NASA Astrophysics Data System (ADS)
Zhang, Haijie; Chen, Shilu; Zhong, Jie; Zhang, Shaowen; Zhang, Yunhong; Zhang, Xiuhui; Li, Zesheng; Zeng, Xiao Cheng
2018-03-01
Sulfate is one of the most important components in the aerosol due to its key role in air pollution and global climate change. Recent work has suggested that reactive nitrogen chemistry in aqueous water can explain the missing source of sulfate in the aqueous water. Herein, we have mapped out the energy profile of the oxidization process of SO2 leading from NO2 and two feasible three-step mechanisms have been proposed. For the oxidation of HOSO2- and HSO3- by the dissolved NO2 in weakly acidic and neutral aerosol (pH ≤ 7), the main contribution to the missing sulfate production comes from the oxidation of HOSO2-. The whole process is a self-sustaining process. For the oxidation of SO32- in alkaline aerosol (pH > 7), the third step - decomposition step of H2O or hydrolysis of SO3 step which are two parallel processes are the rate-limiting steps. The present results are of avail to better understand the missing source of sulfate in the aerosol and hence may lead to better science-based solutions for resolving the severe haze problems in China.
Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China
Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; He, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang
2016-01-01
Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to ~300 μg m−3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. PMID:28028539
Radiative Forcing in the ACCMIP Historical and Future Climate Simulations
NASA Technical Reports Server (NTRS)
Shindell, Drew Todd; Lamarque, J.-F.; Schulz, M.; Flanner, M.; Jiao, C.; Chin, M.; Young, P. J.; Lee, Y. H.; Rotstayn, L.; Mahowald, N.;
2013-01-01
A primary goal of the Atmospheric Chemistry and Climate Model IntercomparisonProject (ACCMIP) was to characterize the short-lived drivers of preindustrial to 2100climate change in the current generation of climate models. Here we evaluate historicaland 5 future radiative forcing in the 10 ACCMIP models that included aerosols, 8 of whichalso participated in the Coupled Model Intercomparison Project phase 5 (CMIP5).The models generally reproduce present-day climatological total aerosol opticaldepth (AOD) relatively well. components to this total, however, and most appear to underestimate AOD over East10 Asia. The models generally capture 1980-2000 AOD trends fairly well, though theyunderpredict AOD increases over the YellowEastern Sea. They appear to strongly underestimate absorbing AOD, especially in East Asia, South and Southeast Asia, SouthAmerica and Southern Hemisphere Africa.We examined both the conventional direct radiative forcing at the tropopause (RF) and the forcing including rapid adjustments (adjusted forcing AF, including direct andindirect effects). The models calculated all aerosol all-sky 1850 to 2000 global meanannual average RF ranges from 0.06 to 0.49 W m(sup -2), with a mean of 0.26 W m(sup -2) and a median of 0.27 W m(sup -2. Adjusting for missing aerosol components in some modelsbrings the range to 0.12 to 0.62W m(sup -2), with a mean of 0.39W m(sup -2). Screen20ing the models based on their ability to capture spatial patterns and magnitudes ofAOD and AOD trends yields a quality-controlled mean of 0.42W m(sup -2) and range of0.33 to 0.50 W m(sup -2) (accounting for missing components). The CMIP5 subset of ACCMIPmodels spans 0.06 to 0.49W m(sup -2), suggesting some CMIP5 simulations likelyhave too little aerosol RF. A substantial, but not well quantified, contribution to histori25cal aerosol RF may come from climate feedbacks (35 to 58). The mean aerosol AF during this period is 1.12W m(sup -2) (median value 1.16W m(sup -2), range 0.72 to1.44W m(sup -2), indicating that adjustments to aerosols, which include cloud, water vaporand temperature, lead to stronger forcing than the aerosol direct RF.
Radiative Forcing of the Direct Aerosol Effect from AeroCom Phase II Simulations
NASA Technical Reports Server (NTRS)
Myhre, G.; Samset, B. H.; Schulz, M.; Balkanski, Y.; Bauer, S.; Berntsen, T. K.; Bian, H.; Bellouin, N.; Chin, M.; Diehl, T.;
2013-01-01
We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02 W m(sup-2), with a mean of -0.27 W m(sup-2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.35 W m(sup-2). Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study.We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results
Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China
NASA Astrophysics Data System (ADS)
Cheng, Yafang; Zheng, Guangjie; Wei, Chao; Mu, Qing; Zheng, Bo; Wang, Zhibin; Gao, Meng; Zhang, Qiang; Wang, Kebin; Carmichael, Gregory; Pöschl, Ulrich; Su, Hang
2017-04-01
Fine-particle pollution associated with winter haze threatens the health of more than 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations of up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models that rely on sulfate production mechanisms requiring photochemical oxidants cannot predict these high levels because of the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor, where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content, leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.
Reactive Nitrogen Chemistry in Aerosol Water as a Source of Sulfate during Haze Events in China
NASA Astrophysics Data System (ADS)
Su, H.; Zheng, G.; Wei, C.; Mu, Q.; Zheng, B.; Wang, Z.; Zhang, Q.; Gao, M.; He, K.; Carmichael, G. R.; Poeschl, U.; Cheng, Y.
2017-12-01
Fine particle pollution associated with winter haze threatens the health of over 400 million people in the North China Plain. Sulfate is a major component of fine haze particles. Record sulfate concentrations up to 300 μg m-3 were observed during the January 2013 winter haze event in Beijing. State-of-the-art air quality models relying on sulfate production mechanisms that require photochemical oxidants, cannot predict these high levels due to the weak photochemistry activity during haze events. We find that the missing source of sulfate and particulate matter can be explained by reactive nitrogen chemistry in aerosol water. The aerosol water serves as a reactor where the alkaline aerosol components trap SO2, which is oxidized by NO2 to form sulfate, whereby high reaction rates are sustained by the high neutralizing capacity of the atmosphere in northern China. This mechanism is self-amplifying because higher aerosol mass concentration corresponds to higher aerosol water content leading to faster sulfate production and more severe haze pollution. Reference: Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Science Advances, 2, 10.1126/sciadv.1601530, 2016.
Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations
DOE Office of Scientific and Technical Information (OSTI.GOV)
Myhre, G.; Samset, B. H.; Schulz, M.
2013-01-01
We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has amore » range from -0.58 to -0.02 Wm -2, with a mean of -0.27 Wm -2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.35 Wm -2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.« less
Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations
NASA Astrophysics Data System (ADS)
Myhre, G.; Samset, B. H.; Schulz, M.; Balkanski, Y.; Bauer, S.; Berntsen, T. K.; Bian, H.; Bellouin, N.; Chin, M.; Diehl, T.; Easter, R. C.; Feichter, J.; Ghan, S. J.; Hauglustaine, D.; Iversen, T.; Kinne, S.; Kirkevåg, A.; Lamarque, J.-F.; Lin, G.; Liu, X.; Lund, M. T.; Luo, G.; Ma, X.; van Noije, T.; Penner, J. E.; Rasch, P. J.; Ruiz, A.; Seland, Ø.; Skeie, R. B.; Stier, P.; Takemura, T.; Tsigaridis, K.; Wang, P.; Wang, Z.; Xu, L.; Yu, H.; Yu, F.; Yoon, J.-H.; Zhang, K.; Zhang, H.; Zhou, C.
2013-02-01
We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02 Wm-2, with a mean of -0.27 Wm-2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.35 Wm-2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.
Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations
NASA Astrophysics Data System (ADS)
Myhre, G.; Samset, B. H.; Schulz, M.; Balkanski, Y.; Bauer, S.; Berntsen, T. K.; Bian, H.; Bellouin, N.; Chin, M.; Diehl, T.; Easter, R. C.; Feichter, J.; Ghan, S. J.; Hauglustaine, D.; Iversen, T.; Kinne, S.; Kirkevåg, A.; Lamarque, J.-F.; Lin, G.; Liu, X.; Luo, G.; Ma, X.; Penner, J. E.; Rasch, P. J.; Seland, Ø.; Skeie, R. B.; Stier, P.; Takemura, T.; Tsigaridis, K.; Wang, Z.; Xu, L.; Yu, H.; Yu, F.; Yoon, J.-H.; Zhang, K.; Zhang, H.; Zhou, C.
2012-08-01
We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 15 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 15 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02 W m-2, with a mean of -0.30 W m-2 for the 15 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.39 W m-2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.
On the Accuracy of Double Scattering Approximation for Atmospheric Polarization Computations
NASA Technical Reports Server (NTRS)
Korkin, Sergey V.; Lyapustin, Alexei I.; Marshak, Alexander L.
2011-01-01
Interpretation of multi-angle spectro-polarimetric data in remote sensing of atmospheric aerosols require fast and accurate methods of solving the vector radiative transfer equation (VRTE). The single and double scattering approximations could provide an analytical framework for the inversion algorithms and are relatively fast, however accuracy assessments of these approximations for the aerosol atmospheres in the atmospheric window channels have been missing. This paper provides such analysis for a vertically homogeneous aerosol atmosphere with weak and strong asymmetry of scattering. In both cases, the double scattering approximation gives a high accuracy result (relative error approximately 0.2%) only for the low optical path - 10(sup -2) As the error rapidly grows with optical thickness, a full VRTE solution is required for the practical remote sensing analysis. It is shown that the scattering anisotropy is not important at low optical thicknesses neither for reflected nor for transmitted polarization components of radiation.
A Backscatter-Lidar Forward-Operator
NASA Astrophysics Data System (ADS)
Geisinger, Armin; Behrendt, Andreas; Wulfmeyer, Volker; Vogel, Bernhard; Mattis, Ina; Flentje, Harald; Förstner, Jochen; Potthast, Roland
2015-04-01
We have developed a forward-operator which is capable of calculating virtual lidar profiles from atmospheric state simulations. The operator allows us to compare lidar measurements and model simulations based on the same measurement parameter: the lidar backscatter profile. This method simplifies qualitative comparisons and also makes quantitative comparisons possible, including statistical error quantification. Implemented into an aerosol-capable model system, the operator will act as a component to assimilate backscatter-lidar measurements. As many weather services maintain already networks of backscatter-lidars, such data are acquired already in an operational manner. To estimate and quantify errors due to missing or uncertain aerosol information, we started sensitivity studies about several scattering parameters such as the aerosol size and both the real and imaginary part of the complex index of refraction. Furthermore, quantitative and statistical comparisons between measurements and virtual measurements are shown in this study, i.e. applying the backscatter-lidar forward-operator on model output.
NASA Astrophysics Data System (ADS)
Ots, Riinu; Young, Dominique E.; Vieno, Massimo; Xu, Lu; Dunmore, Rachel E.; Allan, James D.; Coe, Hugh; Williams, Leah R.; Herndon, Scott C.; Ng, Nga L.; Hamilton, Jacqueline F.; Bergström, Robert; Di Marco, Chiara; Nemitz, Eiko; Mackenzie, Ian A.; Kuenen, Jeroen J. P.; Green, David C.; Reis, Stefan; Heal, Mathew R.
2016-05-01
We present high-resolution (5 km × 5 km) atmospheric chemical transport model (ACTM) simulations of the impact of newly estimated traffic-related emissions on secondary organic aerosol (SOA) formation over the UK for 2012. Our simulations include additional diesel-related intermediate-volatility organic compound (IVOC) emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo) campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA) as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA) components derived from aerosol mass spectrometer (AMS) measurements also made during the ClearfLo campaign at three sites in the London area. According to the model simulations, diesel-related IVOCs can explain on average ˜ 30 % of the annual SOA in and around London. Furthermore, the 90th percentile of modelled daily SOA concentrations for the whole year is 3.8 µg m-3, constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories) is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mills, Michael J.; Schmidt, Anja; Easter, Richard
Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptionsmore » between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.« less
Evidence of Aerosols as a Media for Rapid Daytime HONO Production over China
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liu, Zhen; Wang, Yuhang; Costabile, Francesa
Current knowledge of daytime HONO sources remains incomplete. A large missing daytime HONO source has been found in many places around the world, including polluted regions in China. Conventional understanding and recent studies attributed this missing source mainly to ground surface processes or gas-phase chemistry, while assuming aerosols to be an insignificant media for HONO production. We analyze in situ observations of HONO and its precursors at an urban site in Beijing, China, and report an apparent dependence of the missing HONO source strength on aerosol surface area and solar ultraviolet radiation. Based on extensive correlation analysis and process-modeling, wemore » propose that the rapid daytime HONO production in Beijing can be explained by enhanced hydrolytic disproportionation of NO2 on aqueous aerosol surfaces due to catalysis by dicarboxylic acid anions. The combination of high abundance of NO2, aromatic hydrocarbons, and aerosols over broad regions in China likely leads to elevated HONO levels, rapid OH production, and enhanced oxidizing capacity on a regional basis. Our findings call for attention to aerosols as a media for daytime heterogeneous HONO production in polluted regions like Beijing. This study also highlights the complex and uncertain heterogeneous chemistry in China, which merits future efforts of reconciling regional modeling and laboratory experiments, in order to understand and mitigate the regional particulate and O3 pollutions over China.« less
NASA Astrophysics Data System (ADS)
Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James
2017-10-01
Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength for BB aerosol sources. Our previous work shows that to first order, satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the smoke source strength. We now refine the satellite-snapshot method and investigate where applying simple multiplicative emission adjustment factors alone to the widely used Global Fire Emission Database version 3 emission inventory can achieve regional-scale consistency between Moderate Resolution Imaging Spectroradiometer (MODIS) AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport model. The model and satellite AOD are compared globally, over a set of BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. Regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. We refine our approach to address physically based limitations of our earlier work (1) by expanding the number of fire cases from 124 to almost 900, (2) by using scaled reanalysis-model simulations to fill missing AOD retrievals in the MODIS observations, (3) by distinguishing the BB components of the total aerosol load from background aerosol in the near-source regions, and (4) by including emissions from fires too small to be identified explicitly in the satellite observations. The small-fire emission adjustment shows the complimentary nature of correcting for source strength and adding geographically distinct missing sources. Our analysis indicates that the method works best for fire cases where the BB fraction of total AOD is high, primarily evergreen or deciduous forests. In heavily polluted or agricultural burning regions, where smoke and background AOD values tend to be comparable, this approach encounters large uncertainties, and in some regions, other model- or measurement-related factors might contribute significantly to model-satellite discrepancies. This work sets the stage for a larger study within the Aerosol Comparison between Observations and Models (AeroCOM) multimodel biomass burning experiment. By comparing multiple model results using the refined technique presented here, we aim to separate BB inventory from model-specific contributions to the remaining discrepancies.
A large source of low-volatility secondary organic aerosol
NASA Astrophysics Data System (ADS)
Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B.; Jørgensen, Solvejg; Kjaergaard, Henrik G.; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R.; Wildt, Jürgen; Mentel, Thomas F.
2014-02-01
Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.
A large source of low-volatility secondary organic aerosol.
Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F
2014-02-27
Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.
Geo-Engineering Climate Change with Sulfate Aerosol
NASA Astrophysics Data System (ADS)
Rasch, P. J.; Crutzen, P. J.
2006-12-01
We explore the impact of injecting a precursor of sulfate aerosols into the middle atmosphere where they would act to increase the planetary albedo and thus counter some of the effects of greenhouse gase forcing. We use an atmospheric general circulation model (CAM, the Community Atmosphere Model) coupled to a slab ocean model for this study. Only physical effects are examined, that is we ignore the biogeochemical and chemical implications of changes to greenhouse gases and aerosols, and do not explore the important ethical, legal, and moral issues that are associated with deliberate geo-engineering efforts. The simulations suggest that the sulfate aerosol produced from the SO2 source in the stratosphere is sufficient to counterbalance most of the warming associated with the greenhouse gas forcing. Surface temperatures return to within a few tenths of a degree(K) of present day levels. Sea ice and precipitation distributions are also much closer to their present day values. The polar region surface temperatures remain 1-3 degrees warm in the winter hemisphere than present day values. This study is very preliminary. Only a subset of the relevant effects have been explored. The effect of such an injection of aerosols on middle atmospheric chemistry, and the effect on cirrus clouds are obvious missing components that merit scrutiny. There are probably others that should be considered. The injection of such aerosols cannot help in ameliorating the effects of CO2 changes on ocean PH, or other effects on the biogeochemistry of the earth system.
Missing ozone-induced potential aerosol formation in a suburban deciduous forest
NASA Astrophysics Data System (ADS)
Nakayama, T.; Kuruma, Y.; Matsumi, Y.; Morino, Y.; Sato, K.; Tsurumaru, H.; Ramasamy, S.; Sakamoto, Y.; Kato, S.; Miyazaki, Y.; Mochizuki, T.; Kawamura, K.; Sadanaga, Y.; Nakashima, Y.; Matsuda, K.; Kajii, Y.
2017-12-01
As a new approach to investigating formation processes of secondary organic aerosol (SOA) in the atmosphere, ozone-induced potential aerosol formation was measured in summer at a suburban forest site surrounded by deciduous trees, near Tokyo, Japan. After passage through a reactor containing high concentrations of ozone, increases in total particle volume (average of 1.4 × 109 nm3/cm3, which corresponds to 17% that of pre-existing particles) were observed, especially during daytime. The observed aerosol formations were compared with the results of box model simulations using simultaneously measured concentrations of gaseous and particulate species. According to the model, the relative contributions of isoprene, monoterpene, and aromatic hydrocarbon oxidation to SOA formation in the reactor were 24, 21, and 55%, respectively. However, the model could explain, on average, only ∼40% of the observed particle formation, and large discrepancies between the observations and model were found, especially around noon and in the afternoon when the concentrations of isoprene and oxygenated volatile organic compounds were high. The results suggest a significant contribution of missing (unaccounted-for) SOA formation processes from identified and/or unidentified volatile organic compounds, especially those emitted during daytime. Further efforts should be made to explore and parameterize this missing SOA formation to assist in the improvement of atmospheric chemistry and climate models.
Many recent models underpredict secondary organic aerosol (SOA) particulate matter(PM) concentrations in polluted regions, indicating serious deficiencies in the models' chemical mechanisms and/or missing SOA precursors. Since tropospheric photochemical ozone production is much b...
Williams, Monique; Villarreal, Amanda; Bozhilov, Krassimir; Lin, Sabrina; Talbot, Prue
2013-01-01
Electronic cigarettes (EC) deliver aerosol by heating fluid containing nicotine. Cartomizer EC combine the fluid chamber and heating element in a single unit. Because EC do not burn tobacco, they may be safer than conventional cigarettes. Their use is rapidly increasing worldwide with little prior testing of their aerosol. We tested the hypothesis that EC aerosol contains metals derived from various components in EC. Cartomizer contents and aerosols were analyzed using light and electron microscopy, cytotoxicity testing, x-ray microanalysis, particle counting, and inductively coupled plasma optical emission spectrometry. The filament, a nickel-chromium wire, was coupled to a thicker copper wire coated with silver. The silver coating was sometimes missing. Four tin solder joints attached the wires to each other and coupled the copper/silver wire to the air tube and mouthpiece. All cartomizers had evidence of use before packaging (burn spots on the fibers and electrophoretic movement of fluid in the fibers). Fibers in two cartomizers had green deposits that contained copper. Centrifugation of the fibers produced large pellets containing tin. Tin particles and tin whiskers were identified in cartridge fluid and outer fibers. Cartomizer fluid with tin particles was cytotoxic in assays using human pulmonary fibroblasts. The aerosol contained particles >1 µm comprised of tin, silver, iron, nickel, aluminum, and silicate and nanoparticles (<100 nm) of tin, chromium and nickel. The concentrations of nine of eleven elements in EC aerosol were higher than or equal to the corresponding concentrations in conventional cigarette smoke. Many of the elements identified in EC aerosol are known to cause respiratory distress and disease. The presence of metal and silicate particles in cartomizer aerosol demonstrates the need for improved quality control in EC design and manufacture and studies on how EC aerosol impacts the health of users and bystanders.
A multi-model evaluation of aerosols over South Asia: common problems and possible causes
NASA Astrophysics Data System (ADS)
Pan, X.; Chin, M.; Gautam, R.; Bian, H.; Kim, D.; Colarco, P. R.; Diehl, T. L.; Takemura, T.; Pozzoli, L.; Tsigaridis, K.; Bauer, S.; Bellouin, N.
2015-05-01
Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, water cycle and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions. In this study, the spatio-temporal aerosol distributions over South Asia from seven global aerosol models are evaluated against aerosol retrievals from NASA satellite sensors and ground-based measurements for the period of 2000-2007. Overall, substantial underestimations of aerosol loading over South Asia are found systematically in most model simulations. Averaged over the entire South Asia, the annual mean aerosol optical depth (AOD) is underestimated by a range 15 to 44% across models compared to MISR (Multi-angle Imaging SpectroRadiometer), which is the lowest bound among various satellite AOD retrievals (from MISR, SeaWiFS (Sea-Viewing Wide Field-of-View Sensor), MODIS (Moderate Resolution Imaging Spectroradiometer) Aqua and Terra). In particular during the post-monsoon and wintertime periods (i.e., October-January), when agricultural waste burning and anthropogenic emissions dominate, models fail to capture AOD and aerosol absorption optical depth (AAOD) over the Indo-Gangetic Plain (IGP) compared to ground-based Aerosol Robotic Network (AERONET) sunphotometer measurements. The underestimations of aerosol loading in models generally occur in the lower troposphere (below 2 km) based on the comparisons of aerosol extinction profiles calculated by the models with those from Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data. Furthermore, surface concentrations of all aerosol components (sulfate, nitrate, organic aerosol (OA) and black carbon (BC)) from the models are found much lower than in situ measurements in winter. Several possible causes for these common problems of underestimating aerosols in models during the post-monsoon and wintertime periods are identified: the aerosol hygroscopic growth and formation of secondary inorganic aerosol are suppressed in the models because relative humidity (RH) is biased far too low in the boundary layer and thus foggy conditions are poorly represented in current models, the nitrate aerosol is either missing or inadequately accounted for, and emissions from agricultural waste burning and biofuel usage are too low in the emission inventories. These common problems and possible causes found in multiple models point out directions for future model improvements in this important region.
NASA Astrophysics Data System (ADS)
Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; Abel, S.
2016-12-01
Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for regional and global climate change predictions. Our understanding of aerosol-cloud interactions in the SE Atlantic is severely limited. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We describe first results from various synergistic, international research activities aimed at studying aerosol-cloud interactions in the region: NASA's airborne ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) deployment in August/September of 2016, the DoE's LASIC (Layered Atlantic Smoke Interactions with Clouds) deployment of the ARM Mobile Facility to Ascension Island (June 2016 - October 2017), the ground-based components of CNRS' AEROCLO-sA (Aerosols Clouds and Fog over the west coast of southern Africa), and ongoing regional-scale integrative, process-oriented science efforts as part of SEALS-sA (Sea Earth Atmosphere Linkages Study in southern Africa). We expect to describe experimental setups as well as showcase initial aerosol and cloud property distributions. Furthermore, we discuss the implementation of future activities in these programs in coordination with the UK Met Office's CLARIFY (CLoud-Aerosol-Radiation Interactions and Forcing) experiment in 2017.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Russell, Lynn M.; Somerville, Richard C.J.; Burrows, Susannah
Description of the Project: This project has improved the aerosol formulation in a global climate model by using innovative new field and laboratory observations to develop and implement a novel wind-driven sea ice aerosol flux parameterization. This work fills a critical gap in the understanding of clouds, aerosol, and radiation in polar regions by addressing one of the largest missing particle sources in aerosol-climate modeling. Recent measurements of Arctic organic and inorganic aerosol indicate that the largest source of natural aerosol during the Arctic winter is emitted from crystal structures, known as frost flowers, formed on a newly frozen seamore » ice surface [Shaw et al., 2010]. We have implemented the new parameterization in an updated climate model making it the first capable of investigating how polar natural aerosol-cloud indirect effects relate to this important and previously unrecognized sea ice source. The parameterization is constrained by Arctic ARM in situ cloud and radiation data. The modified climate model has been used to quantify the potential pan-Arctic radiative forcing and aerosol indirect effects due to this missing source. This research supported the work of one postdoc (Li Xu) for two years and contributed to the training and research of an undergraduate student. This research allowed us to establish a collaboration between SIO and PNNL in order to contribute the frost flower parameterization to the new ACME model. One peer-reviewed publications has already resulted from this work, and a manuscript for a second publication has been completed. Additional publications from the PNNL collaboration are expected to follow.« less
NASA Astrophysics Data System (ADS)
Boustead, G.; Blitz, M. A.; Heard, D. E.; Ingham, T.; Stone, D. J.; Whalley, L.
2017-12-01
The hydroxyl radical (OH) is the primary oxidant in the atmosphere with its concentration determining the lifetime of many species and its reaction with volatile organic compounds (VOCs) leading to the production of secondary organic aerosols (SOA) and tropospheric ozone. Nitrous acid (HONO) is an important source of OH as it builds up overnight and is photolysed to form OH in the morning. HONO is also present during the day, with several hundred pptv observed in urban environments. Atmospheric models currently under predict the concentration of HONO observed during the day, indicating a missing source. Heterogeneous reactions on ground and aerosol surfaces are now recognised as potentially important HONO sources. To identify and quantify some of these missing heterogeneous sources, a photo-fragmentation laser induced fluorescence (PF-LIF) instrument has been developed to provide a fast and sensitive measurement of HONO. The PF-LIF instrument detects the OH fragment at 308 nm after the photolysis of HONO at 355 nm. This instrument is coupled to an aerosol flow tube and can be used to measure HONO production from aerosols under illuminated conditions. We will present an overview of the instrument and its development as well as preliminary results including the production of HONO from illuminated TiO2 aerosols.
NASA Astrophysics Data System (ADS)
Calvello, Mariarosaria; Caggiano, Rosa; Esposito, Francesco; Lettino, Antonio; Sabia, Serena; Summa, Vito; Pavese, Giulia
2017-11-01
A short-term intensive multi-instrumental measurement campaign (Integrated Measurements of Aerosol in Agri valley - IMAA) was carried out near the largest European oil and gas pre-treatment plant (Centro Olio Val d'Agri - COVA) in a populated area, where, so far, ample characterization of aerosol loading is missing. As such, between the 2 and 17 July in 2013, using a number of instruments analyses were carried out on physical, chemical, morphological and optical properties of aerosol at this distinctive site, at both ground and over the atmospheric column, including the investigation of the mixing and transformation of particles. The observation of slag silicates with a rough surface texture is consistent with the presence of oil-related activities which represent the only industrial activity in the area. Desulfurization/sulfur liquefaction processes occurring at COVA can explain the peculiar morphology of calcium-sodium-aluminum particles. The common COVA source was associated with high concentrations of sulfur, nickel and zinc, and with significant correlations between zinc-sulfur and zinc-nickel. The Optical Particle Sizer (OPS) data, hygroscopicity and optical properties of atmospheric aerosol are consistent with the typical oil-derived gaseous emissions (e.g. sulfur dioxide and methane) that strongly influence the mixing state of particles and their size distributions. Continuous combustion processes at COVA were found to be responsible for Equivalent Black Carbon (EBC) concentrations from their relevant contribution to the total number of fine particles. The expected significant contribution of WS (water soluble) and BC (Black Carbon) components to the total Aerosol Optical Depth (AOD) are consistent with the results from the radiometric model especially for July 3 and 16.
Kim, Hyun-Ha; Ogata, Atsushi
2011-01-01
This paper presents some experimental data on gas-to-particle conversion of benzene using nonthermal plasma (NTP) technology and discusses the possibility of its technical application in atmospheric chemistry. Aerosol measurement using a differential mobility analyzer (DMA) revealed that the parts of benzene molecules were converted into a nanometer-sized aerosol. Aerosol formation was found to be highly related with the missing part in carbon balance. Scanning electron microscopy analysis showed that the aerosols formed in synthetic humid air are the collection of nanoparticles. The carbonyl band (C=O) was found to be an important chemical constituent in the aerosol. The potential of the NTP as an accelerated test tool in studying secondary organic aerosol (SOA) formation from VOCs will be also addressed. PMID:22163781
A Global Aerosol Model Forecast for the ACE-Asia Field Experiment
NASA Technical Reports Server (NTRS)
Chin, Mian; Ginoux, Paul; Lucchesi, Robert; Huebert, Barry; Weber, Rodney; Anderson, Tad; Masonis, Sarah; Blomquist, Byron; Bandy, Alan; Thornton, Donald
2003-01-01
We present the results of aerosol forecast during the Aerosol Characterization Experiment (ACE-Asia) field experiment in spring 2001, using the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model and the meteorological forecast fields from the Goddard Earth Observing System Data Assimilation System (GEOS DAS). The aerosol model forecast provides direct information on aerosol optical thickness and concentrations, enabling effective flight planning, while feedbacks from measurements constantly evaluate the model, making successful model improvements. We verify the model forecast skill by comparing model predicted total aerosol extinction, dust, sulfate, and SO2 concentrations with those quantities measured by the C-130 aircraft during the ACE-Asia intensive operation period. The GEOS DAS meteorological forecast system shows excellent skills in predicting winds, relative humidity, and temperature for the ACE-Asia experiment area as well as for each individual flight, with skill scores usually above 0.7. The model is also skillful in forecast of pollution aerosols, with most scores above 0.5. The model correctly predicted the dust outbreak events and their trans-Pacific transport, but it constantly missed the high dust concentrations observed in the boundary layer. We attribute this missing dust source to the desertification regions in the Inner Mongolia Province in China, which have developed in recent years but were not included in the model during forecasting. After incorporating the desertification sources, the model is able to reproduce the observed high dust concentrations at low altitudes over the Yellow Sea. Two key elements for a successful aerosol model forecast are correct source locations that determine where the emissions take place, and realistic forecast winds and convection that determine where the aerosols are transported. We demonstrate that our global model can not only account for the large-scale intercontinental transport, but also produce the small-scale spatial and temporal variations that are adequate for aircraft measurements planning.
A randomized, controlled trial of an aerosolized vaccine against measles.
Low, Nicola; Bavdekar, Ashish; Jeyaseelan, Lakshmanan; Hirve, Siddhivinayak; Ramanathan, Kavitha; Andrews, Nicholas J; Shaikh, Naseem; Jadi, Ramesh S; Rajagopal, Arunachalam; Brown, Kevin E; Brown, David; Fink, James B; John, Oommen; Scott, Pippa; Riveros-Balta, A Ximena; Greco, Michel; Dhere, Rajeev; Kulkarni, Prasad S; Henao Restrepo, Ana Maria
2015-04-16
Aerosolized vaccine can be used as a needle-free method of immunization against measles, a disease that remains a major cause of illness and death. Data on the immunogenicity of aerosolized vaccine against measles in children are inconsistent. We conducted an open-label noninferiority trial involving children 9.0 to 11.9 months of age in India who were eligible to receive a first dose of measles vaccine. Children were randomly assigned to receive a single dose of vaccine by means of either aerosol inhalation or a subcutaneous injection. The primary end points were seropositivity for antibodies against measles and adverse events 91 days after vaccination. The noninferiority margin was 5 percentage points. A total of 1001 children were assigned to receive aerosolized vaccine, and 1003 children were assigned to receive subcutaneous vaccine; 1956 of all the children (97.6%) were followed to day 91, but outcome data were missing for 331 children because of thawed specimens. In the per-protocol population, data on 1560 of 2004 children (77.8%) could be evaluated. At day 91, a total of 662 of 775 children (85.4%; 95% confidence interval [CI], 82.5 to 88.0) in the aerosol group, as compared with 743 of 785 children (94.6%; 95% CI, 92.7 to 96.1) in the subcutaneous group, were seropositive, a difference of -9.2 percentage points (95% CI, -12.2 to -6.3). Findings were similar in the full-analysis set (673 of 788 children in the aerosol group [85.4%] and 754 of 796 children in the subcutaneous group [94.7%] were seropositive at day 91, a difference of -9.3 percentage points [95% CI, -12.3 to -6.4]) and after multiple imputation of missing results. No serious adverse events were attributable to measles vaccination. Adverse-event profiles were similar in the two groups. Aerosolized vaccine against measles was immunogenic, but, at the prespecified margin, the aerosolized vaccine was inferior to the subcutaneous vaccine with respect to the rate of seropositivity. (Funded by the Bill and Melinda Gates Foundation; Measles Aerosol Vaccine Project Clinical Trials Registry-India number, CTRI/2009/091/000673.).
Effects of mineral dust on global atmospheric nitrate concentrations
NASA Astrophysics Data System (ADS)
Karydis, V. A.; Tsimpidi, A. P.; Pozzer, A.; Astitha, M.; Lelieveld, J.
2016-02-01
This study assesses the chemical composition and global aerosol load of the major inorganic aerosol components, focusing on mineral dust and aerosol nitrate. The mineral dust aerosol components (i.e., Ca2+, Mg2+, K+, Na+) and their emissions are included in the ECHAM5/MESSy Atmospheric Chemistry model (EMAC). Gas/aerosol partitioning is simulated using the ISORROPIA-II thermodynamic equilibrium model that considers K+, Ca2+, Mg2+, NH4+, Na+, SO42-, NO3-, Cl-, and H2O aerosol components. Emissions of mineral dust are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. Presence of metallic ions can substantially affect the nitrate partitioning into the aerosol phase due to thermodynamic interactions. The model simulates highest fine aerosol nitrate concentration over urban and industrialized areas (1-3 µg m-3), while coarse aerosol nitrate is highest close to deserts (1-4 µg m-3). The influence of mineral dust on nitrate formation extends across southern Europe, western USA, and northeastern China. The tropospheric burden of aerosol nitrate increases by 44 % when considering interactions of nitrate with mineral dust. The calculated global average nitrate aerosol concentration near the surface increases by 36 %, while the coarse- and fine-mode concentrations of nitrate increase by 53 and 21 %, respectively. Other inorganic aerosol components are affected by reactive dust components as well (e.g., the tropospheric burden of chloride increases by 9 %, ammonium decreases by 41 %, and sulfate increases by 7 %). Sensitivity tests show that nitrate aerosol is most sensitive to the chemical composition of the emitted mineral dust, followed by the soil size distribution of dust particles, the magnitude of the mineral dust emissions, and the aerosol state assumption.
Aerosol in the Pacific troposphere
NASA Technical Reports Server (NTRS)
Clarke, Antony D.
1989-01-01
The use of near real-time optical techniques is emphasized for the measurement of mid-tropospheric aerosol over the Central Pacific. The primary focus is on measurement of the aerosol size distribution over the range of particle diameters from 0.15 to 5.0 microns that are essential for modeling CO2 backscatter values in support of the laser atmospheric wind sounder (LAWS) program. The measurement system employs a LAS-X (Laser Aerosol Spectrometer-PMS, Boulder, CO) with a custom 256 channel pulse height analyzer and software for detailed measurement and analysis of aerosol size distributions. A thermal preheater system (Thermo Optic Aerosol Descriminator (TOAD) conditions the aerosol in a manner that allows the discrimination of the size distribution of individual aerosol components such as sulfuric acid, sulfates and refractory species. This allows assessment of the relative contribution of each component to the BCO2 signal. This is necessary since the different components have different sources, exhibit independent variability and provide different BCO2 signals for a given mass and particle size. Field activities involve experiments designed to examine both temporal and spatial variability of these aerosol components from ground based and aircraft platforms.
NASA Astrophysics Data System (ADS)
Rodriguez, E.; Kolmonen, P.; Virtanen, T. H.; Sogacheva, L.; Sundstrom, A.-M.; de Leeuw, G.
2015-08-01
The Advanced Along-Track Scanning Radiometer (AATSR) on board the ENVISAT satellite is used to study aerosol properties. The retrieval of aerosol properties from satellite data is based on the optimized fit of simulated and measured reflectances at the top of the atmosphere (TOA). The simulations are made using a radiative transfer model with a variety of representative aerosol properties. The retrieval process utilizes a combination of four aerosol components, each of which is defined by their (lognormal) size distribution and a complex refractive index: a weakly and a strongly absorbing fine-mode component, coarse mode sea salt aerosol and coarse mode desert dust aerosol). These components are externally mixed to provide the aerosol model which in turn is used to calculate the aerosol optical depth (AOD). In the AATSR aerosol retrieval algorithm, the mixing of these components is decided by minimizing the error function given by the sum of the differences between measured and calculated path radiances at 3-4 wavelengths, where the path radiances are varied by varying the aerosol component mixing ratios. The continuous variation of the fine-mode components allows for the continuous variation of the fine-mode aerosol absorption. Assuming that the correct aerosol model (i.e. the correct mixing fractions of the four components) is selected during the retrieval process, also other aerosol properties could be computed such as the single scattering albedo (SSA). Implications of this assumption regarding the ratio of the weakly/strongly absorbing fine-mode fraction are investigated in this paper by evaluating the validity of the SSA thus obtained. The SSA is indirectly estimated for aerosol plumes with moderate-to-high AOD resulting from wildfires in Russia in the summer of 2010. Together with the AOD, the SSA provides the aerosol absorbing optical depth (AAOD). The results are compared with AERONET data, i.e. AOD level 2.0 and SSA and AAOD inversion products. The RMSE (root mean square error) is 0.03 for SSA and 0.02 for AAOD lower than 0.05. The SSA is further evaluated by comparison with the SSA retrieved from the Ozone Monitoring Instrument (OMI). The SSA retrieved from both instruments show similar features, with generally lower AATSR-estimated SSA values over areas affected by wildfires.
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.
Aerosol loading in the Southeastern United States: reconciling surface and satellite observations
NASA Astrophysics Data System (ADS)
Ford, B.; Heald, C. L.
2013-04-01
We investigate the seasonality in aerosols over the Southeastern United States using observations from several satellite instruments (MODIS, MISR, CALIOP) and surface network sites (IMPROVE, SEARCH, AERONET). We find that the strong summertime enhancement in satellite-observed aerosol optical depth (factor 2-3 enhancement over wintertime AOD) is not present in surface mass concentrations (25-55% summertime enhancement). Goldstein et al. (2009) previously attributed this seasonality in AOD to biogenic organic aerosol; however, surface observations show that organic aerosol only accounts for ~35% of PM2.5 mass and exhibits similar seasonality to total PM2.5. The GEOS-Chem model generally reproduces these surface aerosol measurements, but under represents the AOD seasonality observed by satellites. We show that seasonal differences in water uptake cannot sufficiently explain the magnitude of AOD increase. As CALIOP profiles indicate the presence of additional aerosol in the lower troposphere (below 700 hPa), which cannot be explained by vertical mixing; we conclude that the discrepancy is due to a missing source of aerosols above the surface in summer.
NASA Astrophysics Data System (ADS)
Zhang, Ying; Li, Zhengqiang; Sun, Yele; Lv, Yang; Xie, Yisong
2018-04-01
Aerosols have adverse effects on human health and air quality, changing Earth's energy balance and lead to climate change. The components of aerosol are important because of the different spectral characteristics. Based on the low hygroscopic and high scattering properties of organic matter (OM) in fine modal atmospheric aerosols, we develop an inversion algorithm using remote sensing to obtain aerosol components including black carbon (BC), organic matter (OM), ammonium nitrate-like (AN), dust-like (DU) components and aerosol water content (AW). In the algorithm, the microphysical characteristics (i.e. volume distribution and complex refractive index) of particulates are preliminarily separated to fine and coarse modes, and then aerosol components are retrieved using bimodal parameters. We execute the algorithm using remote sensing measurements of sun-sky radiometer at AERONET site (Beijing RADI) in a period from October of 2014 to January of 2015. The results show a reasonable distribution of aerosol components and a good fit for spectral feature calculations. The mean OM mass concentration in atmospheric column is account for 14.93% of the total and 56.34% of dry and fine-mode aerosol, being a fairly good correlation (R = 0.56) with the in situ observations near the surface layer.
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.
NASA Astrophysics Data System (ADS)
Nishizawa, Tomoaki; Sugimoto, Nobuo; Shimizu, Atsushi; Uno, Itsushi; Hara, Yukari; Kudo, Rei
2018-04-01
We deployed multi-wavelength Mie-Raman lidars (MMRL) at three sites of the AD-Net and have conducted continuous measurements using them since 2013. To analyze the MMRL data and better understand the externally mixing state of main aerosol components (e.g., dust, sea-salt, and black carbon) in the atmosphere, we developed an integrated package of aerosol component retrieval algorithms, which have already been developed or are being developed, to estimate vertical profiles of the aerosol components. This package applies to the other ground-based lidar network data (e.g., EARLINET) and satellite-borne lidar data (e.g., CALIOP/CALIPSO and ATLID/EarthCARE) as well as the other lidar data of the AD-Net.
Host Model Uncertainty in Aerosol Radiative Effects: the AeroCom Prescribed Experiment and Beyond
NASA Astrophysics Data System (ADS)
Stier, Philip; Schutgens, Nick; Bian, Huisheng; Boucher, Olivier; Chin, Mian; Ghan, Steven; Huneeus, Nicolas; Kinne, Stefan; Lin, Guangxing; Myhre, Gunnar; Penner, Joyce; Randles, Cynthia; Samset, Bjorn; Schulz, Michael; Yu, Hongbin; Zhou, Cheng; Bellouin, Nicolas; Ma, Xiaoyan; Yu, Fangqun; Takemura, Toshihiko
2013-04-01
Anthropogenic and natural aerosol radiative effects are recognized to affect global and regional climate. Multi-model "diversity" in estimates of the aerosol radiative effect is often perceived as a measure of the uncertainty in modelling aerosol itself. However, current aerosol models vary considerably in model components relevant for the calculation of aerosol radiative forcings and feedbacks and the associated "host-model uncertainties" are generally convoluted with the actual uncertainty in aerosol modelling. In the AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in eleven participating models. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention. However, uncertainties in aerosol radiative effects also include short-term and long-term feedback processes that will be systematically explored in future intercomparison studies. Here we will present an overview of the proposals for discussion and results from early scoping studies.
NASA Astrophysics Data System (ADS)
Córdoba-Jabonero, Carmen; Sicard, Michaël; Ansmann, Albert; Águila, Ana del; Baars, Holger
2018-04-01
POLIPHON (POlarization-LIdar PHOtometer Networking) retrieval consists in the vertical separation of two/three particle components in aerosol mixtures, highlighting their relative contributions in terms of the optical properties and mass concentrations. This method is based on the specific particle linear depolarization ratio given for different types of aerosols, and is applied to the new polarized Micro-Pulse Lidar (P-MPL). Case studies of specific climate-relevant aerosols (dust particles, fire smoke, and pollen aerosols, including a clean case as reference) observed over Barcelona (Spain) are presented in order to evaluate firstly the potential of P-MPLs measurements in combination with POLIPHON for retrieving the vertical separation of those particle components forming aerosol mixtures and their properties.
What is the "Clim-Likely" aerosol product?
Atmospheric Science Data Center
2014-12-08
... identifying a range of components and mixtures for the MISR Standard Aerosol Retrieval Algorithm climatology, and as one standard against ... retrieval results. Six component aerosols included in the model were medium and coarse mode mineral dust, sulfate, sea salt, black ...
Aerosol loading in the Southeastern United States: reconciling surface and satellite observations
NASA Astrophysics Data System (ADS)
Ford, B.; Heald, C. L.
2013-09-01
We investigate the seasonality in aerosols over the Southeastern United States using observations from several satellite instruments (MODIS, MISR, CALIOP) and surface network sites (IMPROVE, SEARCH, AERONET). We find that the strong summertime enhancement in satellite-observed aerosol optical depth (AOD) (factor 2-3 enhancement over wintertime AOD) is not present in surface mass concentrations (25-55% summertime enhancement). Goldstein et al. (2009) previously attributed this seasonality in AOD to biogenic organic aerosol; however, surface observations show that organic aerosol only accounts for ∼35% of fine particulate matter (smaller than 2.5 μm in aerodynamic diameter, PM2.5) and exhibits similar seasonality to total surface PM2.5. The GEOS-Chem model generally reproduces these surface aerosol measurements, but underrepresents the AOD seasonality observed by satellites. We show that seasonal differences in water uptake cannot sufficiently explain the magnitude of AOD increase. As CALIOP profiles indicate the presence of additional aerosol in the lower troposphere (below 700 hPa), which cannot be explained by vertical mixing, we conclude that the discrepancy is due to a missing source of aerosols above the surface layer in summer.
NASA Technical Reports Server (NTRS)
Remer, L. A.; Kaufman, Y. J.
2006-01-01
A four year record of MODIS spaceborne data provides a new measurement tool to assess the aerosol direct radiative effect at the top of the atmosphere. MODIS derives the aerosol optical thickness and microphysical properties from the scattered sunlight at 0.55-2.1 microns. The monthly MODIS data used here are accumulated measurements across a wide range of view and scattering angles and represent the aerosol s spectrally resolved angular properties. We use these data consistently to compute with estimated accuracy of +/-0.6W/sq m the reflected sunlight by the aerosol over global oceans in cloud free conditions. The MODIS high spatial resolution (0.5 km) allows observation of the aerosol impact between clouds that can be missed by other sensors with larger footprints. We found that over the clear-sky global ocean the aerosol reflected 5.3+/-0.6W/sq m with an average radiative efficiency of 49+/-2W/sq m per unit optical thickness. The seasonal and regional distribution of the aerosol radiative effects are discussed. The analysis adds a new measurement perspective to a climate change problem dominated so far by models.
The GRAPE aerosol retrieval algorithm
NASA Astrophysics Data System (ADS)
Thomas, G. E.; Poulsen, C. A.; Sayer, A. M.; Marsh, S. H.; Dean, S. M.; Carboni, E.; Siddans, R.; Grainger, R. G.; Lawrence, B. N.
2009-11-01
The aerosol component of the Oxford-Rutherford Aerosol and Cloud (ORAC) combined cloud and aerosol retrieval scheme is described and the theoretical performance of the algorithm is analysed. ORAC is an optimal estimation retrieval scheme for deriving cloud and aerosol properties from measurements made by imaging satellite radiometers and, when applied to cloud free radiances, provides estimates of aerosol optical depth at a wavelength of 550 nm, aerosol effective radius and surface reflectance at 550 nm. The aerosol retrieval component of ORAC has several incarnations - this paper addresses the version which operates in conjunction with the cloud retrieval component of ORAC (described by Watts et al., 1998), as applied in producing the Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) data-set. The algorithm is described in detail and its performance examined. This includes a discussion of errors resulting from the formulation of the forward model, sensitivity of the retrieval to the measurements and a priori constraints, and errors resulting from assumptions made about the atmospheric/surface state.
The GRAPE aerosol retrieval algorithm
NASA Astrophysics Data System (ADS)
Thomas, G. E.; Poulsen, C. A.; Sayer, A. M.; Marsh, S. H.; Dean, S. M.; Carboni, E.; Siddans, R.; Grainger, R. G.; Lawrence, B. N.
2009-04-01
The aerosol component of the Oxford-Rutherford Aerosol and Cloud (ORAC) combined cloud and aerosol retrieval scheme is described and the theoretical performance of the algorithm is analysed. ORAC is an optimal estimation retrieval scheme for deriving cloud and aerosol properties from measurements made by imaging satellite radiometers and, when applied to cloud free radiances, provides estimates of aerosol optical depth at a wavelength of 550 nm, aerosol effective radius and surface reflectance at 550 nm. The aerosol retrieval component of ORAC has several incarnations - this paper addresses the version which operates in conjunction with the cloud retrieval component of ORAC (described by Watts et al., 1998), as applied in producing the Global Retrieval of ATSR Cloud Parameters and Evaluation (GRAPE) data-set. The algorithm is described in detail and its performance examined. This includes a discussion of errors resulting from the formulation of the forward model, sensitivity of the retrieval to the measurements and a priori constraints, and errors resulting from assumptions made about the atmospheric/surface state.
Estimate of the Aerosol Anthropogenic Component and Focusing from Satellite Data
NASA Technical Reports Server (NTRS)
Kaufman, Yoram; Remer, Lorraine A.; Chin, Mian
2004-01-01
Satellite measurements of aerosol do not contain information on the chemical composition needed to resolve anthropogenic vs. natural aerosol components. Besides, the same chemical species can have natural and anthropogenic origins. However the ability of the new satellite instruments (MODIS, MISR, POLDER) to distinguish fine from coarse aerosols over the oceans, can be used as a signature of the presence of anthropogenic component and used to measure the fraction of the aerosol originating from anthropogenic activity with an uncertainty of 10 percent for aerosol optical thickness larger than 0.1. We develop the methods and investigated it using model calculations (GOCART) and satellite data (MODIS). Preliminary application to 2 years of global MODIS data shows that 0.200.08 of the aerosol optical thickness and radiative effect has anthropogenic origin. The resultant aerosol forcing over cloud free oceans is 1.30.6 W/sq m, larger than model simulations. Further research until the presentation will probably modify these values.
MODELS-3 COMMUNITY MULTISCALE AIR QUALITY (CMAQ) MODEL AEROSOL COMPONENT 1: MODEL DESCRIPTION
The aerosol component of the Community Multiscale Air Quality (CMAQ) model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdis...
Chatterjee, Abhijit; Ghosh, Sanjay K; Adak, Anandamay; Singh, Ajay K; Devara, Panuganti C S; Raha, Sibaji
2012-01-01
The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca(2+)) during pre-monsoon (Apr-May) which was higher by 162% than its annual mean whereas during winter (Dec-Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO(4)(2-) and black carbon) were higher (76% for black carbon and 96% for fine mode SO(4)(2-)) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas.
Aerosol composition and source apportionment in Santiago de Chile
NASA Astrophysics Data System (ADS)
Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto
1999-04-01
Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (2
NASA Technical Reports Server (NTRS)
Gordon, Keith; Rutherford, Gugu; Aranda, Denisse
2017-01-01
Nonvolatile residue (NVR), sometimes referred to as molecular contamination is the term used for the total composition of the inorganic and high boiling point organic components in particulates and molecular films deposited on critical surfaces surrounding space structures, with the particulate and NVR contamination originating primarily from pre-launch operations. The "nonvolatile" suggestion from the terminology NVR implies that the collected residue will not experience much loss under ambient conditions. NVR has been shown to have a dramatic impact on the ability to perform optical measurements from platforms based in space. Such contaminants can be detected early by the controlled application of various detection techniques and contamination analyses. Contamination analyses are the techniques used to determine if materials, components, and subsystems can be expected to meet the performance requirements of a system. Of particular concern is the quantity of NVR contaminants that might be deposited on critical payload surfaces from these sources. Subsequent chemical analysis of the contaminant samples by infrared spectroscopy and gas chromatography mass spectrometry identifies the components, gives semi-quantitative estimates of contaminant thickness, indicates possible sources of the NVR, and provides guidance for effective cleanup procedures. In this report, a method for the collection and determination of the mass of NVR was generated by the authors at NASA Langley Research Center. This report describes the method developed and implemented for collecting NVR contaminants, and procedures for gravimetric and chemical analysis of the residue obtained. The result of this NVR analysis collaboration will help pave the way for Langley's ability to certify flight hardware outgassing requirements in support of flight projects such as Stratospheric Aerosol and Gas Experiment III (SAGE III), Clouds and the Earth's Radiant Energy System (CERES), Materials International Space Station Experiment - X (MISSE-X), and Doppler Aerosol Wind Lidar (DAWN).
NASA Technical Reports Server (NTRS)
Welton, Ellsworth; Spinhirne, James D.; Palm, Steven P.; Hlavka, Dennis; Hart, William
2003-01-01
On January 12, 2003 NASA launched the first satellite-based lidar, the Geoscience Laser -Altimeter System (GLAS), onboard the ICESat spacecraft. The GLAS atmospheric measurements introduce a fundamentally new and important tool for understanding the atmosphere and climate. In the past, aerosols have only been studied from space using images gathered by passive sensors. Analysis of this passive data has lead to an improved understanding of aerosol properties, spatial distribution, and their effect on the earth's climate. However, these images do not show the aerosol's vertical distribution. As a result, a key piece of information has been missing. The measurements now obtained by GLAS will provide information on the vertical distribution of aerosols and clouds, and improve our ability to study their transport processes and aerosol-cloud interactions. Here we show an overview of GLAS, provide an update of its current status, and present initial observations of dust profiles. In particular, a strategy of characterizing the height profile of dust plumes over source regions will be presented.
