Global Distribution of Dust, Smoke, Volcanic Ash, and Pollutant Aerosols Seen from Space

NASA Technical Reports Server (NTRS)

Herman, Jay R.; Hsu, Christina; Krotkov, Nickolay; Torres, Omar

1998-01-01

New technique for observing aerosols from space, using ultraviolet (UV) wavelengths, have been developed during the past three years. The chief benefit from observing aerosols in the UV is that they are easily visible over both land and water. While there is presently more than one satellite that can observe aerosols in the UV, only Total Ozone Mapping Spectrometer (TOMS) has a long-term record (since 1979) and adequate spatial resolutions (50 to 100 km) to observe the seasonal and interannual variations, and to locate some of the land sources of dust, smoke, volcanic ash and sulfate pollutants. The data has been assembled into daily images of the atmospheric aerosol loading in terms of optical depth and UV transmittance. For the major sources of aerosols, it is common for at least 50% of the total UV to be absorbed underneath aerosol plumes. This is particularly true for the spectacular smoke plumes originating from the recent Indonesian and Mexican fires, as well as under the huge African dust plumes. The sulfate pollutants are mostly present in the Northern Hemisphere and are associated with regions of high industrial activity. The location and seasonal dependence of these aerosol plumes over Europe and North America will be contrasted with the relatively clean Southern Hemisphere. Because of the success of this technique, it has formed the basis for a new generation of space-borne aerosol detection instruments. These new instruments combine the UV observations with the more traditional visible-wavelength data to obtain a more comprehensive characterization of aerosols that is possible with either UV or visible techniques by themselves.

ESPC Coupled Global Prediction System

DTIC Science & Technology

2014-09-30

active, and cloud- nucleating aerosols into NAVGEM for use in long-term simulations and forecasts and for use in the full coupled system. APPROACH...cloud- nucleating aerosols into NAVGEM for use in long-term simulations and forecasts for ESPC applications. We are relying on approaches, findings...function. For sea salt we follow NAAPS and use a source that depends on ocean surface winds and relative humidity . In lieu of the relevant

Aerosol contribution to the rapid warming of near-term climate under RCP 2.6

NASA Astrophysics Data System (ADS)

Chalmers, N.; Highwood, E. J.; Hawkins, E.; Sutton, R.; Wilcox, L. J.

2012-09-01

The importance of aerosol emissions for near term climate projections is investigated by analysing simulations with the HadGEM2-ES model under two different emissions scenarios: RCP2.6 and RCP4.5. It is shown that the near term warming projected under RCP2.6 is greater than under RCP4.5, even though the greenhouse gas forcing is lower. Rapid and substantial reductions in sulphate aerosol emissions due to a reduction of coal burning in RCP2.6 lead to a reduction in the negative shortwave forcing due to aerosol direct and indirect effects. Indirect effects play an important role over the northern hemisphere oceans, especially the subtropical northeastern Pacific where an anomaly of 5-10 Wm-2 develops. The pattern of surface temperature change is consistent with the expected response to this surface radiation anomaly, whilst also exhibiting features that reflect redistribution of energy, and feedbacks, within the climate system. These results demonstrate the importance of aerosol emissions as a key source of uncertainty in near term projections of global and regional climate.

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

NASA Astrophysics Data System (ADS)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado region compared with the Rainforest environment. This was reflected in the single scattering albedo of the regional smoke haze, with values of 0.9 observed in the Rainforest environments compared with a value of 0.8 in the Cerrado region. This contrast results in a net cooling and warming respectively in terms of the aerosol direct radiative effect. BC-containing particles were found to be rapidly coated in the near-field, with little evidence for additional coating upon advection and dilution. This is consistent with organic aerosol mass being approximately constant when accounting for dilution both close to source and on the regional scale. However, the bulk organic aerosol composition became increasingly oxidised with distance from source. Such properties have important implications for the life cycle and formation of particulate material, which governs its subsequent impacts. Biomass burning layers were observed aloft in the free troposphere, which has potential implications for atmospheric stability profiles and cloud formation. The results presented enhance our knowledge of biomass burning aerosol in a sensitive region of the globe, where relatively few measurement campaigns have taken place previously.

Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

NASA Astrophysics Data System (ADS)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-07-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates contributes 63-100 % to the total measured nitrates in summer. Furthermore, the contribution of organic nitrates to total OA is estimated to be 5-12 % in summer, suggesting that organic nitrates are important components in the ambient aerosol in the southeastern USA. The spatial distribution of OA is investigated by comparing simultaneous HR-ToF-AMS measurements with ACSM measurements at two different sampling sites. OA is found to be spatially homogeneous in summer due possibly to stagnant air mass and a dominant amount of regional secondary organic aerosol (SOA) in the southeastern USA. The homogeneity is less in winter, which is likely due to spatial variation of primary emissions. We observe that the seasonality of OA concentration shows a clear urban/rural contrast. While OA exhibits weak seasonal variation in the urban sites, its concentration is higher in summer than winter for rural sites. This observation from our year-long measurements is consistent with 14 years of organic carbon (OC) data from the SouthEastern Aerosol Research and Characterization (SEARCH) network. The comparison between short-term measurements with advanced instruments and long-term measurements of basic air quality indicators not only tests the robustness of the short-term measurements but also provides insights in interpreting long-term measurements. We find that OA factors resolved from PMF analysis on HR-ToF-AMS measurements have distinctly different diurnal variations. The compensation of OA factors with different diurnal trends is one possible reason for the repeatedly observed, relatively flat OA diurnal profile in the southeastern USA. In addition, analysis of long-term measurements shows that the correlation between OC and sulfate is substantially stronger in summer than winter. This seasonality could be partly due to the effects of sulfate on isoprene SOA formation as revealed by the short-term intensive measurements.

Aerosol typing - key information from aerosol studies

NASA Astrophysics Data System (ADS)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the classification. The harmonization of the aerosol typing procedures is a fundamental need in aerosol studies for long-term perspectives, satellite validation, and accuracy. However, the possibilities and limits in defining a common set of aerosol types for satellite missions and ground-based measurements depends on different information content among measurement techniques and for different retrieval conditions (e.g. for low aerosol content there is smaller satellite aerosol type retrieval sensitivity), as well as different historical choices. The concept of aReference database for aerosol typing (REDAT) is developed with the specific purpose of providing a dataset suitable for the comparison of typing procedures (from ground-based, and satellite measurements) and to be used as reference dataset for the modelling community. It will also allow the definition of translating rules between the different aerosol typing nomenclature, information strongly needed for the more and more increased audience of scientific data with no scientific background, as well as policy and decision makers. Acknowledgments: The research leading to these results is partially funded by ACTRIS2 Research Infrastructure Project by the European Union's Horizon 2020 research and innovation programme under the grant agreement n. 654169.

Long-term aerosol climatology over Indo-Gangetic Plain: Trend, prediction and potential source fields

NASA Astrophysics Data System (ADS)

Kumar, M.; Parmar, K. S.; Kumar, D. B.; Mhawish, A.; Broday, D. M.; Mall, R. K.; Banerjee, T.

2018-05-01

Long-term aerosol climatology is derived using Terra MODIS (Collection 6) enhanced Deep Blue (DB) AOD retrieval algorithm to investigate decadal trend (2006-2015) in columnar aerosol loading, future scenarios and potential source fields over the Indo-Gangetic Plain (IGP), South Asia. Satellite based aerosol climatology was analyzed in two contexts: for the entire IGP considering area weighted mean AOD and for nine individual stations located at upper (Karachi, Multan, Lahore), central (Delhi, Kanpur, Varanasi, Patna) and lower IGP (Kolkata, Dhaka). A comparatively high aerosol loading (AOD: 0.50 ± 0.25) was evident over IGP with a statistically insignificant increasing trend of 0.002 year-1. Analysis highlights the existing spatial and temporal gradients in aerosol loading with stations over central IGP like Varanasi (decadal mean AOD±SD; 0.67 ± 0.28) and Patna (0.65 ± 0.30) exhibit the highest AOD, followed by stations over lower IGP (Kolkata: 0.58 ± 0.21; Dhaka: 0.60 ± 0.24), with a statistically significant increasing trend (0.0174-0.0206 year-1). In contrast, stations over upper IGP reveal a comparatively low aerosol loading, having an insignificant increasing trend. Variation in AOD across IGP is found to be mainly influenced by seasonality and topography. A distinct "aerosol pool" region over eastern part of Ganges plain is identified, where meteorology, topography, and aerosol sources favor the persistence of airborne particulates. A strong seasonality in aerosol loading and types is also witnessed, with high AOD and dominance of fine particulates over central to lower IGP, especially during post-monsoon and winter. The time series analyses by autoregressive integrated moving average (ARIMA) indicate contrasting patterns in randomness of AOD over individual stations with better performance especially over central IGP. Concentration weighted trajectory analyses identify the crucial contributions of western dry regions and partial contributions from central Highlands and north-eastern India, in regulating AOD over stations across IGP. Although our analyses provide some attributes to the observed changes in aerosol loading, we conclude that the spatial and temporal pattern of aerosol properties is highly complex and dynamic over IGP, and require further investigation in order to reduce uncertainty in aerosol-climate model.

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

NASA Astrophysics Data System (ADS)

Qian, Yun; Giorgi, Filippo

1999-03-01

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

A Global Model Simulation of Aerosol Effects of Surface Radiation Budget- Toward Understanding of the "Dimming to Brightening" Transition

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Bian, Huisheng; Yu, Hongbin

2008-01-01

We present a global model study on the role aerosols play in the change of solar radiation at Earth's surface that transitioned from a decreasing (dimming) trend to an increasing (brightening) trend. Our primary objective is to understand the relationship between the long-term trends of aerosol emission, atmospheric burden, and surface solar radiation. More specifically, we use the recently compiled comprehensive global emission datasets of aerosols and precursors from fuel combustion, biomass burning, volcanic eruptions and other sources from 1980 to 2006 to simulate long-term variations of aerosol distributions and optical properties, and then calculate the multi-decadal changes of short-wave radiative fluxes at the surface and at the top of the atmosphere by coupling the GOCART model simulated aerosols with the Goddard radiative transfer model. The model results are compared with long-term observational records from ground-based networks and satellite data. We will address the following critical questions: To what extent can the observed surface solar radiation trends, known as the transition from dimming to brightening, be explained by the changes of anthropogenic and natural aerosol loading on global and regional scales? What are the relative contributions of local emission and long-range transport to the surface radiation budget and how do these contributions change with time?

Two years of near real-time chemical composition of submicron aerosols in the region of Paris using an Aerosol Chemical Speciation Monitor (ACSM) and a multi-wavelength Aethalometer

NASA Astrophysics Data System (ADS)

Petit, J.-E.; Favez, O.; Sciare, J.; Crenn, V.; Sarda-Estève, R.; Bonnaire, N.; Močnik, G.; Dupont, J.-C.; Haeffelin, M.; Leoz-Garziandia, E.

2015-03-01

Aerosol mass spectrometer (AMS) measurements have been successfully used towards a better understanding of non-refractory submicron (PM1) aerosol chemical properties based on short-term campaigns. The recently developed Aerosol Chemical Speciation Monitor (ACSM) has been designed to deliver quite similar artifact-free chemical information but for low cost, and to perform robust monitoring over long-term periods. When deployed in parallel with real-time black carbon (BC) measurements, the combined data set allows for a quasi-comprehensive description of the whole PM1 fraction in near real time. Here we present 2-year long ACSM and BC data sets, between mid-2011 and mid-2013, obtained at the French atmospheric SIRTA supersite that is representative of background PM levels of the region of Paris. This large data set shows intense and time-limited (a few hours) pollution events observed during wintertime in the region of Paris, pointing to local carbonaceous emissions (mainly combustion sources). A non-parametric wind regression analysis was performed on this 2-year data set for the major PM1 constituents (organic matter, nitrate, sulfate and source apportioned BC) and ammonia in order to better refine their geographical origins and assess local/regional/advected contributions whose information is mandatory for efficient mitigation strategies. While ammonium sulfate typically shows a clear advected pattern, ammonium nitrate partially displays a similar feature, but, less expectedly, it also exhibits a significant contribution of regional and local emissions. The contribution of regional background organic aerosols (OA) is significant in spring and summer, while a more pronounced local origin is evidenced during wintertime, whose pattern is also observed for BC originating from domestic wood burning. Using time-resolved ACSM and BC information, seasonally differentiated weekly diurnal profiles of these constituents were investigated and helped to identify the main parameters controlling their temporal variations (sources, meteorological parameters). Finally, a careful investigation of all the major pollution episodes observed over the region of Paris between 2011 and 2013 was performed and classified in terms of chemical composition and the BC-to-sulfate ratio used here as a proxy of the local/regional/advected contribution of PM. In conclusion, these first 2-year quality-controlled measurements of ACSM clearly demonstrate their great potential to monitor on a long-term basis aerosol sources and their geographical origin and provide strategic information in near real time during pollution episodes. They also support the capacity of the ACSM to be proposed as a robust and credible alternative to filter-based sampling techniques for long-term monitoring strategies.

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

Barry, Kenneth

The Nuclear Energy Institute (NEI) Small Modular Reactor (SMR) Licensing Task Force (TF) has been evaluating licensing issues unique and important to iPWRs, ranking these issues, and developing NEI position papers for submittal to the U.S. Nuclear Regulatory Commission (NRC) during the past three years. Papers have been developed and submitted to the NRC in a range of areas including: Price-Anderson Act, NRC annual fees, security, modularity, and staffing. In December, 2012, NEI completed a draft position paper on SMR source terms and participated in an NRC public meeting presenting a summary of this paper, which was subsequently submitted tomore » the NRC. One important conclusion of the source term paper was the evaluation and selection of high importance areas where additional research would have a significant impact on source terms. The highest ranked research area was iPWR containment aerosol natural deposition. The NRC accepts the use of existing aerosol deposition correlations in Regulatory Guide 1.183, but these were developed for large light water reactor (LWR) containments. Application of these correlations to an iPWR design has resulted in greater than a ten-fold reduction of containment airborne aerosol inventory as compared to large LWRs. Development and experimental justification of containment aerosol natural deposition correlations specifically for the unique iPWR containments is expected to result in a large reduction of design basis and beyond-design-basis accident source terms with concomitantly smaller dose to workers and the public. Therefore, NRC acceptance of iPWR containment aerosol natural deposition correlations will directly support the industry’s goal of reducing the Emergency Planning Zone (EPZ) for SMRs. Based on the results in this work, it is clear that thermophoresis is relatively unimportant for iPWRs. Gravitational settling is well understood, and may be the dominant process for a dry environment. Diffusiophoresis and enhanced settling by particle growth are the dominant processes for determining DFs for expected conditions in an iPWR containment. These processes are dependent on the areato-volume (A/V) ratio, which should benefit iPWR designs because these reactors have higher A/Vs compared to existing LWRs.« less

Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

NASA Astrophysics Data System (ADS)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-04-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates contributes 63-100% of total measured nitrates in summer. Further, the contribution of organic nitrates to total OA is estimated to be 5-12% in summer, suggesting that organic nitrates are important components in the ambient aerosol in the southeastern US. The spatial distribution of OA is investigated by comparing simultaneous HR-ToF-AMS measurements with ACSM measurements at two different sampling sites. OA is found to be spatially homogeneous in summer, possibly due to stagnant air mass and a dominant amount of regional SOA in the southeastern US. The homogeneity is less in winter, which is likely due to spatial variation of primary emissions. We observed that the seasonality of OA concentration shows a clear urban/rural contrast. While OA exhibits weak seasonal variation in the urban sites, its concentration is higher in summer than winter for rural sites. This observation from our year-long measurements is consistent with 14 years of organic carbon (OC) data from the SouthEastern Aerosol Research and Characterization (SEARCH) network. The comparison between short-term measurements with advanced instruments and long-term measurements of basic air quality indicators not only tests the robustness of the short-term measurements but also provides insights in interpreting long-term measurements. We find that OA factors resolved from PMF analysis on HR-ToF-AMS measurements have distinctly different diurnal variations. The compensation of OA factors with different diurnal trends is one possible reason for the repeatedly observed, relatively flat OA diurnal profile in the southeastern US. In addition, analysis of long-term measurements shows that the correlation between OC and sulfate is substantially higher in summer than winter. This seasonality could be partly due to the effects of sulfate on isoprene SOA formation as revealed by the short-term, intensive measurements.

Characterization of distinct Arctic aerosol accumulation modes and their sources

NASA Astrophysics Data System (ADS)

Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

2018-06-01

In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the Arctic.

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

Parworth, Caroline; Fast, Jerome D.; Mei, Fan

In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the U.S. Department of Energy’s Southern Great Plains (SGP) site are discussed. Over the period of 19 months (Nov. 20, 2010 – June 2012) highly time resolved (~30 min.) NR-PM1 data was recorded. Using this dataset the value-added product (VAP) of deriving organic aerosol components (OACOMP) is introduced. With this VAP, multivariate analysis of the measured organic mass spectral matrix can be performed on long term data to return organic aerosol (OA) factors that are associatedmore » with distinct sources, evolution processes, and physiochemical properties. Three factors were obtained from this VAP including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when nitrate increased due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations showed little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increased and were mainly associated with local fires. Isoprene and carbon monoxide emission rates were computed by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) to represent the spatial distribution of biogenic and anthropogenic sources, respectively. From this model there is evidence to support that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

Stable carbon isotope ratios of low molecular weight dicarboxylic acids, ketoacids and glyoxal in marine aerosols from the western North Pacific: Long-term trends in Chichijima Island

NASA Astrophysics Data System (ADS)

Kawamura, K.; Tachibana, E.

2012-12-01

Dicarboxylic acids such as oxalic, malonic and succinic acids are the most abundant water-soluble organic compound class in aerosols. To better understand the source and photochemical processes of water-soluble organic aerosols in the remote marine aerosols, we measured stable carbon isotopic composition (δ13C) of dicarboxylic acids and related compounds using a GC/IR/MS technique. The aerosol samples were collected in 2001-2011 at a remote island, Chichijima (27°04'E; 142°13'N) in the western North Pacific. Here we present decadal variations of the isotopic composition of dicarboxylic acids (C2-C9), ketoacids (C2-C8) and glyoxal in summertime aerosols (June, July and August). The molecular distributions of diacids were characterized by the predominance of oxalic (C2) acid followed by malonic (C3) and succinic (C4) acids. Oxalic acid showed higher δ13C values than other species ranging from -18‰ to -2‰ with no clear decadal trend. In contrast, C3 and C4 diacids showed δ13C values of -24 to -5‰ and -40 to -12‰ with a decadal decline. Glyoxal (-60 to -10‰) and ωC7 acid (-34 to -12‰) also showed lower values toward 2011. However, azelaic acid (C9) (-32 to -24‰) stayed relatively constant throughout the observation period. We will discuss the detailed isotopic compositions of these organic species in terms of the photochemical aging and processing in the western North Pacific and the changes in the sources and source regions.

Long-term trends in California mobile source emissions and ambient concentrations of black carbon and organic aerosol.

PubMed

McDonald, Brian C; Goldstein, Allen H; Harley, Robert A

2015-04-21

A fuel-based approach is used to assess long-term trends (1970-2010) in mobile source emissions of black carbon (BC) and organic aerosol (OA, including both primary emissions and secondary formation). The main focus of this analysis is the Los Angeles Basin, where a long record of measurements is available to infer trends in ambient concentrations of BC and organic carbon (OC), with OC used here as a proxy for OA. Mobile source emissions and ambient concentrations have decreased similarly, reflecting the importance of on- and off-road engines as sources of BC and OA in urban areas. In 1970, the on-road sector accounted for ∼90% of total mobile source emissions of BC and OA (primary + secondary). Over time, as on-road engine emissions have been controlled, the relative importance of off-road sources has grown. By 2010, off-road engines were estimated to account for 37 ± 20% and 45 ± 16% of total mobile source contributions to BC and OA, respectively, in the Los Angeles area. This study highlights both the success of efforts to control on-road emission sources, and the importance of considering off-road engine and other VOC source contributions when assessing long-term emission and ambient air quality trends.

Long-term Satellite Observations of Asian Dust Storm: Source, Pathway, and Interannual Variability

NASA Technical Reports Server (NTRS)

Hsu, N. Christina

2008-01-01

Among the many components that contribute to air pollution, airborne mineral dust plays an important role due to its biogeochemical impact on the ecosystem and its radiative-forcing effect on the climate system. In East Asia, dust storms frequently accompany the cold and dry air masses that occur as part of springtime cold front systems. Outbreaks of Asian dust storms occur often in the arid and semi-arid areas of northwestern China -about 1.6x10(exp 6) square kilometers including the Gobi and Taklimakan deserts- with continuous expanding of spatial coverage. These airborne dust particles, originating in desert areas far from polluted regions, interact with anthropogenic sulfate and soot aerosols emitted from Chinese megacities during their transport over the mainland. Adding the intricate effects of clouds and marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from their sources. Furthermore, these aerosols, once generated over the source regions, can be transported out of the boundary layer into the free troposphere and can travel thousands of kilometers across the Pacific into the United States and beyond. In this paper, we will demonstrate the capability of a new satellite algorithm to retrieve aerosol properties (e.g., optical thickness, single scattering albedo) over bright-reflecting surfaces such as urban areas and deserts. Such retrievals have been difficult to perform using previously available algorithms that use wavelengths from the mid-visible to the near IR because they have trouble separating the aerosol signal from the contribution due to the bright surface reflectance. This new algorithm, called Deep Blue, utilizes blue-wavelength measurements from instruments such as SeaWiFS and MODIS to infer the properties of aerosols, since the surface reflectance over land in the blue part of the spectrum is much lower than for longer wavelength channels. Reasonable agreements have been achieved between Deep Blue retrievals of aerosol optical thickness and those directly from AERONET sunphotometers over desert and semi-desert regions. New Deep Blue products will allow scientists to determine quantitatively the aerosol properties near sources using high spatial resolution measurements from SeaWiFS and MODIS-like instruments. Long-term satellite measurements (1998 - 2007) from SeaWiFS will be utilized to investigate the interannual variability of source, pathway, and dust loading associated with the Asian dust storm outbreaks. In addition, monthly averaged aerosol optical thickness during the springtime from SeaWiFS will also be compared with the MODIS Deep Blue products.

Impact of Emissions and Long-Range Transport on Multi-Decadal Aerosol Trends: Implications for Air Quality and Climate

NASA Technical Reports Server (NTRS)

Chin, Mian

2012-01-01

We present a global model analysis of the impact of long-range transport and anthropogenic emissions on the aerosol trends in the major pollution regions in the northern hemisphere and in the Arctic in the past three decades. We will use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze the multi-spatial and temporal scale data, including observations from Terra, Aqua, and CALIPSO satellites and from the long-term surface monitoring stations. We will analyze the source attribution (SA) and source-receptor (SR) relationships in North America, Europe, East Asia, South Asia, and the Arctic at the surface and free troposphere and establish the quantitative linkages between emissions from different source regions. We will discuss the implications for regional air quality and climate change.

Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

DOE PAGES

Parworth, Caroline; Tilp, Alison; Fast, Jerome; ...

2015-04-01

In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

Climatology of Aerosol Optical Properties in Southern Africa

NASA Technical Reports Server (NTRS)

Queface, Antonio J.; Piketh, Stuart J.; Eck, Thomas F.; Tsay, Si-Chee

2011-01-01

A thorough regionally dependent understanding of optical properties of aerosols and their spatial and temporal distribution is required before we can accurately evaluate aerosol effects in the climate system. Long term measurements of aerosol optical depth, Angstrom exponent and retrieved single scattering albedo and size distribution, were analyzed and compiled into an aerosol optical properties climatology for southern Africa. Monitoring of aerosol parameters have been made by the AERONET program since the middle of the last decade in southern Africa. This valuable information provided an opportunity for understanding how aerosols of different types influence the regional radiation budget. Two long term sites, Mongu in Zambia and Skukuza in South Africa formed the core sources of data in this study. Results show that seasonal variation of aerosol optical thicknesses at 500 nm in southern Africa are characterized by low seasonal multi-month mean values (0.11 to 0.17) from December to May, medium values (0.20 to 0.27) between June and August, and high to very high values (0.30 to 0.46) during September to November. The spatial distribution of aerosol loadings shows that the north has high magnitudes than the south in the biomass burning season and the opposite in none biomass burning season. From the present aerosol data, no long term discernable trends are observable in aerosol concentrations in this region. This study also reveals that biomass burning aerosols contribute the bulk of the aerosol loading in August-October. Therefore if biomass burning could be controlled, southern Africa will experience a significant reduction in total atmospheric aerosol loading. In addition to that, aerosol volume size distribution is characterized by low concentrations in the non biomass burning period and well balanced particle size contributions of both coarse and fine modes. In contrast high concentrations are characteristic of biomass burning period, combined with significant dominance of fine mode particles.

Biomass burning source characterization requirements in air quality models with and without data assimilation: challenges and opportunities

NASA Astrophysics Data System (ADS)

Hyer, E. J.; Zhang, J. L.; Reid, J. S.; Curtis, C. A.; Westphal, D. L.

2007-12-01

Quantitative models of the transport and evolution of atmospheric pollution have graduated from the laboratory to become a part of the operational activity of forecast centers. Scientists studying the composition and variability of the atmosphere put great efforts into developing methods for accurately specifying sources of pollution, including natural and anthropogenic biomass burning. These methods must be adapted for use in operational contexts, which impose additional strictures on input data and methods. First, only input data sources available in near real-time are suitable for use in operational applications. Second, operational applications must make use of redundant data sources whenever possible. This is a shift in philosophy: in a research context, the most accurate and complete data set will be used, whereas in an operational context, the system must be designed with maximum redundancy. The goal in an operational context is to produce, to the extent possible, consistent and timely output, given sometimes inconsistent inputs. The Naval Aerosol Analysis and Prediction System (NAAPS), a global operational aerosol analysis and forecast system, recently began incorporating assimilation of satellite-derived aerosol optical depth. Assimilation of satellite AOD retrievals has dramatically improved aerosol analyses and forecasts from this system. The use of aerosol data assimilation also changes the strategy for improving the smoke source function. The absolute magnitude of emissions events can be refined through feedback from the data assimilation system, both in real- time operations and in post-processing analysis of data assimilation results. In terms of the aerosol source functions, the largest gains in model performance are now to be gained by reducing data latency and minimizing missed detections. In this presentation, recent model development work on the Fire Locating and Monitoring of Burning Emissions (FLAMBE) system that provides smoke aerosol boundary conditions for NAAPS is described, including redundant integration of multiple satellite platforms and development of feedback loops between the data assimilation system and smoke source.

Spectral solar attenuation due to aerosol loading over an urban area in India

NASA Astrophysics Data System (ADS)

Latha, K. Madhavi; Badarinath, K. V. S.

2005-06-01

Anthropogenic activities in urban areas are sources for atmospheric aerosols and are increasing due to population explosion and migration. Many large cities in the developing world are presently plagued by high levels of atmospheric pollution and long-term effect of urban aerosol on climate is an important topic. In the present study, ground-based measurements of solar irradiance, aerosol loading and black carbon (BC) aerosol concentration have been analyzed during different aerosol loading conditions during 2003 over an urban environment. BC aerosols concentration has been observed to be enhanced during high aerosol optical depth day suggesting influence of local anthropogenic activities. The analysis of wind fields over the study area during the measurement period is from north with continental air mass prevailing over the region. Spectral measurements of solar irradiance exhibited variations based on aerosol loading in urban atmosphere. Relative attenuations caused by aerosols have been found to be of the order of 21% and 17% on the irradiance on visible and near infrared respectively.

Source and long-term behavior of transuranic aerosols in the WIPP environment.

PubMed

Thakur, P; Lemons, B G

2016-10-01

Source and long-term behavior transuranic aerosols ((239+240)Pu, (238)Pu, and (241)Am) in the ambient air samples collected at and near the Waste Isolation Pilot Plant (WIPP) deep geologic repository site were investigated using historical data from an independent monitoring program conducted by the Carlsbad Environmental Monitoring and Research Center and an oversight monitoring program conducted by the management and operating contractor for WIPP at and near the facility. An analysis of historical data indicates frequent detections of (239+240)Pu and (241)Am, whereas (238)Pu is detected infrequently. Peaks in (239+240)Pu and (241)Am concentrations in ambient air generally occur from March to June timeframe, which is when strong and gusty winds in the area frequently give rise to blowing dust. Long-term measurements of plutonium isotopes (1985-2015) in the WIPP environment suggest that the resuspension of previously contaminated soils is likely the primary source of plutonium in the ambient air samples from WIPP and its vicinity. There is no evidence that WIPP is a source of environmental contamination that can be considered significant by any health-based standard.

Chemical characterization and source apportionment of fine particulate matter in Yangzhou, China, using offline aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Li, L.; Ge, X.; Xu, J.; Ye, Z.

2016-12-01

In recent years, Aerodyne Aerosol Mass Spectrometer (AMS) has been widely used for online and real-time monitoring of fine aerosol particles all over the world. However, due to the high cost and complex maintenance, the AMS was typically deployed for short-term intense field measurements, limiting its ability in elucidating the long-term behaviors and dominant sources of regional fine particles (PM2.5). In this study, we collected daily PM2.5 filter samples across a relatively long period (November 2015 to April 2016, in total >100 samples) using a high-volume sampler, in urban Yangzhou - a city in the Yangtze River Delta region, China. These samples were analyzed by using a suite of analytical techniques, for the water-soluble inorganic ions (WSIs), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and total nitrogen (TN), trace metal elements, etc. More importantly, an Aerodyne soot particle aerosol mass spectrometer (SP-AMS) was for the first time introduced for the offline characterization of the PM2.5 samples collected in this region. In particular, Positive matrix factorization was conducted on the SP-AMS determined water-soluble fraction of organic aerosols (WSOA), and three distinct sources were separated, including a primary OA (POA), a less oxygenated OA (LOOA), and a more oxygenated OA (MOOA). Chemical characteristics and evolution processes of these OA subcomponents were further discussed. Our results are useful for the air pollution management in the YRD region, and the technique developed can be applied elsewhere as well.

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

NASA Technical Reports Server (NTRS)

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

2010-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2010-08-01

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

Remote Sensing of Aerosol in the Terrestrial Atmosphere from Space: New Missions

NASA Technical Reports Server (NTRS)

Milinevsky, G.; Yatskiv, Ya.; Degtyaryov, O.; Syniavskyi, I.; Ivanov, Yu.; Bovchaliuk, A.; Mishchenko, M.; Danylevsky, V.; Sosonkin, M.; Bovchaliuk, V.

2015-01-01

The distribution and properties of atmospheric aerosols on a global scale are not well known in terms of determination of their effects on climate. This mostly is due to extreme variability of aerosol concentrations, properties, sources, and types. Aerosol climate impact is comparable to the effect of greenhouse gases, but its influence is more difficult to measure, especially with respect to aerosol microphysical properties and the evaluation of anthropogenic aerosol effect. There are many satellite missions studying aerosol distribution in the terrestrial atmosphere, such as MISR/Terra, OMI/Aura, AVHHR, MODIS/Terra and Aqua, CALIOP/CALIPSO. To improve the quality of data and climate models, and to reduce aerosol climate forcing uncertainties, several new missions are planned. The gap in orbital instruments for studying aerosol microphysics has arisen after the Glory mission failed during launch in 2011. In this review paper, we describe several planned aerosol space missions, including the Ukrainian project Aerosol-UA that obtains data using a multi-channel scanning polarimeter and wide-angle polarimetric camera. The project is designed for remote sensing of the aerosol microphysics and cloud properties on a global scale.

Importance of Anthropogenic Aerosols for Climate Prediction: a Study on East Asian Sulfate Aerosols

NASA Astrophysics Data System (ADS)

Bartlett, R. E.; Bollasina, M. A.

2017-12-01

Climate prediction is vital to ensure that we are able to adapt to our changing climate. Understandably, the main focus for such prediction is greenhouse gas forcing, as this will be the main anthropogenic driver of long-term global climate change; however, other forcings could still be important. Atmospheric aerosols represent one such forcing, especially in regions with high present-day aerosol loading such as Asia; yet, uncertainty in their future emissions are under-sampled by commonly used climate forcing projections, such as the Representative Concentration Pathways (RCPs). Globally, anthropogenic aerosols exert a net cooling, but their effects show large variation at regional scales. Studies have shown that aerosols impact locally upon temperature, precipitation and hydroclimate, and also upon larger scale atmospheric circulation (for example, the Asian monsoon) with implications for climate remote from aerosol sources. We investigate how future climate could evolve differently given the same greenhouse gas forcing pathway but differing aerosol emissions. Specifically, we use climate modelling experiments (using HadGEM2-ES) of two scenarios based upon RCP2.6 greenhouse gas forcing but with large differences in sulfur dioxide emissions over East Asia. Results show that increased sulfate aerosols (associated with increased sulfur dioxide) lead to large regional cooling through aerosol-radiation and aerosol-cloud interactions. Focussing on dynamical mechanisms, we explore the consequences of this cooling for the Asian summer and winter monsoons. In addition to local temperature and precipitation changes, we find significant changes to large scale atmospheric circulation. Wave-like responses to upper-level atmospheric changes propagate across the northern hemisphere with far-reaching effects on surface climate, for example, cooling over Europe. Within the tropics, we find alterations to zonal circulation (notably, shifts in the Pacific Walker cell) and monsoon systems outside of Asia. These results indicate that anthropogenic aerosols have significant climate impacts against a background of greenhouse gas-induced climate change, and thus represent a key source of uncertainty in near-term climate projection that should be seriously considered in future climate assessments.

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.;

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 precipitation seesaw between eastern and western Siberia. The results of this study raise the possibility that global aerosol forcing during boreal spring may play an important role in spawning atmospheric teleconnections that affect regional and global climates.

Marine Aerosols and Clouds.

PubMed

Brooks, Sarah D; Thornton, Daniel C O

2018-01-03

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

Chemical signatures of urban, open burning and dust transportation in an urban environment- megacity in South Asia

NASA Astrophysics Data System (ADS)

Priyadharshini, B.; Verma, S.

2016-12-01

A sub-micron aerosol sampler (SAS) consisting of two parallel stacked filter units (SFU) was deployed at an urban location (Kolkata) to study the sub-micron aerosols (water soluble inorganic ions (WSII) and carbonaceous aerosols (elemental carbon (EC) and organic carbon (OC)) collected over a year (September 2010 to August 2011). Quantification of 10 WSII species using Ion Chromatograph (IC) indicated alkaline nature of aerosols with calcium (Ca2+) being the major neutralizing factor of acidity at the study site. In terms of WSII percentage contribution, the most abundant were crustal species (Ca2+, magnesium (Mg2+) and marine species (chloride (Cl-)), followed by the secondary species sulphate (SO42-), nitrate (NO3-) and ammonium (NH4+) . Ca2+ (fugitive and transported dust) was dominant throughout the study period with K+ concentrations exhibiting seasonality with agricultural residue burning. Further, results of carbonaceous aerosols analyzed using the OC-EC aerosol analyzer following Interagency Monitoring of Protected Visual Environment (IMPROVE) protocol exhibited pronounced seasonality in OC than EC with the overall mean concentration of OC being three folds than EC. Primary organic carbon (POC) and secondary organic carbon concentrations (SOC) estimated using EC tracer method showed 57% (43%) of POC (SOC) from various emission sources. Investigation of OC/EC ratio along with non-sea salt potassium (nss-K+) values revealed influence of season specific anthropogenic activities on both OC and EC concentrations (viz. Open burning (OB)) besides fossil fuel (FF) and biofuel (BF) usage for cooking and heating prevalent over the region. Source apportionment was discerned using positive matrix factorization (PMF) with four major factors (crustal, agricultural, anthropogenic sources and mixed source (crustal + agriculture + anthropogenic) as the primary contributors to the sub-micron aerosols at the study site.

Preferential aerosolization of bacteria in bioaerosols generated in vitro.

PubMed

Perrott, P; Turgeon, N; Gauthier-Levesque, L; Duchaine, C

2017-09-01

Little is known about how bacteria are aerosolized in terms of whether some bacteria will be found in the air more readily than others that are present in the source. This report describes in vitro experiments to compare aerosolization rates (also known as preferential aerosolization) of Gram-positive and Gram-negative bacteria as well as rod- and coccus-shaped bacteria, using two nebulization conditions. A consortium of five bacterial species was aerosolized in a homemade chamber. Aerosols generated with a commercial nebulizer and a homemade bubble-burst aerosol generator were compared. Data suggest that Pseudomonas aeruginosa was preferentially aerosolized in comparison to Moraxella catarrhalis, Lactobacillus paracasei, Staphylococcus aureus and Streptococcus suis, independently of the method of aerosolization. Bacterial integrity of Strep. suis was more preserved compared to other bacteria studied as revealed with PMA-qPCR. We reported the design of an aerosol chamber and bubble-burst generator for the in vitro study of preferential aerosolization. In our setting, preferential aerosolization was influenced by bacterial properties instead of aerosolization mechanism. These findings could have important implications for predicting the composition of bioaerosols in various locations such as wastewater treatment plants, agricultural settings and health care settings. © 2017 The Society for Applied Microbiology.

Atmospheric aerosol source identification and estimates of source contributions to air pollution in Dundee, UK

NASA Astrophysics Data System (ADS)

Qin, Y.; Oduyemi, K.

Anthropogenic aerosol (PM 10) emission sources sampled at an air quality monitoring station in Dundee have been analysed. However, the information on local natural aerosol emission sources was unavailable. A method that combines receptor model and atmospheric dispersion model was used to identify aerosol sources and estimate source contributions to air pollution. The receptor model identified five sources. These are aged marine aerosol source with some chlorine replaced by sulphate, secondary aerosol source of ammonium sulphate, secondary aerosol source of ammonium nitrate, soil and construction dust source, and incinerator and fuel oil burning emission source. For the vehicle emission source, which has been comprehensively described in the atmospheric emission inventory but cannot be identified by the receptor model, an atmospheric dispersion model was used to estimate its contributions. In Dundee, a significant percentage, 67.5%, of the aerosol mass sampled at the study station could be attributed to the six sources named above.

Future Arctic temperature change resulting from a range of aerosol emissions scenarios

DOE PAGES

Wobus, Cameron; Flanner, Mark; Sarofim, Marcus C.; ...

2016-05-17

The Arctic temperature response to emissions of aerosols – specifically black carbon (BC), organic carbon (OC), and sulfate – depends on both the sector and the region where these emissions originate. Thus, the net Arctic temperature response to global aerosol emissions reductions will depend strongly on the blend of emissions sources being targeted. We use recently published equilibrium Arctic temperature response factors for BC, OC, and sulfate to estimate the range of present-day and future Arctic temperature changes from seven different aerosol emissions scenarios. Globally, Arctic temperature changes calculated from all of these emissions scenarios indicate that present-day emissions frommore » the domestic and transportation sectors generate the majority of present-day Arctic warming from BC. However, in all of these scenarios, this warming is more than offset by cooling resulting from SO 2 emissions from the energy sector. Thus, long-term climate mitigation strategies that are focused on reducing carbon dioxide (CO 2) emissions from the energy sector could generate short-term, aerosol-induced Arctic warming. As a result, a properly phased approach that targets BC-rich emissions from the transportation sector as well as the domestic sectors in key regions – while simultaneously working toward longer-term goals of CO 2 mitigation – could potentially avoid some amount of short-term Arctic warming.« less

A study of remotely sensed aerosol properties from ground-based sun and sky scanning radiometers

NASA Astrophysics Data System (ADS)

Giles, David M.

Aerosol particles impact human health by degrading air quality and affect climate by heating or cooling the atmosphere. The Indo-Gangetic Plain (IGP) of Northern India, one of the most populous regions in the world, produces and is impacted by a variety of aerosols including pollution, smoke, dust, and mixtures of them. The NASA Aerosol Robotic Network (AERONET) mesoscale distribution of Sun and sky-pointing instruments in India was established to measure aerosol characteristics at sites across the IGP and around Kanpur, India, a large urban and industrial center in the IGP, during the 2008 pre-monsoon (April-June). This study focused on detecting spatial and temporal variability of aerosols, validating satellite retrievals, and classifying the dominant aerosol mixing states and origins. The Kanpur region typically experiences high aerosol loading due to pollution and smoke during the winter and high aerosol loading due to the addition of dust to the pollution and smoke mixture during the pre-monsoon. Aerosol emissions in Kanpur likely contribute up to 20% of the aerosol loading during the pre-monsoon over the IGP. Aerosol absorption also increases significantly downwind of Kanpur indicating the possibility of the black carbon emissions from aerosol sources such as coal-fired power plants and brick kilns. Aerosol retrievals from satellite show a high bias when compared to the mesoscale distributed instruments around Kanpur during the pre-monsoon with few high quality retrievals due to imperfect aerosol type and land surface characteristic assumptions. Aerosol type classification using the aerosol absorption, size, and shape properties can identify dominant aerosol mixing states of absorbing dust and black carbon particles. Using 19 long-term AERONET sites near various aerosol source regions (Dust, Mixed, Urban/Industrial, and Biomass Burning), aerosol absorption property statistics are expanded upon and show significant differences when compared to previous work. The sensitivity of absorption properties is evaluated and quantified with respect to aerosol retrieval uncertainty. Using clustering analysis, aerosol absorption and size relationships provide a simple method to classify aerosol mixing states and origins and potentially improve aerosol retrievals from ground-based and satellite-based instrumentation.

ERROR IN ANNUAL AVERAGE DUE TO USE OF LESS THAN EVERYDAY MEASUREMENTS

EPA Science Inventory

Long term averages of the concentration of PM mass and components are of interest for determining compliance with annual averages, for developing exposure surrogated for cross-sectional epidemiologic studies of the long-term of PM, and for determination of aerosol sources by chem...

Is there an aerosol signature of aqueous processing?

NASA Astrophysics Data System (ADS)

Ervens, B.; Sorooshian, A.

2017-12-01

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

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

NASA Astrophysics Data System (ADS)

Daellenbach, Kaspar R.; Stefenelli, Giulia; Bozzetti, Carlo; Vlachou, Athanasia; Fermo, Paola; Gonzalez, Raquel; Piazzalunga, Andrea; Colombi, Cristina; Canonaco, Francesco; Hueglin, Christoph; Kasper-Giebl, Anne; Jaffrezo, Jean-Luc; Bianchi, Federico; Slowik, Jay G.; Baltensperger, Urs; El-Haddad, Imad; Prévôt, André S. H.

2017-11-01

Long-term monitoring of organic aerosol is important for epidemiological studies, validation of atmospheric models, and air quality management. In this study, we apply a recently developed filter-based offline methodology using an aerosol mass spectrometer (AMS) to investigate the regional and seasonal differences of contributing organic aerosol sources. We present offline AMS measurements for particulate matter smaller than 10 µm at nine stations in central Europe with different exposure characteristics for the entire year of 2013 (819 samples). The focus of this study is a detailed source apportionment analysis (using positive matrix factorization, PMF) including in-depth assessment of the related uncertainties. Primary organic aerosol (POA) is separated in three components: hydrocarbon-like OA related to traffic emissions (HOA), cooking OA (COA), and biomass burning OA (BBOA). We observe enhanced production of secondary organic aerosol (SOA) in summer, following the increase in biogenic emissions with temperature (summer oxygenated OA, SOOA). In addition, a SOA component was extracted that correlated with an anthropogenic secondary inorganic species that is dominant in winter (winter oxygenated OA, WOOA). A factor (sulfur-containing organic, SC-OA) explaining sulfur-containing fragments (CH3SO2+), which has an event-driven temporal behaviour, was also identified. The relative yearly average factor contributions range from 4 to 14 % for HOA, from 3 to 11 % for COA, from 11 to 59 % for BBOA, from 5 to 23 % for SC-OA, from 14 to 27 % for WOOA, and from 15 to 38 % for SOOA. The uncertainty of the relative average factor contribution lies between 2 and 12 % of OA. At the sites north of the alpine crest, the sum of HOA, COA, and BBOA (POA) contributes less to OA (POA / OA = 0.3) than at the southern alpine valley sites (0.6). BBOA is the main contributor to POA with 87 % in alpine valleys and 42 % north of the alpine crest. Furthermore, the influence of primary biological particles (PBOAs), not resolved by PMF, is estimated and could contribute significantly to OA in PM10.

Characteristics of Fine Particulate Carbonaceous Aerosol at Two Remote Sites in Central Asia

EPA Science Inventory

Central Asia is a relatively understudied region of the world in terms of characterizing ambient particulate matter (PM) and quantifying source impacts of PM at receptor locations, although it is speculated to have an important role as a source region for long-range transport of ...

Integrating multiple remote sensing and surface measurements with models, to quantify and constrain the past decade's total 4D aerosol source profile and impacts

NASA Astrophysics Data System (ADS)

Cohen, J. B.; Lan, R.; Lin, C.; Ng, D. H. L.; Lim, A.

2017-12-01

A multi-instrument, inverse modeling approach, is employed to identify and quantify large-scale global biomass urban aerosol emissions profiles. The approach uses MISR, MODIS, OMI and MOPITT, with data from 2006 to 2016, to generate spatial and temporal loads, as well as some information about composition. The method is able to identify regions impacted by stable urban sources, changing urban sources, intense fires, and linear-combinations. Subsequent quantification is a unified field, leading to a less biased profile, with the result not requiring arbitrary scaling to match long-term means. Additionally, the result reasonably reproduces inter and intra annual variation. Both meso-scale (WRF-CHEM) and global (MIT-AERO, multi-mode, multi-mixing state aerosol model) models of aerosol transport, chemistry, and physics, are used to generate resulting 4D aerosol fields. Comparisons with CALIOP, AERONET, and surface chemical and aerosol networks, provide unbiased confirmation, while column and vertical loadings provide additional feedback. There are three significant results. First, there is a reduction in sources over existing urban areas in East Asia. Second, there is an increase in sources over new urban areas in South, South East, and East Asia. Third, that there is an increase in fire sources in South and South East Asia. There are other initial findings relevant to the global tropics, which have not been as deeply investigated. The results improve the model match with both the mean and variation, which is essential if we hope to understand seasonal extremes. The results also quantify impacts of both local and long-range sources. This is of extreme urgency, in particular in developing nations, where there are considerable contributions from long-range or otherwise unknown sources, that impact hundreds of millions of people throughout Asia. It is hoped that the approach provided here can help us to make critical decisions about total sources, as well as point out the many missing scientific and analytical issues still required to address.

Deep Blue Retrievals of Asian Aerosol Properties During ACE-Asia

NASA Technical Reports Server (NTRS)

Hsu, N. Christina; Tsay, Si-Cee; King, Michael D.; Herman, Jay R.

2006-01-01

During the ACE-Asia field campaign, unprecedented amounts of aerosol property data in East Asia during springtime were collected from an array of aircraft, shipboard, and surface instruments. However, most of the observations were obtained in areas downwind of the source regions. In this paper, the newly developed satellite aerosol algorithm called "Deep Blue" was employed to characterize the properties of aerosols over source regions using radiance measurements from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) and Moderate Resolution Imaging Spectroradiometer (MODIS). Based upon the ngstr m exponent derived from the Deep Blue algorithm, it was demonstrated that this new algorithm is able to distinguish dust plumes from fine-mode pollution particles even in complex aerosol environments such as the one over Beijing. Furthermore, these results were validated by comparing them with observations from AERONET sites in China and Mongolia during spring 2001. These comparisons show that the values of satellite-retrieved aerosol optical thickness from Deep Blue are generally within 20%-30% of those measured by sunphotometers. The analyses also indicate that the roles of mineral dust and anthropogenic particles are comparable in contributing to the overall aerosol distributions during spring in northern China, while fine-mode particles are dominant over southern China. The spring season in East Asia consists of one of the most complex environments in terms of frequent cloudiness and wide ranges of aerosol loadings and types. This paper will discuss how the factors contributing to this complexity influence the resulting aerosol monthly averages from various satellite sensors and, thus, the synergy among satellite aerosol products.

Constraining Upper Troposphere/Lower Stratosphere Aerosol Physical Processes with High-Altitude Aircraft Measurements

NASA Technical Reports Server (NTRS)

Jensen, Eric; Rosenlof, Karen H.; Thornberry, Troy

2018-01-01

Interest in a more complete understanding of the sources, composition and microphysics of stratospheric aerosol particles has intensified during recent years for several reasons: (1) small volcanic eruptions have been recognized as a driver of short-term changes in climate forcing; (2) emissions of sulfur dioxide (SO2) and other aerosol precursors have shifted to south Asia and other low latitude regions with intense vertical transport; (3) organic material has been recognized as a key contributor to lower stratospheric aerosol mass; and (4) interest in possible solar radiation management (geoengineering) through significant enhancements in stratospheric aerosols has intensified. To address stratospheric aerosol science issues, we are proposing a NASA Earth Ventures mission to NASA to provide extensive high-altitude aircraft measurements of critical gas-phase and aerosol properties at multiple locations across the planet. In this presentation, we will discuss the objectives of the proposed campaign, the measurements provided, the sampling strategy, and the modeling and analysis approaches that would be used to address specific science questions.

Updates on the development of Deep Blue aerosol algorithm for constructing consistent long-term data records from MODIS to VIIRS

NASA Astrophysics Data System (ADS)

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

2017-12-01

The impacts of natural and anthropogenic sources of air pollution on climate and human health have continued to gain attention from the scientific community. In order to facilitate these effects, high quality consistent long-term global aerosol data records from satellites are essential. Several EOS-era instruments (e.g., SeaWiFS, MODIS, and MISR) are able to provide such information with a high degree of fidelity. However, with the aging MODIS sensors and the launch of the VIIRS instrument on Suomi NPP in late 2011, the continuation of long-term aerosol data records suitable for climate studies from MODIS to VIIRS is needed urgently. Recently, we have successfully modified our MODIS Deep Blue algorithm to process the VIIRS data. Extensive works were performed in refining the surface reflectance determination scheme to account for the wavelength differences between MODIS and VIIRS. Better aerosol models (including non-spherical dust) are also now implemented in our VIIRS algorithm compared to the MODIS C6 algorithm. We will show the global (land and ocean) distributions of various aerosol products from Version 1 of the VIIRS Deep Blue data set. The preliminary validation results of these new VIIRS Deep Blue aerosol products using data from AERONET sunphotometers over land and ocean will be discussed. We will also compare the monthly averaged Deep Blue aerosol optical depth (AOD) from VIIRS with the MODIS C6 products to investigate if any systematic biases may exist between MODIS C6 and VIIRS AOD. The Version 1 VIIRS Deep Blue aerosol products are currently scheduled to be released to the public in 2018.

Monthly and diurnal variations in aerosol size distributions, downwind of the Seoul metropolitan area

NASA Astrophysics Data System (ADS)

Kim, B. S.; Choi, Y.; Ghim, Y. S.

2014-12-01

The size distribution of aerosols is a physical property. However, since major aerosol types such as mineral dust, secondary inorganic ions, and carbonaceous aerosols are typically in specific size ranges, we can estimate the chemical composition of aerosols from the size distribution. We measured the mass size distribution of aerosols using an optical particle counter (Grimm Model 1.109) for a year from February 2013 to February 2014 at intervals of 10 minutes. The optical particle counter measures number concentrations between 0.25 and 32 μm in 31 bins and converts them into mass concentrations assuming a sphere and densities of aerosols in urban environment which originate from traffic and other combustion sources and are secondarily formed from photochemical reactions. The measurement site is at the rooftop of the five-story building on the hill (37.34 °N, 127.27 °E, 167 m above sea level), about 35 km southeast of downtown Seoul, the downwind area of which is affected by prevailing northwesterlies. There are no major emission sources nearby except a 4-lane road running about 1.4 km to the west. We tried to characterize the bimodal property of the mass size distribution, consisting of fine and coarse modes, in terms of mass concentration and mean diameter. Monthly and diurnal variations in mass concentration and mean diameter of each mode were investigated to estimate major aerosol types as well as major factors causing those variations.

Using the Aerosol Single Scattering Albedo and Angstrom Exponent from AERONET to Determine Aerosol Origins and Mixing States over the Indo-Gangetic Plain

NASA Astrophysics Data System (ADS)

Giles, D. M.; Holben, B. N.; Eck, T. F.; Sinyuk, A.; Slutsker, I.; Smirnov, A.; Schafer, J. S.; Dickerson, R. R.; Thompson, A. M.; Tripathi, S. N.; Singh, R. P.; Ghauri, B.

2012-12-01

Aerosol mixtures—whether dominated by dust, carbon, sulfates, nitrates, sea salt, or mixtures of them—complicate the retrieval of remotely sensed aerosol properties from satellites and possibly increase the uncertainty of the aerosol radiative impact on climate. Major aerosol source regions in South Asia include the Thar Desert as well as agricultural lands, Himalayan foothills, and large urban centers in and near the Indo-Gangetic Plain (IGP). Over India and Pakistan, seasonal changes in meteorology, including the monsoon (June-September), significantly affect the transport, lifetime, and type of aerosols. Strong monsoonal winds can promote long range transport of dust resulting in mixtures of dust and carbonaceous aerosols, while more stagnant synoptic conditions (e.g., November-January) can prolong the occurrence of urban/industrial pollution, biomass burning smoke, or mixtures of them over the IGP. Aerosol Robotic Network (AERONET) Sun/sky radiometer data are analyzed to show the aerosol optical depth (AOD) seasonality and aerosol dominant mixing states. The Single Scattering Albedo (SSA) and extinction Angstrom exponent (EAE) relationship has been shown to provide sound clustering of dominant aerosol types using long term AERONET site data near known source regions [Giles et al., 2012]. In this study, aerosol type partitioning using the SSA (440 nm) and EAE (440-870 nm) relationship is further developed to quantify the occurrence of Dust, Mixed (e.g., dust and carbonaceous aerosols), Urban/Industrial (U/I) pollution, and Biomass Burning (BB) smoke. Based on EAE thresholds derived from the cluster analysis (for AOD440nm>0.4), preliminary results (2001-2010) for Kanpur, India, show the overall contributions of each dominant particle type (rounded to the nearest 10%): 10% for Dust (EAE≤0.25), 60% for Mixed (0.251.25). In the IGP, BB aerosols may have varying sizes (e.g., corresponding to 1.2

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

NASA Astrophysics Data System (ADS)

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

2010-02-01

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

Multidecadal variations of solar radiation reaching the surface and the role of aerosol direct radiative effects

NASA Astrophysics Data System (ADS)

Chin, M.; Diehl, T. L.; Bian, H.; Yu, H.; Kucsera, T. L.; Wild, M., Sr.; Hakuba, M. Z.; Qian, Y.; Stackhouse, P. W., Jr.; Pinker, R. T.; Zhang, Y.; Kato, S.; Loeb, N. G.; Kinne, S.; Streets, D. G.

2017-12-01

Incoming solar radiation drives the Earth's climate system. Long-term surface observations of the solar radiation reaching the surface (RSFC) have shown decreasing or increasing trends, often referred to as solar "dimming" or "brightening", in many regions of the world in the past several decades. Such long-term variation of RSFC mostly reflects the change of the solar-attenuation components within the atmosphere. Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past decades with 50-80% reduction in North America and Europe but an increase of similar magnitude in East and South Asia since 1980, mirroring the change in RSFC over those regions. This has led to suggestions that aerosols play a critical role in determining RSFC trends. This work is to assess the role of direct radiative effects of aerosols on the solar "dimming" and "brightening" trends with modeling studies. First, we will show the trends of aerosol optical depth (AOD) and aerosol surface concentrations in different regions from 1980 to 2009 with remote sensing and in-situ data as well as model simulations, and attribute those changes to anthropogenic or natural sources. We will then show the trends of RSFC from the model and compare the results with observations from the surface networks and satellite-based products. Furthermore, we will use the GOCART model to attribute the "dimming/ brightening" trends to the changes of aerosols through the direct radiative effects. Finally, we will discuss the way forward to understand the aerosol effects on RSFC (as well as on other climate variables) through aerosol-cloud-radiation interactions.

The Impact of Biogenic and Anthropogenic Atmospheric Aerosol on Climate in Egypt

NASA Astrophysics Data System (ADS)

Ibrahim, A. I.; Zakey, A.; Steiner, A. L.; Shokr, M. E.; El-Raey, M.; Ahmed, Y.; Al-Hadidi, A.; Zakey, A.

2014-12-01

Aerosols are indicators of air quality as they reduce visibility and adversely affect public health. Aerosol optical depth (AOD) is a measure of the radiation extinction due to interaction of radiation with aerosol particles in the atmosphere. Using this optical measure of atmospheric aerosols we explore the seasonal and annual patterns of aerosols from both anthropogenic and biogenic sources over Egypt. Here, we use an integrated environment-climate-aerosol model in conjunction with inversion technique to identify the aerosol particle size distribution over different locations in Egypt. The online-integrated Environment-Climate-Aerosol model (EnvClimA), which is based on the International Center for Theoretical Physics Regional Climate Model (ICTP-RegCM), is used to study the emission of different aerosols and their impact on climate parameters for a long-term base line simulation run over Egypt and North Africa. The global emission inventory is downscaled and remapping them over Egypt using local factors such as population, traffic and industrial activities to identify the sources of anthropogenic and biogenic emission from local emission over Egypt. The results indicated that the dominant natural aerosols over Egypt are dust emissions that frequently occur during the transitional seasons (Spring and Autumn). From the local observation we identify the number of dust and sand storm occurrences over Egypt. The Multiangle Imaging SpectroRadiometer (MISR) is used to identify the optical characterizations of different types of aerosols over Egypt. Modeled aerosol optical depth and MISR observed (at 555 nm) are compared from March 2000 through November 2013. The results identify that the MISR AOD captures the maximum peaks of AOD in March/April that coincide with the Khamasin dust storms. However, peaks in May are either due to photochemical reactions or anthropogenic activities. Note: This presentation is for a Partnerships for Enhanced Engagement in Research (PEER) project sponsored by USAID/NSF/NAS. Project Link (at National Academies website): http://sites.nationalacademies.org/PGA/dsc/peerscience/PGA_084046.htmwebsite: http://CleanAirEgypt.org

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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

The world's megacities are the sites of production of a variety of aerosols and are themselves affected by natural and human-induced aerosols. In particular, sources of aerosols impacting cities include: industrial and automobile emission; sand and dust storms from, e.g., the Sahara and Gobi Deserts; as well as fire-induced aerosols. Improving the ability of various stakeholder organizations to respond effectively to high concentrations of aerosols, with special emphasis on mineral dust from dust storms; smoke from controlled burns, wild fires and agricultural burning; and anthropogenic aerosols, would be an important goal not just to understand climate forcings but also to be able to better respond to the increasing amounts of aerosols at global and regional levels. Cities and surrounding areas are affected without good estimates of the current and future conditions of the aerosols and their impact on regional and global climate. Remotely sensed (RS) NASA, NOAA and international platform data can be used to characterize the properties of aerosol clouds and special hazard events such as sand and dust storms (SDS). Aerosol analysis and prediction-model capabilities from which stakeholders can choose the tools that best match their needs and technological expertise are important. Scientists validating mesoscale and aerosol-transport models, aerosol retrievals from satellite measurements are indispensable for robust climate predictions. Here we give two examples of generic SDS cases and urban pollution and their possible impact on climate: The Sahara desert is a major source of dust aerosols dust transport is an important climatic process. The aerosols in the form of dust particles reflect the incoming solar radiation to space, thereby reducing the amount of radiation available to the ground, known as `direct' radiative forcing of aerosols. The aerosols also change the cloud albedo and microphysical properties of clouds, known as `indirect' radiative forcing of 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.

Regional and Global Aspects of Aerosols in Western Africa: From Air Quality to Climate

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Kucsera, Tom; Spinhime, Jim; Palm, Stephen; Holben, Brent; Ginoux, Paul

2006-01-01

Western Africa is one of the most important aerosol source regions in the world. Major aerosol sources include dust from the world's largest desert Sahara, biomass burning from the Sahel, pollution aerosols from local sources and long-range transport from Europe, and biogenic sources from vegetation. Because these sources have large seasonal variations, the aerosol composition over the western Africa changes significantly with time. These aerosols exert large influences on local air quality and regional climate. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to analyze satellite lidar data from the GLAS instrument on the ICESat and the sunphotometer data from the ground-based network AERONET taken in both the wet (September - October 2003) and dry (February - March 2004) seasons over western Africa. We will quantify the seasonal variations of aerosol sources and compositions and aerosol spatial (horizontal and vertical) distributions over western Africa. We will also assess the climate impact of western African aerosols. Such studies will be applied to support the international project, Africa Monsoon Multidisciplinary Analysis (AMMA) and to analyze the AMMA data.

Development of dual-wavelength Mie polarization Raman lidar for aerosol and cloud vertical structure probing

NASA Astrophysics Data System (ADS)

Wang, Zhenzhu; Liu, Dong; Wang, Yingjian; Wang, Bangxin; Zhong, Zhiqing; Xie, Chenbo; Wu, Decheng; Bo, Guangyu; Shao, Jie

2014-11-01

A Dual-wavelength Mie Polarization Raman Lidar has been developed for cloud and aerosol optical properties measurement. This idar system has built in Hefei and passed the performance assessment in 2012, and then moved to Jinhua city to carry out the long-term continuous measurements of vertical distribution of regional cloud and aerosol. A double wavelengths (532 and 1064 nm) Nd-YAG laser is employed as emitting source and four channels are used for detecting back-scattering signals from atmosphere aerosol and cloud including 1064 nm Mie, 607 nm N2 Raman, two 532 nm Orthogonal Polarization channels. The temporal and spatial resolutions for this system, which is operating with a continuing mode (24/7) automatically, are 30s and 7.5m, respectively. The measured data are used for investigating the aerosol and cloud vertical structure and cloud phase from combining of cloud signal intensity, polarization ratio and color ratio.

Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements

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

Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn

2009-03-01

Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that themore » equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.« less

An Assessment of Fission Product Scrubbing in Sodium Pools Following a Core Damage Event in a Sodium Cooled Fast Reactor

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

Bucknor, M.; Farmer, M.; Grabaskas, D.

The U.S. Nuclear Regulatory Commission has stated that mechanistic source term (MST) calculations are expected to be required as part of the advanced reactor licensing process. A recent study by Argonne National Laboratory has concluded that fission product scrubbing in sodium pools is an important aspect of an MST calculation for a sodium-cooled fast reactor (SFR). To model the phenomena associated with sodium pool scrubbing, a computational tool, developed as part of the Integral Fast Reactor (IFR) program, was utilized in an MST trial calculation. This tool was developed by applying classical theories of aerosol scrubbing to the decontamination ofmore » gases produced as a result of postulated fuel pin failures during an SFR accident scenario. The model currently considers aerosol capture by Brownian diffusion, inertial deposition, and gravitational sedimentation. The effects of sodium vapour condensation on aerosol scrubbing are also treated. This paper provides details of the individual scrubbing mechanisms utilized in the IFR code as well as results from a trial mechanistic source term assessment led by Argonne National Laboratory in 2016.« less

An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

NASA Technical Reports Server (NTRS)

Giles, David M.; Holben, Brent N.; Eck, Thomas F.; Sinyuk, Aliaksandr; Smirnov, Alexander; Slutsker, Ilya; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

2012-01-01

Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 < delta omega (sub 0) <= 0.02 decrease) than in previous work and optical mixtures of pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

NASA Astrophysics Data System (ADS)

Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

2014-05-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado region compared with the Rainforest environment. This was reflected in the single scattering albedo of the regional smoke haze, with values of 0.9 observed in the Rainforest environments compared with a value of 0.8 in the Cerrado region. This contrast results in a net cooling and warming respectively in terms of the aerosol direct radiative effect. BC-containing particles were found to be rapidly coated in the near-field, while the organic aerosol component was observed to oxidise rapidly upon advection and dilution downwind of major smoke plumes. Significant differences in the coating thickness of the BC-containing particles were observed when comparing the Rainforest and Cerrado environments. Such properties have important implications for the life cycle and formation of particulate material, as well as their optical and radiative properties. The results presented enhance our knowledge of biomass burning aerosol in a sensitive region of the globe, where relatively few measurement campaigns have taken place previously.

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.

Sources, seasonality, and trends of Southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

NASA Astrophysics Data System (ADS)

Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

2015-07-01

We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the Southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 km × 25 km resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the Southeast US. GEOS-Chem simulation of sulfate requires a missing oxidant, taken here to be stabilized Criegee intermediates, but which could alternatively reflect an unaccounted for heterogeneous process. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 20 % in the cloud convective layer at 1.5-3 km, and 20 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-])) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by organic aerosol. This would explain the long-term decline of ammonium aerosol in the Southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the Southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the Southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 21 %. The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD due to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are fundamentally consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.

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

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

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

Aerosol Sources, Absorption, and Intercontinental Transport: Synergies among Models, Remote Sensing, and Atmospheric Measurements

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Dubovik, Oleg; Holben, Brent; Kaufman, Yoram; chu, Allen; Anderson, Tad; Quinn, Patricia

2003-01-01

Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERONET at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

Aerosol Sources, Absorption, and Intercontinental Transport: Synergies Among Models, Remote Sensing, and Atmospheric Measurements

NASA Technical Reports Server (NTRS)

Chin, Mian; Chu, Allen; Levy, Robert; Remer, Lorraine; Kaufman, Yoram; Dubovik, Oleg; Holben, Brent; Eck, Tom; Anderson, Tad; Quinn, Patricia

2004-01-01

Aerosol climate forcing is one of the largest uncertainties in assessing the anthropogenic impact on the global climate system. This uncertainty arises from the poorly quantified aerosol sources, especially black carbon emissions, our limited knowledge of aerosol mixing state and optical properties, and the consequences of intercontinental transport of aerosols and their precursors. Here we use a global model GOCART to simulate atmospheric aerosols, including sulfate, black carbon, organic carbon, dust, and sea salt, from anthropogenic, .biomass burning, and natural sources. We compare the model calculated aerosol extinction and absorption with those quantities from the ground-based sun photometer measurements from AERON" at several different wavelengths and the field observations from ACE-Asia, and model calculated total aerosol optical depth and fine mode fractions with the MODIS satellite retrieval. We will also estimate the intercontinental transport of pollution and dust aerosols from their source regions to other areas in different seasons.

Organic Functional Group Composition of Submicron Aerosol Particles at Alert, Nunavut, during 2012-2014

NASA Astrophysics Data System (ADS)

Russell, L. M.; Leaitch, W. R.; Liu, J.; Desiree, T. S.; Huang, L.; Sharma, S.; Chivulescu, A.; Veber, D.; Zhang, W.

2016-12-01

Long-term measurements of submicron aerosol particle chemical composition and size distributions are essential for evaluating whether global climate models correctly transport particles from lower latitudes to polar regions, especially in the winter months when satellite retrieval of aerosol properties is limited. In collaboration with ongoing measurements by the Dr. Neil Trivett Global Atmospheric Watch observatory at Alert, Nunavut (82.5°N; elevation 185 m-ASL), we measured the organic functional group composition of submicron aerosol particles sampled from the 10-m inlet from April 2012 to October 2014. The sampling site is approximately 10 km from the Alert station, and vehicle traffic is restricted except when filter sampling is stopped, making the impact of local emissions on submicron particle mass concentrations small. The organic functional group (OFG) composition is measured by Fourier Transform Infrared spectroscopy of samples collected on pre-loaded Teflon filters and stored and shipped frozen to La Jolla, California, for analysis. Samples were collected weekly to complement the twice hourly online measurements of non-refractory organic and inorganic composition by an Aerodyne ACSM. Organic components are shown to contribute a substantial fraction of the measured aerosol submicron mass year round. These measurements illustrate the seasonal contributions to the aerosol size distribution from OFG and illustrate the potential sources of the OFG at this remote site. The three largest OFG sources are transported fossil fuel combustion emissions from lower latitudes, sea spray and other marine particles, and episodic contributions from wildfires, volcanoes, and other high-latitude events. These sources are similar to those identified from earlier OFG measurements at Barrow, Alaska, and during the ICEALOT cruise in the Arctic Ocean.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses.

PubMed

Kahn, Ralph A; Berkoff, Tim A; Brock, Charles; Chen, Gao; Ferrare, Richard A; Ghan, Steven; Hansico, Thomas F; Hegg, Dean A; Martins, J Vanderlei; McNaughton, Cameron S; Murphy, Daniel M; Ogren, John A; Penner, Joyce E; Pilewskie, Peter; Seinfeld, John H; Worsnop, Douglas R

2017-10-01

A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ . The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling , help interrelate remote-sensing, in situ, and modeling aerosol-type definitions , and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable , even if aerosol loading varies.

The short-term association of selected components of fine particulate matter and mortality in the Denver Aerosol Sources and Health (DASH) study

EPA Science Inventory

Associations of short-term exposure to fine particulate matter (PM2.5) with daily mortality may be due to specific PM2.5 chemical components. Objectives: Daily concentrations of PM2.5 chemical species were measured over five consecutive years in Denver, CO to investigate whethe...

Evaluation of Long-term Aerosol Data Records from SeaWiFS over Land and Ocean

NASA Astrophysics Data System (ADS)

Bettenhausen, C.; Hsu, C.; Jeong, M.; Huang, J.

2010-12-01

Deserts around the globe produce mineral dust aerosols that may then be transported over cities, across continents, or even oceans. These aerosols affect the Earth’s energy balance through direct and indirect interactions with incoming solar radiation. They also have a biogeochemical effect as they deliver scarce nutrients to remote ecosystems. Large dust storms regularly disrupt air traffic and are a general nuisance to those living in transport regions. In the past, measuring dust aerosols has been incomplete at best. Satellite retrieval algorithms were limited to oceans or vegetated surfaces and typically neglected desert regions due to their high surface reflectivity in the mid-visible and near-infrared wavelengths, which have been typically used for aerosol retrievals. The Deep Blue aerosol retrieval algorithm was developed to resolve these shortcomings by utilizing the blue channels from instruments such as the Sea-Viewing Wide-Field-of-View Sensor (SeaWiFS) and the Moderate Resolution Imaging Spectroradiometer (MODIS) to infer aerosol properties over these highly reflective surfaces. The surface reflectivity of desert regions is much lower in the blue channels and thus it is easier to separate the aerosol and surface signals than at the longer wavelengths used in other algorithms. More recently, the Deep Blue algorithm has been expanded to retrieve over vegetated surfaces and oceans as well. A single algorithm can now follow dust from source to sink. In this work, we introduce the SeaWiFS instrument and the Deep Blue aerosol retrieval algorithm. We have produced global aerosol data records over land and ocean from 1997 through 2009 using the Deep Blue algorithm and SeaWiFS data. We describe these data records and validate them with data from the Aerosol Robotic Network (AERONET). We also show the relative performance compared to the current MODIS Deep Blue operational aerosol data in desert regions. The current results are encouraging and this dataset will be useful to future studies in understanding the effects of dust aerosols on global processes, long-term aerosol trends, quantifying dust emissions, transport, and inter-annual variability.

Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model

NASA Astrophysics Data System (ADS)

Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.

2015-09-01

We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5-3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-]) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8-28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.

Geochemical, Sulfur Isotopic Characteristics and Source Contributions of Size-Aggregated Aerosols Collected in Baring Head, New Zealand.

NASA Astrophysics Data System (ADS)

Li, J.; Michalski, G. M.; Davy, P.; Harvey, M.; Wilkins, B. P.; Katzman, T. L.

2017-12-01

Sulfate aerosols are critical to the climate, human health, and the hydrological cycle in the atmosphere, yet the sources of sulfate in aerosols are not completely understood. In this work, we evaluated the sources of sulfate in size-aggregated aerosols from the Southern Pacific Ocean and the land of New Zealand using geochemical and isotopic analyses. Aerosols were collected at Baring Head, New Zealand between 6/30/15 to 8/4/16 using two collectors, one only collects Southern Pacific Ocean derived aerosols (open-ocean collector), the other collects aerosols from both the ocean and the land (all-direction collector). Each collector is equipped with two filters to sample size-aggregated aerosols (fine aerosols: <0.5 um and coarse aerosols: 0.5-10 um). Our results show that fine and coarse aerosols show distinctive sulfate sources: sulfate in fine aerosols is a mixture of sea-salt sulfate ( 30%) and Non-Sea-Salt sulfate (NSS-SO42-, 70%), while coarse aerosols are dominated by sea-salt sulfate. However, some NSS-SO42- was also observed in coarse aerosols collected in summer, suggesting the presence of accumulation mode NSS-SO42- aerosols, which is possibly due to high summer biogenic DMS flux. The sources of sulfur in NSS-SO42- could be further determined by their d34S values. DMS emission is likely the sole sulfur source in the open-ocean collector as it shows constant DMS-like d34S signatures (15-18‰) throughout the year. Meanwhile, the d34S of NSS-SO42- in the all-direction collector display a seasonal trend: summer time d34S values are higher and DMS-like (15-18‰), indicating DMS emission is the dominant sulfur source; winter time d34S values are lower ( 6-12‰), therefore the sulfur is likely sourced from both DMS emission and terrestrial S input with low d34S values, such as volcanic activities, fossil fuel and wood burning.

