Aerosol and Cloud Interaction Observed From High Spectral Resolution Lidar Data

NASA Technical Reports Server (NTRS)

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

2008-01-01

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

Development and Applications of a New, High-Resolution, Operational MISR Aerosol Product

NASA Astrophysics Data System (ADS)

Garay, M. J.; Diner, D. J.; Kalashnikova, O.

2014-12-01

Since early 2000, the Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has been providing aerosol optical depth (AOD) and particle property retrievals at 17.6 km spatial resolution. Capitalizing on the capabilities provided by multi-angle viewing, the operational MISR algorithm performs well, with about 75% of MISR AOD retrievals falling within 0.05 or 20% × AOD of the paired validation data from the ground-based Aerosol Robotic Network (AERONET), and is able to distinguish aerosol particles by size and sphericity, over both land and water. These attributes enable a variety of applications, including aerosol transport model validation and global air quality assessment. Motivated by the adverse impacts of aerosols on human health at the local level, and taking advantage of computational speed advances that have occurred since the launch of Terra, we have implemented an operational MISR aerosol product with 4.4 km spatial resolution that maintains, and sometimes improves upon, the quality of the 17.6 km resolution product. We will describe the performance of this product relative to the heritage 17.6 km product, the global AERONET validation network, and high spatial density AERONET-DRAGON sites. Other changes that simplify product content, and make working with the data much easier for users, will also be discussed. Examples of how the new product demonstrates finer spatial variability of aerosol fields than previously retrieved, and ways this new dataset can be used for studies of local aerosol effects, will be shown.

Quantification of marine aerosol subgrid variability and its correlation with clouds based on high-resolution regional modeling: Quantifying Aerosol Subgrid Variability

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

Lin, Guangxing; Qian, Yun; Yan, Huiping

One limitation of most global climate models (GCMs) is that with the horizontal resolutions they typically employ, they cannot resolve the subgrid variability (SGV) of clouds and aerosols, adding extra uncertainties to the aerosol radiative forcing estimation. To inform the development of an aerosol subgrid variability parameterization, here we analyze the aerosol SGV over the southern Pacific Ocean simulated by the high-resolution Weather Research and Forecasting model coupled to Chemistry. We find that within a typical GCM grid, the aerosol mass subgrid standard deviation is 15% of the grid-box mean mass near the surface on a 1 month mean basis.more » The fraction can increase to 50% in the free troposphere. The relationships between the sea-salt mass concentration, meteorological variables, and sea-salt emission rate are investigated in both the clear and cloudy portion. Under clear-sky conditions, marine aerosol subgrid standard deviation is highly correlated with the standard deviations of vertical velocity, cloud water mixing ratio, and sea-salt emission rates near the surface. It is also strongly connected to the grid box mean aerosol in the free troposphere (between 2 km and 4 km). In the cloudy area, interstitial sea-salt aerosol mass concentrations are smaller, but higher correlation is found between the subgrid standard deviations of aerosol mass and vertical velocity. Additionally, we find that decreasing the model grid resolution can reduce the marine aerosol SGV but strengthen the correlations between the aerosol SGV and the total water mixing ratio (sum of water vapor, cloud liquid, and cloud ice mixing ratios).« less

A New Satellite Aerosol Retrieval Using High Spectral Resolution Oxygen A-Band Measurements

NASA Astrophysics Data System (ADS)

Winker, D. M.; Zhai, P.

2014-12-01

Efforts to advance current satellite aerosol retrieval capabilities have mostly focused on polarimetric techniques. While there has been much interest in recent decades in the use of the oxygen A-band for retrievals of cloud height or surface pressure, these techniques are mostly based on A-band measurements with relatively low spectral resolution. We report here on a new aerosol retrieval technique based on high-resolution A-band spectra. Our goal is the development of a technique to retrieve aerosol absorption, one of the critical parameters affecting the global radiation budget and one which is currently poorly constrained by satellite measurements. Our approach relies on two key factors: 1) the use of high spectral resolution measurements which resolve the A-band line structure, and 2) the use of co-located lidar profile measurements to constrain the vertical distribution of scatterers. The OCO-2 satellite, launched in July this year and now flying in formation with the CALIPSO satellite, carries an oxygen A-band spectrometer with a spectral resolution of 21,000:1. This is sufficient to resolve the A-band line structure, which contains information on atmospheric photon path lengths. Combining channels with oxygen absorption ranging from weak to strong allows the separation of atmospheric and surface scattering. An optimal estimation algorithm for simultaneous retrieval of aerosol optical depth, aerosol absorption, and surface albedo has been developed. Lidar profile data is used for scene identification and to provide constraints on the vertical distribution of scatterers. As calibrated OCO-2 data is not expected until the end of this year, the algorithm has been developed and tested using simulated OCO-2 spectra. The simulations show that AOD and surface albedo can be retrieved with high accuracy. Retrievals of aerosol single scatter albedo are encouraging, showing good performance when AOD is larger than about 0.15. Retrieval performance improves as the

High temporal resolution aerosol retrieval using Geostationary Ocean Color Imager: application and initial validation

NASA Astrophysics Data System (ADS)

Zhang, Yuhuan; Li, Zhengqiang; Zhang, Ying; Hou, Weizhen; Xu, Hua; Chen, Cheng; Ma, Yan

2014-01-01

The Geostationary Ocean Color Imager (GOCI) provides multispectral imagery of the East Asia region hourly from 9:00 to 16:00 local time (GMT+9) and collects multispectral imagery at eight spectral channels (412, 443, 490, 555, 660, 680, 745, and 865 nm) with a spatial resolution of 500 m. Thus, this technology brings significant advantages to high temporal resolution environmental monitoring. We present the retrieval of aerosol optical depth (AOD) in northern China based on GOCI data. Cross-calibration was performed against Moderate Resolution Imaging Spectrometer (MODIS) data in order to correct the land calibration bias of the GOCI sensor. AOD retrievals were then accomplished using a look-up table (LUT) strategy with assumptions of a quickly varying aerosol and a slowly varying surface with time. The AOD retrieval algorithm calculates AOD by minimizing the surface reflectance variations of a series of observations in a short period of time, such as several days. The monitoring of hourly AOD variations was implemented, and the retrieved AOD agreed well with AErosol RObotic NETwork (AERONET) ground-based measurements with a good R2 of approximately 0.74 at validation sites at the cities of Beijing and Xianghe, although intercept bias may be high in specific cases. The comparisons with MODIS products also show a good agreement in AOD spatial distribution. This work suggests that GOCI imagery can provide high temporal resolution monitoring of atmospheric aerosols over land, which is of great interest in climate change studies and environmental monitoring.

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

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

Dubey, Manvendra; Aiken, Allison; Berg, Larry

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

Airborne High Spectral Resolution Lidar Aerosol Measurements during MILAGRO and TEXAQS/GOMACCS

NASA Technical Reports Server (NTRS)

Ferrare, Richard; Hostetler, Chris; Hair, John; Cook Anthony; Harper, David; Burton, Sharon; Clayton, Marian; Clarke, Antony; Russell, Phil; Redemann, Jens

2007-01-01

Two1 field experiments conducted during 2006 provided opportunities to investigate the variability of aerosol properties near cities and the impacts of these aerosols on air quality and radiative transfer. The Megacity Initiative: Local and Global Research Observations (MILAGRO) /Megacity Aerosol Experiment in Mexico City (MAX-MEX)/Intercontinental Chemical Transport Experiment-B (INTEX-B) joint experiment conducted during March 2006 investigated the evolution and transport of pollution from Mexico City. The Texas Air Quality Study (TEXAQS)/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) (http://www.al.noaa.gov/2006/) conducted during August and September 2006 investigated climate and air quality in the Houston/Gulf of Mexico region. During both missions, the new NASA Langley airborne High Spectral Resolution Lidar (HSRL) was deployed on the NASA Langley B200 King Air aircraft and measured profiles of aerosol extinction, backscattering, and depolarization to: 1) characterize the spatial and vertical distributions of aerosols, 2) quantify aerosol extinction and optical thickness contributed by various aerosol types, 3) investigate aerosol variability near clouds, 4) evaluate model simulations of aerosol transport, and 5) assess aerosol optical properties derived from a combination of surface, airborne, and satellite measurements.

Chemical Characteristics of Particulate Matter from Vehicle emission using High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS)

NASA Astrophysics Data System (ADS)

Park, T.; Lee, T.; Kang, S.; Lee, J.; Kim, J.; Son, J.; Yoo, H. M.; Kim, K.; Park, G.

2015-12-01

Car emissions are major contributors of particulate matter (PM) in the urban environment and effects of air pollution, climate change, and human activities. By increasing of interest in research of car emission for assessment of the PM control, it became require to understand the chemical composition and characteristics of the car exhaust gases and particulate matter. To understand car emission characteristics of PM, we will study PM of car emissions for five driving modes (National Institute Environmental Research (NIER)-5, NIER-9, NIER-12, NIER-14) and three fixed speed driving modes (30km/h, 70km/h, 110km/h) using different fuel types (gasoline, diesel, and LPG) at Transportation Pollution Research Center (TPRC) of NIER in Incheon, South Korea. PM chemical composition of car emission was measured for concentrations of organics, sulfate, nitrate, ammonium, PAHs, oxidation states and size distribution using an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and engine exhaust particle sizer (EEPS) on real-time. In the study, organics concentration was dominated for all cases of driving modes and the concentration of organics was increased in 110km/h fixed speed mode for gasoline and diesel. The presentation will provide an overview of the chemical composition of PM in the car emissions.

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

NASA Astrophysics Data System (ADS)

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

2012-11-01

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

A High-Resolution Aerosol Retrieval Method for Urban Areas Using MISR Data

NASA Astrophysics Data System (ADS)

Moon, T.; Wang, Y.; Liu, Y.; Yu, B.

2012-12-01

Satellite-retrieved Aerosol Optical Depth (AOD) can provide a cost-effective way to monitor particulate air pollution without using expensive ground measurement sensors. One of the current state-of-the-art AOD retrieval method is NASA's Multi-angle Imaging SpectroRadiometer (MISR) operational algorithm, which has the spatial resolution of 17.6 km x 17.6 km. While the MISR baseline scheme already leads to exciting research opportunities to study particle compositions at regional scale, its spatial resolution is too coarse for analyzing urban areas where the AOD level has stronger spatial variations. We develop a novel high-resolution AOD retrieval algorithm that still uses MISR's radiance observations but has the resolution of 4.4km x 4.4km. We achieve the high resolution AOD retrieval by implementing a hierarchical Bayesian model and Monte-Carlo Markov Chain (MCMC) inference method. Our algorithm not only improves the spatial resolution, but also extends the coverage of AOD retrieval and provides with additional composition information of aerosol components that contribute to the AOD. We validate our method using the recent NASA's DISCOVER-AQ mission data, which contains the ground measured AOD values for Washington DC and Baltimore area. The validation result shows that, compared to the operational MISR retrievals, our scheme has 41.1% more AOD retrieval coverage for the DISCOVER-AQ data points and 24.2% improvement in mean-squared error (MSE) with respect to the AERONET ground measurements.

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.

Validation of high-resolution MAIAC aerosol product over South America

NASA Astrophysics Data System (ADS)

Martins, V. S.; Lyapustin, A.; de Carvalho, L. A. S.; Barbosa, C. C. F.; Novo, E. M. L. M.

2017-07-01

Multiangle Implementation of Atmospheric Correction (MAIAC) is a new Moderate Resolution Imaging Spectroradiometer (MODIS) algorithm that combines time series approach and image processing to derive surface reflectance and atmosphere products, such as aerosol optical depth (AOD) and columnar water vapor (CWV). The quality assessment of MAIAC AOD at 1 km resolution is still lacking across South America. In the present study, critical assessment of MAIAC AOD550 was performed using ground-truth data from 19 Aerosol Robotic Network (AERONET) sites over South America. Additionally, we validated the MAIAC CWV retrievals using the same AERONET sites. In general, MAIAC AOD Terra/Aqua retrievals show high agreement with ground-based measurements, with a correlation coefficient (R) close to unity (RTerra:0.956 and RAqua: 0.949). MAIAC accuracy depends on the surface properties and comparisons revealed high confidence retrievals over cropland, forest, savanna, and grassland covers, where more than 2/3 ( 66%) of retrievals are within the expected error (EE = ±(0.05 + 0.05 × AOD)) and R exceeding 0.86. However, AOD retrievals over bright surfaces show lower correlation than those over vegetated areas. Both MAIAC Terra and Aqua retrievals are similarly comparable to AERONET AOD over the MODIS lifetime (small bias offset 0.006). Additionally, MAIAC CWV presents quantitative information with R 0.97 and more than 70% of retrievals within error (±15%). Nonetheless, the time series validation shows an upward bias trend in CWV Terra retrievals and systematic negative bias for CWV Aqua. These results contribute to a comprehensive evaluation of MAIAC AOD retrievals as a new atmospheric product for future aerosol studies over South America.

Validation of High-Resolution MAIAC Aerosol Product over South America

NASA Technical Reports Server (NTRS)

Martins, V. S.; Lyapustin, A.; de Carvalho, L. A. S.; Barbosa, C. C. F.; Novo, E. M. L. M.

2017-01-01

Multiangle Implementation of Atmospheric Correction (MAIAC) is a new Moderate Resolution Imaging Spectroradiometer (MODIS) algorithm that combines time series approach and image processing to derive surface reflectance and atmosphere products, such as aerosol optical depth (AOD) and columnar water vapor (CWV). The quality assessment of MAIAC AOD at 1 km resolution is still lacking across South America. In the present study, critical assessment of MAIAC AOD(sub 550) was performed using ground-truth data from 19 Aerosol Robotic Network (AERONET) sites over South America. Additionally, we validated the MAIAC CWV retrievals using the same AERONET sites. In general, MAIAC AOD Terra/Aqua retrievals show high agreement with ground-based measurements, with a correlation coefficient (R) close to unity (R(sub Terra):0.956 and R(sub Aqua):0.949). MAIAC accuracy depends on the surface properties and comparisons revealed high confidence retrievals over cropland, forest, savanna, and grassland covers, where more than 2/3 (approximately 66%) of retrievals are within the expected error (EE = +/-(0.05 + 0.05 × AOD)) and R exceeding 0.86. However, AOD retrievals over bright surfaces show lower correlation than those over vegetated areas. Both MAIAC Terra and Aqua retrievals are similarly comparable to AERONET AOD over the MODIS lifetime (small bias offset approximately 0.006). Additionally, MAIAC CWV presents quantitative information with R approximatley 0.97 and more than 70% of retrievals within error (+/-15%). Nonetheless, the time series validation shows an upward bias trend in CWV Terra retrievals and systematic negative bias for CWV Aqua. These results contribute to a comprehensive evaluation of MAIAC AOD retrievals as a new atmospheric product for future aerosol studies over South America.

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

NASA Astrophysics Data System (ADS)

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

2013-05-01

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

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.

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

NASA Astrophysics Data System (ADS)

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

2014-08-01

method would be even more useful for HR-ToF-AMS data, due to the ability to understand better the chemical nature of atypical factors from high-resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of the extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

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

NASA Astrophysics Data System (ADS)

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

2014-02-01

to better understand the chemical nature of atypical factors from high resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

An operational MODIS aerosol retrieval algorithm at high spatial resolution, and its application over a complex urban region

NASA Astrophysics Data System (ADS)

Wong, Man Sing; Nichol, Janet E.; Lee, Kwon Ho

2011-03-01

Aerosol retrieval algorithms for the MODerate Resolution Imaging Spectroradiometer (MODIS) have been developed to estimate aerosol and microphysical properties of the atmosphere, which help to address aerosol climatic issues at global scale. However, higher spatial resolution aerosol products for urban areas have not been well-researched mainly due to the difficulty of differentiating aerosols from bright surfaces in urban areas. Here, an aerosol retrieval algorithm using the MODIS 500-m resolution bands is described, to retrieve aerosol properties over Hong Kong and the Pearl River Delta region. The rationale of our technique is to first estimate the aerosol reflectances by decomposing the top-of-atmosphere reflectances from surface reflectances and Rayleigh path reflectances. For the determination of surface reflectances, a Minimum Reflectance Technique (MRT) is used, and MRT images are computed for different seasons. For conversion of aerosol reflectance to aerosol optical thickness (AOT), comprehensive Look Up Tables specific to the local region are constructed, which consider aerosol properties and sun-viewing geometry in the radiative transfer calculations. Four local aerosol types, namely coastal urban, polluted urban, dust, and heavy pollution, were derived using cluster analysis on 3 years of AERONET measurements in Hong Kong. The resulting 500 m AOT images were found to be highly correlated with ground measurements from the AERONET (r2 = 0.767) and Microtops II sunphotometers (r2 = 0.760) in Hong Kong. This study further demonstrates the application of the fine resolution AOT images for monitoring inter-urban and intra-urban aerosol distributions and the influence of trans-boundary flows. These applications include characterization of spatial patterns of AOT within the city, and detection of regional biomass burning sources.

Vertical Profiles of Aerosol Volume from High Spectral Resolution Infrared Transmission Measurements: Results

NASA Technical Reports Server (NTRS)

Eldering, Annmarie; Kahn, Brian H.; Mills, Franklin P.; Irion, Fredrick W.; Steele, Helen M.; Gunson, Michael R.

2004-01-01

The high-resolution infrared absorption spectra of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment are utilized to derive vertical profiles of sulfate aerosol volume density and extinction coefficient. Following the eruption of Mt. Pinatubo in June 1991, the ATMOS spectra obtained on three Space Shuttle missions (1992, 1993, and 1994) provide a unique opportunity to study the global stratospheric sulfate aerosol layer shortly after a major volcanic eruption and periodically during the decay phase. Synthetic sulfate aerosol spectra are fit to the observed spectra, and a global fitting inversion routine is used to derive vertical profiles of sulfate aerosol volume density. Vertical profiles of sulfate aerosol volume density for the three missions over portions of the globe are presented, with the peak in aerosol volume density occurring from as low as 10 km (polar latitudes) to as high as 20 km (subtropical latitudes). Derived aerosol volume density is as high as 2-3.5 (mu)m(exp 3) per cubic centimeter +/-10% in 1992, decreasing to 0.2-0.5 (mu)m(exp 3) per cubic centimeter +/-20% in 1994, in agreement with other experiments. Vertical extinction profiles derived from ATMOS are compared with profiles from Improved Stratospheric And Mesospheric Sounder (ISAMS) and Cryogenic Limb Array Etalon Spectrometer (CLAES) that coincide in space and time and show good general agreement. The uncertainty of the ATMOS vertical profiles is similar to CLAES and consistently smaller than ISAMS at similar altitudes.

DEVELOPMENT AND APPLICATION OF A MASS SPECTRA-VOLATILITY DATABASE OF COMBUSTION AND SECONDARY ORGANIC AEROSOL SOURCES FOR THE AERODYNE AEROSOL MASS SPECTROMETER

EPA Science Inventory

1. Thermodenuder Development:

Two TD systems were designed, constructed, and tested at Aerodyne. In this design, the vaporizer consists of a 50 cm long, 1 inch OD stainless steel tube wrapped with three heating tapes and fiberglass insulation and then mounted in a sta...

Aerosol Profile Measurements from the NASA Langley Research Center Airborne High Spectral Resolution Lidar

NASA Technical Reports Server (NTRS)

Obland, Michael D.; Hostetler, Chris A.; Ferrare, Richard A.; Hair, John W.; Roers, Raymond R.; Burton, Sharon P.; Cook, Anthony L.; Harper, David B.

2008-01-01

Since achieving first light in December of 2005, the NASA Langley Research Center (LaRC) Airborne High Spectral Resolution Lidar (HSRL) has been involved in seven field campaigns, accumulating over 450 hours of science data across more than 120 flights. Data from the instrument have been used in a variety of studies including validation and comparison with the Cloud- Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite mission, aerosol property retrievals combining passive and active instrument measurements, aerosol type identification, aerosol-cloud interactions, and cloud top and planetary boundary layer (PBL) height determinations. Measurements and lessons learned from the HSRL are leading towards next-generation HSRL instrument designs that will enable even further studies of aerosol intensive and extensive parameters and the effects of aerosols on the climate system. This paper will highlight several of the areas in which the NASA Airborne HSRL is making contributions to climate science.

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.

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

NASA Astrophysics Data System (ADS)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Kittaka, C.; Vaughn, M. A.; Remer, L. A.

2010-01-01

We derive aerosol extinction profiles from airborne and space-based lidar backscatter signals by constraining the retrieval with column aerosol optical thickness (AOT), with no need to rely on assumptions about aerosol type or lidar ratio. The backscatter data were acquired by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. The HSRL also simultaneously measures aerosol extinction coefficients independently using the high spectral resolution lidar technique, thereby providing an ideal data set for evaluating the retrieval. We retrieve aerosol extinction profiles from both HSRL and CALIOP attenuated backscatter data constrained with HSRL, Moderate-Resolution Imaging Spectroradiometer (MODIS), and Multiangle Imaging Spectroradiometer column AOT. The resulting profiles are compared with the aerosol extinction measured by HSRL. Retrievals are limited to cases where the column aerosol thickness is greater than 0.2 over land and 0.15 over water. In the case of large AOT, the results using the Aqua MODIS constraint over water are poorer than Aqua MODIS over land or Terra MODIS. The poorer results relate to an apparent bias in Aqua MODIS AOT over water observed in August 2007. This apparent bias is still under investigation. Finally, aerosol extinction coefficients are derived from CALIPSO backscatter data using AOT from Aqua MODIS for 28 profiles over land and 9 over water. They agree with coincident measurements by the airborne HSRL to within +/-0.016/km +/- 20% for at least two-thirds of land points and within +/-0.028/km +/- 20% for at least two-thirds of ocean points.

Demonstration of a diode-laser-based high spectral resolution lidar (HSRL) for quantitative profiling of clouds and aerosols.

PubMed

Hayman, Matthew; Spuler, Scott

2017-11-27

We present a demonstration of a diode-laser-based high spectral resolution lidar. It is capable of performing calibrated retrievals of aerosol and cloud optical properties at a 150 m range resolution with less than 1 minute integration time over an approximate range of 12 km during day and night. This instrument operates at 780 nm, a wavelength that is well established for reliable semiconductor lasers and detectors, and was chosen because it corresponds to the D2 rubidium absorption line. A heated vapor reference cell of isotopic rubidium 87 is used as an effective and reliable aerosol signal blocking filter in the instrument. In principle, the diode-laser-based high spectral resolution lidar can be made cost competitive with elastic backscatter lidar systems, yet delivers a significant improvement in data quality through direct retrieval of quantitative optical properties of clouds and aerosols.

Aerosol Optical Depth Retrievals From High-Resolution Commercial Satellite Imagery Over Areas of High Surface Reflectance

NASA Astrophysics Data System (ADS)

Vincent, D. A.; Nielsen, K. E.; Durkee, P. A.; Reid, J. S.

2005-12-01

The advancement and proliferation of high-resolution commercial imaging satellites presents a new opportunity for overland aerosol characterization. Current aerosol optical depth retrieval methods typically fail over areas with high surface reflectance, such as urban areas and deserts, since the upwelling radiance due to scattering by aerosols is small compared to the radiance resulting from surface reflection. The method proposed here uses shadows cast on the surface to exploit the differences between radiance from the adjacent shaded and unshaded areas of the scene. Shaded areas of the scene are primarily illuminated by diffuse irradiance that is scattered downward from the atmosphere, while unshaded areas are illuminated by both diffuse and direct solar irradiance. The first-order difference between the shaded and unshaded areas is the direct component. Given uniform surface reflectance for the shaded and unshaded areas, the difference in reflected radiance measured by a satellite sensor is related to the direct transmission of solar radiation and inversely proportional to total optical depth. Using an iterative approach, surface reflectance and mean aerosol reflectance can be partitioned to refine the retrieved total optical depth. Aerosol optical depth can then be determined from its contribution to the total atmospheric optical depth (following correction for molecular Rayleigh scattering). Intitial results based on QuickBird imagery and AERONET data collected during the United Arab Emirates Unified Aerosol Experiment (UAE2) indicate that aerosol optical depth retrievals are possible in the visible and near-infrared region with an accuracy of ~0.04.

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.

New in situ Aerosol Spectral Optical Measurements over 300-700 nm, Extinction and Total Absorption, Paired with Absorption from Water- and Methanol-soluble Aerosol Extracts

NASA Astrophysics Data System (ADS)

Jordan, C. E.; Stauffer, R. M.; Lamb, B.; Novak, M. G.; Mannino, A.; Hudgins, C.; Thornhill, K. L., II; Crosbie, E.; Winstead, E.; Anderson, B.; Martin, R.; Shook, M.; Ziemba, L. D.; Beyersdorf, A. J.; Corr, C.

2017-12-01

A new in situ spectral aerosol extinction instrument (custom built, SpEx) built to cover the 300-700 nm range at 1 nm spectral resolution and temporal resolution of 4 minutes was deployed on the top deck ( 10 m above the water surface) of the R/V Onnuri during the KORUS-OC research cruise around South Korea in spring 2016. This new instrument was one component of a suite of in situ aerosol optical measurements that included 3-visible-wavelength scattering (Airphoton IN101 Nephelometer, at 450, 532, & 632 nm) and absorption (Brechtel Tricolor Absorption Photometer Model 2901, at 467, 528, & 652 nm) with sub-minute temporal resolution; two sets of filters (Teflon and glass fiber, both collected over 3 hour daytime and 12 hour overnight intervals) to provide aerosol absorption spectra over the same wavelength range as SpEx. The glass fiber filters were placed in the center of an integrating sphere (Labsphere DRA-CA-30) attached to a dual beam spectrophotometer (Cary 100 Bio UV-Visible Spectrophotometer) to measure total aerosol absorption spectra via an established method used by the ocean color community to obtain absorption spectra from particles suspended in sea water. Adapting this methodology for atmospheric aerosol measurements provides a new avenue to obtain spectral total aerosol absorption, particularly useful for expanding in situ measurement capabilities into the UV range. The Teflon filters were cut in half with one half extracted in deionized water and the other half extracted in methanol. The solutions were filtered and injected into a liquid waveguide capillary cell (World Precision Instruments LWCC-3100, 100 cm pathlength) to measure the absorption spectra for each solution. In addition, the water extracts were measured via ion chromatography (Dionex ICS-3000 Ion Chromatography System) to obtain water-soluble inorganic ion concentrations, as well as via aerosol mass spectrometry (Aerodyne Research, Inc. HR-ToF High Resolution Aerosol Mass Spectrometer

AeroDyn V15.04: Design tool for wind and MHK turbines

DOE Data Explorer

Murray, Robynne; Hayman, Greg; Jonkman, Jason

2017-04-28

AeroDyn is a time-domain wind and MHK turbine aerodynamics module that can be coupled into the FAST version 8 multi-physics engineering tool to enable aero-elastic simulation of horizontal-axis wind turbines. AeroDyn V15.04 has been updated to include a cavitation check for MHK turbines, and can be driven as a standalone code to compute wind turbine aerodynamic response uncoupled from FAST. Note that while AeroDyn has been updated to v15.04, FAST v8.16 has not yet been updated and still uses AeroDyn v15.03.

Cookstove Emissions Quantified with the Aerodyne Mobile Laboratory During the Short Lived Climate Forcing (SLCF) 2013 Campaign in Pátzcuaro Mexico

NASA Astrophysics Data System (ADS)

Gonzalez Abraham, R.; Zavala, M.; Molina, L. T.; Fortner, E.; Wormhoudt, J.; Knighton, B.; Herndon, S.; Roscioli, J. R.; Onasch, T. B.; Jayne, J. T.; Worsnop, D. R.; Kolb, C. E.; Masera, O.; Berrueta, V.

2013-12-01

Black carbon emissions are a major contributor to climate change, with cookstoves being one of the top sources. The SLCF cookstove study was conducted in March 2013 at the Interdisciplinary Group for Appropriate Rural Technology (GIRA) in Pátzcuaro, Mexico. Seven different types of wood-burning cookstoves were measured giving insight to the effects of different designs and operating conditions on particle and gas phase emissions. High-time resolution measurements of emissions were made. For most of the cookstoves, measurements were made throughout a standard water boiling test. The Aerodyne Mobile Laboratory conducted these emission measurements utilizing extractive sampling from the stove exhaust. Sample flow to the gas phase instruments was extracted directly from the stovepipe and then quickly diluted with nitrogen. Sample flows for the particulate instruments were taken at points under a meter from the exit of the stovepipe, after dilution with ambient air. The key particulate instrument was the Aerodyne soot particle aerosol mass spectrometer (SP-AMS), which provided measurements of black carbon, divided into several sub-components, along with other classes of particulate matter classified by chemical composition. Gas phase measurements conducted included CO, CO2, NO, NOx, SO2, CH4, C2H2, C2H6, and a variety of VOCs (including benzene, methanol, acetaldehyde, toluene, acetone, acetonitrile, and terpene) measured with a PTR-MS instrument. All of these measurements will be examined to construct emission ratios evaluating how these vary with different cookstove types and different stove operating conditions. Comparisons will be made to previous measurements of cookstove emissions in the literature, with a focus on the variety of particulate measurements reported.

Development of a new corona discharge based ion source for high resolution time-of-flight chemical ionization mass spectrometer to measure gaseous H2SO4 and aerosol sulfate

NASA Astrophysics Data System (ADS)

Zheng, Jun; Yang, Dongsen; Ma, Yan; Chen, Mindong; Cheng, Jin; Li, Shizheng; Wang, Ming

2015-10-01

A new corona discharge (CD) based ion source was developed for a commercial high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) (Aerodyne Research Inc.) to measure both gaseous sulfuric acid (H2SO4) and aerosol sulfate after thermal desorption. Nitrate core ions (NO3-) were used as reagent ions and were generated by a negative discharge in zero air followed by addition of excess nitrogen dioxide (NO2) to convert primary ions and hydroxyl radicals (OH) into NO3- ions and nitric acid (HNO3). The CD-HRToF-CIMS showed no detectable interference from hundreds parts per billion by volume (ppbv) of sulfur dioxide (SO2). Unlike the atmospheric pressure ionization (API) ToF-CIMS, the CD ion source was integrated onto the ion-molecule reaction (IMR) chamber and which made it possible to measure aerosol sulfate by coupling to a filter inlet for gases and aerosols (FIGAERO). Moreover, compared with a quadrupole-based mass spectrometer, the desired HSO4- signal was detected by its exact mass of m/z 96.960, which was well resolved from the potential interferences of HCO3-ṡ(H2O)2 (m/z 97.014) and O-ṡH2OṡHNO3 (m/z 97.002). In this work, using laboratory-generated standards the CD-HRToF-CIMS was demonstrated to be able to detect as low as 3.1 × 105 molecules cm-3 gaseous H2SO4 and 0.5 μg m-3 ammonium sulfate based on 10-s integration time and two times of the baseline noise. The CD ion source had the advantages of low cost and a simple but robust structure. Since the system was non-radioactive and did not require corrosive HNO3 gas, it can be readily field deployed. The CD-HRToF-CIMS can be a powerful tool for both field and laboratory studies of aerosol formation mechanism and the chemical processes that were critical to understand the evolution of aerosols in the atmosphere.

Global Survey of Submicron Aerosol Acidity (pH)

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Submicron particles influenced by mixed biogenic and anthropogenic emissions: high-resolution aerosol mass spectrometry results from the Carbonaceous Aerosols and Radiative Effects Study (CARES)

NASA Astrophysics Data System (ADS)

Setyan, A.; Zhang, Q.; Merkel, M.; Knighton, W. B.; Sun, Y.; Song, C.; Shilling, J. E.; Onasch, T. B.; Herndon, S. C.; Worsnop, D. R.; Fast, J. D.; Zaveri, R. A.; Berg, L. K.; Wiedensohler, A.; Flowers, B. A.; Dubey, M. K.; Subramanian, R.

2012-02-01

The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project (~40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 μg m-3 on average) and dominated by organics (80 % of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at ˜400 nm in vacuum aerodynamic diameter (Dva), and a condensation mode at ~150 nm, while organics generally displayed a broad distribution in 60-600 nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a~nominal formula of C1H1.38N0.004O0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90 % of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high-resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly due to local traffic. Twenty three periods of

High resolution simulations of aerosol microphysics in a global and regionally nested chemical transport model

NASA Astrophysics Data System (ADS)

Adams, P. J.; Marks, M.

2015-12-01

The aerosol indirect effect is the largest source of forcing uncertainty in current climate models. This effect arises from the influence of aerosols on the reflective properties and lifetimes of clouds, and its magnitude depends on how many particles can serve as cloud droplet formation sites. Assessing levels of this subset of particles (cloud condensation nuclei, or CCN) requires knowledge of aerosol levels and their global distribution, size distributions, and composition. A key tool necessary to advance our understanding of CCN is the use of global aerosol microphysical models, which simulate the processes that control aerosol size distributions: nucleation, condensation/evaporation, and coagulation. Previous studies have found important differences in CO (Chen, D. et al., 2009) and ozone (Jang, J., 1995) modeled at different spatial resolutions, and it is reasonable to believe that short-lived, spatially-variable aerosol species will be similarly - or more - susceptible to model resolution effects. The goal of this study is to determine how CCN levels and spatial distributions change as simulations are run at higher spatial resolution - specifically, to evaluate how sensitive the model is to grid size, and how this affects comparisons against observations. Higher resolution simulations are necessary supports for model/measurement synergy. Simulations were performed using the global chemical transport model GEOS-Chem (v9-02). The years 2008 and 2009 were simulated at 4ox5o and 2ox2.5o globally and at 0.5ox0.667o over Europe and North America. Results were evaluated against surface-based particle size distribution measurements from the European Supersites for Atmospheric Aerosol Research project. The fine-resolution model simulates more spatial and temporal variability in ultrafine levels, and better resolves topography. Results suggest that the coarse model predicts systematically lower ultrafine levels than does the fine-resolution model. Significant

Desorption atmospheric pressure photoionization high-resolution mass spectrometry: a complementary approach for the chemical analysis of atmospheric aerosols.

PubMed

Parshintsev, Jevgeni; Vaikkinen, Anu; Lipponen, Katriina; Vrkoslav, Vladimir; Cvačka, Josef; Kostiainen, Risto; Kotiaho, Tapio; Hartonen, Kari; Riekkola, Marja-Liisa; Kauppila, Tiina J

2015-07-15

On-line chemical characterization methods of atmospheric aerosols are essential to increase our understanding of physicochemical processes in the atmosphere, and to study biosphere-atmosphere interactions. Several techniques, including aerosol mass spectrometry, are nowadays available, but they all suffer from some disadvantages. In this research, desorption atmospheric pressure photoionization high-resolution (Orbitrap) mass spectrometry (DAPPI-HRMS) is introduced as a complementary technique for the fast analysis of aerosol chemical composition without the need for sample preparation. Atmospheric aerosols from city air were collected on a filter, desorbed in a DAPPI source with a hot stream of toluene and nitrogen, and ionized using a vacuum ultraviolet lamp at atmospheric pressure. To study the applicability of the technique for ambient aerosol analysis, several samples were collected onto filters and analyzed, with the focus being on selected organic acids. To compare the DAPPI-HRMS data with results obtained by an established method, each filter sample was divided into two equal parts, and the second half of the filter was extracted and analyzed by liquid chromatography/mass spectrometry (LC/MS). The DAPPI results agreed with the measured aerosol particle number. In addition to the targeted acids, the LC/MS and DAPPI-HRMS methods were found to detect different compounds, thus providing complementary information about the aerosol samples. DAPPI-HRMS showed several important oxidation products of terpenes, and numerous compounds were tentatively identified. Thanks to the soft ionization, high mass resolution, fast analysis, simplicity and on-line applicability, the proposed methodology has high potential in the field of atmospheric research. Copyright © 2015 John Wiley & Sons, Ltd.

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

NASA Technical Reports Server (NTRS)

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

2002-01-01

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

Retrieval of high-spectral-resolution lidar for atmospheric aerosol optical properties profiling

NASA Astrophysics Data System (ADS)

Liu, Dong; Luo, Jing; Yang, Yongying; Cheng, Zhongtao; Zhang, Yupeng; Zhou, Yudi; Duan, Lulin; Su, Lin

2015-10-01

High-spectral-resolution lidars (HSRLs) are increasingly being developed for atmospheric aerosol remote sensing applications due to the straightforward and independent retrieval of aerosol optical properties without reliance on assumptions about lidar ratio. In HSRL technique, spectral discrimination between scattering from molecules and aerosol particles is one of the most critical processes, which needs to be accomplished by means of a narrowband spectroscopic filter. To ensure a high retrieval accuracy of an HSRL system, the high-quality design of its spectral discrimination filter should be made. This paper reviews the available algorithms that were proposed for HSRLs and makes a general accuracy analysis of the HSRL technique focused on the spectral discrimination, in order to provide heuristic guidelines for the reasonable design of the spectral discrimination filter. We introduce a theoretical model for retrieval error evaluation of an HSRL instrument with general three-channel configuration. Monte Carlo (MC) simulations are performed to validate the correctness of the theoretical model. Results from both the model and MC simulations agree very well, and they illustrate one important, although not well realized fact: a large molecular transmittance and a large spectral discrimination ratio (SDR, i.e., ratio of the molecular transmittance to the aerosol transmittance) are beneficial t o promote the retrieval accuracy. The application of the conclusions obtained in this paper in the designing of a new type of spectroscopic filter, that is, the field-widened Michelson interferometer, is illustrated in detail. These works are with certain universality and expected to be useful guidelines for HSRL community, especially when choosing or designing the spectral discrimination filter.

Separating Dust Mixtures and Other External Aerosol Mixtures Using Airborne High Spectral Resolution Lidar Data

NASA Astrophysics Data System (ADS)

Burton, S. P.; Ferrare, R. A.; Vaughan, M.; Hostetler, C. A.; Rogers, R. R.; Hair, J. W.; Cook, A. L.; Harper, D. B.

2013-12-01

Knowledge of aerosol type is important for source attribution and for determining the magnitude and assessing the consequences of aerosol radiative forcing. The NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-1) has acquired considerable datasets of both aerosol extensive parameters (e.g. aerosol optical depth) and intensive parameters (e.g. aerosol depolarization ratio, lidar ratio) that can be used to infer aerosol type. An aerosol classification methodology has been used extensively to classify HSRL-1 aerosol measurements of different aerosol types including dust, smoke, urban pollution, and marine aerosol. However, atmospheric aerosol is frequently not a single pure type, but instead occurs as a mixture of types, and this mixing affects the optical and radiative properties of the aerosol. Here we present a comprehensive and unified set of rules for characterizing external mixtures using several key aerosol intensive parameters: extinction-to-backscatter ratio (i.e. lidar ratio), backscatter color ratio, and depolarization ratio. Our mixing rules apply not just to the scalar values of aerosol intensive parameters, but to multi-dimensional normal distributions with variance in each measurement dimension. We illustrate the applicability of the mixing rules using examples of HSRL-1 data where mixing occurred between different aerosol types, including advected Saharan dust mixed with the marine boundary layer in the Caribbean Sea and locally generated dust mixed with urban pollution in the Mexico City surroundings. For each of these cases we infer a time-height cross section of mixing ratio along the flight track and we partition aerosol extinction into portions attributed to the two pure types. Since multiple aerosol intensive parameters are measured and included in these calculations, the techniques can also be used for cases without significant depolarization (unlike similar work by earlier researchers), and so a third example of a

Retrieving Aerosol in a Cloudy Environment: Aerosol Availability as a Function of Spatial and Temporal Resolution

NASA Technical Reports Server (NTRS)

Remer, Lorraine A.; Mattoo, Shana; Levy, Robert C.; Heidinger, Andrew; Pierce, R. Bradley; Chin, Mian

2011-01-01

The challenge of using satellite observations to retrieve aerosol properties in a cloudy environment is to prevent contamination of the aerosol signal from clouds, while maintaining sufficient aerosol product yield to satisfy specific applications. We investigate aerosol retrieval availability at different instrument pixel resolutions, using the standard MODIS aerosol cloud mask applied to MODIS data and a new GOES-R cloud mask applied to GOES data for a domain covering North America and surrounding oceans. Aerosol availability is not the same as the cloud free fraction and takes into account the technqiues used in the MODIS algorithm to avoid clouds, reduce noise and maintain sufficient numbers of aerosol retrievals. The inherent spatial resolution of each instrument, 0.5x0.5 km for MODIS and 1x1 km for GOES, is systematically degraded to 1x1 km, 2x2 km, 4x4 km and 8x8 km resolutions and then analyzed as to how that degradation would affect the availability of an aerosol retrieval, assuming an aerosol product resolution at 8x8 km. The results show that as pixel size increases, availability decreases until at 8x8 km 70% to 85% of the retrievals available at 0.5 km have been lost. The diurnal pattern of aerosol retrieval availability examined for one day in the summer suggests that coarse resolution sensors (i.e., 4x4 km or 8x8 km) may be able to retrieve aerosol early in the morning that would otherwise be missed at the time of current polar orbiting satellites, but not the diurnal aerosol properties due to cloud cover developed during the day. In contrast finer resolution sensors (i.e., 1x1 km or 2x2 km) have much better opportunity to retrieve aerosols in the partly cloudy scenes and better chance of returning the diurnal aerosol properties. Large differences in the results of the two cloud masks designed for MODIS aerosol and GOES cloud products strongly reinforce that cloud masks must be developed with specific purposes in mind and that a generic cloud mask

Development and Validation of a New Blade Element Momentum Skewed-Wake Model within AeroDyn: Preprint

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

Ning, S. A.; Hayman, G.; Damiani, R.

Blade element momentum methods, though conceptually simple, are highly useful for analyzing wind turbines aerodynamics and are widely used in many design and analysis applications. A new version of AeroDyn is being developed to take advantage of new robust solution methodologies, conform to a new modularization framework for National Renewable Energy Laboratory's FAST, utilize advanced skewed-wake analysis methods, fix limitations with previous implementations, and to enable modeling of highly flexible and nonstraight blades. This paper reviews blade element momentum theory and several of the options available for analyzing skewed inflow. AeroDyn implementation details are described for the benefit of usersmore » and developers. These new options are compared to solutions from the previous version of AeroDyn and to experimental data. Finally, recommendations are given on how one might select from the various available solution approaches.« less

High Resolution Aerosol Data from MODIS Satellite for Urban Air Quality Studies

NASA Technical Reports Server (NTRS)

Chudnovsky, A.; Lyapustin, A.; Wang, Y.; Tang, C.; Schwartz, J.; Koutrakis, P.

2013-01-01

The Moderate Resolution Imaging Spectroradiometer (MODIS) provides daily global coverage, but the 10 km resolution of its aerosol optical depth (AOD) product is not suitable for studying spatial variability of aerosols in urban areas. Recently, a new Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm was developed for MODIS which provides AOD at 1 km resolution. Using MAIAC data, the relationship between MAIAC AOD and PM(sub 2.5) as measured by the 27 EPA ground monitoring stations was investigated. These results were also compared to conventional MODIS 10 km AOD retrievals (MOD04) for the same days and locations. The coefficients of determination for MOD04 and for MAIAC are R(exp 2) =0.45 and 0.50 respectively, suggested that AOD is a reasonably good proxy for PM(sub 2.5) ground concentrations. Finally, we studied the relationship between PM(sub 2.5) and AOD at the intra-urban scale (10 km) in Boston. The fine resolution results indicated spatial variability in particle concentration at a sub-10 kilometer scale. A local analysis for the Boston area showed that the AOD-PM(sub 2.5) relationship does not depend on relative humidity and air temperatures below approximately 7 C. The correlation improves for temperatures above 7 - 16 C. We found no dependence on the boundary layer height except when the former was in the range 250-500 m. Finally, we apply a mixed effects model approach to MAIAC aerosol optical depth (AOD) retrievals from MODIS to predict PM(sub 2.5) concentrations within the greater Boston area. With this approach we can control for the inherent day-to-day variability in the AOD-PM(sub 2.5) relationship, which depends on time-varying parameters such as particle optical properties, vertical and diurnal concentration profiles and ground surface reflectance. Our results show that the model-predicted PM(sub 2.5) mass concentrations are highly correlated with the actual observations (out-of-sample R(exp 2) of 0.86). Therefore, adjustment

Volatility-resolved Measurements of the Chemical Composition of Arctic Aerosol Particles

NASA Astrophysics Data System (ADS)

Ehn, M.; Kroll, J.; Coffman, D.; Quinn, P.; Bates, T.; Williams, E.; Kulmala, M.; Worsnop, D.

2008-12-01

Here we describe measurements of the chemical composition of submicron particles in the Arctic marine boundary layer, taken on board the R/V Knorr during the IPY-ICEALOT mission (March-April 2008). Measurements were made with an Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) for the measurement of the non-refractory fraction of the aerosol, in particular allowing for the determination of the oxygen/carbon (O/C) ratio of the particulate organics and the unambiguous identification of trace inorganic species. Sampling alternated between ambient air and air sent through a thermodenuder (TD), continually scanned between 50 and 250C in order to remove aerosol components by volatility. The mass spectra of particulate matter in the Arctic (including Arctic haze) were dominated by sulfur-containing peaks and the CO2+ ion (at m/z 44), indicating the main non-refractory components of the aerosol are acidic sulfate and highly oxygenated organics. Thermodenuder measurements allow for the clear speciation of sulfate compounds by volatility, as well as the comparison of the degree of atmospheric aging of the organics to measurements taken elsewhere (including at terrestrial sites). AMS measurements will be compared to results from a hygroscopicity tandem differential mobility analyzer (HTDMA), also downstream of the thermodenuder, as well as from semicontinuous (PILS) and offline (filter) measurements of particle composition.

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

NASA Astrophysics Data System (ADS)

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

2016-07-01

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

A new application of hierarchical cluster analysis to investigate organic peaks in bulk mass spectra obtained with an Aerodyne Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Middlebrook, A. M.; Marcolli, C.; Canagaratna, M. R.; Worsnop, D. R.; Bahreini, R.; de Gouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; Lerner, B. M.; Roberts, J. M.; Meagher, J. F.; Fehsenfeld, F. C.; Marchewka, M. L.; Bertman, S. B.

2006-12-01

We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel Ronald H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter probably originating from both anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent on average 17% of the total organic mass that stems likely from biogenic sources during the ship's cruise. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

Aerosol Chemical and Physical Characterization in Central Amazonia during the 2013 Dry Season

NASA Astrophysics Data System (ADS)

Artaxo, P.; Stern, R.; Brito, J.; Carbone, S.

2015-12-01

During the dry season, the central Amazon forest is highly influenced by forest fires transported through large distances, changing drastically the atmospheric composition even in remote places. This work focuses on a physical-chemical characterization of the aerosol population over a pristine site in Central Amazonia during the dry season. The submicrometer organic aerosols were measured with the Aerodyne ACSM (Aerosol Chemical Speciation Monitor, Aerodyne Inc). Optical properties, size distribution and other micro-physical characteristics were also analyzed. Other instruments were simultaneously used. The measurements were taken during the dry season of 2013 in the Cuieiras ecological reserve (ZF2), northwest of Manaus. The statistical analysis of the data was done with the PMF (Positive Matrix Factorization) technique, in which the organic aerosol was separated into different factors, and then its sources and forming processes were attributed. Results show that the mean aerosol loading was 5,91 μg m-3, from which 78% are of organic composition, 8.5% are sulfate, 6.5% are equivalent black carbon, 4% are ammonium and 3% are nitrate. The mass spectra variability can be explained by 3 factors only, determined with the PMF technique. They were identified as BBOA (Biomass Burning Organic Aerosol), representing 12% of the total organic mass, OOA (Oxygenated Organic Aerosol), representing 66% of the total organic mass and IEPOX-SOA (Isoprene derived Epoxydiol-Secondary Organic Aerosol), representing 21% of the total organic mass. Even in remote and pristine regions, Central Amazonia is highly impacted by biomass burning. Biogenic secondary organic aerosols are also present during the dry season, and the suppression of its wet deposition processes increases their concentration. The oxidation level and other physical-chemical characteristics indicate that the long range transport is responsible for the regional range of this impact.

Effect of Vaporizer Temperature on Ambient Non-Refractory Submicron Aerosol Composition and Mass Spectra Measured by the Aerosol Mass Spectrometer

EPA Science Inventory

Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (Tvap) of 600^oC in order to facilitate quantitative detection of non-refractory submicron (NR-PM1) species. By analogy with other thermal desorption instrument...

Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Kittaka, C.; Hostetler, C. A.; Hair, J. W.; Obland, M. D.; Rogers, R. R.; Cook, A. L.; Haper, D. B.

