducted. Results show that SDE-induced surface heating accelerates snow melts and increases surface temperature over 4K in the entire Tibetan Plateau regions during boreal summer. Warmer Tibetan Plateau further accelerates seasonal warming in the upper troposphere and increases the north-south temperature gradient between the Tibetan Plateau and the equatorial Indian Ocean. This reversal of the north-south temperature gradient is a primary cause of the onset of the South Asian monsoon. SDE-induced increase of the meridional temperature gradient drives meridional circulation and enhanced upper tropospheric easterlies and lower tropospheric westerlies, and intensifies monsoon circulation and rainfall. This pattern enhances the EHP-like circulation anomalies induced by atmospheric heating of absorbing aerosols over the northern India. SDE-induced change in the India subcontinent differs that in Eurasia. SDE-induced land-atmospheric interactions in two regions will be also compared.

Impacts of Snow Darkening by Absorbing Aerosols on Eurasian Climate

NASA Technical Reports Server (NTRS)

Kim, Kyu-Myong; Lau, William K M.; Yasunari, Teppei J.; Kim, Maeng-Ki; Koster, Randal D.

2016-01-01

The deposition of absorbing aerosols on snow surfaces reduces snow-albedo and allows snowpack to absorb more sunlight. This so-called snow darkening effect (SDE) accelerates snow melting and leads to surface warming in spring. To examine the impact of SDE on weather and climate during late spring and early summer, two sets of NASA GEOS-5 model simulations with and without SDE are conducted. Results show that SDE-induced surface heating is particularly pronounced in Eurasian regions where significant depositions of dust transported from the North African deserts, and black carbon from biomass burning from Asia and Europe occur. In these regions, the surface heating due to SDE increases surface skin temperature by 3-6 degrees Kelvin near the snowline in spring. Surface energy budget analysis indicates that SDE-induced excess heating is associated with a large increase in surface evaporation, subsequently leading to a significant reduction in soil moisture, and increased risks of drought and heat waves in late spring to early summer. Overall, we find that rainfall deficit combined with SDE-induced dry soil in spring provide favorable condition for summertime heat waves over large regions of Eurasia. Increased frequency of summer heat waves with SDE and the region of maximum increase in heat-wave frequency are found along the snow line, providing evidence that early snowmelt by SDE may increase the risks of extreme summer heat wave. Our results suggest that climate models that do not include SDE may significantly underestimate the effect of global warming over extra-tropical continental regions.

The physical properties of black carbon and other light-absorbing material emitted from prescribed fires in the United States

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Kreidenweis, S. M.; Yokelson, R. J.; Sullivan, A. P.; Lee, T.; Collett, J. L.; Fortner, E.; Onasch, T. B.; Akagi, S. K.; Taylor, J.; Coe, H.

2012-12-01

Black carbon (BC) aerosol emitted from fires absorbs light, leading to visibility degradation as well as regional and global climate impacts. Fires also emit a wide range of trace gases and particulates that can interact with emitted BC and alter its optical properties and atmospheric lifetime. Non-BC particulate species emitted by fires can also scatter and absorb light, leading to additional effects on visibility. Recent work has shown that certain organic species can absorb light strongly at shorter wavelengths, giving it a brown or yellow color. This material has been classified as brown carbon, though it is not yet well defined. Land managers must find a balance between the negative impacts of prescribed fire emissions on visibility and air quality and the need to prevent future catastrophic wildfire as well as manage ecosystems for habitat restoration or other purposes. This decision process requires accurate assessments of the visibility impacts of fire emissions, including BC and brown carbon, which in turn depend on their optical properties. We present recent laboratory and aircraft measurements of black carbon and aerosol optical properties emitted from biomass burning. All measurement campaigns included a single particle soot photometer (SP2) instrument capable of providing size-resolved measurements of BC mass and number distributions and mixing state, which are needed to separate the BC and brown carbon contributions to total light absorption. The laboratory experiments also included a three-wavelength photoacoustic spectrometer that provided accurate measurements of aerosol light absorption. The laboratory systems also characterized emissions after they had been treated with a thermal denuder to remove semi-volatile coatings, allowing an assessment of the role of non-BC coatings on bulk aerosol optical properties. Emissions were also aged in an environmental smog chamber to examine the role of secondary aerosol production on aerosol optical properties.

Current Status of Aerosol Retrievals from TOMS

NASA Technical Reports Server (NTRS)

Torres, O.; Herman, J. R.; Bhartia, P. K.; Ginoux, P.

1999-01-01

Properties of atmospheric aerosols over all land and water surfaces are retrieved from TOMS measurements of backscattered radiances. The TOMS technique, uses observations at two wavelengths. In the near ultraviolet (330-380 nm) range, where the effects of gaseous absorption are negligible. The retrieved properties are optical depth and a measure of aerosol absorptivity, generally expressed as single scattering albedo. The main sources of error of the TOMS aerosol products are sub-pixel cloud contamination and uncertainty on the height above the surface of UV-absorbing aerosol layers. The first error source is related to the large footprint (50 x 50 km at nadir) of the sensor, and the lack of detection capability of sub-pixel size clouds. The uncertainty associated with the height of the absorbing aerosol layers, on the other hand, is related to the pressure dependence of the molecular scattering process, which is the basis of the near-UV method of absorbing aerosol detection. The detection of non-absorbing aerosols is not sensitive to aerosol layer height. We will report on the ongoing work to overcome both of these difficulties. Coincident measurements of high spatial resolution thermal infrared radiances are used to address the cloud contamination issue. Mostly clear scenes for aerosol retrieval are selected by examining the spatial homogeneity of the IR radiance measurements within a TOMS pixel. The approach to reduce the uncertainty associated with the height of the aerosol layer by making use of a chemical transport model will also be discussed.

Stratospheric aerosols and climatic change

NASA Technical Reports Server (NTRS)

Toon, O. B.; Pollack, J. B.

1978-01-01

Stratospht1ic sulfuric acid particles scatter and absorb sunlight and they scatter, absorb and emit terrestrial thermal radiation. These interactions play a role in the earth's radiation balance and therefore affect climate. The stratospheric aerosols are perturbed by volcanic injection of SO2 and ash, by aircraft injection of SO2, by rocket exhaust of Al2O3 and by tropospheric mixing of particles and pollutant SO2 and COS. In order to assess the effects of these perturbations on climate, the effects of the aerosols on the radiation balance must be understood and in order to understand the radiation effects the properties of the aerosols must be known. The discussion covers the aerosols' effect on the radiation balance. It is shown that the aerosol size distribution controls whether the aerosols will tend to warm or cool the earth's surface. Calculations of aerosol properties, including size distribution, for various perturbation sources are carried out on the basis of an aerosol model. Calculations are also presented of the climatic impact of perturbed aerosols due to volcanic eruptions and Space Shuttle flights.

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.

Molecular-Size-Separated Brown Carbon Absorption for Biomass-Burning Aerosol at Multiple Field Sites.

PubMed

Di Lorenzo, Robert A; Washenfelder, Rebecca A; Attwood, Alexis R; Guo, Hongyu; Xu, Lu; Ng, Nga L; Weber, Rodney J; Baumann, Karsten; Edgerton, Eric; Young, Cora J

2017-03-21

Biomass burning is a known source of brown carbon aerosol in the atmosphere. We collected filter samples of biomass-burning emissions at three locations in Canada and the United States with transport times of 10 h to >3 days. We analyzed the samples with size-exclusion chromatography coupled to molecular absorbance spectroscopy to determine absorbance as a function of molecular size. The majority of absorption was due to molecules >500 Da, and these contributed an increasing fraction of absorption as the biomass-burning aerosol aged. This suggests that the smallest molecular weight fraction is more susceptible to processes that lead to reduced light absorption, while larger-molecular-weight species may represent recalcitrant brown carbon. We calculate that these large-molecular-weight species are composed of more than 20 carbons with as few as two oxygens and would be classified as extremely low volatility organic compounds (ELVOCs).

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

Secondary brown carbon - Formation of light-absorbing compounds in atmospheric particulates from selected dicarbonyls and amines

NASA Astrophysics Data System (ADS)

Kampf, Christopher; Filippi, Alexander; Hoffmann, Thorsten

2015-04-01

One of the main open questions regarding organic compounds in atmospheric chemistry today is related to the formation of optically-active compounds and the occurrence of so called brown carbon (Andreae and Gelencsér, 2006). While organic compounds in ambient fine particles for decades have been assumed to not absorb solar radiation, thus resulting in a net cooling effect on climate (IPCC, 2007), it is now generally accepted that a continuum of light-absorbing carbonaceous species is present in fine aerosols (Pöschl, 2003). In this study, light-absorbing compounds from reactions between dicarbonyl compounds, i.e., glyoxal, methylglyoxal, acetylacetone, 2,3-butanedione, 2,5-hexanedione, and glutaraldehyde, and amine species, i.e., ammonia and glycine, were investigated at atmospherically relevant concentrations in bulk solution experiments mimicking atmospheric particulates. Product analyses were performed using UV/Vis spectrophotometry and (ultra) high performance liquid chromatography coupled to diode array detection and ion trap mass spectrometry (HPLC-DAD-ESI-MS/MS), as well as ultra-high resolution (Orbitrap) mass spectrometry (UHPLC-ESI-HRMS/MS). We demonstrate that light-absorbing compounds are formed from a variety of atmospherically relevant dicarbonyls via particle phase reactions with amine nucleophiles. Single dicarbonyl and mixed dicarbonyl experiments were performed and products were analyzed. The reaction products are suggested to be cyclic nitrogen containing compounds such as imidazoles or dihydropyridines as well as open chain compounds resulting from aldol condensation reactions. Further, the reactive turnover was found to be higher at increasing pH values. The aforementioned processes may be of higher relevance in regions with high aerosol pH, e.g., resulting from high ammonia emissions as for example in northern India (Clarisse et al., 2009). References Andreae, M.O., and Gelencsér, A. (2006): Black carbon or brown carbon? The nature of light-absorbing

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes During Boreal Spring and Summer

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, M. K.; Kim, K. M.; Chin, Mian

2005-01-01

Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer

NASA Technical Reports Server (NTRS)

Lau, William K. M.; Kim, M. K.; Chin, Mian; Kim, K. M.

2005-01-01

Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol

Modeled Response of Greenland Climate to the Presence of Biomass Burning-Based Absorbing Aerosols in the Atmosphere and Snow

NASA Astrophysics Data System (ADS)

Ward, J. L.; Flanner, M.; Bergin, M. H.; Courville, Z.; Dibb, J. E.; Polashenski, C.; Soja, A. J.; Strellis, B. M.; Thomas, J. L.

2016-12-01

Combustion of biomass material results in the emission of microscopic particles, some of which absorb incoming solar radiation. Including black carbon (BC), these absorbing species can affect regional climate through changes in the local column energy budgets, cloud direct and indirect effects, and atmospheric dynamical processes. The cryosphere, which consists of both snow and ice, is unusually susceptible to changes in radiation due to its characteristically high albedo. As the largest element of the cryosphere in the Northern Hemisphere, the Greenland Ice Sheet (GrIS) covers most of Greenland's terrestrial surface and, if subjected to the increased presence of light-absorbing impurities, could experience enhanced melt. A particularly enhanced melt episode of the GrIS occurred during July 2012; at the same time, large-scale biomass burning events were observed in Eurasia and North America. Observations showed that, at the same time, single-scattering albedo (SSA) was lower than average while aerosol optical depth (AOD) was high for the Greenland region. In this study, we apply idealized climate simulations to analyze how various aspects of Greenland's climate are affected by the enhanced presence of particulate matter in the atmospheric and on the surface of the GrIS. We employ the Community Earth System Model (CESM) with prescribed sea surface temperatures and active land and atmospheric components. Using four sets of modeling experiments, we perturb 1) only AOD, 2) only SSA, 3) mass mixing ratios of BC and dust in snow, and 4) both AOD and in-snow impurity concentrations. The chosen values for each of these modeling experiments are based on field measurements taken in 2011 (AOD, SSA) and the summers of 2012-2014 (mass mixing ratios of BC and dust). Comparing the results of these experiments provides information on how the overall climate of Greenland could be affected by large biomass burning events.

Multi-wavelength aerosol light absorption measurements in the Amazon rainforest

NASA Astrophysics Data System (ADS)

Saturno, Jorge; Chi, Xuguang; Pöhlker, Christopher; Morán, Daniel; Ditas, Florian; Massabò, Dario; Prati, Paolo; Rizzo, Luciana; Artaxo, Paulo; Andreae, Meinrat

2015-04-01

The most important light-absorbing aerosol is black carbon (BC), which is emitted by incomplete combustion of fossil fuels and biomass. BC is considered the second anthropogenic contributor to global warming. Beyond BC, other aerosols like some organics, dust, and primary biological aerosol particles are able to absorb radiation. In contrast to BC, the light absorption coefficient of these aerosols is wavelength dependent. Therefore, multi-wavelength measurements become important in environments where BC is not the predominant light-absorbing aerosol like in the Amazon. The Amazon Tall Tower Observatory (ATTO) site is located in the remote Amazon rainforest, one of the most pristine continental sites in the world during the wet season. In the dry season, winds coming from the southern hemisphere are loaded with biomass burning aerosol particles originated by farming-related deforestation. BC and aerosol number concentration data from the last two years indicate this is the most polluted period. Two different techniques have been implemented to measure the light absorption at different wavelengths; one of them is the 7-wavelengths Aethalometer, model AE30, an instrument that measures the light attenuation on a filter substrate and requires multiple scattering and filter-loading corrections to retrieve the light absorption coefficient. The other method is an offline technique, the Multi-Wavelength Absorbance Analysis (MWAA), which is able to measure reflectance and absorbance by aerosols collected on a filter and, by means of a radiative model, can retrieve the light absorption coefficient. Filters collected during May-September 2014, comprehending wet-to-dry transition and most of the dry season, were analyzed. The results indicate that the Absorption Ångström Exponent (AAE), a parameter that is directly proportional to the wavelength dependence of the aerosol light absorption, is close to 1.0 during the transition period and slightly decreases in the beginning of

Experiment to Characterize Aircraft Volatile Aerosol and Trace-Species Emissions (EXCAVATE)

NASA Technical Reports Server (NTRS)

Anderson, B. E.; Branham, H.-S.; Hudgins, C. H.; Plant, J. V.; Ballenthin, J. O.; Miller, T. M.; Viggiano, A. A.; Blake, D. R.; Boudries, H.; Canagaratna, M.

2005-01-01

The Experiment to Characterize Aircraft Volatile and Trace Species Emissions (EXCAVATE) was conducted at Langley Research Center (LaRC) in January 2002 and focused upon assaying the production of aerosols and aerosol precursors by a modern commercial aircraft, the Langley B757, during ground-based operation. Remaining uncertainty in the postcombustion fate of jet fuel sulfur contaminants, the need for data to test new theories of particle formation and growth within engine exhaust plumes, and the need for observations to develop air quality models for predicting pollution levels in airport terminal areas were the primary factors motivating the experiment. NASA's Atmospheric Effects of Aviation Project (AEAP) and the Ultra Effect Engine Technology (UEET) Program sponsored the experiment which had the specific objectives of determining ion densities; the fraction of fuel S converted from S(IV) to S(VI); the concentration and speciation of volatile aerosols and black carbon; and gas-phase concentrations of long-chain hydrocarbon and PAH species, all as functions of engine power, fuel composition, and plume age.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

NASA Astrophysics Data System (ADS)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Disturbance of light-absorbing aerosols on the albedo in a winter snowpack of Central Tibet.

PubMed

Ming, Jing; Wang, Pengling; Zhao, Shuyu; Chen, Pengfei

2013-08-01

A field observation on the albedo of the snowpack in Central Tibet was conducted in the Nam Co region in the winter of 2011. Snow properties, including grain size and density, were measured in the field, and surface-layer snow samples (down to 5 cm) were collected. The average concentrations of black carbon and dust were 72 ppbm (close to that in the glaciers of Mt. Nyainqentanglha) and 120 ppmm, respectively. Inverse trends were found to exist between the albedo of the snowpack and light-absorbing aerosols (LAAs) as well as grain size growth. Modeling showed that black carbon, dust, and grain growth in the winter snowpack can reduce the broadband albedo by 11%, 28%, and 61%, respectively.

Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region

DOE PAGES

Manoharan, Vani Starry; Kotamarthi, R.; Feng, Yan; ...

2014-02-03

Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by largermore » particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Furthermore, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.« less

Photochemical Cycling of Humic-Like Substances in Atmospheric Aerosols

NASA Astrophysics Data System (ADS)

Rincon, A. G.; Guzman, M. I.; Hoffmann, M. R.; Colussi, A. J.

2007-12-01

Colored, humic-like substances (HULIS) arising from the biodegradation of organic detritus are widespread in natural surface waters, where they ultimately undergo solar photolysis into small alpha-dicarbonylic species, such as glyoxal, glyoxylic and pyruvic acids. Diversely generated and chemically dissimilar HULIS are also found in the atmospheric aerosol. How are significant levels of colored HULIS produced and sustained in the concentrated aerosol phase under intense solar irradiation? Here, this issue is tackled by investigating the solar photolysis of aqueous pyruvic acid (PA) solutions at concentrations representative of the atmospheric aerosol using UV-absorption, high resolution electrospray mass, and nuclear magnetic resonance spectrometries. Under such conditions, PA is not photodegraded but yields polyfunctional polymers, whose mass and UV-absorption spectra remain unaffected after 3, 8 and 22 h photolysis. Unless diluted, these polymers undergo condensation/polymerization in the post-photolysis period into mass < 700 Da species that absorb in the visible, and are bleached upon resuming irradiation. The re- photolyzed solutions recover the mass and UV-absorption spectra of first photolyzed solutions. Whereas initial pH has no effect on the mechanism of reaction, ammonium bisulfate, a major component of the aerosol, markedly influences these processes. These findings suggest that the chemical identity and concentration levels of complex organic substances in the aerosol are the result of dynamic photochemical processing in the condensed phase.

Characterization of Wildfire-Induced Aerosol Emissions From the Maritime Continent Peatland and Central African Dry Savannah with MISR and CALIPSO Aerosol Products

NASA Astrophysics Data System (ADS)

Lee, Huikyo; Jeong, Su-Jong; Kalashnikova, Olga; Tosca, Mika; Kim, Sang-Woo; Kug, Jong-Seong

2018-03-01

Aerosol plumes from wildfires affect the Earth's climate system through regulation of the radiative budget and clouds. However, optical properties of aerosols from individual wildfire smoke plumes and their resultant impact on regional climate are highly variable. Therefore, there is a critical need for observations that can constrain the partitioning between different types of aerosols. Here we present the apparent influence of regional ecosystem types on optical properties of wildfire-induced aerosols based on remote sensing observations from two satellite instruments and three ground stations. The independent observations commonly show that the ratio of the absorbing aerosols is significantly lower in smoke plumes from the Maritime Continent than those from Central Africa, so that their impacts on regional climate are different. The observed light-absorbing properties of wildfire-induced aerosols are explained by dominant ecosystem types such as wet peatlands for the Maritime Continent and dry savannah for Central Africa, respectively. These results suggest that the wildfire-aerosol-climate feedback processes largely depend on the terrestrial environments from which the fires originate. These feedbacks also interact with climate under greenhouse warming. Our analysis shows that aerosol optical properties retrieved based on satellite observations are critical in assessing wildfire-induced aerosols forcing in climate models. The optical properties of carbonaceous aerosol mixtures used by state-of-the-art chemistry climate models may overestimate emissions for absorbing aerosols from wildfires over the Maritime Continent.

Seasonality of major aerosol species and their transformations in Cairo megacity

NASA Astrophysics Data System (ADS)

Favez, Olivier; Cachier, Hélène; Sciare, Jean; Alfaro, Stéphane C.; El-Araby, Tarek M.; Harhash, Maha A.; Abdelwahab, Magdy M.

Bulk aerosols sampled on a weekly basis at two Cairo (Egypt) urban sites from January 2003 to May 2006 were analysed for their chemical composition of major aerosol species (elemental carbon, water soluble/insoluble organic carbon, nitrate, sulphate, ammonium, chloride, sodium and calcium). Data subsequently obtained constitute one of the longest and more detailed dataset related to Cairo aerosols, and offer the opportunity to investigate seasonal trends. Dust aerosols (derived from calcium measurements) displayed maximum concentrations in spring and winter, due to frequent dust storms, but also high background concentration levels (˜50 μg m -3) all year long. Within these particles, about 40% on average of Ca 2+ was found to be associated with SO 42-, NO 3- and/or Cl -, pointing out "dust anthropization" processes and their subsequent climatic impact on a regional scale. Seasonal variations of non-dust aerosols, equally distributed between carbonaceous aerosols and ions, were also observed, with concentrations of the order of 100 μg m -3 in autumn and winter, and of 60 μg m -3 in spring and summer. High concentration levels of non-sea-salt chloride (up to 15 μg m -3 on a monthly basis), likely of industrial origin, were observed in autumn and winter. During the autumn "Black Cloud" event, biomass burning aerosols originating from rice straw burning in the Nile Delta have shown to account for 12%, 35% and 50% of Cairo EC, WIOC and WSOC mass concentrations, respectively. Finally, relatively low WSOC/OC ratios (˜1/3) were obtained all the year long, calling for more investigation on the water-solubility of organic aerosols originating from the burning of agricultural waste, and on that of secondary organic aerosols formed in dry urban atmospheres.

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.

Daytime variations of absorbing aerosols above clouds in the southeast Atlantic

NASA Astrophysics Data System (ADS)

Chang, Y. Y.; Christopher, S. A.

2016-12-01

The daytime variation of aerosol optical depth (AOD) above maritime stratocumulus clouds in the southeast Atlantic is investigated by merging geostationary data from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) with NASA A-Train data sets. SEVIRI's 15-minute above cloud AOD and below aerosol cloud optical depth (COD) retrieval provides the opportunity to assess their direct radiative forcing using actual cloud and aerosol properties instead of using fixed values from polar-orbiting measurements. The impact of overlying aerosols above clouds on the cloud mask products are compared with active spaceborne lidar to examine the performance of the product. Uncertainty analyses of aerosol properties on the estimation of optical properties and radiative forcing are addressed.

Evaluation of species-dependent detection efficiencies in the aerosol mass spectrometer

USDA-ARS?s Scientific Manuscript database

Mass concentrations of chemical species calculated from the aerosol mass spectrometer (AMS) depend on two factors: particle collection efficiency (CE) and relative ionization efficiency (RIE, relative to the primary calibrant ammonium nitrate). While previous studies have characterized CE, RIE is re...

A new approach to correct for absorbing aerosols in OMI UV

NASA Astrophysics Data System (ADS)

Arola, A.; Kazadzis, S.; Lindfors, A.; Krotkov, N.; Kujanpää, J.; Tamminen, J.; Bais, A.; di Sarra, A.; Villaplana, J. M.; Brogniez, C.; Siani, A. M.; Janouch, M.; Weihs, P.; Webb, A.; Koskela, T.; Kouremeti, N.; Meloni, D.; Buchard, V.; Auriol, F.; Ialongo, I.; Staneck, M.; Simic, S.; Smedley, A.; Kinne, S.

2009-11-01

Several validation studies of surface UV irradiance based on the Ozone Monitoring Instrument (OMI) satellite data have shown a high correlation with ground-based measurements but a positive bias in many locations. The main part of the bias can be attributed to the boundary layer aerosol absorption that is not accounted for in the current satellite UV algorithms. To correct for this shortfall, a post-correction procedure was applied, based on global climatological fields of aerosol absorption optical depth. These fields were obtained by using global aerosol optical depth and aerosol single scattering albedo data assembled by combining global aerosol model data and ground-based aerosol measurements from AERONET. The resulting improvements in the satellite-based surface UV irradiance were evaluated by comparing satellite and ground-based spectral irradiances at various European UV monitoring sites. The results generally showed a significantly reduced bias by 5-20%, a lower variability, and an unchanged, high correlation coefficient.

Possible combined influences of absorbing aerosols and anomalous atmospheric circulation on summertime diurnal temperature range variation over the middle and lower reaches of the Yangtze River

NASA Astrophysics Data System (ADS)

Cai, Jiaxi; Guan, Zhaoyong; Ma, Fenhua

2016-12-01

Based on the temperature data from the China Meteorological Administration, NCEP-NCAR reanalysis data, and the TOMS Aerosol Index (AI), we analyze the variations in the summertime diurnal temperature range (DTR) and temperature maxima in the middle and lower reaches of the Yangtze River (MLRYR) in China. The possible relationships between the direct warming effect of the absorbing aerosol and temperature variations are further investigated, although with some uncertainties. It is found that the summertime DTR exhibits a decreasing trend over the most recent 50 years, along with a slight increasing tendency since the 1980s. The trend of the maximum temperature is in agreement with those of the DTR and the absorbing aerosols. To investigate the causes of the large anomalies in the temperature maxima, composite analyses of the circulation anomalies are performed. When anomalous AI and anomalous maximum temperature over the MLRYR have the same sign, an anomalous circulation with a quasi-barotropic structure occurs there. This anomalous circulation is modulated by the Rossby wave energy propagations from the regions northwest of the MLRYR and influences the northwestern Pacific subtropical high over the MLRYR. In combination with aerosols, the anomalous circulation may increase the maximum temperature in this region. Conversely, when the anomalous AI and anomalous maximum temperature in the MLRYR have opposite signs, the anomalous circulation is not equivalently barotropic, which possibly offsets the warming effect of aerosols on the maximum temperature changes in this region. These results are helpful for a better understanding of the DTR changes and the occurrences of temperature extremes in the MLRYR region during boreal summer.

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

Inferring Absorbing Organic Carbon Content from AERONET Data

NASA Technical Reports Server (NTRS)

Arola, A.; Schuster, G.; Myhre, G.; Kazadzis, S.; Dey, S.; Tripathi, S. N.

2011-01-01

Black carbon, light-absorbing organic carbon (often called brown carbon) and mineral dust are the major light-absorbing aerosols. Currently the sources and formation of brown carbon aerosol in particular are not well understood. In this study we estimated globally the amount of light absorbing organic carbon and black carbon from AERONET measurements. We find that the columnar absorbing organic carbon (brown carbon) levels in biomass burning regions of South-America and Africa are relatively high (about 15-20 magnesium per square meters during biomass burning season), while the concentrations are significantly lower in urban areas in US and Europe. However, we estimated significant absorbing organic carbon amounts from the data of megacities of newly industrialized countries, particularly in India and China, showing also clear seasonality with peak values up to 30-35 magnesium per square meters during the coldest season, likely caused by the coal and biofuel burning used for heating. We also compared our retrievals with the modeled organic carbon by global Oslo CTM for several sites. Model values are higher in biomass burning regions than AERONET-based retrievals, while opposite is true in urban areas in India and China.

Effects of Absorbing Aerosols on Accelerated Melting of Snowpack in the Hindu-Kush-Himalayas-Tibetan Plateau Region

NASA Technical Reports Server (NTRS)

Lau, William K.; Kyu-Myong, Kim; Yasunari, Teppei; Gautam, Ritesh; Hsu, Christina

2011-01-01

The impacts of absorbing aerosol on melting of snowpack in the Hindu-Kush-Himalayas-Tibetan Plateau (HKHT) region are studied using in-situ, satellite observations, and GEOS-5 GCM. Based on atmospheric black carbon measurements from the Pyramid observation ( 5 km elevation) in Mt. Everest, we estimate that deposition of black carbon on snow surface will give rise to a reduction in snow surface albedo of 2- 5 %, and an increased annual runoff of 12-34% for a typical Tibetan glacier. Examination of satellite reflectivity and re-analysis data reveals signals of possible impacts of dust and black carbon in darkening the snow surface, and accelerating spring melting of snowpack in the HKHT, following a build-up of absorbing aerosols in the Indo-Gangetic Plain. Results from GCM experiments show that 8-10% increase in the rate of melting of snowpack over the western Himalayas and Tibetan Plateau can be attributed to the elevated-heat-pump (EHP) feedback effect, initiated from the absorption of solar radiation by dust and black carbon accumulated to great height ( 5 km) over the Indo-Gangetic Plain and Himalayas foothills in the pre-monsoon season (April-May). The accelerated melting of the snowpack is enabled by an EHP-induced atmosphere-land-snowpack positive feedback involving a) orographic forcing of the monsoon flow by the complex terrain, and thermal forcing of the HKHT region, leading to increased moisture, cloudiness and rainfall over the Himalayas foothills and northern India, b) warming of the upper troposphere over the Tibetan Plateau, and c) an snow albedo-temperature feedback initiated by a transfer of latent and sensible heat from a warmer atmosphere over the HKHT to the underlying snow surface. Results from ongoing modeling work to assess the relative roles of EHP vs. snow-darkening effects on accelerated melting of snowpack in HKHT region will also be discussed.

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.

Synergic use of TOMS and Aeronet Observations for Characterization of Aerosol Absorption

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.; Dubovik, O.; Holben, B.; Siniuk, A.

2003-01-01

The role of aerosol absorption on the radiative transfer balance of the earth-atmosphere system is one of the largest sources of uncertainty in the analysis of global climate change. Global measurements of aerosol single scattering albedo are, therefore, necessary to properly assess the radiative forcing effect of aerosols. Remote sensing of aerosol absorption is currently carried out using both ground (Aerosol Robotic Network) and space (Total Ozone Mapping Spectrometer) based observations. The satellite technique uses measurements of backscattered near ultraviolet radiation. Carbonaceous aerosols, resulting from the combustion of biomass, are one of the most predominant absorbing aerosol types in the atmosphere. In this presentation, TOMS and AERONET retrievals of single scattering albedo of carbonaceous aerosols, are compared for different environmental conditions: agriculture related biomass burning in South America and Africa and peat fires in Eastern Europe. The AERONET and TOMS derived aerosol absorption information are in good quantitative agreement. The most absorbing smoke is detected over the African Savanna. Aerosol absorption over the Brazilian rain forest is less absorbing. Absorption by aerosol particles resulting from peat fires in Eastern Europe is weaker than the absorption measured in Africa and South America. This analysis shows that the near UV satellite method of aerosol absorption characterization has the sensitivity to distinguish different levels of aerosol absorption. The analysis of the combined AERONET-TOMS observations shows a high degree of synergy between satellite and ground based observations.

Regional Aerosol Forcing over India: Preliminary Results from the South West Asian Aerosol-Monsoon Interactions (SWAAMI) Aircraft Experiment

NASA Astrophysics Data System (ADS)

Morgan, W.; Brooks, J.; Fox, C.; Haslett, S.; Liu, D.; Kompalli, S. K.; Pathak, H.; Manoj, M. R.; Allan, J. D.; Haywood, J. M.; Highwood, E.; Langridge, J.; Nanjundaiah, R. S.; Krishnamoorthy, K.; Babu, S. S.; Satheesh, S. K.; Turner, A. G.; Coe, H.

2016-12-01

Aerosol particles from multiple sources across the Indian subcontinent build up to form a dense and extensive haze across the region in advance of the monsoon. These aerosols are thought to perturb the regional radiative balance and hydrological cycle, which may have a significant impact on the monsoon circulation, as well as influencing the associated cloud and rainfall of the system. However the nature and magnitude of such impacts are poorly understood or constrained. Major uncertainties relevant to the regional aerosol burden include its vertical distribution, the relative contribution of different pollution sources and natural emissions and the role of absorbing aerosol species (black carbon and mineral dust). The South West Asian Aerosol-Monsoon Interactions (SWAAMI) project sought to address these major uncertainties by conducting an airborne experiment during June/July 2016 on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft. Based out of Lucknow in the), The aircraft conducted multiple flights from Lucknow in the heart of the Indo-Gangetic Plain (IGP) in advance of the monsoon and during the onset phase. The spatial and vertical distribution of aerosol was evaluated across northern India, encompassing drier desert-like regions to the west, heavily populated urban and industrial centres over the IGP and air masses in outflow regions to the south-east towards the Bay of Bengal. Principal measurements included aerosol chemical composition using an Aerodyne Aerosol Mass Spectrometer and a DMT Single Particle Soot Photometer, alongside a Leosphere backscatter LIDAR. Sulphate was a major contributor to the aerosol burden across India, while the organic aerosol was elevated and more dominant over the most polluted regions of the IGP. Substantial aerosol concentrations were frequently observed up to altitudes of approximately 6km, with notable changes in aerosol chemical and physical properties when comparing different

Variability of oxygen radical absorbance capacity (ORAC) in different animal species.

PubMed

Ninfali, P; Aluigi, G

1998-11-01

The oxygen radical absorbance capacity (ORAC) was measured both in whole (ORAC-T) and deproteinized (ORAC-AS) plasma samples of human, pig, cow, rabbit, dog, cat, sheep, horse, dolphin, turkey, guinea-hen and chicken. In the 12 species, ORAC-T data, expressed as micromoles of peroxyl radicals trapped by 11 of sample, were found scattered between 8,600 and 23,000 micromol/l. The species with the highest ORAC-T values were cat among mammals and chicken among avies. ORAC-AS values ranged between 600 and 2000 micromol/l, with the highest values found in dolphin and sheep among mammals, while chicken was first among avies. In the 12 species, the relative contribution of ORAC-AS in relation to ORAC-T ranged from 5% to 20%. Protein SH-groups and uric acid were measured in plasma of all species, but no significant correlation was found between thiols and ORAC-T values or between uric acid and ORAC-AS values. Our results show that: (1) the ORAC method is reproducible and sensitive enough to be used in the comparison of the peroxyl-radical absorbance capacity of protein and non-protein plasma components in different animal species; (2) both in mammals and in avies, there is a deep intra-class heterogeneity of ORAC-T and ORAC-AS values; (3) by considering most species, plasma proteins and lipoproteins account for about 85-90% of the overall peroxyl-radical trapping capacity. In the dolphin only, the protein contribution decreases to 80%; (4) uric acid accounts for about one-half of the ORAC-AS value in human, guinea-hen and for about one-third in chicken, while it provides a very limited contribution in other species. We conclude that species with the highest ORAC-T, like cat and chicken, or with the highest ORAC-AS, like dolphin, are interesting models to study the reasons of such a marked antioxidant defense in the plasma.

A Global Data Assimilation System for Atmospheric Aerosol

NASA Technical Reports Server (NTRS)

daSilva, Arlindo

1999-01-01

We will give an overview of an aerosol data assimilation system which combines advances in remote sensing of atmospheric aerosols, aerosol modeling and data assimilation methodology to produce high spatial and temporal resolution 3D aerosol fields. Initially, the Goddard Aerosol Assimilation System (GAAS) will assimilate TOMS, AVHRR and AERONET observations; later we will include MODIS and MISR. This data assimilation capability will allows us to integrate complementing aerosol observations from these platforms, enabling the development of an assimilated aerosol climatology as well as a global aerosol forecasting system in support of field campaigns. Furthermore, this system provides an interactive retrieval framework for each aerosol observing satellites, in particular TOMS and AVHRR. The Goddard Aerosol Assimilation System (GAAS) takes advantage of recent advances in constituent data assimilation at DAO, including flow dependent parameterizations of error covariances and the proper consideration of model bias. For its prognostic transport model, GAAS will utilize the Goddard Ozone, Chemistry, Aerosol, Radiation and Transport (GOCART) model developed at NASA/GSFC Codes 916 and 910.3. GOCART includes the Lin-Rood flux-form, semi-Langrangian transport model with parameterized aerosol chemistry and physical processes for absorbing (dust and black carbon) and non-absorbing aerosols (sulfate and organic carbon). Observations and model fields are combined using a constituent version of DAO's Physical-space Statistical Analysis System (PSAS), including its adaptive quality control system. In this talk we describe the main components of this assimilation system and present preliminary results obtained by assimilating TOMS data.

Applications of broadband cavity enhanced spectroscopy for measurements of trace gases and aerosols

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Brown, S. S.; Dube, W. P.; Flores, J. M.; Langford, A. O.; Min, K. E.; Rudich, Y.; Stutz, J.; Wagner, N.; Young, C.; Zarzana, K. J.

2015-12-01

Broadband cavity enhanced spectroscopy (BBCES) uses a broadband light source, optical cavity, and multichannel detector to measure light extinction with high sensitivity. This method differs from cavity ringdown spectroscopy, because it uses an inexpensive, incoherent light source and allows optical extinction to be determined simultaneously across a broad wavelength region.Spectral fitting methods can be used to retrieve multiple absorbers across the observed wavelength region. We have successfully used this method to measure glyoxal (CHOCHO), nitrous acid (HONO), and nitrogen dioxide (NO2) from ground-based and aircraft-based sampling platforms. The detection limit (2-sigma) in 5 s for retrievals of CHOCHO, HONO and NO2 is 32, 250 and 80 parts per trillion (pptv).Alternatively, gas-phase absorbers can be chemically removed to allow the accurate determination of aerosol extinction. In the laboratory, we have used the aerosol extinction measurements to determine scattering and absorption as a function of wavelength. We have deployed a ground-based field instrument to measure aerosol extinction, with a detection limit of approximately 0.2 Mm-1 in 1 min.BBCES methods are most widely used in the near-ultraviolet and visible spectral region. Recently, we have demonstrated measurements at 315-350 nm for formaldehyde (CH2O) and NO2. Extending the technique further into the ultraviolet spectral region will allow important additional measurements of trace gas species and aerosol extinction.

Using OMI Observations to Measure Aerosol Absorption of Biomass Burning Aerosols Above Clouds

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, P. K.; Jethva, Hiren

2011-01-01

The presence of absorbing aerosol layers above clouds is unambiguously detected by the TOMS/OMI UV Aerosol Index (AI) that uses satellite observations at two near-UV channels. A sensitivity study using radiative transfer calculations shows that the AI signal of resulting from the presence of aerosols above clouds is mainly driven by the aerosol absorption optical depth and the optical depth of the underlying cloud. Based on these results, an inversion algorithm has been developed to retrieve the aerosol optical depth (AOD) of aerosol layers above clouds. In this presentation we will discuss the sensitivity analysis, describe the retrieval approach, and present results of applications of the retrieval method to OMI observations over the South Atlantic Ocean. Preliminary error analyses, to be discussed, indicate that the AOD can be underestimated (up to -30%) or overestimated (up to 60%) depending on algorithmic assumptions.