Aerosol pollution potential from major population centers

NASA Astrophysics Data System (ADS)

Kunkel, D.; Tost, H.; Lawrence, M. G.

2012-09-01

Major population centers (MPCs) or mega-cities represent the largest of growing urban agglomerations with major societal and environmental implications. In terms of air quality they are seen as localized but strong emission sources of aerosols and trace gases which in turn affect air pollution levels in the city or in downwind regions. In the state-of-the-art atmospheric chemistry general circulation model EMAC, generic aerosol and gas phase tracers with equal emission source strengths at 46 MPC locations are used to study the balance between local pollution build up and pollution export, either vertically into the upper troposphere or horizontally, but remaining in the lower atmosphere. The insoluble gas phase tracers with fixed lifetimes are transported with the atmospheric circulation, while the aerosol tracers also undergo gravitational sedimentation as well as dry and wet deposition processes. The strength of low-level tracer export depends on the location of the emission source and prevailing meteorology, in particular on atmospheric stability and the height of the boundary layer and the mixing out of this layer. In contrast, vertical transport of tracer mass depends on the tracer's solubility: the more soluble a tracer is the less mass reaches altitudes above five kilometers. Hence, the mass of insoluble gas phase tracer above five kilometers can be up to ten times higher than the hydrophilic aerosol mass from the same source. In the case of aerosol tracers, pollution build up around the source is determined by meteorological factors which have only indirect effects on tracer lifetime, like surface wind, boundary layer height, and turbulent mixing as well as those which affect the lifetime of the tracers such as precipitation. The longer a tracer stays in the atmosphere, the lower is the relative importance of the location of the source to the atmospheric mass and thus the lower is the relative local pollution build up. We further use aerosol deposition fields to estimate regions with high deposition, that is more than 1% or more than 5% of the corresponding tracer emission deposited in this region. In doing so, we find that the high deposition areas are larger for larger aerosols, and these differ less between the MPCs than for smaller aerosols due to faster deposition. Furthermore, cities in regions with high precipitation rates or unfavorable geographic location, e.g. in a basin, suffer most of this high deposition. Most of the high deposition occurs over land, although about 50% of the MPCs are located along coastlines. By folding the aerosol deposition fields with geographical distributions of cropland, pasture, and forest, the impact on different land ecosystems is assessed. In general, forest are exhibited most to deposition from MPCs while pasture land is least affected. Moreover, the impact on humans, measured with a threshold exceedance of pollutant surface mixing ratios, is more dependent on population densities than on the size of the area holding a certain mixing ratio.

Aerosol pollution potential from major population centers

NASA Astrophysics Data System (ADS)

Kunkel, D.; Tost, H.; Lawrence, M. G.

2013-04-01

Major population centers (MPCs), or megacities, represent the largest of growing urban agglomerations with major societal and environmental implications. In terms of air quality, they are seen as localized but strong emission sources of aerosols and trace gases which in turn affect air pollution levels in the city or in downwind regions. In the state-of-the-art atmospheric chemistry general circulation model EMAC, generic aerosol and gas-phase tracers with equal emission source strengths at 46 MPC locations are used to study the balance between local pollution build-up and pollution export, either vertically into the upper troposphere or horizontally in the lower troposphere. The insoluble gas-phase tracers with fixed lifetimes are transported with the atmospheric circulation, while the aerosol tracers also undergo gravitational sedimentation as well as dry and wet deposition processes. The strength of low-level tracer export depends on the location of the emission source and prevailing meteorology, in particular on atmospheric stability and the height of the boundary layer and the mixing out of this layer. In contrast, vertical transport of tracer mass depends on the tracer's solubility: the more soluble a tracer is, the less mass reaches altitudes above five kilometers. Hence, the mass of insoluble gas-phase tracer above five kilometers can be up to ten times higher than the hydrophilic aerosol mass from the same source. In the case of aerosol tracers, pollution build-up around the source is determined by meteorological factors which have only indirect effects on tracer lifetime, like surface wind, boundary layer height, and turbulent mixing, as well as those which affect the lifetime of the tracers such as precipitation. The longer a tracer stays in the atmosphere, the lower is the relative importance of the location of the source to the atmospheric mass, and thus the lower is the relative local pollution build-up. We further use aerosol deposition fields to estimate regions with high deposition, that is more than 1% or more than 5% of the corresponding tracer emission deposited in this region. In doing so, we find that the high deposition areas are larger for aerosols with diameters of 10.0 μm, and these differ less between the MPCs than for aerosols with diameters smaller than 2.5 μm due to faster deposition. Furthermore, cities in regions with high precipitation rates or unfavorable geographic locations, e.g., in a basin, suffer most of this high deposition. Most of the high deposition occurs over land, although about 50% of the MPCs are located along coastlines. By folding the aerosol deposition fields with geographical distributions of cropland, pasture, and forest, the impact on different land ecosystems is assessed. In general, forest is exposed most to deposition from MPCs while pastureland is least affected. Moreover, the impact on humans, measured with a threshold exceedance of pollutant surface mixing ratios, is more dependent on population densities than on the size of the area with a certain mixing ratio.

Urban light pollution - The effect of atmospheric aerosols on astronomical observations at night

NASA Astrophysics Data System (ADS)

Joseph, J. H.; Kaufman, Y. J.; Mekler, Y.

1991-07-01

The transfer of diffuse city light from a localized source through a dust-laden atmosphere with optical depth less than 0.5 has been analyzed in the source-observer plane on the basis of an approximate treatment. The effect on several types of astronomical observation at night has been studied, considering different size distributions and amounts as well as particle shapes of the aerosols. The analysis is made in terms of the signal-to-noise ratios for a given amount of aerosol. The model is applied to conditions at the Wise Astronomical Observatory in the Negev desert, and limiting backgrounds for spectroscopy, photometry, and photography of stars and extended objects have been calculated for a variety of signal-to-noise ratios. Applications to observations with different equipment at various distances from an urban area of any size are possible. Due to the use of signal-to-noise ratios, the conclusions are different for the different experimental techniques used in astronomy.

Urban light pollution - The effect of atmospheric aerosols on astronomical observations at night

NASA Technical Reports Server (NTRS)

Joseph, Joachim H.; Mekler, Yuri; Kaufman, Yoram J.

1991-01-01

The transfer of diffuse city light from a localized source through a dust-laden atmosphere with optical depth less than 0.5 has been analyzed in the source-observer plane on the basis of an approximate treatment. The effect on several types of astronomical observation at night has been studied, considering different size distributions and amounts as well as particle shapes of the aerosols. The analysis is made in terms of the signal-to-noise ratios for a given amount of aerosol. The model is applied to conditions at the Wise Astronomical Observatory in the Negev desert, and limiting backgrounds for spectroscopy, photometry, and photography of stars and extended objects have been calculated for a variety of signal-to-noise ratios. Applications to observations with different equipment at various distances from an urban area of any size are possible. Due to the use of signal-to-noise ratios, the conclusions are different for the different experimental techniques used in astronomy.

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.

Historical (1850-2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols:methodology and application

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

Lamarque, J. F.; Bond, Tami C.; Eyring, Veronika

2010-08-11

We present and discuss a new dataset of gridded emissions covering the historical period (1850-2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report. Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available atmore » this point; 40 regions and 12 sectors were used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, was then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Application of these emissions into two chemistry-climate models is used to test their ability to capture long-term changes in atmospheric ozone, carbon monoxide and aerosols distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations consistently underestimate the carbon monoxide trend, while capturing the long-term trend at the Mace Head station. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates.« less

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

NASA Technical Reports Server (NTRS)

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

Easy Volcanic Aerosol

NASA Astrophysics Data System (ADS)

Toohey, Matthew; Stevens, Bjorn; Schmidt, Hauke; Timmreck, Claudia

2016-04-01

Radiative forcing by stratospheric sulfate aerosol of volcanic origin is one of the strongest drivers of natural climate variability. Transient model simulations attempting to match observed climate variability, such as the CMIP historical simulations, rely on volcanic forcing reconstructions based on observations of a small sample of recent eruptions and coarse proxy data for eruptions before the satellite era. Volcanic forcing data sets used in CMIP5 were provided either in terms of optical properties, or in terms of sulfate aerosol mass, leading to significant inter-model spread in the actual volcanic radiative forcing produced by models and in their resulting climate responses. It remains therefore unclear to what degree inter-model spread in response to volcanic forcing represents model differences or variations in the forcing. In order to isolate model differences, Easy Volcanic Aerosol (EVA) provides an analytic representation of volcanic stratospheric aerosol forcing, based on available observations and aerosol model results, prescribing the aerosol's radiative properties and primary modes of spatial and temporal variability. In contrast to regriddings of observational data, EVA allows for the production of physically consistent forcing for historic and hypothetical eruptions of varying magnitude, source latitude, and season. Within CMIP6, EVA will be used to reconstruct volcanic forcing over the past 2000 years for use in the Paleo-Modeling Intercomparison Project (PMIP), and will provide forcing sets for VolMIP experiments aiming to quantify model uncertainty in the response to volcanic forcing. Here, the functional form of EVA will be introduced, along with illustrative examples including the EVA-based reconstruction of volcanic forcing over the historical period, and that of the 1815 Tambora eruption.

PARAGON: A Systematic, Integrated Approach to Aerosol Observation and Modeling

NASA Technical Reports Server (NTRS)

Diner, David J.; Kahn, Ralph A.; Braverman, Amy J.; Davies, Roger; Martonchik, John V.; Menzies, Robert T.; Ackerman, Thomas P.; Seinfeld, John H.; Anderson, Theodore L.; Charlson, Robert J.;

Overview of the Capstone Depleted Uranium Study of Aerosols from Impact with Armored Vehicles: Test Setup and Aerosol Generation, Characterization, and Application in Assessing Dose and Risk

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

Parkhurst, MaryAnn; Guilmette, Raymond A.

2009-03-01

The Capstone Depleted Uranium (DU) Aerosol Characterization and Risk Assessment Study was conducted to generate data about DU aerosols generated during the perforation of armored combat vehicles with large-caliber DU penetrators, and to apply the data in assessments of human health risks to personnel exposed to these aerosols, primarily through inhalation, during the 1991 Gulf War or in future military operations. The Capstone study consisted of two components: 1) generating, sampling and characterizing DU aerosols by firing at and perforating combat vehicles and 2) applying the source-term quantities and characteristics of the aerosols to the evaluation of doses and risks.more » This paper reviews the background of the study including the bases for the study, previous reviews of DU particles and health assessments from DU used by the U.S. military, the objectives of the study components, the participants and oversight teams, and the types of exposures it was intended to evaluate. It then discusses exposure scenarios used in the dose and risk assessment and provides an overview of how the field tests and dose and risk assessments were conducted.« less

Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

NASA Technical Reports Server (NTRS)

Pueschel , R. F.; Gore, Waren J. Y. (Technical Monitor)

1997-01-01

Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

Novel measurement technologies for ambient and combustion source aerosols

EPA Science Inventory

Thie presentaiton examines the chemical properties of atmospheric and combustion source aerosols. It describes the aerosol chemical fractions and the specific chemical constituents in these aerosols. The presentation will cover (i) the limitatins and benefits of hyphenated chroma...

pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol.

PubMed

Shi, Guoliang; Xu, Jiao; Peng, Xing; Xiao, Zhimei; Chen, Kui; Tian, Yingze; Guan, Xinbei; Feng, Yinchang; Yu, Haofei; Nenes, Athanasios; Russell, Armistead G

2017-04-18

Acidity (pH) plays a key role in the physical and chemical behavior of PM 2.5 . However, understanding of how specific PM sources impact aerosol pH is rarely considered. Performing source apportionment of PM 2.5 allows a unique link of sources pH of aerosol from the polluted city. Hourly water-soluble (WS) ions of PM 2.5 were measured online from December 25th, 2014 to June 19th, 2015 in a northern city in China. Five sources were resolved including secondary nitrate (41%), secondary sulfate (26%), coal combustion (14%), mineral dust (11%), and vehicle exhaust (9%). The influence of source contributions to pH was estimated by ISORROPIA-II. The lowest aerosol pH levels were found at low WS-ion levels and then increased with increasing total ion levels, until high ion levels occur, at which point the aerosol becomes more acidic as both sulfate and nitrate increase. Ammonium levels increased nearly linearly with sulfate and nitrate until approximately 20 μg m -3 , supporting that the ammonium in the aerosol was more limited by thermodynamics than source limitations, and aerosol pH responded more to the contributions of sources such as dust than levels of sulfate. Commonly used pH indicator ratios were not indicative of the pH estimated using the thermodynamic model.

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

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

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

SAM-CAAM: A Concept for Acquiring Systematic Aircraft Measurements to Characterize Aerosol Air Masses

DOE PAGES

Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles; ...

2017-10-30

A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less

Influence of measurement frequency on the evaluation of short-term dose of sub-micrometric particles during indoor and outdoor generation events

NASA Astrophysics Data System (ADS)

Manigrasso, M.; Stabile, L.; Avino, P.; Buonanno, G.

2013-03-01

Aerosol generation events due to combustion processes are characterized by high particle emissions in the nucleation mode range. Such particles are characterized by very short atmospheric lifetimes, leading to rapid decay in time and space from the emission point. Therefore, the deposited fraction of inhaled particles (dose) also changes. In fact, close to the emission source, high short-term peak exposures occur. The related exposure estimates should therefore rely on measurements of aerosol number-size distributions able to track rapid aerosol dynamics. In order to study the influence of the time resolution on such estimates, simultaneous measurements were carried out via Scanning Mobility Particle Sizer (SMPS) and Fast Mobility Particle Sizer (FMPS) spectrometers during particle generation events in both indoor (cooking activities) and outdoor (airstrip and urban street canyons) microenvironments. Aerosol size distributions in the range 16-520 nm were measured by SMPS and FMPS at frequencies of 0.007 s-1 and 1 s-1, respectively. Based on the two datasets, respiratory dosimetry estimates were made on the basis of the deposition model of the International Commission on Radiological Protection. During cooking activities, SMPS measurements give an approximate representation of aerosol temporal evolution. Consequently, the related instant doses can be approximated to a fair degree. In the two outdoor microenvironments considered, aerosol size distributions change rapidly: the FMPS is able to follow such evolution, whereas the SMPS is not. The high short-term peak concentrations, and the consequent respiratory doses, evidenced by FMPS data are hardly described by SMPS, which is unable to track the fast aerosol changes. The health relevance of such short peak exposures has not been thoroughly investigated in scientific literature, therefore, in the present paper highly time-resolved and size-resolved dosimetry estimates were provided in order to deepen this aspect.

Apportionment of urban aerosol sources in Chongqing (China) using synergistic on-line techniques

NASA Astrophysics Data System (ADS)

Chen, Yang; Yang, Fumo

2016-04-01

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Chongqing (southwestern China) have been determined. Aerosol chemical composition analyses were performed using multiple on-line techniques, such as single particle aerosol mass spectrometer (SPAMS) for single particle chemical composition, on-line elemental carbon-organic carbon analyzer (on-line OC-EC), on-line X-ray fluorescence (XRF) for elements, and in-situ Gas and Aerosol Compositions monitor (IGAC) for water-soluble ions in PM2.5. All the datasets from these techniques have been adjusted to a 1-h time resolution for receptor model input. Positive matrix factorization (PMF) has been used for resolving aerosol sources. At least six sources, including domestic coal burning, biomass burning, dust, traffic, industrial and secondary/aged factors have been resolved and interpreted. The synergistic on-line techniques were helpful for identifying aerosol sources more clearly than when only employing the results from the individual techniques. This results are useful for better understanding of aerosol sources and atmospheric processes.

Characteristics and Source Apportionment of Marine Aerosols over East China Sea Using a Source-oriented Chemical Transport Model

NASA Astrophysics Data System (ADS)

Kang, M.; Zhang, H.; Fu, P.

2017-12-01

Marine aerosols exert a strong influence on global climate change and biogeochemical cycling, as oceans cover beyond 70% of the Earth's surface. However, investigations on marine aerosols are relatively limited at present due to the difficulty and inconvenience in sampling marine aerosols as well as their diverse sources. East China Sea (ECS), lying over the broad shelf of the western North Pacific, is adjacent to the Asian mainland, where continental-scale air pollution could impose a heavy load on the marine atmosphere through long-range atmospheric transport. Thus, contributions of major sources to marine aerosols need to be identified for policy makers to develop cost effective control strategies. In this work, a source-oriented version of the Community Multiscale Air Quality (CMAQ) model, which can directly track the contributions from multiple emission sources to marine aerosols, is used to investigate the contributions from power, industry, transportation, residential, biogenic and biomass burning to marine aerosols over the ECS in May and June 2014. The model simulations indicate significant spatial and temporal variations of concentrations as well as the source contributions. This study demonstrates that the Asian continent can greatly affect the marine atmosphere through long-range transport.

Comparative source apportionment of PM10 in Switzerland for 2008/2009 and 1998/1999 by Positive Matrix Factorisation

NASA Astrophysics Data System (ADS)

Gianini, M. F. D.; Fischer, A.; Gehrig, R.; Ulrich, A.; Wichser, A.; Piot, C.; Besombes, J.-L.; Hueglin, C.

2012-07-01

PM10 speciation data from various sites in Switzerland for two time periods (January 1998-March 1999 and August 2008-July 2009) have been analysed for major sources by receptor modelling using Positive Matrix Factorisation (PMF). For the 2008/2009 period, it was found that secondary aerosols (sulphate- and nitrate-rich secondary aerosols, SSA and NSA) are the most abundant components of PM10 at sites north of the Alps. Road traffic and wood combustion were found to be the largest sources of PM10 at these sites. Except at the urban roadside site where road traffic is dominating (40% of PM10 -- including road salt), the annual average contribution of these two sources is of similar importance (17% and 14% of PM10, respectively). At a rural site south of the Alps wood combustion and road traffic contributions to PM10 were higher (31% and 24%, respectively), and the fraction of secondary aerosols lower (29%) than at similar site types north of the Alps. Comparison of PMF analyses for the two time periods (1998/1999 and 2008/2009) revealed decreasing average contributions of road traffic and SSA to PM10 at all sites. This indicates that the measures that were implemented in Switzerland and in neighbouring countries to reduce emissions of sulphur dioxide and PM10 from road traffic were successful. On the other hand, contributions of wood combustion did not change during this ten year period, and the contribution of nitrate-rich secondary aerosols has even increased. It is shown that PMF can be a helpful tool for the assessment of long-term changes of source contributions to ambient particulate matter.

Capstone Depleted Uranium Aerosol Biokinetics, Concentrations, and Doses

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

Guilmette, Raymond A.; Miller, Guthrie; Parkhurst, MaryAnn

2009-02-26

One of the principal goals of the Capstone Depleted Uranium (DU) Aerosol Study was to quantify and characterize DU aerosols generated inside armored vehicles by perforation with a DU penetrator. This study consequently produced a database in which the DU aerosol source terms were specified both physically and chemically for a variety of penetrator-impact geometries and conditions. These source terms were used to calculate radiation doses and uranium concentrations for various scenarios as part of the Capstone DU Human Health Risk Assessment (HHRA). This paper describes the scenario-related biokinetics of uranium, and summarizes intakes, chemical concentrations to the organs, andmore » E(50) and HT(50) for organs and tissues based on exposure scenarios for personnel in vehicles at the time of perforation as well as for first responders. For a given exposure scenario (duration time and breathing rates), the range of DU intakes among the target vehicles and shots was not large, about a factor of 10, with the lowest being from a ventilated operational Abrams tank and the highest being for an unventilated Abrams with DU penetrator perforating DU armor. The ranges of committed effective doses were more scenario-dependent than were intakes. For example, the largest range, a factor of 20, was shown for scenario A, a 1-min exposure, whereas, the range was only a factor of two for the first-responder scenario (E). In general, the committed effective doses were found to be in the tens of mSv. The risks ascribed to these doses are discussed separately.« less

Investigating aerosol properties in Peninsular Malaysia via the synergy of satellite remote sensing and ground-based measurements

NASA Astrophysics Data System (ADS)

Kanniah, Kasturi Devi; Lim, Hui Qi; Kaskaoutis, Dimitris G.; Cracknell, Arthur P.

2014-03-01

Spatio-temporal variation and trends in atmospheric aerosols as well as their impact on solar radiation and clouds are crucial for regional and global climate change assessment. These topics are not so well-documented over Malaysia, the fact that it receives considerable amounts of pollutants from both local and trans-boundary sources. The present study aims to analyse the spatio-temporal evolution and decadal trend of Aerosol Optical Depth (AOD) from Terra and Aqua MODIS sensors, to identify different types and origin of aerosols and explore the link between aerosols and solar radiation. AOD and fine-mode fraction (FMF) products from MODIS, AOD and Ångström Exponent (AE) values from AERONET stations along with ground-based PM10 measurements and solar radiation recordings at selected sites in Peninsular Malaysia are used for this scope. The MODIS AODs exhibit a wide spatio-temporal variation over Peninsular Malaysia, while Aqua AOD is consistently lower than that from Terra. The AOD shows a neutral-to-declining trend during the 2000s (Terra satellite), while that from Aqua exhibits an increasing trend (~ 0.01 per year). AERONET AODs exhibit either insignificant diurnal variation or higher values during the afternoon, while their short-term availability does not allow for a trend analysis. Moreover, the PM10 concentrations exhibit a general increasing trend over the examined locations. The sources and destination of aerosols are identified via the HYSPLIT trajectory model, revealing that aerosols during the dry season (June to September) are mainly originated from the west and southwest (Sumatra, Indonesia), while in the wet season (November to March) they are mostly associated with the northeast monsoon winds from the southern China Sea. Different aerosol types are identified via the relationship of AOD with FMF, revealing that the urban and biomass-burning aerosols are the most abundant over the region contributing to a significant reduction (~- 0.21 MJ m- 2) of the solar radiation.

Substantial large-scale feedbacks between natural aerosols and climate

NASA Astrophysics Data System (ADS)

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

2018-01-01

The terrestrial biosphere is an important source of natural aerosol. Natural aerosol sources alter climate, but are also strongly controlled by climate, leading to the potential for natural aerosol-climate feedbacks. Here we use a global aerosol model to make an assessment of terrestrial natural aerosol-climate feedbacks, constrained by observations of aerosol number. We find that warmer-than-average temperatures are associated with higher-than-average number concentrations of large (>100 nm diameter) particles, particularly during the summer. This relationship is well reproduced by the model and is driven by both meteorological variability and variability in natural aerosol from biogenic and landscape fire sources. We find that the calculated extratropical annual mean aerosol radiative effect (both direct and indirect) is negatively related to the observed global temperature anomaly, and is driven by a positive relationship between temperature and the emission of natural aerosol. The extratropical aerosol-climate feedback is estimated to be -0.14 W m-2 K-1 for landscape fire aerosol, greater than the -0.03 W m-2 K-1 estimated for biogenic secondary organic aerosol. These feedbacks are comparable in magnitude to other biogeochemical feedbacks, highlighting the need for natural aerosol feedbacks to be included in climate simulations.

An Investigation of the Radiative Effects and Climate Feedbacks of Sea Ice Sources of Sea Salt Aerosol

NASA Astrophysics Data System (ADS)

Horowitz, H. M.; Alexander, B.; Bitz, C. M.; Jaegle, L.; Burrows, S. M.

2017-12-01

In polar regions, sea ice is a major source of sea salt aerosol through lofting of saline frost flowers or blowing saline snow from the sea ice surface. Under continued climate warming, an ice-free Arctic in summer with only first-year, more saline sea ice in winter is likely. Previous work has focused on climate impacts in summer from increasing open ocean sea salt aerosol emissions following complete sea ice loss in the Arctic, with conflicting results suggesting no net radiative effect or a negative climate feedback resulting from a strong first aerosol indirect effect. However, the radiative forcing from changes to the sea ice sources of sea salt aerosol in a future, warmer climate has not previously been explored. Understanding how sea ice loss affects the Arctic climate system requires investigating both open-ocean and sea ice sources of sea-salt aerosol and their potential interactions. Here, we implement a blowing snow source of sea salt aerosol into the Community Earth System Model (CESM) dynamically coupled to the latest version of the Los Alamos sea ice model (CICE5). Snow salinity is a key parameter affecting blowing snow sea salt emissions and previous work has assumed constant regional snow salinity over sea ice. We develop a parameterization for dynamic snow salinity in the sea ice model and examine how its spatial and temporal variability impacts the production of sea salt from blowing snow. We evaluate and constrain the snow salinity parameterization using available observations. Present-day coupled CESM-CICE5 simulations of sea salt aerosol concentrations including sea ice sources are evaluated against in situ and satellite (CALIOP) observations in polar regions. We then quantify the present-day radiative forcing from the addition of blowing snow sea salt aerosol with respect to aerosol-radiation and aerosol-cloud interactions. The relative contributions of sea ice vs. open ocean sources of sea salt aerosol to radiative forcing in polar regions is discussed.

Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

PubMed

Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

2014-09-15

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic aerosol factor (AMS_PMF_COA) to oxidized organic aerosol, chloride and locally produced nitrate, indicating that AMS_PMF_COA cannot be attributed to primary cooking emissions only. Overall, there are clear benefits from factor analysis applied to results obtained from multiple techniques, which allows better association of aerosols with sources and atmospheric processes. Copyright © 2014 Elsevier B.V. All rights reserved.

MACv2-SP: a parameterization of anthropogenic aerosol optical properties and an associated Twomey effect for use in CMIP6

NASA Astrophysics Data System (ADS)

Stevens, Bjorn; Fiedler, Stephanie; Kinne, Stefan; Peters, Karsten; Rast, Sebastian; Müsse, Jobst; Smith, Steven J.; Mauritsen, Thorsten

2017-02-01

A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shape of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850-2016) are derived by scaling the plumes with associated national emission sources of SO2 and NH3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be -0.6 and -0.5 W m-2, respectively. Forcing from aerosol-cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.

Using long-term ground-based HSRL and geostationary observations in combination with model re-analysis to help disentangle local and long-range transported aerosols in Seoul, South Korea

NASA Astrophysics Data System (ADS)

Phillips, C.; Holz, R.; Eloranta, E. W.; Reid, J. S.; Kim, S. W.; Kuehn, R.; Marais, W.

2017-12-01

The University of Wisconsin High Spectral Resolution Lidar (HSRL) has been continuously operating at Seoul National University as part of the Korea-United States Air Quality Study (KORUS-AQ). The instrument was installed in March of 2016 and continues to operate as of August 2017, providing a truly unique data set to monitor aerosol and cloud properties. With its capability to separate the molecular and particulate scattering, the HSRL is able to detect extremely thin aerosol layers with sub-molecular scattering sensitivity. The system deployed in Seoul has depolarization measurements at 532 nm as well as a near IR channel at 1064 nm providing discrimination between dust, smoke, pollution, water clouds, and ice clouds. As will be presented, these capabilities can be used to produce three channel combined RGB images that provide visualization of small changes in the aerosol properties. A primary motivation of KORUS-AQ was to determine the relative effects of transported pollution and local pollution on air quality in Seoul. We hypothesize that HSRL-based image analysis algorithms combined with satellite and model re-analysis has the potential to identify cases when remote sources of aerosols and pollution are advected into the boundary layer with impacts to the surface air quality. To facilitate this research we have developed the capability to combine ten-minute geostationary imagery from Himawari-8, nearby radiosondes, model output, surface PM measurements, and AERONET data over the HSRL site. On a case-by-case basis, it is possible to separate layers of aerosols with different scattering properties using these tools. Additionally, a preliminary year-long aerosol climatology with integrated geo-stationary retrievals and modeling data will be presented. The focus is on investigating correlations between the HSRL aerosol measurements (depolarization, color ratio, extinction, and lidar ratio) with the model output and aerosol sources. This analysis will use recently developed algorithms that automate the HSRL cloud and aerosol masking, providing the capability to characterize the seasonal changes in aerosol radiative properties and supplement the month-long field campaign with almost two years of continuous HSRL observations.

Marine CCN Activation: A Battle Between Primary and Secondary Sources

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Impact of Aerosols on Convective Clouds and Precipitation

NASA Technical Reports Server (NTRS)

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

2012-01-01

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

Long-term measurements of aerosols and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian Taiga

NASA Astrophysics Data System (ADS)

Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A. V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M. O.

2013-07-01

Siberia is one of few background regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September~2006 and December 2010 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 90° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, like equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted and near-pristine air masses and characterize them separately. Depending on the season, 15-47% of the sampling time at ZOTTO was representative of a clean atmosphere. The summer pristine data indicates that primary biogenic and/or secondary organic aerosol formation are quite strong particle sources in the Siberian Taiga. The summer seasons 2007-2008 are dominated by an Aitken mode of 80 nm size, whereas the summer 2009 with prevailing easterly winds produced aerosols in the accumulation mode around 200 nm size. We found these differences mainly related to air temperature, in parallel with production rates of biogenic volatile organic compounds (VOC). In winter, the footprint and aerosol size distribution (with a peak at 160 nm) of the clean background air are characteristic for aged aerosols from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from heating. The wintertime polluted air originates from the large cities to the south and southwest of the site; these aerosols have a dominant mode around 100 nm, and the Δ BCe/Δ CO ratio of 7-11 ng m-3 ppb-1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution aerosols at ZOTTO, while only 12% of the polluted events are classified as biomass burning dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different Δ BCe/Δ CO ratios from different fire types, with the agricultural fires in April 2008 yielding a very high ratio of 21 ng m-3 ppb-1. Overall, we find that anthropogenic sources dominate the aerosol population at our site most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only episodically in the growing season.

Apportionment of Primary and Secondary Organic Aerosols in Southern California During the 2005 Study of Organic Aerosols in Riverside (SOAR-1)

EPA Science Inventory

Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionment techniques.

Spectroscopic characterization of Antarctic marine aerosol

NASA Astrophysics Data System (ADS)

Paglione, Marco; Zanca, Nicola; Rinaldi, Matteo; Dall'osto, Manuel; Simo, Rafel; Facchini, Maria Cristina; Decesari, Stefano

2017-04-01

Marine aerosol constitutes an important and not thoroughly investigated natural aerosol system. In particular, the poor knowledge of the physical-chemical properties of primary (sea-spray) and secondary particles, especially over biologically active seawaters, affects the current capability of modeling the effect of marine aerosol on climate (O'Dowd et al., 2004). In polar regions, surface seawater composition and its exchanges with the atmosphere is complicated also by the presence of sea-ice and of the variety of micro-organisms (viruses, prokaryotes and microalgae) living within it (Levasseur,2013). In the framework of the Spanish project PEGASO (Plankton-derived Emission of Gases and Aerosols in the Southern Ocean) submicron aerosol samples were collected during a 6 weeks long oceanographic cruise (2nd January 2015 - 11th February 2015) conducted in the regions of Antarctic Peninsula, South Orkney and South Georgia Islands, an area of the Southern Ocean characterized every summer by both large patches of productive waters (phytoplankton blooms) and sea-ice cover. The collected samples were analyzed by means of proton-Nuclear Magnetic Resonance (H-NMR) spectroscopy with aim of organic compounds characterization in terms of functional groups and specific molecular tracers identification (Decesari et al., 2011). H-NMR spectral features resulted quite variable among the different samples both in terms of relative abundance of main functional groups and in terms of presence of specific compounds. In all the samples were found biogenic markers, like low-molecular-weight alkyl-amines and methanesulphonate (MSA), of secondary origin (formed by the condensation of vapors onto particles). Resonance signals of other aliphatic compounds of possible primary origin, like lipids, aminoacids (e.g. alanine) and sugars (e.g. sucrose) are present in variable concentrations in the samples. A hierarchical cluster analysis applied on the NMR spectra allowed to identify similarities in the samples collected close the Weddell-Sea area, showing an enhancement of biogenic alkyl-amines (including mono-, di- and tri-methylamine) and MSA and suggesting a common source probably linked with the sea-ice cover dominating that region. As such, our results point to secondary organic aerosol (SOA) sources from precursors emitted by sea ice regions around Antarctica and call for better representation of the sea ice-ocean-atmosphere biogeochemistry in Earth system models. References: Decesari, S. et al., JGR-Atmospheres 116 (2011). Levasseur, M., Nature Geoscience, Vol. 6, September (2013). O'Dowd, C. et al., Nature 431, 676-680 (2004). Acknowledgments: The cruise was funded by the Spanish Ministry of Economy through projects PEGASO (CTM2012-37615) and Bio-Nuc (CGL2013-49020-R), and by the EU though the FP7-PEOPLE-2013-IOF program (Project number 624680, MANU - Marine Aerosol NUcleations).

The impact of Mount Etna's sulphur emissions to the atmospheric composition, aerosol properties and radiative transfer in the central Mediterranean: 14 years of statistic analysis using observations and Lagrangian modelling

NASA Astrophysics Data System (ADS)

Sellitto, Pasquale; Zanetel, Claudia; di Sarra, Alcide; Salerno, Giuseppe; Tapparo, Andrea; Briole, Pierre; Legras, Bernard

2016-04-01

Volcanic eruptions influence tropospheric and stratospheric composition, the Earth's radiation budget from the regional to the global scale, and then the Earth's climate. While the impact of the strong explosive eruptions reaching the stratosphere is relatively well known, the influence of the more frequent weak volcanic activity, including passive degassing, on the tropospheric aerosol properties and on the radiation budget is still largely unknown. Most of the radiative effects of moderate eruptions are associated with changes of the aerosol size distribution, composition, and shape. Emission of primary particles, mainly ash, and secondary aerosols through gas-to-particle conversion of volatile sulphur compounds contribute to affect the aerosol properties. Mount Etna's continuous degassing and episodic explosive eruptions is an important source of particles and gases for the Mediterranean atmosphere, with, e.g., ten times larger emissions of volatile sulphur compounds than the anthropogenic sulphur emissions in the Mediterranean area. The impact of Mount Etna on the atmospheric composition, the aerosol chemical, microphysical and optical properties, the clouds occurrence and properties, the radiative balance and the regional climate in the Mediterranean are not known and probably underestimated. In this contribution, the downwind impact of Mount Etna's sulphur emissions in the central Mediterranean is estimated over the period 2000-2013 using long-term series of sulphur dioxide column and Ångströms exponent observations at the the ENEA (Ente Nazionale per l'Energia e l'Ambiente) Station for Climate Observations on the small island of Lampedusa (35.5°N, 12.6°E). These observations are linked to the information on the volcanic source, in terms of 1) the local dynamics, using a long series of trajectories and plume dispersion information obtained with the FLEXPART Lagrangian mode, and 2) the emission strength, using the long-term series of daily sulphur dioxide emission rates measured at Mount Etna with the FLAME network (a near-crater network of ground-based ultraviolet spectrophotometers, operated by the INGV - Istituto Nazionale di Geofisica e Vulcanologia). This statistical analysis has allowed, for the first time, the characterization of the impact of Mount Etna's sulphur emissions to the sulfur dioxide distributions and the aerosol microphysical/optical characterisation in the central Mediterranean. This impact is here presented and critically discussed. Finally, the radiative forcing of simulated Mount Etna's plumes is estimated for different optical properties and vertical distributions of the volcanic aerosols. We have found that the radiative forcing efficiency of Mount Etna's plumes can be as important as the efficiency related to the most frequent Saharan dust or pollution transport events, in the same area.

Challenges to producing a long-term stratospheric aerosol climatology for chemistry and climate

NASA Astrophysics Data System (ADS)

Thomason, Larry; Vernier, Jean-Paul; Bourassa, Adam; Rieger, Landon; Luo, Beiping; Peter, Thomas; Arfeuille, Florian

2016-04-01

Stratospheric aerosol data sets are key inputs for climate models (GCMs, CCMs) particularly for understanding the role of volcanoes on climate and as a surrogate for understanding the potential of human-derived stratospheric aerosol as mitigation for global warming. In addition to supporting activities of individual climate models, the data sets also act as a historical input to the activities of SPARC's Chemistry-Climate Model Initiative (CCMI) and the World Climate Research Programme's Coupled Model Intercomparison Project (CMIP). One such data set was produced in 2004 as a part of the SPARC Assessment of Stratospheric Aerosol Properties (ASAP), extending from 1979 and 2004. It was primarily constructed from the Stratospheric Aerosol and Gas Experiment series of instruments but supplemented by data from other space-based sources and a number of ground-based and airborne instruments. Updates to this data set have expanded the timeframe to span from 1850 through 2014 through the inclusion of data from additional sources, such as photometer data and ice core analyses. Fundamentally, there are limitations to the reliability of the optical properties of aerosol inferred from even the most complete single instrument data sets. At the same time, the heterogeneous nature of the underlying data to this historical data set produces considerable challenges to the production of a climate data set which is both homogeneous and reliable throughout its timespan. In this presentation, we will discuss the impact of this heterogeneity showing specific examples such as the SAGE II to OSIRIS/CALIPSO transition in 2005. Potential solutions to these issues will also be discussed.

Long-term Satellite Observations of Cloud and Aerosol Radiative Effects Using the (A)ATSR Satellite Data Record

NASA Astrophysics Data System (ADS)

Christensen, M.; McGarragh, G.; Thomas, G.; Povey, A.; Proud, S.; Poulsen, C. A.; Grainger, R. G.

2016-12-01

Radiative forcing by clouds, aerosols, and their interactions constitute some of the largest sources of uncertainties in the climate system (Chapter 7 IPCC, 2013). It is essential to understand the past through examination of long-term satellite observation records to provide insight into the uncertainty characteristics of these radiative forcers. As part of the ESA CCI (Climate Change Initiative) we have recently implemented a broadband radiative flux algorithm (known as BUGSrad) into the Optimal Retrieval for Aerosol and Cloud (ORAC) scheme. ORAC achieves radiative consistency of its aerosol and cloud products through an optimal estimation scheme and is highly versatile, enabling retrievals for numerous satellite sensors: ATSR, MODIS, VIIRS, AVHRR, SLSTR, SEVIRI, and AHI. An analysis of the 17-year well-calibrated Along Track Scanning Radiometer (ATSR) data is used to quantify trends in cloud and aerosol radiative effects over a wide range of spatiotemporal scales. The El Niño Southern Oscillation stands out as the largest contributing mode of variability to the radiative energy balance (long wave and shortwave fluxes) at the top of the atmosphere. Furthermore, trends in planetary albedo show substantial decreases across the Arctic Ocean (likely due to the melting of sea ice and snow) and modest increases in regions dominated by stratocumulus (e.g., off the coast of California) through notable increases in cloud fraction and liquid water path. Finally, changes in volcanic activity and biomass burning aerosol over this period show sizeable radiative forcing impacts at local-scales. We will demonstrate that radiative forcing from aerosols and clouds have played a significant role in the identified key climate processes using 17 years of satellite observational data.

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

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

Zhang, Qi

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

Global View of Aerosol Vertical Distributions from CALIPSO Lidar Measurements and GOCART Simulations: Regional and Seasonal Variations

NASA Technical Reports Server (NTRS)

Yu, Hongbin; Chin, Mian; Winker, David M.; Omar, Ali H.; Liu, Zhaoyan; Kittaka, Chieko; Diehl, Thomas

2010-01-01

This study examines seasonal variations of the vertical distribution of aerosols through a statistical analysis of the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) lidar observations from June 2006 to November 2007. A data-screening scheme is developed to attain good quality data in cloud-free conditions, and the polarization measurement is used to separate dust from non-dust aerosol. The CALIPSO aerosol observations are compared with aerosol simulations from the Goddard Chemistry Aerosol Radiation Transport (GOCART) model and aerosol optical depth (AOD) measurements from the MODerate resolution Imaging Spectroradiometer (MODIS). The CALIPSO observations of geographical patterns and seasonal variations of AOD are generally consistent with GOCART simulations and MODIS retrievals especially near source regions, while the magnitude of AOD shows large discrepancies in most regions. Both the CALIPSO observation and GOCART model show that the aerosol extinction scale heights in major dust and smoke source regions are generally higher than that in industrial pollution source regions. The CALIPSO aerosol lidar ratio also generally agrees with GOCART model within 30% on regional scales. Major differences between satellite observations and GOCART model are identified, including (1) an underestimate of aerosol extinction by GOCART over the Indian sub-continent, (2) much larger aerosol extinction calculated by GOCART than observed by CALIPSO in dust source regions, (3) much weaker in magnitude and more concentrated aerosol in the lower atmosphere in CALIPSO observation than GOCART model over transported areas in midlatitudes, and (4) consistently lower aerosol scale height by CALIPSO observation than GOCART model. Possible factors contributing to these differences are discussed.

Incorporation of dosimetry in the derivation of reference concentrations for ambient or workplace air: a conceptual approach.

PubMed

Oller, Adriana R; Oberdörster, Günter

2016-09-01

Dosimetric models are essential tools to refine inhalation risk assessments based on local respiratory effects. Dosimetric adjustments to account for differences in aerosol particle size and respiratory tract deposition and/or clearance among rodents, workers, and the general public can be applied to experimentally- and epidemiologically-determined points of departure (PODs) to calculate size-selected (e.g., PM 10 , inhalable aerosol fraction, respirable aerosol fraction) equivalent concentrations (e.g., HEC or Human Equivalent Concentration; REC or Rodent Equivalent Concentration). A modified POD (e.g., HEC) can then feed into existing frameworks for the derivation of occupational or ambient air concentration limits or reference concentrations. HECs that are expressed in terms of aerosol particle sizes experienced by humans but are derived from animal studies allow proper comparison of exposure levels and associated health effects in animals and humans. This can inform differences in responsiveness between animals and humans, based on the same deposited or retained doses and can also allow the use of both data sources in an integrated weight of evidence approach for hazard and risk assessment purposes. Whenever possible, default values should be replaced by substance-specific and target population-specific parameters. Assumptions and sources of uncertainty need to be clearly reported.

Incorporation of dosimetry in the derivation of reference concentrations for ambient or workplace air: a conceptual approach

PubMed Central

Oberdörster, Günter

2016-01-01

Dosimetric models are essential tools to refine inhalation risk assessments based on local respiratory effects. Dosimetric adjustments to account for differences in aerosol particle size and respiratory tract deposition and/or clearance among rodents, workers, and the general public can be applied to experimentally- and epidemiologically-determined points of departure (PODs) to calculate size-selected (e.g., PM10, inhalable aerosol fraction, respirable aerosol fraction) equivalent concentrations (e.g., HEC or Human Equivalent Concentration; REC or Rodent Equivalent Concentration). A modified POD (e.g., HEC) can then feed into existing frameworks for the derivation of occupational or ambient air concentration limits or reference concentrations. HECs that are expressed in terms of aerosol particle sizes experienced by humans but are derived from animal studies allow proper comparison of exposure levels and associated health effects in animals and humans. This can inform differences in responsiveness between animals and humans, based on the same deposited or retained doses and can also allow the use of both data sources in an integrated weight of evidence approach for hazard and risk assessment purposes. Whenever possible, default values should be replaced by substance-specific and target population-specific parameters. Assumptions and sources of uncertainty need to be clearly reported. PMID:27721518

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

NASA Astrophysics Data System (ADS)

Turekian, Vaughan Charles

2000-12-01

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

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

NASA Technical Reports Server (NTRS)

Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic matter, and dust found for the ACE Asia aerosol are comparable to values estimated for ACE 1, Aerosols99, and INDOEX. Unique to the ACE Asia aerosol was the large mass fractions of dust, the dominance of dust in controlling the aerosol optical properties, and the interaction of dust with soot aerosol.

Long term atmospheric aerosol characterization in the Amazon Basin

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Gerab, Fábio; Yamasoe, Marcia A.

This chapter presents a characterization of atmospheric aerosols collected in different places in the Amazon Basin. Both the biogenic aerosol emission from the forest and the particulate material which is emitted to the atmosphere due to the large scale man-made burns during the dry season were studied. The samples were collected during a three year period at three different locations in the Amazon (Cuiabá, Alta Floresta and Serra do Navio), using stacked filter units. Aerosol samples were also collected directly over fires of cerrado vegetation and tropical primary forest burns The samples were analyzed using several techniques for a number of elements. Gravimetric analyses were used to determine the total atmospheric aerosol concentration. Multivariate statistical analysis was used in order to identify and characterize the sources of the atmospheric aerosol present in the sampled regions. Cerrado burning emissions were enriched compared to forest ones, specially for Cl, K and Zn. High atmospheric aerosol concentrations were observed in large amazonian areas due to emissions from man-made burns in the period from June to September. The emissions from burns dominate the fine fraction of the atmospheric aerosol with characteristic high contents of black carbon, S and K. Aerosols emitted in biomass burning process are correlated to the increase in the aerosol optical thickness of the atmosphere during the Amazonian dry season. The Serra do Navio aerosol is characterized by biogenic emissions with strong marine influence. The presence of trace elements characteristic of soil particulate associated with this marine contribution indicates the existence of aerosol transport from Africa to South America. Similar composition characteristics were observed in the biogenic emission aerosols from Serra do Navio and Alta Floresta.

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

NASA Astrophysics Data System (ADS)

Kumar, Sudhanshu

2012-07-01

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

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.

The source identification of ambient aerosols in Beijing, China by multivariate analysis coupled with {sup 14}C tracer

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

Xiaoyan Tang; Min Shao; Yuanhang Zhang

1996-12-31

Ambient aerosol is one of most important pollutants in China. This paper showed the results of aerosol sources of Beijing area revealed by combination of multivariate analysis models and 14C tracer measured on Accelerator Mass Spectrometry (AMS). The results indicated that the mass concentration of particulate (<100 (M)) didn`t increase rapidly, compared with economic development in Beijing city. The multivariate analysis showed that the predominant source was soil dust which contributed more than 50% to atmospheric particles. However, it would be a risk to conclude that the aerosol pollution from anthropogenic sources was less important in Beijing city based onmore » above phenomenon. Due to lack of reliable tracers, it was very hard to distinguish coal burning from soil source. Thus, it was suspected that the soil source above might be the mixture of soil dust and coal burning. The 14C measurement showed that carbonaceous species of aerosol had quite different emission sources. For carbonaceous aerosols in Beijing, the contribution from fossil fuel to ambient particles was nearly 2/3, as the man-made activities ( coal-burning, etc.) increased, the fossil part would contribute more to atmospheric carbonaceous particles. For example, in downtown Beijing at space-heating seasons, the fossil fuel even contributed more than 95% to carbonaceous particles, which would be potential harmful to population. By using multivariate analysis together with 14C data, two important sources of aerosols in Beijing (soil and coal) combustion were more reliably distinguished, which was critical important for the assessment of aerosol problem in China.« less

A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

NASA Technical Reports Server (NTRS)

Liu, Hongyu; Moore, Richard; Hostetler, Chris A.; Ferrare, Richard Anthony; Fairlie, Thomas Duncan; Hu, Youngxiang; Chen, Gao; Hair, Johnathan W.; Johnson, Matthew S.

2016-01-01

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

Surface-based observations of volcanic emissions to the stratosphere

NASA Astrophysics Data System (ADS)

Hofmann, Dave; Barnes, John; Dutton, Ellsworth; Deshler, Terry; Jäger, Horst; Keen, Richard; Osborn, Mary

Long-term, surface-based observations of the stratospheric aerosol layer are presented and compared. These include three LIDAR aerosol backscatter measurements, at Mauna Loa Observatory (Hawaii), Langley Research Center (Virginia), and Garmisch-Partenkirchen (Germany); balloonborne in situ particle concentration measurements at Laramie, Wyoming, solar visible transmission measurements at Mauna Loa Observatory; aerosol optical depth measurements at South Pole Station and Mauna Loa Observatory; and lunar eclipse optical depth determinations, which is a globally integrating technique. Surface-based measurements have provided a useful historical record of volcanic effects on the stratospheric aerosol and the agreement between the various techniques is very good. However, some uncertainties exist when the stratosphere is relatively free of volcanic aerosol and some of the techniques are not able to easily resolve the very small amount of aerosol from natural and/or anthropogenic sources. The lunar eclipse data, which go back to the late 1800s, suggest that the Pinatubo eruption in 1991 probably perturbed the stratospheric aerosol layer at least as much as that of Krakatau in 1883. This is an important observation as it is one of the few ways to accurately compare the stratospheric effects of eruptions prior to modern measurements that began in the late 1950s. At the time of this writing (September 2002) the stratosphere appears to be at background with the lowest level of aerosol observed since the layer was discovered in 1959.

Cloud-Aerosol Interaction and Its Impact on the Onset of the East Asian Summer Monsoon

NASA Technical Reports Server (NTRS)

Kim, Kyu-Myong; Lau, William K.-M.; Hsu, N. Christina; Tsay, Si-Chee

2004-01-01

Effect of aerosols from biomass burning on the early development of East Asian monsoon is investigated using various satellites and in situ observations including TOMS Aerosol Index (AI). GPCP precipitation, ISCCP cloud cover, and GISS surface air temperature. Based on TRMM fire produce and mean winds fields at 85Omb. we identified the source and interaction regions of aerosols and investigated aerosol-cloud-precipitation characteristics in those regions. During March-April, northern Thailand, Myanmar. and Laos are major source of smoke from the combustion of agricultural waste. Excessive smoke. represented by high AI, is observed especially during dry and cloud-free year. On the other hand. there is no ground source of smoke in the interaction region. The most of aerosols in this area are believed to be transported from the source region. AI is appeared to be correlated with more clouds and less precipitation in interaction region. It suggests that the aerosol-cloud interaction can alter the distribution of cloud and the characteristics of regional hydrology. Aerosol-induced changes in atmospheric stability and associated circulation turns out to be very important to pre-monsoon rainfall pattern in southern China. Prolonged biomass burning is especially effective in changing rainfall pattern during April and May. Results suggest that excessive aerosol transported from source region may intensify pre-monsoon rain band over central China in May and lead to early monsoon onset.

MACv2-SP: a parameterization of anthropogenic aerosol optical properties and an associated Twomey effect for use in CMIP6

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

Stevens, Bjorn; Fiedler, Stephanie; Kinne, Stefan

A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shapemore » of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850–2016) are derived by scaling the plumes with associated national emission sources of SO 2 and NH 3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be -0.6 and -0.5 W m -2, respectively. Forcing from aerosol–cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.« less

Physico-chemical characterization of African urban aerosols (Abidjan in Cote d'Ivoire and Cotonou in Benin) and their toxic effects in human bronchial epithelial cells during the dry season 2016.

NASA Astrophysics Data System (ADS)

Adon, Jacques; Liousse, Cathy; Yoboue, Veronique; Baeza, Armelle; Akpo, Aristide; Bahino, Julien; Chiron, Christelle; Galy-Lacaux, Corinne; Keita, Sékou

2017-04-01

This study is a contribution to the WP2-DACCIWA program with the aim to characterize particulate pollution on domestic fire site, traffic sites and waste burning site of two West-African capitals (Abidjan, Cote d'Ivoire and Cotonou, Benin) and to study aerosol biological impacts on lung inflammation. Such an impact is still largely unknown, especially for the particles emitted by intense African traffic sources and domestic fires. In this context, fundamental research of this study is centered on the following key scientific question: what is the link between aerosol size differentiated composition and inflammation markers for the main combustion sources prevailing in South West Africa during dry and wet seasons? To tackle this question, intensive campaigns in Abidjan and Cotonou have been conducted in July 2015, January and July 2016, and January 2017. In this paper, we will present our first results for the campaign of January 2016. In terms of aerosol size differentiated composition, main aerosol components (mass, black carbon, organic carbon, water soluble particles ...) were measured. We may notice that PM measured for all the sites is generally higher than WHO norms. Organic carbon and dust particles are the two more important contributors for the ultra-fine and fine particle sizes with more organic carbon in Abidjan and dust particles in Cotonou respectively. In terms of in vitro biological studies on sampled aerosols on these sites, size-fractionated PM from the different sampling sites were compared for their ability to induce a proinflammatory response characterized by the release of the cytokine IL-6 by human bronchial epithelial cells. PM from waste burning site did not induce significant IL-6 release whatever the size fraction whereas PM from domestic fire were the most reactive especially the ultra-fine fraction. Ultra-fine particles from traffic (Abidjan and Cotonou) always induced a dose-dependent IL-6 release. A tentative cross-analysis between physico-chemical and toxicological results will be proposed.

Distribution of Aerosols in the Arctic as Observed by CALIOP

NASA Astrophysics Data System (ADS)

Winker, D.; Kittaka, C.

2007-12-01

The Arctic climate is now recognized to be uniquely sensitive to atmospheric perturbations. Pollution aerosols and smoke from boreal fires have potentially important impacts on Arctic climate but there are many uncertainties. Aerosol in the Arctic, generally referred to as "Arctic haze", has been studied with great interest for over thirty years. Much has been learned about the composition and sources of the haze yet our knowledge is largely based on long term measurements at a very few widely dispersed sites, augmented by modeling activities and occasional field campaigns. Transport pathways from source regions into the Arctic are not well understood. Emission patterns have changed over the last several decades, but the impact of this on concentrations and distribution of Arctic haze are understood only in the crudest sense. Due to poor lighting conditions, extended periods of darkness, and surfaces covered by snow and ice, satellite sensors have been unable to provide much information on Arctic haze to date. The CALIPSO satellite carries CALIOP, a two-wavelength polarization lidar, optimized for profiling clouds and aerosols. CALIOP has been acquiring global observations since June 2006 and provides our first opportunity to observe the distribution and seasonal variation of aerosol in the Arctic. The Arctic is characterized by the prevalence of optically thin ice clouds and clouds composed of supercooled water, often occurring in the same atmospheric column along with aerosol. CALIOP depolarization signals are used to discriminate Arctic haze from optically thin cirrus and diamond dust. Two-wavelength returns aid in the discrimination of aerosol and optically thin water cloud. Results of initial analyses of CALIOP aerosol observations in the Arctic will be presented. This work is a preliminary analysis in support of the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign planned for April 2008.

A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

NASA Astrophysics Data System (ADS)

Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

2017-08-01

To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions. Secondary inorganic aerosols accounted for about 60 % of aerosol extinction coefficient (bext) at RH greater than 70 %. The mass scattering efficiency (MSE) of PM2. 5 ranged from 3.0 to 5.0 m2 g-1 for aerosols produced from anthropogenic emissions and from 0.7 to 1.0 m2 g-1 for natural dust aerosols. The mass absorption efficiency (MAE) of EC ranged from 6.5 to 12.4 m2 g-1 in urban environments, but the MAE of water-soluble organic carbon was only 0.05 to 0.11 m2 g-1. Historical emission control policies in China and their effectiveness were discussed based on available chemically resolved PM2. 5 data, which provides the much needed knowledge for guiding future studies and emissions policies.

Interrelationships Between Aerosol Characteristics and Light Scattering During Late-winter in a Eastern Mediterranean Arid Environment

NASA Technical Reports Server (NTRS)

Ichoku, C.; Andreae, M. O.; Meixner, F. X.; Schebeske, G.; Formenti, P.; Maenhaut, W.; Cafmeyer, J.; Ptasinski, J.; Karnieli, A.; Orlovsky, L.

1999-01-01

An intensive field campaign involving measurement of various aerosol physical, chemical, and radiative properties was conducted at Sde Boker in the Negev Desert of Israel, from 18 February to 15 March 1997. Nephelometer measurements gave average background scattering coefficient values of about 25 M/m at 550 nm wavelength, but strong dust events caused the value of this parameter to rise up to about 800 M/m Backscattering fractions did not depend on aerosol loading, and generally fell in the range of 0.1 to 0.25, comparable to values reported for marine and Arctic environments. Chemical analysis of the aerosol revealed that, in the coarse size range (2 - 10 micrometer equivalent aerodynamic diameter (EAD)), calcium (Ca) was by far the most abundant element followed by silicon (Si), both of which are indicators for mineral dust. In the fine size fraction (< 2 micrometers EAD), sulfur (S) generally was the dominant element, except during high dust episodes when Ca and Si were again the most abundant. Furthermore, fine black carbon (BC) correlates with S, suggesting that they may have originated from the same sources or source regions. An indication of the short-term effect of aerosol loading on radiative forcing was provided by measurements of global and diffuse solar radiation, which showed that during high turbidity periods (strong dust events) almost all of the solar radiation reaching the area is scattered or absorbed.

Interrelationships between aerosol characteristics and light scattering during late winter in an Eastern Mediterranean arid environment

NASA Astrophysics Data System (ADS)

Ichoku, Charles; Andreae, Meinrat O.; Andreae, Tracey W.; Meixner, Franz X.; Schebeske, Guenther; Formenti, Paola; Maenhaut, Willy; Cafmeyer, Jan; Ptasinski, Jacek; Karnieli, Arnon; Orlovsky, Leah

1999-10-01

An intensive field campaign involving measurement of various aerosol physical, chemical, and radiative properties was conducted at Sde Boker (also written as Sede Boqer) in the Negev Desert of Israel, from 18 February to 15 March 1997. Nephelometer measurements gave average background scattering coefficient values of about 25 Mm-1 at 550 nm wavelength, but strong dust events caused the value of this parameter to rise up to about 800 Mm-1. Backscattering fractions did not depend on aerosol loading and generally fell in the range of 0.1 to 0.25, comparable to values reported for marine and Arctic environments. Chemical analysis of the aerosol revealed that in the coarse size range (2-10 μm equivalent aerodynamic diameter (EAD)), calcium (Ca) was by far the most abundant element followed by silicon (Si), both of which are indicators for mineral dust. In the fine size fraction (<2 μm EAD), sulfur (S) generally was the dominant element, except during high dust episodes when Ca and Si were again the most abundant. Furthermore, fine black carbon (BC) correlates with S, suggesting that they may have originated from the same sources or source regions. An indication of the short-term effect of aerosol loading on radiative forcing was provided by measurements of global and diffuse solar radiation, which showed that during high-turbidity periods (strong dust events), almost all of the solar radiation reaching the area is scattered or absorbed.

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.

Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

NASA Technical Reports Server (NTRS)

Gorzelska, K.; Talbot, R. W.; Klemm, K.; Lefer, B.; Klemm, O.; Gregory, G. L.; Anderson, B.; Barrie, L. A.

1994-01-01

Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

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

Parworth, Caroline; Tilp, Alison; Fast, Jerome

In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

The dynamic surface tension of atmospheric aerosol surfactants reveals new aspects of cloud activation.

PubMed

Nozière, Barbara; Baduel, Christine; Jaffrezo, Jean-Luc

2014-02-25

The activation of aerosol particles into cloud droplets in the Earth's atmosphere is both a key process for the climate budget and a main source of uncertainty. Its investigation is facing major experimental challenges, as no technique can measure the main driving parameters, the Raoult's term and surface tension, σ, for sub-micron atmospheric particles. In addition, the surfactant fraction of atmospheric aerosols could not be isolated until recently. Here we present the first dynamic investigation of the total surfactant fraction of atmospheric aerosols, evidencing adsorption barriers that limit their gradient (partitioning) in particles and should enhance their cloud-forming efficiency compared with current models. The results also show that the equilibration time of surfactants in sub-micron atmospheric particles should be beyond the detection of most on-line instruments. Such instrumental and theoretical shortcomings would be consistent with atmospheric and laboratory observations and could have limited the understanding of cloud activation until now.

Major 20th century changes of the content and chemical speciation of organic carbon archived in Alpine ice cores: Implications for the long-term change of organic aerosol over Europe

NASA Astrophysics Data System (ADS)

Legrand, M.; Preunkert, S.; May, B.; Guilhermet, J.; Hoffman, H.; Wagenbach, D.

2013-05-01

Dissolved organic carbon (DOC) and an extended array of organic compounds were investigated in an Alpine ice core covering the 1920-1988 time period. Based on this, a reconstruction was made of the long-term trends of water-soluble organic carbon (WSOC) aerosol in the European atmosphere. It is shown that light mono- and dicarboxylates, humic-like substances, and formaldehyde account together for more than half of the DOC content of ice. This extended chemical speciation of DOC is used to estimate the DOC fraction present in ice that is related to WSOC aerosol and its change over the past. It is suggested that after World War II, the WSOC levels have been enhanced by a factor of 2 and 3 in winter and summer, respectively. In summer, the fossil fuel contribution to the enhancement is estimated to be rather small, suggesting that it arises mainly from an increase in biogenic sources of WSOC.

Urban impacts on regional carbonaceous aerosols: case study in central Texas.

PubMed

Barrett, Tate E; Sheesley, Rebecca J

2014-08-01

Rural and background sites provide valuable information on the concentration and optical properties of organic, elemental, and water-soluble organic carbon (OC, EC, and WSOC), which are relevant for understanding the climate forcing potential of regional atmospheric aerosols. To quantify climate- and air quality-relevant characteristics of carbonaceous aerosol in the central United States, a regional background site in central Texas was chosen for long-term measurement. Back trajectory (BT) analysis, ambient OC, EC, and WSOC concentrations and absorption parameters are reported for the first 15 months of a long-term campaign (May 2011-August 2012). BT analysis indicates consistent north-south airflow connecting central Texas to the Central Plains. Central Texas aerosols exhibited seasonal trends with increased fine particulate matter (< 2.5 microm aerodynamic diameter, PM2.5) and OC during the summer (PM2.5 = 10.9 microg m(-3) and OC = 3.0 microg m(-3)) and elevated EC during the winter (0.22 microg m(-3)). When compared to measurements in Dallas and Houston, TX, central Texas OC appears to have mixed urban and rural sources. However central Texas EC appears to be dominated by transport of urban emissions. WSOC averaged 63% of the annual OC, with little seasonal variability in this ratio. To monitor brown carbon (BrC), absorption was measured for the aqueous WSOC extracts. Light absorption coefficients for EC and BrC were highest during summer (EC MAC = 11 m2 g(-1) and BRC MAE365 = 0.15 m2 g(-1)). Results from optical analysis indicate that regional aerosol absorption is mostly due to EC with summertime peaks in BrC attenuation. This study represents the first reported values of WSOC absorption, MAE365, for the central United States. Implications: Background concentration and absorption measurements are essential in determining regional potential radiative forcing due to atmospheric aerosols. Back trajectory, chemical, and optical analysis of PM2.5 was used to determine climatic and air quality implications of urban outflow to a regional receptor site, representative of the central United States. Results indicate that central Texas organic carbon has mixed urban and rural sources, while elemental carbon is controlled by the transport of urban emissions. Analysis of aerosol absorption showed black carbon as the dominant absorber, with less brown carbon absorption than regional studies in California and the southeastern United States.

17 years of aerosol and clouds from the ATSR Series of Instruments

NASA Astrophysics Data System (ADS)

Poulsen, C. A.

2015-12-01

Aerosols play a significant role in Earth's climate by scattering and absorbing incoming sunlight and affecting the formation and radiative properties of clouds. The extent to which aerosols affect cloud remains one of the largest sources of uncertainty amongst all influences on climate change. Now, a new comprehensive datasets has been developed under the ESA Climate Change Initiative (CCI) programme to quantify how changes in aerosol levels affect these clouds. The unique dataset is constructed from the Optimal Retrieval of Aerosol and Cloud (ORAC) algorithm used in (A)ATSR (Along Track Scanning Radiometer) retrievals of aerosols generated in the Aerosol CCI and the CC4CL ( Community Code for CLimate) for cloud retrieval in the Cloud CCI. The ATSR instrument is a dual viewing instrument with on board visible and infra red calibration systems making it an ideal instrument to study trends of Aerosol and Clouds and their interactions. The data set begins in 1995 and ends in 2012. A new instrument in the series SLSTR(Sea and Land Surface Temperature Radiometer) will be launch in 2015. The Aerosol and Clouds are retreived using similar algorithms to maximise the consistency of the results These state-of-the-art retrievals have been merged together to quantify the susceptibility of cloud properties to changes in aerosol concentration. Aerosol-cloud susceptibilities are calculated from several thousand samples in each 1x1 degree globally gridded region. Two-D histograms of the aerosol and cloud properties are also included to facilitate seamless comparisons between other satellite and modelling data sets. The analysis of these two long term records will be discussed individually and the initial comparisons between these new joint products and models will be presented.

Constraining Aerosol-Cloud-Precipitation Interactions of Orographic Mixed-Phase Clouds with Trajectory Budgets

NASA Astrophysics Data System (ADS)

Glassmeier, F.; Lohmann, U.

2016-12-01

Orographic precipitation is prone to strong aerosol-cloud-precipitation interactions because the time for precipitation development is limited to the ascending section of mountain flow. At the same time, cloud microphysical development is constraint by the strong dynamical forcing of the orography. In this contribution, we discuss how changes in the amount and composition of droplet- and ice-forming aerosols influence precipitation in idealized simulations of stratiform orographic mixed-phase clouds. We find that aerosol perturbations trigger compensating responses of different precipitation formation pathways. The effect of aerosols is thus buffered. We explain this buffering by the requirement to fulfill aerosol-independent dynamical constraints. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with a bell-shaped mountain. The model is coupled to a 2-moment warm and cold cloud microphysics scheme. Activation and freezing rates are parameterized based on prescribed aerosol fields that are varied in number, size and composition. Our analysis is based on the budget of droplet water along trajectories of cloud parcels. The budget equates condensation as source term with precipitation formation from autoconversion, accretion, riming and the Wegener-Bergeron-Findeisen process as sink terms. Condensation, and consequently precipitation formation, is determined by dynamics and largely independent of the aerosol conditions. An aerosol-induced change in the number of droplets or crystals perturbs the droplet budget by affecting precipitation formation processes. We observe that this perturbation triggers adjustments in liquid and ice water content that re-equilibrate the budget. As an example, an increase in crystal number triggers a stronger glaciation of the cloud and redistributes precipitation formation from collision-coalescence to riming and from riming to vapor deposition. We theoretically confirm the dominant effect of water content adjustments over number changes by estimating susceptibilities d ln P / d ln N of precipitation formation P to droplet or crystal number N from the budget equation. The susceptibility analysis also reveals that aerosol perturbations to droplet and crystal number compensate each other.

Coarse and fine aerosol source apportionment in Rio de Janeiro, Brazil

NASA Astrophysics Data System (ADS)

Godoy, Maria Luiza D. P.; Godoy, José Marcus; Roldão, Luiz Alfredo; Soluri, Daniela S.; Donagemma, Raquel A.

The metropolitan area of Rio de Janeiro is one of the twenty biggest urban agglomerations in the world, with 11 million inhabitants in the metropolitan area, and has a high population density, with 1700 hab. km -2. For this aerosol source apportionment study, the atmospheric aerosol sampling was performed at ten sites distributed in different locations of the metropolitan area from September/2003 to December/2005, with sampling during 24 h on a weekly basis. Stacked filter units (SFU) were used to collect fine and coarse aerosol particles with a flow rate of 17 L min -1. In both size fractions trace elements were analyzed by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) as well as water-soluble species by Ion-Chromatography (IC). Also gravimetric analysis and reflectance measurements provided aerosol mass and black carbon concentrations. Very good detection limits for up to 42 species were obtained. Mean annual PM 10 mass concentration ranged from 20 to 37 μg m -3, values that are within the Brazilian air quality standards. Receptor models such as principal factor analysis, cluster analysis and absolute principal factor analysis were applied in order to identify and quantify the aerosol sources. For fine and coarse modes, circa of 100% of the measured mass was quantitatively apportioned to relatively few identified aerosol sources. A very similar and consistent source apportionment was obtained for both fine and coarse modes for all 10 sampling sites. Soil dust is an important component, accounting for 22-72% and for 25-48% of the coarse and fine mass respectively. On the other hand, anthropogenic sources as vehicle traffic and oil combustion represent a relatively high contribution (52-75%) of the fine aerosol mass. The joint use of ICP-MS and IC analysis of species in aerosols has proven to be reliable and feasible for the analysis of large amount of samples, and the coupling with receptor models provided an excellent method for quantitative aerosol source apportionment in large urban areas.

Aerosol source apportionment based on multi-wavelength photoacoustic light absorption measurements: a simulation method for system's optimisation

NASA Astrophysics Data System (ADS)

Simon, Károly; Ajtai, Tibor; Kiss-Albert, Gergely; Utry, Noémi; Pintér, Máté; Szabó, Gábor; Bozóki, Zoltán

2017-04-01

Aerosol source apportionment is currently one of the outstanding challenges for environmental monitoring. In most cases atmospheric aerosol is a heterogeneous mixture as it typically originates from various sources. Consequently, each aerosol type has distinct chemical and physical properties. Contrary to chemical properties, optical absorption and size distribution of airborne particles can be measured in real time with high time resolution i.e. their measurement facilitates real time source apportionment (Favez et al (2009), Ajtai et al (2011), Favez et al (2010)). The wavelength dependency of the optical absorption coefficient (OAC) is usually characterised by the Absorption Angström Exponent (AAE). So far, the selection of light sources (lasers) into a photoacoustic aerosol measuring system was based on rule of thumb type estimations only. Recently, we proposed a simulation method that can be used to estimate the accuracy of aerosol source apportionment in case of a dual wavelength photoacoustic system (Simon et al., (2017)). This simulation is based on the assumption that the atmospheric aerosol load is dominated by two distinct sources and each of them is strongly light absorbing with specific AAE values. This is a typical scenario e.g. for urban measurements under wintry conditions when dominating aerosol sources are fossil fuel and wood burning with characteristic AAE 1 and 2, respectively. The wavelength pair of 405 and 1064 nm was found to be optimal for source apportionment in this case. In the presented study we investigated the situation when there are aerosol components with only slightly different AAE values and searched for a photoacoustic system which is optimal for distinguishing these components. Ajtai, T.; Filep, Á.; Utry, N.; Schnaiter, M.; Linke, C.; Bozóki, Z.; Szabó, G. and Leisner T. (2011) Journal of Aerosol Science 42, 859-866. Favez, O.; Cachier, H.; Sciare, J.; Sarda-Estève, R. and Martinon, L. (2009) Atmospheric Environment 43, 3640-3644. Favez, O.; El Haddad, I.; Piot, C.; Boréave, A.; Abidi, E.; Marchand, N.; Jaffrezo, J. L.; Besombes, J. L.; Personnaz, M. B.; Sciare, J.; Wortham, H.; George, C. and D'Anna, B. (2010), Atmos. Chem. Phys. 10, 5295-5314. Simon, K.A.; Ajtai, T; Gulyas, G; Utry, N; Pinter, M; Szabo, G. and Bozoki, Bozoki, Z. (2017), Journal of Aerosol Science 104, 10-15.

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Potential origin of organic CNN observed at a marine site

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

Andrews, E.; Kreidenweis, S.M.; Penner, J.E.

1995-12-31

Observations by Novakov and Penner (1993) suggest that organic aerosol particles may make up a significant portion of cloud condensation nuclei (CCN) comparable, perhaps, to the sulfate aerosol contribution to CCN. Because organic CCN would influence the albedo and radiative properties of clouds and play a role in climate change, it is important to identify the sources of these aerosols. In their research Novakov and Penner assumed that particles larger than 0.05 {mu}m could act as CCN. Therefore the origins of nucleation mode aerosol (0.03 < dp < 0.1 {mu}m) are the focus of our research. In our research, wemore » apply a dynamic aerosol model (MAEROS) to explore potential sources of the nucleation mode organic aerosol observed at a marine site in Puerto Rico. Novakov and Penner measured the size segregated mass and composition of the atmospheric aerosol at this site and found that organic aerosol mass dominated the sulfate mass in the nucleation size range. The presence of organics in this size range suggests that these organic aerosol particles were generated by nucleation of a gas phase organic followed by condensational processes, i.e., identifying sources of the gas phase precursors is important to determining the organic CCN origins. Back trajectory analysis shows that the air mass was without continental contact for 12 days prior to being sampled. This implicates two possible sources for the gas phase organic: biogenic emissions from the Puerto Rican forest and emissions from the ocean surface. In this research we explore both the forest and ocean source scenarios, showing that the forest is more likely to be the ultimate source of the observed organic aerosol particles. Using MAEROS (modified to include nucleation) and reasonable input parameters taken from the literature we were able to show that an organic vapor flux very similar to the measured biogenic fluxes reported by Zimmerman et al. generated size distributions similar to the observed aerosol.« less

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.

Model evaluation using a geo-stationary satellite and in-situ measurements around Japan in May 2016

NASA Astrophysics Data System (ADS)

Goto, D.; Kikuchi, M.; Suzuki, K.; Hayasaki, M.; Yoshida, M.; Nagao, T. M.; Sugimoto, N.; Shimizu, A.; Teruyuki, N.

2017-12-01

A semi-regional aerosol-transport model with high resolution has been evaluated by multiple measurements of in-situ sampling and lidar. Here, we evaluate the aerosol simulation of the non-hydrostatic icosahedral atmospheric model (NICAM) around East Asia by using Advanced Himawari Imager (AHI-08) onboard a geostationary satellite, Himawari. The AHI-08 can estimate both aerosol and cloud optical properties with much higher-time resolution than orbital satellites. Since only a combination of in-situ sampling and lidar at sites can detect an arrival of air pollutants at the limited areas, the geo-stationary satellite can greatly help us to understand the three-dimensional structures of the air pollutants from the sources to the outflow regions. In May 2016 where Siberian biomass burning is active, AHI-08 often detects remarkable plumes from Siberia to Japan. The observed plumes including the detail horizontal distribution of aerosol optical thickness are successfully captured by NICAM on 18 May 2016. Multiple validations using in-situ measurements also show that NICAM generally reproduces the temporal variations of the representative transboundary pollutions including carbonaceous aerosols from biomass burning and sulfate aerosols from anthropogenic sources. In terms of the vertical profile, however, the evaluation also suggests that the vertical air mixing in NICAM is stronger at the heights of less than 6 km than that shown in lidar. These comprehensive findings to address for the further model development are clarified by a new evaluation using the combination of new results obtained from the geo-stationary satellite and widely-used results by in-situ sampling and lidar for the first time.