2008-01-01

Aerosol extinction profiles are derived from backscatter data by constraining the retrieval with column aerosol optical thickness (AOT), for example from coincident MODIS observations and without reliance on a priori assumptions about aerosol type or optical properties. The backscatter data were acquired with the NASA Langley High Spectral Resolution Lidar (HSRL). The HSRL also simultaneously measures extinction independently, thereby providing an ideal data set for evaluating the constrained retrieval of extinction from backscatter. We will show constrained extinction retrievals using various sources of column AOT, and examine comparisons with the HSRL extinction measurements and with a similar retrieval using data from the CALIOP lidar on the CALIPSO satellite.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

NASA Astrophysics Data System (ADS)

Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; Denier van der Gon, Hugo A. C.; Crippa, Monica; Prévôt, André S. H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.

2016-03-01

We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 µg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

NASA Astrophysics Data System (ADS)

Fountoukis, C.; Megaritis, A. G.; Skyllakou, K.; Charalampidis, P. E.; Denier van der Gon, H. A. C.; Crippa, M.; Prévôt, A. S. H.; Freutel, F.; Wiedensohler, A.; Pilinis, C.; Pandis, S. N.

2015-09-01

We use a three dimensional regional chemical transport model (PMCAMx) with high grid resolution and high resolution emissions (4 km × 4 km) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (Megacities: Emissions, urban, regional, and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 μg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 μg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 μg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Cluster analysis of the organic peaks in bulk mass spectra obtained during the 2002 New England Air Quality Study with an Aerodyne aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Marcolli, C.; Canagaratna, M. R.; Worsnop, D. R.; Bahreini, R.; de Gouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; Lerner, B. M.; Roberts, J. M.; Meagher, J. F.; Fehsenfeld, F. C.; Marchewka, M. L.; Bertman, S. B.; Middlebrook, A. M.

2006-06-01

We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel Ronald H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter most probably originating from both, anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent as much as 5 µg/m3 organic aerosol mass - 17% of the total organic mass - that can be attributed to biogenic sources. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

Secondary organic aerosol formation from low-NO(x) photooxidation of dodecane: evolution of multigeneration gas-phase chemistry and aerosol composition.

PubMed

Yee, Lindsay D; Craven, Jill S; Loza, Christine L; Schilling, Katherine A; Ng, Nga Lee; Canagaratna, Manjula R; Ziemann, Paul J; Flagan, Richard C; Seinfeld, John H

2012-06-21

The extended photooxidation of and secondary organic aerosol (SOA) formation from dodecane (C(12)H(26)) under low-NO(x) conditions, such that RO(2) + HO(2) chemistry dominates the fate of the peroxy radicals, is studied in the Caltech Environmental Chamber based on simultaneous gas and particle-phase measurements. A mechanism simulation indicates that greater than 67% of the initial carbon ends up as fourth and higher generation products after 10 h of reaction, and simulated trends for seven species are supported by gas-phase measurements. A characteristic set of hydroperoxide gas-phase products are formed under these low-NO(x) conditions. Production of semivolatile hydroperoxide species within three generations of chemistry is consistent with observed initial aerosol growth. Continued gas-phase oxidation of these semivolatile species produces multifunctional low volatility compounds. This study elucidates the complex evolution of the gas-phase photooxidation chemistry and subsequent SOA formation through a novel approach comparing molecular level information from a chemical ionization mass spectrometer (CIMS) and high m/z ion fragments from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Combination of these techniques reveals that particle-phase chemistry leading to peroxyhemiacetal formation is the likely mechanism by which these species are incorporated in the particle phase. The current findings are relevant toward understanding atmospheric SOA formation and aging from the "unresolved complex mixture," comprising, in part, long-chain alkanes.

High Resolution Mass Spectrometry of Seasonal Aerosol Samples From an Urban Location in the Italian Po Valley

NASA Astrophysics Data System (ADS)

Mahon, Brendan; Giorio, Chiara; Gallimore, Peter J.; Zielinski, Arthur T.; Tapparo, Andrea; Kalberer, Markus

2016-04-01

The Po Valley in Northern Italy represents one of the most polluted environments in Europe, with PM2.5 and ozone concentrations regularly exceeding 100μg/m3 and 50ppb respectively. Particularly during winter, prolonged inversion conditions together with biomass burning and anthropogenic emissions regularly lead to severe air pollution events. Over the course of several months in 2013-14, we carried out a sampling program at a city-centre site in Padova, Italy, collecting 24-hour high-volume aerosol filter samples, 18 in winter (mid December - mid March) and 20 in summer (late May - late July). Utilising high-resolution Orbitrap mass spectrometry techniques, we have characterised these sample sets to examine the long-term variation in aerosol composition over the sampling campaign and to determine the effect of anthropogenic gaseous pollutants such as NOx and SO2 on the composition of organic particle components. The results showed that between ca. 450-700 ions were measured in each sample in both the summer and winter sample sets, however the majority (90%) of ions in the winter samples were below 300m/z and below 380m/z in the summer samples. A much higher percentage of CHO-only ions were found in winter (ca. 27%) compared to the summer samples (ca. 6%), indicating a higher degree of photochemical reactions taking place involving pollutants such as NOx and SO2 in summer. Our results represent the first long term data set of high-resolution measurements of aerosol composition and demonstrate that this technique is an important tool in evaluating the composition of aerosol particles in complex polluted urban areas.

Predicting Cavitation on Marine and Hydrokinetic Turbine Blades with AeroDyn V15.04

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

Murray, Robynne

Cavitation is an important consideration in the design of marine and hydrokinetic (MHK) turbines. The National Renewable Energy Laboratory's AeroDyn performance code was originally developed for horizontal-axis wind turbines and did not have the capability to predict cavitation inception. Therefore, AeroDyn has been updated to include the ability to predict cavitation on MHK turbines based on user-specified vapor pressure and submerged depth. This report outlines a verification of the AeroDyn V15.04 performance code for MHK turbines through a comparison to publicly available performance data.

Chemical composition of aerosol measurements in the air pollution plume during KORUS-AQ

NASA Astrophysics Data System (ADS)

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

2017-12-01

The Korean peninsula is a great place to study different sources of the aerosols: urban, rural and marine. In addition, Seoul is one of the large metropolitan areas in the world and has a variety of sources because half of the Korean population lives in Seoul, which comprises only 12% of the country's area. To understand the chemical composition of aerosol form long-range transport and local sources better, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on an airborne platform (NASA DC-8 aircraft). The HR-ToF-AMS is capable of measuring non-refractory size resolved chemical composition of submicron particle(NR-PM1) in the air pollution plume, including mass concentration of organic carbon, nitrate, sulfate, and ammonium with 10 seconds time resolution. The measurements were performed twenty times research flight for understanding characteristic of the air pollution from May to June, 2016 on the South Korean peninsula during KORUS-AQ 2016 campaign. The scientific goal of this study is to characterize aerosol chemical properties and mass concentration in order to understand the role of the long-range transport from northeast Asia to South Korea, and influence of the local sources. To brief, organics dominated during all of flights. Also, organics and nitrate were dominant around energy industrial complex near by Taean, South Korea. The presentation will provide an overview of the composition of NR-PM1 measured in air pollution plumes, and deliver detail information about width, depth and spatial distribution of the pollutant in the air pollution plumes. The results of this study will provide high temporal and spatial resolved details on the air pollution plumes, which are valuable input parameters of aerosol properties for the current air quality models.

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

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.;

Aerosol midlatitude cyclone indirect effects in observations and high-resolution simulations

NASA Astrophysics Data System (ADS)

McCoy, Daniel T.; Field, Paul R.; Schmidt, Anja; Grosvenor, Daniel P.; Bender, Frida A.-M.; Shipway, Ben J.; Hill, Adrian A.; Wilkinson, Jonathan M.; Elsaesser, Gregory S.

2018-04-01

Aerosol-cloud interactions are a major source of uncertainty in inferring the climate sensitivity from the observational record of temperature. The adjustment of clouds to aerosol is a poorly constrained aspect of these aerosol-cloud interactions. Here, we examine the response of midlatitude cyclone cloud properties to a change in cloud droplet number concentration (CDNC). Idealized experiments in high-resolution, convection-permitting global aquaplanet simulations with constant CDNC are compared to 13 years of remote-sensing observations. Observations and idealized aquaplanet simulations agree that increased warm conveyor belt (WCB) moisture flux into cyclones is consistent with higher cyclone liquid water path (CLWP). When CDNC is increased a larger LWP is needed to give the same rain rate. The LWP adjusts to allow the rain rate to be equal to the moisture flux into the cyclone along the WCB. This results in an increased CLWP for higher CDNC at a fixed WCB moisture flux in both observations and simulations. If observed cyclones in the top and bottom tercile of CDNC are contrasted it is found that they have not only higher CLWP but also cloud cover and albedo. The difference in cyclone albedo between the cyclones in the top and bottom third of CDNC is observed by CERES to be between 0.018 and 0.032, which is consistent with a 4.6-8.3 Wm-2 in-cyclone enhancement in upwelling shortwave when scaled by annual-mean insolation. Based on a regression model to observed cyclone properties, roughly 60 % of the observed variability in CLWP can be explained by CDNC and WCB moisture flux.

High Spectral Resolution Lidar: System Calibration

NASA Astrophysics Data System (ADS)

Vivek Vivekanandan, J.; Morley, Bruce; Spuler, Scott; Eloranta, Edwin

2015-04-01

One of the unique features of the high spectral resolution lidar (HSRL) is simultaneous measurements of backscatter and extinction of atmosphere. It separates molecular scattering from aerosol and cloud particle backscatter based on their Doppler spectrum width. Scattering from aerosol and cloud particle are referred as Mie scattering. Molecular or Rayleigh scattering is used as a reference for estimating aerosol extinction and backscatter cross-section. Absolute accuracy of the backscattered signals and their separation into Rayleigh and Mie scattering depends on spectral purity of the transmitted signals, accurate measurement of transmit power, and precise performance of filters. Internal calibration is used to characterize optical subsystems Descriptions of high spectral resolution lidar system and its measurement technique can be found in Eloronta (2005) and Hair et al.(2001). Four photon counting detectors are used to measure the backscatter from the combined Rayleigh and molecular scattering (high and low gain), molecular scattering and cross-polarized signal. All of the detectors are sensitive to crosstalk or leakage through the optical filters used to separate the received signals and special data files are used to remove these effects as much as possible. Received signals are normalized with respect to the combined channel response to Mie and Rayleigh scattering. The laser transmit frequency is continually monitored and tuned to the 1109 Iodine absorption line. Aerosol backscatter cross-section is measured by referencing the aerosol return signal to the molecular return signal. Extinction measurements are calculated based on the differences between the expected (theoretical) and actual change in the molecular return. In this paper an overview of calibration of the HSRL is presented. References: Eloranta, E. W., High Spectral Resolution Lidar in Lidar: Range-Resolved Optical Remote Sensing of the Atmosphere, Klaus Weitkamp editor, Springer Series in Optical

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.

Characterizing Aerosol Distributions and Optical Properties Using the NASA Langley High Spectral Resolution Lidar

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

Hostetler, Chris; Ferrare, Richard

The objective of this project was to provide vertically and horizontally resolved data on aerosol optical properties to assess and ultimately improve how models represent these aerosol properties and their impacts on atmospheric radiation. The approach was to deploy the NASA Langley Airborne High Spectral Resolution Lidar (HSRL) and other synergistic remote sensors on DOE Atmospheric Science Research (ASR) sponsored airborne field campaigns and synergistic field campaigns sponsored by other agencies to remotely measure aerosol backscattering, extinction, and optical thickness profiles. Synergistic sensors included a nadir-viewing digital camera for context imagery, and, later in the project, the NASA Goddard Institutemore » for Space Studies (GISS) Research Scanning Polarimeter (RSP). The information from the remote sensing instruments was used to map the horizontal and vertical distribution of aerosol properties and type. The retrieved lidar parameters include profiles of aerosol extinction, backscatter, depolarization, and optical depth. Products produced in subsequent analyses included aerosol mixed layer height, aerosol type, and the partition of aerosol optical depth by type. The lidar products provided vertical context for in situ and remote sensing measurements from other airborne and ground-based platforms employed in the field campaigns and was used to assess the predictions of transport models. Also, the measurements provide a data base for future evaluation of techniques to combine active (lidar) and passive (polarimeter) measurements in advanced retrieval schemes to remotely characterize aerosol microphysical properties. The project was initiated as a 3-year project starting 1 January 2005. It was later awarded continuation funding for another 3 years (i.e., through 31 December 2010) followed by a 1-year no-cost extension (through 31 December 2011). This project supported logistical and flight costs of the NASA sensors on a dedicated aircraft, the

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated

High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

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

Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia

2010-10-01

This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities,more » types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.« less

Operational remote sensing of tropospheric aerosol over land from EOS moderate resolution imaging spectroradiometer

NASA Astrophysics Data System (ADS)

Kaufman, Y. J.; Tanré, D.; Remer, L. A.; Vermote, E. F.; Chu, A.; Holben, B. N.

1997-07-01

Daily distribution of the aerosol optical thickness and columnar mass concentration will be derived over the continents, from the EOS moderate resolution imaging spectroradiometer (MODIS) using dark land targets. Dark land covers are mainly vegetated areas and dark soils observed in the red and blue channels; therefore the method will be limited to the moist parts of the continents (excluding water and ice cover). After the launch of MODIS the distribution of elevated aerosol concentrations, for example, biomass burning in the tropics or urban industrial aerosol in the midlatitudes, will be continuously monitored. The algorithm takes advantage of the MODIS wide spectral range and high spatial resolution and the strong spectral dependence of the aerosol opacity for most aerosol types that result in low optical thickness in the mid-IR (2.1 and 3.8 μm). The main steps of the algorithm are (1) identification of dark pixels in the mid-IR; (2) estimation of their reflectance at 0.47 and 0.66 μm; and (3) derivation of the optical thickness and mass concentration of the accumulation mode from the detected radiance. To differentiate between dust and aerosol dominated by accumulation mode particles, for example, smoke or sulfates, ratios of the aerosol path radiance at 0.47 and 0.66 μm are used. New dynamic aerosol models for biomass burning aerosol, dust and aerosol from industrial/urban origin, are used to determine the aerosol optical properties used in the algorithm. The error in the retrieved aerosol optical thicknesses, τa is expected to be Δτa = 0.05±0.2τa. Daily values are stored on a resolution of 10×10 pixels (1 km nadir resolution). Weighted and gridded 8-day and monthly composites of the optical thickness, the aerosol mass concentration and spectral radiative forcing are generated for selected scattering angles to increase the accuracy. The daily aerosol information over land and oceans [Tanré et al., this issue], combined with continuous aerosol remote

Aerosol mass spectrometric features of biogenic SOA: observations from a plant chamber and in rural atmospheric environments.

PubMed

Kiendler-Scharr, Astrid; Zhang, Qi; Hohaus, Thorsten; Kleist, Einhard; Mensah, Amewu; Mentel, Thomas F; Spindler, Christian; Uerlings, Ricarda; Tillmann, Ralf; Wildt, Jürgen

2009-11-01

Secondary organic aerosol (SOA) is known to form from a variety of anthropogenic and biogenic precursors. Current estimates of global SOA production vary over 2 orders of magnitude. Since no direct measurement technique for SOA exists, quantifying SOA remains a challenge for atmospheric studies. The identification of biogenic SOA (BSOA) based on mass spectral signatures offers the possibility to derive source information of organic aerosol (OA) with high time resolution. Here we present data from simulation experiments. The BSOA from tree emissions was characterized with an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS). Collection efficiencies were close to 1, and effective densities of the BSOA were found to be 1.3 +/- 0.1 g/cm(3). The mass spectra of SOA from different trees were found to be highly similar. The average BSOA mass spectrum from tree emissions is compared to a BSOA component spectrum extracted from field data. It is shown that overall the spectra agree well and that the mass spectral features of BSOA are distinctively different from those of OA components related to fresh fossil fuel and biomass combustions. The simulation chamber mass spectrum may potentially be useful for the identification and interpretation of biogenic SOA components in ambient data sets.

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

PubMed

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

Development of a High Spectral Resolution Lidar (HSRL) Based on a Confocal Optical Filter for Aerosol Studies

NASA Astrophysics Data System (ADS)

Repasky, K. S.; Hoffman, D. S.; Reagan, J. A.; Carlsten, J.

2010-12-01

Aerosols are an important constituent in atmospheric composition affecting climate, weather, and air quality. Active remote sensing instruments provide tools for in-situ studies of atmospheric aerosols that can help understand the role of aerosols on the radiative forcing of the climate system. In this paper, the design and initial performance of a high spectral resolution lidar (HSRL) based on a unique confocal cavity for optically filtering the aerosol and molecular returns is presented. An injection seeded pulsed Nd:YAG laser with a fundamental and frequency doubled output is used as the laser transmitter for the HSRL. A small portion of fiber coupled injection seeded signal at 1064 nm is split before the laser oscillator and, after modulation using an acousto-optic modulator, is used to produce a discriminating signal for locking a confocal cavity that is resonant at the 1064 and 532 nm wavelengths to the injection seeded source. Light scattered in the atmosphere is collected using a commercial telescope. After the telescope, the 1064 nm light is split from the 532 nm light using a dielectric mirror with the 1064 nm light monitored using a PMT. The 532 nm light is launched into a multimode fiber. The output from the fiber is next incident on a beamsplitter with part of the light sent to a PMT to monitor the total return for the 532 nm channel. The light that passes through the beamsplitter is mode matched into a confocal optical cavity that allows the light scattered by the atmospheric aerosols to be transmitted while the light scattered from the atmospheric molecules is reflected. The transmitted light from the aerosol scattering is incident on a PMT while the reflected molecular signal is incident on a PMT. The transmission of the confocal cavity is monitored before and after the data collection using a continuous wave frequency doubled Nd:YAG laser that is fiber coupled. Data is collected and processed in the following manner. Each of the four voltage

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

Cluster Analysis of the Organic Peaks in Bulk Mass Spectra Obtained During the 2002 New England Air Quality Study with an Aerodyne Aerosol Mass Spectrometer

NASA Astrophysics Data System (ADS)

Marcolli, C.; Canagaratna, M. R.; Worsnop, D. R.; Bahreini, R.; de Gouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; Lerner, B. M.; Roberts, J. M.; Meagher, J. F.; Fehsenfeld, F. C.; Marchewka, M.; Bertman, S. B.; Middlebrook, A. M.

2006-12-01

We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel R. H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter probably originating from both anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent on average 17% of the total organic mass that stems likely from biogenic sources during the ship's cruise. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

Aircraft-Based measurement of the physico-chemical evolution of atmospheric aerosols in the air pollution plume over a megacity and a remote area

NASA Astrophysics Data System (ADS)

Park, J. S.; Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Kim, J.; Park, S.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly (scattering and absorption) and indirectly (cloud condensation nuclei), also adverse health effects. The Korean peninsula is a great place to study different sources of the aerosols: urban, rural and marine. In addition, Seoul is one of the large metropolitan areas in the world and has a variety of sources because half of the Korean population lives in Seoul, which comprises only 12% of the country's area. To understand the physico-chemical evolution of atmospheric aerosols in the air pollution plume over a megacity and a remote area, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on an airborne platform (NASA DC-8 and Beechcraft King Air) in June, 2015 and May-June, 2016 during MAPS-Seoul and KORUS-AQ campaigns, respectively, in Korea. The HR-ToF-AMS is capable of measuring non-refractory size resolved chemical composition of submicron particle (NR-PM1). NR-PM1 includes mass concentration of organics, nitrate, sulfate, and ammonium with 10 seconds time resolution. Organics was dominated species in aerosol during all of flights. Organics and nitrate were dominant around energy industrial complex near by Taean, South Korea. The presentation will provide an overview of the composition of NR-PM1 measured in air pollution plumes, and deliver detail information about width, depth and spatial distribution of the pollutant in the air pollution plumes. The results of this study will provide high temporal and spatial resolved details on the air pollution plumes, which are valuable input parameters of aerosol properties for the current air quality models.

Evolution of Asian aerosols during transpacific transport in INTEX-B

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

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

2009-10-01

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

Chemical Composition and Source Apportionment of high temporal resolution PM1 data for January-August 2017 in Delhi, India

NASA Astrophysics Data System (ADS)

Bhandari, S.; Wang, D. S.; Gani, S.; Seraj, S.; Arub, Z.; Habib, G.; Apte, J.; Hildebrandt Ruiz, L.

2017-12-01

Exposure to fine particulate matter (PM) poses significant health risks, especially to residents in heavily populated areas. The current understanding of the sources and dynamics of PM pollution in developing countries like India is limited. Delhi, India is the second most populated city in the world that has extremely high winter PM concentrations and frequent severe pollution episodes. This study reports on composition measurements of submicron aerosol at 1 minute time resolution from January to August of 2017, collected at the Indian Institute of Technology Delhi using an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and black carbon (BC) measurements using an Aethalometer. Source apportionment was conducted on organic and inorganic mass spectra measured by the ACSM and black carbon data measured using Positive Matrix Factorization (PMF). High concentrations of particulate matter were observed with total PM1 at times exceeding 200 µg m-3 in winter. A significant drop in PM1 concentrations was observed in the winter-spring transition. As observed elsewhere, organic species dominated the submicron mass, contributing 60% of the total mass over the duration of the campaign. However, this fractional contribution varied substantially over the day: from 48% early in the morning to 73% late at night. Along with diurnal variation in total PM1 mass loadings, particulate chloride levels also exhibited a strong diurnal cycle, with concentrations as high as 50 µg m-3 observed in the early mornings of January 2017. Literature review on identification of winter chloride sources in Delhi points to local and regional sources such as biomass/open-waste burning and coal combustion. PMF receptor modeling identified several factors with distinct diurnal patterns. While hydrocarbon-like organic aerosol (HOA) factor has the largest mass fraction contribution, PMF results consistently suggest chloride presence as attributable to ammonium chloride. Interestingly, aerosol

Measurement of the temperature dependent partitioning of semi-volatile organics onto aerosol near roadways

NASA Astrophysics Data System (ADS)

Wentzell, J. J.; Liggio, J.; Li, S.; Brook, J.; Staebler, R. M.; Evans, G. J.; Jeong, C.; Sheppard, A.; Lu, G.; Gordon, M.; Mihele, C.

2010-12-01

The volatility of the organic aerosol fraction has received a great deal of attention recently in light of new volatility-based modelling approaches and due to the inability of current models to fully account for secondary organic aerosol (SOA). In this regard, evaporation of primary organic aerosol species and their subsequent oxidation may contribute significantly to SOA downwind of sources. This implies that moderate ambient temperature fluctuations can significantly increase or decrease the aerosol bound fraction of semi-volatile and intermediate volatility (SVOC + IVOC) compounds. In order to examine the importance of these more volatile organic components, a temperature controlled inlet was developed with the ability to heat and cool the aerosol in 2 C increments to 15 C above or below ambient temperature. The inlet was coupled to an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and deployed on a mobile platform upwind and downwind of a major Southern Ontario highway as part of the Fast Evolution of Vehicle Emissions near Roadways (FEVER 2010) campaign. Preliminary results suggest that changes in temperature of 5-10 C can alter the partitioning of volatile organic aerosol components by up to 30%. Although the largest affect was observed 10-13 meters downwind of the vehicle emissions, a measurable affect was observed beyond 500 m and in aerosol upwind of the highway. These results suggest that a significant pool of semi-volatile organics exist, which can condense onto particles at slightly lower temperatures or evaporate to the gas phase and be further oxidized. The nature of these organic species at locations upwind and downwind of vehicle emissions will be discussed.

Evaluation of Organic Aerosol Formation and Apportionment in a polluted Megacity

NASA Astrophysics Data System (ADS)

Tsimpidi, A. P.; Karydis, V. A.; Zavala, M.; Lei, W.; Decarlo, P. F.; Ulbrich, I.; Jimenez, J. L.; Molina, L. T.; Pandis, S. N.

2009-04-01

Pollution from megacities and large urban areas is important not only for local effects on health, visibility, and ecosystems but also because of their collective influence on atmospheric chemistry and radiative forcing in regional and global scale. Organic species account for a large fraction of the submicron aerosol mass at most megacities. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) have been difficult to quantify. In this study, new primary and secondary organic aerosol modules were added to PMCAMx, a three dimensional chemical transport model (Gaydos et al., 2007). The new modeling framework is based on the volatility basis-set approach (Lane et al., 2007): both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments (Robinson et al., 2007). PMCAMx is applied in the Mexico City Metropolitan Area during April 2003 and March 2006. The model predictions are compared with Aerodyne's Aerosol Mass Spectrometer (AMS) observations from the MCMA and MILAGRO campaigns respectively. Furthermore, the predicted concentrations over Mexico City are compared against measurements from a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) which was onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign (DeCarlo et al., 2008). The organic aerosol (OA) to CO ratio is used as an indicator in order to evaluate the photo-oxidation of the predicted OA after its horizontal and vertical advection. References Gaydos, T.M.; Pinder, R.W.; Koo, B.; Fahey, K.M.; Pandis, S.N., 2007. Development and application of a three-dimensional aerosol chemical transport model, PMCAMx. Atmospheric Environment 41, 2594-2611. Lane, T

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Real time measurements of submicrometer aerosols in Seoul, Korea: Sources, characteristics, and processing of organic aerosols during winter time.

NASA Astrophysics Data System (ADS)

Kim, H.; Zhang, Q.

2016-12-01

Highly time-resolved chemical characterization of non-refractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter when persistent air quality problems associated with elevated PM concentrations were observed. The average NR-PM1 concentration was 27.5 µg m-3 and the average mass was dominated by organics (44%), followed by nitrate (24%) and sulfate (10%). Five distinct sources of organic aerosol (OA) were identified from positive matrix factorization (PMF) analysis of the AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA), cooking represented by a cooking OA factor (COA), wood combustion represented by a biomass burning OA factor (BBOA), and secondary aerosol formation in the atmosphere that is represented by a semi-volatile oxygenated OA factor (SVOOA) and a low volatile oxygenated OA factor (LVOOA). These factors, on average, contributed 16, 20, 23, 15 and 26% to the total OA mass, respectively, with primary organic aerosol (POA = HOA + COA + BBOA) accounting for 59% of the OA mass. On average, both primary emissions and secondary aerosol formation are important factors affecting air quality in Seoul during winter, contributing approximately equal. However, differences in the fraction of PM source and properties were observed between high and low loading PM period. For example, during stagnant period with low wind speed (WS) (0.99 ± 0.7 m/s) and high RH (71%), high PM loadings (43.6 ± 12.4 µg m-3) with enhanced fractions of nitrate (27%) and SVOOA (8%) were observed, indicating a strong influence from locally generated secondary aerosol. On the other hand, when low PM loadings (12.6 ± 7.1 µg m-3), which were commonly associated with high WS (1.8 ± 1.1 m/s) and low RH (50 %), were observed, the fraction of regional sources, such as sulfate (12%) and LVOOA (21

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.

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

Moderate Imaging Resolution Spectroradiometer (MODIS) Aerosol Optical Depth Retrieval for Aerosol Radiative Forcing

NASA Astrophysics Data System (ADS)

Asmat, A.; Jalal, K. A.; Ahmad, N.

2018-02-01

The present study uses the Aerosol Optical Depth (AOD) retrieved from Moderate Imaging Resolution Spectroradiometer (MODIS) data for the period from January 2011 until December 2015 over an urban area in Kuching, Sarawak. The results show the minimum AOD value retrieved from MODIS is -0.06 and the maximum value is 6.0. High aerosol loading with high AOD value observed during dry seasons and low AOD monitored during wet seasons. Multi plane regression technique used to retrieve AOD from MODIS (AODMODIS) and different statistics parameter is proposed by using relative absolute error for accuracy assessment in spatial and temporal averaging approach. The AODMODIS then compared with AOD derived from Aerosol Robotic Network (AERONET) Sunphotometer (AODAERONET) and the results shows high correlation coefficient (R2) for AODMODIS and AODAERONET with 0.93. AODMODIS used as an input parameters into Santa Barbara Discrete Ordinate Radiative Transfer (SBDART) model to estimate urban radiative forcing at Kuching. The observed hourly averaged for urban radiative forcing is -0.12 Wm-2 for top of atmosphere (TOA), -2.13 Wm-2 at the surface and 2.00 Wm-2 in the atmosphere. There is a moderate relationship observed between urban radiative forcing calculated using SBDART and AERONET which are 0.75 at the surface, 0.65 at TOA and 0.56 in atmosphere. Overall, variation in AOD tends to cause large bias in the estimated urban radiative forcing.

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

NASA Astrophysics Data System (ADS)

Rao, Roshan

2016-04-01

Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. We look into the approach where ground based spectral radiation flux measurement is made and along with an Radtiative transfer (RT) model, radiative forcing is estimated. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and a 3nm resolution during around 54 clear-sky days during which AOD range was around 0.01 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. The primary study involved in understanding the sensitivity of spectral flux due to change in individual aerosol species (Optical properties of Aerosols and Clouds (OPAC) classified aerosol species) using the SBDART RT model. This made us clearly distinguish the influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves matching different combinations of aerosol species in OPAC model and RT model as long as the combination which gives the minimum root mean squared deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model, aerosol radiative forcing is estimated. Also an alternate method to estimate the spectral SSA is discussed. Here, the RT model, the observed spectral flux and spectral AOD is used. Spectral AOD is input to RT model and SSA is varied till the minimum root mean squared difference between observed and simulated spectral flux from RT model is obtained. The methods discussed are limited to clear sky scenes and its accuracy to derive

Characterizing aerosol transport into the Canadian High Arctic using aerosol mass spectrometry and Lagrangian modelling

NASA Astrophysics Data System (ADS)

Kuhn, T.; Damoah, R.; Bacak, A.; Sloan, J. J.

2010-05-01

We report the analysis of measurements made using an aerosol mass spectrometer (AMS; Aerodyne Research Inc.) that was installed in the Polar Environment Atmospheric Research Laboratory (PEARL) in summer 2006. PEARL is located in the Canadian high Arctic at 610 m above sea level on Ellesmere Island (80° N 86° W). PEARL is unique for its remote location in the Arctic and because most of the time it is situated within the free troposphere. It is therefore well suited as a receptor site to study the long range tropospheric transport of pollutants into the Arctic. Some information about the successful year-round operation of an AMS at a high Arctic site such as PEARL will be reported here, together with design considerations for reliable sampling under harsh low-temperature conditions. Computational fluid dynamics calculations were made to ensure that sample integrity was maintained while sampling air at temperatures that average -40 °C in the winter and can be as low as -55 °C. Selected AMS measurements of aerosol mass concentration, size, and chemical composition recorded during the months of August, September and October 2006 will be reported. During this period, sulfate was at most times the predominant aerosol component with on average 0.115 μg m-3 (detection limit 0.003 μg m-3). The second most abundant component was undifferentiated organic aerosol, with on average 0.11 μg m-3 detection limit (0.04 μg m-3). The nitrate component, which averaged 0.007 μg m-3, was above its detection limit (0.002 μg m-3), whereas the ammonium ion had an apparent average concentration of 0.02 μg m-3, which was approximately equal to its detection limit. A few episodes having increased mass concentrations and lasting from several hours to several days are apparent in the data. These were investigated further using a statistical analysis to determine their common characteristics. High correlations among some of the components arriving during the short term episodes provide

Synchronised Aerosol Mass Spectrometer Measurements across Europe

NASA Astrophysics Data System (ADS)

Nemitz, Eiko

2010-05-01

sites concentrations of inorganic precursor gases (e.g. NH3, HNO3, SO2) were measured simultaneously, mainly with a denuder based wet chemistry technique. The database provides a powerful dataset against which to compare the performance of European scale Chemistry and Transport Models (CTMs) in reproducing transport patterns, thermodynamics (e.g. daytime vs. night-time concentrations and gas/aerosol partitioning) and organic aerosol partitioning (e.g. primary versus oxidised aerosol). Future analysis will include a detailed analysis of the organic aerosol composition, through statistical factor analysis and based on the high mass resolution data provided by a subset of the AMS instruments.

Time-Resolved Molecular Characterization of Limonene/Ozone Aerosol using High-Resolution Electrospray Ionization Mass Spectrometry

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

Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia

2009-09-09

Molecular composition of limonene/O3 secondary organic aerosol (SOA) was investigated using high-resolution electrospray ionization mass spectrometry (HR-ESI-MS) as a function of reaction time. SOA was generated by ozonation of D-limonene in a reaction chamber and sampled at different time intervals using a cascade impactor. The SOA samples were extracted into acetonitrile and analyzed using a HR-ESI-MS instrument with a resolving power of 100,000 (m/Δm). The resulting mass spectra provided detailed information about the extent of oxidation inferred from the O:C ratios, double bond equivalency (DBE) factors, and aromaticity indexes (AI) in hundreds of identified individual SOA species.

Near-Cloud Aerosol Properties from the 1 Km Resolution MODIS Ocean Product

NASA Technical Reports Server (NTRS)

Varnai, Tamas; Marshak, Alexander

2014-01-01

This study examines aerosol properties in the vicinity of clouds by analyzing high-resolution atmospheric correction parameters provided in the MODIS (Moderate Resolution Imaging Spectroradiometer) ocean color product. The study analyzes data from a 2 week long period of September in 10 years, covering a large area in the northeast Atlantic Ocean. The results indicate that on the one hand, the Quality Assessment (QA) flags of the ocean color product successfully eliminate cloud-related uncertainties in ocean parameters such as chlorophyll content, but on the other hand, using the flags introduces a sampling bias in atmospheric products such as aerosol optical thickness (AOT) and Angstrom exponent. Therefore, researchers need to select QA flags by balancing the risks of increased retrieval uncertainties and sampling biases. Using an optimal set of QA flags, the results reveal substantial increases in optical thickness near clouds-on average the increase is 50% for the roughly half of pixels within 5 km from clouds and is accompanied by a roughly matching increase in particle size. Theoretical simulations show that the 50% increase in 550nm AOT changes instantaneous direct aerosol radiative forcing by up to 8W/m2 and that the radiative impact is significantly larger if observed near-cloud changes are attributed to aerosol particles as opposed to undetected cloud particles. These results underline that accounting for near-cloud areas and understanding the causes of near-cloud particle changes are critical for accurate calculations of direct aerosol radiative forcing.

Evaluating Satellite Retrievals of Smoke Aerosol above Clouds using Airborne High Spectral Resolution Lidar Measurements during ORACLES

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Burton, S. P.; Cook, A. L.; Harper, D. B.; Hostetler, C. A.; Hair, J. W.; Vaughan, M.; Hu, Y.; Fenn, M. A.; Clayton, M.; Scarino, A. J.; Jethva, H. T.; Sayer, A. M.; Meyer, K.; Torres, O.; Josset, D. B.; Redemann, J.

2017-12-01

The NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-2) provided extensive measurements of smoke above shallow marine clouds while deployed from the NASA ER-2 aircraft during the NASA EV-S Observations of Aerosols above Clouds and their Interactions (ORACLES) mission. During the first ORACLES field campaign in September 2016, the ER-2 was deployed from Walvis Bay, Namibia and conducted flights over the southeastern Atlantic Ocean. HSRL-2 measured profiles of aerosol backscattering, extinction and aerosol optical depth (AOD) at 355 and 532 nm and aerosol backscattering and depolarization at 1064 nm and so provided an excellent characterization of the widespread smoke layers above shallow marine clouds. OMI, MODIS, and CALIOP satellite retrievals of above cloud AOD (ACAOD) are compared to the HSRL-2 measurements. The OMI above-cloud aerosols data product (OMACA) ACAOD product relies on the spectral contrast produced by aerosol absorption in two near-UV measurements (354 and 388 nm) to derive ACAOD. Two MODIS ACAOD products are examined; the first ("multichannel') relies on the spectral contrast in aerosol absorption derived from reflectance measurements at six MODIS channels from the visible to the shortwave infrared (swIR). The second method is an extension of the "Deep Blue" method and differs from the multichannel method in that it does not use swIR channels. The CALIOP V4 operational and "depolarization ratio (DR)" methods of retrieving ACAOD are also examined. The MODIS and OMI ACAOD values were well correlated (r2>0.6) with the HSRL-2 ACAOD values; bias differences were generally less than about 0.1 at 532 nm (10-30%). The CALIOP operational retrievals missed a significant amount of aerosol and so were biased low by 50-75% compared to HSRL-2. In contrast, the CALIOP DR method produced ACAOD values in excellent agreement (bias differences less than 0.03 (5%)) with HSRL-2. Aerosol extinction profiles computed for the smoke layer using

Evaluation of applicability of high-resolution multiangle imaging photo-polarimetric observations for aerosol atmospheric correction

NASA Astrophysics Data System (ADS)

Kalashnikova, Olga; Garay, Michael; Xu, Feng; Diner, David; Seidel, Felix

2016-07-01

Multiangle spectro-polarimetric measurements have been advocated as an additional tool for better understanding and quantifying the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of this work is the assessment of the effects of absorbing aerosol properties on remote sensing reflectance measurement uncertainty caused by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. In this work a vector Markov Chain radiative transfer code including bio-optical models was used to quantitatively evaluate in water leaving radiances between atmospheres containing realistic UV-enhanced and non-spherical aerosols and the SEADAS carbonaceous and dust-like aerosol models. The phase matrices for the spherical smoke particles were calculated using a standard Mie code, while those for non-spherical dust particles were calculated using the numerical approach developed for modeling dust for the AERONET network of ground-based sunphotometers. As a next step, we have developed a retrieval code that employs a coupled Markov Chain (MC) and adding/doubling radiative transfer method for joint retrieval of aerosol properties and water leaving radiance from Airborne Multiangle SpectroPolarimetric Imager-1 (AirMSPI-1) polarimetric observations. The AirMSPI-1 instrument has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. AirMSPI typically acquires observations of a target area at 9 view angles between ±67° at 10 m resolution. AirMSPI spectral channels are centered at 355, 380, 445, 470, 555, 660, and 865 nm, with 470, 660, and 865 reporting linear polarization. We

Aerosol correction for remotely sensed sea surface temperatures from the National Oceanic and Atmospheric Administration advanced very high resolution radiometer

NASA Astrophysics Data System (ADS)

Nalli, Nicholas R.; Stowe, Larry L.

2002-10-01

This research presents the first-phase derivation and implementation of daytime aerosol correction algorithms for remotely sensed sea surface temperature (SST) from the advanced very high resolution radiometer (AVHRR) instrument flown onboard NOAA polar orbiting satellites. To accomplish this, a long-term (1990-1998), global AVHRR-buoy match-up database was created by merging the NOAA/NASA Pathfinder Atmospheres and Pathfinder Oceans data sets. The merged data set is unique in that it includes daytime estimates of aerosol optical depth (AOD) derived from AVHRR channel 1 (0.63 μm) under global conditions of significant aerosol loading. Histograms of retrieved AOD reveal monomodal, lognormal distributions for both tropospheric and stratospheric aerosol modes. It is then shown empirically that the SST depression caused under each aerosol mode can be expressed as a linear function in two predictors, these being the slant path AOD retrieved from AVHRR channel 1 along with the ratio of channels 1 and 2 normalized reflectances. On the basis of these relationships, parametric equations are derived to provide an aerosol correction for retrievals from the daytime NOAA operational multichannel and nonlinear SST algorithms. Separate sets of coefficients are utilized for two aerosol modes: tropospheric (i.e., dust, smoke, haze) and stratospheric/tropospheric (i.e., following a major volcanic eruption). The equations are shown to significantly reduce retrieved SST bias using an independent set of match-ups. Eliminating aerosol-induced bias in both real-time and retrospective processing will enhance the utility of the AVHRR SST for the general user community and in climate research.

Applications of High-Resolution Electrospray Ionization Mass Spectrometry to Measurements of Average Oxygen to Carbon Ratios in Secondary Organic Aerosols

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

Bateman, Adam P.; Laskin, Julia; Laskin, Alexander

2012-07-02

The applicability of high resolution electrospray ionization mass spectrometry (HR ESI-MS) to measurements of the average oxygen to carbon ratio (O/C) in organic aerosols was investigated. Solutions with known average O/C containing up to 10 standard compounds representative of secondary organic aerosol (SOA) were analyzed and corresponding electrospray ionization efficiencies were quantified. The assumption of equal ionization efficiency commonly used in estimating O/C ratios of organic aerosols was found to be reasonably accurate. We found that the accuracy of the measured O/C ratios increases by averaging the values obtained from both (+) and (-) modes. A correlation was found betweenmore » the ratio of the ionization efficiencies in the positive and negative ESI modes with the octanol-water partition constant, and more importantly, with the compound's O/C. To demonstrate the utility of this correlation for estimating average O/C values of unknown mixtures, we analyzed the ESI (+) and ESI (-) data for SOA produced by oxidation of limonene and isoprene and compared to online O/C measurements using an aerosol mass spectrometer (AMS). This work demonstrates that the accuracy of the HR ESI-MS methods is comparable to that of the AMS, with the added benefit of molecular identification of the aerosol constituents.« less

Characterization of the aerosol over the sub-arctic north east Pacific Ocean

NASA Astrophysics Data System (ADS)

Phinney, Lisa; Richard Leaitch, W.; Lohmann, Ulrike; Boudries, Hacene; Worsnop, Douglas R.; Jayne, John T.; Toom-Sauntry, Desiree; Wadleigh, Moire; Sharma, Sangeeta; Shantz, Nicole

2006-10-01

Time series measurements of the size and composition of aerosol particles made near Ocean Station Papa during the Canadian SOLAS SERIES experiment in July 2002 indicate major contributions to the aerosol mass from the oxidation of dimethyl sulphide, from primary emissions of sea salt, and from ship emissions. The high temporal resolution of the AMS revealed significant variability in the fine mode species mass concentrations in this area. The background fine mode composition was dominated by non-sea-salt-sulphate (nss-SO 4), sea salt, organics, and methanesulphonic acid (MSA), with average mass concentrations of 0.74±0.04, 0.6±0.1, 0.3±0.1, and 0.16±0.05 μg m -3, respectively. The fine mode MSA:nss-SO 4 ratio varied from 0.01 to 3.19±0.2, with a mean of 0.23. The average fine mode mass distribution was internally mixed with a mode vacuum aerodynamic diameter of 475 nm. The concentration of MSA was an order of magnitude higher than previously reported values in the North Pacific, indicating significant oxidation of DMS. A diurnal signal in particulate products of DMS oxidation (i.e. MSA and sulphate) and in gaseous DMS and SO 2 indicates daytime photochemistry and in-cloud oxidation. A simple examination of chemical reaction pathways is used to help elucidate the relationships among the sulphur species and oxidants. The relationship between sea salt mass and wind speed is examined. This study marks the first time atmospheric measurements have been included in an iron enrichment experiment, and the first time an Aerodyne Aerosol Mass Spectrometer (AMS) has been deployed in a remote marine setting. Due to the proximity of the ship to the fertilized patch and the relatively high wind speeds, no impact of the SERIES iron fertilization on the local aerosol was observed.

Improved source apportionment of organic aerosols in complex urban air pollution using the multilinear engine (ME-2)

NASA Astrophysics Data System (ADS)

Zhu, Qiao; Huang, Xiao-Feng; Cao, Li-Ming; Wei, Lin-Tong; Zhang, Bin; He, Ling-Yan; Elser, Miriam; Canonaco, Francesco; Slowik, Jay G.; Bozzetti, Carlo; El-Haddad, Imad; Prévôt, André S. H.

2018-02-01

Organic aerosols (OAs), which consist of thousands of complex compounds emitted from various sources, constitute one of the major components of fine particulate matter. The traditional positive matrix factorization (PMF) method often apportions aerosol mass spectrometer (AMS) organic datasets into less meaningful or mixed factors, especially in complex urban cases. In this study, an improved source apportionment method using a bilinear model of the multilinear engine (ME-2) was applied to OAs collected during the heavily polluted season from two Chinese megacities located in the north and south with an Aerodyne high-resolution aerosol mass spectrometer (HR-ToF-AMS). We applied a rather novel procedure for utilization of prior information and selecting optimal solutions, which does not necessarily depend on other studies. Ultimately, six reasonable factors were clearly resolved and quantified for both sites by constraining one or more factors: hydrocarbon-like OA (HOA), cooking-related OA (COA), biomass burning OA (BBOA), coal combustion (CCOA), less-oxidized oxygenated OA (LO-OOA) and more-oxidized oxygenated OA (MO-OOA). In comparison, the traditional PMF method could not effectively resolve the appropriate factors, e.g., BBOA and CCOA, in the solutions. Moreover, coal combustion and traffic emissions were determined to be primarily responsible for the concentrations of PAHs and BC, respectively, through the regression analyses of the ME-2 results.

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

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

Simultaneous polarimeter retrievals of microphysical aerosol and ocean color parameters from the "MAPP" algorithm with comparison to high-spectral-resolution lidar aerosol and ocean products.

PubMed

Stamnes, S; Hostetler, C; Ferrare, R; Burton, S; Liu, X; Hair, J; Hu, Y; Wasilewski, A; Martin, W; van Diedenhoven, B; Chowdhary, J; Cetinić, I; Berg, L K; Stamnes, K; Cairns, B

2018-04-01

We present an optimal-estimation-based retrieval framework, the microphysical aerosol properties from polarimetry (MAPP) algorithm, designed for simultaneous retrieval of aerosol microphysical properties and ocean color bio-optical parameters using multi-angular total and polarized radiances. Polarimetric measurements from the airborne NASA Research Scanning Polarimeter (RSP) were inverted by MAPP to produce atmosphere and ocean products. The RSP MAPP results are compared with co-incident lidar measurements made by the NASA High-Spectral-Resolution Lidar HSRL-1 and HSRL-2 instruments. Comparisons are made of the aerosol optical depth (AOD) at 355 and 532 nm, lidar column-averaged measurements of the aerosol lidar ratio and Ångstrøm exponent, and lidar ocean measurements of the particulate hemispherical backscatter coefficient and the diffuse attenuation coefficient. The measurements were collected during the 2012 Two-Column Aerosol Project (TCAP) campaign and the 2014 Ship-Aircraft Bio-Optical Research (SABOR) campaign. For the SABOR campaign, 73% RSP MAPP retrievals fall within ±0.04 AOD at 532 nm as measured by HSRL-1, with an R value of 0.933 and root-mean-square deviation of 0.0372. For the TCAP campaign, 53% of RSP MAPP retrievals are within 0.04 AOD as measured by HSRL-2, with an R value of 0.927 and root-mean-square deviation of 0.0673. Comparisons with HSRL-2 AOD at 355 nm during TCAP result in an R value of 0.959 and a root-mean-square deviation of 0.0694. The RSP retrievals using the MAPP optimal estimation framework represent a key milestone on the path to a combined lidar + polarimeter retrieval using both HSRL and RSP measurements.

Organic aerosol in the summertime southeastern United States: components and their link to volatility distribution, oxidation state and hygroscopicity

NASA Astrophysics Data System (ADS)

Kostenidou, Evangelia; Karnezi, Eleni; Hite, James R., Jr.; Bougiatioti, Aikaterini; Cerully, Kate; Xu, Lu; Ng, Nga L.; Nenes, Athanasios; Pandis, Spyros N.

2018-04-01

The volatility distribution of the organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS; Centreville, Alabama) was constrained using measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a thermodenuder (TD). Positive matrix factorization (PMF) analysis was applied on both the ambient and thermodenuded high-resolution mass spectra, leading to four factors: more oxidized oxygenated OA (MO-OOA), less oxidized oxygenated OA (LO-OOA), an isoprene epoxydiol (IEPOX)-related factor (isoprene-OA) and biomass burning OA (BBOA). BBOA had the highest mass fraction remaining (MFR) at 100 °C, followed by the isoprene-OA, and the LO-OOA. Surprisingly the MO-OOA evaporated the most in the TD. The estimated effective vaporization enthalpies assuming an evaporation coefficient equal to unity were 58 ± 13 kJ mol-1 for the LO-OOA, 89 ± 10 kJ mol-1 for the MO-OOA, 55 ± 11 kJ mol-1 for the BBOA, and 63 ± 15 kJ mol-1 for the isoprene-OA. The estimated volatility distribution of all factors covered a wide range including both semi-volatile and low-volatility components. BBOA had the lowest average volatility of all factors, even though it had the lowest O : C ratio among all factors. LO-OOA was the more volatile factor and its high MFR was due to its low enthalpy of vaporization according to the model. The isoprene-OA factor had intermediate volatility, quite higher than suggested by a few other studies. The analysis suggests that deducing the volatility of a factor only from its MFR could lead to erroneous conclusions. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.