NASA Astrophysics Data System (ADS)
Pfrang, C.; Shiraiwa, M.; Pöschl, U.
2011-04-01
Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles representative of atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant time scales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.
NASA Astrophysics Data System (ADS)
Pfrang, C.; Shiraiwa, M.; Pöschl, U.
2011-07-01
Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.
Single Aerosol Particle Studies Using Optical Trapping Raman And Cavity Ringdown Spectroscopy
NASA Astrophysics Data System (ADS)
Gong, Z.; Wang, C.; Pan, Y. L.; Videen, G.
2017-12-01
Due to the physical and chemical complexity of aerosol particles and the interdisciplinary nature of aerosol science that involves physics, chemistry, and biology, our knowledge of aerosol particles is rather incomplete; our current understanding of aerosol particles is limited by averaged (over size, composition, shape, and orientation) and/or ensemble (over time, size, and multi-particles) measurements. Physically, single aerosol particles are the fundamental units of any large aerosol ensembles. Chemically, single aerosol particles carry individual chemical components (properties and constituents) in particle ensemble processes. Therefore, the study of single aerosol particles can bridge the gap between aerosol ensembles and bulk/surface properties and provide a hierarchical progression from a simple benchmark single-component system to a mixed-phase multicomponent system. A single aerosol particle can be an effective reactor to study heterogeneous surface chemistry in multiple phases. Latest technological advances provide exciting new opportunities to study single aerosol particles and to further develop single aerosol particle instrumentation. We present updates on our recent studies of single aerosol particles optically trapped in air using the optical-trapping Raman and cavity ringdown spectroscopy.
Missing Peroxy Radical Sources within a Summertime Ponderosa Pine Forest
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wolfe, G. M.; Cantrell, Chris; Kim, S.
2014-05-13
Organic peroxy (RO2) and hydroperoxy (HO2) radicals are key intermediates in the photochemical processes that generate ozone, secondary organic aerosol and reactive nitrogen reservoirs throughout the troposphere. In regions with ample biogenic hydrocarbons, the richness and complexity of peroxy radical chemistry presents a significant challenge to current-generation models, especially given the scarcity of measurements in such environments. We present peroxy radical observations acquired within a Ponderosa pine forest during the summer 2010 Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen – Rocky Mountain Organic Carbon Study (BEACHON-ROCS). Total peroxy radical mixing ratios reach as high as 180 pptvmore » and are among the highest yet recorded. Using the comprehensive measurement suite to constrain a near-explicit 0-D box model, we investigate the sources, sinks and distribution of peroxy radicals below the forest canopy. The base chemical mechanism underestimates total peroxy radicals by as much as a factor of 3. Peroxy radical sinks are unlikely to be overestimated, suggesting missing sources. A close comparison of model results with observations reveals at least two distinct source signatures. The first missing source, characterized by a sharp midday maximum and a strong dependence on solar radiation, is consistent with photolytic production of HO2. The diel profile of the second missing source peaks in the afternoon and suggests a process that generates RO2 independently of sun-driven photochemistry, such as ozonolysis of reactive hydrocarbons. The maximum magnitudes of these missing sources (~120 and 50 pptv min-1, respectively) are consistent with previous observations alluding to unexpectedly intense oxidation within the forest, and we conclude that a similar mechanism may underlie many such anomalous findings.« less
Missing Peroxy Radical Sources Within a Rural Forest Canopy
NASA Technical Reports Server (NTRS)
Wolfe, G. M.; Cantrell, C.; Kim, S.; Mauldin, R. L., III; Karl, T.; Harley, P.; Turnipseed, A.; Zheng, W.; Flocke, F.; Apel, E. C.;
2013-01-01
Organic peroxy (RO2) and hydroperoxy (HO2) radicals are key intermediates in the photochemical processes that generate ozone, secondary organic aerosol and reactive nitrogen reservoirs throughout the troposphere. In regions with ample biogenic hydrocarbons, the richness and complexity of peroxy radical chemistry presents a significant challenge to current-generation models, especially given the scarcity of measurements in such environments. We present peroxy radical observations acquired within a Ponderosa pine forest during the summer 2010 Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen - Rocky Mountain Organic Carbon Study (BEACHON-ROCS). Total peroxy radical mixing ratios reach as high as 180 pptv and are among the highest yet recorded. Using the comprehensive measurement suite to constrain a near-explicit 0-D box model, we investigate the sources, sinks and distribution of peroxy radicals below the forest canopy. The base chemical mechanism underestimates total peroxy radicals by as much as a factor of 3. Since primary reaction partners for peroxy radicals are either measured (NO) or under-predicted (HO2 and RO2, i.e. self-reaction), missing sources are the most likely explanation for this result. A close comparison of model output with observations reveals at least two distinct source signatures. The first missing source, characterized by a sharp midday maximum and a strong dependence on solar radiation, is consistent with photolytic production of HO2. The diel profile of the second missing source peaks in the afternoon and suggests a process that generates RO2 independently of sun-driven photochemistry, such as ozonolysis of reactive hydrocarbons. The maximum magnitudes of these missing sources (approximately 120 and 50 pptv min-1, respectively) are consistent with previous observations alluding to unexpectedly intense oxidation within forests. We conclude that a similar mechanism may underlie many such observations.
Heterogeneous Production of Sulfate Aerosol over China.
NASA Astrophysics Data System (ADS)
Shao, J.; Alexander, B.; Chen, Q.; Zhang, L.; Wang, Y.; Xie, Z.; He, P.
2017-12-01
Sulfate is thought to be the main contributor to the growth of PM2.5 during the severe haze pollution over China, but most studies have shown that traditional gas- and aqueous-phase chemistry cannot explain the rapid sulfate production during haze events, suggesting a missing heterogeneous oxidation mechanism. In this work, we implement heterogeneous sulfate formation into a 3-D global chemical transport model (GEOS-Chem) to evaluate the different pathways for global and regional sulfate production, including SO2 oxidation by NO2, O3, H2O2, and TMI+O2. Heterogeneous sulfate production rates and the dominant heterogeneous sulfate formation mechanism depends on calculations of aerosol pH, which is in turn is dependent upon thermodynamic state assumptions. We evaluate the influence of aerosol pH and potential impacts of aerosol ionic strength on sulfate production rates and mechanisms in the model, and its implications for PM2.5 in Chinese haze events.
What We Can Say About the Roles of Natural and Anthropogenic Aerosols in Climate Change
NASA Astrophysics Data System (ADS)
Kahn, Ralph
2016-07-01
Although particles from natural sources dominate the globally averaged aerosol load, it is widely understood that human activity has added significantly to the atmospheric aerosol inventory in many regions. Anthropogenic contributions include pollution particles from industrial activity, transportation, cook-stoves, and other combustion sources, smoke from agricultural fires and those wildfires that result from land-management practices, soil and mineral dust mobilized in regions where overgrazing, severe tilling, or overuse of surface water resources have occurred, and biogenic particles from vegetation planted and maintained by the populance. The history of human influence is complex - in the 18th and 19th centuries agricultural burning tended to dominate the anthropogenic component in most places, whereas more recently, fossil fuel combustion leads the human contribution is many areas. However, identifying and quantifying the anthropogenic aerosol component on global scales is a challenging endeavor at present. Most estimates of the anthropogenic component come from aerosol transport models that are initialized with aerosol and precursor-gas source locations, emission strengths, and injection heights. The aerosol is then advected based on meteorological modeling, possibly modified chemically or physically, and removed by parameterized wet or dry deposition processes. Aerosol effects on clouds are also represented in some climate models, but with even greater uncertainty than the direct aerosol effects on Earth's radiation balance. Even for present conditions, aerosol source inventories are deduced from whatever constraints can be found, along with much creativity and many assumptions. Aerosol amount (i.e., aerosol optical depth) is routinely measured globally from space, but observational constraints on the anthropogenic component require some knowledge of the aerosol type as well, a much more difficult quantity to derive. As large-swath, multi-spectral, single-view instruments such as MODIS can provide some information about fine-mode vs. coarse-mode dominated aerosol over dark water, early efforts to constrain aerosol type assumed that some or all the fine-mode fraction is anthropogenic. However, this information is not sufficient to make the key anthropogenic vs. natural distinction in most places where the likely answer is not already known. Instruments providing more detailed measurements, such as multi-spectral, multi-angle and polarimetric imagers and multi-channel lidars, can offer tighter aerosol-type constraints in some circumstances, though generally not enough to specifically identify anthropogenic aerosols. The best we seem to be able to do with current data is to combine satellite and suborbital observations with models. And for the "pre-industrial" period, the analogy is usually made to the "natural" component of present-day aerosol, although there are ambiguities in our ability to distinguish natural from anthropogenic particles on regional-to-global scales, and the natural component itself might have changed over time. This talk will review where we stand, and what might be possible to say in the future.
Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM)
NASA Astrophysics Data System (ADS)
Mills, Michael J.; Schmidt, Anja; Easter, Richard; Solomon, Susan; Kinnison, Douglas E.; Ghan, Steven J.; Neely, Ryan R.; Marsh, Daniel R.; Conley, Andrew; Bardeen, Charles G.; Gettelman, Andrew
2016-03-01
Accurate representation of global stratospheric aerosols from volcanic and nonvolcanic sulfur emissions is key to understanding the cooling effects and ozone losses that may be linked to volcanic activity. Attribution of climate variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the rate of global average temperature increases. We have compiled a database of volcanic SO2 emissions and plume altitudes for eruptions from 1990 to 2014 and developed a new prognostic capability for simulating stratospheric sulfate aerosols in the Community Earth System Model. We used these combined with other nonvolcanic emissions of sulfur sources to reconstruct global aerosol properties from 1990 to 2014. Our calculations show remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD) and with in situ measurements of stratospheric aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD calculations represent a clear improvement over available satellite-based analyses, which generally ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at middle and high latitudes. Our SAD calculations greatly improve on that provided for the Chemistry-Climate Model Initiative, which misses about 60% of the SAD measured in situ on average during both volcanically active and volcanically quiescent periods.
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.
NASA Technical Reports Server (NTRS)
Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.
2004-01-01
During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic matter, and dust found for the ACE Asia aerosol are comparable to values estimated for ACE 1, Aerosols99, and INDOEX. Unique to the ACE Asia aerosol was the large mass fractions of dust, the dominance of dust in controlling the aerosol optical properties, and the interaction of dust with soot aerosol.
NASA Astrophysics Data System (ADS)
Voitsekhovskaya, O. K.; Egorov, O. V.; Kashirskii, D. E.; Shefer, O. V.
2015-11-01
Calculated absorption spectra of the mixture of gases (H2O, CO, CO2, NO, NO2, and SO2) and aerosol (soot and Al2O3), contained in the exhausts of aircraft and rocket engines are demonstrated. Based on the model of gas-aerosol medium, a numerical study of the spectral dependence of the absorptance for different ratios of gas and aerosol components was carried out. The influence of microphysical and optical properties of the components of the mixture on the spectral features of absorption of gas-aerosol medium was established.
Chatterjee, Abhijit; Ghosh, Sanjay K.; Adak, Anandamay; Singh, Ajay K.; Devara, Panuganti C. S.; Raha, Sibaji
2012-01-01
Background The loading of atmospheric particulate matter (aerosol) in the eastern Himalaya is mainly regulated by the locally generated anthropogenic aerosols from the biomass burning and by the aerosols transported from the distance sources. These different types of aerosol loading not only affect the aerosol chemistry but also produce consequent signature on the radiative properties of aerosol. Methodology/Principal Findings An extensive study has been made to study the seasonal variations in aerosol components of fine and coarse mode aerosols and black carbon along with the simultaneous measurements of aerosol optical depth on clear sky days over Darjeeling, a high altitude station (2200 masl) at eastern Himalayas during the year 2008. We observed a heavy loading of fine mode dust component (Ca2+) during pre-monsoon (Apr – May) which was higher by 162% than its annual mean whereas during winter (Dec – Feb), the loading of anthropogenic aerosol components mainly from biomass burning (fine mode SO4 2− and black carbon) were higher (76% for black carbon and 96% for fine mode SO4 2−) from their annual means. These high increases in dust aerosols during pre-monsoon and anthropogenic aerosols during winter enhanced the aerosol optical depth by 25 and 40%, respectively. We observed that for every 1% increase in anthropogenic aerosols, AOD increased by 0.55% during winter whereas for every 1% increase in dust aerosols, AOD increased by 0.46% during pre-monsoon. Conclusion/Significance The natural dust transport process (during pre-monsoon) plays as important a role in the radiation effects as the anthropogenic biomass burning (during winter) and their differential effects (rate of increase of the AOD with that of the aerosol concentration) are also very similar. This should be taken into account in proper modeling of the atmospheric environment over eastern Himalayas. PMID:22792264
The Carbonaceous Aerosols and Radiative Effects Study (CARES), a field campaign held in central California in June 2010, provides a unique opportunity to assess the aerosol optics modeling component of the two-way coupled Weather Research and Forecasting (WRF) – Community Multisc...
Detecting Thin Cirrus in Multiangle Imaging Spectroradiometer Aerosol Retrievals
NASA Technical Reports Server (NTRS)
Pierce, Jeffrey R.; Kahn, Ralph A.; Davis, Matt R.; Comstock, Jennifer M.
2010-01-01
Thin cirrus clouds (optical depth (OD) < 03) are often undetected by standard cloud masking in satellite aerosol retrieval algorithms. However, the Mu]tiangle Imaging Spectroradiometer (MISR) aerosol retrieval has the potential to discriminate between the scattering phase functions of cirrus and aerosols, thus separating these components. Theoretical tests show that MISR is sensitive to cirrus OD within Max{0.05 1 20%l, similar to MISR's sensitivity to aerosol OD, and MISR can distinguish between small and large crystals, even at low latitudes, where the range of scattering angles observed by MISR is smallest. Including just two cirrus components in the aerosol retrieval algorithm would capture typical MISR sensitivity to the natural range of cinus properties; in situations where cirrus is present but the retrieval comparison space lacks these components, the retrieval tends to underestimate OD. Generally, MISR can also distinguish between cirrus and common aerosol types when the proper cirrus and aerosol optical models are included in the retrieval comparison space and total column OD is >-0.2. However, in some cases, especially at low latitudes, cirrus can be mistaken for some combinations of dust and large nonabsorbing spherical aerosols, raising a caution about retrievals in dusty marine regions when cirrus is present. Comparisons of MISR with lidar and Aerosol Robotic Network show good agreement in a majority of the cases, but situations where cirrus clouds have optical depths >0.15 and are horizontally inhomogeneous on spatial scales shorter than 50 km pose difficulties for cirrus retrieval using the MISR standard aerosol algorithm..
NASA Astrophysics Data System (ADS)
Cerully, K. M.; Bougiatioti, A.; Hite, J. R., Jr.; Guo, H.; Xu, L.; Ng, N. L.; Weber, R.; Nenes, A.
2014-12-01
The formation of secondary organic aerosol (SOA) combined with the partitioning of semi-volatile organic components can impact numerous aerosol properties including cloud condensation nuclei (CCN) activity, hygroscopicity and volatility. During the summer 2013 Southern Oxidant and Aerosol Study (SOAS) field campaign in a rural site in the Southeastern United States, a suite of instruments including a CCN counter, a thermodenuder (TD) and a high resolution time-of-flight aerosol mass spectrometer (AMS) were used to measure CCN activity, aerosol volatility, composition and oxidation state. Particles were either sampled directly from ambient or through a Particle Into Liquid Sampler (PILS), allowing the investigation of the water-soluble aerosol component. Ambient aerosol exhibited size-dependent composition with larger particles being more hygroscopic. The hygroscopicity of thermally-denuded aerosol was similar between ambient and PILS-generated aerosol and showed limited dependence on volatilization. Results of AMS 3-factor Positive Matrix Factorization (PMF) analysis for the PILS-generated aerosol showed that the most hygroscopic components are most likely the most and the least volatile features of the aerosol. No clear relationship was found between organic hygroscopicity and oxygen-to-carbon ratio; in fact, Isoprene organic aerosol (Isoprene-OA) was found to be the most hygroscopic factor, while at the same time being the least oxidized and likely most volatile of all PMF factors. Considering the diurnal variation of each PMF factor and its associated hygroscopicity, Isoprene-OA and More Oxidized - Oxidized Oxygenated Organic Aerosol (MO-OOA) are the prime contributors to hygroscopicity and covary with Less Oxidized - Oxidized Oxygenated Organic Aerosol (LO-OOA) in a way that induces the observed diurnal invariance in total organic hygroscopicity. Biomass Burning Organic Aerosol (BBOA) contributed little to aerosol hygroscopicity, which is expected since there was little biomass burning activity during the sampling period examined.
Reactive intermediates revealed in secondary organic aerosol formation from isoprene
Surratt, Jason D.; Chan, Arthur W. H.; Eddingsaas, Nathan C.; Chan, ManNin; Loza, Christine L.; Kwan, Alan J.; Hersey, Scott P.; Flagan, Richard C.; Wennberg, Paul O.; Seinfeld, John H.
2010-01-01
Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ-IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NOx conditions, respectively. Isoprene low-NOx SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NOx conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NOx SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO2 and NO2, respectively) could be a substantial source of “missing urban SOA” not included in current atmospheric models. PMID:20080572
Direct radiative effect by multicomponent aerosol over China
DOE Office of Scientific and Technical Information (OSTI.GOV)
Huang, Xin; Song, Yu; Zhao, Chun
The direct radiative effect (DRE) of multiple aerosol species (sulfate, nitrate, ammonium, black carbon (BC), organic carbon (OC), and mineral aerosol) and their spatiotemporal variations over China were investigated using a fully coupled meteorology–chemistry model (WRF-Chem) for the entire year of 2006. We made modifications to improve model performance, including updating land surface parameters, improving the calculation of transition metal-catalyzed oxidation of SO 2, and adding in heterogeneous reactions between mineral aerosol and acid gases. The modified model well reproduced the magnitude, seasonal pattern, and spatial distribution of the measured meteorological conditions, concentrations of PM 10 and its components, andmore » aerosol optical depth (AOD). A diagnostic iteration method was used to estimate the overall DRE of aerosols and contributions from different components. At the land surface, all kinds of aerosol species reduced the incident net radiation flux with a total DRE of 10.2 W m -2 over China. Aerosols significantly warm the atmosphere with the national mean DRE of +10.8 W m -2. BC was the leading radiative-heating component (+8.7 W m -2), followed by mineral aerosol (+1.1 W m -2). At the top of the atmosphere (TOA), BC introduced the largest radiative perturbation (+4.5 W m -2), followed by sulfate (-1.4 W m -2). The overall perturbation of aerosols on radiation transfer is quite small over China, demonstrating the counterbalancing effect between scattering and adsorbing aerosols. Aerosol DRE at the TOA had distinct seasonality, generally with a summer maximum and winter minimum, mainly determined by mass loadings, hygroscopic growth, and incident radiation flux.« less
The Detroit Exposure and Aerosol Research Study (DEARS) measured personal exposures, ambient, residential indoor and residential outdoor concentrations of select PM2.5 aerosol components (SO4, NO3, Fe, Si, Ca, K, Mn, Pb, Zn, EC and OC) over a thr...
NASA Technical Reports Server (NTRS)
Hung, R. J.; Liaw, G. S.
1980-01-01
The effects of multi-disperse distribution of the aerosol population are presented. Single component and multi-component aerosol species on the condensation/nucleation processes which affect the reduction in visibility are described. The aerosol population with a high particle concentration provided more favorable conditions for the formation of a denser fog than the aerosol population with a greater particle size distribution when the value of the mass concentration of the aerosols was kept constant. The results were used as numerical predictions of fog formation. Two dimensional observations in horizontal and vertical coordinates, together with time-dependent measurements were needed as initial values for the following physical parameters: (1)wind profiles; (2) temperature profiles; (3) humidity profiles; (4) mass concentration of aerosol particles; (5) particle size distribution of aerosols; and (6) chemical composition of aerosols. Formation and dissipation of advection fog, thus, can be forecasted numerically by introducing initial values obtained from the observations.
Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols.
Jacobson, M Z
2001-02-08
Aerosols affect the Earth's temperature and climate by altering the radiative properties of the atmosphere. A large positive component of this radiative forcing from aerosols is due to black carbon--soot--that is released from the burning of fossil fuel and biomass, and, to a lesser extent, natural fires, but the exact forcing is affected by how black carbon is mixed with other aerosol constituents. From studies of aerosol radiative forcing, it is known that black carbon can exist in one of several possible mixing states; distinct from other aerosol particles (externally mixed) or incorporated within them (internally mixed), or a black-carbon core could be surrounded by a well mixed shell. But so far it has been assumed that aerosols exist predominantly as an external mixture. Here I simulate the evolution of the chemical composition of aerosols, finding that the mixing state and direct forcing of the black-carbon component approach those of an internal mixture, largely due to coagulation and growth of aerosol particles. This finding implies a higher positive forcing from black carbon than previously thought, suggesting that the warming effect from black carbon may nearly balance the net cooling effect of other anthropogenic aerosol constituents. The magnitude of the direct radiative forcing from black carbon itself exceeds that due to CH4, suggesting that black carbon may be the second most important component of global warming after CO2 in terms of direct forcing.
Revisiting AVHRR Tropospheric Aerosol Trends Using Principal Component Analysis
NASA Technical Reports Server (NTRS)
Li, Jing; Carlson, Barbara E.; Lacis, Andrew A.
2014-01-01
The advanced very high resolution radiometer (AVHRR) satellite instruments provide a nearly 25 year continuous record of global aerosol properties over the ocean. It offers valuable insights into the long-term change in global aerosol loading. However, the AVHRR data record is heavily influenced by two volcanic eruptions, El Chichon on March 1982 and Mount Pinatubo on June 1991. The gradual decay of volcanic aerosols may last years after the eruption, which potentially masks the estimation of aerosol trends in the lower troposphere, especially those of anthropogenic origin. In this study, we show that a principal component analysis approach effectively captures the bulk of the spatial and temporal variability of volcanic aerosols into a single mode. The spatial pattern and time series of this mode provide a good match to the global distribution and decay of volcanic aerosols. We further reconstruct the data set by removing the volcanic aerosol component and reestimate the global and regional aerosol trends. Globally, the reconstructed data set reveals an increase of aerosol optical depth from 1985 to 1990 and decreasing trend from 1994 to 2006. Regionally, in the 1980s, positive trends are observed over the North Atlantic and North Arabian Sea, while negative tendencies are present off the West African coast and North Pacific. During the 1994 to 2006 period, the Gulf of Mexico, North Atlantic close to Europe, and North Africa exhibit negative trends, while the coastal regions of East and South Asia, the Sahel region, and South America show positive trends.
Arctic Sea Salt Aerosol from Blowing Snow and Sea Ice Surfaces - a Missing Natural Source in Winter
NASA Astrophysics Data System (ADS)
Frey, M. M.; Norris, S. J.; Brooks, I. M.; Nishimura, K.; Jones, A. E.
2015-12-01
Atmospheric particles in the polar regions consist mostly of sea salt aerosol (SSA). SSA plays an important role in regional climate change through influencing the surface energy balance either directly or indirectly via cloud formation. SSA irradiated by sunlight also releases very reactive halogen radicals, which control concentrations of ozone, a pollutant and greenhouse gas. However, models under-predict SSA concentrations in the Arctic during winter pointing to a missing source. It has been recently suggested that salty blowing snow above sea ice, which is evaporating, to be that source as it may produce more SSA than equivalent areas of open ocean. Participation in the 'Norwegian Young Sea Ice Cruise (N-ICE 2015)' on board the research vessel `Lance' allowed to test this hypothesis in the Arctic sea ice zone during winter. Measurements were carried out from the ship frozen into the pack ice North of 80º N during February to March 2015. Observations at ground level (0.1-2 m) and from the ship's crows nest (30 m) included number concentrations and size spectra of SSA (diameter range 0.3-10 μm) as well as snow particles (diameter range 50-500 μm). During and after blowing snow events significant SSA production was observed. In the aerosol and snow phase sulfate is fractionated with respect to sea water, which confirms sea ice surfaces and salty snow, and not the open ocean, to be the dominant source of airborne SSA. Aerosol shows depletion in bromide with respect to sea water, especially after sunrise, indicating photochemically driven release of bromine. We discuss the SSA source strength from blowing snow in light of environmental conditions (wind speed, atmospheric turbulence, temperature and snow salinity) and recommend improved model parameterisations to estimate regional aerosol production. N-ICE 2015 results are then compared to a similar study carried out previously in the Weddell Sea during the Antarctic winter.
Changes in organic aerosol composition with aging inferred from aerosol mass spectra
NASA Astrophysics Data System (ADS)
Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.
2011-07-01
Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows for the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C) (Van Krevelen, 1950). Heald et al. (2010) examined the evolution of total OA in the Van Krevelen diagram. In this work total OA is deconvolved into components that correspond to primary (HOA and others) and secondary (OOA) organic aerosols. By deconvolving total OA into different components, we remove physical mixing effects between secondary and primary aerosols which allows for examination of the evolution of OOA components alone in the Van Krevelen space. This provides a unique means of following ambient secondary OA evolution that is analogous to and can be compared with trends observed in chamber studies of secondary organic aerosol formation. The triangle plot in Ng et al. (2010) indicates that f44 of OOA components increases with photochemical age, suggesting the importance of acid formation in OOA evolution. Once they are transformed with the new parameterization, the triangle plot of the OOA components from all sites occupy an area in Van Krevelen space which follows a ΔH:C/ΔO:C slope of ~ -0.5. This slope suggests that ambient OOA aging results in net changes in chemical composition that are equivalent to the addition of both acid and alcohol/peroxide functional groups without fragmentation (i.e. C-C bond breakage), and/or the addition of acid groups with fragmentation. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.
NASA Technical Reports Server (NTRS)
2005-01-01
Under funding from this proposal three in situ profile measurements of stratospheric sulfate aerosol and ozone were completed from balloon-borne platforms. The measured quantities are aerosol size resolved number concentration and ozone. The one derived product is aerosol size distribution, from which aerosol moments, such as surface area, volume, and extinction can be calculated for comparison with SAGE III measurements and SAGE III derived products, such as surface area. The analysis of these profiles and comparison with SAGE III extinction measurements and SAGE III derived surface areas are provided in Yongxiao (2005), which comprised the research thesis component of Mr. Jian Yongxiao's M.S. degree in Atmospheric Science at the University of Wyoming. In addition analysis continues on using principal component analysis (PCA) to derive aerosol surface area from the 9 wavelength extinction measurements available from SAGE III. Ths paper will present PCA components to calculate surface area from SAGE III measurements and compare these derived surface areas with those available directly from in situ size distribution measurements, as well as surface areas which would be derived from PCA and Thomason's algorithm applied to the four wavelength SAGE II extinction measurements.
CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS
This chapter surveys the analytical techniques used to determine the concentrations of aerosol mass and its chemical components. The techniques surveyed include mass, major ions (sulfate, nitrate, ammonium), organic carbon, elemental carbon, and trace elements. As reported in...
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 presented and are discussed together with field results, showing that measurements of typical continental or urban aerosols are not significantly affected, while measurements of semi-refractory aerosol in the laboratory, close to anthropogenic sources or in marine environments, can be biased by these effects.
New Versions of MISR Aerosol and Land Surface Products Available
Atmospheric Science Data Center
2018-02-14
New Versions of MISR Aerosol and Land Surface Products Available Monday, February 12, ... the release of new versions of the MISR Level 2 (L2) Aerosol Product, the MISR L2 Land Surface Product, and the Level 3 (L3) Component Global Aerosol and Land Surface Products. The new MISR L2 Aerosol Product ...
NASA Astrophysics Data System (ADS)
Smirnov, A.; Holben, B. N.; Kinne, S.; Nelson, N. B.; Stenchikov, G. L.; Broccardo, S. P.; Sowers, D.; Lobecker, E.; Ondrusek, M.; Zielinski, T. P.; Gray, L. M.; Frouin, R.; Radionov, V. F.; Smyth, T. J.; Zibordi, G.; Heller, M. I.; Slabakova, V.; Krüger, K.; Reid, E. A.; Istomina, L.; Vandermeulen, R. A.; O'Neill, N. T.; Levy, G.; Giles, D. M.; Slutsker, I.; Sorokin, M. G.; Eck, T. F.
2016-02-01
Sea-salt aerosol plays an important role in radiation balance and chemistry of marine atmosphere. Sea-salt production depends on various factors. There is a significant uncertainty in the parametrization of the sea-salt production and budget. Ship-based aerosol optical depth (AOD) measurements can be used as an important validation tool for various global models and in-situ measurements. The paper presents the current status of the Maritime Aerosol Network (MAN) which is a component of Aerosol Robotic Network. Since 2006 over 300 cruises were completed and data archive of more than 5500 measurement days is accessible at http://aeronet.gsfc.nasa.gov/new_web/maritime_aerosol_network.html . AOD measurements from ships of opportunity complemented island-based AERONET measurements and provided important reference points for satellite retrieved and modelled AOD climatology over the oceans. The program exemplifies mutually beneficial international, multi-agency effort in atmospheric aerosol optical studies over the oceans.
Source resolution of the organic component of the fine fraction of the ambient aerosol (d(sub p) < 3.5 micrometers) has been carried out by combining source information from the organic component with thermal analysis and local emission inventories. The primary and secondary carb...
Bukstein, Donald; Parikh, Ruchir; Eid, Sherrine; Ferro, Thomas; Morello, Jean-Pierre
2016-01-01
Perennial allergic rhinitis (PAR) exerts significant quality-of-life and economic burdens on society. Beclomethasone dipropionate (BDP) nasal aerosol is the first nonaqueous, hydrofluoroalkane-propelled intranasal corticosteroid approved for patients in the United States to treat PAR and seasonal allergic rhinitis. To evaluate real-world effectiveness of BDP nasal aerosol from the patient's perspective by using a postmarketing observational registry. Patients (N = 824) from 43 U.S. study sites completed monthly patient-reported outcome instruments, including the Rhinitis Control Assessment Test (primary outcome variable), Treatment Satisfaction Questionnaire for Medication, Work Productivity and Activity Impairment Questionnaire plus Classroom Impairment Questions: Allergy-Specific, Pittsburgh Sleep Quality Index, and Mini Rhinoconjunctivitis Quality of Life Questionnaire for 6 months. The primary outcome assessment (Rhinitis Control Assessment Test score) (N = 527) indicated significant symptomatic improvement over baseline beginning at month 1 (p < 0.001), with >78.8% of respondents who achieved clinically meaningful improvement over 6 months. Secondary outcome measures Mini Rhinoconjunctivitis Quality of Life Questionnaire (p < 0.001), Pittsburgh Sleep Quality Index (p < 0.001), and Treatment Satisfaction Questionnaire for Medication-9 scales of effectiveness (p < 0.001), global satisfaction (p = 0.001), and patient-rated convenience (p = 0.03), significantly increased from baseline to month 6. Five of seven measurements of the Work Productivity and Activity Impairment Questionnaire plus Classroom Impairment Questions: Allergy-Specific, with the exception of work time missed and class time missed, were significantly (p < 0.001) improved in patients treated with BDP compared with baseline. Treatment with nonaqueous BDP nasal aerosol in a real-world setting significantly improved PAR symptoms and measures of quality of life, work, and school-related activities, and is associated with high patient satisfaction, reduced productivity loss and activity impairment, and improvement in sleep quality.
Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)
NASA Astrophysics Data System (ADS)
Thompson, J. E.
2013-12-01
Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.
simplified aerosol representations in global modeling
NASA Astrophysics Data System (ADS)
Kinne, Stefan; Peters, Karsten; Stevens, Bjorn; Rast, Sebastian; Schutgens, Nick; Stier, Philip
2015-04-01
The detailed treatment of aerosol in global modeling is complex and time-consuming. Thus simplified approaches are investigated, which prescribe 4D (space and time) distributions of aerosol optical properties and of aerosol microphysical properties. Aerosol optical properties are required to assess aerosol direct radiative effects and aerosol microphysical properties (in terms of their ability as aerosol nuclei to modify cloud droplet concentrations) are needed to address the indirect aerosol impact on cloud properties. Following the simplifying concept of the monthly gridded (1x1 lat/lon) aerosol climatology (MAC), new approaches are presented and evaluated against more detailed methods, including comparisons to detailed simulations with complex aerosol component modules.
NASA Astrophysics Data System (ADS)
Choi, Yongjoo; Ghim, Young Sung
2016-11-01
Columnar concentrations of absorbing and scattering components of fine mode aerosols were estimated using Aerosol Robotic Network (AERONET) data for a site downwind of Seoul. The study period was between March 2012 and April 2013 including the period of the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-Asia campaign in March to May 2012. The Maxwell Garnett mixing rule was assumed for insoluble components embedded in a host solution, while the volume average mixing rule was assumed for the aqueous solution of soluble components. During the DRAGON-Asia campaign the surface concentrations of major components of fine particles were measured. The columnar mass fractions of black carbon (BC), organic carbon (OC), mineral dust (MD), and ammonium sulfate (AS) were 1.5, 5.9, 6.6, and 52%, respectively, which were comparable to the mass fractions measured at the surface for BC, OC, and secondary inorganic aerosols at 2.3, 18, and 55%. The vertical distributions of BC and AS were investigated by employing the concept of a column height. While the column height for BC was similar to the planetary boundary layer (PBL) height, that for AS was 4.4 times higher than the PBL height and increased with air temperature from March to May. The monthly variations of the columnar mass concentrations during the study period were generally well explained in term of meteorology and emission characteristics. However, certain variations of MD were different from those typically observed primarily because only fine mode aerosols were considered.
High Concentration Standard Aerosol Generator.
1985-07-31
Noncommercial Components .. .. ........ A-1 B. Maintenance Instructions and material Properties of Purchased Components . .. .. .. ... . . . . . . B-1...tration (if a lower flow or a wider size distribution is acceptable and 2) precautions and suggestions for use of different aerosol materials . Additional...details of the system (including shop drawings, i4t lists of materials , and maintenance of commercially available components) are given in
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 applied to an independent aerosol retrieval will likely fail.
NASA Astrophysics Data System (ADS)
Neubauer, D.; Christensen, M.; Lohmann, U.; Poulsen, C. A.
2016-12-01
Studies using present day variability to assess statistical relationships between aerosol and cloud properties find different strengths of these relationships between satellite data and general circulation model (GCM) data. This discrepancy can be explained by structural uncertainties due to differences in the analysis/observational scale and the process scale or spurious relationships between aerosol and cloud properties. Such spurious relationships are the growth of aerosol particles in the humid environment surrounding clouds, misclassification of partly cloudy satellite pixels as cloud free pixels, brightening of aerosol particles by sunlight reflected at cloud edges, or effects of clouds on aerosol like processing of aerosol particles in clouds by nucleation or impact scavenging and subsequent growth by heterogeneous chemistry and release by cloud droplet evaporation or wet scavenging of aerosol particles. To minimize the effects of spatial aggregation and spurious relationships we apply a new nearest neighbour approach to high resolution (A)ATSR datasets from the Aerosol_cci and Cloud_cci projects of the Climate Change Initiative (CCI) programme of ESA. For the ECHAM6-HAM GCM we quantify the impact of using dry aerosol (without aerosol water) in the analysis to mimic the effect of the nearest neighbour approach. The aerosol-liquid water path relationship in ECHAM6-HAM is systematically stronger than in (A)ATSR data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM the strength of the aerosol-liquid water path relationship agrees much better with the ones of (A)ATSR or MODIS. We further find that while the observed relationships of different satellite sensors ((A)ATSR vs. MODIS) are not always consistent for tested environmental conditions the relationships in ECHAM6-HAM are missing a strong dependence on environmental conditions which is critical for bridging the gap between satellite and model estimates of aerosol indirect forcing.
NASA Astrophysics Data System (ADS)
Stier, P.; Schutgens, N. A. J.; Bian, H.; Boucher, O.; Chin, M.; Ghan, S.; Huneeus, N.; Kinne, S.; Lin, G.; Myhre, G.; Penner, J. E.; Randles, C.; Samset, B.; Schulz, M.; Yu, H.; Zhou, C.
2012-09-01
Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in nine participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is -4.51 W m-2 and the inter-model standard deviation is 0.70 W m-2, corresponding to a relative standard deviation of 15%. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.26 W m-2, and the standard deviation increases to 1.21 W m-2, corresponding to a significant relative standard deviation of 96%. However, the top-of-atmosphere forcing variability owing to absorption is low, with relative standard deviations of 9% clear-sky and 12% all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment, demonstrates that host model uncertainties could explain about half of the overall sulfate forcing diversity of 0.13 W m-2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention.
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 probability) is termed an outlier and those DM values that can belong to multiple types (i.e. showing weak probability of belonging to a specific cluster) are termed as Overlap. MODIS active fires are overlaid on the model domain to qualitatively evaluate the model-predicted Smoke aerosol types.
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 probability) is termed an outlier and those DM values that can belong to multiple types (i.e. showing weak probability of belonging to a specific cluster) are termed as Overlap. MODIS active fires are overlaid on the model domain to qualitatively evaluate the model-predicted Smoke aerosol types.
NASA Technical Reports Server (NTRS)
Redemann, Jens; Wood, R.; Zuidema, P.; Haywood, J.; Piketh, S.; Formenti, P.; L'Ecuyer, T.; Kacenelenbogen, M.; Segal-Rosenheimer, M.; Shinozuka, Y.;
2016-01-01
Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. Our understanding of aerosol-cloud interactions in the SE Atlantic is hindered both by the lack of knowledge on aerosol and cloud properties, as well as the lack of knowledge about detailed physical processes involved. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling. Recent efforts to make full use of A-Train aerosol sensor synergies will be highlighted. We describe planned field campaigns in the region to address the existing knowledge gaps. Specifically, we describe the scientific objectives and implementation of the five synergistic, international research activities aimed at providing some of the key aerosol and cloud properties and a process-level understanding of aerosol-cloud interactions over the SE Atlantic: NASA's ORACLES, the UK Met Office's CLARIFY-2016, the DoE's LASIC, NSF's ONFIRE, and CNRS' AEROCLO-SA.
NASA Astrophysics Data System (ADS)
Redemann, J.; Wood, R.; Zuidema, P.; Haywood, J. M.; Piketh, S.; Formenti, P.; L'Ecuyer, T. S.; Kacenelenbogen, M. S.; Segal-Rosenhaimer, M.; Shinozuka, Y.; LeBlanc, S. E.; Vaughan, M. A.; Schmidt, S.; Flynn, C. J.; Song, S.; Schmid, B.; Luna, B.; Abel, S.
2015-12-01
Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and may mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. Our understanding of aerosol-cloud interactions in the SE Atlantic is hindered both by the lack of knowledge on aerosol and cloud properties, as well as the lack of knowledge about detailed physical processes involved. Most notably, we are missing knowledge on the absorptive and cloud nucleating properties of aerosols, including their vertical distribution relative to clouds, on the locations and degree of aerosol mixing into clouds, on the processes that govern cloud property adjustments, and on the importance of aerosol effects on clouds relative to co-varying synoptic scale meteorology. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling. Recent efforts to make full use of A-Train aerosol sensor synergies will be highlighted. We describe planned field campaigns in the region to address the existing knowledge gaps. Specifically, we describe the scientific objectives and implementation of the five synergistic, international research activities aimed at providing some of the key aerosol and cloud properties and a process-level understanding of aerosol-cloud interactions over the SE Atlantic: NASA's ORACLES, the UK Met Office's CLARIFY-2016, the DoE's LASIC, NSF's ONFIRE, and CNRS' AEROCLO-SA.
NASA Astrophysics Data System (ADS)
Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilde, S.; Zhang, Y.; Dall'Osto, M.
2014-04-01
The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterized by a less dense urbanization. We present here the results obtained in San Pietro Capofiume, which is located in a sparsely inhabited sector of the Po Valley, Italy. The experiment was carried out in summer 2009 in the framework of the EUCAARI project ("European Integrated Project on Aerosol, Cloud Climate Aerosol Interaction"). For the first time in Europe, six state-of-the-art techniques were used in parallel: (1) on-line TSI aerosol time-of-flight mass spectrometer (ATOFMS), (2) on-line Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS), (3) soot particle aerosol mass spectrometer (SP-AMS), (4) on-line high resolution time-of-flight mass spectrometer-thermal desorption aerosol gas chromatograph (HR-ToFMS-TAG), (5) off-line twelve-hour resolution proton nuclear magnetic resonance (H-NMR) spectroscopy, and (6) chemical ionization mass spectrometry (CIMS) for the analysis of gas-phase precursors of secondary aerosol. Data from each aerosol spectroscopic method were analysed individually following ad-hoc tools (i.e. PMF for AMS, Art-2a for ATOFMS). The results obtained from each techniques are herein presented and compared. This allows us to clearly link the modifications in aerosol chemical composition to transitions in air mass origin and meteorological regimes. Under stagnant conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), only partly internally mixed with secondary semivolatile compounds such as ammonium nitrate and amines. Other organic components originating from anthropogenic sources at night include monocarboxylic acids which correspond to an AMS factor analogous to the "cooking" organic aerosol (COA) already identified in urban areas. In daytime, enhanced mixing in the planetary boundary layer (PBL) along with increasing temperature determined dramatic changes in aerosol composition caused by the evaporation of semivolatile components and by the entrainment of aged aerosols transported downwards from residual layers. In other words, the entrainment of aged air masses is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOAs) and also for the recycling of primary species such as black carbon. The LV-OOA concentrations were shown to correlate to the simple meteorological tracers of humid PBL air produced by daytime convection over land areas. In particular, both PMF-AMS and PMF-NMR could resolve two components of LV-OOA: one from long-range transport from Central Europe, the second from recirculated PBL air from the Po Valley. According to organic aerosol source apportionment by PMF-AMS, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in North Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. Overall, the deployment of six state-of-the-art spectrometric techniques provided a comprehensive picture of the nature and source contributions of aerosols and aerosol precursors at a European rural site with unprecedented level of details.
NASA Astrophysics Data System (ADS)
Cohen, J. B.
2016-12-01
Due to intense and changing levels of emissions as well as highly non-linear chemical processing, the concentrations of aerosols and thus their impacts are not well known. Urban areas consist of the majority of the emissions of these species and their precursors over large periods of time, while wildfires contribute very large spikes, concentrated in space and over a period of weeks to months. Yet due to urban and economic expansion, as well as clouds amd low intensity burning, the spatial and temporal profiles of these species are changing, with both new sources appearing and old sources decreasing. New work incorporates measurements at different spatial andboptical resolutions from MODIS, MISR, and OMI, coupled with new sampling approaches with CALIOP and AERONET to search for, characterize, and spatially and temporally constrain aerosols. An advanced modeling system including aerosol chemistry, physics, optics, and transport, using a multi-modal and both externally mixed and core-shell mixing is used to quantify the magnitudes of these missing sources. Comparisons between the model and additional dozens of ground stations show extreme improvement when these new sources are included. This new approach is shown to identify new source regions of emissions, many of which were previously non-urbanized or were not found to contain any fire hotspots. In addition, the use of new models run under conditions including both missing local sources from regions such as the expanded urban areas in Southeast and East Asia and advanced chemical and aerosol routines, allow for a comprehensive analysis to be performed. The impacts of insitu chemistry, horizontal, and vertical transport of species, both on the Regional and Continental scale are also included. It is shown that for proper identification, especially on intra-annual and inter-annual variations, this approach is a large improvement throughout Asia, ranging from India, to Indonesia, to China and Japan. Results specific to Southern China and Southeast East Asia demonstrate the additional importance of the climate, as additional variations are identified. Such knowledge can allow us to better understand the consequences and impacts of the rapid ongoing changes occurring in these regions.
NASA Astrophysics Data System (ADS)
Zhuang, Bingliang; Wang, Tijian; Liu, Jane; Che, Huizheng; Han, Yong; Fu, Yu; Li, Shu; Xie, Min; Li, Mengmeng; Chen, Pulong; Chen, Huimin; Yang, Xiu-qun; Sun, Jianning
2018-02-01
The optical and physical properties as well as the direct radiative forcings (DRFs) of fractionated aerosols in the urban area of the western Yangtze River Delta (YRD) are investigated with measurements from a Cimel sun photometer combined with a radiation transfer model. Ground-based observations of aerosols have much higher temporal resolutions than satellite retrievals. An initial analysis reveals the characteristics of the optical properties of different types of fractionated aerosols in the western YRD. The total aerosols, mostly composed of scattering components (93.8 %), have mean optical depths of 0.65 at 550 nm and refractive index of 1.44 + 0.0084i at 440 nm. The fine aerosols are approximately four times more abundant and have very different compositions from coarse aerosols. The absorbing components account for only ˜ 4.6 % of fine aerosols and 15.5 % of coarse aerosols and have smaller sizes than the scattering aerosols within the same mode. Therefore, fine particles have stronger scattering than coarse ones, simultaneously reflecting the different size distributions between the absorbing and scattering aerosols. The relationships among the optical properties quantify the aerosol mixing and imply that approximately 15 and 27.5 % of the total occurrences result in dust- and black-carbon-dominating mixing aerosols, respectively, in the western YRD. Unlike the optical properties, the size distributions of aerosols in the western YRD are similar to those found at other sites over eastern China on a climatological scale, peaking at radii of 0.148 and 2.94 µm. However, further analysis reveals that the coarse-dominated particles can also lead to severe haze pollution over the YRD. Observation-based estimations indicate that both fine and coarse aerosols in the western YRD exert negative DRFs, and this is especially true for fine aerosols (-11.17 W m-2 at the top of atmosphere, TOA). A higher absorption fraction leads directly to the negative DRF being further offset for coarse aerosols (-0.33 W m-2) at the TOA. Similarly, the coarse-mode DRF contributes to only 13.3 % of the total scattering aerosols but > 33.7 % to the total absorbing aerosols. A sensitivity analysis states that aerosol DRFs are not highly sensitive to their profiles in clear-sky conditions. Most of the aerosol properties and DRFs have substantial seasonality in the western YRD. The results further reveal the contributions of each component of the different size particles to the total aerosol optical depths (AODs) and DRFs. Additionally, these results can be used to improve aerosol modelling performance and the modelling of aerosol effects in the eastern regions of China.
aerosol radiative effects and forcing: spatial and temporal distributions
NASA Astrophysics Data System (ADS)
Kinne, Stefan
2014-05-01
A monthly climatology for aerosol optical properties based on a synthesis from global modeling and observational data has been applied to illustrate spatial distributions and global averages of aerosol radiative impacts. With the help of a pre-industrial reference for aerosol optical properties from global modeling, also the aerosol direct forcing (ca -0.35W/m2 globally and annual averaged) and their spatial and seasonal distributions and contributions by individual aerosol components are estimated. Finally, CCN and IN concentrations associated with this climatology are applied to estimate aerosol indirect effects and forcing.
NASA Technical Reports Server (NTRS)
Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin
2003-01-01
During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.
Time resolved aerosol monitoring in the urban centre of Soweto
NASA Astrophysics Data System (ADS)
Formenti, P.; Annegarn, H. J.; Piketh, S. J.
1998-03-01
A programme of aerosol sampling was conducted from 1982 to 1984 in the urban area of Soweto, Johannesburg, South Africa. The particulate matter (aerodynamic diameter <15 μm) was collected using a two hours time resolution single stage streaker sampler and elemental concentrations were resolved via Particle Induced X-ray Emission (PIXE) analysis. Samples have been selected for analysis from an aerosol sample archive to establish base-line atmospheric conditions that existed in Soweto prior to large scale electrification, and to establish source apportionment of crustal elements between coal smoke and traffic induced road dust, based on chemical elemental measurements. A novel technique is demonstrated for processing PIXE-derived time sequence elemental concentration vectors. Slowly varying background components have been extracted from sulphur and crustal aerosol components, using alternatively two digital filters: a moving minimum, and a moving average. The residuals of the crustal elements, assigned to locally generated aerosol components, were modelled using surrogate tracers: sulphur as a surrogate for coal smoke; and Pb as a surrogate for traffic activity. Results from this source apportionment revealed coal emissions contributed between 40% and 50% of the aerosol mineral matter, while 18-22% originated from road dust. Background aerosol, characteristic of the regional winter aerosol burden over the South African Highveld, was between 12% and 21%. Minor contributors identified included a manganese smelter, located 30 km from the sampling site, and informal trash burning, as the source of intermittent heavy metals (Cu, Zn). Elemental source profiles derived for these various sources are presented.
NASA Technical Reports Server (NTRS)
Jethva, H.; Torres, O.
2012-01-01
We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by the Ozone Monitoring Instrument (OMI) during 2005-2007. In the current near-UV OMI aerosol algorithm (OMAERUV), it is implicitly assumed that the only absorbing component in carbonaceous aerosols is black carbon whose imaginary component of the refractive index is wavelength independent. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be significantly over-estimated compared to that of AERONET at several sites during intense biomass burning events (August-September). Other well-known sources of error affecting the near-UV method of aerosol retrieval do not explain the large observed AOD discrepancies between the satellite and the ground-based observations. A number of studies have revealed strong spectral dependence in carbonaceous aerosol absorption in the near-UV region suggesting the presence of organic carbon in biomass burning generated aerosols. A sensitivity analysis examining the importance of accounting for the presence of wavelength-dependent aerosol absorption in carbonaceous particles in satellite-based remote sensing was carried out in this work. The results convincingly show that the inclusion of spectrally-dependent aerosol absorption in the radiative transfer calculations leads to a more accurate characterization of the atmospheric load of carbonaceous aerosols.
NASA Astrophysics Data System (ADS)
Stewart, D. R.; Stockwell, W. R.; Morris, V. R.; Fitzgerald, R. M.
2016-12-01
The major photochemical processes that produce ozone and aerosols are coupled together strongly in the polluted urban atmosphere. Aerosols are either directly emitted or formed through the same kind of chemistry that leads to the production of ozone. The aerosols produced through atmospheric chemistry are known as secondary aerosols and they may be composed of inorganic (nitrates, sulfates) or organic compounds. Wind blown dust and soot are two examples of primary aerosols. The component of secondary inorganic aerosols includes compounds such as ammonium nitrate, ammonium bisulfate and ammonium sulfate. Secondary organic aerosols are a very important component of PM with strong implications for health. The formation of secondary organic aerosol is linked with ozone photochemistry through the reactions of volatile organic compounds (VOC). The oxidation of VOC produces radicals that convert nitric oxide to nitrogen dioxide that photolyze to produce ozone. Larger VOC (those with more carbon atoms) undergo a number of oxidation cycles that add oxygen atoms to large organic molecules. The vapor pressure of many of these highly oxidized compounds is sufficiently low that they condense to produce secondary organic aerosols. The Community Multi-scale Air Quality model (CMAQ) and other chemical simulations have been made to quantify the relationship between varying emissions of VOC and NOx and the production of inorganic and secondary organic aerosols. The results from this analysis will be presented.
Performance Testing of Lidar Components Subjected to Space Exposure in Space via MISSE 7 Mission
NASA Technical Reports Server (NTRS)
Prasad, Narasimha S.
2012-01-01
.The objective of the Materials International Space Station Experiment (MISSE) is to study the performance of novel materials when subjected to the synergistic effects of the harsh space environment for several months. MISSE missions provide an opportunity for developing space qualifiable materials. Several laser and lidar components were sent by NASA Langley Research Center (LaRC) as a part of the MISSE 7 mission. The MISSE 7 module was transported to the international space station (ISS) via STS 129 mission that was launched on Nov 16, 2009. Later, the MISSE 7 module was brought back to the earth via the STS 134 that landed on June 1, 2011. The MISSE 7 module that was subjected to exposure in space environment for more than one and a half year included fiber laser, solid-state laser gain materials, detectors, and semiconductor laser diode. Performance testing of these components is now progressing. In this paper, the current progress on post-flight performance testing of a high-speed photodetector and a balanced receiver is discussed. Preliminary findings show that detector characteristics did not undergo any significant degradation.
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 to different air mass histories, to determine the generality of the campaign-wide findings described above.
NASA Astrophysics Data System (ADS)
Stier, P.; Schutgens, N. A. J.; Bellouin, N.; Bian, H.; Boucher, O.; Chin, M.; Ghan, S.; Huneeus, N.; Kinne, S.; Lin, G.; Ma, X.; Myhre, G.; Penner, J. E.; Randles, C. A.; Samset, B.; Schulz, M.; Takemura, T.; Yu, F.; Yu, H.; Zhou, C.