Effects of aerosol species on atmospheric visibility in Kaohsiung City, Taiwan

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

Chang-Gai Lee; Chung-Shin Yuan; Jui-Cheng Chang

2005-07-01

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During the study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition ofmore » Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 {mu}m, corresponding with the wavelength region of visible light, which accounted for {approximately} 72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH{sub 4}){sup 2}SO{sub 4}, NH{sub 4}NO{sub 3}, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein. 35 refs., 10 figs., 4 tabs.« less

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

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

NASA Astrophysics Data System (ADS)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

Study of atmospheric scattering and absorbing aerosols at 550 nm over nearby western Indian tropical sites of Thar Desert effected region

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

Vyas, B. M., E-mail: bmvyas@yahoo.com; Saxenna, Abhishek; Panwar, Chhagan

The first time experimental results based on spaced satellite observations of different kinds of aerosols properties have been described over two different contrast environmental conditions locations in western tropical Indian region specifically first at Jaisalmer (26.90°N, 69.90°E, 220 m above mean sea level (amsl)) located in central Thar dessert vicinity of western Indian site over Indian Thar Desert region and another at Udaipur (24.6° N, 73.7° E, 560 m amsl) site concerning to semi-urban and semi arid place of hilly areas. The daily values of aerosols optical depth absorption at 500nm (AOD abs 500nm), aerosols optical depth extinction at 500nmmore » (AOD ext 500nm) along with aerosols optical depth at 500nmon (AOD 500nm) of eleven year period from Jan., 2004 to Dec., 2014 are basis of primary database of the present investigation. From the synthesis if the above database and the basis of rigorous statistical approach, following some of interesting facts are noted (i) larger annual monthly AOD variation of 0.93 is noted over JSM when compared to observed annual monthly change in AOD cycle, over UDP, of only 0.50 clearly indicating the more impact of desert influence activities about more than double times over JSM than UDP (ii) The higher abundance of absorbing aerosols occurrences about two time higher are seen in JSM in comparison to UDP. It indicates the clear evidence of strong optical absorption properties of useful solar mid visible wavelength at 550nm as the results of presence of more availability of dust aerosols as mineral natural type in pre-monsoon to post-monsoon over JSM which is also more predominant over JSM than the UDP region located far away from desert activity regime (iii) The greater sharing of extinction solar radiation effect on aerosols are more effective in pre-monsoon in UDP in reference to over JSM, where as in case of UDP, the aerosols effect through the scattering mechanism gradually reduce from monsoon to winter months as

Light absorption by secondary organic aerosol from α-pinene: Effects of oxidants, seed aerosol acidity, and relative humidity

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

Song, Chen; Gyawali, Madhu; Zaveri, Rahul A.

2013-10-25

It is well known that light absorption from dust and black carbon aerosols has a warming effect on climate while light scattering from sulfate, nitrate, and sea salt aerosols has a cooling effect. However, there are large uncertainties associated with light absorption and scattering by different types of organic aerosols, especially in the near-UV and UV spectral regions. In this paper, we present the results from a systematic laboratory study focused on measuring light absorption by secondary organic aerosols (SOAs) generated from dark α-pinene + O 3 and α-pinene + NO x + O 3 systems in the presence ofmore » neutral and acidic sulfate seed aerosols. Light absorption was monitored using photoacoustic spectrometers at four different wavelengths: 355, 405, 532, and 870 nm. Significant light absorption at 355 and 405 nm was observed for the SOA formed from α-pinene + O 3 + NO 3 system only in the presence of highly acidic sulfate seed aerosols under dry conditions. In contrast, no absorption was observed when the relative humidity was elevated to greater than 27% or in the presence of neutral sulfate seed aerosols. Organic nitrates in the SOA formed in the presence of neutral sulfate seed aerosols were found to be nonabsorbing, while the light-absorbing compounds are speculated to be aldol condensation oligomers with nitroxy organosulfate groups that are formed in highly acidic sulfate aerosols. Finally and overall, these results suggest that dark α-pinene + O 3 and α-pinene + NO x + O 3 systems do not form light-absorbing SOA under typical atmospheric conditions.« less

Retrieval of Aerosol Absorption Properties from Satellite Observations

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, Pawan K.; Jethva, H.; Ahn, Chang-Woo

2012-01-01

The Angstrom Absorption Exponent (AAE) is a parameter commonly used to characterize the wavelength-dependence of aerosol absorption optical depth (AAOD). It is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses multi-spectral measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measurement can be explained, using an approximations of Beer's Law (BL), as the upwelling reflectance at the cloud top attenuated by the absorption effects of the overlying aerosol layer. The upwelling reflectance at the cloud-top in an aerosol-free atmospheric column is mainly a function of cloud optical depth (COD). In the proposed method of AAE derivation, the first step is determining COD which is retrieved using a previously developed color-ratio based approach. In the second step, corrections for molecular scattering effects are applied to both the observed ad the calculated cloud reflectance terms, and the spectral AAOD is then derived by an inversion of the BL approximation. The proposed technique will be discussed in detail and application results making use of OMI multi-spectral measurements in the UV-Vis. will be presented.

Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

NASA Technical Reports Server (NTRS)

Lau, William K. M.

2006-01-01

Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called "direct effect", aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called "indirect effects", whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will

Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

NASA Technical Reports Server (NTRS)

Lau, William K. M.

2006-01-01

Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called direct effect , aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called indirect effects, whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will discuss

Measurements of SO/sub x/, NO/sub x/ and aerosol species in Bermuda

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

Wolff, G.T.; Ruthkosky, M.S.; Stroup, D.P.

1985-01-01

This paper presents a unique set of concurrent aerosol and gas measurements made in Bermuda. These measurements were made during August 1-31, 1982 and January 25-February 28, 1983. Topics discussed include the sources of these species, the transport of these species from North American and their seasonal behavior. When possible, comparisons are made with measurements made by others on Bermuda and over the adjacent North Atlantic waters.

Global and Seasonal Aerosol Optical Depths Derived From Ultraviolet Observations by Satellites (TOMS)

NASA Technical Reports Server (NTRS)

Herman, J. R.; Torres, O.

1999-01-01

It has been shown that absorbing aerosols (dust, smoke, volcanic ash) can be detected in the ultraviolet wavelengths (331 nm to 380 nm) from satellite observations (TOMS, Total Ozone Mapping Spectrometer) over both land and water. The theoretical basis for these observations and their conversions to optical depths is discussed in terms of an aerosol index AI or N-value residue (assigned positive for absorbing aerosols). The theoretical considerations show that negative values of the AI frequently represent the presence of non-absorbing aerosols (NA) in the troposphere (mostly pollution in the form of sulfates, hydrocarbons, etc., and some natural sulfate aerosols) with particle sizes near 0.1 to 0.2 microns or less. The detection of small-particle non-absorbing aerosols from the measured backscattered radiances is based on the observed wavelength dependence from Mie scattering after the background Rayleigh scattering is subtracted. The Mie scattering from larger particles, 1 micron or more (e.g., cloud water droplets) has too small a wavelength dependence to be detected by this method. In regions that are mostly cloud free, aerosols of all sizes can be seen in the single channel 380 nm or 360 nm radiance data. The most prominent Al feature observed is the strong asymmetry in aerosol amount between the Northern and Southern Hemispheres, with the large majority of NA occurring above 20degN latitude. The maximum values of non-absorbing aerosols are observed over the eastern U.S. and most of western Europe corresponding to the areas of highest industrial pollution. Annual cycles in the amount of NA are observed over Europe and North America with maxima occurring in the summer corresponding to times of minimum wind transport. Similarly, the maxima in the winter over the Atlantic Ocean occurs because of wind borne transport from the land. Most regions of the world have the maximum amount of non-absorbing aerosol in the December to January period except for the eastern

Quantifying the Aerosol Semi-Direct Effect in the NASA GEOS-5 AGCM

NASA Technical Reports Server (NTRS)

Randles, Cynthia A.; Colarco, Peter R.; daSilva, Arlindo

2011-01-01

Aerosols such as black carbon, dust, and some organic carbon species both scatter and absorb incoming solar radiation. This direct aerosol radiative forcing (DARF) redistributes solar energy both by cooling the surface and warming the atmosphere. As a result, these aerosols affect atmospheric stability and cloud cover (the semi-direct effect, or SDE). Furthermore, in regions with persistent high loadings of absorbing aerosols (e.g. Asia), regional circulation patterns may be altered, potentially resulting in changes in precipitation patterns. Here we investigate aerosol-climate coupling using the NASA Goddard Earth Observing System model version 5 (GEOS-5) atmospheric general circulation model (AGCM), in which we have implemented an online version of the Goddard Chemistry, Aerosol, Radiation and Transport (GOCART) model. GOCART includes representations of the sources, sinks, and chemical transformation of externally mixed dust, sea salt, sulfate, and carbonaceous aerosols. We examine a series of free-running ensemble climate simulations of the present-day period (2000-2009) forced by observed sea surface temperatures to determine the impact of aerosols on the model climate. The SDE and response of each simulation is determined by differencing with respect to the control simulation (no aerosol forcing). In a free-running model, any estimate of the SDE includes changes in clouds due both to atmospheric heating from aerosols and changes in circulation. To try and quantify the SDE without these circulation changes we then examine the DARF and SDE in GEOS-5 with prescribed meteorological analyses introduced by the MERRA analysis. By doing so, we are able to examine changes in model clouds that occur on shorter scales (six hours). In the GEOS-5 data assimilation system (DAS), the analysis is defined as the best estimate of the atmospheric state at any given time, and it is determined by optimally combining a first-guess short-term GCM forecast with all available

A Long-term Record of Saharan Dust Aerosol Properties from TOMS Observations: Optical Depth and Single Scattering Albedo

NASA Technical Reports Server (NTRS)

Torres, Omar; Bhartia, P. K.; Herman, J. R.; Einaudi, Franco (Technical Monitor)

2000-01-01

The interaction between the strong Rayleigh scattering in the near UV spectral region (330-380 nm) and the processes of aerosol absorption and scattering, produce a clear spectral signal in the upwelling radiance at the top of the atmosphere. This interaction is the basis of the TOMS (Total Ozone Mapping Spectrometer) aerosol retrieval technique that can be used for their characterization and to differentiate non-absorbing sulfates from strongly UV-absorbing aerosols such as mineral dust. For absorbing aerosols, the characterization is in terms of the optical depth and single scattering albedo with assumptions about the aerosol plume height. The results for non-absorbing aerosols are not dependent on plume height. Although iron compounds represent only between 5% to 8% of desert dust aerosol mass, hematite (Fe2O3) accounts for most of the near UV absorption. Because of the large ultraviolet absorption characteristic of hematite, the near UV method of aerosol sensing is especially suited for the detection and characterization of desert dust aerosols. Using the combined record of near UV measurements by the Nimbus7 (1978-1992) and Earth Probe (1996-present) TOMS instruments, a global longterm climatology of near UV optical depth and single scattering albedo has been produced. The multi-year long record of mineral aerosol properties over the area of influence of the Saharan desert, will be discussed.

Lidar remote sensing of laser-induced incandescence on light absorbing particles in the atmosphere.

PubMed

Miffre, Alain; Anselmo, Christophe; Geffroy, Sylvain; Fréjafon, Emeric; Rairoux, Patrick

2015-02-09

Carbon aerosol is now recognized as a major uncertainty on climate change and public health, and specific instruments are required to address the time and space evolution of this aerosol, which efficiently absorbs light. In this paper, we report an experiment, based on coupling lidar remote sensing with Laser-Induced-Incandescence (LII), which allows, in agreement with Planck's law, to retrieve the vertical profile of very low thermal radiation emitted by light-absorbing particles in an urban atmosphere over several hundred meters altitude. Accordingly, we set the LII-lidar formalism and equation and addressed the main features of LII-lidar in the atmosphere by numerically simulating the LII-lidar signal. We believe atmospheric LII-lidar to be a promising tool for radiative transfer, especially when combined with elastic backscattering lidar, as it may then allow a remote partitioning between strong/less light absorbing carbon aerosols.

Remote Sensing of Aerosol and Aerosol Radiative Forcing of Climate from EOS Terra MODIS Instrument

NASA Technical Reports Server (NTRS)

Kaufman, Yoram; Tanre, Didier; Remer, Lorraine; Einaudi, Franco (Technical Monitor)

2000-01-01

The recent launch of EOS-Terra into polar orbit has begun to revolutionize remote sensing of aerosol and their effect on climate. Terra has five instruments, two of them,Moderate Resolution Imaging Spectroradiometer (MODIS) and Multiangle Imaging Spectro-Radiometer (MISR) are designed to monitor global aerosol in two different complementary ways. Here we shall discuss the use of the multispectral measurements of MODIS to derive: (1) the global distribution of aerosol load (and optical thickness) over ocean and land; (2) to measure the impact of aerosol on reflection of sunlight to space; and (3) to measure the ability of aerosol to absorb solar radiation. These measurements have direct applications on the understanding of the effect of aerosol on climate, the ability to predict climate change, and on the monitoring of dust episodes and man-made pollution. Principles of remote sensing of aerosol from MODIS will be discussed and first examples of measurements from MODIS will be provided.

A contribution of black and brown carbon to the aerosol light absorption

NASA Astrophysics Data System (ADS)

Kim, Sang-Woo; Cho, Chaeyoon; Jo, Duseong; Park, Rokjin

2017-04-01

Black carbon (BC) is functionally defined as the absorbing component of atmospheric total carbonaceous aerosols and is typically dominated by soot-like elemental carbon (EC). Organic carbon (OC) has also been shown to absorb strongly at visible to UV wavelengths and the absorbing organics are referred to as brown carbon (BrC; Alexander et al., 2008). These two aerosols contribute to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer, but most optical instruments that quantify light absorption are unable to distinguish one type of absorbing aerosol from another (Moosmüller et al. 2009). In this study, we separate total aerosol absorption from these two different light absorbers from co-located simultaneous in-situ measurements, such as Continuous Soot Monitoring System (COSMOS), Continuous Light Absorption Photometer (CLAP) and Sunset EC/OC analyzer, at Gosan climate observatory, Korea. We determine the mass absorption cross-section (MAC) of BC, and then estimate the contribution of BC and BrC on aerosol light absorption, together with a global 3-D chemical transport model (GEOS-Chem) simulation. At 565 nm wavelength, BC MAC is found to be about 5.4±2.8 m2 g-1 from COSMOS and Sunset EC/OC analyzer measurements during January-May 2012. This value is similar to those from Alexander et al. (2008; 4.3 ˜ 4.8 m2 g-1 at 550 nm) and Chung et al. (2012; 5.1 m2 g-1 at 520 nm), but slightly lower than Bond and Bergstrom (2006; 7.5±1.2 m2 g-1 at 550 nm). The COMOS BC mass concentration calculated with 5.4 m2 g-1 of BC MAC shows a good agreement with thermal EC concentration, with a good slope (1.1). Aerosol absorption coefficient and BC mass concentration from COSMOS, meanwhile, are approximately 25 ˜ 30 % lower than those of CLAP. This difference can be attributable to the contribution of volatile light-absorbing aerosols (i.e., BrC). The absorption coefficient of BrC, which is determined by the difference of

Towards a Global Aerosol Climatology: Preliminary Trends in Tropospheric Aerosol Amounts and Corresponding Impact on Radiative Forcing between 1950 and 1990

NASA Technical Reports Server (NTRS)

Tegen, Ina; Koch, Dorothy; Lacis, Andrew A.; Sato, Makiko

1999-01-01

A global aerosol climatology is needed in the study of decadal temperature change due to natural and anthropogenic forcing of global climate change. A preliminary aerosol climatology has been developed from global transport models for a mixture of sulfate and carbonaceous aerosols from fossil fuel burning, including also contributions from other major aerosol types such as soil dust and sea salt. The aerosol distributions change for the period of 1950 to 1990 due to changes in emissions of SO2 and carbon particles from fossil fuel burning. The optical thickness of fossil fuel derived aerosols increased by nearly a factor of 3 during this period, with particularly strong increase in eastern Asia over the whole time period. In countries where environmental laws came into effect since the early 1980s (e.g. US and western Europe), emissions and consequently aerosol optical thicknesses did not increase considerably after 1980, resulting in a shift in the global distribution pattern over this period. In addition to the optical thickness, aerosol single scattering albedos may have changed during this period due to different trends in absorbing black carbon and reflecting sulfate aerosols. However, due to the uncertainties in the emission trends, this change cannot be determined with any confidence. Radiative forcing of this aerosol distribution is calculated for several scenarios, resulting in a wide range of uncertainties for top-of-atmosphere (TOA) forcings. Uncertainties in the contribution of the strongly absorbing black carbon aerosol leads to a range in TOA forcings of ca. -0.5 to + 0.1 Wm (exp. -2), while the change in aerosol distributions between 1950 to 1990 leads to a change of -0.1 to -0.3 Wm (exp. -2), for fossil fuel derived aerosol with a "moderate" contribution of black carbon aerosol.

Impact of absorbing aerosol deposition on snow albedo reduction over the southern Tibetan plateau based on satellite observations

NASA Astrophysics Data System (ADS)

Lee, Wei-Liang; Liou, K. N.; He, Cenlin; Liang, Hsin-Chien; Wang, Tai-Chi; Li, Qinbin; Liu, Zhenxin; Yue, Qing

2017-08-01

We investigate the snow albedo variation in spring over the southern Tibetan Plateau induced by the deposition of light-absorbing aerosols using remote sensing data from moderate resolution imaging spectroradiometer (MODIS) aboard Terra satellite during 2001-2012. We have selected pixels with 100 % snow cover for the entire period in March and April to avoid albedo contamination by other types of land surfaces. A model simulation using GEOS-Chem shows that aerosol optical depth (AOD) is a good indicator for black carbon and dust deposition on snow over the southern Tibetan Plateau. The monthly means of satellite-retrieved land surface temperature (LST) and AOD over 100 % snow-covered pixels during the 12 years are used in multiple linear regression analysis to derive the empirical relationship between snow albedo and these variables. Along with the LST effect, AOD is shown to be an important factor contributing to snow albedo reduction. We illustrate through statistical analysis that a 1-K increase in LST and a 0.1 increase in AOD indicate decreases in snow albedo by 0.75 and 2.1 % in the southern Tibetan Plateau, corresponding to local shortwave radiative forcing of 1.5 and 4.2 W m-2, respectively.

Particle phase photosensitized radical production and aerosol aging.

PubMed

Corral-Arroyo, Pablo; Bartels-Rausch, Thorsten; Alpert, Peter Aaron; Dumas, Stephane; Perrier, Sebastien; George, Christian; Ammann, Markus

2018-06-13

Atmospheric aerosol particles may contain light absorbing (brown carbon, BrC), triplet forming organic compounds that can sustain catalytic radical reactions and thus contribute to oxidative aerosol aging. We quantify UVA induced radical production initiated by imidazole-2-carboxaldehyde (IC), benzophenone (BPh) and 4-Benzoylbenzoic acid (BBA) in the presence of the non-absorbing organics citric acid (CA), shikimic acid (SA) and syringol (Syr) at varying mixing ratios. We observed a maximum HO 2 release of 10 13 molecules min -1 cm -2 at a mole ratio Χ BPh <0.02 for BPh in CA. Mixtures of either IC or BBA with CA resulted in 10 11 -10 12 molecules min -1 cm -2 of HO 2 at mole ratios (Χ IC and Χ BBA ) between 0.01 and 0.15. HO 2 release was affected by relative humidity (RH) and film thickness suggesting coupled photochemical reaction and diffusion processes. Quantum yields of HO 2 formed per absorbed photon for IC, BBA and BPh were between 10 -7 and 5∙10 -5 . The non-photoactive organics, Syr and SA, increased HO 2 production due to the reaction with the triplet excited species ensuing ketyl radical production. Rate coefficients of the triplet of IC with Syr and SA measured by laser flash photolysis experiments were k Syr =9.4±0.3∙10 8 M -1 s -1 and k SA =2.7±0.5∙10 7 M -1 s -1 . A simple kinetic model was used to assess total HO 2 and organic radical production in the condensed phase and to upscale to ambient aerosol, indicating that BrC induced radical production may amount to an upper limit of 20 and 200 M day -1 of HO 2 and organic radical respectively, which is greater or in the same order of magnitude as the internal radical production from other processes, previously estimated to be around 15 M per day.

Using the OMI Aerosol Index and Absorption Aerosol Optical Depth to evaluate the NASA MERRA Aerosol Reanalysis

NASA Astrophysics Data System (ADS)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2014-12-01

A radiative transfer interface has been developed to simulate the UV Aerosol Index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and Aerosol Absorption Optical Depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of Aerosol Optical Depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the Aerosol Robotic Network (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the South African and South American biomass burning regions indicates that revising the spectrally-dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

NASA Astrophysics Data System (ADS)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons

Vertical structure of aerosol distribution and radiative properties over Svalbard - observations and modelling

NASA Astrophysics Data System (ADS)

Kaminski, Jacek W.; Struzewska, Joanna; Markowicz, Krzysztof; Jefimow, Maciej

2015-04-01

In the scope of the iAREA projects (Impact of absorbing aerosols on radiative forcing in the European Arctic - http://www.igf.fuw.edu.pl/iAREA) a field campaign was undertaken in March and April 2014 on Spitzbergen. Analysis of measurements was supported by the GEM-AQ model simulations. The GEM-AQ model is a chemical weather model. The core of the model is based on a weather prediction model with environmental processes (chemistry and aerosols) implanted on-line and are interactive (i.e. providing feedback of chemistry on radiation and dynamics). Numerical experiments were performed with the computational grid resolution of ˜15 km. The emission inventory developed by NILU in the ECLIPSE project was used. Preliminary analysis revealed small but systematic overestimation of modelled AOD and background BC levels. We will present the analysis of the vertical distribution of different aerosol species and its contribution to AOD for two stations on Svalbard. Also, changes of modelled chemical composition of aerosols with altitude will be analyzed.

Simulating Aerosol Optical Properties With the Aerosol Simulation Program (ASP): Closure Studies Using ARCTAS Data

NASA Astrophysics Data System (ADS)

Alvarado, M. J.; Macintyre, H. L.; Bian, H.; Chin, M.; Wang, C.

2012-12-01

The scattering and absorption of ultraviolet and visible radiation by aerosols can significantly alter actinic fluxes and photolysis rates. Accurate modeling of aerosol optical properties is thus essential to simulating atmospheric chemistry, air quality, and climate. Here we evaluate the aerosol optical property predictions of the Aerosol Simulation Program (ASP) with in situ data on aerosol scattering and absorption gathered during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The model simulations are initialized with in situ data on the aerosol size distribution and composition. We perform a set of sensitivity studies (e.g., internal vs. external mixture, core-in-shell versus Maxwell-Garnett, fraction of the organic carbon mass that is light-absorbing "brown carbon," etc.) to determine the model framework and parameters most consistent with the observations. We compare the ASP results to the aerosol optical property lookup tables in FAST-JX and suggest improvements that will better enable FAST-JX to simulate the impact of aerosols on photolysis rates and atmospheric chemistry.

Comprehensive characterisation of atmospheric aerosols in Budapest, Hungary: physicochemical properties of inorganic species

NASA Astrophysics Data System (ADS)

Salma, Imre; Maenhaut, Willy; Zemplén-Papp, Éva; Záray, Gyula

As part of an air pollution project in Budapest, aerosol samples were collected by stacked filter units and cascade impactors at an urban background site, two downtown sites, and within a road tunnel in field campaigns conducted in 1996, 1998 and 1999. Some criteria pollutants were also measured at one of the downtown sites. The aerosol samples were analysed by one or more of the following methods: instrumental neutron activation analysis, particle-induced X-ray emission analysis, a light reflection technique, gravimetry, thermal profiling carbon analysis and capillary electrophoresis. The quantities measured or derived include atmospheric concentrations of elements (from Na to U), of particulate matter, of black and elemental carbon, and total carbonaceous fraction, of some ionic species (e.g., nitrate and sulphate) in the fine ( <2 μm equivalent aerodynamic diameter, EAD) or in both coarse (10- 2 μm EAD) and fine size fractions, atmospheric concentrations of NO, NO 2, SO 2, CO and total suspended particulate matter, and meteorological parameters. The analytical results were used for characterisation of the concentration levels, elemental composition, time trends, enrichment of and relationships among the aerosol species in coarse and fine size fractions, for studying their fine-to-coarse concentration ratios, spatial and temporal variability, for determining detailed elemental mass size distributions, and for examining the extent of chemical mass closure.

Light-absorbing carbon from prescribed and laboratory biomass burning and gasoline vehicle emissions

EPA Science Inventory

Carbonaceous aerosols are ubiquitous in the atmosphere and can directly affect Earth’s climate by absorbing and scattering incoming solar radiation. Both field and laboratory measurements have confirmed that biomass burning (BB) is an important primary source of light absorbing o...

Retrieving Smoke Aerosol Height from DSCOVR/EPIC

NASA Astrophysics Data System (ADS)

Xu, X.; Wang, J.; Wang, Y.

2017-12-01

Unlike industrial pollutant particles that are often confined within the planetary boundary layer, smoke from forest and agriculture fires can inject massive carbonaceous aerosols into the upper troposphere due to the intense pyro-convection. Sensitivity of weather and climate to absorbing carbonaceous aerosols is regulated by the altitude of those aerosol layers. However, aerosol height information remains limited from passive satellite sensors. Here we present an algorithm to estimate smoke aerosol height from radiances in the oxygen A and B bands measured by the Earth Polychromatic Imaging Camera (EPIC) from the Deep Space Climate Observatory (DSCOVR). With a suit of case studies and validation efforts, we demonstrate that smoke aerosol height can be well retrieved over both ocean and land surfaces multiple times daily.

Real-Time Studies of Iron Oxalate-Mediated Oxidation of Glycolaldehyde as a Model for Photochemical Aging of Aqueous Tropospheric Aerosols.

PubMed

Thomas, Daniel A; Coggon, Matthew M; Lignell, Hanna; Schilling, Katherine A; Zhang, Xuan; Schwantes, Rebecca H; Flagan, Richard C; Seinfeld, John H; Beauchamp, J L

2016-11-15

The complexation of iron(III) with oxalic acid in aqueous solution yields a strongly absorbing chromophore that undergoes efficient photodissociation to give iron(II) and the carbon dioxide anion radical. Importantly, iron(III) oxalate complexes absorb near-UV radiation (λ > 350 nm), providing a potentially powerful source of oxidants in aqueous tropospheric chemistry. Although this photochemical system has been studied extensively, the mechanistic details associated with its role in the oxidation of dissolved organic matter within aqueous aerosol remain largely unknown. This study utilizes glycolaldehyde as a model organic species to examine the oxidation pathways and evolution of organic aerosol initiated by the photodissociation of aqueous iron(III) oxalate complexes. Hanging droplets (radius 1 mm) containing iron(III), oxalic acid, glycolaldehyde, and ammonium sulfate (pH ∼3) are exposed to irradiation at 365 nm and sampled at discrete time points utilizing field-induced droplet ionization mass spectrometry (FIDI-MS). Glycolaldehyde is found to undergo rapid oxidation to form glyoxal, glycolic acid, and glyoxylic acid, but the formation of high molecular weight oligomers is not observed. For comparison, particle-phase experiments conducted in a laboratory chamber explore the reactive uptake of gas-phase glycolaldehyde onto aqueous seed aerosol containing iron and oxalic acid. The presence of iron oxalate in seed aerosol is found to inhibit aerosol growth. These results suggest that photodissociation of iron(III) oxalate can lead to the formation of volatile oxidation products in tropospheric aqueous aerosols.

Improving aerosol vertical retrieval for NWP application: Studying the impact of IR-sensed aerosol on data assimilation systems.

NASA Astrophysics Data System (ADS)

Oyola, Mayra; Marquis, Jared; Ruston, Benjamin; Campbell, James; Baker, Nancy; Westphal, Douglas; Zhang, Jianglong; Hyer, Edward

2017-04-01

Radiometric measurements from passive infrared (IR) sensors are important in numerical weather prediction (NWP) because they are sensitive to surface temperatures and atmospheric temperature profiles. However, these measurements are also sensitive to absorbing and scattering constituents in the atmosphere. Dust aerosols absorb in the IR and are found over many global regions with irregular spatial and temporal frequency. Retrievals of temperature using IR data are thus vulnerable to dust-IR radiance biases, most notably over tropical oceans where accurate surface and atmospheric temperatures are critical to accurate prediction of tropical cyclone development. Previous studies have shown that dust aerosols can bias retrieved brightness temperatures (BT) by up to 10K in some IR channels that are assimilated to constrain atmospheric temperature and water vapor profiles. Other BT-derived parameters such as sea surface temperatures (SSTs) are susceptible to negative biases of at least 1K or higher, which conflicts with the accuracy requirement for most research and operational applications (i.e., +/- 0.3 K). This problem is not limited to just satellite retrievals. BT bias also impacts the incorporation of background fields from NWP analyses in data assimilation (DA) systems. The effect of aerosols on IR fluxes at the ocean surface is a function of both aerosol loading and vertical profile. Therefore, knowledge of the aerosol vertical distribution, and understanding of how well this distribution is captured by NWP models, is necessary to ensuring proper treatment of aerosol-affected radiances in both retrieval and data assimilation. This understanding can be achieved by conducting modeling studies and by the exploitation of a robust observational dataset, such as satellite-based lidar profiling, which can be used to characterize aerosol type and distribution. In this talk, we describe such an application using the Navy Aerosol Analysis Prediction System (NAAPS) and

An aerosol climatology for a rapidly growing arid region (southern Arizona): Major aerosol species and remotely sensed aerosol properties

NASA Astrophysics Data System (ADS)

Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.

2011-10-01

This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March-May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls.

Remote Sensing of Aerosol and Non-Aerosol Absorption

NASA Technical Reports Server (NTRS)

Kaufman, Y. J.; Dubovik, O.; Holben, B. N.; Remer, L. A.; Tanre, D.; Lau, William K. M. (Technical Monitor)

2001-01-01

Remote sensing of aerosol from the new satellite instruments (e.g. MODIS from Terra) and ground based radiometers (e.g. the AERONET) provides the opportunity to measure the absorption characteristics of the ambient undisturbed aerosol in the entire atmospheric column. For example Landsat and AERONET data are used to measure spectral absorption of sunlight by dust from West Africa. Both Application of the Landsat and AERONET data demonstrate that Saharan dust absorption of solar radiation is several times smaller than the current international standards. This is due to difficulties of measuring dust absorption in situ, and due to the often contamination of dust properties by the presence of air pollution or smoke. We use the remotely sensed aerosol absorption properties described by the spectral sin le scattering albedo, together with statistics of the monthly optical thickness for the fine and coarse aerosol derived from the MODIS data. The result is an estimate of the flux of solar radiation absorbed by the aerosol layer in different regions around the globe where aerosol is prevalent. If this aerosol forcing through absorption is not included in global circulation models, it may be interpreted as anomalous absorption in these regions. In a preliminary exercise we also use the absorption measurements by AERONET, to derive the non-aerosol absorption of the atmosphere in cloud free conditions. The results are obtained for the atmospheric windows: 0.44 microns, 0.66 microns, 0.86 microns and 1.05 microns. In all the locations over the land and ocean that were tested no anomalous absorption in these wavelengths, was found within absorption optical thickness of +/- 0.005.

Retrieval of Aerosol Optical Depth Above Clouds from OMI Observations: Sensitivity Analysis, Case Studies

NASA Technical Reports Server (NTRS)

Torres, O.; Jethva, H.; Bhartia, P. K.

2012-01-01

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originated in arid and semi-arid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth atmosphere system is especially important. The generally negative (cooling) top of the atmosphere direct effect of absorbing aerosols, may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. In this paper we discuss the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol-cloud separation. The technique was applied to above-cloud aerosol events over the Southern Atlantic Ocean yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

Aerosol layer height from synergistic use of VIIRS and OMPS

NASA Astrophysics Data System (ADS)

Lee, J.; Hsu, N. Y. C.; Sayer, A. M.; Kim, W.; Seftor, C. J.

2017-12-01

This study presents an Aerosol Single-scattering albedo and Height Estimation (ASHE) algorithm, which retrieves the height of UV-absorbing aerosols by synergistically using the Visible Infrared Imaging Radiometer Suite (VIIRS) and the Ozone Mapping and Profiler Suite (OMPS). ASHE provides height information over a much broader area than ground-based or spaceborne lidar measurements by benefitting from the wide swaths of the two instruments used. As determination of single-scattering albedo (SSA) of the aerosol layer is the most critical part for the performance and coverage of ASHE, here we demonstrate three different strategies to constrain the SSA. First, ASHE is able to retrieve the SSA of UV-absorbing aerosols when Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) provides vertical profiles of the aerosol layer of interest. Second, Aerosol Robotic Network (AERONET) inversions can directly constrain the SSA of the aerosol layer when collocated with VIIRS or OMPS. Last, a SSA climatology from ASHE, AERONET, or other data sources can be used for large-scale, aged aerosol events, for which climatological SSA is well-known, at the cost of a slight decrease in retrieval accuracy. The same algorithm can be applied to measurements of similar type, such as those made by the Moderate Resolution Imaging Spectroradiometer (MODIS) and Ozone Monitoring Instrument (OMI), for a long-term, consistent data record.

Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Flores, J. M.; Brock, C. A.; Brown, S. S.; Rudich, Y.

2013-04-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We determined aerosol extinction cross sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with the literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (± 0.03) + 0.19 (± 0.08)i at 360 nm and 1.63 (± 0.03) + 0.21 (± 0.05)i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (± 0.02) + 0.07 (± 0.06)i at 360 nm and 1.66 (± 0.02) + 0.06 (± 0.04)i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross section, and complex refractive index as a function of wavelength.

Broadband measurements of aerosol extinction in the ultraviolet spectral region

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Flores, J. M.; Brock, C. A.; Brown, S. S.; Rudich, Y.

2013-01-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross-sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We determined aerosol extinction cross-sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross-sections over the 360-420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (±0.03) + 0.19 (±0.08) i at 360 nm and 1.53 (±0.03) + 0.21 (±0.05) i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (±0.02) + 0.07 (±0.06) i at 360 nm and 1.66 (±0.02) + 0.06 (±0.04) i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross-section, and complex refractive index as a function of wavelength.

SPEX: a highly accurate spectropolarimeter for atmospheric aerosol characterization

NASA Astrophysics Data System (ADS)

Rietjens, J. H. H.; Smit, J. M.; di Noia, A.; Hasekamp, O. P.; van Harten, G.; Snik, F.; Keller, C. U.

2017-11-01

Global characterization of atmospheric aerosol in terms of the microphysical properties of the particles is essential for understanding the role aerosols in Earth climate [1]. For more accurate predictions of future climate the uncertainties of the net radiative forcing of aerosols in the Earth's atmosphere must be reduced [2]. Essential parameters that are needed as input in climate models are not only the aerosol optical thickness (AOT), but also particle specific properties such as the aerosol mean size, the single scattering albedo (SSA) and the complex refractive index. The latter can be used to discriminate between absorbing and non-absorbing aerosol types, and between natural and anthropogenic aerosol. Classification of aerosol types is also very important for air-quality and health-related issues [3]. Remote sensing from an orbiting satellite platform is the only way to globally characterize atmospheric aerosol at a relevant timescale of 1 day [4]. One of the few methods that can be employed for measuring the microphysical properties of aerosols is to observe both radiance and degree of linear polarization of sunlight scattered in the Earth atmosphere under different viewing directions [5][6][7]. The requirement on the absolute accuracy of the degree of linear polarization PL is very stringent: the absolute error in PL must be smaller then 0.001+0.005.PL in order to retrieve aerosol parameters with sufficient accuracy to advance climate modelling and to enable discrimination of aerosol types based on their refractive index for air-quality studies [6][7]. In this paper we present the SPEX instrument, which is a multi-angle spectropolarimeter that can comply with the polarimetric accuracy needed for characterizing aerosols in the Earth's atmosphere. We describe the implementation of spectral polarization modulation in a prototype instrument of SPEX and show results of ground based measurements from which aerosol microphysical properties are retrieved.

Chemical Properties of Brown Carbon Aerosol Generated at the Missoula Fire Sciences Laboratory

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Womack, C.; Franchin, A.; Middlebrook, A. M.; Wagner, N.; Manfred, K.

2017-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Biomass burning is a major source of light-absorbing carbonaceous aerosol in the United States. These aerosol are generally classified into two categories: black carbon (graphitic-like aerosol that absorbs broadly across the ultraviolet and visible spectral regions) and brown carbon (organic aerosol that absorbs strongly in the ultraviolet and near-visible spectral regions). The composition, volatility, and chemical aging of brown carbon are poorly known, but are important to understanding its radiative effects. We deployed three novel instruments to the Missoula Fire Sciences Laboratory in 2016 to measure brown carbon absorption: a photoacoustic spectrometer, broadband cavity enhanced spectrometer, and particle-into-liquid sampler coupled to a liquid waveguide capillary cell. The instruments sampled from a shared inlet with well-characterized dilution and thermal denuding. We sampled smoke from 32 controlled burns of fuels relevant to western U.S. wildfires. We use these measurements to determine the volatility of water-soluble brown carbon, and compare this to the volatility of water-soluble organic aerosol and total organic aerosol. We further examine the wavelength-dependence of the water-soluble brown carbon absorption as a function of denuder temperature. Together this gives new information about the solubility, volatility, and chemical composition of brown carbon.

Satellite Detection of Smoke Aerosols Over a Snow/Ice Surface by TOMS

NASA Technical Reports Server (NTRS)

Hsu, N. Christina; Herman, Jay R.; Gleason, J. F.; Torres, O.; Seftor, C. J.

1998-01-01

The use of TOMS (Total Ozone Mapping Spectrometer) satellite data demonstrates the recently developed technique of using satellite UV radiance measurements to detect absorbing tropospheric aerosols is effective over snow/ice surfaces. Instead of the traditional single wavelength (visible or infrared) method of measuring tropospheric aerosols, this method takes advantage of the wavelength dependent reduction in the backscattered radiance due to the presence of absorbing aerosols over snow/ice surfaces. An example of the resulting aerosol distribution derived from TOMS data is shown for an August 1998 event in which smoke generated by Canadian forest fires drifts over and across Greenland. As the smoke plume moved over Greenland, the TOMS observed 380 nm reflectivity over the snow/ice surface dropped drastically from 90-100% down to 30-40%. To study the effects of this smoke plume in both the UV and visible regions of the spectrum, we compared a smoke-laden spectrum taken over Greenland by the high spectral resolution (300 to 800 nm) GOME instrument with one that is aerosol-free. We also discuss the results of modeling the darkening effects of various types of absorbing aerosols over snow/ice surfaces using a radiative transfer code. Finally, we investigated the history of such events by looking at the nearly twenty year record of TOMS aerosol index measurements and found that there is a large interannual variability in the amount of smoke aerosols observed over Greenland. This information will be available for studies of radiation and transport properties in the Arctic.