Micrometeorological flux measurements of aerosol and gases above Beijing

NASA Astrophysics Data System (ADS)

Nemitz, Eiko; Langford, Ben; Mullinger, Neil; Cowan, Nicholas; Coyle, Mhairi; Acton, William Joe; Lee, James; Fu, Pingqing

2017-04-01

Air pollution is estimated to cause 1.6 million premature deaths in China every year and in the winter 2016/17 Beijing had to issue health alerts and put in place ad hoc limitations on industrial and vehicular activity. Much of this pollution is attributed to emissions from industrial processes and in particular coal combustion. By contrast, the diffuse pollutant sources within the city are less well understood. This includes, e.g., emissions from the Beijing traffic fleet, the sewage system, food preparation, solid fuel combustion in the streets and small industrial processes. Within the framework of a major UK-Chinese collaboration to study air pollution and its impact on human health in Beijing, we therefore measured fluxes of a large range of pollutants from a height of 102 m on the 325 m meteorological tower at the Institute of Atmospheric Physics. Several instruments were mounted at 102 m: fluxes of CO2 and H2O were measured with an infrared gas analyser (LiCOR 7500) and fluxes of ozone with a combination of a relative fast-response ozone analyser (ROFI) and a 2B absolute O3 instrument. Total particle number fluxes were measured with a condensation particle counter (TSI CPC 3785), and size-segregated fluxes over the size range 0.06 to 20 μm with a combination of an optical Ultrafine High Sensitivity Aerosol Spectrometer (UHSAS) and an Aerodynamic Particle Sizer Spectrometer (TSI APS3321). Ammonia (NH3) fluxes were measured for the first time above the urban environment using an Aerodyne compact quantum cascade laser (QCL). In addition, composition resolved aerosol fluxes were measured with an Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS), operated in a measurement container at the bottom of the tower, which subsampled from a 120 m long copper tube (15 mm OD). The analysis so far suggests that, due to often low wind speeds, fluxes were at times de-coupled from the surface. Fluxes normalised by CO2, a tracer for the amount of fossil fuel consumed, should be

Introducing MISR Version 23: Resolution and Content Improvements to MISR Aerosol and Land Surface Product

NASA Astrophysics Data System (ADS)

Garay, M. J.; Bull, M. A.; Witek, M. L.; Diner, D. J.; Seidel, F.

2017-12-01

Since early 2000, the Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has been providing operational Level 2 (swath-based) aerosol optical depth (AOD) and particle property retrievals at 17.6 km spatial resolution and atmospherically corrected land surface products at 1.1 km resolution. A major, multi-year development effort has led to the release of updated operational MISR Level 2 aerosol and land surface retrieval products. The spatial resolution of the aerosol product has been increased to 4.4 km, allowing more detailed characterization of aerosol spatial variability, especially near local sources and in urban areas. The product content has been simplified and updated to include more robust measures of retrieval uncertainty and other fields to benefit users. The land surface product has also been updated to incorporate the Version 23 aerosol product as input and to improve spatial coverage, particularly over mountainous terrain and snow/ice-covered surfaces. We will describe the major upgrades incorporated in Version 23, present validation of the aerosol product, and describe some of the applications enabled by these product updates.

High Resolution Trajectory-Based Smoke Forecasts Using VIIRS Aerosol Optical Depth and NUCAPS Carbon Monoxide Retrievals

NASA Astrophysics Data System (ADS)

Pierce, R. B.; Smith, N.; Barnet, C.; Barnet, C. D.; Kondragunta, S.; Davies, J. E.; Strabala, K.

2016-12-01

We use Suomi National Polar-orbiting Partnership (S-NPP) Visible Infrared Imaging Radiometer Suite (VIIRS) Aerosol Optical Depth (AOD) and combined Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) NOAA-Unique CrIS-ATMS Processing System (NUCAPS) carbon monoxide (CO) retrievals to initialize trajectory-based, high spatial resolution North American smoke dispersion forecasts during the May 2016 Fort McMurray wildfire in northern Alberta and the July 2016 Soberanes Fire in Northern California. These two case studies illustrate how long range transport of wild fire smoke can adversely impact surface air quality thousands of kilometers downwind and how local topographic flow can lead to complex transport patterns near the wildfire source region. The NUCAPS CO retrievals are shown to complement the high resolution VIIRS AOD retrievals by providing retrievals in partially cloudy scenes and also providing information on the vertical distribution of the wildfire smoke. This work addresses the need for low latency, web-based, high resolution forecasts of smoke dispersion for use by NWS Incident Meteorologists (IMET) to support on-site decision support services for fire incident management teams. The primary user community for the IDEA-I smoke forecasts is the Western regions of the NWS and US EPA due to the significant impacts of wildfires in these regions. Secondary users include Alaskan NWS offices and Western State and Local air quality management agencies such as the Western Regional Air Partnership (WRAP).

Secondary organic aerosol formation from isoprene photooxidation

NASA Astrophysics Data System (ADS)

Kroll, J. H.; Ng, N. L.; Murphy, S. M.; Flagan, R. C.; Seinfeld, J. H.

2005-12-01

We report chamber studies of the formation of secondary organic aerosol (SOA) from the oxidation of isoprene (2-methyl-1,3-butadiene). Isoprene is the most abundant non-methane hydrocarbon emitted into the troposphere (source strength of ~500 Tg/year), so even small SOA yields may have a large impact on global SOA production. Reactions are carried out in Caltech's dual 28 m3 Teflon chambers, and aerosol growth is monitored by a differential mobility analyzer (DMA) and an Aerodyne time-of-flight aerosol mass spectrometer (AMS). Isoprene oxidation is initiated by the UV irradiation of isoprene in the presence of hydrogen peroxide, with NO added for high-NOx experiments. These conditions ensure that isoprene oxidation is initiated by reaction with the OH radical, with negligible interference from other oxidants (ozone, nitrate radicals, and O atoms). Aerosol growth is observed under both high-NOx and low-NOx conditions, at isoprene concentrations lower than measured in previous studies (down to 8 ppb). SOA yields are found to be in the range of 1-2%. Yields exhibit a complex dependence on NOx concentration, likely a result of changes in the chemistry of organic peroxy radicals. It is shown that condensable compounds are formed from further reactions of first-generation isoprene oxidation products; the rates and products of such gas-phase reactions are at present poorly understood. Additionally, measurements of SOA composition indicate that these products undergo reactions in the aerosol phase, leading to the formation of low-volatility oligomeric products.

Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

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

Richard A. Ferrare; David D. Turner

Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

Coarse mode aerosols in the High Arctic

NASA Astrophysics Data System (ADS)

Baibakov, K.; O'Neill, N. T.; Chaubey, J. P.; Saha, A.; Duck, T. J.; Eloranta, E. W.

2014-12-01

Fine mode (submicron) aerosols in the Arctic have received a fair amount of scientific attention in terms of smoke intrusions during the polar summer and Arctic haze pollution during the polar winter. Relatively little is known about coarse mode (supermicron) aerosols, notably dust, volcanic ash and sea salt. Asian dust is a regular springtime event whose optical and radiative forcing effects have been fairly well documented at the lower latitudes over North America but rarely reported for the Arctic. Volcanic ash, whose socio-economic importance has grown dramatically since the fear of its effects on aircraft engines resulted in the virtual shutdown of European civil aviation in the spring of 2010 has rarely been reported in the Arctic in spite of the likely probability that ash from Iceland and the Aleutian Islands makes its way into the Arctic and possibly the high Arctic. Little is known about Arctic sea salt aerosols and we are not aware of any literature on the optical measurement of these aerosols. In this work we present preliminary results of the combined sunphotometry-lidar analysis at two High Arctic stations in North America: PEARL (80°N, 86°W) for 2007-2011 and Barrow (71°N,156°W) for 2011-2014. The multi-years datasets were analyzed to single out potential coarse mode incursions and study their optical characteristics. In particular, CIMEL sunphotometers provided coarse mode optical depths as well as information on particle size and refractive index. Lidar measurements from High Spectral Resolution lidars (AHSRL at PEARL and NSHSRL at Barrow) yielded vertically resolved aerosol profiles and gave an indication of particle shape and size from the depolarization ratio and color ratio profiles. Additionally, we employed supplementary analyses of HYSPLIT backtrajectories, OMI aerosol index, and NAAPS (Navy Aerosol Analysis and Prediction System) outputs to study the spatial context of given events.

The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

NASA Astrophysics Data System (ADS)

Pfaffenberger, L.; Barmet, P.; Slowik, J. G.; Praplan, A. P.; Dommen, J.; Prévôt, A. S. H.; Baltensperger, U.

2013-07-01

A series of smog chamber (SC) experiments was conducted to identify factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of particulate CO2+, a surrogate for carboxylic acids, vs. the fraction of C2H3O+, a surrogate for aldehydes, alcohols and ketones, as well as in the Van Krevelen space, where the evolution of the atomic hydrogen-to-carbon ratio (H : C) vs. the atomic oxygen-to-carbon ratio (O : C) is investigated. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. An OH exposure between 3 and 25 × 107 cm-3 h is needed to increase O : C by 0.05 during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.2 and 18 μg m-3 at an OH exposure of 4 × 107 cm-3 h, corresponding to about two days of oxidation time in the atmosphere, based on a global mean OH concentration of ~ 1 × 106 cm-3. α-Pinene SOA is more oxygenated at low organic mass loadings. Because the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near-ambient concentrations to accurately simulate

Characterizing Atmospheric Processing of Aerosols from Forest Fires at the Mt. Bachelor Observatory during BBOP

NASA Astrophysics Data System (ADS)

Zhou, S.; Collier, S.; Hee, J.; Wigder, N. L.; Jaffe, D. A.; Zhang, Q.

2014-12-01

This study investigates the physical and chemical characteristics and atmospheric processing of aerosols from uncontrolled forest fires across the Pacific Northwest. The measurements were made at the Mt. Bachelor Observatory (MBO) located at the summit of Mt. Bachelor in central Oregon (43.9794° N, 121.6885° W, 2,763 m asl) in summer 2013 during the DOE sponsored Biomass Burning Observation Project (BBOP) field campaign. We utilized an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) coupled with a thermodenuder. Observations during periods affected by biomass burning (BB) pollution showed elevated non-refractory submicron aerosol (NR-PM1) concentration up to 140 μg/m3. NR-PM1 correlated well with PM light scattering (up to ~ 600 Mm-1 at 550 nm) and gas phase CO (up to ~0.4 ppmv). The AMS BB tracer, f60, i.e., fraction of organic signals at m/z = 60, was also enhanced with a maximum of ~ 2%. Organic aerosol (OA) dominated the PM composition in BB plumes (94.1% of the NR-PM1 mass) with an average concentration of 13.9 μg/m3. Three distinctive BBOA factors were identified by Positive Matrix Factorization (PMF): a fresh BBOA-I factor (O/C=0.27, H/C=1.52, f60 = 2.26%) that correlates well with ammonium nitrate; an intermediately oxidized BBOA-II (O/C=0.52, H/C=1.47, f60 = 1.05%), and a highly oxidized BBOA-III (O/C=0.95, H/C=1.02) with a low f60 (< 0.01%) and enhanced tracer ions for carboxylic acids (e.g., CHO2+). During persistent BB plume events from fixed fire sources, fresh BBOA-I initially dominated the OA composition, but decreased as the more oxidized BBOA-II increased while BBOA-III remained unchanged. These events shed light on the chemical transformation of BB aerosol during atmospheric aging. We will examine the enhancement of different BBOA factors relative to CO to investigate secondary organic aerosol (SOA) formation processes in BB plumes.

Variations in the OM/OC ratio of urban organic aerosol next to a major roadway.

PubMed

Brown, Steven G; Lee, Taehyoung; Roberts, Paul T; Collett, Jeffrey L

2013-12-01

Understanding the organic matter/organic carbon (OM/OC) ratio in ambient particulate matter (PM) is critical to achieve mass closure in routine PM measurements, to assess the sources of and the degree of chemical processing organic aerosol particles have undergone, and to relate ambient pollutant concentrations to health effects. Of particular interest is how the OM/OC ratio varies in the urban environment, where strong spatial and temporal gradients in source emissions are common. We provide results of near-roadway high-time-resolution PM1 OM concentration and OM/OC ratio observations during January 2008 at Fyfe Elementary School in Las Vegas, NV, 18 m from the U.S. 95 freeway soundwall, measured with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The average OM/OC ratio was 1.54 (+/- 0.20 standard deviation), typical of environments with a low amount of secondary aerosol formation. The 2-min average OM/OC ratios varied between 1.17 and 2.67, and daily average OM/OC ratios varied between 1.44 and 1.73. The ratios were highest during periods of low OM concentrations and generally low during periods of high OM concentrations. OM/OC ratios were low (1.52 +/- 0.14, on average) during the morning rush hour (average OM = 2.4 microg/m3), when vehicular emissions dominate this near-road measurement site. The ratios were slightly lower (1.46 +/- 0.10) in the evening (average OM = 6.3 microg/m3), when a combination of vehicular and fresh residential biomass burning emissions was typically present during times with temperature inversions. The hourly averaged OM/OC ratio peaked at 1.66 at midday. OM concentrations were similar regardless of whether the monitoring site was downwind or upwind of the adjacent freeway throughout the day, though they were higher during stagnant conditions (wind speed < 0.5 m/sec). The OM/OC ratio generally varied more with time of day than with wind direction and speed.

Development and evaluation of a high-resolution aerosol optical depth product for the southern California region during the October 2007 wildfires

NASA Astrophysics Data System (ADS)

McCarthy, M. C.; Raffuse, S. M.; Dewinter, J. L.; Lurmann, F.; Craig, K. J.; Fruin, S.

2010-12-01

Current methods for estimating acute exposure to high levels of air pollution (e.g., particles, CO, NOx, aldehydes) during fire events require spatial interpolation over the study area using concentrations at central air quality monitors to represent the population of interest. This may inaccurately represent the magnitude of exposure because pollutant concentrations vary widely depending on the location of the fire plume, vertical mixing, and prevailing winds dispersing the pollutant. Remotely sensed datasets, such as aerosol optical depth (AOD) from the NASA MODIS instrument, can provide greater spatial coverage than ground-based air quality monitors. Past studies have shown positive correlations between AOD, a measure of aerosols in an atmospheric column, and ground-level measurements of PM2.5 and PM10 concentrations. However, current standard AOD products are not sufficient for assessing intra-urban variability due to the low spatial resolution (e.g., 10x10 km for MODIS) of datasets. In addition such products typically perform poorly with very dense smoke in the atmosphere and over reflective, semi-arid land surfaces such as southern California. A highly resolved AOD product (500m resolution) was developed for southern California during the October 2007 fires using radiance data obtained from the National Aeronautics and Space Administration (NASA) MODIS instrument. AOD was calculated at 0.55µm wavelength using a unique algorithm tailored to the southern California region and for an atmosphere dominated by biomass burning aerosols. The AOD product was compared with column measurements of AOD from surface-based AERONET sites. AOD was not predictive of surface PM during the October 2007 fires when compared to surface PM concentrations throughout southern California; R-square correlation coefficients were low. However, the relationship varied during the time period studied: correlations were weak early in the event (0.02) but improved during the later days of the

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

Simultaneous polarimeter retrievals of microphysical aerosol and ocean color parameters from the “MAPP” algorithm with comparison to high-spectral-resolution lidar aerosol and ocean products

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

Stamnes, S.; Hostetler, C.; Ferrare, R.

We present an optimal estimation based retrieval framework, the Microphysical Aerosol Properties from Polarimetry (MAPP) algorithm, designed for simultaneous retrieval of aerosol microphysical properties and ocean color bio-optical parameters using multi-angular polarized radiances. Polarimetric measurements from the airborne NASA Research Scanning Polarimeter (RSP) were inverted by MAPP to produce atmosphere and ocean products. The RSP MAPP results are compared with co-incident lidar measurements made by the NASA High Spectral Resolution Lidar HSRL-1 and HSRL-2 instruments. Comparisons are made of the aerosol optical depth (AOD) at 355, 532, and 1064 nm, lidar column-averaged measurements of the aerosol lidar ratio and Ã…ngstrømmore » exponent, and lidar ocean measurements of the particulate hemispherical backscatter coefficient and the diffuse attenuation coefficient. The measurements were collected during the 2012 Two-Column Aerosol Project (TCAP) campaign and the 2014 Ship-Aircraft Bio- Optical Research (SABOR) campaign. For the SABOR campaign, 71% RSP MAPP retrievals fall within 0.04 AOD at 532 nm as measured by HSRL-1, with an R value of 0.925 and root-mean-square deviation of 0.04. For the TCAP campaign, 55% of RSP MAPP retrievals are within 0.04 AOD as measured by HSRL-2, with an R value of 0.925 and root-mean-square deviation of 0.07. Comparisons with HSRL-2 AOD at 355 nm during TCAP result in an R value of 0.96 and a root-mean-square deviation of also 0.07. The RSP retrievals using the MAPP optimal estimation framework represent a key milestone on the path to a combined lidar+polarimeter retrieval using both HSRL and RSP measurements.« less

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

DOE PAGES

Zhou, Shan; Collier, Sonya; Xu, Jianzhong; ...

2016-05-19

Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m –3 with 64% of the mass being organic. Organic aerosol (OA) atmore » BNL was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

Influences of upwind emission sources and atmospheric processing on aerosol chemistry and properties at a rural location in the Northeastern U.S.

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

Zhou, Shan; Collier, Sonya; Xu, Jianzhong

Continuous real-time measurements of atmospheric aerosol with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer coupled with a fast temperature-stepping thermodenuder were carried out in summer 2011 at Brookhaven National Laboratory (BNL, 40.871°N, 72.89°W) during the Department of Energy Aerosol Life Cycle Intensive Operational Period campaign. BNL was frequently downwind of emissions from the New York metropolitan area and was exposed to various combinations of anthropogenic, biogenic, and marine emissions based on air mass history. The average concentration of submicrometer aerosol (PM1) during this study was 12.6 µg m –3 with 64% of the mass being organic. Organic aerosol (OA) atmore » BNL was found to be overwhelmingly secondary, consisting of (1) a fresher, semivolatile oxygenated organic aerosol (SV-OOA; oxygen-to-carbon ratio (O/C) = 0.54; 63% of OA mass) that was strongly influenced by transported urban plumes; (2) a regional, more aged, low-volatility OOA (LV-OOA; O/C = 0.97; 29% of OA mass) influenced by aqueous-phase processing; and (3) a nitrogen-enriched OA (NOA; nitrogen-to-carbon ratio (N/C) = 0.185; 8% of OA mass) likely composed of amine salts formed from acid-base reactions in industrial emissions. Urban emissions from the New York metropolitan areas to the W and SW in particular led to elevated PM1 mass concentration and altered aerosol composition at BNL. Transported urban plumes and local biogenic emissions likely interacted to enhance secondary organic aerosol production, primarily represented by SV-OOA. Lastly, these results suggest an important role that urban anthropogenic emissions play in affecting ambient PM concentration, composition, and physical-chemical properties at rural areas in the Northeast U.S.« less

Gas phase emissions from cooking processes and their secondary aerosol production potential

NASA Astrophysics Data System (ADS)

Klein, Felix; Platt, Stephen; Bruns, Emily; Termime-roussel, Brice; Detournay, Anais; Mohr, Claudia; Crippa, Monica; Slowik, Jay; Marchand, Nicolas; Baltensperger, Urs; Prevot, Andre; El Haddad, Imad

2014-05-01

Long before the industrial evolution and the era of fossil fuels, high concentrations of aerosol particles were alluded to in heavily populated areas, including ancient Rome and medieval London. Recent radiocarbon measurements (14C) conducted in modern megacities came as a surprise: carbonaceous aerosol (mainly organic aerosol, OA), a predominant fraction of particulate matter (PM), remains overwhelmingly non-fossil despite extensive fossil fuel combustion. Such particles are directly emitted (primary OA, POA) or formed in-situ in the atmosphere (secondary OA, SOA) via photochemical reactions of volatile organic compounds (VOCs). Urban levels of non-fossil OA greatly exceed the levels measured in pristine environments strongly impacted by biogenic emissions, suggesting a contribution from unidentified anthropogenic non-fossil sources to urban OA. Positive matrix factorization (PMF) techniques applied to ambient aerosol mass spectrometer (AMS, Aerodyne) data identify primary cooking emissions (COA) as one of the main sources of primary non-fossil OA in major cities like London (Allan et al., 2010), New York (Sun et al., 2011) and Beijing (Huang et al., 2010). Cooking processes can also emit VOCs that can act as SOA precursors, potentially explaining in part the high levels of oxygenated OA (OOA) identified by the AMS in urban areas. However, at present, the chemical nature of these VOCs and their secondary aerosol production potential (SAPP) remain virtually unknown. The approach adopted here involves laboratory quantification of PM and VOC emission factors from the main primary COA emitting processes and their SAPP. Primary emissions from deep-fat frying, vegetable boiling, vegetable frying and meat cooking for different oils, meats and vegetables were analysed under controlled conditions after ~100 times dilution. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a high resolution proton transfer time-of-flight mass spectrometer (PTR

Identification of amines in wintertime ambient particulate material using high resolution aerosol mass spectrometry

NASA Astrophysics Data System (ADS)

Bottenus, Courtney L. H.; Massoli, Paola; Sueper, Donna; Canagaratna, Manjula R.; VanderSchelden, Graham; Jobson, B. Thomas; VanReken, Timothy M.

2018-05-01

Significant amounts of amines were detected in fine particulate matter (PM) during ambient wintertime conditions in Yakima, WA, using a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Positive matrix factorization (PMF) of the organic aerosol (OA) signal resulted in a six-factor solution that included two previously unreported amine OA factors. The contributions of the amine factors were strongly episodic, but the concentration of the combined amine factors was as high as 10-15 μg m-3 (2-min average) during those episodes. In one occasion, the Amine-II component was 45% of total OA signal. The Amine-I factor was dominated by spectral peaks at m/z 86 (C5H12N+) and m/z 100 (C6H14N+), while the Amine-II factor was dominated by spectral peaks at m/z 58 (C3H8N+ and C2H6N2+) and m/z 72 (C4H10N+ and C3H8N2+). The ions dominating each amine factor showed distinct time traces, suggesting different sources or formation processes. Investigation into the chemistry of the amine factors suggests a correlation with inorganic anions for Amine-I, but no evidence that the Amine-II was being neutralized by the same inorganic ions. We also excluded the presence of organonitrates (ON) in the OA. The presence of C2H4O2+ at m/z 60 (a levoglucosan fragment) in the Amine-I spectrum suggests some influence of biomass burning emissions (more specifically residential wood combustion) in this PMF factor, but wind direction suggested that the most likely sources of these amines were agricultural activities and feedlots to the S-SW of the site.

Aerosol Retrieval from Multiangle Multispectral Photopolarimetric Measurements: Importance of Spectral Range and Angular Resolution

NASA Technical Reports Server (NTRS)

Wu, L.; Hasekamp, O.; Van Diedenhoven, B.; Cairns, B.

2015-01-01

We investigated the importance of spectral range and angular resolution for aerosol retrieval from multiangle photopolarimetric measurements over land. For this purpose, we use an extensive set of simulated measurements for different spectral ranges and angular resolutions and subsets of real measurements of the airborne Research Scanning Polarimeter (RSP) carried out during the PODEX and SEAC4RS campaigns over the continental USA. Aerosol retrievals performed from RSP measurements show good agreement with ground-based AERONET measurements for aerosol optical depth (AOD), single scattering albedo (SSA) and refractive index. Furthermore, we found that inclusion of shortwave infrared bands (1590 and/or 2250 nm) significantly improves the retrieval of AOD, SSA and coarse mode microphysical properties. However, accuracies of the retrieved aerosol properties do not improve significantly when more than five viewing angles are used in the retrieval.

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

NASA Astrophysics Data System (ADS)

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

2007-12-01

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

High time-resolved chemical compositions, sources and evolution for atmospheric submicron aerosols in the winter of Beijing

NASA Astrophysics Data System (ADS)

Min, H.; Hu, W.; Zheng, J.; Guo, S.; Wu, Y.; Zeng, L.; Lu, S.; Xie, S.; Zhang, Y.

2017-12-01

Severe regional haze problem in the megacity Beijing and surrounding areas has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, intensive campaigns were conducted in the winter of 2010 and 2013 at an urban site in Beijing. An Aerodyne high resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure chemical components of PM1, coupled with multiple state of the art online instruments. In the winter of 2010, PM1 mass concentrations changed dramatically along with meteorological conditions. The high average fraction (58%) of primary species in PM1 indicated that primary emissions usually played a more important role. Based on the source apportionment results, 45% POA are from non-fossil sources, contributed by cooking OA and biomass burning OA (BBOA). Cooking OA, accounting for 13-24% of OA, is an important non-fossil carbon source in all years of Beijing and should not be neglected. The fossil sources of POA include hydrocarbon-like OA from vehicle emissions and coal combustion OA (CCOA). The CCOA and BBOA were the two main contributors (57% of OA) for the highest OA concentrations (>100 μg m-3). In the winter of 2013, OOA (MO-OOA and LO-OOA), accounted for 50% of PM1, while (OOA+SNA) contributed 60-80%, suggesting that secondary formation played an important role in the PM pollution. In the winter of 2010 higher OOA/Ox (= NO2 + O3) ratio (0.49 μg m-3 ppb-1) than these ratios from western cities (0.03-0.16 μg m-3 ppb-1) was observed, which may be due to the aqueous reaction or extra SOA formation contributed by semi-VOCs from various primary sources (e.g., BBOA or CCOA). However, aqueous chemistry resulting in efficient secondary formation during occasional periods with high relative humidity may also contribute substantially to haze in winter. CCOA was only identified in winter due to domestic heating. These results signified that the comprehensive

High Spectral Resolution Lidar and MPLNET Micro Pulse Lidar Aerosol Optical Property Retrieval Intercomparison During the 2012 7-SEAS Field Campaign at Singapore

NASA Technical Reports Server (NTRS)

Lolli, Simone; Welton, Ellsworth J.; Campbell, James R.; Eloranta, Edwin; Holben, Brent N.; Chew, Boon Ning; Salinas, Santo V.

2014-01-01

From August 2012 to February 2013 a High Resolution Spectral Lidar (HSRL; 532 nm) was deployed at that National University of Singapore near a NASA Micro Pulse Lidar NETwork (MPLNET; 527 nm) site. A primary objective of the MPLNET lidar project is the production and dissemination of reliable Level 1 measurements and Level 2 retrieval products. This paper characterizes and quantifies error in Level 2 aerosol optical property retrievals conducted through inversion techniques that derive backscattering and extinction coefficients from MPLNET elastic single-wavelength datasets. MPLNET Level 2 retrievals for aerosol optical depth and extinction/backscatter coefficient profiles are compared with corresponding HSRL datasets, for which the instrument collects direct measurements of each using a unique optical configuration that segregates aerosol and cloud backscattered signal from molecular signal. The intercomparison is performed, and error matrices reported, for lower (0-5km) and the upper (>5km) troposphere, respectively, to distinguish uncertainties observed within and above the MPLNET instrument optical overlap regime.

Interfacing the NRL 1-D High Vertical Resolution Aerosol Model with COAMPS

DTIC Science & Technology

2006-09-30

model integrated with mesoscale meterological data to study marine boundary layer aerosol dynamics, J. Geophys. Res., in press, 2006. Hoppel, W. A...W.A. Hoppel, J.J. Shi: A one-dimensional sectional aerosol model integrated with mesoscale meterological data to study marine boundary layer aerosol

A dichotomy in primary marine organic aerosol-cloud-climate system

NASA Astrophysics Data System (ADS)

Ceburnis, D.; Ovadnevaite, J.; Martucci, G.; Bialek, J.; Monahan, C.; Rinaldi, M.; Facchini, C.; Berresheim, H.; Worsnop, D. R.; O'Dowd, C.

2011-12-01

D. Ceburnis1, J. Ovadnevaite1, G. Martucci1, J. Bialek1, C. Monahan1, M. Rinaldi2, M. C. Facchini2, H. Berresheim1, D. R. Worsnop3,4 and C. D. O'Dowd1 1School of Physics & Centre for Climate and Air Pollution Studies, National University of Ireland Galway, University Road, Galway, Ireland 2Institute of Atmospheric Sciences and Climate, National Research Council, Bologna, 20129, Italy. 3 Aerodyne Research, Inc., 45 Manning Road, Billerica, MA 01821-3976, USA 4 Physics Department, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland Organic matter has been observed to significantly contribute to particulate matter in every environment including pristine remote oceans. A significant if not dominant contribution of insoluble organic matter to marine aerosol has been proved to be of biogenic origin1,2. High time resolution measurements of marine organic matter have demonstrated a dynamic system with regular organic matter plume events occurring during summer3 as well as frequent open ocean particle formation events4. High-time resolution measurements of primary marine organic sea-spray physico-chemical properties reveal an apparent dichotomous behavior in terms of water uptake: specifically sea-spray aerosol enriched in organic matter possesses a low hygroscopic Growth Factor (GF~1.25) while simultaneously having a cloud condensation nucleus/condensation nuclei (CCN/CN) activation efficiency of between 83% at 0.25% supersaturation and 100% at 0.75%5. Simultaneous retrieval of Cloud Droplet Number Concentration (CDNC) during primary organic aerosol plumes reveal CDNC concentrations of 350 cm-3 in newly formed marine stratocumulus cloud for boundary layer organic mass concentrations of 3-4 ug m-36. It is suggested that marine hydrogels are responsible for this dichotomous behavior which has profound impacts to aerosol-cloud-climate system along with a better understood process analysis of aerosol formation by sea-spray7. A hydrophobic character of organic matter

Constructing An Event Based Aerosol Product Under High Aerosol Loading Conditions

NASA Astrophysics Data System (ADS)

Levy, R. C.; Shi, Y.; Mattoo, S.; Remer, L. A.; Zhang, J.

2016-12-01

High aerosol loading events, such as the Indonesia's forest fire in Fall 2015 or the persistent wintertime haze near Beijing, gain tremendous interests due to their large impact on regional visibility and air quality. Understanding the optical properties of these events and further being able to simulate and predict these events are beneficial. However, it is a great challenge to consistently identify and then retrieve aerosol optical depth (AOD) from passive sensors during heavy aerosol events. Some reasons include:1). large differences between optical properties of high-loading aerosols and those under normal conditions, 2) spectral signals of optically thick aerosols can be mistaken with surface depending on aerosol types, and 3) Extremely optically thick aerosol plumes can also be misidentified as clouds due to its high optical thickness. Thus, even under clear-sky conditions, the global distribution of extreme aerosol events is not well captured in datasets such as the MODIS Dark-Target (DT) aerosol product. In this study, with the synthetic use of OMI Aerosol Index, MODIS cloud product, and operational DT product, the heavy smoke events over the seven sea region are identified and retrieved over the dry season. An event based aerosol product that would compensate the standard "global" aerosol retrieval will be created and evaluated. The impact of missing high AOD retrievals on the regional aerosol climatology will be studied using this newly developed research product.

Seasonal monitoring and estimation of regional aerosol distribution over Po valley, northern Italy, using a high-resolution MAIAC product

NASA Astrophysics Data System (ADS)

Arvani, Barbara; Pierce, R. Bradley; Lyapustin, Alexei I.; Wang, Yujie; Ghermandi, Grazia; Teggi, Sergio

2016-09-01

In this work, the new 1 km-resolved Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm is employed to characterize seasonal PM10 - AOD correlations over northern Italy. The accuracy of the new dataset is assessed compared to the widely used Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5.1 Aerosol Optical Depth (AOD) data, retrieved at 0.55 μm with spatial resolution of 10 km (MYD04_L2). We focused on evaluating the ability of these two products to characterize both temporal and spatial distributions of aerosols within urban and suburban areas. Ground PM10 measurements were obtained from 73 of the Italian Regional Agency for Environmental Protection (ARPA) monitoring stations, spread across northern Italy, during a three-year period from 2010 to 2012. The Po Valley area (northern Italy) was chosen as the study domain because of its severe urban air pollution, resulting from it having the highest population and industrial manufacturing density in the country, being located in a valley where two surrounding mountain chains favor the stagnation of pollutants. We found that the global correlations between the bin-averaged PM10 and AOD are R2 = 0.83 and R2 = 0.44 for MYD04_L2 and for MAIAC, respectively, suggesting a greater sensitivity of the high-resolution product to small-scale deviations. However, the introduction of Relative Humidity (RH) and Planetary Boundary Layer (PBL) depth corrections allowed for a significant improvement to the bin-averaged PM - AOD correlation, which led to a similar performance: R2 = 0.96 for MODIS and R2 = 0.95 for MAIAC. Furthermore, the introduction of the PBL information in the corrected AOD values was found to be crucial in order to capture the clear seasonal cycle shown by measured PM10 values. The study allowed us to define four seasonal linear correlations that estimate PM10 concentrations satisfactorily from the remotely sensed MAIAC AOD retrieval. Overall, the results show that the high

Seasonal Monitoring and Estimation of Regional Aerosol Distribution over Po Valley, Northern Italy, Using a High-Resolution MAIAC Product

NASA Technical Reports Server (NTRS)

Arvani, Barbara; Pierce, R. Bradley; Lyapustin, Alexei I.; Wang, Yujie; Ghermandi, Grazia; Teggi, Sergio

2016-01-01

In this work, the new 1-km-resolved Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm is employed to characterize seasonal AOD-PM10 correlations over northern Italy. The accuracy of the new dataset is assessed versus the widely used Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5.1 Aerosol Optical Depth (AOD) data, retrieved at 0.55 microns with spatial resolution of 10 km (MYD04). We focused on evaluating the ability of these two products to characterize both temporal and spatial distributions of aerosols within urban and suburban areas. Ground PM10 measurements were obtained from 73 of the Italian Regional Agency for Environmental Protection (ARPA) monitoring stations, spread across northern Italy, for a three-year period from 2010 to 2012. The Po Valley area (northern Italy) was chosen as the study domain because of severe urban air pollution, resulting from the highest population and industrial manufacturing density in the country, being located in a valley where two surrounding mountain chains favor the stagnation of pollutants. We found that the global correlations between PM10 and AOD are R(sup 2) = 0.83 and R(sup 2) = 0.44 for MYD04_L2 and for MAIAC, respectively, suggesting for a greater sensitiveness of the high-resolution product to small-scale deviations. However, the introduction of Relative Humidity (RH) and Planetary Boundary Layer (PBL) depth corrections gave a significant improvement to the PM AOD correlation, which led to similar performance: R(sup 2) = 0.96 for MODIS and R(sup 2) = 0.95 for MAIAC. Furthermore, the introduction of the PBL information in the corrected AOD values was found to be crucial in order to capture the clear seasonal cycle shown by measured PM10 values. The study allowed us to define four seasonal linear correlations that estimate PM10 concentrations satisfactorily from the remotely sensed MAIAC AOD retrieval. Overall, the results show that the high resolution provided by MAIAC

Sensitivity of high-spectral resolution and broadband thermal infrared nadir instruments to the chemical and microphysical properties of secondary sulfate aerosols in the upper-troposphere/lower-stratosphere

NASA Astrophysics Data System (ADS)

Sellitto, Pasquale; Legras, Bernard

2016-04-01

The observation of upper-tropospheric/lower-stratospheric (UTLS) secondary sulfate aerosols (SSA) and their chemical and microphysical properties from satellite nadir observations (with better spatial resolution than limb observations) is a fundamental tool to better understand their formation and evolution processes and then to estimate their impact on UTLS chemistry, and on regional and global radiative balance. Thermal infrared (TIR) observations are sensitive to the chemical composition of the aerosols due to the strong spectral variations of the imaginary part of the refractive index in this band and, correspondingly, of the absorption, as a function of the composition Then, these observations are, in principle, well adapted to detect and characterize UTLS SSA. Unfortunately, the exploitation of nadir TIR observations for sulfate aerosol layer monitoring is today very limited. Here we present a study aimed at the evaluation of the sensitivity of TIR satellite nadir observations to the chemical composition and the size distribution of idealised UTLS SSA layers. The sulfate aerosol particles are assumed as binary systems of sulfuric acid/water solution droplets, with varying sulphuric acid mixing ratios. The extinction properties of the SSA, for different sulfuric acid mixing ratios and temperatures, are systematically analysed. The extinction coefficients are derived by means of a Mie code, using refractive indices taken from the GEISA (Gestion et Étude des Informations Spectroscopiques Atmosphériques: Management and Study of Spectroscopic Information) spectroscopic database and log-normal size distributions with different effective radii and number concentrations. High-spectral resolution pseudo-observations are generated using forward radiative transfer calculations performed with the 4A (Automatized Atmospheric Absorption Atlas) radiative transfer model, to estimate the impact of the extinction of idealised aerosol layers, at typical UTLS conditions, on

Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0). Part 2: Analysis of the Biomass Burning Contribution and the Modern Carbon Fraction

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

Aiken, Allison; de Foy, B.; Wiedinmyer, Christine

2010-06-16

Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive Matrix Factorization (PMF) of high resolution AMS spectra identified a biomass burning OA (BBOA) component, which includes several large plumes that appear to be from forest fires within the region. Here, we show that the AMS BBOA concentration at T0 correlates with fire counts in the vicinity of Mexico City and that most of the BBOA variability is captured when the FLEXPART model is used for the dispersion ofmore » fire emissions as estimated from satellite fire counts. The resulting FLEXPART fire impact index correlates well with the observed BBOA, CH3CN, levoglucosan, and potassium, indicating that wildfires in the region surrounding Mexico City are the dominant source of BBOA at T0 during MILAGRO. The impact of distant BB sources such as the Yucatan is very small during this period. All fire tracers are correlated, with BBOA and levoglucosan showing little background, acetonitrile having a well-known tropospheric background of ~100-150 ppt, and PM2.5 potassium having a background of ~160 ng m-3 (two-thirds of its average concentration), which does not appear to be related to BB sources.« less

Open-path, closed-path and reconstructed aerosol extinction at a rural site.

PubMed

Gordon, Timothy D; Prenni, Anthony J; Renfro, James R; McClure, Ethan; Hicks, Bill; Onasch, Timothy B; Freedman, Andrew; McMeeking, Gavin R; Chen, Ping

2018-04-09

The Handix Scientific Open-Path Cavity Ringdown Spectrometer (OPCRDS) was deployed during summer 2016 in Great Smoky Mountains National Park (GRSM). Extinction coefficients from the relatively new OPCRDS and from a more well-established extinction instrument agreed to within 7%. Aerosol hygroscopic growth (f(RH)) was calculated from the ratio of ambient extinction measured by the OPCRDS to dry extinction measured by a closed-path extinction monitor (Aerodyne's Cavity Attenuated Phase Shift Particulate Matter Extinction Monitor, CAPS PMex). Derived hygroscopicity (RH < 95%) from this campaign agreed with data from 1995 at the same site and time of year, which is noteworthy given the decreasing trend for organics and sulfate in the eastern U.S. However, maximum f(RH) values in 1995 were less than half as large as those recorded in 2016-possibly due to nephelometer truncation losses in 1995. Two hygroscopicity parameterizations were investigated using high time resolution OPCRDS+CAPS PMex data, and the K ext model was more accurate than the γ model. Data from the two ambient optical instruments, the OPCRDS and the open-path nephelometer, generally agreed; however, significant discrepancies between ambient scattering and extinction were observed, apparently driven by a combination of hygroscopic growth effects, which tend to increase nephelometer truncation losses and decrease sensitivity to the wavelength difference between the two instruments as a function of particle size. There was not a statistically significant difference in the mean reconstructed extinction values obtained from the original and the revised IMPROVE (Interagency Monitoring of Protected Visual Environments) equations. On average IMPROVE reconstructed extinction was ~25% lower than extinction measured by the OPCRDS, which suggests that the IMPROVE equations and 24-hr aerosol data are moderately successful in estimating current haze levels at GRSM. However, this conclusion is limited by the coarse

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

Molecular composition of rainwater and aerosol during rain events in León, Spain, using high resolution mass spectrometry.

NASA Astrophysics Data System (ADS)

Fee, Anna

2017-04-01

Anna Fee (1), Markus Kalberer (1), Roberto Fraile (2), Amaya Castro (2), Ana. I. Calvo (2), Carlos Blanco-Alegre (2), Fernanda Oduber (2) and Mário Cerqueira (3). 1 Department of Chemistry, University of Cambridge, UK. 2 Department of Applied Chemistry and Physics, IMARENAB, University of León, Spain. 3 Department of Environmental Planning, University of Aveiro, Portugal. A wide range of atmospheric compounds which are present in rainwater are often also present in aerosol. They can be taken up during cloud droplet formation (in-cloud scavenging) or washed out during precipitation (below-cloud scavenging). Such compounds including aromatic hydrocarbons and organic nitrogen containing compounds are hazardous to health. In this study, the organic chemical composition of rainwater and aerosol from rain events in León, Spain, is being analysed using high resolution mass spectrometry. Collected rainwater along with high volume and low volume filters from rain events which occurred during spring, summer and winter of 2016 have been selected for analysis. Rainwater samples were prepared using Polymeric Reversed Phase Solid Phase Extraction (SPE) and filters have been extracted in water with and without SPE. Three different SPE polymer based sorbents were tested; one for extracting neutral compounds and two which are more suitable for extracting organic compounds containing sulphate and other polar functional groups. The sorbent for extracting neutral compounds was found to yield a higher number of compounds from the sample extraction than the other two varieties. Kendrick masses, Van Krevelen plots and carbon oxidation states have been investigated to identify compounds and patterns. Preliminary results show a predominance in peaks with O/C ratios between 0.2 and 0.7 and H/C ratios between 1 and 2 in both rain and aerosol samples which indicates substituted aromatic compounds. Cellulose material and fatty acids may also be present. The rain samples also have a

Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

NASA Astrophysics Data System (ADS)

Hu, Wei; Hu, Min; Hu, Wei-Wei; Zheng, Jing; Chen, Chen; Wu, Yusheng; Guo, Song

2017-08-01

A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m-3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60-80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations

Aerosol Lidar and MODIS Satellite Comparisons for Future Aerosol Loading Forecast

NASA Technical Reports Server (NTRS)

DeYoung, Russell; Szykman, James; Severance, Kurt; Chu, D. Allen; Rosen, Rebecca; Al-Saadi, Jassim

2006-01-01

Knowledge of the concentration and distribution of atmospheric aerosols using both airborne lidar and satellite instruments is a field of active research. An aircraft based aerosol lidar has been used to study the distribution of atmospheric aerosols in the California Central Valley and eastern US coast. Concurrently, satellite aerosol retrievals, from the MODIS (Moderate Resolution Imaging Spectroradiometer) instrument aboard the Terra and Aqua satellites, were take over the Central Valley. The MODIS Level 2 aerosol data product provides retrieved ambient aerosol optical properties (e.g., optical depth (AOD) and size distribution) globally over ocean and land at a spatial resolution of 10 km. The Central Valley topography was overlaid with MODIS AOD (5x5 sq km resolution) and the aerosol scattering vertical profiles from a lidar flight. Backward air parcel trajectories for the lidar data show that air from the Pacific and northern part of the Central Valley converge confining the aerosols to the lower valley region and below the mixed layer. Below an altitude of 1 km, the lidar aerosol and MODIS AOD exhibit good agreement. Both data sets indicate a high presence of aerosols near Bakersfield and the Tehachapi Mountains. These and other results to be presented indicate that the majority of the aerosols are below the mixed layer such that the MODIS AOD should correspond well with surface measurements. Lidar measurements will help interpret satellite AOD retrievals so that one day they can be used on a routine basis for prediction of boundary layer aerosol pollution events.

Receptor modeling of near-roadway aerosol mass spectrometer data in Las Vegas, Nevada, with EPA PMF

NASA Astrophysics Data System (ADS)

Brown, S. G.; Lee, T.; Norris, G. A.; Roberts, P. T.; Collett, J. L., Jr.; Paatero, P.; Worsnop, D. R.

2012-01-01

Ambient non-refractory PM1 aerosol particles were measured with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) at an elementary school 18 m from the US 95 freeway soundwall in Las Vegas, Nevada, during January 2008. Additional collocated continuous measurements of black carbon (BC), carbon monoxide (CO), nitrogen oxides (NOx), and meteorological data were collected. The US~Environmental Protection Agency's~(EPA) positive matrix factorization (PMF) data analysis tool was used to apportion organic matter (OM) as measured by HR-AMS, and rotational tools in EPA PMF were used to better characterize the solution space and pull resolved factors toward known source profiles. Three- to six-factor solutions were resolved. The four-factor solution was the most interpretable, with the typical AMS PMF factors of hydrocarbon-like organic aerosol (HOA), low-volatility oxygenated organic aerosol (LV-OOA), biomass burning organic aerosol (BBOA), and semi-volatile oxygenated organic aerosol (SV-OOA). When the measurement site was downwind of the freeway, HOA composed about half the OM, with SV-OOA and LV-OOA accounting for the rest. Attempts to pull the PMF factor profiles toward source profiles were successful but did not qualitatively change the results, indicating that these factors are very stable. Oblique edges were present in G-space plots, suggesting that the obtained rotation may not be the most plausible one. Since solutions found by pulling the profiles or using Fpeak retained these oblique edges, there appears to be little rotational freedom in the base solution. On average, HOA made up 26% of the OM, while LV-OOA was highest in the afternoon and accounted for 26% of the OM. BBOA occurred in the evening hours, was predominantly from the residential area to the north, and on average constituted 12% of the OM; SV-OOA accounted for the remaining third of the OM. Use of the pulling techniques available in EPA PMF and ME-2 suggested that the four

Impact of resolution on aerosol radiative feedbacks with in online-coupled chemistry/climate simulations (WRF-Chem) for EURO-CORDEX compliant domains

NASA Astrophysics Data System (ADS)

López-Romero, Jose Maria; Baró, Rocío; Palacios-Peña, Laura; Jerez, Sonia; Jiménez-Guerrero, Pedro; Montávez, Juan Pedro

2016-04-01

Several studies have shown that a high spatial resolution in atmospheric model runs improves the simulation of some meteorological variables, such as precipitation, particularly extreme events and in regions with complex orography [1]. However, increasing model spatial resolution makes the computational time rise exponentially. Hence, very high resolution experiments on large domains can hamper the execution of climatic runs. This problem shoots up when using online-coupled chemistry climate models, making a careful evaluation of improvements versus costs mandatory. Under this umbrella, the objective of this work is to investigate the sensitivity of aerosol radiative feedbacks from online-coupled chemistry regional model simulations to the spatial resolution. For that, the WRF-Chem [2] model is used for a case study to simulate the episode occurring between July 25th and August 15th of 2010. It is characterized by a high loading of atmospheric aerosol particles coming mainly from wildfires over large European regions (Russia, Iberian Peninsula). Three spatial resolutions are used defined for Euro-Cordex compliant domains [3]: 0.44°, 0.22° and 0.11°. Anthropogenic emissions come from TNO databases [4]. The analysis focuses on air quality variables (mainly PM10, PM2.5), meteorological variables (temperature, radiation) and other aerosol optical properties (aerosol optical depth). The CPU time ratio for the different domains is 1 (0.44°), 4(0.22°) and 28(0.11°) (normalized times). Comparison among simulations and observations are analyzed. Preliminary results show the difficulty to justify the much larger computational cost of high-resolution experiments when comparing with observations from a meteorological point of view, despite the finer spatio-temporal detail of the obtained pollutant fields. [1] Prein, A. F. (2014, December). Precipitation in the EURO-CORDEX 0.11° and 0.44° simulations: high resolution, high benefits?. In AGU Fall Meeting Abstracts (Vol

Wintertime aerosol in Las Vegas, Nevada

NASA Astrophysics Data System (ADS)

Brown, Steven G.