2013-03-01
Simulated multi-model "diversity" in aerosol direct radiative forcing estimates is often perceived as a measure of aerosol uncertainty. However, current models used for aerosol radiative forcing calculations vary considerably in model components relevant for forcing calculations and the associated "host-model uncertainties" are generally convoluted with the actual aerosol uncertainty. In this AeroCom Prescribed intercomparison study we systematically isolate and quantify host model uncertainties on aerosol forcing experiments through prescription of identical aerosol radiative properties in twelve participating models. Even with prescribed aerosol radiative properties, simulated clear-sky and all-sky aerosol radiative forcings show significant diversity. For a purely scattering case with globally constant optical depth of 0.2, the global-mean all-sky top-of-atmosphere radiative forcing is -4.47 Wm-2 and the inter-model standard deviation is 0.55 Wm-2, corresponding to a relative standard deviation of 12%. For a case with partially absorbing aerosol with an aerosol optical depth of 0.2 and single scattering albedo of 0.8, the forcing changes to 1.04 Wm-2, and the standard deviation increases to 1.01 W-2, corresponding to a significant relative standard deviation of 97%. However, the top-of-atmosphere forcing variability owing to absorption (subtracting the scattering case from the case with scattering and absorption) is low, with absolute (relative) standard deviations of 0.45 Wm-2 (8%) clear-sky and 0.62 Wm-2 (11%) all-sky. Scaling the forcing standard deviation for a purely scattering case to match the sulfate radiative forcing in the AeroCom Direct Effect experiment demonstrates that host model uncertainties could explain about 36% of the overall sulfate forcing diversity of 0.11 Wm-2 in the AeroCom Direct Radiative Effect experiment. Host model errors in aerosol radiative forcing are largest in regions of uncertain host model components, such as stratocumulus cloud decks or areas with poorly constrained surface albedos, such as sea ice. Our results demonstrate that host model uncertainties are an important component of aerosol forcing uncertainty that require further attention.
NASA Astrophysics Data System (ADS)
Thornhill, K. L.; Anderson, B.; Chen, G.; Beyersdorf, A. J.; Winstead, E. L.; Dibb, J. E.; Scheuer, E. M.; Weber, R.; Lathem, T. L.; Jimenez, J. L.; Cubison, M.; Kondo, Y.; Wennberg, P. O.; Weinheimer, A. J.; Wisthaler, A.
2009-12-01
In the summer of 2008, measurements of aerosols were made on-board the NASA DC-8 over the state of California, as part of the second phase of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) on behalf of the California Air resources Board (CARB). The DC-8 made four flights, between 18 June and 26 June, totaling 33 hours, to examine California’s atmosphere to better understand the chemical dynamics of smog and greenhouse gases over the state. Serendipitously, from a science perspective, this time period was marked by numerous wildfires spread throughout the state. The NASA DC-8 had a suite of aerosol instruments, capable of measuring the number concentrations, optical properties, and size distributions of aerosols between 0.003 and 1500 um. In this presentation, we will characterize aerosols sampled over the Los Angeles basin, which included several missed approaches at Los Angeles International Airport (LAX), traverses through the Long Beach and Santa Barbara ship channels, sampling in and out of the marine boundary layer, and encounters with outflow of forest fires mixed with urban smog. The evolution of the aerosols during the day will be examined, as the smog builds up within the basin and the plume travels out of the basin into the surrounding atmosphere.
Lu, Cheng-Hsuan; da Silva, Arlindo; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S.; Chen, Shen-Po; Chuang, Hui-Ya; Juang, Hann-Ming Henry; McQueen, Jeffery; Iredell, Mark
2018-01-01
The NOAA National Centers for Environmental Prediction (NCEP) implemented NEMS GFS Aerosol Component (NGAC) for global dust forecasting in collaboration with NASA Goddard Space Flight Center (GSFC). NGAC Version 1.0 has been providing 5 day dust forecasts at 1°×1° resolution on a global scale, once per day at 00:00 Coordinated Universal Time (UTC), since September 2012. This is the first global system capable of interactive atmosphere aerosol forecasting at NCEP. The implementation of NGAC V1.0 reflects an effective and efficient transitioning of NASA research advances to NCEP operations, paving the way for NCEP to provide global aerosol products serving a wide range of stakeholders as well as to allow the effects of aerosols on weather forecasts and climate prediction to be considered. PMID:29652411
Lu, Cheng-Hsuan; da Silva, Arlindo; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S; Chen, Shen-Po; Chuang, Hui-Ya; Juang, Hann-Ming Henry; McQueen, Jeffery; Iredell, Mark
2016-01-01
The NOAA National Centers for Environmental Prediction (NCEP) implemented NEMS GFS Aerosol Component (NGAC) for global dust forecasting in collaboration with NASA Goddard Space Flight Center (GSFC). NGAC Version 1.0 has been providing 5 day dust forecasts at 1°×1° resolution on a global scale, once per day at 00:00 Coordinated Universal Time (UTC), since September 2012. This is the first global system capable of interactive atmosphere aerosol forecasting at NCEP. The implementation of NGAC V1.0 reflects an effective and efficient transitioning of NASA research advances to NCEP operations, paving the way for NCEP to provide global aerosol products serving a wide range of stakeholders as well as to allow the effects of aerosols on weather forecasts and climate prediction to be considered.
Comprehensive characterization of PM2.5 aerosols in Singapore
NASA Astrophysics Data System (ADS)
Balasubramanian, R.; Qian, W.-B.; Decesari, S.; Facchini, M. C.; Fuzzi, S.
2003-08-01
A comprehensive characterization of PM2.5 aerosols collected in Singapore from January through December 2000 is presented. The annual average mass concentration of PM2.5 was 27.2 μg/m3. The atmospheric loading of PM2.5 was elevated sporadically from March through May, mainly due to advection of biomass burning (deliberate fires to clear plantation areas) impacted air masses from Sumatra, Indonesia. Satellite images of the area, trajectory calculations, and surface wind direction data are in support of the transport of pyrogenic products from Sumatra toward Singapore. Aerosol samples collected during the dry season were analyzed for water-soluble ions, water-soluble organic compounds (WSOC), elemental carbon (EC), organic carbon, and trace elements using a number of analytical techniques. The major components were sulfate, EC, water-soluble carbonaceous materials, and water-insoluble carbonaceous materials. Aerosol WSOC were characterized based on a combination of chromatographic separations by ion exchange chromatography, functional group investigation by proton nuclear magnetic resonance, and total organic carbon determination. The comprehensive chemical characterization of PM2.5 particles revealed that both non-sea-salt sufate (nss-SO42-) and carbonaceous aerosols mainly contributed to the increase in the mass concentration of aerosols during the smoke haze period. Using a mass closure test (a mass balance), we determined whether the physical measurement of gravimetric fine PM concentration of a sample is equal to the summed concentrations of the individually identified chemical constituents (measured or inferred) in the sample. The sum of the determined groups of aerosol components and the gravimetrically determined mass agreed reasonably well. Principal component analysis was performed from the combined data set, and five factors were observed: a soil dust component, a metallurgical industry factor, a factor representing emissions from biomass burning and automobiles, a sea-salt component, and an oil combustion factor.
Increased absorption by coarse aerosol particles over the Gangetic–Himalayan region
Manoharan, Vani Starry; Kotamarthi, R.; Feng, Yan; ...
2014-02-03
Each atmospheric aerosol type has distinctive light-absorption characteristics related to its physical/chemical properties. Climate models treat black carbon as the main light-absorbing component of carbonaceous atmospheric aerosols, while absorption by some organic aerosols is also considered, particularly at ultraviolet wavelengths. Most absorbing aerosols are assumed to be < 1 μm in diameter (sub-micron). Here we present results from a recent field study in India, primarily during the post-monsoon season (October–November), suggesting the presence of absorbing aerosols sized 1–10 μm. Absorption due to super-micron-sized particles was nearly 30% greater than that due to smaller particles. Periods of increased absorption by largermore » particles ranged from a week to a month. Radiative forcing calculations under clear-sky conditions show that super-micron particles account for nearly 44% of the total aerosol forcing. The origin of the large aerosols is unknown, but meteorological conditions indicate that they are of local origin. Such economic and habitation conditions exist throughout much of the developing world. Furthermore, large absorbing particles could be an important component of the regional-scale atmospheric energy balance.« less
Impact of aerosols on solar energy production - Scenarios from the Sahel Zone
NASA Astrophysics Data System (ADS)
Neher, Ina; Meilinger, Stefanie; Crewell, Susanne
2017-04-01
Solar energy is one option to serve the rising global energy demand with low environmental impact. Building an energy system with a considerable share of solar power requires long-term investment and a careful investigation of potential sites. Therefore, understanding the impacts from varying regionally and locally determined meteorological conditions on solar energy production will influence energy yield projections. Aerosols reduce global solar radiation due to absorption and scattering and therewith solar energy yields. Depending on aerosol size distribution they reduce the direct component of the solar radiation and modify the direction of the diffuse component compared to standard atmospheric conditions without aerosols. The aerosol size distribution and composition in the atmosphere is highly variable due to meteorological and land surface conditions. A quantitative assessment of aerosol effects on solar power yields and its relation to land use change is of particular interest for developing countries countries when analyzing the potential of local power production. This study aims to identify the effect of atmospheric aerosols in three different land use regimes, namely desert, urban/polluted and maritime on the tilted plane of photovoltaic energy modules. Here we focus on the Sahel zone, i.e. Niamey, Niger (13.5 N;2.1 E), located at the edge of the Sahara where also detailed measurements of the atmospheric state are available over the year 2006. Guided by observations a model chain is used to determine power yields. The atmospheric aerosol composition will be defined by using the Optical Properties of Aerosols and Clouds (OPAC) library. Direct and diffuse radiation (up- and downward component) are then calculated by the radiative transfer model libRadtran which allows to calculate the diffuse component of the radiance from different azimuth and zenith angles. Then the diffuse radiance will be analytically transformed to an east, south and west facing module with different tilting angles (between 0° and 45°) from each direction and compared to the tilted diffuse radiation derived by the Perez-model (Loutzenhiser et al. 2007) which is widely used in the photovoltaic community. This will allow an assessment how well standard approaches work in tropical region under various aerosol conditions including strong dust outbreaks from the Sahara. This presentation will introduce the modeling chain to assess solar power yields for different photovoltaic modules in the Sahel zone and address their relative dependence on aerosol conditions.
Chen, Qingcai; Ikemori, Fumikazu; Mochida, Michihiro
2016-10-18
The present study used a combination of solvent and solid-phase extractions to fractionate organic compounds with different polarities from total suspended particulates in Nagoya, Japan, and their optical characteristics were obtained on the basis of their UV-visible absorption spectra and excitation-emission matrices (EEMs). The relationship between their optical characteristics and chemical structures was investigated based on high-resolution aerosol mass spectra (HR-AMS spectra), soft ionization mass spectra and Fourier transform infrared (FT-IR) spectra. The major light-absorption organics were less polar organic fractions, which tended to have higher mass absorption efficiencies (MAEs) and lower wavelength dependent Ångström exponents (Å) than the more polar organic fractions. Correlation analyses indicate that organic compounds with O and N atoms may contribute largely to the total light absorption and fluorescence of the organic aerosol components. The extracts from the aerosol samples were further characterized by a classification of the EEM profiles using a PARAFAC model. Different fluorescence components in the aerosol organic EEMs were associated with specific AMS ions and with different functional groups from the FT-IR analysis. These results may be useful to determine and further classify the chromophores in atmospheric organic aerosols using EEM spectroscopy.
Global volcanic aerosol properties derived from emissions, 1990-2015, using CESM1(WACCM)
NASA Astrophysics Data System (ADS)
Mills, Michael; Schmidt, Anja; Easter, Richard; Solomon, Susan; Kinnison, Douglas; Ghan, Steven; Neely, Ryan; Marsh, Daniel; Conley, Andrew; Bardeen, Charles; Gettelman, Andrew
2016-04-01
Accurate representation of global stratospheric aerosols from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-losses that may be linked to volcanic activity. Attribution of climate variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the rate of global average temperature increases. We have compiled a database of volcanic SO2 emissions and plume altitudes for eruptions from 1990 to 2015, and developed a new prognostic capability for simulating stratospheric sulfate aerosols in the Community Earth System Model (CESM). We combined these with other non-volcanic emissions of sulfur sources to reconstruct global aerosol properties from 1990 to 2015. Our calculations show remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of stratospheric aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD calculations represent a clear improvement over available satellite-based analyses, which generally ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD calculations greatly improve on that provided for the Chemistry-Climate Model Initiative, which misses about 60% of the SAD measured in situ on average during both volcanically active and volcanically quiescent periods. The stark differences in SAOD and SAD compared to other data sets will have significant effects on calculations of the radiative forcing of climate and global stratospheric chemistry over the period 2005-2015. In light of these results, the impact of volcanic aerosols in reducing the rate of global average temperature increases since the year 2000 should be revisited. We have made our calculated aerosol properties from January 1990 to November 2015 available for public download.
NASA Astrophysics Data System (ADS)
Shukurova, L. M.; Gruzdev, A. N.
2010-06-01
The temporal variability of the chemical composition of surface aerosol with particle diameters of 0.7-2 μm is analyzed. This analysis is based on the results of measurements of infrared transmission spectra of aerosol samples collected with the use of a cascade impactor at the Zvenigorod Scientific Station of the Institute of Atmospheric Physics (IAP) in 1999-2005. Seasonal features of the aerosol chemical composition and its dependence on the particle size are revealed. The interdiurnal variability of the aerosol composition depends on the season, and it manifests itself more strongly in winter and spring. Air-mass changes lead to changes in the relation of sulfates and nitrates in the micron fraction of aerosol. The enrichment of samples in nitrates is especially characteristic of the winter and spring seasons. Compounds containing the NO2 group are often met in the samples of aerosol with particle sizes of 0.7-1.3 μm during the cold time of the year. The estimates of the optical thickness of micron aerosol in the sulfate absorption band are obtained, and optical-thickness variations of some scales are detected. The quantitative characteristics of statistical relations between different chemical components of aerosol inside individual fractions and between chemical components of the micron and submicron fractions are obtained and analyzed.
Atmospheric Sampling of Aerosols to Stratospheric Altitudes using High Altitude Balloons
NASA Astrophysics Data System (ADS)
Jerde, E. A.; Thomas, E.
2010-12-01
Although carbon dioxide represents a long-lived atmospheric component relevant to global climate change, it is also understood that many additional contributors influence the overall climate of Earth. Among these, short-lived components are more difficult to incorporate into models due to uncertainties in the abundances of these both spatially and temporally. Possibly the most significant of these short-lived components falls under the heading of “black carbon” (BC). There are numerous overlapping definitions of BC, but it is basically carbonaceous in nature and light absorbing. Due to its potential as a climate forcer, an understanding of the BC population in the atmosphere is critical for modeling of radiative forcing. Prior measurements of atmospheric BC generally consist of airplane- and ground-based sampling, typically below 5000 m and restricted in time and space. Given that BC has a residence time on the order of days, short-term variability is easily missed. Further, since the radiative forcing is a result of BC distributed through the entire atmospheric column, aircraft sampling is by definition incomplete. We are in the process of planning a more comprehensive sampling of the atmosphere for BC using high-altitude balloons. Balloon-borne sampling is a highly reliable means to sample air through the entire troposphere and into the lower stratosphere. Our system will incorporate a balloon and a flight train of two modules. One module will house an atmospheric sampler. This sampler will be single-stage (samples all particle sizes together), and will place particles directly on an SEM sample stub for analysis. The nozzle depositing the sample will be offset from the center of the stub, placing the aerosol particles toward the edge. At various altitudes, the stub will be rotated 45 degrees, providing 6-8 sample “cuts” of particle populations through the atmospheric column. The flights will reach approximately 27 km altitude, above which the balloons burst and the modules return to the surface. The second module will contain instrumentation recording temperature, pressure, and humidity, plus a radio beacon to track the location, facilitating recovery. Another instrument we are planning is a small, lightweight optical aerosol spectrometer probe. This would provide a valuable secondary set of data to compare with the actual sampling. The aerosol particle population will be assessed using the SEM at Morehead State University. Over the next several years, sampling is planned at locations both near and far from urban areas, and at intermediate locations. Sampling will be conducted at four times during the year to assess seasonal variations and, at some sites, repeated short-term samplings (e.g., 5 flights in 10 days) will be undertaken to assess short-term variations. In addition, the SEM should permit the assessment of the ratio of BC to organic carbon (OC). Like BC, organic carbon species are produced through biomass burning, but are not as effective as light absorbers, so are not responsible for as much forcing as black carbon. The atmosphere is sampled at a known volumetric rate, resulting in a picture of the atmospheric column density for both BC and OC, information of great use in modeling of the aerosol contribution to climate change.
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 component (LV-OOA), both of which were found to be secondary species and could be formed from precursors co-emitted with BC. Using the total potential source contribution function model, the likely source areas of the major PM1 components at both sites were a on large regional scale in East Asia. The possible sources may include not only emissions from the Chinese mainland but also emissions from ocean-going cargo ships and biomass burning in neighboring countries.
NASA Astrophysics Data System (ADS)
Neubauer, David; Christensen, Matthew W.; Poulsen, Caroline A.; Lohmann, Ulrike
2017-11-01
Aerosol-cloud interactions (ACIs) are uncertain and the estimates of the ACI effective radiative forcing (ERFaci) magnitude show a large variability. Within the Aerosol_cci project the susceptibility of cloud properties to changes in aerosol properties is derived from the high-resolution AATSR (Advanced Along-Track Scanning Radiometer) data set using the Cloud-Aerosol Pairing Algorithm (CAPA) (as described in our companion paper) and compared to susceptibilities from the global aerosol climate model ECHAM6-HAM2 and MODIS-CERES (Moderate Resolution Imaging Spectroradiometer - Clouds and the Earth's Radiant Energy System) data. For ECHAM6-HAM2 the dry aerosol is analysed to mimic the effect of CAPA. Furthermore the analysis is done for different environmental regimes. The aerosol-liquid water path relationship in ECHAM6-HAM2 is systematically stronger than in AATSR-CAPA data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM2 the strength of the susceptibilities of liquid water path, cloud droplet number concentration and cloud albedo as well as ERFaci agree much better with those of AATSR-CAPA or MODIS-CERES. When comparing satellite-derived to model-derived susceptibilities, this study finds it more appropriate to use dry aerosol in the computation of model susceptibilities. We further find that the statistical relationships inferred from different satellite sensors (AATSR-CAPA vs. MODIS-CERES) as well as from ECHAM6-HAM2 are not always of the same sign for the tested environmental conditions. In particular the susceptibility of the liquid water path is negative in non-raining scenes for MODIS-CERES but positive for AATSR-CAPA and ECHAM6-HAM2. Feedback processes like cloud-top entrainment that are missing or not well represented in the model are therefore not well constrained by satellite observations. In addition to aerosol swelling, wet scavenging and aerosol processing have an impact on liquid water path, cloud albedo and cloud droplet number susceptibilities. Aerosol processing leads to negative liquid water path susceptibilities to changes in aerosol index (AI) in ECHAM6-HAM2, likely due to aerosol-size changes by aerosol processing. Our results indicate that for statistical analysis of aerosol-cloud interactions the unwanted effects of aerosol swelling, wet scavenging and aerosol processing need to be minimised when computing susceptibilities of cloud variables to changes in aerosol.
Retrieval of the atmospheric compounds using a spectral optical thickness information
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ioltukhovski, A.A.
A spectral inversion technique for retrieval of the atmospheric gases and aerosols contents is proposed. This technique based upon the preliminary measurement or retrieval of the spectral optical thickness. The existence of a priori information about the spectral cross sections for some of the atmospheric components allows to retrieve the relative contents of these components in the atmosphere. Method of smooth filtration makes possible to estimate contents of atmospheric aerosols with known cross sections and to filter out other aerosols; this is done independently from their relative contribution to the optical thickness.
NASA Astrophysics Data System (ADS)
Wonaschuetz, Anna
Atmospheric aerosols are a highly relevant component of the climate system affecting atmospheric radiative transfer and the hydrological cycle. As opposed to other key atmospheric constituents with climatic relevance, atmospheric aerosol particles are highly heterogeneous in time and space with respect to their size, concentration, chemical composition and physical properties. Many aspects of their life cycle are not understood, making them difficult to represent in climate models and hard to control as a pollutant. Aerosol-cloud interactions in particular are infamous as a major source of uncertainty in future climate predictions. Field measurements are an important source of information for the modeling community and can lead to a better understanding of chemical and microphysical processes. In this study, field data from urban, marine, and arid settings are analyzed and the impact of meteorological conditions on the evolution of aerosol particles while in the atmosphere is investigated. Particular attention is given to organic aerosols, which are a poorly understood component of atmospheric aerosols. Local wind characteristics, solar radiation, relative humidity and the presence or absence of clouds and fog are found to be crucial factors in the transport and chemical evolution of aerosol particles. Organic aerosols in particular are found to be heavily impacted by processes in the liquid phase (cloud droplets and aerosol water). The reported measurements serve to improve the process-level understanding of aerosol evolution in different environments and to inform the modeling community by providing realistic values for input parameters and validation of model calculations.
MODELING THE FORMATION OF SECONDARY ORGANIC AEROSOL WITHIN A COMPREHENSIVE AIR QUALITY MODEL SYSTEM
The aerosol component of the CMAQ model is designed to be an efficient and economical depiction of aerosol dynamics in the atmosphere. The approach taken represents the particle size distribution as the superposition of three lognormal subdistributions, called modes. The proces...
NASA Technical Reports Server (NTRS)
Lu, Cheng-Hsuan; Da Silva, Arlindo M.; Wang, Jun; Moorthi, Shrinivas; Chin, Mian; Colarco, Peter; Tang, Youhua; Bhattacharjee, Partha S.; Chen, Shen-Po; Chuang, Hui-Ya;
2016-01-01
The NOAA National Centers for Environmental Prediction (NCEP) implemented the NOAA Environmental Modeling System (NEMS) Global Forecast System (GFS) Aerosol Component (NGAC) for global dust forecasting in collaboration with NASA Goddard Space Flight Center (GSFC). NGAC Version 1.0 has been providing 5-day dust forecasts at 1deg x 1deg resolution on a global scale, once per day at 00:00 Coordinated Universal Time (UTC), since September 2012. This is the first global system capable of interactive atmosphere aerosol forecasting at NCEP. The implementation of NGAC V1.0 reflects an effective and efficient transitioning of NASA research advances to NCEP operations, paving the way for NCEP to provide global aerosol products serving a wide range of stakeholders, as well as to allow the effects of aerosols on weather forecasts and climate prediction to be considered.
NASA Technical Reports Server (NTRS)
Fymat, A. L.; Mease, K. D.
1978-01-01
The technique proposed by Fymat (1976) for retrieving the complex refractive index of atmospheric aerosols using narrowband spectral transmission ratios, taken within an overall narrow spectral interval, is investigated in the case of modelled polydispersions of rural, maritime-continental, maritime-sea spray and meteoric dust aerosols. It is confirmed that for not too broad size distributions most of the information comes from a narrow size range of 'active' aerosols so that, under these circumstances, the refractive index components can indeed be retrieved essentially independently of the size distribution. For 0.1% accurate data in three colors, the technique can provide the real and imaginary components of the index respectively within 0.07% and 0.3% accuracy.
Impacts of different aerosol climatologies on the European climate during the last decades
NASA Astrophysics Data System (ADS)
Schultze, Markus; Rockel, Burkhardt
2015-04-01
As summarized in the 5th Assessment Report of the IPCC, the effects of aerosols on the Earth's energy budget are one of the largest uncertainties in a changing climate. Despite a better understanding of aerosol processes since the previous report, it remains unclear to which degree of complexity these processes need to be represented within the climate models to consider their effects in a sufficient manner. Within the nonhydrostatic regional climate model COSMO-CLM, the aerosol climatology of Tanre from 1984 is widely used to simulate the direct effect of aerosols on radiative processes. Apart from a very low spatial resolution and a missing temporal variability, this climatology is dominated by high values of Aerosol Optical Depth (AOD) over Northern Africa, caused by an overestimation of Saharan dust. To investigate the impacts of different aerosol distributions on the European climate, the Tanre aerosol climatology is replaced by the more realistic climatologies of Tegen from 1997 and AEROCOM from 2006 with constant annual cycles of AOD. In addition a control simulation without any aerosol feedbacks was performed. The simulations cover a period of 30 years from 1980 to 2010. In parts of the regions surveyed, we found a near surface cooling, which is strongly linked to AOD, and a broad mid-troposphere warming for all simulations in comparison to the control simulation. A decrease in convective precipitation is mainly caused by stabilization of stratification and by less evapotranspiration resulting from surface cooling. The horizontal differing mid-troposphere warming induces a drop in surface pressure and therefore leads to changes in circulation patterns which are still under investigation. The largest impacts of direct and semi direct aerosol effects was found in summer season. As next step, pre-calculated transient aerosol data will be used to compile an up-to-date aerosol climatology including temporal changes. One main focus of the study will be to investigate whether a decrease in anthropogenic aerosol load in Europe during the last decades enhances the GHG induced near surface warming.
NASA Technical Reports Server (NTRS)
Russell, Philip B.; Valero, F. P. J.; Flatau, P. J.; Bergin, M.; Holben, B.; Nakajima, T.; Pilewskie, P.; Bergstrom, R.; Hipskind, R. Stephen (Technical Monitor)
2001-01-01
A primary, ACE-Asia objective was to quantify the interactions between aerosols and radiation in the Asia-Pacific region. Toward this end, radiometric and related aerosol measurements were made from ocean, land, air and space platforms. Models that predict aerosol fields guided the measurements and are helping integrate and interpret results. Companion overview's survey these measurement and modeling components. Here we illustrate how these components were combined to determine aerosol radiative. impacts and their relation to aerosol properties. Because clouds can obscure or change aerosol direct radiative effects, aircraft and ship sorties to measure these effects depended on predicting and finding cloud-free areas and times with interesting aerosols present. Pre-experiment satellite cloud climatologies, pre-flight aerosol and cloud forecasts, and in-flight guidance from satellite imagery all helped achieve this. Assessments of aerosol regional radiative impacts benefit from the spatiotemporal coverage of satellites, provided satellite-retrieved aerosol properties are accurate. Therefore, ACE-Asia included satellite retrieval tests, as part of many comparisons to judge the consistency (closure) among, diverse measurements. Early results include: (1) Solar spectrally resolved and broadband irradiances and optical depth measurements from the C-130 aircraft and at Kosan, Korea yielded aerosol radiative forcing efficiencies, permitting comparisons between efficiencies of ACE-Asia and INDOEX aerosols, and between dust and "pollution" aerosols. Detailed results will be presented in separate papers. (2) Based on measurements of wavelength dependent aerosol optical depth (AOD) and single scattering albedo the estimated 24-h a average aerosol radiative forcing efficiency at the surface for photosynthetically active radiation (400 - 700 nm) in Yulin, China is approx. 30 W sq m per AOD(500 nm). (3) The R/V Brown cruise from Honolulu to Sea of Japan sampled an aerosol optical depth gradient, with AOD(500 nm) extremes from 0.1 to 1.1. On the Pacific transit from Honolulu to Hachijo AOD(500 nm) averaged 0.2, including increases to 0.4 after several storms, suggesting the strong impact of wind-generated seasalt. The AOD maximum, found in the Sea of Japan, was influenced by dust and anthropogenic sources. (4) In Beijing, single scattering albedo retrieved from AERONET sun-sky radiometry yielded midvisible SSA=0.88 with strong wavelength dependence, suggesting a significant black carbon component. SSA retrieved during dust episodes was approx. 0.90 and variable but wavelength neutral reflecting the presence of urban haze with the dust. Downwind at Anmyon Island SSA was considerably higher, approx. 0.94, but wavelength neutral for dust episodes and spectrally dependent during non dust periods. (5) Satellite retrievals show major aerosol features moving from Asia over the Pacific; however, determining seasonal-average aerosol effects is hampered by sampling frequency and large-scale cloud systems that obscure key parts of aerosol patterns. Preliminary calculations using, satellite-retrieved AOD fields and initial ACE-Asia aerosol properties (including sulfates, soot, and dust) yield clear-sky aerosol radiative effects in the seasonal-average ACE-Asia plume exceeding those of manmade greenhouse gases. Quantifying all-sky direct aerosol radiative effects is complicated by the need to define the height of absorbing aerosols with respect to cloud decks.
“Assessment of the two-way Coupled WRF-CMAQ Model with Observations from the CARES”
The main goal of this assessment is to evaluate the improved aerosol component of two-way coupled WRF-CMAQ model particularly in representing aerosol physical and optical properties by utilizing observations from the Carbonaceous Aerosol and Radiative Effects Study (CARES) in May...
USDA-ARS?s Scientific Manuscript database
One component of the Department of Defense (DoD) pest management system is ultra-low volume (ULV) and/or thermal fog aerosol pesticide application. Despite widespread implementations of this and other components of the system, such as use of repellents and permethrin, US military operations in hot-a...
NASA Astrophysics Data System (ADS)
Christensen, J. N.; Cliff, S. S.; Vancuren, R. A.; Perry, K. D.; Depaolo, D. J.
2006-12-01
Research over the past decade has highlighted the importance of intercontinental transport and exchange of atmospheric aerosols, including soil-derived dust and industrial pollutants. Far-traveled aerosols can affect air quality, atmospheric radiative forcing and cloud formation and can be an important component in soils. Principal component analysis of elemental data for aerosols collected over California has identified a persistent Asian soil dust component that peaks with Asian dust storm events [1]. Isotopic fingerprinting can provide an additional and potentially more discriminating tool for tracing sources of dust. For example, the naturally variable isotopic compositions of Sr and Nd reflect both the geochemistry of the dust source and its pre- weathering geologic history. Sr and Nd isotopic data and chemical data have been collected for a time series of PM2.5 filter samples from Hefei, China taken from eraly April into early May, 2002. This period encompassed a series of dust storms. The sampling time frame overlapped with the 2002 Intercontinental Transport and Chemical Transformation (ITCT-2K2) experiment along the Pacific coast of North America and inland California. Highs in 87Sr/86Sr in the Hefei time series coincide with peaks in Ca and Si representing peaks in mineral particulate loading resulting from passing dust storms. Mixing diagrams combining isotopic data with chemical data identify several components; a high 87Sr/86Sr component that we identify with mineral dust (loess), and two different low 87Sr/86Sr components (local sources and marine aerosol). Using our measured isotopic composition of the "loess" standard CJ-1 [2] as representative of the pure high 87Sr/86Sr component, we calculate 24 hour average loess particulate concentrations in air which range up to 35 micrograms per cubic meter. Marine aerosol was a major component on at least one of the sampled days. The results for the Hefei samples provide a basis for our isotopic study of California mineral aerosols, including the identification and apportionment of local and far-traveled Asian dust components and their variation in time. [1]VanCuren R.A., Cliff, S.S., Perry, K.D. and Jimenez-Cruz, M. (2005) J. Geophys. Res., 110, D09S90, doi: 10.1029/2004JD004973 [2]Nishikawa, M., Hao, Q. and Morita, M. (2000) Global Environ. Res. 4, 1:103-113.
Significance of aerosol radiative effect in energy balance control on global precipitation change
DOE Office of Scientific and Technical Information (OSTI.GOV)
Suzuki, Kentaroh; Stephens, Graeme L.; Golaz, Jean-Christophe
Historical changes of global precipitation in the 20th century simulated by a climate model are investigated. The results simulated with alternate configurations of cloud microphysics are analyzed in the context of energy balance controls on global precipitation, where the latent heat changes associated with the precipitation change is nearly balanced with changes to atmospheric radiative cooling. The atmospheric radiative cooling is dominated by its clear-sky component, which is found to correlate with changes to both column water vapor and aerosol optical depth (AOD). The water vapor-dependent component of the clear-sky radiative cooling is then found to scale with global temperaturemore » change through the Clausius–Clapeyron relationship. This component results in a tendency of global precipitation increase with increasing temperature at a rate of approximately 2%K -1. Another component of the clear-sky radiative cooling, which is well correlated with changes to AOD, is also found to vary in magnitude among different scenarios with alternate configurations of cloud microphysics that controls the precipitation efficiency, a major factor influencing the aerosol scavenging process that can lead to different aerosol loadings. These results propose how different characteristics of cloud microphysics can cause different aerosol loadings that in turn perturb global energy balance to significantly change global precipitation. This implies a possible coupling of aerosol–cloud interaction with aerosol–radiation interaction in the context of global energy balance.« less
Significance of aerosol radiative effect in energy balance control on global precipitation change
Suzuki, Kentaroh; Stephens, Graeme L.; Golaz, Jean-Christophe
2017-10-17
Historical changes of global precipitation in the 20th century simulated by a climate model are investigated. The results simulated with alternate configurations of cloud microphysics are analyzed in the context of energy balance controls on global precipitation, where the latent heat changes associated with the precipitation change is nearly balanced with changes to atmospheric radiative cooling. The atmospheric radiative cooling is dominated by its clear-sky component, which is found to correlate with changes to both column water vapor and aerosol optical depth (AOD). The water vapor-dependent component of the clear-sky radiative cooling is then found to scale with global temperaturemore » change through the Clausius–Clapeyron relationship. This component results in a tendency of global precipitation increase with increasing temperature at a rate of approximately 2%K -1. Another component of the clear-sky radiative cooling, which is well correlated with changes to AOD, is also found to vary in magnitude among different scenarios with alternate configurations of cloud microphysics that controls the precipitation efficiency, a major factor influencing the aerosol scavenging process that can lead to different aerosol loadings. These results propose how different characteristics of cloud microphysics can cause different aerosol loadings that in turn perturb global energy balance to significantly change global precipitation. This implies a possible coupling of aerosol–cloud interaction with aerosol–radiation interaction in the context of global energy balance.« less
NASA Technical Reports Server (NTRS)
Lee, Huikyo; Kalashnikova, Olga V.; Suzuki, Kentaroh; Braverman, Amy; Garay, Michael J.; Kahn, Ralph A.
2016-01-01
The Multi-angle Imaging Spectroradiometer (MISR) Joint Aerosol (JOINT_AS) Level 3 product has provided a global, descriptive summary of MISR Level 2 aerosol optical depth (AOD) and aerosol type information for each month over 16+ years since March 2000. Using Version 1 of JOINT_AS, which is based on the operational (Version 22) MISR Level 2 aerosol product, this study analyzes, for the first time, characteristics of observed and simulated distributions of AOD for three broad classes of aerosols: spherical nonabsorbing, spherical absorbing, and nonspherical - near or downwind of their major source regions. The statistical moments (means, standard deviations, and skew-nesses) and distributions of AOD by components derived from the JOINT_AS are compared with results from two chemistry transport models (CTMs), the Goddard Chemistry Aerosol Radiation and Transport (GOCART) and SPectral RadIatioN-TrAnSport (SPRINTARS). Overall, the AOD distributions retrieved from MISR and modeled by GOCART and SPRINTARS agree with each other in a qualitative sense. Marginal distributions of AOD for each aerosol type in both MISR and models show considerable high positive skewness, which indicates the importance of including extreme AOD events when comparing satellite retrievals with models. The MISR JOINT_AS product will greatly facilitate comparisons between satellite observations and model simulations of aerosols by type.
Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth
NASA Astrophysics Data System (ADS)
Russell, L. M.
2017-12-01
Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray emissions to particles, addressing the persistent question of the sources of cloud condensation nuclei in clean marine conditions.
Seinfeld, John H; Bretherton, Christopher; Carslaw, Kenneth S; Coe, Hugh; DeMott, Paul J; Dunlea, Edward J; Feingold, Graham; Ghan, Steven; Guenther, Alex B; Kahn, Ralph; Kraucunas, Ian; Kreidenweis, Sonia M; Molina, Mario J; Nenes, Athanasios; Penner, Joyce E; Prather, Kimberly A; Ramanathan, V; Ramaswamy, Venkatachalam; Rasch, Philip J; Ravishankara, A R; Rosenfeld, Daniel; Stephens, Graeme; Wood, Robert
2016-05-24
The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.
NASA Technical Reports Server (NTRS)
Seinfeld, John H.; Bretherton, Christopher; Carslaw, Kenneth S.; Coe, Hugh; DeMott, Paul J.; Dunlea, Edward J.; Feingold, Graham; Ghan, Steven; Guenther, Alex B.; Kahn, Ralph;
2016-01-01
The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Parkhurst, MaryAnn; Guilmette, Raymond A.
2009-03-01
The Capstone Depleted Uranium (DU) Aerosol Characterization and Risk Assessment Study was conducted to generate data about DU aerosols generated during the perforation of armored combat vehicles with large-caliber DU penetrators, and to apply the data in assessments of human health risks to personnel exposed to these aerosols, primarily through inhalation, during the 1991 Gulf War or in future military operations. The Capstone study consisted of two components: 1) generating, sampling and characterizing DU aerosols by firing at and perforating combat vehicles and 2) applying the source-term quantities and characteristics of the aerosols to the evaluation of doses and risks.more » This paper reviews the background of the study including the bases for the study, previous reviews of DU particles and health assessments from DU used by the U.S. military, the objectives of the study components, the participants and oversight teams, and the types of exposures it was intended to evaluate. It then discusses exposure scenarios used in the dose and risk assessment and provides an overview of how the field tests and dose and risk assessments were conducted.« less
Seinfeld, John H.; Bretherton, Christopher; Carslaw, Kenneth S.; ...
2016-05-24
The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth’s clouds is the most uncertain component of the overall global radiative forcing from pre-industrial time. General Circulation Models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions but significant challengesmore » exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. Lastly, we suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.« less
NASA Technical Reports Server (NTRS)
Xiao, Qingyang; Wang, Yujie; Chang, Howard H.; Meng, Xia; Geng, Guannan; Lyapustin, Alexei Ivanovich; Liu, Yang
2017-01-01
Satellite aerosol optical depth (AOD) has been used to assess population exposure to fine particulate matter (PM (sub 2.5)). The emerging high-resolution satellite aerosol product, Multi-Angle Implementation of Atmospheric Correction(MAIAC), provides a valuable opportunity to characterize local-scale PM(sub 2.5) at 1-km resolution. However, non-random missing AOD due to cloud snow cover or high surface reflectance makes this task challenging. Previous studies filled the data gap by spatially interpolating neighboring PM(sub 2.5) measurements or predictions. This strategy ignored the effect of cloud cover on aerosol loadings and has been shown to exhibit poor performance when monitoring stations are sparse or when there is seasonal large-scale missngness. Using the Yangtze River Delta of China as an example, we present a Multiple Imputation (MI) method that combines the MAIAC high-resolution satellite retrievals with chemical transport model (CTM) simulations to fill missing AOD. A two-stage statistical model driven by gap-filled AOD, meteorology and land use information was then fitted to estimate daily ground PM(sub 2.5) concentrations in 2013 and 2014 at 1 km resolution with complete coverage in space and time. The daily MI models have an average R(exp 2) of 0.77, with an inter-quartile range of 0.71 to 0.82 across days. The overall Ml model 10-fold cross-validation R(exp 2) (root mean square error) were 0.81 (25 gm(exp 3)) and 0.73 (18 gm(exp 3)) for year 2013 and 2014, respectively. Predictions with only observational AOD or only imputed AOD showed similar accuracy.Comparing with previous gap-filling methods, our MI method presented in this study performed bette rwith higher coverage, higher accuracy, and the ability to fill missing PM(sub 2.5) predictions without ground PM(sub 2.5) measurements. This method can provide reliable PM(sub 2.5)predictions with complete coverage that can reduce biasin exposure assessment in air pollution and health studies.
Materials International Space Station Experiment (MISSE) Arrival
2017-10-02
The Materials International Space Station Experiment-Flight Facility, or MISSE-FF, hardware arrived at the Space Station Processing Facility low bay at NASA's Kennedy Space Center in Florida. Technicians assist as one of the components is lowered and secured onto another MISSE component. MISSE will be used to test various materials and computing elements on the exterior of the space station. They will be exposed to the harsh environment of low-Earth orbit, including to a vacuum, atomic oxygen, ultraviolet radiation, direct sunlight and extreme heat and cold. The experiment will provide a better understanding of material durability, from coatings to electronic sensors, which could be applied to future spacecraft designs. MISSE will be delivered to the space station on a future commercial resupply mission.
Materials International Space Station Experiment (MISSE) Arrival
2017-10-02
The Materials International Space Station Experiment-Flight Facility, or MISSE-FF, hardware arrived at the Space Station Processing Facility low bay at NASA's Kennedy Space Center in Florida. Technicians assist as one of the components is lowered onto another MISSE component. MISSE will be used to test various materials and computing elements on the exterior of the space station. They will be exposed to the harsh environment of low-Earth orbit, including to a vacuum, atomic oxygen, ultraviolet radiation, direct sunlight and extreme heat and cold. The experiment will provide a better understanding of material durability, from coatings to electronic sensors, which could be applied to future spacecraft designs. MISSE will be delivered to the space station on a future commercial resupply mission.
Atmospheric nanoparticles in photocatalytic and thermal production of atmospheric pollutants
DOE Office of Scientific and Technical Information (OSTI.GOV)
Chianelli, R.R.; Yacaman, M.J.
1997-12-31
Atmospheric aerosols which occur above heavily polluted areas such as Mexico City are characterized and found to be complex materials which have the potential to accelerate important ozone-forming reactions photocatalytically and thermocatalytically. In addition, because the particles are respirable, they represent a considerable health hazard. The aerosols consist of two intermixed components. The first component consists of amorphous carbonaceous materials of variable composition with fullerene like materials dispersed throughout. The second component is an inorganic material consisting of nanoparticles of oxides and sulfides supported on clay minerals. This inorganic component has all of the characteristics of an airborne photocatalyst. Nanoparticlesmore » of Fe{sub 2}O{sub 3}, MnO{sub 2} and FeS{sub 2} have demonstrated catalytic properties, particularly when occurring in the nanoparticle range as they do in the subject aerosol materials. These materials have band-gaps which occur in the broad solar spectrum enhancing the photocatalytic adsorption of solar radiation beyond that of the wider band-gap aluminosilicate and titanate materials which also occur in the aerosols. In addition, the materials are acidic and probably are coated with moisture when suspended in air, further enhancing the catalytic ability to crack hydrocarbons and create free radicals.« less
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 and will be useful in reconstructing exposure histories for epidemiological studies across this region.
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 reconstructing exposure histories for epidemiological studies across this region.
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 and will be useful in reconstructing exposure histories for epidemiological studies across this region. PMID:28966552
Ice nucleation by soil dust compared to desert dust aerosols
NASA Astrophysics Data System (ADS)
Moehler, O.; Steinke, I.; Ullrich, R.; Höhler, K.; Schiebel, T.; Hoose, C.; Funk, R.
2015-12-01
A minor fraction of atmospheric aerosol particles, so-called ice-nucleating particles (INPs), initiates the formation of the ice phase in tropospheric clouds and thereby markedly influences the Earth's weather and climate systems. Whether an aerosol particle acts as an INP depends on its size, morphology and chemical compositions. The INP fraction of certain aerosol types also strongly depends on the temperature and the relative humidity. Because both desert dust and soil dust aerosols typically comprise a variety of different particles, it is difficult to assess and predict their contribution to the atmospheric INP abundance. This requires both accurate modelling of the sources and atmospheric distribution of atmospheric dust components and detailed investigations of their ice nucleation activities. The latter can be achieved in laboratory experiments and parameterized for use in weather and climate models as a function of temperature and particle surface area, a parameter called ice-nucleation active site (INAS) density. Concerning ice nucleation activity studies, the soil dust is of particular interest because it contains a significant fraction of organics and biological components, both with the potential for contributing to the atmospheric INP abundance at relatively high temperatures compared to mineral components. First laboratory ice nucleation experiments with a few soil dust samples indicated their INP fraction to be comparable or slightly enhanced to that of desert dust. We have used the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud simulation chamber to study the immersion freezing ability of four different arable soil dusts, sampled in Germany, China and Argentina. For temperatures higher than about -20°C, we found the INP fraction of aerosols generated from these samples by a dry dispersion technique to be significantly higher compared to various desert dust aerosols also investigated in AIDA experiments. In this contribution, we will summarize the experimental results, introduce related INP parameterizations for use in weather and climate models, and briefly discuss possible reasons for the discrepancy between the INP fraction of desert and soil dust aerosols.
NASA Astrophysics Data System (ADS)
ten Brink, Harry; Henzing, Bas; Otjes, René; Weijers, Ernie
2018-01-01
The visibility on New Year's nights in the Netherlands is low during stagnant weather. This is due to the scattering and absorption of light by the aerosol-smoke from the fireworks. We made an assessment of the responsible aerosol-species. The investigation took place during the New Year's night of 2009. Measurements were made at a regional site in the centre of the country away from specific local sources. An Integrating Nephelometer measured the light-scattering by the inherent compounds after removal of water from the aerosol by drying the air. The actual light-scattering was determined in an open-air scatterometer; it was a factor of five higher than the ;dry; value. The difference in actual and ;dry; light-scattering can only be explained by water-uptake of the salty hygroscopic components of the aerosol. This hypothesis is substantiated by measurements of the composition of the aerosol. The size-dependent concentrations of the salty ionic species were determined on-line with a MARGA-;sizer;. These components were for a large part in particles in the size range that most effectively scatter light. The ;dry; light-scattering was exerted by the inorganic salt components and the sooty carbonaceous material alike. However, the salty products from the fireworks are hygroscopic and take up water at the high relative humidities occurring that night. This explains the fivefold larger light-scattering by the wet ambient aerosol as compared to that by the dry aerosol in the integrating nephelometer. The visibility, which is the inverse of the open-air scattering, is thus indirectly governed by the salty products of the fireworks due to their uptake of water. Under stagnant weather conditions during New Year's nights in the Netherlands both the aerosol concentrations and the relative humidity are high; this implies that the ionic species govern the low visibilities in general, be it via their uptake of water.
NASA Technical Reports Server (NTRS)
Peltier, R. E.; Sullivan, A. P.; Weber, R. J.; Brock, C. A.; Wollny, A. G.; Holloway, J. S.; deGouw, J. A.; Warneke, C.
2007-01-01
During the New England Air Quality Study (NEAQS) in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC) of the submicron (PM(sub 1.0)) aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM) was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S.) and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (approximately 60% micro gram /micro gram) and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km), but was significantly higher at altitude layers in the free troposphere (above 2.5 km). A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were largely comprised of organic aerosol components (approximtely 60%).
14 CFR 60.25 - Operation with missing, malfunctioning, or inoperative components.
Code of Federal Regulations, 2010 CFR
2010-01-01
... 14 Aeronautics and Space 2 2010-01-01 2010-01-01 false Operation with missing, malfunctioning, or inoperative components. 60.25 Section 60.25 Aeronautics and Space FEDERAL AVIATION ADMINISTRATION, DEPARTMENT OF TRANSPORTATION (CONTINUED) AIRMEN FLIGHT SIMULATION TRAINING DEVICE INITIAL AND CONTINUING...
14 CFR 60.25 - Operation with missing, malfunctioning, or inoperative components.
Code of Federal Regulations, 2011 CFR
2011-01-01
... 14 Aeronautics and Space 2 2011-01-01 2011-01-01 false Operation with missing, malfunctioning, or inoperative components. 60.25 Section 60.25 Aeronautics and Space FEDERAL AVIATION ADMINISTRATION, DEPARTMENT OF TRANSPORTATION (CONTINUED) AIRMEN FLIGHT SIMULATION TRAINING DEVICE INITIAL AND CONTINUING...
14 CFR 60.25 - Operation with missing, malfunctioning, or inoperative components.
Code of Federal Regulations, 2013 CFR
2013-01-01
... 14 Aeronautics and Space 2 2013-01-01 2013-01-01 false Operation with missing, malfunctioning, or inoperative components. 60.25 Section 60.25 Aeronautics and Space FEDERAL AVIATION ADMINISTRATION, DEPARTMENT OF TRANSPORTATION (CONTINUED) AIRMEN FLIGHT SIMULATION TRAINING DEVICE INITIAL AND CONTINUING...
14 CFR 60.25 - Operation with missing, malfunctioning, or inoperative components.
Code of Federal Regulations, 2012 CFR
2012-01-01
... 14 Aeronautics and Space 2 2012-01-01 2012-01-01 false Operation with missing, malfunctioning, or inoperative components. 60.25 Section 60.25 Aeronautics and Space FEDERAL AVIATION ADMINISTRATION, DEPARTMENT OF TRANSPORTATION (CONTINUED) AIRMEN FLIGHT SIMULATION TRAINING DEVICE INITIAL AND CONTINUING...
14 CFR 60.25 - Operation with missing, malfunctioning, or inoperative components.
Code of Federal Regulations, 2014 CFR
2014-01-01
... 14 Aeronautics and Space 2 2014-01-01 2014-01-01 false Operation with missing, malfunctioning, or inoperative components. 60.25 Section 60.25 Aeronautics and Space FEDERAL AVIATION ADMINISTRATION, DEPARTMENT OF TRANSPORTATION (CONTINUED) AIRMEN FLIGHT SIMULATION TRAINING DEVICE INITIAL AND CONTINUING...
NASA Astrophysics Data System (ADS)
Ran, L.; Deng, Z. Z.; Wang, P. C.; Xia, X. A.
2016-10-01
Light-absorbing components of atmospheric aerosols have gained particular attention in recent years due to their climatic and environmental effects. Based on two-year measurements of aerosol absorption at seven wavelengths, aerosol absorption properties and black carbon (BC) were investigated in the North China Plain (NCP), one of the most densely populated and polluted regions in the world. Aerosol absorption was stronger in fall and the heating season (from November to March) than in spring and summer at all seven wavelengths. Similar spectral dependence of aerosol absorption was observed in non-heating seasons despite substantially strong absorption in fall. With an average absorption Angström exponent (α) of 1.36 in non-heating seasons, freshly emitted BC from local fossil fuel burning was thought to be the major component of light-absorbing aerosols. In the heating season, strong ultraviolet absorption led to an average α of 1.81, clearly indicating the importance of non-BC light-absorbing components, which were possibly from coal burning for domestic heating and aging processes on a regional scale. Diurnally, the variation of BC mass concentrations experienced a double-peak pattern with a higher level at night throughout the year. However, the diurnal cycle of α in the heating season was distinctly different from that in non-heating seasons. α peaked in the late afternoon in non-heating seasons with concomitantly observed low valley in BC mass concentrations. In contrast, α peaked around the midnight in the heating season and lowered down during the daytime. The relationship of aerosol absorption and winds in non-heating seasons also differed from that in the heating season. BC mass concentrations declined while α increased with increasing wind speed in non-heating seasons, which suggested elevated non-BC light absorbers in transported aged aerosols. No apparent dependence of α on wind speed was found in the heating season, probably due to well mixed regional pollution. Pollution episodes were mostly encountered under low winds and had a low level of α, implying aerosol absorption should be largely attributed to freshly emitted BC from local sources under such conditions. Extensive field campaigns and long-term chemical and optical measurements of light-absorbing aerosols are needed in the future to further advance our understanding on optical properties of light-absorbing aerosols and their radiative forcing in this region.
Ensemble-Based Assimilation of Aerosol Observations in GEOS-5
NASA Technical Reports Server (NTRS)
Buchard, V.; Da Silva, A.
2016-01-01
MERRA-2 is the latest Aerosol Reanalysis produced at NASA's Global Modeling Assimilation Office (GMAO) from 1979 to present. This reanalysis is based on a version of the GEOS-5 model radiatively coupled to GOCART aerosols and includes assimilation of bias corrected Aerosol Optical Depth (AOD) from AVHRR over ocean, MODIS sensors on both Terra and Aqua satellites, MISR over bright surfaces and AERONET data. In order to assimilate lidar profiles of aerosols, we are updating the aerosol component of our assimilation system to an Ensemble Kalman Filter (EnKF) type of scheme using ensembles generated routinely by the meteorological assimilation. Following the work performed with the first NASA's aerosol reanalysis (MERRAero), we first validate the vertical structure of MERRA-2 aerosol assimilated fields using CALIOP data over regions of particular interest during 2008.