The DRAGON scale concept and results for remote sensing of aerosol properties

NASA Astrophysics Data System (ADS)

Holben, B. N.; Eck, T. F.; Schafer, J.; Giles, D. M.; Kim, J.; Sano, I.; Mukai, S.; Kim, Y. J.; Reid, J. S.; Pickering, K. E.; Crawford, J. H.; Smirnov, A.; Sinyuk, A.; Slutsker, I.; Sorokin, M.; Rodriguez, J.; Liew, S.; Trevino, N.; Lim, H.; Lefer, B. L.; Nadkarni, R.; Macke, A.; Kinne, S. A.; Anderson, B. E.; Russell, P. B.; Maring, H. B.; Welton, E. J.; da Silva, A.; Toon, O. B.; Redemann, J.

2013-12-01

Aerosol processes occur at microscales but are typically observed and reported at continental to global scales. Often observable aerosol processes that have significant anthropogenic impact occur on spatial scales of tens to a few hundred km, representative of convective cloud processing, urban/megacity sources, anthropogenic burning and natural wildfires, dry lakebed dust sources etc. Historically remote sensing of aerosols has relied on relatively coarse temporal and spatial resolution satellite observations or high temporal resolution point observations from ground-based monitoring sites from networks such as AERONET, SKYNET, MPLNET and many other surface observation platforms. Airborne remote and in situ observations combined with assimilation models were/are to be the mesoscale link between the ground- and space-based RS scales. However clearly the in situ and ground-based RS characterizations of aerosols require a convergence of thought, parameterization and actual scale measurements in order to advance this goal. This has been served by periodic multidisciplinary field campaigns yet only recently has a concerted effort been made to establish these ground-based networks in an effort to capture the mesoscale processes through measurement programs such as DISCOVER AQ and NASA AERONET's effort to foster such measurements and analysis through the Distributed Regional Aerosol Gridded Observation Networks (DRAGON), short term meso-networks, with partners in Asia and Europe and N. America. This talk will review the historical need for such networks and discuss some of the results and in some cases unexpected findings from the eight DRAGON campaigns conducted the last several years. Emphasis will be placed on the most recent DISCOVER AQ campaign conducted in Houston TX and the synergism with a regional to global network plan through the SEAC4RS US campaign.

Investigating Source Contributions of Size-Aggregated Aerosols Collected in Southern Ocean and Baring Head, New Zealand Using Sulfur Isotopes

NASA Astrophysics Data System (ADS)

Li, Jianghanyang; Michalski, Greg; Davy, Perry; Harvey, Mike; Katzman, Tanya; Wilkins, Benjamin

2018-04-01

Marine sulfate aerosols in the Southern Ocean are critical to the global radiation balance, yet the sources of sulfate and their seasonal variations are unclear. We separately sampled marine and ambient aerosols at Baring Head, New Zealand for 1 year using two collectors and evaluated the sources of sulfate in coarse (1-10 μm) and fine (0.05-1 μm) aerosols using sulfur isotopes (δ34S). In both collectors, sea-salt sulfate (SO42-SS) mainly existed in coarse aerosols and nonsea-salt sulfate (SO42-NSS) dominated the sulfate in fine aerosols, although some summer SO42-NSS appeared in coarse particles due to aerosol coagulation. SO42-NSS in the marine aerosols was mainly (88-100%) from marine biogenic dimethylsulfide (DMS) emission, while the SO42-NSS in the ambient aerosols was a combination of DMS (73-79%) and SO2 emissions from shipping activities ( 21-27%). The seasonal variations of SO42-NSS concentrations inferred from the δ34S values in both collectors were mainly controlled by the DMS flux.

Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach

NASA Astrophysics Data System (ADS)

Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Ceburnis, D.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J. L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Laaksonen, A.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2014-06-01

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

Towards mechanistic representations of SOA from BVOC + NO3 reactions

EPA Science Inventory

Monoterpene reaction with nitrate radicals is a significant source of organic aerosol in the southeast United States. This source of organic aerosol represents an anthropogenic control on biogenic organic aerosol since nitrate radicals result from NOx emissions and are generally ...

Molecular identification of organic compounds in atmospheric complex mixtures and relationship to atmospheric chemistry and sources.

PubMed

Mazurek, Monica A

2002-12-01

This article describes a chemical characterization approach for complex organic compound mixtures associated with fine atmospheric particles of diameters less than 2.5 m (PM2.5). It relates molecular- and bulk-level chemical characteristics of the complex mixture to atmospheric chemistry and to emission sources. Overall, the analytical approach describes the organic complex mixtures in terms of a chemical mass balance (CMB). Here, the complex mixture is related to a bulk elemental measurement (total carbon) and is broken down systematically into functional groups and molecular compositions. The CMB and molecular-level information can be used to understand the sources of the atmospheric fine particles through conversion of chromatographic data and by incorporation into receptor-based CMB models. Once described and quantified within a mass balance framework, the chemical profiles for aerosol organic matter can be applied to existing air quality issues. Examples include understanding health effects of PM2.5 and defining and controlling key sources of anthropogenic fine particles. Overall, the organic aerosol compositional data provide chemical information needed for effective PM2.5 management.

Source Term Experiments Project (STEP): Aerosol characterization system

NASA Astrophysics Data System (ADS)

Schlenger, B. J.; Dunn, P. F.

A series of four experiments is being conducted at Argonne National Laboratory's TREAT Reactor. They were designed to provide some of the necessary data regarding magnitude and release rates of fission products from degraded fuel pins, physical and chemical characteristics of released fission products, and aerosol formation and transport phenomena. These are in pile experiments, whereby the test fuel is heated by neutron induced fission and subsequent clad oxidation in steam environments that simulate as closely as practical predicted reactor accident conditions. The test sequences cover a range of pressure and fuel heatup rate, and include the effect of Aq/In/Cd control rod material.

Tropospheric Chemistry Studies using Observations from GOME and TOMS

NASA Technical Reports Server (NTRS)

Chance, Kelly; Spurr, Robert J. D.; Kurosu, Thomas P.; Jacob, Daniel J.; Gleason, James F.

2003-01-01

Studies to quantitatively determine trace gas and aerosol amounts from the Global Ozone Monitoring Experiment (GOME) and the Total Ozone Monitoring Experiment (TOMS) and to perform chemical modeling studies which utilize these results are given. This includes: 1. Analysis of measurements from the GOME and TOMS instruments for troposphere distributions of O3 and HCHO; troposphere enhancements of SO2, NO2 and aerosols associated with major sources; and springtime events of elevated BrO in the lower Arctic troposphere. 2. Application of a global 3-dimensional model of troposphere chemistry to interpret the GOME observations in terms of the factors controlling the abundances of troposphere ozone and OH.

Methods of analysis for complex organic aerosol mixtures from urban emission sources of particulate carbon

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

Mazurek, M.A.; Hildemann, L.M.; Cass, G.R.

1990-04-01

Extractable organic compounds having between 6 to 40 carbon atoms comprise an important mass fraction of the fine particulate matter samples from major urban emission sources. Depending on the emission source type, this solvent-soluble fraction accounts for <20% to 100% of the total organic aerosol mass, as measured by quantitative high-resolution has chromatography (HRGC) with flame ionization detection. In addition to total extract quantitation, HRGC can be applied to further analyses of the mass distributions of elutable organics present in the complex aerosol extract mixtures, thus generating profiles that serve as fingerprints'' for the sources of interest. This HRGC analyticalmore » method is applied to emission source samples that contain between 7 to 12,000 {mu}g/filter organic carbon. It is shown to be a sensitive technique for analysis of carbonaceous aerosol extract mixtures having diverse mass loadings and species distributions. This study describes the analytical chemical methods that have been applied to: the construction of chemical mass balances based on the mass of fine organic aerosol emitted for major urban sources of particulate carbon; and the generation of discrete emission source chemical profiles derived from chromatographic characteristics of the organic aerosol components. 21 refs., 1 fig., 2 tabs.« less

Process evaluation of sea salt aerosol concentrations at remote marine locations

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

Radiative Effect of Springtime Biomass-Burning Aerosols over Northern Indochina During 7-SEAS Baseline 2013 Campaign

NASA Technical Reports Server (NTRS)

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

2016-01-01

The direct aerosol radiative effects of biomass-burning (BB) aerosols over northern Indochina were estimated by using aerosol properties (physical, chemical, and optical) along with the vertical profile measurements from ground-based measurements with integration of an optical and a radiative transfer model during the Seven South East Asian Studies Biomass-Burning Aerosols Stratocumulus Environment: Lifecycles Interactions Experiment (7-SEASBASELInE) conducted in spring 2013. Cluster analysis of backward trajectories showed the air masses arriving at mountainous background site (Doi Ang Khang; 19.93degN, 99.05degE, 1536 m above mean sea level) in northern Indochina, mainly from near-source inland BB activities and being confined in the planetary boundary layer. The PM(sub10) and black carbon (BC)mass were 87 +/- 28 and 7 +/- 2 micrograms m(exp -3), respectively. The aerosol optical depth (AOD (sub 500) was found to be 0.26--1.13 (0.71 +/- 0.24). Finer (fine mode fraction is approximately or equal to 0.95, angstrom-exponent at 440-870 nm is approximately or equal to 1.77) and significantly absorbing aerosols(single scattering albedo is approximately or equal to 0.89, asymmetry-parameter is approximately or equal to 0.67, and absorption AOD 0.1 at 440 nm) dominated over this region. BB aerosols (water soluble and BC) were the main contributor to the aerosol radiative forcing (ARF), while others (water insoluble, sea salt and mineral dust) were negligible mainly due to their low extinction efficiency. BC contributed only 6 to the surface aerosol mass but its contribution to AOD was 12 (2 times higher). The overall mean ARF was 8.0 and -31.4 W m(exp -2) at top-of-atmosphere (TOA) and at the surface (SFC), respectively. Likely, ARF due to BC was +10.7 and -18.1 W m(exp -2) at TOA and SFC, respectively. BC imposed the heating rate of +1.4 K d(exp -1) within the atmosphere and highlighting its pivotal role in modifying the radiation budget. We propose that to upgrade our knowledge on BB aerosol radiative effects in BB source region, the long-term and extensive field measurements are needed.

Lipid geochemistry of remote aerosols from the southwestern Pacific Ocean sector

NASA Astrophysics Data System (ADS)

Sicre, Marie-Alexandrine; Peltzer, Edward T.

Aerosol samples collected on Ninety Mile Beach on the West coast of the North Island of New Zealand were analyzed for three classes of naturally occurring organic compounds ( n-alkanes, fatty alcohols and long-chain n-aldehydes) which are major constituents of epicuticular waxes of terrestrial plants. In the eight samples analyzed, we identified three distinct regional source signatures for these aerosols depending upon their origin: southwest Pacific Ocean, New Zealand or Australia. Source identifications were entirely consistent with the origin of the aerosols derived by isentropic air mass trajectories. Impactor studies provided additional information as to the source of the aerosols and the mode of introduction of the material into the atmosphere.

Long-range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the western Mediterranean basin

NASA Astrophysics Data System (ADS)

Ancellet, Gerard; Pelon, Jacques; Totems, Julien; Chazette, Patrick; Bazureau, Ariane; Sicard, Michaël; Di Iorio, Tatiana; Dulac, Francois; Mallet, Marc

2016-04-01

Long-range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground-based and airborne lidar measurements were deployed in the western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three-dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Minorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agrees very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (i) pure BB layer, (ii) weakly dusty BB, (iii) significant mixture of BB and dust transported from the trade wind region, and (iv) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at an altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS aerosol optical depth horizontal distribution during this episode over the western Mediterranean Sea shows that the Canadian fire contributions were as large as the direct northward dust outflow from Sahara.

Global and Regional Temperature-change Potentials for Near-term Climate Forcers

NASA Technical Reports Server (NTRS)

Collins, W.J.; Fry, M. M.; Yu, H.; Fuglestvedt, J. S.; Shindell, D. T.; West, J. J.

2013-01-01

The emissions of reactive gases and aerosols can affect climate through the burdens of ozone, methane and aerosols, having both cooling and warming effects. These species are generally referred to near-term climate forcers (NTCFs) or short-lived climate pollutants (SLCPs), because of their short atmospheric residence time. The mitigation of these would be attractive for both air quality and climate on a 30-year timescale, provided it is not at the expense of CO2 mitigation. In this study we examine the climate effects of the emissions of NTCFs from 4 continental regions (East Asia, Europe, North America and South Asia) using results from the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model simulations. We address 3 aerosol species (sulphate, particulate organic matter and black carbon - BC) and 4 ozone precursors (methane, reactive nitrogen oxides - NOx, volatile organic compounds VOC, and carbon monoxide - CO). For the aerosols the global warming potentials (GWPs) and global temperature change potentials (GTPs) are simply time-dependent scaling of the equilibrium radiative forcing, with the GTPs decreasing more rapidly with time than the GWPs. While the aerosol climate metrics have only a modest dependence on emission region, emissions of NOx and VOCs from South Asia have GWPs and GTPs of higher magnitude than from the other northern hemisphere regions. On regional basis, the northern mid-latitude temperature response to northern mid-latitude emissions is approximately twice as large as the global average response for aerosol emission, and about 20-30% larger than the global average for methane, VOC and CO emissions. We also found that temperatures in the Arctic latitudes appear to be particularly sensitive to black carbon emissions from South Asia.

Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: insights into nitrate chemistry

NASA Astrophysics Data System (ADS)

Reyes-Villegas, Ernesto; Priestley, Michael; Ting, Yu-Chieh; Haslett, Sophie; Bannan, Thomas; Le Breton, Michael; Williams, Paul I.; Bacak, Asan; Flynn, Michael J.; Coe, Hugh; Percival, Carl; Allan, James D.

2018-03-01

Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires or fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrogen chemistry was observed during Bonfire Night with nitrogen containing compounds in both gas and aerosol phases and further N2O5 and ClNO2 concentrations, which depleted early next morning due to photolysis of NO3 radicals and ceasing production. Particulate organic oxides of nitrogen (PONs) concentrations of 2.8 µg m-3 were estimated using the m / z 46 : 30 ratios from aerosol mass spectrometer (AMS) measurements, according to previously published methods. Multilinear engine 2 (ME-2) source apportionment was performed to determine organic aerosol (OA) concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2) and secondary (sPON_ME2) contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table) to determine PON sources, which resulted in an r2 = 0.894 between biomass burning organic aerosol (BBOA) and babs_470wb compared to an r2 = 0.861 obtained without the modification. Correlations between OA sources and measurements made using time-of-flight chemical ionisation mass spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During Bonfire Night, strong correlations (r2) were observed between BBOA and methacrylic acid (0.92), acrylic acid (0.90), nitrous acid (0.86), propionic acid, (0.85) and hydrogen cyanide (0.76). A series of oxygenated species and chlorine compounds showed good correlations with sPON_ME2 and the low volatility oxygenated organic aerosol (LVOOA) factor during Bonfire Night and an event with low pollutant concentrations. Further analysis of pPON_ME2 and sPON_ME2 was performed in order to determine whether these PON sources absorb light near the UV region using an Aethalometer. This hypothesis was tested by doing multilinear regressions between babs_470wb and BBOA, sPON_ME2 and pPON_ME2. Our results suggest that sPON_ME2 does not absorb light at 470 nm, while pPON_ME2 and LVOOA do absorb light at 470 nm. This may inform black carbon (BC) source apportionment studies from Aethalometer measurements, through investigation of the brown carbon contribution to babs_470wb.

Variability of aerosol vertical distribution in the Sahel

NASA Astrophysics Data System (ADS)

Cavalieri, O.; Cairo, F.; Fierli, F.; di Donfrancesco, G.; Snels, M.; Viterbini, M.; Cardillo, F.; Chatenet, B.; Formenti, P.; Marticorena, B.; Rajot, J. L.

2010-12-01

In this work, we have studied the seasonal and inter-annual variability of the aerosol vertical distribution over Sahelian Africa for the years 2006, 2007 and 2008, characterizing the different kind of aerosols present in the atmosphere in terms of their optical properties observed by ground-based and satellite instruments, and their sources searched for by using trajectory analysis. This study combines data acquired by three ground-based micro lidar systems located in Banizoumbou (Niger), Cinzana (Mali) and M'Bour (Senegal) in the framework of the African Monsoon Multidisciplinary Analysis (AMMA), by the AEROsol RObotic NETwork (AERONET) sun-photometers and by the space-based Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard the CALIPSO satellite (Cloud-Aerosol Lidar and Infrared Pathfinder Observations). During winter, the lower levels air masses arriving in the Sahelian region come mainly from North, North-West and from the Atlantic area, while in the upper troposphere air flow generally originates from West Africa, crossing a region characterized by the presence of large biomass burning sources. The sites of Cinzana, Banizoumbou and M'Bour, along a transect of aerosol transport from East to West, are in fact under the influence of tropical biomass burning aerosol emission during the dry season, as revealed by the seasonal pattern of the aerosol optical properties, and by back-trajectory studies. Aerosol produced by biomass burning are observed mainly during the dry season and are confined in the upper layers of the atmosphere. This is particularly evident for 2006, which was characterized by a large presence of biomass burning aerosols in all the three sites. Biomass burning aerosol is also observed during spring when air masses originating from North and East Africa pass over sparse biomass burning sources, and during summer when biomass burning aerosol is transported from the southern part of the continent by the monsoon flow. During summer months, the entire Sahelian region is under the influence of Saharan dust aerosols: the air masses in low levels arrive from West Africa crossing the Sahara desert or from the Southern Hemisphere crossing the Guinea Gulf while in the upper layers air masses still originate from North, North-East. The maximum of the desert dust activity is observed in this period which is characterized by large AOD (above 0.2) and backscattering values. It also corresponds to a maximum in the extension of the aerosol vertical distribution (up to 6 km of altitude). In correspondence, a progressive cleaning up of the lowermost layers of the atmosphere is occurring, especially evident in the Banizoumbou and Cinzana sites. Summer is in fact characterized by extensive and fast convective phenomena. Lidar profiles show at times large dust events loading the atmosphere with aerosol from the ground up to 6 km of altitude. These events are characterized by large total attenuated backscattering values, and alternate with very clear profiles, sometimes separated by only a few hours, indicative of fast removal processes occurring, likely due to intense convective and rain activity. The inter-annual variability in the three year monitoring period is not very significant. An analysis of the aerosol transport pathways, aiming at detecting the main source regions, revealed that air originated from the Saharan desert is present all year long and it is observed in the lower levels of the atmosphere at the beginning and at the end of the year. In the central part of the year it extends upward and the lower levels are less affected by air masses from Saharan desert when the monsoon flow carries air from the Guinea Gulf and the Southern Hemisphere inland.

“A significant source of isoprene aerosol controlled by acidity”

EPA Science Inventory

“A significant source of isoprene aerosol controlled by acidity” by Pye et al.Abstract: Isoprene is a significant contributor to organic aerosol in the southeastern United States where biogenic hydrocarbons mix with anthropogenic emissions. In this work, CMAQ provides explicit p...

Modern dust aerosol availability in northwestern China.

PubMed

Wang, Xunming; Cheng, Hong; Che, Huizheng; Sun, Jimin; Lu, Huayu; Qiang, Mingrui; Hua, Ting; Zhu, Bingqi; Li, Hui; Ma, Wenyong; Lang, Lili; Jiao, Linlin; Li, Danfeng

2017-08-18

The sources of modern dust aerosols and their emission magnitudes are fundamental for linking dust with climate and environment. Using field sample data, wind tunnel experiments and statistical analysis, we determined the contributions of wadis, gobi (stony desert), lakebeds, riverbeds, and interdunes to modern dust aerosol availability in the three important potential dust sources including the Tarim Basin, Qaidam Basin, and Ala Shan Plateau of China. The results show that riverbeds are the dominant landscape for modern dust aerosol availabilities in the Qaidam Basin, while wadis, gobi, and interdunes are the main landscapes over the Ala Shan Plateau and Tarim Basin. The Ala Shan Plateau and Tarim Basin are potential dust sources in northwestern China, while the Qaidam Basin is not a major source of the modern dust aerosols nowadays, and it is not acting in a significant way to the Loess Plateau presently. Moreover, most of modern dust aerosol emissions from China originated from aeolian processes with low intensities rather than from major dust events.

Long-term particulate matter modeling for health effect studies in California - Part 2: Concentrations and sources of ultrafine organic aerosols

NASA Astrophysics Data System (ADS)

Hu, Jianlin; Jathar, Shantanu; Zhang, Hongliang; Ying, Qi; Chen, Shu-Hua; Cappa, Christopher D.; Kleeman, Michael J.

2017-04-01

Organic aerosol (OA) is a major constituent of ultrafine particulate matter (PM0. 1). Recent epidemiological studies have identified associations between PM0. 1 OA and premature mortality and low birth weight. In this study, the source-oriented UCD/CIT model was used to simulate the concentrations and sources of primary organic aerosols (POA) and secondary organic aerosols (SOA) in PM0. 1 in California for a 9-year (2000-2008) modeling period with 4 km horizontal resolution to provide more insights about PM0. 1 OA for health effect studies. As a related quality control, predicted monthly average concentrations of fine particulate matter (PM2. 5) total organic carbon at six major urban sites had mean fractional bias of -0.31 to 0.19 and mean fractional errors of 0.4 to 0.59. The predicted ratio of PM2. 5 SOA / OA was lower than estimates derived from chemical mass balance (CMB) calculations by a factor of 2-3, which suggests the potential effects of processes such as POA volatility, additional SOA formation mechanism, and missing sources. OA in PM0. 1, the focus size fraction of this study, is dominated by POA. Wood smoke is found to be the single biggest source of PM0. 1 OA in winter in California, while meat cooking, mobile emissions (gasoline and diesel engines), and other anthropogenic sources (mainly solvent usage and waste disposal) are the most important sources in summer. Biogenic emissions are predicted to be the largest PM0. 1 SOA source, followed by mobile sources and other anthropogenic sources, but these rankings are sensitive to the SOA model used in the calculation. Air pollution control programs aiming to reduce the PM0. 1 OA concentrations should consider controlling solvent usage, waste disposal, and mobile emissions in California, but these findings should be revisited after the latest science is incorporated into the SOA exposure calculations. The spatial distributions of SOA associated with different sources are not sensitive to the choice of SOA model, although the absolute amount of SOA can change significantly. Therefore, the spatial distributions of PM0. 1 POA and SOA over the 9-year study period provide useful information for epidemiological studies to further investigate the associations with health outcomes.

Aerosol and monsoon climate interactions over Asia

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Single particle characterization, source apportionment, and aging effects of ambient aerosols in Southern California

NASA Astrophysics Data System (ADS)

Shields, Laura Grace

Composed of a mixture of chemical species and phases and existing in a variety of shapes and sizes, atmospheric aerosols are complex and can have serious influence on human health, the environment, and climate. In order to better understand the impact of aerosols on local to global scales, detailed measurements on the physical and chemical properties of ambient particles are essential. In addition, knowing the origin or the source of the aerosols is important for policymakers to implement targeted regulations and effective control strategies to reduce air pollution in their region. One of the most ground breaking techniques in aerosol instrumentation is single particle mass spectrometry (SPMS), which can provide online chemical composition and size information on the individual particle level. The primary focus of this work is to further improve the ability of one specific SPMS technique, aerosol time-of-flight mass spectrometry (ATOFMS), for the use of identifying the specific origin of ambient aerosols, which is known as source apportionment. The ATOFMS source apportionment method utilizes a library of distinct source mass spectral signatures to match the chemical information of the single ambient particles. The unique signatures are obtained in controlled source characterization studies, such as with the exhaust emissions of heavy duty diesel vehicles (HDDV) operating on a dynamometer. The apportionment of ambient aerosols is complicated by the chemical and physical processes an individual particle can undergo as it spends time in the atmosphere, which is referred to as "aging" of the aerosol. Therefore, the performance of the source signature library technique was investigated on the ambient dataset of the highly aged environment of Riverside, California. Additionally, two specific subsets of the Riverside dataset (ultrafine particles and particles containing trace metals), which are known to cause adverse health effects, were probed in greater detail. Finally, the impact of large wildfires on the ambient levels of particulate matter in Southern California is discussed. The results of this work provide insight into single particles impacting the Southern California region, the relative source contributions to this region, and finally an examination of how atmospheric aging influences the ability to perform source apportionment.

Climate response of the South Asian monsoon system to anthropogenic aerosols

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

Ganguly, Dilip; Rasch, Philip J.; Wang, Hailong

2012-07-13

The equilibrium climate response to the total effects (direct, indirect and semi-direct effects) of aerosols arising from anthropogenic and biomass burning emissions on the South Asian summer monsoon system is studied using a coupled atmosphere-slab ocean model. Our results suggest that anthropogenic and biomass burning aerosols generally induce a reduction in mean summer monsoon precipitation over most parts of the Indian subcontinent, strongest along the western coastline of the Indian peninsula and eastern Nepal region, but modest increases also occur over the north western part of the subcontinent. While most of the noted reduction in precipitation is triggered by increasedmore » emissions of aerosols from anthropogenic activities, modest increases in the north west are mostly associated with decreases in local emissions of aerosols from forest fire and grass fire sources. Anthropogenic aerosols from outside Asia also contribute to the overall reduction in precipitation but the dominant contribution comes from aerosol sources within Asia. Local emissions play a more important role in the total rainfall response to anthropogenic aerosol sources during the early monsoon period, whereas both local as well as remote emissions of aerosols play almost equally important roles during the later part of the monsoon period. While precipitation responses are primarily driven by local aerosol forcing, regional surface temperature changes over the region are strongly influenced by anthropogenic aerosols from sources further away (non-local changes). Changes in local anthropogenic organic and black carbon emissions by as much as a factor of two (preserving their ratio) produce the same basic signatures in the model's summer monsoon temperature and precipitation responses.« less

Po-210 and Pb-210 as atmospheric tracers and global atmospheric Pb-210 fallout: a review.

PubMed

Baskaran, M

2011-05-01

Over the past ∼ 5 decades, the distribution of (222)Rn and its progenies (mainly (210)Pb, (210)Bi and (210)Po) have provided a wealth of information as tracers to quantify several atmospheric processes that include: i) source tracking and transport time scales of air masses; ii) the stability and vertical movement of air masses iii) removal rate constants and residence times of aerosols; iv) chemical behavior of analog species; and v) washout ratios and deposition velocities of aerosols. Most of these applications require that the sources and sink terms of these nuclides are well characterized. Utility of (210)Pb, (210)Bi and (210)Po as atmospheric tracers requires that data on the (222)Rn emanation rates is well documented. Due to low concentrations of (226)Ra in surface waters, the (222)Rn emanation rates from the continent is about two orders of magnitude higher than that of the ocean. This has led to distinctly higher (210)Pb concentrations in continental air masses compared to oceanic air masses. The highly varying concentrations of (210)Pb in air as well the depositional fluxes have yielded insight on the sources and transit times of aerosols. In an ideal enclosed air mass (closed system with respect to these nuclides), the residence times of aerosols obtained from the activity ratios of (210)Pb/(222)Rn, (210)Bi/(210)Pb, and (210)Po/(210)Pb are expected to agree with each other, but a large number of studies have indicated discordance between the residence times obtained from these three pairs. Recent results from the distribution of these nuclides in size-fractionated aerosols appear to yield consistent residence time in smaller-size aerosols, possibly suggesting that larger size aerosols are derived from resuspended dust. The residence times calculated from the (210)Pb/(222)Rn, (210)Bi/(210)Pb, and (210)Po/(210)Pb activity ratios published from 1970's are compared to those data obtained in size-fractionated aerosols in this decade and possible reasons for the discordance is discussed with some key recommendations for future studies. The existing global atmospheric inventory data of (210)Pb is re-evaluated and a 'global curve' for the depositional fluxes of (210)Pb is established. A current global budget for atmospheric (210)Po and (210)Pb is also established. The relative importance of dry fallout of (210)Po and (210)Pb at different latitudes is evaluated. The global values for the deposition velocities of aerosols using (210)Po and (210)Pb are synthesized. Copyright © 2010 Elsevier Ltd. All rights reserved.

Aerosol, cloud, and precipitation interactions in Eastern North Atlantic

NASA Astrophysics Data System (ADS)

Wang, J.; Wood, R.; Dong, X.

2017-12-01

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, ENA is periodically impacted by anthropogenic aerosol both from North American and from continental Europe, making it an excellent location to study the CCN budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA), funded by DOE Atmospheric Radiation Measurement (ARM) program, is designed to improve the understanding of marine boundary CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation in the ENA by combining airborne observations and long term surface based measurements. The study has two airborne deployments. The first deployment took place from June 15 to July 25, 2017, and the second one will take place from January 10 to February 20, 2018. Flights during the first deployment were carried out in the Azores, near the ARM ENA site on Graciosa Island. The long term measurements at the ENA site provide important Climatological context for the airborne observations during the two deployments, and the cloud structures provided by the scanning radars at the ENA site put the detailed in-situ measurements into mesoscale and cloud lifecycle contexts. Another important aspect of this study is to provide high quality in-situ measurements for validating and improving ground-based retrieval algorithms at the ENA site. This presentation will describe the setup and strategies of the study, early results from the first deployment on vertical structures and horizontal variabilities of aerosol properties, cloud and drizzle microphysics, and insights into the processes that drive the properties and interactions of aerosol and marine low clouds.

Evidencing lead deposition at the urban scale using "short-lived" isotopic signatures of the source term (Pb-Zn refinery)

NASA Astrophysics Data System (ADS)

Franssens, Matthias; Flament, Pascal; Deboudt, Karine; Weis, Dominique; Perdrix, Espéranza

2004-09-01

To demonstrate the ability of the lead isotope signature technique to evidence the spatial extent of an industrial Pb deposition plume at a local scale, dry deposition of lead in the urban environment of a Pb-Zn refinery was investigated, as a study case, using transient ("short-lived") isotopic signatures of the industrial source. Sampling campaigns were achieved in representative weather conditions, on an 8-h basis. Dry deposition rates measured downwind from refinery emissions (≈102-103 μg Pb m-2 h-1), cross-sectionally in a 3-5 km radius area around the plant, represent 10-100 times the urban background dry fallout, measured upwind, as well as fallout measured near other potential sources of anthropogenic Pb. The Pb-Zn refinery isotopic signature (approx. 1.100<206Pb/207Pb<1.135) is made identifiable, using the same set of Pb and Zn ores for 2 days before sampling and during field experiments, by agreement with the executive staff of the plant. This source signature is less radiogenic than signatures of urban background Pb aerosols (1.155<206Pb/207Pb<1.165) and minor sources of Pb aerosols (1.147<206Pb/207Pb<1.165). By a simple binary mixing model calculation, we established the extension of the industrial Pb deposition plume. Fifty to eighty percents of total lead settled by the dry deposition mode, 3-4 km away from the refinery, still have an industrial origin. That represents from 40 to 80 μg Pb m-2 h-1, in an area where the blood lead level exceeds 100 μg Pb l-1 for 30% of men and 12% of women living there. We demonstrate here that stable Pb isotope analysis is able to evidence the Pb dry deposition plume in stabilised aerodynamic conditions, using a short-lived source term, suggesting that this methodology is able to furnish valuable data to validate industrial Pb aerosols dispersion models, at the urban scale.

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

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

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

DOE PAGES

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; ...

2018-01-21

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well-constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (N a). These terms are further parameterized, and by assuming that on seasonal timescales N a is in steady state, the budget equation is rearranged to form a diagnostic equation for Nmore » a based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter N a concentrations are made using the simplified steady-state model and seasonal mean observed variables, and are found to match well with the observed N a. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g. precipitation rate, free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in N a, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.« less

Cough aerosol in healthy participants: fundamental knowledge to optimize droplet-spread infectious respiratory disease management

PubMed Central

2012-01-01

Background The Influenza A H1N1 virus can be transmitted via direct, indirect, and airborne route to non-infected subjects when an infected patient coughs, which expels a number of different sized droplets to the surrounding environment as an aerosol. The objective of the current study was to characterize the human cough aerosol pattern with the aim of developing a standard human cough bioaerosol model for Influenza Pandemic control. Method 45 healthy non-smokers participated in the open bench study by giving their best effort cough. A laser diffraction system was used to obtain accurate, time-dependent, quantitative measurements of the size and number of droplets expelled by the cough aerosol. Results Voluntary coughs generated droplets ranging from 0.1 - 900 microns in size. Droplets of less than one-micron size represent 97% of the total number of measured droplets contained in the cough aerosol. Age, sex, weight, height and corporal mass have no statistically significant effect on the aerosol composition in terms of size and number of droplets. Conclusions We have developed a standard human cough aerosol model. We have quantitatively characterized the pattern, size, and number of droplets present in the most important mode of person-to-person transmission of IRD: the cough bioaerosol. Small size droplets (< 1 μm) predominated the total number of droplets expelled when coughing. The cough aerosol is the single source of direct, indirect and/or airborne transmission of respiratory infections like the Influenza A H1N1 virus. Study design Open bench, Observational, Cough, Aerosol study PMID:22436202

Drivers of Seasonal Variability in Marine Boundary Layer Aerosol Number Concentration Investigated Using a Steady State Approach

NASA Astrophysics Data System (ADS)

Mohrmann, Johannes; Wood, Robert; McGibbon, Jeremy; Eastman, Ryan; Luke, Edward

2018-01-01

Marine boundary layer (MBL) aerosol particles affect the climate through their interaction with MBL clouds. Although both MBL clouds and aerosol particles have pronounced seasonal cycles, the factors controlling seasonal variability of MBL aerosol particle concentration are not well constrained. In this paper an aerosol budget is constructed representing the effects of wet deposition, free-tropospheric entrainment, primary surface sources, and advection on the MBL accumulation mode aerosol number concentration (Na). These terms are then parameterized, and by assuming that on seasonal time scales Na is in steady state, the budget equation is rearranged to form a diagnostic equation for Na based on observable variables. Using data primarily collected in the subtropical northeast Pacific during the MAGIC campaign (Marine ARM (Atmospheric Radiation Measurement) GPCI (GCSS Pacific Cross-Section Intercomparison) Investigation of Clouds), estimates of both mean summer and winter Na concentrations are made using the simplified steady state model and seasonal mean observed variables. These are found to match well with the observed Na. To attribute the modeled difference between summer and winter aerosol concentrations to individual observed variables (e.g., precipitation rate and free-tropospheric aerosol number concentration), a local sensitivity analysis is combined with the seasonal difference in observed variables. This analysis shows that despite wintertime precipitation frequency being lower than summer, the higher winter precipitation rate accounted for approximately 60% of the modeled seasonal difference in Na, which emphasizes the importance of marine stratocumulus precipitation in determining MBL aerosol concentrations on longer time scales.

Cough aerosol in healthy participants: fundamental knowledge to optimize droplet-spread infectious respiratory disease management.

PubMed

Zayas, Gustavo; Chiang, Ming C; Wong, Eric; MacDonald, Fred; Lange, Carlos F; Senthilselvan, Ambikaipakan; King, Malcolm

2012-03-21

The Influenza A H1N1 virus can be transmitted via direct, indirect, and airborne route to non-infected subjects when an infected patient coughs, which expels a number of different sized droplets to the surrounding environment as an aerosol. The objective of the current study was to characterize the human cough aerosol pattern with the aim of developing a standard human cough bioaerosol model for Influenza Pandemic control. 45 healthy non-smokers participated in the open bench study by giving their best effort cough. A laser diffraction system was used to obtain accurate, time-dependent, quantitative measurements of the size and number of droplets expelled by the cough aerosol. Voluntary coughs generated droplets ranging from 0.1 - 900 microns in size. Droplets of less than one-micron size represent 97% of the total number of measured droplets contained in the cough aerosol. Age, sex, weight, height and corporal mass have no statistically significant effect on the aerosol composition in terms of size and number of droplets. We have developed a standard human cough aerosol model. We have quantitatively characterized the pattern, size, and number of droplets present in the most important mode of person-to-person transmission of IRD: the cough bioaerosol. Small size droplets (< 1 μm) predominated the total number of droplets expelled when coughing. The cough aerosol is the single source of direct, indirect and/or airborne transmission of respiratory infections like the Influenza A H1N1 virus. Open bench, Observational, Cough, Aerosol study. © 2012 Zayas et al; licensee BioMed Central Ltd.

Chemical characteristics of North American surface layer outflow: Insights from Chebogue Point, Nova Scotia

NASA Astrophysics Data System (ADS)

Millet, Dylan B.; Goldstein, Allen H.; Holzinger, Rupert; Williams, Brent J.; Allan, James D.; Jimenez, José L.; Worsnop, Douglas R.; Roberts, James M.; White, Allen B.; Hudman, Rynda C.; Bertschi, Isaac T.; Stohl, Andreas

2006-12-01

We present a factor analysis-based method for differentiating air masses on the basis of source influence and apply the method to a broad suite of trace gas and aerosol measurements collected at Chebogue Point, Nova Scotia, during the summer of 2004 to characterize the chemical composition of atmospheric outflow from eastern North America. CO, ozone, and aerosol mass were elevated by 30%, 56%, and more than 300% at Chebogue Point during U.S. outflow periods. Organic aerosol mass was highest during U.S. pollution events, but made up the largest fraction (70%) of the total aerosol during periods of primary and especially secondary biogenic influence, indicating the importance of both anthropogenic and biogenic organic aerosol. Anthropogenic and oxygenated volatile organic compounds account for the bulk of the gas-phase organic carbon under most conditions; however, biogenic compounds are important in terms of chemical reactivity. Biogenic emissions thus have a significant impact on the chemistry of air masses downwind of the polluted northeastern United States. Using output from a global 3-D model of atmospheric composition (GEOS-Chem), we estimate that CO directly emitted from U.S. pollution sources makes up 28% of the total CO observed at Chebogue Point during U.S. outflow events and 19% at other times, although more work is needed to improve U.S. emission estimates for CO and other pollutants. We conclude that the effects of North American pollution on the chemistry of the western North Atlantic boundary layer are pervasive and not restricted to particular events.

A scoping review on bio-aerosols in healthcare and the dental environment.

PubMed

Zemouri, Charifa; de Soet, Hans; Crielaard, Wim; Laheij, Alexa

2017-01-01

Bio-aerosols originate from different sources and their potentially pathogenic nature may form a hazard to healthcare workers and patients. So far no extensive review on existing evidence regarding bio-aerosols is available. This study aimed to review evidence on bio-aerosols in healthcare and the dental setting. The objectives were 1) What are the sources that generate bio-aerosols?; 2) What is the microbial load and composition of bio-aerosols and how were they measured?; and 3) What is the hazard posed by pathogenic micro-organisms transported via the aerosol route of transmission? Systematic scoping review design. Searched in PubMed and EMBASE from inception to 09-03-2016. References were screened and selected based on abstract and full text according to eligibility criteria. Full text articles were assessed for inclusion and summarized. The results are presented in three separate objectives and summarized for an overview of evidence. The search yielded 5,823 studies, of which 62 were included. Dental hand pieces were found to generate aerosols in the dental settings. Another 30 sources from human activities, interventions and daily cleaning performances in the hospital also generate aerosols. Fifty-five bacterial species, 45 fungi genera and ten viruses were identified in a hospital setting and 16 bacterial and 23 fungal species in the dental environment. Patients with certain risk factors had a higher chance to acquire Legionella in hospitals. Such infections can lead to irreversible septic shock and death. Only a few studies found that bio-aerosol generating procedures resulted in transmission of infectious diseases or allergic reactions. Bio-aerosols are generated via multiple sources such as different interventions, instruments and human activity. Bio-aerosols compositions reported are heterogeneous in their microbiological composition dependent on the setting and methodology. Legionella species were found to be a bio-aerosol dependent hazard to elderly and patients with respiratory complaints. But all aerosols can be can be hazardous to both patients and healthcare workers.

Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

EPA Science Inventory

ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

Time resolved aerosol monitoring in the urban centre of Soweto

NASA Astrophysics Data System (ADS)

Formenti, P.; Annegarn, H. J.; Piketh, S. J.

1998-03-01

A programme of aerosol sampling was conducted from 1982 to 1984 in the urban area of Soweto, Johannesburg, South Africa. The particulate matter (aerodynamic diameter <15 μm) was collected using a two hours time resolution single stage streaker sampler and elemental concentrations were resolved via Particle Induced X-ray Emission (PIXE) analysis. Samples have been selected for analysis from an aerosol sample archive to establish base-line atmospheric conditions that existed in Soweto prior to large scale electrification, and to establish source apportionment of crustal elements between coal smoke and traffic induced road dust, based on chemical elemental measurements. A novel technique is demonstrated for processing PIXE-derived time sequence elemental concentration vectors. Slowly varying background components have been extracted from sulphur and crustal aerosol components, using alternatively two digital filters: a moving minimum, and a moving average. The residuals of the crustal elements, assigned to locally generated aerosol components, were modelled using surrogate tracers: sulphur as a surrogate for coal smoke; and Pb as a surrogate for traffic activity. Results from this source apportionment revealed coal emissions contributed between 40% and 50% of the aerosol mineral matter, while 18-22% originated from road dust. Background aerosol, characteristic of the regional winter aerosol burden over the South African Highveld, was between 12% and 21%. Minor contributors identified included a manganese smelter, located 30 km from the sampling site, and informal trash burning, as the source of intermittent heavy metals (Cu, Zn). Elemental source profiles derived for these various sources are presented.

Urban emission, Santa Ana wind, and fire sources of aerosol nitrogen in Southern California

NASA Astrophysics Data System (ADS)

Mackey, K. R.; Stragier, S.; Robledo, L.; Cat, L. A.; Czimczik, C. I.

2017-12-01

Southern California is a highly urbanized region surrounded by extensive areas of agriculture and wilderness. While emissions from fossil fuel combustion are a large source of aerosol NOx in urban areas, fires contribute considerable aerosol NOx and ammonium in undeveloped regions. Southern California also has frequent wildfires, particularly during dry Santa Ana wind events that occur periodically throughout the winter. To explore the relative contributions of these sources to aerosol nitrogen content, we collected aerosol samples over two years in Irvine, a city in Southern California approximately 6 km from the Pacific coast. Samples were analyzed for total nitrogen and carbon content and isotopic composition (δ15N and δ13C), and nitrate and ammonium content. Carbon content was higher and δ13C values were lower in the winter than the summer. The C/N ratios of two samples collected during a Santa Ana wind event in January of 2012 were particularly elevated (C/N of 22 and 30) relative to other samples (C/N 3-6). We found that ammonium comprised 35% of total aerosol N across samples (R2=0.65), and that the δ15N of aerosol nitrogen decreased logarithmically as the proportion of nitrate in the sample increased (R2=0.60). Aerosol deposition of bioavailable nitrate and ammonium from these sources may support primary productivity in Southern California's coastal waters, particularly during the winter months and El Nino periods when upwelled nutrient sources are limited.

Long range transport and mixing of aerosol sources during the 2013 North American biomass burning episode: analysis of multiple lidar observations in the Western Mediterranean basin

NASA Astrophysics Data System (ADS)

Ancellet, G.; Pelon, J.; Totems, J.; Chazette, P.; Bazureau, A.; Sicard, M.; Di Iorio, T.; Dulac, F.; Mallet, M.

2015-11-01

Long range transport of biomass burning (BB) aerosols between North America and the Mediterranean region took place in June 2013. A large number of ground based and airborne lidar measurements were deployed in the Western Mediterranean during the Chemistry-AeRosol Mediterranean EXperiment (ChArMEx) intensive observation period. A detailed analysis of the potential North American aerosol sources is conducted including the assessment of their transport to Europe using forward simulations of the FLEXPART Lagrangian particle dispersion model initialized using satellite observations by MODIS and CALIOP. The three dimensional structure of the aerosol distribution in the ChArMEx domain observed by the ground-based lidars (Menorca, Barcelona and Lampedusa), a Falcon-20 aircraft flight and three CALIOP tracks, agree very well with the model simulation of the three major sources considered in this work: Canadian and Colorado fires, a dust storm from Western US and the contribution of Saharan dust streamers advected from the North Atlantic trade wind region into the Westerlies region. Four aerosol types were identified using the optical properties of the observed aerosol layers (aerosol depolarization ratio, lidar ratio) and the transport model analysis of the contribution of each aerosol source: (I) pure BB layer, (II) weakly dusty BB, (III) significant mixture of BB and dust transported from the trade wind region (IV) the outflow of Saharan dust by the subtropical jet and not mixed with BB aerosol. The contribution of the Canadian fires is the major aerosol source during this episode while mixing of dust and BB is only significant at altitude above 5 km. The mixing corresponds to a 20-30 % dust contribution in the total aerosol backscatter. The comparison with the MODIS AOD horizontal distribution during this episode over the Western Mediterranean sea shows that the Canadian fires contribution were as large as the direct northward dust outflow from Sahara.

Source apportionment of airborne particulates through receptor modeling: Indian scenario

NASA Astrophysics Data System (ADS)

Banerjee, Tirthankar; Murari, Vishnu; Kumar, Manish; Raju, M. P.

2015-10-01

Airborne particulate chemistry mostly governed by associated sources and apportionment of specific sources is extremely essential to delineate explicit control strategies. The present submission initially deals with the publications (1980s-2010s) of Indian origin which report regional heterogeneities of particulate concentrations with reference to associated species. Such meta-analyses clearly indicate the presence of reservoir of both primary and secondary aerosols in different geographical regions. Further, identification of specific signatory molecules for individual source category was also evaluated in terms of their scientific merit and repeatability. Source signatures mostly resemble international profile while, in selected cases lack appropriateness. In India, source apportionment (SA) of airborne particulates was initiated way back in 1985 through factor analysis, however, principal component analysis (PCA) shares a major proportion of applications (34%) followed by enrichment factor (EF, 27%), chemical mass balance (CMB, 15%) and positive matrix factorization (PMF, 9%). Mainstream SA analyses identify earth crust and road dust resuspensions (traced by Al, Ca, Fe, Na and Mg) as a principal source (6-73%) followed by vehicular emissions (traced by Fe, Cu, Pb, Cr, Ni, Mn, Ba and Zn; 5-65%), industrial emissions (traced by Co, Cr, Zn, V, Ni, Mn, Cd; 0-60%), fuel combustion (traced by K, NH4+, SO4-, As, Te, S, Mn; 4-42%), marine aerosols (traced by Na, Mg, K; 0-15%) and biomass/refuse burning (traced by Cd, V, K, Cr, As, TC, Na, K, NH4+, NO3-, OC; 1-42%). In most of the cases, temporal variations of individual source contribution for a specific geographic region exhibit radical heterogeneity possibly due to unscientific orientation of individual tracers for specific source and well exaggerated by methodological weakness, inappropriate sample size, implications of secondary aerosols and inadequate emission inventories. Conclusively, a number of challenging issues and specific recommendations have been included which need to be considered for a scientific apportionment of particulate sources in different geographical regions of India.

Organic aerosol components derived from 25 AMS datasets across Europe using a newly developed ME-2 based source apportionment strategy

NASA Astrophysics Data System (ADS)

Crippa, M.; Canonaco, F.; Lanz, V. A.; Äijälä, M.; Allan, J. D.; Carbone, S.; Capes, G.; Dall'Osto, M.; Day, D. A.; DeCarlo, P. F.; Di Marco, C. F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J.-L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Mensah, A. A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S. N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2013-09-01

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of EUCAARI and the intensive campaigns of EMEP during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we propose a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 datasets accounting for urban, rural, remote and high altitude sites and therefore it is likely suitable for the treatment of AMS-related ambient datasets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling evaluation purposes.

Antarctic new particle formation from continental biogenic precursors

NASA Astrophysics Data System (ADS)

Kyrö, E.-M.; Kerminen, V.-M.; Virkkula, A.; Dal Maso, M.; Parshintsev, J.; Ruíz-Jimenez, J.; Forsström, L.; Manninen, H. E.; Riekkola, M.-L.; Heinonen, P.; Kulmala, M.

2012-12-01

Over Antarctica, aerosol particles originate almost entirely from marine areas, with minor contribution from long-range transported dust or anthropogenic material. The Antarctic continent itself, unlike all other continental areas, has been thought to be practically free of aerosol sources. Here we present evidence of local aerosol production associated with melt-water ponds in the continental Antarctica. We show that in air masses passing such ponds, new aerosol particles are efficiently formed and these particles grow up to sizes where they may act as cloud condensation nuclei (CCN). The precursor vapours responsible for aerosol formation and growth originate very likely from highly abundant cyanobacteria Nostoc commune (Vaucher) communities of local ponds. This is the first time when freshwater vegetation has been identified as an aerosol precursor source. The influence of the new source on clouds and climate may increase in future Antarctica, and possibly elsewhere undergoing accelerating summer melting of semi-permanent snow cover.

Antarctic new particle formation from continental biogenic precursors

NASA Astrophysics Data System (ADS)

Kyrö, E.-M.; Kerminen, V.-M.; Virkkula, A.; Dal Maso, M.; Parshintsev, J.; Ruíz-Jimenez, J.; Forsström, L.; Manninen, H. E.; Riekkola, M.-L.; Heinonen, P.; Kulmala, M.

2013-04-01

Over Antarctica, aerosol particles originate almost entirely from marine areas, with minor contribution from long-range transported dust or anthropogenic material. The Antarctic continent itself, unlike all other continental areas, has been thought to be practically free of aerosol sources. Here we present evidence of local aerosol production associated with melt-water ponds in continental Antarctica. We show that in air masses passing such ponds, new aerosol particles are efficiently formed and these particles grow up to sizes where they may act as cloud condensation nuclei (CCN). The precursor vapours responsible for aerosol formation and growth originate very likely from highly abundant cyanobacteria Nostoc commune (Vaucher) communities of local ponds. This is the first time freshwater vegetation has been identified as an aerosol precursor source. The influence of the new source on clouds and climate may increase in future Antarctica, and possibly elsewhere undergoing accelerating summer melting of semi-permanent snow cover.

Physical and Chemical Properties of Anthropogenic Aerosols: An overview

EPA Science Inventory

A wide variety of anthropogenic sources emit fine aerosols to the atmosphere. The physical and chemical properties of these aerosols are of interest due to their influence on climate, human health, and visibility. Aerosol chemical composition is complex. Combustion aerosols can c...

Day-night differences in the composition and sources of carbonaceous aerosol at a polluted regional background site in the Netherlands

NASA Astrophysics Data System (ADS)

Dusek, Ulrike; Broekema, Elise; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro

2017-04-01

The origin of carbonaceous aerosol differs during day- and night-time, because emissions from major sources such as traffic, biomass combustion, and secondary organic aerosol formation show a distinct diurnal pattern. Moreover, photochemical processing and evaporation of semi-volatile organic compounds are enhanced during day-time, due to the availability of sunlight and higher temperatures. Assessing day-night differences in sources and chemical composition can give an indication of the importance of local/regional carbon sources and processing, since day-night differences should be averaged out during long-range transport. If local sources dominate, one could expect a strong diurnal variation in the source profile, but if long-range transport dominates the diurnal variation would be much weaker. In this study we measure the isotopic (14C and 13C) and detailed chemical composition of the organic fraction of the aerosol on high volume PM2.5 filter samples that were collected separately during day and night time. Radiocarbon (14C) measurements are used to estimate three main aerosol sources of organic and elemental carbon (OC and EC): Fossil fuel combustion (ff), biomass combustion (bb), and biogenic sources (bio). The detailed chemical and stable isotopic composition are measured at different desorption temperatures from the filter, which separates the more and less refractory organic compounds. The composition of the organic aerosol is measured using an thermal-desporption Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) method (Holzinger et al, 2010) and the stable isotopic composition is measured using a thermal desorption IRMS method (Dusek et al., 2013). Source apportionment results using 14C show that the contribution of fossil fuel combustion to EC and OC is higher during day-time than during night-time. This is valid for all seasons. During night-time biomass combustion plays a bigger role as a source of carbonaceous aerosol. Even in the summer, when biomass combustion is a small source, its relative contribution increases between 19:00 and 07:00. However, the diurnal changes in source contributions are relatively moderate (e.g., the biomass burning contribution to TC increased from 31% to 43% for the winter sample with the most distinct day-night difference.) This highlights the importance of long-range transport as a source of the carbonaceous aerosol in this region. First results from chemical composition measurements on four of the samples show that the concentration of less refractory organic carbon (desorption temperature up to 200 °C) increases at night-time much more strongly than the concentration of the more refractory carbon. Similarly, the concentration of small organic compounds with m/z < 100 also increases more strongly than heavier compounds. This indicates partitioning of semi-volatile OC as a possible additional night-time source. The chemical composition will be studied in more detail, focusing on diurnal changes in O/C ratios, individual compounds and compound classes, such as hydrocarbons or organic acids. Dusek, U., Meusinger, C., Oyama, B., Ramon, W., de Wilde, P., Holzinger, R., and Röckmann, T.: A thermal desorption system for measuring δ 13 C ratios on organic aerosol, Journal of aerosol science, 66, 72-82, 2013. Holzinger, R., Williams, J., Herrmann, F., Lelieveld, J., Donahue, N., Röckmann, T., 2010. Aerosol analysis using a Thermal-Desorption Proton-Transfer-Reaction Mass Spectrometer (TD-PTR-MS): a new approach to study processing of organic aerosols. Atmospheric chemistry and physics 10, 2257-2267.

Potential source identification for aerosol concentrations over a site in Northwestern India

NASA Astrophysics Data System (ADS)

Payra, Swagata; Kumar, Pramod; Verma, Sunita; Prakash, Divya; Soni, Manish

2016-03-01

The collocated measurements of aerosols size distribution (ASD) and aerosol optical thickness (AOT) are analyzed simultaneously using Grimm aerosol spectrometer and MICROTOP II Sunphotometer over Jaipur, capital of Rajasthan in India. The contrast temperature characteristics during winter and summer seasons of year 2011 are investigated in the present study. The total aerosol number concentration (TANC, 0.3-20 μm) during winter season was observed higher than in summer time and it was dominated by fine aerosol number concentration (FANC < 2 μm). Particles smaller than 0.8 μm (at aerodynamic size) constitute ~ 99% of all particles in winter and ~ 90% of particles in summer season. However, particles greater than 2 μm contribute ~ 3% and ~ 0.2% in summer and winter seasons respectively. The aerosols optical thickness shows nearly similar AOT values during summer and winter but corresponding low Angstrom Exponent (AE) values during summer than winter, respectively. In this work, Potential Source Contribution Function (PSCF) analysis is applied to identify locations of sources that influenced concentrations of aerosols over study area in two different seasons. PSCF analysis shows that the dust particles from Thar Desert contribute significantly to the coarse aerosol number concentration (CANC). Higher values of the PSCF in north from Jaipur showed the industrial areas in northern India to be the likely sources of fine particles. The variation in size distribution of aerosols during two seasons is clearly reflected in the log normal size distribution curves. The log normal size distribution curves reveals that the particle size less than 0.8 μm is the key contributor in winter for higher ANC.

A Water Mass Tracer Detected in Aerosols Demonstrates Ocean-Atmosphere Mass Transfer and Links Sea Spray Aerosol to Source Waters

NASA Astrophysics Data System (ADS)

Pendergraft, M.; Grimes, D. J.; Giddings, S. N.; Feddersen, F.; Prather, K. A.; Santander, M.; Lee, C.; Beall, C.

2016-12-01

During September and October of 2015 the Cross Surfzone/Inner-shelf Dye Exchange (CSIDE) project released rhodamine WT dye to study nearshore water movement and exchange offshore along a Southern California sandy beach. We utilized this opportunity to investigate ocean-atmosphere mass transfer via sea spray aerosol and linkage to source waters. Aerosol-concentrating sampling equipment was deployed at beachside and inland locations during three dye releases. Concentrated aerosol samples were analyzed for dye content using fluorescence spectroscopy. Here we present the ocean and atmosphere conditions associated with the presence and absence of dye in aerosol samples. Dye was identified in aerosol samples collected 0.1-0.3 km from the shoreline for 6 hs during the first and third dye releases of the CSIDE project. During these releases the dye persisted in the waters upwind of the sampling equipment. Dye was not detected in aerosol samples collected during the second release during which dye was moved away from waters upwind of the sampling equipment. Recovery of a chemical tracer in sea spray aerosol allows direct linkage to a known source area in the ocean that is independent of, but supported by, wind data. Our observations demonstrate: a tight ocean-atmosphere spatial coupling; a short residence time of coastal marine constituents before transfer to the atmosphere; that the ocean is both a sink for and a source of atmospheric and terrestrial material; and that human inputs to the ocean can return to us in sea spray aerosol.

Wintertime characteristics of aerosols over middle Indo-Gangetic Plain: Vertical profile, transport and radiative forcing

NASA Astrophysics Data System (ADS)

Kumar, M.; Raju, M. P.; Singh, R. K.; Singh, A. K.; Singh, R. S.; Banerjee, T.

2017-01-01

Winter-specific characteristics of airborne particulates over middle Indo-Gangetic Plain (IGP) were evaluated in terms of aerosol chemical and micro-physical properties under three-dimensional domain. Emphases were made for the first time to identify intra-seasonal variations of aerosols sources, horizontal and vertical transport, effects of regional meteorology and estimating composite aerosol short-wave radiative forcing over an urban region (25°10‧-25°19‧N; 82°54‧-83°4‧E) at middle-IGP. Space-borne passive (Aqua and Terra MODIS, Aura OMI) and active sensor (CALIPSO-CALIOP) based observations were concurrently used with ground based aerosol mass measurement for entire winter and pre-summer months (December, 1, 2014 to March, 31, 2015). Exceptionally high aerosol mass loading was recorded for both PM10 (267.6 ± 107.0 μg m- 3) and PM2.5 (150.2 ± 89.4 μg m- 3) typically exceeding national standard. Aerosol type was mostly dominated by fine particulates (particulate ratio: 0.61) during pre to mid-winter episodes before being converted to mixed aerosol types (ratio: 0.41-0.53). Time series analysis of aerosols mass typically identified three dissimilar aerosol loading episodes with varying attributes, well resemble to that of previous year's observation representing its persisting nature. Black carbon (9.4 ± 3.7 μg m- 3) was found to constitute significant proportion of fine particulates (2-27%) with a strong diurnal profile. Secondary inorganic ions also accounted a fraction of particulates (PM2.5: 22.5%; PM10: 26.9%) having SO4- 2, NO3- and NH4+ constituting major proportion. Satellite retrieved MODIS-AOD (0.01-2.30) and fine mode fractions (FMF: 0.01-1.00) identified intra-seasonal variation with transport of aerosols from upper to middle-IGP through continental westerly. Varying statistical association of columnar and surface aerosol loading both in terms of fine (r; PM2.5: MODIS-AOD: 0.51) and coarse particulates (PM10: MODIS-AOD: 0.53) was found influenced by local meteorology (boundary layer and humidity) and aerosol vertical profile. A gradual increase in aerosol vertical profile (surface to 4.9 km) was evident with dominance of polluted continental, polluted dust and smoke at lower altitude. Presence of mineral dusts in higher altitude during later phase was linked with its transboundary transport, originating from western dry regions. Conclusively, winter-specific short-wave aerosol radiative forcing revealed an ATM warming effect (31-47 W m- 2) while cooling both at TOA (- 20 to - 32 W m- 2) and SUF (- 51 to - 80 W m- 2) with significant level of intra-seasonal variations in heating rates (0.86-1.32 K day- 1).

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 particle formation has not been observed.

Properties of transported African mineral dust aerosols in the Mediterranean region

NASA Astrophysics Data System (ADS)

Denjean, Cyrielle; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Triquet, Sylvain; Zapf, Pascal; Loisil, Rodrigue; Bourrianne, Thierry; Freney, Evelyn; Dupuy, Regis; Sellegri, Karine; Schwarzenbock, Alfons; Torres, Benjamin; Mallet, Marc; Cassola, Federico; Prati, Paolo; Formenti, Paola

2015-04-01

The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), one intensive airborne campaign (ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) has been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport from known but differing origins (source regions in Tunisia, Algeria, and Mauritania) and at different times after transport, will be presented. Results will be compared to equivalent measurements over source regions interpreted in terms of the evolution of the particle size distribution, chemical composition and optical properties.

Differences in the OC/EC Ratios that Characterize Ambient and Source Aerosols due to Thermal-Optical Analysis

EPA Science Inventory

Thermal-optical analysis (TOA) is typically used to measure the OC/EC (organic carbon/elemental carbon) and EC/TC (elemental carbon/total carbon) ratios in source and atmospheric aerosols. The present study utilizes a dual-optical carbon aerosol analyzer to examine the effects of...

Intercontinental Transport of Aerosols: Implication for Regional Air Quality

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Ginoux, Paul

2006-01-01

Aerosol particles, also known as PM2.5 (particle diameter less than 2.5 microns) and PM10 (particle diameter less than 10 microns), is one of the key atmospheric components that determine ambient air quality. Current US air quality standards for PM10 (particles with diameter < 10 microns) and PM2.5 (particles with diameter 2.5 microns) are 50 pg/cu m and 15 pg/cu m, respectively. While local and regional emission sources are the main cause of air pollution problems, aerosols can be transported on a hemispheric or global scale. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to quantify contributions of long-range transport vs. local/regional pollution sources and from natural vs. anthropogenic sources to PM concentrations different regions. In particular, we estimate the hemispheric impact of anthropogenic sulfate aerosols and dust from major source areas on other regions in the world. The GOCART model results are compared with satellite remote sensing and ground-based network measurements of aerosol optical depth and concentrations.

Regional transport of a chemically distinctive dust: Gypsum from White Sands, New Mexico (USA)

NASA Astrophysics Data System (ADS)

White, Warren H.; Hyslop, Nicole P.; Trzepla, Krystyna; Yatkin, Sinan; Rarig, Randy S.; Gill, Thomas E.; Jin, Lixin

2015-03-01

The White Sands complex, a National Monument and adjoining Missile Range in southern New Mexico, occupies the dry bed of an ice-age lake where an active gypsum dunefield abuts erodible playa sediments. Aerosols entrained from White Sands are sometimes visible on satellite images as distinct, light-colored plumes crossing the Sacramento Mountains to the east and northeast. The IMPROVE network (Interagency Monitoring of PROtected Visual Environments) operates long-term aerosol samplers at two sites east of the Sacramento range. In recent years a spring pulse of sulfate aerosol has appeared at these sites, eclipsing the regional summer peak resulting from atmospheric reactions of sulfur dioxide emissions. A significant fraction of this spring sulfate is contributed by gypsum and other salts from White Sands, with much of the sulfur in coarse particles and concentrations of calcium and strontium above regional levels. The increase in these gypsiferous species coincides with a drought following a period of above-average precipitation. White Sands and the IMPROVE samplers together provide a natural laboratory: a climatically sensitive dust source that is both well characterized and chemically distinct from its surroundings, with a signature that remains identifiable at long-term observatories 100-200 km downwind.

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

NASA Astrophysics Data System (ADS)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

Monitoring the industrial sources of aerosol in Cubatao, Brazil, using a scanning elastic lidar and a lidar doppler

NASA Astrophysics Data System (ADS)

da Costa, Renata F.; Marques, Marcia T. A.; M Macedo, Fernanda de; Andrade, Izabel da Silva; Araujo, Elaine Cristina; Correa, Thais; de Andrade Salani, Maria Helena Goncalves; Lopes, Daniel Silveira; Goncalves Guardani, Maria Lucia; Landulfo, Eduardo; Guardani, Roberto

2018-04-01

Field campaigns with a scanning multiwavelength elastic lidar coupled with a Doppler system to monitor industrial atmospheric aerosol emissions were carried out, with the objective of monitoring aerosol emission sources and plume dispersion. Since the technique provides information on the spatial and temporal distribution of aerosol concentration, the implementation of a systematic monitoring procedure is proposed as a valuable tool in air quality monitoring applied to regions of interest.

Determination of mixing state and sources of wintertime organic aerosol in Paris using single particle mass spectrometry

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Wiedensohler, A.; Jeong, C.; McGuire, M.; Evans, G. J.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Wenger, J.

2012-12-01

The size-resolved chemical composition of single particles at an urban background site in Paris, France, was determined using an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) as part of the MEGAPOLI winter campaign in January/February 2010. A variety of mixing states were identified for organic aerosol by mass spectral clustering and apportioned to both fossil fuel and biomass burning sources. The ATOFMS data were scaled in order to produce mass concentration estimates for each organic aerosol particle type identified. Potassium-containing organic aerosol internally mixed with nitrate, associated with local wood burning, was observed to dominate during periods characterised by marine air masses. Sulfate-rich potassium-containing organic aerosol, associated with transboundary transport of biomass burning emissions, dominated during periods influenced by continental air masses. The scaled total mass concentration for potassium-containing particles was well correlated (R2 = 0.79) with concurrent measurements of potassium mass concentration measured with a Particle-Into-Liquid-Sampler (PILS). Another organic particle type, also containing potassium but rich in trimethylamine and sulfate, was detected exclusively during continental air mass events. These particles are postulated to have accumulated gas phase trimethylamine through heterogeneous reaction before arriving at the sampling site. Potential source regions for transboundary organic aerosols have been investigated using the potential source contribution function (PSCF). Comparison with aerosol mass spectrometer (AMS) measurements will also be discussed.

Long term change in atmospheric dust absorption, dust scattering and black carbon aerosols scattering coefficient parameters over western Indian locations

NASA Astrophysics Data System (ADS)

Satoliya, Anil Kumar; Vyas, B. M.; Shekhawat, M. S.

2018-05-01

The first time satellite space based measurement of atmospheric black carbon (BC) aerosols scattering coefficient at 550nm (BC SC at 550nm), dust aerosols scattering and dust aerosols extinction coefficient (DSC at 550nm and DEC at 550nm) parameters have been used to understand their long term trend of natural and anthropogenic aerosols behavior with its close association with ground based measured precipitation parameters such as Total Rain Fall (TRF), and Total Number of Rainy Days (TNRD) for the same period over western Indian regions concerned to the primary aerosols sources of natural activities. The basic objective of this study is an attempt to investigate the inter-correlation between dust and black carbon aerosols loading characteristics with a variation of rainfall pattern parameters as indirect aerosols induced effect i.e., aerosols-cloud interaction. The black carbon aerosols generated by diverse anthropogenic or human made activities are studied by choosing of measured atmospheric BC SC at 550nm parameter, whereas desert dust mineral aerosols primarily produced by varieties of natural activities pre-dominated of dust mineral desert aerosols mainly over Thar desert influenced area of hot climate and rural tropical site are investigated by selecting DSC at 550nm and DEC at 550nm of first semi-urban site i.e., Udaipur (UDP, 24.6°N, 73.35°E, 580m above surface level (asl)) situated in southern Rajasthan part as well as over other two Great Indian Thar desert locations i.e., Jaisalmer (JSM, 26.90°N, 69.90°E, 220m asl)) and Bikaner (BKN, 28.03°N, 73.30°E, 224m asl) located in the vicinity of the Thar desert region situated in Rajasthan state of the western Indian region. The source of the present study would be collection of longer period of monthly values of the above parameters of spanning 35 years i.e., 1980 to 2015. Such types of atmospheric aerosols-cloud monsoon interaction investigation is helpful in view of understanding their direct and indirect aerosols active role of optical absorption and scattering of solar light radiation at useful wavelength 550nm as well as heating of clouds over least explored region, i.e., the Thar desert region and also away from less dust dominated influenced provinces for longer period. The analysis of the above the result would also give a clear scientific evidence of alteration in enhancement in DSC at 550nm and DEC at 550nm and BC SC at 550nm variables with simultaneous corresponding reduction in the five yearly mean precipitation activity parameters such as TRF and TNRD. It is quite evident that anthropogenic BC aerosols activity are showing the significant increasing trend at all three locations, but it is more prominent over central Thar Desert influenced regime, i.e., JSM and BKN relative to semi-urban region i.e., UDP. The systematic increasing pattern of average monthly mean value of DSC at 550nm and DEC at 550nm or increasing aerosol loading have been revealed from acquiring their lowest value in January month and the highest values in July and retained with the broad peak values in pre-monsoon months. Subsequently, their respective values reduce sharply downward from August to December onwards. The mountain value of dust aerosols parameters, i.e., DSC at 550nm and DEC at 550nm are systematically enhanced toward from UDP to BKN and then maximized at JSM. It is clearly obvious fact that the following ascending order of desert aerosols loading influenced activity in different areas has been recorded, i.e., JSM> BKN>UDP. Several other interesting features of the earth-climate change implication in reference to the altering nature of reduction of precipitation parameter pattern with simultaneous observed elevated dust aerosol and BC aerosol loading have been also noticed in the course of present investigation. Overall reduction in rainfall pattern effect with increasing of dust aerosols loading or vice versa are seen more pronounced over JSM and lees prevalence over UDP. The more detailed investigations about other interesting results of Aerosols-Indian monsoon over western Indian locations are also discussed thoroughly in this paper.

Impact of aerosol particle sources on optical properties in urban, regional and remote areas in the north-western Mediterranean

NASA Astrophysics Data System (ADS)

Ealo, Marina; Alastuey, Andrés; Pérez, Noemí; Ripoll, Anna; Querol, Xavier; Pandolfi, Marco

2018-01-01

Further research is needed to reduce the existing uncertainties on the effect that specific aerosol particle sources have on light extinction and consequently on climate. This study presents a new approach that aims to quantify the mass scattering and absorption efficiencies (MSEs and MAEs) of different aerosol sources at urban (Barcelona - BCN), regional (Montseny - MSY) and remote (Montsec - MSA) background sites in the north-western (NW) Mediterranean. An analysis of source apportionment to the measured multi-wavelength light scattering (σsp) and absorption (σap) coefficients was performed by means of a multilinear regression (MLR) model for the periods 2009-2014, 2010-2014 and 2011-2014 at BCN, MSY and MSA respectively. The source contributions to PM10 mass concentration, identified by means of the positive matrix factorization (PMF) model, were used as dependent variables in the MLR model. With this approach we addressed both the effect that aerosol sources have on air quality and their potential effect on light extinction through the determination of their MSEs and MAEs. An advantage of the presented approach is that the calculated MSEs and MAEs take into account the internal mixing of atmospheric particles. Seven aerosol sources were identified at MSA and MSY, and eight sources at BCN. Mineral, aged marine, secondary sulfate, secondary nitrate and V-Ni bearing sources were common at the three sites. Traffic, industrial/metallurgy and road dust resuspension sources were isolated at BCN, whereas mixed industrial/traffic and aged organics sources were identified at MSY and MSA. The highest MSEs were observed for secondary sulfate (4.5 and 10.7 m2 g-1, at MSY and MSA), secondary nitrate (8.8 and 7.8 m2 g-1) and V-Ni bearing source (8 and 3.5 m2 g-1). These sources dominated the scattering throughout the year with marked seasonal trends. The V-Ni bearing source, originating mainly from shipping in the area under study, simultaneously contributed to both σsp and σap, being the second most efficient light-absorbing source in BCN (MAE = 0.9 m2 g-1). The traffic source at BCN and the industrial/traffic at MSY exhibited the highest MAEs (1.7 and 0.9 m2 g-1). These sources were major contributors to σap at BCN and MSY; however at MSA, secondary nitrate exerted the highest influence on σap (MAE = 0.4 m2 g-1). The sources which were predominantly composed of fine and relatively dark particles, such as industrial/traffic, aged organics and V-Ni, were simultaneously characterized by low single scattering albedo (SSA) and a high scattering Ångström exponent (SAE). Conversely, mineral and aged marine showed the lowest SAE and the highest SSA, being scattering the dominant process in the light extinction. The good agreement found between modelled and measured particle optical properties allowed the reconstruction of σsp and σap long-term series over the period 2004-2014 at MSY. Significant decreasing trends were found for the modelled σsp and σap (-4.6 and -4.1 % yr-1).

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

NASA Astrophysics Data System (ADS)

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

2007-12-01

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

Observation of carbonaceous aerosols and carbon monoxide in Mid-Atlantic region: Seasonal and inter-annual variations

NASA Astrophysics Data System (ADS)

Chen, L. A.; Doddridge, B. G.; Doddridge, B. G.; Dickerson, R. R.; Dickerson, R. R.