Numerous studies have found adverse health effects in subjects who live next to major roadways due to air pollution; in particular, there can be severe impacts on lung function and development in children living and/or attending school next to major roadways due to their exposure to air pollutants, including particulate matter (PM) or aerosol. The composition of aerosol at an elementary school next to a major freeway in Las Vegas, Nevada during winter 2008 was measured using a suite of measurements. An Aerodyne High Resolution Aerosol Mass Spectrometer (HR-AMS) was used to quantify the composition of non-refractory PM1 aerosol, including organic matter (OM); an Aethalometer was used to quantify black carbon (BC); a Sunset OCEC analyzer was used to measure organic and elemental carbon (OC, EC); and a particle-into-liquid system (PILS) coupled to two ion chromatographs (IC) was used to measure fine particle ions. Hi-volume PM2.5 samplers were used to collect aerosol on quartz fiber filters at between 2 and 24 hour intervals during the study, a subset of which were analyzed for PAHs and the biomass burning tracer levoglucosan. Data were analyzed by positive matrix factorization (PMF) to determine the amount of fresh, hydrocarbon-like organic aerosol (HOA), more oxidized OA (low-volatility and semi-volatile OA [LV-OOA, SV-OOA]) and biomass burning OA (BBOA). PM1 aerosol was predominantly carbonaceous, with OM plus BC accounting for 74% of the overall average 6.9 mug/m3 of PM measured. BC had a diurnal pattern similar to traffic volume, while OM was higher in the evening compared to the morning. OM was a mixture of fresh HOA, urban- and regional-scale OOA, and BBOA; in the evening, SV-OOA and BBOA peaked, while HOA concentrations were on average the same in the morning and evening, similar to BC. OM/OC ratios were low (1.52 +/-0.14 on average) during the morning rush hour (average OM = 2.4 mug/m3) when vehicular emissions dominate this near-road measurement site, and

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

PubMed

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

2017-02-01

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

Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

2010-10-01

Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during the summer 2009 Field Intensive Study at Queens College in New York City. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of total PM1 mass on average. The average mass size distribution of OA presents a small mode peaking at ~150 nm (Dva) in addition to an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of sulfate and OA both show pronounced peaks between 01:00-02:00 p.m. EST due to photochemical production. The average (±1σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012(±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62(±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified five OA components: a hydrocarbon-like OA (HOA), two types of oxygenated OA (OOA) including a low-volatility OOA (LV-OOA) and a semi-volatile OOA (SV-OOA), a cooking-emission related OA (COA), and a unique nitrogen-enriched OA (NOA). HOA appears to represent primary OA (POA) from urban traffic emissions. It comprises primarily of reduced species (H/C=1.83; O/C=0.06) and shows a mass spectral pattern very similar to those of POA from fossil fuel combustion, and correlates tightly with traffic emission tracers including elemental carbon and NOx. LV-OOA, which is highly oxidized (O/C=0.63) and correlates well with sulfate, appears to be representative for regional, aged secondary OA (SOA). SV-OOA, which is less oxidized (O/C=0.38) and correlates well with non-refractory chloride, likely represents less photo-chemically aged, semi-volatile SOA. COA shows a similar spectral pattern to the reference spectra of POA from cooking emissions and a distinct diurnal pattern

Monitoring the Impacts of Wildfires on Forest Ecosystems and Public Health in the Exo-Urban Environment Using High-Resolution Satellite Aerosol Products from the Visible Infrared Imaging Radiometer Suite (VIIRS).

PubMed

Huff, Amy K; Kondragunta, Shobha; Zhang, Hai; Hoff, Raymond M

2015-01-01

Increasing development of exo-urban environments and the spread of urbanization into forested areas is making humans and forest ecosystems more susceptible to the risks associated with wildfires. Larger and more damaging wildfires are having a negative impact on forest ecosystem services, and smoke from wildfires adversely affects the public health of people living in exo-urban environments. Satellite aerosol measurements are valuable tools that can track the evolution of wildfires and monitor the transport of smoke plumes. Operational users, such as air quality forecasters and fire management officials, can use satellite observations to complement ground-based and aircraft measurements of wildfire activity. To date, wildfire applications of satellite aerosol products, such as aerosol optical depth (AOD), have been limited by the relatively coarse resolution of available AOD data. However, the new Visible Infrared Imaging Radiometer Suite (VIIRS) instrument on the Suomi National Polar-orbiting Partnership (S-NPP) satellite has high-resolution AOD that is ideally suited to monitoring wildfire impacts on the exo-urban scale. Two AOD products are available from VIIRS: the 750-m × 750-m nadir resolution Intermediate Product (IP) and the 6-km × 6-km resolution Environmental Data Record product, which is aggregated from IP measurements. True color (red, green, and blue [RGB]) imagery and a smoke mask at 750-m × 750-m resolution are also available from VIIRS as decision aids for wildfire applications; they serve as counterparts to AOD measurements by providing visible information about areas of smoke in the atmosphere. To meet the needs of operational users, who do not have time to process raw data files and need access to VIIRS products in near-real time (NRT), VIIRS AOD and RGB NRT imagery are available from the Infusing satellite Data into Environmental Applications (IDEA) web site. A key feature of IDEA is an interactive visualization tool that allows users to

Monitoring the Impacts of Wildfires on Forest Ecosystems and Public Health in the Exo-Urban Environment Using High-Resolution Satellite Aerosol Products from the Visible Infrared Imaging Radiometer Suite (VIIRS)

PubMed Central

Huff, Amy K; Kondragunta, Shobha; Zhang, Hai; Hoff, Raymond M

2015-01-01

Increasing development of exo-urban environments and the spread of urbanization into forested areas is making humans and forest ecosystems more susceptible to the risks associated with wildfires. Larger and more damaging wildfires are having a negative impact on forest ecosystem services, and smoke from wildfires adversely affects the public health of people living in exo-urban environments. Satellite aerosol measurements are valuable tools that can track the evolution of wildfires and monitor the transport of smoke plumes. Operational users, such as air quality forecasters and fire management officials, can use satellite observations to complement ground-based and aircraft measurements of wildfire activity. To date, wildfire applications of satellite aerosol products, such as aerosol optical depth (AOD), have been limited by the relatively coarse resolution of available AOD data. However, the new Visible Infrared Imaging Radiometer Suite (VIIRS) instrument on the Suomi National Polar-orbiting Partnership (S-NPP) satellite has high-resolution AOD that is ideally suited to monitoring wildfire impacts on the exo-urban scale. Two AOD products are available from VIIRS: the 750-m × 750-m nadir resolution Intermediate Product (IP) and the 6-km × 6-km resolution Environmental Data Record product, which is aggregated from IP measurements. True color (red, green, and blue [RGB]) imagery and a smoke mask at 750-m × 750-m resolution are also available from VIIRS as decision aids for wildfire applications; they serve as counterparts to AOD measurements by providing visible information about areas of smoke in the atmosphere. To meet the needs of operational users, who do not have time to process raw data files and need access to VIIRS products in near-real time (NRT), VIIRS AOD and RGB NRT imagery are available from the Infusing satellite Data into Environmental Applications (IDEA) web site. A key feature of IDEA is an interactive visualization tool that allows users to

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

NASA Astrophysics Data System (ADS)

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

2015-04-01

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

Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

DOE PAGES

Lopez-Hilfiker, F. D.; Mohr, C.; Ehn, M.; ...

2015-07-16

We measured a large suite of gas- and particle-phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gas andmore » particle phases, the latter being detected by temperature-programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO–HR-ToF-CIMS are highly correlated with, and explain at least 25–50 % of, the organic aerosol mass measured by an Aerodyne aerosol mass spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from high molecular weight organics and/or oligomers (i.e., multi-phase accretion reaction products). Approximately 50 % of the HR-ToF-CIMS particle-phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption-temperature-based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas-particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the

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

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

Impacts of Cross-Platform Vicarious Calibration on the Deep Blue Aerosol Retrievals for Moderate Resolution Imaging Spectroradiometer Aboard Terra

NASA Technical Reports Server (NTRS)

Jeong, Myeong-Jae; Hsu, N. Christina; Kwiatkowska, Ewa J.; Franz, Bryan A.; Meister, Gerhard; Salustro, Clare E.

2012-01-01

The retrieval of aerosol properties from spaceborne sensors requires highly accurate and precise radiometric measurements, thus placing stringent requirements on sensor calibration and characterization. For the Terra/Moderate Resolution Imaging Spedroradiometer (MODIS), the characteristics of the detectors of certain bands, particularly band 8 [(B8); 412 nm], have changed significantly over time, leading to increased calibration uncertainty. In this paper, we explore a possibility of utilizing a cross-calibration method developed for characterizing the Terral MODIS detectors in the ocean bands by the National Aeronautics and Space Administration Ocean Biology Processing Group to improve aerosol retrieval over bright land surfaces. We found that the Terra/MODIS B8 reflectance corrected using the cross calibration method resulted in significant improvements for the retrieved aerosol optical thickness when compared with that from the Multi-angle Imaging Spectroradiometer, Aqua/MODIS, and the Aerosol Robotic Network. The method reported in this paper is implemented for the operational processing of the Terra/MODIS Deep Blue aerosol products.

New 4.4 km-resolution aerosol product from NASA's Multi-angle Imaging SpectroRadiometer: A user's guide

NASA Astrophysics Data System (ADS)

Nastan, A.; Garay, M. J.; Witek, M. L.; Seidel, F.; Bull, M. A.; Kahn, R. A.; Diner, D. J.

2017-12-01

The NASA Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has provided an 18-year-and-growing aerosol data record. MISR's V22 aerosol product has been used extensively in studies of regional and global climate and the health effects of particulate air pollution. The MISR team recently released a new version of this product (V23), which increases the spatial resolution from 17.6 km to 4.4 km, improves performance versus AERONET, and provides better spatial coverage, more accurate cloud screening, and improved radiometric conditioning relative to V22. The product formatting was also completely revamped to improve clarity and usability. Established and prospective users of the MISR aerosol product are invited to learn about the features and performance of the new product and to participate in one-on-one demonstrations of how to obtain, visualize, and analyze the new product. Because the aerosol product is used in generating atmospherically-corrected surface bidirectional reflectance factors, improvements in MISR's 1.1 km resolution land surface product are a by-product of the updated aerosol retrievals. Illustrative comparisons of the V22 and V23 aerosol and surface products will be shown.

Contribution of bacteria-like particles to PM2.5 aerosol in urban and rural environments

NASA Astrophysics Data System (ADS)

Wolf, R.; El-Haddad, I.; Slowik, J. G.; Dällenbach, K.; Bruns, E.; Vasilescu, J.; Baltensperger, U.; Prévôt, A. S. H.

2017-07-01

We report highly time-resolved estimates of airborne bacteria-like particle concentrations in ambient aerosol using an Aerodyne aerosol mass spectrometer (AMS). AMS measurements with a newly developed PM2.5 and the standard (PM1) aerodynamic lens were performed at an urban background site (Zurich) and at a rural site (Payerne) in Switzerland. Positive matrix factorization using the multilinear engine (ME-2) implementation was used to estimate the contribution of bacteria-like particles to non-refractory organic aerosol. The success of the method was evaluated by a size-resolved analysis of the organic mass and the analysis of single particle mass spectra, which were detected with a light scattering system integrated into the AMS. Use of the PM2.5 aerodynamic lens increased measured bacteria-like concentrations, supporting the analysis method. However, at all sites, the low concentrations of this component suggest that airborne bacteria constitute a minor fraction of non-refractory PM2.5 organic aerosol mass. Estimated average mass concentrations were below 0.1 μg/m3 and relative contributions were lower than 2% at both sites. During rainfall periods, concentrations of the bacteria-like component increased considerably reaching a short-time maximum of approximately 2 μg/m3 at the Payerne site in summer.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Comparison of Aerosol Classification From Airborne High Spectral Resolution Lidar and the CALIPSO Vertical Feature Mask

NASA Technical Reports Server (NTRS)

Burton, Sharon P.; Ferrare, Rich A.; Omar, Ali H.; Vaughan, Mark A.; Rogers, Raymond R.; Hostetler, Chris a.; Hair, Johnathan W.; Obland, Michael D.; Butler, Carolyn F.; Cook, Anthony L.;

Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments

NASA Astrophysics Data System (ADS)

Chirico, R.; Decarlo, P. F.; Heringa, M. F.; Tritscher, T.; Richter, R.; Prévôt, A. S. H.; Dommen, J.; Weingartner, E.; Wehrle, G.; Gysel, M.; Laborde, M.; Baltensperger, U.

2010-12-01

Diesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the third vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC < 0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging ~80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23-0.56 g/kg fuel burned. In presence of both a DOC and a DPF, only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.10 to 0.19. Five hours of oxidation led to a more oxidized OA with an O/C range of 0

Examining the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol formation during the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee ground site

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Li, X.; Bairai, S. T.; Renfro, J.; Liu, Y.; Liu, Y. J.; McKinney, K. A.; Martin, S. T.; McNeill, V. F.; Pye, H. O. T.; Nenes, A.; Neff, M. E.; Stone, E. A.; Mueller, S.; Knote, C.; Shaw, S. L.; Zhang, Z.; Gold, A.; Surratt, J. D.

2015-08-01

A suite of offline and real-time gas- and particle-phase measurements was deployed at Look Rock, Tennessee (TN), during the 2013 Southern Oxidant and Aerosol Study (SOAS) to examine the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol (SOA) formation. High- and low-time-resolution PM2.5 samples were collected for analysis of known tracer compounds in isoprene-derived SOA by gas chromatography/electron ionization-mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography/diode array detection-electrospray ionization-high-resolution quadrupole time-of-flight mass spectrometry (UPLC/DAD-ESI-HR-QTOFMS). Source apportionment of the organic aerosol (OA) was determined by positive matrix factorization (PMF) analysis of mass spectrometric data acquired on an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Campaign average mass concentrations of the sum of quantified isoprene-derived SOA tracers contributed to ~ 9 % (up to 28 %) of the total OA mass, with isoprene-epoxydiol (IEPOX) chemistry accounting for ~ 97 % of the quantified tracers. PMF analysis resolved a factor with a profile similar to the IEPOX-OA factor resolved in an Atlanta study and was therefore designated IEPOX-OA. This factor was strongly correlated (r2 > 0.7) with 2-methyltetrols, C5-alkene triols, IEPOX-derived organosulfates, and dimers of organosulfates, confirming the role of IEPOX chemistry as the source. On average, IEPOX-derived SOA tracer mass was ~ 26 % (up to 49 %) of the IEPOX-OA factor mass, which accounted for 32 % of the total OA. A low-volatility oxygenated organic aerosol (LV-OOA) and an oxidized factor with a profile similar to 91Fac observed in areas where emissions are biogenic-dominated were also resolved by PMF analysis, whereas no primary organic aerosol (POA) sources could be resolved. These findings were consistent with low levels of primary pollutants, such as nitric oxide (NO ~ 0.03 ppb), carbon monoxide (CO ~ 116 ppb), and black

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

NASA Technical Reports Server (NTRS)

Talbot, Robert W.; Dibb, Jack E.

2004-01-01

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

High-Resolution Mass Spectrometric Analysis of Secondary Organic Aerosol Produced by Ozonation of Limonene

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

Walser, Maggie L.; Dessiaterik, Yury; Laskin, Julia

2008-02-08

Secondary organic aerosol (SOA) particles formed from the ozone-initiated oxidation of limonene are characterized by high-resolution electrospray ionization mass spectrometry in both the positive and negative ion modes. The mass spectra reveal a large number of both monomeric (m/z < 300) and oligomeric (m/z > 300) products of oxidation. A combination of high resolving power (m/Δm ~60,000) and Kendrick mass defect analysis makes it possible to unambiguously determine the composition for hundreds of individual compounds in SOA samples. Van Krevelen analysis shows that the SOA compounds are heavily oxidized, with average O:C ratios of 0.43 and 0.50 determined from themore » positive and negative ion mode spectra, respectively. An extended reaction mechanism for the formation of the first generation SOA molecular components is proposed. The mechanism includes known isomerization and addition reactions of the carbonyl oxide intermediates generated during the ozonation of limonene, and numerous isomerization pathways for alkoxy radicals resulting from the decomposition of unstable carbonyl oxides. The isomerization reactions yield numerous products with a progressively increasing number of alcohol and carbonyl groups, whereas C-C bond scission reactions in alkoxy radicals shorten the carbon chain. Together these reactions yield a large number of isomeric products with broadly distributed masses. A qualitative agreement is found between the number and degree of oxidation of the predicted and measured reaction products in the monomer range.« less

Seasonal dependence of aerosol processing in urban Philadelphia

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Receptor modeling of near-roadway aerosol mass spectrometer data in Las Vegas, Nevada, with EPA PMF

NASA Astrophysics Data System (ADS)

Brown, S. G.; Lee, T.; Norris, G. A.; Roberts, P. T.; Collett, J. L., Jr.; Paatero, P.; Worsnop, D. R.

2011-08-01

Ambient non-refractory PM1 aerosol particles were measured with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) at an elementary school 20 m from the US 95 freeway in Las Vegas, Nevada, during January 2008. Additional collocated continuous measurements of black carbon (BC), carbon monoxide (CO), nitrogen oxides (NOx), and meteorological data were collected. The US Environmental Protection Agency's (EPA) positive matrix factorization (PMF) data analysis tool was used to apportion organic matter (OM) as measured by HR-AMS, and rotational tools in EPA PMF were used to better characterize the solution space and pull resolved factors toward known source profiles. Three- to six-factor solutions were resolved. The four-factor solution was the most interpretable, with the typical AMS PMF factors of hydrocarbon-like organic aerosol (HOA), low-volatility oxygenated organic aerosol (LV-OOA), biomass burning organic aerosol (BBOA), and semi-volatile oxygenated organic aerosol (SV-OOA). When the measurement site was downwind of the freeway, HOA composed about half the OM, with SV-OOA and LV-OOA accounting for the rest. Attempts to pull the PMF factor profiles toward source profiles were successful but did not qualitatively change the results, indicating that these factors are very stable. Oblique edges were present in G-space plots, suggesting that the obtained rotation may not be the most plausible one. Since solutions found by pulling the profiles or using Fpeak retained these oblique edges, there appears to be little rotational freedom in the base solution. On average, HOA made up 26 % of the OM, and it made up nearly half of the OM when the monitoring site was downwind of US 95 during morning rush hour. LV-OOA was highest in the afternoon and accounted for 26 % of the OM. BBOA occurred in the evening hours, was predominantly from the residential area to the north, and on average constituted 12 % of the OM; SV-OOA accounted for the remaining

High resolution Doppler lidar

NASA Technical Reports Server (NTRS)

Abreu, Vincent J.; Hays, Paul B.; Barnes, John E.

1989-01-01

A high resolution lidar system was implemented to measure winds in the lower atmosphere. The wind speed along the line of sight was determined by measuring the Doppler shift of the aerosol backscattered laser signal. The system in its present configuration is stable, and behaves as indicated by theoretical simulations. This system was built to demonstrate the capabilities of the detector system as a prototype for a spaceborne lidar. The detector system investigated consisted of a plane Fabry-Perot etalon, and a 12-ring anode detector. This system is generically similar to the Fabry-Perot interferometer developed for passive wind measurements on board the Dynamics Explorer satellite. That this detector system performs well in a lidar configuration was demonstrated.

Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

DOE PAGES

Lopez-Hilfiker, F. D.; Mohr, C.; Ehn, M.; ...

2015-02-18

We measured a large suite of gas and particle phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gasmore » and particle phases, the latter being detected upon temperature programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO HR-ToF-CIMS are highly correlated with, and explain at least 25–50% of, the organic aerosol mass measured by an Aerodyne Aerosol Mass Spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from large molecular weight organics and/or oligomers (i.e. multi-phase accretion reaction products). Approximately 50% of the HR-ToF-CIMS particle phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption temperature based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas–particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the

Characterizing the Hygroscopicity of Nascent Sea Spray Aerosol from Synthetic Blooms

NASA Astrophysics Data System (ADS)

Forestieri, S.; Cappa, C. D.; Sultana, C. M.; Lee, C.; Wang, X.; Helgestad, T.; Moore, K.; Prather, K. A.; Cornwell, G.; Novak, G.; Bertram, T. H.

2015-12-01

Marine sea spray aerosol (SSA) particles make up a significant portion of natural aerosols and are therefore important in establishing the baseline for anthropogenic aerosol climate impacts. Scattering of solar radiation by aerosols affects Earth's radiative budget and the degree of scattering is size-dependent. Thus, aerosols scatter more light at elevated relative humidities when they grow larger via water uptake. This growth depends critically on chemical composition. SSA can become enriched in organics during phytoplankton blooms, becoming less salty and therefore less hygroscopic. Subsaturated hygroscopic growth factors at 85% relative humidity (GF(85%)) of SSA particles were quantified during two mesocosm experiments in enclosed marine aerosol reference tanks (MARTs). The two experiments were conducted with filtered seawater collected at separate times from the Scripps Institute of Oceanography Pier in La Jolla, CA. Phytoplankton blooms in each tank were induced via the addition of nutrients and photosynthetically active radiation. The "indoor" MART was illuminated with fluorescent light and the other "outdoor" MART was illuminated with sunlight. The peak chlorophyll-a concentrations were 59 micrograms/L and 341 micrograms /L for the indoor and outdoor MARTs, respectively. GF(85%) values for SSA particles were quantified using a humidified cavity ringdown spectrometer and particle size distributions. Particle composition was monitored with a single particle aerosol mass spectrometer (ATOFMS) and an Aerodyne aerosol mass spectrometer (AMS). Relationships between the observed particle GFs and the particle composition markers will be discussed.

Examining the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol formation during the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee, ground site

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Li, X.; Bairai, S. T.; Renfro, J.; Liu, Y.; Liu, Y. J.; McKinney, K. A.; Martin, S. T.; McNeill, V. F.; Pye, H. O. T.; Nenes, A.; Neff, M. E.; Stone, E. A.; Mueller, S.; Knote, C.; Shaw, S. L.; Zhang, Z.; Gold, A.; Surratt, J. D.

2015-03-01

A suite of offline and real-time gas- and particle-phase measurements was deployed at Look Rock, Tennessee (TN), during the 2013 Southern Oxidant and Aerosol Study (SOAS) to examine the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol (SOA) formation. High- and low-time resolution PM2.5 samples were collected for analysis of known tracer compounds in isoprene-derived SOA by gas chromatography/electron ionization-mass spectrometry (GC/EI-MS) and ultra performance liquid chromatography/diode array detection-electrospray ionization-high-resolution quadrupole time-of-flight mass spectrometry (UPLC/DAD-ESI-HR-QTOFMS). Source apportionment of the organic aerosol (OA) was determined by positive matrix factorization (PMF) analysis of mass spectrometric data acquired on an Aerodyne Aerosol Chemical Speciation Monitor (ACSM). Campaign average mass concentrations of the sum of quantified isoprene-derived SOA tracers contributed to ~9% (up to 26%) of the total OA mass, with isoprene-epoxydiol (IEPOX) chemistry accounting for ~97% of the quantified tracers. PMF analysis resolved a factor with a profile similar to the IEPOX-OA factor resolved in an Atlanta study and was therefore designated IEPOX-OA. This factor was strongly correlated (r2>0.7) with 2-methyltetrols, C5-alkene triols, IEPOX-derived organosulfates, and dimers of organosulfates, confirming the role of IEPOX chemistry as the source. On average, IEPOX-derived SOA tracer mass was ~25% (up to 47%) of the IEPOX-OA factor mass, which accounted for 32% of the total OA. A low-volatility oxygenated organic aerosol (LV-OOA) and an oxidized factor with a profile similar to 91Fac observed in areas where emissions are biogenic-dominated were also resolved by PMF analysis, whereas no primary organic aerosol (POA) sources could be resolved. These findings were consistent with low levels of primary pollutants, such as nitric oxide (NO~0.03ppb), carbon monoxide (CO~116 ppb), and black carbon (BC~0

PFB Coal Fired Combined Cycle Development Program. Advanced hot gas cleanup concept evaluation (Task 4. 3). Volume A. Aerodyne cyclone evaluation

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

Not Available

This report summarizes the results of testing of a rotary flow cyclone, manufactured by Aerodyne Development Corporation under license by Siemens Kraftwerk Union. This cyclone was selected for evaluation due to the unusually high separative efficiencies claimed by the manufacturer (based on developer data), and relative lack of open literature data. The most significant finding of this work was the observation that electrostatic forces could enhance or, in fact, dominate the separation process. Separative efficiencies, with electrostatic forces present, were found to be substantially independent of flow rate and, by inference, could be independent of unit size. Hence this findingmore » offers a major hope that large cyclones employed in the hot gas cleanup train of the CFCC system may not suffer the performance degradation compared to small cyclones, as projected from conventional inertial theory. The separative efficiencies of the Aerodyne cyclone separator were found from both the cold flow and the hot flow tests to be disappointingly poorer than expectations (in agreement with Westinghouse results), and even poorer than conventional cyclones. (LTN)« less

The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation

NASA Astrophysics Data System (ADS)

Chang, R. Y.-W.; Slowik, J. G.; Shantz, N. C.; Vlasenko, A.; Liggio, J.; Sjostedt, S. J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-06-01

Cloud condensation nuclei (CCN) concentrations were measured at Egbert, a rural site in Ontario, Canada during the spring of 2007. The CCN concentrations were compared to values predicted from the aerosol chemical composition and size distribution using κ-Köhler theory, with the specific goal of this work being to determine the hygroscopic parameter (κ) of the oxygenated organic component of the aerosol, assuming that oxygenation drives the hygroscopicity for the entire organic fraction of the aerosol. The hygroscopicity of the oxygenated fraction of the organic component, as determined by an Aerodyne aerosol mass spectrometer (AMS), was characterised by two methods. First, positive matrix factorization (PMF) was used to separate oxygenated and unoxygenated organic aerosol factors. By assuming that the unoxygenated factor is completely non-hygroscopic and by varying κ of the oxygenated factor so that the predicted and measured CCN concentrations are internally consistent and in good agreement, κ of the oxygenated organic factor was found to be 0.22±0.04 for the suite of measurements made during this five-week campaign. In a second, equivalent approach, we continue to assume that the unoxygenated component of the aerosol, with a mole ratio of atomic oxygen to atomic carbon (O/C) ≈ 0, is completely non-hygroscopic, and we postulate a simple linear relationship between κorg and O/C. Under these assumptions, the κ of the entire organic component for bulk aerosols measured by the AMS can be parameterised as κorg=(0.29±0.05)·(O/C), for the range of O/C observed in this study (0.3 to 0.6). These results are averaged over our five-week study at one location using only the AMS for composition analysis. Empirically, our measurements are consistent with κorg generally increasing with increasing particle oxygenation, but high uncertainties preclude us from testing this hypothesis. Lastly, we examine select periods of different aerosol composition, corresponding

Using Aerosol Reflectance for Dust Detection

NASA Astrophysics Data System (ADS)

Bahramvash Shams, S.; Mohammadzade, A.

2013-09-01

In this study we propose an approach for dust detection by aerosol reflectance over arid and urban region in clear sky condition. In urban and arid areas surface reflectance in red and infrared spectral is bright and hence shorter wavelength is required for this detections. Main step of our approach can be mentioned as: cloud mask for excluding cloudy pixels from our calculation, calculate Rayleigh path radiance, construct a surface reflectance data base, estimate aerosol reflectance, detect dust aerosol, dust detection and evaluations of dust detection. Spectral with wavelength 0.66, 0.55, 0.47 μm has been used in our dust detection. Estimating surface reflectance is the most challenging step of obtaining aerosol reflectance from top of atmosphere (TOA) reflectance. Hence for surface estimation we had created a surface reflectance database of 0.05 degree latitude by 0.05 degree longitude resolution by using minimum reflectivity technique (MRT). In order to evaluate our dust detection algorithm MODIS aerosol product MOD04 and common dust detection method named Brightness Temperature Difference (BTD) had been used. We had implemented this method to Moderate Resolution Imaging Spectroradiometer (MODIS) image of part of Iran (7 degree latitude and 8 degree longitude) spring 2005 dust phenomenon from April to June. This study uses MODIS LIB calibrated reflectance high spatial resolution (500 m) MOD02Hkm on TERRA spacecraft. Hence our dust detection spatial resolution will be higher spatial resolution than MODIS aerosol product MOD04 which has 10 × 10 km2 and BTD resolution is 1 km due to the band 29 (8.7 μm), 31 (11 μm), and 32 (12 μm) spatial resolutions.

Feasibility of the detection of trace elements in particulate matter using online High-Resolution Aerosol Mass Spectrometry

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

Salcedo, D.; Laskin, Alexander; Shutthanandan, V.

The feasibility of using an online thermal-desorption electron-ionization high-resolution aerosol mass spectrometer (AMS) for the detection of particulate trace elements was investigated analyzing data from Mexico City obtained during the MILAGRO 2006 field campaign, where relatively high concentrations of trace elements have been reported. This potential application is of interest due to the real-time data provided by the AMS, its high sensitivity and time resolution, and the widespread availability and use of this instrument. High resolution mass spectral analysis, isotopic ratios, and ratios of different ions containing the same elements are used to constrain the chemical identity of the measuredmore » ions. The detection of Cu, Zn, As, Se, Sn, and Sb is reported. There was no convincing evidence for the detection of other trace elements commonly reported in PM. The elements detected tend to be those with lower melting and boiling points, as expected given the use of a vaporizer at 600oC in this instrument. Operation of the AMS vaporizer at higher temperatures is likely to improve trace element detection. The detection limit is estimated at approximately 0.3 ng m-3 for 5-min of data averaging. Concentration time series obtained from the AMS data were compared to concentration records determined from offline analysis of particle samples from the same times and locations by ICP (PM2.5) and PIXE (PM1.1 and PM0.3). The degree of correlation and agreement between the three instruments (AMS, ICP, and PIXE) varied depending on the element. The AMS shows promise for real-time detection of some trace elements, although additional work including laboratory calibrations with different chemical forms of these elements are needed to further develop this technique and to understand the differences with the ambient data from the other techniques. The trace elements peaked in the morning as expected for primary sources, and the many detected plumes suggest the presence of

Observations of fluorescent and biological aerosol at a high-altitude site in central France

NASA Astrophysics Data System (ADS)

Gabey, A. M.; Vaitilingom, M.; Freney, E.; Boulon, J.; Sellegri, K.; Gallagher, M. W.; Crawford, I. P.; Robinson, N. H.; Stanley, W. R.; Kaye, P. H.

2013-08-01

an aerosol mass spectrometer (AMS; Aerodyne Inc.) suggests that aerosol reaching the site at night was more aged than that during the day, indicative of sampling the residual layer at night. Supplementary meteorological data and previous work also show that PdD lies in the residual layer/free troposphere at night, and this is thought to cause the observed diurnal cycles in organic-type and fluorescent aerosol particles. Based on the observed disparity between bacteria and fluorescent particle concentrations, fluorescent non-PBA is likely to be important in the WIBS-3 data and the surprisingly high fluorescent concentration in the residual layer/free troposphere raises questions about a ubiquitous background in continental air during the summer.

Observations of fluorescent and biological aerosol at a high-altitude site in Central France

NASA Astrophysics Data System (ADS)

Gabey, A. M.; Vaitilingom, M.; Freney, E.; Boulon, J.; Sellegri, K.; Gallagher, M. W.; Crawford, I. P.; Robinson, N. H.; Stanley, W. R.; Kaye, P. H.

2013-01-01

Total bacteria, fungal spore and yeast counts were compared with UV Light-Induced Fluorescence (UV-LIF) measurements of ambient aerosol at the summit of the Puy de Dôme (pdD) mountain in Central France (1465 m a.s.l), which represents a background elevated site. Bacteria, fungal spores and yeast were enumerated by epifluorescence microscopy (EFM) and found to number 2.2 to 23 L-1 and 0.8 to 2 L-1, respectively. Bacteria counts on two successive nights were an order of magnitude larger than in the intervening day. A Wide Issue Bioaerosol Spectrometer, version 3 (WIBS-3) was used to perform UV-LIF measurements on ambient aerosol sized 0.8 to 20 μm. Mean total number concentration was 270 L-1 (σ = 66 L-1) found predominantly in a size mode at 2 μm for most of the campaign. Total concentration (fluorescent + non-fluorescent aerosol) peaked at 500 L-1 with a size mode at 1 μm because of a change in air mass origin lasting around 48 h. The WIBS-3 features two excitation and fluorescence detection wavelengths corresponding to different biological molecules. The mean fluorescent particle concentration after short-wave (280 nm; Tryptophan) excitation was 12 L-1 (σ = 6 L-1), and did not vary much through the campaign. In contrast the mean concentration of particles fluorescent after long-wave (370 nm; NADH) excitation was 95 L-1 (σ = 25 L-1), and a nightly rise and subsequent fall of up to 100 L-1 formed a strong diurnal cycle in the latter. The fluorescent populations exhibited size modes at 3 μm and 2 to 3 μm, respectively. A hierarchical agglomerative cluster analysis algorithm was applied to the data and used to extract different particle factors. A cluster concentration time series representative of bacteria was identified. This was found to exhibit a diurnal cycle with a maximum peak appearing during the day. Analysis of organic mass spectra recorded using an Aerosol Mass Spectrometer (AMS; Aerodyne Inc.) suggests that aerosol reaching the site at night was

Impact of aerosol size representation on modeling aerosol-cloud interactions

DOE PAGES

Zhang, Y.; Easter, R. C.; Ghan, S. J.; ...

2002-11-07

In this study, we use a 1-D version of a climate-aerosol-chemistry model with both modal and sectional aerosol size representations to evaluate the impact of aerosol size representation on modeling aerosol-cloud interactions in shallow stratiform clouds observed during the 2nd Aerosol Characterization Experiment. Both the modal (with prognostic aerosol number and mass or prognostic aerosol number, surface area and mass, referred to as the Modal-NM and Modal-NSM) and the sectional approaches (with 12 and 36 sections) predict total number and mass for interstitial and activated particles that are generally within several percent of references from a high resolution 108-section approach.more » The modal approach with prognostic aerosol mass but diagnostic number (referred to as the Modal-M) cannot accurately predict the total particle number and surface areas, with deviations from the references ranging from 7-161%. The particle size distributions are sensitive to size representations, with normalized absolute differences of up to 12% and 37% for the 36- and 12-section approaches, and 30%, 39%, and 179% for the Modal-NSM, Modal-NM, and Modal-M, respectively. For the Modal-NSM and Modal-NM, differences from the references are primarily due to the inherent assumptions and limitations of the modal approach. In particular, they cannot resolve the abrupt size transition between the interstitial and activated aerosol fractions. For the 12- and 36-section approaches, differences are largely due to limitations of the parameterized activation for non-log-normal size distributions, plus the coarse resolution for the 12-section case. Differences are larger both with higher aerosol (i.e., less complete activation) and higher SO2 concentrations (i.e., greater modification of the initial aerosol distribution).« less

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

NASA Astrophysics Data System (ADS)

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

2010-10-01

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

Identification and characterisation of local aerosol sources using high temporal resolution measurements.

PubMed

Contini, D; Donateo, A; Cesari, D; Belosi, F; Francioso, S

2010-09-01

Aerosol and gaseous pollution measurements were carried out at an urban background site in the south of Italy located near an industrial complex. Collection of 24 h samples of PM10 and PM2.5 and successive chemical quantification of metals were performed. Data were compared with measurements taken at a suburban background site, located at 25 km distance. The comparison showed the presence of an industrial contribution with a well defined chemical emission profile, similar, in terms of metals content, to urban emissions. As this made difficult the quantitative characterisation of the contribution of the two sources to atmospheric PM, a statistical method based on the treatment of data arising from high temporal resolution measurements was developed. Data were taken with a micrometeorological station based on an integrating nephelometer (Mie pDR-1200) for optical detection of PM2.5 concentration, with successive evaluation of vertical turbulent fluxes using the eddy-correlation method. Results show that the contribution from the two sources (urban emissions and industrial releases) have a very different behaviour, with the industrial contribution being present at high wind velocity with short concentration peaks (average duration 4 min) associated to strong positive and negative vertical fluxes. The estimated contribution to PM2.5 is 2.3% over long-term averages. The urban emissions are mainly present at low wind velocity, with longer concentration peaks in the morning and late evening hours, generally associated to small positive vertical fluxes. The characterisation of the contribution was performed using deposition velocity V(d) that is on average -3.5 mm s(-1) and has a diurnal pattern, with negligible values during the night and a minimum value of around -9 mm s(-1) late in the afternoon. Results show a correlation between V(d), friction velocity and wind velocity that could be the basis for a parameterisation of V(d) to be used in dispersion codes.

Effective resolution concepts for lidar observations

NASA Astrophysics Data System (ADS)

Iarlori, M.; Madonna, F.; Rizi, V.; Trickl, T.; Amodeo, A.

2015-12-01

Since its establishment in 2000, EARLINET (European Aerosol Research Lidar NETwork) has provided, through its database, quantitative aerosol properties, such as aerosol backscatter and aerosol extinction coefficients, the latter only for stations able to retrieve it independently (from Raman or high-spectral-resolution lidars). These coefficients are stored in terms of vertical profiles, and the EARLINET database also includes the details of the range resolution of the vertical profiles. In fact, the algorithms used in the lidar data analysis often alter the spectral content of the data, mainly acting as low-pass filters to reduce the high-frequency noise. Data filtering is described by the digital signal processing (DSP) theory as a convolution sum: each filtered signal output at a given range is the result of a linear combination of several signal input data samples (relative to different ranges from the lidar receiver), and this could be seen as a loss of range resolution of the output signal. Low-pass filtering always introduces distortions in the lidar profile shape. Thus, both the removal of high frequency, i.e., the removal of details up to a certain spatial extension, and the spatial distortion produce a reduction of the range resolution. This paper discusses the determination of the effective resolution (ERes) of the vertical profiles of aerosol properties retrieved from lidar data. Large attention has been dedicated to providing an assessment of the impact of low-pass filtering on the effective range resolution in the retrieval procedure.

Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in downtown Atlanta, Georgia

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

2014-07-01

Currently, there are a limited number of field studies that evaluate the long-term performance of the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) against established monitoring networks. In this study, we present seasonal intercomparisons of the ACSM with collocated fine aerosol (PM2.5) measurements at the Southeastern Aerosol Research and Characterization (SEARCH) Jefferson Street (JST) site near downtown Atlanta, GA, during 2011-2012. Intercomparison of two collocated ACSMs resulted in strong correlations (r2 > 0.8) for all chemical species, except chloride (r2 = 0.21) indicating that ACSM instruments are capable of stable and reproducible operation. In general, speciated ACSM mass concentrations correlate well (r2 > 0.7) with the filter-adjusted continuous measurements from JST, although the correlation for nitrate is weaker (r2 = 0.55) in summer. Correlations of the ACSM NR-PM1 (non-refractory particulate matter with aerodynamic diameter less than or equal to 1 μm) plus elemental carbon (EC) with tapered element oscillating microbalance (TEOM) PM2.5 and Federal Reference Method (FRM) PM1 mass are strong with r2 > 0.7 and r2 > 0.8, respectively. Discrepancies might be attributed to evaporative losses of semi-volatile species from the filter measurements used to adjust the collocated continuous measurements. This suggests that adjusting the ambient aerosol continuous measurements with results from filter analysis introduced additional bias to the measurements. We also recommend to calibrate the ambient aerosol monitoring instruments using aerosol standards rather than gas-phase standards. The fitting approach for ACSM relative ionization for sulfate was shown to improve the comparisons between ACSM and collocated measurements in the absence of calibrated values, suggesting the importance of adding sulfate calibration into the ACSM calibration routine.

Characterization of Organic Nitrate Formation in Limonene Secondary Organic Aerosol using High-Resolution Chemical Ionization Mass Spectrometry

NASA Astrophysics Data System (ADS)

Faxon, Cameron; Hammes, Julia; Peng, Jianfei; Hallquist, Mattias; Pathak, Ravi

2016-04-01

Previous work has shown that organic nitrates (RONO2) are prevalent in the boundary layer, and can contribute significantly to secondary organic aerosol formation. Monoterpenes, including limonene, have been shown to be precursors for the formation of these organic nitrates. Limonene has two double bonds, either of which may be oxidized by NO3 or O3. This leads to the generation of products that can subsequently condense or partition into the particle phase, producing secondary organic aerosol. In order to further elucidate the particle and gas phase product distribution of organic nitrates forming from the reactions of limonene and the nitrate radical (NO3), a series of experiments were performed in the Gothenburg Flow Reactor for Oxidation Studies at Low Temperatures (G-FROST), described by previous work. N2O5 was used as the source for NO3 and NO2, and a characterized diffusion source was used to introduce limonene into the flow reactor. All experiments were conducted in the absence of light, and the concentration of limonene was increased step-wise throughout each experiment to modify the ratio of N2O5to limonene. The experiments were conducted such that both limonene- and N2O5-limited regimes were present. Gas and particle phase products were measured using an iodide High-Resolution Time-of-Flight Mass Spectrometer (HR-ToF-CIMS) coupled to a Filter Inlet for Gases and AEROsols (FIGAERO, and particle size and SOA mass concentrations were derived using a Scanning Mobility Particle Sizer (SMPS). CIMS measurement techniques have previously been employed for the measurement of organic nitrate products of such compounds using multiple reagent ions. The use of this instrumentation allowed for the identification of chemical formulas for gas and particle phase species. The findings from the experiments will be presented in terms of the relative gas-particle partitioning of major products and the effects of N2O5/limonene ratios on product distributions. Additionally, a

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

Air-Quality and Climate Coupling in High Resolution for Urban Heat Island Study

NASA Astrophysics Data System (ADS)

Halenka, T.; Huszar, P.; Belda, M.

2012-04-01

Recent studies show considerable effect of atmospheric chemistry and aerosols on climate on regional and local scale. For the purpose of qualifying and quantifying the magnitude of climate forcing due to atmospheric chemistry/aerosols on regional scale and climate change effects on air-quality the regional climate model RegCM and chemistry/aerosol model CAMx was coupled. Climate change impacts on air-quality have been studied in high resolution of 10km with interactive two-way coupling of the effects of air-quality on climate. The experiments with the couple were performed for EC FP7 project MEGAPOLI assessing the impact of the megacities and industrialized areas on climate. New experiments in high resolution are prepared andsimulated for Urban Heat Island studies within the OP Central Europe Project UHI. Meteorological fields generated by RCM drive CAMx transport, chemistry and a dry/wet deposition. A preprocessor utility was developed for transforming RegCM provided fields to CAMx input fields and format. There is critical issue of the emission inventories available for 10km resolution including the urban hot-spots, TNO emissions are adopted for the experiments. Sensitivity tests switching on/off urban areas emissions are analysed as well. The results for year 2005 are presented and discussed, interactive coupling is compared to study the potential of possible impact of urban air-pollution to the urban area climate.

Development and assessment of a higher-spatial-resolution (4.4 km) MISR aerosol optical depth product using AERONET-DRAGON data

NASA Astrophysics Data System (ADS)

Garay, Michael J.; Kalashnikova, Olga V.; Bull, Michael A.

2017-04-01

Since early 2000, the Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has been acquiring data that have been used to produce aerosol optical depth (AOD) and particle property retrievals at 17.6 km spatial resolution. Capitalizing on the capabilities provided by multi-angle viewing, the current operational (Version 22) MISR algorithm performs well, with about 75 % of MISR AOD retrievals globally falling within 0.05 or 20 % × AOD of paired validation data from the ground-based Aerosol Robotic Network (AERONET). This paper describes the development and assessment of a prototype version of a higher-spatial-resolution 4.4 km MISR aerosol optical depth product compared against multiple AERONET Distributed Regional Aerosol Gridded Observations Network (DRAGON) deployments around the globe. In comparisons with AERONET-DRAGON AODs, the 4.4 km resolution retrievals show improved correlation (r = 0. 9595), smaller RMSE (0.0768), reduced bias (-0.0208), and a larger fraction within the expected error envelope (80.92 %) relative to the Version 22 MISR retrievals.

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.

Elemental composition of ambient aerosols measured with high temporal resolution using an online XRF spectrometer

NASA Astrophysics Data System (ADS)

Furger, Markus; Cruz Minguillón, María; Yadav, Varun; Slowik, Jay G.; Hüglin, Christoph; Fröhlich, Roman; Petterson, Krag; Baltensperger, Urs; Prévôt, André S. H.

2017-06-01

The Xact 625 Ambient Metals Monitor was tested during a 3-week field campaign at the rural, traffic-influenced site Härkingen in Switzerland during the summer of 2015. The field campaign encompassed the Swiss National Day fireworks event, providing increased concentrations and unique chemical signatures compared to non-fireworks (or background) periods. The objective was to evaluate the data quality by intercomparison with other independent measurements and test its applicability for aerosol source quantification. The Xact was configured to measure 24 elements in PM10 with 1 h time resolution. Data quality was evaluated for 10 24 h averages of Xact data by intercomparison with 24 h PM10 filter data analysed with ICP-OES for major elements, ICP-MS for trace elements, and gold amalgamation atomic absorption spectrometry for Hg. Ten elements (S, K, Ca, Ti, Mn, Fe, Cu, Zn, Ba, Pb) showed excellent correlation between the compared methods, with r2 values ≥ 0.95. However, the slopes of the regressions between Xact 625 and ICP data varied from 0.97 to 1.8 (average 1.28) and thus indicated generally higher Xact elemental concentrations than ICP for these elements. Possible reasons for these differences are discussed, but further investigations are needed. For the remaining elements no conclusions could be drawn about their quantification for various reasons, mainly detection limit issues. An indirect intercomparison of hourly values was performed for the fireworks peak, which brought good agreement of total masses when the Xact data were corrected with the regressions from the 24 h value intercomparison. The results demonstrate that multi-metal characterization at high-time-resolution capability of Xact is a valuable and practical tool for ambient monitoring.

Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-04-01

Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

NASA Astrophysics Data System (ADS)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-09-01

Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

Field and Laboratory Studies of Atmospheric Organic Aerosol

NASA Astrophysics Data System (ADS)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 < f42 < 0.15; 0.01 < f99 < 0.04), and negligible (f42 < 0.05; f99 < 0.01) ship influence. Application of

High-Resolution Mass Spectrometry and Molecular Characterization of Aqueous Photochemistry Products of Common Types of Secondary Organic Aerosols

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

Romonosky, Dian E.; Laskin, Alexander; Laskin, Julia

2015-03-19

A significant fraction of atmospheric organic compounds is predominantly found in condensed phases, such as aerosol particles and cloud droplets. Many of these compounds are photolabile and can degrade through direct photolysis or indirect photooxidation processes on time scales that are comparable to the typical lifetimes of aqueous droplets (hours) and particles (days). This paper presents a systematic investigation of the molecular level composition and the extent of aqueous photochemical processing in different types of secondary organic aerosol (SOA) from biogenic and anthropogenic precursors including α-pinene, β-pinene, β-myrcene, d- limonene, α-humulene, 1,3,5-trimethylbenzene, and guaiacol, oxidized by ozone (to simulate amore » remote atmosphere) or by OH in the presence of NOx (to simulate an urban atmosphere). Chamber- and flow tube-generated SOA samples were collected, extracted in a methanol/water solution, and photolyzed for 1 h under identical irradiation conditions. In these experiments, the irradiation was equivalent to about 3-8 h of exposure to the sun in its zenith. The molecular level composition of the dissolved SOA was probed before and after photolysis with direct-infusion electrospray ionization high-resolution mass spectrometry (ESI-HR-MS). The mass spectra of unphotolyzed SOA generated by ozone oxidation of monoterpenes showed qualitatively similar features, and contained largely overlapping subsets of identified compounds. The mass spectra of OH/NOx generated SOA had more unique visual appearance, and indicated a lower extent of products overlap. Furthermore, the fraction of nitrogen containing species (organonitrates and nitroaromatics) was highly sensitive to the SOA precursor. These observations suggest that attribution of high-resolution mass spectra in field SOA samples to specific SOA precursors should be more straightforward under OH/NOx oxidation conditions compared to the ozone driven oxidation. Comparison of the SOA

Compact high-power shipborne doppler lidar based on high spectral resolution techniques

NASA Astrophysics Data System (ADS)

Wu, Songhua; Liu, Bingyi; Dai, Guangyao; Qin, Shenguang; Liu, Jintao; Zhang, Kailin; Feng, Changzhong; Zhai, Xiaochun; Song, Xiaoquan

2018-04-01

The Compact High-Power Shipborne Doppler Wind Lidar (CHiPSDWiL) based on highspectral-resolution technique has been built up at the Ocean University of China for the measurement of the wind field and the properties of the aerosol and clouds in the troposphere. The design of the CHiPSDWiL including the transceiver, the injection seeding, the locking and the frequency measurement will be presented. Preliminary results measured by the CHiPSDWiL are provided.