Strategies to Reduce Tin and Other Metals in Electronic Cigarette Aerosol
Williams, Monique; To, An; Bozhilov, Krassimir; Talbot, Prue
2015-01-01
Background Metals are present in electronic cigarette (EC) fluid and aerosol and may present health risks to users. Objective The objective of this study was to measure the amounts of tin, copper, zinc, silver, nickel and chromium in the aerosol from four brands of EC and to identify the sources of these metals by examining the elemental composition of the atomizer components. Methods Four brands of popular EC were dissected and the cartomizers were examined microscopically. Elemental composition of cartomizer components was determined using integrated energy dispersive X-ray microanalysis, and the concentrations of the tin, copper, zinc silver, nickel, and chromium in the aerosol were determined for each brand using inductively coupled plasma optical emission spectroscopy. Results All filaments were made of nickel and chromium. Thick wires were copper coated with either tin or silver. Wires were joined to each other by tin solder, brazing, or by brass clamps. High concentrations of tin were detected in the aerosol when tin solder joints were friable. Tin coating on copper wires also contributed to tin in the aerosol. Conclusions Tin concentrations in EC aerosols varied both within and between brands. Tin in aerosol was reduced by coating the thick wire with silver rather than tin, placing stable tin solder joints outside the atomizing chamber, joining wires with brass clamps or by brazing rather than soldering wires. These data demonstrate the feasibility of removing tin and other unwanted metals from EC aerosol by altering designs and using materials of suitable quality. PMID:26406602
Climatological Aspects of the Optical Properties of Fine/Coarse Mode Aerosol Mixtures
NASA Technical Reports Server (NTRS)
Eck, T. F.; Holben, B. N.; Sinyuk, A.; Pinker, R. T.; Goloub, P.; Chen, H.; Chatenet, B.; Li, Z.; Singh, R. P.; Tripathi, S.N.;
2010-01-01
Aerosol mixtures composed of coarse mode desert dust combined with fine mode combustion generated aerosols (from fossil fuel and biomass burning sources) were investigated at three locations that are in and/or downwind of major global aerosol emission source regions. Multiyear monitoring data at Aerosol Robotic Network sites in Beijing (central eastern China), Kanpur (Indo-Gangetic Plain, northern India), and Ilorin (Nigeria, Sudanian zone of West Africa) were utilized to study the climatological characteristics of aerosol optical properties. Multiyear climatological averages of spectral single scattering albedo (SSA) versus fine mode fraction (FMF) of aerosol optical depth at 675 nm at all three sites exhibited relatively linear trends up to 50% FMF. This suggests the possibility that external linear mixing of both fine and coarse mode components (weighted by FMF) dominates the SSA variation, where the SSA of each component remains relatively constant for this range of FMF only. However, it is likely that a combination of other factors is also involved in determining the dynamics of SSA as a function of FMF, such as fine mode particles adhering to coarse mode dust. The spectral variation of the climatological averaged aerosol absorption optical depth (AAOD) was nearly linear in logarithmic coordinates over the wavelength range of 440-870 nm for both the Kanpur and Ilorin sites. However, at two sites in China (Beijing and Xianghe), a distinct nonlinearity in spectral AAOD in logarithmic space was observed, suggesting the possibility of anomalously strong absorption in coarse mode aerosols increasing the 870 nm AAOD.
Changes in organic aerosol composition with aging inferred from aerosol mass spectra
NASA Astrophysics Data System (ADS)
Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.
2011-03-01
Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C). Heald et al. (2010) suggested that the bulk composition of OA line up in the Van Krevelen diagram with a slope ~ -1; such slope can potentially arise from the physical mixing of HOA and OOA, and/or from chemical aging of these components. In this study, we find that the OOA components from all sites occupy an area in the Van Krevelen space, with the evolution of OOA following a shallower slope of ~ -0.5, consistent with the additions of both acid and alcohol functional groups without fragmentation, and/or the addition of acid groups with C-C bond breakage. The importance of acid formation in OOA evolution is consistent with increasing f44 in the triangle plot with photochemical age. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.
NASA Astrophysics Data System (ADS)
Wang, Shuo; Zhao, Weixiong; Xu, Xuezhe; Fang, Bo; Zhang, Qilei; Qian, Xiaodong; Zhang, Weijun; Chen, Weidong; Pu, Wei; Wang, Xin
2017-11-01
Seasonal dependence of the columnar aerosol optical and chemical properties on regional transport in Beijing over 10 years (from January 2005 to December 2014) were analyzed by using the ground-based remote sensing combined with backward trajectory analysis. Daily air mass backward trajectories terminated in Beijing were computed with HYSPLIT-4 model and were categorized into five clusters. The columnar mass concentrations of black carbon (BC), brown carbon (BrC), dust (DU), aerosol water content (AW), and ammonium sulfate like aerosol (AS) of each cluster were retrieved from the optical data obtained from the Aerosol Robotic NETwork (AERONET) with five-component model. It was found that the columnar aerosol properties in different seasons were changed, and they were related to the air mass origins. In spring, aerosol was dominated by coarse particles. Summer was characterized by higher single scattering albedo (SSA), lower real part of complex refractive index (n), and obvious hygroscopic growth due to humid air from the south. During autumn and winter, there was an observable increase in absorption aerosol optical thickness (AAOT) and the imaginary part of complex refraction (k), with high levels of retrieved BC and BrC. However, concentrations of BC showed less dependence on the clusters during the two seasons owing to the widely spread coal heating in north China.
Testing of NASA LaRC Materials under MISSE 6 and MISSE 7 Missions
NASA Technical Reports Server (NTRS)
Prasad, Narasimha S.
2009-01-01
The objective of the Materials International Space Station Experiment (MISSE) is to study the performance of novel materials when subjected to the synergistic effects of the harsh space environment for several months. MISSE missions provide an opportunity for developing space qualifiable materials. Two lasers and a few optical components from NASA Langley Research Center (LaRC) were included in the MISSE 6 mission for long term exposure. MISSE 6 items were characterized and packed inside a ruggedized Passive Experiment Container (PEC) that resembles a suitcase. The PEC was tested for survivability due to launch conditions. MISSE 6 was transported to the international Space Station (ISS) via STS 123 on March 11. 2008. The astronauts successfully attached the PEC to external handrails of the ISS and opened the PEC for long term exposure to the space environment. The current plan is to bring the MISSE 6 PEC back to the Earth via STS 128 mission scheduled for launch in August 2009. Currently, preparations for launching the MISSE 7 mission are progressing. Laser and lidar components assembled on a flight-worthy platform are included from NASA LaRC. MISSE 7 launch is scheduled to be launched on STS 129 mission. This paper will briefly review recent efforts on MISSE 6 and MISSE 7 missions at NASA Langley Research Center (LaRC).
A Climatology of Global Aerosol Mixtures to Support Sentinel-5P and Earthcare Mission Applications
NASA Astrophysics Data System (ADS)
Taylor, M.; Kazadzis, S.; Amaridis, V.; Kahn, R. A.
2015-11-01
Since constraining aerosol type with satellite remote sensing continues to be a challenge, we present a newly derived global climatology of aerosol mixtures to support atmospheric composition studies that are planned for Sentinel-5P and EarthCARE.The global climatology is obtained via application of iterative cluster analysis to gridded global decadal and seasonal mean values of the aerosol optical depth (AOD) of sulfate, biomass burning, mineral dust and marine aerosol as a proportion of the total AOD at 500nm output from the Goddard Chemistry Aerosol Radiation and Transport (GOCART). For both the decadal and seasonal means, the number of aerosol mixtures (clusters) identified is ≈10. Analysis of the percentage contribution of the component aerosol types to each mixture allowed development of a straightforward naming convention and taxonomy, and assignment of primary colours for the generation of true colour-mixing and easy-to-interpret maps of the spatial distribution of clusters across the global grid. To further help characterize the mixtures, aerosol robotic network (AERONET) Level 2.0 Version 2 inversion products were extracted from each cluster‟s spatial domain and used to estimate climatological values of key optical and microphysical parameters.The aerosol type climatology represents current knowledge that would be enhanced, possibly corrected, and refined by high temporal and spectral resolution, cloud-free observations produced by Sentinel-5P and EarthCARE instruments. The global decadal mean and seasonal gridded partitions comprise a preliminary reference framework and global climatology that can help inform the choice of components and mixtures in aerosol retrieval algorithms used by instruments such as TROPOMI and ATLID, and to test retrieval results.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fast, J; Zhang, Q; Tilp, A
Significantly improved returns in their aerosol chemistry data can be achieved via the development of a value-added product (VAP) of deriving OA components, called Organic Aerosol Components (OACOMP). OACOMP is primarily based on multivariate analysis of the measured organic mass spectral matrix. The key outputs of OACOMP are the concentration time series and the mass spectra of OA factors that are associated with distinct sources, formation and evolution processes, and physicochemical properties.
Aerosol retrieval experiments in the ESA Aerosol_cci project
NASA Astrophysics Data System (ADS)
Holzer-Popp, T.; de Leeuw, G.; Griesfeller, J.; Martynenko, D.; Klüser, L.; Bevan, S.; Davies, W.; Ducos, F.; Deuzé, J. L.; Graigner, R. G.; Heckel, A.; von Hoyningen-Hüne, W.; Kolmonen, P.; Litvinov, P.; North, P.; Poulsen, C. A.; Ramon, D.; Siddans, R.; Sogacheva, L.; Tanre, D.; Thomas, G. E.; Vountas, M.; Descloitres, J.; Griesfeller, J.; Kinne, S.; Schulz, M.; Pinnock, S.
2013-08-01
Within the ESA Climate Change Initiative (CCI) project Aerosol_cci (2010-2013), algorithms for the production of long-term total column aerosol optical depth (AOD) datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1) a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2) a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome) applied to four months of global data to identify mature algorithms, and (3) a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008) of data: qualitatively by inspection of monthly mean AOD maps and quantitatively by comparing daily gridded satellite data against daily averaged AERONET sun photometer observations for the different versions of each algorithm globally (land and coastal) and for three regions with different aerosol regimes. The analysis allowed for an assessment of sensitivities of all algorithms, which helped define the best algorithm versions for the subsequent round robin exercise; all algorithms (except for MERIS) showed some, in parts significant, improvement. In particular, using common aerosol components and partly also a priori aerosol-type climatology is beneficial. On the other hand the use of an AATSR-based common cloud mask meant a clear improvement (though with significant reduction of coverage) for the MERIS standard product, but not for the algorithms using AATSR. It is noted that all these observations are mostly consistent for all five analyses (global land, global coastal, three regional), which can be understood well, since the set of aerosol components defined in Sect. 3.1 was explicitly designed to cover different global aerosol regimes (with low and high absorption fine mode, sea salt and dust).
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 HR-ToF-AMS. The measurements are interpreted in the context of the measurements over tropical rain forest at Danum and aircraft measurements across Sabah.
Three-beam aerosol backscatter correlation lidar for wind profiling
NASA Astrophysics Data System (ADS)
Prasad, Narasimha S.; Radhakrishnan Mylapore, Anand
2017-03-01
The development of a three-beam aerosol backscatter correlation (ABC) light detection and ranging (lidar) to measure wind characteristics for wake vortex and plume tracking applications is discussed. This is a direct detection elastic lidar that uses three laser transceivers, operating at 1030-nm wavelength with ˜10-kHz pulse repetition frequency and nanosec class pulse widths, to directly obtain three components of wind velocities. By tracking the motion of aerosol structures along and between three near-parallel laser beams, three-component wind speed profiles along the field-of-view of laser beams are obtained. With three 8-in. transceiver modules, placed in a near-parallel configuration on a two-axis pan-tilt scanner, the lidar measures wind speeds up to 2 km away. Optical flow algorithms have been adapted to obtain the movement of aerosol structures between the beams. Aerosol density fluctuations are cross-correlated between successive scans to obtain the displacements of the aerosol features along the three axes. Using the range resolved elastic backscatter data from each laser beam, which is scanned over the volume of interest, a three-dimensional map of aerosol density can be generated in a short time span. The performance of the ABC wind lidar prototype, validated using sonic anemometer measurements, is discussed.
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.
NASA Astrophysics Data System (ADS)
Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.
2013-11-01
Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.
NASA Astrophysics Data System (ADS)
Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.
2013-06-01
Multiwavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentrations profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analyzed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical to distinguish between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.
NASA Astrophysics Data System (ADS)
Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos
2016-07-01
Emissions of organic compounds from biomass, biofuel, and fossil fuel combustion strongly influence the global atmospheric aerosol load. Some of the organics are directly released as primary organic aerosol (POA). Most are emitted in the gas phase and undergo chemical transformations (i.e., oxidation by hydroxyl radical) and form secondary organic aerosol (SOA). In this work we use the global chemistry climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) with a computationally efficient module for the description of organic aerosol (OA) composition and evolution in the atmosphere (ORACLE). The tropospheric burden of open biomass and anthropogenic (fossil and biofuel) combustion particles is estimated to be 0.59 and 0.63 Tg, respectively, accounting for about 30 and 32 % of the total tropospheric OA load. About 30 % of the open biomass burning and 10 % of the anthropogenic combustion aerosols originate from direct particle emissions, whereas the rest is formed in the atmosphere. A comprehensive data set of aerosol mass spectrometer (AMS) measurements along with factor-analysis results from 84 field campaigns across the Northern Hemisphere are used to evaluate the model results. Both the AMS observations and the model results suggest that over urban areas both POA (25-40 %) and SOA (60-75 %) contribute substantially to the overall OA mass, whereas further downwind and in rural areas the POA concentrations decrease substantially and SOA dominates (80-85 %). EMAC does a reasonable job in reproducing POA and SOA levels during most of the year. However, it tends to underpredict POA and SOA concentrations during winter indicating that the model misses wintertime sources of OA (e.g., residential biofuel use) and SOA formation pathways (e.g., multiphase oxidation).
Aerosol indirect effect on tropospheric ozone via lightning
NASA Astrophysics Data System (ADS)
Yuan, Tianle; Remer, Lorraine A.; Bian, Huisheng; Ziemke, Jerald R.; Albrecht, Rachel; Pickering, Kenneth E.; Oreopoulos, Lazaros; Goodman, Steven J.; Yu, Hongbin; Allen, Dale J.
2012-09-01
Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. Inadequate understanding of processes related to O3 production, in particular those natural ones such as lightning, contributes to this uncertainty. Here we demonstrate a new effect of aerosol particles on O3production by affecting lightning activity and lightning-generated NOx (LNOx). We find that lightning flash rate increases at a remarkable rate of 30 times or more per unit of aerosol optical depth. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses show O3is increased as a result of aerosol-induced increase in lightning and LNOx, which is supported by modle simulations with prescribed lightning change. O3production increase from this aerosol-lightning-ozone link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. In the face of anthropogenic aerosol increase our findings suggest that lightning activity, LNOx and O3, especially in the upper troposphere, have all increased substantially since preindustrial time due to the proposed aerosol-lightning-ozone link, which implies a stronger O3 historical radiative forcing. Aerosol forcing therefore has a warming component via its effect on O3 production and this component has mostly been ignored in previous studies of climate forcing related to O3and aerosols. Sensitivity simulations suggest that 4-8% increase of column tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Longo, Amelia F.; Feng, Yan; Lai, Barry
Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation statemore » became more reduced, and aerosol acidity increased. As a result, atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.« less
Influence of atmospheric processes on the solubility and composition of iron in Saharan dust
Longo, Amelia F.; Feng, Yan; Lai, Barry; ...
2016-06-10
Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation statemore » became more reduced, and aerosol acidity increased. As a result, atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.« less
Influence of Atmospheric Processes on the Solubility and Composition of Iron in Saharan Dust.
Longo, Amelia F; Feng, Yan; Lai, Barry; Landing, William M; Shelley, Rachel U; Nenes, Athanasios; Mihalopoulos, Nikolaos; Violaki, Kalliopi; Ingall, Ellery D
2016-07-05
Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet-chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated the aerosol iron in Mediterranean samples. In Atlantic samples, iron(II and III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation state became more reduced, and aerosol acidity increased. Atmospheric processing including acidic reactions and photoreduction likely influence the form of iron minerals and oxidation state in Saharan dust aerosols and contribute to increases in aerosol-iron solubility.
Maritime Aerosol Network (MAN) as a Component of AERONET
NASA Technical Reports Server (NTRS)
Smirnov, A.; Holben, B. N.; Slutsker, I.; Giles, D. M.; McClain, C. R.; Eck, T. F.; Sakerin, S. M.; Macke, A.; Croot, P.; Zibordi, G.;
2008-01-01
The World Ocean produces a large amount of natural aerosols that have all impact on the Earth's albedo and climate. Sea-salt is the major contributor to aerosol optical depth over the oceans. [Mahowald et al. 2006; Chin et al. 2002; Satheesh et al. 1999; Winter and Chylek, 1997] and therefore affects the radiative balance over the ocean through the direct [Haywood et al. 1999] and indirect aerosol effect [O'Dowd et al. 1999]. Aerosols over the oceans (produced marine and advected from land sources) are important for various atmospheric processes [Lewis and Schwartz, 2004] and remote sensing studies [Gordon, 1997].
Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq
NASA Astrophysics Data System (ADS)
Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.
2015-04-01
Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.
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.
NASA Astrophysics Data System (ADS)
Hara, Keiichiro; Matoba, Sumito; Hirabayashi, Motohiro; Yamasaki, Tetsuhide
2017-07-01
Sea salts and halogens in aerosols, frost flowers, and brine play an important role in atmospheric chemistry in polar regions. Simultaneous sampling and observations of frost flowers, brine, and aerosol particles were conducted around Siorapaluk in northwestern Greenland during December 2013 to March 2014. Results show that water-soluble frost flower and brine components are sea-salt components (e.g., Na+, Cl-, Mg2+, K+, Ca2+, Br-, and iodine). Concentration factors of sea-salt components of frost flowers and brine relative to seawater were 1.14-3.67. Sea-salt enrichment of Mg2+, K+, Ca2+, and halogens (Cl-, Br-, and iodine) in frost flowers is associated with sea-salt fractionation by precipitation of mirabilite and hydrohalite. High aerosol number concentrations correspond to the occurrence of higher abundance of sea-salt particles in both coarse and fine modes, and blowing snow and strong winds. Aerosol number concentrations, particularly in coarse mode, are increased considerably by release from the sea-ice surface under strong wind conditions. Sulfate depletion by sea-salt fractionation was found to be limited in sea-salt aerosols because of the presence of non-sea-salt (NSS) SO42-. However, coarse and fine sea-salt particles were found to be rich in Mg. Strong Mg enrichment might be more likely to proceed in fine sea-salt particles. Magnesium-rich sea-salt particles might be released from the surface of snow and slush layer (brine) on sea ice and frost flowers. Mirabilite-like and ikaite-like particles were identified only in aerosol samples collected near new sea-ice areas. From the field evidence and results from earlier studies, we propose and describe sea-salt cycles in seasonal sea-ice areas.
On the mixing and evaporation of secondary organic aerosol components.
Loza, Christine L; Coggon, Matthew M; Nguyen, Tran B; Zuend, Andreas; Flagan, Richard C; Seinfeld, John H
2013-06-18
The physical state and chemical composition of an organic aerosol affect its degree of mixing and its interactions with condensing species. We present here a laboratory chamber procedure for studying the effect of the mixing of organic aerosol components on particle evaporation. The procedure is applied to the formation of secondary organic aerosol (SOA) from α-pinene and toluene photooxidation. SOA evaporation is induced by heating the chamber aerosol from room temperature (25 °C) to 42 °C over 7 h and detected by a shift in the peak diameter of the SOA size distribution. With this protocol, α-pinene SOA is found to be more volatile than toluene SOA. When SOA is formed from the two precursors sequentially, the evaporation behavior of the SOA most closely resembles that of SOA from the second parent hydrocarbon, suggesting that the structure of the mixed SOA resembles a core of SOA from the initial precursor coated by a layer of SOA from the second precursor. Such a core-and-shell configuration of the organic aerosol phases implies limited mixing of the SOA from the two precursors on the time scale of the experiments, consistent with a high viscosity of at least one of the phases.
NASA Technical Reports Server (NTRS)
Petrenko, Mariya; Kahn, Ralph; Chin, Mian; Limbacher, James
2017-01-01
Simulations of biomass burning (BB) emissions in global chemistry and aerosol transport models depend on external inventories, which provide location and strength of burning aerosol sources. Our previous work (Petrenko et al., 2012) shows that satellite snapshots of aerosol optical depth (AOD) near the emitted smoke plume can be used to constrain model-simulated AOD, and effectively, the assumed source strength. We now refine the satellite-snapshot method and investigate applying simple multiplicative emission correction factors for the widely used Global Fire Emission Database version 3 (GFEDv3) emission inventory can achieve regional-scale consistency between MODIS AOD snapshots and the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. The model and satellite AOD are compared over a set of more than 900 BB cases observed by the MODIS instrument during the 2004, and 2006-2008 biomass burning seasons. The AOD comparison presented here shows that regional discrepancies between the model and satellite are diverse around the globe yet quite consistent within most ecosystems. Additional analysis of including small fire emission correction shows the complimentary nature of correcting for source strength and adding missing sources, and also indicates that in some regions other factors may be significant in explaining model-satellite discrepancies. This work sets the stage for a larger intercomparison within the Aerosol Inter-comparisons between Observations and Models (AeroCom) multi-model biomass burning experiment. We discuss here some of the other possible factors affecting the remaining discrepancies between model simulations and observations, but await comparisons with other AeroCom models to draw further conclusions.
NASA Astrophysics Data System (ADS)
Rao, R. R.
2015-12-01
Aerosol radiative forcing estimates with high certainty are required in climate change studies. The approach in estimating the aerosol radiative forcing by using the chemical composition of aerosols is not effective as the chemical composition data with radiative properties are not widely available. In this study we look into the approach where ground based spectral radiation flux measurements along with an RT model is used to estimate radiative forcing. Measurements of spectral flux were made using an ASD spectroradiometer with 350 - 1050 nm wavelength range and 3nm resolution for around 54 clear-sky days during which AOD range was around 0.1 to 0.7. Simultaneous measurements of black carbon were also made using Aethalometer (Magee Scientific) which ranged from around 1.5 ug/m3 to 8 ug/m3. All the measurements were made in the campus of Indian Institute of Science which is in the heart of Bangalore city. The primary study involved in understanding the sensitivity of spectral flux to change in the mass concentration of individual aerosol species (Optical properties of Aerosols and Clouds -OPAC classified aerosol species) using the SBDART RT model. This made us clearly distinguish the region of influence of different aerosol species on the spectral flux. Following this, a new technique has been introduced to estimate an optically equivalent mixture of aerosol species for the given location. The new method involves an iterative process where the mixture of aerosol species are changed in OPAC model and RT model is run as long as the mixture which mimics the measured spectral flux within 2-3% deviation from measured spectral flux is obtained. Using the optically equivalent aerosol mixture and RT model aerosol radiative forcing is estimated. The new method is limited to clear sky scenes and its accuracy to derive an optically equivalent aerosol mixture reduces when diffuse component of flux increases. Our analysis also showed that direct component of spectral flux is more sensitive to different aerosol species than total spectral flux which was also supported by our observed data.
Mason, B J; Cotterell, M I; Preston, T C; Orr-Ewing, A J; Reid, J P
2015-06-04
We present measurements of the evolving extinction cross sections of individual aerosol particles (spanning 700-2500 nm in radius) during the evaporation of volatile components or hygroscopic growth using a combination of a single particle trap formed from a Bessel light beam and cavity ring-down spectroscopy. For single component organic aerosol droplets of 1,2,6-hexanetriol, polyethylene glycol 400, and glycerol, the slow evaporation of the organic component (over time scales of 1000 to 10,000 s) leads to a time-varying size and extinction cross section that can be used to estimate the refractive index of the droplet. Measurements on binary aqueous-inorganic aerosol droplets containing one of the inorganic solutes ammonium bisulfate, ammonium sulfate, sodium nitrate, or sodium chloride (over time scales of 1000 to 15,000 s) under conditions of changing relative humidity show that extinction cross-section measurements are consistent with expectations from accepted models for the variation in droplet refractive index with hygroscopic growth. In addition, we use these systems to establish an experimental protocol for future single particle extinction measurements. The advantages of mapping out the evolving light extinction cross-section of an individual particle over extended time frames accompanied by hygroscopic cycling or component evaporation are discussed.
Lerner, Chad A.; Sundar, Isaac K.; Watson, Richard M.; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J.; Robinson, Risa; McIntosh, Scott; Rahman, Irfan
2014-01-01
To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. PMID:25577651
NASA Astrophysics Data System (ADS)
Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.
2017-12-01
NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.
Informing Aerosol Transport Models With Satellite Multi-Angle Aerosol Measurements
NASA Technical Reports Server (NTRS)
Limbacher, J.; Patadia, F.; Petrenko, M.; Martin, M. Val; Chin, M.; Gaitley, B.; Garay, M.; Kalashnikova, O.; Nelson, D.; Scollo, S.
2011-01-01
As the aerosol products from the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR) mature, we are placing greater focus on ways of using the aerosol amount and type data products, and aerosol plume heights, to constrain aerosol transport models. We have demonstrated the ability to map aerosol air-mass-types regionally, and have identified product upgrades required to apply them globally, including the need for a quality flag indicating the aerosol type information content, that varies depending upon retrieval conditions. We have shown that MISR aerosol type can distinguish smoke from dust, volcanic ash from sulfate and water particles, and can identify qualitative differences in mixtures of smoke, dust, and pollution aerosol components in urban settings. We demonstrated the use of stereo imaging to map smoke, dust, and volcanic effluent plume injection height, and the combination of MISR and MODIS aerosol optical depth maps to constrain wildfire smoke source strength. This talk will briefly highlight where we stand on these application, with emphasis on the steps we are taking toward applying the capabilities toward constraining aerosol transport models, planet-wide.
Evolution of aerosol loading in Santiago de Chile between 1997 and 2014
NASA Astrophysics Data System (ADS)
Pistone, Kristina; Gallardo, Laura
2015-04-01
While aerosols produced by major cities are a significant component of anthropogenic climate forcing as well as an important factor in public health, many South American cities have not been a major focus of aerosol studies due in part to relatively few long-term observations in the region. Here we present a synthesis of the available data for the emerging megacity of Santiago, Chile. We report new results from a recent NASA AERONET (AErosol RObotic NETwork) site in the Santiago basin, combining these with previous AERONET observations in Santiago as well as with a new assessment of the 11-station air quality monitoring network currently administered by the Chilean Environment Ministry (MMA, Ministerio del Medio Ambiente) to assess changes in aerosol composition since 1997. While the average surface concentration of pollution components (specifically PM2.5 and PM10) has decreased, no significant change in total aerosol optical depth was observed. However, changes in aerosol size and composition are suggested by the proxy measurements. Previous studies have revealed limitations in purely satellite-based studies over Santiago due to biases from high surface reflection in the region, particularly in summer months (e.g. Escribano et al 2014). To overcome this difficulty and certain limitations in the air quality data, we next incorporate analysis of aerosol products from the Multi-angle Imaging SpectroRadiometer (MISR) instrument along with those from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument, both on NASA's Terra satellite, to better quantify the high bias of MODIS. Thus incorporating these complementary datasets, we characterize the aerosol over Santiago over the period 1997 to 2014, including the evolution of aerosol properties over time and seasonal dependencies in the observed trends. References: Escribano et al (2014), "Satellite Retrievals of Aerosol Optical Depth over a Subtropical Urban Area: The Role of Stratification and Surface Reflectance," Aerosol and Air Quality Research, doi:10.4209/aaqr.2013.03.0082.
What types of Level 3 products are available?
Atmospheric Science Data Center
2016-02-19
The Level 3 Component Global Georectified Radiation Product (CGGRP), Component Global Land Surface Product (CGLS), Component Global Aerosol Product (CGAS), and Component Global Albedo Product (CGAL) are generated for daily, monthly, quarterly,...
Laskina, Olga; Morris, Holly S; Grandquist, Joshua R; Qin, Zhen; Stone, Elizabeth A; Tivanski, Alexei V; Grassian, Vicki H
2015-05-14
Understanding the interactions of water with atmospheric aerosols is crucial for determining the size, physical state, reactivity, and climate impacts of this important component of the Earth's atmosphere. Here we show that water uptake and hygroscopic growth of multicomponent, atmospherically relevant particles can be size dependent when comparing 100 nm versus ca. 6 μm sized particles. It was determined that particles composed of ammonium sulfate with succinic acid and of a mixture of chlorides typical of the marine environment show size-dependent hygroscopic behavior. Microscopic analysis of the distribution of components within the aerosol particles show that the size dependence is due to differences in the mixing state, that is, whether particles are homogeneously mixed or phase separated, for different sized particles. This morphology-dependent hygroscopicity has consequences for heterogeneous atmospheric chemistry as well as aerosol interactions with electromagnetic radiation and clouds.
Missing data is a common problem in the application of statistical techniques. In principal component analysis (PCA), a technique for dimensionality reduction, incomplete data points are either discarded or imputed using interpolation methods. Such approaches are less valid when ...
Hannan, M A; Chowdhury, M T H; Khan, M A I; Chowdhury, A F M A; Shahidullah, K M; Saha, A K; Anjum, A
2014-08-01
A cross-sectional survey, using cluster sampling technique, of slum population, was done to explore the oral health status and the prevalence of common oral diseases. A close ended questionnaire comprising Decayed, Missing and Filled Teeth (DMFT) Index, Gingival Index (Löe and Silness) and Plaque Index was applied to evaluate and record oral diseases, in both male and female population, covering a wide range of age groups. Clinical examination was carried out in different shum set ups, including slum schools by trained and calibrated examiners. Three thousand nine hundred and four (3904) slum dwellers participated in the survey. Prevalence of Caries was expressed in mean DMFT, recording of gingival status followed the method of Löe and Silness, oral hygiene status was evaluated using Plaque index. Mean decayed component, of the DMFT, was significantly higher than filling and missing component. Both decayed and missing components showed increasing trend, and filling components decreased as the age progressed. Prevalence of gingivitis and plaque accumulation was remarkably high among slum dwellers. Significantly high level of common oral diseases was found among Tongi slum dwellers.
NASA Technical Reports Server (NTRS)
Jongeward, Andrew R.; Li, Zhanqing; He, Hao; Xiong, Xiaoxiong
2016-01-01
Aerosols contribute to Earths radiative budget both directly and indirectly, and large uncertainties remain in quantifying aerosol effects on climate. Variability in aerosol distribution and properties, as might result from changing emissions and transport processes, must be characterized. In this study, variations in aerosol loading across the eastern seaboard of theUnited States and theNorthAtlanticOcean during 2002 to 2012 are analyzed to examine the impacts of anthropogenic emission control measures using monthly mean data from MODIS, AERONET, and IMPROVE observations and Goddard Chemistry Aerosol Radiation and Transport (GOCART) model simulation.MODIS observes a statistically significant negative trend in aerosol optical depth (AOD) over the midlatitudes (-0.030 decade(sup-1)). Correlation analyses with surface AOD from AERONET sites in the upwind region combined with trend analysis from GOCART component AOD confirm that the observed decrease in the midlatitudes is chiefly associated with anthropogenic aerosols that exhibit significant negative trends from the eastern U.S. coast extending over the western North Atlantic. Additional analysis of IMPROVE surface PM(sub 2.5) observations demonstrates statistically significant negative trends in the anthropogenic components with decreasing mass concentrations over the eastern United States. Finally, a seasonal analysis of observational datasets is performed. The negative trend seen by MODIS is strongest during spring (MAM) and summer (JJA) months. This is supported by AERONET seasonal trends and is identified from IMPROVE seasonal trends as resulting from ammonium sulfate decreases during these seasons.
NASA Astrophysics Data System (ADS)
Topping, David; Barley, Mark; McFiggans, Gordon; Aumont, Bernard
2016-04-01
The many thousands of individual aerosol components ensure that explicit manual calculation of properties that influence their environmental impacts is laborious and time-consuming. The emergence of explicit automatic mechanism generation techniques, including up to many millions of individual gas phase products as aerosol precursors, renders manual calculations impossible and automation is necessary. It can be difficult to establish what factors are responsible for the outcome of a model prediction. This is particularly true when the number of components might be high in, for example, SOA mass partitioning simulations. It then becomes difficult for others in the community to assess the results presented. This might be complicated by the need to include pure component vapour pressures or activity coefficient predictions for a wide range of highly multifunctional compounds. It isn't clear to what extent replication of results is ever achieved for a range of aerosol simulations. Whilst this might also be an issue with results from instrumentation, the development of community driven software at least enables modellers to tackle this problem directly. Here we describe the development and application of a new web based facility, UManSysProp, to tackle such issues. Current facilities include: pure component vapour pressures, critical properties and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential of mixed inorganic/organic aerosol particles with associated Kappa-Kohler values; absorptive partitioning calculations with/without a treatment of non-ideality. The website can be found here: http://umansysprop.seaes.manchester.ac.uk/
Low Temperature Fluorination of Aerosol Suspensions of Hydrocarbons Utilizing Elemental Fluorine.
1982-09-01
admitting boron trifluoride into the aerosol direct florination of neopentane. The aerosol direct fluorination of ketones indicates the carbonyl group...fluorination of molecules with primary, secondary and tertiary hydro- gens is also included as is the effect of admitting boron trifluoride into the...significantly different physical and chemical properties than either of their components. For example, both ammonia and boron trifluoride are low
Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China
NASA Astrophysics Data System (ADS)
Cao, Li-Ming; Huang, Xiao-Feng; Li, Yuan-Yuan; Hu, Min; He, Ling-Yan
2018-02-01
Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS) system was deployed to study the volatility of non-refractory submicron particulate matter (PM1) species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM1 mass concentration during the experiment was 42.7±20.1 µg m-3, with organic aerosol (OA) being the most abundant component (43.2 % of the total mass). The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR) of 0.57 at 50 °C. Organics showed semi-volatile characteristics (the MFR was 0.88 at 50 °C), and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 °C), with an evaporation rate of 0.45 % °C-1. Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF) for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbon-like OA (HOA, accounting for 13.5 %), a cooking OA (COA, 20.6 %), a biomass-burning OA (BBOA, 8.9 %), and two oxygenated OAs (OOAs): a less-oxidized OOA (LO-OOA, 39.1 %) and a more-oxidized OOA (MO-OOA, 17.9 %). Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 °C was HOA (MFR of 0.56) > LO-OOA (0.70) > COA (0.85) ≈ BBOA (0.87) > MO-OOA (0.99), which was not completely consistent with the sequence of their O / C ratios. The high volatility of HOA implied that it had a high potential to be oxidized to secondary species in the gas phase. The aerosol volatility measurement results in this study provide useful parameters for the modeling work of aerosol evolution in China and are also helpful in understanding the formation mechanisms of secondary aerosols.
NASA Astrophysics Data System (ADS)
Dawson, Kyle William
The study of climate and the associated impacts imposed by human activity has garnered the attention of scientists and policy makers since the 1950s. Research into the various atmospheric constituents that interact with solar radiation thus modulating Earth's radiative budget has been largely focused on the contributions from greenhouse gases and later focused on the role of atmospheric aerosol. The role of atmospheric aerosol, i.e. a solid or aqueous phase particulate, is complex and presents an opportunity for bettering the assessments of climate radiative forcing (i.e. the fraction of climate change due to anthropogenic, rather than natural, activities) in several ways. First, motivated to better understand the radiative effects of the Earth's background aerosol state to improve the assessment of anthropogenic effects, an experimental study on the water uptake ability of xanthan gum as a proxy for marine hydrogel, a component of natural primary emitted seaspray aerosol, is presented. Marine hydrogel comprises an organic component of the ocean surface microlayer that is released to the atmosphere via the bursting of bubbles generated by entrainment of air through crashing waves. This study investigates the water uptake ability (i.e. hygroscopicity) of these particles when exposed to a range of relative humidity (RH). The hydration characteristics of aerosolized pure xanthan gum as well as xanthan gum/salt mixtures were studied using a hygroscopic tandem differential mobility analyzer (HTDMA) and cloud condensation nuclei counter (CCNc). The hygroscopicity of the various solutions were compared to theoretical thermodynamic calculations accounting for the component volume fractions as a function of relative humidity. The data show that pure xanthan gum aerosol hygroscopicity behaves as other organic polysaccharides and, when combined with salts, is reasonably approximated by the volume fraction mixing rules above 90% RH. Deviations occur below 90% RH as well as for CCNc measured hygroscopicity and HTDMA measured hygroscopicity at 90% RH, and are discussed in terms of hydration regimes associated with structural changes imposed by polymer/salt crosslinks. Second, motivated by a necessity to provide better constraints for climate model assessments of radiative forcing, a computational study for developing a link between climate models and observations from remote sensing techniques is presented. The Creating Aerosol Types from CHemistry (CATCH) algorithm has been developed for providing atmospheric models with estimated aerosol types, analogous to those that are retrieved by remote sensing methods. To date, the link between models and remote sensing retrievals is crude and is based on the total column attenuation of radiation by aerosol called the aerosol optical depth (AOD). In this study, through multivariate clustering techniques, this link is expanded to produce model-calculated aerosol types of dusty mix, maritime, urban, smoke, and fresh smoke, that are analogous to those retrieved by remote sensing. The CATCH algorithm shows that vertically-resolved aerosol types compare well to those measured by aircraft-mounted High Spectral Resolution Lidar - version 1 (HSRL-1) during the Ship-Aircraft Bio-Optical Research (SABOR) field campaign during July/August of 2014. Flight-by-flight comparisons of the type-apportioned AOD and vertically-resolved aerosol extinction also compare well. The CATCH algorithm is then applied to a high-resolution nested grid domain over North America and found to produce encouraging results of spatially relevant aerosol types such as dusty mix aerosol over the Caribbean, maritime aerosol over oceans, urban aerosol over large cities, smoke aerosol over weak forest fires, and fresh smoke aerosol over strong forest fires.
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.
NASA Astrophysics Data System (ADS)
Ji, Hongzhu; Zhang, Yinchao; Chen, Siying; Chen, He; Guo, Pan
2018-06-01
An iterative method, based on a derived inverse relationship between atmospheric backscatter coefficient and aerosol lidar ratio, is proposed to invert the lidar ratio profile and aerosol extinction coefficient. The feasibility of this method is investigated theoretically and experimentally. Simulation results show the inversion accuracy of aerosol optical properties for iterative method can be improved in the near-surface aerosol layer and the optical thick layer. Experimentally, as a result of the reduced insufficiency error and incoherence error, the aerosol optical properties with higher accuracy can be obtained in the near-surface region and the region of numerical derivative distortion. In addition, the particle component can be distinguished roughly based on this improved lidar ratio profile.
AERONET derived (BC) aerosol absorption
NASA Astrophysics Data System (ADS)
Kinne, S.
2015-12-01
AERONET is a ground-based sun-/sky-photometer network with good annual statistics at more than 400 sites worldwide. Inversion methods applied to these data define all relevant column aerosol optical properties and reveal even microphysical detail. The extracted data include estimates for aerosol size-distributions and for aerosol refractive indices at four different solar wavelengths. Hereby, the imaginary parts of the refractive indices define the aerosol column absorption. For regional and global averages and radiative impact assessment with off-line radiative transfer, these local data have been extended with distribution patterns offered by AeroCom modeling experiments. Annual and seasonal absorption distributions for total aerosol and estimates for component contributions (such as BC) are presented and associated direct forcing impacts are quantified.
NASA Astrophysics Data System (ADS)
Attwood, A. R.; Washenfelder, R. A.; Brock, C. A.; Hu, W.; Baumann, K.; Campuzano-Jost, P.; Day, D. A.; Edgerton, E. S.; Murphy, D. M.; Palm, B. B.; McComiskey, A.; Wagner, N. L.; Sá, S. S.; Ortega, A.; Martin, S. T.; Jimenez, J. L.; Brown, S. S.
2014-11-01
Emissions of SO2 in the United States have declined since the early 1990s, resulting in a decrease in aerosol sulfate mass in the Southeastern U.S. of -4.5(±0.9)% yr-1 between 1992 and 2013. Organic aerosol mass, the other major aerosol component in the Southeastern U.S., has decreased more slowly despite concurrent emission reductions in anthropogenic precursors. Summertime measurements in rural Alabama quantify the change in aerosol light extinction as a function of aerosol composition and relative humidity. Application of this relationship to composition data from 2001 to 2013 shows that a -1.1(±0.7)% yr-1 decrease in extinction can be attributed to decreasing aerosol water mass caused by the change in aerosol sulfate/organic ratio. Calculated reductions in extinction agree with regional trends in ground-based and satellite-derived aerosol optical depth. The diurnally averaged summertime surface radiative effect has changed by 8.0 W m-2, with 19% attributed to the decrease in aerosol water.
Han, Yunping; Li, Lin; Liu, Junxin; Zhang, Mengzhu
2012-11-01
Bacterial community structure and the chemical components in aerosols caused by rotating brushes in an Orbal oxidation ditch were assessed in a Beijing municipal wastewater treatment plant. Air samples were collected at different distances from the aerosol-generating rotating brushes. Molecular culture-independent methods were used to characterize the community structure of the airborne bacteria in each sample regardless of cell culturability. A clone library of 16S rDNA directly amplified from air DNA of each sample was constructed and sequenced to analyze the community composition and diversity. Insoluble particles and water-soluble ions emitted with microorganisms in aerosols were analysis by a scanning electron microscope together with energy dispersive X-ray spectroscopy and ion chromatogram analyzer. In total, most of the identified bacteria were Proteobacteria. The majority of sequences near the rotating brushes (the main source of the bioaerosols) were Proteobacteria (62.97 %) with β-(18.52 %) and γ-(44.45 %) subgroups and Bacteroidetes (29.63 %). Complex patterns were observed for each sampling location, suggesting a highly diverse community structure, comparable to that found in water in the Orbal oxidation ditch. Accompany with microorganisms, 46.36 μg/m(3) of SO (4) (2-) , 29.35 μg/m(3) of Cl(-), 21.51 μg/m(3) of NO (3) (-) , 19.76 μg/m(3) of NH (4) (+) , 11.42 μg/m(3) of PO (4) (3-) , 6.18 μg/m(3) of NO (2) (-) , and elements of Mg, Cl, K, Na, Fe, S, and P were detected from the air near the aerosols source. Differences in the structure of the bacterial communities and chemical components in the aerosols observed between sampling sites indicated important site-related variability. The composition of microorganisms in water was one of the most important sources of bacterial communities in bioaerosols. Chemical components in bioaerosols may provide a media for airborne microorganism attachment, as well as a suitable microenvironment for their growth and survival in the air. This study will be benefit for the formulation of pollution standards, especially for aerosols, that take into account plant workers' health.
Investigation of the Aerosols Over the Los Angeles Basin during the ARCTAS-CARB 2008 Pilot Study
NASA Astrophysics Data System (ADS)
Thornhill, L.; Anderson, B. E.; Beyersdorf, A.; Chen, G.; Winstead, E. L.; Lathem, T.; Diskin, G.; Sachse, G.; Dibb, J.; Scheuer, E.
2008-12-01
In the summer of 2008 during preparation for the second phase of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS), detailed measurements of atmospheric composition were made on-board the NASA DC-8 over the state of California on behalf of the California Air resources Board (CARB). Four flights were conducted between 18 July and 24 July, totaling 31 hours, over southern and central California to establish upwind chemical boundary conditions and gain a better understanding of the sources, chemical characteristics and spatial distribution of smog and greenhouse gases over the state. Serendipitously, from a science perspective, this time period was marked by numerous wildfires spread throughout the state. The DC-8 sensor suite included aerosol instruments capable of measuring the number concentrations, optical properties, and size distributions of aerosols between 0.003 and 20 um in diameter. In this presentation, we will characterize aerosols sampled during sorties over the Los Angeles basin, which included several missed approaches at Los Angeles International Airport (LAX), traverses through the Long Beach and Santa Barbara ship channels, sampling in and out of the marine boundary layer, and encounters with outflow of forest fires mixed with urban smog. We will examine the evolution of the aerosols over the course of the day, as the smog accumulates within the basin and is then transported out of the basin into the surrounding atmosphere.
Aerosol physical properties from satellite horizon inversion
NASA Technical Reports Server (NTRS)
Gray, C. R.; Malchow, H. L.; Merritt, D. C.; Var, R. E.; Whitney, C. K.
1973-01-01
The feasibility is investigated of determining the physical properties of aerosols globally in the altitude region of 10 to 100 km from a satellite horizon scanning experiment. The investigation utilizes a horizon inversion technique previously developed and extended. Aerosol physical properties such as number density, size distribution, and the real and imaginary components of the index of refraction are demonstrated to be invertible in the aerosol size ranges (0.01-0.1 microns), (0.1-1.0 microns), (1.0-10 microns). Extensions of previously developed radiative transfer models and recursive inversion algorithms are displayed.
NASA Astrophysics Data System (ADS)
Nicolae, Doina; Talianu, Camelia; Vasilescu, Jeni; Nicolae, Victor; Stachlewska, Iwona S.
2018-04-01
A Python code was developed to automatically retrieve the aerosol type (and its predominant component in the mixture) from EARLINET's 3 backscatter and 2 extinction data. The typing relies on Artificial Neural Networks which are trained to identify the most probable aerosol type from a set of mean-layer intensive optical parameters. This paper presents the use and limitations of the code with respect to the quality of the inputed lidar profiles, as well as with the assumptions made in the aerosol model.
NASA Astrophysics Data System (ADS)
Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.
2014-11-01
The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in residual layers but still originating in northern Italy, while a substantial fraction (41%) was due to the most aged aerosols imported from transalpine areas. The different meteorological regimes also affected the BC mixing state: in periods of enhanced stagnation and recirculation of pollutants, the number fraction of the BC-containing particles determined by ATOFMS was 75% of the total, while in the days of enhanced ventilation of the planetary boundary layer (PBL), such fraction was significantly lower (50%) because of the relative greater influence of non-BC-containing aerosol local sources in the Po Valley. Overall, a full internal mixing between BC and the non-refractory aerosol chemical components was not observed during the experiment in this environment.
NASA Astrophysics Data System (ADS)
Zhang, Kequan; Ma, Yongjing; Xin, Jinyuan; Liu, Zirui; Ma, Yining; Gao, Dongdong; Wu, Junsong; Zhang, Wenyu; Wang, Yuesi; Shen, Pengke
2018-03-01
To achieve an in-depth understanding of the aerosol optical properties in the highly-industrial region of Tangshan, we provided systematic aerosol optical properties analysis in this largest industrial zone for the first time. The aerosol optical datasets (2013.05-2015.04) and chemical component data of PM2.5 (2014-2015) obtained from the Tangshan site of the campaign on atmospheric aerosol research (CARE-China) network were analyzed. The results showed that the Tangshan region was seriously affected by fine-mode industrial aerosols all year, which would promote the accumulation of pollutants and influence the atmospheric circulation through changing the vertical temperature gradient. The annual average aerosol optical depth (AOD) and Ångstrӧm exponent (α) were 0.80 ± 0.26 and 1.05 ± 0.10, respectively. The aerosol optical properties revealed significant seasonal characteristics. The maximum seasonal average AOD (1.03 ± 0.62) and α (1.12 ± 0.19) accompanied the highest seasonal secondary inorganic aerosol concentrations (SIA: SO42 -, NO3-, NH4+), 53.33 μg/m3, occurred in summer, and this phenomenon was attributed to the photochemical reactions favored by the high temperature and humidity. During the spring, frequent dust events led to the maximum Ca2 + concentration of 6.57 μg/m3 and the lowest seasonal α of 0.98 ± 0.31. Coal was used for generating heat in winter, resulting in the highest levels of pollutant emissions (Cl-, Elemental carbon (EC) and organic carbon (OC)). The aerosol type classifications showed that the industrial aerosols were the main controls in the summer and fall, representing 56%-58% of the total aerosols. While for spring and winter, mixed aerosols represented 53%-54% of the total aerosols. Hygroscopic growth effect of aerosols existed all year, which could enhance the negative radiative forcing and eventually cool the earth-atmosphere system. The classification Wing for Tangshan data showed high AOD values (> 0.70) were mainly clustered in the fine-mode growth wing and coarse-mode. Of these values, summer showed a dense AOD distribution and the highest magnitude of fine-mode AODs, with a corresponding fine particle fraction of η 90% and an Rf 0.20 μm. In addition, spring showed the most coarse-mode aerosols.
NASA Astrophysics Data System (ADS)
McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.
2014-08-01
Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this 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.
NASA Astrophysics Data System (ADS)
McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.
2014-02-01
Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability 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.
NASA Astrophysics Data System (ADS)
Bougiatioti, Aikaterini; Bezantakos, Spiros; Stavroulas, Iasonas; Kalivitis, Nikos; Kokkalis, Panagiotis; Biskos, George; Mihalopoulos, Nikolaos; Papayannis, Alexandros; Nenes, Athanasios
2016-06-01
This study investigates the concentration, cloud condensation nuclei (CCN) activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean and their impacts on cloud droplet formation. Air masses sampled were subject to a range of atmospheric processing (several hours up to 3 days). Values of the hygroscopicity parameter, κ, were derived from CCN measurements and a Hygroscopic Tandem Differential Mobility Analyzer (HTDMA). An Aerosol Chemical Speciation Monitor (ACSM) was also used to determine the chemical composition and mass concentration of non-refractory components of the submicron aerosol fraction. During fire events, the increased organic content (and lower inorganic fraction) of the aerosol decreases the values of κ, for all particle sizes. Particle sizes smaller than 80 nm exhibited considerable chemical dispersion (where hygroscopicity varied up to 100 % for particles of same size); larger particles, however, exhibited considerably less dispersion owing to the effects of condensational growth and cloud processing. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles (having a diameter of ˜ 100 nm at dry conditions) sampled. Based on positive matrix factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend as the biomass-burning organic aerosol (BBOA) component, with the former being enhanced between 65 and 150 % (for supersaturations ranging between 0.2 and 0.7 %) with the arrival of the smoke plumes. Using multilinear regression of the PMF factors (BBOA, OOA-BB and OOA) and the observed hygroscopicity parameter, the inferred hygroscopicity of the oxygenated organic aerosol components is determined. We find that the transformation of freshly emitted biomass burning (BBOA) to more oxidized organic aerosol (OOA-BB) can result in a 2-fold increase of the inferred organic hygroscopicity; about 10 % of the total aerosol hygroscopicity is related to the two biomass-burning components (BBOA and OOA-BB), which in turn contribute almost 35 % to the fine-particle organic water of the aerosol. Observation-derived calculations of the cloud droplet concentrations that develop for typical boundary layer cloud conditions suggest that biomass burning increases droplet number, on average by 8.5 %. The strongly sublinear response of clouds to biomass-burning (BB) influences is a result of strong competition of CCN for water vapor, which results in very low maximum supersaturation (0.08 % on average). Attributing droplet number variations to the total aerosol number and the chemical composition variations shows that the importance of chemical composition increases with distance, contributing up to 25 % of the total droplet variability. Therefore, although BB may strongly elevate CCN numbers, the impact on droplet number is limited by water vapor availability and depends on the aerosol particle concentration levels associated with the background.