2001-05-01

As part of Maryland Aerosol Research and Characterization (MARCH-Atlantic) study, a long-term monitoring of ambient elemental and organic carbon (EC and OC) aerosols has been made at Fort Meade, MD (39.16° N 76.51° W; elevation 46 m MSL), a suburban site within the Baltimore-Washington (B-W) corridor, since July 1999. 24-hr average EC and OC are measured every day during the season-representative months (July 1999, October 1999, January 2000, April 2000 and July 2000). Carbon monoxide (CO) was also measured nearly continuously over the period. Strong correlation between EC and CO (r = 0.7 ~ 0.9) in every month suggests common or proximate sources, likely traffic emissions. The EC versus CO slope, however, varies in different seasons and is found to increase nonlinearly with the ambient temperature. EC source strength may peak in summer. OC shows strong correlation with EC (r ~ 0.95) only in winter, suggesting that OC is also of the same primary sources during wintertime. The Interagency Monitoring of Protected Visual Environments (IMPROVE) network has been measuring EC and OC around the United States since 1988. The FME data during July 1999 are also compared with simultaneous measurements at nearby IMPROVE sites, showing B-W corridor could be a major contributor to the carbonaceous aerosols in the Mid-Atlantic region. A decreasing trend of EC level is found in three IMPROVE sites in this region. This actually agrees with the decreasing trend of CO observed previously at Big Meadow, Shenandoah National Park if CO and EC are both influenced by traffic emissions.

SOURCE APPORTIONMENT OF PHOENIX PM2.5 AEROSOL WITH THE UNMIX RECEPTOR MODEL

EPA Science Inventory

The multivariate receptor model Unmix has been used to analyze a 3-yr PM2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall percentage source contribution estimates (SCE) for five source categories: ga...

Characterization of infectious aerosols in health care facilities: an aid to effective engineering controls and preventive strategies.

PubMed

Cole, E C; Cook, C E

1998-08-01

Assessment of strategies for engineering controls for the prevention of airborne infectious disease transmission to patients and to health care and related workers requires consideration of the factors relevant to aerosol characterization. These factors include aerosol generation, particle size and concentrations, organism viability, infectivity and virulence, airflow and climate, and environmental sampling and analysis. The major focus on attention to engineering controls comes from recent increases in tuberculosis, particularly the multidrug-resistant varieties in the general hospital population, the severely immunocompromised, and those in at-risk and confined environments such as prisons, long-term care facilities, and shelters for the homeless. Many workers are in close contact with persons who have active, undiagnosed, or insufficiently treated tuberculosis. Additionally, patients and health care workers may be exposed to a variety of pathogenic human viruses, opportunistic fungi, and bacteria. This report therefore focuses on the nature of infectious aerosol transmission in an attempt to determine which factors can be systematically addressed to result in proven, applied engineering approaches to the control of infectious aerosols in hospital and health care facility environments. The infectious aerosols of consideration are those that are generated as particles of respirable size by both human and environmental sources and that have the capability of remaining viable and airborne for extended periods in the indoor environment. This definition precludes skin and mucous membrane exposures occurring from splashes (rather than true aerosols) of blood or body fluids containing infectious disease agents. There are no epidemiologic or laboratory studies documenting the transmission of bloodborne virus by way of aerosols.

AERONET-Based Nonspherical Dust Optical Models and Effects on the VIIRS Deep Blue/SOAR Over Water Aerosol Product

NASA Astrophysics Data System (ADS)

Lee, Jaehwa; Hsu, N. Christina; Sayer, Andrew M.; Bettenhausen, Corey; Yang, Ping

2017-10-01

Aerosol Robotic Network (AERONET)-based nonspherical dust optical models are developed and applied to the Satellite Ocean Aerosol Retrieval (SOAR) algorithm as part of the Version 1 Visible Infrared Imaging Radiometer Suite (VIIRS) NASA "Deep Blue" aerosol data product suite. The optical models are created using Version 2 AERONET inversion data at six distinct sites influenced frequently by dust aerosols from different source regions. The same spheroid shape distribution as used in the AERONET inversion algorithm is assumed to account for the nonspherical characteristics of mineral dust, which ensures the consistency between the bulk scattering properties of the developed optical models and the AERONET-retrieved microphysical and optical properties. For the Version 1 SOAR aerosol product, the dust optical model representative for Capo Verde site is used, considering the strong influence of Saharan dust over the global ocean in terms of amount and spatial coverage. Comparisons of the VIIRS-retrieved aerosol optical properties against AERONET direct-Sun observations at five island/coastal sites suggest that the use of nonspherical dust optical models significantly improves the retrievals of aerosol optical depth (AOD) and Ångström exponent by mitigating the well-known artifact of scattering angle dependence of the variables, which is observed when incorrectly assuming spherical dust. The resulting removal of these artifacts results in a more natural spatial pattern of AOD along the transport path of Saharan dust to the Atlantic Ocean; that is, AOD decreases with increasing distance transported, whereas the spherical assumption leads to a strong wave pattern due to the spurious scattering angle dependence of AOD.

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

PubMed

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

2016-08-16

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

Can Biomass Burning Explain Isotopically Light Fe in Marine Aerosols?

NASA Astrophysics Data System (ADS)

Sherry, A. M.; Anbar, A. D.; Herckes, P.; Romaniello, S. J.

2016-02-01

Iron (Fe) is an important micronutrient that limits primary productivity in large parts of the ocean. In these regions, atmospheric aerosol deposition is an important source of Fe to the surface ocean and thus has a critical impact on ocean biogeochemistry. Fe-bearing aerosols originate from many sources with potentially distinct Fe isotopic compositions. Consequently, Fe isotopes may provide a new tool to trace the sources of aerosol Fe to the oceans. Mead et al. (2013) first discovered that Fe in the fine fraction of Bermuda aerosols is often isotopically lighter than Fe from known anthropogenic and crustal sources. 1 These authors suggested that this light isotopic signature was likely the result of biomass burning, since Fe in plants is the only known source of isotopically light Fe. More recently, Conway et al. found that Fe in the soluble fraction of aerosols collected during 2010-2011 North Atlantic GEOTRACES cruises also showed light isotope values, which they likewise attributed to biomass burning.2 These studies are further supported by new modeling work which suggests that biomass burning aerosols should contribute significant amounts of soluble Fe to tropical and southern oceans.3To test if biomass burning releases aerosols with a light Fe isotope composition, we are conducting lab-scale biomass burning experiments using natural samples of vegetation and leaf litter. Burn aerosols were collected on cellulose filters, then digested and analyzed for trace metal concentrations using inductively-coupled mass spectrometry (ICP-MS). Fe isotopes were determined by using multiple collector ICP-MS following separation and purification of Fe using anion exchange chromatography. We will discuss metal concentration and isotope data from these experiments with implications for the interpretation of Fe isotope signals in aerosol samples. 1Mead, C et al. GRL, 2013, 40, 5722-5727. 2 Conway, T et al. Goldschmidt Abs 2015 593. 3Ito, A. ES&T Lett, 2015, 2, 70-75.

Submicron organic aerosol in Tijuana, Mexico, from local and Southern California sources during the CalMex campaign

NASA Astrophysics Data System (ADS)

Takahama, S.; Johnson, A.; Guzman Morales, J.; Russell, L. M.; Duran, R.; Rodriguez, G.; Zheng, J.; Zhang, R.; Toom-Sauntry, D.; Leaitch, W. R.

2013-05-01

The CalMex campaign was conducted from May 15 to June 30 of 2010 to study the properties and sources of air pollution in Tijuana, Mexico. In this study, submicron organic aerosol mass (OM) composition measured by Fourier Transform Infrared Spectroscopy (FTIR), Aerosol Chemical Speciation Monitor (ACSM), and X-ray spectromicroscopy are combined with statistical analysis and measurements of other atmospheric constituents. The average (±one standard deviation) OM concentration was 3.3 ± 1.7 μg m-3. A large source of submicron aerosol mass at this location was determined to be vehicular sources, which contributed approximately 40% to the submicron OM; largely during weekday mornings. The O/C ratio estimated from ACSM measurements was 0.64 ± 0.19; diurnal variations in this value and the more oxygenated fraction of OM as determined from Positive Matrix Factorization and classification analyses suggest the high degree of oxygenation originates from aged OM, rather than locally-produced secondary organic aerosol. A large contribution of this oxygenated aerosol to Tijuana from various source classes was observed; some fraction of this aerosol mass may be associated with non-refractory components, such as dust or BC. Backtrajectory simulations using the HYSPLIT model suggest that the mean wind vector consistently originated from the northwest region, over the Pacific Ocean and near the Southern California coast, which suggests that the origin of much of the oxygenated organic aerosol observed in Tijuana (as much as 60% of OM) may have been the Southern California Air Basin. The marine aerosol contribution to OM during the period was on average 23 ± 24%, though its contribution varied over synoptic rather than diurnal timescales. BB aerosol contributed 20 ± 20% of the OM during the campaign period, with notable BB events occurring during several weekend evenings.

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

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

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

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

Characterize Aerosols from MODIS MISR OMI MERRA-2: Dynamic Image Browse Perspective

NASA Technical Reports Server (NTRS)

Wei, Jennifer; Yang, Wenli; Albayrak, Arif; Zhao, Peisheng; Zeng, Jian; Shen, Suhung; Johnson, James; Kempler, Steve

2016-01-01

Among the known atmospheric constituents, aerosols still represent the greatest uncertainty in climate research. To understand the uncertainty is to bring altogether of observational (in-situ and remote sensing) and modeling datasets and inter-compare them synergistically for a wide variety of applications that can bring far-reaching benefits to the science community and the broader society. These benefits can best be achieved if these earth science data (satellite and modeling) are well utilized and interpreted. Unfortunately, this is not always the case, despite the abundance and relative maturity of numerous satellite-borne sensors routinely measure aerosols. There is often disagreement between similar aerosol parameters retrieved from different sensors, leaving users confused as to which sensors to trust for answering important science questions about the distribution, properties, and impacts of aerosols. NASA Goddard Earth Sciences Data and Information Services Center (GES DISC) have developed a new visualization service (NASA Level 2 Data Quality Visualization, DQViz)supporting various visualization and data accessing capabilities from satellite Level 2(MODISMISROMI) and long term assimilated aerosols from NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2 displaying at their own native physical-retrieved spatial resolution. Functionality will include selecting data sources (e.g., multiple parameters under the same measurement), defining area-of-interest and temporal extents, zooming, panning, overlaying, sliding, and data subsetting and reformatting.

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.

Dynamics of phytoplankton community structure in the South China Sea in response to the East Asian aerosol input

NASA Astrophysics Data System (ADS)

Guo, C.; Yu, J.; Ho, T.-Y.; Wang, L.; Song, S.; Kong, L.; Liu, H.

2012-04-01

Recent studies have demonstrated atmospheric deposition as an important source of bioreactive compounds to the ocean. The South China Sea (SCS), where aerosol loading is among the highest in the world, however, is poorly studied, particularly on the in situ response of phytoplankton community structures to atmospheric deposition. By conducting a series of microcosm bioassays at different hydrographical locations and simulating different aerosol event scales, we observed both positive and negative responses to the input of East Asian (EA) aerosol with high nitrogen (N) and trace metal contents, in terms of biomass, composition and physiological characteristics of phytoplankton communities. High levels of aerosol loading relieved phytoplankton nitrogen and trace metal limitations in SCS, and thus increased total phytoplankton biomass, enhanced their physiological indicators (e.g. photosynthetic efficiency) and shifted phytoplankton assemblages from being dominated by picoplankton to microphytoplanton, especially diatoms. However, under low levels of aerosol loading, the composition shift and biomass accumulation were not apparent, suggesting that the stimulation effects might be counterbalanced by enhanced grazing mortality indicated by increased abundance of protist grazers. Trace metal toxicity of the aerosols might also be the reason for the reduction of picocyanobacteria when amended with high EA aerosols. The magnitude and duration of the deposition event, as well as the hydrographical and trophic conditions of receiving waters are also important factors when predicting the influence of an aerosol deposition event. Our results demonstrated different responses of phytoplankton and microbial food web dynamics to different scales of atmospheric input events in SCS and highlighted the need for achieving an accurate comprehension of atmospheric nutrient on the biogeochemical cycles of the oceans.

Coupling Satellite and Ground-Based Instruments to Map Climate Forcing by Anthropogenic Aerosols

NASA Technical Reports Server (NTRS)

Charlson, Robert J.; Anderson, Theodore L.; Hostetler, Chris (Technical Monitor)

2000-01-01

Climate forcing by anthropogenic aerosols is a significant but highly uncertain factor in global climate change. Only satellites can offer the global coverage essential to reducing this uncertainty; however, satellite measurements must be coupled with correlative, in situ measurements both to constrain the aerosol optical properties required in satellite retrieval algorithms and to provide chemical identification of aerosol sources. This grant funded the first two years of a three-year project which seeks to develop methodologies for combining spaceborne lidar with in-situ aerosol data sets to improve estimates of direct aerosol climate forcing. Progress under this two-year grant consisted in the development and deployment of a new in-situ capability for measuring aerosol 180' backscatter and the extinction-to-backscatter ratio. This new measurement capacity allows definitive lidar/in-situ comparisons and improves our ability to interpret lidar data in terms of climatically relevant quantities such as the extinction coefficient and optical depth. Measurements were made along the coast of Washington State, in Central Illinois, over the Indian Ocean, and in the Central Pacific. Thus, this research, combined with previous measurements by others, is rapidly building toward a global data set of extinction-to-backscatter ratio for key aerosol types. Such information will be critical to interpreting lidar data from the upcoming PICASSO-CENA, or P-C, satellite mission. Another aspect of this project is to investigate innovative ways to couple the lidar-satellite signal with targeted in-situ measurements toward a direct determination of aerosol forcing. This aspect is progressing in collaboration with NASA Langley's P-C lidar simulator and radiative transfer modeling by the University of Lille, France.

Coupling Satellite and Ground-Based Instruments to Map Climate Forcing by Anthropogenic Aerosol

NASA Technical Reports Server (NTRS)

Charlson, Robert J.; Anderson, Theodore L.; Hostetler, Chris (Technical Monitor)

2000-01-01

Climate forcing by anthropogenic aerosols is a significant but highly uncertain factor in global climate change. Only satellites can offer the global coverage essential to reducing this uncertainty; however, satellite measurements must be coupled with correlative, in situ measurements both to constrain the aerosol optical properties required in satellite retrieval algorithms and to provide chemical identification of aerosol sources. This grant funded the third year of a three-year project which seeks to develop methodologies for combining spaceborne lidar with in-situ aerosol data sets to improve estimates of direct aerosol climate forcing. Progress under this one-year grant consisted in analysis and publication of field studies using a new in-situ capability for measuring aerosol 180 deg backscatter and the extinction-to-backscatter ratio. This new measurement capacity allows definitive lidar/in-situ comparisons and improves our ability to interpret lidar data in terms of climatically relevant quantities such as the extinction coefficient and optical depth. Analyzed data consisted of measurements made along the coast of Washington State, in Central Illinois, over the Indian Ocean, and in the Central Pacific. Thus, this research, combined with previous measurements by others, is rapidly building toward a global data set of extinction-to-backscatter ratio for key aerosol types. Such information will be critical to interpreting lidar data from the upcoming PICASSO-CENA, or P-C, satellite mission. Another aspect of this project is to investigate innovative ways to couple the lidar-satellite signal with target in-situ measurements toward a direct determination of aerosol forcing. This aspect is progressing in collaboration with NASA Langley's P-C lidar simulator.

Investigation of short-term effective radiative forcing of fire aerosols over North America using nudged hindcast ensembles

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

Liu, Yawen; Zhang, Kai; Qian, Yun

Aerosols from fire emissions can potentially have large impact on clouds and radiation. However, fire aerosol sources are often intermittent, and their effect on weather and climate is difficult to quantify. Here we investigated the short-term effective radiative forcing of fire aerosols using the global aerosol–climate model Community Atmosphere Model version 5 (CAM5). Different from previous studies, we used nudged hindcast ensembles to quantify the forcing uncertainty due to the chaotic response to small perturbations in the atmosphere state. Daily mean emissions from three fire inventories were used to consider the uncertainty in emission strength and injection heights. The simulated aerosolmore » optical depth (AOD) and mass concentrations were evaluated against in situ measurements and reanalysis data. Overall, the results show the model has reasonably good predicting skills. Short (10-day) nudged ensemble simulations were then performed with and without fire emissions to estimate the effective radiative forcing. Results show fire aerosols have large effects on both liquid and ice clouds over the two selected regions in April 2009. Ensemble mean results show strong negative shortwave cloud radiative effect (SCRE) over almost the entirety of southern Mexico, with a 10-day regional mean value of –3.0 W m –2. Over the central US, the SCRE is positive in the north but negative in the south, and the regional mean SCRE is small (–0.56 W m –2). For the 10-day average, we found a large ensemble spread of regional mean shortwave cloud radiative effect over southern Mexico (15.6 % of the corresponding ensemble mean) and the central US (64.3 %), despite the regional mean AOD time series being almost indistinguishable during the 10-day period. Moreover, the ensemble spread is much larger when using daily averages instead of 10-day averages. In conclusion, this demonstrates the importance of using a large ensemble of simulations to estimate the short-term aerosol effective radiative forcing.« less

Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

NASA Astrophysics Data System (ADS)

Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

2015-12-01

The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which revealed four different organic aerosol components with very distinct chemical characteristics for the dry season and three for the wet season.

Investigation of short-term effective radiative forcing of fire aerosols over North America using nudged hindcast ensembles

DOE PAGES

Liu, Yawen; Zhang, Kai; Qian, Yun; ...

2018-01-03

Aerosols from fire emissions can potentially have large impact on clouds and radiation. However, fire aerosol sources are often intermittent, and their effect on weather and climate is difficult to quantify. Here we investigated the short-term effective radiative forcing of fire aerosols using the global aerosol–climate model Community Atmosphere Model version 5 (CAM5). Different from previous studies, we used nudged hindcast ensembles to quantify the forcing uncertainty due to the chaotic response to small perturbations in the atmosphere state. Daily mean emissions from three fire inventories were used to consider the uncertainty in emission strength and injection heights. The simulated aerosolmore » optical depth (AOD) and mass concentrations were evaluated against in situ measurements and reanalysis data. Overall, the results show the model has reasonably good predicting skills. Short (10-day) nudged ensemble simulations were then performed with and without fire emissions to estimate the effective radiative forcing. Results show fire aerosols have large effects on both liquid and ice clouds over the two selected regions in April 2009. Ensemble mean results show strong negative shortwave cloud radiative effect (SCRE) over almost the entirety of southern Mexico, with a 10-day regional mean value of –3.0 W m –2. Over the central US, the SCRE is positive in the north but negative in the south, and the regional mean SCRE is small (–0.56 W m –2). For the 10-day average, we found a large ensemble spread of regional mean shortwave cloud radiative effect over southern Mexico (15.6 % of the corresponding ensemble mean) and the central US (64.3 %), despite the regional mean AOD time series being almost indistinguishable during the 10-day period. Moreover, the ensemble spread is much larger when using daily averages instead of 10-day averages. In conclusion, this demonstrates the importance of using a large ensemble of simulations to estimate the short-term aerosol effective radiative forcing.« less

Characteristics of regional aerosols: Southern Arizona and eastern Pacific Ocean

NASA Astrophysics Data System (ADS)

Prabhakar, Gouri

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

Atmospheric aerosol composition and source apportionments to aerosol in southern Taiwan

NASA Astrophysics Data System (ADS)

Tsai, Ying I.; Chen, Chien-Lung

In this study, the chemical characteristics of winter aerosol at four sites in southern Taiwan were determined and the Gaussian Trajectory transfer coefficient model (GTx) was then used to identify the major air pollutant sources affecting the study sites. Aerosols were found to be acidic at all four sites. The most important constituents of the particulate matter (PM) by mass were SO 42-, organic carbon (OC), NO 3-, elemental carbon (EC) and NH 4+, with SO 42-, NO 3-, and NH 4+ together constituting 86.0-87.9% of the total PM 2.5 soluble inorganic salts and 68.9-78.3% of the total PM 2.5-10 soluble inorganic salts, showing that secondary photochemical solution components such as these were the major contributors to the aerosol water-soluble ions. The coastal site, Linyuan (LY), had the highest PM mass percentage of sea salts, higher in the coarse fraction, and higher sea salts during daytime than during nighttime, indicating that the prevailing daytime sea breeze brought with it more sea-salt aerosol. Other than sea salts, crustal matter, and EC in PM 2.5 at Jenwu (JW) and in PM 2.5-10 at LY, all aerosol components were higher during nighttime, due to relatively low nighttime mixing heights limiting vertical and horizontal dispersion. At JW, a site with heavy traffic loadings, the OC/EC ratio in the nighttime fine and coarse fractions of approximately 2.2 was higher than during daytime, indicating that in addition to primary organic aerosol (POA), secondary organic aerosol (SOA) also contributed to the nighttime PM 2.5. This was also true of the nighttime coarse fraction at LY. The GTx produced correlation coefficients ( r) for simulated and observed daily concentrations of PM 10 at the four sites (receptors) in the range 0.45-0.59 and biases from -6% to -20%. Source apportionment indicated that point sources were the largest PM 10 source at JW, LY and Daliao (DL), while at Meinung (MN), a suburban site with less local PM 10, SO x and NO x emissions, upwind boundary concentration was the major PM 10 source, followed by point sources and top boundary concentration.

10-year record of atmospheric composition in the high Himalayas: source, transport and impact

NASA Astrophysics Data System (ADS)

Bonasoni, Paolo; Laj, Paolo; Marinoni, Angela; Cristofanelli, Paolo; Maione, Michela; Putero, Davide; Calzolari, Francescopiero; Decesari, Stefano; Facchini, Maria Cristina; Fuzzi, Sandro; Gobbi, Gianpaolo; Sellegri, Karine; Verza, Gianpietro; Vuillermoz, Elisa; Arduini, Jgor

2016-04-01

South Asia represents a global "hot-spot" for air-quality and climate impacts. Since the end of the 20th Century, field experiments and satellite observations identified a thick layer of atmospheric pollutants extending from the Indian Ocean up to the atmosphere of the Himalayas. Since large amount of short-lived climate pollutants (SLCPs) - like atmospheric aerosol (in particular, the light-absorbing aerosol) and ozone - characterize this region, severe implications were recognized for population health, ecosystem integrity as well as regional climate impacts, especially for what concerns hydrological cycle, monsoon regimes and cryosphere. Since 2006, the Nepal Climate Observatory - Pyramid (NCO-P, 27.95N, 86.82 E, 5079 m a.s.l.), a global station of the WMO/GAW programme has been active in the eastern Nepal Himalaya, not far from the Mt. Everest. NCO-P is located away from large direct anthropogenic pollution sources. The closest major urban area is Kathmandu (200 km south-west from the measurement site). As being located along the Khumbu valley, the observations are representative of synoptic-scale and mountain thermal circulation, providing direct information about the vertical transport of pollutants/climate-altering compounds to the Himalayas and to the free troposphere. In the framework of international programmes (GAW/WMO, UNEP-ABC, AERONET) the following continuous measurement programmes have been carried out at NCO-P: surface ozone, aerosol size distribution (from 10 nm to 25 micron), total particle number, aerosol scattering and absorption coefficients, equivalent BC, PM1-PM10, AOD by sun-photometry, global solar radiation (SW and LW), meteorology. Long-term sampling programmes for the off-line determination of halogenated gases and aerosol chemistry have been also activated. The atmospheric observation records at NCO-P, now representing the longest time series available for the high Himalayas, provided the first direct evidences about the systematic occurrence of pollution transport and high rate of new particle formation events in this region. Here we provide an overview of the main scientific results obtained during these ten years of research. In particular, we will discuss the impact of atmospheric transport and monsoon variability on atmospheric composition by disentangling the role played by mountain breeze system and synoptic-scale transport. We will provide specific information about the role of stratospheric intrusions, long-range mineral dust transport and open biomass burning emissions in determining the variability of ozone, aerosol and equivalent black carbon concentrations. The effect of particle nucleation processes on aerosol number concentrations will be shown. Finally, we discuss the climatic impact of aerosols observed at NCO-P both in terms of direct atmospheric radiative forcing and black carbon deposition on Himalayan snow.

Exploring the Contribution of Primary Marine Organic Matter to the Arctic Boundary Layer

NASA Astrophysics Data System (ADS)

Collins, D. B.; Chang, R. Y. W.; Boyer, M.; Abbatt, J.

2016-12-01

The ocean is a significant source of aerosol to the atmosphere, and contributes significantly to the aerosol population especially in remote locations. Both primary and secondary processes connect the ocean to ambient aerosol loadings, but the extent to which the ocean is a source of organic material to the atmosphere is a current topic of scientific debate. The contribution of primary marine aerosol to atmospheric organic matter may have an influence on the water uptake properties and chemical reactivity of primary marine aerosol particles, influencing their climate-relevant properties. In this study, we characterize the contribution of primary marine aerosol to the arctic marine boundary layer using coincident quantitative measurements of freshly-produced sea spray aerosol and ambient marine aerosol to the arctic boundary layer during an expedition aboard the CCGS Amundsen. Sea spray production experiments were conducted during the cruise using a tank fitted with a plunging waterfall apparatus, a technique which has been recently shown to closely mimic the aerosol production behavior of controlled breaking waves. Comparison of the chemical composition of sea spray particles generated from water samples in various locations throughout the Canadian Archipelago will be presented. A tracer analysis of specific compounds known to be important contributors to primary marine organic material are tracked using GC/MS, along with those known to be tracers of biological aerosol and other organic matter sources. Size-segregated trends in tracer concentrations and ratios with inorganic components will be discussed in the context of understanding the contribution of primary organics to the Arctic atmosphere and in comparison with other sources of organic material observed during the ship-board campaign.

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

NASA Astrophysics Data System (ADS)

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

2012-08-01

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

Organic aerosols over Indo-Gangetic Plain: Sources, distributions and climatic implications

NASA Astrophysics Data System (ADS)

Singh, Nandita; Mhawish, Alaa; Deboudt, Karine; Singh, R. S.; Banerjee, Tirthankar

2017-05-01

Organic aerosol (OA) constitutes a dominant fraction of airborne particulates over Indo-Gangetic Plain (IGP) especially during post-monsoon and winter. Its exposure has been associated with adverse health effects while there are evidences of its interference with Earth's radiation balance and cloud condensation (CC), resulting possible alteration of hydrological cycle. Therefore, presence and effects of OA directly link it with food security and thereby, sustainability issues. In these contexts, atmospheric chemistry involving formation, volatility and aging of primary OA (POA) and secondary OA (SOA) have been reviewed with specific reference to IGP. Systematic reviews on science of OA sources, evolution and climate perturbations are presented with databases collected from 82 publications available throughout IGP till 2016. Both gaseous and aqueous phase chemical reactions were studied in terms of their potential to form SOA. Efforts were made to recognize the regional variation of OA, its chemical constituents and sources throughout IGP and inferences were made on its possible impacts on regional air quality. Mass fractions of OA to airborne particulate showed spatial variation likewise in Lahore (37 and 44% in fine and coarse fractions, respectively), Patiala (28 and 37%), Delhi (25 and 38%), Kanpur (24 and 30%), Kolkata (11 and 21%) and Dhaka. Source apportionment studies indicate biomass burning, coal combustion and vehicular emissions as predominant OA sources. However, sources represent considerable seasonal variations with dominance of gasoline and diesel emissions during summer and coal and biomass based emissions during winter and post-monsoon. Crop residue burning over upper-IGP was also frequently held responsible for massive OA emission, mostly characterized by its hygroscopic nature, thus having potential to act as CC nuclei. Conclusively, climatic implication of particulate bound OA has been discussed in terms of its interaction with radiation balance.

Estimation of the contributions of long range transported aerosol in East Asia to carbonaceous aerosol and PM concentrations in Seoul, Korea using highly time resolved measurements: a PSCF model approach.

PubMed

Jeong, Ukkyo; Kim, Jhoon; Lee, Hanlim; Jung, Jinsang; Kim, Young J; Song, Chul H; Koo, Ja-Ho

2011-07-01

The contributions of long range transported aerosol in East Asia to carbonaceous aerosol and particulate matter (PM) concentrations in Seoul, Korea were estimated with potential source contribution function (PSCF) calculations. Carbonaceous aerosol (organic carbon (OC) and elemental carbon (EC)), PM(2.5), and PM(10) concentrations were measured from April 2007 to March 2008 in Seoul, Korea. The PSCF and concentration weighted trajectory (CWT) receptor models were used to identify the spatial source distributions of OC, EC, PM(2.5), and coarse particles. Heavily industrialized areas in Northeast China such as Harbin and Changchun and East China including the Pearl River Delta region, the Yangtze River Delta region, and the Beijing-Tianjin region were identified as high OC, EC and PM(2.5) source areas. The conditional PSCF analysis was introduced so as to distinguish the influence of aerosol transported from heavily polluted source areas on a receptor site from that transported from relatively clean areas. The source contributions estimated using the conditional PSCF analysis account for not only the aerosol concentrations of long range transported aerosols but also the number of transport days effective on the measurement site. Based on the proposed algorithm, the condition of airmass pathways was classified into two types: one condition where airmass passed over the source region (PS) and another condition where airmass did not pass over the source region (NPS). For most of the seasons during the measurement period, 249.5-366.2% higher OC, EC, PM(2.5), and coarse particle concentrations were observed at the measurement site under PS conditions than under NPS conditions. Seasonal variations in the concentrations of OC, EC, PM(2.5), and coarse particles under PS, NPS, and background aerosol conditions were quantified. The contributions of long range transported aerosols on the OC, EC, PM(2.5), and coarse particle concentrations during several Asian dust events were also estimated. We also investigated the performance of the PSCF results obtained from combining highly time resolved measurement data and backward trajectory calculations via comparison with those from data in low resolutions. Reduced tailing effects and the larger coverage over the area of interest were observed in the PSCF results obtained from using the highly time resolved data and trajectories.

Organic aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis

NASA Astrophysics Data System (ADS)

Reyes-Villegas, Ernesto; Green, David C.; Priestman, Max; Canonaco, Francesco; Coe, Hugh; Prévôt, André S. H.; Allan, James D.

2016-12-01

The multilinear engine (ME-2) factorization tool is being widely used following the recent development of the Source Finder (SoFi) interface at the Paul Scherrer Institute. However, the success of this tool, when using the a value approach, largely depends on the inputs (i.e. target profiles) applied as well as the experience of the user. A strategy to explore the solution space is proposed, in which the solution that best describes the organic aerosol (OA) sources is determined according to the systematic application of predefined statistical tests. This includes trilinear regression, which proves to be a useful tool for comparing different ME-2 solutions. Aerosol Chemical Speciation Monitor (ACSM) measurements were carried out at the urban background site of North Kensington, London from March to December 2013, where for the first time the behaviour of OA sources and their possible environmental implications were studied using an ACSM. Five OA sources were identified: biomass burning OA (BBOA), hydrocarbon-like OA (HOA), cooking OA (COA), semivolatile oxygenated OA (SVOOA) and low-volatility oxygenated OA (LVOOA). ME-2 analysis of the seasonal data sets (spring, summer and autumn) showed a higher variability in the OA sources that was not detected in the combined March-December data set; this variability was explored with the triangle plots f44 : f43 f44 : f60, in which a high variation of SVOOA relative to LVOOA was observed in the f44 : f43 analysis. Hence, it was possible to conclude that, when performing source apportionment to long-term measurements, important information may be lost and this analysis should be done to short periods of time, such as seasonally. Further analysis on the atmospheric implications of these OA sources was carried out, identifying evidence of the possible contribution of heavy-duty diesel vehicles to air pollution during weekdays compared to those fuelled by petrol.

Potential for wind extraction from 4D-Var assimilation of aerosols and moisture

NASA Astrophysics Data System (ADS)

Zaplotnik, Žiga; Žagar, Nedjeljka

2017-04-01

We discuss the potential of the four-dimensional variational data assimilation (4D-Var) to retrieve the unobserved wind field from observations of atmospheric tracers and the mass field through internal model dynamics and the multivariate relationships in the background-error term for 4D-Var. The presence of non-linear moist dynamics makes the wind retrieval from tracers very difficult. On the other hand, it has been shown that moisture observations strongly influence both tropical and mid-latitude wind field in 4D-Var. We present an intermediate complexity model that describes nonlinear interactions between the wind, temperature, aerosols and moisture including their sinks and sources in the framework of the so-called first baroclinic mode atmosphere envisaged by A. Gill. Aerosol physical processes, which are included in the model, are the non-linear advection, diffusion and sources and sinks that exist as dry and wet deposition and diffusion. Precipitation is parametrized according to the Betts-Miller scheme. The control vector for 4D-Var includes aerosols, moisture and the three dynamical variables. The former is analysed univariately whereas wind field and mass field are analysed in a multivariate fashion taking into account quasi-geostrophic and unbalanced dynamics. The OSSE type of studies are performed for the tropical region to assess the ability of 4D-Var to extract wind-field information from the time series of observations of tracers as a function of the flow nonlinearity, the observations density and the length of the assimilation window (12 hours and 24 hours), in dry and moist environment. Results show that the 4D-Var assimilation of aerosols and temperature data is beneficial for the wind analysis with analysis errors strongly dependent on the moist processes and reliable background-error covariances.

Aerosol composition and source apportionment in Santiago de Chile

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (2

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Greenland records of aerosol source and atmospheric lifetime changes from the Eemian to the Holocene.

PubMed

Schüpbach, S; Fischer, H; Bigler, M; Erhardt, T; Gfeller, G; Leuenberger, D; Mini, O; Mulvaney, R; Abram, N J; Fleet, L; Frey, M M; Thomas, E; Svensson, A; Dahl-Jensen, D; Kettner, E; Kjaer, H; Seierstad, I; Steffensen, J P; Rasmussen, S O; Vallelonga, P; Winstrup, M; Wegner, A; Twarloh, B; Wolff, K; Schmidt, K; Goto-Azuma, K; Kuramoto, T; Hirabayashi, M; Uetake, J; Zheng, J; Bourgeois, J; Fisher, D; Zhiheng, D; Xiao, C; Legrand, M; Spolaor, A; Gabrieli, J; Barbante, C; Kang, J-H; Hur, S D; Hong, S B; Hwang, H J; Hong, S; Hansson, M; Iizuka, Y; Oyabu, I; Muscheler, R; Adolphi, F; Maselli, O; McConnell, J; Wolff, E W

2018-04-16

The Northern Hemisphere experienced dramatic changes during the last glacial, featuring vast ice sheets and abrupt climate events, while high northern latitudes during the last interglacial (Eemian) were warmer than today. Here we use high-resolution aerosol records from the Greenland NEEM ice core to reconstruct the environmental alterations in aerosol source regions accompanying these changes. Separating source and transport effects, we find strongly reduced terrestrial biogenic emissions during glacial times reflecting net loss of vegetated area in North America. Rapid climate changes during the glacial have little effect on terrestrial biogenic aerosol emissions. A strong increase in terrestrial dust emissions during the coldest intervals indicates higher aridity and dust storm activity in East Asian deserts. Glacial sea salt aerosol emissions in the North Atlantic region increase only moderately (50%), likely due to sea ice expansion. Lower aerosol concentrations in Eemian ice compared to the Holocene are mainly due to shortened atmospheric residence time, while emissions changed little.

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 associated with the regional circulations.

Long-Term Observations on Aerosol Elemental Carbon and Mass Concentrations in Winter-Time in New Delhi: Implications for Local Source Changes

NASA Astrophysics Data System (ADS)

Aggarwal, S. G.; Singh, K.; Singh, N.; Gupta, P. K.

2009-12-01

Fossil-fuel and bio-fuel burning are the two major sources identified for high carbonaceous aerosol loadings in several mega cities in India. In the last decade, according to a report from the Central Pollution Control Board (CPCB, 1999), the vehicular emission (mostly diesel-powered engines) was contributed to ~67% of the total air pollution load in New Delhi. Therefore, a policy decision was taken by the government, and most of the diesel-powered engines were converted to compressed natural gas (CNG) -powered engines by 2003. To better understand the effect of these changes on air quality, we collected high volume aerosol samples (total suspended particles, TSP) mostly for a day basis at our institute building in New Delhi almost everyday during winter season (November to January) from 2002 to 2008. We found very high mean aerosol loading, i.e., 488±47 μg m-3 in 2002 winter, which dropped significantly to 280±73 μg m-3 in 2003 winter. Thereafter, a steadily increased trend of aerosol mass loadings was observed, i.e., 339±112, 339±120, 412±107 and 444±55 μg m-3 in 2004, 2005, 2006 and 2007 winters, respectively. Similar trend was also observed for elemental carbon (EC) concentration in TSP, which was peaked in 2002 (47±11 μg m-3) and minimized in 2003 (32±6 μg m-3), and then gradually increased to 41±8 μg m-3 in 2007 winter. These decline trends of aerosol mass and EC concentrations in 2003 can be explained well, because of the conversion of diesel engine to CNG engines of public transport facilities. However, again increase in aerosol mass and EC concentrations possibly because of a high increase in road traffic in recent years. According to the economic survey of New Delhi 2008-09, the number of vehicles (which includes all types of engines, i.e., petrol, diesel and CNG) has grown from ~3.3 millions in 1997-98 to ~5.6 millions in 2007-08. The influence of engine types and vehicle population on aerosol loading can also be explained well by SO2 and NO2 concentration trend (data obtained from the local agency) for the study period. On the other hand, during winter-time from 2002 to 2008, meteorological data (e.g., mean temperature, humidity, precipitation) did not change significantly. This study suggests that winter aerosol loadings in New Delhi are largely influenced by the local sources (fossil fuel combustion).

Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols

NASA Astrophysics Data System (ADS)

Claeys, Marine; Roberts, Greg; Mallet, Marc; Arndt, Jovanna; Sellegri, Karine; Sciare, Jean; Wenger, John; Sauvage, Bastien

2017-06-01

As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based in situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m a.s.l.) to characterise the optical, physical and chemical properties of aerosols. During the observation period, a major influence of primary marine aerosols was detected (22-26 June), with a mass concentration reaching up to 6.5 µg m-3 and representing more than 40 % of the total PM10 mass concentration. Its relatively low ratio of chloride to sodium (average of 0.57) indicates a fairly aged sea salt aerosol at Ersa. In this work, an original data set, obtained from online real-time instruments (ATOFMS, PILS-IC) has been used to characterise the ageing of primary marine aerosols (PMAs). During this PMA period, the mixing of fresh and aged PMAs was found to originate from both local and regional (Gulf of Lion) emissions, according to local wind measurements and FLEXPART back trajectories. Two different aerosol regimes have been identified: a dust outbreak (dust) originating from Algeria/Tunisia, and a pollution period with aerosols originating from eastern Europe, which includes anthropogenic and biomass burning sources (BBP). The optical, physical and chemical properties of the observed aerosols, as well as their local shortwave (SW) direct radiative effect (DRE) in clear-sky conditions, are compared for these three periods in order to assess the importance of the direct radiative impact of PMAs compared to other sources above the western Mediterranean Basin. As expected, AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of -11 ± 4 at the surface and -8 ± 3 W m-2 at the top of the atmosphere (TOA). In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3-0.4 at 440 nm and column-integrated SSA of 0.90-0.95), induced a local instantaneous SW DRF that is nearly 3 times the effect calculated during the PMA period, with maximum values up to -40 W m-2 at the surface. A similar range of values were found for the BBP period to those during the dust period (SW DRF at the surface and TOA of -23 ± 6 and -15 ± 4 W m-2 respectively). The multiple sources of measurements at Ersa allowed the detection of a PMA-dominant period and their characterisation in terms of ageing, origin, transport, optical and physical properties and direct climatic impact.

Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) Final Campaign Report

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

Wood, R.

2016-01-01

The extensive coverage of low clouds over the subtropical eastern oceans greatly impacts the current climate. In addition, the response of low clouds to changes in atmospheric greenhouse gases and aerosols is a major source of uncertainty, which thwarts accurate prediction of future climate change. Low clouds are poorly simulated in climate models, partly due to inadequate long-term simultaneous observations of their macrophysical and microphysical structure, radiative effects, and associated aerosol distribution in regions where their impact is greatest. The thickness and extent of subtropical low clouds is dependent on tight couplings between surface fluxes of heat and moisture, radiativemore » cooling, boundary layer turbulence, and precipitation (much of which evaporates before reaching the ocean surface and is closely connected to the abundance of cloud condensation nuclei). These couplings have been documented as a result of past field programs and model studies. However, extensive research is still required to achieve a quantitative understanding sufficient for developing parameterizations, which adequately predict aerosol indirect effects and low cloud response to climate perturbations. This is especially true of the interactions between clouds, aerosol, and precipitation. These processes take place in an ever-changing synoptic environment that can confound interpretation of short time period observations.« less

Temporal variation in airborne microbial populations and microbially-derived allergens in a tropical urban landscape

NASA Astrophysics Data System (ADS)

Woo, Anthony C.; Brar, Manreetpal S.; Chan, Yuki; Lau, Maggie C. Y.; Leung, Frederick C. C.; Scott, James A.; Vrijmoed, Lilian L. P.; Zawar-Reza, Peyman; Pointing, Stephen B.

2013-08-01

The microbial component of outdoor aerosols was assessed along a gradient of urban development from inner-city to rural in the seasonal-tropical metropolis of Hong Kong. Sampling over a continuous one-year period was conducted, with molecular analyses to characterize bacterial and eukaryal microbial populations, immuno-assays to detect microbially-derived allergens and extensive environmental and meteorological observations. The data revealed bio-aerosol populations were not significantly impacted by the level of urban development as measured by anthropogenic pollutants and human population levels, but instead exhibited a strong seasonal trend related to general climatic variables. We applied back-trajectory analysis to establish sources of air masses and this allowed further explanation of urban bio-aerosols largely in terms of summer-marine and winter-continental origins. We also evaluated bio-aerosols for the potential to detect human health threats. Many samples supported bacterial and fungal phylotypes indicative of known pathogenic taxa, together with common indicators of human presence. The occurrence of allergenic endotoxins and beta-glucans generally tracked trends in microbial populations, with levels known to induce symptoms detected during summer months when microbial loading was higher. This strengthens calls for bio-aerosols to be considered in future risk assessments and surveillance of air quality, along with existing chemical and particulate indices.

SOURCES OF ORGANIC AEROSOL: SEMIVOLATILE EMISSIONS AND PHOTOCHEMICAL AGING

EPA Science Inventory

The proposed research integrates emissions testing, smog chamber experiments, and regional chemical transport models (CTMs) to investigate the sources of organic aerosol in urban and regional environments.

Biomarkers as indicators of fungal biomass in the atmosphere of São Paulo, Brazil.

PubMed

Emygdio, Ana Paula Mendes; Andrade, Maria de Fátima; Gonçalves, Fabio Luiz Teixeira; Engling, Guenter; Zanetti, Rafael Henrique de Souza; Kumar, Prashant

2018-01-15

The biogenic aerosol contribution to atmospheric particulate matter (PM) mass concentration is usually neglected due to the difficulty in identifying its components, although it can be significant. In the Metropolitan Area of São Paulo (MASP)-Brazil, several studies have been performed to identify sources for PM, revealing vehicular emissions and soil re-suspension as the main identified sources. The organic fraction has been related primarily to biomass burning (BB) and fuel combustion, although there is significant presence of green areas in the city which render biogenic emissions as an additional source of organic carbon (OC). The objectives of this work are to (i) characterise the composition of the PM 10 (ii) estimate the relative mass contribution of fungal spores to PM concentrations with sizes smaller than 10μm (PM 10 ) in MASP and (iii) assess the main sources of PM 10 . To achieve these objectives, we measured markers of biogenic sources and BB, during the fall-winter transition, which along with other constituents, such as ions, organic/elemental carbon, elemental composition and fungal spore concentrations, help assess the PM 10 sources. We used receptor models to identify distinct source-related PM 10 fractions and conversion factors to convert biomarker concentrations to fungal mass. Our results show the mean contributions of fungal aerosol to PM 10 and OC mass were 2% and 8%, respectively, indicating the importance of fungal spores to the aerosol burden in the urban atmosphere. Using specific rotation factor analysis, we identified the following factors contributing to PM: soil re-suspension, biogenic aerosol, secondary inorganic aerosol, vehicular emissions and BB/isoprene-related secondary organic aerosol (I-SOA). BB/I-SOA was the main source representing 28% of the PM 10 mass, while biogenic aerosol explained a significant (11%) fraction of the PM 10 mass as well. Our findings suggest that primary biogenic aerosol is an important fraction of PM 10 mass, yet not considered in most studies. Copyright © 2017 Elsevier B.V. All rights reserved.

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

Gaffney, Jeffrey

This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

Important fossil source contribution to brown carbon in Beijing during winter

NASA Astrophysics Data System (ADS)

Yan, Caiqing; Zheng, Mei; Bosch, Carme; Andersson, August; Desyaterik, Yury; Sullivan, Amy P.; Collett, Jeffrey L.; Zhao, Bin; Wang, Shuxiao; He, Kebin; Gustafsson, Örjan

2017-03-01

Organic aerosol (OA) constitutes a substantial fraction of fine particles and affects both human health and climate. It is becoming clear that OA absorbs light substantially (hence termed Brown Carbon, BrC), adding uncertainties to global aerosol radiative forcing estimations. The few current radiative-transfer and chemical-transport models that include BrC primarily consider sources from biogenic and biomass combustion. However, radiocarbon fingerprinting here clearly indicates that light-absorbing organic carbon in winter Beijing, the capital of China, is mainly due to fossil sources, which contribute the largest part to organic carbon (OC, 67 ± 3%) and its sub-constituents (water-soluble OC, WSOC: 54 ± 4%, and water-insoluble OC, WIOC: 73 ± 3%). The dual-isotope (Δ14C/δ13C) signatures, organic molecular tracers and Beijing-tailored emission inventory identify that this fossil source is primarily from coal combustion activities in winter, especially from the residential sector. Source testing on Chinese residential coal combustion provides direct evidence that intensive coal combustion could contribute to increased light-absorptivity of ambient BrC in Beijing winter. Coal combustion is an important source to BrC in regions such as northern China, especially during the winter season. Future modeling of OA radiative forcing should consider the importance of both biomass and fossil sources.

Important fossil source contribution to brown carbon in Beijing during winter

PubMed Central

Yan, Caiqing; Zheng, Mei; Bosch, Carme; Andersson, August; Desyaterik, Yury; Sullivan, Amy P.; Collett, Jeffrey L.; Zhao, Bin; Wang, Shuxiao; He, Kebin; Gustafsson, Örjan

2017-01-01

Organic aerosol (OA) constitutes a substantial fraction of fine particles and affects both human health and climate. It is becoming clear that OA absorbs light substantially (hence termed Brown Carbon, BrC), adding uncertainties to global aerosol radiative forcing estimations. The few current radiative-transfer and chemical-transport models that include BrC primarily consider sources from biogenic and biomass combustion. However, radiocarbon fingerprinting here clearly indicates that light-absorbing organic carbon in winter Beijing, the capital of China, is mainly due to fossil sources, which contribute the largest part to organic carbon (OC, 67 ± 3%) and its sub-constituents (water-soluble OC, WSOC: 54 ± 4%, and water-insoluble OC, WIOC: 73 ± 3%). The dual-isotope (Δ14C/δ13C) signatures, organic molecular tracers and Beijing-tailored emission inventory identify that this fossil source is primarily from coal combustion activities in winter, especially from the residential sector. Source testing on Chinese residential coal combustion provides direct evidence that intensive coal combustion could contribute to increased light-absorptivity of ambient BrC in Beijing winter. Coal combustion is an important source to BrC in regions such as northern China, especially during the winter season. Future modeling of OA radiative forcing should consider the importance of both biomass and fossil sources. PMID:28266611

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 these organic aerosol species as sources of organic carbon in surface waters is also addressed. 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 Science Program.

Chemical Properties of Combustion Aerosols: An Overview

EPA Science Inventory

A wide variety of pyrogenic and anthropogenic sources emit fine aerosols to the atmosphere. The physical and chemical properties of these aerosols are of interest due to their influence on climate, human health, and visibility. Aerosol chemical composition is remarkably complex. ...

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

NASA Astrophysics Data System (ADS)

Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray emissions to particles, addressing the persistent question of the sources of cloud condensation nuclei in clean marine conditions.

A reference aerosol for a radon reference chamber

NASA Astrophysics Data System (ADS)

Paul, Annette; Keyser, Uwe

1996-02-01

The measurement of radon and radon progenies and the calibration of their detection systems require the production and measurement of aerosols well-defined in size and concentration. In the German radon reference chamber, because of its unique chemical and physical properties, carnauba wax is used to produce standard aerosols. The aerosol size spectra are measured on-line by an aerosol measurement system in the range of 10 nm to 1 μm aerodynamic diameter. The experimental set-ups for the study of adsorption of radioactive ions on aerosols as function of their size and concentration will be described, the results presented and further adaptations for an aerosol jet introduced (for example, for the measurement of short-lived neutron-rich isotopes). Data on the dependence of aerosol radius, ion concentration and element selectivity is collected by using a 252Cf-sf source. The fission products of this source range widely in elements, isotopes and charges. Adsorption and the transport of radioactive ions on aerosols have therefore been studied for various ions for the first time, simultaneously with the aerosol size on-line spectrometry.

Physico-chemical characterization of Mediterranean background aerosol at the Capogranitola observatory (Sicily)

NASA Astrophysics Data System (ADS)

Rinaldi, Matteo; Gilardoni, Stefania; Paglione, Marco; Sandrini, Silvia; Decesari, Stefano; Zanca, Nicola; Marinoni, Angela; Cristofanelli, Paolo; Bonasoni, Paolo; Ielpo, Piera; Fossum, Kirsten; Gobbi, Gian Paolo; Facchini, Maria Cristina

2017-04-01

The Mediterranean basin is characterized by elevated aerosol amounts and co-existence of different aerosol types, both natural and anthropogenic, while it is one of the most climatically sensitive areas. Therefore, it offers ideal conditions for studying aerosol processes and aerosol-climate interactions. An intensive aerosol physico-chemical characterization campaign was held at the Environmental-Climatic Observatory at Capo Granitola (Sicily; 37.5753° N, 12.6595° E) during April 2016, under the framework of the project Air-Sea Lab. The Observatory is located at the coast-line, facing the Strait of Sicily, and is part of the national I-AMICA network (http://www.i-amica.it/i-amica/?lang=en). Sub-micrometer aerosol chemical composition was measured by high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS), for the first time at Capogranitola. Sea-salt concentration was estimated from AMS measurements following Ovadnevaite et al. (2012). For a complete mass closure of the submicron aerosol, black carbon (BC) concentration was derived from multiangle absorption photometer (MAAP) measurements. Positive matrix factorization was deployed to investigate organic aerosol (OA) sources at the site. Aerosol chemical composition confirms that Capogranitola is a representative background site, with generally low contribution of BC and nitrate and highly oxidized OA. In particular, aerosol sampled in the marine sector (130-310°) is less affected by local sources and it is likely representative of the central Mediterranean background. Aerosol in background conditions is dominated by sulfate and OA (37% and 31%), followed by ammonium (12%), sea-salt (10%), BC (6%) and nitrate (3%). The average reconstructed sub-micrometer aerosol mass in background conditions is 3.7±2.3 μg m-3. OA source apportionment shows a minor contribution from primary sources, with hydrocarbon-like OA (HOA), from fossil fuel combustion, contributing for 3% and biomass burning OA (BBOA) for 2%. Oxidized OA (OOA) dominates the rest of OA mass. In particular, OOA1 and OOA2 (70% in total, OM:OC ˜ 2.5) represent the result of prolonged atmospheric processing of OA, while OOA3 (25%, OM:OC ˜ 2.0) clearly represents fresher inputs of OOA from land. Investigation of HOA and BC time trends suggests that HOA in background conditions may be strongly contributed by ship traffic more than by land sources. The representativity of the background aerosol collected at Capogranitola will be discussed by comparing with measurements performed in parallel at the other I-AMICA southern Italy coastal stations and with those acquired in a subsequent cruise (May-June 2016) around the Italian Peninsula. Aerosol climate relevant properties, in relation with chemical composition, will be also presented and discussed. Ovadnevaite J. et al. (2012), J. Geophys. Res., 117, D16201.

Impacts of wind stilling on solar radiation variability in China

PubMed Central

Lin, Changgui; Yang, Kun; Huang, Jianping; Tang, Wenjun; Qin, Jun; Niu, Xiaolei; Chen, Yingying; Chen, Deliang; Lu, Ning; Fu, Rong

2015-01-01

Solar dimming and wind stilling (slowdown) are two outstanding climate changes occurred in China over the last four decades. The wind stilling may have suppressed the dispersion of aerosols and amplified the impact of aerosol emission on solar dimming. However, there is a lack of long-term aerosol monitoring and associated study in China to confirm this hypothesis. Here, long-term meteorological data at weather stations combined with short-term aerosol data were used to assess this hypothesis. It was found that surface solar radiation (SSR) decreased considerably with wind stilling in heavily polluted regions at a daily scale, indicating that wind stilling can considerably amplify the aerosol extinction effect on SSR. A threshold value of 3.5 m/s for wind speed is required to effectively reduce aerosols concentration. From this SSR dependence on wind speed, we further derived proxies to quantify aerosol emission and wind stilling amplification effects on SSR variations at a decadal scale. The results show that aerosol emission accounted for approximately 20% of the typical solar dimming in China, which was amplified by approximately 20% by wind stilling. PMID:26463748

Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

2012-08-01

Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban Environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter <2.5 μm) resolved Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie FP7-EU framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the unique approach used is the simultaneous PIXE measurements at two monitoring sites: urban background (UB) and a street canyon traffic road site (RS). Elements related to primary non exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (secondary sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non exhaust brake dust (Fe-Cu) - 7%), and three types industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%). The validity of the PMF solution of the PIXE data is supported by strong correlations with external single particle mass spectrometry measurements. Beside apportioning the aerosol sources, some important air quality related conclusions can be drawn about the PM2.5 fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with industrial combustion emissions) is found a to be the major (82%) source of Cl in the urban agglomerate; (4) PM2.5 traffic brake dust (Fe-Cu) is mainly primarily emitted and not resuspended, whereas PM2.5 urban crustal dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing dust concentrations in road sites, far more effective than street sweeping activities.

Resolving the Aerosol Piece of the Global Climate Picture

NASA Astrophysics Data System (ADS)

Kahn, R. A.

2017-12-01

Factors affecting our ability to calculate climate forcing and estimate model predictive skill include direct radiative effects of aerosols and their indirect effects on clouds. Several decades of Earth-observing satellite observations have produced a global aerosol column-amount (AOD) record, but an aerosol microphysical property record required for climate and many air quality applications is lacking. Surface-based photometers offer qualitative aerosol-type classification, and several space-based instruments map aerosol air-mass types under favorable conditions. However, aerosol hygroscopicity, mass extinction efficiency (MEE), and quantitative light absorption, must be obtained from in situ measurements. Completing the aerosol piece of the climate picture requires three elements: (1) continuing global AOD and qualitative type mapping from space-based, multi-angle imagers and aerosol vertical distribution from near-source stereo imaging and downwind lidar, (2) systematic, quantitative in situ observations of particle properties unobtainable from space, and (3) continuing transport modeling to connect observations to sources, and extrapolate limited sampling in space and time. At present, the biggest challenges to producing the needed aerosol data record are: filling gaps in particle property observations, maintaining global observing capabilities, and putting the pieces together. Obtaining the PDFs of key particle properties, adequately sampled, is now the leading observational deficiency. One simplifying factor is that, for a given aerosol source and season, aerosol amounts often vary, but particle properties tend to be repeatable. SAM-CAAM (Systematic Aircraft Measurements to Characterize Aerosol Air Masses), a modest aircraft payload deployed frequently could fill this gap, adding value to the entire satellite data record, improving aerosol property assumptions in retrieval algorithms, and providing MEEs to translate between remote-sensing optical constraints and aerosol mass book-kept in climate models [Kahn et al., BAMS 2017]. This will also improve connections between remote-sensing particle types and those defined in models. The third challenge, maintaining global observing capabilities, requires continued community effort and good budgetary fortune.

Spatial Variability of AERONET Aerosol Optical Properties and Satellite Data in South Korea during NASA DRAGON-Asia Campaign.

PubMed

Lee, Hyung Joo; Son, Youn-Suk

2016-04-05

We investigated spatial variability in aerosol optical properties, including aerosol optical depth (AOD), fine-mode fraction (FMF), and single scattering albedo (SSA), observed at 21 Aerosol Robotic Network (AERONET) sites and satellite remote sensing data in South Korea during the spring of 2012. These dense AERONET networks established in a National Aeronautics and Space Administration (NASA) field campaign enabled us to examine the spatially detailed aerosol size distribution and composition as well as aerosol levels. The springtime particle air quality was characterized by high background aerosol levels and high contributions of coarse-mode aerosols to total aerosols. We found that between-site correlations and coefficient of divergence for AOD and FMF strongly relied on the distance between sites, particularly in the south-north direction. Higher AOD was related to higher population density and lower distance from highways, and the aerosol size distribution and composition reflected source-specific characteristics. The ratios of satellite NO2 to AOD, which indicate the relative contributions of local combustion sources to aerosol levels, represented higher local contributions in metropolitan Seoul and Pusan. Our study demonstrates that the aerosol levels were determined by both local and regional pollution and that the relative contributions of these pollutions to aerosols generated spatial heterogeneity in the particle air quality.

Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site during SAPUSS - diurnal variations and PMF receptor modelling

NASA Astrophysics Data System (ADS)

Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

2013-04-01

Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter < 2.5 μm) resolved aerosol samples analysed by Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie European Union framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the approach used is the simultaneous sampling at two monitoring sites in Barcelona (Spain) during September-October 2010: an urban background site (UB) and a street canyon traffic road site (RS). Elements related to primary non-exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (regional sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non-exhaust brake dust (Fe-Cu) - 7%), and three types of industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%, percentages presented are average source contributions to the total elemental mass measured). The validity of the PMF solution of the PIXE data is supported by very good correlations with external single particle mass spectrometry measurements. Some important conclusions can be drawn about the PM2.5 mass fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with combustion emissions) is found to be the major (82%) source of fine Cl in the urban agglomerate; (4) the mean diurnal variation of PM2.5 primary traffic non-exhaust brake dust (Fe-Cu) suggests that this source is mainly emitted and not resuspended, whereas PM2.5 urban dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing urban dust concentrations.

A study of impact of Asian dusts and their transport pathways to Hong Kong using multiple AERONET data, trajectory, and in-situ measurements

NASA Astrophysics Data System (ADS)

Wong, Man Sing; Nichol, Janet Elizabeth; Lee, Kwon Ho

2010-10-01

Hong Kong, a commercial and financial city located in south-east China has suffered serious air pollution for the last decade due largely to rapid urban and industrial expansion of the cities of mainland China. However, the potential sources and pathways of aerosols transported to Hong Kong have not been well researched due to the lack of air quality monitoring stations in southern China. Here, an integrated method combining the AErosol RObotic NETwork (AERONET) data, trajectory and Potential Source Contribution Function (PSCF) modeling is used to identify the potential transport pathways and contribution of sources from four characteristic aerosol types. Four characteristic aerosol types were defined using a total of 730 AERONET data measurements between 2005 and 2008. They are coastal urban, polluted urban, dust (likely to be long distance desert dust), and heavy pollution. Results show that the sources of polluted urban and heavy pollution are associated with industrial emissions in southern China, whereas coastal urban aerosols have been affected both from natural marine aerosol and emissions. The PSCF map of dust shows a wide range of pathways followed by east- and south-eastwards trajectories from northwest China to Hong Kong. Although the contribution from dust sources is small compared to the anthropogenic aerosols, a serious recent dust outbreak has been observed in Hong Kong with an elevation of the Air Pollution Index to 500, compared with 50-100 on normal days. Therefore, the combined use of clustered AERONET data, trajectory and the PSCF models can help to resolve the longstanding issue about source regions and characteristics of pollutants carried to Hong Kong.

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

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

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

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

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

DOE PAGES

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

2016-07-11

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

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

NASA Astrophysics Data System (ADS)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging processes were further illustrated in a case study of a severe haze episode. Our results elucidated a complex response of aerosol chemistry to emission controls, which has significant implications that emission controls over regional scales can substantially reduce secondary particulates. However, stricter emission controls for local source emissions are needed for further mitigating air pollution in the megacity of Beijing.

Current and future contributions of local emissions from shipping and hydrocarbon extraction flaring to short lived pollutants in the Arctic

NASA Astrophysics Data System (ADS)

Marelle, L.; Raut, J. C.; Law, K.; Thomas, J. L.; Fast, J. D.; Berg, L. K.; Shrivastava, M. B.; Easter, R. C.; Herber, A. B.

2015-12-01

The Arctic is increasingly open to human activity due to rapid Arctic warming, associated with decreased sea ice extent and snow cover. While pollution from in-Arctic sources is currently low, oil and gas extraction and marine traffic could become a significant future source of short-lived pollutants (aerosols, ozone) in the Arctic. It is currently unclear if these local sources might become significant compared to the long-range transport of anthropogenic pollution from the midlatitudes, which is currently the main source of Arctic pollution. Here, we investigate the current (2012) and future (2050) impact of emissions from shipping and oil and gas extraction on Arctic aerosols and ozone, in relation to emissions from long-range transport. These impacts are determined by performing 6-month long, quasi-hemispheric simulations over the Arctic region with the WRF-Chem model. Our regional simulations include up-to-date representations of cloud/aerosol interactions and secondary organic aerosol formation developed recently for WRF-Chem. In order to determine the impact of Arctic shipping and oil and gas extraction, we use recent emission inventories by Winther et al., 2014 for local shipping and ECLIPSEv5 for oil and gas flaring. Both inventories suggest that current and future emissions from these sources are higher than previous estimates. Simulations are evaluated using measurements at Arctic surface sites and aircraft campaigns (ACCESS, YAK) in 2012. Model results are then used to assess the impact of Arctic shipping and oil and gas flaring on modeled surface aerosol and ozone concentrations, direct aerosol and ozone radiative effects, indirect aerosol radiative effects, and aerosol deposition. Results are used to determine if these local emissions are expected to have a significant influence on these quantities at the local or the regional scale, compared to emissions transported from the midlatitudes and to other emission sources, including boreal fires.

Light-absorbing oligomer formation in secondary organic aerosol from reactive uptake of isoprene epoxydiols.

PubMed

Lin, Ying-Hsuan; Budisulistiorini, Sri Hapsari; Chu, Kevin; Siejack, Richard A; Zhang, Haofei; Riva, Matthieu; Zhang, Zhenfa; Gold, Avram; Kautzman, Kathryn E; Surratt, Jason D

2014-10-21

Secondary organic aerosol (SOA) produced from reactive uptake and multiphase chemistry of isoprene epoxydiols (IEPOX) has been found to contribute substantially (upward of 33%) to the fine organic aerosol mass over the Southeastern U.S. Brown carbon (BrC) in rural areas of this region has been linked to secondary sources in the summer when the influence of biomass burning is low. We demonstrate the formation of light-absorbing (290 < λ < 700 nm) SOA constituents from reactive uptake of trans-β-IEPOX onto preexisting sulfate aerosols as a potential source of secondary BrC. IEPOX-derived BrC generated in controlled chamber experiments under dry, acidic conditions has an average mass absorption coefficient of ∼ 300 cm(2) g(-1). Chemical analyses of SOA constituents using UV-visible spectroscopy and high-resolution mass spectrometry indicate the presence of highly unsaturated oligomeric species with molecular weights separated by mass units of 100 (C5H8O2) and 82 (C5H6O) coincident with the observations of enhanced light absorption, suggesting such oligomers as chromophores, and potentially explaining one source of humic-like substances (HULIS) ubiquitously present in atmospheric aerosol. Similar light-absorbing oligomers were identified in fine aerosol collected in the rural Southeastern U.S., supporting their atmospheric relevance and revealing a previously unrecognized source of oligomers derived from isoprene that contributes to ambient fine aerosol mass.

Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions

PubMed Central

Gentner, Drew R.; Isaacman, Gabriel; Worton, David R.; Chan, Arthur W. H.; Dallmann, Timothy R.; Davis, Laura; Liu, Shang; Day, Douglas A.; Russell, Lynn M.; Wilson, Kevin R.; Weber, Robin; Guha, Abhinav; Harley, Robert A.; Goldstein, Allen H.

2012-01-01

Emissions from gasoline and diesel vehicles are predominant anthropogenic sources of reactive gas-phase organic carbon and key precursors to secondary organic aerosol (SOA) in urban areas. Their relative importance for aerosol formation is a controversial issue with implications for air quality control policy and public health. We characterize the chemical composition, mass distribution, and organic aerosol formation potential of emissions from gasoline and diesel vehicles, and find diesel exhaust is seven times more efficient at forming aerosol than gasoline exhaust. However, both sources are important for air quality; depending on a region’s fuel use, diesel is responsible for 65% to 90% of vehicular-derived SOA, with substantial contributions from aromatic and aliphatic hydrocarbons. Including these insights on source characterization and SOA formation will improve regional pollution control policies, fuel regulations, and methodologies for future measurement, laboratory, and modeling studies. PMID:23091031

Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions.

PubMed

Gentner, Drew R; Isaacman, Gabriel; Worton, David R; Chan, Arthur W H; Dallmann, Timothy R; Davis, Laura; Liu, Shang; Day, Douglas A; Russell, Lynn M; Wilson, Kevin R; Weber, Robin; Guha, Abhinav; Harley, Robert A; Goldstein, Allen H

2012-11-06

Emissions from gasoline and diesel vehicles are predominant anthropogenic sources of reactive gas-phase organic carbon and key precursors to secondary organic aerosol (SOA) in urban areas. Their relative importance for aerosol formation is a controversial issue with implications for air quality control policy and public health. We characterize the chemical composition, mass distribution, and organic aerosol formation potential of emissions from gasoline and diesel vehicles, and find diesel exhaust is seven times more efficient at forming aerosol than gasoline exhaust. However, both sources are important for air quality; depending on a region's fuel use, diesel is responsible for 65% to 90% of vehicular-derived SOA, with substantial contributions from aromatic and aliphatic hydrocarbons. Including these insights on source characterization and SOA formation will improve regional pollution control policies, fuel regulations, and methodologies for future measurement, laboratory, and modeling studies.

Fine mode aerosol chemistry over a rural atmosphere near the north-east coast of Bay of Bengal in India

NASA Astrophysics Data System (ADS)

Adak, Anandamay; Chatterjee, Abhijit; Ghosh, Sanjay; Raha, Sibaji; Roy, Arindam

2016-07-01

A study was conducted on the chemical characterization of fine mode aerosol or PM2.5 over a rural atmosphere near the coast of Bay of Bengal in eastern India. Samples were collected and analyzed during March 2013 - February 2014. The concentration of PM2.5 was found span over a wide range from as low as 3 µg m-3 to as high as 180 µg m-3. The average concentration of PM2.5 was 62 µg m-3. Maximum accumulation of fine mode aerosol was observed during winter whereas minimum was observed during monsoon. Water soluble ionic species of fine mode aerosol were characterized over this rural atmosphere. In spite of being situated near the coast of Bay of Bengal, we observed significantly higher concentrations for anthropogenic species like ammonium and sulphate. The concentrations of these two species were much higher than the sea-salt aerosols. Ammonium and sulphate contributed around 30 % to the total fine mode aerosols. Even dust aerosol species like calcium also showed higher concentrations. Chloride to sodium ratio was found to be much less than that in standard sea-water indicating strong interaction between sea-salt and anthropogenic aerosols. Use of fertilizers in various crop fields and human and animal wastes significantly increased ammonium in fine mode aerosols. Dust aerosol species were accumulated in the atmosphere which could be due to transport of finer dust species from nearby metropolis or locally generated. Non-sea-sulphate and nitrate showed significant contributions in fine mode aerosols having both local and transported sources. Source apportionment shows prominent emission sources of anthropogenic aerosols from local anthropogenic activities and transported from nearby Kolkata metropolis as well.

Contribution of regional-scale fire events to ozone and PM2.5 air quality estimated by photochemical modeling approaches

NASA Astrophysics Data System (ADS)

Baker, K. R.; Woody, M. C.; Tonnesen, G. S.; Hutzell, W.; Pye, H. O. T.; Beaver, M. R.; Pouliot, G.; Pierce, T.

2016-09-01

Two specific fires from 2011 are tracked for local to regional scale contribution to ozone (O3) and fine particulate matter (PM2.5) using a freely available regulatory modeling system that includes the BlueSky wildland fire emissions tool, Spare Matrix Operator Kernel Emissions (SMOKE) model, Weather and Research Forecasting (WRF) meteorological model, and Community Multiscale Air Quality (CMAQ) photochemical grid model. The modeling system was applied to track the contribution from a wildfire (Wallow) and prescribed fire (Flint Hills) using both source sensitivity and source apportionment approaches. The model estimated fire contribution to primary and secondary pollutants are comparable using source sensitivity (brute-force zero out) and source apportionment (Integrated Source Apportionment Method) approaches. Model estimated O3 enhancement relative to CO is similar to values reported in literature indicating the modeling system captures the range of O3 inhibition possible near fires and O3 production both near the fire and downwind. O3 and peroxyacetyl nitrate (PAN) are formed in the fire plume and transported downwind along with highly reactive VOC species such as formaldehyde and acetaldehyde that are both emitted by the fire and rapidly produced in the fire plume by VOC oxidation reactions. PAN and aldehydes contribute to continued downwind O3 production. The transport and thermal decomposition of PAN to nitrogen oxides (NOX) enables O3 production in areas limited by NOX availability and the photolysis of aldehydes to produce free radicals (HOX) causes increased O3 production in NOX rich areas. The modeling system tends to overestimate hourly surface O3 at routine rural monitors in close proximity to the fires when the model predicts elevated fire impacts on O3 and Hazard Mapping System (HMS) data indicates possible fire impact. A sensitivity simulation in which solar radiation and photolysis rates were more aggressively attenuated by aerosol in the plume reduced model O3 but does not eliminate this bias. A comparison of model predicted daily average speciated PM2.5 at surface rural routine network sites when the model predicts fire impacts from either of these fires shows a tendency toward overestimation of PM2.5 organic aerosol in close proximity to these fires. The standard version of the CMAQ treats primarily emitted organic aerosol as non-volatile. An alternative approach for treating organic aerosol as semi-volatile resulted in lower PM2.5 organic aerosol from these fires but does not eliminate the bias. Future work should focus on modeling specific fire events that are well characterized in terms of size, emissions, and have extensive measurements taken near the fire and downwind to better constrain model representation of important physical and chemical processes (e.g. aerosol photolysis attenuation and organic aerosol treatment) related to wild and prescribed fires.

Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

PubMed

Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

2009-04-01

Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

Long-term atmospheric deposition of nitrogen, phosphorus and sulfate in a large oligotrophic lake

PubMed Central

Craft, James A.; Stanford, Jack A.

2015-01-01

We documented significantly increasing trends in atmospheric loading of ammonium (NH4) and nitrate/nitrite (NO2/3) and decreasing trends in total phosphorus (P) and sulfate (SO4) to Flathead Lake, Montana, from 1985 to 2004. Atmospheric loading of NO2/3 and NH4 increased by 48 and 198% and total P and SO4 decreased by 135 and 39%. The molar ratio of TN:TP also increased significantly. Severe air inversions occurred periodically year-round and increased the potential for substantial nutrient loading from even small local sources. Correlations between our loading data and various measures of air quality in the basin (e.g., particulate matter <10 µm in size, aerosol fine soil mass, aerosol nutrient species, aerosol index, hectares burned) suggest that dust and smoke are important sources. Ammonium was the primary form of N in atmospheric deposition, whereas NO3 was the primary N form in tributary inputs. Atmospheric loading of NH4 to Flathead Lake averaged 44% of the total load and on some years exceeded tributary loading. Primary productivity in the lake is colimited by both N and P most of the year; and in years of high atmospheric loading of inorganic N, deposition may account for up to 6.9% of carbon converted to biomass. PMID:25802810

Long-term atmospheric deposition of nitrogen, phosphorus and sulfate in a large oligotrophic lake.

PubMed

Ellis, Bonnie K; Craft, James A; Stanford, Jack A

2015-01-01

We documented significantly increasing trends in atmospheric loading of ammonium (NH4) and nitrate/nitrite (NO2/3) and decreasing trends in total phosphorus (P) and sulfate (SO4) to Flathead Lake, Montana, from 1985 to 2004. Atmospheric loading of NO2/3 and NH4 increased by 48 and 198% and total P and SO4 decreased by 135 and 39%. The molar ratio of TN:TP also increased significantly. Severe air inversions occurred periodically year-round and increased the potential for substantial nutrient loading from even small local sources. Correlations between our loading data and various measures of air quality in the basin (e.g., particulate matter <10 µm in size, aerosol fine soil mass, aerosol nutrient species, aerosol index, hectares burned) suggest that dust and smoke are important sources. Ammonium was the primary form of N in atmospheric deposition, whereas NO3 was the primary N form in tributary inputs. Atmospheric loading of NH4 to Flathead Lake averaged 44% of the total load and on some years exceeded tributary loading. Primary productivity in the lake is colimited by both N and P most of the year; and in years of high atmospheric loading of inorganic N, deposition may account for up to 6.9% of carbon converted to biomass.