A High Spectral Resolution Lidar Based on Absorption Filter

NASA Technical Reports Server (NTRS)

Piironen, Paivi

1996-01-01

A High Spectral Resolution Lidar (HSRL) that uses an iodine absorption filter and a tunable, narrow bandwidth Nd:YAG laser is demonstrated. The iodine absorption filter provides better performance than the Fabry-Perot etalon that it replaces. This study presents an instrument design that can be used a the basis for a design of a simple and robust lidar for the measurement of the optical properties of the atmosphere. The HSRL provides calibrated measurements of the optical properties of the atmospheric aerosols. These observations include measurements of aerosol backscatter cross sections, optical depth, backscatter phase function depolarization, and multiple scattering. The errors in the HSRL data are discussed and the effects of different errors on the measured optical parameters are shown.

Seasonal Variations of High Time-Resolved Chemical Compositions, Sources and Evolution for Atmospheric Submicron Aerosols in the Megacity of Beijing

NASA Astrophysics Data System (ADS)

Hu, Min; Hu, Wei; Hu, Weiwei; Zheng, Jing; Guo, Song; Wu, Yusheng; Lu, Sihua; Zeng, Limin

2016-04-01

This study aims to investigate aerosol secondary formation and aging process in the megacity of Beijing. Seasonal intensive campaigns were conducted from March 2012 to March 2013 at an urban site located at the campus of Peking University (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) and other relevant instrumentations for gaseous and particulate pollutants were deployed. The average submicron aerosol (PM1) mass concentrations were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7 and 81.7 ± 72.4 μg m-3 in spring, summer, autumn and winter, respectively. Organic matter was the most abundant component, accounting for 31%, 33%, 44% and 36% in PM1 correspondingly, followed by sulfate and nitrate. Distinct seasonal and diurnal patterns of the components of PM1 tracking primary sources (e.g., BC and HOA) and secondary formation (e.g., sulfate, nitrate, ammonium, LV-OOA and SV-OOA) were significantly influenced by primary emissions and mesoscale meteorology. Combining positive matrix factorization (PMF) analysis with the mass spectrometry of organics measured by AMS, the contributions of primary and secondary sources to submicron organic aerosols (OA) were apportioned. In spring and summer, the primary sources were hydrocarbon-like OA (HOA) and cooking OA (COA), and the secondary components were low volatility (LV-OOA) and semi-volatile oxygenated OA (SV-OOA). In winter biomass burning OA (BBOA) was also resolved. In autumn, four factors were resolved, that is, OOA, HOA, COA and BBOA. In general, OOA (sum of LV-OOA and SV-OOA) was important in OA in four seasons, accounting for about 63%, 70%, 47% and 50%, respectively. SV-OOA dominated OA in summer (44%) due to the fresh secondary formation from strong photochemical oxidations; whereas, LV-OOA was dominant in OA in winter (33%), maybe because the transported air masses were more aged in heavily polluted days. The POA (sum of HOA, COA and BBOA) in OA was dominant in

Diurnal Evolution of Aerosol Optical Properties and Morphology at Pico Tres Padres: A Phenomenological Analysis

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; Chakrabarty, R.; Dubey, M. K.; Moosmuller, H.; Chylek, P.; Onasch, T. B.; Herndon, S.; Zavala, M.; Kolb, C.

2007-05-01

Aerosol optical properties affect planetary radiative balance and therefore climate. The optical properties are related to chemical composition, size distribution, and morphology, which also have implications for human health and environmental degradation. During the MILAGRO field campaign, we measured ensemble aerosol absorption and angle-integrated scattering in Mexico City. These measurements were performed using the Los Alamos aerosol photoacoustic instrument with an integrated nephelometer (LAPA) operating at 781 nm. The LAPA was mounted on-board the Aerodyne Inc. mobile laboratory, which hosted a wide variety of gaseous and aerosol instruments. During the campaign, the Aerodyne mobile laboratory was moved to different sites, capturing the influence of spatial and temporal parameters including location, aging, elevation, and sources on ambient air pollution. The LAPA operated almost continuously between the 3rd and the 28th of March 2006. During the same period we collected ambient aerosols on more than 100 Nuclepore filters for scanning electron microscopy (SEM) analysis. Filter samples were collected during specific pollution events and different times of the day. Subsequently, SEM images of selected filters were taken to study particle morphology. The elemental composition of a few individual particles was also qualitatively assessed by energy dispersive X-ray spectroscopy. Between March 7th and 19th the laboratory was sampling air close to the top of the Pico Tres Padres, a ~3000 m high mountain on the north side of the Mexico City. Daily changes of aerosol loading and pollutant concentrations followed the expected diurnal variations of the boundary layer height. Here we report a preliminary analysis of aerosol absorption, scattering, and morphology at Pico Tres Padres for three specific days (9th, 11th and 12th of March 2006). The single scattering albedo (ratio of scattering to total extinction) during these three days showed a characteristic drop in the

Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments

NASA Astrophysics Data System (ADS)

Chirico, R.; Decarlo, P. F.; Heringa, M. F.; Tritscher, T.; Richter, R.; Prevot, A. S. H.; Dommen, J.; Weingartner, E.; Wehrle, G.; Gysel, M.; Laborde, M.; Baltensperger, U.

2010-06-01

Diesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the final vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC<0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging ~80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23-0.56 g/kg fuel burned. In presence of both a DOC and a DPF, primary particles with a mobility diameter above 5 nm were 300±19 cm-3, and only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.097 to 0

The Retrieval of Aerosol Optical Thickness Using the MERIS Instrument

NASA Astrophysics Data System (ADS)

Mei, L.; Rozanov, V. V.; Vountas, M.; Burrows, J. P.; Levy, R. C.; Lotz, W.

2015-12-01

Retrieval of aerosol properties for satellite instruments without shortwave-IR spectral information, multi-viewing, polarization and/or high-temporal observation ability is a challenging problem for spaceborne aerosol remote sensing. However, space based instruments like the MEdium Resolution Imaging Spectrometer (MERIS) and the successor, Ocean and Land Colour Instrument (OLCI) with high calibration accuracy and high spatial resolution provide unique abilities for obtaining valuable aerosol information for a better understanding of the impact of aerosols on climate, which is still one of the largest uncertainties of global climate change evaluation. In this study, a new Aerosol Optical Thickness (AOT) retrieval algorithm (XBAER: eXtensible Bremen AErosol Retrieval) is presented. XBAER utilizes the global surface spectral library database for the determination of surface properties while the MODIS collection 6 aerosol type treatment is adapted for the aerosol type selection. In order to take the surface Bidirectional Reflectance Distribution Function (BRDF) effect into account for the MERIS reduce resolution (1km) retrieval, a modified Ross-Li mode is used. The AOT is determined in the algorithm using lookup tables including polarization created using Radiative Transfer Model SCIATRAN3.4, by minimizing the difference between atmospheric corrected surface reflectance with given AOT and the surface reflectance calculated from the spectral library. The global comparison with operational MODIS C6 product, Multi-angle Imaging SpectroRadiometer (MISR) product, Advanced Along-Track Scanning Radiometer (AATSR) aerosol product and the validation using AErosol RObotic NETwork (AERONET) show promising results. The current XBAER algorithm is only valid for aerosol remote sensing over land and a similar method will be extended to ocean later.

Gas- and Particle-phase Chemical Composition Measurements Onboard the G1 Research Aircraft during the CARES Campaign

NASA Astrophysics Data System (ADS)

Shilling, J. E.; Alexander, L.; Jayne, J.; Fortner, E.

2010-12-01

An Aerodyne High Resolution Aerosol Mass Spectrometer (AMS) and an Ionicon Proton Transfer Reaction Mass Spectrometer (PTRMS) were deployed on the G1 research aircraft during the CARES campaign in Sacramento, CA to investigate aerosol gas- and particle-phase chemical composition. Preliminary analysis of PTRMS data suggests that biogenic volatile organic compounds (VOCs), particularly isoprene, dominate the region with anthropogenic VOCs, such as benzene and toluene, providing much smaller contributions to the VOC pool. Data from the AMS shows that the particle phase is dominated by organic material with smaller concentrations of ammonium sulfate and ammonium nitrate observed. Organic particle mass concentration strongly correlated with isoprene and gas-phase isoprene oxidation products, suggesting isoprene chemistry is largely controlling the organic aerosol loading in the area. The chemical evolution of the plume as it traveled downwind from Sacramento and into the foothills will also be discussed.

Intercomparison of an Aerosol Chemical Speciation Monitor (ACSM) with ambient fine aerosol measurements in Downtown Atlanta, Georgia

NASA Astrophysics Data System (ADS)

Budisulistiorini, S. H.; Canagaratna, M. R.; Croteau, P. L.; Baumann, K.; Edgerton, E. S.; Kollman, M. S.; Ng, N. L.; Verma, V.; Shaw, S. L.; Knipping, E. M.; Worsnop, D. R.; Jayne, J. T.; Weber, R. J.; Surratt, J. D.

2013-12-01

-25%, and 34-51% for sulfate, ammonium, and nitrate, respectively. These comparisons are all close to the stated ±30% accuracy of the ACSM except for nitrate. These discrepancies could be due to positive biases in the ACSM nitrate concentrations from interferences at the NO+ (m/z 30) fragment ion and/or negative artifacts in the nitrate filter measurement (from volatilization of NH4NO3) are also possible. The organic matter OM/OC ratios derived from linear regression of ACSM OM vs. Sunset OC/EC analyzer are 4.18 ± 0.04 and 3.59 ± 0.02 for summer and fall, respectively. Linear correlations of the ACSM NR-PM1 plus EC with TEOM PM2.5 mass are strong (r2 > 0.7) with percentage difference of 19% and 80% during summer and fall, respectively. On the other hand, the ACSM NR-PM1 correlation with FRM PM1 is high (r2 > 0.8) with percentage difference of ±47% over three seasons. Correlation of ACSM NR-PM1 plus EC mass with SEMS-MCPC PM1 volume concentration results in an estimation of aerosol density of 1.61 g cm-3 for fall 2012 period. ACSM organic concentrations measured during this study were obtained using relative ionization efficiency (RIE) values observed in Aerodyne Aerosol Mass Spectrometer (AMS). Explicit calibration of the ACSM relative ionizations for ammonium, nitrate, and sulfate, during this study was shown to improve the comparisons between ACSM and collocated measurements for these species. The accuracy of the organic and total mass concentrations would likely also be improved if organic relative ionization efficiency values for the ACSM were available during this study. Laboratory calibrations of ACSM relative ionization efficiencies using organic particles of known composition are recommended for future studies.

Assessing the influence of NOx concentrations and relative humidity on secondary organic aerosol yields from α-pinene photo-oxidation through smog chamber experiments and modelling calculations

NASA Astrophysics Data System (ADS)

Stirnweis, Lisa; Marcolli, Claudia; Dommen, Josef; Barmet, Peter; Frege, Carla; Platt, Stephen M.; Bruns, Emily A.; Krapf, Manuel; Slowik, Jay G.; Wolf, Robert; Prévôt, Andre S. H.; Baltensperger, Urs; El-Haddad, Imad

2017-04-01

Secondary organic aerosol (SOA) yields from the photo-oxidation of α-pinene were investigated in smog chamber (SC) experiments at low (23-29 %) and high (60-69 %) relative humidity (RH), various NOx / VOC ratios (0.04-3.8) and with different aerosol seed chemical compositions (acidic to neutralized sulfate-containing or hydrophobic organic). A combination of a scanning mobility particle sizer and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer was used to determine SOA mass concentration and chemical composition. We used a Monte Carlo approach to parameterize smog chamber SOA yields as a function of the condensed phase absorptive mass, which includes the sum of OA and the corresponding bound liquid water content. High RH increased SOA yields by up to 6 times (1.5-6.4) compared to low RH. The yields at low NOx / VOC ratios were in general higher compared to yields at high NOx / VOC ratios. This NOx dependence follows the same trend as seen in previous studies for α-pinene SOA. A novel approach of data evaluation using volatility distributions derived from experimental data served as the basis for thermodynamic phase partitioning calculations of model mixtures in this study. These calculations predict liquid-liquid phase separation into organic-rich and electrolyte phases. At low NOx conditions, equilibrium partitioning between the gas and liquid phases can explain most of the increase in SOA yields observed at high RH, when in addition to the α-pinene photo-oxidation products described in the literature, fragmentation products are added to the model mixtures. This increase is driven by both the increase in the absorptive mass and the solution non-ideality described by the compounds' activity coefficients. In contrast, at high NOx, equilibrium partitioning alone could not explain the strong increase in the yields with RH. This suggests that other processes, e.g. reactive uptake of semi-volatile species into the liquid phase, may occur and be

Mexico city aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 2: Analysis of the biomass burning contribution and the non-fossil carbon fraction

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

Aiken, A.C.; Wang, J.; de Foy, B.

2010-06-16

Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive Matrix Factorization (PMF) of high resolution AMS spectra identified a biomass burning organic aerosol (BBOA) component, which includes several large plumes that appear to be from forest fires within the region. Here, we show that the AMS BBOA concentration at T0 correlates with fire counts in the vicinity of Mexico City and that most of the BBOA variability is captured when the FLEXPART model is used for the dispersionmore » of fire emissions as estimated from satellite fire counts. The resulting FLEXPART fire impact factor (FIF) correlates well with the observed BBOA, acetonitrile (CH3CN), levoglucosan, and potassium, indicating that wildfires in the region surrounding Mexico City are the dominant source of BBOA at T0 during MILAGRO. The impact of distant BB sources such as the Yucatan is small during this period. All fire tracers are correlated, with BBOA and levoglucosan showing little background, acetonitrile having a well-known tropospheric background of {approx}100-150 pptv, and PM2.5 potassium having a background of {approx}160 ng m3 (two-thirds of its average concentration), which does not appear to be related to BB sources. We define two high fire periods based on satellite fire counts and FLEXPART-predicted FIFs. We then compare these periods with a low fire period when the impact of regional fires is about a factor of 5 smaller. Fire tracers are very elevated in the high fire periods whereas tracers of urban pollution do not change between these periods. Dust is also elevated during the high BB period but this appears to be coincidental due to the drier conditions and not driven by direct dust emission from the fires. The AMS oxygenated organic aerosol (OA) factor (OOA, mostly secondary OA or SOA) does not show an increase during the

The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

NASA Astrophysics Data System (ADS)

Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

All-fiber upconversion high spectral resolution wind lidar using a Fabry-Perot interferometer.

PubMed

Shangguan, Mingjia; Xia, Haiyun; Wang, Chong; Qiu, Jiawei; Shentu, Guoliang; Zhang, Qiang; Dou, Xiankang; Pan, Jian-Wei

2016-08-22

An all-fiber, micro-pulse and eye-safe high spectral resolution wind lidar (HSRWL) at 1.5 μm is proposed and demonstrated by using a pair of upconversion single-photon detectors and a fiber Fabry-Perot scanning interferometer (FFP-SI). In order to improve the optical detection efficiency, both the transmission spectrum and the reflection spectrum of the FFP-SI are used for spectral analyses of the aerosol backscatter and the reference laser pulse. Taking advantages of high signal-to-noise ratio of the detectors and high spectral resolution of the FFP-SI, the center frequencies and the bandwidths of spectra of the aerosol backscatter are obtained simultaneously. Continuous LOS wind observations are carried out on two days at Hefei (31.843 °N, 117.265 °E), China. The horizontal detection range of 4 km is realized with temporal resolution of 1 minute. The spatial resolution is switched from 30 m to 60 m at distance of 1.8 km. In a comparison experiment, LOS wind measurements from the HSRWL show good agreement with the results from an ultrasonic wind sensor (Vaisala windcap WMT52). An empirical method is adopted to evaluate the precision of the measurements. The standard deviation of the wind speed is 0.76 m/s at 1.8 km. The standard deviation of bandwidth variation is 2.07 MHz at 1.8 km.

Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

NASA Technical Reports Server (NTRS)

da Silva, Arlindo

2010-01-01

A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

Atmospheric aerosol compositions and sources at two national background sites in northern and southern China

NASA Astrophysics Data System (ADS)

Zhu, Qiao; He, Ling-Yan; Huang, Xiao-Feng; Cao, Li-Ming; Gong, Zhao-Heng; Wang, Chuan; Zhuang, Xin; Hu, Min

2016-08-01

Although China's severe air pollution has become a focus in the field of atmospheric chemistry and the mechanisms of urban air pollution there have been researched extensively, few field sampling campaigns have been conducted at remote background sites in China, where air pollution characteristics on a larger scale are highlighted. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), together with an Aethalometer, was deployed at two of China's national background sites in northern (Lake Hongze site; 33.23° N, 118.33° E; altitude 21 m) and southern (Mount Wuzhi site; 18.84° N, 109.49° E; altitude 958 m) China in the spring seasons in 2011 and 2015, respectively, in order to characterize submicron aerosol composition and sources. The campaign-average PM1 concentration was 36.8 ± 19.8 µg m-3 at the northern China background (NCB) site, which was far higher than that at the southern China background (SCB) site (10.9 ± 7.8 µg m-3). Organic aerosol (OA) (27.2 %), nitrate (26.7 %), and sulfate (22.0 %) contributed the most to the PM1 mass at NCB, while OA (43.5 %) and sulfate (30.5 %) were the most abundant components of the PM1 mass at SCB, where nitrate only constituted a small fraction (4.7 %) and might have contained a significant amount of organic nitrates (5-11 %). The aerosol size distributions and organic aerosol elemental compositions all indicated very aged aerosol particles at both sites. The OA at SCB was more oxidized with a higher average oxygen to carbon (O / C) ratio (0.98) than that at NCB (0.67). Positive matrix factorization (PMF) analysis was used to classify OA into three components, including a hydrocarbon-like component (HOA, attributed to fossil fuel combustion) and two oxygenated components (OOA1 and OOA2, attributed to secondary organic aerosols from different source areas) at NCB. PMF analysis at SCB identified a semi-volatile oxygenated component (SV-OOA) and a low-volatility oxygenated

Development of a balloon-borne device for analysis of high-altitude ice and aerosol particulates: Ice Cryo Encapsulator by Balloon (ICE-Ball)

NASA Astrophysics Data System (ADS)

Boaggio, K.; Bandamede, M.; Bancroft, L.; Hurler, K.; Magee, N. B.

2016-12-01

We report on details of continuing instrument development and deployment of a novel balloon-borne device for capturing and characterizing atmospheric ice and aerosol particles, the Ice Cryo Encapsulator by Balloon (ICE-Ball). The device is designed to capture and preserve cirrus ice particles, maintaining them at cold equilibrium temperatures, so that high-altitude particles can recovered, transferred intact, and then imaged under SEM at an unprecedented resolution (approximately 3 nm maximum resolution). In addition to cirrus ice particles, high altitude aerosol particles are also captured, imaged, and analyzed for geometry, chemical composition, and activity as ice nucleating particles. Prototype versions of ICE-Ball have successfully captured and preserved high altitude ice particles and aerosols, then returned them for recovery and SEM imaging and analysis. New improvements include 1) ability to capture particles from multiple narrowly-defined altitudes on a single payload, 2) high quality measurements of coincident temperature, humidity, and high-resolution video at capture altitude, 3) ability to capture particles during both ascent and descent, 4) better characterization of particle collection volume and collection efficiency, and 5) improved isolation and characterization of capture-cell cryo environment. This presentation provides detailed capability specifications for anyone interested in using measurements, collaborating on continued instrument development, or including this instrument in ongoing or future field campaigns.

Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

NASA Astrophysics Data System (ADS)

Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Flynn, M. J.; Harrison, R. M.; Yin, J.; Gallagher, M. W.; Coe, H.

2014-07-01

For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±one standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52) and 0.15 (±0.24) μg m-3, contributing 43, 28, 14, 13 and 2% to the total submicron mass, respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF) where five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3, respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species, due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual pollution events influence London

Investigating the annual behaviour of submicron secondary inorganic and organic aerosols in London

NASA Astrophysics Data System (ADS)

Young, D. E.; Allan, J. D.; Williams, P. I.; Green, D. C.; Flynn, M. J.; Harrison, R. M.; Yin, J.; Gallagher, M. W.; Coe, H.

2015-06-01

For the first time, the behaviour of non-refractory inorganic and organic submicron particulate through an entire annual cycle is investigated using measurements from an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) located at a UK urban background site in North Kensington, London. We show that secondary aerosols account for a significant fraction of the submicron aerosol burden and that high concentration events are governed by different factors depending on season. Furthermore, we demonstrate that on an annual basis there is no variability in the extent of secondary organic aerosol (SOA) oxidation, as defined by the oxygen content, irrespective of amount. This result is surprising given the changes in precursor emissions and contributions as well as photochemical activity throughout the year; however it may make the characterisation of SOA in urban environments more straightforward than previously supposed. Organic species, nitrate, sulphate, ammonium, and chloride were measured during 2012 with average concentrations (±1 standard deviation) of 4.32 (±4.42), 2.74 (±5.00), 1.39 (±1.34), 1.30 (±1.52), and 0.15 (±0.24) μg m-3, contributing 44, 28, 14, 13, and 2 % to the total non-refractory submicron mass (NR-PM1) respectively. Components of the organic aerosol fraction are determined using positive matrix factorisation (PMF), in which five factors are identified and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2). OOA1 and OOA2 represent more and less oxygenated OA with average concentrations of 1.27 (±1.49) and 0.14 (±0.29) μg m-3 respectively, where OOA1 dominates the SOA fraction (90%). Diurnal, monthly, and seasonal trends are observed in all organic and inorganic species due to meteorological conditions, specific nature of the aerosols, and availability of precursors. Regional and transboundary pollution as well as other individual

Variability of Marine Aerosol Fine-Mode Fraction and Estimates of Anthropogenic Aerosol Component Over Cloud-Free Oceans from the Moderate Resolution Imaging Spectroradiometer (MODIS)

NASA Technical Reports Server (NTRS)

Yu, Hongbin; Chin, Mian; Remer, Lorraine A.; Kleidman, Richard G.; Bellouin, Nicolas; Bian, Huisheng; Diehl, Thomas

2009-01-01

In this study, we examine seasonal and geographical variability of marine aerosol fine-mode fraction (f(sub m)) and its impacts on deriving the anthropogenic component of aerosol optical depth (tau(sub a)) and direct radiative forcing from multispectral satellite measurements. A proxy of f(sub m), empirically derived from the Moderate Resolution Imaging Spectroradiometer (MODIS) Collection 5 data, shows large seasonal and geographical variations that are consistent with the Goddard Chemistry Aerosol Radiation Transport (GOCART) and Global Modeling Initiative (GMI) model simulations. The so-derived seasonally and spatially varying f(sub m) is then implemented into a method of estimating tau(sub a) and direct radiative forcing from the MODIS measurements. It is found that the use of a constant value for fm as in previous studies would have overestimated Ta by about 20% over global ocean, with the overestimation up to 45% in some regions and seasons. The 7-year (2001-2007) global ocean average tau(sub a) is 0.035, with yearly average ranging from 0.031 to 0.039. Future improvement in measurements is needed to better separate anthropogenic aerosol from natural ones and to narrow down the wide range of aerosol direct radiative forcing.

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.

Characteristics of aerosol particles and trace gases in ship exhaust plumes

NASA Astrophysics Data System (ADS)

Drewnick, F.; Diesch, J.; Borrmann, S.

2011-12-01

Gaseous and particulate matter from marine vessels gain increasing attention due to their significant contribution to the anthropogenic burden of the atmosphere, implying the change of the atmospheric composition and the impact on local and regional air quality and climate (Eyring et al., 2010). As ship emissions significantly affect air quality of onshore regions, this study deals with various aspects of gas and particulate plumes from marine traffic measured near the Elbe river mouth in northern Germany. In addition to a detailed investigation of the chemical and physical particle properties from different types of commercial marine vessels, we will focus on the chemistry of ship plumes and their changes while undergoing atmospheric processing. Measurements of the ambient aerosol, various trace gases and meteorological parameters using a mobile laboratory (MoLa) were performed on the banks of the Lower Elbe which is passed on average, daily by 30 ocean-going vessels reaching the port of Hamburg, the second largest freight port of Europe. During 5 days of sampling from April 25-30, 2011 170 commercial marine vessels were probed at a distance of about 1.5-2 km with high temporal resolution. Mass concentrations in PM1, PM2.5 and PM10 and number as well as PAH and black carbon (BC) concentrations in PM1 were measured; size distribution instruments covered the size range from 6 nm up to 32 μm. The chemical composition of the non-refractory aerosol in the submicron range was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase species analyzers monitored various trace gas concentrations in the air and a weather station provided meteorological parameters. Additionally, a wide spectrum of ship information for each vessel including speed, size, vessel type, fuel type, gross tonnage and engine power was recorded via Automatic Identification System (AIS) broadcasts. Although commercial marine vessels powered by diesel engines consume high

Shear Flow Instabilities and Droplet Size Effects on Aerosol Jet Printing Resolution

NASA Astrophysics Data System (ADS)

Chen, Guang; Gu, Yuan; Hines, Daniel; Das, Siddhartha; LaboratoryPhysical Science Collaboration; Soft Matter, Interfaces, Energy Laboratory Collaboration

2017-11-01

Aerosol Jet printing (AJP) is an additive technology utilizing aerodynamic focusing to produce fine feature down to 10 micrometers that can be used in the manufacture of wearable electronics and biosensors. The main concern of the current technology is related to unstable printing resolution, which is usually assessed by effective line width, edge smoothness, overspray and connectivity. In this work, we perform a 3D CFD model to study the aerodynamic instabilities induced by the annular shear flow (sheath gas flow or ShGF) trapped with the aerosol jet (carried gas flow or CGF) with ink droplets. Extensive experiments on line morphology have shown that by increasing ShGF, one can first obtain thinner line width, and then massive overspray is witnessed at very large ShGF/ CGF ratio. Besides the fact that shear-layer instabilities usually trigger eddy currents at comparatively low Reynolds number 600, the tolerance of deposition components assembling will also propagate large offsets of the deposited feather. We also carried out detailed analysis on droplet size and deposition range on the printing resolution. This study is intended to come up with a solution on controlling the operating parameters for finer printed features, and offer an improvement strategy on next generation.

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

NASA Astrophysics Data System (ADS)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

Evaluation of Meteorological and Aerosol Sensing with small Unmanned Aerial Systems

NASA Astrophysics Data System (ADS)

Claussen, Johanna; Möhler, Ottmar; Leisner, Thomas; Brooks, Ian; Norris, Sarah; Brooks, Barbara; Hill, Martin; Haunold, Werner; Schrod, Jann; Danielczok, Anja

2013-04-01

Atmospheric aerosols have a large impact on the climate system due to their influence on the global radiation budget. Local aerosol sources such as vegetation, (bare) soil or industrial sites have to be quantified with high resolution data to validate aerosol transport models and improve the input for high resolution weather models. Our goal is to evaluate the use of Unmanned Aerial Systems (UAS) as a method for acquisition of high resolution meteorological and aerosol data. During the INUIT measurement campaign in August 2012 at mount Großer Feldberg near Frankfurt, Germany, several flights with different sensor packages were carried out. We measured basic meteorological parameters such as temperature, relative humidity and air pressure with miniaturized onboard sensors. In addition, the Compact Lightweight Aerosol Spectrometer Probe (CLASP) for aerosol size distribution measurement or the Electrostatic Aerosol Collector (EAC) for aerosol sample collection was installed on board. CLASP measures aerosol particles with diameters from 0.17 μm to 9.5 μm in up to 32 channels at a frequency of 10 Hz. The EAC collects air samples at 2 l/min onto a sample holder. After the flight the ice nuclei on the sample holder are activated and counted in the isothermal static diffusion chamber FRIDGE. The results from the INUIT campaign and additional calibration laboratory measurements show that UAS are a valuable platform for miniaturized sensors. The number of ice nuclei was determined with the EAC at 200m above ground level and compared to the reference measurement on the ground.

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.

Does the Madden-Julian Oscillation influence aerosol variability?

NASA Astrophysics Data System (ADS)

Tian, Baijun; Waliser, Duane E.; Kahn, Ralph A.; Li, Qinbin; Yung, Yuk L.; Tyranowski, Tomasz; Geogdzhayev, Igor V.; Mishchenko, Michael I.; Torres, Omar; Smirnov, Alexander

2008-06-01

We investigate the modulation of aerosols by the Madden-Julian Oscillation (MJO) using multiple, global satellite aerosol products: aerosol index (AI) from the Total Ozone Mapping Spectrometer (TOMS) on Nimbus-7, and aerosol optical thickness (AOT) from the Moderate Resolution Imaging Spectroradiometer (MODIS) on Terra and Aqua and the Advanced Very High Resolution Radiometer (AVHRR) on NOAA satellites. A composite MJO analysis indicates that large variations in the TOMS AI and MODIS/AVHRR AOT are found over the equatorial Indian and western Pacific Oceans where MJO convection is active, as well as the tropical Africa and Atlantic Ocean where MJO convection is weak but the background aerosol level is high. A strong inverse linear relationship between the TOMS AI and rainfall anomalies, but a weaker, less coherent positive correlation between the MODIS/AVHRR AOT and rainfall anomalies, were found. The MODIS/AVHRR pattern is consistent with ground-based Aerosol Robotic Network data. These results indicate that the MJO and its associated cloudiness, rainfall, and circulation variability systematically influence the variability in remote sensing aerosol retrieval results. Several physical and retrieval algorithmic factors that may contribute to the observed aerosol-rainfall relationships are discussed. Preliminary analysis indicates that cloud contamination in the aerosol retrievals is likely to be a major contributor to the observed relationships, although we cannot exclude possible contributions from other physical mechanisms. Future research is needed to fully understand these complex aerosol-rainfall relationships.

Citizen-Enabled Aerosol Measurements for Satellites (CEAMS): A Network for High-Resolution Measurements of PM2.5 and Aerosol Optical Depth

NASA Astrophysics Data System (ADS)

Pierce, J. R.; Volckens, J.; Ford, B.; Jathar, S.; Long, M.; Quinn, C.; Van Zyl, L.; Wendt, E.

2017-12-01

Atmospheric particulate matter with diameter smaller than 2.5 μm (PM2.5) is a pollutant that contributes to the development of human disease. Satellite-derived estimates of surface-level PM2.5 concentrations have the potential to contribute greatly to our understanding of how particulate matter affects health globally. However, these satellite-derived PM2.5 estimates are often uncertain due to a lack of information about the ratio of surface PM2.5 to aerosol optical depth (AOD), which is the primary aerosol retrieval made by satellite instruments. While modelling and statistical analyses have improved estimates of PM2.5:AOD, large uncertainties remain in situations of high PM2.5 exposure (such as urban areas and in wildfire-smoke plumes) where the health impacts of PM2.5 may be the greatest. Surface monitoring networks for co-incident PM2.5 and AOD measurements are extremely rare, even in the North America. To provide constraints for the PM2.5:AOD relationship, we have developed a relatively low-cost (<$1000) monitor for citizen use that provides sun-photometer AOD measurements and filter-based PM2.5 measurements. The instrument is solar-powered, lightweight (< 1kg), and operated wirelessly via smartphone application (iOS and Android). Sun photometry is performed across 4 discrete wavelengths that match those reported by the Aerosol Robotic Network (AERONET). Aerosol concentration is reported using both time-integrated filter mass (analyzed in an academic laboratory and reported as a 24-48hr average) and a continuous PM sensor within the instrument. Citizen scientists use the device to report daily AOD and PM2.5 measurements made in their backyards to a central server for data display and download. In this presentation, we provide an overview of (1) AOD and PM2.5 measurement calibration; (2) citizen recruiting and training efforts; and (3) results from our pilot citizen-science measurement campaign.

Production of Highly Charged Pharmaceutical Aerosols Using a New Aerosol Induction Charger

PubMed Central

Golshahi, Laleh; Longest, P. Worth; Holbrook, Landon; Snead, Jessica; Hindle, Michael

2015-01-01

Purpose Properly charged particles can be used for effective lung targeting of pharmaceutical aerosols. The objective of this study was to characterize the performance of a new induction charger that operates with a mesh nebulizer for the production of highly charged submicrometer aerosols to bypass the mouth-throat and deliver clinically relevant doses of medications to the lungs. Methods Variables of interest included combinations of model drug (i.e. albuterol sulfate) and charging excipient (NaCl) as well as strength of the charging field (1–5 kV/cm). Aerosol charge and size were measured using a modified electrical low pressure impactor system combined with high performance liquid chromatography. Results At the approximate mass median aerodynamic diameter (MMAD) of the aerosol (~ 0.4 μm), the induction charge on the particles was an order of magnitude above the field and diffusion charge limit. The nebulization rate was 439.3 ± 42.9 μl/min, which with a 0.1 % w/v solution delivered 419.5 ± 34.2 μg of medication per minute. A new correlation was developed to predict particle charge produced by the induction charger. Conclusions The combination of the aerosol induction charger and predictive correlations will allow for the practical generation and control of charged submicrometer aerosols for targeting deposition within the lungs. PMID:25823649

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.

Study of satellite retrieved aerosol optical depth spatial resolution effect on particulate matter concentration prediction

NASA Astrophysics Data System (ADS)

Strandgren, J.; Mei, L.; Vountas, M.; Burrows, J. P.; Lyapustin, A.; Wang, Y.

2014-10-01

The Aerosol Optical Depth (AOD) spatial resolution effect is investigated for the linear correlation between satellite retrieved AOD and ground level particulate matter concentrations (PM2.5). The Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm was developed for the Moderate Resolution Imaging Spectroradiometer (MODIS) for obtaining AOD with a high spatial resolution of 1 km and provides a good dataset for the study of the AOD spatial resolution effect on the particulate matter concentration prediction. 946 Environmental Protection Agency (EPA) ground monitoring stations across the contiguous US have been used to investigate the linear correlation between AOD and PM2.5 using AOD at different spatial resolutions (1, 3 and 10 km) and for different spatial scales (urban scale, meso-scale and continental scale). The main conclusions are: (1) for both urban, meso- and continental scale the correlation between PM2.5 and AOD increased significantly with increasing spatial resolution of the AOD, (2) the correlation between AOD and PM2.5 decreased significantly as the scale of study region increased for the eastern part of the US while vice versa for the western part of the US, (3) the correlation between PM2.5 and AOD is much more stable and better over the eastern part of the US compared to western part due to the surface characteristics and atmospheric conditions like the fine mode fraction.

Molecular characterization of organosulfates in organic aerosols from Shanghai and Los Angeles urban areas by nanospray-desorption electrospray ionization high-resolution mass spectrometry.

PubMed

Tao, Shikang; Lu, Xiaohui; Levac, Nicole; Bateman, Adam P; Nguyen, Tran B; Bones, David L; Nizkorodov, Sergey A; Laskin, Julia; Laskin, Alexander; Yang, Xin

2014-09-16

Fine aerosol particles in the urban areas of Shanghai and Los Angeles were collected on days that were characterized by their stagnant air and high organic aerosol concentrations. They were analyzed by nanospray-desorption electrospray ionization mass spectrometry with high mass resolution (m/Δm = 100,000). Solvent mixtures of acetonitrile and water and acetonitrile and toluene were used to extract and ionize polar and nonpolar compounds, respectively. A diverse mixture of oxygenated hydrocarbons, organosulfates, organonitrates, and organics with reduced nitrogen were detected in the Los Angeles sample. A majority of the organics in the Shanghai sample were detected as organosulfates. The dominant organosulfates that were detected at two locations have distinctly different molecular characteristics. Specifically, the organosulfates in the Los Angeles sample were dominated by biogenic products, while the organosulfates of a yet unknown origin found in the Shanghai sample had distinctive characteristics of long aliphatic carbon chains and low degrees of oxidation and unsaturation. The use of the acetonitrile and toluene solvent facilitated the observation of this type of organosulfates, which suggests that they could have been missed in previous studies that relied on sample extraction using common polar solvents. The high molecular weight and low degree of unsaturation and oxidization of the uncommon organosulfates suggest that they may act as surfactants and plausibly affect the surface tension and hygroscopicity of atmospheric particles. We propose that direct esterification of carbonyl or hydroxyl compounds by sulfates or sulfuric acid in the liquid phase could be the formation pathway of these special organosulfates. Long-chain alkanes from vehicle emissions might be their precursors.

Spatiotemporal variability and contribution of different aerosol types to the aerosol optical depth over the Eastern Mediterranean

NASA Astrophysics Data System (ADS)

Georgoulias, Aristeidis K.; Alexandri, Georgia; Kourtidis, Konstantinos A.; Lelieveld, Jos; Zanis, Prodromos; Pöschl, Ulrich; Levy, Robert; Amiridis, Vassilis; Marinou, Eleni; Tsikerdekis, Athanasios

2016-11-01

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the aerosol optical depth (AOD) over the Eastern Mediterranean as derived from MODIS (Moderate Resolution Imaging Spectroradiometer) Terra (March 2000-December 2012) and Aqua (July 2002-December 2012) satellite instruments. For this purpose, a 0.1° × 0.1° gridded MODIS dataset was compiled and validated against sun photometric observations from the AErosol RObotic NETwork (AERONET). The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium-sized cities, industrial zones and power plant complexes, seasonal variabilities and decadal averages. The average AOD at 550 nm (AOD550) for the entire region is ˜ 0.22 ± 0.19, with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in central and eastern Europe and transport of dust from the Sahara and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry-aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine-mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine-mode natural aerosols account for ˜ 51, ˜ 34 and ˜ 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account ˜ 40, ˜ 34 and ˜ 26 % of the total AOD550 over the sea, based on

Spatiotemporal Variability and Contribution of Different Aerosol Types to the Aerosol Optical Depth over the Eastern Mediterranean

NASA Technical Reports Server (NTRS)

Georgoulias, Aristeidis K.; Alexandri, Georgia; Kourtidis, Konstantinos A.; Lelieveld, Jos; Zanis, Prodromos; Poeschl, Ulrich; Levy, Robert; Amiridis, Vassilis; Marinou, Eleni; Tsikerdekis, Athanasios

2016-01-01

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the aerosol optical depth (AOD) over the Eastern Mediterranean as derived from MODIS (Moderate Resolution Imaging Spectroradiometer) Terra (March 2000-December 2012) and Aqua (July 2002-December 2012) satellite instruments. For this purpose, a 0.1deg × 0.1deg gridded MODIS dataset was compiled and validated against sun photometric observations from the AErosol RObotic NETwork (AERONET). The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium-sized cities, industrial zones and power plant complexes, seasonal variabilities and decadal averages. The average AOD at 550 nm (AOD550) for the entire region is approx. 0.22 +/- 0.19, with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in central and eastern Europe and transport of dust from the Sahara and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry-aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine-mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine-mode natural aerosols account for approx. 51, approx. 34 and approx. 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account approx. 40, approx. 34 and approx. 26 % of

Chemical characteristics of size-resolved aerosols in winter in Beijing.

PubMed

Sun, Kang; Qu, Yu; Wu, Qiong; Han, Tingting; Gu, Jianwei; Zhao, Jingjing; Sun, Yele; Jiang, Qi; Gao, Ziqi; Hu, Min; Zhang, Yuanhang; Lu, Keding; Nordmann, Stephan; Cheng, Yafang; Hou, Li; Ge, Hui; Furuuchi, Masami; Hata, Mitsuhiko; Liu, Xingang

2014-08-01

Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM (Aerodyne Aerosol Chemical Speciation Monitor) were compared. Between the data sets, similar trends and strong correlations were observed, demonstrating the validity of the Nano Sampler. PM₁₀ and PM₂.₅ concentrations during the measurement were 150.5 ± 96.0 μg/m³ (mean ± standard variation) and 106.9 ± 71.6 μg/m³, respectively. The PM₂.₅/PM₁₀ ratio was 0.70 ± 0.10, indicating that PM₂.₅ dominated PM₁₀. The aerosol size distributions showed that three size bins of 0.5-1, 1-2.5 and 2.5-10 μm contributed 21.8%, 23.3% and 26.0% to the total mass concentration (TMC), respectively. OM (organic matter) and SIA (secondary ionic aerosol, mainly SO₄(2-), NO₃(-) and NH₄(+)) were major components of PM₂.₅. Secondary compounds (SIA and secondary organic carbon) accounted for half of TMC (about 49.8%) in PM₂.₅, and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning, biomass combustion, vehicle emissions and SIA were found to be the main sources of PM₂.₅. Mass concentrations of water-soluble ions and undetected materials, as well as their fractions in TMC, strikingly increased with deteriorating particle pollution conditions, while OM and EC (elemental carbon) exhibited different variations, with mass concentrations slightly increasing but fractions in TMC decreasing. Copyright © 2014. Published by Elsevier B.V.

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

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

PubMed

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

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

Aging of Diesel and Wood Burning Emissions in Smogchamber Experiments

NASA Astrophysics Data System (ADS)

Prevot, Andre S. H.

2010-05-01

Photochemical aging experiments were performed for emissions of a diesel passenger car and logwood-burner at the smogchamber at the Paul Scherrer Institute in Switzerland. The measurements include black carbon measurements (with Aethalometer, Multi-Angle Absorption Photometer, Single Particle Soot Photometer (SP-2), and Photoacoustic Spectrometer), organic mass measurements with the Aerodyne high-resolution Aerosol mass spectrometer and off-line GC-MS measurements. Single particle composition was measured with the TSI-Aerosol time-of-flight mass spectrometer. The size distribution is characterized with a scanning mobility particle sizer, and the hygroscopicity with a hygroscopicity tandem differential mobility analyzer. The given overview of the results of experiments during the last 1.5 years will focus on the formation secondary organic aerosol and include the oxidation of primary organic aerosols and the change of optical and hygroscopic properties. A considerable variability of most results is found for different after treatment systems of diesel cars and for different burning conditions of the log-wood burner which will be discussed in detail.

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

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

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.

2016-01-08

The Two-Column Aerosol Project (TCAP), which was conducted from June 2012 through June 2013, was a unique field study that was designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere at a number of altitudes, from near the surface to as high as 8 km, within two atmospheric columns; one located near the coast of North America (over Cape Cod, MA) and a second over the Atlantic Ocean several hundredmore » kilometers from the coast. TCAP included the yearlong deployment of the U.S. Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) that was located at the base of the Cape Cod column, as well as summer and winter aircraft intensive observation periods of the ARM Aerial Facility. One important finding from TCAP is the relatively common occurrence (on four of six nearly cloud-free flights) of elevated aerosol layers in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total aerosol optical depth (AOD) observed in the column. Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning aerosol and nitrate compared to the aerosol found near the surface.« less

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.

Application of FIGAERO (Filter Inlet for Gases and AEROsol) coupled to a high resolution time of flight chemical ionization mass spectrometer to field and chamber organic aerosol: Implications for carboxylic acid formation and gas-particle partitioning from monoterpene oxidation

NASA Astrophysics Data System (ADS)

Lopez-Hilfiker, F.; Mohr, C.; Ehn, M.; Rubach, F.; Mentel, T. F.; Kleist, E.; Wildt, J.; Thornton, J. A.

2013-12-01

We present measurements of a large suite of gas and particle phase carboxylic acid containing compounds made with a Filter Inlet for Gas and AEROsol (FIGAERO) coupled to a high resolution time of flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. A prototype operated with acetate negative ion proton transfer chemistry was deployed on the Julich Plant Atmosphere Chamber to study a-pinene oxidation, and a modified version was deployed at the SMEAR II forest station in Hyytiälä, Finland and SOAS, in Brent Alabama. We focus here on results from JPAC and Hyytiälä, where we utilized the same ionization method most selective towards carboxylic acids. In all locations, 100's of organic acid compounds were observed in the gas and particles and many of the same composition acids detected in the gas-phase were detected in the particles upon temperature programmed thermal desorption. Particulate organics detected by FIGAERO are highly correlated with organic aerosol mass measured by an AMS, providing additional volatility and molecular level information about collected aerosol. The fraction of a given compound measured in the particle phase follows expected trends with elemental composition, but many compounds would not be well described by an absorptive partitioning model assuming unity activity coefficients. Moreover the detailed structure in the thermal desorption signals reveals a contribution from thermal decomposition of large molecular weight organics and or oligomers with implications for partitioning measurements and model validation

NASA Langley Airborne High Spectral Resolution Lidar Instrument Description

NASA Technical Reports Server (NTRS)

Harper, David B.; Cook, Anthony; Hostetler, Chris; Hair, John W.; Mack, Terry L.

2006-01-01

NASA Langley Research Center (LaRC) recently developed the LaRC Airborne High Spectral Resolution Lidar (HSRL) to make measurements of aerosol and cloud distribution and optical properties. The Airborne HSRL has undergone as series of test flights and was successfully deployed on the Megacity Initiative: Local and Global Research Observations (MILAGRO) field mission in March 2006 (see Hair et al. in these proceedings). This paper provides an overview of the design of the Airborne HSRL and descriptions of some key subsystems unique to this instrument.

Source characterization of ambient fine aerosol in Singapore during a haze episode in 2015

NASA Astrophysics Data System (ADS)

Hapsari Budisulistiorini, Sri; Riva, Matthieu; Williams, Michael; Miyakawa, Takuma; Komazaki, Yuichi; Chen, Jing; Surratt, Jason; Kuwata, Mikinori

2017-04-01

Recurring transboundary haze from Indonesia peatland fires in the previous decades has significantly elevated particulate matter (PM) concentration in Southeast Asia, particularly during the 2015 El Niño event. Previous studies have investigated chemical composition of particles emitted during haze episodes; however, they were limited to time-integrated samples and the number of identified compounds. Low time-resolution measurement results in co-variance of PM sources; therefore, higher time-resolution measurement is important in PM source apportionment. Between October 10-31, 2015, Aerodyne Time-of-Flight Aerosol Chemical Speciation Monitor (ToF-ACSM) was deployed for real-time chemical characterization of ambient submicron PM (NR-PM1) in Singapore. Simultaneously, PM2.5 filter samples were collected for molecular-level organic aerosol (OA) constituents, organic carbon (OC), elemental carbon (EC) and water-soluble OC (WSOC) analyses. OA constituents were quantified by gas chromatography interfaced to electron ionization mass spectrometry (GC/EI-MS) and ultra-performance liquid chromatography interfaced to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer operated in the negative ion mode (UPLC/(-)ESI-HR-Q-TOFMS). OA and SO42- are dominant components of the haze particles, accounting for ˜77% and ˜12% of the total NR-PM1 mass, respectively. OC/EC ratio of 4.8 might indicate formation of secondary OA (SOA) and aerosols from biomass burning, including those from peat burning. OA fraction from ToF-ACSM measurements was analyzed for source apportionment using a bilinear model through multi-linear engine algorithm (ME-2) in graphical user interface SoFi (Source Finder). Five OA factors were identified: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), peat burning OA (PBOA), low-volatility oxygenated OA (LV-OOA), and semi-volatile oxygenated OA (SV-OOA). The HOA factor shows a distinct diurnal profile peaking in the morning and

MODIS 3 Km Aerosol Product: Applications over Land in an Urban/suburban Region

NASA Technical Reports Server (NTRS)

Munchak, L. A.; Levy, R. C.; Mattoo, S.; Remer, L. A.; Holben, B. N.; Schafer, J. S.; Hostetler, C. A.; Ferrare, R. A.

2013-01-01

MODerate resolution Imaging Spectroradiometer (MODIS) instruments aboard the Terra and Aqua satellites have provided a rich dataset of aerosol information at a 10 km spatial scale. Although originally intended for climate applications, the air quality community quickly became interested in using the MODIS aerosol data. However, 10 km resolution is not sufficient to resolve local scale aerosol features. With this in mind, MODIS Collection 6 is including a global aerosol product with a 3 km resolution. Here, we evaluate the 3 km product over the Baltimore/Washington D.C., USA, corridor during the summer of 2011, by comparing with spatially dense data collected as part of the DISCOVER-AQ campaign these data were measured by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and a network of 44 sun photometers (SP) spaced approximately 10 km apart. The HSRL instrument shows that AOD can vary by up to 0.2 within a single 10 km MODIS pixel, meaning that higher resolution satellite retrievals may help to characterize aerosol spatial distributions in this region. Different techniques for validating a high-resolution aerosol product against SP measurements are considered. Although the 10 km product is more statistically reliable than the 3 km product, the 3 km product still performs acceptably, with more than two-thirds of MODIS/SP collocations falling within the expected error envelope with high correlation (R > 0.90). The 3 km product can better resolve aerosol gradients and retrieve closer to clouds and shorelines than the 10 km product, but tends to show more significant noise especially in urban areas. This urban degradation is quantified using ancillary land cover data. Overall, we show that the MODIS 3 km product adds new information to the existing set of satellite derived aerosol products and validates well over the region, but due to noise and problems in urban areas, should be treated with some degree of caution.