NASA Astrophysics Data System (ADS)
Li, Shenshen; Yu, Chao; Chen, Liangfu; Tao, Jinhua; Letu, Husi; Ge, Wei; Si, Yidan; Liu, Yang
2016-09-01
China's large aerosol emissions have major impacts on global climate change as well as regional air pollution and its associated disease burdens. A detailed understanding of the spatiotemporal patterns of aerosol components is necessary for the calculation of aerosol radiative forcing and the development of effective emission control policy. Model-simulated and satellite-retrieved aerosol components can support climate change research, PM2.5 source appointment and epidemiological studies. This study evaluated the total and componential aerosol optical depth (AOD) from the GEOS-Chem model (GC) and the Global Ozone Chemistry Aerosol Radiation and Transport model (GOCART), and the Multiangle Imaging Spectroradiometer (MISR) from 2006 to 2009 in China. Linear regression analysis between the GC and AErosol RObotic NETwork (AERONET) in China yielded similar correlation coefficients (0.6 daily, 0.71 monthly) but lower slopes (0.41 daily, 0.58 monthly) compared with those in the U.S. This difference was attributed to GC's underestimation of water-soluble AOD (WAOD) west of the Heihe-Tengchong Line, the dust AOD (DAOD) in the fall and winter, and the soot AOD (SAOD) throughout the year and throughout the country. GOCART exhibits the strongest dust estimation capability among all datasets. However, the GOCART soot distribution in the Northeast and Southeast has significant errors, and its WAOD in the polluted North China Plain (NCP) and the South is underestimated. MISR significantly overestimates the water-soluble aerosol levels in the West, and does not capture the high dust loadings in all seasons and regions, and the SAOD in the NCP. These discrepancies can mainly be attributed to the uncertainties in the emission inventories of both models, the poor performance of GC under China's high aerosol loading conditions, the omission of certain aerosol tracers in GOCART, and the tendency of MISR to misidentify dust and non-dust mixtures.
Simulation of Aerosol Transport and Radiative Effects In Lmd-gcm During Indoex-ifp 1999
NASA Astrophysics Data System (ADS)
Reddy, M. S.; Boucher, O.; Léon, J.-F.; Venkataraman, C.; Pham, M.
During the January-March 1999, an international collaborative field experiment, In- dian Ocean Experiment (INDOEX) was carried out to understand the anthropogenic aerosol effects on radiative forcing (Ramanathan, 2001). In the present work we sim- ulated the cycle of the multi-component aerosol (sulphate, black carbon, organic car- bon, dust, sea-salt and fly-ash) in the Laboratoire de Météorologie Dynamique General Circulation Model (LMD GCM) and estimated the consequent radiative forcing. Sim- ulations are carried out in the zoomed version of the model focusing on the Indian sub- continent and Indian Ocean regions, for January-April 1999. To account correctly for the aerosol emissions in the source regions (Indian subcontinent) we have integrated newly developed SO2 and aerosol emission inventory for India for 1999 (Reddy and Venkataraman, 2002a and b) into the global emission data set input to model. Model performance is evaluated by comparing the simulated aerosol concentration fields against measurements over continental and oceanic stations. Model predicted concentrations agree well in the oceanic stations but are in the lower end of mea- surements in the continental stations. A large plume of sulphate and other aerosols ex- tended from the Indian sub-continent into the Indian Ocean, from surface and elevated flows, extending down to 5S in the pristine southern Indian Ocean. Predicted spec- trally resolved aerosol optical depths (AOD) will be compared with sun-photometer measurements in the region. We also present a comparison of model predicted aerosol optical depths with satellite (Meteosat) derived AOD for the same period. An assess- ment of the multi-component aerosol radiative forcing will be made and results will be discussed in the context of the possible climate effects over the region. Finally, the regional source contributions to sulphate and carbonaceous aerosol loadings in the Indian Ocean will be presented.
Cai, Chen; Stewart, David J; Reid, Jonathan P; Zhang, Yun-hong; Ohm, Peter; Dutcher, Cari S; Clegg, Simon L
2015-01-29
Measurements of the hygroscopic response of aerosol and the particle-to-gas partitioning of semivolatile organic compounds are crucial for providing more accurate descriptions of the compositional and size distributions of atmospheric aerosol. Concurrent measurements of particle size and composition (inferred from refractive index) are reported here using optical tweezers to isolate and probe individual aerosol droplets over extended timeframes. The measurements are shown to allow accurate retrievals of component vapor pressures and hygroscopic response through examining correlated variations in size and composition for binary droplets containing water and a single organic component. Measurements are reported for a homologous series of dicarboxylic acids, maleic acid, citric acid, glycerol, or 1,2,6-hexanetriol. An assessment of the inherent uncertainties in such measurements when measuring only particle size is provided to confirm the value of such a correlational approach. We also show that the method of molar refraction provides an accurate characterization of the compositional dependence of the refractive index of the solutions. In this method, the density of the pure liquid solute is the largest uncertainty and must be either known or inferred from subsaturated measurements with an error of <±2.5% to discriminate between different thermodynamic treatments.
Tiny Ultraviolet Polarimeter for Earth Stratosphere from Space Investigation
NASA Astrophysics Data System (ADS)
Nevodovskyi, P. V.; Morozhenko, O. V.; Vidmachenko, A. P.; Ivakhiv, O.; Geraimchuk, M.; Zbrutskyi, O.
2015-09-01
One of the reasons for climate change (i.e., stratospheric ozone concentrations) is connected with the variations in optical thickness of aerosols in the upper sphere of the atmosphere (at altitudes over 30 km). Therefore, aerosol and gas components of the atmosphere are crucial in the study of the ultraviolet (UV) radiation passing upon the Earth. Moreover, a scrupulous study of aerosol components of the Earth atmosphere at an altitude of 30 km (i.e., stratospheric aerosol), such as the size of particles, the real part of refractive index, optical thickness and its horizontal structure, concentration of ozone or the upper border of the stratospheric ozone layer is an important task in the research of the Earth climate change. At present, the Main Astronomical Observatory of the National Academy of Sciences (NAS) of Ukraine, the National Technical University of Ukraine "KPI"and the Lviv Polytechnic National University are engaged in the development of methodologies for the study of stratospheric aerosol by means of ultraviolet polarimeter using a microsatellite. So fare, there has been created a sample of a tiny ultraviolet polarimeter (UVP) which is considered to be a basic model for carrying out space experiments regarding the impact of the changes in stratospheric aerosols on both global and local climate.
NASA Astrophysics Data System (ADS)
Cai, C.; Zhao, C.
2017-12-01
Quantifying the gas/particle partitioning of organic compounds is of great significance to the understanding of atmospheric aerosol indirect effect. Accurate determination of the hygroscopicities and vapor pressures of semi-volatile organic compounds (SVOC) is of crucial importance in studying their partitioning behavior into atmospheric aerosol, as current published vapor pressures results of compounds of interest (usually with vapor pressures smaller than 0.01 Pa) vary by several orders of magnitude. On the other hand, influences on SVOCs evaporation from participation of inorganic species remains ambiguous. In this study we present quantitative investigation of hygroscopicities and volatilities of single aerosol droplets in an aerosol optical tweezers. The trapped droplet (3-7 µm radii) in the aerosol optical tweezers acts as a micro cavity, which stimulates the cavity enhanced Raman spectroscopy (CERS) signal. Size and composition of the particle are calculated from Mie fit to the positions of the "whispering gallery modes" in the CERS fingerprint. Hygroscopic behaviors and SVOC pure component vapor pressure can then be extracted from the correlation between the changing droplet radius and solute concentration (derived from experimentally determined RI real part). We will further present the influences between mass transfer on the gas-particle interface and within the droplet.
Properties of aerosols and formation mechanisms over southern China during the monsoon season
NASA Astrophysics Data System (ADS)
Chen, Weihua; Wang, Xuemei; Blake Cohen, Jason; Zhou, Shengzhen; Zhang, Zhisheng; Chang, Ming; Chan, Chuen-Yu
2016-10-01
Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May-June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm). Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.
How Models Simulate the Radiative Effect in the Transition Zone of the Aerosol-Cloud Continuum
NASA Astrophysics Data System (ADS)
Calbo Angrill, J.; González, J. A.; Long, C. N.; McComiskey, A. C.
2017-12-01
Several studies have pointed towards dealing with clouds and aerosols as two manifestations of what is essentially the same physical phenomenon: a suspension of tiny particles in the air. Although the two extreme cases (i.e., pure aerosol and well-defined cloud) are easily distinguished, and obviously produce different radiative effects, there are many situations in the transition (or "twilight") zone. In a recent paper [Calbó et al., Atmos. Res. 2017, j.atmosres.2017.06.010], the authors of the current communication estimated that about 10% of time there might be a suspension of particles in the air that is difficult to distinguish as either cloud or aerosol. Radiative transfer models, however, simulate the effect of clouds and aerosols with different modules, routines, or parameterizations. In this study, we apply a sensitivity analysis approach to assess the ability of two radiative transfer models (SBDART and RRTM) in simulating the radiative effect of a suspension of particles with characteristics in the boundary between cloud and aerosol. We simulate this kind of suspension either in "cloud mode" or in "aerosol mode" and setting different values of optical depth, droplet size, water path, aerosol type, cloud height, etc. Irradiances both for solar and infrared bands are studied, both at ground level and at the top of the atmosphere, and all analyses are repeated for different solar zenith angles. We obtain that (a) water clouds and ice clouds have similar radiative effects if they have the same optical depth; (b) the spread of effects regarding different aerosol type/aerosol characteristics is remarkable; (c) radiative effects of an aerosol layer and of a cloud layer are different, even if they have similar optical depth; (d) for a given effect on the diffuse component, the effect on the direct component is usually greater (more extinction of direct beam) by aerosols than by clouds; (e) radiative transfer models are somewhat limited when simulating the effects of a suspension of particles in the transition zone, as the approach to this zone as an aerosol or as a cloud produces different results.
NASA Astrophysics Data System (ADS)
Chuang, Ming-Tung; Lee, Chung-Te; Chou, Charles C.-K.; Engling, Guenter; Chang, Shih-Yu; Chang, Shuenn-Chin; Sheu, Guey-Rong; Lin, Neng-Huei; Sopajaree, Khajornsak; Chang, You-Jia; Hong, Guo-Jun
2016-07-01
The transport of biomass burning (BB) aerosol from Indochina may cause a potential effect on climate change in Southeast Asia, East Asia, and the Western Pacific. Up to now, the understanding of BB aerosol composition modification during long-range transport (LRT) is still very limited due to the lack of observational data. In this study, atmospheric aerosols were collected at the Suthep/Doi Ang Khang (DAK) mountain sites in Chiang Mai, Thailand and the Lulin Atmospheric Background Station (Mt. Lulin) in central Taiwan from March to April 2010 and from February to April 2013, respectively. During the study period, an upwind and downwind relationship between the Suthep/DAK and Lulin sites (2400 km apart) was validated by backward trajectories. Comprehensive aerosol properties were resolved for PM2.5 water-soluble inorganic ions, carbonaceous content, water-soluble/insoluble organic carbon (WSOC/WIOC), dicarboxylic acids and their salts (DCAS), and anhydrosugars. A Modification Factor (MF) is proposed by employing non-sea-salt potassium ion (nss-K+) or fractionalized elemental carbon evolved at 580 °C after pyrolized OC correction (EC1-OP) as a BB aerosol tracer to evaluate the mass fraction changes of aerosol components from source to receptor regions during LRT. The MF values of nss-SO42-, NH4+, NO3-, OC1 (fractionalized organic carbon evolved from room temperature to 140 °C), OP (pyrolized OC fraction), DCAS, and WSOC were above unity, which indicated that these aerosol components were enhanced during LRT as compared with those in the near-source region. In contrast, the MF values of anhydrosugars ranged from 0.1 to 0.3, indicating anhydrosugars have degraded during LRT.
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.
NASA Astrophysics Data System (ADS)
Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Maalick, Z.; Korhonen, H.; Liqing, H.
2015-12-01
A new cloud-resolving model setup for studying aerosol-cloud interactions, with a special emphasis on partitioning and wet deposition of semi-volatile aerosol species, is presented. The model is based on modified versions of two well-established model components: the Large-Eddy Simulator (LES) UCLALES, and the sectional aerosol model SALSA, previously employed in the ECHAM climate model family. Implementation of the UCLALES-SALSA is described in detail. As the basis for this work, SALSA has been extended to include a sectional representation of the size distributions of cloud droplets and precipitation. Microphysical processes operating on clouds and precipitation have also been added. Given our main motivation, the cloud droplet size bins are defined according to the dry particle diameter. The droplet wet diameter is solved dynamically through condensation equations, but represents an average droplet diameter inside each size bin. This approach allows for accurate tracking of the aerosol properties inside clouds, but minimizes the computational cost. Since the actual cloud droplet diameter is not fully resolved inside the size bins, processes such as precipitation formation rely on parameterizations. For realistic growth of drizzle drops to rain, which is critical for the aerosol wet deposition, the precipitation size bins are defined according to the actual drop size. With these additions, the implementation of the SALSA model replaces most of the microphysical and thermodynamical components within the LES. The cloud properties and aerosol-cloud interactions simulated by the model are analysed and evaluated against detailed cloud microphysical boxmodel results and in-situ aerosol-cloud interaction observations from the Puijo measurement station in Kuopio, Finland. The ability of the model to reproduce the impacts of wet deposition on the aerosol population is demonstrated.
Impact of teamwork on missed care in four Australian hospitals.
Chapman, Rose; Rahman, Asheq; Courtney, Mary; Chalmers, Cheyne
2017-01-01
Investigate effects of teamwork on missed nursing care across a healthcare network in Australia. Missed care is universally used as an indicator of quality nursing care, however, little is known about mitigating effects of teamwork on these events. A descriptive exploratory study. Missed Care and Team Work surveys were completed by 334 nurses. Using Stata software, nursing staff demographic information and components of missed care and teamwork were compared across the healthcare network. Statistical tests were performed to identify predicting factors for missed care. The most commonly reported components of missed care were as follows: ambulation three times per day (43·3%), turning patient every two hours (29%) and mouth care (27·7%). The commonest reasons mentioned for missed care were as follows: inadequate labour resources (range 69·8-52·7%), followed by material resources (range 59·3-33·3%) and communication (range 39·3-27·2%). There were significant differences in missed care scores across units. Using the mean scores in regression correlation matrix, the negative relationship of missed care and teamwork was supported (r = -0·34, p < 0·001). Controlling for occupation of the staff member and staff characteristics in multiple regression models, teamwork alone accounted for about 9% of missed nursing care. Similar to previous international research findings, our results showed nursing teamwork significantly impacted on missed nursing care. Teamwork may be a mitigating factor to address missed care and future research is needed. These results may provide administrators, educators and clinicians with information to develop practices and policies to improve patient care internationally. © 2016 John Wiley & Sons Ltd.
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 an optically equivalent aerosol mixture reduces when diffuse component of flux increases. In our analysis, RT model clearly shows that direct component of spectral flux is more sensitive to different aerosol species than total spectral flux which is also supported by our observed data.
SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels
NASA Technical Reports Server (NTRS)
Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas
2008-01-01
Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.
NASA Astrophysics Data System (ADS)
Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C.; Crumeyrolle, S.; Giles, D. M.; Holben, B. N.; Hudgins, C.; Martin, R.; Moore, R.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.
2014-12-01
Understanding the vertical profile of atmospheric aerosols plays a vital role in utilizing spaceborne, column-integrated satellite observations. The properties and distribution of light-absorbing aerosol are particularly uncertain despite significant air quality and climate ramifications. Advanced retrieval algorithms are able to derive complex aerosol properties (e.g., wavelength-dependent absorption coefficient and single scattering albedo) from remote-sensing measurements, but quantitative relationships to surface conditions remain a challenge. Highly systematic atmospheric profiling during four unique deployments for the NASA DISCOVER-AQ project (Baltimore, MD, 2011; San Joaquin Valley, CA, 2013; Houston, TX, 2013; Denver, CO, 2014) allow statistical assessment of spatial, temporal, and source-related variability for light-absorbing aerosol properties in these distinct regions. In-situ sampling in conjunction with a dense network of AERONET sensors also allows evaluation of the sensitivity, limitations, and advantages of remote-sensing data products over a wide range of conditions. In-situ aerosol and gas-phase observations were made during DISCOVER-AQ aboard the NASA P-3B aircraft. Aerosol absorption coefficients were measured by a Particle Soot Absorption Photometer (PSAP). Approximately 200 profiles for each of the four deployments were obtained, from the surface (25-300m altitude) to 5 km, and are used to calculate absorption aerosol optical depths (AAODs). These are quantitatively compared to AAOD derived from AERONET Level 1.5 retrievals to 1) explore discrepancies between measurements, 2) quantify the fraction of AAOD that exists directly at the surface and is often missed by airborne sampling, and 3) evaluate the potential for deriving ground-level black carbon (BC) concentrations for air quality prediction. Aerosol size distributions are used to assess absorption contributions from mineral dust, both at the surface and aloft. SP2 (Single Particle Soot Photometer) mixing state and coating thickness analyses will be explored to explain in-situ/AERONET discrepancies, and ground-based absorption coefficient and BC-mass observations will be utilized whenever possible to fully obtain the true absorption vertical profile.
PREDICTION OF MULTICOMPONENT INORGANIC ATMOSPHERIC AEROSOL BEHAVIOR. (R824793)
Many existing models calculate the composition of the atmospheric aerosol system by solving a set of algebraic equations based on reversible reactions derived from thermodynamic equilibrium. Some models rely on an a priori knowledge of the presence of components in certain relati...
Lerner, Chad A; Sundar, Isaac K; Watson, Richard M; Elder, Alison; Jones, Ryan; Done, Douglas; Kurtzman, Rachel; Ossip, Deborah J; Robinson, Risa; McIntosh, Scott; Rahman, Irfan
2015-03-01
To narrow the gap in our understanding of potential oxidative properties associated with Electronic Nicotine Delivery Systems (ENDS) i.e. e-cigarettes, we employed semi-quantitative methods to detect oxidant reactivity in disposable components of ENDS/e-cigarettes (batteries and cartomizers) using a fluorescein indicator. These components exhibit oxidants/reactive oxygen species reactivity similar to used conventional cigarette filters. Oxidants/reactive oxygen species reactivity in e-cigarette aerosols was also similar to oxidant reactivity in cigarette smoke. A cascade particle impactor allowed sieving of a range of particle size distributions between 0.450 and 2.02 μm in aerosols from an e-cigarette. Copper, being among these particles, is 6.1 times higher per puff than reported previously for conventional cigarette smoke. The detection of a potentially cytotoxic metal as well as oxidants from e-cigarette and its components raises concern regarding the safety of e-cigarettes use and the disposal of e-cigarette waste products into the environment. Copyright © 2014 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Zhang, X. Y.; Wang, J. Z.; Wang, Y. Q.; Liu, H. L.; Sun, J. Y.; Zhang, Y. M.
2015-11-01
Since there have been individual reports of persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PM10 at 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements - PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PM10 in 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 μg m-3, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM10, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without significant changes. In the Pearl River Delta (PRD) area, the regional background concentrations of the major chemical components were similar to those in the YRD, accounting for approximately 60-80 % of those in HBP. Since 2010, a decline has been found for winter concentrations, which can be partially attributable to persistently improving meteorological conditions and emission cutting with an emphasis on coal combustion in this area. In addition to the scattered and centralized coal combustion for heating, burning biomass fuels contributed to the large increase in concentrations of carbonaceous aerosol in major haze regions in winter, except in the PRD. No obvious changes were found for the proportions of each chemical components of PM10 from 2006 to 2013. Among all of the emissions recorded in chemical compositions in 2013, coal combustion was still the largest anthropogenic source of aerosol pollution in various areas in China, with a higher sulfate proportion of PM10 in most areas of China, and OC was normally ranked third. PM10 concentrations increased by approximately 25 % in January of 2013 relative to 2012, which caused persistent haze-fog events in HBP; emissions also reduced by approximately 35 % in Beijing and its vicinity (BIV) in late autumn of 2014, thereby producing the Asia Pacific Economic Cooperation (APEC) blue (extremely good air quality); thus, one can expect that the persistent haze-fog events would be reduced significantly in the BIV, if approx. one-third of the 2013 winter emissions were reduced, which can also be viewed as the upper limit of atmospheric aerosol pollution capacity in this area.
ERIC Educational Resources Information Center
Hernandez, Oscar H.; Vogel-Sprott, Muriel
2009-01-01
This within-subjects experiment tested the relationship between the premotor (cognitive) component of reaction time (RT) to a missing stimulus and parameters of the omitted stimulus potential (OSP) brain wave. Healthy young men (N = 28) completed trials with an auditory stimulus that recurred at 2 s intervals and ceased unpredictably. Premotor RT…
NASA Astrophysics Data System (ADS)
Handa, Daishi; Somada, Yuka; Ijyu, Moriaki; Azechi, Sotaro; Nakaema, Fumiya; Arakaki, Takemitsu; Tanahara, Akira
2010-05-01
The economic development and population growth in recent Asia spread air pollution. Emission rate of air pollutants from Asia, in particular oxides of nitrogen, surpassed those from North America and Europe and should continue to exceed them for decades. The study of the long-range transported air pollution from Asian continent has gained a special attention in Japan because of increase in photochemical oxidants in relatively remote islands. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location in Asia is well suited for studying long-range transport of air pollutants in East Asia because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. Bulk aerosol samples were collected on quartz filters by using a high volume air sampler. Sampling duration was one week for each sample. We determined the concentrations of water-soluble anions, cations and dissolved organic carbon (DOC) in the bulk aerosols collected at the Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. We will report water-soluble chemical components data of anions, cations and DOC in bulk atmospheric aerosols collected at CHAAMS during August, 2005 to April, 2010. Seasonal variation of water-soluble chemical components showed that the concentrations were relatively low in summer, higher in fall and winter, and the highest in spring. When air mass came from Asian Continent, the concentrations of water-soluble chemical components were much higher compared to the other directions. In addition, we calculated background concentration of water-soluble chemical components at Okinawa, Japan.
Spectral Absorption Properties of Aerosol Particles from 350-2500nm
NASA Technical Reports Server (NTRS)
Martins, J. Vanderlei; Artaxo, Paulo; Kaufman, Yoram J.; Castanho, Andrea D.; Remer, Lorraine A.
2009-01-01
The aerosol spectral absorption efficiency (alpha (sub a) in square meters per gram) is measured over an extended wavelength range (350 2500 nm) using an improved calibrated and validated reflectance technique and applied to urban aerosol samples from Sao Paulo, Brazil and from a site in Virginia, Eastern US, that experiences transported urban/industrial aerosol. The average alpha (sub a) values (approximately 3 square meters per gram at 550 nm) for Sao Paulo samples are 10 times larger than alpha (sub a) values obtained for aerosols in Virginia. Sao Paulo aerosols also show evidence of enhanced UV absorption in selected samples, probably associated with organic aerosol components. This extra UV absorption can double the absorption efficiency observed from black carbon alone, therefore reducing by up to 50% the surface UV fluxes, with important implications for climate, UV photolysis rates, and remote sensing from space.
Using radiocarbon to constrain black and organic carbon aerosol sources in Salt Lake City
NASA Astrophysics Data System (ADS)
Mouteva, Gergana O.; Randerson, James T.; Fahrni, Simon M.; Bush, Susan E.; Ehleringer, James R.; Xu, Xiaomei; Santos, Guaciara M.; Kuprov, Roman; Schichtel, Bret A.; Czimczik, Claudia I.
2017-09-01
Black carbon (BC) and organic carbon (OC) aerosols are important components of fine particulate matter (PM2.5) in polluted urban environments. Quantifying the contribution of fossil fuel and biomass combustion to BC and OC concentrations is critical for developing and validating effective air quality control measures and climate change mitigation policy. We used radiocarbon (14C) to measure fossil and contemporary biomass contributions to BC and OC at three locations in Salt Lake City, Utah, USA, during 2012-2014, including during winter inversion events. Aerosol filters were analyzed with the Swiss_4S thermal-optical protocol to isolate BC. We measured fraction modern (fM) of BC and total carbon in PM2.5 with accelerator mass spectrometry and derived the fM of OC using isotope mass balance. Combined with 14C information of end-member composition, our data set of 31 14C aerosol measurements provided a baseline of the fossil and contemporary biomass components of carbonaceous aerosol. We show that fossil fuels were the dominant source of carbonaceous aerosol during winter, contributing 88% (80-98%) of BC and 58% (48-69%) of OC. While the concentration of both BC and OC increased during inversion events, the relative source contributions did not change. The sources of BC also did not vary throughout the year, while OC had a considerably higher contemporary biomass component in summer at 62% (49-76%) and was more variable. Our results suggest that in order to reduce PM2.5 levels in Salt Lake City to meet national standards, a more stringent policy targeting mobile fossil fuel sources may be necessary.
NASA Astrophysics Data System (ADS)
Kaku, Kathleen C.; Reid, Jeffrey S.; Reid, Elizabeth A.; Ross-Langerman, Kristy; Piketh, Stuart; Cliff, Steven; Al Mandoos, Abdulla; Broccardo, Stephen; Zhao, Yongjing; Zhang, Jianglong; Perry, Kevin D.
2016-03-01
The aerosol chemistry environment of the Arabian Gulf region is extraordinarily complex, with high concentrations of dust aerosols from surrounding deserts mixed with anthropogenic aerosols originating from a large petrochemical industry and pockets of highly urbanized areas. Despite the high levels of aerosols experienced by this region, little research has been done to explore the chemical composition of both the anthropogenic and mineral dust portion of the aerosol burden. The intensive portion of the United Arab Emirates Unified Aerosol Experiment (UAE2), conducted during August and September 2004 was designed in part to resolve the aerosol chemistry through the use of multiple size-segregated aerosol samplers. The coarse mode mass (derived by subtracting the PM2.5 aerosol mass from the PM10 mass) is largely dust at 76% ± 7% of the total coarse mode mass, but is significantly impacted by anthropogenic pollution, primarily sulfate and nitrate. The PM2.5 aerosol mass also contains a large dust burden, at 38% ± 26%, but the anthropogenic component dominates. The total aerosol burden has significant impact not only on the atmosphere, but also the local population, as the air quality levels for both the PM10 and PM2.5 aerosol masses reached unhealthy levels for 24% of the days sampled.
Constraining the instantaneous aerosol influence on cloud albedo.
Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine; Gettelman, Andrew; Ghan, Steven; Lohmann, Ulrike; Morrison, Hugh; Neubauer, David; Partridge, Daniel G; Stier, Philip; Takemura, Toshihiko; Wang, Hailong; Wang, Minghuai; Zhang, Kai
2017-05-09
Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol-cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d ), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol-climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol-cloud interactions in satellite data.
NASA Technical Reports Server (NTRS)
Chin, Mian; Ginoux, Paul; Flatau, Piotr; Anderson, Tad; Masonis, Sarah; Russell, Phil; Schmid, Beat; Livingston, John; Redemann, Jens; Kahn, Ralph;
2001-01-01
The Aerosol Characterization Experiment-Asia (ACE-Asia) took place in Spring 2001 in the East Asia-West Pacific Ocean. During the ACE-Asia intensive field operation period, high concentrations of dust and anthropogenic aerosols were observed over the Yellow Sea and the Sea of Japan, which were transported out from the Asian continent, with the plume often extending to 6-8 km altitude. The multi-component aerosols originated from Asia are expected to exert a significant radiative forcing over the Pacific region. We present here results from the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model of aerosol transport and radiative forcing in the context of ACE-Asia. The model calculated aerosol concentrations, extinctions, optical thickness, size distributions, and vertical profiles are compared with the aircraft and ship measurements, and the distributions of aerosols are compared with satellite data. The model will be used to understand the origins of the aerosols observed in ACE-Asia, estimate the contributions from anthropogenic and natural aerosols to the total aerosol optical thickness, investigate the effects of humidification and clouds on aerosol properties, and assess the radiative forcing of Asian aerosols over the Pacific region and in the northern hemisphere.
NASA Astrophysics Data System (ADS)
Zappoli, S.; Andracchio, A.; Fuzzi, S.; Facchini, M. C.; Gelencsér, A.; Kiss, G.; Krivácsy, Z.; Molnár, Á.; Mészáros, E.; Hansson, H.-C.; Rosman, K.; Zebühr, Y.
A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m -3 at the background site Aspvreten, 24 μg m -3 at the rural K-puszta and 38 μg m -3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65-75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20-50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.
Field Studies of Broadband Aerosol Optical Extinction in the Ultraviolet Spectral Region
NASA Astrophysics Data System (ADS)
Washenfelder, R. A.; Attwood, A.; Brock, C. A.; Brown, S. S.
2013-12-01
Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. In the case of brown carbon, its wavelength-dependent absorption in the ultraviolet spectral region has been suggested as an important component of aerosol radiative forcing. We describe a new field instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360-390 and 385-420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We deployed this instrument during the Fire Lab at Missoula Experiment during Fall 2012 to measure biomass burning aerosol, and again during the Southern Oxidant and Aerosol Study in summer 2013 to measure organic aerosol in the Southeastern U.S. In both field experiments, we determined aerosol optical extinction as a function of wavelength and can interpret this together with size distribution and composition measurements to characterize the aerosol optical properties and radiative forcing.
Toxicity of atmospheric aerosols on marine phytoplankton
Paytan, A.; Mackey, K.R.M.; Chen, Y.; Lima, I.D.; Doney, S.C.; Mahowald, N.; Labiosa, R.; Post, A.F.
2009-01-01
Atmospheric aerosol deposition is an important source of nutrients and trace metals to the open ocean that can enhance ocean productivity and carbon sequestration and thus influence atmospheric carbon dioxide concentrations and climate. Using aerosol samples from different back trajectories in incubation experiments with natural communities, we demonstrate that the response of phytoplankton growth to aerosol additions depends on specific components in aerosols and differs across phytoplankton species. Aerosol additions enhanced growth by releasing nitrogen and phosphorus, but not all aerosols stimulated growth. Toxic effects were observed with some aerosols, where the toxicity affected picoeukaryotes and Synechococcus but not Prochlorococcus.We suggest that the toxicity could be due to high copper concentrations in these aerosols and support this by laboratory copper toxicity tests preformed with Synechococcus cultures. However, it is possible that other elements present in the aerosols or unknown synergistic effects between these elements could have also contributed to the toxic effect. Anthropogenic emissions are increasing atmospheric copper deposition sharply, and based on coupled atmosphere-ocean calculations, we show that this deposition can potentially alter patterns of marine primary production and community structure in high aerosol, low chlorophyll areas, particularly in the Bay of Bengal and downwind of South and East Asia.
2003-01-31
mechanisms. 109 The main sources of atmospheric pollution are gas cutting and air-arc shaving, used to clean the cutting line from paint and varnish ...and varnish covering and from the metal of the dismantled construction. The dust content is determined by the type of the paint- varnish covering and...Submarines Solid aerosol component, kg Gas aerosol component, kg Design Total amount Including Carbon oxide Nitrogen dioxide Fluorine Manganese
NASA Astrophysics Data System (ADS)
Fahey, D. W.; Gao, R.; Thornberry, T. D.; Rollins, D. W.; Schwarz, J. P.; Perring, A. E.
2013-12-01
In-situ sampling with particle size spectrometers is an important method to provide detailed size spectra for atmospheric aerosol in the troposphere and stratosphere. The spectra are essential for understanding aerosol sources and aerosol chemical evolution and removal, and for aerosol remote sensing validation. These spectrometers are usually bulky, heavy, and expensive, thereby limiting their application to specific airborne platforms. Here we report a new type of small and light-weight optical aerosol particle size spectrometer that is sensitive enough for many aerosol applications yet is inexpensive enough to be disposable. 3D printing is used for producing structural components for simplicity and low cost. Weighing less than 1 kg individually, we expect these spectrometers can be deployed successfully on small unmanned aircraft systems (UASs) and up to 25 km on weather balloons. Immediate applications include the study of Arctic haze using the Manta UAS, detection of the Asian Tropopause Aerosol Layer in the Asian monsoon system and SAGE III validation onboard weather balloons.
Jaafar, Shoffian Amin; Latif, Mohd Talib; Chian, Chong Woan; Han, Wong Sook; Wahid, Nurul Bahiyah Abd; Razak, Intan Suraya; Khan, Md Firoz; Tahir, Norhayati Mohd
2014-07-15
This study was conducted to determine the composition of surfactants in the sea-surface microlayer (SML) and atmospheric aerosol around the southern region of the Peninsular Malaysia. Surfactants in samples taken from the SML and atmospheric aerosol were determined using a colorimetric method, as either methylene blue active substances (MBAS) or disulphine blue active substances (DBAS). Principal component analysis with multiple linear regressions (PCA-MLR), using the anion and major element composition of the aerosol samples, was used to determine possible sources of surfactants in atmospheric aerosol. The results showed that the concentrations of surfactants in the SML and atmospheric aerosol were dominated by anionic surfactants and that surfactants in aerosol were not directly correlated (p>0.05) with surfactants in the SML. Further PCA-MLR from anion and major element concentrations showed that combustion of fossil fuel and sea spray were the major contributors to surfactants in aerosol in the study area. Copyright © 2014 Elsevier Ltd. All rights reserved.
Constraining Carbonaceous Aerosol Climate Forcing by Bridging Laboratory, Field and Modeling Studies
NASA Astrophysics Data System (ADS)
Dubey, M. K.; Aiken, A. C.; Liu, S.; Saleh, R.; Cappa, C. D.; Williams, L. R.; Donahue, N. M.; Gorkowski, K.; Ng, N. L.; Mazzoleni, C.; China, S.; Sharma, N.; Yokelson, R. J.; Allan, J. D.; Liu, D.
2014-12-01
Biomass and fossil fuel combustion emits black (BC) and brown carbon (BrC) aerosols that absorb sunlight to warm climate and organic carbon (OC) aerosols that scatter sunlight to cool climate. The net forcing depends strongly on the composition, mixing state and transformations of these carbonaceous aerosols. Complexities from large variability of fuel types, combustion conditions and aging processes have confounded their treatment in models. We analyse recent laboratory and field measurements to uncover fundamental mechanism that control the chemical, optical and microphysical properties of carbonaceous aerosols that are elaborated below: Wavelength dependence of absorption and the single scattering albedo (ω) of fresh biomass burning aerosols produced from many fuels during FLAME-4 was analysed to determine the factors that control the variability in ω. Results show that ω varies strongly with fire-integrated modified combustion efficiency (MCEFI)—higher MCEFI results in lower ω values and greater spectral dependence of ω (Liu et al GRL 2014). A parameterization of ω as a function of MCEFI for fresh BB aerosols is derived from the laboratory data and is evaluated by field data, including BBOP. Our laboratory studies also demonstrate that BrC production correlates with BC indicating that that they are produced by a common mechanism that is driven by MCEFI (Saleh et al NGeo 2014). We show that BrC absorption is concentrated in the extremely low volatility component that favours long-range transport. We observe substantial absorption enhancement for internally mixed BC from diesel and wood combustion near London during ClearFlo. While the absorption enhancement is due to BC particles coated by co-emitted OC in urban regions, it increases with photochemical age in rural areas and is simulated by core-shell models. We measure BrC absorption that is concentrated in the extremely low volatility components and attribute it to wood burning. Our results support enhanced light absorption by internally mixed BC parameterizations in models and identify mixed biomass and fossil combustion regions where this effect is large. We unify the treatment of carbonaceous aerosol components and their interactions to simplify and verify their representation in climate models, and re-evaluate their direct radiative forcing.
Impact of dimethylsulfide chemistry on sulfate over the Northern Hemisphere
Sulfate aerosol forms from the gas- and aqueous-phase oxidation of sulfur dioxide and is an important component of atmospheric aerosols. Dimethylsulfide (DMS) present in sea-water can be emitted into the atmosphere which can then react with atmospheric oxidants to produce sulfur ...
Cellular component of lavage fluid from broilers with normal versus aerosol-primed airways
USDA-ARS?s Scientific Manuscript database
Previously we reported that intratracheal administration of lipopolysaccharide (LPS) elicits pulmonary hypertension (PH) in broilers reared under commercial conditions, in broilers reared in environmental chambers and pre-treated with aerosolized red food colorant # 3 and propylene glycol (Red#3+PG)...
Cloud forming potential of oligomers relevant to secondary organic aerosols
NASA Astrophysics Data System (ADS)
Xu, Wen; Guo, Song; Gomez-Hernandez, Mario; Zamora, Misti L.; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Zhang, Annie L.; Collins, Don R.; Zhang, Renyi
2014-09-01
The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity are measured for surrogates that mimic atmospherically relevant oligomers, including glyoxal trimer dihydrate, methyl glyoxal trimer dihydrate, sucrose, methyl glyoxal mixtures with sulfuric acid and glycolic acid, and 2,4-hexandienal mixtures with sulfuric acid and glycolic acid. For the single-component aerosols, the measured HGF ranges from 1.3 to 1.4 at a relative humidity of 90%, and the hygroscopicity parameter (κ) is in the range of 0.06 to 0.19 on the basis of the measured CCN activity and 0.13 to 0.22 on the basis of the measured HGF, compared to the calculated values of 0.08 to 0.16. Large differences exist in the κ values derived using the measured HGF and CCN data for the multi-component aerosols. Our results reveal that, in contrast to the oxidation process, oligomerization decreases particle hygroscopicity and CCN activity and provides guidance for analyzing the organic species in ambient aerosols.
NASA Astrophysics Data System (ADS)
Ogorodnikov, B. I.
2018-06-01
The results of the physicochemical studies of radioactive aerosols inside and outside the Shelter construction at the Arch construction stage of the Chernobyl Nuclear Power Plant (ChNPP) in 2000-2015 were presented. The dominant isotopes were shown to be cesium, strontium, americium, plutonium, and uranium. They are carried by disperse particles of 2-7 μm. In subreactor rooms, in particular, 012/7, the composition of aerosols is affected by the erosion of the fuel-containing mass formed in 1986. Submicron cesium carrier aerosols appear as a result of evaporation and condensation during fires and welding works. Radiocesium is a well-soluble component of aerosols, while plutonium isotopes are not readily soluble components. In several rooms, the contents of radon, thoron, and their daughter products exceeded the permissible values. In April-June 2011, the intake of radionuclides from the accident at the Japanese Fukushima-1 NPP, which had AMAD of 0.5 μm, was detected and tracked using Petryanov multilayer filters. The productivity of filtration units under the dusty conditions in the exclusion zone of ChNPP and in fogs and haze was investigated. Hydrophilic prefilters with 7-10 μm fibers were recommended.
NASA Astrophysics Data System (ADS)
Hyer, E. J.; Zhang, J. L.; Reid, J. S.; Curtis, C. A.; Westphal, D. L.
2007-12-01
Quantitative models of the transport and evolution of atmospheric pollution have graduated from the laboratory to become a part of the operational activity of forecast centers. Scientists studying the composition and variability of the atmosphere put great efforts into developing methods for accurately specifying sources of pollution, including natural and anthropogenic biomass burning. These methods must be adapted for use in operational contexts, which impose additional strictures on input data and methods. First, only input data sources available in near real-time are suitable for use in operational applications. Second, operational applications must make use of redundant data sources whenever possible. This is a shift in philosophy: in a research context, the most accurate and complete data set will be used, whereas in an operational context, the system must be designed with maximum redundancy. The goal in an operational context is to produce, to the extent possible, consistent and timely output, given sometimes inconsistent inputs. The Naval Aerosol Analysis and Prediction System (NAAPS), a global operational aerosol analysis and forecast system, recently began incorporating assimilation of satellite-derived aerosol optical depth. Assimilation of satellite AOD retrievals has dramatically improved aerosol analyses and forecasts from this system. The use of aerosol data assimilation also changes the strategy for improving the smoke source function. The absolute magnitude of emissions events can be refined through feedback from the data assimilation system, both in real- time operations and in post-processing analysis of data assimilation results. In terms of the aerosol source functions, the largest gains in model performance are now to be gained by reducing data latency and minimizing missed detections. In this presentation, recent model development work on the Fire Locating and Monitoring of Burning Emissions (FLAMBE) system that provides smoke aerosol boundary conditions for NAAPS is described, including redundant integration of multiple satellite platforms and development of feedback loops between the data assimilation system and smoke source.
Recent advances in understanding secondary organic aerosols: implications for global climate forcing
NASA Astrophysics Data System (ADS)
Shrivastava, Manish
2017-04-01
Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the 'climate sensitivity'). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, often represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This presentation is based on a US Department of Energy Atmospheric Systems Research sponsored workshop, which highlighted key SOA processes overlooked in climate models that could greatly affect climate forcing estimates. We will highlight the importance of processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. We also highlight some of the recently discovered important processes that involve interactions between natural biogenic emissions and anthropogenic emissions such as effects of sulfur and NOx emissions on SOA. We will present examples of integrated model-measurement studies that relate the observed evolution of organic aerosol mass and number with knowledge of particle properties such as volatility and viscosity. We will also highlight the importance of continuing efforts to rank the most influential SOA processes that affect climate forcing, but are often missing in climate models. Ultimately, gas- and particle-phase chemistry processes that capture the dynamic evolution of number and mass concentrations of SOA particles need to be accurately and efficiently represented in regional and global atmospheric chemistry-climate models.
How accurately can the instantaneous aerosol effect on cloud albedo be constrained?
NASA Astrophysics Data System (ADS)
Gryspeerdt, E.; Quaas, J.; Ferrachat, S.; Gettelman, A.; Ghan, S. J.; Lohmann, U.; Neubauer, D.; Morrison, H.; Partridge, D.; Stier, P.; Takemura, T.; Wang, H.; Wang, M.; Zhang, K.
2017-12-01
Aerosol-cloud interactions are the most uncertain component of the anthropogenic radiative forcing, with a significant fraction of this uncertainty coming from uncertainty in the radiative forcing due to instantaneous changes in cloud albedo (the RFaci). Aerosols can have a strong influence on the cloud droplet number concentration (CDNC), so previous studies have used the sensitivity of CDNC to aerosol properties as a method of estimating the RFaci. However, recent studies have suggested that this sensitivity is unsuitable as a constraint on the RFaci, as it differs in the present day and pre-industrial atmosphere. This would place significant limits on our ability to constrain the RFaci from satellite observations. In this study, a selection of global aerosol-climate models are used to investigate the suitability of various aerosol proxies and methods for calculating the RFaci from present day data. A linear-regression based sensitivity of CDNC to aerosol perturbations can lead to large errors in the diagnosed RFaci, as can the use of the aerosol optical depth (AOD) as an aerosol proxy. However, we show that if suitable choices of aerosol proxy are made and the anthropogenic aerosol contribution is known, it is possible to diagnose the anthropogenic change in CDNC, and so the RFaci, using present day aerosol-cloud relationships.
NASA Astrophysics Data System (ADS)
Gorzynski, Mark; Derocher, Mike; Mitchell, April Slayden
Research underway at Hewlett-Packard on remote communication resulted in the identification of three important components typically missing in existing systems. These missing components are: group nonverbal communication capabilities, high-resolution interactive data capabilities, and global services. Here we discuss some of the design elements in these three areas as part of the Halo program at HP, a remote communication system shown to be effective to end-users.
MODELS-3 COMMUNITY MULTISCALE AIR QUALITY (CMAQ) MODEL AEROSOL COMPONENT 2. MODEL EVALUATION
Ambient air concentrations of particulate matter (atmospheric suspensions of solid of liquid materials, i.e., aerosols) continue to be a major concern for the U.S. Environmental Protection Agency (EPA). High particulate matter (PM) concentrations are associated not only with adv...
Organic Aerosol Composition and Sources in Pasadena, California during the 2010 CalNex Campaign
Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) ...
USING CMAQ-AIM TO EVALUATE THE GAS-PARTICLE PARTITIONING TREATMENT IN CMAQ
The Community Multi-scale Air Quality model (CMAQ) aerosol component utilizes a modal representation, where the size distribution is represented as a sum of three lognormal modes. Though the aerosol treatment in CMAQ is quite advanced compared to other operational air quality mo...
Error reporting in transfusion medicine at a tertiary care centre: a patient safety initiative.
Elhence, Priti; Shenoy, Veena; Verma, Anupam; Sachan, Deepti
2012-11-01
Errors in the transfusion process can compromise patient safety. A study was undertaken at our center to identify the errors in the transfusion process and their causes in order to reduce their occurrence by corrective and preventive actions. All near miss, no harm events and adverse events reported in the 'transfusion process' during 1 year study period were recorded, classified and analyzed at a tertiary care teaching hospital in North India. In total, 285 transfusion related events were reported during the study period. Of these, there were four adverse (1.5%), 10 no harm (3.5%) and 271 (95%) near miss events. Incorrect blood component transfusion rate was 1 in 6031 component units. ABO incompatible transfusion rate was one in 15,077 component units issued or one in 26,200 PRBC units issued and acute hemolytic transfusion reaction due to ABO incompatible transfusion was 1 in 60,309 component units issued. Fifty-three percent of the antecedent near miss events were bedside events. Patient sample handling errors were the single largest category of errors (n=94, 33%) followed by errors in labeling and blood component handling and storage in user areas. The actual and near miss event data obtained through this initiative provided us with clear evidence about latent defects and critical points in the transfusion process so that corrective and preventive actions could be taken to reduce errors and improve transfusion safety.
NASA Astrophysics Data System (ADS)
Jing, Bo; Wang, Zhen; Tan, Fang; Guo, Yucong; Tong, Shengrui; Wang, Weigang; Zhang, Yunhong; Ge, Maofa
2018-04-01
While nitrate salts have critical impacts on environmental effects of atmospheric aerosols, the effects of coexisting species on hygroscopicity of nitrate salts remain uncertain. The hygroscopic behaviors of nitrate salt aerosols (NH4NO3, NaNO3, Ca(NO3)2) and their internal mixtures with water-soluble organic acids were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA). The nitrate salt / organic acid mixed aerosols exhibit varying phase behavior and hygroscopic growth depending upon the type of components in the particles. Whereas pure nitrate salt particles show continuous water uptake with increasing relative humidity (RH), the deliquescence transition is still observed for ammonium nitrate particles internally mixed with organic acids such as oxalic acid and succinic acid with a high deliquescence point. The hygroscopicity of submicron aerosols containing sodium nitrate and an organic acid is also characterized by continuous growth, indicating that sodium nitrate tends to exist in a liquid-like state under dry conditions. It is observed that in contrast to the pure components, the water uptake is hindered at low and moderate RH for calcium nitrate particles containing malonic acid or phthalic acid, suggesting the potential effects of mass transfer limitation in highly viscous mixed systems. Our findings improve fundamental understanding of the phase behavior and water uptake of nitrate-salt-containing aerosols in the atmospheric environment.
Spread of acid rain over India
NASA Astrophysics Data System (ADS)
Khemani, L. T.; Momin, G. A.; Rao, P. S. Prakasa; Safai, P. D.; Singh, G.; Kapoor, R. K.
Rain water and aerosol samples were collected at a few locations representative of urban and non-urban regions in India. Also, rain water samples were collected in and around a coal-fired power plant. All the rain water and aerosol samples were analyzed for major chemical components along with pH. The rain water at all the places of measurement, except near the industrial sources, has been found to be alkaline and was characterized by the presence of excess cations, particularly by Ca 2+. The acid rain near the industrial sources was associated with excess anions, especially SO 42-. The atmospheric aerosols at all the places of measurement were found rich with basic components, suggesting that the alkaline soil dust and fly ash are responsible at present for preventing the spread of acid rain in India.
NASA Technical Reports Server (NTRS)
Buchard, Virginie; Da Silva, Arlindo; Todling, Ricardo
2017-01-01
In the GEOS near real-time system, as well as in MERRA-2 which is the latest reanalysis produced at NASAs Global Modeling and Assimilation Office(GMAO), the assimilation of aerosol observations is performed by means of a so-called analysis splitting method. In line with the transition of the GEOS meteorological data assimilation system to a hybrid Ensemble-Variational formulation, we are updating the aerosol component of our assimilation system to an ensemble square root filter(EnSRF; Whitaker and Hamill (2002)) type of scheme.We present a summary of our preliminary results of the assimilation of column integrated aerosol observations (Aerosol Optical Depth; AOD) using an Ensemble Square Root Filters (EnSRF) scheme and the ensemble members produced routinely by the meteorological assimilation.
Solar Spectral Radiative Forcing Due to Dust Aerosol During the Puerto Rico Dust Experiment
NASA Technical Reports Server (NTRS)
Pilewskie, P.; Bergstrom, R.; Rabbette, M.; Livingston, J.; Russell, P.; Gore, Warren J. (Technical Monitor)
2000-01-01
During the Puerto Rico Dust Experiment (PRIDE) upwelling and downwelling solar spectral irradiance was measured on board the SPAWAR Navajo and downwelling solar spectral flux was measured at a surface site using the NASA Ames Solar Spectral Flux Radiometer. These data will be used to determine the net solar radiative forcing of dust aerosol and to quantify the solar spectral radiative energy budget in the presence of elevated aerosol loading. We will assess the variability in spectral irradiance using formal principal component analysis procedures and relate the radiative variability to aerosol microphysical properties. Finally, we will characterize the sea surface reflectance to improve aerosol optical depth retrievals from the AVHRR satellite and to validate SeaWiFS ocean color products.
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 the CALIOP attenuated backscatter profiles and constrained by the CALIOP DR ACAOD retrievals are also found to agree well on average with coincident HSRL-2 extinction profiles. These constrained CALIOP extinction profiles are used to characterize the smoke distribution over this region.
Translations on Narcotics and Dangerous Drugs, Number 312
1977-07-29
to be sold P wn’v Sol Tn another search, seven blank tubes and two orders f 200 tLs te discovered. The aspects were identified as Miss...he shot a couple in the La Brasa restaurant, and made a quick get-away on a motor- cycle. Sergio Anibal Velasquez Perez and Luz Elpidia Murillo...messengers Resistol 5,000, Pega Todo, sol - vents, aerosol and gasoline." As to these persons’ guilt, he said, We cannot say that they are directly
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.
NASA Astrophysics Data System (ADS)
Meng, X.; Liu, Y.; Diner, D. J.; Garay, M. J.
2016-12-01
Ambient fine particle (PM2.5) has been positively associated with increased mortality and morbidity worldwide. Recent studies highlight the characteristics and differential toxicity of PM2.5 chemical components, which are important for identifying sources, developing targeted particulate matter (PM) control strategies, and protecting public health. Modelling with satellite retrieved data has been proved as the most cost-effective way to estimate ground PM2.5 levels; however, limited studies have predict PM2.5 chemical components with this method. In this study, the experimental MISR 4.4 km aerosol retrievals were used to predict ground-level particle sulfate, nitrite, organic carbon and element carbon concentrations in 16 counties of southern California. The PM2.5 chemical components concentrations were obtained from the National Chemical Speciation Network (CSN) and the Interagency Monitoring of Protected Visual Environments (IMPROVE) network. A generalized additive model (GAM) was developed based on 16-years data (2000-2015) by combining the MISR aerosol retrievals, meteorological variables and geographical indicators together. Model performance was assessed by model fitted R2 and root-mean-square error (RMSE) and 10-fold cross validation. Spatial patterns of sulfate, nitrate, OC and EC concentrations were also examined with 2-D prediction surfaces. This is the first attempt to develop high-resolution spatial models to predict PM2.5 chemical component concentrations with MISR retrieved aerosol properties, which will provide valuable population exposure estimates for future studies on the characteristics and differential toxicity of PM2.5 speciation.
Aerosol retrieval experiments in the ESA Aerosol_cci project
NASA Astrophysics Data System (ADS)
Holzer-Popp, T.; de Leeuw, G.; Martynenko, D.; Klüser, L.; Bevan, S.; Davies, W.; Ducos, F.; Deuzé, J. L.; Graigner, R. G.; Heckel, A.; von Hoyningen-Hüne, W.; Kolmonen, P.; Litvinov, P.; North, P.; Poulsen, C. A.; Ramon, D.; Siddans, R.; Sogacheva, L.; Tanre, D.; Thomas, G. E.; Vountas, M.; Descloitres, J.; Griesfeller, J.; Kinne, S.; Schulz, M.; Pinnock, S.
2013-03-01
Within the ESA Climate Change Initiative (CCI) project Aerosol_cci (2010-2013) algorithms for the production of long-term total column aerosol optical depth (AOD) datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1) a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2) a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome) applied to four months of global data to identify mature algorithms, and (3) a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components and their mixing ratios. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008) of data qualitatively by visible analysis of monthly mean AOD maps and quantitatively by comparing global daily gridded satellite data against daily average AERONET sun photometer observations for the different versions of each algorithm. The analysis allowed an assessment of sensitivities of all algorithms which helped define the best algorithm version for the subsequent round robin exercise; all algorithms (except for MERIS) showed some, in parts significant, improvement. In particular, using common aerosol components and partly also a priori aerosol type climatology is beneficial. On the other hand the use of an AATSR-based common cloud mask meant a clear improvement (though with significant reduction of coverage) for the MERIS standard product, but not for the algorithms using AATSR.