Local and remote impacts of aerosol species on Indian summer monsoon rainfall in a GCM

NASA Astrophysics Data System (ADS)

Turner, A. G.; Guo, L.; Highwood, E.

2016-12-01

The HadGEM2 AGCM is used to determine the most important anthropogenic aerosols in the Indian monsoon using experiments in which observed trends in individual aerosol species are imposed. Sulphur dioxide (SD) emissions are shown to impact rainfall more strongly than black carbon (BC) aerosols, causing reduced rainfall especially over northern India. Significant perturbations due to BC are not noted until its emissions are scaled up in a sensitivity test, resulting in rainfall increases over northern India due to the Elevated Heat Pump mechanism, enhancing convection during the premonsoon and bringing forward the monsoon onset. Secondly, the impact of anthropogenic aerosols is compared to that of increasing greenhouse-gas concentrations and observed sea-surface temperature (SST) warming. The tropospheric temperature gradient driving the monsoon shows weakening when forced by either SD or imposed SST trends. However the observed SST trend is dominated by warming in the deep tropics; when the component of SST trend related to aerosol emissions is removed, further warming is found in the extratropical northern hemisphere that tends to offset monsoon weakening. This suggests caution is needed when using SST forcing as a proxy for greenhouse warming. Finally, aerosol emissions are decomposed into those from the Indian region and those elsewhere, in pairs of experiments with SD and BC. Both local and remote aerosol emissions are found to lead to rainfall changes over India; for SD, remote aerosols contribute around 75% of the rainfall decrease over India, while for BC the remote forcing is even more dominant.

Local and remote impacts of aerosol species on Indian summer monsoon rainfall in a GCM

NASA Astrophysics Data System (ADS)

Guo, Liang; Turner, Andrew; Highwood, Eleanor

2016-04-01

The HadGEM2 AGCM is used to determine the most important anthropogenic aerosols in the Indian monsoon using experiments in which observed trends in individual aerosol species are imposed. Sulphur dioxide (SD) emissions are shown to impact rainfall more strongly than black carbon (BC) aerosols, causing reduced rainfall especially over northern India. Significant perturbations due to BC are not noted until its emissions are scaled up in a sensitivity test, in which rainfall increases over northern India as a result of the Elevated Heat Pump mechanism, enhancing convection during the pre-monsoon and bringing forward the monsoon onset. Secondly, the impact of anthropogenic aerosols is compared to that of increasing greenhouse-gas concentrations and observed sea-surface temperature (SST) warming. The tropospheric temperature gradient driving the monsoon shows weakening when forced by either SD or imposed SST trends. However the observed SST trend is dominated by warming in the deep tropics; when the component of SST trend related to aerosol emissions is removed, further warming is found in the extratropical northern hemisphere that tends to offset monsoon weakening. This suggests caution is needed when using SST forcing as a proxy for greenhouse warming. Finally, aerosol emissions are decomposed into those from the Indian region and those elsewhere, in pairs of experiments with SD and BC. Both local and remote aerosol emissions are found to lead to rainfall changes over India; for SD, remote aerosols contribute around 75% of the rainfall decrease over India, while for BC the remote forcing is even more dominant.

Two-photon or higher-order absorbing optical materials for generation of reactive species

NASA Technical Reports Server (NTRS)

Marder, Seth R. (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Perry, Joseph W. (Inventor)

2003-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Two-photon or higher-order absorbing optical materials for generation of reactive species

NASA Technical Reports Server (NTRS)

Perry, Joseph W (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R (Inventor)

2007-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Two-Photon or Higher-Order Absorbing Optical Materials for Generation of Reactive Species

NASA Technical Reports Server (NTRS)

Perry, Joseph W. (Inventor); Cumpston, Brian (Inventor); Lipson, Matthew (Inventor); Marder, Seth R. (Inventor)

2013-01-01

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Absorption Ångström exponents of aerosols and light absorbing carbon (LAC) obtained from in situ data in Covilhã, central Portugal.

PubMed

Mogo, S; Cachorro, V E; de Frutos, A; Rodrigues, A

2012-12-01

A field campaign was conducted from October 2009 to July 2010 at Covilhã, a small town located in the region of Beira Interior (Portugal) in the interior of the Iberian Peninsula. The ambient light-absorption coefficient, σ(a) (522 nm), obtained from a Particle Soot Absorption Photometer (PSAP), presented a daily mean value of 12.1 Mm⁻¹ (StD = 7.3 Mm⁻¹). The wavelength dependence of aerosol light absorption is investigated through the Ångström parameter, α(a). The α(a) values for the pair of wavelengths 470-660 nm ranged from 0.86 to 1.47 during the period of measurements. The PSAP data were used to infer the mass of light absorbing carbon (LAC) and the daily mean varied from 0.1 to 6.8 μg m⁻³. A detailed study of special events with different aerosol characteristics is carried out and, to support data interpretation, air masses trajectory analysis is performed.

Identification and Quantification of Regional Aerosol Trends and Impact on Clouds Over the North Atlantic Ocean

NASA Astrophysics Data System (ADS)

Jongeward, Andrew R.

Aerosols and clouds contribute to atmospheric variability and Earth's radiative balance across local, regional, and global scales. Originating from both natural and anthropogenic sources, aerosols can cause adverse health effects and can interact directly with solar radiation as well as indirectly through complex interactions with clouds. Aerosol optical depth (AOD) has been observed from satellite platforms for over 30 years. During this time, regional changes in emissions, arising from air quality policies and socioeconomic factors, have been suggested as causes for some observed AOD trends. In the United States, the Clean Air Act and amendments have produced improvements in air quality. In this work the impacts of improved air quality on the aerosol loading and aerosol direct and indirect effects over the North Atlantic Ocean are explored using satellite, ground, and model datasets on the monthly timescale during 2002 to 2012. It is established that two trends exist in the total AOD observed by MODIS over the North Atlantic. A decreasing AOD trend between ?0.02 and ?0.04 per decade is observed over the mid-latitude region. Using the GOCART aerosol model it is shown that this trend results from decreases in anthropogenic species. Ground based aerosol networks (AERONET and IMPROVE) support a decreasing trend in AOD and further strengthen links to anthropogenic aerosol species, particularly sulfate species. This anthropogenic decrease occurs primarily during spring and summer. During the same time period, MODIS also observes an increasing AOD trend of 0.02 per decade located in the sub-tropical region. This trend is shown to occur during summer and is the result of natural dust aerosol. Changes in the North African environment seen in the MERRA reanalysis suggest an accelerated warming over the Saharan Desert leads to changes in the African Easterly Jet, related Easterly Waves, and baroclinicity playing a role in an increase and northward shift in African dust

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

NASA Astrophysics Data System (ADS)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

SW radiative effect of aerosol in GRAPES_GFS

NASA Astrophysics Data System (ADS)

Chen, Qiying

2017-04-01

The aerosol particles can scatter and absorb solar radiation, and so change the shortwave radiation absorbed by the atmosphere, reached the surface and that reflected back to outer space at TOA. Since this process doesn't interact with other processes, it is called direct radiation effect. The clear sky downward SW and net SW fluxes at the surface in GRAPES_GFS of China Meteorological Administration are overestimated in Northern multitudes and Tropics. The main source of these errors is the absence of aerosol SW effect in GRAPES_GFS. The climatic aerosol mass concentration data, which include 13 kinds of aerosol and their 14 SW bands optical properties are considered in GRAPES_GFS. The calculated total optical depth, single scatter albedo and asymmetry factor are used as the input to radiation scheme. Compared with the satellite observation from MISER, the calculated total optical depth is in good consistent. The seasonal experiments show that, the summer averaged clear sky radiation fluxes at the surface are improved after including the SW effect of aerosol. The biases in the clear sky downward SW and net SW fluxes at the surface in Northern multitudes and Tropic reduced obviously. Furthermore, the weather forecast experiments also show that the skill scores in Northern hemisphere and East Asia also become better.

Intercomparison between CMIP5 model and MODIS satellite-retrieved data of aerosol optical depth, cloud fraction, and cloud-aerosol interactions

NASA Astrophysics Data System (ADS)

Sockol, Alyssa; Small Griswold, Jennifer D.

2017-08-01

Aerosols are a critical component of the Earth's atmosphere and can affect the climate of the Earth through their interactions with solar radiation and clouds. Cloud fraction (CF) and aerosol optical depth (AOD) at 550 nm from the Moderate Resolution Imaging Spectroradiometer (MODIS) are used with analogous cloud and aerosol properties from Historical Phase 5 of the Coupled Model Intercomparison Project (CMIP5) model runs that explicitly include anthropogenic aerosols and parameterized cloud-aerosol interactions. The models underestimate AOD by approximately 15% and underestimate CF by approximately 10% overall on a global scale. A regional analysis is then used to evaluate model performance in two regions with known biomass burning activity and absorbing aerosol (South America (SAM) and South Africa (SAF)). In SAM, the models overestimate AOD by 4.8% and underestimate CF by 14%. In SAF, the models underestimate AOD by 35% and overestimate CF by 13.4%. Average annual cycles show that the monthly timing of AOD peaks closely match satellite data in both SAM and SAF for all except the Community Atmosphere Model 5 and Geophysical Fluid Dynamics Laboratory (GFDL) models. Monthly timing of CF peaks closely match for all models (except GFDL) for SAM and SAF. Sorting monthly averaged 2° × 2.5° model or MODIS CF as a function of AOD does not result in the previously observed "boomerang"-shaped CF versus AOD relationship characteristic of regions with absorbing aerosols from biomass burning. Cloud-aerosol interactions, as observed using daily (or higher) temporal resolution data, are not reproducible at the spatial or temporal resolution provided by the CMIP5 models.

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

NASA Technical Reports Server (NTRS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Corr, C. A.; Dibb, J. E.; Greenslade, M. E.; Martin, R. F.; Moore, R. H.; Scheuer, E.; Shook, M. A.;

Dependence of atmospheric refractive index structure parameter (Cn2) on the residence time and vertical distribution of aerosols.

PubMed

Anand, N; Satheesh, S K; Krishna Moorthy, K

2017-07-15

Effects of absorbing atmospheric aerosols in modulating the tropospheric refractive index structure parameter (Cn2) are estimated using high resolution radiosonde and multi-satellite data along with a radiative transfer model. We report the influence of variations in residence time and vertical distribution of aerosols in modulating Cn2 and why the aerosol induced atmospheric heating needs to be considered while estimating a free space optical communication link budget. The results show that performance of the link is seriously affected if large concentrations of absorbing aerosols reside for a long time in the atmospheric path.

Black carbon and wavelength-dependent aerosol absorption in the North China Plain based on two-year aethalometer measurements

NASA Astrophysics Data System (ADS)

Ran, L.; Deng, Z. Z.; Wang, P. C.; Xia, X. A.

2016-10-01

Light-absorbing components of atmospheric aerosols have gained particular attention in recent years due to their climatic and environmental effects. Based on two-year measurements of aerosol absorption at seven wavelengths, aerosol absorption properties and black carbon (BC) were investigated in the North China Plain (NCP), one of the most densely populated and polluted regions in the world. Aerosol absorption was stronger in fall and the heating season (from November to March) than in spring and summer at all seven wavelengths. Similar spectral dependence of aerosol absorption was observed in non-heating seasons despite substantially strong absorption in fall. With an average absorption Angström exponent (α) of 1.36 in non-heating seasons, freshly emitted BC from local fossil fuel burning was thought to be the major component of light-absorbing aerosols. In the heating season, strong ultraviolet absorption led to an average α of 1.81, clearly indicating the importance of non-BC light-absorbing components, which were possibly from coal burning for domestic heating and aging processes on a regional scale. Diurnally, the variation of BC mass concentrations experienced a double-peak pattern with a higher level at night throughout the year. However, the diurnal cycle of α in the heating season was distinctly different from that in non-heating seasons. α peaked in the late afternoon in non-heating seasons with concomitantly observed low valley in BC mass concentrations. In contrast, α peaked around the midnight in the heating season and lowered down during the daytime. The relationship of aerosol absorption and winds in non-heating seasons also differed from that in the heating season. BC mass concentrations declined while α increased with increasing wind speed in non-heating seasons, which suggested elevated non-BC light absorbers in transported aged aerosols. No apparent dependence of α on wind speed was found in the heating season, probably due to well mixed

Aerosol Climate Time Series Evaluation In ESA Aerosol_cci

NASA Astrophysics Data System (ADS)

Popp, T.; de Leeuw, G.; Pinnock, S.

2015-12-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. By the end of 2015 full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which are also validated. The paper will summarize and discuss the results of major reprocessing and validation conducted in 2015. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension with successor instruments of the Sentinel family will be described and the complementarity of the different satellite aerosol products

In situ aerosol optics in Reno, NV, USA during and after the summer 2008 California wildfires and the influence of aerosol coatings

NASA Astrophysics Data System (ADS)

Gyawali, M.; Arnott, W. P.; Lewis, K.; Moosmüller, H.

2009-06-01

Hundreds of wildfires in Northern California were sparked by lightning during the summer of 2008, resulting in downwind smoke for the months of June and July. Comparisons are reported for aerosol optics measurements in Reno Nevada made during the very smoky summer month of July and the relatively clean month of August. Photoacoustic instruments equipped with integrating nephelometers were used to measure aerosol light scattering and absorption at wavelengths of 405 nm and 870 nm, revealing a strong variation of the aerosol light absorption with wavelength. Coated sphere calculations were used to show that Ångström exponents of absorption (AEA) as large as 1.6 are possible even with non-absorbing organic coatings on black carbon cores, suggesting care be exercised when diagnosing AEA. Insight on fuels burned is gleaned from comparison of AEA versus single scattering albedo (SSA) of the ambient measurements with laboratory biomass smoke measurements for many fuels. Measurements during the month of August, which were largely unaffected by fire smoke, exhibit surprisingly low AEA for aerosol light absorption when the SSA is highest, again likely as a consequence of the underappreciated wavelength dependence of aerosol light absorption by particles coated with non absorbing organic and inorganic matter.

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].

Characterization of urban aerosol in Cork city (Ireland) using aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Kourtchev, I.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2013-05-01

Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC), sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS) and was also found to comprise organic aerosol as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA) comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA) comprised 18%, "biomass burning" organic aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA) comprised 21%, and finally a species type characterized by primary {m/z} peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA), but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively).

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

Characterization of urban aerosol in Cork City (Ireland) using aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Ovadnevaite, J.; Ceburnis, D.; Martin, D.; Healy, R. M.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J. C.; O'Dowd, C.

2012-11-01

Ambient wintertime background urban aerosol in Cork City, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the 1 200 000 single particles characterized by an Aerosol Time-Of-Flight Mass Spectrometer (TSI ATOFMS) were classified into five organic-rich particle types, internally-mixed to different proportions with Elemental Carbon (EC), sulphate and nitrate while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was also characterized using a High Resolution Time-Of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS) and was also found to comprise organic matter as the most abundant species (62%), followed by nitrate (15%), sulphate (9%) and ammonium (9%), and then chloride (5%). Positive matrix factorization (PMF) was applied to the HR-ToF-AMS organic matrix and a five-factor solution was found to describe the variance in the data well. Specifically, "Hydrocarbon-like" Organic Aerosol (HOA) comprised 19% of the mass, "Oxygenated low volatility" Organic Aerosols (LV-OOA) comprised 19%, "Biomass wood Burning" Organic Aerosol (BBOA) comprised 23%, non-wood solid-fuel combustion "Peat and Coal" Organic Aerosol (PCOA) comprised 21%, and finally, a species type characterized by primary m/z peaks at 41 and 55, similar to previously-reported "Cooking" Organic Aerosol (COA) but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Despite wood, cool and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosols mass and non refractory PM1, respectively).

Aerosol Climate Time Series in ESA Aerosol_cci

NASA Astrophysics Data System (ADS)

Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon

2016-04-01

Within the ESA Climate Change Initiative (CCI) Aerosol_cci (2010 - 2017) conducts intensive work to improve algorithms for the retrieval of aerosol information from European sensors. Meanwhile, full mission time series of 2 GCOS-required aerosol parameters are completely validated and released: Aerosol Optical Depth (AOD) from dual view ATSR-2 / AATSR radiometers (3 algorithms, 1995 - 2012), and stratospheric extinction profiles from star occultation GOMOS spectrometer (2002 - 2012). Additionally, a 35-year multi-sensor time series of the qualitative Absorbing Aerosol Index (AAI) together with sensitivity information and an AAI model simulator is available. Complementary aerosol properties requested by GCOS are in a "round robin" phase, where various algorithms are inter-compared: fine mode AOD, mineral dust AOD (from the thermal IASI spectrometer, but also from ATSR instruments and the POLDER sensor), absorption information and aerosol layer height. As a quasi-reference for validation in few selected regions with sparse ground-based observations the multi-pixel GRASP algorithm for the POLDER instrument is used. Validation of first dataset versions (vs. AERONET, MAN) and inter-comparison to other satellite datasets (MODIS, MISR, SeaWIFS) proved the high quality of the available datasets comparable to other satellite retrievals and revealed needs for algorithm improvement (for example for higher AOD values) which were taken into account for a reprocessing. The datasets contain pixel level uncertainty estimates which were also validated and improved in the reprocessing. For the three ATSR algorithms the use of an ensemble method was tested. The paper will summarize and discuss the status of dataset reprocessing and validation. The focus will be on the ATSR, GOMOS and IASI datasets. Pixel level uncertainties validation will be summarized and discussed including unknown components and their potential usefulness and limitations. Opportunities for time series extension

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.

Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles

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

Lin, Peng; Aiona, Paige K.; Li, Ying

Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly-emitted biomass burning organic aerosol (BBOA) samples collected during test burns of selected biomass fuels: sawgrass, peat, ponderosa pine, and black spruce. We characterize individual BrC chromophores present in these samples using high performance liquid chromatography coupled to a photodiode array detector and a high-resolution mass spectrometer. We demonstrate that both the overall BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels and burning conditions. Common BrC chromophoresmore » in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as potential markers of BrC originating from different biomass burning sources. On average, ~50% of the light absorption above 300 nm can be attributed to a limited number of strong BrC chromophores, which may serve as representative light-absorbing species for studying atmospheric processing of BrC aerosol. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of 16 hours. A “molecular corridors” analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low volatility (<1 g m-1) and will be retained in the particle phase under atmospherically relevant conditions.« less

Spectral Absorption Properties of Atmospheric Aerosols

NASA Technical Reports Server (NTRS)

Bergstrom, R. W.; Pilewskie, P.; Russell, P. B.; Redemann, J.; Bond, T. C.; Quinn, P. K.; Sierau, B.

2007-01-01

We have determined the solar spectral absorption optical depth of atmospheric aerosols for specific case studies during several field programs (three cases have been reported previously; two are new results). We combined airborne measurements of the solar net radiant flux density and the aerosol optical depth with a detailed radiative transfer model for all but one of the cases. The field programs (SAFARI 2000, ACE Asia, PRIDE, TARFOX, INTEX-A) contained aerosols representing the major absorbing aerosol types: pollution, biomass burning, desert dust and mixtures. In all cases the spectral absorption optical depth decreases with wavelength and can be approximated with a power-law wavelength dependence (Absorption Angstrom Exponent or AAE). We compare our results with other recent spectral absorption measurements and attempt to briefly summarize the state of knowledge of aerosol absorption spectra in the atmosphere. We discuss the limitations in using the AAE for calculating the solar absorption. We also discuss the resulting spectral single scattering albedo for these cases.

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.

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

NASA Technical Reports Server (NTRS)

Perkins, P. J.; Papathakos, L. C.

1978-01-01

The Global Atmospheric Sampling Program (GASP) is collecting and analyzing data on gaseous and aerosol trace contaminants in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei, and mass concentration of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to identify the source of the air mass as being typically tropospheric or stratospheric.

Spectral Absorption of Solar Radiation by Aerosols during ACE-Asia

NASA Technical Reports Server (NTRS)

Bergstrom, R. W.; Pilewskie, P.; Pommier, J.; Rabbette, M.; Russell, P. B.; Schmid, B.; Redermann, J.; Higurashi, A.; Nakajima, T.; Quinn, P. K.

2004-01-01

As part of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia), the upward and downward spectral solar radiant fluxes were measured with the Spectral Solar Flux Radiometer (SSFR), and the aerosol optical depth was measured with the Ames Airborne Tracking Sunphotometer (AATS-14) aboard the Center for INterdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. IN this paper, we examine the data obtained for two cases: a moderately thick aerosol layer, 12 April, and a relatively thin aerosol case, 16 April 2001. ON both days, the Twin Otter flew vertical profiles in the Korean Strait southeast of Gosan Island. For both days we determine the aerosol spectral absorption of the layer and estimate the spectral aerosol absorption optical depth and single-scattering albedo. The results for 12 April show that the single-scattering albedo increases with wavelength from 0.8 at 400 nm to 0.95 at 900 nm and remains essentially constant from 950 to 1700 nm. On 16 April the amount of aerosol absorption was very low; however, the aerosol single-scattering albedo appears to decrease slightly with wavelength in the visible region. We interpret these results in light of the two absorbing aerosol species observed during the ACE-asia study: mineral dust and black carbon. The results for 12 April are indicative of a mineral dust-black carbon mixture. The 16 April results are possibly caused by black carbon mixed with nonabsorbing pollution aerosols. For the 12 April case we attempt to estimate the relative contributions of the black carbon particles and the mineral dust particles. We compare our results with other estimates of the aerosol properties from a Sea-Viewing Wide Field-of-View Sensor (SeaWiFS) satellite analysis and aerosol measurements made aboard the Twin Otter, aboard the National Oceanic and Atmospheric Administration Ronald H Brown ship, and at ground sites in Gosan and Japan. The results indicate a relatively complicated aerosol

Evaluation of the new capture vapourizer for aerosol mass spectrometers (AMS) through laboratory studies of inorganic species

NASA Astrophysics Data System (ADS)

Hu, Weiwei; Campuzano-Jost, Pedro; Day, Douglas A.; Croteau, Philip; Canagaratna, Manjula R.; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose L.

2017-08-01

Aerosol mass spectrometers (AMSs) and Aerosol Chemical Speciation Monitors (ACSMs) commercialized by Aerodyne are widely used to measure the non-refractory species in submicron particles. With the standard vapourizer (SV) that is installed in all commercial instruments to date, the quantification of ambient aerosol mass concentration requires the use of the collection efficiency (CE) to correct for the loss of particles due to bounce. A new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction. Two high-resolution AMS instruments, one with a SV and one with a CV, were operated side by side in the laboratory. Four standard species, NH4NO3, NaNO3, (NH4)2SO4 and NH4Cl, which typically constitute the majority of the mass of ambient submicron inorganic species, are studied. The effect of vapourizer temperature (Tv ˜ 200-800 °C) on the detected fragments, CE and size distributions are investigated. A Tv of 500-550 °C for the CV is recommended. In the CV, CE was identical (around unity) for more volatile species (e.g. NH4NO3) and comparable to or higher than the SV for less-volatile species (e.g. (NH4)2SO4), demonstrating an improvement in CE for laboratory inorganic species in the CV. The detected relative intensities of fragments of NO3 and SO4 species observed with the CV are different from those observed with the SV, and are consistent with additional thermal decomposition arising from the increased residence time and multiple collisions. Increased residence times with the CV also lead to broader particle size distribution measurements than with the SV. A method for estimating whether pure species will be detected in AMS sizing mode is proposed. Production of CO2(g) from sampled nitrate on the vapourizer surface, which has been reported for the SV, is negligible for the CV for NH4NO3 and comparable to the SV for NaNO3. . We observe an extremely consistent fragmentation for ammonium compared to very large changes for the

Aerosol scattering and absorption modulation transfer function

NASA Astrophysics Data System (ADS)

Sadot, Dan; Kopeika, Norman S.

1993-08-01

Recent experimental measurements of overall atmospheric modulation transfer function (MTF) indicate significant difference between the turbulence and overall atmospheric MTFs, except often at midday when turbulence is strong. We suggest here a physical explanation for those results which essentially relates to what we call a practical instrumentation-based atmospheric aerosol MTF which is a modification of the classical aerosol MTF theory. It is shown that system field-of-view and dynamic range affect strongly aerosol and overall atmospheric MTFs. It is often necessary to choose between MTF and SNR depending upon dynamic range requirements. Also, a new approach regarding aerosol absorption is presented. It is shown that aerosol-absorbed irradiance is spatial frequency dependent and enhances the degradation in image quality arising from received scattered light. This is most relevant for thermal imaging. An analytically corrected model for the aerosol MTF is presented which is relevant for imaging. An important conclusion is that the aerosol MTF is often the dominant part in the actual overall atmospheric MTF all across the optical spectral region.

Aerosol optical properties and direct radiative forcing based on measurements from the China Aerosol Remote Sensing Network (CARSNET) in eastern China

NASA Astrophysics Data System (ADS)

Che, Huizheng; Qi, Bing; Zhao, Hujia; Xia, Xiangao; Eck, Thomas F.; Goloub, Philippe; Dubovik, Oleg; Estelles, Victor; Cuevas-Agulló, Emilio; Blarel, Luc; Wu, Yunfei; Zhu, Jun; Du, Rongguang; Wang, Yaqiang; Wang, Hong; Gui, Ke; Yu, Jie; Zheng, Yu; Sun, Tianze; Chen, Quanliang; Shi, Guangyu; Zhang, Xiaoye

2018-01-01

Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71-0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (˜ 0.40-0.60) than in January and February (0.71-0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ˜ 0.04-0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was -93 ± 44 to -79 ± 39 W m-2 at the Earth's surface and ˜ -40 W m-2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80°) under cloud-free conditions. The fine mode

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.

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

Simultaneous reductions in emissions of black carbon and co-emitted species will weaken the aerosol net cooling effect

NASA Astrophysics Data System (ADS)

Wang, Z. L.; Zhang, H.; Zhang, X. Y.

2015-04-01

Black carbon (BC), a distinct type of carbonaceous material formed from the incomplete combustion of fossil and biomass based fuels under certain conditions, can interact with solar radiation and clouds through its strong light-absorption ability, thereby warming the Earth's climate system. Some studies have even suggested that global warming could be slowed down in the short term by eliminating BC emission due to its short lifetime. In this study, we estimate the influence of removing some sources of BC and other co-emitted species on the aerosol radiative effect by using an aerosol-climate atmosphere-only model BCC_AGCM2.0.1_CUACE/Aero with prescribed sea surface temperature and sea ice cover, in combination with the aerosol emissions from the Representative Concentration Pathways (RCPs) scenarios. We find that the global annual mean aerosol net cooling effect at the top of the atmosphere (TOA) will be enhanced by 0.12 W m-2 compared with recent past year 2000 levels if the emissions of only BC are reduced to the level projected for 2100 based on the RCP2.6 scenario. This will be beneficial~for the mitigation of global warming. However, both aerosol negative direct and indirect radiative effects are weakened when BC and its co-emitted species (sulfur dioxide and organic carbon) are simultaneously reduced. Relative to year 2000 levels, the global annual mean aerosol net cooling effect at the TOA will be weakened by 1.7-2.0 W m-2 if the emissions of all these aerosols are decreased to the levels projected for 2100 in different ways based on the RCP2.6, RCP4.5, and RCP8.5 scenarios. Because there are no effective ways to remove the BC exclusively without influencing the other co-emitted components, our results therefore indicate that a reduction in BC emission can lead to an unexpected warming on the Earth's climate system in the future.

Exploring the ionic strength effects on the photochemical degradation of pyruvic acid in atmospheric deliquescent aerosol particles

NASA Astrophysics Data System (ADS)

Mekic, Majda; Brigante, Marcello; Vione, Davide; Gligorovski, Sasho

2018-07-01

There is increasing evidence that aqueous-phase atmospheric chemistry is an important source of secondary organic aerosols (SOA), but the related processes are currently not adequately represented in atmospheric chemistry models. Here we show that the absorption spectrum of pyruvic acid (PA) exhibits both an increase of the absorption intensity and a red shift of 13 nm while going from a dilute aqueous phase to a solution containing the inert salt sodium perchlorate (5M NaClO4). If this phenomenon turns out to be more general, many compounds that do not absorb actinic light in clouds and fog could become light absorbers at elevated salt concentrations in aerosol deliquescent particles. Compared to the direct photolysis of PA in dilute aqueous solution, the photolysis rate is increased by three times at high ionic strength (5M NaClO4). Such a considerable enhancement can be rationalized in the framework of the Debye-McAulay approach for reactions of ionic + neutral (or neutral + neutral) species, considering that the PA direct photolysis likely involves interaction between the photogenerated triplet state and water. This is, to our knowledge, the first report of a significant effect of the ionic strength on the rate of an atmospheric photochemical reaction. The phenomenon has important implications for the fate of PA and, potentially, of other organic compounds in atmospheric aerosol deliquescent particles.

Tropospheric Aerosols

NASA Astrophysics Data System (ADS)

Buseck, P. R.; Schwartz, S. E.

2003-12-01

�m, PM10=1.1 μg m-3; estimated coefficient of light scattering by particulate matter, σep, at 570 nm=12 Mm-1). (b) High aerosol concentration (PM2.5=43.9 μg m-3; PM10=83.4 μg m-3; estimated σep at 570 nm=245 Mm-1) (reproduced by permission of National Park Service, 2002). Although comprising only a small fraction of the mass of Earth's atmosphere, aerosol particles are highly important constituents of the atmosphere. Special interest has focused on aerosols in the troposphere, the lowest part of the atmosphere, extending from the land or ocean surface typically to ˜8 km at high latitudes, ˜12 km in mid-latitudes, and ˜16 km at low latitudes. That interest arises in large part because of the importance of aerosol particles in geophysical processes, human health impairment through inhalation, environmental effects through deposition, visibility degradation, and influences on atmospheric radiation and climate.Anthropogenic aerosols are thought to exert a substantial influence on Earth's climate, and the need to quantify this influence has sparked much of the current interest in and research on tropospheric aerosols. The principal mechanisms by which aerosols influence the Earth radiation budget are scattering and absorbing solar radiation (the so-called "direct effects") and modifying clouds and precipitation, thereby affecting both radiation and hydrology (the so-called "indirect effects"). Light scattering by aerosols increases the brightness of the planet, producing a cooling influence. Light-absorbing aerosols such as black carbon exert a warming influence. Aerosols increase the reflectivity of clouds, another cooling influence. These radiative influences are quantified as forcings, where a forcing is a perturbation to the energy balance of the atmosphere-Earth system, expressed in units of watts per square meter, W m-2. A warming influence is denoted a positive forcing, and a cooling influence, negative. The radiative direct and indirect forcings by

Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

NASA Astrophysics Data System (ADS)

Persad, Geeta Gayatri

Short-lived anthropogenic aerosols are concentrated in regions of high human activity, where they interact with radiation and clouds, causing horizontally heterogeneous radiative forcing between polluted and unpolluted regions. Aerosols can absorb shortwave energy in the atmosphere, but deplete it at the surface, producing opposite radiative perturbations between the surface and atmosphere. This thesis investigates climate and policy implications of this horizontal and vertical heterogeneity of anthropogenic aerosol forcing, employing the Geophysical Fluid Dynamics Laboratory's AM2.1 and AM3 models, both at a global scale and using East Asia as a regional case study. The degree of difference between spatial patterns of climate change due to heterogeneous aerosol forcing versus homogeneous greenhouse gas forcing deeply impacts the detection, attribution, and prediction of regional climate change. This dissertation addresses a gap in current understanding of these two forcings' response pattern development, using AM2.1 historical forcing simulations. The results indicate that fast atmospheric and land-surface processes alone substantially homogenize the global pattern of surface energy flux response to heterogeneous aerosol forcing. Aerosols' vertical redistribution of energy significantly impacts regional climate, but is incompletely understood. It is newly identified here, via observations and historical and idealized forcing simulations, that increased aerosol-driven atmospheric absorption may explain half of East Asia's recent surface insolation decline. Further, aerosols' surface and atmospheric effects counteract each other regionally---atmospheric heating enhances summer monsoon circulation, while surface dimming suppresses it---but absorbing aerosols' combined effects reduce summer monsoon rainfall. This thesis constitutes the first vertical decomposition of aerosols' impacts in this high-emissions region and elucidates the monsoonal response to aerosols

Critical Reflectance Derived from MODIS: Application for the Retrieval of Aerosol Absorption over Desert Regions

NASA Technical Reports Server (NTRS)

Wells, Kelley C.; Martins, J. Vanderlei; Remer, Lorraine A.; Kreidenweis, Sonia M.; Stephens, Graeme L.

2012-01-01

Aerosols are tiny suspended particles in the atmosphere that scatter and absorb sunlight. Smoke particles are aerosols, as are sea salt, particulate pollution and airborne dust. When you look down at the earth from space sometimes you can see vast palls of whitish smoke or brownish dust being transported by winds. The reason that you can see these aerosols is because they are reflecting incoming sunlight back to the view in space. The reason for the difference in color between the different types of aerosol is that the particles arc also absorbing sunlight at different wavelengths. Dust appears brownish or reddish because it absorbs light in the blue wavelengths and scatters more reddish light to space, Knowing how much light is scattered versus how much is absorbed, and knowin that as a function of wavelength is essential to being able to quantify the role aerosols play in the energy balance of the earth and in climate change. It is not easy measuring the absorption properties of aerosols when they are suspended in the atmosphere. People have been doing this one substance at a time in the laboratory, but substances mix when they are in the atmosphere and the net absorption effect of all the particles in a column of air is a goal of remote sensing that has not yet been completely successful. In this paper we use a technique based on observing the point at which aerosols change from brightening the surface beneath to darkening it. If aerosols brighten a surface. they must scatter more light to space. If they darken the surface. they must be absorbing more. That cross over point is called the critical reflectance and in this paper we show that critical reflectance is a monotonic function of the intrinsic absorption properties of the particles. This parameter we call the single scattering albedo. We apply the technique to MODIS imagery over the Sahara and Sahel regions to retrieve the single scattering albedo in seven wavelengths, compare these retrievals to ground

Changing transport processes in the stratosphere by radiative heating of sulfate aerosols

NASA Astrophysics Data System (ADS)

Niemeier, Ulrike; Schmidt, Hauke

2017-12-01

The injection of sulfur dioxide (SO2) into the stratosphere to form an artificial stratospheric aerosol layer is discussed as an option for solar radiation management. Sulfate aerosol scatters solar radiation and absorbs infrared radiation, which warms the stratospheric sulfur layer. Simulations with the general circulation model ECHAM5-HAM, including aerosol microphysics, show consequences of this warming, including changes of the quasi-biennial oscillation (QBO) in the tropics. The QBO slows down after an injection of 4 Tg(S) yr-1 and completely shuts down after an injection of 8 Tg(S) yr-1. Transport of species in the tropics and sub-tropics depends on the phase of the QBO. Consequently, the heated aerosol layer not only impacts the oscillation of the QBO but also the meridional transport of the sulfate aerosols. The stronger the injection, the stronger the heating and the simulated impact on the QBO and equatorial wind systems. With increasing injection rate the velocity of the equatorial jet streams increases, and the less sulfate is transported out of the tropics. This reduces the global distribution of sulfate and decreases the radiative forcing efficiency of the aerosol layer by 10 to 14 % compared to simulations with low vertical resolution and without generated QBO. Increasing the height of the injection increases the radiative forcing only for injection rates below 10 Tg(S) yr-1 (8-18 %), a much smaller value than the 50 % calculated previously. Stronger injection rates at higher levels even result in smaller forcing than the injections at lower levels.

The complex refractive index of atmospheric and model humic-like substances (HULIS) retrieved by a cavity ring down aerosol spectrometer (CRD-AS).

PubMed

Dinar, E; Riziq, A Abo; Spindler, C; Erlick, C; Kiss, G; Rudich, Y

2008-01-01

Atmospheric aerosols absorb and reflect solar radiation causing surface cooling and heating of the atmosphere. The interaction between aerosols and radiation depends on their complex index of refraction, which is related to the particles' chemical composition. The contribution of light absorbing organic compounds, such as HUmic-LIke Substances (HULIS) to aerosol scattering and absorption is among the largest uncertainties in assessing the direct effect of aerosols on climate. Using a Cavity Ring Down Aerosol Spectrometer (CRD-AS), the complex index of refraction of aerosols containing HULIS extracted from pollution, smoke, and rural continental aerosols, and molecular weight-fractionated fulvic acid was measured at 390 nm and 532 nm. The imaginary part of the refractive index (absorption) substantially increases towards the UV range with increasing molecular weight and aromaticity. At both wavelengths, HULIS extracted from pollution and smoke particles absorb more than HULIS from the rural aerosol. Sensitivity calculations for a pollution-type aerosol containing ammonium sulfate, organic carbon (HULIS), and soot suggests that accounting for absorption by HULIS leads in most cases to a significant decrease in the single scattering albedo and to a significant increase in aerosol radiative forcing efficiency, towards more atmospheric absorption and heating. This indicates that HULIS in biomass smoke and pollution aerosols, in addition to black carbon, can contribute significantly to light absorption in the ultraviolet and visible spectral regions.

Light absorption of secondary organic aerosol: Composition and contribution of nitro-aromatic compounds

EPA Science Inventory

Secondary organic aerosol (SOA) might affect the atmospheric radiation balance through absorbing light at shorter visible and UV wavelengths. However, the composition and optical properties of light-absorbing SOA is poorly understood. In this work, SOA filter samples were collect...

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

ACCURATE: Influence of Cloud Layers and Aerosol on Infrared Laser Occultation Signals for Sensing of Greenhouse Gases

NASA Astrophysics Data System (ADS)

Proschek, V.; Schweitzer, S.; Emde, C.; Ladstädter, F.; Fritzer, J.; Kirchengast, G.