PFB coal fired combined cycle development program. Advanced hot gas cleanup concept evaluation (Task 4. 3). Volume A. Aerodyne cyclone evaluation

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

Not Available

This report summarizes the results of testing of a rotary flow cyclone, manufactured by Aerodyne Development Corporation under license by Siemens Kraftwerk Union. This cyclone was selected for evaluation due to the unusually high separative efficiencies claimed by the manufacturer (based on developer data), and relative lack of open literature data. The most significant finding of this work was the observation that electrostatic forces could enhance or, in fact, dominate the separation process. Separative efficiencies, with electrostatic forces present, were found to be substantially independent of flow rate and, by inference, could be independent of unit size. This finding suggestsmore » that large cyclones with natural or augmented electrostatic forces employed in the hot gas cleanup train of the CFCC system may not suffer the performance degradation compared to small cyclones, as projected from conventional inertial theory. This is of special importance since the use of many small cyclones in parallel, or multicyclones, commonly suffers from fouling and this approach is not recommended in the CFCC application. The original objective of this investigation was to assess the relative merits of the Aerodyne cyclone separator. It was found from both the cold flow and the hot flow tests that its separative efficiencies are disappointingly poorer than expectations (in agreement with Westinghouse results), and even poorer than conventional cyclones.« less

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

2013-11-01

Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding these transformation processes has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a Southeast Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high-resolution aerosol mass spectrometry and Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyl tetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

NASA Astrophysics Data System (ADS)

Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

2013-07-01

Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding the process of these transformations has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a South East Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high resolution aerosol mass spectrometry and fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyltetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

How does increasing horizontal resolution in a global climate model improve the simulation of aerosol-cloud interactions?

DOE PAGES

Ma, Po-Lun; Rasch, Philip J.; Wang, Minghuai; ...

2015-06-23

We report the Community Atmosphere Model Version 5 is run at horizontal grid spacing of 2, 1, 0.5, and 0.25°, with the meteorology nudged toward the Year Of Tropical Convection analysis, and cloud simulators and the collocated A-Train satellite observations are used to explore the resolution dependence of aerosol-cloud interactions. The higher-resolution model produces results that agree better with observations, showing an increase of susceptibility of cloud droplet size, indicating a stronger first aerosol indirect forcing (AIF), and a decrease of susceptibility of precipitation probability, suggesting a weaker second AIF. The resolution sensitivities of AIF are attributed to those ofmore » droplet nucleation and precipitation parameterizations. Finally, the annual average AIF in the Northern Hemisphere midlatitudes (where most anthropogenic emissions occur) in the 0.25° model is reduced by about 1 W m -2 (-30%) compared to the 2° model, leading to a 0.26 W m -2 reduction (-15%) in the global annual average AIF.« less

Simulating return signals of a spaceborne high-spectral resolution lidar channel at 532 nm

NASA Astrophysics Data System (ADS)

Xiao, Yu; Binglong, Chen; Min, Min; Xingying, Zhang; Lilin, Yao; Yiming, Zhao; Lidong, Wang; Fu, Wang; Xiaobo, Deng

2018-06-01

High spectral resolution lidar (HSRL) system employs a narrow spectral filter to separate the particulate (cloud/aerosol) and molecular scattering components in lidar return signals, which improves the quality of the retrieved cloud/aerosol optical properties. To better develop a future spaceborne HSRL system, a novel simulation technique was developed to simulate spaceborne HSRL return signals at 532 nm using the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) cloud/aerosol extinction coefficients product and numerical weather prediction data. For validating simulated data, a mathematical particulate extinction coefficient retrieval method for spaceborne HSRL return signals is described here. We compare particulate extinction coefficient profiles from the CALIPSO operational product with simulated spaceborne HSRL data. Further uncertainty analysis shows that relative uncertainties are acceptable for retrieving the optical properties of cloud and aerosol. The final results demonstrate that they agree well with each other. It indicates that the return signals of the spaceborne HSRL molecular channel at 532 nm will be suitable for developing operational algorithms supporting a future spaceborne HSRL system.

Effective resolution concepts for lidar observations

NASA Astrophysics Data System (ADS)

Iarlori, M.; Madonna, F.; Rizi, V.; Trickl, T.; Amodeo, A.

2015-05-01

Since its first establishment in 2000, EARLINET (European Aerosol Research Lidar NETwork) has been devoted to providing, through its database, exclusively quantitative aerosol properties, such as aerosol backscatter and aerosol extinction coefficients, the latter only for stations able to retrieve it independently (from Raman or High Spectral Resolution Lidars). As these coefficients are provided in terms of vertical profiles, EARLINET database must also include the details on the range resolution of the submitted data. In fact, the algorithms used in the lidar data analysis often alter the spectral content of the data, mainly working as low pass filters with the purpose of noise damping. Low pass filters are mathematically described by the Digital Signal Processing (DSP) theory as a convolution sum. As a consequence, this implies that each filter's output, at a given range (or time) in our case, will be the result of a linear combination of several lidar input data relative to different ranges (times) before and after the given range (time): a first hint of loss of resolution of the output signal. The application of filtering processes will also always distort the underlying true profile whose relevant features, like aerosol layers, will then be affected both in magnitude and in spatial extension. Thus, both the removal of noise and the spatial distortion of the true profile produce a reduction of the range resolution. This paper provides the determination of the effective resolution (ERes) of the vertical profiles of aerosol properties retrieved starting from lidar data. Large attention has been addressed to provide an assessment of the impact of low-pass filtering on the effective range resolution in the retrieval procedure.

Comparison of Aerosol Classification Results from Airborne High Spectral Resolution Lidar (HSRL) Measurements and the Calipso Vertical Feature Mask

NASA Technical Reports Server (NTRS)

Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Rogers, R. R.; Obland, M. D.; Butler, C. F.; Cook, A. L.; Harper, D. B.; Froyd, K. D.;

Chemical characterization of secondary organic aerosol constituents from isoprene ozonolysis in the presence of acidic aerosol

NASA Astrophysics Data System (ADS)

Riva, Matthieu; Budisulistiorini, Sri Hapsari; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.

2016-04-01

Isoprene is the most abundant non-methane hydrocarbon emitted into Earth's atmosphere and is predominantly derived from terrestrial vegetation. Prior studies have focused largely on the hydroxyl (OH) radical-initiated oxidation of isoprene and have demonstrated that highly oxidized compounds, such as isoprene-derived epoxides, enhance the formation of secondary organic aerosol (SOA) through heterogeneous (multiphase) reactions on acidified sulfate aerosol. However, studies on the impact of acidified sulfate aerosol on SOA formation from isoprene ozonolysis are lacking and the current work systematically examines this reaction. SOA was generated in an indoor smog chamber from isoprene ozonolysis under dark conditions in the presence of non-acidified or acidified sulfate seed aerosol. The effect of OH radicals on SOA chemical composition was investigated using diethyl ether as an OH radical scavenger. Aerosols were collected and chemically characterized by ultra performance liquid chromatography/electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS) and gas chromatography/electron impact ionization-mass spectrometry (GC/EI-MS). Analysis revealed the formation of highly oxidized compounds, including organosulfates (OSs) and 2-methylterols, which were significantly enhanced in the presence of acidified sulfate seed aerosol. OSs identified in the chamber experiments were also observed and quantified in summertime fine aerosol collected from two rural locations in the southeastern United States during the 2013 Southern Oxidant and Aerosol Study (SOAS).

The Aerosol/Cloud/Ecosystems Mission (ACE)

NASA Technical Reports Server (NTRS)

Schoeberl, Mark

2008-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2014-02-01

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

OMPS Limb Profiler: Extending SAGE and CALIPSO Stratospheric Aerosol Records

NASA Astrophysics Data System (ADS)

Taha, G.; Bhartia, P. K.; Chen, Z.; Xu, P.; Loughman, R. P.; Jaross, G.

2017-12-01

The OMPS LP instrument is designed to provide high vertical resolution ozone and aerosol profiles from measurements of the scattered solar radiation in the 290-1000 nm spectral range. It collected its first Earth limb measurement in January 10, 2012, and continues to provide daily global measurements of ozone and aerosol profiles from the cloud top up to 60 km and 40 km respectively. The relatively high vertical and spatial sampling allow detection and tracking periodic events when aerosol particles are injected into the stratosphere, such as volcanic eruptions or meteor explosions. OMPS LP can extend the long-term records of stratospheric aerosol at high vertical resolution produced by variety of sensors, such as SAGEII, GOMOS, OSIRIS and CALIPSO. Most of these instruments ceased to operate or well beyond their designed lifetime. After an absence of over a decade, SAGE III/ISS was launched earlier this year and expected to resume the high quality aerosol data record. OMPS LP is also schedule to fly on JPSS-2 and 3. In this study we will examine the suitability of using LP profiles to continue the stratospheric aerosol records beyond SAGE, OSIRIS, and CALIPSO. We will compare OMPS LP released V1.0 aerosol extinction measurements to OSIRIS and CALIPSO. Initial results shows good agreement with OSIRIS measurements to within 20%, with larger bias in the southern hemisphere. To test the effect of the assumed aerosol size model (ASD) and phase function, we compare measurements taken at similar location and time with different viewing geometry. Comparison of ascending and descending aerosol extinction daily zonal means at high latitudes shows systematic bias that is well correlated with the solar scattering angle, indicating ASD uncertainties up to 30%. In addition, results showing latitudinal, and temporal variability of stratospheric aerosol extinction and optical depth for the three instruments will also be presented and compared. We will also present OMPS LP aerosol

Aerosol optical extinction during the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) 2014 summertime field campaign, Colorado, USA

NASA Astrophysics Data System (ADS)

Dingle, Justin H.; Vu, Kennedy; Bahreini, Roya; Apel, Eric C.; Campos, Teresa L.; Flocke, Frank; Fried, Alan; Herndon, Scott; Hills, Alan J.; Hornbrook, Rebecca S.; Huey, Greg; Kaser, Lisa; Montzka, Denise D.; Nowak, John B.; Reeves, Mike; Richter, Dirk; Roscioli, Joseph R.; Shertz, Stephen; Stell, Meghan; Tanner, David; Tyndall, Geoff; Walega, James; Weibring, Petter; Weinheimer, Andrew

2016-09-01

Summertime aerosol optical extinction (βext) was measured in the Colorado Front Range and Denver metropolitan area as part of the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ) campaign during July-August 2014. An Aerodyne cavity attenuated phase shift particle light extinction monitor (CAPS-PMex) was deployed to measure βext (at average relative humidity of 20 ± 7 %) of submicron aerosols at λ = 632 nm at 1 Hz. Data from a suite of gas-phase instrumentation were used to interpret βext behavior in various categories of air masses and sources. Extinction enhancement ratios relative to CO (Δβext / ΔCO) were higher in aged urban air masses compared to fresh air masses by ˜ 50 %. The resulting increase in Δβext / ΔCO for highly aged air masses was accompanied by formation of secondary organic aerosols (SOAs). In addition, the impacts of aerosol composition on βext in air masses under the influence of urban, natural oil and gas operations (O&G), and agriculture and livestock operations were evaluated. Estimated non-refractory mass extinction efficiency (MEE) values for different air mass types ranged from 1.51 to 2.27 m2 g-1, with the minimum and maximum values observed in urban and agriculture-influenced air masses, respectively. The mass distribution for organic, nitrate, and sulfate aerosols presented distinct profiles in different air mass types. During 11-12 August, regional influence of a biomass burning event was observed, increasing the background βext and estimated MEE values in the Front Range.

Influence of intense secondary aerosol formation and long-range transport on aerosol chemistry and properties in the Seoul Metropolitan Area during spring time: results from KORUS-AQ

NASA Astrophysics Data System (ADS)

Kim, Hwajin; Zhang, Qi; Heo, Jongbae

2018-05-01

Non-refractory submicrometer particulate matter (NR-PM1) was measured in the Seoul Metropolitan Area (SMA), Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) from 14 April to 15 June 2016, as a part of the Korea-US Air Quality Study (KORUS-AQ) campaign. This was the first highly time-resolved, real-time measurement study of springtime aerosol in SMA and the results reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicrometer aerosol (PM1 = NR-PM1 + black carbon (BC)) was 22.1 µg m-3, which was composed of 44 % organics, 20 % sulfate, 17 % nitrate, 12 % ammonium, and 7 % BC. Organics had an average atomic oxygen-to-carbon (O / C) ratio of 0.49 and an average organic mass-to-carbon (OM/OC) ratio of 1.82. Four distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA; O / C = 0.15; 17 % of OA mass), food cooking activities represented by a cooking-influenced OA factor (COA; O / C = 0.19; 22 % of OA mass), and secondary organic aerosol (SOA) represented by a semi-volatile oxygenated OA factor (SV-OOA; O / C = 0.44; 27 % of OA mass) and a low-volatility oxygenated OA factor (LV-OOA; O / C = 0.91; 34 % of OA mass). Our results indicate that air quality in SMA during KORUS-AQ was influenced strongly by secondary aerosol formation, with sulfate, nitrate, ammonium, SV-OOA, and LV-OOA together accounting for 76 % of the PM1 mass. In particular, the formation of LV-OOA and sulfate was mainly promoted by elevated ozone concentrations and photochemical reactions during daytime, whereas SV-OOA and nitrate formation was contributed by both nocturnal processing of VOC and nitrogen oxides, respectively, and daytime photochemical reactions. In addition, lower nighttime temperature promoted gas-to-particle partitioning of

High Spectral Resolution Lidar Measurements of Multiple Scattering

NASA Technical Reports Server (NTRS)

Eloranta, E. W.; Piironen, P.

1996-01-01

The University of Wisconsin High Spectral Resolution Lidar (HSRL) provides unambiguous measurements of backscatter cross section, backscatter phase function, depolarization, and optical depth. This is accomplished by dividing the lidar return into separate particulate and molecular contributions. The molecular return is then used as a calibration target. We have modified the HSRL to use an I2 molecular absorption filter to separate aerosol and molecular signals. This allows measurement in dense clouds. Useful profiles extend above the cloud base until the two way optical depth reaches values between 5 and 6; beyond this, photon counting errors become large. In order to observe multiple scattering, the HSRL includes a channel which records the combined aerosol and molecular lidar return simultaneously with the spectrometer channel measurements of optical properties. This paper describes HSRL multiple scattering measurements from both water and ice clouds. These include signal strengths and depolarizations as a function of receiver field of view. All observations include profiles of extinction and backscatter cross sections. Measurements are also compared to predictions of a multiple scattering model based on small angle approximations.

Interglacial Greenland aerosol deposition: comparison of continuous high resolution chemical ice core records from the Eemian and Holocene

NASA Astrophysics Data System (ADS)

Gfeller, Gideon; Bigler, Matthias; Schüpbach, Simon; Mini, Olivia; Leuenberger, Daiana; Fischer, Hubertus

2014-05-01

Earth's climate system has been oscillating over the last million years between cold glacials and warm interglacials, leaving the imprints of their climate states in form of isotopes variations and chemical impurities in polar ice caps. In the course of the North Greenland Eemian Ice Drilling (NEEM) project, the NEEM ice core has been entirely analysed in very high depth resolution with a Continuous Flow Analysis (CFA) system for the concentrations of chemical aerosol tracers in the ice. Only in the brittle ice zone (600-1100 m depth equivalent to the time interval 3000-8000 years before present) most of the ice had to be discarded due to multifractured core material. Based on the unique reconstructed age scale to unfold the stratigraphically disturbed part from about 2200 m depth downwards (NEEM community members, Nature, 2013), we are able to present the first Greenland chemistry record over the entire last interglacial, the so called Eemian period (about 128'000 to 115'000 years ago). As the Eemian is believed to have been 4 to 8 degrees C warmer than the modern climate, it can be used as an analogue for our present warming climate and, thus, contributes to a better understanding of processes causing natural variations. By means of the chemistry records we are able to assess the natural variability of Greenland Eemian climate and gain insight in its biogeochemical state. Here, short-term variability as well as long term trends of soluble chemical impurities in the Eemian are investigated and compared with those in the Holocene. Changes of organic processes in soils and biomass burning for example are assessed through soluble ammonium and nitrate concentrations. In comparison to the Holocene, ammonium concentrations were about 25% higher during the Eemian. Nitrate, on the other hand, shows about 25% lower concentrations. Sodium concentrations, reflecting changes in sea salt aerosol, are about 35% lower during the Eemian than during the Holocene. Calcium

Aerosol chemical composition at Cabauw, The Netherlands as observed in two intensive periods in May 2008 and March 2009

NASA Astrophysics Data System (ADS)

Mensah, A. A.; Holzinger, R.; Otjes, R.; Trimborn, A.; Mentel, Th. F.; ten Brink, H.; Henzing, B.; Kiendler-Scharr, A.

2012-05-01

Observations of aerosol chemical composition in Cabauw, the Netherlands, are presented for two intensive measurement periods in May 2008 and March 2009. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and is compared to observations from aerosol size distribution measurements as well as composition measurements with a Monitor for AeRosol and GAses (MARGA) based instrument and a Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS). An overview of the data is presented and the data quality is discussed. In May 2008 enhanced pollution was observed with organics contributing 40% to the PM1 mass. In contrast the observed average mass loading was lower in March 2009 and a dominance of ammonium nitrate (42%) was observed. The semi-volatile nature of ammonium nitrate is evident in the diurnal cycles with maximum concentrations observed in the morning hours in May 2008 and little diurnal variation observed in March 2009. Size dependent composition data from AMS measurements are presented and show a dominance of organics in the size range below 200 nm. A higher O:C ratio of the organics is observed for May 2008 than for March 2009. Together with the time series of individual tracer ions this shows the dominance of OOA over HOA in May 2008.

Fine-scale application of WRF-CAM5 during a dust storm episode over East Asia: Sensitivity to grid resolutions and aerosol activation parameterizations

NASA Astrophysics Data System (ADS)

Wang, Kai; Zhang, Yang; Zhang, Xin; Fan, Jiwen; Leung, L. Ruby; Zheng, Bo; Zhang, Qiang; He, Kebin

2018-03-01

An advanced online-coupled meteorology and chemistry model WRF-CAM5 has been applied to East Asia using triple-nested domains at different grid resolutions (i.e., 36-, 12-, and 4-km) to simulate a severe dust storm period in spring 2010. Analyses are performed to evaluate the model performance and investigate model sensitivity to different horizontal grid sizes and aerosol activation parameterizations and to examine aerosol-cloud interactions and their impacts on the air quality. A comprehensive model evaluation of the baseline simulations using the default Abdul-Razzak and Ghan (AG) aerosol activation scheme shows that the model can well predict major meteorological variables such as 2-m temperature (T2), water vapor mixing ratio (Q2), 10-m wind speed (WS10) and wind direction (WD10), and shortwave and longwave radiation across different resolutions with domain-average normalized mean biases typically within ±15%. The baseline simulations also show moderate biases for precipitation and moderate-to-large underpredictions for other major variables associated with aerosol-cloud interactions such as cloud droplet number concentration (CDNC), cloud optical thickness (COT), and cloud liquid water path (LWP) due to uncertainties or limitations in the aerosol-cloud treatments. The model performance is sensitive to grid resolutions, especially for surface meteorological variables such as T2, Q2, WS10, and WD10, with the performance generally improving at finer grid resolutions for those variables. Comparison of the sensitivity simulations with an alternative (i.e., the Fountoukis and Nenes (FN) series scheme) and the default (i.e., AG scheme) aerosol activation scheme shows that the former predicts larger values for cloud variables such as CDNC and COT across all grid resolutions and improves the overall domain-average model performance for many cloud/radiation variables and precipitation. Sensitivity simulations using the FN series scheme also have large impacts on

Aerosol Absorption Retrievals from the PACE Broad Spectrum Ocean Color Instrument (OCI)

NASA Technical Reports Server (NTRS)

Mattoo, Shana; Remer, Lorraine A.; Levy, Robert C.; Gupta, Pawan; Ahmad, Ziauddin; Martins, J. Vanderlei; Lima, Adriana Rocha; Torres, Omar

2016-01-01

The PACE (Pre-­Aerosol, Clouds and ocean Ecosystem) mission, anticipated for launch in the early 2020s, is designed to characterize oceanic and atmospheric properties. The primary instrument on-­-board will be a moderate resolution (approximately 1 km nadir) radiometer, called the Ocean Color Instrument (OCI). OCI will provide high spectral resolution (5 nm) from the UV to NIR (350 - 800 nm), with additional spectral bands in the NIR and SWIR. The OCI itself is an excellent instrument for atmospheric objectives, providing measurements across a broad spectral range that in essence combines the capabilities of MODIS and OMI, but with the UV channels from OMI to be available at moderate resolution. (Image credit: PACE Science Definition Team Report). Objective: Can we make use of the UV-­SWIR measurements to derive information about aerosol absorption when aerosol loading is high?

Airborne Lidar Measurements of Aerosol Optical Properties During SAFARI-2000

NASA Technical Reports Server (NTRS)

McGill, M. J.; Hlavka, D. L.; Hart, W. D.; Welton, E. J.; Campbell, J. R.; Starr, David OC. (Technical Monitor)

2002-01-01

The Cloud Physics Lidar (CPL) operated onboard the NASA ER-2 high altitude aircraft during the SAFARI-2000 field campaign. The CPL provided high spatial resolution measurements of aerosol optical properties at both 1064 nm and 532 nm. We present here results of planetary boundary layer (PBL) aerosol optical depth analysis and profiles of aerosol extinction. Variation of optical depth and extinction are examined as a function of regional location. The wide-scale aerosol mapping obtained by the CPL is a unique data set that will aid in future studies of aerosol transport. Comparisons between the airborne CPL and ground-based MicroPulse Lidar Network (MPL-Net) sites are shown to have good agreement.

Combining low- to high-resolution transit spectroscopy of HD 189733b. Linking the troposphere and the thermosphere of a hot gas giant

NASA Astrophysics Data System (ADS)

Pino, Lorenzo; Ehrenreich, David; Wyttenbach, Aurélien; Bourrier, Vincent; Nascimbeni, Valerio; Heng, Kevin; Grimm, Simon; Lovis, Christophe; Malik, Matej; Pepe, Francesco; Piotto, Giampaolo

2018-04-01

Space-borne low- to medium-resolution (ℛ 102-103) and ground-based high-resolution spectrographs (ℛ 105) are commonly used to obtain optical and near infrared transmission spectra of exoplanetary atmospheres. In this wavelength range, space-borne observations detect the broadest spectral features (alkali doublets, molecular bands, scattering, etc.), while high-resolution, ground-based observations probe the sharpest features (cores of the alkali lines, molecular lines). The two techniques differ by several aspects. (1) The line spread function of ground-based observations is 103 times narrower than for space-borne observations; (2) Space-borne transmission spectra probe up to the base of thermosphere (P ≳ 10-6 bar), while ground-based observations can reach lower pressures (down to 10-11 bar) thanks to their high resolution; (3) Space-borne observations directly yield the transit depth of the planet, while ground-based observations can only measure differences in the apparent size of the planet at different wavelengths. These differences make it challenging to combine both techniques. Here, we develop a robust method to compare theoretical models with observations at different resolutions. We introduce πη, a line-by-line 1D radiative transfer code to compute theoretical transmission spectra over a broad wavelength range at very high resolution (ℛ 106, or Δλ 0.01 Å). An hybrid forward modeling/retrieval optimization scheme is devised to deal with the large computational resources required by modeling a broad wavelength range 0.3-2 μm at high resolution. We apply our technique to HD 189733b. In this planet, HST observations reveal a flattened spectrum due to scattering by aerosols, while high-resolution ground-based HARPS observations reveal sharp features corresponding to the cores of sodium lines. We reconcile these apparent contrasting results by building models that reproduce simultaneously both data sets, from the troposphere to the thermosphere

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

NASA Astrophysics Data System (ADS)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Simulating Aerosol Indirect Effects with Improved Aerosol-Cloud- Precipitation Representations in a Coupled Regional Climate Model

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

Zhang, Yang; Leung, L. Ruby; Fan, Jiwen

This is a collaborative project among North Carolina State University, Pacific Northwest National Laboratory, and Scripps Institution of Oceanography, University of California at San Diego to address the critical need for an accurate representation of aerosol indirect effect in climate and Earth system models. In this project, we propose to develop and improve parameterizations of aerosol-cloud-precipitation feedbacks in climate models and apply them to study the effect of aerosols and clouds on radiation and hydrologic cycle. Our overall objective is to develop, improve, and evaluate parameterizations to enable more accurate simulations of these feedbacks in high resolution regional and globalmore » climate models.« less

Arrange and average algorithm for the retrieval of aerosol parameters from multiwavelength high-spectral-resolution lidar/Raman lidar data.

PubMed

Chemyakin, Eduard; Müller, Detlef; Burton, Sharon; Kolgotin, Alexei; Hostetler, Chris; Ferrare, Richard

2014-11-01

We present the results of a feasibility study in which a simple, automated, and unsupervised algorithm, which we call the arrange and average algorithm, is used to infer microphysical parameters (complex refractive index, effective radius, total number, surface area, and volume concentrations) of atmospheric aerosol particles. The algorithm uses backscatter coefficients at 355, 532, and 1064 nm and extinction coefficients at 355 and 532 nm as input information. Testing of the algorithm is based on synthetic optical data that are computed from prescribed monomodal particle size distributions and complex refractive indices that describe spherical, primarily fine mode pollution particles. We tested the performance of the algorithm for the "3 backscatter (β)+2 extinction (α)" configuration of a multiwavelength aerosol high-spectral-resolution lidar (HSRL) or Raman lidar. We investigated the degree to which the microphysical results retrieved by this algorithm depends on the number of input backscatter and extinction coefficients. For example, we tested "3β+1α," "2β+1α," and "3β" lidar configurations. This arrange and average algorithm can be used in two ways. First, it can be applied for quick data processing of experimental data acquired with lidar. Fast automated retrievals of microphysical particle properties are needed in view of the enormous amount of data that can be acquired by the NASA Langley Research Center's airborne "3β+2α" High-Spectral-Resolution Lidar (HSRL-2). It would prove useful for the growing number of ground-based multiwavelength lidar networks, and it would provide an option for analyzing the vast amount of optical data acquired with a future spaceborne multiwavelength lidar. The second potential application is to improve the microphysical particle characterization with our existing inversion algorithm that uses Tikhonov's inversion with regularization. This advanced algorithm has recently undergone development to allow automated and

Characterization of organic nitrate constituents of secondary organic aerosol (SOA) from nitrate-radical-initiated oxidation of limonene using high-resolution chemical ionization mass spectrometry

NASA Astrophysics Data System (ADS)

Faxon, Cameron; Hammes, Julia; Le Breton, Michael; Kant Pathak, Ravi; Hallquist, Mattias

2018-04-01

The gas-phase nitrate radical (NO3⚫) initiated oxidation of limonene can produce organic nitrate species with varying physical properties. Low-volatility products can contribute to secondary organic aerosol (SOA) formation and organic nitrates may serve as a NOx reservoir, which could be especially important in regions with high biogenic emissions. This work presents the measurement results from flow reactor studies on the reaction of NO3⚫ with limonene using a High-Resolution Time-of-Flight Chemical Ionization Mass Spectrometer (HR-ToF-CIMS) combined with a Filter Inlet for Gases and AEROsols (FIGAERO). Major condensed-phase species were compared to those in the Master Chemical Mechanism (MCM) limonene mechanism, and many non-listed species were identified. The volatility properties of the most prevalent organic nitrates in the produced SOA were determined. Analysis of multiple experiments resulted in the identification of several dominant species (including C10H15NO6, C10H17NO6, C8H11NO6, C10H17NO7, and C9H13NO7) that occurred in the SOA under all conditions considered. Additionally, the formation of dimers was consistently observed and these species resided almost completely in the particle phase. The identities of these species are discussed, and formation mechanisms are proposed. Cluster analysis of the desorption temperatures corresponding to the analyzed particle-phase species yielded at least five distinct groupings based on a combination of molecular weight and desorption profile. Overall, the results indicate that the oxidation of limonene by NO3⚫ produces a complex mixture of highly oxygenated monomer and dimer products that contribute to SOA formation.

A New Hybrid Spatio-temporal Model for Estimating Daily Multi-year PM2.5 Concentrations Across Northeastern USA Using High Resolution Aerosol Optical Depth Data

NASA Technical Reports Server (NTRS)

Kloog, Itai; Chudnovsky, Alexandra A.; Just, Allan C.; Nordio, Francesco; Koutrakis, Petros; Coull, Brent A.; Lyapustin, Alexei; Wang, Yujie; Schwartz, Joel

2014-01-01

The use of satellite-based aerosol optical depth (AOD) to estimate fine particulate matter PM(sub 2.5) for epidemiology studies has increased substantially over the past few years. These recent studies often report moderate predictive power, which can generate downward bias in effect estimates. In addition, AOD measurements have only moderate spatial resolution, and have substantial missing data. We make use of recent advances in MODIS satellite data processing algorithms (Multi-Angle Implementation of Atmospheric Correction (MAIAC), which allow us to use 1 km (versus currently available 10 km) resolution AOD data.We developed and cross validated models to predict daily PM(sub 2.5) at a 1X 1 km resolution across the northeastern USA (New England, New York and New Jersey) for the years 2003-2011, allowing us to better differentiate daily and long term exposure between urban, suburban, and rural areas. Additionally, we developed an approach that allows us to generate daily high-resolution 200 m localized predictions representing deviations from the area 1 X 1 km grid predictions. We used mixed models regressing PM(sub 2.5) measurements against day-specific random intercepts, and fixed and random AOD and temperature slopes. We then use generalized additive mixed models with spatial smoothing to generate grid cell predictions when AOD was missing. Finally, to get 200 m localized predictions, we regressed the residuals from the final model for each monitor against the local spatial and temporal variables at each monitoring site. Our model performance was excellent (mean out-of-sample R(sup 2) = 0.88). The spatial and temporal components of the out-of-sample results also presented very good fits to the withheld data (R(sup 2) = 0.87, R(sup)2 = 0.87). In addition, our results revealed very little bias in the predicted concentrations (Slope of predictions versus withheld observations = 0.99). Our daily model results show high predictive accuracy at high spatial resolutions

A New Hybrid Spatio-Temporal Model For Estimating Daily Multi-Year PM2.5 Concentrations Across Northeastern USA Using High Resolution Aerosol Optical Depth Data

PubMed Central

Kloog, Itai; Chudnovsky, Alexandra A.; Just, Allan C.; Nordio, Francesco; Koutrakis, Petros; Coull, Brent A.; Lyapustin, Alexei; Wang, Yujie; Schwartz, Joel

2017-01-01

Background The use of satellite-based aerosol optical depth (AOD) to estimate fine particulate matter (PM2.5) for epidemiology studies has increased substantially over the past few years. These recent studies often report moderate predictive power, which can generate downward bias in effect estimates. In addition, AOD measurements have only moderate spatial resolution, and have substantial missing data. Methods We make use of recent advances in MODIS satellite data processing algorithms (Multi-Angle Implementation of Atmospheric Correction (MAIAC), which allow us to use 1 km (versus currently available 10 km) resolution AOD data. We developed and cross validated models to predict daily PM2.5 at a 1×1km resolution across the northeastern USA (New England, New York and New Jersey) for the years 2003–2011, allowing us to better differentiate daily and long term exposure between urban, suburban, and rural areas. Additionally, we developed an approach that allows us to generate daily high-resolution 200 m localized predictions representing deviations from the area 1×1 km grid predictions. We used mixed models regressing PM2.5 measurements against day-specific random intercepts, and fixed and random AOD and temperature slopes. We then use generalized additive mixed models with spatial smoothing to generate grid cell predictions when AOD was missing. Finally, to get 200 m localized predictions, we regressed the residuals from the final model for each monitor against the local spatial and temporal variables at each monitoring site. Results Our model performance was excellent (mean out-of-sample R2=0.88). The spatial and temporal components of the out-of-sample results also presented very good fits to the withheld data (R2=0.87, R2=0.87). In addition, our results revealed very little bias in the predicted concentrations (Slope of predictions versus withheld observations = 0.99). Conclusion Our daily model results show high predictive accuracy at high spatial resolutions

A New Hybrid Spatio-Temporal Model For Estimating Daily Multi-Year PM2.5 Concentrations Across Northeastern USA Using High Resolution Aerosol Optical Depth Data.

PubMed

Kloog, Itai; Chudnovsky, Alexandra A; Just, Allan C; Nordio, Francesco; Koutrakis, Petros; Coull, Brent A; Lyapustin, Alexei; Wang, Yujie; Schwartz, Joel

2014-10-01

The use of satellite-based aerosol optical depth (AOD) to estimate fine particulate matter (PM 2.5 ) for epidemiology studies has increased substantially over the past few years. These recent studies often report moderate predictive power, which can generate downward bias in effect estimates. In addition, AOD measurements have only moderate spatial resolution, and have substantial missing data. We make use of recent advances in MODIS satellite data processing algorithms (Multi-Angle Implementation of Atmospheric Correction (MAIAC), which allow us to use 1 km (versus currently available 10 km) resolution AOD data. We developed and cross validated models to predict daily PM 2.5 at a 1×1km resolution across the northeastern USA (New England, New York and New Jersey) for the years 2003-2011, allowing us to better differentiate daily and long term exposure between urban, suburban, and rural areas. Additionally, we developed an approach that allows us to generate daily high-resolution 200 m localized predictions representing deviations from the area 1×1 km grid predictions. We used mixed models regressing PM 2.5 measurements against day-specific random intercepts, and fixed and random AOD and temperature slopes. We then use generalized additive mixed models with spatial smoothing to generate grid cell predictions when AOD was missing. Finally, to get 200 m localized predictions, we regressed the residuals from the final model for each monitor against the local spatial and temporal variables at each monitoring site. Our model performance was excellent (mean out-of-sample R 2 =0.88). The spatial and temporal components of the out-of-sample results also presented very good fits to the withheld data (R 2 =0.87, R 2 =0.87). In addition, our results revealed very little bias in the predicted concentrations (Slope of predictions versus withheld observations = 0.99). Our daily model results show high predictive accuracy at high spatial resolutions and will be useful in

Gas/Particle Partitioning of Organic Acids and Organic Aerosols in a Ponderosa Pine Forest in Colorado during BEACHON-RoMBAS 2011

NASA Astrophysics Data System (ADS)

Jimenez, J. L.; Yatavelli, L.; Stark, H.; Hayes, P. L.; Campuzano-Jost, P.; Thompson, S.; Kimmel, J. R.; Day, D. A.; Cubison, M. J.; Thornton, J. A.; Jayne, J.; Worsnop, D. R.

2012-12-01

The Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS) took place at Manitou Forest, CO, during July-Aug. 2011. Gas and particle-phase organic acids were analyzed in real time using a micro-orifice volatilization impactor chemical ionization high-resolution time-of-flight mass spectrometer (MOVI-HRToF-CIMS; Yatavelli et al., AS&T 2012; Yatavelli & Thornton, AS&T 2010) with acetate as the reagent ion. During the gas sampling phase (when the MOVI was at room temperature) aerosol was collected on the MOVI impactor, and was subsequently thermally desorbed over 10 min. under nitrogen, allowing the collection of temperature-programmed thermal desorption (TPTD) mass spectra of particle-phase species. The high resolution of the instrument allows the determination of the elemental composition of most detected ions. Positive Matrix Factorization (PMF) is shown to be very useful to quantify the CIMS backgrounds during the different phases of operation. Two methods were used to estimate the volatility of the detected species. First, the fraction of each species in the particle phase (Fp) vs carbon number was found to approximately follow partitioning theory, both for the alkanoic acids and also for the total acid signal, after accounting for the effect of the oxidation state on vapor pressure. Fp was found to respond on timescales of ~1 h to changes in ambient temperature, indicating that diffusion limitations to evaporation are not major for the aerosol at this site. Preliminary results suggest that Fp depends more strongly on vapor pressure and temperature than on RH, suggesting preferential partitioning for the organic phase rather than the water phase. Secondly, the volatility of individual or groups of acids can be quantified based on the TPTD signal based on calibration with multiple acids of known vapor pressure at concentrations similar to ambient, analogous to the methods of

Improved Cloud and Snow Screening in MAIAC Aerosol Retrievals Using Spectral and Spatial Analysis

NASA Technical Reports Server (NTRS)

Lyapustin, A.; Wang, Y.; Laszlo, I.; Kokrkin, S.

2012-01-01

An improved cloud/snow screening technique in the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm is described. It is implemented as part of MAIAC aerosol retrievals based on analysis of spectral residuals and spatial variability. Comparisons with AERONET aerosol observations and a large-scale MODIS data analysis show strong suppression of aerosol optical thickness outliers due to unresolved clouds and snow. At the same time, the developed filter does not reduce the aerosol retrieval capability at high 1 km resolution in strongly inhomogeneous environments, such as near centers of the active fires. Despite significant improvement, the optical depth outliers in high spatial resolution data are and will remain the problem to be addressed by the application-dependent specialized filtering techniques.

“Lidar Investigations of Aerosol, Cloud, and Boundary Layer Properties Over the ARM ACRF Sites”

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

Ferrare, Richard; Turner, David

2015-01-13

Project goals; Characterize the aerosol and ice vertical distributions over the ARM NSA site, and in particular to discriminate between elevated aerosol layers and ice clouds in optically thin scattering layers; Characterize the water vapor and aerosol vertical distributions over the ARM Darwin site, how these distributions vary seasonally, and quantify the amount of water vapor and aerosol that is above the boundary layer; Use the high temporal resolution Raman lidar data to examine how aerosol properties vary near clouds; Use the high temporal resolution Raman lidar and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thinmore » continental cumulus clouds; and Use the high temporal Raman lidar data to continue to characterize the turbulence within the convective boundary layer and how the turbulence statistics (e.g., variance, skewness) is correlated with larger scale variables predicted by models.« less

Evaluation of Aerosol Properties over Ocean from Moderate Resolution Imaging Spectroradiometer (MODIS) during ACE-Asia

NASA Technical Reports Server (NTRS)

Chu, D. A.; Remer, L. A.; Kaufman, Y. J.; Schmid, B.; Redemann, J.; Knobelspiesse, K.; Chern, J.-D.; Livingston, J.; Russell, P. B.; Xiong, X.;

Slow aging in Secondary Organic Aerosol observed by Liquid Chromatography coupled with High-Resolution Mass Spectrometry

NASA Astrophysics Data System (ADS)

Bones, D. L.; Bateman, A. P.; Nguyen, T. B.; Laskin, J.; Laskin, A.; Nizkorodov, S.

2009-12-01

This study investigated long term changes in the chemical composition of model biogenic secondary organic aerosol (SOA) prepared via ozonolysis of the terpene limonene. This SOA has been observed to turn brown when exposed to NH4+. Our hypothesis is that the chromophoric compounds responsible for this color change are suspected to be imidazole-like or pyridinium-like compounds. These compounds are only present in small relative amounts, hence standard mass spectrometry is insufficient to unambiguously detect these compounds. However, a combination of HPLC and high resolution electrospray ionization mass spectrometry allows assignments of chemical formulae to individual peaks. These and other experiments confirm the presence of N-containing compounds in treated SOA. We are in the process of determining the exact identity of these species by MS/MS methods. LC-MS can also provide information about the polarity of the compounds in SOA. Most compounds in limonene-O3 SOA are polar and are detected at short retention times; peaks suggesting trimeric species appear at longer retention times in the case of fresh SOA, but at shorter times with the bulk of the components for aged SOA. Limonene SOA has been shown to be composed of monomers, dimers, trimers and larger oligomers. The appearance of trimers in specific regions of the chromatogram suggests these species are genuine SOA components and not an artifact of electrospray ionization. Changes in biogenic SOA over time are important because of the propensity of SOA to affect direct and indirect radiative forcing.

High-resolution Sulfur Isotopes in Ice Cores Identify Large Stratospheric Eruptions

NASA Astrophysics Data System (ADS)

Burke, A.; Sigl, M.; Moore, K.; Nita, D. C.; Adkins, J. F.; Paris, G.; McConnell, J.

2016-12-01

The record of the volcanic forcing of climate over the past 2500 years is reconstructed primarily from sulfate concentrations in ice cores. Of particular interest are stratospheric eruptions, as these afford sulfate aerosols the longest residence time and largest dispersion in the atmosphere, and thus the greatest impact on radiative forcing. Identification of stratospheric eruptions currently relies on the successful matching of the same volcanic sulfate peak in ice cores from both the Northern and Southern hemispheres (a "bipolar event"). These are interpreted to reflect the global distribution of sulfur aerosols by the stratospheric winds. Despite its recent success, this method relies on precise and accurate dating of ice cores, in order to distinguish between a true `bipolar event' and two separate eruptions that occurred in close temporal succession. Sulfur isotopes can been used to distinguish between these two scenarios since stratospheric sulfur aerosols are exposed to UV radiation which imparts a mass independent fractionation (Baroni et al., 2007). Mass independent fractionation of sulfate in ice cores thus offers a novel method of fingerprinting stratospheric eruptions, and thus refining the historic record of explosive volcanism and its forcing of climate. Here we present new high-resolution (sub-annual) sulfur isotope data from the Tunu Ice core in Greenland over seven eruptions. Sulfur isotopes were measured by MC-ICP-MS, which substantially reduces sample size requirements and allows high temporal resolution from a single ice core. We demonstrate the efficacy of the method on recent, well-known eruptions (including Pinatubo and Katmai/Novarupta), and then apply it to unidentified sulfate peaks, allowing us to identify new stratospheric eruptions. Baroni, M., Thiemens, M. H., Delmas, R. J., & Savarino, J. (2007). Mass-independent sulfur isotopic compositions in stratospheric volcanic eruptions. Science, 315(5808), 84-87. http://doi.org/10

Aerosol mass spectrometry: particle-vaporizer interactions and their consequences for the measurements

NASA Astrophysics Data System (ADS)

Drewnick, F.; Diesch, J.-M.; Faber, P.; Borrmann, S.

2015-09-01

The Aerodyne aerosol mass spectrometer (AMS) is a frequently used instrument for on-line measurement of the ambient sub-micron aerosol composition. With the help of calibrations and a number of assumptions on the flash vaporization and electron impact ionization processes, this instrument provides robust quantitative information on various non-refractory ambient aerosol components. However, when measuring close to certain anthropogenic or marine sources of semi-refractory aerosols, several of these assumptions may not be met and measurement results might easily be incorrectly interpreted if not carefully analyzed for unique ions, isotope patterns, and potential slow vaporization associated with semi-refractory species. Here we discuss various aspects of the interaction of aerosol particles with the AMS tungsten vaporizer and the consequences for the measurement results: semi-refractory components - i.e., components that vaporize but do not flash-vaporize at the vaporizer and ionizer temperatures, like metal halides (e.g., chlorides, bromides or iodides of Al, Ba, Cd, Cu, Fe, Hg, K, Na, Pb, Sr, Zn) - can be measured semi-quantitatively despite their relatively slow vaporization from the vaporizer. Even though non-refractory components (e.g., NH4NO3 or (NH4)2SO4) vaporize quickly, under certain conditions their differences in vaporization kinetics can result in undesired biases in ion collection efficiency in thresholded measurements. Chemical reactions with oxygen from the aerosol flow can have an influence on the mass spectra for certain components (e.g., organic species). Finally, chemical reactions of the aerosol with the vaporizer surface can result in additional signals in the mass spectra (e.g., WO2Cl2-related signals from particulate Cl) and in conditioning or contamination of the vaporizer, with potential memory effects influencing the mass spectra of subsequent measurements. Laboratory experiments that investigate these particle-vaporizer interactions are

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

PubMed

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

2017-12-19

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

Predicting daily PM2.5 concentrations in Texas using high-resolution satellite aerosol optical depth.

PubMed

Zhang, Xueying; Chu, Yiyi; Wang, Yuxuan; Zhang, Kai

2018-08-01

The regulatory monitoring data of particulate matter with an aerodynamic diameter <2.5μm (PM 2.5 ) in Texas have limited spatial and temporal coverage. The purpose of this study is to estimate the ground-level PM 2.5 concentrations on a daily basis using satellite-retrieved Aerosol Optical Depth (AOD) in the state of Texas. We obtained the AOD values at 1-km resolution generated through the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm based on the images retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) satellites. We then developed mixed-effects models based on AODs, land use features, geographic characteristics, and weather conditions, and the day-specific as well as site-specific random effects to estimate the PM 2.5 concentrations (μg/m 3 ) in the state of Texas during the period 2008-2013. The mixed-effects models' performance was evaluated using the coefficient of determination (R 2 ) and square root of the mean squared prediction error (RMSPE) from ten-fold cross-validation, which randomly selected 90% of the observations for training purpose and 10% of the observations for assessing the models' true prediction ability. Mixed-effects regression models showed good prediction performance (R 2 values from 10-fold cross validation: 0.63-0.69). The model performance varied by regions and study years, and the East region of Texas, and year of 2009 presented relatively higher prediction precision (R 2 : 0.62 for the East region; R 2 : 0.69 for the year of 2009). The PM 2.5 concentrations generated through our developed models at 1-km grid cells in the state of Texas showed a decreasing trend from 2008 to 2013 and a higher reduction of predicted PM 2.5 in more polluted areas. Our findings suggest that mixed-effects regression models developed based on MAIAC AOD are a feasible approach to predict ground-level PM 2.5 in Texas. Predicted PM 2.5 concentrations at the 1-km resolution on a daily basis can be used for

The Two-Column Aerosol Project: Phase I-Overview and impact of elevated aerosol layers on aerosol optical depth

DOE PAGES

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; ...

2016-01-08

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facilitymore » (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). In addition, these layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. Lastly, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.« less

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

NASA Technical Reports Server (NTRS)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.;

The Two-Column Aerosol Project: Phase I—Overview and impact of elevated aerosol layers on aerosol optical depth

NASA Astrophysics Data System (ADS)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

2016-01-01

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

Contrasting online MSn spectra of organic acids in ambient aerosol from the boreal forest at Hyytiälä, Finland and from the mixed forest at the Taunus observatory, Germany

NASA Astrophysics Data System (ADS)

Vogel, Alexander L.; Äijälä, Mikko; Ehn, Mikael; Junninen, Heikki; Petäjä, Tuukka; Worsnop, Douglas R.; Kulmala, Markku; Williams, Jonathan; Schneider, Johannes; Hoffmann, Thorsten

2013-04-01

Emission of biogenic volatile organic compounds (BVOCs) by the vegetation and subsequent atmospheric oxidation leads to the formation of secondary organic aerosol (SOA). Therefore, forests are a main source of aerosols which have significant impact on the earth's climate.[1] The oxidation of BVOCs results in a variety of mostly unidentified organic species in trace level concentrations, which partition between gas- and particle-phase. Organic acids are of particular importance for the particle-phase fraction, since the higher oxidation state and molecular mass, compared to the corresponding precursors, is accompanied by a much lower volatility. Until now, only limited instrumentation exists for the simultaneous online analysis of organic acids in gas- and particle-phase. Here we show the first field application of an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI-IT-MS) in combination with a miniature Versatile Aerosol Concentration Enrichment System (mVACES) for measuring organic acids in gas- and particle-phase[2]. The benefits of the online APCI-IT-MS are soft ionization with low fragmentation, high time resolution and less sampling artifacts than in the common procedure of taking filter samples, extraction and subsequent detection with LC-MS. Furthermore, the capability to perform online MSn of isolated m/z ratios from ambient and laboratory generated aerosol leads to an improved understanding of the composition of secondary organic aerosol. The here described measurements were conducted during the HUMPPA-COPEC 2010 campaign at Hyytiälä, Finland and during the INUIT campaign 2012 on Mt. Kleiner Feldberg, Germany. By merging APCI-IT-MS data with data from the Aerodyné C-ToF-AMS, it can be observed that the gas- to particle-partitioning of organic acids strongly depends on the fraction of aerosol which is organic matter, as it is predicted by a partitioning model[3]. High observed gas-phase concentrations of organic acids at Hyyti

Measurements of aerosol chemical composition in boreal forest summer conditions

NASA Astrophysics Data System (ADS)

ńijälä, M.; Junninen, H.; Ehn, M.; Petäjä, T.; Vogel, A.; Hoffmann, T.; Corrigan, A.; Russell, L.; Makkonen, U.; Virkkula, A.; Mäntykenttä, J.; Kulmala, M.; Worsnop, D.