Final Report for “Simulating the Arctic Winter Longwave Indirect Effects. A New Parameterization for Frost Flower Aerosol Salt Emissions” (DESC0006679) for 9/15/2011 through 9/14/2015

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

Russell, Lynn M.; Somerville, Richard C.J.; Burrows, Susannah

Description of the Project: This project has improved the aerosol formulation in a global climate model by using innovative new field and laboratory observations to develop and implement a novel wind-driven sea ice aerosol flux parameterization. This work fills a critical gap in the understanding of clouds, aerosol, and radiation in polar regions by addressing one of the largest missing particle sources in aerosol-climate modeling. Recent measurements of Arctic organic and inorganic aerosol indicate that the largest source of natural aerosol during the Arctic winter is emitted from crystal structures, known as frost flowers, formed on a newly frozen seamore » ice surface [Shaw et al., 2010]. We have implemented the new parameterization in an updated climate model making it the first capable of investigating how polar natural aerosol-cloud indirect effects relate to this important and previously unrecognized sea ice source. The parameterization is constrained by Arctic ARM in situ cloud and radiation data. The modified climate model has been used to quantify the potential pan-Arctic radiative forcing and aerosol indirect effects due to this missing source. This research supported the work of one postdoc (Li Xu) for two years and contributed to the training and research of an undergraduate student. This research allowed us to establish a collaboration between SIO and PNNL in order to contribute the frost flower parameterization to the new ACME model. One peer-reviewed publications has already resulted from this work, and a manuscript for a second publication has been completed. Additional publications from the PNNL collaboration are expected to follow.« less

Detection of aerosol pollution sources during sandstorms in Northwestern China using remote sensed and model simulated data

NASA Astrophysics Data System (ADS)

Filonchyk, Mikalai; Yan, Haowen; Yang, Shuwen; Lu, Xiaomin

2018-02-01

The present paper has used a comprehensive approach to study atmosphere pollution sources including the study of vertical distribution characteristics, the epicenters of occurrence and transport of atmospheric aerosol in North-West China under intensive dust storm registered in all cities of the region in April 2014. To achieve this goal, the remote sensing data using Moderate Resolution Imaging Spectroradiometer satellite (MODIS) as well as model-simulated data, were used, which facilitate tracking the sources, routes, and spatial extent of dust storms. The results of the study have shown strong territory pollution with aerosol during sandstorm. According to ground-based air quality monitoring stations data, concentrations of PM10 and PM2.5 exceeded 400 μg/m3 and 150 μg/m3, respectively, the ratio PM2.5/PM10 being within the range of 0.123-0.661. According to MODIS/Terra Collection 6 Level-2 aerosol products data and the Deep Blue algorithm data, the aerosol optical depth (AOD) at 550 nm in the pollution epicenter was within 0.75-1. The vertical distribution of aerosols indicates that the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) 532 nm total attenuates backscatter coefficient ranges from 0.01 to 0.0001 km-1 × sr-1 with the distribution of the main types of aerosols in the troposphere of the region within 0-12.5 km, where the most severe aerosol contamination is observed in the lower troposphere (at 3-6 km). According to satellite sounding and model-simulated data, the sources of pollution are the deserted regions of Northern and Northwestern China.

Sources of primary and secondary organic aerosols in Chinese versus European Cities during winter time

NASA Astrophysics Data System (ADS)

Prevot, A. S.; Slowik, J.; El-Haddad, I.; Pieber, S. M.; Yuan, B.; Stefenelli, G.; Pospisilova, V.; Lopez-Hilfiker, F.; Qi, L.; Tong, Y.; Wang, L.; Daellenbach, K.; Klein, F.; Elser, M.; Junji, C.; Huang, R. J. J.; Baltensperger, U.

2017-12-01

In the recent years, aerosol mass spectrometric (AMS) measurements were performed in Beijing (China), Zurich (Switzerland) and other Chinese and European cities indicating the importance of not only primary sources but also secondary organic aerosol (SOA) sources despite low radiation levels for photooxidation. Among the primary sources, residential burning is especially important in winter including wood and coal burning. Also for secondary organic aerosols, VOC emissions of residential burning are likely an important source in winter. An interesting question is whether daytime photooxidation and/or night-time NO3 radical chemistry are important pathways for the SOA formation. Recently we developed a new measurement technique based on exctractive electrospray ionization (EESI) that allow for the study of the organic molecules in the particulate phase without fragmentation. Combined measurements with AMS and EESI will be discussed for smogchamber experiments (simulating both nighttime and daytime chemistry) SOA formation potential, the link between VOCs and SOA and the SOA composition. In-situ and off-line measurements in Europe and China are analyzed in the light of those experiments with a focus on the importance of residential burning to both primary and secondary organic aerosols in cities during winter.

MODELING PHOTOCHEMISTRY AND AEROSOL FORMATION IN POINT SOURCE PLUMES WITH THE CMAQ PLUME-IN-GRID

EPA Science Inventory

Emissions of nitrogen oxides and sulfur oxides from the tall stacks of major point sources are important precursors of a variety of photochemical oxidants and secondary aerosol species. Plumes released from point sources exhibit rather limited dimensions and their growth is gradu...

Compound Specific Isotope Analysis of Fatty Acids in Southern African Aerosols

NASA Astrophysics Data System (ADS)

Billmark, K. A.; Macko, S. A.; Swap, R. J.

2003-12-01

This study, conducted as a part of the Southern African Regional Science Initiative (SAFARI 2000), applied compound specific isotope analysis to describe aerosols at source regions and rural locations. Stable carbon isotopic compositions of individual fatty acids were determined for aerosol samples collected at four sites throughout southern Africa. Mongu, Zambia and Skukuza, South Africa were chosen for their location within intense seasonal Miombo woodland savanna and bushveld savanna biomass burning source regions, respectively. Urban aerosols were collected at Johannesburg, South Africa and rural samples were collected at Sua Pan, Botswana. Fatty acid isotopic compositions varied temporally. Urban aerosols showed significant isotopic enrichment of selected short chain fatty acids (C < 20) compared to aerosols produced during biomass combustion. Sua Pan short chain fatty acid signatures were significantly different from the other non-urban sites, which suggests that sources other than biomass combustion products, such as organic eolian material, impact the Sua Pan aerosol profile. However, a high degree of correlation between Sua Pan and Skukuza long chain fatty acid δ 13C values confirm atmospheric linkages between the two areas and that isotopic signatures of combusted fatty acids are unaltered during atmospheric transport highlighting their potential for use as a conservative tracer.

First Evaluation of the CCAM Aerosol Simulation over Africa: Implications for Regional Climate Modeling

NASA Astrophysics Data System (ADS)

Horowitz, H.; Garland, R. M.; Thatcher, M. J.; Naidoo, M.; van der Merwe, J.; Landman, W.; Engelbrecht, F.

2015-12-01

An accurate representation of African aerosols in climate models is needed to understand the regional and global radiative forcing and climate impacts of aerosols, at present and under future climate change. However, aerosol simulations in regional climate models for Africa have not been well-tested. Africa contains the largest single source of biomass-burning smoke aerosols and dust globally. Although aerosols are short-lived relative to greenhouse gases, black carbon in particular is estimated to be second only to carbon dioxide in contributing to warming on a global scale. Moreover, Saharan dust is exported great distances over the Atlantic Ocean, affecting nutrient transport to regions like the Amazon rainforest, which can further impact climate. Biomass burning aerosols are also exported from Africa, westward from Angola over the Atlantic Ocean and off the southeastern coast of South Africa to the Indian Ocean. Here, we perform the first extensive quantitative evaluation of the Conformal-Cubic Atmospheric Model (CCAM) aerosol simulation against monitored data, focusing on aerosol optical depth (AOD) observations over Africa. We analyze historical regional simulations for 1999 - 2012 from CCAM consistent with the experimental design of CORDEX at 50 km global horizontal resolution, through the dynamical downscaling of ERA-Interim data reanalysis data, with the CMIP5 emissions inventory (RCP8.5 scenario). CCAM has a prognostic aerosol scheme for organic carbon, black carbon, sulfate, and dust, and non-prognostic sea salt. The CCAM AOD at 550nm was compared to AOD (observed at 440nm, adjusted to 550nm with the Ångström exponent) from long-term AERONET stations across Africa. Sites strongly impacted by dust and biomass burning and with long continuous records were prioritized. In general, the model captures the monthly trends of the AERONET data. This presentation provides a basis for understanding how well aerosol particles are represented over Africa in regional climate modeling and the potential impact on climate predictions, and is the first large scale climate model-measurement verification of aerosols over Africa that we are aware of. CCAM is widely used for regional climate modeling applications, and we also discuss further improvements to the aerosol parameterizations based on our results.

Exploring Climatology and Long-Term Variations of Aerosols from NASA Reanalysis MERRA-2 with Giovanni

NASA Technical Reports Server (NTRS)

Shen, Suhung; Ostrenga, Dana; Vollmer, Bruce; Li, Zhanqing

2016-01-01

Dust plays important roles in energy cycle and climate variations. The dust deposition is the major source of iron in the open ocean, which is an essential micronutrient for phytoplankton growth and therefore may influence the ocean uptake of atmospheric CO2. Mineral dust can also act as fertilizer for forests over long time periods. Over 35 years of simulated global aerosol products from NASA atmospheric reanalysis, second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) are available from NASA Goddard Earth Science Data and Information Services Center (GES DISC). The MERRA-2 covers the period 1980-present, continuing as an ongoing climate analysis. Aerosol assimilation is included throughout the period, using MODIS, MISR, AERONET, and AVHRR (in the pre-EOS period). The aerosols are assimilated by using MERRA-2 aerosol model, which interact directly with the radiation parameterization, and radiatively coupled with atmospheric model dynamics in the Goddard Earth Observing System Model, Version 5 (GEOS-5). Dust deposition data along with other major aerosol compositions (e.g. black carbon, sea salt, and sulfate, etc.) are simulated as dry and wet deposition, respectively. The hourly and monthly data are available at spatial resolution of 0.5ox0.625o (latitude x longitude). Quick data exploration of climatology and interannual variations of MERRA-2 aerosol can be done through the online visualization and analysis tool, Giovanni. This presentation, using dust deposition as an example, demonstrates a number of MERRA-2 data services at GES DISC. Global distributions of dust depositions, and their seasonal and inter-annual variations are investigated from MERRA-2 monthly aerosol products.

Clouds, Aerosols, and Precipitation in the Marine Boundary Layer: An Arm Mobile Facility Deployment

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

Wood, Robert; Wyant, Matthew; Bretherton, Christopher S.

The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) 38 deployment at Graciosa Island in the Azores generated a 21 month (April 2009-December 2010) 39 comprehensive dataset documenting clouds, aerosols and precipitation using the Atmospheric 40 Radiation Measurement (ARM) Mobile Facility (AMF). The scientific aim of the deployment is 41 to gain improved understanding of the interactions of clouds, aerosols and precipitation in the 42 marine boundary layer. 43 Graciosa Island straddles the boundary between the subtropics and midlatitudes in the 44 Northeast Atlantic Ocean, and consequently experiences a great diversity of meteorological and 45 cloudiness conditions. Lowmore » clouds are the dominant cloud type, with stratocumulus and cumulus 46 occurring regularly. Approximately half of all clouds contained precipitation detectable as radar 47 echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1-48 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide 49 range of aerosol conditions was sampled during the deployment consistent with the diversity of 50 sources as indicated by back trajectory analysis. Preliminary findings suggest important two-way 51 interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation 52 and cloud radiative properties while being controlled in part by precipitation scavenging. 53 The data from at Graciosa are being compared with short-range forecasts made a variety 54 of models. A pilot analysis with two climate and two weather forecast models shows that they 55 reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well, 56 but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to 57 be a long-term ARM site that became operational in October 2013.« less

Characterize Aerosols from MODIS/MISR/OMI/MERRA-2: Dynamic Image Browse Perspective

NASA Astrophysics Data System (ADS)

Wei, J. C.; Yang, W.; Shen, S.; Zhao, P.; Albayrak, A.; Johnson, J. E.; Kempler, S. J.; Pham, L.

2016-12-01

Among the known atmospheric constituents, aerosols still represent the greatest uncertainty in climate research. To understand the uncertainty is to bring altogether of observational (in-situ and remote sensing) and modeling datasets and inter-compare them synergistically for a wide variety of applications that can bring far-reaching benefits to the science community and the broader society. These benefits can best be achieved if these earth science data (satellite and modeling) are well utilized and interpreted. Unfortunately, this is not always the case, despite the abundance and relative maturity of numerous satellite-borne sensors routinely measure aerosols. There is often disagreement between similar aerosol parameters retrieved from different sensors, leaving users confused as to which sensors to trust for answering important science questions about the distribution, properties, and impacts of aerosols. NASA Goddard Earth Sciences Data and Information Services Center (GES DISC) have developed multiple MAPSS (Multi-sensor Aerosol Products Sampling System) applications as a part of Giovanni (Geospatial Interactive Online Visualization and Analysis Interface) data visualization and analysis tool since 2007. The MAPSS database provides spatio-temporal statistics for multiple spatial spaceborne Level 2 aerosol products (MODIS Terra, MODIS Aqua, MISR, POLDER, OMI, CALIOP, SeaWiFS Deep Blue, and VIIRS) sampled over AERONET ground stations. In this presentation, I will demonstrate a new visualization service (NASA Level 2 Data Quality Visualization, DQViz) supporting various visualization and data accessing capabilities from satellite Level 2 (MODIS/MISR/OMI) and long term assimilated aerosols from NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2 displaying at their own native physical-retrieved spatial resolution. Functionality will include selecting data sources (e.g., multiple parameters under the same measurement), defining area-of-interest and temporal extents, zooming, panning, overlaying, sliding, and data subsetting and reformatting.

Comparison of Aerosol Single Scattering Albedos Derived By Diverse Techniques in Two North Atlantic Experiments

NASA Technical Reports Server (NTRS)

Russell, P. B.; Redemann, J.; Schmid, B.; Bergstrom, R. W.; Livingston, J. M.; McIntosh, D. M.; Hartley, S.; Hobbs, P. V.; Quinn, P. K.; Carrico, C. M.;

Source contributions to black carbon mass fractions in aerosol particles over the northwestern Pacific

NASA Astrophysics Data System (ADS)

Koga, Seizi; Maeda, Takahisa; Kaneyasu, Naoki

Aerosol particle number size distributions above 0.3 μm in diameter and black carbon mass concentrations in aerosols were observed on Chichi-jima of the Ogasawara Islands in the northwestern Pacific from January 2000 to December 2002. Chichi-jima is suitable to observe polluted air masses from East Asia in winter and clean air masses over the western North Pacific in summer. In winter, aerosols over Chichi-jima were strongly affected by anthropogenic emissions in East Asia. The form of energy consumption in East Asia varies in various regions. Hence, each source region is expected to be characterized by an individual black carbon mass fraction. A three-dimensional Eulerian transport model was used to estimate contribution rates to air pollutants from each source region in East Asia. Because the Miyake-jima eruption began at the end of June 2000, the influence of smokes from Miyake-jima was also considered in the model calculation. The results of model calculations represent what must be noticed about smokes from volcanoes including Miyake-jima to interpret temporal variations of sulfur compounds over the northwestern Pacific. To evaluate black carbon mass fractions in anthropogenic aerosols as a function of source region, the relationships between the volume concentration of aerosol particles and the black carbon mass concentration in the winter were classified under each source region in East Asia. Consequently, the black carbon mass fractions in aerosols from China, Japan and the Korean Peninsula, and other regions were estimated to be 9-13%, 5-7%, and 4-5%, respectively.

Characterization of marine aerosol for assessment of human exposure to brevetoxins.

PubMed

Cheng, Yung Sung; Zhou, Yue; Irvin, Clinton M; Pierce, Richard H; Naar, Jerome; Backer, Lorraine C; Fleming, Lora E; Kirkpatrick, Barbara; Baden, Dan G

2005-05-01

Red tides in the Gulf of Mexico are commonly formed by the fish-killing dinoflagellate Karenia brevis, which produces nine potent polyether brevetoxins (PbTxs). Brevetoxins can be transferred from water to air in wind-powered white-capped waves. Inhalation exposure to marine aerosol containing brevetoxins causes respiratory symptoms. We describe detailed characterization of aerosols during an epidemiologic study of occupational exposure to Florida red tide aerosol in terms of its concentration, toxin profile, and particle size distribution. This information is essential in understanding its source, assessing exposure to people, and estimating dose of inhaled aerosols. Environmental sampling confirmed the presence of brevetoxins in water and air during a red tide exposure period (September 2001) and lack of significant toxin levels in the water and air during an unexposed period (May 2002). Water samples collected during a red tide bloom in 2001 showed moderate-to-high concentrations of K. brevis cells and PbTxs. The daily mean PbTx concentration in water samples ranged from 8 to 28 microg/L from 7 to 11 September 2001; the daily mean PbTx concentration in air samples ranged from 1.3 to 27 ng/m(3). The daily aerosol concentration on the beach can be related to PbTx concentration in water, wind speed, and wind direction. Personal samples confirmed human exposure to red tide aerosols. The particle size distribution showed a mean aerodynamic diameter in the size range of 6-12 microm, with deposits mainly in the upper airways. The deposition pattern correlated with the observed increase of upper airway symptoms in healthy lifeguards during the exposure periods.

Atmospheric Aerosols in a Changing World

NASA Astrophysics Data System (ADS)

Heald, C. L.

2015-12-01

Aerosols in the atmosphere impact human and environmental health, visibility, and climate. Exposure to air pollution is the leading environmental cause of premature mortality world-wide. The role of aerosols on the Earth's climate represents the single largest source of uncertainty in our understanding of global radiative forcing. Tremendous strides have been made to clean up the air in recent decades, and yet poor air quality continues to plague many regions of the world, and our understanding of how global change will feedback on to aerosol sources, formation, and impacts is limited. In this talk, I will use recent results from my research group to highlight some of the key uncertainties and research topics in global aerosol lifecycle.

Testing for the Possible Influence of Unknown Climate Forcings upon Global Temperature Increases from 1950-2000

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

Anderson, Bruce T.; Knight, Jeff R.; Ringer, Mark A.

2012-10-15

Global-scale variations in the climate system over the last half of the twentieth century, including long-term increases in global-mean near-surface temperatures, are consistent with concurrent human-induced emissions of radiatively active gases and aerosols. However, such consistency does not preclude the possible influence of other forcing agents, including internal modes of climate variability or unaccounted for aerosol effects. To test whether other unknown forcing agents may have contributed to multidecadal increases in global-mean near-surface temperatures from 1950 to 2000, data pertaining to observed changes in global-scale sea surface temperatures and observed changes in radiatively active atmospheric constituents are incorporated into numericalmore » global climate models. Results indicate that the radiative forcing needed to produce the observed long-term trends in sea surface temperatures—and global-mean near-surface temperatures—is provided predominantly by known changes in greenhouse gases and aerosols. Further, results indicate that less than 10% of the long-term historical increase in global-mean near-surface temperatures over the last half of the twentieth century could have been the result of internal climate variability. In addition, they indicate that less than 25%of the total radiative forcing needed to produce the observed long-term trend in global-mean near-surface temperatures could have been provided by changes in net radiative forcing from unknown sources (either positive or negative). These results, which are derived from simple energy balance requirements, emphasize the important role humans have played in modifying the global climate over the last half of the twentieth century.« less

Size Resolved Measurements of Springtime Aerosol Particles over the Northern South China Sea

NASA Technical Reports Server (NTRS)

Atwood, Samuel A.; Reid, Jeffrey S.; Kreidenweis, Sonia M.; Cliff, Stephen S.; Zhao, Yongjing; Lin, Neng-Huei; Tsay, Si-Chee; Chu, Yu-Chi; Westphal, Douglas L.

2012-01-01

Large sources of aerosol particles and their precursors are ubiquitous in East Asia. Such sources are known to impact the South China Sea (henceforth SCS), a sometimes heavily polluted region that has been suggested as particularly vulnerable to climate change. To help elucidate springtime aerosol transport into the SCS, an intensive study was performed on the remote Dongsha (aka Pratas) Islands Atoll in spring 2010. As part of this deployment, a Davis Rotating-drum Uniform size-cut Monitor (DRUM) cascade impactor was deployed to collect size-resolved aerosol samples at the surface that were analyzed by X-ray fluorescence for concentrations of selected elements. HYSPLIT backtrajectories indicated that the transport of aerosol observed at the surface at Dongsha was occurring primarily from regions generally to the north and east. This observation was consistent with the apparent persistence of pollution and dust aerosol, along with sea salt, in the ground-based dataset. In contrast to the sea-level observations, modeled aerosol transport suggested that the westerly flow aloft (w700 hPa) transported smoke-laden air toward the site from regions from the south and west. Measured aerosol optical depth at the site was highest during time periods of modeled heavy smoke loadings aloft. These periods did not coincide with elevated aerosol concentrations at the surface, although the model suggested sporadic mixing of this free-tropospheric aerosol to the surface over the SCS. A biomass burning signature was not clearly identified in the surface aerosol composition data, consistent with this aerosol type remaining primarily aloft and not mixing strongly to the surface during the study. Significant vertical wind shear in the region also supports the idea that different source regions lead to varying aerosol impacts in different vertical layers, and suggests the potential for considerable vertical inhomogeneity in the SCS aerosol environment.

Type of Aerosols Determination Over Malaysia by AERONET Data

NASA Astrophysics Data System (ADS)

Lim, H.; Tan, F.; Abdullah, K.; Holben, B. N.

2013-12-01

Aerosols are one of the most interesting studies by the researchers due to the complicated of their characteristic and are not yet well quantified. Besides that there still have huge uncertainties associated with changes in Earth's radiation budget. The previous study by other researchers shown a lot of difficulties and challenges in quantifying aerosol influences arise. As well as the heterogeneity from the aerosol loading and properties: spatial, temporal, size, and composition. In this study, we were investigated the aerosol characteristics over two regions with different environmental conditions and aerosol sources contributed. The study sites are Penang and Kuching, Malaysia where ground-based AErosol RObotic NETwork (AERONET) sun-photometer was deployed. The types of the aerosols for both study sites were identified by analyzing aerosol optical depth, angstrom parameter and spectral de-convolution algorithm product from sun-photometer. The analysis was carried out associated with the in-situ meteorological data of relative humidity, visibility and air pollution index. The major aerosol type over Penang found in this study was hydrophobic aerosols. Whereas the hydrophilic type of the aerosols was highly distributed in Kuching. The major aerosol size distributions for both regions were identified in this study. The result also shows that the aerosol optical properties were affected by the types and characteristic of aerosols. Therefore, in this study we generated an algorithm to determine the aerosols in Malaysia by considered the environmental factors. From this study we found that the source of aerosols should always being consider in to retrieve the accurate information of aerosol for air quality study.

An automatic aerosol classification for earlinet: application and results

NASA Astrophysics Data System (ADS)

Papagiannopoulos, Nikolaos; Mona, Lucia; Amiridis, Vassilis; Binietoglou, Ioannis; D'Amico, Giuseppe; Guma-Claramunt, P.; Schwarz, Anja; Alados-Arboledas, Lucas; Amodeo, Aldo; Apituley, Arnoud; Baars, Holger; Bortoli, Daniele; Comeron, Adolfo; Guerrero-Rascado, Juan Luis; Kokkalis, Panos; Nicolae, Doina; Papayannis, Alex; Pappalardo, Gelsomina; Wandinger, Ulla; Wiegner, Matthias

2018-04-01

Aerosol typing is essential for understanding the impact of the different aerosol sources on climate, weather system and air quality. An aerosol classification method for EARLINET (European Aerosol Research Lidar Network) measurements is introduced which makes use the Mahalanobis distance classifier. The performance of the automatic classification is tested against manually classified EARLINET data. Results of the application of the method to an extensive aerosol dataset will be presented.

Accumulation-mode aerosol number concentrations in the Arctic during the ARCTAS aircraft campaign: Long-range transport of polluted and clean air from the Asian continent

NASA Astrophysics Data System (ADS)

Matsui, H.; Kondo, Y.; Moteki, N.; Takegawa, N.; Sahu, L. K.; Koike, M.; Zhao, Y.; Fuelberg, H. E.; Sessions, W. R.; Diskin, G.; Anderson, B. E.; Blake, D. R.; Wisthaler, A.; Cubison, M. J.; Jimenez, J. L.

2011-10-01

We evaluate the impact of transport from midlatitudes on aerosol number concentrations in the accumulation mode (light-scattering particles (LSP) with diameters >180 nm) in the Arctic during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. We focus on transport from the Asian continent. We find marked contrasts in the number concentration (NLSP), transport efficiency (TEN_LSP, the fraction transported from sources to the Arctic), size distribution, and the chemical composition of aerosols between air parcels from anthropogenic sources in East Asia (Asian AN) and biomass burning sources in Russia and Kazakhstan (Russian BB). Asian AN air had lower NLSP and TEN_LSP (25 cm-3 and 18% in spring and 6.2 cm-3 and 3.0% in summer) than Russian BB air (280 cm-3 and 97% in spring and 36 cm-3 and 7.6% in summer) due to more efficient wet scavenging during transport from East Asia. Russian BB in this spring is the most important source of accumulation-mode aerosols over the Arctic, and BB emissions are found to be the primary source of aerosols within all the data in spring during ARCTAS. On the other hand, the contribution of Asian AN transport had a negligible effect on the accumulation-mode aerosol number concentration in the Arctic during ARCTAS. Compared with background air, NLSP was 2.3-4.7 times greater for Russian BB air but 2.4-2.6 times less for Asian AN air in both spring and summer. This result shows that the transport of Asian AN air decreases aerosol number concentrations in the Arctic, despite the large emissions of aerosols in East Asia. The very low aerosol number concentrations in Asian AN air were caused by wet removal during vertical transport in association with warm conveyor belts (WCBs). Therefore, this cleansing effect will be prominent for air transported via WCBs from other midlatitude regions and seasons. The inflow of clean midlatitude air can potentially have an important impact on accumulation-mode aerosol number concentrations in the Arctic.

Azores 2017 Field Campaign Report

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

Wehner, Birgit; Chevallier, Karine; Weinhold, Kay

Aerosol particles play an important role for the regional and global climate. Therefore, a network of measurement sites has been established worldwide, but only a small fraction of them is capturing the marine boundary layer (MBL) while approximately 70% of the Earth’s surface is covered with water. The main focus of this project is to improve the knowledge of sources and exchange processes of aerosol particles in general (German Research Foundation [DFG] project WE 2757/2-1) and of cloud condensation nuclei in particular (DFG project HE 6770/2-1) in the MBL in the northeastern Atlantic Ocean where the influence of local anthropogenicmore » sources is negligible. The main hypothesis of the project is that long-range transport of aerosols from North America as well as new particle formation in the free troposphere (FT) and at cloud edges followed by vertical transport contribute significantly to the aerosol budget in the MBL. The knowledge of sources and sinks of aerosol particles in combination with vertical exchange between FT and MBL is a prerequisite to predict aerosol particle number concentrations in the lowest regions of the MBL and its influence on the formation of clouds. These processes are not sufficiently quantified over the ocean up to now. To verify the hypothesis stated above, vertical exchange processes and particle sources over the Azores will be quantified using data of 17 measurement flights with high spatial resolution using a helicopter-borne platform developed at the Leibniz Institute for Tropospheric Research (TROPOS). Here, aerosol particle number concentration and vertical wind speed have been measured with a temporal resolution allowing the direct estimate of the vertical turbulent flux of aerosol particles in different heights for the first time. In addition, aerosol particle number size distributions, number concentrations of cloud condensation nuclei (CCN), cloud droplet number concentration (CDNC), and particle absorption at three different wavelengths have been determined. The data analysis is ongoing and final results are not available yet. The detailed analysis of these data will be used to conclude sources and origin of the investigated aerosol particles.« less

Optical remote sensing of properties and concentrations of atmospheric trace constituents

NASA Astrophysics Data System (ADS)

Vladutescu, Daniela Viviana

The effect of human activities on the global climate may lead to large disturbances of the economic, social and political circumstances in the middle and long term. Understanding the dynamics of the Earth's climate is therefore of high importance and one of the major scientific challenges of our time. The estimation of the contribution of the Earth's climate system components needs observation and continuous monitoring of various atmospheric physical and chemical parameters. Temperature, water vapor and greenhouse gases concentration, aerosol and clouds loads, and atmospheric dynamics are parameters of particular importance in this respect. The quantification of the anthropogenic influence on the dynamics of these above-mentioned parameters is of crucial importance nowadays but still affected by significant uncertainties. In the present context of these huge uncertainties in our understanding of how these different atmospheric compounds contribute to the radiative forcing, a significant part of my research interest is related to the following topics: (1) Development of lidar (Light Detection and Ranging)-based remote sensing techniques for monitoring atmospheric compounds and processes; (2) Aerosols hygroscopic properties and atmospheric modeling; (3) Water vapor mixing ratio and relative humidity estimation in the troposphere; (4) Characterization of the long-range transported aerosols; (5) Ambient gases detection using Fourier Transform Interferometers (FTIR); (6) Design of inexpensive Fabry Perot Interferometer for visible and near infrared for land and ocean surface remote sensing applications. The lidar-based remote sensing measurement techniques for the monitoring of climate change parameters where implemented at the City College of the City University of New York (CCNY/CUNY) LIDAR station and are presented in the second section of the paper. The geographical location of the CCNY lidar station is 40.86N, -73.86W. Among the lidar retrievals one important application is the detection of water vapor in the atmosphere. Water vapor is an important greenhouse gas due to its high concentration in the atmosphere (parts per thousand), among the trace constituents, and its interaction with tropospheric aerosols particles. The upward convection of water vapor and aerosols due to intense heating of the ground lead to aggregation of water particles or ice on aerosols in the air forming different types of clouds at various altitudes. In this regard a reliable method of retrieving atmospheric water vapor profiles is presented in the third part of the paper. The proposed technique here is the Raman lidar procedure that is calibrated afterwards. The accuracy of the water vapor measurements is obtained by calibration techniques based on different techniques that where compared and validated. The calibration method is based on data fusion from different sources like: GPS (global positioning system) sunphotometer, radiosonde. The condensation of water vapor on aerosols is affecting their size, shape, refractive index and chemical composition. The warming or cooling effect of the clouds hence formed are both possible depending on the cloud location, cover, composition and structure. The effect of these clouds on radiative global forcing and therefore on the short and long term global climate is of high interest in the scientific world. In an effort to understand the hygroscopic properties of aerosols, a major interest is manifested in obtaining accurate vertical water vapor profiles simultaneously with aerosol extinction and backscatter profiles. A reliable method of retrieving atmospheric water vapor profiles and aerosols backscatter and extinction in the same atmospheric volume is presented in the fourth chapter of the paper. As mentioned above the determination of greenhouse gases and other molecular pollutants is important in process control as well as environmental monitoring. Since many molecular vibrational modes are in the infrared, molecules can absorb light from an infrared source (such as the sun or an artificial source such as a glow rod) and therefore, if the source spectrum is known, the absorption spectra of the sample can be measured. Therefore, any spectroscopy method needs a well characterized infrared source as well as an accurate high resolution spectrometer. In the fifth chapter of the paper is presented a standard technique for open-path detection of greenhouse gases which is based on Fourier Transform Infrared Spectroscopy (FTIR). A MIDAC open path FTIR instrument is presented along with measurements and analyses. In the group of spectrometers with a high spatial spectral resolution is found as well the Fabry Perot Interferometer that is presented in chapter 6. A visible-near infrared (VIS-NIR) scanning Fabry Perot Imager design is proposed based on combinations of Fabry Perot etalons and/or broadband interference filters that can in principle be used as a hyperspectral sensors from geostationary spaceborne platforms. Keywords. Lidar, Raman, Mie, water vapor mixing ratio, backscatter, extinction, relative humidity, aerosol hygroscopic properties, atmospheric model, FTIR, FPI, green house gases

Light absorption, optical and microphysical properties of trajectory-clustered aerosols at two AERONET sites in West Africa

NASA Astrophysics Data System (ADS)

Fawole, O. G.; Cai, X.; MacKenzie, A. R.

2015-12-01

Aerosol remote sensing techniques and back-trajectory modeling can be combined to identify aerosol types. We have clustered 7 years of AERONET aerosol signals using trajectory analysis to identify dominant aerosol sources at two AERONET sites in West Africa: Ilorin (4.34 oE, 8.32 oN) and Djougou (1.60 oE, 9.76 oN). Of particular interest are air masses that have passed through the gas flaring region in the Niger Delta area, of Nigeria, en-route the AERONET sites. 7-day back trajectories were calculated using the UK UGAMP trajectory model driven by ECMWF wind analyses data. Dominant sources identified, using literature classifications, are desert dust (DD), Biomass burning (BB) and Urban-Industrial (UI). Below, we use a combination of synoptic trajectories and aerosol optical properties to distinguish a fourth source: that due to gas flaring. Gas flaring, (GF) the disposal of gas through stack in an open-air flame, is believed to be a prominent source of black carbon (BC) and greenhouse gases. For these different aerosol source signatures, single scattering albedo (SSA), refractive index , extinction Angstrom exponent (EEA) and absorption Angstrom exponent (AAE) were used to classify the light absorption characteristics of the aerosols for λ = 440, 675, 870 and1020 nm. A total of 1625 daily averages of aerosol data were collected for the two sites. Of which 245 make up the GF cluster for both sites. For GF cluster, the range of fine-mode fraction is 0.4 - 0.7. Average values SSA(λ), for the total and GF clusters are 0.90(440), 0.93(675), 0.95(870) and 0.96(1020), and 0.93(440), 0.92(675), 0.9(870) and 0.9(1020), respectively. Values of for the GF clusters for both sites are 0.62 - 1.11, compared to 1.28 - 1.66 for the remainder of the clusters, which strongly indicates the dominance of carbonaceous particles (BC), typical of a highly industrial area. An average value of 1.58 for the real part of the refractive index at low SSA for aerosol in the GF cluster is also an indicator of high BC content. Extinction Angstrom exponent, is an indicator of the particle size. EAE values of 0.95-1.32 for aerosol in the GF cluster shows that the aerosols are mainly fine or accumulation mode while values of EAE (0.36-0.6) for the other cluster indicate coarse mode domination of the aerosol. See table 1 for a summary of result.

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

NASA Astrophysics Data System (ADS)

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

2013-05-01

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

Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

NASA Astrophysics Data System (ADS)

Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

2012-11-01

Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish city accounted for around 25-30% of the OC in aerosols. Besides the traffic input (10% of OC), residential wood burning was found to be another dominant emission source contributing to the atmospheric aerosol (up to 38% of OC) at the Swiss urban location. It was estimated that around 10% of the OC mass in the urban sites originates from cooking emissions. Aerosols from the urban area of Zurich presented a much higher PAH content, and benzo(a)pyrene equivalent concentrations sometimes exceeding the mandatory limit.

Comparison of Aerosol Single Scattering Albedos Derived by Diverse Techniques In Two North Atlantic Experiments

NASA Technical Reports Server (NTRS)

Russell, P. B.; Redemann, J.; Schmid, B.; Bergstrom, R. W.; Livingston, J. M.; McIntosh, D. M.; Ramirez, S. A.; Hartley, S.; Hobbs, P. V.; Quinn, P. K.

2002-01-01

Aerosol single scattering albedo omega (the ratio of scattering to extinction) is important in determining aerosol climatic effects, in explaining relationships between calculated and measured radiative fluxes, and in retrieving aerosol optical depths from satellite radiances. Recently, two experiments in the North Atlantic region, the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2), determined aerosol omega by a variety of techniques. The techniques included fitting of calculated to measured radiative fluxes; retrievals of omega from skylight radiances; best fits of complex refractive index to profiles of backscatter extinction, and size distribution; and in situ measurements of scattering and absorption at the surface and aloft. Both TARFOX and ACE-2 found a fairly wide range of values for omega at midvisable wavelengths approx. 550 nm, with omega(sub midvis) greater than or equal to 0.85 and less than or equal to 0.99 for the marine aerosol impacted by continental pollution. Frequency distributions of omega could usually be approximated by lognormals in omega(sub max) - omega, with some occurrence of bimodality, suggesting the influence of different aerosol sources or processing. In both TARFOX and ACE-2, closure tests between measured and calculated radiative fluxes yielded best-fit values of omega(sub midvis) 0.90 +/- 0.04 for the polluted boundary layer. Although these results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., thermal offsets, unknown gas absorption) The other techniques gave larger values for omega(sub midvis) for the polluted boundary layer, with a typical result of omega(sub midvis) = 0.95 +/- 0.04. Current uncertainties in omega are large in terms of climate effects More tests are needed of the consistency among different methods and of humidification effects on omega.

Long-term aerosol measurements in Gran Canaria, Canary Islands: Particle concentration, sources and elemental composition

NASA Astrophysics Data System (ADS)

Gelado-Caballero, MaríA. D.; López-GarcíA, Patricia; Prieto, Sandra; Patey, Matthew D.; Collado, Cayetano; HéRnáNdez-Brito, José J.

2012-02-01

There are very few sets of long-term measurements of aerosol concentrations over the North Atlantic Ocean, yet such data is invaluable in quantifying atmospheric dust inputs to this ocean region. We present an 8-year record of total suspended particles (TSP) collected at three stations on Gran Canaria Island, Spain (Taliarte at sea level, Tafira 269 m above sea level (a.s.l.) and Pico de la Gorra 1930 m a.s.l.). Using wet and dry deposition measurements, the mean dust flux was calculated at 42.3 mg m-2 d-1. Air mass back trajectories (HYSPLIT, NOAA) suggested that the Sahara desert is the major source of African dust (dominant during 32-50% of days), while the Sahel desert was the major source only 2-10% of the time (maximum in summer). Elemental composition ratios of African samples indicate that, despite the homogeneity of the dust in collected samples, some signatures of the bedrocks can still be detected. Differences were found for the Sahel, Central Sahara and North of Sahara regions in Ti/Al, Mg/Al and Ca/Al ratios, respectively. Elements often associated with pollution (Pb, Cd, Ni, Zn) appeared to share a common origin, while Cu may have a predominantly local source, as suggested by a decrease in the enrichment factor (EF) of Cu during dust events. The inter-annual variability of dust concentrations is investigated in this work. During winter, African dust concentration measurements at the Pico de la Gorra station were found to correlate with the North Atlantic Oscillation (NAO) index.

A State-of-the-Art Experimental Laboratory for Cloud and Cloud-Aerosol Interaction Research

NASA Technical Reports Server (NTRS)

Fremaux, Charles M.; Bushnell, Dennis M.

2011-01-01

The state of the art for predicting climate changes due to increasing greenhouse gasses in the atmosphere with high accuracy is problematic. Confidence intervals on current long-term predictions (on the order of 100 years) are so large that the ability to make informed decisions with regard to optimum strategies for mitigating both the causes of climate change and its effects is in doubt. There is ample evidence in the literature that large sources of uncertainty in current climate models are various aerosol effects. One approach to furthering discovery as well as modeling, and verification and validation (V&V) for cloud-aerosol interactions is use of a large "cloud chamber" in a complimentary role to in-situ and remote sensing measurement approaches. Reproducing all of the complex interactions is not feasible, but it is suggested that the physics of certain key processes can be established in a laboratory setting so that relevant fluid-dynamic and cloud-aerosol phenomena can be experimentally simulated and studied in a controlled environment. This report presents a high-level argument for significantly improved laboratory capability, and is meant to serve as a starting point for stimulating discussion within the climate science and other interested communities.

Aerosol Sampling Experiment on the International Space Station

NASA Technical Reports Server (NTRS)

Meyer, Marit E.

2017-01-01

The International Space Station (ISS) is a unique indoor environment which serves as both home and workplace to the astronaut crew. There is currently no particulate monitoring, although particulate matter requirements exist. An experiment to collect particles in the ISS cabin was conducted recently. Two different aerosol samplers were used for redundancy and to collect particles in two size ranges spanning from 10 nm to hundreds of micrometers. The Active Sampler is a battery operated thermophoretic sampler with an internal pump which draws in air and collects particles directly on a transmission electron microscope grid. This commercial-off-the-shelf device was modified for operation in low gravity. The Passive Sampler has five sampling surfaces which were exposed to air for different durations in order to collect at least one sample with an optimal quantity of particles for microscopy. These samples were returned to Earth for analysis with a variety of techniques to obtain long-term average concentrations and identify particle emission sources. Results are compared with the inventory of ISS aerosols which was created based on sparse data and the literature. The goal of the experiment is to obtain data on indoor aerosols on ISS for future particulate monitor design and development.

Autonomous Ozone and Aerosol Lidar Platform: Preliminary Results

NASA Astrophysics Data System (ADS)

Strawbridge, K. B.

2014-12-01

Environment Canada is developing an autonomous tropospheric ozone and aerosol lidar system for deployment in support of short-term field studies. Tropospheric ozone and aerosols (PM10 and PM2.5) are important atmospheric constituents in low altitude pollution affecting human health and vegetation. Ozone is photo-chemically active with nitrogen oxides and can have a distinct diurnal variability. Aerosols contribute to the radiative budget, are a tracer for pollution transport, undergo complex mixing, and contribute to visibility and cloud formation. This particular instrument will employ two separate lidar transmitter and receiver assemblies. The tropospheric ozone lidar, based on the differential absorption lidar (DIAL) technique, uses the fourth harmonics of a Nd:YAG laser directed into a CO2 Raman cell to produce 276 nm, 287nm and 299 nm (first to third Stokes lines) output wavelengths. The aerosol lidar is based on the 3+2 design using a tripled Nd:YAG to output 355 nm, 532 nm and 1064nm wavelengths. Both lidars will be housed in a modified cargo trailer allowing for easy deployment to remote areas. The unit can be operated and monitored 24 hours a day via an internet link and requires an external power source. Simultaneous ozone and aerosol lidar measurements will provide the vertical context necessary to understand the complex mixing and transformation of pollutants - particularly when deployed near other ground-based in-situ sensors. Preliminary results will be shown from a summer field study at the Centre For Atmospheric Research Experiments (CARE).

Long-term (2001-2012) trends of carbonaceous aerosols from a remote island in the western North Pacific: an outflow region of Asian pollutants

NASA Astrophysics Data System (ADS)

Boreddy, Suresh K. R.; Mozammel Haque, M.; Kawamura, Kimitaka

2018-01-01

The present study reports on long-term trends of carbonaceous aerosols in total suspended particulate (TSP) samples collected at Chichijima in the western North Pacific during 2001-2012. Seasonal variations of elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) concentrations showed maxima in winter to spring and minima in summer. These seasonal differences in the concentrations of carbonaceous aerosols were associated with the outflows of polluted air masses from East Asia, which are clearly distinguishable from pristine air masses from the central Pacific. The higher concentrations of carbonaceous aerosols during winter to spring are associated with long-range atmospheric transport of East Asian continental polluted air masses, whereas lower concentrations may be due to pristine air masses from the central Pacific in summer. The annual trends of OC / EC (+0.46 % yr-1), WSOC (+0.18 % yr-1) and WSOC / OC (+0.08 % yr-1) showed significant (p < 0.05) increases during the period of 2001-2012, suggesting that photochemical formation of WSOC and its contributions to secondary organic aerosols (SOAs) have increased over the western North Pacific via long-range atmospheric transport. We found a significant increase (+0.33 % yr-1) in nss-K+ / EC ratios, demonstrating that concentrations of biomass-burning-derived carbonaceous aerosols have increased, while those of primary fossil-fuel-derived aerosols have decreased over the western North Pacific. Further, secondary biogenic emissions are also important over the western North Pacific as inferred from a significant increase (+0.14 % yr-1) in the concentrations of methanesulfonate (MSA-, a tracer for biogenic sources). This point was further supported by a moderate correlation (r = 0.40) between WSOC and MSA-. We also found a significant increase in OC / TC (total carbon) and WSOC / TC ratios, further suggesting that photochemical formation of WSOC and its contributions to SOAs have increased over the western North Pacific during 2001-2012 via long-range atmospheric transport from East Asia.

Source apportionment of airborne particulate matter using organic compounds as tracers

NASA Astrophysics Data System (ADS)

Schauer, James J.; Rogge, Wolfgang F.; Hildemann, Lynn M.; Mazurek, Monica A.; Cass, Glen R.; Simoneit, Bernd R. T.

A chemical mass balance receptor model based on organic compounds has been developed that relates source contributions to airborne fine particle mass concentrations. Source contributions to the concentrations of specific organic compounds are revealed as well. The model is applied to four air quality monitoring sites in southern California using atmospheric organic compound concentration data and source test data collected specifically for the purpose of testing this model. The contributions of up to nine primary particle source types can be separately identified in ambient samples based on this method, and approximately 85% of the organic fine aerosol is assigned to primary sources on an annual average basis. The model provides information on source contributions to fine mass concentrations, fine organic aerosol concentrations and individual organic compound concentrations. The largest primary source contributors to fine particle mass concentrations in Los Angeles are found to include diesel engine exhaust, paved road dust, gasoline-powered vehicle exhaust, plus emissions from food cooking and wood smoke, with smaller contribution from tire dust, plant fragments, natural gas combustion aerosol, and cigarette smoke. Once these primary aerosol source contributions are added to the secondary sulfates, nitrates and organics present, virtually all of the annual average fine particle mass at Los Angeles area monitoring sites can be assigned to its source.

Spatial and Temporal Monitoring of Aerosol over Selected Urban Areas in Egypt

NASA Astrophysics Data System (ADS)

Shokr, Mohammed; El-Tahan, Mohammed; Ibrahim, Alaa

2015-04-01

We utilize remote sensing data of atmospheric aerosols from the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Terra and Aqua satellites to explore spatio-temporal patterns over selected urban sites in Egypt during 2000-2015. High resolution (10 x 10 km^2) Level 2, collection 5, quality-controlled product was used. The selected sites are characterized by different human and industrial activities as well as landscape and meteorological attributes. These have impacts on the dominant types and intensity of aerosols. Aerosol robotic network (AERONET) data were used to validate the calculations from MODIS. The suitability of the MODIS product in terms of spatial and temporal coverage as well as accuracy and robustness has been established. Seasonal patterns of aerosol concentration are identified and compared between the sites. Spatial gradient of aerosol is assessed in the vicinity of major aerosol-emission sites (e.g. Cairo) to determine the range of influence of the generated pollution. Peak aerosol concentrations are explained in terms of meteorological events and land cover. The limited trends found in the temporal records of the aerosol measurements will be confirmed using calibrated long-term ground observations. The study has been conducted under the PEER 2-239 research project titled "The Impact of Biogenic and Anthropogenic Atmospheric Aerosols to Climate in Egypt". Project website is CleanAirEgypt.org

Natural Aerosols Explain Seasonal and Spatial Patterns of Southern Ocean Cloud Albedo

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

McCoy, Daniel; Burrows, Susannah M.; Wood, R.

2015-07-17

Small particles called aerosols act as nucleation sites for cloud drop formation, affecting clouds and cloud properties – ultimately influencing the cloud dynamics, lifetime, water path and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations not only affect cloud properties themselves, but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. Here, it is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more thanmore » half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd over regions of high biological activity is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35-45°S) and by organic matter in sea spray aerosol at higher latitudes (45-55°S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m-2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.« less

Aerosol Production and Growth in the Upper Troposphere over the Amazon Forest Observed during ACRIDICON-CHUVA

NASA Astrophysics Data System (ADS)

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

2016-12-01

Observations during ACRIDICON-CHUVA showed high aerosol concentrations in the upper troposphere (UT) over the Amazon Basin, with aerosol number concentrations after normalization to STP often exceeding those in the boundary layer (BL) by one or two orders of magnitude. The measurements were made during the German-Brazilian cooperative aircraft campaign ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems) on the German research aircraft HALO. The campaign took place over the Amazon Basin in September/October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were consistently observed on all flights, using several aerosol metrics, including condensation nuclei (CN), cloud condensation nuclei (CCN), and chemical species mass concentrations. These UT aerosols were different in their composition and size distribution from the aerosol in the BL, making convective transport of particles unlikely as a source. The regions in the immediate outflow of deep convective clouds were depleted in aerosol particles, whereas dramatically enhanced small (<90 nm diameter) aerosol number concentrations were found in UT regions that had experienced outflow from deep convection in the preceding 24-48 hours. We also found elevated concentrations of larger (>90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest that aerosol production takes place in the UT from volatile material brought up by deep convection, which is converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol may be a source of particles to the BL, where they increase in size by the condensation of biogenic volatile organic carbon (BVOC) oxidation products. This may be an important source of aerosol particles in the Amazonian BL, where aerosol nucleation and new particle formation has not been observed. We propose that this may have been the dominant process supplying secondary aerosols in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.

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

NASA Astrophysics Data System (ADS)

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

2015-04-01

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

An inter-comparison of PM10 source apportionment using PCA and PMF receptor models in three European sites.

PubMed

Cesari, Daniela; Amato, F; Pandolfi, M; Alastuey, A; Querol, X; Contini, D

2016-08-01

Source apportionment of aerosol is an important approach to investigate aerosol formation and transformation processes as well as to assess appropriate mitigation strategies and to investigate causes of non-compliance with air quality standards (Directive 2008/50/CE). Receptor models (RMs) based on chemical composition of aerosol measured at specific sites are a useful, and widely used, tool to perform source apportionment. However, an analysis of available studies in the scientific literature reveals heterogeneities in the approaches used, in terms of "working variables" such as the number of samples in the dataset and the number of chemical species used as well as in the modeling tools used. In this work, an inter-comparison of PM10 source apportionment results obtained at three European measurement sites is presented, using two receptor models: principal component analysis coupled with multi-linear regression analysis (PCA-MLRA) and positive matrix factorization (PMF). The inter-comparison focuses on source identification, quantification of source contribution to PM10, robustness of the results, and how these are influenced by the number of chemical species available in the datasets. Results show very similar component/factor profiles identified by PCA and PMF, with some discrepancies in the number of factors. The PMF model appears to be more suitable to separate secondary sulfate and secondary nitrate with respect to PCA at least in the datasets analyzed. Further, some difficulties have been observed with PCA in separating industrial and heavy oil combustion contributions. Commonly at all sites, the crustal contributions found with PCA were larger than those found with PMF, and the secondary inorganic aerosol contributions found by PCA were lower than those found by PMF. Site-dependent differences were also observed for traffic and marine contributions. The inter-comparison of source apportionment performed on complete datasets (using the full range of available chemical species) and incomplete datasets (with reduced number of chemical species) allowed to investigate the sensitivity of source apportionment (SA) results to the working variables used in the RMs. Results show that, at both sites, the profiles and the contributions of the different sources calculated with PMF are comparable within the estimated uncertainties indicating a good stability and robustness of PMF results. In contrast, PCA outputs are more sensitive to the chemical species present in the datasets. In PCA, the crustal contributions are higher in the incomplete datasets and the traffic contributions are significantly lower for incomplete datasets.

Biomass Burning Dominates Brown Carbon Absorption in the Rural Southeastern U.S.

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Brown, S. S.; Guo, H.; Weber, R. J. J.; Xu, L.; Ng, N. L.; Stone, E. A.; Edgerton, E. S.; Baumann, K.; Hu, W.; Palm, B. B.; Jimenez, J. L.; Fry, J.; Ayres, B. R.; Draper, D.; Allen, H.

2014-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Brown carbon has a wavelength-dependent absorption that increases in the UV spectral region, and its major atmospheric sources include biomass burning, anthropogenic combustion of fossil fuels, and secondary organic aerosol. The rural Southeastern U.S. is influenced by high isoprene concentrations and varying concentrations of biomass burning aerosol, making it an ideal place to compare the relative contributions of these two sources to the brown carbon absorption budget. During the Southern Oxidant and Aerosol Study in summer 2013, we deployed a new field instrument that uses cavity enhanced spectroscopy with a broadband light source to measure aerosol optical extinction as a function of wavelength. 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 combine these data with direct absorption measurements of water-soluble organic carbon obtained from a novel UV/VIS-WSOC instrument, and with aerosol composition measurements. We examine these data sets to determine: 1) the optical closure between measured dry aerosol extinction and values calculated from aerosol composition and size distribution; 2) the magnitude of brown and black carbon absorption; 3) the relative contributions of biomass burning, anthropogenic, and secondary organic aerosol contributions to brown carbon absorption in the Southeast U.S. during the summer. We conclude that biomass burning is a major contributor to optical absorption by organic aerosol in the rural southeastern U.S.

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

NASA Astrophysics Data System (ADS)

Lee, H.-H.; Chen, S.-H.; Kleeman, M. J.; Zhang, H.; DeNero, S. P.; Joe, D. K.

2015-11-01

The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-dimensional chemical variable (X, Z, Y, Size Bins, Source Types, Species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and longwave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into CCN at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

Aerosol carbon isotope composition over Baltic Sea

NASA Astrophysics Data System (ADS)

Garbaras, Andrius; Pabedinskas, Algirdas; Masalaite, Agne; Petelski, Tomasz; Gorokhova, Elena; Sapolaite, Justina; Ezerinskis, Zilvinas; Remeikis, Vidmantas

2017-04-01

Particulate carbonaceous matter is significant contributor to ambient particulate matter originating from intervening sources which contribution is difficult to quantify due to source diversity, chemical complexity and processes during atmospheric transport. Carbon isotope analysis can be extremely useful in source apportionment of organic matter due to the unique isotopic signatures associated with anthropocentric (fossil fuel), continental (terrestrial plants) and marine sources, and is particularly effective when these sources are mixed (Ceburnis et al., 2011;Ceburnis et al., 2016). We will present the isotope ratio measurement results of aerosol collected during the cruise in the Baltic Sea. Sampling campaign of PM10 and size segregated aerosol particles was performed on the R/V "Oceania" in October 2015. Air mass back trajectories were prevailing both from the continental and marine areas during the sampling period. The total carbon concentration varied from 1 µg/m3 to 8 µg/m3. Two end members (δ13C = -25‰ and δ13C = -28 ‰ ) were established from the total stable carbon isotope analysis in PM10 fraction. δ13C analysis in size segregated aerosol particles revealed δ13C values being highest in the 1 - 2.5 µm range (δ13C = -24.9 ‰ ) during continental transport, while lowest TC δ13C values (δ13C ≈ -27 ‰ ) were detected in the size range D50 <1 µm during stormy weather when air mass trajectory prevailed from the western direction. These measurements revealed that simplified isotope mixing model can not be applied for the aerosol source apportionment (Masalaite et al., 2015) in the perturbed marine environment. Additionally, concentration of bacteria and fungi were measured in size segregated and PM10 aerosol fraction. We were able to relate aerosol source δ13C end members with the abundance of bacteria and fungi over Baltic Sea combining air mass trajectories, stable isotope data, fungi and bacteria concentrations. Ceburnis, D., Garbaras, A., Szidat, S., Rinaldi, M., Fahrni, S., Perron, N., Wacker, L., Leinert, S., Remeikis, V., and Facchini, M.: Quantification of the carbonaceous matter origin in submicron marine aerosol by 13 C and 14 C isotope analysis, Atmospheric Chemistry and Physics, 11, 8593-8606, 2011. Ceburnis, D., Masalaite, A., Ovadnevaite, J., Garbaras, A., Remeikis, V., Maenhaut, W., Claeys, M., Sciare, J., Baisnée, D., and O'Dowd, C. D.: Stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in marine aerosol, Scientific Reports, 6, 2016. Masalaite, A., Remeikis, V., Garbaras, A., Dudoitis, V., Ulevicius, V., and Ceburnis, D.: Elucidating carbonaceous aerosol sources by the stable carbon δ13C TC ratio in size-segregated particles, Atmospheric Research, 158, 1-12, 2015.

CARBON CONTAINING COMPONENT OF THE LOS ANGELES AEROSOL: SOURCE APPORTIONMENT AND CONTRIBUTIONS TO THE VISIBILITY BUDGET

EPA Science Inventory

Source resolution of the organic component of the fine fraction of the ambient aerosol (d(sub p) < 3.5 micrometers) has been carried out by combining source information from the organic component with thermal analysis and local emission inventories. The primary and secondary carb...

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.

Impact of Transpacific Aerosol on Air Quality over the United States: A Perspective from Aerosol-Cloud-Radiation Interactions

NASA Technical Reports Server (NTRS)

Tao, Zhining; Yu, Hongbin; Chin, Mian

2015-01-01

Observations have well established that aerosols from various sources in Asia, Europe, and Africa can travel across the Pacific and reach the contiguous United States (U.S.) at least on episodic bases throughout a year, with a maximum import in spring. The imported aerosol not only can serve as an additional source to regional air pollution (e.g., direct input), but also can influence regional air quality through the aerosol-cloud-radiation (ACR) interactions that change local and regional meteorology. This study assessed impacts of the transpacific aerosol on air quality, focusing on surface ozone and PM2.5, over the U.S. using the NASA Unified Weather Research Forecast model. Based on the results of 3- month (April to June of 2010) simulations, the impact of direct input (as an additional source) of transpacific aerosol caused an increase of surface PM2.5 concentration by approximately 1.5 micro-g/cu m over the west coast and about 0.5 micro-g/cu m over the east coast of the U.S. By influencing key meteorological processes through the ACR interactions, the transpacific aerosol exerted a significant effect on both surface PM2.5 (+/-6 micro-g/cu m3) and ozone (+/-12 ppbv) over the central and eastern U.S. This suggests that the transpacific transport of aerosol could either improve or deteriorate local air quality and complicate local effort toward the compliance with the U.S. National Ambient Air Quality Standards.

Long-term Aerosol Lidar Measurements At CNR-IMAA

NASA Astrophysics Data System (ADS)

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

2006-12-01

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

Empirical retrieval of sea spray aerosol production using satellite microwave radiometry

NASA Astrophysics Data System (ADS)

Savelyev, I. B.; Yelland, M. J.; Norris, S. J.; Salisbury, D.; Pascal, R. W.; Bettenhausen, M. H.; Prytherch, J.; Anguelova, M. D.; Brooks, I. M.

2017-12-01

This study presents a novel approach to obtaining global sea spray aerosol (SSA) production source term by relying on direct satellite observations of the ocean surface, instead of more traditional approaches driven by surface meteorology. The primary challenge in developing this empirical algorithm is to compile a calibrated, consistent dataset of SSA surface flux collected offshore over a variety of conditions (i.e., regions and seasons), thus representative of the global SSA production variability. Such dataset includes observations from SEASAW, HiWASE, and WAGES field campaigns, during which the SSA flux was measured from the bow of a research vessel using consistent and state-of-the-art eddy covariance methodology. These in situ data are matched to observations of the state of the ocean surface from Windsat polarimetric microwave satellite radiometer. Previous studies demonstrated the ability of WindSat to detect variations in surface waves slopes, roughness and foam, which led to the development of retrieval algorithms for surface wind vector and more recently whitecap fraction. Similarly, in this study, microwave emissions from the ocean surface are matched to and calibrated against in situ observations of the SSA production flux. The resulting calibrated empirical algorithm is applicable for retrieval of SSA source term throughout the duration of Windsat mission, from 2003 to present.

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 solar spectrum, an effect that is enhanced by the contrast between the bright snow/ice surfaces and the dark BC. When deposited on snow and ice, BC also accelerates melting and lowers the surface albedo. SO4 however is more scattering and, therefore, cooling. The model results are compared among each other and evaluated against ground-based in-situ and remote sensing, as well as active satellite observations. The following questions are addressed in the evaluation: 1) Are the sources and transport pathways of aerosol to the Arctic region captured? 2) Is the annual cycle of aerosol conditions reproduced? 3) What are uncertainties related to the emission database? After thorough evaluation, the model results will provide a state-of-the-art estimate of the aerosol budget and the effective radiative forcing by anthropogenic aerosols in the Arctic region.

Optical, physical and chemical properties of transported African mineral dust aerosols in the Mediterranean region

NASA Astrophysics Data System (ADS)

Denjean, Cyrielle; Di Biagio, Claudia; Chevaillier, Servanne; Gaimoz, Cécile; Grand, Noel; Loisil, Rodrigue; Triquet, Sylvain; Zapf, Pascal; Roberts, Greg; Bourrianne, Thierry; Torres, Benjamin; Blarel, Luc; Sellegri, Karine; Freney, Evelyn; Schwarzenbock, Alfons; Ravetta, François; Laurent, Benoit; Mallet, Marc; Formenti, Paola

2014-05-01

The transport of mineral dust aerosols is a global phenomenon with strong climate implications. Depending on the travel distance over source regions, the atmospheric conditions and the residence time in the atmosphere, various transformation processes (size-selective sedimentation, mixing, condensation of gaseous species, and weathering) can modify the physical and chemical properties of mineral dust, which, in turn, can change the dust's optical properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of these properties, and their temporal evolution with transport time. Within the frame of the ChArMex project (Chemistry-Aerosol Mediterranean experiment, http://charmex.lsce.ipsl.fr/), two intensive airborne campaigns (TRAQA, TRansport and Air QuAlity, 18 June - 11 July 2012, and ADRIMED, Aerosol Direct Radiative Impact in the regional climate in the MEDiterranean region, 06 June - 08 July 2013) have been performed over the Central and Western Mediterranean, one of the two major transport pathways of African mineral dust. In this study we have set up a systematic strategy to determine the optical, physical and optical properties of mineral dust to be compared to an equivalent dataset for dust close to source regions in Africa. This study is based on airborne observations onboard the SAFIRE ATR-42 aircraft, equipped with state of the art in situ instrumentation to measure the particle scattering and backscattering coefficients (nephelometer at 450, 550, and 700 nm), the absorption coefficient (PSAP at 467, 530, and 660 nm), the extinction coefficient (CAPS at 530 nm), the aerosol optical depth (PLASMA at 340 to 1640 nm), the size distribution in the extended range 40 nm - 30 µm by the combination of different particle counters (SMPS, USHAS, FSSP, GRIMM) and the chemical composition obtained by filter sampling. The chemistry and transport model CHIMERE-Dust have been used to classify the air masses according to the dust origin and transport. Case studies of dust transport from known but differing origins (source regions in Tunisia, Algeria, and Mauritania) and at different times after transport, will be presented. Results will be compared to equivalent measurements over source regions interpreted in terms of the evolution of the particle size distribution, chemical composition and optical properties.

African Dust Aerosols as Atmospheric Ice Nuclei

NASA Technical Reports Server (NTRS)

DeMott, Paul J.; Brooks, Sarah D.; Prenni, Anthony J.; Kreidenweis, Sonia M.; Sassen, Kenneth; Poellot, Michael; Rogers, David C.; Baumgardner, Darrel

2003-01-01

Measurements of the ice nucleating ability of aerosol particles in air masses over Florida having sources from North Africa support the potential importance of dust aerosols for indirectly affecting cloud properties and climate. The concentrations of ice nuclei within dust layers at particle sizes below 1 pn exceeded 1/cu cm; the highest ever reported with our device at temperatures warmer than homogeneous freezing conditions. These measurements add to previous direct and indirect evidence of the ice nucleation efficiency of desert dust aerosols, but also confirm their contribution to ice nuclei populations at great distances from source regions.

Transport of Aerosols: Regional and Global Implications for Climate, Weather, and Air Quality

NASA Technical Reports Server (NTRS)

Chin, Mian; Diehl, Thomas; Yu, Hongbin; Bian, Huisheng; Remer, Lorraine; Kahn, Ralph

2008-01-01

Long-range transport of atmospheric aerosols can have a significant impact on global climate, regional weather, and local air quality. In this study, we use a global model GOCART together with satellite data and ground-based measurements to assess the emission and transport of pollution, dust, biomass burning, and volcanic aerosols and their implications. In particular, we will show the impact of emissions and long-range transport of aerosols from major pollution and dust source regions to (1) the surface air quality, (2) the atmospheric heating rates, and (3) surface radiation change near the source and downwind regions.

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

NASA Astrophysics Data System (ADS)

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

2013-04-01

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

ACTRIS ACSM intercomparison - Part 2: Intercomparison of ME-2 organic source apportionment results from 15 individual, co-located aerosol mass spectrometers

NASA Astrophysics Data System (ADS)

Fröhlich, R.; Crenn, V.; Setyan, A.; Belis, C. A.; Canonaco, F.; Favez, O.; Riffault, V.; Slowik, J. G.; Aas, W.; Aijälä, M.; Alastuey, A.; Artiñano, B.; Bonnaire, N.; Bozzetti, C.; Bressi, M.; Carbone, C.; Coz, E.; Croteau, P. L.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Jayne, J. T.; Lunder, C. R.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petralia, E.; Poulain, L.; Priestman, M.; Ripoll, A.; Sarda-Estève, R.; Wiedensohler, A.; Baltensperger, U.; Sciare, J.; Prévôt, A. S. H.

2015-02-01

Chemically resolved atmospheric aerosol data sets from the largest intercomparison of the Aerodyne aerosol chemical speciation monitors (ACSM) performed to date were collected at the French atmospheric supersite SIRTA. In total 13 quadrupole ACSMs (Q-ACSM) from the European ACTRIS ACSM network, one time-of-flight ACSM (ToF-ACSM), and one high-resolution ToF aerosol mass spectrometer (AMS) were operated in parallel for about three weeks in November and December 2013. Part 1 of this study reports on the accuracy and precision of the instruments for all the measured species. In this work we report on the intercomparison of organic components and the results from factor analysis source apportionment by positive matrix factorisation (PMF) utilising the multilinear engine 2 (ME-2). Except for the organic contribution of m/z 44 to the total organics (f44), which varied by factors between 0.6 and 1.3 compared to the mean, the peaks in the organic mass spectra were similar among instruments. The m/z 44 differences in the spectra resulted in a variable f44 in the source profiles extracted by ME-2, but had only a minor influence on the extracted mass contributions of the sources. The presented source apportionment yielded four factors for all 15 instruments: hydrocarbon-like organic aerosol (HOA), cooking-related organic aerosol (COA), biomass burning-related organic aerosol (BBOA) and secondary oxygenated organic aerosol (OOA). Individual application and optimisation of the ME-2 boundary conditions (profile constraints) are discussed together with the investigation of the influence of alternative anchors (reference profiles). A comparison of the ME-2 source apportionment output of all 15 instruments resulted in relative SD from the mean between 13.7 and 22.7% of the source's average mass contribution depending on the factors (HOA: 14.3 ± 2.2%, COA: 15.0 ± 3.4%, OOA: 41.5 ± 5.7%, BBOA: 29.3 ± 5.0%). Factors which tend to be subject to minor factor mixing (in this case COA) have higher relative uncertainties than factors which are recognised more readily like the OOA. Averaged over all factors and instruments the relative first SD from the mean of a source extracted with ME-2 was 17.2%.

Source appointment of fine particle number and volume concentration during severe haze pollution in Beijing in January 2013.

PubMed

Liu, Zirui; Wang, Yuesi; Hu, Bo; Ji, Dongsheng; Zhang, Junke; Wu, Fangkun; Wan, Xin; Wang, Yonghong

2016-04-01

Extreme haze episodes repeatedly shrouded Beijing during the winter of 2012-2013, causing major environmental and health problems. To better understand these extreme events, particle number size distribution (PNSD) and particle chemical composition (PCC) data collected in an intensive winter campaign in an urban site of Beijing were used to investigate the sources of ambient fine particles. Positive matrix factorization (PMF) analysis resolved a total of eight factors: two traffic factors, combustion factors, secondary aerosol, two accumulation mode aerosol factors, road dust, and long-range transported (LRT) dust. Traffic emissions (54%) and combustion aerosol (27%) were found to be the most important sources for particle number concentration, whereas combustion aerosol (33%) and accumulation mode aerosol (37%) dominated particle volume concentrations. Chemical compositions and sources of fine particles changed dynamically in the haze episodes. An enhanced role of secondary inorganic species was observed in the formation of haze pollution. Regional transport played an important role for high particles, contribution of which was on average up to 24-49% during the haze episodes. Secondary aerosols from urban background presented the largest contributions (45%) for the rapid increase of fine particles in the severest haze episode. In addition, the invasion of LRT dust aerosols further elevated the fine particles during the extreme haze episode. Our results showed a clear impact of regional transport on the local air pollution, suggesting the importance of regional-scale emission control measures in the local air quality management of Beijing.

Investigation of air pollution and regional climate change due to anthropogenic aerosols

NASA Astrophysics Data System (ADS)

Nakata, Makiko; Sano, Itaru; Mukai, Sonoyo

2016-10-01

Increased emissions of anthropogenic aerosols associated with economic growth can lead to increased concentrations of hazardous air pollutants. In particular, large cities in East Asia have experienced numerous heavy haze episodes. Atmospheric aerosol distributions in East Asia are complex, being influenced by both natural phenomena and human activity, with urban areas in particular being dominated by fine anthropogenic aerosols released from diesel-powered vehicles and industrial activity. In Japan, air pollution levels have been reduced; nevertheless, in recent years, there is increasing concern regarding air pollution caused by fine particulate matter. The origins of air pollution were examined, focusing on the comparison between aerosol properties observed from satellites and that on the ground. Because of their short life spans, concentrations of anthropogenic aerosols are highest over the source regions, and as a result, the climatic impacts of anthropogenic aerosols are also found to be most pronounced in these regions. In this study, aerosol impacts on climate are assessed by numerical model simulations. The direct effects of aerosols include reduced solar radiation, and hence a decrease in surface temperatures. In addition to these changes in the radiation budget, aerosols have a significant potential to change cloud and precipitation fields. These climatic responses to aerosols can manifest far from their source regions with high industrial activities.

Peak fitting and integration uncertainties for the Aerodyne Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Corbin, J. C.; Othman, A.; Haskins, J. D.; Allan, J. D.; Sierau, B.; Worsnop, D. R.; Lohmann, U.; Mensah, A. A.

2015-04-01

The errors inherent in the fitting and integration of the pseudo-Gaussian ion peaks in Aerodyne High-Resolution Aerosol Mass Spectrometers (HR-AMS's) have not been previously addressed as a source of imprecision for these instruments. This manuscript evaluates the significance of these uncertainties and proposes a method for their estimation in routine data analysis. Peak-fitting uncertainties, the most complex source of integration uncertainties, are found to be dominated by errors in m/z calibration. These calibration errors comprise significant amounts of both imprecision and bias, and vary in magnitude from ion to ion. The magnitude of these m/z calibration errors is estimated for an exemplary data set, and used to construct a Monte Carlo model which reproduced well the observed trends in fits to the real data. The empirically-constrained model is used to show that the imprecision in the fitted height of isolated peaks scales linearly with the peak height (i.e., as n1), thus contributing a constant-relative-imprecision term to the overall uncertainty. This constant relative imprecision term dominates the Poisson counting imprecision term (which scales as n0.5) at high signals. The previous HR-AMS uncertainty model therefore underestimates the overall fitting imprecision. The constant relative imprecision in fitted peak height for isolated peaks in the exemplary data set was estimated as ~4% and the overall peak-integration imprecision was approximately 5%. We illustrate the importance of this constant relative imprecision term by performing Positive Matrix Factorization (PMF) on a~synthetic HR-AMS data set with and without its inclusion. Finally, the ability of an empirically-constrained Monte Carlo approach to estimate the fitting imprecision for an arbitrary number of known overlapping peaks is demonstrated. Software is available upon request to estimate these error terms in new data sets.

Chemical characterization and source apportionment of fine and coarse particulate matter in Lahore, Pakistan

NASA Astrophysics Data System (ADS)

Stone, Elizabeth; Schauer, James; Quraishi, Tauseef A.; Mahmood, Abid

2010-03-01

Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM 2.5 and PM 10) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM 2.5 was 194 ± 94 μg m -3 and PM 10 was 336 ± 135 μg m -3. Coarse aerosol (PM 10-2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM 2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.

Chinese Soot on a Vietnamese Soup

NASA Astrophysics Data System (ADS)

Mari, X.

2015-12-01

Black Carbon (BC) is an aerosol emitted as soot during biomass burning and fossil fuels combustion together with other carbonaceous aerosols such as organic carbon (OC) and polyaromatic hydrocarbons (PAHs). While the impacts of BC on health and climate have been studied for many years, studies about its deposition and impact on marine ecosystems are scares. This is rather surprising considering that a large fraction of atmospheric BC deposits on the surface of the ocean via dry or wet deposition. On a global scale, deposition on the ocean is about 45 Tg C per year, with higher fluxes in the northern hemisphere and in inter-tropical regions, following the occurrence of the hot-spots of concentration. In the present study conducted on shore, in Haiphong and Halong cities, North Vietnam, we measured the seasonal variations of atmospheric BC, OC and PAHs during a complete annual cycle. The presentation will discuss the atmospheric results in terms of seasonal variability and sources. Inputs to the marine system are higher during the dry season, concomitantly with the arrival of air masses enriched in BC coming from the North. However, the carbon fingerprint can significantly differ at shorter time periods depending on the air mass pathway and speed. Our work leads to the characterization and the determination of the relative contribution of more specific sources like local traffic, which includes tourism and fishing boats, coal dust emitted from the nearby mine, and long-range transported aerosols. This variable input of carbonaceous aerosols might have consequences for the cycling and the repartition of carbon and nutrients in the marine ecosystem of Halong Bay.