2009-04-01

ACCURATE (Atmospheric Climate and Chemistry in the UTLS Region And climate Trends Explorer), a new climate satellite concept, enables simultaneous measurement of profiles of greenhouse gases, isotopes, wind and thermodynamic variables from Low Earth Orbit (LEO) satellites. The measurement principle applied is a combination of the novel LEO-LEO infrared laser occultation (LIO) technique and the well-studied but not yet flown LEO-LEO microwave occultation (LMO) technique. As intrinsic to the space-borne occultation technique, the measurements are evenly distributed around the world, have high vertical resolution and high accuracy and are stable over long time periods. The LIO uses near-monochromatic signals in the short-wave infrared range (~2-2.5 m in the case of ACCURATE) which are absorbed by various trace species in the Earth's atmosphere. From signal transmission measurements, profiles of the concentration of the absorbing species can be derived given that temperature and pressure are accurately known from LMO. The current ACCURATE mission design is arranged for the measurement of six greenhouse gases (H2O, CO2, CH4, N2O, O3, CO) and four isotopes (13CO2, C18OO, HDO, H218O) with focus on the upper troposphere/lower stratosphere region (UTLS, 5-35 km). Wind speed in line-of-sight can be derived from a line-symmetric transmission difference which is caused by wind-induced Doppler shift. By-products are information on cloud layering, aerosol extinction and scintillation strength. This contribution presents an overview on the ACCURATE mission design and the expected accuracy of retrieved atmospheric variables and further focuses on the influence of clouds and aerosols on propagating LIO signals. Special emphasis will be given to sub-visible cirrus clouds which are semi-transparent to infrared signals. A simple frequency dependent cloud extinction parametrization was included into the occultation propagation software EGOPS and evaluated against results of the

Remote sensing of aerosols by synergy of caliop and modis

NASA Astrophysics Data System (ADS)

Kudo, Rei; Nishizawa, Tomoaki; Higurashi, Akiko; Oikawa, Eiji

2018-04-01

For the monitoring of the global 3-D distribution of aerosol components, we developed the method to retrieve the vertical profiles of water-soluble, light absorbing carbonaceous, dust, and sea salt particles by the synergy of CALIOP and MODIS data. The aerosol product from the synergistic method is expected to be better than the individual products of CALIOP and MODIS. We applied the method to the biomass-burning event in Africa and the dust event in West Asia. The reasonable results were obtained; the much amount of the water-soluble and light absorbing carbonaceous particles were estimated in the biomass-burning event, and the dust particles were estimated in the dust event.

Can Aerosol Offset Urban Heat Island Effect?

NASA Astrophysics Data System (ADS)

Jin, M. S.; Shepherd, J. M.

2009-12-01

The Urban Heat Island effect (UHI) refers to urban skin or air temperature exceeding the temperatures in surrounding non-urban regions. In a warming climate, the UHI may intensify extreme heat waves and consequently cause significant health and energy problems. Aerosols reduce surface insolation via the direct effect, namely, scattering and absorbing sunlight in the atmosphere. Combining the National Aeronautics and Space Administration (NASA) AERONET (AErosol RObotic NETwork) observations over large cities together with Weather Research and Forecasting Model (WRF) simulations, we find that the aerosol direct reduction of surface insolation range from 40-100 Wm-2, depending on seasonality and aerosol loads. As a result, surface skin temperature can be reduced by 1-2C while 2-m surface air temperature by 0.5-1C. This study suggests that the aerosol direct effect is a competing mechanism for the urban heat island effect (UHI). More importantly, both aerosol and urban land cover effects must be adequately represented in meteorological and climate modeling systems in order to properly characterize urban surface energy budgets and UHI.

Absorption Properties of Mediterranean Aerosols Obtained from Multi-year Ground-based and Satellite Remote Sensing Observations

NASA Technical Reports Server (NTRS)

Mallet, M.; Dubovik, O.; Nabat, P.; Dulac, F.; Kahn, R.; Sciare, J.; Paronis, D.; Leon, J. F.

2013-01-01

Aerosol absorption properties are of high importance to assess aerosol impact on regional climate. This study presents an analysis of aerosol absorption products obtained over the Mediterranean Basin or land stations in the region from multi-year ground-based AERONET and satellite observations with a focus on the Absorbing Aerosol Optical Depth (AAOD), Single Scattering Albedo (SSA) and their spectral dependence. The AAOD and Absorption Angstrom Exponent (AAE) data set is composed of daily averaged AERONET level 2 data from a total of 22 Mediterranean stations having long time series, mainly under the influence of urban-industrial aerosols and/or soil dust. This data set covers the 17 yr period 1996-2012 with most data being from 2003-2011 (approximately 89 percent of level-2 AAOD data). Since AERONET level-2 absorption products require a high aerosol load (AOD at 440 nm greater than 0.4), which is most often related to the presence of desert dust, we also consider level-1.5 SSA data, despite their higher uncertainty, and filter out data with an Angstrom exponent less than 1.0 in order to study absorption by carbonaceous aerosols. The SSA data set includes both AERONET level-2 and satellite level-3 products. Satellite-derived SSA data considered are monthly level 3 products mapped at the regional scale for the spring and summer seasons that exhibit the largest aerosol loads. The satellite SSA dataset includes the following products: (i) Multi-angle Imaging SpectroRadiometer (MISR) over 2000-2011, (ii) Ozone Monitoring Instrument (OMI) near-UV algorithm over 2004-2010, and (iii) MODerate resolution Imaging Spectroradiometer (MODIS) Deep-Blue algorithm over 2005-2011, derived only over land in dusty conditions. Sun-photometer observations show that values of AAOD at 440 nm vary between 0.024 +/- 0.01 (resp. 0.040 +/- 0.01) and 0.050 +/- 0.01 (0.055 +/- 0.01) for urban (dusty) sites. Analysis shows that the Mediterranean urban-industrial aerosols appear "moderately

Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

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

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS)more » ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. As a result, controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures

Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

DOE PAGES

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; ...

2016-07-25

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS)more » ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. As a result, controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures

Ion mobility spectrometry-mass spectrometry (IMS-MS) for on- and offline analysis of atmospheric gas and aerosol species

NASA Astrophysics Data System (ADS)

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; Budisulistiorini, Sri H.; Zhang, Haofei; Surratt, Jason D.; Knochenmuss, Richard; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis; Canagaratna, Manjula R.

2016-07-01

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS-MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS-MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI-IMS-MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS-MS signals are consistent with laboratory IMS-MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS-MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS-MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the

Black carbon's contribution to aerosol absorption optical depth over S. Korea

NASA Astrophysics Data System (ADS)

Lamb, K.; Perring, A. E.; Beyersdorf, A. J.; Anderson, B. E.; Segal-Rosenhaimer, M.; Redemann, J.; Holben, B. N.; Schwarz, J. P.

2017-12-01

Aerosol absorption optical depth (AAOD) monitored by ground-based sites (AERONET, SKYNET, etc.) is used to constrain climate radiative forcing from black carbon (BC) and other absorbing aerosols in global models, but few validation studies between in situ aerosol measurements and ground-based AAOD exist. AAOD is affected by aerosol size distributions, composition, mixing state, and morphology. Megacities provide appealing test cases for this type of study due to their association with very high concentrations of anthropogenic aerosols. During the KORUS-AQ campaign in S. Korea, which took place in late spring and early summer of 2016, in situ aircraft measurements over the Seoul Metropolitan Area and Taehwa Research Forest (downwind of Seoul) were repeated three times per flight over a 6 week period, providing significant temporal coverage of vertically resolved aerosol properties influenced by different meteorological conditions and sources. Measurements aboard the NASA DC-8 by the NOAA Humidified Dual Single Particle Soot Photometers (HD-SP2) quantified BC mass, size distributions, mixing state, and the hygroscopicity of BC containing aerosols. The in situ BC mass vertical profiles are combined with estimated absorption enhancement calculated from observed optical size and hygroscopicity using Mie theory, and then integrated over the depth of the profile to calculate BC's contribution to AAOD. Along with bulk aerosol size distributions and hygroscopicity, bulk absorbing aerosol optical properties, and on-board sky radiance measurements, these measurements are compared with ground-based AERONET site measurements of AAOD to evaluate closure between in situ vertical profiles of BC and AAOD measurements. This study will provide constraints on the relative importance of BC (including lensing and hygroscopicity effects) and non-BC components to AAOD over S. Korea.

Atmospheric Teleconnection over Eurasia Induced by Aerosol Radiative Forcing During Boreal Spring

NASA Technical Reports Server (NTRS)

Kim, Maeng-Ki; Lau, K. M.; Chin, Mian; Kim, Kyu-Myong; Sud, Y. C.; Walker, Greg K.

2005-01-01

The direct effects of aerosols on global and regional climate during boreal spring are investigated based on simulations using the NASA Global Modeling and Assimilation Office (GMAO) finite-volume general circulation model (fvGCM) with Microphyics of clouds in Relaxed Arakawa Schubert Scheme (McRAS). The aerosol loading are prescribed from three-dimensional monthly distribution of tropospheric aerosols viz., sulfate, black carbon, organic carbon, soil dust, and sea salt from output of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol extinction coefficient, single scattering albedo, and asymmetric factor are computed as wavelength-dependent radiative forcing in the radiative transfer scheme of the fvGCM, and as a function of the aerosol loading and ambient relative humidity. We find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excites a planetary scale teleconnection pattern in sea level pressure, temperature and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, i.e., South Asia, East Asia, and northern and western Africa. Additionally, atmospheric heating is found in regions with large loading of dust (over Northern Africa, and Middle East), and black carbon (over South-East Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east-west dipole anomaly with strong cooling over the Caspian Sea, and warming over central and northeastern Asia, where aerosol concentration are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes

Reducing the Uncertainties in Direct Aerosol Radiative Forcing

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.

2011-01-01

Airborne particles, which include desert and soil dust, wildfire smoke, sea salt, volcanic ash, black carbon, natural and anthropogenic sulfate, nitrate, and organic aerosol, affect Earth's climate, in part by reflecting and absorbing sunlight. This paper reviews current status, and evaluates future prospects for reducing the uncertainty aerosols contribute to the energy budget of Earth, which at present represents a leading factor limiting the quality of climate predictions. Information from satellites is critical for this work, because they provide frequent, global coverage of the diverse and variable atmospheric aerosol load. Both aerosol amount and type must be determined. Satellites are very close to measuring aerosol amount at the level-of-accuracy needed, but aerosol type, especially how bright the airborne particles are, cannot be constrained adequately by current techniques. However, satellite instruments can map out aerosol air mass type, which is a qualitative classification rather than a quantitative measurement, and targeted suborbital measurements can provide the required particle property detail. So combining satellite and suborbital measurements, and then using this combination to constrain climate models, will produce a major advance in climate prediction.

Cloud Cover Increase with Increasing Aerosol Absorptivity: A Counterexample to the Conventional Semidirect Aerosol Effect

NASA Technical Reports Server (NTRS)

Perlwitz, Jan; Miller, Ron L.

2010-01-01

We reexamine the aerosol semidirect effect using a general circulation model and four cases of the single-scattering albedo of dust aerosols. Contrary to the expected decrease in low cloud cover due to heating by tropospheric aerosols, we find a significant increase with increasing absorptivity of soil dust particles in regions with high dust load, except during Northern Hemisphere winter. The strongest sensitivity of cloud cover to dust absorption is found over land during Northern Hemisphere summer. Here even medium and high cloud cover increase where the dust load is highest. The cloud cover change is directly linked to the change in relative humidity in the troposphere as a result of contrasting changes in specific humidity and temperature. More absorption by aerosols leads to larger diabatic heating and increased warming of the column, decreasing relative humidity. However, a corresponding increase in the specific humidity exceeds the temperature effect on relative humidity. The net effect is more low cloud cover with increasing aerosol absorption. The higher specific humidity where cloud cover strongly increases is attributed to an enhanced convergence of moisture driven by dust radiative heating. Although in some areas our model exhibits a reduction of low cloud cover due to aerosol heating consistent with the conventional description of the semidirect effect, we conclude that the link between aerosols and clouds is more varied, depending also on changes in the atmospheric circulation and the specific humidity induced by the aerosols. Other absorbing aerosols such as black carbon are expected to have a similar effect.

Observational Evidence of Impacts of Aerosols on Seasonal-to-Interannual Variability of the Asian Monsoon

NASA Technical Reports Server (NTRS)

Lau, K.-M.; Kim, K.-M.; Hsu, N. C.

2006-01-01

Observational evidences are presented showing that the Indian subcontinent and surrounding regions are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle. Increased loading of absorbing aerosols over the Indo-Gangetic Plain in April-May is associated with a) increased heating of the upper troposphere over the Tibetan Plateau, b) an advance of the monsoon rainy season, and c) subsequent enhancement of monsoon rainfall over the South Asia subcontinent, and reduction over East Asia. Also presented are radiative transfer calculations showing how differential solar absorption by aerosols over bright surface (desert or snow cover land) compared to dark surface (vegetated land and ocean), may be instrumental in triggering an aerosol-monsoon large-scale circulation and water cycle feedback, consistent with the elevated heat pump hypothesis (Lau et al. 2006).

Evaluation of the new capture vapourizer for aerosol mass spectrometers (AMS) through laboratory studies of inorganic species

DOE PAGES

Hu, Weiwei; Campuzano-Jost, Pedro; Day, Douglas A.; ...

2017-08-15

Aerosol mass spectrometers (AMSs) and Aerosol Chemical Speciation Monitors (ACSMs) commercialized by Aerodyne are widely used to measure the non-refractory species in submicron particles. With the standard vapourizer (SV) that is installed in all commercial instruments to date, the quantification of ambient aerosol mass concentration requires the use of the collection efficiency (CE) to correct for the loss of particles due to bounce. A new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction. Two high-resolution AMS instruments, one with a SV and one with a CV, were operated side by side in themore » laboratory. Four standard species, NH 4NO 3, NaNO 3, (NH 4) 2SO 4 and NH 4Cl, which typically constitute the majority of the mass of ambient submicron inorganic species, are studied. The effect of vapourizer temperature ( T v ∼ 200–800 °C) on the detected fragments, CE and size distributions are investigated. A T v of 500–550 °C for the CV is recommended. In the CV, CE was identical (around unity) for more volatile species (e.g. NH 4NO 3) and comparable to or higher than the SV for less-volatile species (e.g. (NH 4) 2SO 4), demonstrating an improvement in CE for laboratory inorganic species in the CV. The detected relative intensities of fragments of NO 3 and SO 4 species observed with the CV are different from those observed with the SV, and are consistent with additional thermal decomposition arising from the increased residence time and multiple collisions. Increased residence times with the CV also lead to broader particle size distribution measurements than with the SV. A method for estimating whether pure species will be detected in AMS sizing mode is proposed. Production of CO 2(g) from sampled nitrate on the vapourizer surface, which has been reported for the SV, is negligible for the CV for NH 4NO 3 and comparable to the SV for NaNO 3. . We observe an extremely consistent fragmentation for

Evaluation of the new capture vapourizer for aerosol mass spectrometers (AMS) through laboratory studies of inorganic species

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

Hu, Weiwei; Campuzano-Jost, Pedro; Day, Douglas A.

Aerosol mass spectrometers (AMSs) and Aerosol Chemical Speciation Monitors (ACSMs) commercialized by Aerodyne are widely used to measure the non-refractory species in submicron particles. With the standard vapourizer (SV) that is installed in all commercial instruments to date, the quantification of ambient aerosol mass concentration requires the use of the collection efficiency (CE) to correct for the loss of particles due to bounce. A new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction. Two high-resolution AMS instruments, one with a SV and one with a CV, were operated side by side in themore » laboratory. Four standard species, NH 4NO 3, NaNO 3, (NH 4) 2SO 4 and NH 4Cl, which typically constitute the majority of the mass of ambient submicron inorganic species, are studied. The effect of vapourizer temperature ( T v ∼ 200–800 °C) on the detected fragments, CE and size distributions are investigated. A T v of 500–550 °C for the CV is recommended. In the CV, CE was identical (around unity) for more volatile species (e.g. NH 4NO 3) and comparable to or higher than the SV for less-volatile species (e.g. (NH 4) 2SO 4), demonstrating an improvement in CE for laboratory inorganic species in the CV. The detected relative intensities of fragments of NO 3 and SO 4 species observed with the CV are different from those observed with the SV, and are consistent with additional thermal decomposition arising from the increased residence time and multiple collisions. Increased residence times with the CV also lead to broader particle size distribution measurements than with the SV. A method for estimating whether pure species will be detected in AMS sizing mode is proposed. Production of CO 2(g) from sampled nitrate on the vapourizer surface, which has been reported for the SV, is negligible for the CV for NH 4NO 3 and comparable to the SV for NaNO 3. . We observe an extremely consistent fragmentation for

Enhanced Surface Warming and Accelerated Snow Melt in the Himalayas and Tibetan Plateau Induced by Absorbing Aerosols

NASA Technical Reports Server (NTRS)

Lau, William K.; Kim, Maeng-Ki; Kim, Kyu-Myong; Lee, Woo-Seop

2010-01-01

Numerical experiments with the NASA finite-volume general circulation model show that heating of the atmosphere by dust and black carbon can lead to widespread enhanced warming over the Tibetan Plateau (TP) and accelerated snow melt in the western TP and Himalayas. During the boreal spring, a thick aerosol layer, composed mainly of dust transported from adjacent deserts and black carbon from local emissions, builds up over the Indo-Gangetic Plain, against the foothills of the Himalaya and the TP. The aerosol layer, which extends from the surface to high elevation (approx.5 km), heats the mid-troposphere by absorbing solar radiation. The heating produces an atmospheric dynamical feedback the so-called elevated-heat-pump (EHP) effect, which increases moisture, cloudiness, and deep convection over northern India, as well as enhancing the rate of snow melt in the Himalayas and TP. The accelerated melting of snow is mostly confined to the western TP, first slowly in early April and then rapidly from early to mid-May. The snow cover remains reduced from mid-May through early June. The accelerated snow melt is accompanied by similar phases of enhanced warming of the atmosphere-land system of the TP, with the atmospheric warming leading the surface warming by several days. Surface energy balance analysis shows that the short-wave and long-wave surface radiative fluxes strongly offset each other, and are largely regulated by the changes in cloudiness and moisture over the TP. The slow melting phase in April is initiated by an effective transfer of sensible heat from a warmer atmosphere to land. The rapid melting phase in May is due to an evaporation-snow-land feedback coupled to an increase in atmospheric moisture over the TP induced by the EHP effect.

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

NASA Astrophysics Data System (ADS)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-12-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

NASA Astrophysics Data System (ADS)

Logan, Timothy S.

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

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.

Observation of hydration of single, modified carbon aerosols

NASA Technical Reports Server (NTRS)

Wyslouzil, B. E.; Carleton, K. L.; Sonnenfroh, D. M.; Rawlins, W. T.; Arnold, S.

1994-01-01

We have compared the hydration behavior of single carbon particles that have been treated by exposure to gaseous H2SO4 with that of untreated particles. Untreated carbon particles did not hydrate as the relative humidity varied from 0 to 80% at 23 C. In contrast, treated particles hydrated under subsaturation conditions; mass increases of up to 30% were observed. The mass increase is consistent with sulfuric acid equilibration with the ambient relative humidity in the presence of inert carbon. For the samples studied, the average amount of absorbed acid was 14% +/- 6% by weight, which corresponds to a surface coverage of approximately 0.1 monolayer. The mass fraction of surface-absorbed acid is comparable to the soluble mass fraction observed by Whitefield et al. (1993) in jet aircraft engine aerosols. Estimates indicate this mass fraction corresponds to 0.1% of the available SO2 exiting an aircraft engine ending up as H2SO4 on the carbon aerosol. If this heterogeneous process occurs early enough in the exhaust plume, it may compete with homogeneous nucleation as a mechanism for producing sulfuric acid rich aerosols.

Global sensing of gaseous and aerosol trace species using automated instrumentation on 747 airliners

NASA Technical Reports Server (NTRS)

Perkins, P. J.; Papathakos, L. C.

1977-01-01

The Global Atmospheric Sampling Program (GASP) by NASA is collecting and analyzing data on gaseous and aerosol trace species in the upper troposphere and lower stratosphere. Measurements are obtained from automated systems installed on four 747 airliners flying global air routes. Advances were made in airborne sampling instrumentation. Improved instruments and analysis techniques are providing an expanding data base for trace species including ozone, carbon monoxide, water vapor, condensation nuclei and mass concentrations of sulfates and nitrates. Simultaneous measurements of several trace species obtained frequently can be used to uniquely identify the source of the air mass as being typically tropospheric or stratospheric. A quantitative understanding of the tropospheric-stratospheric exchange processes leads to better knowledge of the atmospheric impact of pollution through the development of improved simulation models of the atmosphere.

Toward Creating A Global Retrospective Climatology of Aerosol Properties

NASA Technical Reports Server (NTRS)

Curran, Robert J.; Mishchenko, Michael I.; Hansen, James E. (Technical Monitor)

2000-01-01

Tropospheric aerosols are thought to cause a significant direct and indirect climate forcing, but the magnitude of this forcing remains highly uncertain because of poor knowledge of global aerosol characteristics and their temporal changes. The standard long-term global product, the one-channel Advanced Very-High-Resolution Radiometer (AVHRR) aerosol optical thickness over the ocean, relies on a single predefined aerosol model and can be inaccurate in many cases. Furthermore, it provides no information on aerosol column number density, thus making it impossible to estimate the indirect aerosol effect on climate. Total Ozone Mapping Spectrometer (TOMS) data can be used to detect absorbing aerosols over land, but are insensitive to aerosols located below one kilometer. It is thus clear that innovative approaches must be employed in order to extract a more quantitative and accurate aerosol climatology from available satellite and other measurements, thus enabling more reliable estimates of the direct and indirect aerosol forcings. The Global Aerosol Climatology Project (GACP) was established in 1998 as part of the Global Energy and Water Cycle Experiment (GEWEX). Its main objective is to analyze satellite radiance measurements and field observations to infer the global distribution of aerosols, their properties, and their seasonal and interannual variations. The overall goal is to develop advanced global aerosol climatologies for the period of satellite data and to make the aerosol climatologies broadly available through the GACP web site.

Antarctic aerosols - A review

NASA Astrophysics Data System (ADS)

Shaw, Glenn E.

1988-02-01

Tropospheric aerosols with the diameter range of half a micron reside in the atmosphere for tens of days and teleconnect Antarctica with other regions by transport that reaches planetary scales of distances; thus, the aerosol on the Antarctic ice represents 'memory modules' of events that took place at regions separated from Antarctica by tens of thousands of kilometers. In terms of aerosol mass, the aerosol species include insoluble crustal products (less than 5 percent), transported sea-salt residues (highly variable but averaging about 10 percent), Ni-rich meteoric material, and anomalously enriched material with an unknown origin. Most (70-90 percent by mass) of the aerosol over the Antarctic ice shield, however, is the 'natural acid sulfate aerosol', apparently deriving from biological processes taking place in the surrounding oceans.

Optical Properties of Black and Brown Carbon Aerosols from Laboratory Combustion of Wildland Fuels

NASA Astrophysics Data System (ADS)

Beres, N. D.; Molzan, J.

2015-12-01

Aerosol light absorption in the solar spectral region (300 nm - 2300 nm) of the atmosphere is key for the direct aerosol radiative forcing, which is determined by aerosol single scattering albedo (SSA), asymmetry parameter, and by the albedo of the underlying surface. SSA is of key importance for the sign and quantity of aerosol direct radiative forcing; that is, does the aerosol make the earth look darker (heating) or whiter (cooling)? In addition, these optical properties are needed for satellite retrievals of aerosol optical depth and properties. During wildland fires, aerosol optical absorption is largely determined by black carbon (BC) and brown carbon (BrC) emissions. BC is strongly absorbing throughout the solar spectrum, while BrC absorption strongly increases toward shorter wavelength and can be neglected in the red and infrared. Optical properties of BrC emitted from wildland fires are poorly understood and need to be studied as function of fuel type and moisture content and combustion conditions. While much more is known about BC optical properties, knowledge for the ultraviolet (UV) spectral region is still lacking and critically needed for satellite remote sensing (e.g., TOMS, OMI) and for modeling of tropospheric photochemistry. Here, a project to better characterize biomass burning aerosol optical properties is described. It utilizes a laboratory biomass combustion chamber to generate aerosols through combustion of different wildland fuels of global and regional importance. Combustion aerosol optics is characterized with an integrating nephelometer to measure aerosol light scattering and a photoacoustic instrument to measure aerosol light absorption. These measurements will yield optical properties that are needed to improve qualitative and quantitative understanding of aerosol radiative forcing and satellite retrievals for absorbing carbonaceous aerosols from combustion of wildland fuels.

Case study of modeled aerosol optical properties during the SAFARI 2000 campaign

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

Kuzmanoski, Maja; Box, Michael A.; Schmid, Beat

2007-08-01

We present modeled aerosol optical properties (single scattering albedo, asymmetry parameter, and lidar ratio) in two layers with different aerosol loadings and particle sizes, observed during the Southern African Regional Science Initiative 2000 (SAFARI 2000) campaign. The optical properties were calculated from aerosol size distributions retrieved from aerosol layer optical thickness spectra, measured using the NASA Ames airborne tracking 14-channel sunphotometer (AATS-14) and the refractive index based on the available information on aerosol chemical composition. The study focuses on sensitivity of modeled optical properties in the 0.3–1.5 μm wavelength range to assumptions regarding the mixing scenario. We considered two modelsmore » for the mixture of absorbing and nonabsorbing aerosol components commonly used to model optical properties of biomass burning aerosol: a layered sphere with absorbing core and nonabsorbing shell and the Maxwell–Garnett effective medium model. In addition, comparisons of modeled optical properties with the measurements are discussed. We also estimated the radiative effect of the difference in aerosol absorption implied by the large difference between the single scattering albedo values (~0.1 at midvisible wavelengths) obtained from different measurement methods for the case with a high amount of biomass burning particles. For that purpose, the volume fraction of black carbon was varied to obtain a range of single scattering albedo values (0.81–0.91 at λ=0.50 μm). Finally, the difference in absorption resulted in a significant difference in the instantaneous radiative forcing at the surface and the top of the atmosphere (TOA) and can result in a change of the sign of the aerosol forcing at TOA from negative to positive.« less

Optical, Physical and Chemical Properties of Tar Balls Observed During the Yosemite Aerosol Characterization Study

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

Hand, Jenny L.; Malm, W. C.; Laskin, Alexander

2005-11-09

The Yosemite Aerosol Characterization Study of summer 2002 (YACS) occurred during an active fire season in the western U. S., and provided an opportunity to investigate many unresolved issues related to the radiative effects of biomass burning aerosols. Single particle analysis was performed on field collected aerosol samples using an array of electron microscopy techniques. Amorphous carbon spheres, or “tar balls”, were present in samples collected during episodes of high particle light scattering coefficients that occurred during the peak of a smoke/haze event. The highest concentrations of light-absorbing carbon from a dual-wavelength aethalometer (λ = 370 and 880 nm) occurredmore » during periods when the particles were predominantly tar balls, indicating they do absorb light in the UV and near-IR range of the solar spectrum. Closure experiments of mass concentrations and light scattering coefficients during periods dominated by tar balls did not require any distinct assumptions of organic carbon molecular weight correction factors, density, or refractive index compared to periods dominated by other types of organic carbon aerosols. Measurements of the hygroscopic behavior of tar balls using an environmental SEM indicate that tar balls do not exhibit deliquescence, but do uptake some water at high (~83 %) relative humidity. The ability of tar balls to efficiently scatter and absorb light, and to absorb water has important implications for their role in regional haze and climate fence.« less

Primary carbonaceous aerosols and climate modeling: Classifications, global emission inventories, and observations

NASA Astrophysics Data System (ADS)

Sun, H.; Bond, T.

2004-12-01

Carbonaceous aerosols, including black carbon (BC) and organic carbon (OC), make up a large fraction of the atmospheric aerosols and affect the radiative balance of the earth either by directly scattering and absorbing solar radiation or through indirect influence on cloud optical properties and cloud lifetimes. The major sources of BC and OC emissions are from combustion processes, mainly.fossil-fuel burning, biofuels burning, and open biomass burning. OC is nearly always emitted with BC. Because different combustion practices contribute to the emission of BC and OC to the atmosphere, the magnitude and characteristics of carbonaceous aerosols vary between regions. Since OC mainly scatters light and BC absorbs it, it is possible that OC can oppose the warming effect of BC, so that the net climatic effect of carbonaceous aerosols is not known. There is presently disagreement on whether carbonaceous aerosols produce a net warming or cooling effect on climate. Some differences in model prediction may result from model differences, such as dynamics and treatment of cloud feedbacks. However, large differences also result from initial assumptions about the properties of BC and OC: optical properties, size distribution, and interaction with water. Although there are hundreds of different organic species in atmospheric aerosols, with widely varying properties, global climate models to date have treated organics as one ¡°compound.¡± In addition, emissions of OC are often derived by multiplying BC emissions by a constant factor, so that the balance between these different compounds is assumed. Addressing these critical model assumptions is a necessary step toward estimating the net climatic impact of carbonaceous aerosols, and different human activities. We aim to contribute to this effort by tabulating important climate-relevant properties of both emissions and ambient measurements. Since one single organic ¡°compound¡± is not sufficient to represent all the

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

NASA Astrophysics Data System (ADS)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-06-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photooxidation under a range of controlled conditions (RH ∼65-89%, VOC/NOx ∼3-9 and NOx ∼2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line, chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene, but low isoprene emitter, and its emissions were observed to produce measureable amounts of SOA via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e., in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photooxidation products of the minor VOCs co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally-isoprene emitting landscapes in Southeast Asia. Moreover, in general the amount of aerosol mass produced from the emissions of the principally

Radiative Effects of Atmospheric Aerosols and Impacts on Solar Photovoltaic Electricity Generation

NASA Astrophysics Data System (ADS)

Lund, Cory Christopher

Atmospheric aerosols, by scattering and absorbing radiation, perturbs the Earth's energy balance and reduces the amount of insolation reaching the surface. This dissertation first studies the radiative effects of aerosols by analyzing the internal mixing of various aerosol species. It then examines the aerosol impact on solar PV efficiency and the resulting influence on power systems, including both atmospheric aerosols and deposition of particulate matter (PM) on PV surfaces,. Chapter 2 studies the radiative effects of black carbon (BC), sulfate and organic carbon (OC) internal mixing using a simple radiative transfer model. I find that internal mixing may not result in a positive radiative forcing compared to external mixing, but blocks additional shortwave radiation from the surface, enhancing the surface dimming effect. Chapter 3 estimates the impact of atmospheric aerosol attenuation on solar PV resources in China using a PV performance model with satellite-derived long-term surface irradiance data. I find that, in Eastern China, annual average reductions of solar resources due to aerosols are more than 20%, with comparable impacts to clouds in winter. Improving air quality in China would increase efficiency of solar PV generation. As a positive feedback, increased PV efficiency and deployment would further reduce air pollutant emissions too. Chapter 4 further quantifies the total aerosol impact on PV efficiency globally, including both atmospheric aerosols and the deposition of PM on PV surfaces. I find that, if panels are uncleaned and soiling is only removed by precipitation, deposition of PM accounts for more than two-thirds of the total aerosol impact in most regions. Cleaning the panels, even every few months, would largely increase PV efficiency in resource-abundant regions. Chapter 5 takes a further step to evaluate the impact of PV generation reduction due to aerosols on a projected 2030 power system in China with 400GW of PV. I find that aerosols

First Chemical Characterization of Refractory Black Carbon Aerosols and Associated Coatings over the Tibetan Plateau (4730 m a.s.l).

PubMed

Wang, Junfeng; Zhang, Qi; Chen, Mindong; Collier, Sonya; Zhou, Shan; Ge, Xinlei; Xu, Jianzhong; Shi, Jinsen; Xie, Conghui; Hu, Jianlin; Ge, Shun; Sun, Yele; Coe, Hugh

2017-12-19

Refractory black carbon (rBC) aerosol is an important climate forcer, and its impacts are greatly influenced by the species associated with rBC cores. However, relevant knowledge is particularly lacking at the Tibetan Plateau (TP). Here we report, for the first time, highly time-resolved measurement results of rBC and its coating species in central TP (4730 m a.s.l), using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS), which selectively measured rBC-containing particles. We found that the rBC was overall thickly coated with an average mass ratio of coating to rBC (R BC ) of ∼7.7, and the coating species were predominantly secondarily formed by photochemical reactions. Interestingly, the thickly coated rBC was less oxygenated than the thinly coated rBC, mainly due to influence of the transported biomass burning organic aerosol (BBOA). This BBOA was relatively fresh but formed very thick coating on rBC. We further estimated the "lensing effect" of coating semiquantitatively by comparing the measurement data from a multiangle absorption photometer and SP-AMS, and found it could lead to up to 40% light absorption enhancement at R BC > 10. Our findings highlight that BBOA can significantly affect the "lensing effect", in addition to its relatively well-known role as light-absorbing "brown carbon."

Measurements of the absorption coefficient of stratospheric aerosols

NASA Technical Reports Server (NTRS)

Ogren, J. A.; Ahlquist, N. C.; Clarke, A. D.; Charlson, R. J.

1981-01-01

The absorption coefficients of stratospheric aerosols are measured using a variation on the integrating plate method. The technique is based on the decrease in the transparency of a substrate when an absorbing aerosol is deposited on it. A Lambert scatterer is placed behind the substrate to integrate forward scattered light and minimize the effect of scattering on the measurement. The low pressure in the stratosphere is used for the direct impaction of particles onto a narrow strip of opal glass. The eight samples collected had a median value of 4 x 10 to the -9th m with an uncertainty of + or - 5 x 10 to the -9th m. If this absorption is due to graphitic carbon, then its concentration is estimated at about 0.4 ng/cu m, or about 0.25% of the total aerosol mass concentration. Estimates of the aerosol scattering coefficients based on satellite extinction inversions result in an aerosol single-scattering albedo in the range of 0.96-1.0.

AOD Distributions and Trends of Major Aerosol Species over a Selection of the World's Most Populated Cities Based on the 1st Version of NASA's MERRA Aerosol Reanalysis

NASA Technical Reports Server (NTRS)

Provencal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

2017-01-01

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

AOD distributions and trends of major aerosol species over a selection of the world's most populated cities based on the 1st Version of NASA's MERRA Aerosol Reanalysis.

PubMed

Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M; Elhacham, Emily; Alpert, Pinhas

2017-06-01

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003-2015) and over a selection of 200 of the world's most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don't tend to

E-Cigarette Aerosol Exposure Induces Reactive Oxygen Species, DNA Damage, and Cell Death in Vascular Endothelial Cells.

PubMed

Anderson, Chastain; Majeste, Andrew; Hanus, Jakub; Wang, Shusheng

2016-12-01

Cigarette smoking remains one of the leading causes of preventable death worldwide. Vascular cell death and dysfunction is a central or exacerbating component in the majority of cigarette smoking related pathologies. The recent development of the electronic nicotine delivery systems known as e-cigarettes provides an alternative to conventional cigarette smoking; however, the potential vascular health risks of e-cigarette use remain unclear. This study evaluates the effects of e-cigarette aerosol extract (EAE) and conventional cigarette smoke extract (CSE) on human umbilical vein endothelial cells (HUVECs). A laboratory apparatus was designed to produce extracts from e-cigarettes and conventional cigarettes according to established protocols for cigarette smoking. EAE or conventional CSE was applied to human vascular endothelial cells for 4-72 h, dependent on the assay. Treated cells were assayed for reactive oxygen species, DNA damage, cell viability, and markers of programmed cell death pathways. Additionally, the anti-oxidants α-tocopherol and n-acetyl-l-cysteine were used to attempt to rescue e-cigarette induced cell death. Our results indicate that e-cigarette aerosol is capable of inducing reactive oxygen species, causing DNA damage, and significantly reducing cell viability in a concentration dependent fashion. Immunofluorescent and flow cytometry analysis indicate that both the apoptosis and programmed necrosis pathways are triggered by e-cigarette aerosol treatment. Additionally, anti-oxidant treatment provides a partial rescue of the induced cell death, indicating that reactive oxygen species play a causal role in e-cigarette induced cytotoxicity. © The Author 2016. Published by Oxford University Press on behalf of the Society of Toxicology. All rights reserved. For Permissions, please e-mail: journals.permissions@oup.com.

Analysis of DIAL/HSRL aerosol backscatter and extinction profiles during the SEAC4RS campaign with an aerosol assimilation system

NASA Astrophysics Data System (ADS)

Weaver, C. J.; da Silva, A. M., Jr.; Colarco, P. R.; Randles, C. A.

2015-12-01

We retrieve aerosol concentrations and optical information from vertical profiles of airborne 532 nm extinction and 532 and 1064 nm backscatter measurements made during the SEAC4RS summer 2013 campaign. The observations are from the High Spectral Resolution Lidar (HSRL) Airborne Differential Absorption Lidar (DIAL) on board the NASA DC-8. Instead of retrieving information about aerosol microphysical properties such as indexes of refraction, we seek information more directly applicable to an aerosol transport model - in our case the Goddard Chemistry Aerosol Radiation and Transport (GOCART) module used in the GEOS-5 Earth modeling system. A joint atmosphere/aerosol mini-reanalysis was performed for the SEAC4RS period using GEOS-5. The meteorological reanalysis followed the MERRA-2 atmospheric reanalysis protocol, and aerosol information from MODIS, MISR, and AERONET provided a constraint on the simulated aerosol optical depth (i.e., total column loading of aerosols). We focus on the simulated concentrations of 10 relevant aerosol species simulated by the GOCART module: dust, sulfate, and organic and black carbon. Our first retrieval algorithm starts with the SEAC4RS mini-reanalysis and adjusts the concentration of each GOCART aerosol species so that differences between the observed and simulated backscatter and extinction measurements are minimized. In this case, too often we are unable to simulate the observations by simple adjustment of the aerosol concentrations. A second retrieval approach adjusts both the aerosol concentrations and the optical parameters (i.e., assigned mass extinction efficiency) associated with each GOCART species. We present results from DC-8 flights over smoke from forest fires over the western US using both retrieval approaches. Finally, we compare our retrieved quantities with in-situ observations of aerosol absorption, scattering, and mass concentrations at flight altitude.

403 nm cavity ring-down measurements of brown carbon aerosol

NASA Astrophysics Data System (ADS)

Kwon, D.; Grassian, V. H.; Kleiber, P.; Young, M. A.

2017-12-01

Atmospheric aerosol influences Earth's climate by absorbing and scattering incoming solar radiation and outgoing terrestrial radiation. One class of secondary organic aerosol (SOA), called brown carbon (BrC), has attracted attention for its wavelength dependent light absorbing properties with absorption coefficients that generally increase from the visible (Vis) to ultraviolet (UV) regions. Here we report results from our investigation of the optical properties of BrC aerosol products from the aqueous phase reaction of ammonium sulfate (AS) with methylglyoxal (MG) using cavity ring-down spectroscopy (CRDS) at 403 nm wavelength. We have measured the optical constants of BrC SOA from the AS/MG reaction as a function of reaction time. Under dry flow conditions, we observed no apparent variation in the BrC refractive index with aging over the course of 22 days. The retrieved BrC optical constants are similar to those of AS with n = 1.52 for the real component. Despite significant UV absorption observed from the bulk BrC solution, the imaginary index value at 403 nm is below our minimum detection limit which puts an upper bound of k as 0.03. These observations are in agreement with results from our recent studies of the light scattering properties of this BrC aerosol.