2012-04-01

Boreal forests are an important biome, covering vast areas of the northern hemisphere and affecting the global climate change via various feedbacks [1]. Despite having relatively few anthropogenic primary aerosol sources, they always contain a non-negligible aerosol population [2]. This study describes aerosol chemical composition measurements using Aerodyne Aerosol Mass Spectrometer (C-ToF AMS, [3]), carried out at a boreal forest area in Hyytiälä, Southern Finland. The site, Helsinki University SMEAR II measurement station [4], is situated at a homogeneous Scots pine (Pinus sylvestris) forest stand. In addition to the station's permanent aerosol, gas phase and meteorological instruments, during the HUMPPA (Hyytiälä United Measurements of Photochemistry and Particles in Air) campaign in July 2010, a very comprehensive set of atmospheric chemistry measurement instrumentation was provided by the Max Planck Institute for chemistry, Johannes Gutenberg-University, University of California and the Finnish Meteorological institute. In this study aerosol chemical composition measurements from the campaign are presented. The dominant aerosol chemical species during the campaign were the organics, although periods with elevated amounts of particulate sulfates were also seen. The overall AMS measured particle mass concentrations varied from near zero to 27 μg/m observed during a forest fire smoke episode. The AMS measured aerosol mass loadings were found to agree well with DMPS derived mass concentrations (r2=0.998). The AMS data was also compared with three other aerosol instruments. The Marga instrument [5] was used to provide a quantitative semi-online measurement of inorganic chemical compounds in particle phase. Fourier Transform Infrared Spectroscopy (FTIR) analysis was performed on daily filter samples, enabling the identification and quantification of organic aerosol subspecies. Finally an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI

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

PubMed Central

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

2013-01-01

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

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

PubMed

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

2013-12-17

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

Characterization of a Quadrotor Unmanned Aircraft System for Aerosol-Particle-Concentration Measurements.

PubMed

Brady, James M; Stokes, M Dale; Bonnardel, Jim; Bertram, Timothy H

2016-02-02

High-spatial-resolution, near-surface vertical profiling of atmospheric chemical composition is currently limited by the availability of experimental platforms that can sample in constrained environments. As a result, measurements of near-surface gradients in trace gas and aerosol particle concentrations have been limited to studies conducted from fixed location towers or tethered balloons. Here, we explore the utility of a quadrotor unmanned aircraft system (UAS) as a sampling platform to measure vertical and horizontal concentration gradients of trace gases and aerosol particles at high spatial resolution (1 m) within the mixed layer (0-100 m). A 3D Robotics Iris+ autonomous quadrotor UAS was outfitted with a sensor package consisting of a two-channel aerosol optical particle counter and a CO2 sensor. The UAS demonstrated high precision in both vertical (±0.5 m) and horizontal positions (±1 m), highlighting the potential utility of quadrotor UAS drones for aerosol- and trace-gas measurements within complex terrain, such as the urban environment, forest canopies, and above difficult-to-access areas such as breaking surf. Vertical profiles of aerosol particle number concentrations, acquired from flights conducted along the California coastline, were used to constrain sea-spray aerosol-emission rates from coastal wave breaking.

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

Aerosol loading impact on Asian monsoon precipitation patterns

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

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

NASA Astrophysics Data System (ADS)

Dreyfus, Matthew A.

. 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

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

NASA Astrophysics Data System (ADS)

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; Easter, Richard C.; Ferrare, Richard A.; Hair, Johnathan W.; Hostetler, Chris A.; Liu, Ying; Ortega, Ivan; Sedlacek, Arthur; Shilling, John E.; Shrivastava, Manish; Springston, Stephen R.; Tomlinson, Jason M.; Volkamer, Rainer; Wilson, Jacqueline; Zaveri, Rahul A.; Zelenyuk, Alla

2016-08-01

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurements during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.

High Spectral Resolution Lidar Measurements Using an I2 Absorption Filter

NASA Technical Reports Server (NTRS)

Eloranta, E. W.; Piironen, P.

1996-01-01

The University of Wisconsin high spectral resolution lidar (HSRL) measures optical properties of the atmosphere by separating the Doppler-broadened molecular backscatter return from the unbroadened aerosol return. The HSRL was modified to use an I2 absorption cell The modified HSRL transmitter uses a continuously pumped, Q-switched, injection seeded, frequency doubled Nd:YAG laser operating at a 4 kHz pulse repetition rate. This laser is tunable over a 124 GHz frequency range by temperature tuning the seed laser under computer control.

Evaluation of spatio-temporal variability of Hamburg Aerosol Climatology against aerosol datasets from MODIS and CALIOP

NASA Astrophysics Data System (ADS)

Pappas, V.; Hatzianastassiou, N.; Papadimas, C.; Matsoukas, C.; Kinne, S.; Vardavas, I.

2013-02-01

The new global aerosol climatology named HAC (Hamburg Aerosol Climatology) is compared against MODIS (MODerate resolution Imaging Spectroradiometer, Collection 5, 2000-2007) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization, Level 2-Version 3, 2006-2011) retrievals. The HAC aerosol optical depth (AOD) values are larger than MODIS in heavy aerosol load conditions (over land) and lower over oceans. Agreement between HAC and MODIS is better over land and for low AOD. Hemispherically, HAC has 16-17% smaller AOD values than MODIS. The discrepancy is slightly larger for the Southern Hemisphere (SH) than for the Northern Hemisphere (NH). Seasonally, the largest absolute differences are from March to August for NH and from September to February for SH. The spectral variability of HAC AOD is also evaluated against AERONET (1998-2007) data for sites representative of main aerosol types (pollutants, sea-salt, biomass and dust). The HAC has a stronger spectral dependence of AOD in the UV wavelengths, compared to AERONET and MODIS. For visible and near-infrared wavelengths, the spectral dependence is similar to AERONET. For specific sites, HAC AOD vertical distribution is compared to CALIOP data by looking at the fraction of columnar AOD at each altitude. The comparison suggests that HAC exhibits a smaller fraction of columnar AOD in the lowest 2-3 km than CALIOP, especially for sites with biomass burning smoke, desert dust and sea salt spray. For the region of the greater Mediterranean basin, the mean profile of HAC AOD is in very good agreement with CALIOP. The HAC AOD is very useful for distinguishing between natural and anthropogenic aerosols and provides high spectral resolution and vertically resolved information.

Quantification of Semi-Volatile gas-phase Organic Compounds (SVOCs) & Organic Aerosol species and the role of SVOCs in Secondary Organic Aerosol formation

NASA Astrophysics Data System (ADS)

Khan, M. H.; Holzinger, R.

2013-12-01

A Thermal-Desorption Proton-Transfer-Reaction Mass-Spectrometer (TD-PTR-MS) with different sampling systems (multi-stage denuder for gas phase and impact on a collector for aerosol phase) has been deployed in summer 2013 during the Southern Oxidant and Aerosol Study (SOAS) at the SEARCH ground site, Centreville, Alabama for in-situ gas phase and aerosol measurements on an hourly time resolution. A bunch of DB-1 column (0.53 mm x 5.0 μm) is used in the denuder for capturing the bulk of SVOCs and a collection-thermal-desorption (CTD) cell is used for collecting aerosol particles. Several hundreds semivolatile organic compounds (SVOCs) in gas phase and aerosol phases have been detected. The high mass resolution capabilities of ~5000, low detection limit (<0.05 pptv for gas species, <0.01 ng m-3 for aerosol species) and good physical and chemical characterization of SVOCs with the TD-PTR-MS allows constraining both, the quantity and the chemical composition. The SEARCH site was highly impacted by Biogenic Volatile Organic Compounds (BVOCs) and occasionally influenced by anthropogenic pollution. BVOCs and their oxidation products are capable of partitioning into the particle phase, so their simultaneous quantification in both phases has been used to determine the gas/particle-phase partitioning. Our results show the expected diurnal variation based on the changes of air temperature for many species. The results from this study give valuable insights into sources and processing of Secondary Organic Aerosols (SOAs) that can be used to improve parameterization algorithms in regional and global climate models.

Occurrence of weak, sub-micron, tropospheric aerosol events at high Arctic latitudes

NASA Astrophysics Data System (ADS)

O'Neill, N. T.; Pancrati, O.; Baibakov, K.; Eloranta, E.; Batchelor, R. L.; Freemantle, J.; McArthur, L. J. B.; Strong, K.; Lindenmaier, R.

2008-07-01

Numerous fine mode (sub-micron) aerosol optical events were observed during the summer of 2007 at the High Arctic atmospheric observatory (PEARL) located at Eureka, Nunavut, Canada. Half of these events could be traced to forest fires in southern and eastern Russia and the Northwest Territories of Canada. The most notable findings were that (a) a combination of ground-based measurements (passive sunphotometry, high spectral resolution lidar) could be employed to determine that weak (near sub-visual) fine mode events had occurred, and (b) this data combined with remote sensing imagery products (MODIS, OMI-AI, FLAMBE fire sources), Fourier transform spectroscopy and back trajectories could be employed to identify the smoke events.

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

NASA Astrophysics Data System (ADS)

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

2011-03-01

As part of the BAQS-Met 2007 field campaign, Aerodyne time-of-flight aerosol mass spectrometers (ToF-AMS) were deployed at two sites in southwestern Ontario from 17 June to 11 July 2007. One instrument was located at Harrow, ON, a rural, agriculture-dominated area approximately 40 km southeast of the Detroit/Windsor/Windsor urban area and 5 km north of Lake Erie. The second instrument was located at Bear Creek, ON, a rural site approximately 70 km northeast of the Harrow site and 50 km east of Detroit/Windsor. Positive matrix factorization analysis of the combined organic mass spectral dataset yields factors related to secondary organic aerosol (SOA), direct emissions, and a factor tentatively attributed to the reactive uptake of isoprene and/or condensation of its early generation reaction products. This is the first application of PMF to simultaneous AMS measurements at different sites, an approach which allows for self-consistent, direct comparison of the datasets. Case studies are utilized to investigate processing of SOA from (1) fresh emissions from Detroit/Windsor and (2) regional aerosol during periods of inter-site flow. A strong correlation is observed between SOA/excess CO and photochemical age as represented by the NOx/NOy ratio for Detroit/Windsor outflow. Although this correlation is not evident for more aged air, measurements at the two sites during inter-site transport nevertheless show evidence of continued atmospheric processing by SOA production. However, the rate of SOA production decreases with airmass age from an initial value of ~10.1 μg m-3 ppmvCO-1 h-1 for the first ~10 h of plume processing to near-zero in an aged airmass (i.e. after several days). The initial SOA production rate is comparable to the observed rate in Mexico City over similar timescales.

Aerosol direct and indirect radiative effect over Eastern Mediterranean

NASA Astrophysics Data System (ADS)

Georgoulias, Aristeidis; Alexandri, Georgia; Zanis, Prodromos; Ntogras, Christos; Poeschl, Ulrich; Kourtidis, Kostas

In this work, we present results from the QUADIEEMS project which is focused on the aerosol-cloud relations and the aerosol direct and indirect radiative effect over the region of Eastern Mediterranean. First, a gridded dataset at a resolution of 0.1x0.1 degrees (~10km) with aerosol and cloud related parameters was compiled, using level-2 satellite observations from MODIS TERRA (3/2000-12/2012) and AQUA (7/2002-12/2012). The aerosol gridded dataset has been validated against sunphotometric measurements from 12 AERONET ground stations, showing that generally MODIS overestimates aerosol optical depth (AOD550). Then, the AOD550 and fine mode ratio (FMR550) data from MODIS were combined with aerosol index (AI) data from the Earth Probe TOMS and OMI satellite sensors, wind field data from the ERA-interim reanalysis and AOD550 data for various aerosol types from the GOCART model and the MACC reanalysis to quantify the relative contribution of different aerosol types (marine, dust, anthropogenic, fine-mode natural) to the total AOD550. The aerosol-cloud relations over the region were investigated with the use of the joint high resolution aerosol-cloud gridded dataset. Specifically, we focused on the seasonal relations between the cloud droplet number concentration (CDNC) and AOD550. The aerosol direct and first indirect radiative effect was then calculated for each aerosol type separately making use of the aerosol relative contribution to the total AOD550, the CDND-AOD550 relations and satellite-based parameterizations. The direct radiative effect was also quantified using simulations from a regional climate model (REGCM4), simulations with a radiative transfer model (SBDART) and the three methods were finally intervalidated.

A Simple and Universal Aerosol Retrieval Algorithm for Landsat Series Images Over Complex Surfaces

NASA Astrophysics Data System (ADS)

Wei, Jing; Huang, Bo; Sun, Lin; Zhang, Zhaoyang; Wang, Lunche; Bilal, Muhammad

2017-12-01

Operational aerosol optical depth (AOD) products are available at coarse spatial resolutions from several to tens of kilometers. These resolutions limit the application of these products for monitoring atmospheric pollutants at the city level. Therefore, a simple, universal, and high-resolution (30 m) Landsat aerosol retrieval algorithm over complex urban surfaces is developed. The surface reflectance is estimated from a combination of top of atmosphere reflectance at short-wave infrared (2.22 μm) and Landsat 4-7 surface reflectance climate data records over densely vegetated areas and bright areas. The aerosol type is determined using the historical aerosol optical properties derived from the local urban Aerosol Robotic Network (AERONET) site (Beijing). AERONET ground-based sun photometer AOD measurements from five sites located in urban and rural areas are obtained to validate the AOD retrievals. Terra MODerate resolution Imaging Spectrometer Collection (C) 6 AOD products (MOD04) including the dark target (DT), the deep blue (DB), and the combined DT and DB (DT&DB) retrievals at 10 km spatial resolution are obtained for comparison purposes. Validation results show that the Landsat AOD retrievals at a 30 m resolution are well correlated with the AERONET AOD measurements (R2 = 0.932) and that approximately 77.46% of the retrievals fall within the expected error with a low mean absolute error of 0.090 and a root-mean-square error of 0.126. Comparison results show that Landsat AOD retrievals are overall better and less biased than MOD04 AOD products, indicating that the new algorithm is robust and performs well in AOD retrieval over complex surfaces. The new algorithm can provide continuous and detailed spatial distributions of AOD during both low and high aerosol loadings.

Final Technical Report for Interagency Agreement No. DE-SC0005453 “Characterizing Aerosol Distributions, Types, and Optical and Microphysical Properties using the NASA Airborne High Spectral Resolution Lidar (HSRL) and the Research Scanning Polarimeter (RSP)”

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

Hostetler, Chris; Ferrare, Richard

Measurements of the vertical profile of atmospheric aerosols and aerosol optical and microphysical characteristics are required to: 1) determine aerosol direct and indirect radiative forcing, 2) compute radiative flux and heating rate profiles, 3) assess model simulations of aerosol distributions and types, and 4) establish the ability of surface and space-based remote sensors to measure the indirect effect. Consequently the ASR program calls for a combination of remote sensing and in situ measurements to determine aerosol properties and aerosol influences on clouds and radiation. As part of our previous DOE ASP project, we deployed the NASA Langley airborne High Spectralmore » Resolution Lidar (HSRL) on the NASA B200 King Air aircraft during major field experiments in 2006 (MILAGRO and MaxTEX), 2007 (CHAPS), 2009 (RACORO), and 2010 (CalNex and CARES). The HSRL provided measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm). These measurements were typically made in close temporal and spatial coincidence with measurements made from DOE-funded and other participating aircraft and ground sites. On the RACORO, CARES, and CalNEX missions, we also deployed the NASA Goddard Institute for Space Studies (GISS) Research Scanning Polarimeter (RSP). RSP provided intensity and degree of linear polarization over a broad spectral and angular range enabling column-average retrievals of aerosol optical and microphysical properties. Under this project, we analyzed observations and model results from RACORO, CARES, and CalNex and accomplished the following objectives. 1. Identified aerosol types, characterize the vertical distribution of the aerosol types, and partition aerosol optical depth by type, for CARES and CalNex using HSRL data as we have done for previous missions. 2. Investigated aerosol microphysical and macrophysical properties using the RSP. 3. Used the aerosol backscatter and extinction profiles measured by

Urban-scale mapping of PM2.5 distribution via data fusion between high-density sensor network and MODIS Aerosol Optical Depth

NASA Astrophysics Data System (ADS)

Ba, Yu Tao; xian Liu, Bao; Sun, Feng; Wang, Li hua; Tang, Yu jia; Zhang, Da wei

2017-04-01

High-resolution mapping of PM2.5 is the prerequisite for precise analytics and subsequent anti-pollution interventions. Considering the large variances of particulate distribution, urban-scale mapping is challenging either with ground-based fixed stations, with satellites or via models. In this study, a dynamic fusion method between high-density sensor network and MODIS Aerosol Optical Depth (AOD) was introduced. The sensor network was deployed in Beijing ( > 1000 fixed monitors across 16000 km2 area) to provide raw observations with high temporal resolution (sampling interval < 1 hour), high spatial resolution in flat areas ( < 1 km), and low spatial resolution in mountainous areas ( > 5 km). The MODIS AOD was calibrated to provide distribution map with low temporal resolution (daily) and moderate spatial resolution ( = 3 km). By encoding the data quality and defects (e.g. could, reflectance, abnormal), a hybrid interpolation procedure with cross-validation generated PM2.5 distribution with both high temporal and spatial resolution. Several no-pollutant and high-pollution periods were tested to validate the proposed fusion method for capturing the instantaneous patterns of PM2.5 emission.

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

NASA Astrophysics Data System (ADS)

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

2017-08-01

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

Validation and understanding of Moderate Resolution Imaging Spectroradiometer aerosol products (C5) using ground-based measurements from the handheld Sun photometer network in China

Treesearch

Zhanqing Li; Feng Niu; Kwon-Ho Lee; Jinyuan Xin; Wei Min Hao; Bryce L. Nordgren; Yuesi Wang; Pucai Wang

2007-01-01

The Moderate Resolution Imaging Spectroradiometer (MODIS) currently provides the most extensive aerosol retrievals on a global basis, but validation is limited to a small number of ground stations. This study presents a comprehensive evaluation of Collection 4 and 5 MODIS aerosol products using ground measurements from the Chinese Sun Hazemeter Network (CSHNET). The...

Toward Creating A Global Retrospective Climatology of Aerosol Properties

NASA Technical Reports Server (NTRS)

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

2000-01-01

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

Chemical properties and morphology of Marine Aerosol in the Mediterranean atmosphere: a mesocosm study

NASA Astrophysics Data System (ADS)

D'Anna, Barbara; Sellegri, Karine; Charrière, Bruno; Sempéré, Richard; Mas, Sébastien; Marchand, Nicolas; George, Christian; Même, Aurèlie; R'mili, Badr; Delmont, Anne; Schwier, Allison; Rose, Clémence; Colomb, Aurèlie; Pey, Jorge; Langley Dewitt, Helen

2014-05-01

The Mediterranean Sea is a special marine environment characterized by low biological activity and high anthropogenic pressure. It is often difficult to discriminate the contribution of Primary Sea Salt Aerosol formed at the sea surface from background level of the aerosol. An alternative tool to study the sea-air exchanges in a controlled environment is provided by the mesocosms, which represent an important link between field studies and laboratory experiments. The sea-air transfer of particles and gases was investigated in relation to water chemical composition and biological activity during a mesocosm experiment within the SAM project (Sources of marine Aerosol in the Mediterranean) at the Oceanographic and Marine Station STARESO in Western Corsica (May 2013). Three 2 m mesocosms were filled with screened (<1000 µm) 2260 L of subsurface (1 m) seawater and covered with a transparent Teflon film dome to minimize atmospheric contamination. The mesocosms were equipped with a pack of optical and physicochemical sensors and received different treatments: one was left unchanged as control and two were enriched by addition of nitrates and phosphates respecting Redfield ratio (N:P = 16). The evolution of the three systems was followed for 20 days. The set of sensors in each mesocosm was allowed to monitor, at high frequency (every 10 min), the water temperature, conductivity, pH, incident light, fluorescence of chlorophyll a and dissolved oxygen concentration. The mesocosm seawaters were daily sampled for chemical (colored dissolved organic matter, particulate matter and related polar compounds, transparent polysaccharides and nutrients concentration) and biological (chlorophyll a, virus, phytoplankton and zooplankton) analyses. Both dissolved and gaseous VOCs were also analyzed. In addition, few liters of seawater from each mesocosm were daily and immediately collected and transferred to a bubble-bursting apparatus to simulate nascent sea spray aerosol. On

High-resolution sulfur isotopes in ice cores identify large stratospheric volcanic eruptions

NASA Astrophysics Data System (ADS)

Burke, Andrea; Sigl, Michael; Adkins, Jess; Paris, Guillaume; McConnell, Joe

2016-04-01

The record of the volcanic forcing of climate over the past 2500 years is reconstructed primarily from sulfate concentrations in ice cores. Of particular interest are stratospheric eruptions, as these afford sulfate aerosols the longest residence time and largest dispersion in the atmosphere, and thus the greatest impact on radiative forcing. Identification of stratospheric eruptions currently relies on the successful matching of the same volcanic sulphate peak in ice cores from both the Northern and Southern hemispheres (a "bipolar event"). These are interpreted to reflect the global distribution of sulfur aerosols by the stratospheric winds. Despite its recent success, this method relies on precise and accurate dating of ice cores, in order to distinguish between a true 'bipolar event' and two separate eruptions that occurred in close temporal succession. Sulfur isotopes can been used to distinguish between these two scenarios since stratospheric sulfur aerosols are exposed to UV radiation which imparts a mass independent fractionation (Baroni et al., 2007). Mass independent fractionation of sulfate in ice cores thus offers a novel method of fingerprinting stratospheric eruptions, and thus refining the historic record of explosive volcanism and its forcing of climate. Here we present new high-resolution (sub-annual) sulfur isotope data from the Tunu Ice core in Greenland over seven eruptions. Sulfur isotopes were measured by MC-ICP-MS, which substantially reduces sample size requirements and allows high temporal resolution from a single ice core. We demonstrate the efficacy of the method on recent, well-known eruptions (including Pinatubo and Katmai/Novarupta), and then apply it to unidentified sulfate peaks, allowing us to identify new stratospheric eruptions. Baroni, M., Thiemens, M. H., Delmas, R. J., & Savarino, J. (2007). Mass-independent sulfur isotopic compositions in stratospheric volcanic eruptions. Science, 315(5808), 84-87. http://doi.org/10

Evolution of aerosol downwind of a major highway

NASA Astrophysics Data System (ADS)

Liggio, J.; Staebler, R. M.; Brook, J.; Li, S.; Vlasenko, A. L.; Sjostedt, S. J.; Gordon, M.; Makar, P.; Mihele, C.; Evans, G. J.; Jeong, C.; Wentzell, J. J.; Lu, G.; Lee, P.

2010-12-01

Primary aerosol from traffic emissions can have a considerable impact local and regional scale air quality. In order to assess the effect of these emissions and of future emissions scenarios, air quality models are required which utilize emissions representative of real world conditions. Often, the emissions processing systems which provide emissions input for the air quality models rely on laboratory testing of individual vehicles under non-ambient conditions. However, on the sub-grid scale particle evolution may lead to changes in the primary emitted size distribution and gas-particle partitioning that are not properly considered when the emissions are ‘instantly mixed’ within the grid volume. The affect of this modeling convention on model results is not well understood. In particular, changes in organic gas/particle partitioning may result in particle evaporation or condensation onto pre-existing aerosol. The result is a change in the particle distribution and/or an increase in the organic mass available for subsequent gas-phase oxidation. These effects may be missing from air-quality models, and a careful analysis of field data is necessary to quantify their impact. A study of the sub-grid evolution of aerosols (FEVER; Fast Evolution of Vehicle Emissions from Roadways) was conducted in the Toronto area in the summer of 2010. The study included mobile measurements of particle size distributions with a Fast mobility particle sizer (FMPS), aerosol composition with an Aerodyne aerosol mass spectrometer (AMS), black carbon (SP2, PA, LII), VOCs (PTR-MS) and other trace gases. The mobile laboratory was used to measure the concentration gradient of the emissions at perpendicular distances from the highway as well as the physical and chemical evolution of the aerosol. Stationary sites at perpendicular distances and upwind from the highway also monitored the particle size distribution. In addition, sonic anemometers mounted on the mobile lab provided measurements of

Advances in atmospheric temperature profile measurements using high spectral resolution lidar

NASA Astrophysics Data System (ADS)

Razenkov, Ilya I.; Eloranta, Edwin W.

2018-04-01

This paper reports the atmospheric temperature profile measurements using a University of Wisconsin-Madison High Spectral Resolution Lidar (HSRL) and describes improvements in the instrument performance. HSRL discriminates between Mie and Rayleigh backscattering [1]. Thermal motion of molecules broadens the spectrum of the transmitted laser light due to Doppler effect. The HSRL exploits this property to allow the absolute calibration of the lidar and measurements of the aerosol volume backscatter coefficient. Two iodine absorption filters with different line widths are used to resolve temperature sensitive changes in Rayleigh backscattering for atmospheric temperature profile measurements.

Airborne testing and demonstration of a new flight system based on an Aerodyne N2O-CO2-CO-H2O mini-spectrometer

NASA Astrophysics Data System (ADS)

Gvakharia, A.; Kort, E. A.; Smith, M. L.; Conley, S.

2017-12-01

Nitrous oxide (N2O) is a powerful greenhouse gas and ozone depleting substance. With high atmospheric backgrounds and small relative signals, N2O emissions have been challenging to observe and understand on regional scales with traditional instrumentation. Fast-response airborne measurements with high precision and accuracy can potentially bridge this observational gap. Here we present flight assessments of a new flight system based on an Aerodyne mini-spectrometer as well as a Los Gatos N2O/CO analyzer during the Fertilizer Emissions Airborne Study (FEAST). With the Scientific Aviation Mooney aircraft, we conducted test flights for both analyzers where a known calibration gas was sampled throughout the flight (`null' tests). Clear altitude/cabin-pressure dependencies were observed for both analyzers if operated in an "off-the-shelf' manner. For the remainder of test flights and the FEAST campaign we used a new flight system based on an Aerodyne mini-spectrometer with the addition of a custom pressure control/calibration system. Instead of using traditional approaches with spectral-zeros and infrequent in-flight calibrations, we employ a high-flow system with stable flow control to enable high frequency (2 minutes), short duration (15 seconds) sampling of a known calibration gas. This approach, supported by the null test, enables correction for spectral drift caused by a variety of factors while maintaining a 90% duty cycle for 1Hz sampling from an aircraft. Preliminary in-flight precisions are estimated at 0.05 ppb, 0.1 ppm, 1 ppb, and 10 ppm for N2O, CO2, CO, and H2O respectively. We also present a further 40 hours of inter-comparison in flight with a Picarro 2301-f ring-down spectrometer demonstrating consistency between CO2 and H2O measurements and no altitude dependent error.

High Spectral Resolution LIDAR as a Tool for Air Quality Research

NASA Astrophysics Data System (ADS)

Eloranta, E. W.; Spuler, S.; Hayman, M. M.

2017-12-01

Many aspects of air quality research require information on the vertical distribution of pollution. Traditional measurements, obtained from surface based samplers, or passive satellite remote sensing, do not provide vertical profiles. Lidar can provide profiles of aerosol properties. However traditional backscatter lidar suffers from uncertain calibrations with poorly constrained algorithms. These problems are avoided using High Spectral Resolution Lidar (HSRL) which provides absolutely calibrated vertical profiles of aerosol properties. The University of Wisconsin HSRL systems measure 532 nm wavelength aerosol backscatter cross-sections, extinction cross-sections, depolarization, and attenuated 1064 nm backscatter. These instruments are designed for long-term deployment at remote sites with minimal local support. Processed data is provided for public viewing and download in real-time on our web site "http://hsrl.ssec.wisc.edu". Air pollution applications of HSRL data will be illustrated with examples acquired during air quality field programs including; KORUS-AQ, DISCOVER-AQ, LAMOS and FRAPPE. Observations include 1) long range transport of dust, air pollution and smoke. 2) Fumigation episodes where elevated pollution is mixed down to the surface. 3) visibility restrictions by aerosols and 4) diurnal variations in atmospheric optical depth. While HSRL is powerful air quality research tool, its application in routine measurement networks is hindered by the high cost of current systems. Recent technical advances promise a next generation HSRL using telcom components to greatly reduce system cost. This paper will present data generated by a prototype low cost system constructed at NCAR. In addition to lower cost, operation at a non-visible near 780 nm infrared wavelength removes all FAA restrictions on the operation.

Spatiotemporal variability and contribution of different aerosol types to the Aerosol Optical Depth over the Eastern Mediterranean.

PubMed

Georgoulias, Aristeidis K; Alexandri, Georgia; Kourtidis, Konstantinos A; Lelieveld, Jos; Zanis, Prodromos; Pöschl, Ulrich; Levy, Robert; Amiridis, Vassilis; Marinou, Eleni; Tsikerdekis, Athanasios

2016-01-01

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the Aerosol Optical Depth (AOD) over the Eastern Mediterranean as derived from MODIS Terra (3/2000-12/2012) and Aqua (7/2002-12/2012) satellite instruments. For this purpose, a 0.1° × 0.1° gridded MODIS dataset was compiled and validated against sunphotometric observations from the AErosol RObotic NETwork (AERONET). The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium sized cities, industrial zones, and power plant complexes, seasonal variabilities, and decadal averages. The average AOD at 550 nm (AOD 550 ) for the entire region is ~ 0.22 ± 0.19 with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in Central and Eastern Europe, and transport of dust from the Sahara Desert and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry-aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD 550 . The spatial and temporal variability of anthropogenic, dust and fine mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD 550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine mode natural aerosols account for ~ 51 %, ~ 34 % and ~ 15 % of the total AOD 550 over land, while, anthropogenic aerosols, dust and marine aerosols account ~ 40 %, ~ 34 % and ~ 26 % of the total AOD 550 over the sea, based on MODIS Terra and Aqua observations.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

NASA Astrophysics Data System (ADS)

Forestieri, Sara D.; Cornwell, Gavin C.; Helgestad, Taylor M.; Moore, Kathryn A.; Lee, Christopher; Novak, Gordon A.; Sultana, Camille M.; Wang, Xiaofei; Bertram, Timothy H.; Prather, Kimberly A.; Cappa, Christopher D.

2016-07-01

The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 %) measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer) and single particle (using an aerosol time-of-flight mass spectrometer) measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 %) values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 %) depression and the peak chlorophyll a (Chl a) concentrations by either 1 (indoor MART) or 3-to-6 (outdoor MART) days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA. The GF(85 %) values exhibited a reasonable negative

Global Aerosol Remote Sensing from MODIS

NASA Technical Reports Server (NTRS)

Ichoku, Charles; Kaufman, Yoram J.; Remer, Lorraine A.; Chu, D. Allen; Mattoo, Shana; Tanre, Didier; Levy, Robert; Li, Rong-Rong; Martins, Jose V.; Lau, William K. M. (Technical Monitor)

2002-01-01

The physical characteristics, composition, abundance, spatial distribution and dynamics of global aerosols are still very poorly known, and new data from satellite sensors have long been awaited to improve current understanding and to give a boost to the effort in future climate predictions. The derivation of aerosol parameters from the MODerate resolution Imaging Spectro-radiometer (MODIS) sensors aboard the Earth Observing System (EOS) Terra and Aqua polar-orbiting satellites ushers in a new era in aerosol remote sensing from space. Terra and Aqua were launched on December 18, 1999 and May 4, 2002 respectively, with daytime equator crossing times of approximately 10:30 am and 1:30 pm respectively. Several aerosol parameters are retrieved at 10-km spatial resolution (level 2) from MODIS daytime data. The MODIS aerosol algorithm employs different approaches to retrieve parameters over land and ocean surfaces, because of the inherent differences in the solar spectral radiance interaction with these surfaces. The parameters retrieved include: aerosol optical thickness (AOT) at 0.47, 0.55 and 0.66 micron wavelengths over land, and at 0.47, 0.55, 0.66, 0.87, 1.2, 1.6, and 2.1 micron over ocean; Angstrom exponent over land and ocean; and effective radii, and the proportion of AOT contributed by the small mode aerosols over ocean. To ensure the quality of these parameters, a substantial part of the Terra-MODIS aerosol products were validated globally and regionally, based on cross correlation with corresponding parameters derived from ground-based measurements from AERONET (AErosol RObotic NETwork) sun photometers. Similar validation efforts are planned for the Aqua-MODIS aerosol products. The MODIS level 2 aerosol products are operationally aggregated to generate global daily, eight-day (weekly), and monthly products at one-degree spatial resolution (level 3). MODIS aerosol data are used for the detailed study of local, regional, and global aerosol concentration

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

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

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai

2016-08-22

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy’s Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surfacemore » measurements during July, and two days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. While a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.« less

Model representations of aerosol layers transported from North America over the Atlantic Ocean during the Two-Column Aerosol Project

DOE PAGES

Fast, Jerome D.; Berg, Larry K.; Zhang, Kai; ...

2016-08-22

The ability of the Weather Research and Forecasting model with chemistry (WRF-Chem) version 3.7 and the Community Atmosphere Model version 5.3 (CAM5) in simulating profiles of aerosol properties is quantified using extensive in situ and remote sensing measurements from the Two-Column Aerosol Project (TCAP) conducted during July of 2012. TCAP was supported by the U.S. Department of Energy's Atmospheric Radiation Measurement program and was designed to obtain observations within two atmospheric columns; one fixed over Cape Cod, Massachusetts, and the other several hundred kilometers over the ocean. The performance is quantified using most of the available aircraft and surface measurementsmore » during July, and 2 days are examined in more detail to identify the processes responsible for the observed aerosol layers. The higher-resolution WRF-Chem model produced more aerosol mass in the free troposphere than the coarser-resolution CAM5 model so that the fraction of aerosol optical thickness above the residual layer from WRF-Chem was more consistent with lidar measurements. We found that the free troposphere layers are likely due to mean vertical motions associated with synoptic-scale convergence that lifts aerosols from the boundary layer. The vertical displacement and the time period associated with upward transport in the troposphere depend on the strength of the synoptic system and whether relatively high boundary layer aerosol concentrations are present where convergence occurs. In conclusion, while a parameterization of subgrid scale convective clouds applied in WRF-Chem modulated the concentrations of aerosols aloft, it did not significantly change the overall altitude and depth of the layers.« less

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

NASA Astrophysics Data System (ADS)

Ulevicius, V.; Byčenkienė, S.; Bozzetti, C.; Vlachou, A.; Plauškaitė, K.; Mordas, G.; Dudoitis, V.; Abbaszade, G.; Remeikis, V.; Garbaras, A.; Masalaite, A.; Blees, J.; Fröhlich, R.; Dällenbach, K. R.; Canonaco, F.; Slowik, J. G.; Dommen, J.; Zimmermann, R.; Schnelle-Kreis, J.; Salazar, G. A.; Agrios, K.; Szidat, S.; El Haddad, I.; Prévôt, A. S. H.

2015-09-01

In early spring the Baltic region is frequently affected by high pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m-3 and black carbon (BC) up to 17 μg m-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26-44 % and 13-23 % to the TC, respectively. 5-8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4-13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13-24 % and 7-12 %, respectively. Isotope ratio of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

NASA Astrophysics Data System (ADS)

Ulevicius, Vidmantas; Byčenkienė, Steigvilė; Bozzetti, Carlo; Vlachou, Athanasia; Plauškaitė, Kristina; Mordas, Genrik; Dudoitis, Vadimas; Abbaszade, Gülcin; Remeikis, Vidmantas; Garbaras, Andrius; Masalaite, Agne; Blees, Jan; Fröhlich, Roman; Dällenbach, Kaspar R.; Canonaco, Francesco; Slowik, Jay G.; Dommen, Josef; Zimmermann, Ralf; Schnelle-Kreis, Jürgen; Salazar, Gary A.; Agrios, Konstantinos; Szidat, Sönke; El Haddad, Imad; Prévôt, André S. H.

2016-05-01

In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m-3 and black carbon (BC) up to 17 µg m-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26-44 % and 13-23 % to the total carbon (TC), respectively. 5-8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4-13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13-24 and 7-13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

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.

Development of Portable Aerosol Mobility Spectrometer for Personal and Mobile Aerosol Measurement

PubMed Central

Kulkarni, Pramod; Qi, Chaolong; Fukushima, Nobuhiko

2017-01-01

We describe development of a Portable Aerosol Mobility Spectrometer (PAMS) for size distribution measurement of submicrometer aerosol. The spectrometer is designed for use in personal or mobile aerosol characterization studies and measures approximately 22.5 × 22.5 × 15 cm and weighs about 4.5 kg including the battery. PAMS uses electrical mobility technique to measure number-weighted particle size distribution of aerosol in the 10–855 nm range. Aerosol particles are electrically charged using a dual-corona bipolar corona charger, followed by classification in a cylindrical miniature differential mobility analyzer. A condensation particle counter is used to detect and count particles. The mobility classifier was operated at an aerosol flow rate of 0.05 L/min, and at two different user-selectable sheath flows of 0.2 L/min (for wider size range 15–855 nm) and 0.4 L/min (for higher size resolution over the size range of 10.6–436 nm). The instrument was operated in voltage stepping mode to retrieve the size distribution, which took approximately 1–2 minutes, depending on the configuration. Sizing accuracy and resolution were probed and found to be within the 25% limit of NIOSH criterion for direct-reading instruments (NIOSH 2012). Comparison of size distribution measurements from PAMS and other commercial mobility spectrometers showed good agreement. The instrument offers unique measurement capability for on-person or mobile size distribution measurements of ultrafine and nanoparticle aerosol. PMID:28413241

Aerosol Airmass Type Mapping Over the Urban Mexico City Region From Space-based Multi-angle Imaging

NASA Technical Reports Server (NTRS)

Patadia, F.; Kahn, R. A.; Limbacher, J. A.; Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.

2013-01-01

Using Multi-angle Imaging SpectroRadiometer (MISR) and sub-orbital measurements from the 2006 INTEX-B/MILAGRO field campaign, in this study we explore MISR's ability to map different aerosol air mass types over the Mexico City metropolitan area. The aerosol air mass distinctions are based on shape, size and single scattering albedo retrievals from the MISR Research Aerosol Retrieval algorithm. In this region, the research algorithm identifies dust-dominated aerosol mixtures based on non-spherical particle shape, whereas spherical biomass burning and urban pollution particles are distinguished by particle size. Two distinct aerosol air mass types based on retrieved particle microphysical properties, and four spatially distributed aerosol air masses, are identified in the MISR data on 6 March 2006. The aerosol air mass type identification results are supported by coincident, airborne high-spectral-resolution lidar (HSRL) measurements. Aerosol optical depth (AOD) gradients are also consistent between the MISR and sub-orbital measurements, but particles having single-scattering albedo of approx. 0.7 at 558 nm must be included in the retrieval algorithm to produce good absolute AOD comparisons over pollution-dominated aerosol air masses. The MISR standard V22 AOD product, at 17.6 km resolution, captures the observed AOD gradients qualitatively, but retrievals at this coarse spatial scale and with limited spherical absorbing particle options underestimate AOD and do not retrieve particle properties adequately over this complex urban region. However, we demonstrate how AOD and aerosol type mapping can be accomplished with MISR data over complex urban regions, provided the retrieval is performed at sufficiently high spatial resolution, and with a rich enough set of aerosol components and mixtures.

Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: Inter- and intra-species variability for six coniferous species

DOE PAGES

Faiola, C. L.; Wen, M.; VanReken, T. M.

2015-04-01

The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- andmore » post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH 3O +), m/z 58 (C 2H 2O 2 +, C 3H 6O +), m/z 29 (C 2H 5 +), m/z 57 (C 3H 5O +), m/z 59 (C 2H 3O 2 +, C 3H 7O +), m/z 71 (C 3H 3O 2 +, C 4H 7O +), and m/z 83 (C 5H 7O +). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Furthermore the results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.« less

Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

NASA Astrophysics Data System (ADS)

Faiola, C. L.; Wen, M.; VanReken, T. M.

2015-04-01

The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- and post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.

An Airborne A-Band Spectrometer for Remote Sensing Of Aerosol and Cloud Optical Properties

NASA Technical Reports Server (NTRS)

Pitts, Michael; Hostetler, Chris; Poole, Lamont; Holden, Carl; Rault, Didier

2000-01-01

Atmospheric remote sensing with the O2 A-band has a relatively long history, but most of these studies were attempting to estimate surface pressure or cloud-top pressure. Recent conceptual studies have demonstrated the potential of spaceborne high spectral resolution O2 A-band spectrometers for retrieval of aerosol and cloud optical properties. The physical rationale of this new approach is that information on the scattering properties of the atmosphere is embedded in the detailed line structure of the O2 A-band reflected radiance spectrum. The key to extracting this information is to measure the radiance spectrum at very high spectral resolution. Instrument performance requirement studies indicate that, in addition to high spectral resolution, the successful retrieval of aerosol and cloud properties from A-band radiance spectra will also require high radiometric accuracy, instrument stability, and high signal-to-noise measurements. To experimentally assess the capabilities of this promising new remote sensing application, the NASA Langley Research Center is developing an airborne high spectral resolution A-band spectrometer. The spectrometer uses a plane holographic grating with a folded Littrow geometry to achieve high spectral resolution (0.5 cm-1) and low stray light in a compact package. This instrument will be flown in a series of field campaigns beginning in 2001 to evaluate the overall feasibility of this new technique. Results from these campaigns should be particularly valuable for future spaceborne applications of A-band spectrometers for aerosol and cloud retrievals.

Enviro-HIRLAM/ HARMONIE Studies in ECMWF HPC EnviroAerosols Project

NASA Astrophysics Data System (ADS)

Hansen Sass, Bent; Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander; Palamarchuk, Julia; Ivanov, Serguei; Pagh Nielsen, Kristian; Penenko, Alexey; Edvardsson, Nellie; Stysiak, Aleksander Andrzej; Bostanbekov, Kairat; Amstrup, Bjarne; Yang, Xiaohua; Ruban, Igor; Bergen Jensen, Marina; Penenko, Vladimir; Nurseitov, Daniyar; Zakarin, Edige

2017-04-01

The EnviroAerosols on ECMWF HPC project (2015-2017) "Enviro-HIRLAM/ HARMONIE model research and development for online integrated meteorology-chemistry-aerosols feedbacks and interactions in weather and atmospheric composition forecasting" is aimed at analysis of importance of the meteorology-chemistry/aerosols interactions and to provide a way for development of efficient techniques for on-line coupling of numerical weather prediction and atmospheric chemical transport via process-oriented parameterizations and feedback algorithms, which will improve both the numerical weather prediction and atmospheric composition forecasts. Two main application areas of the on-line integrated modelling are considered: (i) improved numerical weather prediction with short-term feedbacks of aerosols and chemistry on formation and development of meteorological variables, and (ii) improved atmospheric composition forecasting with on-line integrated meteorological forecast and two-way feedbacks between aerosols/chemistry and meteorology. During 2015-2016 several research projects were realized. At first, the study on "On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies" focused on assessment of scenarios with accidental and continuous emissions of sulphur dioxide for case studies for Atyrau (Kazakhstan) near the northern part of the Caspian Sea and metallurgical enterprises on the Kola Peninsula (Russia), with GIS integration of modelling results into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system. At second, the studies on "The sensitivity of precipitation simulations to the soot aerosol presence" & "The precipitation forecast sensitivity to data assimilation on a very high resolution domain" focused on sensitivity and changes in precipitation life-cycle under black carbon polluted conditions over Scandinavia. At third, studies on "Aerosol effects over China investigated with a high resolution

Observed secondary organic aerosol (SOA) and organic nitrate yields from NO3 oxidation of isoprene

NASA Astrophysics Data System (ADS)

Rollins, A. W.; Fry, J. L.; Kiendler-Scharr, A.; Wooldridge, P. J.; Brown, S. S.; Fuchs, H.; Dube, W.; Mensah, A.; Tillmann, R.; Dorn, H.; Brauers, T.; Cohen, R. C.

2008-12-01

Formation of organic nitrates and secondary organic aerosol (SOA) from the NO3 oxidation of isoprene has been studied at atmospheric concentrations of VOC (10 ppb) and oxidant (<100 ppt NO3) in the presence of ammonium sulfate seed aerosol in the atmosphere simulation chamber SAPHIR at Forschungszentrum Jülich. Cavity Ringdown (CaRDS) and thermal dissociation - CaRDS measurements of NO3 and N2O5 as well as Thermal Dissociation - Laser Induced Fluorescence (TD-LIF) detection of alkyl nitrates (RONO2) and Aerodyne Aerosol Mass Spectrometer (AMS) measurements of aerosol composition were all used in comparison to a Master Chemical Mechanism (MCM) based chemical kinetics box model to quantify the product yields from two stages in isoprene oxidation. We find significant yields of organic nitrate formation from both the initial isoprene + NO3 reaction (71%) as well as from the reaction of NO3 with the initial oxidation products (30% - 60%). Under these low concentration conditions (~1 μg / m3), measured SOA production was greater than instrument noise only for the second oxidation step. Based on the modeled chemistry, we estimate an SOA mass yield of 10% (relative to isoprene mass reacted) for the reaction of the initial oxidation products with NO3. This yield is found to be consistent with the estimated saturation concentration (C*) of the presumed gas products of the doubly oxidized isoprene, where both oxidations lead to the addition of nitrate, carbonyl, and hydroxyl groups.

Fine Particulate Matter Predictions Using High Resolution Aerosol Optical Depth (AOD) Retrievals

NASA Technical Reports Server (NTRS)

Chudnovsky, Alexandra A.; Koutrakis, Petros; Kloog, Itai; Melly, Steven; Nordio, Francesco; Lyapustin, Alexei; Wang, Jujie; Schwartz, Joel

2014-01-01

To date, spatial-temporal patterns of particulate matter (PM) within urban areas have primarily been examined using models. On the other hand, satellites extend spatial coverage but their spatial resolution is too coarse. In order to address this issue, here we report on spatial variability in PM levels derived from high 1 km resolution AOD product of Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm developed for MODIS satellite. We apply day-specific calibrations of AOD data to predict PM(sub 2.5) concentrations within the New England area of the United States. To improve the accuracy of our model, land use and meteorological variables were incorporated. We used inverse probability weighting (IPW) to account for nonrandom missingness of AOD and nested regions within days to capture spatial variation. With this approach we can control for the inherent day-to-day variability in the AOD-PM(sub 2.5) relationship, which depends on time-varying parameters such as particle optical properties, vertical and diurnal concentration profiles and ground surface reflectance among others. Out-of-sample "ten-fold" cross-validation was used to quantify the accuracy of model predictions. Our results show that the model-predicted PM(sub 2.5) mass concentrations are highly correlated with the actual observations, with out-of- sample R(sub 2) of 0.89. Furthermore, our study shows that the model captures the pollution levels along highways and many urban locations thereby extending our ability to investigate the spatial patterns of urban air quality, such as examining exposures in areas with high traffic. Our results also show high accuracy within the cities of Boston and New Haven thereby indicating that MAIAC data can be used to examine intra-urban exposure contrasts in PM(sub 2.5) levels.