NASA Technical Reports Server (NTRS)
Kaufman, Yoram J.; Tanre, Didier; Remer, Lorraine; Martins, Vanderlei; Schoeberl, Mark; Lau, William K. M. (Technical Monitor)
2001-01-01
The MODIS instrument was launched on the NASA Terra satellite in Dec. 1999. Since last Oct, the sensor and the aerosol algorithm reached maturity and provide global daily retrievals of aerosol optical thickness and properties. MODIS has 36 spectral channels in the visible to IR with resolution down to 250 m. This allows accurate cloud screening and multi-spectral aerosol retrievals. We derive the aerosol optical thickness over the ocean and most of the land areas, distinguishing between fine (mainly man-made aerosol) and coarse (mainly natural) aerosol particles. New methods to derive the aerosol absorption of sunlight are also being developed. These measurements are use to track different aerosol sources, transport and the radiative forcing at the top and bottom of the atmosphere. However MODIS or any present satellite sensor cannot measure absorption by Black Carbon over the oceans, a critical component in studying climate change and human health. For this purpose we propose the COBRA mission that observes the ocean at glint and off glint simultaneously measuring the spectral polarized light and deriving precisely the aerosol absorption.
Characterization of Florida red tide aerosol and the temporal profile of aerosol concentration.
Cheng, Yung Sung; Zhou, Yue; Pierce, Richard H; Henry, Mike; Baden, Daniel G
2010-05-01
Red tide aerosols containing aerosolized brevetoxins are produced during the red tide bloom and transported by wind to coastal areas of Florida. This study reports the characterization of Florida red tide aerosols in human volunteer studies, in which an asthma cohort spent 1h on Siesta Beach (Sarasota, Florida) during aerosolized red tide events and non-exposure periods. Aerosol concentrations, brevetoxin levels, and particle size distribution were measured. Hourly filter samples were taken and analyzed for brevetoxin and NaCl concentrations. In addition, the aerosol mass concentration was monitored in real time. The results indicated that during a non-exposure period in October 2004, no brevetoxin was detected in the water, resulting in non-detectable levels of brevetoxin in the aerosol. In March 2005, the time-averaged concentrations of brevetoxins in water samples were moderate, in the range of 5-10 microg/L, and the corresponding brevetoxin level of Florida red tide aerosol ranged between 21 and 39 ng/m(3). The temporal profiles of red tide aerosol concentration in terms of mass, NaCl, and brevetoxin were in good agreement, indicating that NaCl and brevetoxins are components of the red tide aerosol. By continuously monitoring the marine aerosol and wind direction at Siesta Beach, we observed that the marine aerosol concentration varied as the wind direction changed. The temporal profile of the Florida red tide aerosol during a sampling period could be explained generally with the variation of wind direction. Copyright 2009 Elsevier Ltd. All rights reserved.
pH Variance in Aerosols Undergoing Liquid-Liquid Phase Separation
NASA Astrophysics Data System (ADS)
Eddingsaas, N. C.; Dallemagne, M.; Huang, X.
2014-12-01
The water content of aerosols is largely governed by relative humidity (RH). As the relative humidity decreases, and thus the water content of aerosols, a number of processes occur including the shrinking of aerosols, the increase in concentration of components, and potentially the formation of liquid liquid phase separation (llps) due to the salting out of inorganic salts. The most ubiquitous salt in atmospheric aerosols is ammonium sulfate which results in many aerosols to be at least mildly acidic. However, during llps, the pH of the different phases is not necessarily the same. Many reactions that take place within atmospheric aerosols are acid catalyzed so a better understanding of the pH of the individual phases as well as the interface between the phases is important to understanding aerosol processing and aging. Through the use of pH sensitive dyes and confocal microscopy we have directly measured the pH of micron sized model aerosols during high RH where the aerosols are in a single phase, at intermediate while the aerosols are in llps, and low RH where the aerosols consist of one liquid phase and one solid phase. We will discuss the variation in RH during these different phase states in the presence and absence of excess sulfuric acid. We will also discuss how this variation in pH affects aging of aerosols.
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.;
2012-01-01
Knowledge of the vertical profile, composition, concentration, and size of aerosols is required for assessing the direct impact of aerosols on radiation, the indirect effects of aerosols on clouds and precipitation, and attributing these effects to natural and anthropogenic aerosols. Because anthropogenic aerosols are predominantly submicrometer, fine mode fraction (FMF) retrievals from satellite have been used as a tool for deriving anthropogenic aerosols. Although column and profile satellite retrievals of FMF have been performed over the ocean, such retrievals have not yet been been done over land. Consequently, uncertainty in satellite estimates of the anthropogenic component of the aerosol direct radiative forcing is greatest over land, due in large part to uncertainties in the FMF. Satellite measurements have been used to detect and evaluate aerosol impacts on clouds; however, such efforts have been hampered by the difficulty in retrieving vertically-resolved cloud condensation nuclei (CCN) concentration, which is the most direct parameter linking aerosol and clouds. Recent studies have shown correlations between average satellite derived column aerosol optical thickness (AOT) and in situ measured CCN. However, these same studies, as well as others that use detailed airborne in situ measurements have noted that vertical variability of the aerosol distribution, impacts of relative humidity, and the presence of coarse mode aerosols such as dust introduce large uncertainties in such relations.
Secondary organic aerosols (SOA), known to form in the atmosphere from oxidation of volatile organic compounds (VOCs) emitted by anthropogenic and biogenic sources, are a poorly understood but substantial component of atmospheric particles. In this study, we examined the chemic...
Light Absorption Properties and Radiative Effects of Primary Organic Aerosol Emissions
Organic aerosols (OA) in the atmosphere affect Earth’s energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called “brown carbon” (BrC) component. However, the absorptivities of OA are not or poorly represented in current climate m...
ESTIMATION OF DIFFUSION LOSSES WHEN SAMPLING DIESEL AEROSOL: A QUALITY ASSURANCE MEASURE
A fundamental component of the QA work for the assessment of instruments and sampling system performance was the investigation of particle losses in sampling lines. Along the aerosol sample pathway from its source to the collection media or measuring instrument, some nano-size p...
NASA Astrophysics Data System (ADS)
Mamali, Dimitra; Marinou, Eleni; Pikridas, Michael; Kottas, Michael; Binietoglou, Ioannis; Kokkalis, Panagiotis; Tsekeri, Aleksandra; Amiridis, Vasilis; Sciare, Jean; Keleshis, Christos; Engelmann, Ronny; Ansmann, Albert; Russchenberg, Herman W. J.; Biskos, George
2017-04-01
Vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) measurements were compared to airborne dried optical particle counter (OPC MetOne; Model 212) measurements during the INUIT-BACCHUS-ACTRIS campaign. The campaign took place in April 2016 and its main focus was the study of aerosol dust particles. During the campaign the NOA Polly-XT Raman lidar located at Nicosia (35.08° N, 33.22° E) was providing round-the-clock vertical profiles of aerosol optical properties. In addition, an unmanned aerial vehicle (UAV) carrying an OPC flew on 7 days during the first morning hours. The flights were performed at Orounda (35.1018° N, 33.0944° E) reaching altitudes of 2.5 km a.s.l, which allows comparison with a good fraction of the recorded lidar data. The polarization lidar photometer networking method (POLIPHON) was used for the estimation of the fine (non-dust) and coarse (dust) mode aerosol mass concentration profiles. This method uses as input the particle backscatter coefficient and the particle depolarization profiles of the lidar at 532 nm wavelength and derives the aerosol mass concentration. The first step in this approach makes use of the lidar observations to separate the backscatter and extinction contributions of the weakly depolarizing non-dust aerosol components from the contributions of the strongly depolarizing dust particles, under the assumption of an externally mixed two-component aerosol. In the second step, sun photometer retrievals of the fine and the coarse modes aerosol optical thickness (AOT) and volume concentration are used to calculate the associated concentrations from the extinction coefficients retrieved from the lidar. The estimated aerosol volume concentrations were converted into mass concentration with an assumption for the bulk aerosol density, and compared with the OPC measurements. The first results show agreement within the experimental uncertainty. This project received funding from the European Union's Seventh Framework Programme (FP7) project BACCHUS under grant agreement no. 603445, and the European Union's Horizon 2020 research and innovation programme ACTRIS-2 under grant agreement No 654109.
NASA Astrophysics Data System (ADS)
Zhou, Chunhong; Shen, Xiaojing; Liu, Zirui; Zhang, Yangmei; Xin, Jinyuan
2018-04-01
A coupled aerosol-cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES-CUACE [Global/Regional Assimilation and PrEdiction System-China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES-CUACE simulations were verified against observational data during 1-31 January 2013, when a series of heavy regional haze-fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient grew from 0.35 to 0.61, and the mean mass concentration went up from 43% to 87.5% of the observed value. Thus, the simulation of particulate matters in these areas has been improved considerably.
NASA Astrophysics Data System (ADS)
Kaul, D. S.; Gupta, T.; Tripathi, S. N.
2012-06-01
An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by increase in the modal diameter of the size distribution during foggy episodes and growth in the diameter of the particles upon the fog evaporation.
Post-Flight Test Results of Acousto-Optic Modulator Devices Subjected to Space Exposure
NASA Technical Reports Server (NTRS)
Prasad, Narasimha S.; Trivedi, Sudhir; Rosemeier, Jolanta; Diestler, Mark
2014-01-01
The objective of the Materials International Space Station Experiment (MISSE) is to study the performance of novel materials when subjected to the synergistic effects of the harsh space environment for several months. MISSE missions provide an opportunity for developing space qualifiable materials. Several laser and lidar components were sent by NASA Langley Research Center (LaRC) as a part of the MISSE 7 mission. The MISSE 7 module was transported to the international space station (ISS) via STS 129 mission that was launched on Nov 16, 2009. Later, the MISSE 7 module was brought back to the earth via the STS 134 that landed on June 1, 2011. The MISSE 7 module that was subjected to exposure in a space environment for more than one and a half years included fiber laser, solid-state laser gain materials, detectors, and semiconductor laser diode. Performance testing of these components is now progressing. In this paper, the results of performance testing of a laser diode module sent by NASA Langley Research Center on MISSE 7 mission will be discussed. This paper will present the comparison of pre-flight and post-flight performance of two different COTS acousto-optic modulator (AOM) devices. Post-flight measurements indicate that these two devices did not undergo any significant performance degradation.
Post-flight test results of acousto-optic modulator devices subjected to space exposure
NASA Astrophysics Data System (ADS)
Prasad, Narasimha S.; Trivedi, Sudhir; Rosemeier, Jolanta; Diestler, Mark
2014-09-01
The objective of the Materials International Space Station Experiment (MISSE) is to study the performance of novel materials when subjected to the synergistic effects of the harsh space environment for several months. MISSE missions provide an opportunity for developing space qualifiable materials. Several laser and lidar components were sent by NASA Langley Research Center (LaRC) as a part of the MISSE 7 mission. The MISSE 7 module was transported to the international space station (ISS) via STS 129 mission that was launched on Nov 16, 2009. Later, the MISSE 7 modulewas brought back to the earth via the STS 134 that landed on June 1, 2011. The MISSE 7 module that was subjected to exposure in space environment for more than one and a half year included fiber laser, solid-state laser gain materials, detectors, and semiconductor laser diode. Performance testing of these components is now progressing. In this paper, the results of performance testing of a laser diode module sent by NASA Langley Research Center on MISSE 7 mission will be discussed. This paper will present the comparison of pre-flight and post-flight performance of two different COTS acousto-optic modulator devices. Post-flight measurements indicate that these two devices did not undergo any significant performance degradation.
Effects of mixing states on the multiple-scattering properties of soot aerosols.
Cheng, Tianhai; Wu, Yu; Gu, Xingfa; Chen, Hao
2015-04-20
The radiative properties of soot aerosols are highly sensitive to the mixing states of black carbon particles and other aerosol components. Light absorption properties are enhanced by the mixing state of soot aerosols. Quantification of the effects of mixing states on the scattering properties of soot aerosol are still not completely resolved, especially for multiple-scattering properties. This study focuses on the effects of the mixing state on the multiple scattering of soot aerosols using the vector radiative transfer model. Two types of soot aerosols with different mixing states such as external mixture soot aerosols and internal mixture soot aerosols are studied. Upward radiance/polarization and hemispheric flux are studied with variable soot aerosol loadings for clear and haze scenarios. Our study showed dramatic changes in upward radiance/polarization due to the effects of the mixing state on the multiple scattering of soot aerosols. The relative difference in upward radiance due to the different mixing states can reach 16%, whereas the relative difference of upward polarization can reach 200%. The effects of the mixing state on the multiple-scattering properties of soot aerosols increase with increasing soot aerosol loading. The effects of the soot aerosol mixing state on upwelling hemispheric flux are much smaller than in upward radiance/polarization, which increase with increasing solar zenith angle. The relative difference in upwelling hemispheric flux due to the different soot aerosol mixing states can reach 18% when the solar zenith angle is 75°. The findings should improve our understanding of the effects of mixing states on the optical properties of soot aerosols and their effects on climate. The mixing mechanism of soot aerosols is of critical importance in evaluating the climate effects of soot aerosols, which should be explicitly included in radiative forcing models and aerosol remote sensing.
NASA Astrophysics Data System (ADS)
Andrade, Fatima; Orsini, Celso; Maenhaut, Willy
Stacked filter units were used to collect atmospheric particles in separate coarse and fine fractions at the Sao Paulo University Campus during the winter of 1989. The samples were analysed by particle-induced X-ray emission (PIXE) and the data were subjected to an absolute principal component analysis (APCA). Five sources were identified for the fine particles: industrial emissions, which accounted for 13% of the fine mass; emissions from residual oil and diesel, explaining 41%; resuspended soil dust, with 28%; and emissions of Cu and of Mg, together with 18%. For the coarse particles, four sources were identified: soil dust, accounting for 59% of the coarse mass; industrial emissions, with 19%; oil burning, with 8%; and sea salt aerosol, with 14% of the coarse mass. A data set with various meteorological parameters was also subjected to APCA, and a correlation analysis was performed between the meteorological "absolute principal component scores" (APCS) and the APCS from the fine and coarse particle data sets. The soil dust sources for the fine and coarse aerosol were highly correlated with each other and were anticorrelated with the sea breeze component. The industrial components in the fine and coarse size fractions were also highly positively correlated. Furthermore, the industrial component was related with the northeasterly wind direction and, to a lesser extent, with the sea breeze component.
Chemical composition of atmospheric aerosols resolved via positive matrix factorization
NASA Astrophysics Data System (ADS)
Äijälä, Mikko; Junninen, Heikki; Heikkinen, Liine; Petäjä, Tuukka; Kulmala, Markku; Worsnop, Douglas; Ehn, Mikael
2017-04-01
Atmospheric particulate matter is a complex mixture of various chemical species such as organic compounds, sulfates, nitrates, ammonia, chlorides, black carbon and sea salt. As aerosol chemical composition strongly influences aerosol climate effects (via cloud condensation nucleus activation, hygroscopic properties, aerosol optics, volatility and condensation) as well as health effects (toxicity, carcinogenicity, particle morphology), detailed understanding of atmospheric fine particle composition is widely beneficial for understanding these interactions. Unfortunately the comprehensive, detailed measurement of aerosol chemistry remains difficult due to the wide range of compounds present in the atmosphere as well as for the miniscule mass of the particles themselves compared to their carrier gas. Aerosol mass spectrometer (AMS; Canagaratna et al., 2007) is an instrument often used for characterization of non-refractive aerosol types: the near-universal vaporization and ionisation technique allows for measurement of most atmospheric-relevant compounds (with the notable exception of refractory matter such as sea salt, black carbon, metals and crustal matter). The downside of the hard ionisation applied is extensive fragmentation of sample molecules. However, the apparent loss of information in fragmentation can be partly offset by applying advanced statistical methods to extract information from the fragmentation patterns. In aerosol mass spectrometry statistical analysis methods, such as positive matrix factorization (PMF; Paatero, 1999) are usually applied for aerosol organic component only, to keep the number of factors to be resolved manageable, to retain the inorganic components for solution validation via correlation analysis, and to avoid inorganic species dominating the factor model. However, this practice smears out the interactions between organic and inorganic chemical components, and hinders the understanding of the connections between primary and secondary aerosols via atmospheric physicochemical processes (e.g. condensation and evaporation of gases) and on the other hand the potential non-linear summation (Spracklen et al., 2011 2011) of anthropogenic and biogenic aerosol emissions. From the perspective of statistical analysis there is no definite reason why inorganics could not be included, as long as their uncertainties are estimated correctly and their influence is properly weighted in the factor model. For result validation, external, additional information available from most measurement sites, such as correlations with trace gas concentrations or size distribution derived, mode-specific mass loadings can be used instead of AMS inorganics. In recent analyses, nitrate compounds have already been added to PMF analyses and shown to interact with organic semi-volatile compounds (Hao et al., 2014). In this study we tested including all the default AMS chemical species, i.e. organics, sulfates, nitrates, ammonia and chlorides, in a PMF analysis, and present potential interpretations of the results with regard to aerosol sources and the chemical processes shaping the aerosol types. In addition to resolving organic-dominated aerosol classes, the results shed light on inorganic salt formation and may imply formation of organics salts. Canagaratna, M. et al. (2007). Mass Spectrom Rev., 26:185-222. Hao, L. et al. (2014). Atmos. Chem. Phys., 14, 13483-13495. Paatero, P. (1999). J Comput Graph Stat, 8: 854-888. Spracklen, D. et al (2011) Atmos. Chem. Phys., 11, 12109-12136.
NASA Astrophysics Data System (ADS)
Dubey, M. K.; Bixler, S. L.; Romonosky, D.; Lam, J.; Carrico, C.; Aiken, A. C.
2017-12-01
Biomass burning aerosol emissions have substantially increased with observed warming and drying in the southwestern US. While wildfires are projected to intensify missing knowledge on the aerosols hampers assessments. Observations demonstrate that enhanced light absorption by coated black carbon and brown carbon can offset the cooling effects of organic aerosols in wildfires. However, if mixing processes that enhance this absorption reduce the aerosol lifetime it would lower their atmospheric burden. In order to elucidate mechanisms regulating this tradeoff we performed laboratory studies of smoke from biomass burning. We focus on aerosol optical properties and their hygroscopic response. Fresh emissions from burning 30 fuels under flaming and smoldering conditions were investigated. We measured aerosol absorption, scattering and extinction at multiple wavelengths, water uptake at 85% relative humidity (fRH85%) with a humidity controlled dual nephelometer, and black carbon mass with a SP2. Trace gases and the ionic content of the fuel and smoke were also measured We find that whereas the optical properties of smoke were strongly dictated by the flaming versus smoldering nature of the burn, the observed hygroscopicity was intimately linked to the chemical composition of the fuel. The mean hygroscopicity ranged from nearly hydrophobic (fRH85% = 1) to very hydrophilic (fRH85% = 2.1) values typical of pure deliquescent salts. The k values varied from 0.004 to 0.18 and correlated well with inorganic content. Inorganic fuel content was the key driver of hygroscopicity with combustion phase playing a secondary but important role ( 20%). Flaming combustion promoted hygroscopicity by generating refractory black carbon and ions. Smoldering combustion suppressed hygroscopicity by producing hydrogenated organic species. Wildfire smoke was hydrophobic since the evergreen species with low inorganic content dominated in these fires. We also quantify the mass absorption cross-sections at 780nm and 430nm to evaluate the absorbing species. We plan to extend our studies to aged biomass burning smoke with a potential aerosol mass reactor and monitor the ionic content of black carbon with a SP-AMS. Our analysis will develop a mechanistic framework of water uptake and optical properties of biomass burning aerosols.
NASA Technical Reports Server (NTRS)
Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.
2013-01-01
Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad families of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA 0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA 0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savanna at Mongu (Zambia), with average SSA 0.85 in the midvisible. These can serve as candidate sets of aerosol microphysicaloptical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.
A stratospheric aerosol increase
NASA Technical Reports Server (NTRS)
Rosen, J. M.; Hofmann, D. J.
1980-01-01
Large disturbances were noted in the stratospheric aerosol content in the midlatitude Northern Hemisphere commencing about 7 months after the eruption of La Soufriere and less than 1 month after the eruption of Sierra Negra. The aerosol was characterized by a very steep size distribution in the 0.15 to 0.25 micron radius range and contained a volatile component. Measurements near the equator and at the South Pole indicate that the disturbance was widespread. These observations were made before the May 18 eruption of Mt. St. Helens.
Choi, Jong-Kyu; Ban, Soo-Jin; Kim, Yong-Pyo; Kim, Yong-Hee; Yi, Seung-Muk; Zoh, Kyung-Duk
2015-09-01
This study was carried out to identify possible sources and to estimate their contribution to total suspended particle (TSP) organic aerosol (OA) contents. A total of 120 TSP and PM2.5 samples were collected simultaneously every third day over a one-year period in urban area of Incheon, Korea. High concentration in particulate matters (PM) and its components (NO3(-), water soluble organic compounds (WSOCs), and n-alkanoic acids) were observed during the winter season. Among the organics, n-alkanes, n-alkanoic acids, levoglucosan, and phthalates were major components. Positive matrix factorization (PMF) analysis identified seven sources of organic aerosols including combustion 1 (low molecular weight (LMW)-polycyclic aromatic hydrocarbons (PAHs)), combustion 2 (high molecular weight (HMW)-PAHs), biomass burning, vegetative detritus (n-alkane), secondary organic aerosol 1 (SOA1), secondary organic aerosol 2 (SOA2), and motor vehicles. Vegetative detritus increased during the summer season through an increase in biogenic/photochemical activity, while most of the organic sources were prominent in the winter season due to the increases in air pollutant emissions and atmospheric stability. The correlation factors were high among the main components of the organic carbon (OC) in the TSP and PM2.5. The results showed that TSP OAs had very similar characteristics to the PM2.5 OAs. SOA, combustion (PAHs), and motor vehicle were found to be important sources of carbonaceous PM in this region. Our results imply that molecular markers (MMs)-PMF model can provide useful information on the source and characteristics of PM. Copyright © 2015 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Chen, Huizhong; Wu, Dui; Yu, Jianzhen
2016-04-01
Using the data on aerosol observed hourly by Marga ADI 2080 and Grimm 180, we compared the characteristics of aerosol during rainy weather and cold air-dust weather in Guangzhou in late March 2012. The mass concentration of aerosol appeared distinct between the two weather processes. During rainy weather, the mass concentration of PM and total water-soluble components decreased obviously. During cold air-dust weather, the cleaning effect of cold air occurred much more suddenly and about a half day earlier than the dust effect. As a result, the mass concentration of PM and total water-soluble components first dropped dramatically to a below-normal level and then rose gradually to an above-normal level. The ratio of PM2.5/PM10 and PM1/PM10 decreased, suggesting that dust-storm weather mainly brought in coarse particles. The proportion of Ca2+ in the total water-soluble components significantly increased to as high as 50 % because of the effect of dust weather. We further analysed the ionic equilibrium during rainy and cold air-dust weather, and compared it with that during hazy weather during the same period. The aerosol during rainy weather was slightly acidic, whereas that during hazy weather and cold air-dust weather was obviously alkaline, with that during cold air-dust weather being significantly more alkaline. Most of the anions, including SO4 2- and NO3 -, were neutralised by NH4 + during rainy and hazy weather, and by Ca2+ during cold air-dust weather.
The response of thunderstorms and lightning to smoke from Amazonian fires
NASA Astrophysics Data System (ADS)
Altaratz, Orit; Koren, Ilan; Yair, Yoav; Price, Colin
2010-05-01
The effects of man-made aerosols on clouds are long believed to be a key component for model predictions of climate change, yet are one of the least understood. High aerosol concentrations can change the convection intensity and hence the electrical activity of thunderclouds. Focusing on the Amazon dry season in Brazil, where thousands of man-made forest fires inject smoke into the atmosphere, we studied the aerosol effects on thunderclouds and lightning. We used the ground-based World-Wide Lightning Location Network (WWLLN) measurements together with Aqua-MODIS remotely-sensed aerosol and cloud data to study the relationship between aerosol loading and lightning flash occurrence. We present evidence for the transition between two regimes, representing opposing effects of aerosols on clouds. The first is the microphysical effect which is manifested in an increase in convective intensity (and therefore in electrical activity), followed by the radiative effect that becomes dominant with the increase in aerosol loading leading to a decrease in convective intensity, manifested in lower lightning activity.
NASA Technical Reports Server (NTRS)
Penner, Joyce E.
1998-01-01
The indirect effect of anthropogenic aerosols, wherein aerosol particles are thought to increase cloud droplet concentrations and cloud lifetime, is the most uncertain component of climate forcing over the past 100 years. Here, for the first time, we use a mechanistic treatment of droplet nucleation and a prognostic treatment of the number of cloud droplets to study the indirect aerosol effect from changes in carbonaceous and sulfate aerosols. Cloud droplet nucleation is parameterized as a function of total aerosol number concentration, updraft velocity and a shape parameter, which takes into account the mechanism, of sulfate aerosol formation, while cloud droplet number depends on the nucleation as well as on droplet sinks. Whereas previous treatments have predicted annual average indirect effects between -1 and -2 W/sq m, we obtain an indirect aerosol effect between -0.14 W/sq m and -0.42 W/sq m in the global mean.
NASA Astrophysics Data System (ADS)
Obata, Kotaro; Schonewille, Adam; Slobin, Shayna; Hohnholz, Arndt; Unger, Claudia; Koch, Jürgen; Suttmann, Oliver; Overmeyer, Ludger
2017-09-01
The hybrid technique of aerosol jet printing and ultraviolet (UV) laser direct writing was developed for 2D patterning of thin film UV curable polydimethylsiloxane (PDMS). A dual atomizer module in an aerosol jet printing system generated aerosol jet streams from material components of the UV curable PDMS individually and enables the mixing in a controlled ratio. Precise control of the aerosol jet printing achieved the layer thickness of UV curable PDMS as thin as 1.6 μm. This aerosol jet printing system is advantageous because of its ability to print uniform thin-film coatings of UV curable PDMS on planar surfaces as well as free-form surfaces without the use of solvents. In addition, the hybrid 2D patterning using the combination of UV laser direct writing and aerosol jet printing achieved selective photo-initiated polymerization of the UV curable PDMS layer with an X-Y resolution of 17.5 μm.
Regional aerosol chemistry of the Amazon Basin during the dry season
NASA Technical Reports Server (NTRS)
Talbot, R. W.; Harriss, R. C.; Andreae, M. O.; Andreae, T. W.
1988-01-01
The distribution and chemical composition of the atmospheric aerosol over the Amazon Basin forest were determined during the 1985 July-August dry season, using data on the aerosol chemical constituent concentration collected during the NASA Global Tropospheric Experiment Amazon Boundary Layer Experiment 2A mission. The results of the analyses suggest that there is a remarkable compositional and spatial homogeneity of the atmospheric aerosol on an extensive regional scale. Particulate organic carbon is the dominant component of the atmospheric aerosol, exhibiting an average concentration of about 740 nmol/cu m in the mixed layer and about 220 nmol/cu m in free tropospheric air. Oxalate and SO4(2-) exhibited the greatest enrichment in the mixed layer, while Cl(-) showed essentially no enrichment. The aerosol in the Amazonian atmosphere is essentially acid-base neutral, primarily as a result of incorporation of NH(+), which is presumably derived from NH3 released by the forest ecosystem.
Marine CCN Activation: A Battle Between Primary and Secondary Sources
NASA Astrophysics Data System (ADS)
Fossum, K. N.; Ovadnevaite, J.; Ceburnis, D.; Preissler, J.; O'Dowd, C. D. D.
2017-12-01
Low-altitude marine clouds are cooling components of the Earth's radiative budget, and the direct measurements of the properties of these cloud forming particles, called cloud condensation nuclei (CCN), helps modellers reconstruct aerosol-to-cloud droplet processes, improving climate predictions. In this study, CCN are directly measured (CCNC commercially available from Droplet Measurement Technologies, Inc.), resolving activation efficiency at varying supersaturated conditions. Previous studies show that sub-micron sea salt particulates activate competitively, reducing the cloud peak supersaturation and inhibiting the activation of sulphate particulates into cloud droplets, making chemical composition an important component in determining cloud droplet number concentration (CDNC). This effect and the sea salt numbers needed to induce it have not been previously studied long-term in the natural environment. As part of this work, data was analysed from a two month marine research ship campaign during the Antarctic Austral summer, in 2015. Ambient aerosol in the Scotia Sea region was sampled continuously, and through the use of multiple aerosol in-situ instruments, this study shows that CCN number in both the open ocean and ice-pack influenced air masses are largely proportionate to secondary aerosol. However, open ocean air masses show a significant primary aerosol influence which changes the aerosol characteristics. Higher sea salt mass concentrations in the open ocean lead to better CCN activation efficiencies. Coupled with high wind speeds and sea surface turbulence, open ocean air masses show a repression of the CDNC number compared with the theoretical values that should be expected with the sub-cloud aerosol number concentration. This is not seen in the ice-pack air masses. Work is ongoing, looking into a long-term North Atlantic marine aerosol data set, but it would appear that chemical composition plays a large role in aerosol to cloud droplet processes, and can initially restrict CDNC when sea salt is abundant and updraft velocities are relatively low.
NASA Technical Reports Server (NTRS)
Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey
2012-01-01
During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote sensing and climate research studies in dynamic aerosol-rich environments like Dongsha.
Kahn, Ralph A; Berkoff, Tim A; Brock, Charles; Chen, Gao; Ferrare, Richard A; Ghan, Steven; Hansico, Thomas F; Hegg, Dean A; Martins, J Vanderlei; McNaughton, Cameron S; Murphy, Daniel M; Ogren, John A; Penner, Joyce E; Pilewskie, Peter; Seinfeld, John H; Worsnop, Douglas R
2017-10-01
A modest operational program of systematic aircraft measurements can resolve key satellite-aerosol-data-record limitations. Satellite observations provide frequent, global aerosol-amount maps, but offer only loose aerosol property constraints needed for climate and air quality applications. We define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ . The flight program could characterize major aerosol air-mass types statistically, at a level-of-detail unobtainable from space. It would: (1) enhance satellite aerosol retrieval products with better climatology assumptions, and (2) improve translation between satellite-retrieved optical properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space, improve aerosol constraints on climate modeling , help interrelate remote-sensing, in situ, and modeling aerosol-type definitions , and contribute to future satellite aerosol missions. Fifteen Required Variables are identified, and four Payload Options of increasing ambition are defined, to constrain these quantities. "Option C" could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration, and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable , even if aerosol loading varies.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Li, Zhanqing; Lau, W. K. -M.; Ramanathan, V.
Asian monsoons and aerosols have been studied extensively which are intertwined in influencing the climate of Asia. This paper provides a comprehensive review of ample studies on Asian aerosol, monsoon and their interactions. The region is the primary source of aerosol emissions of varies species, influenced by distinct weather and climatic regimes. On continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulation. Themore » atmospheric thermodynamic state may also be altered by the aerosol serving as cloud condensation nuclei or ice nuclei. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of numerous monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcings of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.« less
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.
NASA Astrophysics Data System (ADS)
Cornell, Sarah
2015-04-01
It is time to collate a global community database of atmospheric water-soluble organic nitrogen deposition. Organic nitrogen (ON) has long been known to be globally ubiquitous in atmospheric aerosol and precipitation, with implications for air and water quality, climate, biogeochemical cycles, ecosystems and human health. The number of studies of atmospheric ON deposition has increased steadily in recent years, but to date there is no accessible global dataset, for either bulk ON or its major components. Improved qualitative and quantitative understanding of the organic nitrogen component is needed to complement the well-established knowledge base pertaining to other components of atmospheric deposition (cf. Vet et al 2014). Without this basic information, we are increasingly constrained in addressing the current dynamics and potential interactions of atmospheric chemistry, climate and ecosystem change. To see the full picture we need global data synthesis, more targeted data gathering, and models that let us explore questions about the natural and anthropogenic dynamics of atmospheric ON. Collectively, our research community already has a substantial amount of atmospheric ON data. Published reports extend back over a century and now have near-global coverage. However, datasets available from the literature are very piecemeal and too often lack crucially important information that would enable aggregation or re-use. I am initiating an open collaborative process to construct a community database, so we can begin to systematically synthesize these datasets (generally from individual studies at a local and temporally limited scale) to increase their scientific usability and statistical power for studies of global change and anthropogenic perturbation. In drawing together our disparate knowledge, we must address various challenges and concerns, not least about the comparability of analysis and sampling methodologies, and the known complexity of composition of ON. We need to discuss and develop protocols that work for diverse research needs. The database will need to be harmonized or merged into existing global N data initiatives. This presentation therefore launches a standing invitation for experts to contribute and share rain and aerosol ON and chemical composition data, and jointly refine the preliminary database structure and metadata requirements for optimal mutual use. Reference: Vet et al. (2014) A global assessment of precipitation chemistry… Atmos Environ 93: 3-100
Fast and Slow Responses of the South Asian Monsoon System to Anthropogenic Aerosols
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ganguly, Dilip; Rasch, Philip J.; Wang, Hailong
2012-09-25
Using a global climate model with fully predictive aerosol life cycle, we investigate the fast and slow responses of the South Asian monsoon system to anthropogenic aerosol forcing. Our results show that the feedbacks associated with sea surface temperature (SST) change caused by aerosols play a more important role than the aerosol's direct impact on radiation, clouds and land surface (rapid adjustments) in shaping the total equilibrium climate response of the monsoon system to aerosol forcing. Inhomogeneous SST cooling caused by anthropogenic aerosols eventually reduces the meridional tropospheric temperature gradient and the easterly shear of zonal winds over the region,more » slowing down the local Hadley cell circulation, decreasing the northward moisture transport, and causing a reduction in precipitation over South Asia. Although total responses in precipitation are closer to the slow responses in general, the fast component dominates over land areas north of 25°N. Our results also show an east-west asymmetry in the fast responses to anthropogenic aerosols causing increases in precipitation west of 80°E but decreases east of it.« less
Rainfall-aerosol relationships explained by wet scavenging and humidity
NASA Astrophysics Data System (ADS)
Grandey, Benjamin S.; Gururaj, Anisha; Stier, Philip; Wagner, Till M.
2014-08-01
Relationships between precipitation rate and aerosol optical depth, the extinction of light by aerosol in an atmospheric column, have been observed in satellite-retrieved data. What are the reasons for these precipitation-aerosol relationships? We investigate relationships between convective precipitation rate (Rconv) and aerosol optical depth (τtot) using the ECHAM5-HAM aerosol-climate model. We show that negative Rconv-τtot relationships arise due to wet scavenging of aerosol. The apparent lack of negative Rconv-τtot relationships in satellite-retrieved data is likely because the satellite data do not sample wet scavenging events. When convective wet scavenging is excluded in the model, we find positive Rconv-τtot relationships in regions where convective precipitation is the dominant form of model precipitation. The spatial distribution of these relationships is in good agreement with satellite-based results. We further demonstrate that a substantial component of these positive relationships arises due to covariation with large-scale relative humidity. Although the interpretation of precipitation-aerosol relationships remains a challenging question, we suggest that progress can be made through a synergy between observations and models.
Land, P E; Haigh, J D
1997-12-20
In algorithms for the atmospheric correction of visible and near-IR satellite observations of the Earth's surface, it is generally assumed that the spectral variation of aerosol optical depth is characterized by an Angström power law or similar dependence. In an iterative fitting algorithm for atmospheric correction of ocean color imagery over case 2 waters, this assumption leads to an inability to retrieve the aerosol type and to the attribution to aerosol spectral variations of spectral effects actually caused by the water contents. An improvement to this algorithm is described in which the spectral variation of optical depth is calculated as a function of aerosol type and relative humidity, and an attempt is made to retrieve the relative humidity in addition to aerosol type. The aerosol is treated as a mixture of aerosol components (e.g., soot), rather than of aerosol types (e.g., urban). We demonstrate the improvement over the previous method by using simulated case 1 and case 2 sea-viewing wide field-of-view sensor data, although the retrieval of relative humidity was not successful.
NASA Astrophysics Data System (ADS)
Kim, P. S.; Jacob, D. J.; Fisher, J. A.; Travis, K.; Yu, K.; Zhu, L.; Yantosca, R. M.; Sulprizio, M. P.; Jimenez, J. L.; Campuzano-Jost, P.; Froyd, K. D.; Liao, J.; Hair, J. W.; Fenn, M. A.; Butler, C. F.; Wagner, N. L.; Gordon, T. D.; Welti, A.; Wennberg, P. O.; Crounse, J. D.; St. Clair, J. M.; Teng, A. P.; Millet, D. B.; Schwarz, J. P.; Markovic, M. Z.; Perring, A. E.
2015-07-01
We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the Southeast US during the summer-fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 km × 25 km resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the Southeast US. GEOS-Chem simulation of sulfate requires a missing oxidant, taken here to be stabilized Criegee intermediates, but which could alternatively reflect an unaccounted for heterogeneous process. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 20 % in the cloud convective layer at 1.5-3 km, and 20 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42-] + [NO3-])) is only 0.5-0.7 mol mol-1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by organic aerosol. This would explain the long-term decline of ammonium aerosol in the Southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the Southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the Southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 21 %. The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD due to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are fundamentally consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.
Aerosol Activation Properties within and above Mixing Layer in the North China Plain
NASA Astrophysics Data System (ADS)
Deng, Z.; Ran, L.
2013-12-01
Aerosol particles, serving as cloud condensation nuclei (CCN), may modify the properties of clouds and have an impact on climate. The vertical distribution of aerosols and their activation properties is critical to quantify the effect of aerosols on clouds. An intensive field campaign, Vertical Observations of trace Gases and Aerosols in the North China Plain (VOGA-NCP 2013), was conducted in the North China Plain during the late July and early August 2013 to measure the vertical profiles of atmospheric components in this polluted region and estimate their effects on atmospheric environment and climate. Aerosols were measured with in-situ instruments and Lidar. Particularly, the aerosols were collected at 1000 m height with a 1 m3 bag sampler attached to a tethered balloon, and subsequently measured with combined scanning mobility particle sizer (SMPS) and CCN counter. Comparisons of size-resolved activation ratios at ground level and 1000 m height showed that aerosols in upper atmosphere were not only less concentrated, but also less CCN-active than those at the surface. The difference in aerosol properties between upper atmosphere and the ground indicates that the analysis of impacts of aerosols on cloud might be misleading in heavily polluted region based on the relationship of cloud properties and surface aerosols or column without considering the vertical distribution of aerosol activation abilities.
Simulation of Asia Dust and Cloud Interaction Over Pacific Ocean During Pacdex
NASA Astrophysics Data System (ADS)
Long, X.; Huang, J.; Cheng, C.; Wang, W.
2007-12-01
The effect of dust plume on the Pacific cloud systems and the associated radiative forcing is an outstanding problem for understanding climate change. Many studies showing that dust aerosol might be a good absorber for solar radiation, at the same time dust aerosols could affect the cloud's formation and precipitation by its capability as cloud condensation nuclei (CCN) and ice forming nuclei (IFN). But the role of aerosols in clouds and precipitation is very complex. Simulation of interaction between cloud and dust aerosols requires recognition that the aerosol cloud system comprises coupled components of dynamics, aerosol and cloud microphysics, radiation processes. In this study, we investigated the interaction between dust aerosols and cloud with WRF which coupled with detailed cloud microphysics processes and dust process. The observed data of SACOL (Semi-Arid Climate and Environment Observatory of Lanzhou University) and PACDEX (Pacific Dust Experiment) is used as the initialization which include the vertical distributions and concentration of dust particles. Our results show that dust aerosol not only impacts cloud microphysical processes but also cloud microstructure; Dust aerosols can act as effective ice nuclei and intensify the ice-forming processes.
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.
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.
NASA Astrophysics Data System (ADS)
Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R. M.; Tardivo, R.; Scarnato, B.; Gianelle, V.
2007-01-01
A physicochemical characterization of the urban fine aerosol (aerosol number size distribution, chemical composition and mass concentrations) in Milan, Barcelona and London is presented in this article. The objective is to obtain a comprehensive picture on the involvement of the microphysical processes of the aerosol dynamic in the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of particles >100 nm (which only accounts for <20% of the total number concentration N of fine aerosols) and do not correlate with the number of particles <100 nm ("ultrafine particles", which accounts for >80% of fine particles). Organic matter (OM) and black-carbon (BC) are the only aerosol components showing a significant correlation with ultrafine particles (attributed to vehicles emissions), whereas ammonium-nitrate, ammonium-sulphate and also OM and BC correlate with N>100(nm) (attributed to gas-to-particle transformation mechanisms and some primary emissions). Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100(nm) concentrations, exhibit correlated day-to-day variations which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the fact that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow enough to produce significant concentrations of N>100(nm). In contrast, because the low contribution of ultrafine particles to the fine aerosol mass concentrations, high "ultrafine particles N<100(nm) events" frequently occurs under low PM2.5 conditions. The data of this study point that vehicles emissions are strongly involved in this ultrafine particles aerosol pollution (for example, the "morning-rush-hours to nocturnal-background" concentrations ratio is 1.5-2.5 for "particles 10-100 nm" and <1.5 for both "particle >100 nm and PM2.5").
NASA Astrophysics Data System (ADS)
Rodríguez, S.; van Dingenen, R.; Putaud, J.-P.; Dell'Acqua, A.; Pey, J.; Querol, X.; Alastuey, A.; Chenery, S.; Ho, K.-F.; Harrison, R.; Tardivo, R.; Scarnato, B.; Gemelli, V.
2007-05-01
A physicochemical characterization, including aerosol number size distribution, chemical composition and mass concentrations, of the urban fine aerosol captured in MILAN, BARCELONA and LONDON is presented in this article. The objective is to obtain a comprehensive picture of the microphysical processes involved in aerosol dynamics during the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) the link between "aerosol chemistry and mass concentrations" with the "number size distribution". The mass concentrations of the fine PM2.5 aerosol exhibit a high correlation with the number concentration of >100 nm particles N>100 (nm) ("accumulation mode particles") which only account for <20% of the total number concentration N of fine aerosols; but do not correlate with the number of <100 nm particles ("ultrafine particles"), which accounts for >80% of fine particles number concentration. Organic matter and black-carbon are the only aerosol components showing a significant correlation with the ultrafine particles, attributed to vehicles exhausts emissions; whereas ammonium-nitrate, ammonium-sulphate and also organic matter and black-carbon correlate with N>100 (nm) and attributed to condensation mechanisms, other particle growth processes and some primary emissions. Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM2.5 concentrations and number N>100 (nm) concentrations exhibit correlated day-to-day variations, which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the observation that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow large enough to produce significant number concentrations of N>100 (nm) ("accumulation mode particles"). In contrast, because the low contribution of ultrafine particles to the fine aerosol mass concentrations, high "ultrafine particles N<100(nm) events" frequently occurs under low PM2.5 conditions. The results of this study demonstrate that vehicles exhausts emissions are strongly involved in this ultrafine particles aerosol pollution.
Carbonaceous aerosol over a Pinus taeda forest in Central North Carolina, USA
Organic aerosol is the least understood component of ambient fine particulate matter (PM2.5). Presented in this study are organic and elemental carbon (OC and EC) within ambient PM2.5 over a three-year period at a forested site in the North Carolina Piedmon. EC exhibited signifi...
Biomass burning and its effects on fine aerosol acidity, water content and nitrogen partitioning
NASA Astrophysics Data System (ADS)
Bougiatioti, Aikaterini; Nenes, Athanasios; Paraskevopoulou, Despina; Fourtziou, Luciana; Stavroulas, Iasonas; Liakakou, Eleni; Myriokefalitakis, Stelios; Daskalakis, Nikos; Weber, Rodney; Kanakidou, Maria; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos
2017-04-01
Aerosol acidity is an important property that drives the partitioning of semi-volatile species, the formation of secondary particulate matter and metal and nutrient solubility. Aerosol acidity varies considerably between aerosol types, RH, temperature, the degree of atmospheric chemical aging and may also change during transport. Among aerosol different sources, sea salt and dust have been well studied and their impact on aerosol acidity and water uptake is more or less understood. Biomass burning (BB) on the other hand, despite its significance as a source in a regional and global scale, is much less understood. Currently, there is no practical and accurate enough method, to directly measure the pH of in-situ aerosol. The combination of thermodynamic models, with targeted experimental observations can provide reliable predictions of aerosol particle water and pH, using as input the concentration of gas/aerosol species, temperature (T), and relative humidity (RH). As such an example, ISORROPIA-II (Fountoukis and Nenes, 2007) has been used for the thermodynamic analysis of measurements conducted in downtown Athens during winter 2013, in order to evaluate the effect of BB on aerosol water and acidity. Biomass burning, especially during night time, was found to contribute significantly to the increased organics concentrations, but as well to the BC component associated with wood burning, particulate nitrates, chloride, and potassium. These increased concentrations were found to impact on fine aerosol water, with Winorg having an average concentration of 11±14 μg m-3 and Worg 12±19 μg m-3 with the organic component constituting almost 38% of the total calculated submicron water. When investigating the fine aerosol acidity it was derived that aerosol was generally acidic, with average pH during strong BB influence of 2.8±0.5, value similar to the pH observed for regional aerosol influenced by important biomass burning episodes at the remote background site of Finokalia, Crete. During cleaner days submicron aerosol was found to be more acidic, regardless of the season (winter or summer). This reduced acidity is attributed to the presence of non-volatile cations, such as non-sea salt potassium and the significant excess of ammonium compared to sulfates. The lower pH values leads to the partitioning of the majority of nitrate and chloride to the aerosol phase, which can explain the good correlation found in biomass burning influenced environments between BB tracers and both these species. Finally, we show that these acidity effects of biomass burning can be also seen in regional and global scales, which can have important implications for public health, climate and ecosystems.
Aerosol penetration through respirator exhalation valves.
Bellin, P; Hinds, W C
1990-10-01
Exhalation valves are a critical component of industrial respirators. They are designed to permit minimal inward leakage of air contaminants during inhalation and provide low resistance during exhalation. Under normal conditions, penetration of aerosol through exhalation valves is minimal. The exhalation valve is, however, a vulnerable component of a respirator and under actual working conditions may become dirty or damaged to the point of causing significant leakage. Aerosol penetration was measured for normal exhalation valves and valves compromised by paint or fine copper wires on the valve seat. Penetration increased with increasing wire diameter. A wire 250 microns in diameter allowed greater than 1% penetration into the mask cavity. Dirt or paint accumulated on the exhalation valve allowed a similar level of penetration. Work rate had little effect on observed penetration. Penetration decreased significantly with increasing aerosol particle size. The amount of material on the valve or valve seat necessary for significant (greater than 0.5%) inward leakage in a half-mask respirator could be readily observed by careful inspection of the exhalation valve and its seat in good lighting conditions.
NASA Astrophysics Data System (ADS)
Hou, W. Z.; Li, Z. Q.; Zheng, F. X.; Qie, L. L.
2018-04-01
This paper evaluates the information content for the retrieval of key aerosol microphysical and surface properties for multispectral single-viewing satellite polarimetric measurements cantered at 410, 443, 555, 670, 865, 1610 and 2250 nm over bright land. To conduct the information content analysis, the synthetic data are simulated by the Unified Linearized Vector Radiative Transfer Model (UNLVTM) with the intensity and polarization together over bare soil surface for various scenarios. Following the optimal estimation theory, a principal component analysis method is employed to reconstruct the multispectral surface reflectance from 410 nm to 2250 nm, and then integrated with a linear one-parametric BPDF model to represent the contribution of polarized surface reflectance, thus further to decouple the surface-atmosphere contribution from the TOA measurements. Focusing on two different aerosol models with the aerosol optical depth equal to 0.8 at 550 nm, the total DFS and DFS component of each retrieval aerosol and surface parameter are analysed. The DFS results show that the key aerosol microphysical properties, such as the fine- and coarse-mode columnar volume concentration, the effective radius and the real part of complex refractive index at 550 nm, could be well retrieved with the surface parameters simultaneously over bare soil surface type. The findings of this study can provide the guidance to the inversion algorithm development over bright surface land by taking full use of the single-viewing satellite polarimetric measurements.
Influence of the Surf Zone on the Marine Aerosol Concentration in a Coastal Area
NASA Astrophysics Data System (ADS)
Tedeschi, Gilles; van Eijk, Alexander M. J.; Piazzola, Jacques; Kusmierczyk-Michulec, Jolanta T.
2017-01-01
Sea-salt aerosol concentrations in the coastal zone are assessed with the numerical aerosol-transport model MACMod that applies separate aerosol source functions for open ocean and the surf zone near the sea-land transition. Numerical simulations of the aerosol concentration as a function of offshore distance from the surf zone compare favourably with experimental data obtained during a surf-zone aerosol experiment in Duck, North Carolina in autumn 2007. Based on numerical simulations, the effect of variations in aerosol production (source strength) and transport conditions (wind speed, air-sea temperature difference), we show that the surf-zone aerosols are replaced by aerosols generated over the open ocean as the airmass advects out to sea. The contribution from the surf-generated aerosol is significant during high wind speeds and high wave events, and is significant up to 30 km away from the production zone. At low wind speeds, the oceanic component dominates, except within 1-5 km of the surf zone. Similar results are obtained for onshore flow, where no further sea-salt aerosol production occurs as the airmass advects out over land. The oceanic aerosols that are well-mixed throughout the boundary layer are then more efficiently transported inland than are the surf-generated aerosols, which are confined to the first few tens of metres above the surface, and are therefore also more susceptible to the type of surface (trees or grass) that determines the deposition velocity.
Constraining the instantaneous aerosol influence on cloud albedo
Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine; ...
2017-04-26
Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol andmore » cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. Furthermore, the accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less
Constraining the instantaneous aerosol influence on cloud albedo
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine
Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration ( N d), previous studies have used the sensitivity of the N d to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol andmore » cloud properties in the present-day climate may not be suitable for determining the sensitivity of the N d to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between N d and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. Furthermore, the accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less
Constraining the instantaneous aerosol influence on cloud albedo
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gryspeerdt, Edward; Quaas, Johannes; Ferrachat, Sylvaine
2017-04-26
Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration (Nd), previous studies have used the sensitivity of the Nd to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties inmore » the present-day climate may not be suitable for determining the sensitivity of the Nd to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between Nd and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.« less
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 turbulent dispersion as a function of distance from the highway, and a traffic camera was used to determine traffic density, composition and speed. These measurements differ from previous studies in that turbulence is measured under realistic conditions and hence the relationship of the aerosol evolution to atmospheric stability and mixing will also be quantified. Preliminary results suggest that aerosol size and composition does change on the sub-grid scale, and sub-grid scale parameterizations of turbulence and particle chemistry should be included in models to accurately represent these effects.
Aerosols increase upper tropospheric humidity over the North Western Pacific
NASA Astrophysics Data System (ADS)
Riuttanen, Laura; Bister, Marja; John, Viju; Sundström, Anu-Maija; Dal Maso, Miikka; Räisänen, Jouni; de Leeuw, Gerrit; Kulmala, Markku
2014-05-01
Water vapour in the upper troposphere is highly important for the global radiative transfer. The source of upper tropospheric humidity is deep convection, and aerosol effects on them have got attention only recently. E.g., aerosol effects on deep convective clouds have been missing in general circulation models (Quaas et al., 2009). In deep convection, aerosol effect on cloud microphysics may lead to more ice precipitation and less warm rain (Khain et al., 2005), and thus more water vapour in upper troposphere (Bister & Kulmala, 2011). China outflow region over the Pacific Ocean was chosen as a region for a more detailed study, with latitudes 25-45 N and three longitude slots: 120-149 E, 150-179 E and 150-179 W. In this study, we used satellite measurements of aerosol optical depth (AOD) and upper tropospheric humidity (UTH). AOD was obtained from the MODIS instrument onboard Terra satellite, that crosses the equator southward at 10:30 AM local solar time (Remer et al., 2005). UTH was obtained from a microwave humidity sounder (MHS) onboard MetOp-A satellite, with passing time at 9:30 PM local solar time. It measures relative humidity of a layer extending approximately from 500 to 200 hPa. We binned the AOD and UTH data according to daily rainfall product 3B42 from Tropical Rainfall Measuring Mission (TRMM) satellite. Binning the data according to the amount of precipitation gives us a new way to account for the possible aerosol invigoration effect on convection and to alleviate the contamination and causality problems in aerosol indirect effect studies. In this study, we show for the first time, based on satellite data, that there is a connection between upper tropospheric humidity and aerosols. Anthropogenic aerosols from China increase upper tropospheric humidity, which causes a significant positive local radiative forcing in libRadtran radiative transfer model (Mayer & Kylling, 2005). References: Bister, M. & Kulmala, M. (2011). Atmos. Chem. Phys., 11, 4577-4586. Khain, A., Rosenfeld, D. & Pokrovsky, A. (2005). Q. J. R. Meteorol. Soc., 131, 2639-2663. Mayer, B. & Kylling, A. (2005). Atmos. Chem. Phys., 5, 1855-1877. Remer, L. A. et al. (2005). J. Atmos. Sci., 62, 947-973. Quaas, J. et al. (2009). Atmos. Chem. Phys., 9, 8697-8717.