Geographical Distribution and Sources of Nutrients in Atmospheric Aerosol Over the Pacific Ocean

NASA Astrophysics Data System (ADS)

Uematsu, M.

2016-12-01

The Pacific Ocean, the world's largest (occupying about 30% of the Earth's total surface area) has several distinguishing biogeochemical features. In the western Pacific, dust particles originating from arid and semi-arid regions in Asia and Australia are transported to the north and south, respectively. Biomass burning emissions from Southeast Asia are exported to the tropical Pacific, and anthropogenic substances flowing out of Asia and Eurasia spread both regionally and globally. Over high primary productive areas such as the subarctic North Pacific, the equatorial Pacific and the Southern Ocean, biogenic gasses are released to the atmosphere and transported to other areas. These processes may affect cloud and rainfall patterns, air quality, and the radiative balance of downwind regions. The deposition of atmospheric aerosols containing iron and other essential nutrients is important for biogeochemical cycles in the oceans because this source of nutrients helps sustain primary production and affects food-web structure; these effects in turn influence the chemical properties of marine atmosphere. From an atmospheric chemistry standpoint, sea-salt aerosols produced by strong winds and marine biogenic gases emitted from highly productive waters affect the physicochemical characteristics of marine aerosols. As phytoplankton populations are patchy and atmospheric processes sporadic, the interactions between atmospheric chemical constituents and marine biota vary for different regions as well as seasonally and over longer timescales. To address these and other emerging issues, and more generally to better understand the important biogeochemical processes and interactions occurring over the open oceans, more long-term recurrent research cruises with standardized atmospheric shipboard measurements will be needed in the future.

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

DeMott, PJ; Suski, KJ; Hill, TCJ

The first ever ice nucleating particle (INP) measurements to be collected at the Southern Great Plains site were made during a period from late April to June 2014, as a trial for possible longer-term measurements at the site. These measurements will also be used to lay the foundation for understanding and parameterizing (for cloud resolving modeling) the sources of these climatically important aerosols as well as to augment the existing database containing this knowledge. Siting the measurements during the spring was intended to capture INP sources in or to this region from plant, soil, dust transported over long distances, biomassmore » burning, and pollution aerosols at a time when they may influence warm-season convective clouds and precipitation. Data have been archived of real-time measurements of INP number concentrations as a function of processing conditions (temperature and relative humidity) during 18 days of sampling that spanned two distinctly different weather situations: a warm, dry and windy period with regional dust and biomass burning influences in early May, and a cooler period of frequent precipitation during early June. Precipitation delayed winter wheat harvesting, preventing intended sampling during that perturbation on atmospheric aerosols. INP concentrations were highest and most variable at all temperatures in the dry period, where we attribute the INP activity primarily to soil dust emissions. Additional offline INP analyses are underway to extend the characterization of INP to cover the entire mixed phase cloud regime from -5°C to -35°C during the full study. Initial comparisons between methods on four days show good agreement and excellent future promise. The additional offline immersion freezing data will be archived as soon as completed under separate funding. Analyses of additional specialized studies for specific attribution of INP to biological and smoke sources are continuing via the National Science Foundation and National Aeronautics and Space Administration funding that helped support instrumentation used for the measurements described herein. Aerosol Observing System aerosol data will be vital to the interpretation and parameterization of results as part of analyses for publications in preparation.« less

Source apportionment of airborne particulate matter using organic compounds as tracers

NASA Astrophysics Data System (ADS)

Schauer, James J.; Rogge, Wolfgang F.; Hildemann, Lynn M.; Mazurek, Monica A.; Cass, Glen R.; Simoneit, Bernd R. T.

A chemical mass balance receptor model based on organic compounds has been developed that relates sours; contributions to airborne fine particle mass concentrations. Source contributions to the concentrations of specific organic compounds are revealed as well. The model is applied to four air quality monitoring sites in southern California using atmospheric organic compound concentration data and source test data collected specifically for the purpose of testing this model. The contributions of up to nine primary particle source types can be separately identified in ambient samples based on this method, and approximately 85% of the organic fine aerosol is assigned to primary sources on an annual average basis. The model provides information on source contributions to fine mass concentrations, fine organic aerosol concentrations and individual organic compound concentrations. The largest primary source contributors to fine particle mass concentrations in Los Angeles are found to include diesel engine exhaust, paved road dust, gasoline-powered vehicle exhaust, plus emissions from food cooking and wood smoke, with smaller contribution:; from tire dust, plant fragments, natural gas combustion aerosol, and cigarette smoke. Once these primary aerosol source contributions are added to the secondary sulfates, nitrates and organics present, virtually all of the annual average fine particle mass at Los Angeles area monitoring sites can be assigned to its source.

Numerical simulations of Asian dust storms using a coupled climate-aerosol microphysical model

NASA Astrophysics Data System (ADS)

Su, Lin; Toon, Owen B.

2009-07-01

We have developed a three-dimensional coupled microphysical/climate model based on the National Center for Atmospheric Research Community Atmospheres Model and the University of Colorado/NASA Community Aerosol and Radiation Model for Atmospheres. We have used the model to investigate the sources, removal processes, transport, and optical properties of Asian dust aerosol and its impact on downwind regions. The model simulations are conducted primarily during the time frame of the Aerosol Characterization Experiment-Asia field experiment (March-May 2001) since considerable in situ data are available at that time. Our dust source function follows Ginoux et al. (2001). We modified the dust source function by using the friction velocity instead of the 10-m wind based on wind erosion theory, by adding a size-dependent threshold friction velocity following Marticorena and Bergametti (1995) and by adding a soil moisture correction. A Weibull distribution is implemented to estimate the subgrid-scale wind speed variability. We use eight size bins for mineral dust ranging from 0.1 to 10 μm radius. Generally, the model reproduced the aerosol optical depth retrieved by the ground-based Aerosol Robotic Network (AERONET) Sun photometers at six study sites ranging in location from near the Asian dust sources to the Eastern Pacific region. By constraining the dust complex refractive index from AERONET retrievals near the dust source, we also find the single-scattering albedo to be consistent with AERONET retrievals. However, large regional variations are observed due to local pollution. The timing of dust events is comparable to the National Institute for Environmental Studies (NIES) lidar data in Beijing and Nagasaki. However, the simulated dust aerosols are at higher altitudes than those observed by the NIES lidar.

Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

NASA Astrophysics Data System (ADS)

Zhang, Yan-Lin; El-Haddad, Imad; Huang, Ru-Jin; Ho, Kin-Fai; Cao, Jun-Ji; Han, Yongming; Zotter, Peter; Bozzetti, Carlo; Daellenbach, Kaspar R.; Slowik, Jay G.; Salazar, Gary; Prévôt, André S. H.; Szidat, Sönke

2018-03-01

Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32-47 % of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 %) and Xi'an (26 ± 9 %). The most important primary sources were biomass burning emissions, contributing 17-26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban and background regions in Asia, Europe and the USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 %) to WSOC aerosols in the Northern Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the eastern Asian pollution outflow, especially during winter, due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX

NASA Astrophysics Data System (ADS)

Brown, S. S.; Dubé, W. P.; Bahreini, R.; Middlebrook, A. M.; Brock, C. A.; Warneke, C.; de Gouw, J. A.; Washenfelder, R. A.; Atlas, E.; Peischl, J.; Ryerson, T. B.; Holloway, J. S.; Schwarz, J. P.; Spackman, R.; Trainer, M.; Parrish, D. D.; Fehshenfeld, F. C.; Ravishankara, A. R.

2013-11-01

Organic compounds are a large component of aerosol mass, but organic aerosol (OA) sources remain poorly characterized. Recent model studies have suggested nighttime oxidation of biogenic hydrocarbons as a potentially large OA source, but analysis of field measurements to test these predictions is sparse. We present nighttime vertical profiles of nitrogen oxides, ozone, VOCs and aerosol composition measured during low approaches of the NOAA P-3 aircraft to airfields in Houston, TX. This region has large emissions of both biogenic hydrocarbons and nitrogen oxides. The latter category serves as a source of the nitrate radical, NO3, a key nighttime oxidant. Biogenic VOCs (BVOC) and urban pollutants were concentrated within the nocturnal boundary layer (NBL), which varied in depth from 100-400 m. Despite concentrated NOx at low altitude, ozone was never titrated to zero, resulting in rapid NO3 radical production rates of 0.2-2.7 ppbv h-1 within the NBL. Monoterpenes and isoprene were frequently present within the NBL and underwent rapid oxidation (up to 1 ppbv h-1), mainly by NO3 and to a lesser extent O3. Concurrent enhancement in organic and nitrate aerosol on several profiles was consistent with primary emissions and with secondary production from nighttime BVOC oxidation, with the latter equivalent to or slightly larger than the former. Some profiles may have been influenced by biomass burning sources as well, making quantitative attribution of organic aerosol sources difficult. Ratios of organic aerosol to CO within the NBL ranged from 14 to 38 μg m-3 OA/ppmv CO. A box model simulation incorporating monoterpene emissions, oxidant formation rates and monoterpene SOA yields suggested overnight OA production of 0.5 to 9 μg m-3.

Source apportionment revisited for long-term measurements of fine aerosol trace elements at two locations in southern Norway

NASA Astrophysics Data System (ADS)

Maenhaut, Willy

2018-02-01

Five-year-long (1991-1996) aerosol trace element data sets for the fine (PM2) size fraction from the sites of Birkenes and Skreådalen in southern Norway were reanalysed by US EPA positive matrix factorization PMF5 in order to assess the sources and their contribution to the PM2 aerosol. The data sets contained the concentrations of the particulate mass (PM), black carbon (BC) and 21 elements in over 700 samples for each of the two sites. The PM was obtained from weighing with a microbalance and BC was determined with a light reflectance technique. The data for the elements were obtained by a combination of particle-induced X-ray emission and instrumental neutron activation analysis. Eight source factors were retained for each site, i.e., (i) secondary sulfate, which accounted for around 40% of the average measured PM2 mass, (ii) wood burning, with BC, K, Zn and As, which accounted for about 17%, (iii) an iodine factor (with also Br and Se), which is probably related to a marine biogenic source and was responsible for about 6.5%, (iv) aged sea salt with Na, Mg, Cl and Ca, but heavily depleted in Cl; (v) a crustal factor containing Al, Si, Ca, Ti and Fe; (vi) a heavy oil burning factor with V and Ni in a ratio of 3-4; (vii) a general pollution factor (with Cu, Zn, As, Se, Sb and Pb), and (viii) an almost pure manganese factor, which is attributed to Mn and FeMn industries in southern Norway. The results were substantially different from those of an earlier PMF analysis, in which use was made of PMF2.

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

NASA Astrophysics Data System (ADS)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilde, S.; Zhang, Y.; Dall'Osto, M.

2014-04-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), only partly internally mixed with secondary semivolatile compounds such as ammonium nitrate and amines. Other organic components originating from anthropogenic sources at night include monocarboxylic acids which correspond to an AMS factor analogous to the "cooking" organic aerosol (COA) already identified in urban areas. In daytime, enhanced mixing in the planetary boundary layer (PBL) along with increasing temperature determined dramatic changes in aerosol composition caused by the evaporation of semivolatile components and by the entrainment of aged aerosols transported downwards from residual layers. In other words, the entrainment of aged air masses is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOAs) and also for the recycling of primary species such as black carbon. The LV-OOA concentrations were shown to correlate to the simple meteorological tracers of humid PBL air produced by daytime convection over land areas. In particular, both PMF-AMS and PMF-NMR could resolve two components of LV-OOA: one from long-range transport from Central Europe, the second from recirculated PBL air from the Po Valley. According to organic aerosol source apportionment by PMF-AMS, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in North Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. Overall, the deployment of six state-of-the-art spectrometric techniques provided a comprehensive picture of the nature and source contributions of aerosols and aerosol precursors at a European rural site with unprecedented level of details.

Aerosol composition and sources in the central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Leck, C.; Graus, M.; Müller, M.; Paatero, J.; Burkhart, J. F.; Stohl, A.; Orr, L. H.; Hayden, K.; Li, S.-M.; Hansel, A.; Tjernström, M.; Leaitch, W. R.; Abbatt, J. P. D.

2011-10-01

Measurements of submicron aerosol chemical composition were made over the central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.051 and 0.055 μ g m-3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33% and 36% of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47% of the sulphate apportioned to marine biogenic sources and 48% to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it had a longer photochemical lifetime than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources. In particular, given that the factor does not correlate with common tracers of continental influence, we cannot rule out that the organic factor arises from a primary marine source.

Optical properties and vertical distribution of pollution aerosols in the Mediterranean basin in summertime: airborne observations from the Charmex SOP0, SOP1, and SOP2 campaigns

NASA Astrophysics Data System (ADS)

Di Biagio, Claudia; Beekmann, Matthias; Chevallier, Servanne; Denjean, Cyrielle; Doppler, Lionel; Gaimoz, Cecile; Grand, Noel; Loisil, Rodrigue; Mallet, Marc; Pelon, Jacques; Ravetta, Francois; Sartelet, Karine; Schnitt, Sabrina; Triquet, Sylvain; Zapf, Pascal; Formenti, Paola

2014-05-01

The Mediterranean basin is a very complex area where high concentrations of atmospheric aerosols of different origin and types may be found. The North-Western part of the Mediterranean basin, due to its closeness with high polluted industrialized areas and coastal high populated cities, is frequently affected by severe pollution episodes. The strength of these episodes is particularly intense during summer when stable meteorological conditions favour the accumulation of pollutants in the lowermost atmospheric layers. Three intensive airborne campaigns (TRAQA, TRansport and Air QuAlity, June-July 2012), ADRIMED (Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region, June 2013) and SAFMED (Secondary Aerosol Formation in the MEDiterranean, July 2013) have been conducted over the North-Western and Central Mediterranean basin with the SAFIRE ATR-42 aircraft in the framework of the ChArMex Special Observing Periods 0 and 1. During the different campaigns the ATR-42 was equipped with a large set of instruments for the measurements of the aerosol physico-chemical (GRIMM, SMPS, PCASP, USHAS, FSSP for size distribution, and three lines for filter sampling on polycarbonate and quartz membranes in order to derive the bulk aerosol composition) and optical properties (TSI nephelometer, Magee Sci. aethalomether, and CAPS for scattering, absorption, and extinction coefficients at several wavelengths in the visible). Lidar backscatter profiles at 355, 532, and 1064 nm, meteorological parameters, upward and downward shortwave and longwave radiative fluxes, and atmospheric composition (H2O, CO2, CO, and O3) were also measured from aircraft instrumentation. In this work we present data on the aerosol physico-chemical and optical properties obtained during the 25 scientific flights of TRAQA, ADRIMED, and SAFMED performed in correspondence of pollution episodes. During the campaigns the Western Mediterranean basin was interested by different synoptic conditions which lead to the export of anthropogenic plumes from different polluted source regions (northern Italy and the Po Valley, Marseille and the Fos/Berre region, and Barcelona). The differences in terms of physico-chemical and optical properties for the different cases will be investigated and the variability of optical properties will be discussed in term of aerosol origin and airmass history.

In-situ droplet monitoring for self-tuning spectrometers

DOEpatents

Montaser, Akbar; Jorabchi, Kaveh; Kahen, Kaveh

2010-09-28

A laser scattering based imaging technique is utilized in order to visualize the aerosol droplets in an inductively coupled plasma (ICP) torch from an aerosol source to the site of analytical measurements. The resulting snapshots provide key information about the spatial distribution of the aerosol introduced by direct and indirect injection devices: 1) a direct injection high efficiency nebulizer (DIHEN); 2) a large-bore DIHEN (LB-DIHEN); and 3) a PFA microflow nebulizer with a PFA Scott-type spray chamber. Moreover, particle image velocimetry (PIV) is used to study the in-situ behavior of the aerosol before interaction with, for example, plasma, while the individual surviving droplets are explored by particle tracking velocimetry (PTV). Further, the velocity distribution of the surviving droplets demonstrates the importance of the initial droplet velocities in complete desolvation of the aerosol for optimum analytical performance in ICP spectrometries. These new observations are important in the design of the next-generation direct injection devices for lower sample consumption, higher sensitivity, lower noise levels, suppressed matrix effects, and for developing smart spectrometers. For example, a controller can be provided to control the output of the aerosol source by controlling the configuration of the source or the gas flow rate via feedback information concerning the aerosol.

Effects of Aircraft On Aerosol Abundance in the Upper Troposphere

NASA Technical Reports Server (NTRS)

Ferry, G. V.; Pueschel, R. F.; Strawa, A. W.; Howard, S. D.; Verma, S.; Mahoney, M. J.; Bui, T. P.; Hannan, J. R.; Fuelberg, H. E.; Condon, Estelle P. (Technical Monitor)

1999-01-01

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon on October 23, 1997. The source of this aerosol is ascribed to commercial aircraft operations in flight corridors above 10 km, because (1) a stable atmosphere prevented vertical air mass exchanges and thus eliminated surface sources, (2) air mass back trajectories documented the absence of remote continental sources, and (3) temperature profiler data showed the tropopause at least one kilometers above flight altitude throughout the flight. Particle volatility identified 70% H2SO4, 20% (NH4)2SO4 and 10% nonvolatile aerosol in the proximity of flight corridors, and (10-30)% H2SO4, up to 50% (NH4)2SO4, and (40-60)% nonvolatile aerosols in air that was not affected by aircraft operations below 10 km. Only a very small fraction of the nonvolatile particles (determined with a condensation nucleus counter) could be morphologically identified as soot aerosol (validated by scanning electron microscopy of wire impactor samples). The newly formed H2SO4 particles did not measurably affect surface area and volume of the background aerosol due to their small size, hence did not affect radiative transfer directly.

New Measurements of Aerosol Vertical Structure from Space Using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

NASA Technical Reports Server (NTRS)

Welton, Ellsworth J.; Ginoux, Paul; Colarco, Peter; Chin, Mian; Spinhirne, James D.; Palm, Steven P.; Hlavka, Dennis; Hart, William

2003-01-01

In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GUS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output,

New Measurements of Aerosol Vertical Structure from Space using the NASA Geoscience Laser Altimeter System (GLAS): Applications for Aerosol Transport Models

NASA Technical Reports Server (NTRS)

Welton, E. J.; Spinhime, J.; Palm, S.; Hlavka, D.; Hart, W.; Ginoux, P.; Chin, M.; Colarco, P.

2004-01-01

In the past, satellite measurements of aerosols have only been possible using passive sensors. Analysis of passive satellite data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth,s climate. However, direct measurement of aerosol vertical distribution has not been possible using only the passive data. Knowledge of aerosol vertical distribution is important to correctly assess the impact of aerosol absorption, for certain atmospheric correction procedures, and to help constrain height profiles in aerosol transport models. On January 12,2003 NASA launched the first satellite-based lidar, the Geoscience Laser Altimeter System (GLAS), onboard the ICESat spacecraft. GLAS is both an altimeter and an atmospheric lidar, and obtains direct measurements of aerosol and cloud heights. Here we show an overview of GLAS, provide an update of its current status, and discuss how GLAS data will be useful for modeling efforts. In particular, a strategy of using GLAS to characterize the height profile of dust plumes over source regions will be presented, along with initial results. Such information can be used to validate and improve output from aerosol transport models. Aerosol height profile comparisons between GLAS and transport models will be shown for regions downwind of aerosol sources. We will also discuss the feasibility of assimilating GLAS profiles into the models in order to improve their output.

Evolution of aerosol vertical distribution during particulate pollution events in Shanghai

NASA Astrophysics Data System (ADS)

Zhang, Yunwei; Zhang, Qun; Leng, Chunpeng; Zhang, Deqin; Cheng, Tiantao; Tao, Jun; Zhang, Renjian; He, Qianshan

2015-06-01

A set of micro pulse lidar (MPL) systems operating at 532 nm was used for ground-based observation of aerosols in Shanghai in 2011. Three typical particulate pollution events (e.g., haze) were examined to determine the evolution of aerosol vertical distribution and the planetary boundary layer (PBL) during these pollution episodes. The aerosol vertical extinction coefficient (VEC) at any given measured altitude was prominently larger during haze periods than that before or after the associated event. Aerosols originating from various source regions exerted forcing to some extent on aerosol loading and vertical layering, leading to different aerosol vertical distribution structures. Aerosol VECs were always maximized near the surface owing to the potential influence of local pollutant emissions. Several peaks in aerosol VECs were found at altitudes above 1 km during the dust- and bioburning-influenced haze events. Aerosol VECs decreased with increasing altitude during the local-polluted haze event, with a single maximum in the surface atmosphere. PM2.5 increased slowly while PBL and visibility decreased gradually in the early stages of haze events; subsequently, PM2.5 accumulated and was exacerbated until serious pollution bursts occurred in the middle and later stages. The results reveal that aerosols from different sources impact aerosol vertical distributions in the atmosphere and that the relationship between PBL and pollutant loadings may play an important role in the formation of pollution.

Chemical characteristics of soluble aerosols over the central Himalayas: insights into spatiotemporal variations and sources.

PubMed

Tripathee, Lekhendra; Kang, Shichang; Rupakheti, Dipesh; Cong, Zhiyuan; Zhang, Qianggong; Huang, Jie

2017-11-01

In order to investigate the spatial and temporal variations of aerosols and its soluble chemical compositions of the data gap zone in the central Himalayan region, aerosol samples were collected at four sites. The sampling location were characterized by four different categories, such as urban (Bode), semi-urban site in the northern Indo-Gangetic Plain (Lumbini), rural (Dhunche), and semiarid rural (Jomsom). A total of 230 aerosol samples were collected from four representative sites for a yearlong period and analyzed for water-soluble inorganic ions (WSIIs). The annual average aerosol mass concentration followed the sequence as Bode (238.24 ± 162.24 μg/m 3 )> Lumbini (161.14 ± 105.95 μg/m 3 )> Dhunche (112.40 ± 40.30 μg/m 3 )> Jomsom (78.85 ± 34.28 μg/m 3 ), suggesting heavier particulate pollution in the urban and semi-urban sites. The total soluble ions contributed to 12.61-28.19% of TSP aerosol mass. The results revealed that SO 4 2- and NO 3 - were the major anion and Ca 2+ and NH 4 + were the major cation influencing the aerosol composition over the central Himalayas. Calcium played a major role in neutralizing aerosol acidity followed by NH 4 + at all the sites. The major compound of aerosol was (NH 4 ) 2 SO 4 and NH 4 HSO 4 in the central Himalayas. Clear seasonality was observed at three observation sites, with higher concentrations during non-monsoon (dry periods) and lower during monsoon (wet period), suggesting washing out of aerosol particles by heavy precipitation during monsoon. In contrast, semiarid sites did not show the clear seasonal trend due to limited precipitation. Stationary sources were predominant over the mobile sources mostly in the remote sites. Principal component analysis confirmed that the major sources of WSIIs in the region were industrial emissions, fossil fuel and biomass burning, and crustal fugitive dusts. Nevertheless, transboundary aerosol transport over the region from polluted cities from south Asia could not be ignored as indicated by the clusters of air mass backward trajectory analysis.

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 increase in the modal diameter of the size distribution during foggy episodes and growth in the diameter of the particles upon the fog evaporation.

Aerosol composition and sources in the Central Arctic Ocean during ASCOS

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Leck, C.; Graus, M.; Müller, M.; Paatero, J.; Burkhart, J. F.; Stohl, A.; Orr, L. H.; Hayden, K.; Li, S.-M.; Hansel, A.; Tjernström, M.; Leaitch, W. R.; Abbatt, J. P. D.

2011-05-01

Measurements of submicron aerosol chemical composition were made in the Central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.042 and 0.046 μg m-3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33 % and 36 % of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47 % of the sulphate apportioned to marine biogenic sources and 48 % to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it was more processed and had been present longer in the atmosphere than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources.

ORGANIC MOLECULAR MARKER ANALYSIS OF LOW VOLUME RESIDENTIAL SAMPLES FOR SOURCE APPORTIONMENT IN THE DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY

EPA Science Inventory

This abstract describes a poster on results for organic speciation analysis for Detroit Exposure and Aerosol Research Study (DEARS) to be presented at the 2006 International Aerosol Conference sponsored by the American Association for Aerosol Research in St. Paul, Minnesota on Se...

Aerosol Vacuum-Assisted Plasma Ionization (Aero-VaPI) Coupled to Ion Mobility-Mass Spectrometry

NASA Astrophysics Data System (ADS)

Blair, Sandra L.; Ng, Nga L.; Zambrzycki, Stephen C.; Li, Anyin; Fernández, Facundo M.

2018-02-01

In this communication, we report on the real-time analysis of organic aerosol particles by Vacuum-assisted Plasma Ionization-Mass Spectrometry (Aero-VaPI-MS) using a home-built VaPI ion source coupled to a Synapt G2-S HDMS ion mobility-mass spectrometry (IM-MS) system. Standards of organic molecules of interest in prebiotic chemistry were used to generate aerosols. Monocaprin and decanoic acid aerosol particles were successfully detected in both the positive and negative ion modes, respectively. A complex aerosol mixture of different sizes of polymers of L-malic acid was also examined through ion mobility (IM) separations, resulting in the detection of polymers of up to eight monomeric units. This noncommercial plasma ion source is proposed as a low cost alternative to other plasma ionization platforms used for aerosol analysis, and a higher-performance alternative to more traditional aerosol mass spectrometers. VaPI provides robust online ionization of organics in aerosols without extensive ion activation, with the coupling to IM-MS providing higher peak capacity and excellent mass accuracy. [Figure not available: see fulltext.

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Long term aerosol and trace gas measurements in Central Amazonia

NASA Astrophysics Data System (ADS)

Artaxo, Paulo; Barbosa, Henrique M. J.; Ferreira de Brito, Joel; Carbone, Samara; Rizzo, Luciana V.; Andreae, Meinrat O.; Martin, Scot T.

2016-04-01

The central region of the Amazonian forest is a pristine region in terms of aerosol and trace gases concentrations. In the wet season, Amazonia is actually one of the cleanest continental region we can observe on Earth. A long term observational program started 20 years ago, and show important features of this pristine region. Several sites were used, between then ATTO (Amazon Tall Tower Observatory) and ZF2 ecological research site, both 70-150 Km North of Manaus, receiving air masses that traveled over 1500 km of pristine tropical forests. The sites are GAW regional monitoring stations. Aerosol chemical composition (OC/EC and trace elements) is being analysed using filters for fine (PM2.5) and coarse mode aerosol as well as Aerodyne ACSM (Aerosol Chemical Speciation Monitors). VOCs are measured using PTR-MS, while CO, O3 and CO2 are routinely measured. Aerosol absorption is being studied with AE33 aethalometers and MAAP (Multi Angle Absorption Photometers). Aerosol light scattering are being measured at several wavelengths using TSI and Ecotech nephelometers. Aerosol size distribution is determined using scanning mobility particle sizer at each site. Lidars measure the aerosol column up to 12 Km providing the vertical profile of aerosol extinction. The aerosol column is measures using AERONET sun photometers. In the wet season, organic aerosol comprises 75-85% of fine aerosol, and sulfate and nitrate concentrations are very low (1-3 percent). Aerosols are dominated by biogenic primary particles as well as SOA from biogenic precursors. Black carbon in the wet season accounts for 5-9% of fine mode aerosol. Ozone in the wet season peaks at 10-12 ppb at the middle of the day, while carbon monoxide averages at 50-80 ppb. Aerosol optical thickness (AOT) is a low 0.05 to 0.1 at 550 nm in the wet season. Sahara dust transport events sporadically enhance the concentration of soil dust aerosols and black carbon. In the dry season (August-December), long range transported biomass burning alters atmospheric composition very significantly. AOT can reach values as high as 2-3 at 550 nm, and concentrations of aerosol species and trace gases are strongly enriched.

Eddy covariance measurements of sea spray particles over the Atlantic Ocean

NASA Astrophysics Data System (ADS)

Norris, S.; Brooks, I.; de Leeuw, G.; Smith, M. H.; Moeman, M.; Lingard, J.

2007-09-01

Most estimates of sea spray aerosol source functions have used indirect means to infer the rate of production as a function of wind speed. Only recently has the technology become available to make high frequency measurements of aerosol concentration suitable for direct eddy correlation determination of the particle flux. This was accomplished in this study by combining a newly developed fast aerosol particle counter with an ultrasonic anemometer which allowed for eddy covariance measurements of size-segregated particle fluxes. The aerosol instrument is the Compact Lightweight Aerosol Spectrometer Probe (CLASP) - capable of measuring 8-channel size spectra for mean radii between 0.15 and 0.35 μm at 10 Hz. The first successful measurements were made during the WASFAB (Waves, Air Sea Fluxes, Aerosol and Bubbles) field campaign in October 2005 in Duck (NC, USA). The method and results are presented and comparisons are made with recent sea spray source functions from the literature.

The Remote Sensing of Mineral Aerosols and their Impact on Phytoplankton Productivity

NASA Technical Reports Server (NTRS)

Tindale, Neil W.

1997-01-01

The overall objective of this experiment was to test the iron hypothesis does the addition of iron to nutrient rich surface waters enhance productivity? Our specific objectives in this experiment included sampling and studying the marine aerosol size and type (which are related to chemical reactivity) during the PlumEx cruise to determine the importance of local (Galapagos Islands) versus long-range sources of atmospheric material. Detailed results of single particle analysis of our samples are being prepared for publication in two papers. We collect aerosol samples and they have been analyzed for trace metals and other elements. We are mapped aerosol distribution and the desert source areas around the Arabian Sea region. We did record a clear relationship between the aerosol radiance and synoptic weather patterns with distinct signals over the ocean northwest and southwest of Australia. While the interpretation was limited an aerosol climatology pattern was presented.

Chemical Composition and Oxidation State of Iron-Containing Aerosol Particles Over West Antarctic Peninsula

NASA Astrophysics Data System (ADS)

Fan, S.; Yu, S.; Lai, B.; Gao, Y.

2017-12-01

Iron is a limiting micronutrient element critical for the marine ecosystem. In the extensive high-nutrient low-chlorophyll (HNLC) regions of the Southern Ocean, the activities of phytoplankton are partly controlled by iron (Fe) from different sources, including atmospheric deposition. Among important properties of atmospheric Fe are the elemental composition and Fe oxidation state of Fe-containing aerosol particles, as these properties affect aerosol Fe solubility. To explore these issues, aerosol samples were collected at Palmer Station in West Antarctic Peninsula. Samples were analyzed by submicron synchrotron-based X-ray fluorescence (XRF) and X-ray absorption near edge structure (XANES) spectroscopy for the Fe oxidation state and elemental composition of aerosol particles. The morphological information of aerosol particles was also observed by the high-resolution fluorescence microscopy, revealing possible sources and formation processes of iron-containing particles. More detailed results will be discussed in this presentation.

Radiocarbon-based Source Apportionment of Organic, Elemental and Water-soluble Organic Carbon Aerosols and the Light Absorption of Water-soluble Organic Carbon Aerosols in the East Asia High-intensity Winter Campaigns in 2014

NASA Astrophysics Data System (ADS)

Fang, W.; Andersson, A.; Zheng, M.; Lee, M.; Kim, S. W.; Du, K.; Gustafsson, O.

2016-12-01

Improved understanding of anthropogenic aerosol effects on atmospheric chemistry and climate as well as efficient mitigation actions are hampered by the limited comprehension of the relative contributions of different sources of carbonaceous aerosols and of their subsequent atmospheric processing. Here, we present dual carbon isotope constrained source apportionment and optical properties of carbonaceous aerosols simultaneously both at urban and rural receptor sites, includes North China Plain (NCP, Beijing and Tianjin), Yangtze River Delta (YRD, Shanghai, Zhejiang), and Jeju Island (Korea Climate Observatory at Gosan) during January 2014 field campaigns. The radiocarbon (Δ14C) data show that fossil combustions contribute equally ˜80 ± 5% to elemental carbon (EC) aerosol in Beijing, Tianjin, and Shanghai, and 66 ± 9% to Gosan-EC aerosol, while the specific sources of the dominant fossil fuel component were dramatically different among these sites. The mean fraction coal combustion of Beijing-EC, Tianjin-EC, and Gosan-EC is double that of Shanghai-EC. The other large fraction (72―92%) of carbonaceous aerosol is organic carbon (OC) aerosol which contains water soluble and water insoluble organic carbon (WSOC and WISOC). OC, WISOC, and WSOC in Beijing and Gosan sites were still observed largely from fossil sources (53―75%). The more 13C-enriched signature of Gosan-WSOC (-22.8 ± 0.2‰) compared to Gosan-EC (-23.9 ± 0.4‰) and Beijing-WSOC (-23.5 ± 0.7‰) reflects that WSOC is likely more affected by atmospheric aging during long-rang transport than is EC. The high light absorption coefficients of PM2.5, PM1, and TSP were observed at Gosan during this study and was frequently reaching 20―60 Mm-1 by aethalometer and continuous light absorption photometer. The mass absorption cross section of WSOC (MAC365) for above sites is high (1.5 ± 0.8 m2/g), accounted for ˜14 ± 5% of the total direct absorbance relative to EC, which is significantly higher than the previous findings in S. Asia, N. America, and Europe.

Measurements of Organic Composition of Aerosol and Rainwater Samples Using Offline Aerosol Mass Spectrometry

NASA Astrophysics Data System (ADS)

OBrien, R. E.; Ridley, K. J.; Canagaratna, M. R.; Croteau, P.; Budisulistiorini, S. H.; Cui, T.; Green, H. S.; Surratt, J. D.; Jayne, J. T.; Kroll, J. H.

2016-12-01

A thorough understanding of the sources, evolution, and budgets of atmospheric organic aerosol requires widespread measurements of the amount and chemical composition of atmospheric organic carbon in the condensed phase (within particles and water droplets). Collecting such datasets requires substantial spatial and temporal (long term) coverage, which can be challenging when relying on online measurements by state-of-the-art research-grade instrumentation (such as those used in atmospheric chemistry field studies). Instead, samples are routinely collected using relatively low-cost techniques, such as aerosol filters, for offline analysis of their chemical composition. However, measurements made by online and offline instruments can be fundamentally different, leading to disparities between data from field studies and those from more routine monitoring. To better connect these two approaches, and take advantage of the benefits of each, we have developed a method to introduce collected samples into online aerosol instruments using nebulization. Because nebulizers typically require tens to hundreds of milliliters of solution, limiting this technique to large samples, we developed a new, ultrasonic micro-nebulizer that requires only small volumes (tens of microliters) of sample for chemical analysis. The nebulized (resuspended) sample is then sent into a high-resolution Aerosol Mass Spectrometer (AMS), a widely-used instrument that provides key information on the chemical composition of aerosol particulate matter (elemental ratios, carbon oxidation state, etc.), measurements that are not typically made for collected atmospheric samples. Here, we compare AMS data collected using standard on-line techniques with our offline analysis, demonstrating the utility of this new technique to aerosol filter samples. We then apply this approach to organic aerosol filter samples collected in remote regions, as well as rainwater samples from across the US. This data provides information on the sample composition and changes in key chemical characteristics across locations and seasons.

Summer aerosol particle mixing in different climate and source regions of the United Arab Emirates (UAE)

NASA Astrophysics Data System (ADS)

Semeniuk, T. A.; Bruintjes, R. T.; Salazar, V.; Breed, D. W.; Jensen, T. L.; Buseck, P. R.

2005-12-01

The high aerosol loadings over the UAE reflect local to regional natural and anthropogenic pollution sources. To understand the impact of the high levels of pollution on both local and global climate systems, aerosol characterization flights in summer 2002 were used to sample major source areas, and to provide information on the interaction of aerosol particles within different geographic regions of the UAE. Atmospheric information and aerosol samples were collected from the marine/oil-industry region, NW coastal industries and cities, Oman Mountain Range, and NE coastal region. Aerosol samples were collected with multi-stage impactors and were analysed later using transmission electron microscopy. All samples are dominated by mineral grains or mineral aggregates in the coarse-mode fraction, and ammonium sulfate droplets in the fine-mode fraction. Differences in the types of mineral grains (different regional desert sources), inorganic salt and soot fractions, and types of internally mixed particles occur between regions. Oil-related industry sites have an abundance of coated and internally mixed particles, including sulfate-coated mineral grains, and mineral aggregates with chloride and sulfate. Cities have slightly elevated soot fractions, and typically have metal oxides. The NE coastal area is characterized by high soot fractions (local shipping) and mixed volatile droplets (regional Asian pollution). Particle populations within the convection zone over the Oman Mountain Range comprise an external mixture of particles from NW and NE sources, with many deliquesced particles. Both land-sea breezes in the NW regions and convection systems in the mountains mix aerosol particles from different local and regional sources, resulting in the formation of abundant internally mixed particles. The interaction between desert dust and anthropogenic pollution, and in particular the formation of mineral aggregates with chloride and sulfate, enhances the coarse-mode fraction and droplet fraction in industrial and mountainous regions.

Long-term visibility data in the UK - how does visibility vary with meteorological and pollutant parameters?

NASA Astrophysics Data System (ADS)

Singh, Ajit; Bloss, William J.; Pope, Francis D.

2016-04-01

Poor visibility can be an indicator of poor air quality. Moreover, degradation in visibility can be hazardous to human safety; for example, low visibility can lead to accidents particularly during winter when fogs are prevalent. The present quantitative analysis attempts to explain the influence of aerosol concentration and composition, and meteorology on long-term UK visibility. We use visibility data from eight UK meteorological stations which have been running since the 1950s. The site locations include urban, rural and marine environments. Overall, most stations show a long term trend of visibility increase, which is indicative of reductions in aerosol pollution, especially in urban areas. Additionally, results at all sites show a very clear dependence on relative humidity, indicating the importance of aerosol hygroscopicity on the ability of aerosols to scatter radiation and hence impact upon visibility. The dependence of visibility on other meteorological parameters (e.g. relative humidity, air temperature, wind speed & direction) is also investigated. To explain the long term visibility trends and their dependence on meteorological conditions, a light extinction model was constructed incorporating the concentrations and composition of historic aerosol. The lack of historic aerosol size distributions and aerosol composition data, which determine hygroscopicity and refractive index, leads to an under-constrained model. Aerosol measurements from the last 10 years are used to constrain these model parameters, and hence their historical variation can be estimated; sensitivity analyses are used to estimate errors for the time period before regular aerosol measurements are available. A good agreement is observed between modelled and measured visibility. This work has generated a unique 60 year data set with which to understand how aerosol concentration and composition has varied over the UK. The model is applicable and easily transferrable to other data sets worldwide. Hence, different clean air legislation can be assessed for its effectiveness in reducing aerosol pollution. The implications for the UK will be discussed.

Sources and Variability of Aerosols and Aerosol-Cloud Interactions in the Arctic

NASA Astrophysics Data System (ADS)

Liu, H.; Zhang, B.; Taylor, P. C.; Moore, R.; Barahona, D.; Fairlie, T. D.; Chen, G.; Ham, S. H.; Kato, S.

2017-12-01

Arctic sea ice in recent decades has significantly declined. This requires understanding of the Arctic surface energy balance, of which clouds are a major driver. However, the mechanisms for the formation and evolution of clouds in the Arctic and the roles of aerosols therein are highly uncertain. Here we conduct data analysis and global model simulations to examine the sources and variability of aerosols and aerosol-cloud interactions in the Arctic. We use the MERRA-2 reanalysis data (2006-present) from the NASA Global Modeling and Assimilation Office (GMAO) to (1) quantify contributions of different aerosol types to the aerosol budget and aerosol optical depths in the Arctic, (2) ­examine aerosol distributions and variability and diagnose the major pathways for mid-latitude pollution transport to the Arctic, including their seasonal and interannual variability, and (3) characterize the distribution and variability of clouds (cloud optical depth, cloud fraction, cloud liquid and ice water path, cloud top height) in the Arctic. We compare MERRA-2 aerosol and cloud properties with those from C3M, a 3-D aerosol and cloud data product developed at NASA Langley Research Center and merged from multiple A-Train satellite (CERES, CloudSat, CALIPSO, and MODIS) observations. We also conduct perturbation experiments using the NASA GEOS-5 chemistry-climate model (with GOCART aerosol module coupled with two-moment cloud microphysics), and discuss the roles of various types of aerosols in the formation and evolution of clouds in the Arctic.

Influence of the Surf Zone on the Marine Aerosol Concentration in a Coastal Area

NASA Astrophysics Data System (ADS)

Tedeschi, Gilles; van Eijk, Alexander M. J.; Piazzola, Jacques; Kusmierczyk-Michulec, Jolanta T.

2017-01-01

Sea-salt aerosol concentrations in the coastal zone are assessed with the numerical aerosol-transport model MACMod that applies separate aerosol source functions for open ocean and the surf zone near the sea-land transition. Numerical simulations of the aerosol concentration as a function of offshore distance from the surf zone compare favourably with experimental data obtained during a surf-zone aerosol experiment in Duck, North Carolina in autumn 2007. Based on numerical simulations, the effect of variations in aerosol production (source strength) and transport conditions (wind speed, air-sea temperature difference), we show that the surf-zone aerosols are replaced by aerosols generated over the open ocean as the airmass advects out to sea. The contribution from the surf-generated aerosol is significant during high wind speeds and high wave events, and is significant up to 30 km away from the production zone. At low wind speeds, the oceanic component dominates, except within 1-5 km of the surf zone. Similar results are obtained for onshore flow, where no further sea-salt aerosol production occurs as the airmass advects out over land. The oceanic aerosols that are well-mixed throughout the boundary layer are then more efficiently transported inland than are the surf-generated aerosols, which are confined to the first few tens of metres above the surface, and are therefore also more susceptible to the type of surface (trees or grass) that determines the deposition velocity.

Ozone and haze pollution effects on the contemporary land carbon cycle

NASA Astrophysics Data System (ADS)

Unger, N.

2016-12-01

Atmospheric pollutants have both beneficial and detrimental effects on carbon uptake by land ecosystems. Surface ozone damages leaf photosynthesis by oxidizing plant cells, while aerosols promote carbon uptake by increasing diffuse radiation and exert additional influences through concomitant perturbations to meteorology and hydrology. Here, I present new results from three assessment studies that employ Earth system modeling and multiple measurement datasets. First, we quantify the separate and combined effects of anthropogenic ozone and aerosol pollution on the global land carbon uptake. Second, we evaluate benefits to land ecosystem health from selective emission reductions in specific pollution sources and sectors. Finally, I show that the long-term climatic effects of mid-latitude air pollution boosts plant productivity in the Amazon by 10% on the annual average today.

Size-resolved trace metal characterization of aerosols emitted by four important source types in Switzerland

NASA Astrophysics Data System (ADS)

Buerki, Peter R.; Gaelli, Brigitte C.; Nyffeler, Urs P.

In central Switzerland five types of emission sources are mainly responsible for airborne trace metals: traffic, industrial plants burning heavy oil, resuspension of soil particles, residential heatings and refuse incineration plants. The particulate emissions of each of these source types except refuse incineration were sampled using Berner impactors and the mass and elemental size distributions of Cd, Cu, Mn, Pb, Zn, As and Na determined. Cd, Na and Zn are not characteristic for any of these source types. As and Cu, occurring in the fine particle fractions are characteristic for heavy oil combustion, Mn for soil dust and sometimes for heavy and fuel oil combustion and Pb for traffic aerosols. The mass size distributions of aerosols originating from erosion and abrasion processes show a maximum mass fraction in the coarse particle range larger than about 1 μm aerodynamic equivalent diameters (A.E.D.). Aerosols originating from combustion processes show a second maximum mass fraction in the fine particle range below about 0.5μm A.E.D. Scanning electron microscopy combined with an EDS analyzer was used for the morphological characterization of emission and ambient aerosols.

Modeling the Current and Future Roles of Particulate Organic Nitrates in the Southeastern United States.

PubMed

Pye, Havala O T; Luecken, Deborah J; Xu, Lu; Boyd, Christopher M; Ng, Nga L; Baker, Kirk R; Ayres, Benjamin R; Bash, Jesse O; Baumann, Karsten; Carter, William P L; Edgerton, Eric; Fry, Juliane L; Hutzell, William T; Schwede, Donna B; Shepson, Paul B

2015-12-15

Organic nitrates are an important aerosol constituent in locations where biogenic hydrocarbon emissions mix with anthropogenic NOx sources. While regional and global chemical transport models may include a representation of organic aerosol from monoterpene reactions with nitrate radicals (the primary source of particle-phase organic nitrates in the Southeast United States), secondary organic aerosol (SOA) models can underestimate yields. Furthermore, SOA parametrizations do not explicitly take into account organic nitrate compounds produced in the gas phase. In this work, we developed a coupled gas and aerosol system to describe the formation and subsequent aerosol-phase partitioning of organic nitrates from isoprene and monoterpenes with a focus on the Southeast United States. The concentrations of organic aerosol and gas-phase organic nitrates were improved when particulate organic nitrates were assumed to undergo rapid (τ = 3 h) pseudohydrolysis resulting in nitric acid and nonvolatile secondary organic aerosol. In addition, up to 60% of less oxidized-oxygenated organic aerosol (LO-OOA) could be accounted for via organic nitrate mediated chemistry during the Southern Oxidants and Aerosol Study (SOAS). A 25% reduction in nitrogen oxide (NO + NO2) emissions was predicted to cause a 9% reduction in organic aerosol for June 2013 SOAS conditions at Centreville, Alabama.

Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo

PubMed Central

McCoy, Daniel T.; Burrows, Susannah M.; Wood, Robert; Grosvenor, Daniel P.; Elliott, Scott M.; Ma, Po-Lun; Rasch, Phillip J.; Hartmann, Dennis L.

2015-01-01

Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in Nd is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35o to 45oS) and by organic matter in sea spray aerosol at higher latitudes (45o to 55oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere. PMID:26601216

Natural aerosols explain seasonal and spatial patterns of Southern Ocean cloud albedo.

PubMed

McCoy, Daniel T; Burrows, Susannah M; Wood, Robert; Grosvenor, Daniel P; Elliott, Scott M; Ma, Po-Lun; Rasch, Phillip J; Hartmann, Dennis L

2015-07-01

Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties-ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration N d of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed N d. Enhanced N d is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in N d is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35(o) to 45(o)S) and by organic matter in sea spray aerosol at higher latitudes (45(o) to 55(o)S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m(-2) over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

simplified aerosol representations in global modeling

NASA Astrophysics Data System (ADS)

Kinne, Stefan; Peters, Karsten; Stevens, Bjorn; Rast, Sebastian; Schutgens, Nick; Stier, Philip

2015-04-01

The detailed treatment of aerosol in global modeling is complex and time-consuming. Thus simplified approaches are investigated, which prescribe 4D (space and time) distributions of aerosol optical properties and of aerosol microphysical properties. Aerosol optical properties are required to assess aerosol direct radiative effects and aerosol microphysical properties (in terms of their ability as aerosol nuclei to modify cloud droplet concentrations) are needed to address the indirect aerosol impact on cloud properties. Following the simplifying concept of the monthly gridded (1x1 lat/lon) aerosol climatology (MAC), new approaches are presented and evaluated against more detailed methods, including comparisons to detailed simulations with complex aerosol component modules.

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.

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

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

Liu, Zhen; Wang, Yuhang; Costabile, Francesa

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

Estimation of surface PM10 concentration in Seoul during the DRAGON-Asia campaign based on the physical relationship between AOD and PM

NASA Astrophysics Data System (ADS)

Seo, S.; Kim, J.; Lee, H.; Jeong, U.; Kim, W. V.; Holben, B. N.; Kim, S.

2013-12-01

Atmospheric aerosols are known to play a role in climate change while it also adverse effects on human health such as respiratory and cardiovascular diseases. Especially, in terms of air quality, many studies have been conducted to estimate surface-level particulate matter (PM) concentration by using the satellite measurements to overcome the spatial limitation of ground-based aerosol measurements. In this study, we investigate the relationship between the column aerosol optical depth (AOD) and the surface PM10 concentration using the aerosol measurements during the DRAGON (Distributed Regional Aerosol Gridded Observation Network) - Asia campaign took place in Seoul from March to May, 2012. Based on the physical relationship between AOD and PM concentration, we develop various empirical linear models and evaluate the performance of these models. The best correlation (r = 0.67) is shown when vertical and size distribution of aerosols are additionally considered by using the boundary layer height (BLH) from backscattered lidar signals and the effective radius provided in AERONET inversion products. Similarly, MODIS AOD divided by BLH shows the best correlation with hourly PM10 (r = 0.62). We also identify the variability of correlations between AOD and PM10 depending on the environment characteristics in a complex megacity, Seoul by using the aerosol optical properties measured at mesoscale-level at 10 AERONET sites during the DRAGON campaign. Both AERONET and MODIS show higher correlation in residential area than near source area. Finally, we investigate the seasonal effects on the performance of various empirical linear models and find important factors of each season in PM estimation.

MIPAS observations of volcanic sulfate aerosol and sulfur dioxide in the stratosphere

NASA Astrophysics Data System (ADS)

Günther, Annika; Höpfner, Michael; Sinnhuber, Björn-Martin; Griessbach, Sabine; Deshler, Terry; von Clarmann, Thomas; Stiller, Gabriele

2018-01-01

Volcanic eruptions can increase the stratospheric sulfur loading by orders of magnitude above the background level and are the most important source of variability in stratospheric sulfur. We present a set of vertical profiles of sulfate aerosol volume densities and derived liquid-phase H2SO4 (sulfuric acid) mole fractions for 2005-2012, retrieved from infrared limb emission measurements performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on board of the Environmental Satellite (Envisat). Relative to balloon-borne in situ measurements of aerosol at Laramie, Wyoming, the MIPAS aerosol data have a positive bias that has been corrected, based on the observed differences to the in situ data. We investigate the production of stratospheric sulfate aerosol from volcanically emitted SO2 for two case studies: the eruptions of Kasatochi in 2008 and Sarychev in 2009, which both occurred in the Northern Hemisphere midlatitudes during boreal summer. With the help of chemical transport model (CTM) simulations for the two volcanic eruptions we show that the MIPAS sulfate aerosol and SO2 data are qualitatively and quantitatively consistent with each other. Further, we demonstrate that the lifetime of SO2 is explained well by its oxidation by hydroxyl radicals (OH). While the sedimentation of sulfate aerosol plays a role, we find that the long-term decay of stratospheric sulfur after these volcanic eruptions in midlatitudes is mainly controlled by transport via the Brewer-Dobson circulation. Sulfur emitted by the two midlatitude volcanoes resides mostly north of 30° N at altitudes of ˜ 10-16 km, while at higher altitudes ( ˜ 18-22 km) part of the volcanic sulfur is transported towards the Equator where it is lifted into the stratospheric overworld and can further be transported into both hemispheres.

What We Can Say About the Roles of Natural and Anthropogenic Aerosols in Climate Change

NASA Astrophysics Data System (ADS)

Kahn, Ralph

2016-07-01

Although particles from natural sources dominate the globally averaged aerosol load, it is widely understood that human activity has added significantly to the atmospheric aerosol inventory in many regions. Anthropogenic contributions include pollution particles from industrial activity, transportation, cook-stoves, and other combustion sources, smoke from agricultural fires and those wildfires that result from land-management practices, soil and mineral dust mobilized in regions where overgrazing, severe tilling, or overuse of surface water resources have occurred, and biogenic particles from vegetation planted and maintained by the populance. The history of human influence is complex - in the 18th and 19th centuries agricultural burning tended to dominate the anthropogenic component in most places, whereas more recently, fossil fuel combustion leads the human contribution is many areas. However, identifying and quantifying the anthropogenic aerosol component on global scales is a challenging endeavor at present. Most estimates of the anthropogenic component come from aerosol transport models that are initialized with aerosol and precursor-gas source locations, emission strengths, and injection heights. The aerosol is then advected based on meteorological modeling, possibly modified chemically or physically, and removed by parameterized wet or dry deposition processes. Aerosol effects on clouds are also represented in some climate models, but with even greater uncertainty than the direct aerosol effects on Earth's radiation balance. Even for present conditions, aerosol source inventories are deduced from whatever constraints can be found, along with much creativity and many assumptions. Aerosol amount (i.e., aerosol optical depth) is routinely measured globally from space, but observational constraints on the anthropogenic component require some knowledge of the aerosol type as well, a much more difficult quantity to derive. As large-swath, multi-spectral, single-view instruments such as MODIS can provide some information about fine-mode vs. coarse-mode dominated aerosol over dark water, early efforts to constrain aerosol type assumed that some or all the fine-mode fraction is anthropogenic. However, this information is not sufficient to make the key anthropogenic vs. natural distinction in most places where the likely answer is not already known. Instruments providing more detailed measurements, such as multi-spectral, multi-angle and polarimetric imagers and multi-channel lidars, can offer tighter aerosol-type constraints in some circumstances, though generally not enough to specifically identify anthropogenic aerosols. The best we seem to be able to do with current data is to combine satellite and suborbital observations with models. And for the "pre-industrial" period, the analogy is usually made to the "natural" component of present-day aerosol, although there are ambiguities in our ability to distinguish natural from anthropogenic particles on regional-to-global scales, and the natural component itself might have changed over time. This talk will review where we stand, and what might be possible to say in the future.

Composition and oxidation state of sulfur in atmospheric particulate matter

NASA Astrophysics Data System (ADS)

Longo, Amelia F.; Vine, David J.; King, Laura E.; Oakes, Michelle; Weber, Rodney J.; Huey, Lewis Gregory; Russell, Armistead G.; Ingall, Ellery D.

2016-10-01

The chemical and physical speciation of atmospheric sulfur was investigated in ambient aerosol samples using a combination of sulfur near-edge x-ray fluorescence spectroscopy (S-NEXFS) and X-ray fluorescence (XRF) microscopy. These techniques were used to determine the composition and oxidation state of sulfur in common primary emission sources and ambient particulate matter collected from the greater Atlanta area. Ambient particulate matter samples contained two oxidation states: S0 and S+VI. Ninety-five percent of the individual aerosol particles (> 1 µm) analyzed contain S0. Linear combination fitting revealed that S+VI in ambient aerosol was dominated by ammonium sulfate as well as metal sulfates. The finding of metal sulfates provides further evidence for acidic reactions that solubilize metals, such as iron, during atmospheric transport. Emission sources, including biomass burning, coal fly ash, gasoline, diesel, volcanic ash, and aerosolized Atlanta soil, and the commercially available bacterium Bacillus subtilis, contained only S+VI. A commercially available Azotobacter vinelandii sample contained approximately equal proportions of S0 and S+VI. S0 in individual aerosol particles most likely originates from primary emission sources, such as aerosolized bacteria or incomplete combustion.

Aerosol studies during the ESCOMPTE experiment: an overview

NASA Astrophysics Data System (ADS)

Cachier, Hélène; Aulagnier, Fabien; Sarda, Roland; Gautier, François; Masclet, Pierre; Besombes, Jean-Luc; Marchand, Nicolas; Despiau, Serge; Croci, Delphine; Mallet, Marc; Laj, Paolo; Marinoni, Angela; Deveau, Pierre-Alexandre; Roger, Jean-Claude; Putaud, Jean-Philippe; Van Dingenen, Rita; Dell'Acqua, Alessandro; Viidanoja, Jyrkki; Martins-Dos Santos, Sebastiao; Liousse, Cathy; Cousin, Frédéric; Rosset, Robert; Gardrat, Eric; Galy-Lacaux, Corinne

2005-03-01

The "Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d'Emissions" (ESCOMPTE) experiment took place in the Southern part of France in the Marseilles/Fos-Berre region during 6 weeks in June and July 2001. One task was to document the regional sources of atmospheric particles and to gain some insight into the aerosol transformations in the atmosphere. For this purpose, seven sites were chosen and equipped with the same basic instrumentation to obtain the chemical closure of the bulk aerosol phase and size-segregated samples. Some specific additional experiments were conducted for the speciation of the organic matter and the aerosol size distribution in number. Finally, four multiwavelength sun-photometers were also deployed during the experiment. Interestingly, in this region, three intense aerosol sources (urban, industrial and biogenic) are very active, and data show consistent results, enlightening an important background of particles over the whole ESCOMPTE domain. Notable is the overwhelming importance of the carbonaceous fraction (comprising primary and secondary particles), which is always more abundant than sulphates. Particle size studies show that, on average, more than 90% of the mean regional aerosol number is found on a size range smaller than 300 nm in diameter. The most original result is the evidence of the rapid formation of secondary aerosols occurring in the whole ESCOMPTE domain. This formation is much more important than that usually observed at these latitudes since two thirds of the particulate mass collected off source zones is estimated to be generated during atmospheric transport. On the other hand, the marine source has poor influence in the region, especially during the overlapping pollution events of Intensive Observation Periods (IOP). Preliminary results from the 0D and 3D versions of the MesoNH-aerosol model show that, with optimised gas and particle sources, the model accounts satisfactorily for the measured aerosol concentrations. The formation of secondary particles in the model is currently underway; initial encouraging results show that the model accounts for the formation of secondary species, such as sulphate and organic particles. Finally, radiative calculations suggest that the role of the fine aerosol fraction is predominant mostly due to the presence of black carbon (BC) particles, which could induce a regional atmospheric heating.

Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

NASA Astrophysics Data System (ADS)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-08-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging processes were further illustrated in a case study of a severe haze episode. Our results elucidated a complex response of aerosol chemistry to emission controls, which has significant implications that emission controls over regional scales can substantially reduce secondary particulates. However, stricter emission controls for local source emissions are needed for further mitigating air pollution in the megacity of Beijing.

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Diehl, T. L.; Mian, Chin; Bond, T. C.; Carn, S. A.; Duncan, B. N.; Krotkov, N. A.; Streets, D. G.

2007-01-01

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthopogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ATSR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

Compilation of a Global Emission Inventory from 1980 to 2000 for Global Model Simulations of the Long-term Trend of Tropospheric Aerosols

NASA Technical Reports Server (NTRS)

Diehl, Thomas L.; Chin, Mian; Bond, Tami C.; Carn, SImon A.; Duncan, Bryan N.; Krotkov, Nickolay A.; Streets, David G.

2006-01-01

The approach to create a comprehensive emission inventory for the time period 1980 to 2000 is described in this paper. We have recently compiled an emission database, which we will use for a 21 year simulation of tropospheric aerosols with the GOCART model. Particular attention was paid to the time-dependent SO2, black carbon and organic carbon aerosol emissions. For the emission of SO2 from sporadically erupting volcanoes, we assembled emission data from the Global Volcanism Program of the Smithsonian Institution, using the VEI to derive the volcanic cloud height and the SO2 amount, and amended this dataset by the SO2 emission data from the TOMS instrument when available. 3-dimensional aircraft emission data was obtained for a number of years from the AEAP project, converted from burned fuel to SO2 and interpolated to each year, taking the sparsity of the flight patterns into account. Other anthropogenic SO2 emissions are based on gridded emissions from the EDGAR 2000 database (excluding sources from aircraft, biomass burning and international ship traffic), which were scaled to individual years with country/regional based emission inventories. Gridded SO2 emissions from international ship traffic for 2000 and the scaling factors for other years are from [Eyring et al., 2005]. We used gridded anthropogenic black and organic carbon emissions for 1996 [Bond et al., 2005], again excluding aircraft, biomass burning and ship sources. These emissions were scaled with regional based emission inventories from 1980 to 2000 to derive gridded emissions for each year. The biomass burning emissions are based on a climatology, which is scaled with regional scaling factors derived from the TOMS aerosol index and the AVHRR/ASTR fire counts to each year [Duncan et al., 2003]. Details on the integration of the information from the various sources will be provided and the distribution patterns and total emissions in the final product will be discussed.

Model of the dust-loaded ionospheres of Mars and Titan

NASA Astrophysics Data System (ADS)

Witasse, Olivier; Cardnell, Sandy; Molina-Cuberos, Gregorio; Michael, Mary; Tripathi, Sachi; Deprez, Gregoire; Montmessin, Franck; O'Brien, Keran

2016-10-01

The ionization of lower atmospheres of celestial bodies and the presence of charged species are fundamental in the understanding of atmospheric electricity phenomena, such as electric discharges, large scale electric currents and Schumann resonances. On January 14, 2005, the Huygens Probe measured the electric conductivity of Titan's atmosphere from 140 km down to the surface. Micro-ARES, the electric field and conductivity sensor on board the ExoMars 2016 Schiaparelli lander, will conduct the very first measurement and characterization of Martian atmospheric electricity. The landing is scheduled for October 19, 2016 and the measurements will be performed over 2-4 sols.The present photochemical model is developed to compute the concentration of the most abundant charged species (cluster-ions, electrons and charged aerosols) and electric conductivity in the lower atmospheres of Mars (0-70 km) and Titan (0-145 km). For both cases, the main source of ionization is galactic cosmic rays. In addition, during daytime, photoionization of aerosols due to solar UV radiation is important at Mars. Ion and electron attachment to aerosols is another major source of aerosol charging, which can vary between -50 and +200 elementary charges for Mars and -55 and -25 for Titan. The steady state concentration of charged species is computed by solving the respective balance equations, which include the source and sink terms of the photochemical reactions. Since the amount of suspended dust in the Martian atmosphere can vary considerably and it has an important effect on the atmospheric properties, several dust scenarios, in addition to the day-night variations, are considered to characterize the variability of the concentration of charged species.The agreement between with the results of the model for Titan and the Huygens data suggests an improvement with respect to previous models. This gives confidence in the results of the model for Mars, which characterize the predicted electric environment in which Micro-ARES will operate, being essential to its data analysis and interpretation.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-11-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play an important role in alleviating PM levels and achieving the "APEC blue" effect. The evolution of vertical differences between 260 m and the ground level was also investigated. Our results show complex vertical differences during the formation and evolution of severe haze episodes that are closely related to aerosol sources and boundary-layer dynamics.

Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

NASA Astrophysics Data System (ADS)

Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

2015-08-01

The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play an important role in alleviating PM levels and achieving the "APEC blue" effect. The evolution of vertical differences between 260 m and the ground level was also investigated. Our results show complex vertical differences during the formation and evolution of severe haze episodes that are closely related to aerosol sources and boundary layer dynamics.

Ambient Aerosols in the Southern Hemisphere on Ascension Island during the LASIC Campaign: Biomass Burning Season versus Near Pristine Background Conditions

NASA Astrophysics Data System (ADS)

Aiken, A. C.; Springston, S. R.; Watson, T. B.; Sedlacek, A. J., III; Zuidema, P.; Adebiyi, A. A.; Uin, J.; Kuang, C.; Flynn, C. J.

2017-12-01

Ascension Island is located 8 degrees South of the Equator and 15 degrees West Longitude in the middle of the South Atlantic Ocean, at least 1000 miles from any major shoreline and closest to the continent of Africa. While low Southern Hemisphere background aerosol and trace gas measurements are observed most of the year, that picture changes during the South African Biomass Burning (BB) season. BB emissions are a large source of carbon to the atmosphere via particles and gas phase species and with a potential rise in drought and extreme events in the future, these numbers are expected to increase. From approximately June-October every year, the plume of South African BB emissions, the largest BB source in the world, are advected West and are known to impact both the boundary layer and free troposphere at Ascension Island (Zuidema et al., 2016). During the U.S. DOE ARM field campaign, Layered Atlantic Smoke Interactions with Clouds (LASIC), aerosol and trace gas measurements were collected continuously from June 2016 through October 2017 over a 1.5 year period. Two BB seasons are contrasted with the near pristine background conditions during the campaign from the ARM Aerosol Mobile Facility 1 (AMF1) and Mobile Aerosol Observing System (MAOS). Numerous direct in situ aerosol and trace gas measurements are presented, e.g. black carbon (BC), carbon monoxide (CO), PM1 and PM10 aerosol absorption and scattering, submicron non-refractory chemical composition (Organics, Sulfate, Nitrate, Ammonium, Chloride), etc. Aerosol and trace gas signatures are investigated along with backtrajectories to identify sources. Carbonaceous aerosols emitted with gas-phase CO are used to determine particulate emission ratios along with intrinsic and extrinsic aerosol properties. BC mass concentrations reach 1 µg m-3 during multiday plumes and exceed 25% of the total aerosol submicron mass concentration. Organic Aerosol (OA) to BC Ratios of 2.4 in the plume are much higher than previously observed BB emissions in the Northern Hemisphere from forest fires in the US and also BB sources in Brazil. The differences observed between BB emissions in the Northern versus Southern Hemispheres highlights the need to understand the different atmospheric chemistries within the context of the differing background conditions of the two hemispheres.

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

NASA Astrophysics Data System (ADS)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in northern Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. The different meteorological regimes also affected the BC mixing state: in periods of enhanced stagnation and recirculation of pollutants, the number fraction of the BC-containing particles determined by ATOFMS was 75% of the total, while in the days of enhanced ventilation of the planetary boundary layer (PBL), such fraction was significantly lower (50%) because of the relative greater influence of non-BC-containing aerosol local sources in the Po Valley. Overall, a full internal mixing between BC and the non-refractory aerosol chemical components was not observed during the experiment in this environment.

New directions: Mineral dust and ozone - Heterogeneous chemistry

NASA Astrophysics Data System (ADS)

Ramachandran, S.

2015-04-01

Aerosols, the tiny solid or liquid particles suspended in air and produced from natural sources and anthropogenic activities, continue to contribute the largest uncertainty to radiative forcing (IPCC, 2013). Aerosol particles give rise to radiative forcing directly through scattering and absorption of solar and infrared radiation in the atmosphere. Aerosols also give rise to indirect radiative forcing by modifying the cloud optical properties and lifetimes. Among the aerosol species mineral dust and black carbon cause a warming (positive forcing) while sulphate and sea salt cause a cooling (negative forcing) of the Earth-atmosphere system. In tropics and sub-tropics mineral dust is a major contributor to aerosol loading and optical thickness. The global source strength of dust aerosol varies significantly on spatial and temporal scales. The source regions of dust are mainly deserts, dry lake beds, and semi-arid regions, in addition to drier regions where vegetation has been reduced or soil surfaces that are disturbed by man made activities. Anthropogenic activities mainly related to agriculture such as harvesting, ploughing, overgrazing, and cement production and transport also produce mineral dust. An estimated 2500 terragram (Tg, 1012 g) of mineral dust is emitted into the atmosphere per year, and dominates the aerosol mass over continental regions in south Asia and China accounting for ∼35% of the total aerosol mass (IPCC, 2013). In India, dust is prevalent throughout the north and western India during the year and peaks during premonsoon season.

Marine biogenic sources of organic nitrogen and water-soluble organic aerosols over the western North Pacific in summer

NASA Astrophysics Data System (ADS)

Miyazaki, Y.; Kawamura, K.; Sawano, M.

2009-12-01

Size-segregated aerosol samples of organic nitrogen (ON) as well as water-soluble organic compounds were obtained over the western North Pacific in the summer of 2008. Mass contributions of organics to the total aerosol mass were 20-40% in the supermicron mode and 45-60% in the submicron mode. ON as well as diacids and water-soluble organic carbon (WSOC) showed bimodal size distributions over the remote ocean, where high values of chlorophyll-a concentrations and depth-integrated primary production were observed. The ON concentrations increased with increasing biogenic tracer compounds such as methanesulfuric acid (MSA) and azelaic acid (C9). The average concentrations of ON and organic carbon (OC) in aerosols more influenced by marine biological activity were found to be about two times greater than those in biologically less influenced aerosols. These results provide evidence of marine biogenic sources of ON as well as OC. An average ON/OC ratio in biologically more influenced aerosols was as high as 0.49±0.11, which is higher than that in biologically less influenced aerosols (0.35±0.10). This result indicates that organic aerosol in this region is enriched in organic nitrogen, which linked to oceanic biological activity and comparable in magnitude to the marine biogenic OC source. We discuss possible processes for primary and secondary production of ON and OC in these samples, and stable nitrogen and carbon isotope ratios for total nitrogen (TN) and total carbon (TC).

On-road measurement of black carbon mass, absorption, and single-scattering albedo

EPA Science Inventory

Absorption and scattering of solar radiation by aerosols emitted from combustion sources can affect the earth’s radiative balance and may potentially affect local and regional climate. Optical properties of aerosols emitted from mobile sources have not been thoroughly characteri...

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. The high-time resolution data shows that rapid concentration changes of a common individual species can be lost with traditional bulk sampling, and a time resolution of 30 minutes is suggested to accurately represent these changes. Using the mass spectra collected from the extended sampling campaign, source apportionment was performed with positive matrix factorization (PMF). The resulting model features six factors either correlated to specific sources (meat cooking, car emissions/road dust, diesel exhaust) or types of compounds (phthalates, alkanes/alkanoic acids, PAHs). The high-time resolution data allowed for the observation of specific trends in each factor's behavior as a function of time and wind direction relative to the receptor site. Elemental carbon/organic carbon (EC/OC) data is used to calculate the percentages of primary and secondary organic aerosol. Primary organic aerosol (POA) constituted the vast majority of the total carbon at 91% (an average of 2.8 +/- 1.1mug/m 3); 30% of which came from combustion, and 70% from non-combustion sources. These results can be explained by the PIAMS data: the diesel factor contributes to the combustion-related POA; the car/road dust, meat cooking, and alkane/alkanoic acid factors contribute the majority of non-combustion POA. The remaining factors represent <5% of the remaining OC. Considering the compatibility of data from the EC/OC and PIAMS, the ability of PIAMS to yield molecular species information to further define the primary and secondary organic aerosol factions is a distinct advantage in describing the behavior of the Wilmington organic aerosol. PIAMS was also applied to laboratory experiments. These experiments simulated complex environmental processes in order to focus on answering a central question. By mixing cholesterol aerosol with ozone in a smog chamber, and monitoring the concentration of cholesterol with PIAMS, the rate of reaction was determined. This rate indicates that cholesterol aerosol, which is a suggested source tracer, will remain in the ambient air for a few days under normal conditions. PIAMS was also used to assist in identifying products from the ozonolysis of various monoterpenes. The product ion peaks observed indicates that both the stabilized Criegee intermediate pathway and the hydroperoxide channel are both active pathways in yielding dimers and high-order oligomer.

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.

Characterizing error distributions for MISR and MODIS optical depth data

NASA Astrophysics Data System (ADS)

Paradise, S.; Braverman, A.; Kahn, R.; Wilson, B.

2008-12-01

The Multi-angle Imaging SpectroRadiometer (MISR) and Moderate Resolution Imaging Spectroradiometer (MODIS) on NASA's EOS satellites collect massive, long term data records on aerosol amounts and particle properties. MISR and MODIS have different but complementary sampling characteristics. In order to realize maximum scientific benefit from these data, the nature of their error distributions must be quantified and understood so that discrepancies between them can be rectified and their information combined in the most beneficial way. By 'error' we mean all sources of discrepancies between the true value of the quantity of interest and the measured value, including instrument measurement errors, artifacts of retrieval algorithms, and differential spatial and temporal sampling characteristics. Previously in [Paradise et al., Fall AGU 2007: A12A-05] we presented a unified, global analysis and comparison of MISR and MODIS measurement biases and variances over lives of the missions. We used AErosol RObotic NETwork (AERONET) data as ground truth and evaluated MISR and MODIS optical depth distributions relative to AERONET using simple linear regression. However, AERONET data are themselves instrumental measurements subject to sources of uncertainty. In this talk, we discuss results from an improved analysis of MISR and MODIS error distributions that uses errors-in-variables regression, accounting for uncertainties in both the dependent and independent variables. We demonstrate on optical depth data, but the method is generally applicable to other aerosol properties as well.

Global chemical composition of ambient fine particulate matter for exposure assessment.

PubMed

Philip, Sajeev; Martin, Randall V; van Donkelaar, Aaron; Lo, Jason Wai-Ho; Wang, Yuxuan; Chen, Dan; Zhang, Lin; Kasibhatla, Prasad S; Wang, Siwen; Zhang, Qiang; Lu, Zifeng; Streets, David G; Bittman, Shabtai; Macdonald, Douglas J

2014-11-18

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004-2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weighted PM2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 μg/m(3)), secondary inorganic aerosol (11.1 ± 5.0 μg/m(3)), and mineral dust (11.1 ± 7.9 μg/m(3)). Secondary inorganic PM2.5 concentrations exceeded 30 μg/m(3) over East China. Sensitivity simulations suggested that population-weighted ambient PM2.5 from biofuel burning (11 μg/m(3)) could be almost as large as from fossil fuel combustion sources (17 μg/m(3)). These estimates offer information about global population exposure to the chemical components and sources of PM2.5.

Global Chemical Composition of Ambient Fine Particulate Matter for Exposure Assessment

PubMed Central

2015-01-01

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004–2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weighted PM2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 μg/m3), secondary inorganic aerosol (11.1 ± 5.0 μg/m3), and mineral dust (11.1 ± 7.9 μg/m3). Secondary inorganic PM2.5 concentrations exceeded 30 μg/m3 over East China. Sensitivity simulations suggested that population-weighted ambient PM2.5 from biofuel burning (11 μg/m3) could be almost as large as from fossil fuel combustion sources (17 μg/m3). These estimates offer information about global population exposure to the chemical components and sources of PM2.5. PMID:25343705

Global Chemical Composition of Ambient Fine Particulate Matter for Exposure Assessment

DOE PAGES

Philip, Sajeev; Martin, Randall V.; van Donkelaar, Aaron; ...