Carbonaceous aerosols in the Western Mediterranean during summertime and their contribution to the aerosol optical properties at ground level: First results of the ChArMEx-ADRIMED 2013 intensive campaign in Corsica

NASA Astrophysics Data System (ADS)

Sciare, Jean; Dulac, Francois; Feron, Anais; Crenn, Vincent; Sarda Esteve, Roland; Baisnee, Dominique; Bonnaire, Nicolas; Hamonou, Eric; Mallet, Marc; Lambert, Dominique; Nicolas, Jose B.; Bourrianne, Thierry; Petit, Jean-Eudes; Favez, Olivier; Canonaco, Francesco; Prevot, Andre; Mocnik, Grisa; Drinovec, Luka; Marpillat, Alexandre; Serrie, Wilfrid

2014-05-01

As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx, http://charmex.lsce.ipsl.fr/), the CORSiCA (http://www.obs-mip.fr/corsica) and the ANR-ADRIMED programs, a large set of real-time measurements of carbonaceous aerosols was deployed in June 2013 at the Cape Corsica atmospheric supersite (http://gaw.empa.ch/gawsis/reports.asp?StationID=2076203042). Submicron organic aerosols (OA) were monitored every 30 min using an Aerosol Chemical Speciation Monitor (ACSM; Aerodyne Res. Inc. MA, USA); Fine (PM2.5) Organic Carbon (OC) and Elemental Carbon (EC) were measured every 2h using an OCEC Sunset Field Instrument (Sunset Lab, OR, USA) and every 12h using a low-vol (Leckel) filter sampler running at 2.3m3/h. Equivalent Black Carbon (BC) was monitored using two Aethalometers (models AE31 and AE33, Magee Scientific, US & Aerosol d.o.o., Slovenia) and a MAAP instrument (Thermo). Quality control of this large dataset was performed through chemical mass closure studies (using co-located SMPS and TEOM-FDMS) and direct comparisons with other real-time instruments running in parallel (Particle-Into-Liquid-Sampler-Ion-Chromatograph for ions, filter sampling, ...). Source apportionment of OA was then performed using the SourceFinder software (SoFi v4.5, http://www.psi.ch/acsm-stations/me-2) allowing the distinction between hydrogen- and oxygen-like organic aerosols (HOA and OOA, respectively) and highlighting the major contribution of secondary OA in the Western Mediterranean during summer. Using this time-resolved chemical information, reconstruction of the optical aerosol properties were performed and compared with integrating nephelometer (Model 3563, TSI, US) and photoacoustic extinctiometer (PAX, DMT, US) measurements performed in parallel. Results of these different closure studies (chemical/physical/optical) are presented and discussed here in details. They highlight the central role of carbonaceous aerosols on the optical properties of aerosols at ground level

HSRL-2 Observations of Aerosol Variability During an Aerosol Build-up Event in Houston and Comparisons With WRF-Chem

NASA Technical Reports Server (NTRS)

Burton, Sharon P.; Saide, Pablo; Sawamura, Patricia; Hostetler, Chris; Ferrare, Rich; Scarino, Amy Jo; Berkoff, Tim; Harper, David; Cook, Tony; Rogers, Ray;

High-Resolution Modeling of the Predictability of Convective Systems, and Influences by Absorbing Aerosols Over Northern India and the Himalayas Foothills During Boreal Summer

NASA Technical Reports Server (NTRS)

Kim, Kyu-Myong; Lau, William K.-M.; Tao, Wei-Kuo; Shi, Jainn; Tan, Qian; Chin, Mian; Matsui, Toshihisa; Bian, Huisheng

2011-01-01

The Himalayas foothills region (HFR) is an important component of the South Asian monsoon. To the south, the HFR borders the fertile, populous, and heavily polluted Indo-Gangetic Plain (IGP). To the north, it rises to great height (approx. 4-5 km) to the Tibetan Plateau over a distance of less than 100 km. The HFR itself consists of complex mountainous terrain, with strong orographic forcing for precipitation. During the late spring and early summer, dust aerosol from the Thar and Middle East deserts , as well as moisture from the Arabian Sea were transported to the western part of the western part of the IGP and foothills spurs pre-monsoon severe thunderstorm over the region. During the monsoon season (mid June -August) convection from the Bay of Bengal, spread along the foothills northwestward to northern Pakistan. Recent climate model studies and preliminary observations have indicted not only the importance of dynamical forcing of precipitation in the HFR, but also possible strong impacts by the dense aerosols, from both local sources, and remote transport, that blanket the IGP from late spring up to the onset of the monsoon in June, and during monsoon breaks in July. In this work, we use the NASA Unified Weather Research and Forecasting (Nu-WRF) model to study the predictability ( 1-7 days) South Asian monsoon rainfall system. Results of 7 -day forecast experiments using an embedded domain of 27 km and 9 km resolution were conducted for the period June 11- July 15, 2008, with and without aerosol forcing are carried out to assess the intrinsic predictability of rainfall over the HFR, and possible impacts by aerosol direct effect, and possible connection of large-scale South Asian monsoon system.

Characterization of biomass burning aerosols produced in the laboratory with a light-scattering aerosol mass spectrometer

NASA Astrophysics Data System (ADS)

Middlebrook, A. M.; Adler, G. A.; Coggon, M.; De Gouw, J. A.; Franchin, A.; Gilman, J.; Koss, A.; Krechmer, J. E.; Lamb, K.; Manfred, K.; Roberts, J. M.; Schwarz, J. P.; Sekimoto, K.; Selimovic, V.; Stockwell, C.; Wagner, N.; Warneke, C.; Washenfelder, R. A.; Womack, C.; Yokelson, R. J.; Yuan, B.

2017-12-01

During the 2016 NOAA FIREX project at the Missoula Fire Sciences Laboratory, small fires of known fuel type and properties were ignited to characterize their direct emissions with a large variety of new sampling methods. Two types of experiments were employed: sampling smoke directly from the exhaust stack throughout the lifecycle of the fires (stack burns) or sampling when the exhaust vent was closed to fill the room with smoke (room burns). For both types of burns, photo-oxidation chambers were at times used to mimic aging in the atmosphere. During all these experiments, we measured the non-refractory components of the smoke particles using an Aerodyne compact time-of-flight aerosol mass spectrometer (AMS) with a light scattering module and diluted the sample line as little as possible (usually by a factor of 10) without overwhelming our instrument. For the stack burns, our AMS was placed near the top of the exhaust stack to capture the composition and size distribution during the rapidly changing stages of the fires. We found that the chemical composition of the aerosols varied with fuel type and combustion conditions on time scales of a few minutes as the fuels went through different stages of heating and combustion. For the room burns, we obtained additional measurements with the light-scattering module aimed at understanding how well smoke particles are measured with the AMS, along with characterization of their physical properties. We will present a summary of our results, with connections to their relevance for constraining model treatments of fire emissions on the atmosphere.

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

NASA Astrophysics Data System (ADS)

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

2010-12-01

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

A new processing scheme for ultra-high resolution direct infusion mass spectrometry data

NASA Astrophysics Data System (ADS)

Zielinski, Arthur T.; Kourtchev, Ivan; Bortolini, Claudio; Fuller, Stephen J.; Giorio, Chiara; Popoola, Olalekan A. M.; Bogialli, Sara; Tapparo, Andrea; Jones, Roderic L.; Kalberer, Markus

2018-04-01

High resolution, high accuracy mass spectrometry is widely used to characterise environmental or biological samples with highly complex composition enabling the identification of chemical composition of often unknown compounds. Despite instrumental advancements, the accurate molecular assignment of compounds acquired in high resolution mass spectra remains time consuming and requires automated algorithms, especially for samples covering a wide mass range and large numbers of compounds. A new processing scheme is introduced implementing filtering methods based on element assignment, instrumental error, and blank subtraction. Optional post-processing incorporates common ion selection across replicate measurements and shoulder ion removal. The scheme allows both positive and negative direct infusion electrospray ionisation (ESI) and atmospheric pressure photoionisation (APPI) acquisition with the same programs. An example application to atmospheric organic aerosol samples using an Orbitrap mass spectrometer is reported for both ionisation techniques resulting in final spectra with 0.8% and 8.4% of the peaks retained from the raw spectra for APPI positive and ESI negative acquisition, respectively.

Gas- and particle-phase chemical composition measurements onboard the G-1 research aircraft during the GoAmazon campaign.

NASA Astrophysics Data System (ADS)

Shilling, J.; Pekour, M. S.; Fortner, E.; Hubbe, J. M.; Longo, K.; Martin, S. T.; Mei, F.; Springston, S. R.; Tomlinson, J. M.; Wang, J.

2014-12-01

The Green Ocean Amazon (GoAmazon) campaign conducted from January 2014 - December 2015 in the vicinity of Manaus, Brazil, was designed to study the aerosol lifecycle and aerosol-cloud interactions in both pristine and anthropogenically influenced conditions. As part of this campaign, the DOE G-1 research aircraft was deployed from February 17th - March 25th 2014 and September 6th - October 5th 2014 to investigate aerosol and cloud properties aloft. An Aerodyne High Resolution Aerosol Mass Spectrometer (AMS) and an Ionicon Proton Transfer Reaction Mass Spectrometer (PTRMS) were part of the G-1 research aircraft payload and were used to investigate aerosol gas- and particle-phase chemical composition. Here we present preliminary analysis of the aerosol and gas phase chemical composition. PTR-MS measurements show that isoprene and its oxidation products are the dominant VOCs during research flights. HR-AMS measurements reveal that the particle phase is dominated by organic material with smaller concentrations of sulfate and nitrate observed. Organic particle concentrations are enhanced when encountering the urban plume from Manaus. During the wet season, we observe increased concentrations of organic particle when passing through low-altitude clouds. PMF analysis of the organic mass spectra shows that the chemical composition of the particles observed in-cloud is distinctly different from particles observed outside clouds. We will also compare measurements made during the wet and dry seasons.

A continuous plutonium aerosol monitor for use in high radon environments.

PubMed

Li, HuiBin; Jia, MingYan; Li, GuoShen; Wang, YinDong

2012-01-01

Radon concentration is very high in underground basements and other facilities. Radon concentration in a nuclear facility locates in the granite tunnel can be as high as 10(4) Bq m(-3) in summer. Monitoring plutonium aerosol in this circumstance is seriously interfered by radon daughters. In order to solve this problem, a new continuous aerosol monitor that can monitor very low plutonium aerosol concentration in high radon background was developed. Several techniques were used to reduce interference of radon daughters, and the minimum detectable concentrations in various radon concentrations were measured.

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

Direct Observations of Isoprene Secondary Organic Aerosol Formation in Ambient Cloud Droplets

NASA Astrophysics Data System (ADS)

Zelenyuk, A.; Bell, D.; Thornton, J. A.; Fast, J. D.; Shrivastava, M. B.; Berg, L. K.; Imre, D. G.; Mei, F.; Shilling, J.; Suski, K. J.; Liu, J.; Tomlinson, J. M.; Wang, J.

2017-12-01

Multiphase chemistry of isoprene photooxidation products has been shown to be one of the major sources of secondary organic aerosol (SOA) in the atmosphere. A number of recent studies indicate that aqueous aerosol phase provides a medium for reactive uptake of isoprene photooxidation products, and in particular, isomeric isoprene epoxydiols (IEPOX), with reaction rates and yields being dependent on aerosol acidity, water content, sulfate concentration, and organic coatings. However, very few studies focused on chemistry occurring within actual cloud droplets. We will present data acquired during recent Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign, which provide direct evidence for IEPOX-SOA formation in cloud droplets. Single particle mass spectrometer, miniSPLAT, and a high-resolution, time-of-flight aerosol mass spectrometer were used to characterize the composition of aerosol particles and cloud droplet residuals, while a high-resolution, time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) was used to characterize gas-phase compounds. We find that the composition of cloud droplet residuals was markedly different than that of aerosol particles sampled outside the cloud. Cloud droplet residuals were comprised of individual particles with high relative fractions of sulfate and nitrate and significant fraction of particles with mass spectra that are nearly identical to those of laboratory-generated IEPOX-SOA particles. The observed cloud-induced formation of IEPOX-SOA was accompanied by simultaneous decrease in measured concentrations of IEPOX and other gas-phase isoprene photooxidation products. Ultimately, the combined cloud, aerosol, and gas-phase measurements conducted during HI-SCALE will be used to develop and evaluate model treatments of aqueous-phase isoprene SOA formation.

Linking Remotely Sensed Aerosol Types to Their Chemical Composition

NASA Technical Reports Server (NTRS)

Dawson, Kyle William; Kacenelenbogen, Meloe S.; Johnson, Matthew S.; Burton, Sharon P.; Hostetler, Chris A.; Meskhidze, Nicholas

2016-01-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% +/- 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into 'dark' and 'light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

Linking remotely sensed aerosol types to their chemical composition

NASA Astrophysics Data System (ADS)

Dawson, K. W.; Kacenelenbogen, M. S.; Johnson, M. S.; Burton, S. P.; Hostetler, C. A.; Meskhidze, N.

2016-12-01

Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% ± 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into `dark' and `light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Reallocation in modal aerosol models: impacts on predicting aerosol radiative effects

NASA Astrophysics Data System (ADS)

Korhola, T.; Kokkola, H.; Korhonen, H.; Partanen, A.-I.; Laaksonen, A.; Lehtinen, K. E. J.; Romakkaniemi, S.

2013-08-01

In atmospheric modelling applications the aerosol particle size distribution is commonly represented by modal approach, in which particles in different size ranges are described with log-normal modes within predetermined size ranges. Such method includes numerical reallocation of particles from a mode to another for example during particle growth, leading to potentially artificial changes in the aerosol size distribution. In this study we analysed how this reallocation affects climatologically relevant parameters: cloud droplet number concentration, aerosol-cloud interaction coefficient and light extinction coefficient. We compared these parameters between a modal model with and without reallocation routines, and a high resolution sectional model that was considered as a reference model. We analysed the relative differences of the parameters in different experiments that were designed to cover a wide range of dynamic aerosol processes occurring in the atmosphere. According to our results, limiting the allowed size ranges of the modes and the following numerical remapping of the distribution by reallocation, leads on average to underestimation of cloud droplet number concentration (up to 100%) and overestimation of light extinction (up to 20%). The analysis of aerosol first indirect effect is more complicated as the ACI parameter can be either over- or underestimated by the reallocating model, depending on the conditions. However, for example in the case of atmospheric new particle formation events followed by rapid particle growth, the reallocation can cause around average 10% overestimation of the ACI parameter. Thus it is shown that the reallocation affects the ability of a model to estimate aerosol climate effects accurately, and this should be taken into account when using and developing aerosol models.

Field test of a new instrument to measure UV/Vis (300-700 nm) ambient aerosol extinction spectra in Colorado during DISCOVER-AQ

NASA Astrophysics Data System (ADS)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Dibb, J. E.; Greenslade, M. E.; Martin, R.; Scheuer, E. M.; Shook, M.; Thornhill, K. L., II; Troop, D.; Winstead, E.; Ziemba, L. D.

2014-12-01

An optical instrument has been developed to investigate aerosol extinction spectra in the ambient atmosphere. Based on a White-type cell design and using a differential optical approach, aerosol extinction spectra over the 300-700 nm ultraviolet and visible (UV/Vis) wavelength range are obtained. Laboratory tests conducted at NASA Langley Research Center (NASA LaRC) in March 2014 showed good agreement with Cavity Attenuated Phase Shift (CAPS PMex, Aerodyne Research) extinction measurements (at 450, 530, and 630 nm) for a variety of aerosols, e.g., scatterers such as polystyrene latex spheres and ammonium sulfate; absorbers such as dust (including pigmented minerals), smoke (generated in a miniCAST burning propane) and laboratory smoke analogs (e.g., fullerene soot and aquadag). The instrument was field tested in Colorado in July and August 2014 aboard the NASA mobile laboratory at various ground sites during the DISCOVER-AQ (Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality) field campaign. A description of the instrument, results from the laboratory tests, and summer field data will be presented. The instrument provides a new tool for probing in situ aerosol optical properties that may help inform remote sensing approaches well into the UV range.

Development the EarthCARE aerosol classification scheme

NASA Astrophysics Data System (ADS)

Wandinger, Ulla; Baars, Holger; Hünerbein, Anja; Donovan, Dave; van Zadelhoff, Gerd-Jan; Fischer, Jürgen; von Bismarck, Jonas; Eisinger, Michael; Lajas, Dulce; Wehr, Tobias

2015-04-01

The Earth Clouds, Aerosols and Radiation Explorer (EarthCARE) mission is a joint ESA/JAXA mission planned to be launched in 2018. The multi-sensor platform carries a cloud-profiling radar (CPR), a high-spectral-resolution cloud/aerosol lidar (ATLID), a cloud/aerosol multi-spectral imager (MSI), and a three-view broad-band radiometer (BBR). Three out of the four instruments (ATLID, MSI, and BBR) will be able to sense the global aerosol distribution and contribute to the overarching EarthCARE goals of sensor synergy and radiation closure with respect to aerosols. The high-spectral-resolution lidar ATLID obtains profiles of particle extinction and backscatter coefficients, lidar ratio, and linear depolarization ratio as well as the aerosol optical thickness (AOT) at 355 nm. MSI provides AOT at 670 nm (over land and ocean) and 865 nm (over ocean). Next to these primary observables the aerosol type is one of the required products to be derived from both lidar stand-alone and ATLID-MSI synergistic retrievals. ATLID measurements of the aerosol intensive properties (lidar ratio, depolarization ratio) and ATLID-MSI observations of the spectral AOT will provide the basic input for aerosol-type determination. Aerosol typing is needed for the quantification of anthropogenic versus natural aerosol loadings of the atmosphere, the investigation of aerosol-cloud interaction, assimilation purposes, and the validation of atmospheric transport models which carry components like dust, sea salt, smoke and pollution. Furthermore, aerosol classification is a prerequisite for the estimation of direct aerosol radiative forcing and radiative closure studies. With an appropriate underlying microphysical particle description, the categorization of aerosol observations into predefined aerosol types allows us to infer information needed for the calculation of shortwave radiative effects, such as mean particle size, single-scattering albedo, and spectral conversion factors. In order to ensure

Formation of high-molecular-weight compounds via the heterogeneous reactions of gaseous C8-C10 n-aldehydes in the presence of atmospheric aerosol components

NASA Astrophysics Data System (ADS)

Han, Yuemei; Kawamura, Kimitaka; Chen, Qingcai; Mochida, Michihiro

2016-02-01

A laboratory study on the heterogeneous reactions of straight-chain aldehydes was performed by exposing n-octanal, nonanal, and decanal vapors to ambient aerosol particles. The aerosol and blank filters were extracted using methanol. The extracts were nebulized and the resulting compositions were examined using a high-resolution time-of-flight aerosol mass spectrometer. The mass spectral analysis showed that the exposures of the aldehydes to aerosol samples increased the peak intensities in the high mass range. The peaks in the mass spectra of the aerosol samples after exposure to different aldehydes were characterized by a homologous series of peak shifts due to the addition of multiple CH2 units. This result is explained by the formation of high-molecular-weight (HMW) compounds that contain single or multiple aldehyde moieties. The HMW fragment peaks for the blank filters exposed to n-aldehydes were relatively weak, indicating an important contribution from the ambient aerosol components to the formation of the HMW compounds. Among the factors affecting the overall interaction of aldehydes with atmospheric aerosol components, gas phase diffusion possibly limited the reactions under the studied conditions; therefore, their occurrence to a similar degree in the atmosphere is not ruled out, at least for the reactions involving n-nonanal and decanal. The major formation pathways for the observed HMW products may be the self-reactions of n-aldehydes mediated by atmospheric aerosol components and the reactions of n-aldehydes with organic aerosol components. The observed formation of HMW compounds encourages further investigations into their effects on the aerosol properties as well as the organic aerosol mass in the atmosphere.

Secondary organic aerosol formation from isoprene photo-oxidation during cloud condensation-evaporation cycles (CUMULUS project)

NASA Astrophysics Data System (ADS)

Brégonzio-Rozier, Lola; Siekmann, Frank; Giorio, Chiara; Temime-Roussel, Brice; Pangui, Edouard; Morales, Sébastien; Gratien, Aline; Ravier, Sylvain; Monod, Anne; Doussin, Jean-Francois

2014-05-01

It is acknowledged that atmospheric photo-oxidation of Volatile Organic Compounds (VOC) leads to the formation of less volatile oxidized species. These compounds can undergo gas-to-particle conversion, leading to the formation of Secondary Organic Aerosols (SOA) in the atmosphere. Nevertheless, some of these oxidized species are water soluble and could also partition into cloud droplets. Higher molecular weight and less volatile compounds could be produced in the aqueous phase and remain in the particle phase after water evaporation (Ervens et al., 2011). The aim of the present work is to study SOA formation in the presence of cloud droplets during isoprene photo-oxidation. To this end, an original multiphase approach in a simulation chamber was set up in order to investigate the chemistry occurring in the gaseous, particulate and aqueous phases, and the exchange between these phases. Experiments were performed, within the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere), in the CESAM chamber (Wang et al., 2011). This chamber was designed to investigate multiphase processes under realistic actinic flux, and accurate control of both temperature and relative humidity. A specific protocol was set up to produce cloud events in the simulation chamber exhibiting a significant lifetime in the presence of light (10-12 minutes). By using this protocol, many clouds could be generated in a single experiment. In each experiment, around 800 ppb of isoprene was injected in the chamber together with HONO under dry conditions before irradiation. A Fourier Transform Infrared Spectrometer (FTIR), a Proton Transfer Reaction Mass Spectrometer (PTR-TOF-MS) and NOx and O3 analyzers were used to analyze gas-phase composition. Dried SOA size distributions and total concentrations were measured by a Scanning Mobility Particle Sizer (SMPS). An Aerodyne High Resolution Time-Of-Flight Aerosol Mass Spectrometer (HR-TOF-AMS) was also used to investigate

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

Sub 2 nm Particle Characterization in Systems with Aerosol Formation and Growth

NASA Astrophysics Data System (ADS)

Wang, Yang

Aerosol science and technology enable continual advances in material synthesis and atmospheric pollutant control. Among these advances, one important frontier is characterizing the initial stages of particle formation by real time measurement of particles below 2 nm in size. Sub 2 nm particles play important roles by acting as seeds for particle growth, ultimately determining the final properties of the generated particles. Tailoring nanoparticle properties requires a thorough understanding and precise control of the particle formation processes, which in turn requires characterizing nanoparticle formation from the initial stages. The knowledge on particle formation in early stages can also be applied in quantum dot synthesis and material doping. This dissertation pursued two approaches in investigating incipient particle characterization in systems with aerosol formation and growth: (1) using a high-resolution differential mobility analyzer (DMA) to measure the size distributions of sub 2 nm particles generated from high-temperature aerosol reactors, and (2) analyzing the physical and chemical pathways of aerosol formation during combustion. Part. 1. Particle size distributions reveal important information about particle formation dynamics. DMAs are widely utilized to measure particle size distributions. However, our knowledge of the initial stages of particle formation is incomplete, due to the Brownian broadening effects in conventional DMAs. The first part of this dissertation studied the applicability of high-resolution DMAs in characterizing sub 2 nm particles generated from high-temperature aerosol reactors, including a flame aerosol reactor (FLAR) and a furnace aerosol reactor (FUAR). Comparison against a conventional DMA (Nano DMA, Model 3085, TSI Inc.) demonstrated that the increased sheath flow rates and shortened residence time indeed greatly suppressed the diffusion broadening effect in a high-resolution DMA (half mini type). The incipient particle

Spatiotemporal variability and contribution of different aerosol types to the Aerosol Optical Depth over the Eastern Mediterranean

PubMed Central

Georgoulias, Aristeidis K.; Alexandri, Georgia; Kourtidis, Konstantinos A.; Lelieveld, Jos; Zanis, Prodromos; Pöschl, Ulrich; Levy, Robert; Amiridis, Vassilis; Marinou, Eleni; Tsikerdekis, Athanasios

2018-01-01

This study characterizes the spatiotemporal variability and relative contribution of different types of aerosols to the Aerosol Optical Depth (AOD) over the Eastern Mediterranean as derived from MODIS Terra (3/2000–12/2012) and Aqua (7/2002–12/2012) satellite instruments. For this purpose, a 0.1° × 0.1° gridded MODIS dataset was compiled and validated against sunphotometric observations from the AErosol RObotic NETwork (AERONET). The high spatial resolution and long temporal coverage of the dataset allows for the determination of local hot spots like megacities, medium sized cities, industrial zones, and power plant complexes, seasonal variabilities, and decadal averages. The average AOD at 550 nm (AOD550) for the entire region is ~ 0.22 ± 0.19 with maximum values in summer and seasonal variabilities that can be attributed to precipitation, photochemical production of secondary organic aerosols, transport of pollution and smoke from biomass burning in Central and Eastern Europe, and transport of dust from the Sahara Desert and the Middle East. The MODIS data were analyzed together with data from other satellite sensors, reanalysis projects and a chemistry-aerosol-transport model using an optimized algorithm tailored for the region and capable of estimating the contribution of different aerosol types to the total AOD550. The spatial and temporal variability of anthropogenic, dust and fine mode natural aerosols over land and anthropogenic, dust and marine aerosols over the sea is examined. The relative contribution of the different aerosol types to the total AOD550 exhibits a low/high seasonal variability over land/sea areas, respectively. Overall, anthropogenic aerosols, dust and fine mode natural aerosols account for ~ 51 %, ~ 34 % and ~ 15 % of the total AOD550 over land, while, anthropogenic aerosols, dust and marine aerosols account ~ 40 %, ~ 34 % and ~ 26 % of the total AOD550 over the sea, based on MODIS Terra and Aqua observations. PMID:29755508

Characteristics of Submicron Aerosols in 2013 summer of Beijing

NASA Astrophysics Data System (ADS)

Guo, Song; Hu, Min; Shang, Dongjie; Zheng, Jing; Du, Zhuofei; Wu, Yusheng; Lu, Sihua; Zeng, Limin; Zhang, Renyi

2016-04-01

To characterize the air pollution of North China Plain of China, CAREBEIJING-2013 field campaign (Campaigns of Air quality REsearch in BEIJING and surrounding region) was conducted in summer of 2013. Submicron aerosols were measured at an urban site PKU (Peking University, 39° 59'21"N, 116° 18'25"E) from July 28th to September 31st 2013. A suite of integrated instruments was used to measure the size distribution, effective density and hygroscopicity of ambient particles. The chemical composition of submicron particles were measured by using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) (Billerica, MA, USA). The average PM2.5 concentration was 73.0±70.7 μg m-3 during the measurement. The particulate pollution showed distinct 4-7 days cycles controlled by the meteorological conditions. Each cycle started with low PM2.5 mass concentrations (<20 μg m-3), since the air mass was from relatively clean mountainous area. The particle number concentrations were high, but and the sizes were small (<30 nm) at this stage, which can be explained by the new particle formation. In the succeeding days, both the particle mass and size continuously increased. The PM2.5concentration increased rapidly by >60 μg day-1, and the particle mean diameter grew to >100 nm. It is interesting to note that the mean diameters showed similar trend to PM2.5 mass concentrations, indicating the particle pollution attributed to the growth of the newly formed small particles. During the measurement, the average particle densities are between 1.3-1.5 g cm-3, indicating organics and sulfate were dominant in the particles. The densities of smaller particles, i.e. 46 nm, 81nm, showed single peak at 1.3-1.5 g cm-3, indicating the particles are internal mixed sulfate and organics. While the 150nm and 240 nm particle densities exhibited bimodal distribution with an additional small peak at ˜1.1 g cm-3, which is considered as external mixed organic particles or aged

Increased exposure to pollutant aerosols under high voltage power lines.

PubMed

Fews, A P; Henshaw, D L; Keitch, P A; Close, J J; Wilding, R J

1999-12-01

To assess increased exposure to airborne pollutants near power lines by investigating theoretically and experimentally the behaviour of 222Rn decay product marker aerosols in the 50 Hz electric field under power lines. The behaviour of aerosols in outdoor air including those carrying 222Rn decay products was modelled theoretically in the presence of an AC field. TASTRAK alpha-particle spectroscopy was used to characterize 218Po and 214Po aerosols outdoors. Sampling points were chosen along a line at right angles up to 200 m from a number of high voltage power (transmission) lines. Each sampling point comprised an arrangement of mutually orthogonal TASTRAK detectors. Exposures were carried out at different power line locations in various weather conditions. The model predicts a two- to three-fold increase in deposition of aerosols on spherical surfaces mimicking the human head under high voltage power lines. Experimental measurements using detectors mounted on grounded metal spheres showed an enhanced deposition of both 218Po and 214Po aerosols. Enhanced 218Po deposition on 400 kV lines ranged from 1.96+/-0.15 to 2.86+/-0.32. Enhanced 214Po deposition on 275 kV and 132 kV lines were 1.43+/-0.07 and 1.11+/-0.21, respectively, where the latter value was not significant. The observations demonstrate a mode of increased exposure to pollutant aerosols under high voltage power lines by increased deposition on the body. The total (indoor + outdoor) 218Po and 214Po dose to the basal layer of facial skin is estimated to be increased by between 1.2 and 2.0 for 10% of time spent outdoors under high voltage power lines.

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

Dubey, Manvendra; Aiken, Allison; Berg, Larry K.

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

Multispectral information for gas and aerosol retrieval from TANSO-FTS instrument

NASA Astrophysics Data System (ADS)

Herbin, H.; Labonnote, L. C.; Dubuisson, P.

2012-11-01

The Greenhouse gases Observing SATellite (GOSAT) mission and in particular TANSO-FTS instrument has the advantage to measure simultaneously the same field of view in different spectral ranges with a high spectral resolution. These features are promising to improve, not only, gaseous retrieval in clear sky or scattering atmosphere, but also to retrieve aerosol parameters. Therefore, this paper is dedicated to an Information Content (IC) analysis of potential synergy between thermal infrared, shortwave infrared and visible, in order to obtain a more accurate retrieval of gas and aerosol. The latter is based on Shannon theory and used a sophisticated radiative transfer algorithm developed at "Laboratoire d'Optique Atmosphérique", dealing with multiple scattering. This forward model can be relied to an optimal estimation method, which allows simultaneously retrieving gases profiles and aerosol granulometry and concentration. The analysis of the information provided by the spectral synergy is based on climatology of dust, volcanic ash and biomass burning aerosols. This work was conducted in order to develop a powerful tool that allows retrieving simultaneously not only the gas concentrations but also the aerosol characteristics by selecting the so called "best channels", i.e. the channels that bring most of the information concerning gas and aerosol. The methodology developed in this paper could also be used to define the specifications of future high spectral resolution mission to reach a given accuracy on retrieved parameters.

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: Results from DISCOVER-AQ California

DOE PAGES

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; ...

2016-05-02

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) andmore » an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM 1) concentration was 31.0 µg m −3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C  =  0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C  =  0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C  =  0.33; BBOA2: 20 % of total OA, O / C  =  0.60) most likely

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, Dominique E.; Kim, Hwajin; Parworth, Caroline; Zhou, Shan; Zhang, Xiaolu; Cappa, Christopher D.; Seco, Roger; Kim, Saewung; Zhang, Qi

2016-05-01

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno-Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O / C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O / C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O / C = 0.33; BBOA2: 20 % of total OA, O / C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV

Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

NASA Astrophysics Data System (ADS)

Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

2015-12-01

The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 μg m-3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi

Target categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements

NASA Astrophysics Data System (ADS)

Baars, Holger; Seifert, Patric; Engelmann, Ronny; Wandinger, Ulla

2017-09-01

Absolute calibrated signals at 532 and 1064 nm and the depolarization ratio from a multiwavelength lidar are used to categorize primary aerosol but also clouds in high temporal and spatial resolution. Automatically derived particle backscatter coefficient profiles in low temporal resolution (30 min) are applied to calibrate the lidar signals. From these calibrated lidar signals, new atmospheric parameters in temporally high resolution (quasi-particle-backscatter coefficients) are derived. By using thresholds obtained from multiyear, multisite EARLINET (European Aerosol Research Lidar Network) measurements, four aerosol classes (small; large, spherical; large, non-spherical; mixed, partly non-spherical) and several cloud classes (liquid, ice) are defined. Thus, particles are classified by their physical features (shape and size) instead of by source. The methodology is applied to 2 months of continuous observations (24 h a day, 7 days a week) with the multiwavelength-Raman-polarization lidar PollyXT during the High-Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in spring 2013. Cloudnet equipment was operated continuously directly next to the lidar and is used for comparison. By discussing three 24 h case studies, it is shown that the aerosol discrimination is very feasible and informative and gives a good complement to the Cloudnet target categorization. Performing the categorization for the 2-month data set of the entire HOPE campaign, almost 1 million pixel (5 min × 30 m) could be analysed with the newly developed tool. We find that the majority of the aerosol trapped in the planetary boundary layer (PBL) was composed of small particles as expected for a heavily populated and industrialized area. Large, spherical aerosol was observed mostly at the top of the PBL and close to the identified cloud bases, indicating the importance of hygroscopic growth of the particles at high relative

Lidar characterizations of atmospheric aerosols and clouds

NASA Astrophysics Data System (ADS)

Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Burton, S. P.

2017-12-01

Knowledge of the vertical profile, composition, concentration, and size distribution of aerosols is required to quantify the impacts of aerosols on human health, global and regional climate, clouds and precipitation. In particular, radiative forcing due to anthropogenic aerosols is the most uncertain part of anthropogenic radiative forcing, with aerosol-cloud interactions (ACI) as the largest source of uncertainty in current estimates of global radiative forcing. Improving aerosol transport model predictions of the vertical profile of aerosol optical and microphysical characteristics is crucial for improving assessments of aerosol radiative forcing. Understanding how aerosols and clouds interact is essential for investigating the aerosol indirect effect and ACI. Through its ability to provide vertical profiles of aerosol and cloud distributions as well as important information regarding the optical and physical properties of aerosols and clouds, lidar is a crucial tool for addressing these science questions. This presentation describes how surface, airborne, and satellite lidar measurements have been used to address these questions, and in particular how High Spectral Resolution Lidar (HSRL) measurements provide profiles of aerosol properties (backscatter, extinction, depolarization, concentration, size) important for characterizing radiative forcing. By providing a direct measurement of aerosol extinction, HSRL provides more accurate aerosol measurement profiles and more accurate constraints for models than standard retrievals from elastic backscatter lidar, which loses accuracy and precision at lower altitudes due to attenuation from overlying layers. Information regarding particle size and abundance from advanced lidar retrievals provides better proxies for cloud-condensation-nuclei (CCN), which are required for assessing aerosol-cloud interactions. When combined with data from other sensors, advanced lidar measurements can provide information on aerosol and

Final report for "Characterization of Fine Particulate Matter (PM) and secondary PM Precursor Gases in the Mexico City Metropolitan Area"

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

Prof. Jose-Luis Jimenez

2009-05-18

The objectives of this funded project were (a) to further analyze the data collected by our group and collaborators in Mexico City during the MCMA-2003 field campaign, with the goal of further our understanding of aerosol sources and processes; and (b) to deploy several advanced instruments, including the newly developed high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and thermal-denuder (TD), during the MILAGRO/MAX-Mex/MCMA-2006 field campaign, and to analyze those data (together with the 2003 data) to provide additional insights on the formation and transformation of aerosols in the Mexico City area. These goals were addressed in collaboration with our project partners,more » MIT/Molina Center, and Aerodyne Research. Overall this project was very successful, resulting on 22+ journal papers including six “highly cited papers” and three papers that are the most cited in their respective journals (out of several thousand papers) since the year in which they were published. Multiple discoveries, such as the the underestimation of SOA in urban areas even for short photochemical ages, the demonstration that urban POA is of similar or higher volatility than urban SOA, and the first analysis of organic aerosol elemental composition in real-time have been recently published. Several dozen presentations at major US and international conferences and seminars also acknowledged this grant.« less

Improved MODIS aerosol retrieval in urban areas using a land classification approach and empirical orthogonal functions

NASA Astrophysics Data System (ADS)

Levitan, Nathaniel; Gross, Barry

2016-10-01

New, high-resolution aerosol products are required in urban areas to improve the spatial coverage of the products, in terms of both resolution and retrieval frequency. These new products will improve our understanding of the spatial variability of aerosols in urban areas and will be useful in the detection of localized aerosol emissions. Urban aerosol retrieval is challenging for existing algorithms because of the high spatial variability of the surface reflectance, indicating the need for improved urban surface reflectance models. This problem can be stated in the language of novelty detection as the problem of selecting aerosol parameters whose effective surface reflectance spectrum is not an outlier in some space. In this paper, empirical orthogonal functions, a reconstruction-based novelty detection technique, is used to perform single-pixel aerosol retrieval using the single angular and temporal sample provided by the MODIS sensor. The empirical orthogonal basis functions are trained for different land classes using the MODIS BRDF MCD43 product. Existing land classification products are used in training and aerosol retrieval. The retrieval is compared against the existing operational MODIS 3 KM Dark Target (DT) aerosol product and co-located AERONET data. Based on the comparison, our method allows for a significant increase in retrieval frequency and a moderate decrease in the known biases of MODIS urban aerosol retrievals.

An example of aerosol pattern variability over bright surface using high resolution MODIS MAIAC: The eastern and western areas of the Dead Sea and environs.

PubMed

Lee, Sever; Pinhas, Alpert; Alexei, Lyapustin; Yujie, Wang; Alexandra, Chudnovsky A

2017-09-01

The extreme rate of evaporation of the Dead Sea (DS) has serious implicatios for the surrounding area, including atmospheric conditions. This study analyzes the aerosol properties over the western and eastern parts of the DS during the year 2013, using MAIAC (Multi-Angle Implementation of Atmospheric Correction) for MODIS, which retrieves aerosol optical depth (AOD) data at a resolution of 1km. The main goal of the study is to evaluate MAIAC over the study area and determine, for the first time, the prevailing aerosol spatial patterns. First, the MAIAC-derived AOD data was compared with data from three nearby AERONET sites (Nes Ziona - an urban site, and Sede Boker and Masada - two arid sites), and with the conventional Dark Target (DT) and Deep Blue (DB) retrievals for the same days and locations, on a monthly basis throughout 2013. For the urban site, the correlation coefficient (r) for DT/DB products showed better performance than MAIAC (r=0.80, 0.75, and 0.64 respectively) year-round. However, in the arid zones, MAIAC showed better correspondence to AERONET sites than the conventional retrievals (r=0.58-0.60 and 0.48-0.50 respectively). We investigated the difference in AOD levels, and its variability, between the Dead Sea coasts on a seasonal basis and calculated monthly/seasonal AOD averages for presenting AOD patterns over arid zones. Thus, we demonstrated that aerosol concentrations show a strong preference for the western coast, particularly during the summer season. This preference, is most likely a result of local anthropogenic emissions combined with the typical seasonal synoptic conditions, the Mediterranean Sea breeze, and the region complex topography. Our results also indicate that a large industrial zone showed higher AOD levels compared to an adjacent reference-site, i.e., 13% during the winter season.

Comparison of Coincident Multiangle Imaging Spectroradiometer and Moderate Resolution Imaging Spectroradiometer Aerosol Optical Depths over Land and Ocean Scenes Containing Aerosol Robotic Network Sites

NASA Technical Reports Server (NTRS)

Abdou, Wedad A.; Diner, David J.; Martonchik, John V.; Bruegge, Carol J.; Kahn, Ralph A.; Gaitley, Barbara J.; Crean, Kathleen A.; Remer, Lorraine A.; Holben, Brent

2005-01-01

The Multiangle Imaging Spectroradiometer (MISR) and the Moderate Resolution Imaging Spectroradiometer (MODIS), launched on 18 December 1999 aboard the Terra spacecraft, are making global observations of top-of-atmosphere (TOA) radiances. Aerosol optical depths and particle properties are independently retrieved from these radiances using methodologies and algorithms that make use of the instruments corresponding designs. This paper compares instantaneous optical depths retrieved from simultaneous and collocated radiances measured by the two instruments at locations containing sites within the Aerosol Robotic Network (AERONET). A set of 318 MISR and MODIS images, obtained during the months of March, June, and September 2002 at 62 AERONET sites, were used in this study. The results show that over land, MODIS aerosol optical depths at 470 and 660 nm are larger than those retrieved from MISR by about 35% and 10% on average, respectively, when all land surface types are included in the regression. The differences decrease when coastal and desert areas are excluded. For optical depths retrieved over ocean, MISR is on average about 0.1 and 0.05 higher than MODIS in the 470 and 660 nm bands, respectively. Part of this difference is due to radiometric calibration and is reduced to about 0.01 and 0.03 when recently derived band-to-band adjustments in the MISR radiometry are incorporated. Comparisons with AERONET data show similar patterns.

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

Development of an aerosol assimilation/forecasting system with Himawari-8 aerosol products

NASA Astrophysics Data System (ADS)

Maki, T.; Yumimoto, K.; Tanaka, T. Y.; Yoshida, M.; Kikuchi, M.; Nagao, T. M.; Murakami, H.; Ogi, A.; Sekiyama, T. T.

2016-12-01

A new generation geostationary meteorological satellite (GMS), Himawari-8, was launched on 7 October 2014 and became operational on 7 July 2015. Himawari-8 is equipped with more advanced multispectral imager (Advanced Himawari Imager; AHI) ahead of other planned GMSs (e.g., GEOS-R). The AHI has 16 observational bands including three visible lights (i.e. RGB) with high spatial (0.5-2 km) and temporal (every 10 minutes full-disk images) resolutions, and provides about 50 times more data than previous GMSs. It is attractive characteristics for aerosol study that the visible and near-infrared observational bands allow us to obtain full-disk maps of aerosol optical properties (i.e., aerosol optical thickness (AOT) and ångström exponent) with unprecedented temporal resolution. Meteorological Research Institute (MRI)/JMA and Japan Aerospace Exploration Agency (JAXA) have been developing an aerosol assimilation/forecasting system with a global aerosol transport model (MASINGAR mk-2), 2 dimensional variational (2D-Var) method, and the Himawari-8 AOTs. Forecasting results are quantitatively validated by AOTs measured by AERONET and PM2.5 concentrations obtained by in-situ stations. Figure 1 shows model-predicted and satellite-observed AOTs during the 2016 Siberian wildfire. Upper and lower panels exhibit maps of AOT at analysis time (0000 UTC on May 18, 2016) and 27-hour forecast time (03 UTC on May 19, 2016), respectively. The 27-hour forecasted AOT starting with the analyzed initial condition (Figure 1f) successfully predicts heavy smokes covering the northern part of Japan, which forecast without assimilation (Figure 1e) failed to reproduces. Figure 1: Horizontal distribution of observed and forecasted AOTs at 0000 UTC 18 May, 2016 (analysis time; upper panels) and 0300 UTC 19 May, 2016 (18-h forecast from the analysis time; lower panel). (a, d) observed AOT from Himawari-8, (b, e) forecasted AOT without assimilation, and (c, f) forecast AOT with assimilation.

Determination of particulate lead during MILAGRO/MCMA-2006 using Aerosol Mass Spectrometry

NASA Astrophysics Data System (ADS)

Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

2010-02-01

We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s) and ~75% exhibiting slow evaporation (τ~2.4 min) at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at T0 (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the compounds generating Pb

Determination of particulate lead using aerosol mass spectrometry: MILAGRO/MCMA-2006 observations

NASA Astrophysics Data System (ADS)

Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

2010-06-01

We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s) and ~75% exhibiting slow evaporation (τ~2.4 min) at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the

A Global Data Assimilation System for Atmospheric Aerosol

NASA Technical Reports Server (NTRS)

daSilva, Arlindo

1999-01-01

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

Significant radiative impact of volcanic aerosol in the lowermost stratosphere

PubMed Central

Andersson, Sandra M.; Martinsson, Bengt G.; Vernier, Jean-Paul; Friberg, Johan; Brenninkmeijer, Carl A. M.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, Andreas

2015-01-01

Despite their potential to slow global warming, until recently, the radiative forcing associated with volcanic aerosols in the lowermost stratosphere (LMS) had not been considered. Here we study volcanic aerosol changes in the stratosphere using lidar measurements from the NASA CALIPSO satellite and aircraft measurements from the IAGOS-CARIBIC observatory. Between 2008 and 2012 volcanism frequently affected the Northern Hemisphere stratosphere aerosol loadings, whereas the Southern Hemisphere generally had loadings close to background conditions. We show that half of the global stratospheric aerosol optical depth following the Kasatochi, Sarychev and Nabro eruptions is attributable to LMS aerosol. On average, 30% of the global stratospheric aerosol optical depth originated in the LMS during the period 2008–2011. On the basis of the two independent, high-resolution measurement methods, we show that the LMS makes an important contribution to the overall volcanic forcing. PMID:26158244

Development of IDEA product for GOES-R aerosol data

NASA Astrophysics Data System (ADS)

Zhang, Hai; Hoff, Raymond M.; Kondragunta, Shobha

2009-08-01

The NOAA GOES-R Advanced Baseline Imager (ABI) will have nearly the same capabilities as NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) to generate multi-wavelength retrievals of aerosol optical depth (AOD) with high temporal and spatial resolution, which can be used as a surrogate of surface particulate measurements such as PM2.5 (particulate matter with diameter less than 2.5 μm). To prepare for the launch of GOES-R and its application in the air quality forecasting, we have transferred and enhanced the Infusing satellite Data into Environmental Applications (IDEA) product from University of Wisconsin to NOAA NESDIS. IDEA was created through a NASA/EPA/NOAA cooperative effort. The enhanced IDEA product provides near-real-time imagery of AOD derived from multiple satellite sensors including MODIS Terra, MODIS Aqua, GOES EAST and GOES WEST imager. Air quality forecast guidance is produced through a trajectory model initiated at locations with high AOD retrievals and/or high aerosol index (AI) from OMI (Ozone Monitoring Instrument). The product is currently running at http://www.star.nesdis.noaa.gov/smcd/spb/aq/. The IDEA system will be tested using the GOES-R ABI proxy dataset, and will be ready to operate with GOES-R aerosol data when GOES-R is launched.

Aerosol-cloud interactions in mixed-phase convective clouds - Part 1: Aerosol perturbations

NASA Astrophysics Data System (ADS)

Miltenberger, Annette K.; Field, Paul R.; Hill, Adrian A.; Rosenberg, Phil; Shipway, Ben J.; Wilkinson, Jonathan M.; Scovell, Robert; Blyth, Alan M.

2018-03-01

Changes induced by perturbed aerosol conditions in moderately deep mixed-phase convective clouds (cloud top height ˜ 5 km) developing along sea-breeze convergence lines are investigated with high-resolution numerical model simulations. The simulations utilise the newly developed Cloud-AeroSol Interacting Microphysics (CASIM) module for the Unified Model (UM), which allows for the representation of the two-way interaction between cloud and aerosol fields. Simulations are evaluated against observations collected during the COnvective Precipitation Experiment (COPE) field campaign over the southwestern peninsula of the UK in 2013. The simulations compare favourably with observed thermodynamic profiles, cloud base cloud droplet number concentrations (CDNC), cloud depth, and radar reflectivity statistics. Including the modification of aerosol fields by cloud microphysical processes improves the correspondence with observed CDNC values and spatial variability, but reduces the agreement with observations for average cloud size and cloud top height. Accumulated precipitation is suppressed for higher-aerosol conditions before clouds become organised along the sea-breeze convergence lines. Changes in precipitation are smaller in simulations with aerosol processing. The precipitation suppression is due to less efficient precipitation production by warm-phase microphysics, consistent with parcel model predictions. In contrast, after convective cells organise along the sea-breeze convergence zone, accumulated precipitation increases with aerosol concentrations. Condensate production increases with the aerosol concentrations due to higher vertical velocities in the convective cores and higher cloud top heights. However, for the highest-aerosol scenarios, no further increase in the condensate production occurs, as clouds grow into an upper-level stable layer. In these cases, the reduced precipitation efficiency (PE) dominates the precipitation response and no further

The evolution of Titan's high-altitude aerosols under ultraviolet irradiation

NASA Astrophysics Data System (ADS)

Carrasco, Nathalie; Tigrine, Sarah; Gavilan, Lisseth; Nahon, Laurent; Gudipati, Murthy S.

2018-04-01

The Cassini-Huygens space mission revealed that Titan's thick brownish haze is initiated high in the atmosphere at an altitude of about 1,000 km, before a slow transportation down to the surface. Close to the surface, at altitudes below 130 km, the Huygens probe provided information on the chemical composition of the haze. So far, we have not had insights into the possible photochemical evolution of the aerosols making up the haze during their descent. Here, we address this atmospheric aerosol aging process, simulating in the laboratory how solar vacuum ultraviolet irradiation affects the aerosol optical properties as probed by infrared spectroscopy. An important evolution was found that could explain the apparent contradiction between the nitrogen-poor infrared spectroscopic signature observed by Cassini below 600 km of altitude in Titan's atmosphere and a high nitrogen content as measured by the aerosol collector and pyrolyser of the Huygens probe at the surface of Titan.

The evolution of Titan's high-altitude aerosols under ultraviolet irradiation

NASA Astrophysics Data System (ADS)

Carrasco, Nathalie; Tigrine, Sarah; Gavilan, Lisseth; Nahon, Laurent; Gudipati, Murthy S.

2018-06-01

The Cassini-Huygens space mission revealed that Titan's thick brownish haze is initiated high in the atmosphere at an altitude of about 1,000 km, before a slow transportation down to the surface. Close to the surface, at altitudes below 130 km, the Huygens probe provided information on the chemical composition of the haze. So far, we have not had insights into the possible photochemical evolution of the aerosols making up the haze during their descent. Here, we address this atmospheric aerosol aging process, simulating in the laboratory how solar vacuum ultraviolet irradiation affects the aerosol optical properties as probed by infrared spectroscopy. An important evolution was found that could explain the apparent contradiction between the nitrogen-poor infrared spectroscopic signature observed by Cassini below 600 km of altitude in Titan's atmosphere and a high nitrogen content as measured by the aerosol collector and pyrolyser of the Huygens probe at the surface of Titan.

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

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

NASA Astrophysics Data System (ADS)

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

2015-05-01

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

Source apportionment of submicron organic aerosol collected from Atlanta, Georgia, during 2014-2015 using the aerosol chemical speciation monitor (ACSM)