NASA Astrophysics Data System (ADS)
Twigg, M. M.; Di Marco, C. F.; Leeson, S.; van Dijk, N.; Jones, M. R.; Leith, I. D.; Morrison, E.; Coyle, M.; Proost, R.; Peeters, A. N. M.; Lemon, E.; Frelink, T.; Braban, C. F.; Nemitz, E.; Cape, J. N.
2015-07-01
There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements which can provide further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows for the characterisation of the inorganic components of PM10 and PM2.5 (NH4+, NO3-, SO42-, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP supersite, Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 μg m-3. Anthropogenically derived secondary inorganic aerosols (sum of NH4+, NO3- and nss-SO42-) were the dominating species (63 %) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt was the main component (73 %) of the PMcoarse fraction (PM10-PM2.5), though NO3- was also found to make a relatively large contribution to the measured mass (17 %) providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high K+ concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations > 12 μg m-3) were on average dominated by NH4+ and NO3-, where smaller loadings at the site tended to be dominated by sea salt. As with other western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely that organic acids contributed to the charge balance. This study demonstrates the UK background atmospheric composition is primarily driven by meteorology with sea salt dominating air masses from the Atlantic Ocean and the Arctic, whereas secondary inorganic aerosols tended to dominate air masses from continental Europe.
NASA Astrophysics Data System (ADS)
Huang, X.-F.; He, L.-Y.; Hu, M.; Canagaratna, M. R.; Sun, Y.; Zhang, Q.; Zhu, T.; Xue, L.; Zeng, L.-W.; Liu, X.-G.; Zhang, Y.-H.; Jayne, J. T.; Ng, N. L.; Worsnop, D. R.
2010-09-01
As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m-3; the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA and COA species, probably due to stronger influences from local emissions. The lowest concentration levels for all major species were obtained during the Olympic game days (8 to 24 August 2008), possibly due to the effects of both strict emission controls and favorable meteorological conditions.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Flores, J. M.; Washenfelder, Rebecca; Adler, Gabriela
2014-05-14
Atmospheric absorption by brown carbon aerosol may play an important role in global radiative forcing. Brown carbon arises from both primary and secondary sources, but the mechanisms and reactions for the latter are highly uncertain. One proposed mechanism is the reaction of ammonia or amino acids with carbonyl products in secondary organic aerosol (SOA). We generated SOA in situ by reacting biogenic alkenes (α-pinene, limonene, and α-humulene) with excess ozone, humidifying the resulting aerosol, and reacting the humidified aerosol with gaseous ammonia. We determined the complex refractive indices (RI) in the 360 – 420 nm range for these aerosols usingmore » broadband cavity enhanced spectroscopy (BBCES). The average real part (n) of the measured spectral range of the NH3-aged α-pinene SOA increased from n = 1.50 (±0.01) for the unreacted SOA to n = 1.57 (± 0.01) after a 1.5h exposure to 1.9 ppm NH3; whereas,the imaginary component (k) remained below k < 0.001 (± 0.002). For the limonene and α-humulene SOA the real part did not change significantly, and we observed a small change in the imaginary component of the RI. The imaginary component increased from k = 0.0 to an average k= 0.029 (± 0.021) for α-humulene SOA, and from k < 0.001 (± 0.002) to an average k = 0.032 (±0.019) for limonene SOA after a 1.5 h exposure to 1.3 and 1.9 ppm of NH3, respectively. Collected filter samples of the aged and unreacted α-pinene SOA and limonene SOA were analyzed off-line with nanospray desorption electrospray ionization high resolution mass spectrometry (nano-DESI/HR-MS), and in-situ with a Time-of-Fligh Aerosol Mass Spectrometer, confirming that the SOA reacted and that various nitrogen-containing reaction products formed. If we assume that NH3 aging reactions scale linearly with time and concentration, then a 1.5 h reaction with 1 ppm NH3 in the laboratory is equivalent to 24 h reaction with 63 ppbv NH3, indicating that the observed aerosol absorption will be limited to atmospheric regions with high NH3 concentrations.« less
Flores, J M; Washenfelder, R A; Adler, G; Lee, H J; Segev, L; Laskin, J; Laskin, A; Nizkorodov, S A; Brown, S S; Rudich, Y
2014-06-14
Atmospheric absorption by brown carbon aerosol may play an important role in global radiative forcing. Brown carbon arises from both primary and secondary sources, but the mechanisms and reactions of the latter are highly uncertain. One proposed mechanism is the reaction of ammonia or amino acids with carbonyl products in secondary organic aerosol (SOA). We generated SOA in situ by reacting biogenic alkenes (α-pinene, limonene, and α-humulene) with excess ozone, humidifying the resulting aerosol, and reacting the humidified aerosol with gaseous ammonia. We determined the complex refractive indices (RI) in the 360-420 nm range for these aerosols using broadband cavity enhanced spectroscopy (BBCES). The average real part (n) of the measured spectral range of the NH3-aged α-pinene SOA increased from n = 1.50 (±0.01) for the unreacted SOA to n = 1.57 (±0.01) after 1.5 h of exposure to 1.9 ppm NH3, whereas the imaginary component (k) remained below k < 0.001((+0.002)(-0.001)). For the limonene and α-humulene SOA the real part did not change significantly, and we observed a small change in the imaginary component of the RI. The imaginary component increased from k = 0.000 to an average k = 0.029 (±0.021) for α-humulene SOA, and from k < 0.001((+0.002)(-0.001)) to an average k = 0.032 (±0.019) for limonene SOA after 1.5 h of exposure to 1.3 and 1.9 ppm of NH3, respectively. Collected filter samples of the aged and unreacted α-pinene SOA and limonene SOA were analyzed off-line by nanospray desorption electrospray ionization high resolution mass spectrometry (nano-DESI/HR-MS), and in situ using a Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS), confirming that the SOA reacted and that various nitrogen-containing reaction products formed. If we assume that NH3 aging reactions scale linearly with time and concentration, which will not necessarily be the case in the atmosphere, then a 1.5 h reaction with 1 ppm NH3 in the laboratory is equivalent to 24 h reaction with 63 ppbv NH3, indicating that the observed aerosol absorption will be limited to atmospheric regions with high NH3 concentrations.
NASA Astrophysics Data System (ADS)
Espinosa, R.; Remer, L.; Puthukkudy, A.; Orozco, D.; Dubovik, O.; Martins, J. V.
2017-12-01
Models used to estimate climate change and interpret remote sensing observations must make assumptions regarding aerosol radiation interactions. This presentation will summarize aerosol light scattering measurements made by the Polarized Imaging Nephelometer (PI-Neph) during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry (DC3) experiments. The data presented includes direct measurements of phase function (P11) and polarized phase function (-P12/P11) as well as retrievals of size distribution, sphericity and complex refractive index made using the Generalized Retrieval of Aerosol and Surface Properties (GRASP). An aerosol classification scheme is developed to identify different aerosol types measured during the deployments, making use of ancillary data that includes gas tracers, chemical composition, aerodynamic particle size and geographic location. Principal component analysis (PCA) is then used to reduce the dimensionality of the multi-angle PI-Neph scattering data and a strong link between the PCA scores and the ancillary classification results is observed. The scattering differences that reliable distinguish the different aerosol types are found to be quite subtle and often rely on the relationships between many scattering angles simultaneously. This fact emphasis the value of multi-angle scattering measurements, as well as principal component analysis's ability to reveal the underlying patterns in these datasets. The parameters retrieved from the DC3 scattering data suggest the presence of a significant amount of dust in aerosols influenced by convective systems, with the quantity of dust correlating strongly with sampling location and the underlying surface features. All fine mode dominated aerosol types from SEAC4RS had remarkably similar retrieved properties, except for the real refractive index of the biomass burning cases, which was consistently elevated (n532=1.54) when compared to the other types (n532=1.50). This result suggests that climate and remote sensing models may often be able to capture the differences in optical properties between biomass burning and other fine mode aerosols by only adjusting the real refractive index of the particles.
Dust Modeling with GEOS-Chem: Evidence for Acidic Uptake on Dust Surfaces during INTEX-B
NASA Technical Reports Server (NTRS)
Fairlie, T. Duncan
2007-01-01
We use measurements of aerosol ion composition and size made from the DC8 aircraft during the 2006 INTEX-B airborne campaign to identify mineral dust signatures, and look for evidence for interaction of dust with acidic components. Coating of dust with sulfate or nitrate favors the role of dust particles as cloud condensation nucleii, can promote further uptake of SO2 and N2O5, can impact NOx/HNO3 partitioning, and can shift sulfate or nitrate towards larger sizes, affecting atmospheric lifetimes for both aerosol and gas components. Mineral dust had a pervasive presence on flights made during the Northern Pacific deployment of the INTEX-B mission. We use scatter plots of ion mixing ratios with Na+ and Ca(2+) to distinguish sea salt and mineral components of the aerosol distribution, respectively. Positive correlations of non-sea-salt sulfate and nitrate with calcium indicate that the dusty air stream is associated with polluted air masses. Sulfate-ammonium scatter plots indicate sulfate to be primarily in the form of (NH4)2SO4. A positive correlation between Ca(2+) and NO-, but little evidence of NH4NO3, suggests that NO3- may be associated with mineral dust surfaces. 3-d model simulations conducted with the GEOS-Chem chemical transport model indicate that transpacific transport from East Asia was principally responsible for the dust observed from the aircraft over the Pacific. We compare the aerosol component relationships in the model with those observed. Uptake of sulfate and nitrate on the dust is not yet represented in the model.
Volatility of organic aerosol and its components in the Megacity of Paris
NASA Astrophysics Data System (ADS)
Paciga, A.; Karnezi, E.; Kostenidou, E.; Hildebrandt, L.; Psichoudaki, M.; Engelhart, G. J.; Lee, B.-H.; Crippa, M.; Prévôt, A. S. H.; Baltensperger, U.; Pandis, S. N.
2015-08-01
Using a mass transfer model and the volatility basis set, we estimate the volatility distribution for the organic aerosol (OA) components during summer and winter in Paris, France as part of the collaborative project MEGAPOLI. The concentrations of the OA components as a function of temperature were measured combining data from a thermodenuder and an aerosol mass spectrometer (AMS) with Positive Matrix Factorization (PMF) analysis. The hydrocarbon-like organic aerosol (HOA) had similar volatility distributions for the summer and winter campaigns with half of the material in the saturation concentration bin of 10 μg m-3 and another 35-40 % consisting of low and extremely low volatility organic compounds (LVOCs and ELVOCs, respectively). The winter cooking OA (COA) was more than an order of magnitude less volatile than the summer COA. The low volatility oxygenated OA (LV-OOA) factor detected in the summer had the lowest volatility of all the derived factors and consisted almost exclusively of ELVOCs. The volatility for the semi-volatile oxygenated OA (SV-OOA) was significantly higher than that of the LV-OOA, containing both semi-volatile organic components (SVOCs) and LVOCs. The oxygenated OA (OOA) factor in winter consisted of SVOCs (45 %), LVOCs (25 %) and ELVOCs (30 %). The volatility of marine OA (MOA) was higher than that of the other factors containing around 60 % SVOCs. The biomass burning OA (BBOA) factor contained components with a wide range of volatilities with significant contributions from both SVOCs (50 %) and LVOCs (30 %). Finally, combining the O : C ratio and volatility distributions of the various factors, we incorporated our results into the two-dimensional volatility basis set (2D-VBS). Our results show that the factors cover a broad spectrum of volatilities with no direct link between the average volatility and average O : C of the OA components. Agreement between our findings and previous publications is encouraging for our understanding of the evolution of atmospheric OA.
Modelling total OH reactivity: atmospheric implications of the missing OH sink
NASA Astrophysics Data System (ADS)
Ferracci, V.; Archibald, A. T.; Heimann, I.; Pyle, J. A.
2016-12-01
The removal of the majority of reactive trace gases emitted into the atmosphere is initiated by reaction with the hydroxyl radical (OH). Over the last decade, a number of field campaigns have measured the chemical loss rate of OH, also known as total OH reactivity, in a variety of regions across the planet, from urban areas to remote forests. In most cases, comparison of the measured total OH reactivity with that calculated from the sum of the individual OH sinks (obtained via the simultaneous detection of species such as VOCs and NOx) highlighted the presence of "missing" reactivity (up to 80 % of the total measured reactivity), indicating that a significant sink of the hydroxyl radical is currently not accounted for in tropospheric oxidation schemes. Potential candidates for the missing OH reactivity are previously undetected biogenic VOCs, reactive intermediates of the oxidation of known biogenic VOCs (mainly isoprene), or a combination of the two. In this work the Met Office's Unified Model with the United Kingdom Chemistry and Aerosols scheme (UM-UKCA) was used to investigate the potential impacts of a simulated missing OH sink. UM-UKCA is a chemistry-climate model which includes detailed tropospheric chemistry derived from a combination of the JPL-NASA and IUPAC kinetic evaluations as well as the Master Chemical Mechanism database. The missing OH sink was simulated in a number of scenarios: initially, by including in the model chemical reactions that were only recently characterised (e.g., peroxy radicals + OH), then by adding a new chemical tracer, along with its reaction with OH, that would account for most of the missing reactivity observed in the various campaigns across the globe. Sensitivity of the model to the abundance and regional distribution of the new chemical tracer, and to the kinetics and hypothetical products of its reaction with OH are discussed, as well as the impacts of the missing OH sink on the tropospheric ozone budget and methane lifetime, with associated implications for air quality and global warming respectively.
Retrieval of background surface reflectance with BRD components from pre-running BRDF
NASA Astrophysics Data System (ADS)
Choi, Sungwon; Lee, Kyeong-Sang; Jin, Donghyun; Lee, Darae; Han, Kyung-Soo
2016-10-01
Many countries try to launch satellite to observe the Earth surface. As important of surface remote sensing is increased, the reflectance of surface is a core parameter of the ground climate. But observing the reflectance of surface by satellite have weakness such as temporal resolution and being affected by view or solar angles. The bidirectional effects of the surface reflectance may make many noises to the time series. These noises can lead to make errors when determining surface reflectance. To correct bidirectional error of surface reflectance, using correction model for normalized the sensor data is necessary. A Bidirectional Reflectance Distribution Function (BRDF) is making accuracy higher method to correct scattering (Isotropic scattering, Geometric scattering, Volumetric scattering). To correct bidirectional error of surface reflectance, BRDF was used in this study. To correct bidirectional error of surface reflectance, we apply Bidirectional Reflectance Distribution Function (BRDF) to retrieve surface reflectance. And we apply 2 steps for retrieving Background Surface Reflectance (BSR). The first step is retrieving Bidirectional Reflectance Distribution (BRD) coefficients. Before retrieving BSR, we did pre-running BRDF to retrieve BRD coefficients to correct scatterings (Isotropic scattering, Geometric scattering, Volumetric scattering). In pre-running BRDF, we apply BRDF with observed surface reflectance of SPOT/VEGETATION (VGT-S1) and angular data to get BRD coefficients for calculating scattering. After that, we apply BRDF again in the opposite direction with BRD coefficients and angular data to retrieve BSR as a second step. As a result, BSR has very similar reflectance to one of VGT-S1. And reflectance in BSR is shown adequate. The highest reflectance of BSR is not over 0.4μm in blue channel, 0.45μm in red channel, 0.55μm in NIR channel. And for validation we compare reflectance of clear sky pixel from SPOT/VGT status map data. As a result of comparing BSR with VGT-S1, bias is from 0.0116 to 0.0158 and RMSE is from 0.0459 to 0.0545. They are very reasonable results, so we confirm that BSR is similar to VGT-S1. And weakness of this study is missing pixel in BSR which are observed less time to retrieve BRD components. If missing pixels are filled, BSR is better to retrieve surface products with more accuracy. And we think that after filling the missing pixel and being more accurate, it can be useful data to retrieve surface product which made by surface reflectance like cloud masking and retrieving aerosol.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles
A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less
Kahn, Ralph A.; Berkoff, Tim A.; Brock, Charles; ...
2017-10-30
A modest operational program of systematic aircraft measurements can resolve key satellite aerosol data record limitations. Satellite observations provide frequent global aerosol amount maps but offer only loose aerosol property constraints needed for climate and air quality applications. In this paper, we define and illustrate the feasibility of flying an aircraft payload to measure key aerosol optical, microphysical, and chemical properties in situ. The flight program could characterize major aerosol airmass types statistically, at a level of detail unobtainable from space. It would 1) enhance satellite aerosol retrieval products with better climatology assumptions and 2) improve translation between satellite-retrieved opticalmore » properties and species-specific aerosol mass and size simulated in climate models to assess aerosol forcing, its anthropogenic components, and other environmental impacts. As such, Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM) could add value to data records representing several decades of aerosol observations from space; improve aerosol constraints on climate modeling; help interrelate remote sensing, in situ, and modeling aerosol-type definitions; and contribute to future satellite aerosol missions. Fifteen required variables are identified and four payload options of increasing ambition are defined to constrain these quantities. “Option C” could meet all the SAM-CAAM objectives with about 20 instruments, most of which have flown before, but never routinely several times per week, and never as a group. Aircraft integration and approaches to data handling, payload support, and logistical considerations for a long-term, operational mission are discussed. Finally, SAM-CAAM is feasible because, for most aerosol sources and specified seasons, particle properties tend to be repeatable, even if aerosol loading varies.« less
Post-Flight Test Results of Seed Laser Module Subjected to Space Exposure. Paper No. 8876-9
NASA Technical Reports Server (NTRS)
Prasad, Narasimha S.
2013-01-01
The objective of the Materials International Space Station Experiment (MISSE) is to study the performance of novel materials when subjected to the synergistic effects of the harsh space environment for several months. MISSE missions provide an opportunity for developing space qualifiable materials. Several laser and lidar components were sent by NASA Langley Research Center (LaRC) as a part of the MISSE 7 mission. The MISSE 7 module was transported to the international space station (ISS) via STS 129 mission that was launched on Nov 16, 2009. Later, the MISSE 7 module was brought back to the earth via the STS 134 that landed on June 1, 2011. The MISSE 7 module that was subjected to exposure in space environment for more than one and a half year included fiber laser, solid-state laser gain materials, detectors, and semiconductor laser diode. Performance testing of these components is now progressing. In this paper, the results of performance testing of a laser diode module sent by NASA Langley Research Center on MISSE 7 mission will be discussed. This paper will present the comparison of pre-flight and post-flight performance curves and discuss the effect of space exposure on the laser diode module. Preliminary findings on output power measurements show that the COTS laser diode characteristics did not undergo any significant performance degradation.
Development of a global model for atmospheric backscatter at CO2 wavelengths
NASA Technical Reports Server (NTRS)
Kent, G. S.; Wang, P. H.; Farrukh, U.; Deepak, A.; Patterson, E. M.
1986-01-01
The variation of the aerosol backscattering at 10.6 micrometers within the free troposphere was investigated and a model to describe this variation was developed. The analysis combines theoretical modeling with the results contained within three independent data sets. The data sets used were obtained by the SAGE I/SAM II satellite experiments, the GAMETAG flight series, and by direct backscatter measurements. The theoretical work includes use of a bimodal, two component aerosol model, and the study of the microphysical and associated optical changes occurring within an aerosol plume. A consistent picture is obtained that describes the variation of the aerosol backscattering function in the free troposphere with altitude, latitude, and season.
Aerosol processing in stratiform clouds in ECHAM6-HAM
NASA Astrophysics Data System (ADS)
Neubauer, David; Lohmann, Ulrike; Hoose, Corinna
2013-04-01
Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the chemical components as well as 5 tracers for aerosol particles in ice crystals. This allows simulations of aerosol processing in warm, mixed-phase (e.g. through the Bergeron-Findeisen process) and ice clouds. The fixed scavenging ratios used for wet deposition in clouds in standard HAM are replaced by an explicit treatment of collision of cloud droplets/ice crystals with interstitial aerosol particles. Nucleation scavenging of aerosol particles by acting as cloud condensation nuclei or ice nuclei, freezing and evaporation of cloud droplets and melting and sublimation of ice crystals are treated explicitly. In extension to previous studies, aerosol particles from evaporating precipitation are released to modes which correspond to their size. Cloud processing of aerosol particles changes their size distribution and hence influences cloud droplet and ice crystal number concentrations as well as precipitation rate, which in turn affects aerosol concentrations. Results will be presented at the conference. Hoose et al., JGR, 2008a, doi: 10.1029/2007JD009251 Hoose et al., ACP, 2008b, doi: 10.5194/acp-8-6939-2008 Stevens et al., 2013, submitted Stier et al., ACP, 2005, doi: 10.5194/acp-5-1125-2005
Aerosol generation and measurement of multi-wall carbon nanotubes
NASA Astrophysics Data System (ADS)
Myojo, Toshihiko; Oyabu, Takako; Nishi, Kenichiro; Kadoya, Chikara; Tanaka, Isamu; Ono-Ogasawara, Mariko; Sakae, Hirokazu; Shirai, Tadashi
2009-01-01
Mass production of some kinds of carbon nanotubes (CNT) is now imminent, but little is known about the risk associated with their exposure. It is important to assess the propensity of the CNT to release particles into air for its risk assessment. In this study, we conducted aerosolization of a multi-walled CNT (MWCNT) to assess several aerosol measuring instruments. A Palas RBG-1000 aerosol generator applied mechanical stress to the MWCNT by a rotating brush at feed rates ranging from 2 to 20 mm/h, which the MWCNT was fed to a two-component fluidized bed. The fluidized bed aerosol generator was used to disperse the MWCNT aerosol once more. We monitored the generated MWCNT aerosol concentrations based on number, area, and mass using a condensation particle counter and nanoparticle surface area monitor. Also we quantified carbon mass in MWCNT aerosol samples by a carbon monitor. The shape of aerosolized MWCNT fibers was observed by a scanning electron microscope (SEM). The MWCNT was well dispersed by our system. We found isolated MWCNT fibers in the aerosols by SEM and the count median lengths of MWCNT fibers were 4-6 μm. The MWCNT was quantified by the carbon monitor with a modified condition based on the NIOSH analytical manual. The MWCNT aerosol concentration (EC mass base) was 4 mg/m3 at 2 mm/h in this study.
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.
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.
Cai, Chen; Miles, Rachael E H; Cotterell, Michael I; Marsh, Aleksandra; Rovelli, Grazia; Rickards, Andrew M J; Zhang, Yun-Hong; Reid, Jonathan P
2016-08-25
Representing the physicochemical properties of aerosol particles of complex composition is of crucial importance for understanding and predicting aerosol thermodynamic, kinetic, and optical properties and processes and for interpreting and comparing analysis methods. Here, we consider the representations of the density and refractive index of aqueous-organic aerosol with a particular focus on the dependence of these properties on relative humidity and water content, including an examination of the properties of solution aerosol droplets existing at supersaturated solute concentrations. Using bulk phase measurements of density and refractive index for typical organic aerosol components, we provide robust approaches for the estimation of these properties for aerosol at any intermediate composition between pure water and pure solute. Approximately 70 compounds are considered, including mono-, di- and tricarboxylic acids, alcohols, diols, nitriles, sulfoxides, amides, ethers, sugars, amino acids, aminium sulfates, and polyols. We conclude that the molar refraction mixing rule should be used to predict the refractive index of the solution using a density treatment that assumes ideal mixing or, preferably, a polynomial dependence on the square root of the mass fraction of solute, depending on the solubility limit of the organic component. Although the uncertainties in the density and refractive index predictions depend on the range of subsaturated compositional data available for each compound, typical errors for estimating the solution density and refractive index are less than ±0.1% and ±0.05%, respectively. Owing to the direct connection between molar refraction and the molecular polarizability, along with the availability of group contribution models for predicting molecular polarizability for organic species, our rigorous testing of the molar refraction mixing rule provides a route to predicting refractive indices for aqueous solutions containing organic molecules of arbitrary structure.
NASA Astrophysics Data System (ADS)
Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Ridley, D. A.; Manktelow, P. T.; Chipperfield, M. P.; Pickering, S. J.; Johnson, C. E.
2010-10-01
A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.
NASA Astrophysics Data System (ADS)
Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Ridley, D. A.; Manktelow, P. T.; Chipperfield, M. P.; Pickering, S. J.; Johnson, C. E.
2010-05-01
A new version of the Global Model of Aerosol Processes (GLOMAP) is described, which uses a two-moment modal aerosol scheme rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulphate, sea-salt, dust, black carbon (BC) and particulate organic matter (POM), the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulphuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b) and correlation coefficient (R). Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN) and cloud condensation nuclei (CCN). Surface sulphate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well). Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.
NASA Astrophysics Data System (ADS)
Pavuluri, Chandra Mouli; Kawamura, Kimitaka; Swaminathan, T.
2015-02-01
To better understand the photochemical production and diurnal distributions of organic and inorganic aerosols in the tropical coastal Indian atmosphere, the aerosol (TSP) samples were collected every 3 h during 30-31 January, 14-15 February and 28-29 May 2007 from Chennai and studied for total carbon (TC) and nitrogen (TN) and their stable isotope ratios (δ13CTC and δ15NTN), carbonaceous components, inorganic ions, diacids, ketoacids and α-dicarbonyls. Time-resolved distributions of bulk parameters, inorganic ions, and diacids and related compounds, except for few species, did not show any clear diurnal trend but showed peaks at 6-9 h during all the study periods, except for the peak at 15-18 h on 28 May. SO42-, C2 - C6 diacids, ketoacids and α-dicarbonyls in February and on 29 May showed a diurnal trend. δ13CTC and δ15NTN stayed relatively constant during the study periods but showed 13C depletion (in January) and 15 N enrichment when TC and TN peaked. Based on these results together with air mass trajectories, we found that the diurnal distributions of Chennai aerosols are mainly influenced by land/sea breeze and the aged (photochemically processed) air masses, although in situ photochemical production and nighttime chemistry of secondary aerosol species, particularly C2-C4 diacids and SO42-, are significant. The characteristics of seasonal variations of carbonaceous components, and diacids and related compounds and comparisons of δ13CTC and δ15NTN of Chennai aerosols with the isotopic signatures of the point sources inferred that biofuel/biomass burning in South and Southeast Asia are the major sources of aerosols (TSP).
NASA's Future Active Remote Sensing Missing for Earth Science
NASA Technical Reports Server (NTRS)
Hartley, Jonathan B.
2000-01-01
Since the beginning of space remote sensing of the earth, there has been a natural progression widening the range of electromagnetic radiation used to sense the earth, and slowly, steadily increasing the spatial, spectral, and radiometric resolution of the measurements. There has also been a somewhat slower trend toward active measurements across the electromagnetic spectrum, motivated in part by increased resolution, but also by the ability to make new measurements. Active microwave instruments have been used to measure ocean topography, to study the land surface. and to study rainfall from space. Future NASA active microwave missions may add detail to the topographical studies, sense soil moisture, and better characterize the cryosphere. Only recently have active optical instruments been flown in space by NASA; however, there are currently several missions in development which will sense the earth with lasers and many more conceptual active optical missions which address the priorities of NASA's earth science program. Missions are under development to investigate the structure of the terrestrial vegetation canopy, to characterize the earth's ice caps, and to study clouds and aerosols. Future NASA missions may measure tropospheric vector winds and make vastly improved measurements of the chemical components of the earth's atmosphere.
NASA Technical Reports Server (NTRS)
Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.;
2011-01-01
The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops handheld sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.
NASA Astrophysics Data System (ADS)
Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.; Smyth, T. J.; Zielinski, T.; Zibordi, G.; Goes, J. I.; Harvey, M. J.; Quinn, P. K.; Nelson, N. B.; Radionov, V. F.; Duarte, C. M.; Losno, R.; Sciare, J.; Voss, K. J.; Kinne, S.; Nalli, N. R.; Joseph, E.; Krishna Moorthy, K.; Covert, D. S.; Gulev, S. K.; Milinevsky, G.; Larouche, P.; Belanger, S.; Horne, E.; Chin, M.; Remer, L. A.; Kahn, R. A.; Reid, J. S.; Schulz, M.; Heald, C. L.; Zhang, J.; Lapina, K.; Kleidman, R. G.; Griesfeller, J.; Gaitley, B. J.; Tan, Q.; Diehl, T. L.
2011-01-01
The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurements areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.
NASA Astrophysics Data System (ADS)
Smirnov, A.; Holben, B. N.; Giles, D. M.; Slutsker, I.; O'Neill, N. T.; Eck, T. F.; Macke, A.; Croot, P.; Courcoux, Y.; Sakerin, S. M.; Smyth, T. J.; Zielinski, T.; Zibordi, G.; Goes, J. I.; Harvey, M. J.; Quinn, P. K.; Nelson, N. B.; Radionov, V. F.; Duarte, C. M.; Losno, R.; Sciare, J.; Voss, K. J.; Kinne, S.; Nalli, N. R.; Joseph, E.; Krishna Moorthy, K.; Covert, D. S.; Gulev, S. K.; Milinevsky, G.; Larouche, P.; Belanger, S.; Horne, E.; Chin, M.; Remer, L. A.; Kahn, R. A.; Reid, J. S.; Schulz, M.; Heald, C. L.; Zhang, J.; Lapina, K.; Kleidman, R. G.; Griesfeller, J.; Gaitley, B. J.; Tan, Q.; Diehl, T. L.
2011-03-01
The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.
Methods used to calculate doses resulting from inhalation of Capstone depleted uranium aerosols.
Miller, Guthrie; Cheng, Yung Sung; Traub, Richard J; Little, Tom T; Guilmette, Raymond A
2009-03-01
The methods used to calculate radiological and toxicological doses to hypothetical persons inside either a U.S. Army Abrams tank or Bradley Fighting Vehicle that has been perforated by depleted uranium munitions are described. Data from time- and particle-size-resolved measurements of depleted uranium aerosol as well as particle-size-resolved measurements of aerosol solubility in lung fluids for aerosol produced in the breathing zones of the hypothetical occupants were used. The aerosol was approximated as a mixture of nine monodisperse (single particle size) components corresponding to particle size increments measured by the eight stages plus the backup filter of the cascade impactors used. A Markov Chain Monte Carlo Bayesian analysis technique was employed, which straightforwardly calculates the uncertainties in doses. Extensive quality control checking of the various computer codes used is described.
NASA Astrophysics Data System (ADS)
Ripoll, A.; Minguillón, M. C.; Pey, J.; Jimenez, J. L.; Day, D. A.; Querol, X.; Alastuey, A.
2014-11-01
Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the Western Mediterranean Basin (WMB) were conducted for 10 months (July 2011-April 2012). An Aerosol Chemical Speciation Monitor (ACSM) was co-located with other on-line and off-line PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time for this region. Seasonal trends in PM1 components are attributed to variations in: evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reserve strata at relatively high altitudes. Sporadically, MSC is affected by air masses from North Africa. The combination of all these atmospheric processes at local, regional and continental scales results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly oxygenated organic aerosol (OOA), with two different types: semi-volatile (SV-OOA) and low-volatile (LV-OOA), and both showed marked diurnal cycles regardless of the air mass origin, especially SV-OOA. This different diurnal variation compared to inorganic aerosols suggested that OA components at MSC are not only associated with anthropogenic and long-range-transported secondary OA (SOA), but also with recently-produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. Moreover, in winter sporadic long-range transport from mainland Europe is observed and leads to less marked diurnal patterns. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Additional research is needed to characterize the sources of SOA at remote sites.
NASA Technical Reports Server (NTRS)
Guo, Yanjuan; Tian, Baijun; Kahn, Ralph A.; Kalashnikova, Olga; Wong, Sun; Waliser, Duane E.
2012-01-01
In this study, MODIS fine mode fraction and MISR non-spherical fraction are 2used to derive dust and smoke AOT components (tau(sub dust) and tau(sub smoke)) over the tropical Atlantic, and their variabilities related to the Madden-Julian Oscillation (MJO) are then investigated. Both MODIS and MISR show a very similar dust and smoke winter climatology. tau(sub dust) is found to be the dominant aerosol component over the tropical Atlantic while tau(sub smoke) is significantly smaller than tau(sub dust). The daily MODIS and MISR tau(sub dust) are overall highly correlated, with the correlation coefficients typically about 0.7 over the North Atlantic. The consistency between the MODIS and MISR dust and smoke aerosol climatology and daily variations give us confidence to use these two data sets to investigate their relative contributions to the total AOT variation associated with the MJO. However, unlike the MISR dust discrimination, which is based on particle shape retrievals, the smoke discrimination is less certain, based on assumed partitioning of maritime aerosol for both MISR and MODIS. The temporal evolution and spatial patterns of the tau(sub dust) anomalies associated with the MJO are consistent between MODIS and MISR. The tau(sub dust) anomalies are very similar to those of tau anomalies, and are of comparable magnitude. In contrast, the MJO-related tau(sub smoke) anomalies are rather small, and the tau(sub mar) anomalies are negligible. The consistency between the MODIS and MISR results suggests that dust aerosol is the dominant component on the intra-seasonal time scale over the tropical Atlantic Ocean.
NASA Astrophysics Data System (ADS)
Handa, D.; Nakajima, H.; Nakaema, F.; Arakaki, T.; Tanahara, A.
2008-12-01
The economic development and population growth in recent Asia spread air pollution. Emission rate of air pollutants from Asia, in particular oxides of nitrogen, surpassed those from North America and Europe and should continue to exceed them for decades. The study of the air pollution transported from Asian continent has gained a special attention in Japan. Okinawa Island is situated approximately 1500 km south of Tokyo, Japan, 2000 km southeast of Beijing, China, and 1000 km south of South Korea. Its location is ideal in observing East Asian atmospheric aerosols because maritime air mass prevails during summer, while continental air mass dominates during fall, winter, and spring. The maritime air mass data can be seen as background and can be compared with continental air masses which have been affected by anthropogenic activities. In 2005, Cape Hedo Atmosphere and Aerosol Monitoring Station (CHAAMS) was established by the National Institute for Environmental Studies (NIES) at the northern tip of Okinawa Island, Japan to monitor the air quality of Asia. Bulk aerosol samples were collected on quartz filters by using a high volume air sampler. Sampling duration was one week for each sample. We determined the concentrations of water-soluble anions, cations and dissolved organic carbon in the bulk aerosols collected at the CHAAMS, using ion chromatography, atomic absorption spectrometry, and total organic carbon analyzer, respectively. Seasonal variation of water-soluble chemical components showed that the concentrations were relatively low in summer, higher in fall and winter, and the highest in spring. When air mass came from Asian Continent, the concentrations of water-soluble chemical components were much higher compared to the other directions.
NASA Astrophysics Data System (ADS)
Hecobian, A.; Liu, Z.; Hennigan, C. J.; Huey, L. G.; Jimenez, J. L.; Cubison, M. J.; Vay, S.; Diskin, G. S.; Sachse, G. W.; Wisthaler, A.; Mikoviny, T.; Weinheimer, A. J.; Liao, J.; Knapp, D. J.; Wennberg, P. O.; Kürten, A.; Crounse, J. D.; St. Clair, J.; Wang, Y.; Weber, R. J.
2011-12-01
This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska, USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Approximately 500 smoke plumes from biomass burning emissions that varied in age from minutes to days were segregated by fire source region and urban emission influences. The normalized excess mixing ratios (NEMR) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen and ozone) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared. A detailed statistical analysis of the different plume categories for different gaseous and aerosol species is presented in this paper. The comparison of NEMR values showed that CH4 concentrations were higher in air-masses that were influenced by urban emissions. Fresh biomass burning plumes mixed with urban emissions showed a higher degree of oxidative processing in comparison with fresh biomass burning only plumes. This was evident in higher concentrations of inorganic aerosol components such as sulfate, nitrate and ammonium, but not reflected in the organic components. Lower NOx NEMRs combined with high sulfate, nitrate and ammonium NEMRs in aerosols of plumes subject to long-range transport, when comparing all plume categories, provided evidence of advanced processing of these plumes.
Chemical, physical, and optical evolution of biomass burning aerosols: a case study
NASA Astrophysics Data System (ADS)
Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.
2011-02-01
In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.
Toon, Owen B.; Bardeen, Charles G.; Mills, Michael J.; Fan, Tianyi; English, Jason M.; Neely, Ryan R.
2015-01-01
Abstract A sectional aerosol model (CARMA) has been developed and coupled with the Community Earth System Model (CESM1). Aerosol microphysics, radiative properties, and interactions with clouds are simulated in the size‐resolving model. The model described here uses 20 particle size bins for each aerosol component including freshly nucleated sulfate particles, as well as mixed particles containing sulfate, primary organics, black carbon, dust, and sea salt. The model also includes five types of bulk secondary organic aerosols with four volatility bins. The overall cost of CESM1‐CARMA is approximately ∼2.6 times as much computer time as the standard three‐mode aerosol model in CESM1 (CESM1‐MAM3) and twice as much computer time as the seven‐mode aerosol model in CESM1 (CESM1‐MAM7) using similar gas phase chemistry codes. Aerosol spatial‐temporal distributions are simulated and compared with a large set of observations from satellites, ground‐based measurements, and airborne field campaigns. Simulated annual average aerosol optical depths are lower than MODIS/MISR satellite observations and AERONET observations by ∼32%. This difference is within the uncertainty of the satellite observations. CESM1/CARMA reproduces sulfate aerosol mass within 8%, organic aerosol mass within 20%, and black carbon aerosol mass within 50% compared with a multiyear average of the IMPROVE/EPA data over United States, but differences vary considerably at individual locations. Other data sets show similar levels of comparison with model simulations. The model suggests that in addition to sulfate, organic aerosols also significantly contribute to aerosol mass in the tropical UTLS, which is consistent with limited data. PMID:27668039
NASA Astrophysics Data System (ADS)
Simon, Károly; Ajtai, Tibor; Kiss-Albert, Gergely; Utry, Noémi; Pintér, Máté; Szabó, Gábor; Bozóki, Zoltán
2017-04-01
Aerosol source apportionment is currently one of the outstanding challenges for environmental monitoring. In most cases atmospheric aerosol is a heterogeneous mixture as it typically originates from various sources. Consequently, each aerosol type has distinct chemical and physical properties. Contrary to chemical properties, optical absorption and size distribution of airborne particles can be measured in real time with high time resolution i.e. their measurement facilitates real time source apportionment (Favez et al (2009), Ajtai et al (2011), Favez et al (2010)). The wavelength dependency of the optical absorption coefficient (OAC) is usually characterised by the Absorption Angström Exponent (AAE). So far, the selection of light sources (lasers) into a photoacoustic aerosol measuring system was based on rule of thumb type estimations only. Recently, we proposed a simulation method that can be used to estimate the accuracy of aerosol source apportionment in case of a dual wavelength photoacoustic system (Simon et al., (2017)). This simulation is based on the assumption that the atmospheric aerosol load is dominated by two distinct sources and each of them is strongly light absorbing with specific AAE values. This is a typical scenario e.g. for urban measurements under wintry conditions when dominating aerosol sources are fossil fuel and wood burning with characteristic AAE 1 and 2, respectively. The wavelength pair of 405 and 1064 nm was found to be optimal for source apportionment in this case. In the presented study we investigated the situation when there are aerosol components with only slightly different AAE values and searched for a photoacoustic system which is optimal for distinguishing these components. Ajtai, T.; Filep, Á.; Utry, N.; Schnaiter, M.; Linke, C.; Bozóki, Z.; Szabó, G. and Leisner T. (2011) Journal of Aerosol Science 42, 859-866. Favez, O.; Cachier, H.; Sciare, J.; Sarda-Estève, R. and Martinon, L. (2009) Atmospheric Environment 43, 3640-3644. Favez, O.; El Haddad, I.; Piot, C.; Boréave, A.; Abidi, E.; Marchand, N.; Jaffrezo, J. L.; Besombes, J. L.; Personnaz, M. B.; Sciare, J.; Wortham, H.; George, C. and D'Anna, B. (2010), Atmos. Chem. Phys. 10, 5295-5314. Simon, K.A.; Ajtai, T; Gulyas, G; Utry, N; Pinter, M; Szabo, G. and Bozoki, Bozoki, Z. (2017), Journal of Aerosol Science 104, 10-15.
NASA Astrophysics Data System (ADS)
Basart, S.; Pay, M. T.; Jorba, O.; Pérez, C.; Jiménez-Guerrero, P.; Schulz, M.; Baldasano, J. M.
2012-04-01
The CALIOPE air quality modelling system is developed and applied to Europe with high spatial resolution (12 km × 12 km). The modelled daily-to-seasonal aerosol variability over Europe in 2004 is evaluated and analysed. Aerosols are estimated from two models, CMAQv4.5 (AERO4) and BSC-DREAM8b. CMAQv4.5 calculates biogenic, anthropogenic and sea salt aerosol and BSC-DREAM8b provides the natural mineral dust contribution from North African deserts. For the evaluation, we use daily PM10, PM2.5 and aerosol components data from 55 stations of the EMEP/CREATE network and total, coarse and fine aerosol optical depth (AOD) data from 35 stations of the AERONET sun photometer network. Annual correlations between modelled and observed values for PM10 and PM2.5 are 0.55 and 0.47, respectively. Correlations for total, coarse and fine AOD are 0.51, 0.63, and 0.53, respectively. The higher correlations of the PM10 and the coarse mode AOD are largely due to the accurate representation of the African dust influence in the forecasting system. Overall PM and AOD levels are underestimated. The evaluation of the aerosol components highlights underestimations in the fine fraction of carbonaceous matter (EC and OC) and secondary inorganic aerosols (SIA; i.e. nitrate, sulphate and ammonium). The scores of the bulk parameters are significantly improved after applying a simple model bias correction based on the observed aerosol composition. The simulated PM10 and AOD present maximum values over the industrialized and populated Po Valley and Benelux regions. SIA are dominant in the fine fraction representing up to 80% of the aerosol budget in latitudes north of 40° N. In southern Europe, high PM10 and AOD are linked to the desert dust transport from the Sahara which contributes up to 40% of the aerosol budget. Maximum seasonal ground-level concentrations (PM10 > 30 μg m-3) are found between spring and early autumn. We estimate that desert dust causes daily exceedances of the PM10 European air quality limit value (50 μg m-3) in large areas south of 45° N with more than 75 exceedances per year in the southernmost regions.
Mora, Marco; Braun, Rachel A; Shingler, Taylor; Sorooshian, Armin
2017-08-27
This paper presents an aerosol characterization study from 2003 to 2015 for the Mexico City Metropolitan Area using remotely sensed aerosol data, ground-based measurements, air mass trajectory modeling, aerosol chemical composition modeling, and reanalysis data for the broader Megalopolis of Central Mexico region. The most extensive biomass burning emissions occur between March and May concurrent with the highest aerosol optical depth, ultraviolet aerosol index, and surface particulate matter (PM) mass concentration values. A notable enhancement in coarse PM levels is observed during vehicular rush hour periods on weekdays versus weekends owing to nonengine-related emissions such as resuspended dust. Among wet deposition species measured, PM 2.5 , PM 10 , and PM coarse (PM 10 -PM 2.5 ) were best correlated with NH 4 + , SO 4 2- , and Ca 2+ , suggesting that the latter three constituents are important components of the aerosol seeding raindrops that eventually deposit to the surface in the study region. Reductions in surface PM mass concentrations were observed in 2014-2015 owing to reduced regional biomass burning as compared to 2003-2013.
NASA Astrophysics Data System (ADS)
Smith, Andrew J. A.; Grainger, Roy G.
2014-01-01
Mineral dust aerosol is a major component of natural airborne particulates. Using satellite measurements from the visible and near-infrared, there is insufficient information to retrieve a full microphysical and chemical description of an aerosol distribution. As such, refractive index is one of many parameters that must be implicitly assumed in order to obtain an optical depth retrieval. This is essentially a proxy for the dust mineralogy. Using a global soil map, it is shown that as long as a reasonable refractive index for dust is assumed, global dust variability is unlikely to cause significant variation in the optical properties of a dust aerosol distribution in the short-wave, and so should not greatly affect retrievals of mineral dust aerosol from space by visible and near-infrared radiometers. Errors in aerosol optical depth due to this variation are expected to be ≲ 1 %. The work is framed around the ORAC AATSR aerosol retrieval, but is equally applicable to similar satellite retrievals. In this case, variations in the top-of-atmosphere reflectance caused by mineral variation are within the noise limits of the instrument.
NASA Astrophysics Data System (ADS)
Liu, X.; Stamnes, S.; Ferrare, R. A.; Hostetler, C. A.; Burton, A. S.; Chemyakin, E.; Sawamura, P.; Mueller, D.
2017-12-01
Vertically resolved measurements of aerosol optical, microphysical, and macrophysical parameters are required to better understand the influence of aerosols on climate and air quality. We will describe an Optimal Estimation (OE) retrieval framework which can perform aerosol property retrievals in three modes: 1) lidar-only, 2) polarimeter-only, and 3) combined lidar-polarimeter muti-sensor system. The lidar data can be profile measurements by any high spectral resolution lidar (HSRL) and/or Raman lidar with multiple wavelengths of aerosol backscattering (β) and extinction (α). The polarimeter data can be any multi-angle and multi-wavelength measurements with 2 or 3 polarization components. We will show aerosol microphysical retrieval results from the HSRL-2 data measured from various NASA airborne field campaigns including the recent ORACLES mission. We will also show the OE retrieval results from the polarimeter-only mode. Finally, we will demonstrate how the information content of the aerosol microphysical retrieval is increased by combining the active HSRL and passive polarimeter data in our simultaneous OE retrieval system.
During air cool process aerosol absorption detection with photothermal interferometry
NASA Astrophysics Data System (ADS)
Li, Baosheng; Xu, Limei; Huang, Junling; Ma, Fei; Wang, Yicheng; Li, Zhengqiang
2014-11-01
This paper studies the basic principle of laser photothermal interferometry method of aerosol particles absorption coefficient. The photothermal interferometry method with higher accuracy and lower uncertainty can directly measure the absorption coefficient of atmospheric aerosols and not be affected by scattered light. With Jones matrix expression, the math expression of a special polarization interferometer is described. This paper using folded Jamin interferometer, which overcomes the influence of vibration on measuring system. Interference come from light polarization beam with two orthogonal and then combine to one beam, finally aerosol absorption induced refractive index changes can be gotten with four beam of phase orthogonal light. These kinds of styles really improve the stability of system and resolution of the system. Four-channel detections interact with interference fringes, to reduce the light intensity `zero drift' effect on the system. In the laboratory, this device typical aerosol absorption index, it shows that the result completely agrees with actual value. After heated by laser, cool process of air also show the process of aerosol absorption. This kind of instrument will be used to monitor ambient aerosol absorption and suspended particulate matter chemical component. Keywords: Aerosol absorption coefficient; Photothermal interferometry; Suspended particulate matter.
NASA Astrophysics Data System (ADS)
Sun, C.; Lee, B. P.; Huang, D.; Li, Y. J.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.
2015-07-01
Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 at the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear meal-time concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during meal times, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a~lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and influence of continental air masses.
Urban aerosol hygroscopicity and CCN activity measured during the MAPS-Seoul 2016 campaign
NASA Astrophysics Data System (ADS)
Kim, N.; Park, M.; Yum, S. S.; Kim, D. S.
2016-12-01
While submicron aerosols in atmosphere and their effects on air quality and climate are a rising issue in atmospheric sciences, scientific understanding of them is still limited due to the lack of comprehensive observations. In particular, studies for hygroscopic properties of aerosols, closely related to cloud condensation nuclei (CCN) activity, are essential to aerosol-cloud-interaction study as aerosols can act as CCN, which crucially influence cloud microphysical and radiative properties. Urban aerosol properties were measured at Olympic Park in Seoul, a typical megacity with various anthropogenic sources, during the Megacity Air Pollution Studies (MAPS-Seoul 2016) campaign (9 May- 12 June 2016) for understanding diverse aspects of air quality problem in Korea. Physical properties of aerosols, including aerosol and CCN number concentration, aerosol size distribution and growth factor were measured by CPC, CCNC, SMPS and H-TDMA, respectively. Simultaneously, size-resolved chemical component of aerosol and water-soluble aerosol mass concentration were measured by AMS and PILS-IC. These measurement data are used for comprehensive analysis. A main focus will be on the relationship between overall properties of aerosols and their CCN activity in urban area. Results from MAPS-Seoul 2015 will also be used as reference for comparison with measurements in 2016 campaign. For example, aerosol number concentrations peaked at 0800, 1500 and 2000 LT due to traffic at rush hours and photochemical reaction in the afternoon. This is slightly different from the results of MAPS-Seoul 2015 campaign that showed two dominant peaks in the morning and afternoon.
Polk, William W; Sharma, Monita; Sayes, Christie M; Hotchkiss, Jon A; Clippinger, Amy J
2016-04-23
Aerosol generation and characterization are critical components in the assessment of the inhalation hazards of engineered nanomaterials (NMs). An extensive review was conducted on aerosol generation and exposure apparatus as part of an international expert workshop convened to discuss the design of an in vitro testing strategy to assess pulmonary toxicity following exposure to aerosolized particles. More specifically, this workshop focused on the design of an in vitro method to predict the development of pulmonary fibrosis in humans following exposure to multi-walled carbon nanotubes (MWCNTs). Aerosol generators, for dry or liquid particle suspension aerosolization, and exposure chambers, including both commercially available systems and those developed by independent researchers, were evaluated. Additionally, characterization methods that can be used and the time points at which characterization can be conducted in order to interpret in vitro exposure results were assessed. Summarized below is the information presented and discussed regarding the relevance of various aerosol generation and characterization techniques specific to aerosolized MWCNTs exposed to cells cultured at the air-liquid interface (ALI). The generation of MWCNT aerosols relevant to human exposures and their characterization throughout exposure in an ALI system is critical for extrapolation of in vitro results to toxicological outcomes in humans.
NASA Astrophysics Data System (ADS)
Preunkert, S.; Legrand, M.
2013-07-01
Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps), are here used to reconstruct past aerosol load and composition of the free European troposphere from before World War II to present. Available ice core records include inorganic (Na+, Ca2+, NH4+, Cl-, NO3-, and SO42-) and organic (carboxylates, HCHO, humic-like substances, dissolved organic carbon, water-insoluble organic carbon, and black carbon) compounds and fractions that permit reconstructing the key aerosol components and their changes over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921-1951 to 1971-1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). Thus, not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water-soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarios dealing with climate forcing by atmospheric aerosol.
Stratospheric Aerosol and Gas Experiment (SAGE 3)
NASA Technical Reports Server (NTRS)
Mccormick, M. P.
1993-01-01
The proposed SAGE III instrument would be the principal source of data for global changes of stratospheric aerosols, stratospheric water vapor, and ozone profiles, and a contributing source of data for upper tropospheric water vapor, aerosols, and clouds. The ability to obtain such data has been demonstrated by the predecessor instrument, SAGE II, but SAGE III will be substantially more capable, as discussed below. The capabilities for monitoring the profiles of atmospheric constituents have been verified in detail, including ground-based validations, for aerosol, ozone, and water vapor. Indeed, because of its self-calibrating characteristics, SAGE II was an essential component of the international ozone trend assessments, and SAGE II is now proving to be invaluable in tracking the aerosols from Mt. Pinatubo. Although SAGE profiles generally terminate at the height of the first tropospheric cloud layer, it has been found that the measurements extend down to 3 km altitude more than 40 percent of the time at most latitudes. Thus, useful information can also be obtained on upper tropospheric aerosols, water vapor, and ozone.