Light absorption of organic aerosol from pyrolysis of corn stalk

NASA Astrophysics Data System (ADS)

Li, Xinghua; Chen, Yanju; Bond, Tami C.

2016-11-01

Organic aerosol (OA) can absorb solar radiation in the low-visible and ultra-violet wavelengths thereby modifying radiative forcing. Agricultural waste burning emits a large quantity of organic carbon in many developing countries. In this work, we improved the extraction and analysis method developed by Chen and Bond, and extended the spectral range of OC absorption. We examined light absorbing properties of primary OA from pyrolysis of corn stalk, which is a major type of agricultural wastes. Light absorption of bulk liquid extracts of OA was measured using a UV-vis recording spectrophotometer. OA can be extracted by methanol at 95%, close to full extent, and shows polar character. Light absorption of organic aerosol has strong spectral dependence (Absorption Ångström exponent = 7.7) and is not negligible at ultra-violet and low-visible regions. Higher pyrolysis temperature produced OA with higher absorption. Imaginary refractive index of organic aerosol (kOA) is 0.041 at 400 nm wavelength and 0.005 at 550 nm wavelength, respectively.

The Effect of Aerosol on Gravity Wave Characteristics above the Boundary Layer over a Tropical Location

NASA Astrophysics Data System (ADS)

Rakshit, G.; Jana, S.; Maitra, A.

2017-12-01

The perturbations of temperature profile over a location give an estimate of the potential energy of gravity waves propagating through the atmosphere. Disturbances in the lower atmosphere due to tropical deep convection, orographic effects and various atmospheric disturbances generates of gravity waves. The present study investigates the gravity wave energy estimated from fluctuations in temperature profiles over the tropical location Kolkata (22°34' N, 88°22' E). Gravity waves are most intense during the pre-monsoon period (March-June) at the present location, the potential energy having high values above the boundary layer (2-4 km) as observed from radiosonde profiles. An increase in temperature perturbation, due to high ambient temperature in the presence of heat absorbing aerosols, causes an enhancement in potential energy. As the present study location is an urban metropolitan city experiencing high level of pollution, pollutant aerosols can go much above the normal boundary layer during daytime due to convection causing an extended boundary layer. The Aerosol Index (AAI) obtained from Global Ozone Monitoring Experiment-2 (GOME-2) on MetOp-A platform at 340 nm and 380 nm confirms the presence of absorbing aerosol particles over the present location. The Hysplit back trajectory analysis shows that the aerosol particles at those heights are of local origin and are responsible for depleting liquid water content due to cloud burning. The aerosol extinction coefficient obtained from CALIPSO data exhibits an increasing trend during 2006-2016 accompanied by a similar pattern of gravity wave energy. Thus the absorbing aerosols have a significant role in increasing the potential energy of gravity wave at an urban location in the tropical region.

Direct radiative effect due to brownness in organic carbon aerosols generated from biomass combustion

NASA Astrophysics Data System (ADS)

Rathod, T. D.; Sahu, S. K.; Tiwari, M.; Pandit, G. G.

2016-12-01

We report the enhancement in the direct radiative effect due the presence of Brown carbon (BrC) as a part of organic carbon aerosols. The optical properties of organic carbon aerosols generated from pyrolytic combustion of mango tree wood (Magnifera Indica) and dung cake at different temperatures were considered. Mie codes were used to calculate absorption and scattering coefficients coupled with experimentally derived imaginary complex refractive index. The direct radiative effect (DRE) for sampled organic carbon aerosols was estimated using a wavelength dependent radiative transfer equation. The BrC DRE was estimated taking virtually non absorbing organic aerosols as reference. The BrC DRE from wood and dung cake was compared at different combustion temperatures and conditions. The BrC contributed positively to the direct top of the atmosphere radiative effect. Dung cake generated BrC aerosols were found to be strongly light absorbing as compared to BrC from wood combustion. It was noted that radiative effects of BrC from wood depended on its generation temperature and conditions. For BrC aerosols from dung cake such strong dependence was not observed. The average BrC aerosol DRE values were 1.53±0.76 W g-1 and 17.84±6.45 W g-1 for wood and dung cake respectively. The DRE contribution of BrC aerosols came mainly (67-90%) from visible light absorption though they exhibited strong absorption in shorter wavelengths of the UV-visible spectrum.

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

NASA Astrophysics Data System (ADS)

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-05-01

An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

DOE PAGES

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-03-02

We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized bymore » the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10 -5 to 10 -11. Free molecular heat and mass transfer theory was

The OMI Aerosol Absorption Product: An A-train application

NASA Astrophysics Data System (ADS)

Torres, O.; Jethva, H. T.; Ahn, C.

2017-12-01

Because of the uniquely large sensitivity of satellite-measured near-UV radiances to absorption by desert dust, carbonaceous and volcanic ash aerosols, observations by a variety of UV-capable sensors have been routinely used over the last forty years in both qualitative and quantitative applications for estimating the absorption properties of these aerosol types. In this presentation we will discuss a multi-sensor application involving observations from A-train sensors OMI, AIRS and CALIOP for the creation of a 13-year record of aerosol optical depth (AOD) and single scattering albedo (SSA). Determination of aerosol type, in terms of particle size distribution and refractive index, is an important algorithmic step that requires using external information. AIRS CO measurements are used as carbonaceous aerosols tracer to differentiate this aerosol type from desert dust. On the other hand, the height of the absorbing aerosol layer, an important parameter in UV aerosol retrievals, is prescribed using a CALIOP-based climatology. The combined use of these observations in the developments of the OMI long-term AOD/SSA record will be discussed along with an evaluation of retrieval results using independent observations.

A thermoluminescent method for aerosol characterization

NASA Technical Reports Server (NTRS)

Long, E. R., Jr.; Rogowski, R. S.

1976-01-01

A thermoluminescent method has been used to study the interactions of aerosols with ozone. The preliminary results show that ozone reacts with many compounds found in aerosols, and that the thermoluminescence curves obtained from ozonated aerosols are characteristic of the aerosol. The results suggest several important applications of the thermoluminescent method: development of a detector for identification of effluent sources; a sensitive experimental tool for study of heterogeneous chemistry; evaluation of importance of aerosols in atmospheric chemistry; and study of formation of toxic, electronically excited species in airborne particles.

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

NASA Astrophysics Data System (ADS)

Rao, Roshan

2016-04-01

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. We look into the approach where ground based spectral radiation flux measurement is made and along with an Radtiative transfer (RT) model, radiative forcing is estimated. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and a 3nm resolution during around 54 clear-sky days during which AOD range was around 0.01 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. The primary study involved in understanding the sensitivity of spectral flux due to change in individual aerosol species (Optical properties of Aerosols and Clouds (OPAC) classified aerosol species) using the SBDART RT model. This made us clearly distinguish the 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 matching different combinations of aerosol species in OPAC model and RT model as long as the combination which gives the minimum root mean squared deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model, aerosol radiative forcing is estimated. Also an alternate method to estimate the spectral SSA is discussed. Here, the RT model, the observed spectral flux and spectral AOD is used. Spectral AOD is input to RT model and SSA is varied till the minimum root mean squared difference between observed and simulated spectral flux from RT model is obtained. The methods discussed are limited to clear sky scenes and its accuracy to derive

Two-Column Aerosol Project: Aerosol Light Extinction Measurements Field Campaign Report

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

Dubey, Manvendra; Aiken, Allison; Berg, Larry

We deployed Aerodyne Research Inc.’s first Cavity Attenuated Phase Shift extinction (CAPS PMex) monitor (built by Aerodyne) that measures light extinction by using a visible-light-emitting diode (LED) as a light source, a sample cell incorporating two high-reflectivity mirrors centered at the wavelength of the LED, and a vacuum photodiode detector in Cape Cod in 2012/13 for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Two-Column Aerosol Project (TCAP). The efficacy of this instrument is based on the fact that aerosols are broadband scatterers and absorbers of light. The input LED is square-wave modulated and passedmore » through the sample cell that distorts it due to exponential decay by aerosol light absorption and scattering; this is measured at the detector. The amount of phase shift of the light at the detector is used to determine the light extinction. This extinction measurement provides an absolute value, requiring no calibration. The goal was to compare the CAPS performance with direct measurements of absorption with ARM’s baseline photoacoustic soot spectrometer (PASS-3) and nephelometer instruments to evaluate its performance.« less

Interpreting the Ultraviolet Aerosol Index Observed with the OMI Satellite Instrument to Understand Absorption by Organic Aerosols: Implications for Atmospheric Oxidation and Direct Radiative Effects

NASA Technical Reports Server (NTRS)

Hammer, Melanie S.; Martin, Randall V.; Donkelaar, Aaron van; Buchard, Virginie; Torres, Omar; Ridley, David A.; Spurr, Robert J. D.

2016-01-01

Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOSChem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (-0.32 to -0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from -0.57 to -0.09 over West Africa in January, from -0.32 to +0.0002 over South Asia in April, from -0.97 to -0.22 over southern Africa in July, and from -0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Angstrom exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30% over South America in September, up to 20% over southern Africa in July, and up to 15% over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus

Measurements of HNO3, SO2 High Resolution Aerosol SO4 (sup 2-), and Selected Aerosol Species Aboard the NASA DC-8 Aircraft: During the Transport and Chemical Evolution Over the Pacific Airborne Mission (TRACE-P)

NASA Technical Reports Server (NTRS)

Talbot, Robert W.; Dibb, Jack E.

2004-01-01

The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Bergstrom, Robert A.; Russell, Philip B.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single- scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

North Atlantic Aerosol Radiative Effects Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Bergstrom, Robert W.; Russell, Philip B.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single-scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

North Atlantic Aerosol Radiative Impacts Based on Satellite Measurements and Aerosol Intensive Properties from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Bergstrom, Robert W.; Schmid, Beat; Livingston, John M.

2000-01-01

We estimate the impact of North Atlantic aerosols on the net shortwave flux at the tropopause by combining maps of satellite-derived aerosol optical depth (AOD) with model aerosol properties. We exclude African dust, primarily by restricting latitudes to 25-60 N. Aerosol properties were determined via column closure analyses in two recent experiments, TARFOX and ACE 2. The analyses use in situ measurements of aerosol composition and air- and ship-borne sunphotometer measurements of AOD spectra. The resulting aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. It has a midvisible single-scattering albedo of 0.9, which is in the range obtained from in situ measurements of aerosol scattering and absorption in both TARFOX and ACE 2. Combining seasonal maps of AVHRR-derived midvisible AOD with the aerosol model yields maps of 24-hour average net radiative flux changes at the tropopause. For cloud-free conditions, results range from -9 W/sq m near the eastern US coastline in the summer to -1 W/sq m in the mid-Atlantic during winter; the regional annual average is -3.5 W/sq m. Using a non- absorbing aerosol model increases these values by about 30%. We estimate the effect of clouds using ISCCP cloud-fraction maps. Because ISCCP midlatitude North Atlantic cloud fractions are relatively large, they greatly reduce the computed aerosol-induced flux changes. For example, the regional annual average decreases from -3.5 W/sq m to -0.8 W/sq m. We compare results to previous model calculations for a variety of aerosol types.

Refractive indices of Early Earth organic aerosol analogs

NASA Astrophysics Data System (ADS)

Gavilan, L.; Carrasco, N.; Fleury, B.; Vettier, L.

2017-09-01

Organic hazes in the early Earth atmosphere are hypothesized to provide additional shielding to solar radiation. We simulate the conditions of this primitive atmosphere by adding CO2 to a N2:CH4 gas mixture feeding a plasma. In this plasma, solid organic films were produced simulating early aerosols. We performed ellipsometry on these films from the visible to the near-ultraviolet range. Such measurements reveal how organic aerosols in the early Earth atmosphere preferentially absorb photons of shorter wavelengths than typical Titan tholins, suggesting a coolant role in the early Earth.

Landscape fires dominate terrestrial natural aerosol - climate feedbacks

NASA Astrophysics Data System (ADS)

Scott, C.; Arnold, S.; Monks, S. A.; Asmi, A.; Paasonen, P.; Spracklen, D. V.

2017-12-01

The terrestrial biosphere is an important source of natural aerosol including landscape fire emissions and secondary organic aerosol (SOA) formed from biogenic volatile organic compounds (BVOCs). Atmospheric aerosol alters the Earth's climate by absorbing and scattering radiation (direct radiative effect; DRE) and by perturbing the properties of clouds (aerosol indirect effect; AIE). Natural aerosol sources are strongly controlled by, and can influence, climate; giving rise to potential natural aerosol-climate feedbacks. Earth System Models (ESMs) include a description of some of these natural aerosol-climate feedbacks, predicting substantial changes in natural aerosol over the coming century with associated radiative perturbations. Despite this, the sensitivity of natural aerosols simulated by ESMs to changes in climate or emissions has not been robustly tested against observations. Here we combine long-term observations of aerosol number and a global aerosol microphysics model to assess terrestrial natural aerosol-climate feedbacks. We find a strong positive relationship between the summertime anomaly in observed concentration of particles greater than 100 nm diameter and the anomaly in local air temperature. This relationship is reproduced by the model and driven by variability in dynamics and meteorology, as well as natural sources of aerosol. We use an offline radiative transfer model to determine radiative effects due to changes in two natural aerosol sources: landscape fire and biogenic SOA. We find that interannual variability in the simulated global natural aerosol radiative effect (RE) is negatively related to the global temperature anomaly. The magnitude of global aerosol-climate feedback (sum of DRE and AIE) is estimated to be -0.15 Wm-2 K-1 for landscape fire aerosol and -0.06 Wm-2 K-1 for biogenic SOA. These feedbacks are comparable in magnitude, but opposite in sign to the snow albedo feedback, highlighting the need for natural aerosol feedbacks to

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

Modeling the Relationships Between Aerosol Properties and the Direct and Indirect Effects of Aerosols on Climate

NASA Technical Reports Server (NTRS)

Toon, Owen B.

1994-01-01

Aerosols may affect climate directly by scattering and absorbing visible and infrared energy, They may also affect climate indirectly by modifying the properties of clouds through microphysical processes, and by altering abundances of radiatively important gases through heterogeneous chemistry. Researchers understand which aerosol properties control the direct effect of aerosols on the radiation budget. Unfortunately, despite an abundance of data on certain types of aerosols, much work remains to be done to determine the values of these properties. For instance we have little idea about the global distribution, seasonal variation, or interannual variability of the aerosol optical depth. Also we do not know the visible light absorption properties of tropical aerosols which may contain much debris from slash and burn agriculture. A positive correlation between aerosol concentrations and albedos of marine stratus clouds is observed, and the causative microphysics is understood. However, models suggest that it is difficult to produce new particles in the marine boundary layer. Some modelers have suggested that the particles in the marine boundary layer may originate in the free troposphere and be transported into the boundary layer. Others argue that the aerosols are created in the marine boundary layer. There are no data linking aerosol concentration and cirrus cloud albedo, and models suggest cirrus properties may not be very sensitive to aerosol abundance. There is clear evidence of a radiatively significant change in the global lower stratospheric ozone abundance during the past few decades. These changes are caused by heterogeneous chemical reactions occurring on the surfaces of particles. The rates of these reactions depend upon the chemical composition of the particles. Although rapid advances in understanding heterogeneous chemistry have been made, much remains to be done.

Comparison of on-line and off-line methods to quantify reactive oxygen species (ROS) in atmospheric aerosols

NASA Astrophysics Data System (ADS)

Fuller, S. J.; Wragg, F. P. H.; Nutter, J.; Kalberer, M.

2014-08-01

Atmospheric aerosol particle concentrations have been linked with a wide range of pulmonary and cardio-vascular diseases but the particle properties responsible for these negative health effects are largely unknown. It is often speculated that reactive oxygen species (ROS) present in atmospheric particles lead to oxidative stress in, and ultimately disease of, the human lung. The quantification of ROS is highly challenging because some ROS components such as radicals are highly reactive and therefore short-lived. Thus, fast analysis methods are likely advantageous over methods with a long delay between aerosol sampling and ROS analysis. We present for the first time a detailed comparison of conventional off-line and fast on-line methods to quantify ROS in organic aerosols. For this comparison a new and fast on-line instrument was built and characterized to quantify ROS in aerosol particles with high sensitivity and a limit of detection of 4 nmol H2O2 equivalents per m3 air. ROS concentrations are measured with a time resolution of approximately 15 min, which allows the tracking of fast changing atmospheric conditions. The comparison of the off-line and on-line method shows that, in oxidized organic model aerosol particles, the majority of ROS have a very short lifetime of a few minutes whereas a small fraction is stable for a day or longer. This indicates that off-line techniques, where there is often a delay of hours to days between particle collection and ROS analysis, may severely underestimate true ROS concentrations and that fast on-line techniques are necessary for a reliable ROS quantification in atmospheric aerosol particles and a meaningful correlation with health outcomes.

Impact of Tropospheric Aerosol Absorption on Ozone Retrieval from buv Measurements

NASA Technical Reports Server (NTRS)

Torres, O.; Bhartia, P. K.

1998-01-01

The impact of tropospheric aerosols on the retrieval of column ozone amounts using spaceborne measurements of backscattered ultraviolet radiation is examined. Using radiative transfer calculations, we show that uv-absorbing desert dust may introduce errors as large as 10% in ozone column amount, depending on the aerosol layer height and optical depth. Smaller errors are produced by carbonaceous aerosols that result from biomass burning. Though the error is produced by complex interactions between ozone absorption (both stratospheric and tropospheric), aerosol scattering, and aerosol absorption, a surprisingly simple correction procedure reduces the error to about 1%, for a variety of aerosols and for a wide range of aerosol loading. Comparison of the corrected TOMS data with operational data indicates that though the zonal mean total ozone derived from TOMS are not significantly affected by these errors, localized affects in the tropics can be large enough to seriously affect the studies of tropospheric ozone that are currently undergoing using the TOMS data.

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

MATRIX-VBS Condensing Organic Aerosols in an Aerosol Microphysics Model

NASA Technical Reports Server (NTRS)

Gao, Chloe Y.; Tsigaridis, Konstas; Bauer, Susanne E.

2015-01-01

The condensation of organic aerosols is represented in a newly developed box-model scheme, where its effect on the growth and composition of particles are examined. We implemented the volatility-basis set (VBS) framework into the aerosol mixing state resolving microphysical scheme Multiconfiguration Aerosol TRacker of mIXing state (MATRIX). This new scheme is unique and advances the representation of organic aerosols in models in that, contrary to the traditional treatment of organic aerosols as non-volatile in most climate models and in the original version of MATRIX, this new scheme treats them as semi-volatile. Such treatment is important because low-volatility organics contribute significantly to the growth of particles. The new scheme includes several classes of semi-volatile organic compounds from the VBS framework that can partition among aerosol populations in MATRIX, thus representing the growth of particles via condensation of low volatility organic vapors. Results from test cases representing Mexico City and a Finish forrest condistions show good representation of the time evolutions of concentration for VBS species in the gas phase and in the condensed particulate phase. Emitted semi-volatile primary organic aerosols evaporate almost completely in the high volatile range, and they condense more efficiently in the low volatility range.

Atmospheric Teleconnection over Eurasia Induced by Aerosol Radiative Forcing during Boreal Spring

NASA Technical Reports Server (NTRS)

Kim, Maeng-Ki; Lau, William K. M.; Chin, Mian; Kim, Kyu-Myong; Sud, Y. C.; Walker, Greg K.

2006-01-01

The direct effects of aerosols on global and regional climate during boreal spring are investigated based on numerical simulations with the NASA Global Modeling and Assimilation Office finite-volume general circulation model (fvGCM) with Microphyics of Clouds with the Relaxed Arakawa Schubert Scheme (McRAS), using aerosol forcing functions derived from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The authors find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excite a planetary-scale teleconnection pattern in sea level pressure, temperature, and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, that is, South Asia, East Asia, and northern and western Africa. Significant atmospheric heating is found in regions with large loading of dust (over northern Africa and the Middle East) and black carbon (over Southeast Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east west dipole anomaly with strong cooling over the Caspian Sea and warming over central and northeastern Asia, where aerosol concentrations are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection pattern driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes associated with the regional circulations. The surface temperature signature associated with the aerosol-induced teleconnection bears striking resemblance to the spatial pattern of observed long-term trend in surface temperature over Eurasia. Additionally, the boreal spring wave train pattern is similar to that reported by Fukutomi et al. associated with the boreal summer

Quantifying organic aerosol single scattering albedo over tropical biomass burning regions using ground-based observation

NASA Astrophysics Data System (ADS)

Chu, J. E.

2016-12-01

Despite growing evidence of light-absorbing organic aerosols (OAs), OA light absorption has been poorly understood due to difficulties in aerosol light absorption measurements. In this study, we developed an empirical method to quantify OA single scattering albedo (SSA), the ratio of light scattering to extinction, using ground-based Aerosol Robotic Network (AERONET) observation. Our method includes partitioning fine-mode aerosol optical depth (fAOD) to individual aerosol's optical depth (AOD), separating black carbon and OA absorption aerosol optical depths, and finally binding OA SSA and sulfate+nitrate AOD. Our best estimate of OA SSA over tropical biomass burning region is 0.91 at 550nm with a range of 0.82-0.93. It implies the common OA SSA values of 0.96-1.0 in aerosol CTMs and GCMs significantly underrepresent OA light absorption. Model experiments with prescribed OA SSA showed that the enhanced absorption of solar radiation due to light absorbing OA yields global mean radiative forcing is +0.09 Wm-2 at the TOA, +0.21 Wm-2 at the atmosphere, and -0.12 Wm-2 at the surface. Compared to the previous assessment of OA radiative forcing reported in AeroCom II project, our result indicate that OA light absorption causes TOA radiative forcing by OA to change from negative (i.e., cooling effect) to positive (warming effect).

Study of aerosol effect on accelerated snow melting over the Tibetan Plateau during boreal spring

NASA Astrophysics Data System (ADS)

Lee, Woo-Seop; Bhawar, Rohini L.; Kim, Maeng-Ki; Sang, Jeong

2013-08-01

In the present study, a coupled atmosphere-ocean global climate model (CSIRO-Mk3.6) is used to investigate the role of aerosol forcing agents as drivers of snow melting trends in the Tibetan Plateau (TP) region. Anthropogenic aerosol-induced snow cover changes in a warming climate are calculated from the difference between historical run (HIST) and all forcing except anthropogenic aerosol (NoAA). Absorbing aerosols can influence snow cover by warming the atmosphere, reducing snow reflectance after deposition. The warming the rate of snow melt, exposing darker surfaces below to short-wave radiation sooner, and allowing them to heat up even faster in the Himalayas and TP. The results show a strong spring snow cover decrease over TP when absorbing anthropogenic aerosol forcing is considered, whereas snow cover fraction (SCF) trends in NoAA are weakly negative (but insignificant) during 1951-2005. The enhanced spring snow cover trends in HIST are due to overall effects of different forcing agents: When aerosol forcing (AERO) is considered, a significant reduction of SCF than average can be found over the western TP and Himalayas. The large decreasing trends in SCF over the TP, with the maximum reduction of SCF around 12-15% over the western TP and Himalayas slope. Also accelerated snow melting during spring is due to effects of aerosol on snow albedo, where aerosol deposition cause decreases snow albedo. However, the SCF change in the “NoAA” simulations was observed to be less.

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

NASA Technical Reports Server (NTRS)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Speciation of 127I and 129I in atmospheric aerosols at Risø, Denmark: insight into sources of iodine isotopes and their species transformations

NASA Astrophysics Data System (ADS)

Zhang, Luyuan; Hou, Xiaolin; Xu, Sheng

2016-02-01

Speciation analysis of iodine in aerosols is a very useful approach for understanding geochemical cycling of iodine in the atmosphere. In this study, overall iodine species, including water-soluble iodine species (iodide, iodate and water-soluble organic iodine), NaOH-soluble iodine, and insoluble iodine have been determined for 129I and 127I in the aerosols collected at Risø, Denmark, during March and May 2011 (shortly after the Fukushima nuclear accident) and in December 2014. The measured concentrations of total iodine are in the range of 1.04-2.48 ng m-3 for 127I and (11.3-97.0) × 105 atoms m-3 for 129I, corresponding to 129I / 127I atomic ratios of (17.8-86.8) × 10-8. The contribution of Fukushima-derived 129I (peak value of 6.3 × 104 atoms m-3) is estimated to be negligible (less than 6 %) compared to the total 129I concentration in northern Europe. The concentrations and species of 129I and 127I in the aerosols are found to be strongly related to their sources and atmospheric pathways. Aerosols that were transported over the contaminated seas contained higher concentrations of 129I than aerosols transported over the European continent. The high 129I concentrations of the marine aerosols are attributed to secondary emission of marine discharged 129I in the contaminated seawater in the North Sea, North Atlantic Ocean, English Channel, Kattegat, etc., rather than direct gaseous release from the European nuclear reprocessing plants (NRPs). Water-soluble iodine was found to be a minor fraction to the total iodine for both 127I (7.8-13.7 %) and 129I (6.5-14.1 %) in ocean-derived aerosols, but accounted for 20.2-30.3 % for 127I and 25.6-29.5 % for 129I in land-derived aerosols. Iodide was the predominant form of water-soluble iodine, accounting for more than 97 % of the water-soluble iodine. NaOH-soluble iodine seems to be independent of the sources of aerosols. The significant proportion of 129I and 127I found in NaOH-soluble fractions is likely bound with

The absorption budget of fresh biomass burning aerosol from realistic laboratory fires

NASA Astrophysics Data System (ADS)

Wagner, N. L.; Adler, G. A.; Franchin, A.; Lamb, K.; Manfred, K.; Middlebrook, A. M.; Selimovic, V.; Schwarz, J. P.; Washenfelder, R. A.; Womack, C.; Yokelson, R. J.

2017-12-01

Wildfires are expected to increase globally due to climate change. The smoke from these wildfires has a highly uncertain radiative effect, largely due to the lack of detailed understanding of its optical properties. As part of the NOAA FIREX project, we have measured the optical properties of smoke primarily from laboratory burning of North American fuels at the Missoula Fire Sciences Laboratory. Here, we present a budget of the aerosol absorption from a portion of the laboratory fires. The total aerosol absorption was measured with photoacoustic spectrometers (PAS) at four wavelengths (405 nm, 532 nm, 660 nm, 870 nm) spanning the visible spectral region. The aerosol absorption is attributed to black carbon which absorbs broadly across the visible and ultraviolet (UV) spectral region and brown carbon (BrC) which absorbs in the blue and UV spectral regions. Then aerosol absorption measurements are compared with measurements of refractory black carbon (rBC) concentration by laser induced incandescence (SP2) and measurements of BrC concentration from a particle-into-liquid sampler coupled to a liquid absorption cell (BrC-PILS). Periodically, a thermodenuder was inserted upstream of all of the instruments to constrain the relationship between aerosol volatility and absorption. We synthesize these measurements to constrain the various contributors to total absorption including effects of lensing on rBC absorption, and of BrC that is not volatilized in the thermodenuder.

Climate impact of biofuels in shipping: global model studies of the aerosol indirect effect.

PubMed

Righi, Mattia; Klinger, Carolin; Eyring, Veronika; Hendricks, Johannes; Lauer, Axel; Petzold, Andreas

2011-04-15

Aerosol emissions from international shipping are recognized to have a large impact on the Earth's radiation budget, directly by scattering and absorbing solar radiation and indirectly by altering cloud properties. New regulations have recently been approved by the International Maritime Organization (IMO) aiming at progressive reductions of the maximum sulfur content allowed in marine fuels from current 4.5% by mass down to 0.5% in 2020, with more restrictive limits already applied in some coastal regions. In this context, we use a global bottom-up algorithm to calculate geographically resolved emission inventories of gaseous (NO(x), CO, SO(2)) and aerosol (black carbon, organic matter, sulfate) species for different kinds of low-sulfur fuels in shipping. We apply these inventories to study the resulting changes in radiative forcing, attributed to particles from shipping, with the global aerosol-climate model EMAC-MADE. The emission factors for the different fuels are based on measurements at a test bed of a large diesel engine. We consider both fossil fuel (marine gas oil) and biofuels (palm and soy bean oil) as a substitute for heavy fuel oil in the current (2006) fleet and compare their climate impact to that resulting from heavy fuel oil use. Our simulations suggest that ship-induced surface level concentrations of sulfate aerosol are strongly reduced, up to about 40-60% in the high-traffic regions. This clearly has positive consequences for pollution reduction in the vicinity of major harbors. Additionally, such reductions in the aerosol loading lead to a decrease of a factor of 3-4 in the indirect global aerosol effect induced by emissions from international shipping.

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

NASA Astrophysics Data System (ADS)

Randles, C. A.; Kinne, S.; Myhre, G.; Schulz, M.; Stier, P.; Fischer, J.; Doppler, L.; Highwood, E.; Ryder, C.; Harris, B.; Huttunen, J.; Ma, Y.; Pinker, R. T.; Mayer, B.; Neubauer, D.; Hitzenberger, R.; Oreopoulos, L.; Lee, D.; Pitari, G.; Di Genova, G.; Quaas, J.; Rose, Fred G.; Kato, S.; Rumbold, S. T.; Vardavas, I.; Hatzianastassiou, N.; Matsoukas, C.; Yu, H.; Zhang, F.; Zhang, H.; Lu, P.

2012-12-01

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly -10 to 20%, with over- and underestimates of radiative cooling at higher and lower sun elevation, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as sun elevation increases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

NASA Astrophysics Data System (ADS)

Randles, C. A.; Kinne, S.; Myhre, G.; Schulz, M.; Stier, P.; Fischer, J.; Doppler, L.; Highwood, E.; Ryder, C.; Harris, B.; Huttunen, J.; Ma, Y.; Pinker, R. T.; Mayer, B.; Neubauer, D.; Hitzenberger, R.; Oreopoulos, L.; Lee, D.; Pitari, G.; Di Genova, G.; Quaas, J.; Rose, F. G.; Kato, S.; Rumbold, S. T.; Vardavas, I.; Hatzianastassiou, N.; Matsoukas, C.; Yu, H.; Zhang, F.; Zhang, H.; Lu, P.

2013-03-01

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly -10 to 20%, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Radiative absorption enhancement from coatings on black carbon aerosols.

PubMed

Cui, Xinjuan; Wang, Xinfeng; Yang, Lingxiao; Chen, Bing; Chen, Jianmin; Andersson, August; Gustafsson, Örjan

2016-05-01

The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4±0.8m(2)g(-1) was enhanced to 9.6±1.8m(2)g(-1) at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (EMAC) rises from 1.4±0.3 in fresh combustion emissions to ~3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average EMAC of 2.25±0.55, and sulfates were primary drivers of the enhanced BC absorption. Copyright © 2016 Elsevier B.V. All rights reserved.

Sensitivity of Multiangle Imaging to the Optical and Microphysical Properties of Biomass Burning Aerosols

NASA Technical Reports Server (NTRS)

Chen, Wei-Ting; Kahn, Ralph A.; Nelson, David; Yau, Kevin; Seinfeld, John H.

2008-01-01

The treatment of biomass burning (BB) carbonaceous particles in the Multiangle Imaging SpectroRadiometer (MISR) Standard Aerosol Retrieval Algorithm is assessed, and algorithm refinements are suggested, based on a theoretical sensitivity analysis and comparisons with near-coincident AERONET measurements at representative BB sites. Over the natural ranges of BB aerosol microphysical and optical properties observed in past field campaigns, patterns of retrieved Aerosol Optical Depth (AOD), particle size, and single scattering albedo (SSA) are evaluated. On the basis of the theoretical analysis, assuming total column AOD of 0.2, over a dark, uniform surface, MISR can distinguish two to three groups in each of size and SSA, except when the assumed atmospheric particles are significantly absorbing (mid-visible SSA approx.0.84), or of medium sizes (mean radius approx.0.13 pin); sensitivity to absorbing, medium-large size particles increases considerably when the assumed column AOD is raised to 0.5. MISR Research Aerosol Retrievals confirm the theoretical results, based on coincident AERONET inversions under BB-dominated conditions. When BB is externally mixed with dust in the atmosphere, dust optical model and surface reflection uncertainties, along with spatial variability, contribute to differences between the Research Retrievals and AERONET. These results suggest specific refinements to the MISR Standard Aerosol Algorithm complement of component particles and mixtures. They also highlight the importance for satellite aerosol retrievals of surface reflectance characterization, with accuracies that can be difficult to achieve with coupled surface-aerosol algorithms in some higher AOD situations.

Stratospheric Aerosol Measurements

NASA Technical Reports Server (NTRS)

Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

The optical properties, physical properties and direct radiative forcing of urban columnar aerosols in the Yangtze River Delta, China

NASA Astrophysics Data System (ADS)

Zhuang, Bingliang; Wang, Tijian; Liu, Jane; Che, Huizheng; Han, Yong; Fu, Yu; Li, Shu; Xie, Min; Li, Mengmeng; Chen, Pulong; Chen, Huimin; Yang, Xiu-qun; Sun, Jianning

2018-02-01

The optical and physical properties as well as the direct radiative forcings (DRFs) of fractionated aerosols in the urban area of the western Yangtze River Delta (YRD) are investigated with measurements from a Cimel sun photometer combined with a radiation transfer model. Ground-based observations of aerosols have much higher temporal resolutions than satellite retrievals. An initial analysis reveals the characteristics of the optical properties of different types of fractionated aerosols in the western YRD. The total aerosols, mostly composed of scattering components (93.8 %), have mean optical depths of 0.65 at 550 nm and refractive index of 1.44 + 0.0084i at 440 nm. The fine aerosols are approximately four times more abundant and have very different compositions from coarse aerosols. The absorbing components account for only ˜ 4.6 % of fine aerosols and 15.5 % of coarse aerosols and have smaller sizes than the scattering aerosols within the same mode. Therefore, fine particles have stronger scattering than coarse ones, simultaneously reflecting the different size distributions between the absorbing and scattering aerosols. The relationships among the optical properties quantify the aerosol mixing and imply that approximately 15 and 27.5 % of the total occurrences result in dust- and black-carbon-dominating mixing aerosols, respectively, in the western YRD. Unlike the optical properties, the size distributions of aerosols in the western YRD are similar to those found at other sites over eastern China on a climatological scale, peaking at radii of 0.148 and 2.94 µm. However, further analysis reveals that the coarse-dominated particles can also lead to severe haze pollution over the YRD. Observation-based estimations indicate that both fine and coarse aerosols in the western YRD exert negative DRFs, and this is especially true for fine aerosols (-11.17 W m-2 at the top of atmosphere, TOA). A higher absorption fraction leads directly to the negative DRF being

Observationally constrained estimates of carbonaceous aerosol radiative forcing.

PubMed

Chung, Chul E; Ramanathan, V; Decremer, Damien

2012-07-17

Carbonaceous aerosols (CA) emitted by fossil and biomass fuels consist of black carbon (BC), a strong absorber of solar radiation, and organic matter (OM). OM scatters as well as absorbs solar radiation. The absorbing component of OM, which is ignored in most climate models, is referred to as brown carbon (BrC). Model estimates of the global CA radiative forcing range from 0 to 0.7 Wm(-2), to be compared with the Intergovernmental Panel on Climate Change's estimate for the pre-Industrial to the present net radiative forcing of about 1.6 Wm(-2). This study provides a model-independent, observationally based estimate of the CA direct radiative forcing. Ground-based aerosol network data is integrated with field data and satellite-based aerosol observations to provide a decadal (2001 through 2009) global view of the CA optical properties and direct radiative forcing. The estimated global CA direct radiative effect is about 0.75 Wm(-2) (0.5 to 1.0). This study identifies the global importance of BrC, which is shown to contribute about 20% to 550-nm CA solar absorption globally. Because of the inclusion of BrC, the net effect of OM is close to zero and the CA forcing is nearly equal to that of BC. The CA direct radiative forcing is estimated to be about 0.65 (0.5 to about 0.8) Wm(-2), thus comparable to or exceeding that by methane. Caused in part by BrC absorption, CAs have a net warming effect even over open biomass-burning regions in Africa and the Amazon.

Observationally constrained estimates of carbonaceous aerosol radiative forcing

PubMed Central

Chung, Chul E.; Ramanathan, V.; Decremer, Damien

2012-01-01

Carbonaceous aerosols (CA) emitted by fossil and biomass fuels consist of black carbon (BC), a strong absorber of solar radiation, and organic matter (OM). OM scatters as well as absorbs solar radiation. The absorbing component of OM, which is ignored in most climate models, is referred to as brown carbon (BrC). Model estimates of the global CA radiative forcing range from 0 to 0.7 Wm-2, to be compared with the Intergovernmental Panel on Climate Change’s estimate for the pre-Industrial to the present net radiative forcing of about 1.6 Wm-2. This study provides a model-independent, observationally based estimate of the CA direct radiative forcing. Ground-based aerosol network data is integrated with field data and satellite-based aerosol observations to provide a decadal (2001 through 2009) global view of the CA optical properties and direct radiative forcing. The estimated global CA direct radiative effect is about 0.75 Wm-2 (0.5 to 1.0). This study identifies the global importance of BrC, which is shown to contribute about 20% to 550-nm CA solar absorption globally. Because of the inclusion of BrC, the net effect of OM is close to zero and the CA forcing is nearly equal to that of BC. The CA direct radiative forcing is estimated to be about 0.65 (0.5 to about 0.8) Wm-2, thus comparable to or exceeding that by methane. Caused in part by BrC absorption, CAs have a net warming effect even over open biomass-burning regions in Africa and the Amazon. PMID:22753522

Aerosol single scattering albedo estimated across China from a combination of ground and satellite measurements

Treesearch

Kwon Ho Lee; Zhanqing Li; Man Sing Wong; Jinyuan Xin; Wang Yuesi; Wei Min Hao; Fengsheng Zhao

2007-01-01

Single scattering albedo (SSA) governs the strength of aerosols in absorbing solar radiation, but few methods are available to directly measure this important quantity. There currently exist many ground-based measurements of spectral transmittance from which aerosol optical thickness (AOT) are retrieved under clear sky conditions. Reflected radiances at the top of the...