2014-10-24

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM 2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004–2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM 2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weightedmore » PM 2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 μg/m 3), secondary inorganic aerosol (11.1 ± 5.0 μg/m 3), and mineral dust (11.1 ± 7.9 μg/m 3). Secondary inorganic PM 2.5 concentrations exceeded 30 μg/m 3 over East China. Sensitivity simulations suggested that population-weighted ambient PM 2.5 from biofuel burning (11 μg/m 3) could be almost as large as from fossil fuel combustion sources (17 μg/m 3). In conclusion, these estimates offer information about global population exposure to the chemical components and sources of PM 2.5.« less

Do Regional Aerosols Contribute to the Riverine Export of Dissolved Black Carbon?

NASA Astrophysics Data System (ADS)

Jones, M. W.; Quine, T. A.; de Rezende, C. E.; Dittmar, T.; Johnson, B.; Manecki, M.; Marques, J. S. J.; de Aragão, L. E. O. C.

2017-11-01

The fate of black carbon (BC), a stable form of thermally altered organic carbon produced during biomass and fuel combustion, remains an area of uncertainty in the global carbon cycle. The transfer of photosynthetically derived BC into extremely long-term oceanic storage is of particular significance and rivers are the key linkage between terrestrial sources and oceanic stores. Significant fluvial fluxes of dissolved BC to oceans result from the slow release of BC from degrading charcoal stocks; however, these fluvial fluxes may also include undetermined contributions of aerosol BC, produced by biomass and fossil fuel combustion, which are deposited in river catchments following atmospheric transport. By investigation of the Paraíba do Sul River catchment in Southeast Brazil we show that aerosol deposits can be substantial contributors to fluvial fluxes of BC. We derived spatial distributions of BC stocks within the catchment associated with soil charcoal and with aerosol from both open biomass burning and fuel combustion. We then modeled the fluvial concentrations of dissolved BC (DBC) in scenarios with varying rates of export from each stock. We analyzed the ability of each scenario to reproduce the variability in DBC concentrations measured in four data sets of river water samples collected between 2010 and 2014 and found that the best performing scenarios included a 5-18% (135-486 Mg DBC year-1) aerosol contribution. Our results suggest that aerosol deposits of BC in river catchments have a shorter residence time in catchments than charcoal BC and, therefore, contribute disproportionately (with respect to stock magnitude) toward fluvial fluxes of BC.

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...

Smoke aerosol chemistry and aging of Siberian biomass burning emissions in a large aerosol chamber

NASA Astrophysics Data System (ADS)

Kalogridis, A.-C.; Popovicheva, O. B.; Engling, G.; Diapouli, E.; Kawamura, K.; Tachibana, E.; Ono, K.; Kozlov, V. S.; Eleftheriadis, K.

2018-07-01

Vegetation open fires constitute a significant source of particulate pollutants on a global scale and play an important role in both atmospheric chemistry and climate change. To better understand the emission and aging characteristics of smoke aerosols, we performed small-scale fire experiments using the Large Aerosol Chamber (LAC, 1800 m3) with a focus on biomass burning from Siberian boreal coniferous forests. A series of burn experiments were conducted with typical Siberian biomass (pine and debris), simulating separately different combustion conditions, namely, flaming, smoldering and mixed phase. Following smoke emission and dispersion in the combustion chamber, we investigated aging of aerosols under dark conditions. Here, we present experimental data on emission factors of total, elemental and organic carbon, as well as individual organic compounds, such as anhydrosugars, phenolic and dicarboxylic acids. We found that total carbon accounts for up to 80% of the fine mode (PM2.5) smoke aerosol. Higher PM2.5 emission factors were observed in the smoldering compared to flaming phase and in pine compared to debris smoldering phase. For low-temperature combustion, organic carbon (OC) contributed to more than 90% of total carbon, whereas elemental carbon (EC) dominated the aerosol composition in flaming burns with a 60-70% contribution to the total carbon mass. For all smoldering burns, levoglucosan (LG), a cellulose decomposition product, was the most abundant organic species (average LG/OC = 0.26 for pine smoldering), followed by its isomer mannosan or dehydroabietic acid (DA), an important constituent of conifer resin (DA/OC = 0.033). A levoglucosan-to-mannosan ratio of about 3 was observed, which is consistent with ratios reported for coniferous biomass and more generally softwood. The rates of aerosol removal for OC and individual organic compounds were investigated during aging in the chamber in terms of mass concentration loss rates over time under dark conditions and compared to the loss rate of EC. The latter is used as an inert tracer for estimating aerosol mechanical deposition and wall losses of the otherwise chemically conserved aerosol species. The OC/EC ratio increased with smoke aging for the flaming phase, suggesting a production/partitioning of organic compounds after emission. On the other hand, for smoldering burns OC/EC ratios decreased further with aging due to additional sinks of OC, other than those related to deposition and wall losses alone, such as evaporation of semi-volatile compounds. The chemical fingerprints of the major PM components of fresh and aged smoke found in this study are proposed to be used for the assessment of contributions from Siberian biomass burning to atmospheric pollution in source apportionment studies like those using molecular marker approaches.

Field Measurements of Trace Gases and Aerosols Emitted by Undersampled Combustion Sources Including Wood and Dung Cooking Fires, Garbage and Crop Residue Burning, and Indonesian Peat Fires

NASA Astrophysics Data System (ADS)

Stockwell, C.; Jayarathne, T. S.; Goetz, D.; Simpson, I. J.; Selimovic, V.; Bhave, P.; Blake, D. R.; Cochrane, M. A.; Ryan, K. C.; Putra, E. I.; Saharjo, B.; Stone, E. A.; DeCarlo, P. F.; Yokelson, R. J.

2017-12-01

Field measurements were conducted in Nepal and in the Indonesian province of Central Kalimantan to improve characterization of trace gases and aerosols emitted by undersampled combustion sources. The sources targeted included cooking with a variety of stoves, garbage burning, crop residue burning, and authentic peat fires. Trace gas and aerosol emissions were studied using a land-based Fourier transform infrared spectrometer, whole air sampling, photoacoustic extinctiometers (405 and 870nm), and filter samples that were analyzed off-line. These measurements were used to calculate fuel-based emission factors (EFs) for up to 90 gases, PM2.5, and PM2.5 constituents. The aerosol optical data measured included EFs for the scattering and absorption coefficients, the single scattering albedo (at 870 and 405 nm), as well as the absorption Ångström exponent. The emissions varied significantly by source, although light absorption by both brown and black carbon (BrC and BC, respectively) was important for all non-peat sources. For authentic peat combustion, the emissions of BC were negligible and absorption was dominated by organic aerosol. The field results from peat burning were in reasonable agreement with recent lab measurements of smoldering Kalimantan peat and compare well to the limited data available from other field studies. The EFs can be used with estimates of fuel consumption to improve regional emissions inventories and assessments of the climate and health impacts of these undersampled sources.

Model development of dust emission and heterogeneous chemistry within the Community Multiscale Air Quality modeling system and its application over East Asia

NASA Astrophysics Data System (ADS)

Dong, X.; Fu, J. S.; Huang, K.; Tong, D.

2015-12-01

The Community Multiscale Air Quality (CMAQ) model has been further developed in terms of simulating natural wind-blown dust in this study, with a series of modifications aimed at improving the model's capability to predict the emission, transport, and chemical reactions of dust aerosols. The default parameterization of threshold friction velocity constants in the CMAQ are revised to avoid double counting of the impact of soil moisture based on the re-analysis of field experiment data; source-dependent speciation profiles for dust emission are derived based on local measurements for the Gobi and Taklamakan deserts in East Asia; and dust heterogeneous chemistry is implemented to simulate the reactions involving dust aerosol. The improved dust module in the CMAQ was applied over East Asia for March and April from 2006 to 2010. Evaluation against observations has demonstrated that simulation bias of PM10 and aerosol optical depth (AOD) is reduced from -55.42 and -31.97 % in the original CMAQ to -16.05 and -22.1 % in the revised CMAQ, respectively. Comparison with observations at the nearby Gobi stations of Duolun and Yulin indicates that applying a source-dependent profile helps reduce simulation bias for trace metals. Implementing heterogeneous chemistry is also found to result in better agreement with observations for sulfur dioxide (SO2), sulfate (SO42-), nitric acid (HNO3), nitrous oxides (NOx), and nitrate (NO3-). Investigation of a severe dust storm episode from 19 to 21 March 2010 suggests that the revised CMAQ is capable of capturing the spatial distribution and temporal variations of dust aerosols. Model evaluation indicates potential uncertainties within the excessive soil moisture fraction used by meteorological simulation. The mass contribution of fine mode aerosol in dust emission may be underestimated by 50 %. The revised revised CMAQ provides a useful tool for future studies to investigate the emission, transport, and impact of wind-blown dust over East Asia and elsewhere.

Characterization Of Industrial And Background Aerosols In The RhÔne-alpes Region Using Laser Remote Sensing Device.

NASA Astrophysics Data System (ADS)

Geffroy, S.; Rairoux, P.; Mondelain, D.; Boutou, V.; Wolf, J.-P.; Frejafon, E.

Lack of reliable database on aerosol emission and dispersion is one of the main rea- sons for the incertitude of the impact of aerosol on the climate change. International statements and policies requested improvement on the global and on the regional scale. This new project is related to the characterisation of the spatial and time distribution of the aerosols in the Rhône-Alpes region. Actually, aerosols monitoring is mainly performed at ground level in this region and only few studies have been performed on the 3D distribution of urban aerosols (soot) using remote sensing laser device. The Rhône-Alpes region is representative for the regional impact of industry and traffic emission and also for the long-range transport of pollution over the East part of the Alps. The environmental situation of the region in term of sources and localization is especially dominated by: heavy traffic with several motorways (A6 from Paris, A7 to Marseille - both downtown - and A43 to the Alps and Italy) and industrial pollu- tion in particular for Lyon (refinery and several chemistry plants) and Saint Etienne agglomerations, which have a direct impact on the local air quality and also on the regional and national scale. Characterization of the aerosol load and dispersion in this region will be achieved applying two schemes. The first one will be related to the 3D quantitative characterization of diffuse aerosol emission in the industrial areas. Mon- itoring will be performed using a UV-infrared lidar remote sensing device. Emission cadastre elaboration and microphysical characterisation of the emission will be estab- lished. Direct access to several aerosol distribution modes will be used to describe the aerosol population dynamic: sedimentation, transport and aggregation. Studies on the direct impact of the emission on the region will be achieved coupling the 3D and ground level monitoring with dispersion model. The second scheme will be related to the long term remote sensing of the atmospheric background aerosols. Monitoring of the vertical and time distribution of their optical properties will be performed and this at 6 channels laying from the UV to the infrared spectral region. A high priority will be set on the data quality control and assurance in order to elaborate a reliable database. Several analyses will be performed with this dataset: the characterization of the microphysical properties of the aerosols. The regional and continental impact of the aerosols coupling the data with back-trajectories calculation and the validation of radiative model. By achieving a sufficient data quality, a proposition will be made to integrate the data into the European network Earlinet, which establishes a quantita- tive comprehensive statistical data base of both horizontal and vertical distributions of aerosols on a continental scale using a network of advanced laser remote sensing stations distributed all over Europe. This project will begin in summer 2002 and it will be taking place in cooperation with the national office INERIS.

ACTRIS ACSM intercomparison - Part 2: Intercomparison of ME-2 organic source apportionment results from 15 individual, co-located aerosol mass spectrometers

NASA Astrophysics Data System (ADS)

Fröhlich, R.; Crenn, V.; Setyan, A.; Belis, C. A.; Canonaco, F.; Favez, O.; Riffault, V.; Slowik, J. G.; Aas, W.; Aijälä, M.; Alastuey, A.; Artiñano, B.; Bonnaire, N.; Bozzetti, C.; Bressi, M.; Carbone, C.; Coz, E.; Croteau, P. L.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Jayne, J. T.; Lunder, C. R.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petralia, E.; Poulain, L.; Priestman, M.; Ripoll, A.; Sarda-Estève, R.; Wiedensohler, A.; Baltensperger, U.; Sciare, J.; Prévôt, A. S. H.

2015-06-01

Chemically resolved atmospheric aerosol data sets from the largest intercomparison of the Aerodyne aerosol chemical speciation monitors (ACSMs) performed to date were collected at the French atmospheric supersite SIRTA. In total 13 quadrupole ACSMs (Q-ACSM) from the European ACTRIS ACSM network, one time-of-flight ACSM (ToF-ACSM), and one high-resolution ToF aerosol mass spectrometer (AMS) were operated in parallel for about 3 weeks in November and December~2013. Part 1 of this study reports on the accuracy and precision of the instruments for all the measured species. In this work we report on the intercomparison of organic components and the results from factor analysis source apportionment by positive matrix factorisation (PMF) utilising the multilinear engine 2 (ME-2). Except for the organic contribution of mass-to-charge ratio m/z 44 to the total organics (f44), which varied by factors between 0.6 and 1.3 compared to the mean, the peaks in the organic mass spectra were similar among instruments. The m/z 44 differences in the spectra resulted in a variable f44 in the source profiles extracted by ME-2, but had only a minor influence on the extracted mass contributions of the sources. The presented source apportionment yielded four factors for all 15 instruments: hydrocarbon-like organic aerosol (HOA), cooking-related organic aerosol (COA), biomass burning-related organic aerosol (BBOA) and secondary oxygenated organic aerosol (OOA). ME-2 boundary conditions (profile constraints) were optimised individually by means of correlation to external data in order to achieve equivalent / comparable solutions for all ACSM instruments and the results are discussed together with the investigation of the influence of alternative anchors (reference profiles). A comparison of the ME-2 source apportionment output of all 15 instruments resulted in relative standard deviations (SD) from the mean between 13.7 and 22.7 % of the source's average mass contribution depending on the factors (HOA: 14.3 ± 2.2 %, COA: 15.0 ± 3.4 %, OOA: 41.5 ± 5.7 %, BBOA: 29.3 ± 5.0 %). Factors which tend to be subject to minor factor mixing (in this case COA) have higher relative uncertainties than factors which are recognised more readily like the OOA. Averaged over all factors and instruments the relative first SD from the mean of a source extracted with ME-2 was 17.2 %.

Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China

NASA Astrophysics Data System (ADS)

Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; Wang, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang

2017-04-01

Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

The Asian Tropopause Aerosol Layer: Balloon-Borne Measurements, Satellite Observations and Modeling Approaches

NASA Technical Reports Server (NTRS)

Fairlie, T. D.; Vernier, J.-P.; Natarajan, M.; Deshler, Terry; Liu, H.; Wegner, T.; Baker, N.; Gadhavi, H.; Jayaraman, A.; Pandit, A.;

Reactive Nitrogen Chemistry in Aerosol Water as a Source of Sulfate during Haze Events in China

NASA Astrophysics Data System (ADS)

Su, H.; Zheng, G.; Wei, C.; Mu, Q.; Zheng, B.; Wang, Z.; Zhang, Q.; Gao, M.; He, K.; Carmichael, G. R.; Poeschl, U.; Cheng, Y.

2017-12-01

Fine particle pollution associated with winter haze threatens the health of over 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models relying on sulfate production mechanisms that require photochemical oxidants, cannot predict these high levels due to the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.

Where and What Is Pristine Marine Aerosol?

NASA Astrophysics Data System (ADS)

Russell, L. M.; Frossard, A. A.; Long, M. S.; Burrows, S. M.; Elliott, S.; Bates, T. S.; Quinn, P.

2014-12-01

The sources and composition of atmospheric marine aerosol particles have been measured by functional group composition (from Fourier transform infrared spectroscopy) to identify the organic composition of the pristine primary marine (ocean-derived) particles as 65% hydroxyl, 21% alkane, 6% amine, and 7% carboxylic acid functional groups [Frossard et al., 2014a,b]. Pristine but non-primary components from photochemical reactions (likely from biogenic marine vapor emissions) add carboxylic acid groups. Non-pristine contributions include shipping effluent in seawater and ship emissions, which add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. The pristine primary marine (ocean-derived) organic aerosol composition is nearly identical to model generated primary marine aerosol particles from bubbled seawater, indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the generated primary marine aerosol particles remained nearly constant over a broad range of chlorophyll-a concentrations, the generated primary marine aerosol particle alkane group fraction increased with chlorophyll-a concentrations. In addition, the generated primary marine aerosol particles have a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater hydroxyl group peak location is closer to that of polysaccharides. References Cited Frossard, Amanda A., Lynn M. Russell, Paola Massoli, Timothy S. Bates, and Patricia K. Quinn, "Side-by-Side Comparison of Four Techniques Explains the Apparent Differences in the Organic Composition of Generated and Ambient Marine Aerosol Particles," Aerosol Science and Technology - Aerosol Research Letter, 48:v-x, doi10.1080/02786826.2013.879979, 2014a. Frossard, A.A., L.M. Russell, M.S. Long, S.M. Burrows, S.M. Elliot, T.S. Bates, and P.K. Quinn, "Sources and Composition of Submicron Organic Mass in Marine Aerosol Particles," Journal of Geophysical Research - Atmospheres, submitted 2014b.

Anthropogenic aerosols as a source of ancient dissolved organic matter in glaciers

USGS Publications Warehouse

Stubbins, Aron; Hood, Eran; Raymond, Peter A.; Aiken, George R.; Sleighter, Rachel L.; Hernes, Peter J.; Butman, David; Hatcher, Patrick G.; Striegl, Robert G.; Schuster, Paul F.; Abdulla, Hussain A.N.; Vermilyea, Andrew W.; Scott, Durelle T.; Spencer, Robert G.M.

2012-01-01

Glacier-derived dissolved organic matter represents a quantitatively significant source of ancient, yet highly bioavailable carbon to downstream ecosystems. This finding runs counter to logical perceptions of age–reactivity relationships, in which the least reactive material withstands degradation the longest and is therefore the oldest. The remnants of ancient peatlands and forests overrun by glaciers have been invoked as the source of this organic matter. Here, we examine the radiocarbon age and chemical composition of dissolved organic matter in snow, glacier surface water, ice and glacier outflow samples from Alaska to determine the origin of the organic matter. Low levels of compounds derived from vascular plants indicate that the organic matter does not originate from forests or peatlands. Instead, we show that the organic matter on the surface of the glaciers is radiocarbon depleted, consistent with an anthropogenic aerosol source. Fluorescence spectrophotometry measurements reveal the presence of protein-like compounds of microbial or aerosol origin. In addition, ultrahigh-resolution mass spectrometry measurements document the presence of combustion products found in anthropogenic aerosols. Based on the presence of these compounds, we suggest that aerosols derived from fossil fuel burning are a source of pre-aged organic matter to glacier surfaces. Furthermore, we show that the molecular signature of the organic matter is conserved in snow, glacier water and outflow, suggesting that the anthropogenic carbon is exported relatively unchanged in glacier outflows.

A View of Earth's Aerosol System from Space to Your Office Chair

NASA Technical Reports Server (NTRS)

Colarco, Peter

2008-01-01

Aerosols are tiny particles and droplets suspended in the air. Each day you breathe in about 10 billion of them, about a half a million per breath. They are formed in nature by volcanoes, dust storms, sea spray, and emissions from vegetation. Humans create aerosols and alter their natural sources by burning fossil fuels and modifying land cover. Fires are another important source of aerosols; some are natural, such as wildfires started by lightning strikes, while others are from human-caused burning of vegetation for cooking, heating, and land clearing. Aerosols have complex effects on Earth's climate. In general, they cool the surface by reflecting (scattering) radiation from the sun back into space. Dust and smoke absorb solar radiation and heat the atmosphere where they are concentrated. Aerosols change the properties of clouds. Indeed, it would be very difficult to form clouds in the atmosphere without aerosols to act as 'seeds' for water to condense on. In aerosol polluted environments clouds tend to have smaller droplets than clouds formed in cleaner environments; these polluted clouds appear brighter from space because they reflect more sunlight, and they may persist longer and not rain as intensely. Aerosols also affect local air quality and visibility. Data collected by NASA satellites over the past decade have provided an unprecedented view of Earth's aerosol distribution and dramatically increased our understanding of where aerosols come from and just how far they travel in the atmosphere. In this talk I will discuss observations of aerosols from space and how they inform numerical transport models attempting to simulate the global aerosol system.

Implementation of warm-cloud processes in a source-oriented WRF/Chem model to study the effect of aerosol mixing state on fog formation in the Central Valley of California

NASA Astrophysics Data System (ADS)

Lee, Hsiang-He; Chen, Shu-Hua; Kleeman, Michael J.; Zhang, Hongliang; DeNero, Steven P.; Joe, David K.

2016-07-01

The source-oriented Weather Research and Forecasting chemistry model (SOWC) was modified to include warm cloud processes and was applied to investigate how aerosol mixing states influence fog formation and optical properties in the atmosphere. SOWC tracks a 6-D chemical variable (X, Z, Y, size bins, source types, species) through an explicit simulation of atmospheric chemistry and physics. A source-oriented cloud condensation nuclei module was implemented into the SOWC model to simulate warm clouds using the modified two-moment Purdue Lin microphysics scheme. The Goddard shortwave and long-wave radiation schemes were modified to interact with source-oriented aerosols and cloud droplets so that aerosol direct and indirect effects could be studied. The enhanced SOWC model was applied to study a fog event that occurred on 17 January 2011, in the Central Valley of California. Tule fog occurred because an atmospheric river effectively advected high moisture into the Central Valley and nighttime drainage flow brought cold air from mountains into the valley. The SOWC model produced reasonable liquid water path, spatial distribution and duration of fog events. The inclusion of aerosol-radiation interaction only slightly modified simulation results since cloud optical thickness dominated the radiation budget in fog events. The source-oriented mixture representation of particles reduced cloud droplet number relative to the internal mixture approach that artificially coats hydrophobic particles with hygroscopic components. The fraction of aerosols activating into cloud condensation nuclei (CCN) at a supersaturation of 0.5 % in the Central Valley decreased from 94 % in the internal mixture model to 80 % in the source-oriented model. This increased surface energy flux by 3-5 W m-2 and surface temperature by as much as 0.25 K in the daytime.

Global Distributions of Mineral Dust Properties from SeaWiFS and MODIS: From Sources to Sinks

NASA Technical Reports Server (NTRS)

Hsu, N. Christina; Bettenhausen, C.; Sayer, A.

2011-01-01

The impact of natural and anthropogenic sources of mineral dust has gained increasing attention from scientific communities in recent years. Indeed, these airborne dust particles, once lifted over the source regions, can be transported out of the boundary layer into the free troposphere and can travel thousands of kilometers across the oceans resulting in important biogeochemical impacts on the ecosystem. Due to the relatively short lifetime (a few hours to about a week), the distributions of these mineral dust particles vary extensively in both space and time. Consequently, satellite observations are needed over both source and sink regions for continuous temporal and spatial sampling of aerosol properties. With the launch of SeaWiFS in 1997, Terra/MODIS in 1999, and Aqua/MODIS in 2002, high quality comprehensive aerosol climatology is becoming feasible for the first time. As a result of these unprecedented satellite data records, studies of the radiative and biogeochemical effects due to dust aerosols are now possible. In this study, we will show the comparisons of satellite retrieved aerosol optical thickness using Deep Blue algorithm with data from AERONET sunphotometers over desert and semi-desert regions as well as vegetated areas. Our results indicate reasonable agreements between these two. These new satellite products will allow scientists to determine quantitatively the aerosol properties near sources using high spatial resolution measurements from Sea WiFS and MODIS-like instruments. The multiyear satellite measurements since 1997 from Sea WiFS will be compared with those retrieved from MODIS and MISR, and will be utilized to investigate the interannual variability of source, pathway, and dust loading associated with the dust outbreaks over the entire globe. Finally, the trends observed over the last decade based upon the SeaWiFS time series in the amounts of tropospheric aerosols due to natural and anthropogenic sources (such as changes in the frequency of dust storms) will be discussed.

Long-Term Variability of Airborne Asian Dust Observed from TOMS

NASA Technical Reports Server (NTRS)

Herman, J. R.; Hsu, N. C.; Seftor, C. J.; Holben, B. N.; Holben, B. N.; Einaudi, Franco (Technical Monitor)

2001-01-01

Recent studies suggest that airborne Asian dust may not only play an important role in the regional radiation budget, but also influence the air quality over North America through long-range transport. In this paper, we use satellite data to investigate the long-term variability of airborne Asian dust as well as the daily variation of the dust aerosol distribution. By combining the Total Ozone Mapping Spectrometer (TOMS) aerosol index with National Centers for Environmental Prediction (NCEP) wind data, our analysis shows a strong correlation between the generation of dust storms in the region and the passage of springtime weather fronts. This is consistent with earlier studies performed by other researchers. According to both the Nimbus-7 and Earth-Probe TOMS data the Takla Makan desert, the Gobi desert, and the and region of Inner Mongolia are major sources of the eastward-flowing airborne Asian dust. Heavily populated areas in eastern China (e.g., Beijing) are often on the primary path of the dust storms originating in these desert regions. The increasing desertification north of the Beijing region has served to exacerbate problems stemming from these storms. The time series derived from 20 years of TOMS aerosol index data shows the first significant satellite evidence of the atmospheric effect of increasing desertification, indicating that the amount of dust blown eastward has increased strongly during the past few years including the year 2000.

Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

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

Kleinman L. I.; Daum, P. H.; Lee, Y.-N.

2012-01-04

During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate. Pollutant layers in the free troposphere (FT) can be a result of emissionsmore » to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a boundary layer (BL) contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (D{sub p} > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25 % of aerosol with D{sub p} > 100 nm are interstitial (not activated). A direct comparison of pre-cloud and in-cloud aerosol yields a higher estimate. Artifacts in the measurement of interstitial aerosol due to droplet shatter and evaporation are discussed. Within each of 102 constant altitude cloud transects, CDNC and interstitial aerosol were anti-correlated. An examination of one cloud as a case study shows that the interstitial aerosol appears to have a background, upon which is superimposed a high frequency signal that contains the anti-correlation. The anti-correlation is a possible source of information on particle activation or evaporation.« less

Interpretation of Secondary Organic Aerosol Formation from Diesel Exhaust Photooxidation in an Environmental Chamber

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

Nakao, Shunsuke; Shrivastava, ManishKumar B.; Nguyen, Anh

2011-04-14

Secondary organic aerosol (SOA) formation from diesel exhaust in a smog chamber was investigated. Particle volume measurement based on mobility diameter is shown to underestimate SOA formation from diesel exhaust due to the external void space of agglomerate particles, in which case mass-based measurement technique is necessary. Rapid determination of particle effective density as a function of particle mass was performed by an Aerosol Particle Mass analyzer – Scanning Mobility Particle Sizer (APM-SMPS) to obtain particle mass concentration and fractal dimension. Continuous aging of aerosol was observed in terms of atomic ratio (O/C), from 0.05 to 0.25 in 12 hours,more » underscoring the importance of multi-generational oxidation of low-volatile organic vapors emitted from diesel engine as the significant source of oxygenated SOA. Experimental conditions possibly have strong impacts on physical evolution of diesel particulates in a smog chamber. Higher particle effective densities were observed when raw exhaust was injected into a full bag as opposed to filling a bag with diluted exhaust using an ejector diluter. When longer transfer line was used for injecting diesel exhaust into the smog chamber, rapid particle coagulation was observed, leading to increasing particle volume concentration in dark while its mass concentration is decreasing.« less

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

NASA Technical Reports Server (NTRS)

Ghan, Stephen J.; Rissman, Tracey A.; Ellman, Robert; Ferrare, Richard A.; Turner, David; Flynn, Connor; Wang, Jian; Ogren, John; Hudson, James; Jonsson, Haflidi H.;

AEROSOL CHEMICAL CHARACTERISTION ON BOARD THE DOE G1 AIRCRAFT USING A PARTICLE INTO LIQUID SAMPLER DURING THE TEXAQS 2000 EXPERIMENT.

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

LEE,Y.N.; SONG,Z.; LIU,Y.

2001-01-13

Knowledge of aerosol chemical composition is key to understanding a number of properties of ambient aerosol particles including sources, size/number distribution, chemical evolution, optical properties and human health effects. Although filter based techniques have been widely used to determine aerosol chemical constituents, they generally cannot provide sufficiently fast time resolution needed to investigate sources and chemical evolution that effect aerosol chemical, size and number changes. In order to gain an ability to describe and predict the life cycles of ambient aerosols as a basis for ambient air quality control, fast and sensitive determination of the aerosol chemical composition must bemore » made available. To help to achieve this goal, we deployed a newly developed technique, referred to as PILS (particle-into-liquid-sampler), on the DOE G1 aircraft during the 2000 Texas Air Quality Study (TexAQS 2000) to characterize the major ionic species of aerosol particles with aerodynamic size smaller than 2.5 {micro}m (PM 2.5). The results obtained are examined in the context of other simultaneously collected data for insights into the measurement capability of the PILS system.« less

Implementing Marine Organic Aerosols Into the GEOS-Chem Model

NASA Technical Reports Server (NTRS)

Johnson, Matthew S.

2015-01-01

Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.

Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

NASA Astrophysics Data System (ADS)

Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

2010-03-01

This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source contributions to OC when different biomass profiles were used. The majority of OC was unapportioned to primary sources and was estimated to be of secondary origin, while biomass combustion was the next-largest source of OC. The CMB apportionment of EC to primary sources was unstable due to the diversity of biomass burning conditions in the region. The model results suggested that biomass burning and fossil fuel were important contributors to EC, but could not reconcile their relative contributions.

Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

NASA Astrophysics Data System (ADS)

Slowik, J. G.; Stroud, C.; Bottenheim, J. W.; Brickell, P. C.; Chang, R. Y.-W.; Liggio, J.; Makar, P. A.; Martin, R. V.; Moran, M. D.; Shantz, N. C.; Sjostedt, S. J.; van Donkelaar, A.; Vlasenko, A.; Wiebe, H. A.; Xia, A. G.; Zhang, J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-03-01

Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

Volatility Properties of Internally- and Externally-Mixed Ambient Aerosols at an Anthropogenically-influenced Forest Site in Southeastern USA

NASA Astrophysics Data System (ADS)

Khlystov, A.; Subramanian, R.

2015-12-01

Secondary organic aerosol (SOA) from biogenic sources has a significant contribution to ambient aerosol loadings in Southeastern USA and thus contributes to adverse health effects of air pollution and influences regional and global climate. Volatility properties of biogenic SOA determine its concentration, reactivity, and lifetime, but are still largely unknown. As part of a larger study to assess the effect of biogenic SOA on aerosol optical properties, a set of instruments, including scanning mobility sizers (SMPS), single particle soot photometer (SP2), and a thermodenuder, was deployed during June 2015 at a Duke Forest site near Chapel Hill, NC. The site is characterized by a significant contribution of both biogenic and urban (mostly traffic) sources. Measurements of changes in aerosol volume and optical size upon heating in the thermodenuder at different temperatures are used to derive volatility properties of the ambient aerosol. A limited set of experiments was carried out using the tandem differential mobility analysis (TDMA) approach to investigate whether the ambient aerosol at the Duke Forest site is internally mixed with respect to its volatility properties. In this presentation we will discuss equilibrium and kinetic aspects of aerosol volatility observed during this study and implications of external vs. internal mixing for derivation of bulk volatility properties of ambient aerosol.

Classification of Aerosol Retrievals from Spaceborne Polarimetry Using a Multiparameter Algorithm

NASA Technical Reports Server (NTRS)

Russell, Philip B.; Kacenelenbogen, Meloe; Livingston, John M.; Hasekamp, Otto P.; Burton, Sharon P.; Schuster, Gregory L.; Johnson, Matthew S.; Knobelspiesse, Kirk D.; Redemann, Jens; Ramachandran, S.;

Heavy Ion Formation in Titan's Ionosphere: Magnetospheric Introduction of Free Oxygen and Source of Titan's Aerosols?

NASA Technical Reports Server (NTRS)

Sittler, E. C., Jr.; Hartle, R. E.; Cooper, J. F.; Johnson, R. E.; Coates, A.; dePater, imke; Strom, Daphne; Simoes, F.; Steele, A.; Robb, F.

2007-01-01

With the recent discovery of heavy ions, positive and negative, by the Cassini Plasma Spectrometer (CAPS) instrument in Titan's ionosphere, it reveals new possibilities for aerosol formation at Titan and the introduction of free oxygen to the aerosol chemistry from Saturn's magnetosphere with Enceladus as the primary oxygen source. One can estimate whether the heavy ions in the ionosphere are of sufficient number to account for all the aerosols, under what conditions are favorable for heavy ion formation and how they are introduced as seed particles deeper in Titan's atmosphere where the aerosols form and eventually find themselves on Titan's surface where unknown chemical processes can take place. Finally, what are the possibilities with regard to their chemistry on the surface with some free oxygen present in their seed particles?

Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass at Bakersfield

EPA Science Inventory

Secondary organic aerosols (SOA), known to form in the atmosphere from oxidation of volatile organic compounds (VOCs) emitted by anthropogenic and biogenic sources, are a poorly understood but substantial component of atmospheric particles. In this study, we examined the chemic...

Natural and Anthropogenically Perturbed Biogenic Aerosol over Tropical South East Asia

NASA Astrophysics Data System (ADS)

Coe, H.; Robinson, N.; Allan, J. D.; Hewitt, C. N.

2014-12-01

Tropical forested regions are of interest as sources of atmospheric aerosol since they cover very large areas of the tropics and are a source of a large amount of volatile organic compounds which act as precursors for particle formation. Natural forest regions offer the potential to study the background state of the tropics and so potentially gain some insight into the pre-perturbed atmosphere. However, over the last decade in South East Asia, a considerable fraction of the native tropical deciduous forest has been deforested and replanted with palm oil plantations. This changes the range of volatile organic compounds that are emitted and act as sources of secondary organic aerosol. A suite of intensive ground and airborne measurements were made over both tropical forest and oil palm plantations in Sabah, Malaysia as part of the "Oxidant and Particle Photochemical Processes above a South East Asian tropical rainforest (OP3) during 2008. These data will be used together with recent improvements in our understanding of aerosol formation from biogenic compounds to discuss aerosol formation in tropical regions and the influence of human influence through widespread palm oil agriculture.

A simple parameterization of aerosol emissions in RAMS

NASA Astrophysics Data System (ADS)

Letcher, Theodore

Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical model. Furthermore, SA formation is greatly reduced during the winter months due to the lack of naturally produced organic VOC's. Because of these reasons, it was felt that neglecting SOA within the model was the best course of action. The actual parameterization uses a prescribed source map to add aerosol to the model at two vertical levels that surround an arbitrary height decided by the user. To best represent the real-world, the WRF Chemistry model was run using the National Emissions Inventory (NEI2005) to represent anthropogenic emissions and the Model Emissions of Gases and Aerosols from Nature (MEGAN) to represent natural contributions to aerosol. WRF Chemistry was run for one hour, after which the aerosol output along with the hygroscopicity parameter (κ) were saved into a data file that had the capacity to be interpolated to an arbitrary grid used in RAMS. The comparison of this parameterization to observations collected at Mesa Verde National Park (MVNP) during the Inhibition of Snowfall from Pollution Aerosol (ISPA-III) field campaign yielded promising results. The model was able to simulate the variability in near surface aerosol concentration with reasonable accuracy, though with a general low bias. Furthermore, this model compared much better to the observations than did the WRF Chemistry model using a fraction of the computational expense. This emissions scheme was able to show reasonable solutions regarding the aerosol concentrations and can therefore be used to provide an estimate of the seasonal impact of increased CCN on water resources in Western Colorado with relatively low computational expense.

In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity

NASA Astrophysics Data System (ADS)

Beekmann, M.; Prévôt, A. S. H.; Drewnick, F.; Sciare, J.; Pandis, S. N.; Denier van der Gon, H. A. C.; Crippa, M.; Freutel, F.; Poulain, L.; Ghersi, V.; Rodriguez, E.; Beirle, S.; Zotter, P.; von der Weiden-Reinmüller, S.-L.; Bressi, M.; Fountoukis, C.; Petetin, H.; Szidat, S.; Schneider, J.; Rosso, A.; El Haddad, I.; Megaritis, A.; Zhang, Q. J.; Michoud, V.; Slowik, J. G.; Moukhtar, S.; Kolmonen, P.; Stohl, A.; Eckhardt, S.; Borbon, A.; Gros, V.; Marchand, N.; Jaffrezo, J. L.; Schwarzenboeck, A.; Colomb, A.; Wiedensohler, A.; Borrmann, S.; Lawrence, M.; Baklanov, A.; Baltensperger, U.

2015-08-01

A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies.

In-situ, satellite measurement and model evidence for a~dominant regional contribution to fine particulate matter levels in the Paris Megacity

NASA Astrophysics Data System (ADS)

Beekmann, M.; Prévôt, A. S. H.; Drewnick, F.; Sciare, J.; Pandis, S. N.; Denier van der Gon, H. A. C.; Crippa, M.; Freutel, F.; Poulain, L.; Ghersi, V.; Rodriguez, E.; Beirle, S.; Zotter, P.; von der Weiden-Reinmüller, S.-L.; Bressi, M.; Fountoukis, C.; Petetin, H.; Szidat, S.; Schneider, J.; Rosso, A.; El Haddad, I.; Megaritis, A.; Zhang, Q. J.; Michoud, V.; Slowik, J. G.; Moukhtar, S.; Kolmonen, P.; Stohl, A.; Eckhardt, S.; Borbon, A.; Gros, V.; Marchand, N.; Jaffrezo, J. L.; Schwarzenboeck, A.; Colomb, A.; Wiedensohler, A.; Borrmann, S.; Lawrence, M.; Baklanov, A.; Baltensperger, U.

2015-03-01

A detailed characterization of air quality in Paris (France), a megacity of more than 10 million inhabitants, during two one month intensive campaigns and from additional one year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in-situ measurements during short intensive and longer term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by a comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions contributed less than 20% in winter and 40% in summer to carbonaceous fine PM, unexpectedly little for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e. from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only controlling part of its own average and peak PM levels has important implications for air pollution regulation policies.

Contrasting cloud composition between coupled and decoupled marine boundary layer clouds

NASA Astrophysics Data System (ADS)

Wang, Zhen; Mora Ramirez, Marco; Dadashazar, Hossein; MacDonald, Alex B.; Crosbie, Ewan; Bates, Kelvin H.; Coggon, Matthew M.; Craven, Jill S.; Lynch, Peng; Campbell, James R.; Azadi Aghdam, Mojtaba; Woods, Roy K.; Jonsson, Haflidi; Flagan, Richard C.; Seinfeld, John H.; Sorooshian, Armin

2016-10-01

Marine stratocumulus clouds often become decoupled from the vertical layer immediately above the ocean surface. This study contrasts cloud chemical composition between coupled and decoupled marine stratocumulus clouds for dissolved nonwater substances. Cloud water and droplet residual particle composition were measured in clouds off the California coast during three airborne experiments in July-August of separate years (Eastern Pacific Emitted Aerosol Cloud Experiment 2011, Nucleation in California Experiment 2013, and Biological and Oceanic Atmospheric Study 2015). Decoupled clouds exhibited significantly lower air-equivalent mass concentrations in both cloud water and droplet residual particles, consistent with reduced cloud droplet number concentration and subcloud aerosol (Dp > 100 nm) number concentration, owing to detachment from surface sources. Nonrefractory submicrometer aerosol measurements show that coupled clouds exhibit higher sulfate mass fractions in droplet residual particles, owing to more abundant precursor emissions from the ocean and ships. Consequently, decoupled clouds exhibited higher mass fractions of organics, nitrate, and ammonium in droplet residual particles, owing to effects of long-range transport from more distant sources. Sodium and chloride dominated in terms of air-equivalent concentration in cloud water for coupled clouds, and their mass fractions and concentrations exceeded those in decoupled clouds. Conversely, with the exception of sea-salt constituents (e.g., Cl, Na, Mg, and K), cloud water mass fractions of all species examined were higher in decoupled clouds relative to coupled clouds. Satellite and Navy Aerosol Analysis and Prediction System-based reanalysis data are compared with each other, and the airborne data to conclude that limitations in resolving boundary layer processes in a global model prevent it from accurately quantifying observed differences between coupled and decoupled cloud composition.

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.: URBAN INFLUENCE ON RURAL AEROSOL

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

Zhou, Shan; Collier, Sonya; Xu, Jianzhong

2016-05-19

Continuous real-time measurements of atmospheric aerosol with an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the DOE Aerosol Life Cycle Intensive Operational Period (ALC-IOP) campaign.

On-line measurement of gaseous iodine species during a PWR severe accident

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

Haykal, I.; Doizi, D.; Perrin, A.

A long-range remote sensing of severe accidents in nuclear power plants can be obtained by monitoring the online emission of volatile fission products such as xenon, krypton, caesium and iodine. The nuclear accident in Fukushima was ranked at level 7 of the International Nuclear Event Scale by the NISA (Nuclear and Industrial Safety Agency) according to the importance of the radionuclide release and the off-site impact. Among volatile fission products, iodine species are of high concern, since they can be released under aerosols as well as gaseous forms. Four years after the Fukushima accident, the aerosol/gaseous partition is still notmore » clear. Since the iodine gaseous forms are less efficiently trapped by the Filtered Containment Venting Systems than aerosol forms, it is of crucial importance to monitor them on-line during a nuclear accident, in order to improve the source term assessment in such a situation. Therefore, we propose to detect and quantify these iodine gaseous forms by the use of highly sensitive optical methods. (authors)« less

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Four dimensional variational assimilation of in-situ and remote-sensing aerosol data

NASA Astrophysics Data System (ADS)

Nieradzik, L. P.; Elbern, H.

2012-04-01

Aerosols play an increasingly important role in atmospheric modelling. They have a strong influence on the radiative transfer balance and a significant impact on human health. Their origin is various and so are its effects. Most of the measurement sites in Europe account for an integrated aerosol load PMx (Particulate Matter of less than x μm in diameter) which does not give any qualitative information on the composition of the aerosol. Since very different constituents contribute to PMx, like e.g. mineral dust derived from desert storms or sea salt, it is necessary to make aerosol forecasts not only of load, but also type resolved. The method of four dimensional variational data assimilation (4Dvar) is a widely known technique to enhance forecast skills of CTMs (Chemistry-Transport-Models) by ingesting in-situ and, especially, remote-sensing measurements. The EURAD-IM (EURopean Air pollution Dispersion - Inverse Model), containing a full adjoint gas-phase model, has been expanded with an adjoint of the MADE (Modal Aerosol Dynamics model for Europe) to optimise initial and boundary values for aerosols using 4Dvar. A forward and an adjoint radiative transfer model is driven by the EURAD-IM as mapping between BLAOT (Boundary Layer Aerosol Optical Thickness) and internal aerosol species. Furthermore, its condensation scheme has been bypassed by an HDMR (High-Dimensional-Model-Representation) to ensure differentiability. In this study both in-situ measured PMx as well as satellite retrieved aerosol optical thicknesses have been assimilated and the effect on forecast performance has been investigated. The source of BLAOT is the aerosol retrieval system SYNAER (SYNergetic AErosol Retrieval) from DLR-DFD that retrieves AOT by making use of both AATSR/SCIAMACHY and AVHRR/GOME-2 data respectively. Its strengths are a large spatial coverage, near real-time availability, and the classification of five intrinsic aerosol species, namely water-solubles, water-insolubles, soot, sea salt, and mineral dust which are furthermore size resolved in terms of modes. The skill of the aerosol 4Dvar system was tested in two episodes: 1) July through August 2003, a dry period with strong wildfire activity in Europe, and 2) October through November 2008, the period of the ZEPTER-2 (Second ZEPpelin based Tropospheric photochemical chemistry expERiment) measurement campaign in the area of Lake Constance. In the latter case one-way nesting has been applied from a horizontal grid resolution of 45 km down to 5 km. Overall, the results showed a significant increase in forecast quality of tropospheric aerosol loads.

AEROCAN, the Canadian sub-network of AERONET: Aerosol monitoring and air quality applications

NASA Astrophysics Data System (ADS)

Sioris, Christopher E.; Abboud, Ihab; Fioletov, Vitali E.; McLinden, Chris A.

2017-10-01

Previous studies have demonstrated the utility of AERONET (Aerosol Robotic Network) aerosol optical depth (AOD) data for monitoring the spatial variability of particulate matter (PM) in relatively polluted regions of the globe. AEROCAN, a Canadian sub-network of AERONET, was established 20 years ago and currently consists of twenty sites across the country. In this study, we examine whether the AEROCAN sunphotometer data provide evidence of anthropogenic contributions to ambient particulate matter concentrations in relatively clean Canadian locations. The similar weekly cycle of AOD and PM2.5 over Toronto provides insight into the impact of local pollution on observed AODs. High temporal correlations (up to r = 0.78) between daily mean AOD (or its fine-mode component) and PM2.5 are found at southern Ontario AEROCAN sites during May-August, implying that the variability in the aerosol load resides primarily in the boundary layer and that sunphotometers capture day-to-day PM2.5 variations at moderately polluted sites. The sensitivity of AEROCAN AOD data to anthropogenic surface-level aerosol enhancements is demonstrated using boundary-layer wind information for sites near sources of aerosol or its precursors. An advantage of AEROCAN relative to the Canadian in-situ National Air Pollution Surveillance (NAPS) network is the ability to detect free tropospheric aerosol enhancements, which can be large in the case of lofted forest fire smoke or desert dust. These aerosol plumes eventually descend to the surface, sometimes in populated areas, exacerbating air quality. In cases of large AOD (≥0.4), AEROCAN data are also useful in characterizing the aerosol type. The AEROCAN network includes three sites in the high Arctic, a region not sampled by the NAPS PM2.5 monitoring network. These polar sites show the importance of long-range transport and meteorology in the Arctic haze phenomenon. Also, AEROCAN sunphotometers are, by design and due to regular maintenance, the most valuable monitors available for long term aerosol trends. Using a variety of data analysis techniques and timescales, the usefulness of this ground-based remote-sensing sub-network for providing information relevant to air quality is demonstrated.

Year-round records of bulk and size-segregated aerosol composition in central Antarctica (Concordia site) - Part 1: Fractionation of sea-salt particles

NASA Astrophysics Data System (ADS)

Legrand, Michel; Preunkert, Susanne; Wolff, Eric; Weller, Rolf; Jourdain, Bruno; Wagenbach, Dietmar

2017-11-01

Multiple year-round records of bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located at Dome C in East Antarctica. In parallel, sampling of acidic gases on denuder tubes was carried out to quantify the concentrations of HCl and HNO3 present in the gas phase. These time series are used to examine aerosol present over central Antarctica in terms of chloride depletion relative to sodium with respect to freshly emitted sea-salt aerosol as well as depletion of sulfate relative to sodium with respect to the composition of seawater. A depletion of chloride relative to sodium is observed over most of the year, reaching a maximum of ˜ 20 ng m-3 in spring when there are still large sea-salt amounts and acidic components start to recover. The role of acidic sulfur aerosol and nitric acid in replacing chloride from sea-salt particles is here discussed. HCl is found to be around twice more abundant than the amount of chloride lost by sea-salt aerosol, suggesting that either HCl is more efficiently transported to Concordia than sea-salt aerosol or re-emission from the snow pack over the Antarctic plateau represents an additional significant HCl source. The size-segregated composition of aerosol collected in winter (from 2006 to 2011) indicates a mean sulfate to sodium ratio of sea-salt aerosol present over central Antarctica of 0.16 ± 0.05, suggesting that, on average, the sea-ice and open-ocean emissions equally contribute to sea-salt aerosol load of the inland Antarctic atmosphere. The temporal variability of the sulfate depletion relative to sodium was examined at the light of air mass backward trajectories, showing an overall decreasing trend of the ratio (i.e., a stronger sulfate depletion relative to sodium) when air masses arriving at Dome C had traveled a longer time over sea ice than over open ocean. The findings are shown to be useful to discuss sea-salt ice records extracted at deep drilling sites located inland Antarctica.

Evaluation of climate model aerosol seasonal and spatial variability over Africa using AERONET

NASA Astrophysics Data System (ADS)

Horowitz, Hannah M.; Garland, Rebecca M.; Thatcher, Marcus; Landman, Willem A.; Dedekind, Zane; van der Merwe, Jacobus; Engelbrecht, Francois A.

2017-11-01

The sensitivity of climate models to the characterization of African aerosol particles is poorly understood. Africa is a major source of dust and biomass burning aerosols and this represents an important research gap in understanding the impact of aerosols on radiative forcing of the climate system. Here we evaluate the current representation of aerosol particles in the Conformal Cubic Atmospheric Model (CCAM) with ground-based remote retrievals across Africa, and additionally provide an analysis of observed aerosol optical depth at 550 nm (AOD550 nm) and Ångström exponent data from 34 Aerosol Robotic Network (AERONET) sites. Analysis of the 34 long-term AERONET sites confirms the importance of dust and biomass burning emissions to the seasonal cycle and magnitude of AOD550 nm across the continent and the transport of these emissions to regions outside of the continent. In general, CCAM captures the seasonality of the AERONET data across the continent. The magnitude of modeled and observed multiyear monthly average AOD550 nm overlap within ±1 standard deviation of each other for at least 7 months at all sites except the Réunion St Denis Island site (Réunion St. Denis). The timing of modeled peak AOD550 nm in southern Africa occurs 1 month prior to the observed peak, which does not align with the timing of maximum fire counts in the region. For the western and northern African sites, it is evident that CCAM currently overestimates dust in some regions while others (e.g., the Arabian Peninsula) are better characterized. This may be due to overestimated dust lifetime, or that the characterization of the soil for these areas needs to be updated with local information. The CCAM simulated AOD550 nm for the global domain is within the spread of previously published results from CMIP5 and AeroCom experiments for black carbon, organic carbon, and sulfate aerosols. The model's performance provides confidence for using the model to estimate large-scale regional impacts of African aerosols on radiative forcing, but local feedbacks between dust aerosols and climate over northern Africa and the Mediterranean may be overestimated.

Signatures of Biomass Burning Aerosols in the Plume of a Saltmarsh Wildfire in South Texas.

PubMed

Myers-Pigg, Allison N; Griffin, Robert J; Louchouarn, Patrick; Norwood, Matthew J; Sterne, Amanda; Cevik, Basak Karakurt

2016-09-06

The most conventional and abundant tracers of biomass combustion in aerosol particles include potassium and biomarkers derived from thermally altered cellulose/hemicellulose (anhydrosugars) and lignin (methoxyphenols). However, little is known of the role biomass combustion plays as a particulate source of major plant polymers to the atmosphere. Here, concentrations of solvent-extractable anhydrosugars and methoxyphenols are compared to the yields of polymeric lignin oxidation products (LOPs) during a smoke plume event in Houston, Texas. Downwind aerosol samples (PM2.5) were collected surrounding a two-day wildfire in the McFaddin National Wildlife Refuge, 125 km southeast of Houston, which was 12-16 h directly downwind during the peak of the burn. Concentrations of all organic markers, potassium, and calcium increased by a factor of 2-13 within 1-2 days of the start of the fire and dropped to prefire levels 3 days after the peak event. Source signatures of anhydrosugars and methoxyphenols during the peak of the plume were identical to those of grass charcoals collected from the site, confirming the use of charcoals as end-members for source input reconstruction during atmospheric transport. An enrichment factor of 20 in the anhydrosugar to methoxyphenol ratio of aerosols versus charcoals can be explained partially by differences in degradation rate constants between the biomarker groups. LOPs comprised 73-91% of all lignin material in the aerosols, pointing to fires as major sources of primary biogenic aerosol particles in which lignin phenols occur predominantly in polymeric form.

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

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

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.

Eddy covariance measurements of sea spray particles over the Atlantic Ocean

NASA Astrophysics Data System (ADS)

Norris, S. J.; Brooks, I. M.; de Leeuw, G.; Smith, M. H.; Moerman, M.; Lingard, J. J. N.

2008-02-01

Most estimates of sea spray aerosol source functions have used indirect means to infer the rate of production as a function of wind speed. Only recently has the technology become available to make high frequency measurements of aerosol spectra suitable for direct eddy correlation determination of the sea spray particle flux. This was accomplished in this study by combining a newly developed fast aerosol particle counter with an ultrasonic anemometer which allowed for eddy covariance measurements of size-segregated particle fluxes. The aerosol instrument is the Compact Lightweight Aerosol Spectrometer Probe (CLASP) - capable of measuring 8-channel size spectra for mean radii between 0.15 and 3.5 µm at 10 Hz. The first successful measurements were made during the Waves, Air Sea Fluxes, Aerosol and Bubbles (WASFAB) field campaign in October 2005 in Duck (NC, USA). The method and initial results are presented and comparisons are made with recent sea spray source functions from the literature.

Stratospheric Aerosol and Gas Experiment (SAGE 3)

NASA Technical Reports Server (NTRS)

Mccormick, M. P.

1993-01-01

The proposed SAGE III instrument would be the principal source of data for global changes of stratospheric aerosols, stratospheric water vapor, and ozone profiles, and a contributing source of data for upper tropospheric water vapor, aerosols, and clouds. The ability to obtain such data has been demonstrated by the predecessor instrument, SAGE II, but SAGE III will be substantially more capable, as discussed below. The capabilities for monitoring the profiles of atmospheric constituents have been verified in detail, including ground-based validations, for aerosol, ozone, and water vapor. Indeed, because of its self-calibrating characteristics, SAGE II was an essential component of the international ozone trend assessments, and SAGE II is now proving to be invaluable in tracking the aerosols from Mt. Pinatubo. Although SAGE profiles generally terminate at the height of the first tropospheric cloud layer, it has been found that the measurements extend down to 3 km altitude more than 40 percent of the time at most latitudes. Thus, useful information can also be obtained on upper tropospheric aerosols, water vapor, and ozone.

Monsoonal variations in atmospheric surfactants at different coastal areas of the Malaysian Peninsula.

PubMed

Jaafar, Shoffian Amin; Latif, Mohd Talib; Razak, Intan Suraya; Shaharudin, Muhammad Zulhilmi; Khan, Md Firoz; Wahid, Nurul Bahiyah Abd; Suratman, Suhaimi

2016-08-15

This study determined the effect of monsoonal changes on the composition of atmospheric surfactants in coastal areas. The composition of anions (SO4(2-), NO3(-), Cl(-), F(-)) and the major elements (Ca, K, Mg, Na) in aerosols were used to determine the possible sources of surfactants. Surfactant compositions were determined using a colorimetric method as methylene blue active substances (MBAS) and disulphine blue active substances (DBAS). The anion and major element compositions of the aerosol samples were determined by ion chromatography (IC) and inductively coupled plasma mass spectrometry (ICP-MS), respectively. The results indicated that the concentrations of surfactant in aerosols were dominated by MBAS (34-326pmolm(-3)). Monsoonal changes were found to significantly affect the concentration of surfactants. Using principal component analysis-multiple linear regressions (PCA-MLR), major possible sources for surfactants in the aerosols were motor vehicle emissions, secondary aerosol and the combustion of biomass along with marine aerosol. Copyright © 2016 Elsevier Ltd. All rights reserved.

Aerosol physicochemical properties in relation to meteorology: Case studies in urban, marine, and arid settings

NASA Astrophysics Data System (ADS)

Wonaschuetz, Anna

Atmospheric aerosols are a highly relevant component of the climate system affecting atmospheric radiative transfer and the hydrological cycle. As opposed to other key atmospheric constituents with climatic relevance, atmospheric aerosol particles are highly heterogeneous in time and space with respect to their size, concentration, chemical composition and physical properties. Many aspects of their life cycle are not understood, making them difficult to represent in climate models and hard to control as a pollutant. Aerosol-cloud interactions in particular are infamous as a major source of uncertainty in future climate predictions. Field measurements are an important source of information for the modeling community and can lead to a better understanding of chemical and microphysical processes. In this study, field data from urban, marine, and arid settings are analyzed and the impact of meteorological conditions on the evolution of aerosol particles while in the atmosphere is investigated. Particular attention is given to organic aerosols, which are a poorly understood component of atmospheric aerosols. Local wind characteristics, solar radiation, relative humidity and the presence or absence of clouds and fog are found to be crucial factors in the transport and chemical evolution of aerosol particles. Organic aerosols in particular are found to be heavily impacted by processes in the liquid phase (cloud droplets and aerosol water). The reported measurements serve to improve the process-level understanding of aerosol evolution in different environments and to inform the modeling community by providing realistic values for input parameters and validation of model calculations.

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.

Development of a Photo-fragmentation Laser Induced Fluorescence Instrument for the Measurement of Nitrous Acid

NASA Astrophysics Data System (ADS)

Boustead, G.; Blitz, M. A.; Heard, D. E.; Ingham, T.; Stone, D. J.; Whalley, L.

2017-12-01

The hydroxyl radical (OH) is the primary oxidant in the atmosphere with its concentration determining the lifetime of many species and its reaction with volatile organic compounds (VOCs) leading to the production of secondary organic aerosols (SOA) and tropospheric ozone. Nitrous acid (HONO) is an important source of OH as it builds up overnight and is photolysed to form OH in the morning. HONO is also present during the day, with several hundred pptv observed in urban environments. Atmospheric models currently under predict the concentration of HONO observed during the day, indicating a missing source. Heterogeneous reactions on ground and aerosol surfaces are now recognised as potentially important HONO sources. To identify and quantify some of these missing heterogeneous sources, a photo-fragmentation laser induced fluorescence (PF-LIF) instrument has been developed to provide a fast and sensitive measurement of HONO. The PF-LIF instrument detects the OH fragment at 308 nm after the photolysis of HONO at 355 nm. This instrument is coupled to an aerosol flow tube and can be used to measure HONO production from aerosols under illuminated conditions. We will present an overview of the instrument and its development as well as preliminary results including the production of HONO from illuminated TiO2 aerosols.

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

NASA Astrophysics Data System (ADS)

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

2017-06-01

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

Characterization of Optical Properties of Desert Dust and Other Aerosols Using Postive Matrix Factorization

NASA Astrophysics Data System (ADS)

Lihavainen, H.; Alghamdi, M.; Hyvärinen, A.; Hussein, T.; Neitola, K.; Khoder, M.; Abdelmaksoud, A. S.; Al-Jeelani, H.; Shabbaj, I. I.; Almehmadi, F. M.

2017-12-01

To derive the comprehensive aerosol in situ characteristics at a rural background area in Saudi Arabia, an aerosol measurements station was established to Hada Al Sham, 60 km east from the Red Sea and the city of Jeddah. The present sturdy describes the observational data from February 2013 to February 2015 of scattering and absorption coefficients, Ångström exponents and single scattering albedo over the measurement period. As expected, the scattering coefficient was dominated by large desert dust particles with low Ångström scattering exponent. Especially from February to June the Ångström scattering exponent was clearly lower and scattering coefficients higher than total averages because of the dust outbreak season. Aerosol optical properties had clear diurnal cycle. The lowest scattering and absorption coefficients and aerosol optical depths were observed around noon. The observed diurnal variation is caused by wind direction and speed, during night time very calm easterly winds are dominating whereas during daytime the stronger westerly winds are dominating (sea breeze). Positive Matrix Factorization mathematical tool was applied to the scattering and absorption coefficients and PM2.5 and coarse mode (PM10- PM2.5) mass concentrations to characterise aerosols from different sources. Analysis revealed three clearly different types of sources, anthropogenic, BC source and desert dust. These factors have clearly different seasonal and diurnal variation. The contribution of desert dust factor was dominating from February to May, whereas the contribution of anthropogenic factor is quite steady over the whole year. We estimated the mass absorption and scattering efficiencies for the factors and they agreed well with earlier observations. Hence, this method could be used to distinguish aerosol source characteristics, at least in fairly simple cases.

Signatures of Biomass Burning Aerosols during a Smoke Plume Event from a Saltmarsh Wildfire in South Texas

NASA Astrophysics Data System (ADS)

Louchouarn, P.; Griffin, R. J.; Norwood, M. J.; Sterne, A. M. E.; Karakurt Cevik, B.

2014-12-01

The most conventional and abundant tracers of biomass combustion in aerosol particles include potassium and biomarkers derived from thermally altered cellulose/hemicellulose (anhydrosugars) and lignin (methoxyphenols). However, little is known of the role of biomass combustion as a particulate source of major plant polymers to the atmosphere. Here, concentrations of "free" (solvent-extractable) anhydrosugars and methoxyphenols are compared to the yields of polymeric lignin oxidation products (LOPs) during a smoke plume event in Houston, Texas. Downwind aerosol samples (PM2.5) were collected prior to, during, and following a two-day wildfire event that burned ~5,000 acres of a spartina saltmarsh ecosystem in the McFaddin National Wildlife Refuge, 125 km southeast of Houston. In addition, charcoals of the burned plants were collected within a week of the fire at the wildfire site. HYSPLIT modeling shows that Houston was directly downwind of this wildfire during the peak of the burn, with an approximate travel time from source to aerosol sampling site of 12-16 hrs. Concentrations of all organic markers, K+, and Ca2+ jumped by a factor of 2-13 within 1-2 days of the start of the fire and dropped to pre-fire levels three days after the peak event. Source signatures of anhydrosugars and free methoxyphenols during the peak of the plume were identical to those of grass charcoals collected from the site, confirming the potential use of charcoals as endmembers for source input reconstruction during atmospheric transport. An enrichment factor of 20 in the anhydrosugar to methoxyphenol ratio of aerosols vs. charcoals can partially be explained by differences in degradation rate constants between the two biomarker groups. Polymeric LOP comprised 73-91% of all lignin material in the aerosols, pointing to fires as major sources of primary biogenic aerosol particles and confirming an earlier study that lignin phenols in atmospheric particles occur predominantly in polymeric form.

Aerosol optical properties at a coastal site in Hong Kong, South China: temporal features, size dependencies and source analysis

NASA Astrophysics Data System (ADS)

Wang, Jiaping; Ding, Aijun; Virkkula, Aki; Lee, Shuncheng; Shen, Yicheng; Chi, Xuguang; Xu, Zheng

2016-04-01

Hong Kong is a typical coastal city adjacent to the Pearl River Delta (PRD) region in southern China, which is one of the regions suffering from severe air pollution. Atmospheric aerosols can affect the earth's radiative balance by scattering and absorbing incoming solar radiation. Black Carbon (BC) aerosol is a particularly emphasized component due to its strong light absorption. Aerosol transported from different source areas consists of distinct size distributions, leading to different optical properties. As the byproducts of the incomplete oxidation, BC and CO both have relatively long life time, their relationship is a good indicator for distinguishing different pollutant sources. In this study, temporal variations of aerosol optical properties and concentrations of BC and CO at a coastal background station in Hong Kong were investigated. Transport characteristics and origins of aerosol were elucidated by analyzing backward Lagrangian particle dispersion modeling (LPDM) results, together with related parameters including the relationships between optical properties and particle size, BC-CO correlations, ship location data and meteorological variables. From February 2012 to September 2013 and March 2014 to February 2015, continuous in-situ measurements of light scattering and absorption coefficients, particle size distribution and concentrations of BC and CO were conducted at Hok Tsui (HT), a coastal background station on the southeast tip of Hong Kong Island (22.22°N, 114.25°E, 60 m above the sea level) with few local anthropogenic activities. Affected by the Asian monsoon, this region is dominated by continental outflow in winter and by marine inflow from the South China Sea in summer, which is an ideal station for identifying the transport characteristics of aerosol and their effects on optical properties from different anthropogenic emission sources. 7-day backward Lagrangian particle dispersion modeling was performed for source identification. Three types of cases dominantly influenced by the PRD regional emission, long-range transport and marine exhaust were compared and discussed in detail.

Stable carbon and nitrogen isotopic compositions of ambient aerosols collected from Okinawa Island in the western North Pacific Rim, an outflow region of Asian dusts and pollutants

NASA Astrophysics Data System (ADS)

Kunwar, Bhagawati; Kawamura, Kimitaka; Zhu, Chunmao

2016-04-01

Stable carbon (δ13C) and nitrogen (δ15N) isotope ratios were measured for total carbon (TC) and nitrogen (TN), respectively, in aerosol (TSP) samples collected at Cape Hedo, Okinawa, an outflow region of Asian pollutants, during 2009-2010. The averaged δ13C and δ15N ratios are -22.2‰ and +12.5‰, respectively. The δ13C values are similar in both spring (-22.5‰) and winter (-22.5‰), suggesting the similar sources and/or source regions. We found that δ13C from Okinawa aerosols are ca. 2‰ higher than those reported from Chinese megacities probably due to photochemical aging of organic aerosols. A strong correlation (r = 0.81) was found between nss-Ca and TSP, suggesting that springtime aerosols are influenced from Asian dusts. However, carbonates in the Asian dusts were titrated with acidic species such as sulfuric acid and oxalic acid during atmospheric transport although two samples suggested the presence of remaining carbonate. No correlations were found between δ13C and tracer compounds (levoglucosan, elemental carbon, oxalic acid, and Na+). During winter and spring, coal burning is significant source in China. Based on isotopic mass balance, contribution of coal burning origin particles to total aerosol carbon was estimated as ca. 97% in winter, which is probably associated with the high emissions in China. Contribution of NO3- to TN was on average 45% whereas that of NH4+ was 18%. These results suggest that vehicular exhaust is an important source of TN in Okinawa aerosols. Concentration of water-soluble organic nitrogen (WSON) is higher in summer, suggesting that WSON is more emitted from the ocean in warmer season whereas inorganic nitrogen is more emitted in winter and spring from pollution sources in the Asian continent.

Modeling the Absorbing Aerosol Index

NASA Technical Reports Server (NTRS)

Penner, Joyce; Zhang, Sophia

2003-01-01

We propose a scheme to model the absorbing aerosol index and improve the biomass carbon inventories by optimizing the difference between TOMS aerosol index (AI) and modeled AI with an inverse model. Two absorbing aerosol types are considered, including biomass carbon and mineral dust. A priori biomass carbon source was generated by Liousse et al [1996]. Mineral dust emission is parameterized according to surface wind and soil moisture using the method developed by Ginoux [2000]. In this initial study, the coupled CCM1 and GRANTOUR model was used to determine the aerosol spatial and temporal distribution. With modeled aerosol concentrations and optical properties, we calculate the radiance at the top of the atmosphere at 340 nm and 380 nm with a radiative transfer model. The contrast of radiance at these two wavelengths will be used to calculate AI. Then we compare the modeled AI with TOMS AI. This paper reports our initial modeling for AI and its comparison with TOMS Nimbus 7 AI. For our follow-on project we will model the global AI with aerosol spatial and temporal distribution recomputed from the IMPACT model and DAO GEOS-1 meteorology fields. Then we will build an inverse model, which applies a Bayesian inverse technique to optimize the agreement of between model and observational data. The inverse model will tune the biomass burning source strength to reduce the difference between modelled AI and TOMS AI. Further simulations with a posteriori biomass carbon sources from the inverse model will be carried out. Results will be compared to available observations such as surface concentration and aerosol optical depth.

A new approach to chemically-speciated submicron aerosol fluxes over tropical and temperate forests.

NASA Astrophysics Data System (ADS)

Farmer, D. K.; Kimmel, J. R.; Nemitz, E.; Phillips, G.; Docherty, K.; Chen, Q.; Martin, S.; Cubison, M.; Jimenez, J.

2008-12-01

Aerosols play an important role in the planet's radiation balance; however, their sources and sinks remain highly uncertain. In particular, due to instrumental limitations, there are few measurements of particle fluxes over the Earth's surface. Particles are expected to deposit over forests, leading not only to an aerosol sink, but also to an ecosystem source of nutrients and acids. However, forests emit volatile organic compounds (VOCs) that are known to produce secondary organic aerosol, thus also acting as aerosol sources. We have developed a new approach to measure biosphere-atmosphere exchange of chemically-speciated aerosol using a High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS; DeCarlo et al., Anal. Chem., 2006) in a new Eddy Covariance Flux mode (10 Hz). This approach allows us to directly measure fluxes of non-refractory organic, sulphate, nitrate and ammonium in submicron particles. Measurements have been carried out over two forests: a temperate ponderosa pine plantation at Blodgett Forest (BEARPEX-I campaign, 2007) and a tropical rain forest in the Brazilian Amazon during the wet season (AMAZE campaign, 2008). Data collected at these sites allows us to demonstrate that the flux mode of the HR-ToF-AMS meets the rigorous instrumental requirements of the eddy covariance approach and that fluxes of different chemical species can be quantified. Aerosol fluxes under clean and anthropogenically-impacted conditions are compared. These measurements allow us to better constrain dry deposition over forested environments and to understand the potential of flux measurements to constrain the biogenic SOA budget.

Dust in the Sky: Atmospheric Composition. Modeling of Aerosol Optical Thickness

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Kinne, Stefan; Torres, Omar; Holben, Brent; Duncan, Bryan; Martin, Randall; Logan, Jennifer; Higurashi, Akiko; Nakajima, Teruyuki

2000-01-01

Aerosol is any small particle of matter that rests suspended in the atmosphere. Natural sources, such as deserts, create some aerosols; consumption of fossil fuels and industrial activity create other aerosols. All the microscopic aerosol particles add up to a large amount of material floating in the atmosphere. You can see the particles in the haze that floats over polluted cities. Beyond this visible effect, aerosols can actually lower temperatures. They do this by blocking, or scattering, a portion of the sun's energy from reaching the surface. Because of this influence, scientists study the physical properties of atmospheric aerosols. Reliable numerical models for atmospheric aerosols play an important role in research.

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.

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 regional pollution. Pollution episodes were mostly encountered under low winds and had a low level of α, implying aerosol absorption should be largely attributed to freshly emitted BC from local sources under such conditions. Extensive field campaigns and long-term chemical and optical measurements of light-absorbing aerosols are needed in the future to further advance our understanding on optical properties of light-absorbing aerosols and their radiative forcing in this region.

Follow the Carbon: Isotopic Labeling Studies of Early Earth Aerosol.

PubMed

Hicks, Raea K; Day, Douglas A; Jimenez, Jose L; Tolbert, Margaret A

2016-11-01

Despite the faint young Sun, early Earth might have been kept warm by an atmosphere containing the greenhouse gases CH 4 and CO 2 in mixing ratios higher than those found on Earth today. Laboratory and modeling studies suggest that an atmosphere containing these trace gases could lead to the formation of organic aerosol haze due to UV photochemistry. Chemical mechanisms proposed to explain haze formation rely on CH 4 as the source of carbon and treat CO 2 as a source of oxygen only, but this has not previously been verified experimentally. In the present work, we use isotopically labeled precursor gases and unit-mass resolution (UMR) and high-resolution (HR) aerosol mass spectrometry to examine the sources of carbon and oxygen to photochemical aerosol formed in a CH 4 /CO 2 /N 2 atmosphere. UMR results suggest that CH 4 contributes 70-100% of carbon in the aerosol, while HR results constrain the value from 94% to 100%. We also confirm that CO 2 contributes approximately 10% of the total mass to the aerosol as oxygen. These results have implications for the geochemical interpretations of inclusions found in Archean rocks on Earth and for the astrobiological potential of other planetary atmospheres. Key Words: Atmosphere-Early Earth-Planetary atmospheres-Carbon dioxide-Methane. Astrobiology 16, 822-830.

Using Long-term Satellite Observations to Identify Sensitive Regimes and Active Regions of Aerosol Indirect Effects for Liquid Clouds over Global Oceans

DOE PAGES

Zhao, Xuepeng; Liu, Yangang; Yu, Fangquan; ...

2017-11-16

Long-term (1981-2011) satellite climate data records (CDRs) of clouds and aerosols are used to investigate the aerosol-cloud interaction of marine water cloud from a climatology perspective. Our focus is on identifying the regimes and regions where the aerosol indirect effect (AIE) are evident in long-term averages over the global oceans through analyzing the correlation features between aerosol loading and the key cloud variables including cloud droplet effective radius (CDER), cloud optical depth (COD), cloud water path (CWP), cloud top height (CTH), and cloud top temperature (CTT). An aerosol optical thickness (AOT) range of 0.13 < AOT < 0.3 is identifiedmore » as the sensitive regime of the conventional first AIE where CDER is more susceptible to AOT than the other cloud variables. The first AIE that manifests as the change of long-term averaged CDER appears only in limited oceanic regions. The signature of aerosol invigoration of water clouds as revealed by the increase of cloud cover fraction (CCF) and CTH with increasing AOT at the middle/high latitudes of both hemispheres is identified for a pristine atmosphere (AOT < 0.08). Aerosol invigoration signature is also revealed by the concurrent increase of CDER, COD, and CWP with increasing AOT for a polluted marine atmosphere (AOT > 0.3) in the tropical convergence zones. The regions where the second AIE is likely to manifest in the CCF change are limited to several oceanic areas with high CCF of the warm water clouds near the western coasts of continents. The second AIE signature as represented by the reduction of the precipitation efficiency with increasing AOT is more likely to be observed in the AOT regime of 0.08 < AOT < 0.4. The corresponding AIE active regions manifested themselves as the decline of the precipitation efficiency are mainly limited to the oceanic areas downwind of continental aerosols. Furthermore, the sensitive regime of the conventional AIE identified in this observational study is likely associated with the transitional regime from the aerosol-limited regime to the updraft-limited regime identified for aerosol-cloud interaction in cloud model simulations.« less

Using Long-Term Satellite Observations to Identify Sensitive Regimes and Active Regions of Aerosol Indirect Effects for Liquid Clouds Over Global Oceans

NASA Astrophysics Data System (ADS)

Zhao, Xuepeng; Liu, Yangang; Yu, Fangquan; Heidinger, Andrew K.