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

AOD distributions and trends of major aerosol species over a selection of the world’s most populated cities based on the 1st Version of NASA’s MERRA Aerosol Reanalysis

PubMed Central

Provençal, Simon; Kishcha, Pavel; da Silva, Arlindo M.; Elhacham, Emily; Alpert, Pinhas

2018-01-01

NASA recently extended the Modern-Era Retrospective Analysis for Research and Application (MERRA) with an atmospheric aerosol reanalysis which includes five particulate species: sulfate, organic matter, black carbon, mineral dust and sea salt. The MERRA Aerosol Reanalysis (MERRAero) is an innovative tool to study air quality issues around the world for its global and constant coverage and its distinction of aerosol speciation expressed in the form of aerosol optical depth (AOD). The purpose of this manuscript is to apply MERRAero to the study of urban air pollution at the global scale by analyzing the AOD over a period of 13 years (2003–2015) and over a selection of 200 of the world’s most populated cities in order to assess the impacts of urbanization, industrialization, air quality regulations and regional transport which affect urban aerosol load. Environmental regulations and the recent global economic recession have helped to decrease the AOD and sulfate aerosols in most cities in North America, Europe and Japan. Rapid industrialization in China over the last two decades resulted in Chinese cities having the highest AOD values in the world. China has nevertheless recently implemented emission control measures which are showing early signs of success in many cities of Southern China where AOD has decreased substantially over the last 13 years. The AOD over South American cities, which is dominated by carbonaceous aerosols, has also decreased over the last decade due to an increase in commodity prices which slowed deforestation activities in the Amazon rainforest. At the opposite, recent urbanization and industrialization in India and Bangladesh resulted in a strong increase of AOD, sulfate and carbonaceous aerosols in most cities of these two countries. The AOD over most cities in Northern Africa and Western Asia changed little over the last decade. Emissions of natural aerosols, which cities in these two regions tend to be mostly composed of, don’t tend

Light absorbing organic carbon from prescribed and laboratory biomass burning and gasoline vehicle emissions

EPA Science Inventory

The light absorption of carbonaceous aerosols plays an important role in the atmospheric radiation balance. Light-absorbing organic carbon (OC), also called brown carbon (BrC), from laboratory-based biomass burning (BB) has been studied intensively to understand the contribution ...

The Sensitivity of SeaWiFS Ocean Color Retrievals to Aerosol Amount and Type

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.; Sayer, Andrew M.; Ahmad, Ziauddin; Franz, Bryan A.

2016-01-01

As atmospheric reflectance dominates top-of-the-atmosphere radiance over ocean, atmospheric correction is a critical component of ocean color retrievals. This paper explores the operational Sea-viewing Wide Field-of-View Sensor (SeaWiFS) algorithm atmospheric correction with approximately 13 000 coincident surface-based aerosol measurements. Aerosol optical depth at 440 nm (AOD(sub 440)) is overestimated for AOD below approximately 0.1-0.15 and is increasingly underestimated at higher AOD; also, single-scattering albedo (SSA) appears overestimated when the actual value less than approximately 0.96.AOD(sub 440) and its spectral slope tend to be overestimated preferentially for coarse-mode particles. Sensitivity analysis shows that changes in these factors lead to systematic differences in derived ocean water-leaving reflectance (Rrs) at 440 nm. The standard SeaWiFS algorithm compensates for AOD anomalies in the presence of nonabsorbing, medium-size-dominated aerosols. However, at low AOD and with absorbing aerosols, in situ observations and previous case studies demonstrate that retrieved Rrs is sensitive to spectral AOD and possibly also SSA anomalies. Stratifying the dataset by aerosol-type proxies shows the dependence of the AOD anomaly and resulting Rrs patterns on aerosol type, though the correlation with the SSA anomaly is too subtle to be quantified with these data. Retrieved chlorophyll-a concentrations (Chl) are affected in a complex way by Rrs differences, and these effects occur preferentially at high and low Chl values. Absorbing aerosol effects are likely to be most important over biologically productive waters near coasts and along major aerosol transport pathways. These results suggest that future ocean color spacecraft missions aiming to cover the range of naturally occurring and anthropogenic aerosols, especially at wavelengths shorter than 440 nm, will require better aerosol amount and type constraints.

An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies

NASA Astrophysics Data System (ADS)

Wragg, Francis P. H.; Fuller, Stephen J.; Freshwater, Ray; Green, David C.; Kelly, Frank J.; Kalberer, Markus

2016-10-01

The adverse health effects associated with ambient aerosol particles have been well documented, but it is still unclear which aerosol properties are most important for their negative health impact. Some studies suggest the oxidative effects of particle-bound reactive oxygen species (ROS) are potential major contributors to the toxicity of particles. Traditional ROS measurement techniques are labour-intensive, give poor temporal resolution and generally have significant delays between aerosol sampling and ROS analysis. However, many oxidising particle components are reactive and thus potentially short-lived. Thus, a technique to quantify particle-bound ROS online would be beneficial to quantify also the short-lived ROS components. We introduce a new portable instrument to allow online, continuous measurement of particle-bound ROS using a chemical assay of 2'7'-dichlorofluorescein (DCFH) with horseradish peroxidase (HRP), via fluorescence spectroscopy. All components of the new instrument are attached to a containing shell, resulting in a compact system capable of automated continuous field deployment over many hours or days. From laboratory measurements, the instrument was found to have a detection limit of ˜ 4 nmol [H2O2] equivalents per cubic metre (m3) air, a dynamic range up to at least ˜ 2000 nmol [H2O2] equivalents per m3 air and a time resolution of ≤ 12 min. The instrument allows for ˜ 16 h automated measurement if unattended and shows a fast response to changes in concentrations of laboratory-generated oxidised organic aerosol. The instrument was deployed at an urban site in London, and particulate ROS levels of up to 24 nmol [H2O2] equivalents per m3 air were detected with PM2.5 concentrations up to 28 µg m-3. The new and portable Online Particle-bound ROS Instrument (OPROSI) allows fast-response quantification; this is important due to the potentially short-lived nature of particle-bound ROS as well as fast-changing atmospheric conditions

Improving Aerosol Simulation over South Asia for Climate and Air Quality Studies

NASA Technical Reports Server (NTRS)

Pan, Xiaohua; Chin, Mian; Bian, Huisheng; Gautam, Ritesh

2014-01-01

Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. However, it has been proved quite challenging to adequately represent the aerosol spatial distribution and magnitude over this critical region in global models (Pan et al. 2014), with the surface concentrations, aerosol optical depth (AOD), and absorbing AOD (AAOD) significantly underestimated, especially in October-January when the agricultural waste burning and anthropogenic aerosol dominate over dust aerosol. In this study, we aim to investigate the causes for such discrepancy in winter by conducting sets of model experiments with NASA's GEOS-5 in terms of (1) spatial resolution, (2) emission amount, and (3) meteorological fields.

Aerosols cause intraseasonal short-term suppression of Indian monsoon rainfall.

PubMed

Dave, Prashant; Bhushan, Mani; Venkataraman, Chandra

2017-12-11

Aerosol abundance over South Asia during the summer monsoon season, includes dust and sea-salt, as well as, anthropogenic pollution particles. Using observations during 2000-2009, here we uncover repeated short-term rainfall suppression caused by coincident aerosols, acting through atmospheric stabilization, reduction in convection and increased moisture divergence, leading to the aggravation of monsoon break conditions. In high aerosol-low rainfall regions extending across India, both in deficient and normal monsoon years, enhancements in aerosols levels, estimated as aerosol optical depth and absorbing aerosol index, acted to suppress daily rainfall anomaly, several times in a season, with lags of a few days. A higher frequency of prolonged rainfall breaks, longer than seven days, occurred in these regions. Previous studies point to monsoon rainfall weakening linked to an asymmetric inter-hemispheric energy balance change attributed to aerosols, and short-term rainfall enhancement from radiative effects of aerosols. In contrast, this study uncovers intraseasonal short-term rainfall suppression, from coincident aerosol forcing over the monsoon region, leading to aggravation of monsoon break spells. Prolonged and intense breaks in the monsoon in India are associated with rainfall deficits, which have been linked to reduced food grain production in the latter half of the twentieth century.

A Novel Method for Estimating Shortwave Direct Radiative Effect of Above-Cloud Aerosols Using CALIOP and MODIS Data

NASA Technical Reports Server (NTRS)

Zhang, Z.; Meyer, K.; Platnick, S.; Oreopoulos, L.; Lee, D.; Yu, H.

2014-01-01

This paper describes an efficient and unique method for computing the shortwave direct radiative effect (DRE) of aerosol residing above low-level liquid-phase clouds using CALIOP and MODIS data. It accounts for the overlapping of aerosol and cloud rigorously by utilizing the joint histogram of cloud optical depth and cloud top pressure. Effects of sub-grid scale cloud and aerosol variations on DRE are accounted for. It is computationally efficient through using grid-level cloud and aerosol statistics, instead of pixel-level products, and a pre-computed look-up table in radiative transfer calculations. We verified that for smoke over the southeast Atlantic Ocean the method yields a seasonal mean instantaneous shortwave DRE that generally agrees with more rigorous pixel-level computation within 4. We have also computed the annual mean instantaneous shortwave DRE of light-absorbing aerosols (i.e., smoke and polluted dust) over global ocean based on 4 yr of CALIOP and MODIS data. We found that the variability of the annual mean shortwave DRE of above-cloud light-absorbing aerosol is mainly driven by the optical depth of the underlying clouds.

Spatial distribution and temporal variation of chemical species in the bulk atmospheric aerosols collected at the Okinawa archipelago, Japan

NASA Astrophysics Data System (ADS)

Handa, D.; Somada, Y.; Ijyu, M.; Azechi, S.; Nakaema, F.; Arakaki, T.; Tanahara, A.

2009-12-01

The economic development and population growth in recent Asia have been increasing air pollution. A computer simulation study showed that air pollutants emitted from Asian continent could spread quickly within northern hemisphere. We initiated a study to elucidate the special distribution and chemical characterization of atmospheric aerosols around Okinawa archipelago, Japan. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location in Asia is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. We simultaneously collected bulk aerosol samples by using the same types of high volume air samplers at Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS, Okinawa Island), Kume Island (ca. 160 km south-west of CHAAMS) and Minami-daitou Island (ca. 320 km south-east of CHAAMS). We determined the concentrations of water-soluble anions, cations and dissolved organic carbon (DOC) using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. We report and discuss spatial distribution and temporal variation of chemical species concentrations in bulk atmospheric aerosols collected during July, 2008 to July, 2009. We determine “background” concentration of chemical components in Okinawa archipelago. We then compare each chemical component among CHAAMS, Kume Island and Minami-daito Island to elucidate the influence of the long-range transport of chemical species from Asian continent.

Raman Lidar Measurements of Aerosol Extinction and Backscattering. Report 2; Derivation of Aerosol Real Refractive Index, Single-Scattering Albedo, and Humidification Factor using Raman Lidar and Aircraft Size Distribution

NASA Technical Reports Server (NTRS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Poellot, M.; Kaufman, Y. J.

1998-01-01

Aerosol backscattering and extinction profiles measured by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo Omega(sub 0). Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); Omega(sub 0) varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of Omega(sub 0). The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hattel with the exponent gamma = 0.3 + or - 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

Raman lidar measurements of aerosol extinction and backscattering: 2. Derivation of aerosol real refractive index, single-scattering albedo, and humidification factor using Raman lidar and aircraft size distribution measurements

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Melfi, S. H.; Whiteman, D. N.; Evans, K. D.; Poellot, M.; Kaufman, Y. J.

1998-08-01

Aerosol backscattering and extinction profiles measured by the NASA Goddard Space Flight Center Scanning Raman Lidar (SRL) during the remote cloud sensing (RCS) intensive operations period (IOP) at the Department of Energy Atmospheric Radiation Measurement (ARM) southern Great Plains (SGP) site during two nights in April 1994 are discussed. These profiles are shown to be consistent with the simultaneous aerosol size distribution measurements made by a PCASP (Passive Cavity Aerosol Spectrometer Probe) optical particle counter flown on the University of North Dakota Citation aircraft. We describe a technique which uses both lidar and PCASP measurements to derive the dependence of particle size on relative humidity, the aerosol real refractive index n, and estimate the effective single-scattering albedo ω0. Values of n ranged between 1.4-1.5 (dry) and 1.37-1.47 (wet); ω0 varied between 0.7 and 1.0. The single-scattering albedo derived from this technique is sensitive to the manner in which absorbing particles are represented in the aerosol mixture; representing the absorbing particles as an internal mixture rather than the external mixture assumed here results in generally higher values of ω0. The lidar measurements indicate that the change in particle size with relative humidity as measured by the PCASP can be represented in the form discussed by Hanel [1976] with the exponent γ = 0.3 ± 0.05. The variations in aerosol optical and physical characteristics captured in the lidar and aircraft size distribution measurements are discussed in the context of the meteorological conditions observed during the experiment.

Novel characterization of the aerosol and gas-phase composition of aerosolized jet fuel.

PubMed

Tremblay, Raphael T; Martin, Sheppard A; Fisher, Jeffrey W

2010-04-01

Few robust methods are available to characterize the composition of aerosolized complex hydrocarbon mixtures. The difficulty in separating the droplets from their surrounding vapors and preserving their content is challenging, more so with fuels, which contain hydrocarbons ranging from very low to very high volatility. Presented here is a novel method that uses commercially available absorbent tubes to measure a series of hydrocarbons in the vapor and droplets from aerosolized jet fuels. Aerosol composition and concentrations were calculated from the differential between measured total (aerosol and gas-phase) and measured gas-phase concentrations. Total samples were collected directly, whereas gas-phase only samples were collected behind a glass fiber filter to remove droplets. All samples were collected for 1 min at 400 ml min(-1) and quantified using thermal desorption-gas chromatography-mass spectrometry. This method was validated for the quantification of the vapor and droplet content from 4-h aerosolized jet fuel exposure to JP-8 and S-8 at total concentrations ranging from 200 to 1000 mg/m(3). Paired samples (gas-phase only and total) were collected every approximately 40 min. Calibrations were performed with neat fuel to calculate total concentration and also with a series of authentic standards to calculate specific compound concentrations. Accuracy was good when compared to an online GC-FID (gas chromatography-flame ionization detection) technique. Variability was 15% or less for total concentrations, the sum of all gas-phase compounds, and for most specific compound concentrations in both phases. Although validated for jet fuels, this method can be adapted to other hydrocarbon-based mixtures.

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

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

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

NASA Astrophysics Data System (ADS)

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

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

A Comparison of Aerosol Optical Property Measurements Made During the DOE Aerosol Intensive Operating Period and Their Effects on Regional Climate

NASA Technical Reports Server (NTRS)

Strawa, Anthony W.; Hallar, A. G.; Arnott, W. P.; Covert, D.; Elleman, R.; Ogren, J.; Schmid, B.; Luu, A.

2004-01-01

The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult to measure aerosol properties. One of the main purposes of the DOE Aerosol Intensive Operating Period (IOP) flown in May, 2003 was to assess our ability to measure absorption coefficient in situ. This paper compares measurements of aerosol optical properties made during the IOP. Measurements of aerosol absorption coefficient were made by Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter (U. Washington) and on the DOE Cessna 172 (NOAA-C,MDL). Aerosol absorption coefficient was also measured by a photoacoustic instrument (DRI) that was operated on an aircraft for the first time during the IOP. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-AkC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Measurements of absorption coefficient from all of these instruments during appropriate periods are compared. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model.

1 Mixing state and absorbing properties of black carbon during Arctic haze

NASA Astrophysics Data System (ADS)

Zanatta, Marco; Gysel, Martin; Eleftheriadis, Kosas; Laj, Paolo; Hans-Werner, Jacobi

2016-04-01

The Arctic atmosphere is periodically affected by the Arctic haze occurring in spring. One of its particulate components is the black carbon (BC), which is considered to be an important contributor to climate change in the Arctic region. Beside BC-cloud interaction and albedo reduction of snow, BC may influence Arctic climate interacting directly with the solar radiation, warming the corresponding aerosol layer (Flanner, 2013). Such warming depends on BC atmospheric burden and also on the efficiency of BC to absorb light, in fact the light absorption is enhanced by mixing of BC with other atmospheric non-absorbing materials (lensing effect) (Bond et al., 2013). The BC reaching the Arctic is evilly processed, due to long range transport. Aging promote internal mixing and thus absorption enhancement. Such modification of mixing and is quantification after long range transport have been observed in the Atlantic ocean (China et al., 2015) but never investigated in the Arctic. During field experiments conducted at the Zeppelin research site in Svalbard during the 2012 Arctic spring, we investigated the relative precision of different BC measuring techniques; a single particle soot photometer was then used to assess the coating of Arctic black carbon. This allowed quantifying the absorption enhancement induced by internal mixing via optical modelling; the optical assessment of aged black carbon in the arctic will be of major interest for future radiative forcing assessment.Optical characterization of the total aerosol indicated that in 2012 no extreme smoke events took place and that the aerosol population was dominated by fine and non-absorbing particles. Low mean concentration of rBC was found (30 ng m-3), with a mean mass equivalent diameter above 200 nm. rBC concentration detected with the continuous soot monitoring system and the single particle soot photometer was agreeing within 15%. Combining absorption coefficient observed with an aethalometer and rBC mass

Equilibrium climate response of the East Asian summer monsoon to forcing of anthropogenic aerosol species

NASA Astrophysics Data System (ADS)

Wang, Zhili; Wang, Qiuyan; Zhang, Hua

2017-12-01

We used an online aerosol-climate model to study the equilibrium climate response of the East Asian summer monsoon (EASM) to increases in anthropogenic emissions of sulfate, organic carbon, and black carbon aerosols from 1850 to 2000. Our results show that each of these aerosol species has a different effect on the EASM as a result of changes in the local sea-land thermal contrast and atmospheric circulation. The increased emission of sulfate aerosol leads to a decrease in the thermal contrast between the land and ocean, a southward shift of the East Asian subtropical jet, and significant northerly wind anomalies at 850 hPa over eastern China and the ambient oceans, markedly dampening the EASM. An increase in organic carbon aerosol results in pronounced surface cooling and the formation of an anomalous anticyclone over the oceans north of 30°N. These effects cause a slight increase in the sea-land thermal contrast and southerly flow anomalies to the west of the anticyclonic center, strengthening the northern EASM. An increase in organic carbon emission decreases the sea-land thermal contrast over southern China, which weakens the southern EASM. The response of the summer 850-hPa winds and rainfall over the East Asian monsoon region to an increase in black carbon emission is generally consistent with the response to an increase in organic carbon. The increase in black carbon emission leads to a strengthening of the northern EASM north of 35°N and a slight weakening of the southern EASM south of 35°N. The simulated response of the EASM to the increase in black carbon emission is unchanged when the emission of black carbon is scaled up by five times its year 2000 levels, although the intensities of the response is enhanced. The increase in sulfate emission primarily weakens the EASM, whereas the increases in black carbon and organic carbon emissions mitigate weakening of the northern EASM.

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

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-05-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative budget. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative budget over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local

Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM

NASA Astrophysics Data System (ADS)

Kazil, J.; Stier, P.; Zhang, K.; Quaas, J.; Kinne, S.; O'Donnell, D.; Rast, S.; Esch, M.; Ferrachat, S.; Lohmann, U.; Feichter, J.

2010-11-01

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative forcing. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative forcing over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local

The Influence of Anthropogenic Greenhouse Gases and Aerosols on the Surface Heat and Moisture Budgets.

NASA Astrophysics Data System (ADS)

Ramaswamy, V.; Freidenreich, S.; Ginoux, P. A.; Ming, Y.; Paynter, D.; Persad, G.; Schwarzkopf, M. D.

2017-12-01

Emissions of greenhouse gases and aerosols alter atmospheric composition and `force' major perturbations in the radiative fluxes at the top-of-the-atmosphere and surface. In this paper, we discuss the radiative changes caused by anthropogenic greenhouse gases and aerosols at the surface, and its importance in the context of effects on the global hydrologic cycle. An important characteristic of imbalances forced by radiative species is the tendency for responses to occur in the non-radiative components, in order for the surface energy and moisture budgets to re-establish equilibrium. Using the NOAA/ GFDL global climate models used in CMIP3 and CMIP5, and to be used in CMIP6, we investigate how the surface energy balance has evolved with time under the action of the emissions, and the manner of changes in the surface radiative, sensible and latent heat components. We diagnose the relative importance of the forcings on the global and continental scales, the differing mechanisms due to greenhouse gases and aerosols on surface heat and moisture budgets, and the relative roles of the atmospheric constituents on precipitation and evaporation. Scattering and absorbing properties of aerosols can have contrasting effects on precipitation, with the aerosol indirect effect presenting another complication owing to the uncertainty in its magnitude. We compare the modeled surface flux changes against observations made from multiple platforms over the 20th and the early period of the 21st centuries, and asses the models' strengths and weaknesses. We also explore the consequences for the surface balance and precipitation in the 21st century under various emission scenarios.

CLouds, and Aerosols Radiative Impacts and Forcing: Year 2016 (CLARIFY-2016)

NASA Astrophysics Data System (ADS)

Haywood, J. M.; Bellouin, N.; Carslaw, K. S.; Coe, H.; Field, P.; Highwood, E. J.; Redemann, J.; Stier, P.; Wood, R.; Zuidema, P.

2013-12-01

Strongly absorbing biomass burning aerosols (BBAs) exist above highly reflectant stratocumulus clouds in the SE Atlantic with implications on the direct (e.g. Haywood et al., 2003), semi-direct (e.g. Johnson et al., 2006), and indirect effect of aerosols, implications on the remote sensing of cloud optical properties, development of clouds and feedback processes. Here, we present an analysis of modelled estimates of the direct effect using twelve models from the AEROCOM project (Myhre et al., 2013) to show that estimates of the direct effect in SE Atlantic range from strongly negative to strongly positive. Furthermore, we evaluate the performance of the HadGEM2 model and show it cannot replicate the extreme values of positive forcing inferred from high spectral resolution satellite retrievals. By examining patterns of deposition, we infer that the indirect effect from biomass burning aerosols is very limited in the model, but without detailed measurements we are unsure of the validity of this inference. We conclude that the SE Atlantic is therefore of key importance in determining the radiative forcing of biomass burning aerosols and provides a very stringent test for global climate models as they need to accurately represent the geographic distribution of the aerosol optical depth, the wavelength dependent aerosol single scattering albedo, the vertical profile of the aerosol, the geographic distribution of the cloud, the cloud fraction, the cloud liquid water content, the cloud droplet effective radii, and the vertical profile of the cloud. These results are used as scientific rationale to justify a new measurement campaign: CLouds and Aerosol Radiative Impacts and Forcing: Year-2016 (CLARIFY-2016). Haywood, J.M., Osborne, S.R. Francis, P.N., Keil, A., Formenti, P., Andreae, M.O., and Kaye, P.H., The mean physical and optical properties of regional haze dominated by biomass burning aerosol measured from the C-130 aircraft during SAFARI 2000, J. Geophys. Res., 108

Influence of mineral dust transport on the chemical composition and physical properties of the Eastern Mediterranean aerosol

NASA Astrophysics Data System (ADS)

Koçak, M.; Theodosi, C.; Zarmpas, P.; Séguret, M. J. M.; Herut, B.; Kallos, G.; Mihalopoulos, N.; Kubilay, N.; Nimmo, M.

2012-09-01

Bulk aerosol samples were collected from three different coastal rural sites located around the Eastern Mediterranean, (i) Erdemli (ER), Turkey, (ii) Heraklion (HR), Crete, Greece, and (iii) Tel Shikmona (TS), Israel, during two distinct mineral dust periods (October, 2007 and April, 2008) in order to explore the temporal and geographical variability in the aerosol chemical composition. Samples were analyzed for trace elements (Al, Fe, Mn, Ca, Cr, Zn, Cu, V, Ni, Cd, Pb) and water-soluble ions (Cl-, NO3-, SO42-, C2O42-, Na+, NH4+, K+, Mg2+ and Ca2+). The dust events were categorized on the basis of Al concentrations >1000 ng m-3, SKIRON dust forecast model and 3-day back trajectories into three groups namely, Middle East, Mixed and Saharan desert. ER and TS were substantially affected by dust events originating from the Middle East, particularly in October, whilst HR was not influenced by dust transport from the Middle East. Higher AOT values were particularly associated with higher Al concentrations. Contrary to the highest Al concentration: 6300 ng m-3, TS showed relatively lower AI and AOT. Al concentrations at ER were similar for October and April, whilst OMI-AI and AOT values were ˜2 times higher in April. This might be attributed to the weak sensitivity of the TOMS instrument to absorbing aerosols near the ground and optical difference between Middle East and Saharan desert dusts. The lowest enhancement of anthropogenic aerosol species was observed at HR during dust events (nssSO42-/nssCa2+ ˜ 0.13). These species were particularly enhanced when mineral dust arrived at sites after passing through populated and industrialized urban areas.

Carbonaceous Aerosol Characterization during 2016 KOR-US 2016

NASA Astrophysics Data System (ADS)

Rodriguez, B.; Santos, G. M.; Sanchez, D.; Jeong, D.; Czimczik, C. I.; Kim, S.

2017-12-01

Atmospheric carbonaceous aerosols are a major component of fine particulate matter and assume important roles in Earth's climate and human health. Because atmospheric carbonaceous aerosols exist as a continuum ranging from small, light-scattering organic carbon (OC), to highly-condensed, light-absorbing elemental carbon (EC) they have contrasting effects on interaction with incoming and outgoing radiation, cloud formation, and snow/ice albedo. By strengthening our understanding of the relative contribution and sources of OC and EC we will be able to further describe aerosol formation and mixing at the regional level. To understand the relative anthropogenic and biogenic contributions to carbonaceous aerosol, 12 PM10 aerosols samples were collected on quartz fiber filters at the Mt. Taewha Research Forest in South Korea during the KORUS-AQ 2016 campaign over periods of 24-48 hours with a high-volume air sampler. Analysis of bulk C and N concentrations and absorption properties of filter extracts interspersed with HYSPLIT model results indicated that continental outflow across the Yellow Sea in enriched in bulk nitrogen loading and enhanced bulk absorptive properties of the aerosols. Bulk radiocarbon analysis also indicated enriched values in all samples indicating contamination from a nuclear power plant or the combustion of biomedical waste nearby. Here, we aim to investigate further the chemical characterization of VOCs adsorbed unto the aerosol through TD-GC-TOFMS. With this dataset we aim to determine the relative contribution of anthropogenic and biogenic aerosols by utilizing specific chemical tracers for source apportionment.

Aeronet-based Microphysical and Optical Properties of Smoke-dominated Aerosol near Source Regions and Transported over Oceans, and Implications for Satellite Retrievals of Aerosol Optical Depth

NASA Technical Reports Server (NTRS)

Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

2013-01-01

Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad families of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA 0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA 0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savanna at Mongu (Zambia), with average SSA 0.85 in the midvisible. These can serve as candidate sets of aerosol microphysicaloptical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

Atmospheric aerosol brown carbon in the high Himalayas

NASA Astrophysics Data System (ADS)

Kirillova, Elena; Decesari, Stefano; Marinoni, Angela; Bonasoni, Paolo; Vuillermoz, Elisa; Facchini, M. Cristina; Fuzzi, Sandro

2016-04-01

Anthropogenic light-absorbing atmospheric aerosol can reach very high concentrations in the planetary boundary layer in South-East Asia ("brown clouds"), affecting atmospheric transparency and generating spatial gradients of temperature over land with a possible impact on atmospheric dynamics and monsoon circulation. Besides black carbon (BC), an important light-absorbing component of anthropogenic aerosols is the organic carbon component known as 'brown carbon' (BrC). In this research, we provided first measurements of atmospheric aerosol BrC in the high Himalayas during different seasons. Aerosol sampling was conducted at the GAW-WMO Global station "Nepal Climate Observatory-Pyramid" (NCO-P) located in the high Khumbu valley at 5079 m a.s.l. in the foothills of Mt. Everest. PM10 aerosol samples were collected from July 2013 to November 2014. The sampling strategy was set up in order to discriminate the daytime valley breeze bringing polluted air masses up to the observatory and free tropospheric air during nighttime. Water-soluble BrC (WS-BrC) and methanol-soluble BrC (MeS-BrC) were extracted and analyzed using a UV/VIS spectrophotometer equipped with a 50 cm liquid waveguide capillary cell. In the polluted air masses, the highest levels of the BrC light absorption coefficient at 365 nm (babs365) were observed during the pre-monsoon season (1.83±1.46 Mm-1 for WS-BrC and 2.86±2.49 Mm-1 for MeS-BrC) and the lowest during the monsoon season (0.21±0.22 Mm-1 for WS-BrC and 0.32±0.29 Mm-1 for MeS-BrC). The pre-monsoon season is the most frequently influenced by a strong atmospheric brown cloud (ABC) transport to NCO-P due to increased convection and mixing layer height over South Asia combined with the highest up-valley wind speed and the increase of the emissions from open fires due to the agricultural practice along the Himalayas foothills and the Indo-Gangetic Plain. In contrast, the monsoon season is characterized by a weakened valley wind regime and an

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

NASA Astrophysics Data System (ADS)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Assessment of the aerosol distribution over Indian subcontinent in CMIP5 models

NASA Astrophysics Data System (ADS)

Sanap, S. D.; Ayantika, D. C.; Pandithurai, G.; Niranjan, K.

2014-04-01

This paper examines the aerosol distribution over Indian subcontinent as represented in 21 models from Coupled Model Inter-comparison Project Phase 5 (CMIP5) simulations, wherein model simulated aerosol optical depth (AOD) is compared with Moderate Resolution Imaging Spectro-radiometer (MODIS) satellite observations. The objective of the study is to provide an assessment of the capability of various global models, participating in CMIP5 project, in capturing the realistic spatial and temporal distribution of aerosol species over the Indian subcontinent. Results from our analysis show that majority of the CMIP5 models (excepting HADGEM2-ES, HADGEM2-CC) seriously underestimates the spatio-temporal variability of aerosol species over the Indian subcontinent, in particular over Indo-Gangetic Plains (IGP). Since IGP region is dominated by anthropogenic activities, high population density, and wind driven transport of dust and other aerosol species, MODIS observations reveal high AOD values over this region. Though the representation of black carbon (BC) loading in many models is fairly good, the dust loading is observed to be significantly low in majority of the models. The presence of pronounced dust activity over northern India and dust being one of the major constituent of aerosol species, the biases in dust loading has a great impact on the AOD of that region. We found that considerable biases in simulating the 850 hPa wind field (which plays important role in transport of dust from adjacent deserts) would be the possible reason for poor representation of dust AOD and in turn total AOD over Indian region in CMIP5 models. In addition, aerosol radiative forcing (ARF) underestimated/overestimated in most of the models. However, spatial distribution of ARF in multi-model ensemble mean is comparable reasonably well with observations with bias in magnitudes. This analysis emphasizes the fundamental need to improve the representation of aerosol species in current state of

Absorption of visible radiation in atmosphere containing mixtures of absorbing and nonabsorbing particles

NASA Technical Reports Server (NTRS)

Ackerman, T. P.; Toon, O. B.

1981-01-01

The presence of a strongly absorbing material, tentatively identified as graphitic carbon, or 'soot', is indicated by measurements of single-scattering albedo of tropospheric aerosols. Although theoretical calculations based on models of the ways in which soot may mix with other aerosol materials yield the single-scattering albedo values of 0.6, accounted for by a minimum 20% soot by volume, in urban regions and 0.8, yielded by 1-5% soot by volume, in rural settings, it is found that these same values can be produced by similar amounts of the iron oxide magnetite. Magnetite is shown to be indistinguishable from soot by optical measurements performed on bulk samples, and calculation of various mixtures of soot indicate the difficulty of determining aerosol composition by optical scattering techniques.

Development, Comparisons and Evaluation of Aerosol Retrieval Algorithms

NASA Astrophysics Data System (ADS)

de Leeuw, G.; Holzer-Popp, T.; Aerosol-cci Team

2011-12-01

The Climate Change Initiative (cci) of the European Space Agency (ESA) has brought together a team of European Aerosol retrieval groups working on the development and improvement of aerosol retrieval algorithms. The goal of this cooperation is the development of methods to provide the best possible information on climate and climate change based on satellite observations. To achieve this, algorithms are characterized in detail as regards the retrieval approaches, the aerosol models used in each algorithm, cloud detection and surface treatment. A round-robin intercomparison of results from the various participating algorithms serves to identify the best modules or combinations of modules for each sensor. Annual global datasets including their uncertainties will then be produced and validated. The project builds on 9 existing algorithms to produce spectral aerosol optical depth (AOD and Ångström exponent) as well as other aerosol information; two instruments are included to provide the absorbing aerosol index (AAI) and stratospheric aerosol information. The algorithms included are: - 3 for ATSR (ORAC developed by RAL / Oxford university, ADV developed by FMI and the SU algorithm developed by Swansea University ) - 2 for MERIS (BAER by Bremen university and the ESA standard handled by HYGEOS) - 1 for POLDER over ocean (LOA) - 1 for synergetic retrieval (SYNAER by DLR ) - 1 for OMI retreival of the absorbing aerosol index with averaging kernel information (KNMI) - 1 for GOMOS stratospheric extinction profile retrieval (BIRA) The first seven algorithms aim at the retrieval of the AOD. However, each of the algorithms used differ in their approach, even for algorithms working with the same instrument such as ATSR or MERIS. To analyse the strengths and weaknesses of each algorithm several tests are made. The starting point for comparison and measurement of improvements is a retrieval run for 1 month, September 2008. The data from the same month are subsequently used for

Carbon Isotopic Measurements and Aerosol Optical Determinations during CARES: Indications of the Importance of Background Biogenic Aerosols

NASA Astrophysics Data System (ADS)

Gaffney, J. S.; Marley, N. A.; Begum, M.; Sturchio, N. C.; Guilderson, T. P.

2011-12-01

High volume size-fractionated aerosol samples were obtained in Cool, CA during the Carbonaceous Aerosol and Radiative Effects Study (CARES) in June of 2010. This site was chosen to study the regional impacts of carbonaceous aerosols originating from the Sacramento area. Samples were collected for 6 to 24 hour time periods on quartz fiber filters by using slotted impactors to allow for collection of sample size cuts above and below one micron. Both total carbon content and carbon isotopic composition, including 13C/12C and 14C, were determined on the samples. In addition, Ångstrom absorption exponents (AAEs) were determined for the region of 300-900 nm on the sub-micron size cut by using state of the art diffuse reflectance UV-visible spectroscopy with integrating sphere technology. The overall carbonaceous aerosol loadings were found to be quite low and relatively constant during the study, suggesting that most of the aerosols at the site were locally formed background aerosols. The 14C data is consistent with a substantial fraction (~80 %) being from modern carbon sources and 13C/12C results indicate that the carbon source was from C-3 plants. This is consistent with a significant fraction of the aerosols in the area arising from secondary formation from biogenic precursor emissions from trees, most likely mono- and sesquiterpenes. These results are compared to past results obtained in Mexico City and discussed in terms of the potential importance of biogenic emissions to UV absorbing aerosols as these are anticipated to increase with climate change. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328 and Grant No. DE-FG02-07-ER64329 as part of the Atmospheric Systems Research program.

Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

PubMed

Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

2015-05-14

Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores

Aerosol in the Pacific troposphere

NASA Technical Reports Server (NTRS)

Clarke, Antony D.

1989-01-01

The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.

Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Dreyfus, Matthew A.

Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

Quantification of uncertainty in aerosol optical thickness retrieval arising from aerosol microphysical model and other sources, applied to Ozone Monitoring Instrument (OMI) measurements

NASA Astrophysics Data System (ADS)

Määttä, A.; Laine, M.; Tamminen, J.; Veefkind, J. P.

2014-05-01

Satellite instruments are nowadays successfully utilised for measuring atmospheric aerosol in many applications as well as in research. Therefore, there is a growing need for rigorous error characterisation of the measurements. Here, we introduce a methodology for quantifying the uncertainty in the retrieval of aerosol optical thickness (AOT). In particular, we concentrate on two aspects: uncertainty due to aerosol microphysical model selection and uncertainty due to imperfect forward modelling. We apply the introduced methodology for aerosol optical thickness retrieval of the Ozone Monitoring Instrument (OMI) on board NASA's Earth Observing System (EOS) Aura satellite, launched in 2004. We apply statistical methodologies that improve the uncertainty estimates of the aerosol optical thickness retrieval by propagating aerosol microphysical model selection and forward model error more realistically. For the microphysical model selection problem, we utilise Bayesian model selection and model averaging methods. Gaussian processes are utilised to characterise the smooth systematic discrepancies between the measured and modelled reflectances (i.e. residuals). The spectral correlation is composed empirically by exploring a set of residuals. 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 introduced here. The method and improved uncertainty characterisation is demonstrated by several examples with different aerosol properties: weakly absorbing aerosols, forest fires over Greece and Russia, and Sahara desert dust. The statistical methodology presented is general; it is not restricted to this particular satellite retrieval application.

Aerosols, light, and water: Measurements of aerosol optical properties at different relative humidities

NASA Astrophysics Data System (ADS)

Orozco, Daniel

The Earth's atmosphere is composed of a large number of different gases as well as tiny suspended particles, both in solid and liquid state. These tiny particles, called atmospheric aerosols, have an immense impact on our health and on our global climate. Atmospheric aerosols influence the Earth's radiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence the Earth's radiation budget by modifying the microphysical and radiative properties of clouds as well as their water content and lifetime. In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering coefficient and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground based observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. This dissertation presents the aerosol hygroscopicity experiment investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (sp) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (Jan 10-Feb 6, 2013), Baltimore, MD (Jul 3-30, 2013), and Golden, CO (Jul 12-Aug 10, 2014). Observations in Porterville and Golden were part of the NASA-sponsored DISCOVER-AQ project. The measured sp under varying RH in the three sites was combined with ground aerosol extinction, PM2:5mass concentrations, particle composition measurements, and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of sp

Fingerprinting the Impacts of Aerosols on Long-Term Trends of the Indian Summer Monsoon Regional Rainfall

NASA Technical Reports Server (NTRS)

Laul, K. M.; Kim, K. M.

2010-01-01

In this paper, we present corroborative observational evidences from satellites, in-situ observations, and re-analysis data showing possible impacts of absorbing aerosols (black carbon and dust) on subseasonal and regional summer monsoon rainfall over India. We find that increased absorbing aerosols in the Indo-Gangetic Plain in recent decades may have lead to long-term warming of the upper troposphere over northern India and the Tibetan Plateau, enhanced rainfall in northern India and the Himalayas foothill regions in the early part (may-June) of the monsoon season, followed by diminished rainfall over central and southern India in the latter part (July-August) of the monsoon season. These signals which are consistent with current theories of atmospheric heating and solar dimming by aerosol and induced cloudiness in modulating the Indian monsoon, would have been masked by conventional method of using al-India rainfall averaged over the entire monsoon season.

Remote Sensing of Non-Aerosol (anomalous) Absorption in Cloud Free Atmosphere

NASA Technical Reports Server (NTRS)

Kaufman, Yoram J.; Dubovik, Oleg; Smirnov, Alexander; Holben, Brent N.; Lau, William K. M. (Technical Monitor)

2001-01-01

The interaction of sunlight with atmospheric gases, aerosols and clouds is fundamental to the understanding of climate and its variation. Several studies questioned our understanding of atmospheric absorption of sunlight in cloudy or in cloud free atmospheres. Uncertainty in instruments' accuracy and in the analysis methods makes this problem difficult to resolve. Here we use several years of measurements of sky and sun spectral brightness by selected instruments of the Aerosol Robotic Network (AERONET), that have known and high measurement accuracy. The measurements taken in several locations around the world show that in the atmospheric windows 0.44, 0.06, 0.86 and 1.02 microns the only significant absorbers in cloud free atmosphere is aerosol and ozone. This conclusions is reached using a method developed to distinguish between absorption associated with the presence of aerosol and absorption that is not related to the presence of aerosol. Non-aerosol absorption, defined as spectrally independent or smoothly variable, was found to have an optical thickness smaller than 0.002 corresponding to absorption of sunlight less than 1W/sq m, or essentially zero.

Overview of ACE-Asia Spring 2001 Investigations on Aerosol Radiative Effects and Related Aerosol Properties

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Valero, F. P. J.; Flatau, P. J.; Bergin, M.; Holben, B.; Nakajima, T.; Pilewskie, P.; Bergstrom, R.; Hipskind, R. Stephen (Technical Monitor)

2001-01-01

depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.

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...

A Novel Method for Estimating Shortwave Direct Radiative Effect of Above-cloud Aerosols over Ocean Using CALIOP and MODIS Data

NASA Technical Reports Server (NTRS)

Zhang, Z.; Meyer, K.; Platnick, S.; Oreopoulos, L.; Lee, D.; Yu, H.

2013-01-01

This paper describes an efficient and unique method for computing the shortwave direct radiative effect (DRE) of aerosol residing above low-level liquid-phase clouds using CALIOP and MODIS data. It accounts for the overlapping of aerosol and cloud rigorously by utilizing the joint histogram of cloud optical depth and cloud top pressure. Effects of sub-grid scale cloud and aerosol variations on DRE are accounted for. It is computationally efficient through using grid-level cloud and aerosol statistics, instead of pixel-level products, and a pre-computed look-up table in radiative transfer calculations. We verified that for smoke over the southeast Atlantic Ocean the method yields a seasonal mean instantaneous shortwave DRE that generally agrees with more rigorous pixel-level computation within 4%. We have also computed the annual mean instantaneous shortwave DRE of light-absorbing aerosols (i.e., smoke and polluted dust) over global ocean based on 4 yr of CALIOP and MODIS data. We found that the variability of the annual mean shortwave DRE of above-cloud light-absorbing aerosol is mainly driven by the optical depth of the underlying clouds.

African aerosols and Atlantic tropical cyclone activities

NASA Astrophysics Data System (ADS)

Kafatos, M.; Sun, D.; Sahoo, A.

2006-12-01

Previous studies have shown that the Atlantic basin major hurricane (MH) activity is associated with western Sahelian monsoon rainfall, while rainfall in the Sahel is found to be highly anti-correlated with the African dust storms. So if the Atlantic basin MH activity may be anti-correlated with the African dust aerosols? In order to investigate the relationship between the African dust and the tropical cyclone (including both tropical storms and hurricanes) activities in the Atlantic basin, we explore how the African dust may link to Atlantic TC activity by using the long-term (1982-2005) NCEP Reynolds sea surface temperature (SST) product, and tropical cyclone (TC) data from the National Hurricane Center Best Track Files, and the TOMS aerosol index (AI) data, because the TOMS AI positive values are associated with UV-absorbing aerosols, like dust and smoke. Although no significant negative correlation between the TOMS AI and the Atlantic TC or MH frequency and duration is found, the initial locations of the Atlantic tropical cyclones did occur over the ocean where the aerosol loading was low. Our analysis shows that SST over the north tropical Atlantic ocean is anti-correlated with the TOMS aerosol index. This may be due to the radiative forcing of the aerosols. The effects of the dust aerosols carried across the West African region led to a lowering of SST and therefore inhibited tropical cyclogenesis. During 2005, the aerosol loading along the western African coast was unusually low, while the SST over the main development region (MDR) was abnormally high, and the Atlantic TC/hurricane activities became record strong. We propose future observations to test these results.

Characterization of aerosols over the Indochina peninsula from satellite-surface observations during biomass burning pre-monsoon season

NASA Astrophysics Data System (ADS)

Gautam, Ritesh; Hsu, N. Christina; Eck, Thomas F.; Holben, Brent N.; Janjai, Serm; Jantarach, Treenuch; Tsay, Si-Chee; Lau, William K.

2013-10-01

This paper presents characterization of aerosols over the Indochina peninsular regions of Southeast Asia during pre-monsoon season from satellite and ground-based radiometric observations. Our analysis focuses on the seasonal peak period in aerosol loading and biomass burning, prior to the onset of the Asian summer monsoon, as observed in the inter-annual variations of Aerosol Optical Depth (AOD) and fire count data from MODIS. Multi-year (2007-2011) analysis of spaceborne lidar measurements, from CALIOP, indicates presence of aerosols mostly within boundary layer, however extending to elevated altitudes to ˜4 km over northern regions of Indochina, encompassing Myanmar, northern Thailand and southern China. In addition, a strong gradient in aerosol loading and vertical distribution is observed from the relatively clean equatorial conditions to heavy smoke-laden northern regions (greater aerosol extinction and smaller depolarization ratio). Based on column-integrated ground-based measurements from four AERONET locations distributed over Thailand, the regional aerosol loading is found to be significantly absorbing with spectral single scattering albedo (SSA) below 0.91 ± 0.02 in the 440-1020 nm range, with lowest seasonal mean SSA (most absorbing aerosol) over the northern location of Chiang Mai (SSA ˜ 0.85) during pre-monsoon season. The smoke-laden aerosol loading is found to exhibit a significant diurnal pattern with higher AOD departures during early morning observations relative to late afternoon conditions (peak difference of more than 15% amplitude). Finally, satellite-based aerosol radiative impact is assessed using CERES shortwave Top-of-Atmosphere flux, in conjunction with MODIS AOD. Overall, a consistency in the aerosol-induced solar absorption characteristic is found among selected regions from ground-based sunphotometer-derived spectral SSA retrievals and satellite-based radiative forcing analysis.

Field Studies of Broadband Aerosol Optical Extinction in the Ultraviolet Spectral Region

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A.; Brock, C. A.; Brown, S. S.

2013-12-01

Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. In the case of brown carbon, its wavelength-dependent absorption in the ultraviolet spectral region has been suggested as an important component of aerosol radiative forcing. We describe a new field instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We deployed this instrument during the Fire Lab at Missoula Experiment during Fall 2012 to measure biomass burning aerosol, and again during the Southern Oxidant and Aerosol Study in summer 2013 to measure organic aerosol in the Southeastern U.S. In both field experiments, we determined aerosol optical extinction as a function of wavelength and can interpret this together with size distribution and composition measurements to characterize the aerosol optical properties and radiative forcing.

Vacuum FTIR observation on hygroscopic properties and phase transition of malonic acid aerosols

NASA Astrophysics Data System (ADS)

Shao, Xu; Zhang, Yun; Pang, Shu-Feng; Zhang, Yun-Hong

2017-02-01

A novel approach based on a combination of a pulse relative humidity (RH) controlling system and a rapid scan vacuum FTIR spectrometer was utilized to investigate the hygroscopic property and phase transition of malonic acid (MA) aerosols. By using this approach, both water vapor amount around the aerosols and water content within aerosols with sub-second time resolution were obtained. Based on the features of FTIR absorbing bands, it can be known that the evolution of hydrogen-bonding structures of malonic acid aerosols took place from (H2O)n-MA to MA-MA accompanying with phase transition in the dehumidifying process. And in present paper, the stepwise efflorescence of MA aerosols and nucleation rates at different RHs are first reported. Our observation has shown that the efflorescence of MA started at ∼17% RH and the nucleation rates increased with decreasing RH.

Tropospheric Trace Gas Interactions with Aerosols

NASA Technical Reports Server (NTRS)

Penner, Joyce E.; Maddrea, George L., Jr. (Technical Monitor)

2002-01-01

Tropospheric aerosols are of considerable environmental importance. They modify the radiative budget of Earth by scattering and absorbing radiation, and by providing nuclei for cloud formation. Additionally, they provide surfaces for heterogeneous and multiphase reactions that affect tropospheric chemistry. For example, Dentener and Crutzen (1993) showed that reactions of N2O5 and NO3 with sulfate aerosols may significantly alter the tropospheric concentrations of NO(x), O3, and OH by converting NOx to HNO3 which is rapidly removed by precipitation. Zhang et al. (1994) assumed these same reactions would occur on dust aerosols and showed that dust outbreaks may reduce NO(x) levels by up to 50%. Dentener et al. (1996) studied the possible effect of reactions on dust on sulfate, nitrate, and O3 concentration. Heterogeneous and multiphase reactions on aerosols may also perturb the sulfur cycle the chlorine cycle and the bromine cycle. Because these reactions can release free chlorine and free bromine they might lead to the destruction of ozone in the marine boundary layer that may be important to include in models of tropospheric chemistry. The goal of our proposed work is to examine the role of heterogeneous and multiphase reactions in the tropospheric cycles of reactive nitrogen and sulfur.

Theoretical Characterization of the Radiative Properties of Dust Aerosol for the Air Force Combat Climatology Center Point Analysis Intelligence System

DTIC Science & Technology

2007-03-01

dust aerosol is known to absorb radiation in these wavelengths. Therefore, the absorptive properties of the aerosol must be taken into account to...of the dust aerosol on radiation propagation is complicated. The study addressed this problem by modeling various radiative transfer situations...are ubiquitous in nature and frequently are the determining factor in the amount of radiation received at a sensor.” The horizontal and vertical

Heterogeneous Reduction Pathways for Hg(II) Species on Dry Aerosols: A First-Principles Computational Study

DOE PAGES

Tacey, Sean A.; Xu, Lang; Mavrikakis, Manos; ...

2016-03-25

Here, the atmospheric lifetime of mercury is greatly impacted by redox chemistry resulting from the high deposition rate of reactive mercury (Hg(II)) compared to elemental mercury (Hg 0). Recent laboratory and field studies have observed the reduction of Hg(II) but the chemical mechanism for this reaction has not been identified. Recent laboratory studies have shown that the reduction reaction is heterogeneous and can occur on iron and sodium chloride aerosol surfaces. This study explores the use of density functional theory calculations to discern the reduction pathways of HgCl 2, HgBr 2, Hg(NO 3) 2, and HgSO 4 on clean Fe(110),more » NaCl(100), and NaCl(111) Na surfaces. In doing so, potential energy surfaces have been prepared for the various reduction pathways, indicating that the reduction pathway leading to the production of gas-phase elemental mercury is highly favorable on Fe(110) and NaCl(111) Na. Moreover, the Fe(110) surface requires an external energy source of approximately 0.5 eV to desorb the reduced mercury, whereas the NaCl(111) Na surface requires no energy input. The results indicate that a number of mercury species can be reduced on metallic iron and sodium chloride surfaces, which are known aerosol components, and that a photochemical reaction involving the aerosol surface is likely needed for the reaction to be catalytic.« less

Simultaneously inferring above-cloud absorbing aerosol optical thickness and underlying liquid phase cloud optical and microphysical properties using MODIS

NASA Astrophysics Data System (ADS)

Meyer, Kerry; Platnick, Steven; Zhang, Zhibo

2015-06-01

The regional haze over the southeast (SE) Atlantic Ocean induced by biomass burning in southern Africa can be problematic for passive imager-based retrievals of the underlying quasi-permanent marine boundary layer (MBL) clouds and for estimates of top-of-atmosphere (TOA) aerosol direct radiative effect (DRE). Here an algorithm is introduced to simultaneously retrieve above-cloud aerosol optical thickness (AOT), the cloud optical thickness (COT), and cloud effective particle radius (CER) of the underlying MBL clouds while also providing pixel-level estimates of retrieval uncertainty. This approach utilizes reflectance measurements at six Moderate Resolution Imaging Spectroradiometer (MODIS) channels from the visible to the shortwave infrared. Retrievals are run under two aerosol model assumptions on 8 years (2006-2013) of June-October Aqua MODIS data over the SE Atlantic, from which a regional cloud and above-cloud aerosol climatology is produced. The cloud retrieval methodology is shown to yield COT and CER consistent with those from the MODIS operational cloud product (MOD06) when forcing AOT to zero, while the full COT-CER-AOT retrievals that account for the above-cloud aerosol attenuation increase regional monthly mean COT and CER by up to 9% and 2%, respectively. Retrieved AOT is roughly 3 to 5 times larger than the collocated 532 nm Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) retrievals, though closer agreement is observed with the CALIOP 1064 nm retrievals, a result consistent with previous case study analyses. Regional cloudy-sky above-cloud aerosol DRE calculations are also performed that illustrate the importance of the aerosol model assumption and underlying cloud retrievals.

Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

NASA Technical Reports Server (NTRS)

Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin

2003-01-01

During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

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.

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.

Effect of Aerosols on Surface Radiation and Air Quality in the Central American Region Estimated Using Satellite UV Instruments

NASA Astrophysics Data System (ADS)

Bhartia, P. K.; Torres, O.; Krotkov, N. A.

2007-05-01

Solar radiation reaching the Earth's surface is reduced by both aerosol scattering and aerosol absorption. Over many parts of the world the latter effect can be as large or larger than the former effect, and small changes in the aerosol single scattering albedo can either cancel the former effect or enhance it. In addition, absorbing aerosols embedded in clouds can greatly reduce the amount of radiation reaching the surface by multiple scattering. Though the potential climatic effects of absorbing aerosols have received considerable attention lately, their effect on surface UV, photosynthesis, and photochemistry can be equally important for our environment and may affect human health and agricultural productivity. Absorption of all aerosols commonly found in the Earth's atmosphere becomes larger in the UV and blue wavelengths and has a relatively strong wavelength dependence. This is particularly true of mineral dust and organic aerosols. However, these effects have been very difficult to estimate on a global basis since the satellite instruments that operate in the visible are primarily sensitive to aerosol scattering. A notable exception is the UV Aerosol Index (AI), first produced using NASA's Nimbus-7 TOMS data. AI provides a direct measure of the effect of aerosol absorption on the backscattered UV radiation in both clear and cloudy conditions, as well as over snow/ice. Although many types of aerosols produce a distinct color cast in the visible images, and aerosols absorption over clouds and snow/ice could, in principle be detected from their color, so far this technique has worked well only in the UV. In this talk we will discuss what we have learned from the long-term record of AI produced from TOMS and Aura/OMI about the possible role of aerosols on surface radiation and air quality in the Central American region.

Modeling aerosol water uptake in the arctic based on the κ-Kohler theory

NASA Astrophysics Data System (ADS)

Rastak, N.; Ekman, A.; Silvergren, S.; Zieger, P.; Wideqvist, U.; Ström, J.; Svenningsson, B.; Tunved, P.; Riipinen, I.

2013-05-01

Water uptake or hygroscopicity is one of the most fundamental properties of atmospheric aerosols. Aerosol particles containing soluble materials can grow in size by absorbing water in ambient atmosphere. This property is measured by a parameter known as growth factor (GF), which is defined as the ratio of the wet diameter to the dry diameter. Hygroscopicity controls the size of an aerosol particle and therefore its optical properties in the atmosphere. Hygroscopic growth depends on the dry size of the particle, its chemical composition and the relative humidity in the ambient air (Fitzgerald, 1975; Pilinis et al., 1995). One of the typical problems in aerosol studies is the lack of measurements of aerosol size distributions and optical properties in ambient conditions. The gap between dry measurements and the real humid atmosphere is filled in this study by utilizing a hygroscopic model which calculates the hygroscopic growth of aerosol particles at Mt Zeppelin station, Ny Ålesund, Svalbard during 2008.

Natural and Anthropogenic Aerosols in the World's Megacities and Climate Impacts

NASA Astrophysics Data System (ADS)

Kafatos, M.; Singh, R.; El-Askary, H.; Qu, J.

2005-12-01

aerosols. The highest boundary layer heights are associated with regions where the sensible heat flux is greatest, and latent heat flux is smallest due to lack of vegetation. Boundary layer heights in the deserts may be systematically higher than the slightly wetter regions at the edges of deserts. Latent heat flux model runs and MODIS observations of dust storms affecting the Nile Delta and Cairo indicate strong influence on the local weather and climate forcings. In the Indo-Gangetic, during the pre-monsoon period, dust storms form. We have examined SDS transport using RS data acquired from NASA's MODIS MISR instruments and from sun photometer measurements. The aerosol optical depth and size of the dust particles are found to be significantly higher during such dust storm events. Moreover, our results clearly show that power plants in this region are the key point source of air pollutants. The detailed analysis of aerosol parameters show the existence of absorbing and non-absorbing aerosols emitted from these plants. The combined effects of urban aerosols with dust aerosols in India and Cairo not only affect megacities, they also have long-term climate impacts. We will also discuss how the assimilation of RS data into mesoscale models can improve these models and predictability of hazards and effects on megacities, such as SDS events, and forest fires, all sources of aerosols. Therefore RS data can improve the prediction of climate forcings by aerosols.

Utilization of O4 slant column density to derive aerosol layer height from a spaceborne UV-visible hyperspectral sensor: sensitivity and case study

NASA Astrophysics Data System (ADS)

Park, S. S.; Kim, J.; Lee, H.; Torres, O.; Lee, K.-M.; Lee, S. D.

2015-03-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using simulated radiances by a radiative transfer model, Linearized Discrete Ordinate Radiative Transfer (LIDORT), and Differential Optical Absorption Spectroscopy (DOAS) technique. The sensitivities of the O4 SCDs to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4 SCD at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 414 m (16.5%), 564 m (22.4%), and 1343 m (52.5%) for absorbing, dust, and non-absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution type. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). The retrieved aerosol effective heights are lower by approximately 300 m (27 %) compared to those obtained from the ground-based LIDAR measurements.

Direct radiative effect by multicomponent aerosol over China

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

Huang, Xin; Song, Yu; Zhao, Chun

The direct radiative effect (DRE) of multiple aerosol species (sulfate, nitrate, ammonium, black carbon (BC), organic carbon (OC), and mineral aerosol) and their spatiotemporal variations over China were investigated using a fully coupled meteorology–chemistry model (WRF-Chem) for the entire year of 2006. We made modifications to improve model performance, including updating land surface parameters, improving the calculation of transition metal-catalyzed oxidation of SO 2, and adding in heterogeneous reactions between mineral aerosol and acid gases. The modified model well reproduced the magnitude, seasonal pattern, and spatial distribution of the measured meteorological conditions, concentrations of PM 10 and its components, andmore » aerosol optical depth (AOD). A diagnostic iteration method was used to estimate the overall DRE of aerosols and contributions from different components. At the land surface, all kinds of aerosol species reduced the incident net radiation flux with a total DRE of 10.2 W m -2 over China. Aerosols significantly warm the atmosphere with the national mean DRE of +10.8 W m -2. BC was the leading radiative-heating component (+8.7 W m -2), followed by mineral aerosol (+1.1 W m -2). At the top of the atmosphere (TOA), BC introduced the largest radiative perturbation (+4.5 W m -2), followed by sulfate (-1.4 W m -2). The overall perturbation of aerosols on radiation transfer is quite small over China, demonstrating the counterbalancing effect between scattering and adsorbing aerosols. Aerosol DRE at the TOA had distinct seasonality, generally with a summer maximum and winter minimum, mainly determined by mass loadings, hygroscopic growth, and incident radiation flux.« less

Aerosol Absorption by Black Carbon and Dust: Implications of Climate Change and Air Quality in Asia

NASA Technical Reports Server (NTRS)

Chin, Mian

2010-01-01

Atmospheric aerosol distributions from 2000 to 2007 are simulated with the global model GOCART to attribute light absorption by aerosol to its composition and sources. We show the seasonal and interannual variations of absorbing aerosols in the atmosphere over Asia, mainly black carbon and dust. and their linkage to the changes of anthropogenic and dust emissions in the region. We compare our results with observations from satellite and ground-based networks, and estimate the importance of black carbon and dust on regional climate forcing and air quality.

Aerosol optical properties and radiative effects: Assessment of urban aerosols in central China using 10-year observations

NASA Astrophysics Data System (ADS)

Zhang, Ming; Ma, Yingying; Gong, Wei; Liu, Boming; Shi, Yifan; Chen, ZhongYong

2018-06-01

Poor air quality episodes are common in central China. Here, based on 10 years of ground-based sun-photometric observations, aerosol optical and radiative forcing characteristics were analyzed in Wuhan, the biggest metropolis in central China. Aerosol optical depth (AOD) in the last decade declined significantly, while the Ångström exponent (AE) showed slight growth. Single scattering albedo (SSA) at 440 nm reached the lowest value (0.87) in winter and highest value (0.93) in summer. Aerosol parameters derived from sun-photometric observations were used as input in a radiative transfer model to calculate aerosol radiative forcing (ARF) on the surface in ultraviolet (UV), visible (VIS), near-infrared (NIR), and shortwave (SW) spectra. ARFSW sustained decreases (the absolute values) over the last 10 years. In terms of seasonal variability, due to the increases in multiple scattering effects and attenuation of the transmitted radiation as AOD increased, ARF in summer displayed the largest value (-73.94 W/m2). After eliminating the influence of aerosol loading, the maximum aerosol radiative forcing efficiency in SW range (ARFESW) achieved a value of -64.5 W/m2/AOD in April. The ARFE change in each sub-interval spectrum was related to the change in SSA and effective radius of fine mode particles (Refff), that is, ARFE increased with the decreases in SSA and Refff. The smallest contribution of ARFENIR to ARFESW was 34.11% under strong absorbing and fine particle conditions, and opposite results were found for the VIS range, whose values were always over 51.82%. Finally, due to the serious air pollution and frequency of haze day, aerosol characteristics in haze and clear days were analyzed. The percentage of ARFENIR increased from 35.71% on clear-air days to 37.63% during haze periods, while both the percentage of ARFEUV and ARFENIR in ARFESW kept decreasing. The results of this paper should help us to better understand the effect of aerosols on solar spectral radiation

Morphology and Optical Properties of Mixed Aerosol Particles

NASA Astrophysics Data System (ADS)

Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

2016-04-01

Experiments and modeling studies have shown that deliquesced aerosols can exist not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase (1,2). Recent laboratory studies conducted with model mixtures representing tropospheric aerosols (1,2,3), secondary organic aerosol (SOA) from smog chamber experiments (4), and field measurements (5) suggest that liquid-liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ inorganic particles. During LLPS, particles may adopt different morphologies mainly core-shell and partially engulfed. A core-shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles in particular for organic phases containing absorbing molecules, e.g. brown carbon. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. Our ternary model system consist of ammonium sulfate (AS)/ Polyethylene Glycol (PEG)/ and water (H2O). Carminic acid (CA) was added as a proxy for an absorbing organic compound to the system. The behavior of single droplets of above ternary mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same ternary mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. In addition, Mie-code modeling is used to predict the absorption efficiency of the same ternary system and the result will be compared with the data obtained from EDB experiment. We also intend to determine the occurrence of

Insight into global trends in aerosol composition from 2005 to 2015 inferred from the OMI Ultraviolet Aerosol Index

NASA Astrophysics Data System (ADS)

Hammer, Melanie S.; Martin, Randall V.; Li, Chi; Torres, Omar; Manning, Max; Boys, Brian L.

2018-06-01

Observations of aerosol scattering and absorption offer valuable information about aerosol composition. We apply a simulation of the Ultraviolet Aerosol Index (UVAI), a method of detecting aerosol absorption from satellite observations, to interpret UVAI values observed by the Ozone Monitoring Instrument (OMI) from 2005 to 2015 to understand global trends in aerosol composition. We conduct our simulation using the vector radiative transfer model VLIDORT with aerosol fields from the global chemical transport model GEOS-Chem. We examine the 2005-2015 trends in individual aerosol species from GEOS-Chem and apply these trends to the UVAI simulation to calculate the change in simulated UVAI due to the trends in individual aerosol species. We find that global trends in the UVAI are largely explained by trends in absorption by mineral dust, absorption by brown carbon, and scattering by secondary inorganic aerosol. Trends in absorption by mineral dust dominate the simulated UVAI trends over North Africa, the Middle East, East Asia, and Australia. The UVAI simulation resolves observed negative UVAI trends well over Australia, but underestimates positive UVAI trends over North Africa and Central Asia near the Aral Sea and underestimates negative UVAI trends over East Asia. We find evidence of an increasing dust source from the desiccating Aral Sea that may not be well represented by the current generation of models. Trends in absorption by brown carbon dominate the simulated UVAI trends over biomass burning regions. The UVAI simulation reproduces observed negative trends over central South America and West Africa, but underestimates observed UVAI trends over boreal forests. Trends in scattering by secondary inorganic aerosol dominate the simulated UVAI trends over the eastern United States and eastern India. The UVAI simulation slightly overestimates the observed positive UVAI trends over the eastern United States and underestimates the observed negative UVAI trends over

Aerosol optical properties and radiative impacts in the Pearl River Delta region of China during the dry season

NASA Astrophysics Data System (ADS)

Mai, Boru; Deng, Xuejiao; Li, Zhanqing; Liu, Jianjun; Xia, Xiang'ao; Che, Huizheng; Liu, Xia; Li, Fei; Zou, Yu; Cribb, Maureen

2018-02-01

Aerosol optical properties and direct radiative effects on surface irradiance were examined using seven years (2006-2012) of Cimel sunphotometer data collected at Panyu—the main atmospheric composition monitoring station in the Pearl River Delta (PRD) region of China. During the dry season (October to February), mean values of the aerosol optical depth (AOD) at 550 nm, the Ångström exponent, and the single scattering albedo at 440 nm (SSA) were 0.54, 1.33 and 0.87, respectively. About 90% of aerosols were dominated by fine-mode strongly absorbing particles. The size distribution was bimodal, with fine-mode particles dominating. The fine mode showed a peak at a radius of 0.12 μm in February and October (˜ 0.10 μm3μm-2). The mean diurnal shortwave direct radiative forcing at the surface, inside the atmosphere ( F ATM), and at the top of the atmosphere, was -33.4±7.0, 26.1±5.6 and -7.3±2.7Wm-2, respectively. The corresponding mean values of aerosol direct shortwave radiative forcing per AOD were -60.0 ± 7.8, 47.3 ± 8.3 and -12.8 ± 3.1 W m-2, respectively. Moreover, during the study period, F ATM showed a significant decreasing trend ( p < 0.01) and SSA increased from 0.87 in 2006 to 0.91 in 2012, suggesting a decreasing trend of absorbing particles being released into the atmosphere. Optical properties and radiative impacts of the absorbing particles can be used to improve the accuracy of inversion algorithms for satellite-based aerosol retrievals in the PRD region and to better constrain the climate effect of aerosols in climate models.

The role of iron-oxide aerosols and sunlight in the atmospheric reduction of Hg(II) species: A DFT+ U study

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

Tacey, Sean A.; Szilvasi, Tibor; Xu, Lang

Experimental and field measurements have shown that, in the presence of both iron-containing aerosols and sunlight, oxidized mercury species such as HgCl 2 and HgBr 2 undergo reduction to elemental mercury (Hg°), which remains in the atmosphere longer than oxidized mercury species due to its higher volatility. We performed density functional theory (DFT, PW91+U) calculations to elucidate the reduction mechanism for atmospheric HgCl 2 and HgBr 2 to Hg° on several iron-oxide aerosol surfaces relevant in the troposphere. On the OH-Fe-R-terminated α-Fe 2O 3(0001) surface, predicted to be most prevalent under ambient conditions, we show that: (1) the first Hg-Xmore » bond is broken via either thermal or photolytic activation depending on the ambient temperature; (2) photons with an energy of 2.69 eV (461 nm) are required to break the second Hg-X bond; and (3) a photo-induced surface-to-adsorbate charge-transfer process can promote Hg° desorption with an excitation energy of 2.59 eV (479 nm). All the calculated excitation energies are below the threshold value of 3.9 eV (320 nm) for photons in the troposphere, suggesting that sunlight can facilitate mercury reduction on iron-oxide aerosol surfaces. In contrast, the gas-phase reduction of HgCl 2 (HgBr 2) involves photoexcitation requiring an energy of 4.98 (4.45) eV (249 (279) nm); therefore, the energy range of sunlight is not suitable for gas-phase reduction. Our computational results provide the first evidence on the detailed mechanism for the combined role of aerosols and photons in the reduction of HgCl 2 and HgBr 2. In conclusion, our methodology can be adapted to study other photochemical heterogeneous processes in the atmosphere.« less

The role of iron-oxide aerosols and sunlight in the atmospheric reduction of Hg(II) species: A DFT+ U study

DOE PAGES

Tacey, Sean A.; Szilvasi, Tibor; Xu, Lang; ...

2018-04-22

Experimental and field measurements have shown that, in the presence of both iron-containing aerosols and sunlight, oxidized mercury species such as HgCl 2 and HgBr 2 undergo reduction to elemental mercury (Hg°), which remains in the atmosphere longer than oxidized mercury species due to its higher volatility. We performed density functional theory (DFT, PW91+U) calculations to elucidate the reduction mechanism for atmospheric HgCl 2 and HgBr 2 to Hg° on several iron-oxide aerosol surfaces relevant in the troposphere. On the OH-Fe-R-terminated α-Fe 2O 3(0001) surface, predicted to be most prevalent under ambient conditions, we show that: (1) the first Hg-Xmore » bond is broken via either thermal or photolytic activation depending on the ambient temperature; (2) photons with an energy of 2.69 eV (461 nm) are required to break the second Hg-X bond; and (3) a photo-induced surface-to-adsorbate charge-transfer process can promote Hg° desorption with an excitation energy of 2.59 eV (479 nm). All the calculated excitation energies are below the threshold value of 3.9 eV (320 nm) for photons in the troposphere, suggesting that sunlight can facilitate mercury reduction on iron-oxide aerosol surfaces. In contrast, the gas-phase reduction of HgCl 2 (HgBr 2) involves photoexcitation requiring an energy of 4.98 (4.45) eV (249 (279) nm); therefore, the energy range of sunlight is not suitable for gas-phase reduction. Our computational results provide the first evidence on the detailed mechanism for the combined role of aerosols and photons in the reduction of HgCl 2 and HgBr 2. In conclusion, our methodology can be adapted to study other photochemical heterogeneous processes in the atmosphere.« less

Spectrally-resolved measurements of aerosol extinction at ultraviolet and visible wavelengths

NASA Astrophysics Data System (ADS)

Flores, M.; Washenfelder, R. A.; Brock, C. A.; Brown, S. S.; Rudich, Y.

2012-12-01

Aerosols play an important role in the Earth's radiative budget. Aerosol extinction includes both the scattering and absorption of light, and these vary with wavelength, aerosol diameter, and aerosol composition. Historically, aerosol absorption has been measured using filter-based or extraction methods that are prone to artifacts. There have been few investigations of ambient aerosol optical properties at the blue end of the visible spectrum and into the ultraviolet. Brown carbon is particularly important in this spectral region, because it both absorbs and scatters light, and encompasses a large and variable group of organic compounds from biomass burning and secondary organic aerosol. We have developed a laboratory instrument that combines new, high-power LED light sources with high-finesse optical cavities to achieve sensitive measurements of aerosol optical extinction. This instrument contains two broadband channels, with spectral coverage from 360 - 390 nm and 385 - 420 nm. Using this instrument, we report aerosol extinction in the ultraviolet and near-visible spectral region as a function of chemical composition and structure. We have measured the extinction cross-sections between 360 - 420 nm with 0.5 nm resolution using different sizes and concentrations of polystyrene latex spheres, ammonium sulfate, and Suwannee River fulvic acid. Fitting the real and imaginary part of the refractive index allows the absorption and scattering to be determined.

Consistency between satellite-derived and modeled estimates of the direct aerosol effect.

PubMed

Myhre, Gunnar

2009-07-10

In the Intergovernmental Panel on Climate Change Fourth Assessment Report, the direct aerosol effect is reported to have a radiative forcing estimate of -0.5 Watt per square meter (W m(-2)), offsetting the warming from CO2 by almost one-third. The uncertainty, however, ranges from -0.9 to -0.1 W m(-2), which is largely due to differences between estimates from global aerosol models and observation-based estimates, with the latter tending to have stronger (more negative) radiative forcing. This study demonstrates consistency between a global aerosol model and adjustment to an observation-based method, producing a global and annual mean radiative forcing that is weaker than -0.5 W m(-2), with a best estimate of -0.3 W m(-2). The physical explanation for the earlier discrepancy is that the relative increase in anthropogenic black carbon (absorbing aerosols) is much larger than the overall increase in the anthropogenic abundance of aerosols.

Mycobacterial Aerosols and Respiratory Disease

PubMed Central

2003-01-01

Environmental opportunistic mycobacteria, including Mycobacterium avium, M. terrae, and the new species M. immunogenum, have been implicated in outbreaks of hypersensitivity pneumonitis or respiratory problems in a wide variety of settings. One common feature of the outbreaks has been exposure to aerosols. Aerosols have been generated from metalworking fluid during machining and grinding operations as well as from indoor swimming pools, hot tubs, and water-damaged buildings. Environmental opportunistic mycobacteria are present in drinking water, resistant to disinfection, able to provoke inflammatory reactions, and readily aerosolized. In all outbreaks, the water sources of the aerosols were disinfected. Disinfection may select for the predominance and growth of mycobacteria. Therefore, mycobacteria may be responsible, in part, for many outbreaks of hypersensitivity pneumonitis and other respiratory problems in the workplace and home. PMID:12890314

Mycobacterial aerosols and respiratory disease.

PubMed

Falkinham, Joseph O

2003-07-01

Environmental opportunistic mycobacteria, including Mycobacterium avium, M. terrae, and the new species M. immunogenum, have been implicated in outbreaks of hypersensitivity pneumonitis or respiratory problems in a wide variety of settings. One common feature of the outbreaks has been exposure to aerosols. Aerosols have been generated from metalworking fluid during machining and grinding operations as well as from indoor swimming pools, hot tubs, and water-damaged buildings. Environmental opportunistic mycobacteria are present in drinking water, resistant to disinfection, able to provoke inflammatory reactions, and readily aerosolized. In all outbreaks, the water sources of the aerosols were disinfected. Disinfection may select for the predominance and growth of mycobacteria. Therefore, mycobacteria may be responsible, in part, for many outbreaks of hypersensitivity pneumonitis and other respiratory problems in the workplace and home.

Investigating water soluble organic aerosols: Sources and evolution

NASA Astrophysics Data System (ADS)

Hecobian, Arsineh N.

ratios (NEMR-s) of some gaseous and aerosol compounds were compared. The NEMRs of most species had a high degree of variability that tended to obscure any significant differences between various smoke sources; however, some trends were observed. Smoke plumes associated with long-range transport from Asia and Siberia showed enhanced sulfate and HCN levels. The fire plumes that were influenced by urban emissions (e.g., intercepted over California) had higher levels of CO2, CH4, NOy and toluene. Overall, pronounced differences were observed when comparing the plumes subject to long-range transport to the ones that were intercepted closer to the fire sources (e.g., the plumes intercepted over California and the ones from Canadian Boreal forest fires). Additionally, when comparing the plumes near the fires, the ones that were influenced by urban emissions (some of the plumes encountered over California) displayed more distinct characteristics than the ones that were less or not influenced by urban emissions. Data from Teflon filters from the Southeastern United States were analyzed. The filter data show that the fraction of water-soluble light absorbing carbonaceous material is larger in biomass burning plumes regardless of the urban or rural location of the collection of the filter. Indeed, the slope of light absorption at 365 nm (Abs365) vs. WSOC was about 3.5 times higher in filters that were influenced by biomass burning plumes. Also, when the filters were separated into biomass burning and non-biomass burning categories, the slopes of Abs365 vs. WSOC for each category were uniform for all the sites where the filters were collected. Finally, a new method of simultaneous online measurement of water-soluble aerosol light absorption and WSOC has been presented. The results from an online study are in reasonable agreement with filter studies, although the measurements were collected during two different years and using two different techniques. The hourly averages of the

Aerosol and snow transfer processes: An investigation on the behavior of water-soluble organic compounds and ionic species.

PubMed

Barbaro, Elena; Zangrando, Roberta; Padoan, Sara; Karroca, Ornela; Toscano, Giuseppa; Cairns, Warren R L; Barbante, Carlo; Gambaro, Andrea

2017-09-01

The concentrations of water-soluble compounds (ions, carboxylic acids, amino acids, sugars, phenolic compounds) in aerosol and snow have been determined at the coastal Italian base "Mario Zucchelli" (Antarctica) during the 2014-2015 austral summer. The main aim of this research was to investigate the air-snow transfer processes of a number of classes of chemical compounds and investigate their potential as tracers for specific sources. The composition and particle size distribution of Antarctic aerosol was measured, and water-soluble compounds accounted for 66% of the PM 10 total mass concentration. The major ions Na + , Mg 2+ , Cl - and SO 4 2- made up 99% of the total water soluble compound concentration indicating that sea spray input was the main source of aerosol. These ionic species were found mainly in the coarse fraction of the aerosol resulting in enhanced deposition, as reflected by the snow composition. Biogenic sources were identified using chemical markers such as carboxylic acids, amino acids, sugars and phenolic compounds. This study describes the first characterization of amino acids and sugar concentrations in surface snow. High concentrations of amino acids were found after a snowfall event, their presence is probably due to the degradation of biological material scavenged during the snow event. Alcohol sugars increased in concentration after the snow event, suggesting a deposition of primary biological particles, such as airborne fungal spores. Copyright © 2017 Elsevier Ltd. All rights reserved.

Airborne Aerosol in Situ Measurements during TCAP: A Closure Study of Total Scattering

DOE PAGES

Kassianov, Evgueni I.; Berg, Larry K.; Pekour, Mikhail S.; ...