2018-01-01

Long-term (1981-2011) satellite climate data records of clouds and aerosols are used to investigate the aerosol-cloud interaction of marine water cloud from a climatology perspective. Our focus is on identifying the regimes and regions where the aerosol indirect effects (AIEs) are evident in long-term averages over the global oceans through analyzing the correlation features between aerosol loading and the key cloud variables including cloud droplet effective radius (CDER), cloud optical depth (COD), cloud water path (CWP), cloud top height (CTH), and cloud top temperature (CTT). An aerosol optical thickness (AOT) range of 0.13 < AOT < 0.3 is identified as the sensitive regime of the conventional first AIE where CDER is more susceptible to AOT than the other cloud variables. The first AIE that manifests as the change of long-term averaged CDER appears only in limited oceanic regions. The signature of aerosol invigoration of water clouds as revealed by the increase of cloud cover fraction (CCF) and CTH with increasing AOT at the middle/high latitudes of both hemispheres is identified for a pristine atmosphere (AOT < 0.08). Aerosol invigoration signature is also revealed by the concurrent increase of CDER, COD, and CWP with increasing AOT for a polluted marine atmosphere (AOT > 0.3) in the tropical convergence zones. The regions where the second AIE is likely to manifest in the CCF change are limited to several oceanic areas with high CCF of the warm water clouds near the western coasts of continents. The second AIE signature as represented by the reduction of the precipitation efficiency with increasing AOT is more likely to be observed in the AOT regime of 0.08 < AOT < 0.4. The corresponding AIE active regions manifested themselves as the decline of the precipitation efficiency are mainly limited to the oceanic areas downwind of continental aerosols. The sensitive regime of the conventional AIE identified in this observational study is likely associated with the transitional regime from the aerosol-limited regime to the updraft-limited regime identified for aerosol-cloud interaction in cloud model simulations.

Using Long-Term Satellite Observations to Identify Sensitive Regimes and Active Regions of Aerosol Indirect Effects for Liquid Clouds Over Global Oceans.

PubMed

Zhao, Xuepeng; Liu, Yangang; Yu, Fangquan; Heidinger, Andrew K

2018-01-16

Long-term (1981-2011) satellite climate data records of clouds and aerosols are used to investigate the aerosol-cloud interaction of marine water cloud from a climatology perspective. Our focus is on identifying the regimes and regions where the aerosol indirect effects (AIEs) are evident in long-term averages over the global oceans through analyzing the correlation features between aerosol loading and the key cloud variables including cloud droplet effective radius (CDER), cloud optical depth (COD), cloud water path (CWP), cloud top height (CTH), and cloud top temperature (CTT). An aerosol optical thickness (AOT) range of 0.13 < AOT < 0.3 is identified as the sensitive regime of the conventional first AIE where CDER is more susceptible to AOT than the other cloud variables. The first AIE that manifests as the change of long-term averaged CDER appears only in limited oceanic regions. The signature of aerosol invigoration of water clouds as revealed by the increase of cloud cover fraction (CCF) and CTH with increasing AOT at the middle/high latitudes of both hemispheres is identified for a pristine atmosphere (AOT < 0.08). Aerosol invigoration signature is also revealed by the concurrent increase of CDER, COD, and CWP with increasing AOT for a polluted marine atmosphere (AOT > 0.3) in the tropical convergence zones. The regions where the second AIE is likely to manifest in the CCF change are limited to several oceanic areas with high CCF of the warm water clouds near the western coasts of continents. The second AIE signature as represented by the reduction of the precipitation efficiency with increasing AOT is more likely to be observed in the AOT regime of 0.08 < AOT < 0.4. The corresponding AIE active regions manifested themselves as the decline of the precipitation efficiency are mainly limited to the oceanic areas downwind of continental aerosols. The sensitive regime of the conventional AIE identified in this observational study is likely associated with the transitional regime from the aerosol-limited regime to the updraft-limited regime identified for aerosol-cloud interaction in cloud model simulations.

Using Long-term Satellite Observations to Identify Sensitive Regimes and Active Regions of Aerosol Indirect Effects for Liquid Clouds over Global Oceans

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

Zhao, Xuepeng; Liu, Yangang; Yu, Fangquan

Long-term (1981-2011) satellite climate data records (CDRs) of clouds and aerosols are used to investigate the aerosol-cloud interaction of marine water cloud from a climatology perspective. Our focus is on identifying the regimes and regions where the aerosol indirect effect (AIE) are evident in long-term averages over the global oceans through analyzing the correlation features between aerosol loading and the key cloud variables including cloud droplet effective radius (CDER), cloud optical depth (COD), cloud water path (CWP), cloud top height (CTH), and cloud top temperature (CTT). An aerosol optical thickness (AOT) range of 0.13 < AOT < 0.3 is identifiedmore » as the sensitive regime of the conventional first AIE where CDER is more susceptible to AOT than the other cloud variables. The first AIE that manifests as the change of long-term averaged CDER appears only in limited oceanic regions. The signature of aerosol invigoration of water clouds as revealed by the increase of cloud cover fraction (CCF) and CTH with increasing AOT at the middle/high latitudes of both hemispheres is identified for a pristine atmosphere (AOT < 0.08). Aerosol invigoration signature is also revealed by the concurrent increase of CDER, COD, and CWP with increasing AOT for a polluted marine atmosphere (AOT > 0.3) in the tropical convergence zones. The regions where the second AIE is likely to manifest in the CCF change are limited to several oceanic areas with high CCF of the warm water clouds near the western coasts of continents. The second AIE signature as represented by the reduction of the precipitation efficiency with increasing AOT is more likely to be observed in the AOT regime of 0.08 < AOT < 0.4. The corresponding AIE active regions manifested themselves as the decline of the precipitation efficiency are mainly limited to the oceanic areas downwind of continental aerosols. Furthermore, the sensitive regime of the conventional AIE identified in this observational study is likely associated with the transitional regime from the aerosol-limited regime to the updraft-limited regime identified for aerosol-cloud interaction in cloud model simulations.« less

Diurnal and seasonal trends and source apportionment of redox-active metals in Los Angeles using a novel online metal monitor and Positive Matrix Factorization (PMF)

NASA Astrophysics Data System (ADS)

Mousavi, Amirhosein; Sowlat, Mohammad H.; Sioutas, Constantinos

2018-02-01

In the present study, we identified the sources of four redox-active metals, including Iron (Fe), Chromium (Cr), Cupper (Cu), and Manganese (Mn) and quantified the contribution of these sources to PM2.5 concentrations in central Los Angeles, California, by employing time-resolved measurements (i.e., a time resolution of 2 h) with a recently developed online metal monitor and Positive Matrix Factorization (PMF). Size distribution of ambient PM (14 nm-10 μm) was measured using the Scanning Mobility Particle Sizer (SMPS) and Optical Particle Sizer (OPS). Auxiliary variables were also collected, including elemental (EC) and organic carbon (OC), gaseous pollutants (NO2 and O3), meteorological parameters (including relative humidity (RH) and temperature), and traffic data (for heavy- (HDVs) and light-duty vehicles (LDVs)). A 4-factor solution was found to be optimum for the chemically-speciated dataset, whereas a 5-factor solution appeared to be most plausible for the size distribution data. The factors included fresh traffic, soil/road dust, urban background aerosol, secondary aerosol, and nucleation (only resolved for the size distribution data). Fresh traffic was the major contributor to Fe and Cu concentrations, whereas Cr was mostly found in the urban background aerosol (reflecting a mixture of small local sources as well as aged traffic emissions), and Mn mostly came from both soil/road dust and was to a lesser degree found in urban background aerosol. Secondary aerosol did not contribute to the concentrations of any of these metals, but was associated with very high loading of OC, as expected. Even though the urban background aerosol and secondary aerosol appeared to be characterized by "aged" particles and have a rather homogeneous spatial distribution, the reactions and processes involved in their formation are entirely different. Our results provide insights into the sources of redox-active metals in central Los Angeles. They also underscore the benefits of novel measurement techniques for PM-bound metals, which could enhance our understanding of the sources of atmospheric aerosols by providing us with measurements with finer time resolutions that otherwise would not have been possible using traditional filter-based measurement techniques.

The relationship between aerosol particles chemical composition and optical properties to identify the biomass burning contribution to fine particles concentration: a case study for São Paulo city, Brazil.

PubMed

de Miranda, Regina Maura; Lopes, Fabio; do Rosário, Nilton Évora; Yamasoe, Marcia Akemi; Landulfo, Eduardo; de Fatima Andrade, Maria

2016-12-01

The air quality in the Metropolitan Area of São Paulo (MASP) is primarily determined by the local pollution source contribution, mainly the vehicular fleet, but there is a concern about the role of remote sources to the fine mode particles (PM 2.5 ) concentration and composition. One of the most important remote sources of atmospheric aerosol is the biomass burning emissions from São Paulo state's inland and from the central and north portions of Brazil. This study presents a synergy of different measurements of atmospheric aerosol chemistry and optical properties in the MASP in order to show how they can be used as a tool to identify particles from local and remote sources. For the clear identification of the local and remote source contribution, aerosol properties measurements at surface level were combined with vertical profiles information. Over 15 days in the austral winter of 2012, particulate matter (PM) was collected using a cascade impactor and a Partisol sampler in São Paulo City. Mass concentrations were determined by gravimetry, black carbon concentrations by reflectance, and trace element concentrations by X-ray fluorescence. Aerosol optical properties were studied using a multifilter rotating shadowband radiometer (MFRSR), a Lidar system and satellite data. Optical properties, concentrations, size distributions, and elemental composition of atmospheric particles were strongly related and varied according to meteorological conditions. During the sampling period, PM mean mass concentrations were 17.4 ± 10.1 and 15.3 ± 6.9 μg/m 3 for the fine and coarse fractions, respectively. The mean aerosol optical depths at 415 nm and Ångström exponent (AE) over the whole period were 0.29 ± 0.14 and 1.35 ± 0.11, respectively. Lidar ratios reached values of 75 sr. The analyses of the impacts of an event of biomass burning smoke transport to the São Paulo city revealed significant changing on local aerosol concentrations and optical parameters. The identification of the source contributions, local and remote, to the fine particles in MASP can be more precisely achieved when particle size composition and distribution, vertical profile of aerosols, and air mass trajectories are analyzed in combination.

Biomass burning dominates brown carbon absorption in the rural southeastern United States

NASA Astrophysics Data System (ADS)

Washenfelder, R. A.; Attwood, A. R.; Brock, C. A.; Guo, H.; Xu, L.; Weber, R. J.; Ng, N. L.; Allen, H. M.; Ayres, B. R.; Baumann, K.; Cohen, R. C.; Draper, D. C.; Duffey, K. C.; Edgerton, E.; Fry, J. L.; Hu, W. W.; Jimenez, J. L.; Palm, B. B.; Romer, P.; Stone, E. A.; Wooldridge, P. J.; Brown, S. S.

2015-01-01

carbon aerosol consists of light-absorbing organic particulate matter with wavelength-dependent absorption. Aerosol optical extinction, absorption, size distributions, and chemical composition were measured in rural Alabama during summer 2013. The field site was well located to examine sources of brown carbon aerosol, with influence by high biogenic organic aerosol concentrations, pollution from two nearby cities, and biomass burning aerosol. We report the optical closure between measured dry aerosol extinction at 365 nm and calculated extinction from composition and size distribution, showing agreement within experiment uncertainties. We find that aerosol optical extinction is dominated by scattering, with single-scattering albedo values of 0.94 ± 0.02. Black carbon aerosol accounts for 91 ± 9% of the total carbonaceous aerosol absorption at 365 nm, while organic aerosol accounts for 9 ± 9%. The majority of brown carbon aerosol mass is associated with biomass burning, with smaller contributions from biogenically derived secondary organic aerosol.

Impact of the ozone monitoring instrument row anomaly on the long-term record of aerosol products

NASA Astrophysics Data System (ADS)

Torres, Omar; Bhartia, Pawan K.; Jethva, Hiren; Ahn, Changwoo

2018-05-01

Since about three years after the launch the Ozone Monitoring Instrument (OMI) on the EOS-Aura satellite, the sensor's viewing capability has been affected by what is believed to be an internal obstruction that has reduced OMI's spatial coverage. It currently affects about half of the instrument's 60 viewing positions. In this work we carry out an analysis to assess the effect of the reduced spatial coverage on the monthly average values of retrieved aerosol optical depth (AOD), single scattering albedo (SSA) and the UV Aerosol Index (UVAI) using the 2005-2007 three-year period prior to the onset of the row anomaly. Regional monthly average values calculated using viewing positions 1 through 30 were compared to similarly obtained values using positions 31 through 60, with the expectation of finding close agreement between the two calculations. As expected, mean monthly values of AOD and SSA obtained with these two scattering-angle dependent subsets of OMI observations agreed over regions where carbonaceous or sulphate aerosol particles are the predominant aerosol type. However, over arid regions, where desert dust is the main aerosol type, significant differences between the two sets of calculated regional mean values of AOD were observed. As it turned out, the difference in retrieved desert dust AOD between the scattering-angle dependent observation subsets was due to the incorrect representation of desert dust scattering phase function. A sensitivity analysis using radiative transfer calculations demonstrated that the source of the observed AOD bias was the spherical shape assumption of desert dust particles. A similar analysis in terms of UVAI yielded large differences in the monthly mean values for the two sets of calculations over cloudy regions. On the contrary, in arid regions with minimum cloud presence, the resulting UVAI monthly average values for the two sets of observations were in very close agreement. The discrepancy under cloudy conditions was found to be caused by the parameterization of clouds as opaque Lambertian reflectors. When properly accounting for cloud scattering effects using Mie theory, the observed UVAI angular bias was significantly reduced. The analysis discussed here has uncovered important algorithmic deficiencies associated with the model representation of the angular dependence of scattering effects of desert dust aerosols and cloud droplets. The resulting improvements in the handling of desert dust and cloud scattering have been incorporated in an improved version of the OMAERUV algorithm.

Non-refractory PM1 in SE Asia: Chemically speciated aerosol fluxes and concentrations above contrasting land-uses in SE Asia.

NASA Astrophysics Data System (ADS)

Phillips, Gavin; Farmer, Delphine; di Marco, Chiara; Misztal, Pawel; Sueper, Donna; Kimmel, Joel; Jimenez, Jose; Fowler, David; Nemitz, Eiko

2010-05-01

New measurements of VOC emissions (measured with leaf cuvettes, and ecosystem fluxes obtained from eddy covariance measurements) suggest that oil palm (Elaeis guineensis Jacq) is a significantly larger source of isoprene than tropical forest, in Borneo. These larger sources of isoprene measured over oil palm, allied with a larger anthropogenic component of local emissions, contrasts with the composition of the atmosphere in the semi-remote tropical forest environment. The difference in the atmospheric composition above different land-uses has the potential to lead to contrasting chemistry and physics controlling the formation and processing of particulate matter. Thus land use changes, driven by the economics of biofuels, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions, chemical processing and composition of organic aerosol over both (semi-)natural and anthropogenic land uses in the tropical environment. Ecosystem flux measurements of chemically-speciated non-refractory PM1 were made over two contrasting land uses in the Malaysian state of Sabah, on the island of Borneo during 2008. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at the Global Atmospheric Watch (GAW) site at a tropical rain forest location as well as the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as a collaboration between three UK NERC funded projects (OP3, APPRAISE/ACES and DIASPORA). Recent technical developments using ToF detectors allow us to record 10 Hz full mass spectra at both high resolution (HR) and unit-mass resolution (UMR), suitable for the calculation of local eddy-covariance fluxes. The measurements provide information on the deposition rate of anthropogenic aerosol components (e.g. sulphate, nitrate, ammonium and hydrocarbon-like aerosol) to tropical forest and oil palm. At the same time, any biogenic secondary organic aerosol components formed through fast chemistry below the measurement height would appear as an upward flux, and the direct flux measurement therefore provides an alternative approach to probing BSOA formation mechanisms. In particular, through the calculation of mass spectra in terms of flux and deposition velocity those masses and aerosol fragments can be identified that show similar behaviour. In addition, the contribution of the various chemical species (e.g. nitrate, sulphate, OA sub-types) to the total mass flux will be elucidated.

Using radiocarbon to constrain black and organic carbon aerosol sources in Salt Lake City

NASA Astrophysics Data System (ADS)

Mouteva, Gergana O.; Randerson, James T.; Fahrni, Simon M.; Bush, Susan E.; Ehleringer, James R.; Xu, Xiaomei; Santos, Guaciara M.; Kuprov, Roman; Schichtel, Bret A.; Czimczik, Claudia I.

2017-09-01

Black carbon (BC) and organic carbon (OC) aerosols are important components of fine particulate matter (PM2.5) in polluted urban environments. Quantifying the contribution of fossil fuel and biomass combustion to BC and OC concentrations is critical for developing and validating effective air quality control measures and climate change mitigation policy. We used radiocarbon (14C) to measure fossil and contemporary biomass contributions to BC and OC at three locations in Salt Lake City, Utah, USA, during 2012-2014, including during winter inversion events. Aerosol filters were analyzed with the Swiss_4S thermal-optical protocol to isolate BC. We measured fraction modern (fM) of BC and total carbon in PM2.5 with accelerator mass spectrometry and derived the fM of OC using isotope mass balance. Combined with 14C information of end-member composition, our data set of 31 14C aerosol measurements provided a baseline of the fossil and contemporary biomass components of carbonaceous aerosol. We show that fossil fuels were the dominant source of carbonaceous aerosol during winter, contributing 88% (80-98%) of BC and 58% (48-69%) of OC. While the concentration of both BC and OC increased during inversion events, the relative source contributions did not change. The sources of BC also did not vary throughout the year, while OC had a considerably higher contemporary biomass component in summer at 62% (49-76%) and was more variable. Our results suggest that in order to reduce PM2.5 levels in Salt Lake City to meet national standards, a more stringent policy targeting mobile fossil fuel sources may be necessary.

The impact of biogenic carbon emissions on aerosol absorption inMexico City

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

Marley, N; Gaffney, J; Tackett, M J

2009-02-24

In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbingmore » secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.« less

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.

Direct Radiative Effects of Aerosols Over South Asia From Observations and Modeling

NASA Technical Reports Server (NTRS)

Nair, Vijayakumar S.; Babu, S. Suresh; Manoj, M. R.; Moorthy, Krishna K.; Chin, Mian

2016-01-01

Quantitative assessment of the seasonal variations in the direct radiative effect (DRE) of composite aerosols as well as the constituent species over the Indian sub continent has been carried out using a synergy of observations from a dense network of ground based aerosol observatories and modeling based on chemical transport model simulations. Seasonal variation of aerosol constituents depict significant influence of anthropogenic aerosol sources in winter and the dominance of natural sources in spring, even though the aerosol optical depth doesn't change significantly between these two seasons. A significant increase in the surface cooling and atmospheric warming has been observed as season changes from winter DRE(sub SUR) = -28 +/- 12 W m(exp -2) and DRE(sub ATM) = +19.6 +/- 9 W m(exp -2) to spring DRE(sub SUR) = -33.7 +/- 12 W m(exp -2) and DRE(sub ATM) = +27 +/- 9 W m(exp-2). Interestingly, springtime aerosols are more absorptive in nature compared to winter and consequently the aerosol induced diabatic heating of the atmosphere goes as high as approximately 1 K day(exp -1) during spring, especially over eastern India. The atmospheric DRE due to dust aerosols (+14 +/- 7 W m(exp 2) during spring overwhelms that of black carbon DRE (+11.8 +/- 6 W m(exp -2) during winter. The DRE at the top of the atmosphere is mostly governed by the anthropogenic aerosols during all the seasons. The columnar aerosol loading, its anthropogenic fraction and radiative effects shows a steady increase with latitude across Indian mainland leading to a larger aerosol-induced atmospheric warming during spring than in winter.

Remote sensing for studying atmospheric aerosols in Malaysia

NASA Astrophysics Data System (ADS)

Kanniah, Kasturi D.; Kamarul Zaman, Nurul A. F.

2015-10-01

The aerosol system is Southeast Asia is complex and the high concentrations are due to population growth, rapid urbanization and development of SEA countries. Nevertheless, only a few studies have been carried out especially at large spatial extent and on a continuous basis to study atmospheric aerosols in Malaysia. In this review paper we report the use of remote sensing data to study atmospheric aerosols in Malaysia and document gaps and recommend further studies to bridge the gaps. Satellite data have been used to study the spatial and seasonal patterns of aerosol optical depth (AOD) in Malaysia. Satellite data combined with AERONET data were used to delineate different types and sizes of aerosols and to identify the sources of aerosols in Malaysia. Most of the aerosol studies performed in Malaysia was based on station-based PM10 data that have limited spatial coverage. Thus, satellite data have been used to extrapolate and retrieve PM10 data over large areas by correlating remotely sensed AOD with ground-based PM10. Realising the critical role of aerosols on radiative forcing numerous studies have been conducted worldwide to assess the aerosol radiative forcing (ARF). Such studies are yet to be conducted in Malaysia. Although the only source of aerosol data covering large region in Malaysia is remote sensing, satellite observations are limited by cloud cover, orbital gaps of satellite track, etc. In addition, relatively less understanding is achieved on how the atmospheric aerosol interacts with the regional climate system. These gaps can be bridged by conducting more studies using integrated approach of remote sensing, AERONET and ground based measurements.

Direct radiative effects of aerosols over South Asia from observations and modeling

NASA Astrophysics Data System (ADS)

Nair, Vijayakumar S.; Babu, S. Suresh; Manoj, M. R.; Moorthy, K. Krishna; Chin, Mian

2017-08-01

Quantitative assessment of the seasonal variations in the direct radiative effect (DRE) of composite aerosols as well as the constituent species over the Indian sub continent has been carried out using a synergy of observations from a dense network of ground based aerosol observatories and modeling based on chemical transport model simulations. Seasonal variation of aerosol constituents depict significant influence of anthropogenic aerosol sources in winter and the dominance of natural sources in spring, even though the aerosol optical depth doesn't change significantly between these two seasons. A significant increase in the surface cooling and atmospheric warming has been observed as season changes from winter (DRESUR = -28 ± 12 W m-2 and DREATM = +19.6 ± 9 W m-2) to spring (DRESUR = -33.7 ± 12 W m-2 and DREATM = +27 ± 9 W m-2). Interestingly, springtime aerosols are more absorptive in nature compared to winter and consequently the aerosol induced diabatic heating of the atmosphere goes as high as 1 K day-1 during spring, especially over eastern India. The atmospheric DRE due to dust aerosols (+14 ± 7 W m-2) during spring overwhelms that of black carbon DRE (+11.8 ± 6 W m-2) during winter. The DRE at the top of the atmosphere is mostly governed by the anthropogenic aerosols during all the seasons. The columnar aerosol loading, its anthropogenic fraction and radiative effects shows a steady increase with latitude across Indian mainland leading to a larger aerosol-induced atmospheric warming during spring than in winter.

Spatial and temporal variations of aerosols around Beijing in summer 2006: Model evaluation and source apportionment

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Kita, K.; Miyazaki, Y.; Hu, M.; Chang, S.; Blake, D. R.; Fast, J. D.; Zaveri, R. A.; Streets, D. G.; Zhang, Q.; Zhu, T.

2009-12-01

Regional aerosol model calculations were made using the WRF-CMAQ and WRF-chem models to study spatial and temporal variations of aerosols around Beijing, China, in the summer of 2006, when the CAREBEIJING-2006 intensive campaign was conducted. Model calculations captured temporal variations of primary (such as elemental carbon, EC) and secondary (such as sulfate) aerosols observed in and around Beijing. The spatial distributions of aerosol optical depth observed by the MODIS satellite sensors were also reproduced over northeast China. Model calculations showed distinct differences in spatial distributions between primary and secondary aerosols in association with synoptic-scale meteorology. Secondary aerosols increased in air around Beijing on a scale of about 1000 x 1000 km2 under an anticyclonic pressure system. This airmass was transported northward from the high anthropogenic emission area extending south of Beijing with continuous photochemical production. Subsequent cold front passage brought clean air from the north, and polluted air around Beijing was swept to the south of Beijing. This cycle was repeated about once a week and was found to be responsible for observed enhancements/reductions of aerosols at the intensive measurement sites. In contrast to secondary aerosols, the spatial distributions of primary aerosols (EC) reflected those of emissions, resulting in only slight variability despite the changes in synoptic-scale meteorology. In accordance with these results, source apportionment simulations revealed that primary aerosols around Beijing were controlled by emissions within 100 km around Beijing within the preceding 24 hours, while emissions as far as 500 km and within the preceding 3 days were found to affect secondary aerosols.

Short-term modulation of Indian summer monsoon rainfall by West Asian dust

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

Vinoj, V.; Rasch, Philip J.; Wang, Hailong

The Indian summer monsoon is the result of a complex interplay between radiative heating, dynamics and cloud and aerosol interactions. Despite increased scientific attention, the effect of aerosols on monsoons still remains uncertain. Here we present both observational evidence and numerical modeling results demonstrating a remote aerosol link to Indian summer monsoon rainfall. Rainfall over central India is positively correlated to natural aerosols over the Arabian Sea and West Asia. Simulations using a state-of-the-art global climate model support this remote aerosol link and indicate that dust aerosols induce additional moisture transport and convergence over Central India, producing increased monsoon rainfall.more » The convergence is driven through solar heating and latent heating within clouds over West Asia that increases surface winds over the Arabian Sea. On the other hand, sea-salt aerosol tends to counteract the effect of dust and reduces rainfall. Our findings highlight the importance of natural aerosols in modulating the strength of the Indian summer monsoon, and motivate additional research in how changes in background aerosols of natural origin may be influencing long-term trends in monsoon precipitation.« less

Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy

NASA Astrophysics Data System (ADS)

Saarikoski, S.; Carbone, S.; Decesari, S.; Giulianelli, L.; Angelini, F.; Canagaratna, M.; Ng, N. L.; Trimborn, A.; Facchini, M. C.; Fuzzi, S.; Hillamo, R.; Worsnop, D.

2012-09-01

The chemistry of submicron particles was investigated at San Pietro Capofiume (SPC) measurement station in the Po Valley, Italy, in spring 2008. The measurements were performed by using both off-line and on-line instruments. Organic carbon (OC) and elemental carbon, organic acids and biomass burning tracers were measured off-line by using a 24-h PM1 filter sampling. More detailed particle chemistry was achieved by using a Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and analyzing the data by positive matrix factorization (PMF). Oxalic acid had the highest concentrations of organic acids (campaign-average 97.4 ng m-3) followed by methane sulfonic, formic, malonic, and malic acids. Samples were also analyzed for glyoxylic, succinic, azelaic and maleic acids. In total, the nine acids composed 1.9 and 3.8% of OC and water-soluble OC, respectively (average), in terms of carbon atoms. Levoglucosan concentration varied from 17.7 to 495 ng m-3 with the concentration decreasing in the course of the campaign most likely due to the reduced use of domestic heating with wood. Six factors were found for organic aerosol (OA) at SPC by PMF: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), nitrogen-containing OA (N-OA) and three different oxygenated OAs (OOA-a, OOA-b and OOA-c). Most of the OA mass was composed of OOA-a, HOA and OOA-c (26, 24 and 22%, respectively) followed by OOA-b (13%), BBOA (8%) and N-OA (7%). As expected, OOAs were the most oxygenated factors with organic matter:organic carbon (OM : OC) ratios ranging from 1.9 to 2.2. The diurnal variability of the aerosol chemical composition was greatly affected by the boundary layer meteorology. Specifically, the effect of the nocturnal layer break-up in morning hours was most evident for nitrate and N-OA indicating that these compounds originated mainly from the local sources in the Po Valley. For sulfate and OOA-a the concentration did not change during the break-up suggesting their origin to be mostly regional. That resulted in much more oxidized OA in the daytime mixing layer than in the nocturnal surface layer. In this study, the high mass resolution and source-related aerosol chemistry from the HR-ToF-AMS was combined with the filter measurements in a total new extent elucidating novel features and sources of organic aerosol in the Po Valley region.

Chemical characterization of springtime submicrometer aerosol in Po Valley, Italy

NASA Astrophysics Data System (ADS)

Saarikoski, S.; Carbone, S.; Decesari, S.; Giulianelli, L.; Angelini, F.; Teinilä, K.; Canagaratna, M.; Ng, N. L.; Trimborn, A.; Facchini, M. C.; Fuzzi, S.; Hillamo, R.; Worsnop, D.

2012-03-01

The chemistry of submicron particles was investigated at San Pietro Capofiume (SPC) measurement station in the Po Valley, Italy, in spring 2008. The measurements were performed by using both off-line and on-line instruments. Organic carbon (OC) and elemental carbon, organic acids and biomass burning tracers were measured off-line by using a 24-h PM1 filter sampling. More detailed particle chemistry was achieved by using an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and analyzing the data by positive matrix factorization (PMF). Oxalic acid had the highest concentrations of organic acids (campaign-average 97.4 ng m-3) followed by methane sulfonic, formic, malonic, and malic acids. Samples were also analyzed for glyoxylic, succinic, azelaic and maleic acids. In total, the nine acids composed 1.9 and 3.8% of OC and water-soluble OC, respectively (average), in terms of carbon atoms. Levoglucosan concentration varied from 17.7 to 495 ng m-3 with the concentration decreasing in the course of the campaign most likely due to the reduced use of domestic heating with wood. Six factors were found for organic aerosol (OA) at SPC by PMF: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), nitrogen-containing OA (N-OA) and three different oxygenated OAs (OOA-a, OOA-b and OOA-c). Most of the OA mass was composed of OOA-a, HOA and OOA-c (26, 24 and 22%, respectively) followed by OOA-b (13%), BBOA (8%) and N-OA (7%). As expected, OOAs were the most oxygenated factors with organic matter:organic carbon (OM:OC) ratios ranging from 1.9 to 2.2. The diurnal variability of the aerosol chemical composition was greatly affected by the boundary layer meteorology. Specifically, the effect of the nocturnal layer break-up in morning hours was most evident for nitrate and N-OA indicating that these compounds originated mainly from the local sources in the Po Valley. For sulfate and OOA-a the concentration did not change during the break-up suggesting their origin to be mostly regional. That resulted in much more oxidized OA in the daytime mixing layer than in the nocturnal surface layer. In this study, the high mass resolution and source-related aerosol chemistry from the HR-ToF-AMS was combined with the filter measurements in a total new extent elucidating novel features and sources of organic aerosol in the Po Valley region.

Long-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga

NASA Astrophysics Data System (ADS)

Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A. V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M. O.

2013-12-01

Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23-36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007-2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7-11 ng m-3 ppb-1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m-3 ppb-1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.

Performance of personal inhalable aerosol samplers in very slowly moving air when facing the aerosol source.

PubMed

Witschger, O; Grinshpun, S A; Fauvel, S; Basso, G

2004-06-01

While personal aerosol samplers have been characterized primarily based on wind tunnel tests conducted at relatively high wind speeds, modern indoor occupational environments are usually represented by very slow moving air. Recent surveys suggest that elevated levels of occupational exposure to inhalable airborne particles are typically observed when the worker, operating in the vicinity of the dust source, faces the source. Thus, the first objective of this study was to design and test a new, low cost experimental protocol for measuring the sampling efficiency of personal inhalable aerosol samplers in the vicinity of the aerosol source when the samplers operate in very slowly moving air. In this system, an aerosol generator, which is located in the centre of a room-sized non-ventilated chamber, continuously rotates and omnidirectionally disperses test particles of a specific size. The test and reference samplers are equally distributed around the source at the same distance from the centre and operate in parallel (in most of our experiments, the total number of simultaneously operating samplers was 15). Radial aerosol transport is driven by turbulent diffusion and some natural convection. For each specific particle size and the sampler, the aerosol mass concentration is measured by weighing the collection filter. The second objective was to utilize the new protocol to evaluate three widely used aerosol samplers: the IOM Personal Inhalable Sampler, the Button Personal Inhalable Aerosol Sampler and the 25 mm Millipore filter holder (closed-face C25 cassette). The sampling efficiencies of each instrument were measured with six particle fractions, ranging from 6.9 to 76.9 micro m in their mass median aerodynamic diameter. The Button Sampler efficiency data demonstrated a good agreement with the standard inhalable convention and especially with the low air movement inhalabilty curve. The 25 mm filter holder was found to considerably under-sample the particles larger than 10 micro m; its efficiency did not exceed 7% for particles of 40-100 micro m. The IOM Sampler facing the source was found to over-sample compared with the data obtained previously with a slowly rotating, freely suspended sampler in a low air movement environment. It was also found that the particle wall deposition in the IOM metallic cartridge was rather significant and particle size-dependent. For each sampler (IOM, Button and C25) the precision was characterized through the relative standard deviation (RSD) of the aerosol concentration obtained with identical samplers in a specific experiment. The average RSD was 14% for the IOM Sampler, 11% for the Button Sampler and 35% for the 25 mm filter cassette. A separate set of experiments, performed with the Simplified Torso showed that in very slowly moving air a personal sampler can be adequately evaluated even when it is not attached to a body but freely suspended (confirming the data reported previously).

Direct measurements of near-highway emissions in a high diesel environment

NASA Astrophysics Data System (ADS)

DeWitt, H. L.; Hellebust, S.; Temime-Roussel, B.; Ravier, S.; Polo, L.; Jacob, V.; Buisson, C.; Charron, A.; André, M.; Pasquier, A.; Besombes, J. L.; Jaffrezo, J. L.; Wortham, H.; Marchand, N.

2014-10-01

Diesel-powered passenger cars currently outnumber gasoline-powered cars in many countries, particularly in Europe. In France, diesel cars represented 61% of Light Duty Vehicles in 2011 and this percentage is still increasing (French Environment and Energy Management Agency, ADEME). As part of the September~2011 joint PM-DRIVE (Particulate Matter- DiRect and Indirect on-road Vehicular Emissions) and MOCOPO (Measuring and mOdeling traffic COngestion and POllution) field campaign, the concentration and high-resolution chemical composition of aerosols and volatile organic carbon (VOC) species were measured adjacent to a major urban highway south of Grenoble, France. Alongside these atmospheric measurements, detailed traffic data were collected from nearby traffic cameras and loop detectors, which allowed the identification of vehicle type and characteristics, traffic concentration, and traffic speed to be quantified and compared to measured aerosol and VOCs. Six aerosol age and source profiles were resolved using the positive matrix factorization (PMF) model on real-time high-resolution aerosol mass spectra. These six aerosol source/age categories included a hydrocarbon-like organic aerosol (HOA) commonly associated with primary vehicular emissions, a nitrogen containing aerosol (NOA) with a diurnal pattern similar to that of HOA, oxidized organic aerosol (OOA), and biomass burning aerosol (BBOA). While quantitatively separating the influence of diesel vs. gasoline proved impossible, a low HOA : black carbon ratio, similar to that measured in other high-diesel environments, and high levels of NOx, also indicative of diesel emissions, were observed. A comparison between these high-diesel environment measurements and measurements taken in low-diesel (North American) environments was examined and the potential feedback between vehicular emissions and SOA formation was probed. Although the measurement site was located next to a large source of primary emissions, which are typically found to have low oxygen incorporation, OOA was found to comprise the majority of the measured organic aerosol, and the measured OOA contained mainly modern carbon, not fossil-derived carbon. Thus, even in this heavily vehicular-emission impacted environment, photochemical processes, biogenic emissions, and aerosol oxidation dominated the overall organic aerosol mass measured during most of the campaign.

Aplication of LIRIC algorithm to study aerosol transport over Belsk, Poland

NASA Astrophysics Data System (ADS)

Pietruczuk, Aleksander; Posyniak, Michał

2015-04-01

In this work synergy of measurements done by of a LIDAR and a sun-sky scanning photometer is presented. The LIdar-Radiometer Inversion Code (LIRIC) was applied to study periodic events of increased values of the aerosol optical depth (AOD) observed at Belsk (Poland). Belsk is a background site located in a rural area around 50 km south from Warsaw. Events of increased AOD occur mainly during spring and they coincide with events of elevated concentrations of particulate matter (PM10). This phenomenon is observed in all eastern Europe, e.g. in Minsk, and is caused by long range aerosol transport. Our previous work showed aerosol transport from the border between Belarus, Ukraine and Russia in the planetary boundary layer (PBL), and from north Africa in the free troposphere. The LIRIC algorithm, which uses optical and microphysical properties of the aerosol derived from photometric measurements and LIDAR profiles, was applied to study vertical distribution of fine and coarse modes of aerosol. The analysis of the airmass backward trajectories and models results (DREAM and NAAPS)was also used to determine a possible aerosol type and its source region. This study proved our previous findings. Most of events with increased AODs are observed during spring. In this season the fine mode aerosol is mainly present in the PBL. On the basis of the trajectory analysis and the NAAPS results we presume that it is the absorbing aerosol originating from the regions of seasonal biomass burning in eastern Europe, i.e. the area mentioned above. The events with increased AODs were also found during summer. In this case the fine mode aerosol is transported in the PBL a like to spring season. However, our analysis of trajectories and model results indicated western Europe as a source region. It is probably urban/industrial aerosol. The coarse mode aerosol is transported mainly in the free troposphere as separate layers. The analysis of backward trajectories indicates northern Africa as a possible source region regardless the season. DREAM and NAAPS results suggest presence of mineral dust in this case over Belsk.

Resolving anthropogenic aerosol pollution types - deconvolution and exploratory classification of pollution events

NASA Astrophysics Data System (ADS)

Äijälä, Mikko; Heikkinen, Liine; Fröhlich, Roman; Canonaco, Francesco; Prévôt, André S. H.; Junninen, Heikki; Petäjä, Tuukka; Kulmala, Markku; Worsnop, Douglas; Ehn, Mikael

2017-03-01

Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesizing this raw data into chemical information necessitates the use of advanced, statistics-based data analytical techniques. In the field of analytical aerosol chemistry, statistical, dimensionality reductive methods have become widespread in the last decade, yet comparable advanced chemometric techniques for data classification and identification remain marginal. Here we present an example of combining data dimensionality reduction (factorization) with exploratory classification (clustering), and show that the results cannot only reproduce and corroborate earlier findings, but also complement and broaden our current perspectives on aerosol chemical classification. We find that applying positive matrix factorization to extract spectral characteristics of the organic component of air pollution plumes, together with an unsupervised clustering algorithm, k-means+ + , for classification, reproduces classical organic aerosol speciation schemes. Applying appropriately chosen metrics for spectral dissimilarity along with optimized data weighting, the source-specific pollution characteristics can be statistically resolved even for spectrally very similar aerosol types, such as different combustion-related anthropogenic aerosol species and atmospheric aerosols with similar degree of oxidation. In addition to the typical oxidation level and source-driven aerosol classification, we were also able to classify and characterize outlier groups that would likely be disregarded in a more conventional analysis. Evaluating solution quality for the classification also provides means to assess the performance of mass spectral similarity metrics and optimize weighting for mass spectral variables. This facilitates algorithm-based evaluation of aerosol spectra, which may prove invaluable for future development of automatic methods for spectra identification and classification. Robust, statistics-based results and data visualizations also provide important clues to a human analyst on the existence and chemical interpretation of data structures. Applying these methods to a test set of data, aerosol mass spectrometric data of organic aerosol from a boreal forest site, yielded five to seven different recurring pollution types from various sources, including traffic, cooking, biomass burning and nearby sawmills. Additionally, three distinct, minor pollution types were discovered and identified as amine-dominated aerosols.

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

DOE PAGES

Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; ...

2016-11-25

Here, we present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arrangedmore » into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on other bulk aerosol components commonly observed by the AMS.« less

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

NASA Astrophysics Data System (ADS)

Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.

2016-11-01

We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography-mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on other bulk aerosol components commonly observed by the AMS.

Insights into Submicron Aerosol Composition and Sources from the WINTER Aircraft Campaign Over the Eastern US.

NASA Astrophysics Data System (ADS)

Schroder, J. C.; Campuzano Jost, P.; Day, D. A.; Fibiger, D. L.; McDuffie, E. E.; Blake, N. J.; Hills, A. J.; Hornbrook, R. S.; Apel, E. C.; Weinheimer, A. J.; Campos, T. L.; Brown, S. S.; Jimenez, J. L.

2015-12-01

The WINTER aircraft campaign was a recent field experiment to probe the sources and evolution of gas pollutants and aerosols in Northeast US urban and industrial plumes during the winter. A highly customized Aerodyne aerosol mass spectrometer (AMS) was flown on the NCAR C-130 to characterize submicron aerosol composition and evolution. Thirteen research flights were conducted covering a wide range of conditions, including rural, urban, and marine environments during day and night. Organic aerosol (OA) was a large component of the submicron aerosol in the boundary layer. The fraction of OA (fOA) was smaller (35-40%) than in recent US summer campaigns (~60-70%). Biomass burning was observed to be an important source of OA in the boundary layer, which is consistent with recent wintertime studies that show a substantial contribution of residential wood burning to the OA loadings. OA oxygenation (O/C ratio) shows a broad distribution with a substantial fraction of smaller O/C ratios when compared to previous summertime campaigns. Since measurements were rarely made very close to primary sources (i.e. directly above urban areas), this is consistent with oxidative chemistry being slower during winter. SOA formation and aging in the NYC plume was observed during several flights and compared with summertime results from LA (CalNex) and Mexico City (MILAGRO). Additionally, an oxidation flow reactor (OFR) capable of oxidizing ambient air up to several equivalent days of oxidation was deployed for the first time in an aircraft platform. The aerosol outflow of the OFR was sampled with the AMS to provide real-time snapshots of the potential for aerosol formation and aging. For example, a case study of a flight through the Ohio River valley showed evidence of oxidation of SO2 to sulfate. The measured sulfate enhancements were in good agreement with our OFR chemical model. OFR results for SOA will be discussed.

Long-term visibility variation in Athens (1931-2013): a proxy for local and regional atmospheric aerosol loads

NASA Astrophysics Data System (ADS)

Founda, Dimitra; Kazadzis, Stelios; Mihalopoulos, Nikolaos; Gerasopoulos, Evangelos; Lianou, Maria; Raptis, Panagiotis I.

2016-09-01

This study explores the interdecadal variability and trends of surface horizontal visibility at the urban area of Athens from 1931 to 2013, using the historical archives of the National Observatory of Athens (NOA). A prominent deterioration of visibility in the city was detected, with the long-term linear trend amounting to -2.8 km decade-1 (p < 0.001), over the entire study period. This was not accompanied by any significant trend in relative humidity or precipitation over the same period. A slight recovery of visibility levels seems to be established in the recent decade (2004-2013). It was found that very good visibility (> 20 km) occurred at a frequency of 34 % before the 1950s, while this percentage drops to just 2 % during the decade 2004-2013. The rapid impairment of the visual air quality in Athens around the 1950s points to the increased levels of air pollution on a local and/or regional scale, related to high urbanization rates and/or increased anthropogenic emissions on a global scale at that period. Visibility was found to be negatively/positively correlated with relative humidity/wind speed, the correlation being statistically valid at certain periods. Wind regime and mainly wind direction and corresponding air mass origin were found to highly control visibility levels in Athens. The comparison of visibility variation in Athens and at a non-urban reference site on Crete island revealed similar negative trends over the common period of observations. This suggests that apart local sources, visibility in Athens is highly determined by aerosol load of regional origin. AVHRR and MODIS satellite-derived aerosol optical depth (AOD) retrievals over Athens and surface measurements of PM10 confirmed the relation of visibility to aerosol load.

Global and Regional Temperature-change Potentials for Near-term Climate Forcers

NASA Technical Reports Server (NTRS)

Collins, W.J.; Fry, M.M.; Yu, H.; Fuglestvedt, J. S.; Shindell, D. T.; West, J. J.

2013-01-01

We examine the climate effects of the emissions of near-term climate forcers (NTCFs) from 4 continental regions (East Asia, Europe, North America and South Asia) using results from the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model simulations. We address 3 aerosol species (sulphate, particulate organic matter and black carbon) and 4 ozone precursors (methane, reactive nitrogen oxides (NOx), volatile organic compounds and carbon monoxide). We calculate the global climate metrics: global warming potentials (GWPs) and global temperature change potentials (GTPs). For the aerosols these metrics are simply time-dependent scalings of the equilibrium radiative forcings. The GTPs decrease more rapidly with time than the GWPs. The aerosol forcings and hence climate metrics have only a modest dependence on emission region. The metrics for ozone precursors include the effects on the methane lifetime. The impacts via methane are particularly important for the 20 yr GTPs. Emissions of NOx and VOCs from South Asia have GWPs and GTPs of higher magnitude than from the other Northern Hemisphere regions. The analysis is further extended by examining the temperature-change impacts in 4 latitude bands, and calculating absolute regional temperature-change potentials (ARTPs). The latitudinal pattern of the temperature response does not directly follow the pattern of the diagnosed radiative forcing. We find that temperatures in the Arctic latitudes appear to be particularly sensitive to BC emissions from South Asia. The northern mid-latitude temperature response to northern mid-latitude emissions is approximately twice as large as the global average response for aerosol emission, and about 20-30% larger than the global average for methane, VOC and CO emissions.

Aging of biogenic secondary organic aerosol via gas-phase OH radical reactions

PubMed Central

Donahue, Neil M.; Henry, Kaytlin M.; Mentel, Thomas F.; Kiendler-Scharr, Astrid; Spindler, Christian; Bohn, Birger; Brauers, Theo; Dorn, Hans P.; Fuchs, Hendrik; Tillmann, Ralf; Wahner, Andreas; Saathoff, Harald; Naumann, Karl-Heinz; Möhler, Ottmar; Leisner, Thomas; Müller, Lars; Reinnig, Marc-Christopher; Hoffmann, Thorsten; Salo, Kent; Hallquist, Mattias; Frosch, Mia; Bilde, Merete; Tritscher, Torsten; Barmet, Peter; Praplan, Arnaud P.; DeCarlo, Peter F.; Dommen, Josef; Prévôt, Andre S.H.; Baltensperger, Urs

2012-01-01

The Multiple Chamber Aerosol Chemical Aging Study (MUCHACHAS) tested the hypothesis that hydroxyl radical (OH) aging significantly increases the concentration of first-generation biogenic secondary organic aerosol (SOA). OH is the dominant atmospheric oxidant, and MUCHACHAS employed environmental chambers of very different designs, using multiple OH sources to explore a range of chemical conditions and potential sources of systematic error. We isolated the effect of OH aging, confirming our hypothesis while observing corresponding changes in SOA properties. The mass increases are consistent with an existing gap between global SOA sources and those predicted in models, and can be described by a mechanism suitable for implementation in those models. PMID:22869714

Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

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

Kleinman, L.I.; Daum, P. H.; Lee, Y.-N.

2011-06-21

During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO{sub 2} from Cu smeltersmore » and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25% of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50% of aerosol with D{sub p} > 110 nm were not activated, the difference between the two approaches possibly representing shattered cloud droplets or unknown artifact. CDNC and interstitial aerosol were anti-correlated in all cloud transects, consistent with the occurrence of dry in-cloud areas due to entrainment or circulation mixing.« less

Aerosol Chemical Speciation Monitor (ACSM) Instrument Handbook

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

Watson, Thomas B.

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) measures particle mass loading and chemical composition in real time for non-refractory sub-micron aerosol particles. The ACSM is designed for long-term unattended deployment and routine monitoring applications.

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

EPA Science Inventory

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

Aerosol Absorption Effects in the TOMS UV Algorithm

NASA Technical Reports Server (NTRS)

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

2004-01-01

The availability of global long-term estimates of surface UV radiation is very important, not only for preventive medicine considerations, but also as an important tool to monitor the effects of the stratospheric ozone recovery expected to occur in the next few decades as a result of the decline of the stratospheric chlorine levels. In addition to the modulating effects of ozone and clouds, aerosols also affect the levels of UV-A and W-B radiation reaching the surface. Oscillations in surface W associated with the effects of aerosol absorption may be comparable in magnitude to variations associated with the stratospheric ozone recovery. Thus, the accurate calculation of surface W radiation requires that both the scattering and absorption effects of tropospheric aerosols be taken into account. Although absorption effects of dust and elevated carbonaceous aerosols are already accounted for using Aerosol Index technique, this approach does not work for urban/industrial aerosols in the planetary boundary layer. The use of the new TOMS long-term global data record on UV aerosol absorption optical depth, can improve the accuracy of TOMS spectral UV products, by properly including the spectral attenuation effects of carbonaceous, urban/industrial and mineral aerosols. The TOMS data set on aerosol properties will be discussed, and results of its use in the TOMS surface W algorithm will be presented.

Molecular marker characterization and source appointment of particulate matter and its organic aerosols.

PubMed

Choi, Jong-Kyu; Ban, Soo-Jin; Kim, Yong-Pyo; Kim, Yong-Hee; Yi, Seung-Muk; Zoh, Kyung-Duk

2015-09-01

This study was carried out to identify possible sources and to estimate their contribution to total suspended particle (TSP) organic aerosol (OA) contents. A total of 120 TSP and PM2.5 samples were collected simultaneously every third day over a one-year period in urban area of Incheon, Korea. High concentration in particulate matters (PM) and its components (NO3(-), water soluble organic compounds (WSOCs), and n-alkanoic acids) were observed during the winter season. Among the organics, n-alkanes, n-alkanoic acids, levoglucosan, and phthalates were major components. Positive matrix factorization (PMF) analysis identified seven sources of organic aerosols including combustion 1 (low molecular weight (LMW)-polycyclic aromatic hydrocarbons (PAHs)), combustion 2 (high molecular weight (HMW)-PAHs), biomass burning, vegetative detritus (n-alkane), secondary organic aerosol 1 (SOA1), secondary organic aerosol 2 (SOA2), and motor vehicles. Vegetative detritus increased during the summer season through an increase in biogenic/photochemical activity, while most of the organic sources were prominent in the winter season due to the increases in air pollutant emissions and atmospheric stability. The correlation factors were high among the main components of the organic carbon (OC) in the TSP and PM2.5. The results showed that TSP OAs had very similar characteristics to the PM2.5 OAs. SOA, combustion (PAHs), and motor vehicle were found to be important sources of carbonaceous PM in this region. Our results imply that molecular markers (MMs)-PMF model can provide useful information on the source and characteristics of PM. Copyright © 2015 Elsevier Ltd. All rights reserved.

Marine biogenic source of atmospheric organic nitrogen in the subtropical North Atlantic

PubMed Central

Altieri, Katye E.; Fawcett, Sarah E.; Peters, Andrew J.; Sigman, Daniel M.; Hastings, Meredith G.

2016-01-01

Global models estimate that the anthropogenic component of atmospheric nitrogen (N) deposition to the ocean accounts for up to a third of the ocean’s external N supply and 10% of anthropogenic CO2 uptake. However, there are few observational constraints from the marine atmospheric environment to validate these findings. Due to the paucity of atmospheric organic N data, the largest uncertainties related to atmospheric N deposition are the sources and cycling of organic N, which is 20–80% of total N deposition. We studied the concentration and chemical composition of rainwater and aerosol organic N collected on the island of Bermuda in the western North Atlantic Ocean over 18 mo. Here, we show that the water-soluble organic N concentration ([WSON]) in marine aerosol is strongly correlated with surface ocean primary productivity and wind speed, suggesting a marine biogenic source for aerosol WSON. The chemical composition of high-[WSON] aerosols also indicates a primary marine source. We find that the WSON in marine rain is compositionally different from that in concurrently collected aerosols, suggesting that in-cloud scavenging (as opposed to below-cloud “washout”) is the main contributor to rain WSON. We conclude that anthropogenic activity is not a significant source of organic N to the marine atmosphere over the North Atlantic, despite downwind transport from large pollution sources in North America. This, in conjunction with previous work on ammonium and nitrate, leads to the conclusion that only 27% of total N deposition to the global ocean is anthropogenic, in contrast to the 80% estimated previously. PMID:26739561

Isotopic evidence for enhanced fossil fuel sources of aerosol ammonium in the urban atmosphere.

PubMed

Pan, Yuepeng; Tian, Shili; Liu, Dongwei; Fang, Yunting; Zhu, Xiaying; Gao, Meng; Gao, Jian; Michalski, Greg; Wang, Yuesi

2018-07-01

The sources of aerosol ammonium (NH 4 + ) are of interest because of the potential of NH 4 + to impact the Earth's radiative balance, as well as human health and biological diversity. Isotopic source apportionment of aerosol NH 4 + is challenging in the urban atmosphere, which has excess ammonia (NH 3 ) and where nitrogen isotopic fractionation commonly occurs. Based on year-round isotopic measurements in urban Beijing, we show the source dependence of the isotopic abundance of aerosol NH 4 + , with isotopically light (-33.8‰) and heavy (0 to +12.0‰) NH 4 + associated with strong northerly winds and sustained southerly winds, respectively. On an annual basis, 37-52% of the initial NH 3 concentrations in urban Beijing arises from fossil fuel emissions, which are episodically enhanced by air mass stagnation preceding the passage of cold fronts. These results provide strong evidence for the contribution of non-agricultural sources to NH 3 in urban regions and suggest that priority should be given to controlling these emissions for haze regulation. This study presents a carefully executed application of existing stable nitrogen isotope measurement and mass-balance techniques to a very important problem: understanding source contributions to atmospheric NH 3 in Beijing. This question is crucial to informing environmental policy on reducing particulate matter concentrations, which are some of the highest in the world. However, the isotopic source attribution results presented here still involve a number of uncertain assumptions and they are limited by the incomplete set of chemical and isotopic measurements of gas NH 3 and aerosol NH 4 + . Further field work and lab experiments are required to adequately characterize endmember isotopic signatures and the subsequent isotopic fractionation process under different air pollution and meteorological conditions. Copyright © 2018 Elsevier Ltd. All rights reserved.

North Atlantic Aerosol Properties and Direct Radiative Effects: Key Results from TARFOX and ACE-2

NASA Technical Reports Server (NTRS)

Russell, P. B.; Livingston, J. M.; Schmid, B.; Bergstrom, Robert A.; Hignett, P.; Hobbs, P. V.; Durkee, P. A.

2000-01-01

Aerosol effects on atmospheric radiative fluxes provide a forcing function that can change the climate In potentially significant ways. This aerosol radiative forcing is a major source of uncertainty in understanding the observed climate change of the past century and in predicting future climate. To help reduce this uncertainty, the International Global Atmospheric Chemistry Project (IGAC) has endorsed a series of multiplatform aerosol field campaigns. The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the second Aerosol Characterization Experiment (ACE-2) were the first IGAC campaigns to address the impact of anthropogenic aerosols, Both TARFOX and ACE-2 gathered extensive data sets on aerosol properties and radiative effects, TARFOX focused on the urban-industrial haze plume flowing from the eastern United States over the western Atlantic Ocean, whereas ACE-2 studied aerosols carried over the eastern Atlantic from both European urban/industrial and African mineral sources. These aerosols often have a marked influence on the top-of-atmosphere radiances measured by satellites. Shown there are contours of aerosol optical depth derived from radiances measured by the AVHRR sensor on the NOAA-11 satellite. The contours readily show that aerosols originating in North America, Europe, and Africa impact the radiative properties of air over the North Atlantic. However, the accurate derivation of flux changes, or radiative forcing, from the satellite measured radiances or retrieved optical depths remains a difficult challenge. In this paper we summarize key initial results from TARFOX and, to a lesser extent, ACE-2, with a focus on those results that allow an improved assessment of the flux changes caused by North Atlantic aerosols at middle latitudes.

Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

NASA Technical Reports Server (NTRS)

DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.;

Known and Newly Identified Semi-Volatile Organic Compounds from Biomass Burning in Amazonia: Variability and Relationship to Aerosol Physical Properties

NASA Astrophysics Data System (ADS)

Wernis, R. A.; Yee, L.; Isaacman-VanWertz, G. A.; Kreisberg, N. M.; de Sá, S. S.; Liu, Y.; Martin, S. T.; Alexander, M. L. L.; Palm, B. B.; Hu, W.; Campuzano-Jost, P.; Day, D. A.; Jimenez, J. L.; Artaxo, P.; Viegas, J.; Manzi, A. O.; Souza, R. A. F. D.; Hering, S. V.; Goldstein, A. H.

2016-12-01

Aerosols are a source of great uncertainty in radiative forcing predictions and have poorly understood impacts on human health. In many environments, biomass burning contributes a significant source of primary aerosol as well as reactive gas-phase precursors that can form secondary organic aerosol (SOA). One class of these precursors, semi-volatile organic compounds (SVOCs), has been shown to have a large contribution to the amount of SOA formed from fire emissions. At present, SVOC emissions from biomass burning are poorly constrained and understanding their contributions to SOA formation is an important research challenge. In the Amazonian dry season, biomass burning is a major source of gases and aerosols reducing regional air quality. As part of the GoAmazon 2014/5 field campaign, we deployed the Semi-Volatile Thermal desorption Aerosol Gas Chromatograph (SV-TAG) instrument at the rural T3 site, 60 km to the west of Manaus, Brazil to measure hourly concentrations of SVOCs in the gas and particle phases. This comprehensive technique detects thousands of compounds, enabling the discovery of previously unidentified compounds. In this work we explore compounds for which a correlation with well-known biomass burning tracers is observed to discover the identities of new markers. We discuss contributions to the total organic aerosol from over 30 well-known, rarely reported and newly identified biomass burning markers. We examine the relationship between biomass burning aerosol composition and aerosol physical properties as measured at the T3 site. Additionally, we report gas-particle partitioning of all identified compounds with comparison to theoretical predictions. We find that the commonly used biomass burning tracer levoglucosan existed entirely in the particle phase and contributed 0.6% and 0.3% of total organic aerosol mass in the dry and wet seasons, respectively.

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

NASA Astrophysics Data System (ADS)

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

2016-04-01

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

A Global Aerosol Model Forecast for the ACE-Asia Field Experiment

NASA Technical Reports Server (NTRS)

Chin, Mian; Ginoux, Paul; Lucchesi, Robert; Huebert, Barry; Weber, Rodney; Anderson, Tad; Masonis, Sarah; Blomquist, Byron; Bandy, Alan; Thornton, Donald

2003-01-01

We present the results of aerosol forecast during the Aerosol Characterization Experiment (ACE-Asia) field experiment in spring 2001, using the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model and the meteorological forecast fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). The aerosol model forecast provides direct information on aerosol optical thickness and concentrations, enabling effective flight planning, while feedbacks from measurements constantly evaluate the model, making successful model improvements. We verify the model forecast skill by comparing model predicted total aerosol extinction, dust, sulfate, and SO2 concentrations with those quantities measured by the C-130 aircraft during the ACE-Asia intensive operation period. The GEOS DAS meteorological forecast system shows excellent skills in predicting winds, relative humidity, and temperature for the ACE-Asia experiment area as well as for each individual flight, with skill scores usually above 0.7. The model is also skillful in forecast of pollution aerosols, with most scores above 0.5. The model correctly predicted the dust outbreak events and their trans-Pacific transport, but it constantly missed the high dust concentrations observed in the boundary layer. We attribute this missing dust source to the desertification regions in the Inner Mongolia Province in China, which have developed in recent years but were not included in the model during forecasting. After incorporating the desertification sources, the model is able to reproduce the observed high dust concentrations at low altitudes over the Yellow Sea. Two key elements for a successful aerosol model forecast are correct source locations that determine where the emissions take place, and realistic forecast winds and convection that determine where the aerosols are transported. We demonstrate that our global model can not only account for the large-scale intercontinental transport, but also produce the small-scale spatial and temporal variations that are adequate for aircraft measurements planning.

Technical note: Intercomparison of three AATSR Level 2 (L2) AOD products over China

NASA Astrophysics Data System (ADS)

Che, Yahui; Xue, Yong; Mei, Linlu; Guang, Jie; She, Lu; Guo, Jianping; Hu, Yincui; Xu, Hui; He, Xingwei; Di, Aojie; Fan, Cheng

2016-08-01

One of four main focus areas of the PEEX initiative is to establish and sustain long-term, continuous, and comprehensive ground-based, airborne, and seaborne observation infrastructure together with satellite data. The Advanced Along-Track Scanning Radiometer (AATSR) aboard ENVISAT is used to observe the Earth in dual view. The AATSR data can be used to retrieve aerosol optical depth (AOD) over both land and ocean, which is an important parameter in the characterization of aerosol properties. In recent years, aerosol retrieval algorithms have been developed both over land and ocean, taking advantage of the features of dual view, which can help eliminate the contribution of Earth's surface to top-of-atmosphere (TOA) reflectance. The Aerosol_cci project, as a part of the Climate Change Initiative (CCI), provides users with three AOD retrieval algorithms for AATSR data, including the Swansea algorithm (SU), the ATSR-2ATSR dual-view aerosol retrieval algorithm (ADV), and the Oxford-RAL Retrieval of Aerosol and Cloud algorithm (ORAC). The validation team of the Aerosol-CCI project has validated AOD (both Level 2 and Level 3 products) and AE (Ångström Exponent) (Level 2 product only) against the AERONET data in a round-robin evaluation using the validation tool of the AeroCOM (Aerosol Comparison between Observations and Models) project. For the purpose of evaluating different performances of these three algorithms in calculating AODs over mainland China, we introduce ground-based data from CARSNET (China Aerosol Remote Sensing Network), which was designed for aerosol observations in China. Because China is vast in territory and has great differences in terms of land surfaces, the combination of the AERONET and CARSNET data can validate the L2 AOD products more comprehensively. The validation results show different performances of these products in 2007, 2008, and 2010. The SU algorithm performs very well over sites with different surface conditions in mainland China from March to October, but it slightly underestimates AOD over barren or sparsely vegetated surfaces in western China, with mean bias error (MBE) ranging from 0.05 to 0.10. The ADV product has the same precision with a low root mean square error (RMSE) smaller than 0.2 over most sites and the same error distribution as the SU product. The main limits of the ADV algorithm are underestimation and applicability; underestimation is particularly obvious over the sites of Datong, Lanzhou, and Urumchi, where the dominant land cover is grassland, with an MBE larger than 0.2, and the main aerosol sources are coal combustion and dust. The ORAC algorithm has the ability to retrieve AOD at different ranges, including high AOD (larger than 1.0); however, the stability deceases significantly with increasing AOD, especially when AOD > 1.0. In addition, the ORAC product is consistent with the CARSNET product in winter (December, January, and February), whereas other validation results lack matches during winter.

Chemical transport model simulations of organic aerosol in southern California: model evaluation and gasoline and diesel source contributions

EPA Science Inventory

Gasoline- and diesel-fueled engines are ubiquitous sources of air pollution in urban environments. They emit both primary particulate matter and precursor gases that react to form secondary particulate matter in the atmosphere. In this work, we updated the organic aerosol module ...

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 observations. The Incremental Analysis Update (IAU) is added to the model forecast tendencies to align them with the analysis every six hours, thus preventing longer timescale feedbacks due to the aerosol forcing. We calculate the SDE by comparing model runs with and without aerosols, and the difference in the IAU between these runs is a useful metric with which to evaluate the impact of the SDE on the model atmosphere and clouds. Decreasing the IAU indicates that the aerosol direct and semi-direct effects act to reduce the bias between the model and observations and vice versa.

Assessment of carbonaceous aerosols in Shanghai, China - Part 1: long-term evolution, seasonal variations, and meteorological effects

NASA Astrophysics Data System (ADS)

Chang, Yunhua; Deng, Congrui; Cao, Fang; Cao, Chang; Zou, Zhong; Liu, Shoudong; Lee, Xuhui; Li, Jun; Zhang, Gan; Zhang, Yanlin

2017-08-01

Carbonaceous aerosols are major chemical components of fine particulate matter (PM2. 5) with major impacts on air quality, climate change, and human health. Gateway to fast-rising China and home of over twenty million people, Shanghai throbs as the nation's largest mega city and the biggest industrial hub. From July 2010 to December 2014, hourly mass concentrations of ambient organic carbon (OC) and elemental carbon (EC) in the PM2. 5 fraction were quasi-continuously measured in Shanghai's urban center. The annual OC and EC concentrations (mean ±1σ) in 2013 (8.9 ± 6.2 and 2.6 ± 2.1 µg m-3, n = 5547) and 2014 (7.8 ± 4.6 and 2.1 ± 1.6 µg m-3, n = 6914) were higher than those of 2011 (6.3 ± 4.2 and 2.4 ± 1.8 µg m-3, n = 8039) and 2012 (5.7 ± 3.8 and 2.0 ± 1.6 µg m-3, n = 4459). We integrated the results from historical field measurements (1999-2012) and satellite observations (2003-2013), concluding that carbonaceous aerosol pollution in Shanghai has gradually reduced since 2006. In terms of monthly variations, average OC and EC concentrations ranged from 4.0 to 15.5 and from 1.4 to 4.7 µg m-3, accounting for 13.2-24.6 and 3.9-6.6 % of the seasonal PM2. 5 mass (38.8-94.1 µg m-3), respectively. The concentrations of EC (2.4, 2.0, 2.2, and 3.0 µg m-3 in spring, summer, fall, and winter, respectively) showed little seasonal variation (except in winter) and weekend-weekday dependence, indicating EC is a relatively stable constituent of PM2. 5 in the Shanghai urban atmosphere. In contrast to OC (7.3, 6.8, 6.7, and 8.1 µg m-3 in spring, summer, fall, and winter, respectively), EC showed marked diurnal cycles and correlated strongly with CO across all seasons, confirming vehicular emissions as the dominant source of EC at the targeted site. Our data also reveal that both OC and EC showed concentration gradients as a function of wind direction (WD) and wind speed (WS), generally with higher values associated with winds from the southwest, west, and northwest. This was consistent with their higher potential as source areas, as determined by the potential source contribution function (PSCF) analysis. A common high-potential source area, located along the middle and lower reaches of the Yangtze River instead of northern China, was pinpointed during all seasons. These results demonstrate that the measured carbonaceous aerosols were driven by the interplay of local emissions and regional transport.

A smog chamber study coupling a photoionization aerosol electron/ion spectrometer to VUV synchrotron radiation: organic and inorganic-organic mixed aerosol analysis

NASA Astrophysics Data System (ADS)

Baeza-Romero, María Teresa; Gaie-Levrel, Francois; Mahjoub, Ahmed; López-Arza, Vicente; Garcia, Gustavo A.; Nahon, Laurent

2016-07-01

A reaction chamber was coupled to a photoionization aerosol time-of-flight mass spectrometer based on an electron/ion coincidence scheme and applied for on-line analysis of organic and inorganic-organic mixed aerosols using synchrotron tunable vacuum ultraviolet (VUV) photons as the ionization source. In this proof of principle study, both aerosol and gas phase were detected simultaneously but could be differentiated. Present results and perspectives for improvement for this set-up are shown in the study of ozonolysis ([O3] = 0.13-3 ppm) of α-pinene (2-3 ppm), and the uptake of glyoxal upon ammonium sulphate. In this work the ozone concentration was monitored in real time, together with the particle size distributions and chemical composition, the latter taking advantage of the coincidence spectrometer and the tuneability of the synchrotron radiation as a soft VUV ionization source.

Development of Atmospheric Chemistry-Aerosol Transport Model for Bioavailable Iron From Dust and Combustion Source

NASA Astrophysics Data System (ADS)

Ito, A.; Feng, Y.

2009-12-01

An accurate prediction of bioavailable iron fraction for ocean biota is hampered by uncertainties in modeling soluble iron fractions in atmospheric aerosols. It has been proposed that atmospheric processing of mineral aerosols by anthropogenic pollutants may be a key pathway to transform insoluble iron into soluble forms. The dissolution of dust minerals strongly depends on solution pH, which is sensitive to the heterogeneous uptake of soluble gases by the dust particle. Due to the complexity, previous model assessments generally use a common assumption in thermodynamical equilibrium between gas and aerosol phases. Here, we compiled an emission inventory of iron from combustion and dust source, and incorporated a dust iron dissolution scheme in a global chemistry-aerosol transport model (IMPACT). We will examine and discuss the uncertainties in estimation of dissolved iron as well as comparisons of the model results with available observations.

From OLS to VIIRS, an overview of nighttime satellite aerosol retrievals using artificial light sources

NASA Astrophysics Data System (ADS)

Zhang, J.; Miller, S. D.; Reid, J. S.; Hyer, E. J.; McHardy, T. M.

2015-12-01

Compared to abundant daytime satellite-based observations of atmospheric aerosol, observations at night are relatively scarce. In particular, conventional satellite passive imaging radiometers, which offer expansive swaths of spatial coverage compared to non-scanning lidar systems, lack sensitivity to most aerosol types via the available thermal infrared bands available at night. In this talk, we make the fundamental case for the importance of nighttime aerosol information in forecast models, and the need to mitigate the existing nocturnal gap. We review early attempts at estimating nighttime aerosol optical properties using the modulation of stable artificial surface lights. Initial algorithm development using DMSP Operational Linescan System (OLS) has graduated to refined techniques based on the Suomi-NPP Visible Infrared Imaging Radiometer Suite (VIIRS) Day/Night Band (DNB). We present examples of these retrievals for selected cases and compare the results to available surface-based point-source validation data.

Semi-continuous measurement and characteristics of water-soluble organic carbon and ions of PM2.5 aerosol with PILS-TOC-IC in Baengnyeong Island

NASA Astrophysics Data System (ADS)

Kang, S.; Kim, K.; Park, G.; Ban, J.; Park, D.; Bae, M. S.; Shin, H. J.; Lee, M.; Seo, Y.; Choi, J.; Jung, D.; Seo, S.; Lee, T.; Kim, D. S.

2016-12-01

Aerosols have an important effect from scattering and absorbing the solar energy and indirectly by acting as cloud condensation nuclei and also some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. In various experimental results were showed that organic compounds have an important fraction from 10 to 70% of the total aerosol mass. Organic carbon contains water-soluble organic carbon (WSOC) and water insoluble organic carbon. WSOC are involved in the most unknown liquid-phase chemistry of wet aerosol and clouds. It is also worked as cloud condensation nuclei (CCN). Formation of secondary organic aerosol by chemical reaction of hydrocarbon compounds is a source of main pollution of WSOC compounds. Study of pollution source of WSOC is important method for creation process of secondary organic aerosol that completely has not studied.Analysis of WSOC is important and need to real-time measurement system for definition of chemical cause and sources. In this study, Particle-into-liquid sampler (PILS) coupled with total organic carbon (TOC) analyser and ion chromatography (PILS-TOC-IC), was used for semi-continuous measurement of WSOC and ionic compounds of PM2.5 during April-June 2016 at Baengnyeong Island Atmospheric Research Center, operated by the Korea National Institute of Environmental Research (NIER). PILS-TOC-IC can provide chemical information about real-time changes from ions composition and concentrations of WSOC and ionic compounds.

[Composition and source of atmosphere aerosol water soluble ions over the East China Sea in winter].

PubMed

He, Yu-Hui; Yang, Gui-Peng; Zhang, Hong-Hai

2011-08-01

With the ion chromatographic method, the water-soluble ion concentrations of Cl(-), NO3(-), SO4(2-) , CH3SO3(-) (MSA), Na+, K+, NH4+, Mg2+ and Ca2+ in the atmospheric aerosol over the East China Sea in winter 2009 was determined and the sources of these ions was investigated through correlation analysis by SPSS (statistical package for social sciences) software. The results indicated that the concentrations of secondary ions in aerosol were the highest (non-sea-salt sulfates nss-SO4(2-), NO3(-), NH4+), accounting for 78.4% of total determining ions. The calculation results of equivalent concentration of anions and cations showed that the acid ions of aerosol were neutralized inadequately. The stoichiometry of NH4+ in different compounds showed that NH4HSO4 was the main binding form of NH4+ and SO4(2-) in the aerosol. The concentration of methanesulfonic acid (MSA) was low, and the average value was (0.0088 +/- 0.0037) microg x m(-3). According to calculation, the contribution of sea-salt sulfates was 4.5% to total sulfates, and that of biogenous sulfates was 1.4% to non-sea-salt sulfate (nss-SO4(2-)), showing that human input was the main source of sulfates in aerosol over the East China Sea. In addition, nss-SO4(2-)/NO3(-) in the aerosol was 1.08, reflecting that China's energy structure adjustment played an important role in recent years.

Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

2015-11-01

To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since airflow into eastern China during the Asian Monsoon generally prevents transport of emissions eastward to the Korean Peninsula. Concentrations of the m/z 60 AMS biomass burning marker were more abundant in autumn, when transport patterns appeared to bring some smoke from fires in northern Asia to the island.

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.