2015-07-31

We present here a framework for calculating the total scattering of both non-absorbing and absorbing aerosol at ambient conditions from aircraft data. The synergistically employed aircraft data involve aerosol microphysical, chemical, and optical components and ambient relative humidity measurements. Our framework is developed emphasizing the explicit use of the complementary chemical composition data for estimating the complex refractive index (RI) of particles, and thus obtaining improved ambient size spectra derived from Optical Particle Counter (OPC) measurements. The feasibility of our framework for improved calculations of total aerosol scattering is demonstrated for different ambient conditions with a wide range of relativemore » humidities (from 5 to 80%) using three types of data collected by the U.S. Department of Energy (DOE) G-1 aircraft during the recent Two-Column Aerosol Project (TCAP). Namely, these three types of data employed are: (1) size distributions measured by an Ultra High Sensitivity Aerosol Spectrometer (UHSAS; 0.06-1 µm), a Passive Cavity Aerosol Spectrometer (PCASP; 0.1-3 µm) and a Cloud and Aerosol Spectrometer (CAS; 0.6- >10 µm), (2) chemical composition data measured by an Aerosol Mass Spectrometer (AMS; 0.06-0.6 µm) and a Single Particle Soot Photometer (SP2; 0.06-0.6 µm), and (3) the dry total scattering coefficient measured by a TSI integrating nephelometer at three wavelengths (0.45, 0.55, 0.7 µm) and scattering enhancement factor measured with a humidification system at three RHs (near 45%, 65% and 90%) at a single wavelength (0.525 µm). We demonstrate that good agreement (~10% on average) between the observed and calculated scattering at these three wavelengths can be obtained using the best available chemical composition data for the RI-based correction of the OPC-derived size spectra. We also demonstrate that ignoring the RI-based correction and using non-representative RI values can cause a substantial

Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

NASA Astrophysics Data System (ADS)

Xu, Lingling; Chen, Jinsheng

2016-04-01

Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

Aerosol counterflow two-jets unit for continuous measurement of the soluble fraction of atmospheric aerosols.

PubMed

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

A new type of aerosol collector employing a liquid at laboratory temperature for continuous sampling of atmospheric particles is described. The collector operates on the principle of a Venturi scrubber. Sampled air flows at high linear velocity through two Venturi nozzles "atomizing" the liquid to form two jets of a polydisperse aerosol of fine droplets situated against each other. Counterflow jets of droplets collide, and within this process, the aerosol particles are captured into dispersed liquid. Under optimum conditions (air flow rate of 5 L/min and water flow rate of 2 mL/min), aerosol particles down to 0.3 microm in diameter are quantitatively collected in the collector into deionized water while the collection efficiency of smaller particles decreases. There is very little loss of fine aerosol within the aerosol counterflow two-jets unit (ACTJU). Coupling of the aerosol collector with an annular diffusion denuder located upstream of the collector ensures an artifact-free sampling of atmospheric aerosols. Operation of the ACTJU in combination with on-line detection devices allows in situ automated analysis of water-soluble aerosol species (e.g., NO2-, NO3-)with high time resolution (as high as 1 s). Under the optimum conditions, the limit of detection for particulate nitrite and nitrate is 28 and 77 ng/m(3), respectively. The instrument is sufficiently rugged for its application at routine monitoring of aerosol composition in the real time.

Multiangle Imaging Spectroradiometer (MISR) Global Aerosol Optical Depth Validation Based on 2 Years of Coincident Aerosol Robotic Network (AERONET) Observations

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.; Gaitley, Barbara J.; Martonchik, John V.; Diner, David J.; Crean, Kathleen A.; Holben, Brent

2005-01-01

Performance of the Multiangle Imaging Spectroradiometer (MISR) early postlaunch aerosol optical thickness (AOT) retrieval algorithm is assessed quantitatively over land and ocean by comparison with a 2-year measurement record of globally distributed AERONET Sun photometers. There are sufficient coincident observations to stratify the data set by season and expected aerosol type. In addition to reporting uncertainty envelopes, we identify trends and outliers, and investigate their likely causes, with the aim of refining algorithm performance. Overall, about 2/3 of the MISR-retrieved AOT values fall within [0.05 or 20% x AOT] of Aerosol Robotic Network (AERONET). More than a third are within [0.03 or 10% x AOT]. Correlation coefficients are highest for maritime stations (approx.0.9), and lowest for dusty sites (more than approx.0.7). Retrieved spectral slopes closely match Sun photometer values for Biomass burning and continental aerosol types. Detailed comparisons suggest that adding to the algorithm climatology more absorbing spherical particles, more realistic dust analogs, and a richer selection of multimodal aerosol mixtures would reduce the remaining discrepancies for MISR retrievals over land; in addition, refining instrument low-light-level calibration could reduce or eliminate a small but systematic offset in maritime AOT values. On the basis of cases for which current particle models are representative, a second-generation MISR aerosol retrieval algorithm incorporating these improvements could provide AOT accuracy unprecedented for a spaceborne technique.

Utilization of O4 slant column density to derive aerosol layer height from a space-borne UV-visible hyperspectral sensor: sensitivity and case study

NASA Astrophysics Data System (ADS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-02-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 1040 molecules2 cm-5, to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 m for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 % of retrieved aerosol effective heights are within the error range of 1 km compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Identification of light absorbing oligomers from glyoxal and methylglyoxal aqueous processing: a comparative study at the molecular level

NASA Astrophysics Data System (ADS)

Finessi, Emanuela; Hamilton, Jacqueline; Rickard, Andrew; Baeza-Romero, Maria; Healy, Robert; Peppe, Salvatore; Adams, Tom; Daniels, Mark; Ball, Stephen; Goodall, Iain; Monks, Paul; Borras, Esther; Munoz, Amalia

2014-05-01

Numerous studies point to the reactive uptake of gaseous low molecular weight carbonyls onto atmospheric waters (clouds/fog droplets and wet aerosols) as an important SOA formation route not yet included in current models. However, the evaluation of these processes is challenging because water provides a medium for a complex array of reactions to take place such as self-oligomerization, aldol condensation and Maillard-type browning reactions in the presence of ammonium salts. In addition to adding to SOA mass, aqueous chemistry products have been shown to include light absorbing, surface-active and high molecular weight oligomeric species, and can therefore affect climatically relevant aerosol properties such as light absorption and hygroscopicity. Glyoxal (GLY) and methylglyoxal (MGLY) are the gaseous carbonyls that have perhaps received the most attention to date owing to their ubiquity, abundance and reactivity in water, with the majority of studies focussing on bulk physical properties. However, very little is known at the molecular level, in particular for MGLY, and the relative potential of these species as aqueous SOA precursors in ambient air is still unclear. We have conducted experiments with both laboratory solutions and chamber-generated particles to simulate the aqueous processing of GLY and MGLY with ammonium sulphate (AS) under typical atmospheric conditions and investigated their respective aging products. Both high performance liquid chromatography coupled with UV-Vis detection and ion trap mass spectrometry (HPLC-DAD-MSn) and high resolution mass spectrometry (FTICRMS) have been used for molecular identification purposes. Comprehensive gas chromatography with nitrogen chemiluminescence detection (GCxGC-NCD) has been applied for the first time to these systems, revealing a surprisingly high number of nitrogen-containing organics (ONs), with a large extent of polarities. GCxGC-NCD proved to be a valuable tool to determine overall amount and rates of

Simulating the effect of photochemical aging on the oxidation state and hygroscopicity of organic aerosol

NASA Astrophysics Data System (ADS)

Tsimpidi, A.; Karydis, V.; Pandis, S. N.; Lelieveld, J.

2016-12-01

Hygroscopicity is an important property of aerosols which describes their propensity to absorb water vapor. The hygroscopicity of organic aerosol (OA) can change during its atmospheric aging affecting the total aerosol hygroscopicity. A more hygroscopic particle will grow more rapidly under humid conditions, scatter incident sunlight more efficiently; and it will more likely form cloud droplets. Both phenomena strongly influence the radiative forcing of climate through the direct and indirect effects of aerosols. Therefore, taking into account the hygrscopicity changes of OA during its atmospheric aging is of prime importance to accurately estimate the aerosol climatic impact. Here, we use a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) (Tsimpidi et al., 2014) in the frame of the global chemistry climate model EMAC to simulate the global distribution of the OA oxidation state and hygroscopicity. To track the evolution of the OA oxidation state during its atmospheric aging, ORACLE is modified to include the description of the OA oxygen content change when mass from any OA surrogate species reacts with the OH radical. Subsequently, it is assumed that the cloud condensation nuclei (CCN) activity of OA, expressed in the form of the hygroscopicity parameter κ, will increase with increasing oxygen content (expressed by the oxygen per carbon ratio, O:C) and will range from κ = 0 (for O:C ≤ 0.2) to κ = 0.35 (for O:C = 1). The exact relationship between O:C and κ is determined based on aerosol mass spectrometer (AMS) and continuous flow CCN (CCNC) measurements of SOA (Lambe et al., 2011). Following a straightforward mixing rule, the hygroscopicity and oxygen content of total OA is calculated based on the hygroscopicities of the individual OA compounds and their degree of oxidation. A global dataset of O:C measurements is used to validate the model results. ReferencesLambe, A. T., et al. : Laboratory

Aerosol-Cloud-Precipitation Interactions over Indo-Gangetic Basin

NASA Technical Reports Server (NTRS)

Tsay, S.-C.; Lau, K. .; Holben, B. N.; Hsu, N. C.; Bhartia, P. K.

2005-01-01

About 60% of world population reside in Asia, in term of which sheer population density presents a major environmental stress. Economic expansion in this region is, in fact, accompanied by increases in bio-fuel burning, industrial pollution, and land cover and land use changes. With a growth rate of approx. 8%/yr for Indian economy, more than 600 million people from Lahore, Pakistan to Calcutta, India over the Indo-Gangetic Basin have particularly witnessed increased frequencies of floods and droughts as well as a dramatic increase in atmospheric loading of aerosols (i.e., anthropogenic and natural aerosol) in recent decades. This regional change (e.g., aerosol, cloud, precipitation, etc.) will constitute a vital part of the global change in the 21st century. Better understanding of the impacts of aerosols in affecting monsoon climate and water cycles is crucial in providing the physical basis to improve monsoon climate prediction and for disaster mitigation. Based on climate model simulations, absorbing aerosols (dust and black carbon) play a critical role in affecting interannual and intraseasonal variability of the Indian monsoon. An initiative on the integrated (aerosols, clouds, and precipitation) measurements approach over the Indo-Gangetic Basin will be discussed. An array of ground-based (e.g., AERONET, MPLNET, SMART-COMMIT, etc.) and satellite (e.g., Terra, A-Train, etc.) sensors will be utilized to acquire aerosol characteristics, sources/sinks, and transport processes during the pre-monsoon (April-May, aerosol forcing) season, and to obtain cloud and precipitation properties during the monsoon (May-June, water cycle response) season. Close collaboration with other international programs, such as ABC, CLIVAR, GEWEX, and CEOP in the region is anticipated.

Ground-based Network and Supersite Measurements for Studying Aerosol Properties and Aerosol-Cloud Interactions

NASA Technical Reports Server (NTRS)

Tsay, Si-Chee; Holben, Brent N.

2008-01-01

capability of AERONET SMART-COMMIT in current Asian Monsoon Year-2008 campaigns that are designed and being executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., airborne dust, smoke, mega-city pollutant). Feedback mechanisms between aerosol radiative effects and monsoon dynamics have been recently proposed, however there is a lack of consensus on whether aerosol forcing would be more likely to enhance or reduce the strength of the monsoon circulation. We envision robust approaches which well-collocated ground-based measurements and space-borne observations will greatly advance our understanding of absorbing aerosols (e.g., "Global Dimming" vs. "Elevated Heat-Pump" effects) on aerosol cloud water cycle interactions.

Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions

EPA Science Inventory

Organic aerosols (OA) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OA are not or poorly represented in current climate m...

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

NASA Technical Reports Server (NTRS)

Thomason, L. W.

2012-01-01

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Elucidating the Chemical Complexity of Organic Aerosol Constituents Measured During the Southeastern Oxidant and Aerosol Study (SOAS)

NASA Astrophysics Data System (ADS)

Yee, L.; Isaacman, G. A.; Spielman, S. R.; Worton, D. R.; Zhang, H.; Kreisberg, N. M.; Wilson, K. R.; Hering, S. V.; Goldstein, A. H.

2013-12-01

Thousands of volatile organic compounds are uniquely created in the atmosphere, many of which undergo chemical transformations that result in more highly-oxidized and often lower vapor pressure species. These species can contribute to secondary organic aerosol, a complex mixture of organic compounds that is still not chemically well-resolved. Organic aerosol collected on filters taken during the Southeastern Oxidant and Aerosol Study (SOAS) constitute hundreds of unique chemical compounds. Some of these include known anthropogenic and biogenic tracers characterized using standardized analytical techniques (e.g. GC-MS, UPLC, LC-MS), but the majority of the chemical diversity has yet to be explored. By employing analytical techniques involving sample derivatization and comprehensive two-dimensional gas chromatography (GC x GC) with high-resolution-time-of-flight mass spectrometry (HR-ToF-MS), we elucidate the chemical complexity of the organic aerosol matrix along the volatility and polarity grids. Further, by utilizing both electron impact (EI) and novel soft vacuum ultraviolet (VUV) ionization mass spectrometry, a greater fraction of the organic mass is fully speciated. The GC x GC-HR-ToF-MS with EI/VUV technique efficiently provides an unprecedented level of speciation for complex ambient samples. We present an extensive chemical characterization and quantification of organic species that goes beyond typical atmospheric tracers in the SOAS samples. We further demonstrate that complex organic mixtures can be chemically deconvoluted by elucidation of chemical formulae, volatility, functionality, and polarity. These parameters provide insight into the sources (anthropogenic vs. biogenic), chemical processes (oxidation pathways), and environmental factors (temperature, humidity), controlling organic aerosol growth in the Southeastern United States.

Impact of springtime biomass-burning aerosols on radiative forcing over northern Thailand during the 7SEAS campaign

NASA Astrophysics Data System (ADS)

Pani, Shantanu Kumar; Wang, Sheng-Hsiang; Lin, Neng-Huei; Lee, Chung-Te; Tsay, Si-Chee; Holben, Brent; Janjai, Serm; Hsiao, Ta-Chih; Chuang, Ming-Tung; Chantara, Somporn

2016-04-01

Biomass-burning (BB) aerosols are the significant contributor to the regional/global aerosol loading and radiation budgets. BB aerosols affect the radiation budget of the earth and atmosphere by scattering and absorbing directly the incoming solar and outgoing terrestrial radiation. These aerosols can exert either cooling or warming effect on climate, depending on the balance between scattering and absorption. BB activities in the form of wildland forest fires and agricultural crop burning are very pronounced in the Indochina peninsular regions in Southeast Asia mainly in spring (late February to April) season. The region of interest includes Doi Ang Khang (19.93° N, 99.05° E, 1536 msl) in northern Thailand, as part of the Seven South East Asian Studies (7-SEAS)/BASELInE (Biomass-burning Aerosols & Stratocumulus Environment: Lifecycles & Interactions Experiment) campaign in 2013. In this study, for the first time, the direct aerosol radiative effects of BB aerosols over near-source BB emissions, during the peak loading spring season, in northern Indochina were investigated by using ground-based physical, chemical, and optical properties of aerosols as well as the aerosol optical and radiative transfer models. Information on aerosol parameters in the field campaign was used in the OPAC (Optical Properties of Aerosols and Clouds) model to estimate various optical properties corresponding to aerosol compositions. Clear-sky shortwave direct aerosol radiative effects were further estimated with a raditive transfer model SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer). The columnar aerosol optical depth (AOD500) was found to be ranged from 0.26 to 1.13 (with the mean value 0.71 ± 0.24). Fine-mode (fine mode fraction ≈0.98, angstrom exponent ≈1.8) and significantly absorbing aerosols (columnar single-scattering albedo ≈0.89, asymmetry-parameter ≈0.67 at 441 nm wavelength) dominated in this region. Water soluble and black carbon (BC) aerosols mainly

Use of A-Train Aerosol Observations to Constrain Direct Aerosol Radiative Effects (DARE) Comparisons with Aerocom Models and Uncertainty Assessments

NASA Technical Reports Server (NTRS)

Redemann, J.; Shinozuka, Y.; Kacenelenbogen, M.; Segal-Rozenhaimer, M.; LeBlanc, S.; Vaughan, M.; Stier, P.; Schutgens, N.

2017-01-01

We describe a technique for combining multiple A-Train aerosol data sets, namely MODIS spectral AOD (aerosol optical depth), OMI AAOD (absorption aerosol optical depth) and CALIOP aerosol backscatter retrievals (hereafter referred to as MOC retrievals) to estimate full spectral sets of aerosol radiative properties, and ultimately to calculate the 3-D distribution of direct aerosol radiative effects (DARE). We present MOC results using almost two years of data collected in 2007 and 2008, and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. Use of the MODIS Collection 6 AOD data derived with the dark target and deep blue algorithms has extended the coverage of the MOC retrievals towards higher latitudes. The MOC aerosol retrievals agree better with AERONET in terms of the single scattering albedo (ssa) at 441 nm than ssa calculated from OMI and MODIS data alone, indicating that CALIOP aerosol backscatter data contains information on aerosol absorption. We compare the spatio-temporal distribution of the MOC retrievals and MOC-based calculations of seasonal clear-sky DARE to values derived from four models that participated in the Phase II AeroCom model intercomparison initiative. Overall, the MOC-based calculations of clear-sky DARE at TOA over land are smaller (less negative) than previous model or observational estimates due to the inclusion of more absorbing aerosol retrievals over brighter surfaces, not previously available for observationally-based estimates of DARE. MOC-based DARE estimates at the surface over land and total (land and ocean) DARE estimates at TOA are in between previous model and observational results. Comparisons of seasonal aerosol property to AeroCom Phase II results show generally good agreement best agreement with forcing results at TOA is found with GMI-MerraV3. We discuss sampling issues that affect the comparisons and the major challenges in extending our clear-sky DARE results to all

Aerosol loading impact on Asian monsoon precipitation patterns

NASA Astrophysics Data System (ADS)

Biondi, Riccardo; Cagnazzo, Chiara; Costabile, Francesca; Cairo, Francesco

2017-04-01

Solar light absorption by aerosols such as black carbon and dust assume a key role in driving the precipitation patterns in the Indian subcontinent. The aerosols stack up against the foothills of the Himalayas in the pre-monsoon season and several studies have already demonstrated that this can cause precipitation anomalies during summer. Despite its great significance in climate change studies, the link between absorbing aerosols loading and precipitation patterns remains highly uncertain. The main challenge for this kind of studies is to find consistent and reliable datasets. Several aerosol time series are available from satellite and ground based instruments and some precipitation datasets from satellite sensors, but they all have different time/spatial resolution and they use different assumptions for estimating the parameter of interest. We have used the aerosol estimations from the Ozone Monitoring Instrument (OMI), the Along-Track Scanning Radiometer (AATSR) and the MODerate resolution Imaging Spectroradiometer (MODIS) and validated them against the Aerosol Robotic Network (AERONET) measurements in the Indian area. The precipitation has been analyzed by using the Tropical Rainfall Measuring Mission (TRMM) estimations and the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2). From our results it is evident the discrepancy between the aerosol loading on the area of interest from the OMI, AATSR, and MODIS, but even between 3 different algorithms applied to the MODIS data. This uncertainty does not allow to clearly distinguishing high aerosol loading years from low aerosol loading years except in a couple of cases where all the estimations agree. Similar issues are also present in the precipitation estimations from TRMM and MERRA-2. However, all the aerosol datasets agree in defining couples of consecutive years with a large gradient of aerosol loading. Based on this assumption we have compared the precipitation anomalies and

Aerosol as a player in the Arctic Amplification - an aerosol-climate model evaluation study

NASA Astrophysics Data System (ADS)

Schacht, Jacob; Heinold, Bernd; Tegen, Ina

2017-04-01

Climate warming is much more pronounced in the Arctic than in any other region on Earth - a phenomenon referred to as the "Arctic Amplification". This is closely related to a variety of specific feedback mechanisms, which relative importance, however, is not yet sufficiently understood. The local changes in the Arctic climate are far-reaching and affect for example the general atmospheric circulation and global energy transport. Aerosol particles from long-range transport and local sources play an important role in the Arctic system by modulating the energy balance (directly by interaction with solar and thermal infrared radiation and indirectly by changing cloud properties and atmospheric dynamics). The main source regions of anthropogenic aerosol are Europe and East Asia, but also local shipping and oil/gas extraction may contribute significantly. In addition, important sources are widespread, mainly natural boreal forest fires. Most of the European aerosol is transported through the lower atmospheric layers in wintertime. The Asian aerosol is transported through higher altitudes. Because of the usually pristine conditions in the Arctic even small absolute changes in aerosol concentration can have large impacts on the Arctic climate. Using global and Arctic-focused model simulations, we aim at investigating the sources and transport pathways of natural and anthropogenic aerosol to the Arctic region, as well as their impact on radiation and clouds. Here, we present first results from an aerosol-climate model evaluation study. Simulations were performed with the global aerosol-climate model ECHAM6-HAM2, using three different state-of-the-art emission inventories (ACCMIP, ACCMIP + GFAS emissions for wildfires and ECLIPSE). The runs were performed in nudged mode at T63 horizontal resolution (approximately 1.8°) with 47 vertical levels for the 10-year period 2006-2015. Black carbon (BC) and sulphate (SO4) are of particular interest. BC is highly absorbing in the

Optical properties of aerosol contaminated cloud derived from MODIS instrument

NASA Astrophysics Data System (ADS)

Mei, Linlu; Rozanov, Vladimir; Lelli, Luca; Vountas, Marco; Burrows, John P.

2016-04-01

The presence of absorbing aerosols above/within cloud can reduce the amount of up-welling radiation in visible (VIS) and short-wave infrared and darken the spectral reflectance when compared with a spectrum of a clean cloud observed by satellite instruments (Jethva et al., 2013). Cloud properties retrieval for aerosol contaminated cases is a great challenge. Even small additional injection of aerosol particles into clouds in the cleanest regions of Earth's atmosphere will cause significant effect on those clouds and on climate forcing (Koren et al., 2014; Rosenfeld et al., 2014) because the micro-physical cloud process are non-linear with respect to the aerosol loading. The current cloud products like Moderate Resolution Imaging Spectroradiometer (MODIS) ignoring the aerosol effect for the retrieval, which may cause significant error in the satellite-derived cloud properties. In this paper, a new cloud properties retrieval method, considering aerosol effect, based on the weighting-function (WF) method, is presented. The retrieval results shows that the WF retrieved cloud properties (e.g COT) agrees quite well with MODIS COT product for relative clear atmosphere (AOT ≤ 0.4) while there is a large difference for large aerosol loading. The MODIS COT product is underestimated for at least 2 - 3 times for AOT>0.4, and this underestimation increases with the increase of AOT.

On the implications of aerosol liquid water and phase ...

EPA Pesticide Factsheets

Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were hig

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Spaceborne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

NASA Technical Reports Server (NTRS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-01-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the Differential Optical Absorption Spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(exp 40) sq molecules cm(exp -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nm, the O4 absorption band at 477 nm is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nm is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 m for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80% of retrieved aerosol effective heights are within the error range of 1 km compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

MISR Global Aerosol Product Assessment by Comparison with AERONET

NASA Technical Reports Server (NTRS)

Kahn, Ralph A.; Gaitley, Barbara J.; Garay, Michael J.; Diner, David J.; Eck, Thomas F.; Smirnov, Alexander; Holben, Brent N.

2010-01-01

A statistical approach is used to assess the quality of the MISR Version 22 (V22) aerosol products. Aerosol Optical Depth (AOD) retrieval results are improved relative to the early post- launch values reported by Kahn et al. [2005a], varying with particle type category. Overall, about 70% to 75% of MISR AOD retrievals fall within 0.05 or 20% AOD of the paired validation data, and about 50% to 55% are within 0.03 or 10% AOD, except at sites where dust, or mixed dust and smoke, are commonly found. Retrieved particle microphysical properties amount to categorical values, such as three groupings in size: "small," "medium," and "large." For particle size, ground-based AERONET sun photometer Angstrom Exponents are used to assess statistically the corresponding MISR values, which are interpreted in terms of retrieved size categories. Coincident Single-Scattering Albedo (SSA) and fraction AOD spherical data are too limited for statistical validation. V22 distinguishes two or three size bins, depending on aerosol type, and about two bins in SSA (absorbing vs. non-absorbing), as well as spherical vs. non-spherical particles, under good retrieval conditions. Particle type sensitivity varies considerably with conditions, and is diminished for mid-visible AOD below about 0.15 or 0.2. Based on these results, specific algorithm upgrades are proposed, and are being investigated by the MISR team for possible implementation in future versions of the product.

Aerosol Enhancements in the Upper Troposphere Over The Amazon Forest: Do Amazonian Clouds Produce Aerosols?

NASA Astrophysics Data System (ADS)

Andreae, M. O.; Afchine, A.; Albrecht, R. I.; Artaxo, P.; Borrmann, S.; Cecchini, M. A.; Costa, A.; Dollner, M.; Fütterer, D.; Järvinen, E.; Klimach, T.; Konemann, T.; Kraemer, M.; Krüger, M. L.; Machado, L.; Mertes, S.; Pöhlker, C.; Poeschl, U.; Sauer, D. N.; Schnaiter, M.; Schneider, J.; Schulz, C.; Spanu, A.; Walser, A.; Weinzierl, B.; Wendisch, M.

2015-12-01

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 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. The aircraft was equipped with about 30 remote sensing and in-situ instruments for meteorological, trace gas, aerosol, cloud, precipitation, and solar radiation measurements. Fourteen research flights were conducted during this campaign. Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with concentrations after normalization to standard conditions often exceeding those in the boundary layer (BL). This behavior was consistent between 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 found to be depleted in aerosol particles, whereas enhanced aerosol number and mass concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. This suggests that aerosol production takes place in the UT based on volatile and condensable material brought up by deep convection. 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

Photochemical Formation of Sulfur-Containing Aerosols

NASA Astrophysics Data System (ADS)

Kroll, Jay A.; Vaida, Veronica

2017-06-01

In order to understand planetary climate systems, modeling the properties of atmospheric aerosols is vital. Aerosol formation plays an important role in planetary climates and is tied to feedback loops that can either warm or cool a planet. Sulfur compounds are known to play an important role in new particle aerosol formation and have been observed in a number of planetary atmospheres throughout our solar system. Our current understanding of sulfur chemistry explains much of what we observe in Earth's atmosphere; however, several discrepancies arise when comparing observations of the Venusian atmosphere with model predictions. This suggests that there are still problems in our fundamental understanding of sulfur chemistry. This is concerning given recent renewed interest in sulfate injections in the stratosphere for solar radiation management geo-engineering schemes. We investigate the role of sunlight as a potential driver of the formation of sulfur-containing aerosols. I will present recent work investigating the generation of large quantities of aerosol from the irradiation of mixtures of SO_2 with water and organic species, using a solar simulator that mimics the light that is available in the Earth's troposphere and the Venusian middle atmosphere. I will present on recent work done in our lab suggesting the formation of sulfurous acid, H_2SO_3, and describe experimental work that supports this proposed mechanism. Additionally I will present on new work showing the highly reactive nature of electronically excited SO_2 with saturated alkane species. The implications of this photochemically induced sulfur aerosol formation in the atmosphere of Earth and other planetary atmospheres will be discussed.

ACTRIS Aerosol, Clouds and Trace Gases Research Infrastructure

NASA Astrophysics Data System (ADS)

Pappalardo, Gelsomina

2018-04-01

The Aerosols, Clouds and Trace gases Research Infrastructure (ACTRIS) is a distributed infrastructure dedicated to high-quality observation of aerosols, clouds, trace gases and exploration of their interactions. It will deliver precision data, services and procedures regarding the 4D variability of clouds, short-lived atmospheric species and the physical, optical and chemical properties of aerosols to improve the current capacity to analyse, understand and predict past, current and future evolution of the atmospheric environment.

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.

Characterization of particulate products for aging of ethylbenzene secondary organic aerosol in the presence of ammonium sulfate seed aerosol.

PubMed

Huang, Mingqiang; Zhang, Jiahui; Cai, Shunyou; Liao, Yingmin; Zhao, Weixiong; Hu, Changjin; Gu, Xuejun; Fang, Li; Zhang, Weijun

2016-09-01

Aging of secondary organic aerosol (SOA) particles formed from OH- initiated oxidation of ethylbenzene in the presence of high mass (100-300μg/m(3)) concentrations of (NH4)2SO4 seed aerosol was investigated in a home-made smog chamber in this study. The chemical composition of aged ethylbenzene SOA particles was measured using an aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with a Fuzzy C-Means (FCM) clustering algorithm. Experimental results showed that nitrophenol, ethyl-nitrophenol, 2,4-dinitrophenol, methyl glyoxylic acid, 5-ethyl-6-oxo-2,4-hexadienoic acid, 2-ethyl-2,4-hexadiendioic acid, 2,3-dihydroxy-5-ethyl-6-oxo-4-hexenoic acid, 1H-imidazole, hydrated N-glyoxal substituted 1H-imidazole, hydrated glyoxal dimer substituted imidazole, 1H-imidazole-2-carbaldehyde, N-glyoxal substituted hydrated 1H-imidazole-2-carbaldehyde and high-molecular-weight (HMW) components were the predominant products in the aged particles. Compared to the previous aromatic SOA aging studies, imidazole compounds, which can absorb solar radiation effectively, were newly detected in aged ethylbenzene SOA in the presence of high concentrations of (NH4)2SO4 seed aerosol. These findings provide new information for discussing aromatic SOA aging mechanisms. Copyright © 2016. Published by Elsevier B.V.

Quantifying Wildfire Emissions and associated Aerosol Species using Assimilation of Satellite Carbon Monoxide Retrievals

NASA Astrophysics Data System (ADS)

Edwards, David; Barre, Jerome; Worden, Helen; Gaubert, Benjamin

2017-04-01

Intense and costly wildfires tend are predicted to increase in frequency under a warming climate. For example, the recent August 2015 Washington State fires were the largest in the state's history. Also in September and October 2015 very intense fires over Indonesia produced some of the highest concentrations of carbon monoxide (CO) ever seen from satellite. Such larges fires impact not only the local environment but also affect air quality far downwind through the long-range transport of pollutants. Global to continental scale coverage showing the evolution of CO resulting from fire emission is available from satellite observations. Carbon monoxide is the only atmospheric trace gas for which satellite multispectral retrievals have demonstrated reliable independent profile information close to the surface and also higher in the free troposphere. The unique CO profile product from Terra/MOPITT clearly distinguishes near-surface CO from the free troposphere CO. Also previous studies have suggested strong correlations between primary emissions of fire organic and black carbon aerosols and CO. We will present results from the Ensemble Adjustement Kalman Filter (DART) system that has been developed to assimilate MOPITT CO in the global-scale chemistry-climate model CAM-Chem. The ensemble technique allows inference on various fire model state variables such as CO emissions, and also aerosol species resulting from fires such as organic and black carbon. The benefit of MOPITT CO profile assimilation for estimating the CO emissions from the Washington and Indonesian fire cases will be discussed, along with the ability of the ensemble approach to infer information on the black and organic carbon aerosol distribution. This study builds on capability to quantitatively integrate satellite observations and models developed in recent years through projects funded by the NASA ACMAP Program.

Optical, microphysical and radiative properties of aerosols over a tropical rural site in Kenya, East Africa: Source identification, modification and aerosol type discrimination

NASA Astrophysics Data System (ADS)

Boiyo, Richard; Kumar, K. Raghavendra; Zhao, Tianliang

2018-03-01

A better understanding of aerosol optical, microphysical and radiative properties is a crucial challenge for climate change studies. In the present study, column-integrated aerosol optical and radiative properties observed at a rural site, Mbita (0.42°S, 34.20 °E, and 1125 m above sea level) located in Kenya, East Africa (EA) are investigated using ground-based Aerosol Robotic Network (AERONET) data retrieved during January, 2007 to December, 2015. The annual mean aerosol optical depth (AOD500 nm), Ångström exponent (AE440-870 nm), fine mode fraction of AOD500 nm (FMF500 nm), and columnar water vapor (CWV, cm) were found to be 0.23 ± 0.08, 1.01 ± 0.16, 0.60 ± 0.07, and 2.72 ± 0.20, respectively. The aerosol optical properties exhibited a unimodal distribution with substantial seasonal heterogeneity in their peak values being low (high) during the local wet (dry) seasons. The observed data showed that Mbita and its environs are significantly influenced by various types of aerosols, with biomass burning and/or urban-industrial (BUI), mixed (MXD), and desert dust (DDT) aerosol types contributing to 37.72%, 32.81%, and 1.40%, respectively during the local dry season (JJA). The aerosol volume size distribution (VSD) exhibited bimodal lognormal structure with a geometric mean radius of 0.15 μm and 3.86-5.06 μm for fine- and coarse-mode aerosols, respectively. Further, analysis of single scattering albedo (SSA), asymmetry parameter (ASY) and refractive index (RI) revealed dominance of fine-mode absorbing aerosols during JJA. The averaged aerosol direct radiative forcing (ARF) retrieved from the AERONET showed a strong cooling effect at the bottom of the atmosphere (BOA) and significant warming within the atmosphere (ATM), representing the important role of aerosols played in this rural site of Kenya. Finally, the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model revealed that aerosols from distinct sources resulted in enhanced loading

A Study of Aerosol Direct Radiative Effect and Its Impacts on Global Terrestrial Ecosystem Cycles

NASA Astrophysics Data System (ADS)

Zhang, J.; Shao, S.; Zhou, L.

2017-12-01

Aerosols can absorb and scatter solar radiation, thus cause the total solar radiation reaching the surface to drop and the fraction of diffuse radiation to increase, which influence the surface radiation budget. The global surface radiation with and without consideration of aerosols are calculated by the Fu-Liou atmospheric radiative transfer model based on the MODIS aerosol products, CERES cloud products and other remote sensing data. The aerosol direct radiative effect is calculated based on the two scenarios of aerosols. Our calculation showed that in 2007, aerosols decreased the global total radiation by 9.16 W m-2 on average. Large decrease generally occurred in places with high AOD. As for the diffuse radiation, aerosol-induced changes were either positive or negative. Large increase generally occurred in places with high surface albedo, while large decrease generally occurred in places with high cloud fraction. The global aerosol-induced diffuse radiation change averaged 8.17 W m-2 in 2007. The aerosol direct radiative effect causes the photosynthetic active radiation to increase, and its influences on the global carbon cycle of terrestrial ecosystem are studied by using the Community Land Model (CLM). Calculations show that the aerosol direct radiative effects caused the global averages of terrestrial gross primary productivity (GPP), net primary productivity (NPP), heterotrophic respiration (RH), autotrophic respiration (RA), and net ecosystem productivity (Reco) to increase in 2007, with significant spatial variations however. The global average changes of GPP, NPP, NEP, RA, RH and Reco in 2007 were +6.47 gC m-2, +2.23 gC m-2, +0.34 gC m-2, +4.24 gC m-2, +1.89 gC m-2, +6.13 gC m-2, respectively. Examinations of the carbon fluxes show that the aerosol direct radiative effects influence the terrestrial ecosystem carbon cycles via the following two approaches: First, the diffuse fertilization effect, i.e. more diffuse radiation absorbed by vegetation shade

Aerosol-Monsoon Interaction, maintenance and variability of the Asian Tropopause Aerosol Layer (ATAL)

NASA Astrophysics Data System (ADS)

Yuan, C.; Lau, W. K. M.; Li, Z.

2016-12-01

In recent years, the discovery of the Asian Tropopause Aerosol Layer (ATAL) from NASA satellite observations has sparked much interests in research on its composition, origin and relationships to the transport processes of atmospheric constituents in the upper troposphere and lower stratosphere (UTLS) and the variability of the Asian Monsoon Anticyclone (AMA). In this paper, based on analysis of MERRA2 reanalysis data, we present results showing that: 1) water vapor, aerosols and chemical gases (BC, OC, dust and CO) originated for the earth surface contribute significantly to the composition of the ATAL during the Asian summer monsoon, 2) one of the major pathways is via the strong large-scale vertical motion, and convective ascent over the Northern Himalayan Foothills during the peak phase of the Indian monsoon, 3) once transported into the UTLS , atmospheric constituents are capped by the Tropopuase inversion Layer (TIL) and advected around within and in the vicinity of the AMA forming the ATAL, 4) the ATAL is modulated by UTLS transport processes which undergo intrinsic monsoon intraseasonal oscillations with 20-30 day quasi-periodicity, coupled to lower tropospheric monsoon dynamics and diabatic heating processes, 5) the pre-monsoon accumulation of absorbing aerosols (BC, OC and dust) over the Indo-Gangetic Plain is more than likely to play an important role in enhancing the UTLS transport of atmospheric constituents from the earth surface to the ATAL.

Aromatic Structure in Simulates Titan Aerosol

NASA Technical Reports Server (NTRS)

Trainer, Melissa G.; Loeffler, M. J.; Anderson, C. M.; Hudson, R. L.; Samuelson, R. E.; Moore, M. A.

2011-01-01

Observations of Titan by the Cassini Composite Infrared Spectrometer (CIRS) between 560 and 20 per centimeter (approximately 18 to 500 micrometers) have been used to infer the vertical variations of Titan's ice abundances, as well as those of the aerosol from the surface to an altitude of 300 km [1]. The aerosol has a broad emission feature centered approximately at 140 per centimeter (71 micrometers). As seen in Figure 1, this feature cannot be reproduced using currently available optical constants from laboratory-generated Titan aerosol analogs [2]. The far-IR is uniquely qualified for investigating low-energy vibrational motions within the lattice structures of COITIDlex aerosol. The feature observed by CIRS is broad, and does not likely arise from individual molecules, but rather is representative of the skeletal movements of macromolecules. Since Cassini's arrival at Titan, benzene (C6H6) has been detected in the atmosphere at ppm levels as well as ions that may be polycyclic aromatic hydrocarbons (PAHs) [3]. We speculate that the feature may be a blended composite that can be identified with low-energy vibrations of two-dimensional lattice structures of large molecules, such as PAHs or nitrogenated aromatics. Such structures do not dominate the composition of analog materials generated from CH4 and N2 irradiation. We are performing studies forming aerosol analog via UV irradiation of aromatic precursors - specifically C6H6 - to understand how the unique chemical architecture of the products will influence the observable aerosol characteristics. The optical and chemical properties of the aromatic analog will be compared to those formed from CH4/N2 mixtures, with a focus on the as-yet unidentified far-IR absorbance feature. Preliminary results indicate that the photochemically-formed aromatic aerosol has distinct chemical composition, and may incorporate nitrogen either into the ring structure or adjoined chemical groups. These compositional differences are

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Space-Borne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

NASA Technical Reports Server (NTRS)

Park, Sang Seo; Kim, Jhoon; Lee, Hanlim; Torres, Omar; Lee, Kwang-Mog; Lee, Sang Deok

2016-01-01

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(sup 40) molecules (sup 2) per centimeters(sup -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nanometers, the O4 absorption band at 477 nanometers is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nanometers is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 meters for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 percent of retrieved aerosol effective heights are within the error range of 1 kilometer compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.