Aerosol Sample Inhomogeneity with Debris from the Fukushima Daiichi Nuclear Accident
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gomez, Reynaido; Biegalski, Steven R.; Woods, Vincent T.
2014-09-01
Radionuclide aerosol sampling is a vital component in the detection of nuclear explosions, nuclear accidents, and other radiation releases. This was proven by the detection and tracking of emissions from the Fukushima Daiichi incident across the globe by IMS stations. Two separate aerosol samplers were operated in Richland, WA following the event and debris from the accident were measured at levels well above detection limits. While the atmospheric activity concentration of radionuclides generally compared well between the two stations, they did not agree within uncertainties. This paper includes a detailed study of the aerosol sample homogeneity of 134Cs and 137Cs,more » then relates it to the overall uncertainty of the original measurement. Our results show that sample inhomogeneity adds an additional 5–10% uncertainty to each aerosol measurement and that this uncertainty is in the same range as the discrepancies between the two aerosol sample measurements from Richland, WA.« less
Jaafar, Shoffian Amin; Latif, Mohd Talib; Razak, Intan Suraya; Shaharudin, Muhammad Zulhilmi; Khan, Md Firoz; Wahid, Nurul Bahiyah Abd; Suratman, Suhaimi
2016-08-15
This study determined the effect of monsoonal changes on the composition of atmospheric surfactants in coastal areas. The composition of anions (SO4(2-), NO3(-), Cl(-), F(-)) and the major elements (Ca, K, Mg, Na) in aerosols were used to determine the possible sources of surfactants. Surfactant compositions were determined using a colorimetric method as methylene blue active substances (MBAS) and disulphine blue active substances (DBAS). The anion and major element compositions of the aerosol samples were determined by ion chromatography (IC) and inductively coupled plasma mass spectrometry (ICP-MS), respectively. The results indicated that the concentrations of surfactant in aerosols were dominated by MBAS (34-326pmolm(-3)). Monsoonal changes were found to significantly affect the concentration of surfactants. Using principal component analysis-multiple linear regressions (PCA-MLR), major possible sources for surfactants in the aerosols were motor vehicle emissions, secondary aerosol and the combustion of biomass along with marine aerosol. Copyright © 2016 Elsevier Ltd. All rights reserved.
Aerosol Microphysical Effects on Cloud Fraction over the Nighttime Arctic Ocean
NASA Astrophysics Data System (ADS)
Zamora, L. M.; Kahn, R. A.; Stohl, A.; Eckhardt, S.
2017-12-01
Cloud fraction is a key component affecting the surface energy balance in the Arctic. Aerosol microphysical processes can affect cloud fraction, for example through cloud lifetime effects. However, the importance of aerosol impacts on cloud fraction is not well constrained on a regional scale at high latitudes. Here we discuss a new method for identifying and comparing clean and aerosol-influenced cloud characteristics using a combination of multi-year remote sensing data (CALIPSO, CloudSat) and the FLEXPART aerosol model. We use this method to investigate a variety of aerosol microphysical impacts on nighttime Arctic Ocean clouds on regional and local scales. We observe differences in factors that can impact cloud lifetime, including cloud thickness and phase, within a subset of clean vs. polluted clouds. We will also discuss cumulative cloud fraction differences in clean and non-clean environments, as well as their likely impact on longwave cloud radiative effects at the Arctic Ocean surface during polar night.
Effect of Mineral Dust on Ocean Color Retrievals From Space: A Radiative Transfer Simulation Study
NASA Astrophysics Data System (ADS)
Ahmad, Z.; Franz, B. A.
2016-02-01
In this paper we examine the effect of mineral aerosols (dust) on the retrieval of ocean colors from space. Mineral aerosols are one of the major components of all aerosols found in the earth's atmosphere. These are mainly soil particles that originate from arid and semiarid regions of the world and are blown away by winds thousands of kilometers away from their source regions. The radii of these aerosols are between 0.1 and 1.0 μm and their resident time in the atmosphere is about 21 days. The primary focus of this paper is to estimate the remote sensing reflectance (Rrs) errors in the presence of absorbing aerosols over ocean. The present study is based on radiative transfer (RT) simulations, and it is particularly relevant to ocean color retrievals from sensors like MODIS, MERIS, VIIRS, and the future PACE/OCI. In the simulations, we have used mineralogy to determine the spectral dependence of aerosol refractive index, and modeled the aerosols to represent dust over Cape Verde (Sal Island). As a part of this study, we will present the results for retrieved aerosol optical thickness (τ), Angstrom exponent (α), and remote sensing reflectance (Rrs) and compare them with similar results for non-absorbing aerosols. In addition, we will show how aerosol layer height affects the ocean color retrievals.
NASA Astrophysics Data System (ADS)
Arapi, A.; Wu, Y.; Moshary, F.; Blake, R.; Liou-Mark, J.
2017-12-01
Aerosol and cloud play important roles on the Earth's energy budget, which is an important component of climate research. The radiative effects of aerosol-cloud interaction are still highly uncertain and the accuracy of their representation in climate models depends on the accuracy of their measurements. This study evaluates the potential to determine the existence of hydrated aerosols near clouds based on a ground-based multiple-wavelength elastic-Raman lidar at 1064-532-355nm and satellite measurement in New York City area (NYC), east coast of US. The main goal of this study is to examine the variations of color-ratio (spectral or wavelength dependence of backscatter) and relative backscatter to identify patterns between aerosol and cloud. In this presentation, we show the time-height distribution and variation of lidar-measured relative backscatter and color-ratio for some case studies. Then, we employ an aerosol-cloud discrimination algorithm to separate aerosols and clouds according to the color-ratio differences. We demonstrate the significant variation of aerosol optical properties near the low-level clouds in summer, which indicates the potential interaction or transient zone between aerosols and clouds. Finally, we show the preliminary evaluation of the aerosol and cloud product from the satellite retrievals when the ground-lidar observes the transported smoke plumes in NYC area.
NASA Astrophysics Data System (ADS)
Ramaswamy, V.; Freidenreich, S.; Ginoux, P. A.; Ming, Y.; Paynter, D.; Persad, G.; Schwarzkopf, M. D.
2017-12-01
Emissions of greenhouse gases and aerosols alter atmospheric composition and `force' major perturbations in the radiative fluxes at the top-of-the-atmosphere and surface. In this paper, we discuss the radiative changes caused by anthropogenic greenhouse gases and aerosols at the surface, and its importance in the context of effects on the global hydrologic cycle. An important characteristic of imbalances forced by radiative species is the tendency for responses to occur in the non-radiative components, in order for the surface energy and moisture budgets to re-establish equilibrium. Using the NOAA/ GFDL global climate models used in CMIP3 and CMIP5, and to be used in CMIP6, we investigate how the surface energy balance has evolved with time under the action of the emissions, and the manner of changes in the surface radiative, sensible and latent heat components. We diagnose the relative importance of the forcings on the global and continental scales, the differing mechanisms due to greenhouse gases and aerosols on surface heat and moisture budgets, and the relative roles of the atmospheric constituents on precipitation and evaporation. Scattering and absorbing properties of aerosols can have contrasting effects on precipitation, with the aerosol indirect effect presenting another complication owing to the uncertainty in its magnitude. We compare the modeled surface flux changes against observations made from multiple platforms over the 20th and the early period of the 21st centuries, and asses the models' strengths and weaknesses. We also explore the consequences for the surface balance and precipitation in the 21st century under various emission scenarios.
NASA Astrophysics Data System (ADS)
Torres, O.; Jethva, H. T.; Ahn, C.
2016-12-01
Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes of the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regions of the world. Contrary to the known cooling effects of these aerosols in cloud-free scenario over dark surface, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing (warming) at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud directly depends on the aerosol loading, microphysical and optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of above-cloud aerosol optical depth (ACAOD) of absorbing aerosols retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. Physically based on the strong `color ratio' effect in the near-UV caused by the spectral absorption of aerosols above cloud, the algorithm, formally named as OMACA, retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. Here, we present the algorithm architecture and results from an 11-year global record (2005-2015) including global climatology of frequency of occurrence and ACAOD. The theoretical uncertainty analysis and planned validation activities using measurements from upcoming field campaigns are also discussed.
A Ten-Year Global Record of Absorbing Aerosols Above Clouds from OMI's Near-UV Observations
NASA Technical Reports Server (NTRS)
Jethva, Hiren; Torres, Omar; Ahn, Changwoo
2016-01-01
Aerosol-cloud interaction continues to be one of the leading uncertain components of climate models, primarily due to the lack of an adequate knowledge of the complex microphysical and radiative processes associated with the aerosol-cloud system. The situations when aerosols and clouds are found in the same atmospheric column, for instance, when light-absorbing aerosols such as biomass burning generated carbonaceous particles or wind-blown dust overlay low-level cloud decks, are commonly found over several regional of the world. Contrary to the cloud-free scenario over dark surface, for which aerosols are known to produce a net cooling effect (negative radiative forcing) on climate, the overlapping situation of absorbing aerosols over cloud can potentially exert a significant level of atmospheric absorption and produces a positive radiative forcing at top-of-atmosphere. The magnitude of direct radiative effects of aerosols above cloud depends directly on the aerosol loading, microphysical-optical properties of the aerosol layer and the underlying cloud deck, and geometric cloud fraction. We help in addressing this problem by introducing a novel product of optical depth of absorbing aerosols above clouds retrieved from near-UV observations made by the Ozone Monitoring Instrument (OMI) on board NASA's Aura platform. The presence of absorbing aerosols above cloud reduces the upwelling radiation reflected by cloud and produces a strong 'color ratio' effect in the near-UV region, which can be unambiguously detected in the OMI measurements. Physically based on this effect, the OMACA algorithm retrieves the optical depths of aerosols and clouds simultaneously under a prescribed state of atmosphere. The algorithm architecture and results from a ten-year global record including global climatology of frequency of occurrence and above-cloud aerosol optical depth, and a discussion on related future field campaigns are presented.
NASA Technical Reports Server (NTRS)
Fox, Robert; Prins, Elaine Mae; Feltz, Joleen M.
2001-01-01
In recent years, modeling and analysis efforts have suggested that the direct and indirect radiative effects of both anthropogenic and natural aerosols play a major role in the radiative balance of the earth and are an important factor in climate change calculations. The direct effects of aerosols on radiation and indirect effects on cloud properties are not well understood at this time. In order to improve the characterization of aerosols within climate models it is important to accurately parameterize aerosol forcing mechanisms at the local, regional, and global scales. This includes gaining information on the spatial and temporal distribution of aerosols, transport regimes and mechanisms, aerosol optical thickness, and size distributions. Although there is an expanding global network of ground measurements of aerosol optical thickness and size distribution at specific locations, satellite data must be utilized to characterize the spatial and temporal extent of aerosols and transport regimes on regional and global scales. This study was part of a collaborative effort to characterize aerosol radiative forcing over the Atlantic basin associated with the following three major aerosol components in this region: urban/sulfate, Saharan dust, and biomass burning. In-situ ground measurements obtained by a network of sun photometers during the Smoke Clouds and Radiation Experiment in Brazil (SCAR-B) and the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) were utilized to develop, calibrate, and validate a Geostationary Operational Environmental Satellite (GOES)-8 aerosol optical thickness (AOT) product. Regional implementation of the GOES-8 AOT product was used to augment point source measurements to gain a better understanding of the spatial and temporal distributions of Atlantic basin aerosols during SCAR-B and TARFOX.
Radiative absorption enhancement of dust mixed with anthropogenic pollution over East Asia
NASA Astrophysics Data System (ADS)
Tian, Pengfei; Zhang, Lei; Ma, Jianmin; Tang, Kai; Xu, Lili; Wang, Yuan; Cao, Xianjie; Liang, Jiening; Ji, Yuemeng; Jiang, Jonathan H.; Yung, Yuk L.; Zhang, Renyi
2018-06-01
The particle mixing state plays a significant yet poorly quantified role in aerosol radiative forcing, especially for the mixing of dust (mineral absorbing) and anthropogenic pollution (black carbon absorbing) over East Asia. We have investigated the absorption enhancement of mixed-type aerosols over East Asia by using the Aerosol Robotic Network observations and radiative transfer model calculations. The mixed-type aerosols exhibit significantly enhanced absorbing ability than the corresponding unmixed dust and anthropogenic aerosols, as revealed in the spectral behavior of absorbing aerosol optical depth, single scattering albedo, and imaginary refractive index. The aerosol radiative efficiencies for the dust, mixed-type, and anthropogenic aerosols are -101.0, -112.9, and -98.3 Wm-2 τ-1 at the bottom of the atmosphere (BOA); -42.3, -22.5, and -39.8 Wm-2 τ-1 at the top of the atmosphere (TOA); and 58.7, 90.3, and 58.5 Wm-2 τ-1 in the atmosphere (ATM), respectively. The BOA cooling and ATM heating efficiencies of the mixed-type aerosols are significantly higher than those of the unmixed aerosol types over the East Asia region, resulting in atmospheric stabilization. In addition, the mixed-type aerosols correspond to a lower TOA cooling efficiency, indicating that the cooling effect by the corresponding individual aerosol components is partially counteracted. We conclude that the interaction between dust and anthropogenic pollution not only represents a viable aerosol formation pathway but also results in unfavorable dispersion conditions, both exacerbating the regional air pollution in East Asia. Our results highlight the necessity to accurately account for the mixing state of aerosols in atmospheric models over East Asia in order to better understand the formation mechanism for regional air pollution and to assess its impacts on human health, weather, and climate.
Influence of Atmospheric Processes on the Solubility and Composition of Iron in Saharan Dust
NASA Astrophysics Data System (ADS)
Ingall, E. D.; Longo, A.; Feng, Y.; Lai, B.; Landing, W. M.; Shelley, R.; Nenes, A.; Mihalopoulos, N.; Violaki, K.
2016-12-01
Iron is a key micronutrient that is vital for all organisms. The supply of bioavailable, soluble iron controls primary productivity in approximately 30% of the world's oceans. The significant contribution of atmospheric aerosols to the bioavailable iron budget in vast ocean regions, underscores the need to understand the controls and transformations of aerosol iron solubility during atmospheric transport. The Sahara Desert contains the largest and most active sources of aerosol dust globally and can be a key source of nutrients to the Mediterranean Sea, much of the North Atlantic Ocean, and even as far as the Gulf of Mexico. Aerosol iron was examined in Saharan dust plumes using a combination of iron near-edge X-ray absorption spectroscopy and wet chemical techniques. Aerosol samples were collected at three sites located in the Mediterranean, the Atlantic, and Bermuda to characterize iron at different atmospheric transport lengths and time scales. Iron(III) oxides were a component of aerosols at all sampling sites and dominated aerosol iron in Mediterranean samples. In Atlantic samples, iron(II & III) sulfate, iron(III) phosphate, and iron(II) silicates were also contributors to aerosol composition. With increased atmospheric transport time, iron(II) sulfates are found to become more abundant, aerosol iron oxidation state became more reduced, and aerosol acidity increased. Atmospheric processing, including acidic reactions and photo-reduction, likely influence the form of iron minerals and the oxidation state in Saharan dust aerosols and contribute to increases in aerosol iron solubility. Overall, these findings suggest that a combination of factors affects aerosol iron solubility during long-distance atmospheric transport and emphasize the need to consider reductive mechanisms as well as proton-induced solubilization of aerosol iron in modeling studies.
Atmospheric aerosol composition and source apportionments to aerosol in southern Taiwan
NASA Astrophysics Data System (ADS)
Tsai, Ying I.; Chen, Chien-Lung
In this study, the chemical characteristics of winter aerosol at four sites in southern Taiwan were determined and the Gaussian Trajectory transfer coefficient model (GTx) was then used to identify the major air pollutant sources affecting the study sites. Aerosols were found to be acidic at all four sites. The most important constituents of the particulate matter (PM) by mass were SO 42-, organic carbon (OC), NO 3-, elemental carbon (EC) and NH 4+, with SO 42-, NO 3-, and NH 4+ together constituting 86.0-87.9% of the total PM 2.5 soluble inorganic salts and 68.9-78.3% of the total PM 2.5-10 soluble inorganic salts, showing that secondary photochemical solution components such as these were the major contributors to the aerosol water-soluble ions. The coastal site, Linyuan (LY), had the highest PM mass percentage of sea salts, higher in the coarse fraction, and higher sea salts during daytime than during nighttime, indicating that the prevailing daytime sea breeze brought with it more sea-salt aerosol. Other than sea salts, crustal matter, and EC in PM 2.5 at Jenwu (JW) and in PM 2.5-10 at LY, all aerosol components were higher during nighttime, due to relatively low nighttime mixing heights limiting vertical and horizontal dispersion. At JW, a site with heavy traffic loadings, the OC/EC ratio in the nighttime fine and coarse fractions of approximately 2.2 was higher than during daytime, indicating that in addition to primary organic aerosol (POA), secondary organic aerosol (SOA) also contributed to the nighttime PM 2.5. This was also true of the nighttime coarse fraction at LY. The GTx produced correlation coefficients ( r) for simulated and observed daily concentrations of PM 10 at the four sites (receptors) in the range 0.45-0.59 and biases from -6% to -20%. Source apportionment indicated that point sources were the largest PM 10 source at JW, LY and Daliao (DL), while at Meinung (MN), a suburban site with less local PM 10, SO x and NO x emissions, upwind boundary concentration was the major PM 10 source, followed by point sources and top boundary concentration.
A Global Modeling Study on Carbonaceous Aerosol Microphysical Characteristics and Radiative Effects
NASA Technical Reports Server (NTRS)
Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.
2010-01-01
Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.
A global modeling study on carbonaceous aerosol microphysical characteristics and radiative effects
NASA Astrophysics Data System (ADS)
Bauer, S. E.; Menon, S.; Koch, D.; Bond, T. C.; Tsigaridis, K.
2010-08-01
Recently, attention has been drawn towards black carbon aerosols as a short-term climate warming mitigation candidate. However the global and regional impacts of the direct, indirect and semi-direct aerosol effects are highly uncertain, due to the complex nature of aerosol evolution and the way that mixed, aged aerosols interact with clouds and radiation. A detailed aerosol microphysical scheme, MATRIX, embedded within the GISS climate model is used in this study to present a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative effects. Our best estimate for net direct and indirect aerosol radiative flux change between 1750 and 2000 is -0.56 W/m2. However, the direct and indirect aerosol effects are quite sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative flux change can vary between -0.32 to -0.75 W/m2 depending on these carbonaceous particle properties at emission. Taking into account internally mixed black carbon particles let us simulate correct aerosol absorption. Absorption of black carbon aerosols is amplified by sulfate and nitrate coatings and, even more strongly, by organic coatings. Black carbon mitigation scenarios generally showed reduced radiative fluxeswhen sources with a large proportion of black carbon, such as diesel, are reduced; however reducing sources with a larger organic carbon component as well, such as bio-fuels, does not necessarily lead to a reduction in positive radiative flux.
Occurrence of pristine aerosol environments on a polluted planet.
Hamilton, Douglas S; Lee, Lindsay A; Pringle, Kirsty J; Reddington, Carly L; Spracklen, Dominick V; Carslaw, Kenneth S
2014-12-30
Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol-cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present--day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions-the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty.
Sun, Kang; Liu, Xingang; Gu, Jianwei; Li, Yunpeng; Qu, Yu; An, Junling; Wang, Jingli; Zhang, Yuanhang; Hu, Min; Zhang, Fang
2015-06-01
Size-resolved aerosol samples were collected by MOUDI in four seasons in 2007 in Beijing. The PM10 and PM1.8 mass concentrations were 166.0±120.5 and 91.6±69.7 μg/m3, respectively, throughout the measurement, with seasonal variation: nearly two times higher in autumn than in summer and spring. Serious fine particle pollution occurred in winter with the PM1.8/PM10 ratio of 0.63, which was higher than other seasons. The size distribution of PM showed obvious seasonal and diurnal variation, with a smaller fine mode peak in spring and in the daytime. OM (organic matter=1.6×OC (organic carbon)) and SIA (secondary inorganic aerosol) were major components of fine particles, while OM, SIA and Ca2+ were major components in coarse particles. Moreover, secondary components, mainly SOA (secondary organic aerosol) and SIA, accounted for 46%-96% of each size bin in fine particles, which meant that secondary pollution existed all year. Sulfates and nitrates, primarily in the form of (NH4)2SO4, NH4NO3, CaSO4, Na2SO4 and K2SO4, calculated by the model ISORROPIA II, were major components of the solid phase in fine particles. The PM concentration and size distribution were similar in the four seasons on non-haze days, while large differences occurred on haze days, which indicated seasonal variation of PM concentration and size distribution were dominated by haze days. The SIA concentrations and fractions of nearly all size bins were higher on haze days than on non-haze days, which was attributed to heterogeneous aqueous reactions on haze days in the four seasons. Copyright © 2015. Published by Elsevier B.V.
Effects of Aerosol Pollution on Clouds over Megacities
NASA Astrophysics Data System (ADS)
Sechrist, B.; Jacobson, M. Z.
2013-12-01
The correlation between aerosol optical depth (AOD) and cloud properties - principally cloud fraction and cloud optical depth (COD) - is examined using satellite retrievals from the MODIS satellites over Los Angeles and Beijing. Ten Hoeve et al. (2011, Atmos. Chem. Phys, 11(7), 3021-3036) used satellite data to examine the impact of aerosols on warm clouds around Rondonia, Brazil, during the biomass burning season. They found that the COD-AOD relationship exhibits a 'boomerang' shape in which COD initially increases with increasing AOD but then decreases as AOD continues to increase beyond some critical level. This result is thought to reflect the balance between the microphysical and radiative components of a cloud's response to aerosols. The microphysical process dominates at low AOD, while the radiative process dominates at high AOD. This study is analogous to Ten Hoeve et al., but for aerosols derived primarily from fossil fuel combustion rather than biomass burning. Preliminary results will be presented.
The aerosol-monsoon climate system of Asia: A new paradigm
NASA Astrophysics Data System (ADS)
Lau, William K. M.
2016-02-01
This commentary is based on a series of recent lectures on aerosol-monsoon interactions I gave at the Beijing Normal University in August 2015. A main theme of the lectures is on a new paradigm of "An Aerosol-Monsoon-Climate-System", which posits that aerosol, like rainfall, cloud, and wind, is an integral component of the monsoon climate system, influencing monsoon weather and climate on all timescales. Here, salient issues discussed in my lectures and my personal perspective regarding interactions between atmospheric dynamics and aerosols from both natural and anthropogenic sources are summarized. My hope is that under this new paradigm, we can break down traditional disciplinary barriers, advance a deeper understanding of weather and climate in monsoon regions, as well as entrain a new generation of geoscientists to strive for a sustainable future for one of the most complex and challenging human-natural climate sub-system of the earth.
Enhanced Deep Blue Aerosol Retrieval Algorithm: The Second Generation
NASA Technical Reports Server (NTRS)
Hsu, N. C.; Jeong, M.-J.; Bettenhausen, C.; Sayer, A. M.; Hansell, R.; Seftor, C. S.; Huang, J.; Tsay, S.-C.
2013-01-01
The aerosol products retrieved using the MODIS collection 5.1 Deep Blue algorithm have provided useful information about aerosol properties over bright-reflecting land surfaces, such as desert, semi-arid, and urban regions. However, many components of the C5.1 retrieval algorithm needed to be improved; for example, the use of a static surface database to estimate surface reflectances. This is particularly important over regions of mixed vegetated and non- vegetated surfaces, which may undergo strong seasonal changes in land cover. In order to address this issue, we develop a hybrid approach, which takes advantage of the combination of pre-calculated surface reflectance database and normalized difference vegetation index in determining the surface reflectance for aerosol retrievals. As a result, the spatial coverage of aerosol data generated by the enhanced Deep Blue algorithm has been extended from the arid and semi-arid regions to the entire land areas.
Seasonal dependence of aerosol processing in urban Philadelphia
NASA Astrophysics Data System (ADS)
Avery, A. M.; Waring, M. S.; DeCarlo, P. F.
2017-12-01
Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower temperatures. Aerosol compositional differences in winter and summer indicate Philadelphia resident's aerosol exposures vary significantly with season.
Gentner, Drew R; Jathar, Shantanu H; Gordon, Timothy D; Bahreini, Roya; Day, Douglas A; El Haddad, Imad; Hayes, Patrick L; Pieber, Simone M; Platt, Stephen M; de Gouw, Joost; Goldstein, Allen H; Harley, Robert A; Jimenez, Jose L; Prévôt, André S H; Robinson, Allen L
2017-02-07
Secondary organic aerosol (SOA) is formed from the atmospheric oxidation of gas-phase organic compounds leading to the formation of particle mass. Gasoline- and diesel-powered motor vehicles, both on/off-road, are important sources of SOA precursors. They emit complex mixtures of gas-phase organic compounds that vary in volatility and molecular structure-factors that influence their contributions to urban SOA. However, the relative importance of each vehicle type with respect to SOA formation remains unclear due to conflicting evidence from recent laboratory, field, and modeling studies. Both are likely important, with evolving contributions that vary with location and over short time scales. This review summarizes evidence, research needs, and discrepancies between top-down and bottom-up approaches used to estimate SOA from motor vehicles, focusing on inconsistencies between molecular-level understanding and regional observations. The effect of emission controls (e.g., exhaust aftertreatment technologies, fuel formulation) on SOA precursor emissions needs comprehensive evaluation, especially with international perspective given heterogeneity in regulations and technology penetration. Novel studies are needed to identify and quantify "missing" emissions that appear to contribute substantially to SOA production, especially in gasoline vehicles with the most advanced aftertreatment. Initial evidence suggests catalyzed diesel particulate filters greatly reduce emissions of SOA precursors along with primary aerosol.
Evaluating the mutagenic potential of aerosol organic compounds using informatics-based screening
NASA Astrophysics Data System (ADS)
Decesari, Stefano; Kovarich, Simona; Pavan, Manuela; Bassan, Arianna; Ciacci, Andrea; Topping, David
2018-02-01
Whilst general policy objectives to reduce airborne particulate matter (PM) health effects are to reduce exposure to PM as a whole, emerging evidence suggests that more detailed metrics associating impacts with different aerosol components might be needed. Since it is impossible to conduct toxicological screening on all possible molecular species expected to occur in aerosol, in this study we perform a proof-of-concept evaluation on the information retrieved from in silico toxicological predictions, in which a subset (N = 104) of secondary organic aerosol (SOA) compounds were screened for their mutagenicity potential. An extensive database search showed that experimental data are available for 13 % of the compounds, while reliable predictions were obtained for 82 %. A multivariate statistical analysis of the compounds based on their physico-chemical, structural, and mechanistic properties showed that 80 % of the compounds predicted as mutagenic were grouped into six clusters, three of which (five-membered lactones from monoterpene oxidation, oxygenated multifunctional compounds from substituted benzene oxidation, and hydroperoxides from several precursors) represent new candidate groups of compounds for future toxicological screenings. These results demonstrate that coupling model-generated compositions to in silico toxicological screening might enable more comprehensive exploration of the mutagenic potential of specific SOA components.
Giorio, Chiara; Tapparo, Andrea; Dall'Osto, Manuel; Beddows, David C S; Esser-Gietl, Johanna K; Healy, Robert M; Harrison, Roy M
2015-03-17
Positive matrix factorization (PMF) has been applied to single particle ATOFMS spectra collected on a six lane heavily trafficked road in central London (Marylebone Road), which well represents an urban street canyon. PMF analysis successfully extracted 11 factors from mass spectra of about 700,000 particles as a complement to information on particle types (from K-means cluster analysis). The factors were associated with specific sources and represent the contribution of different traffic related components (i.e., lubricating oils, fresh elemental carbon, organonitrogen and aromatic compounds), secondary aerosol locally produced (i.e., nitrate, oxidized organic aerosol and oxidized organonitrogen compounds), urban background together with regional transport (aged elemental carbon and ammonium) and fresh sea spray. An important result from this study is the evidence that rapid chemical processes occur in the street canyon with production of secondary particles from road traffic emissions. These locally generated particles, together with aging processes, dramatically affected aerosol composition producing internally mixed particles. These processes may become important with stagnant air conditions and in countries where gasoline vehicles are predominant and need to be considered when quantifying the impact of traffic emissions.
[Tracing Sources of Sulfate Aerosol in Nanjing Northern Suburb Using Sulfur and Oxygen Isotopes].
Wei, Ying; Guo, Zhao-bing; Ge, Xin; Zhu, Sheng-nan; Jiang, Wen-juan; Shi, Lei; Chen, Shu
2015-04-01
Abstract: To trace the sources of sulfate contributing to atmospheric aerosol, PM2.5 samples for isotopic analysis were collected in Nanjing northern suburb during January 2014. The sulfur and oxygen isotopic compositions of sulfate from these samples were determined by EA-IRMS. Source identification and apportionment were carried out using stable isotopic and chemical evidences, combined with absolute principal component analysis (APCA) method. The Δ34S values of aerosol sulfate ranged from 2.7 per thousand to 6.4 per thousand, with an average of 5.0 per thousand ± 0.9 per thousand, while the Δ18O values ranged from 10.6 per thousand to 16.1 per thousand, with an average of 12.5 per thousand ± 1.37 per thousand. In conjunction with air mass trajectories, the results suggested that aerosol sulfates were controlled by a dominance of local anthropogenic sulfate, followed by the contributions of long-distance transported sulfate. There was a minor effect of some other low-Δ34S valued sulfates, which might be expected from biogenic sources. Absolute principal component analysis results showed that the contributions of anthropogenic sulfate and long-distance transported sulfate were 46.74% and 31.54%, respectively.
The impact of biogenic carbon emissions on aerosol absorption inMexico City
DOE Office of Scientific and Technical Information (OSTI.GOV)
Marley, N; Gaffney, J; Tackett, M J
2009-02-24
In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbingmore » secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.« less
NASA Astrophysics Data System (ADS)
Sorooshian, Armin; Wonaschütz, Anna; Jarjour, Elias G.; Hashimoto, Bryce I.; Schichtel, Bret A.; Betterton, Eric A.
2011-10-01
This study reports a comprehensive characterization of atmospheric aerosol particle properties in relation to meteorological and back trajectory data in the southern Arizona region, which includes two of the fastest growing metropolitan areas in the United States (Phoenix and Tucson). Multiple data sets (MODIS, AERONET, OMI/TOMS, MISR, GOCART, ground-based aerosol measurements) are used to examine monthly trends in aerosol composition, aerosol optical depth (AOD), and aerosol size. Fine soil, sulfate, and organics dominate PM2.5 mass in the region. Dust strongly influences the region between March and July owing to the dry and hot meteorological conditions and back trajectory patterns. Because monsoon precipitation begins typically in July, dust levels decrease, while AOD, sulfate, and organic aerosol reach their maximum levels because of summertime photochemistry and monsoon moisture. Evidence points to biogenic volatile organic compounds being a significant source of secondary organic aerosol in this region. Biomass burning also is shown to be a major contributor to the carbonaceous aerosol budget in the region, leading to enhanced organic and elemental carbon levels aloft at a sky-island site north of Tucson (Mt. Lemmon). Phoenix exhibits different monthly trends for aerosol components in comparison with the other sites owing to the strong influence of fossil carbon and anthropogenic dust. Trend analyses between 1988 and 2009 indicate that the strongest statistically significant trends are reductions in sulfate, elemental carbon, and organic carbon, and increases in fine soil during the spring (March-May) at select sites. These results can be explained by population growth, land-use changes, and improved source controls.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kanniah, K. D.; Beringer, J.; Tapper, N. J.
2010-05-01
We investigated the effect of aerosols and clouds on the Net Ecosystem Productivity (NEP) of savannas in northern Australia using aerosol optical depth, clouds and radiation data from the Atmospheric Radiation Measurement (ARM) site in Darwin and carbon flux data measured from eddy covariance techniques from a site at Howard Springs, 35km southeast of Darwin. Generally we found that the concentration of aerosols in this region was relatively low than observed at other sites, therefore the proportion of diffuse radiation reaching the earths surface was only ~ 30%. As a result, we observed only a modest change in carbon uptakemore » under aerosol laden skies and there was no significant difference for dry season Radiation Use Efficiency (RUE) between clear sky, aerosols or thin clouds. On the other hand thick clouds in the wet season produce much more diffuse radiation than aerosols or thin clouds and therefore the initial canopy quantum efficiency was seen to increase 45 and 2.5 times more than under thin clouds and aerosols respectively. The normalized carbon uptake under thick clouds is 57% and 50% higher than under aerosols and thin clouds respectively even though the total irradiance received under thick clouds was reduced 59% and 50% than under aerosols and thin clouds respectively. However, reduction in total irradiance decreases the mean absolute carbon uptake as much as 22% under heavy cloud cover compared to thin clouds or aerosols. Thus, any increase in aerosol concentration or cloud cover that can enhance the diffuse component may have large impacts on productivity in this region.« less
Fog and Cloud Induced Aerosol Modification Observed by AERONET
NASA Technical Reports Server (NTRS)
Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M. A.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Platnick, S. E.; Arnold, G. T.;
2011-01-01
Large fine mode (sub-micron radius) dominated aerosols in size distributions retrieved from AERONET have been observed after fog or low-altitude cloud dissipation events. These column-integrated size distributions have been obtained at several sites in many regions of the world, typically after evaporation of low altitude cloud such as stratocumulus or fog. Retrievals with cloud processed aerosol are sometimes bimodal in the accumulation mode with the larger size mode often approx.0.4 - 0.5 microns radius (volume distribution); the smaller mode typically approx.0.12 to aprrox.0.20 microns may be interstitial aerosol that were not modified by incorporation in droplets and/or aerosol that are less hygroscopic in nature. Bimodal accumulation mode size distributions have often been observed from in situ measurements of aerosols that have interacted with clouds, and AERONET size distribution retrievals made after dissipation of cloud or fog are in good agreement with particle sizes measured by in situ techniques for cloud-processed aerosols. Aerosols of this type and large size range (in lower concentrations) may also be formed by cloud processing in partly cloudy conditions and may contribute to the shoulder of larger size particles in the accumulation mode retrievals, especially in regions where sulfate and other soluble aerosol are a significant component of the total aerosol composition. Observed trends of increasing aerosol optical depth (AOD) as fine mode radius increased suggests higher AOD in the near cloud environment and therefore greater aerosol direct radiative forcing than typically obtained from remote sensing, due to bias towards sampling at low cloud fraction.
Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS
NASA Astrophysics Data System (ADS)
Hamilton, J. F.; Webb, P. J.; Lewis, A. C.; Hopkins, J. R.; Smith, S.; Davy, P.
2004-08-01
Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-TOF/MS). Over 10000 individual organic components were isolated from around 10µg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.
Partially oxidised organic components in urban aerosol using GCXGC-TOF/MS
NASA Astrophysics Data System (ADS)
Hamilton, J.; Webb, P.; Lewis, A.; Hopkins, J.; Smith, S.; Davy, P.
2004-03-01
Partially oxidised organic compounds associated with PM2.5 aerosol collected in London, England, have been analysed using direct thermal desorption coupled to comprehensive gas chromatography-time of flight mass spectrometry (GCXGC-OF/MS). Over 10 000 individual organic components were isolated from around 10 μg of aerosol material in a single procedure and with no sample pre-treatment. Chemical functionalities observed using this analytical technique ranged from alkanes to poly-oxygenated species. The chemical band structures commonly used in GCXGC for group type identifications overlap for this sample type, and have required mass spectrometry as an additional level of instrument dimensionality. An investigation of oxygenated volatile organic compounds (o-VOC) contained within urban aerosol has been performed and in a typical sample around 130 o-VOCs were identified based on retention behaviour and spectral match. In excess of 100 other oxygenated species were also observed but lack of mass spectral library or pure components prevents positive identification. Many of the carbonyl species observed could be mechanistically linked to gas phase aromatic hydrocarbon oxidation and there is good agreement in terms of speciation between the urban samples analysed here and those degradation products observed in smog chamber experiments of aromatic oxidation. The presence of partially oxidised species such as linear chain aldehydes and ketones and cyclic products such as furanones suggests that species generated relatively early in the oxidative process may undergo gas to particle partitioning despite their relatively high volatility.
NASA Astrophysics Data System (ADS)
Shaw, Patrick
The Dust REgional Atmospheric Model (DREAM) predicts concentrations of mineral dust aerosols in time and space, but validation is challenging with current in situ particulate matter (PM) concentration measurements. Measured levels of ambient PM often contain anthropogenic components as well as windblown mineral dust. In this study, two approaches to model validation were performed with data from preexisting air quality monitoring networks: using hourly concentrations of total PM with aerodynamic diameter less than 2.5 μm (PM 2.5); and using a daily averaged speciation-derived soil component. Validation analyses were performed for point locations within the cities of El Paso (TX), Austin (TX), Phoenix (AZ), Salt Lake City (UT) and Bakersfield (CA) for most of 2006. Hourly modeled PM 2.5 did not validate at all with hourly observations among the sites (combined R < 0.00, N = 24,302 hourly values). Aerosol chemical speciation data distinguished between mineral (soil) dust from anthropogenic ambient PM. As expected, statistically significant improvements in correlation among all stations (combined R = 0.16, N = 343 daily values) were found when the soil component alone was used to validate DREAM. The validation biases that result from anthropogenic aerosols were also reduced using the soil component. This is seen in the reduction of the root mean square error between hourly in situ versus hourly modeled (RMSE hourly = 18.6 μg m -3) and 24-h in situ speciation values versus daily averaged observed (RMSE soil = 12.0 μg m -3). However, the lack of a total reduction in RMSE indicates there is still room for improvement in the model. While the soil component is the theoretical proxy of choice for a dust transport model, the current sparse and infrequent sampling is not ideal for routine hourly air quality forecast validation.
Detailed budget analysis of HONO in central London reveals a missing daytime source
NASA Astrophysics Data System (ADS)
Lee, J. D.; Whalley, L. K.; Heard, D. E.; Stone, D.; Dunmore, R. E.; Hamilton, J. F.; Young, D. E.; Allan, J. D.; Laufs, S.; Kleffmann, J.
2016-03-01
Measurements of HONO were carried out at an urban background site near central London as part of the Clean air for London (ClearfLo) project in summer 2012. Data were collected from 22 July to 18 August 2014, with peak values of up to 1.8 ppbV at night and non-zero values of between 0.2 and 0.6 ppbV seen during the day. A wide range of other gas phase, aerosol, radiation, and meteorological measurements were made concurrently at the same site, allowing a detailed analysis of the chemistry to be carried out. The peak HONO/NOx ratio of 0.04 is seen at ˜ 02:00 UTC, with the presence of a second, daytime, peak in HONO/NOx of similar magnitude to the night-time peak, suggesting a significant secondary daytime HONO source. A photostationary state calculation of HONO involving formation from the reaction of OH and NO and loss from photolysis, reaction with OH, and dry deposition shows a significant underestimation during the day, with calculated values being close to 0, compared to the measurement average of 0.4 ppbV at midday. The addition of further HONO sources from the literature, including dark conversion of NO2 on surfaces, direct emission, photolysis of ortho-substituted nitrophenols, the postulated formation from the reaction of HO2 × H2O with NO2, photolysis of adsorbed HNO3 on ground and aerosols, and HONO produced by photosensitized conversion of NO2 on the surface increases the daytime modelled HONO to 0.1 ppbV, still leaving a significant missing daytime source. The missing HONO is plotted against a series of parameters including NO2 and OH reactivity (used as a proxy for organic material), with little correlation seen. Much better correlation is observed with the product of these species with j(NO2), in particular NO2 and the product of NO2 with OH reactivity. This suggests the missing HONO source is in some way related to NO2 and also requires sunlight. Increasing the photosensitized surface conversion rate of NO2 by a factor of 10 to a mean daytime first-order loss of ˜ 6 × 10-5 s-1 (but which varies as a function of j(NO2)) closes the daytime HONO budget at all times (apart from the late afternoon), suggesting that urban surfaces may enhance this photosensitized source. The effect of the missing HONO to OH radical production is also investigated and it is shown that the model needs to be constrained to measured HONO in order to accurately reproduce the OH radical measurements.
NASA Astrophysics Data System (ADS)
Twigg, M. M.; Di Marco, C. F.; Leeson, S.; van Dijk, N.; Jones, M. R.; Leith, I. D.; Morrison, E.; Coyle, M.; Proost, R.; Peeters, A. N. M.; Lemon, E.; Frelink, T.; Braban, C. F.; Nemitz, E.; Cape, J. N.
2015-02-01
There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements, which can lead to further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows characterisation of the inorganic components of PM10 and PM2.5 (NH4+, NO3-, SO42-, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP "Supersite", Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 μg m-3. Anthropogenically derived secondary inorganic aerosols (sum of NH4+, NO3- and nss-SO42-), were the dominating species (63%) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt, was the main component (73%) of the PMcoarse fraction (PM10-PM2.5), though NO3- was also found to make a relatively large contribution to the measured mass (17%) as providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high K+ concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations > 12 μg m-3) were on average dominated by NH4+ and NO3-, where as smaller loadings at the site tended to be dominated by sea salt. As with other Western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely, that organic acids contributed to the charge balance. This study demonstrates the UK background atmospheric composition is primarily driven by meteorology with sea salt dominating air masses from the Atlantic Ocean and the Arctic, whereas secondary inorganic aerosols tended to dominate air masses from continental Europe.
NASA Astrophysics Data System (ADS)
Phillips, Gavin; Farmer, Delphine; di Marco, Chiara; Misztal, Pawel; Sueper, Donna; Kimmel, Joel; Jimenez, Jose; Fowler, David; Nemitz, Eiko
2010-05-01
New measurements of VOC emissions (measured with leaf cuvettes, and ecosystem fluxes obtained from eddy covariance measurements) suggest that oil palm (Elaeis guineensis Jacq) is a significantly larger source of isoprene than tropical forest, in Borneo. These larger sources of isoprene measured over oil palm, allied with a larger anthropogenic component of local emissions, contrasts with the composition of the atmosphere in the semi-remote tropical forest environment. The difference in the atmospheric composition above different land-uses has the potential to lead to contrasting chemistry and physics controlling the formation and processing of particulate matter. Thus land use changes, driven by the economics of biofuels, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions, chemical processing and composition of organic aerosol over both (semi-)natural and anthropogenic land uses in the tropical environment. Ecosystem flux measurements of chemically-speciated non-refractory PM1 were made over two contrasting land uses in the Malaysian state of Sabah, on the island of Borneo during 2008. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at the Global Atmospheric Watch (GAW) site at a tropical rain forest location as well as the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as a collaboration between three UK NERC funded projects (OP3, APPRAISE/ACES and DIASPORA). Recent technical developments using ToF detectors allow us to record 10 Hz full mass spectra at both high resolution (HR) and unit-mass resolution (UMR), suitable for the calculation of local eddy-covariance fluxes. The measurements provide information on the deposition rate of anthropogenic aerosol components (e.g. sulphate, nitrate, ammonium and hydrocarbon-like aerosol) to tropical forest and oil palm. At the same time, any biogenic secondary organic aerosol components formed through fast chemistry below the measurement height would appear as an upward flux, and the direct flux measurement therefore provides an alternative approach to probing BSOA formation mechanisms. In particular, through the calculation of mass spectra in terms of flux and deposition velocity those masses and aerosol fragments can be identified that show similar behaviour. In addition, the contribution of the various chemical species (e.g. nitrate, sulphate, OA sub-types) to the total mass flux will be elucidated.
Speciation of iron in ambient aerosol and cloudwater
NASA Astrophysics Data System (ADS)
Siefert, Ronald Lyn
1997-03-01
Atmospheric iron (Fe) is thought to play an important role in cloudwater chemistry (e.g., S(IV) oxidation, oxidant production, etc.), and is also an important source of Fe to certain regions of the world's oceans where Fe is believed to be a rate-limiting nutrient for primary productivity. This thesis focuses on understanding the chemistry, speciation and abundance of Fe in cloudwater and aerosol in the troposphere, through observations of Fe speciation in the cloudwater and aerosol samples collected over the continental United States and the Arabian Sea. Different chemical species of atmospheric Fe were measured in aerosol and cloudwater samples to help assess the role of Fe in cloudwater chemistry. Chapter 2 presents a set of experiments which used ambient aerosol samples suspended in aqueous solution and then irradiated with uv-light to simulate cloudwater conditions. These experiments found Fe to be a critical component for the production of H2O2. Chapter 3 discusses the development and application of a novel photochemical extraction method for the determination of photochemically-available Fe in ambient aerosol samples. Photochemically-available Fe ranged from <4 ng m-3 to 308 ng m-3, and accounted for 2.8% to 100% of the total Fe in aerosol samples collected in California and New York. Calculations based on the results of these experiments predicted that redox reactions of Fe in cloudwater could be an important in situ source of oxidants (ċOH, HO2ċ/O2/cdot/sb- ). Chapter 4 presents results of several field studies which measured the redox states of Fe and other transition metals (Mn, Cu and Cr) in cloudwater. These measurements were then used in thermodynamic models which predicted Fe(III) to be either as Fe(III)-hydroxy species or Fe(III)-oxalate species. However, an unidentified strong chelating ligand with Fe(III) was also suggested by the thermodynamic model results. Chapter 5 presents results of a field study conducted on the Arabian Sea. Total atmospheric labile-Fe(II) ranged between <0.09 ng m-3 to 7.5 ng m-3 during the inter-monsoon period, and was consistently below the detection limit during the southwest-monsoon period. The labile-Fe(II) measured during the inter-monsoon period was predominantly found in the fine fraction of the aerosol. Principal component analysis revealed a significant source of Fe and Mn which was not associated with the main aeolian dust component.
Nano- and Microparticles in Welding Aerosol: Granulometric Analysis
NASA Astrophysics Data System (ADS)
Kirichenko, K. Yu.; Drozd, V. A.; Chaika, V. V.; Gridasov, A. V.; Kholodov, A. S.; Golokhvast, K. S.
The paper presents the first results of the study of the size of particles appearing in the welding process by means of laser granulometry. It is shown that welding aerosol is the source of nano-and micro-sized particles extremely dangerous for human and animal health. Particle size distribution in the microrange was from 1 to 10 μm and up to 100%. It is shown that in 9 cases out of 28 with the use of various welding modes, welding rods and components the emission of aerosol with nano-sized particles (from 45.5% to 99.4%) is observed.
Fractional solubility of aerosol iron: Synthesis of a global-scale data set
NASA Astrophysics Data System (ADS)
Sholkovitz, Edward R.; Sedwick, Peter N.; Church, Thomas M.; Baker, Alexander R.; Powell, Claire F.
2012-07-01
Aerosol deposition provides a major input of the essential micronutrient iron to the open ocean. A critical parameter with respect to biological availability is the proportion of aerosol iron that enters the oceanic dissolved iron pool - the so-called fractional solubility of aerosol iron (%FeS). Here we present a global-scale compilation of total aerosol iron loading (FeT) and estimated %FeS values for ∼1100 samples collected over the open ocean, the coastal ocean, and some continental sites, including a new data set from the Atlantic Ocean. Despite the wide variety of methods that have been used to define 'soluble' aerosol iron, our global-scale compilation reveals a remarkably consistent trend in the fractional solubility of aerosol iron as a function of total aerosol iron loading, with the great bulk of the data defining an hyperbolic trend. The hyperbolic trends that we observe for both global- and regional-scale data are adequately described by a simple two-component mixing model, whereby the fractional solubility of iron in the bulk aerosol reflects the conservative mixing of 'lithogenic' mineral dust (high FeT and low %FeS) and non-lithogenic 'combustion' aerosols (low FeT and high %FeS). An increasing body of empirical and model-based evidence points to anthropogenic fuel combustion as the major source of these non-lithogenic 'combustion' aerosols, implying that human emissions are a major determinant of the fractional solubility of iron in marine aerosols. The robust global-scale relationship between %FeS and FeT provides a simple heuristic method for estimating aerosol iron solubility at the regional to global scale.
NASA Astrophysics Data System (ADS)
Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J.; Healy, R.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; Ehn, M.; Mikkilä, J.; Kulmala, M.; O'Dowd, C. D.
2010-09-01
As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were highest in marine tropical air - even higher than in continental air. MSA was present at twice the concentrations of previously-reported concentrations at the same location and the same season. Both continental and marine air exhibited aerosol GFs significantly less than ammonium sulphate aerosol pointing to a significant organic contribution to all air mass aerosol properties.
NASA Astrophysics Data System (ADS)
Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona
2018-05-01
Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition, inorganic nitrate evaporated in the PAM reactor as sulfate was added to the particles. These results suggest that the chemical composition of aerosols and their degree of photochemical aging, particularly for organics, are also crucial in determining aerosol mass concentrations.
The Hygroscopicity Parameter of Marine Organics in Sea Spray Aerosols
NASA Astrophysics Data System (ADS)
Boyer, M.; Chang, R. Y. W.
2015-12-01
The effects of aerosols on climate are poorly understood, specifically with respect to their influence on cloud properties. Since oceans cover >70% of Earth's surface, sea spray aerosols (SSA), which act efficiently as cloud condensation nuclei (CCN), may have important implications on Earth's radiation budget. Surface active organic species readily accumulate in the sea surface microlayer (SML), located at the ocean-atmosphere interface, and transfer onto nascent SSA. While it is understood that SSA are commonly enriched with organics, the resulting effect of the organic content on CCN activation remains unresolved. The hygroscopicity parameter, kappa (k), allows for the cloud nucleating properties of individual components to be predicted in particles of mixed composition; however, most studies typically infer k from ambient measurements without assessing the contribution of the individual components to the overall k. In this study, a method for quantifying the cloud nucleating properties of the organic species in surface seawater using k-Kohler theory is proposed. Ambient SML and bulk water samples will be collected and atomized to generate particles such that the overall k can be inferred from CCN measurements. The inorganic and organic components will be quantified, and the organic component will be separated so that the hygroscopicity of only the organic constituents can be determined. By comparing the inferred k values for the samples before and after removal of the inorganic component, the hygroscopicity of the organic constituents alone can be calculated, providing insight on the effect of organic species on CCN activation in SSA.
NASA Technical Reports Server (NTRS)
Kipling, Zak; Stier, Philip; Johnson, Colin E.; Mann, Graham W.; Bellouin, Nicolas; Bauer, Susanne E.; Bergman, Tommi; Chin, Mian; Diehl, Thomas; Ghan, Steven J.;
2016-01-01
The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3-UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3-UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN >3 nm), while the profiles of larger particles (e.g. CN>100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. We also show that the processes that affect the AOD-normalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions.
NASA Astrophysics Data System (ADS)
Koutzenogii, K. P.; Savchenko, T. I.; Chankina, O. V.; Popova, S. A.
2009-05-01
High correlation has been revealed both between the content of chemical elements in human blood and atmospheric aerosols and between blood elements and food components. The element compositions of blood and hair have been established to be strongly related to each other. These biosubstrates can be used to estimate the health of the population of the northern hemisphere. Variability of the multielement composition of the blood and hair of the inhabitants of Novosibirsk, the Tundra Nenetz, Yakuts, Chukchi and the Eskimos, food components and aerosols in the regions where they live was determined by the SRXFA method.
Aerosol and monsoon climate interactions over Asia
NASA Astrophysics Data System (ADS)
Li, Zhanqing; Lau, W. K.-M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S.-S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.
2016-12-01
The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from biomass burning, and biogenic aerosols from vegetation are considered integral components of an intrinsic aerosol-monsoon climate system, subject to external forcing of global warming, anthropogenic aerosols, and land use and change. Future research on aerosol-monsoon interactions calls for an integrated approach and international collaborations based on long-term sustained observations, process measurements, and improved models, as well as using observations to constrain model simulations and projections.
Aerosol Direct Radiative Effects and Heating in the New Era of Active Satellite Observations
NASA Astrophysics Data System (ADS)
Matus, Alexander V.
Atmospheric aerosols impact the global energy budget by scattering and absorbing solar radiation. Despite their impacts, aerosols remain a significant source of uncertainty in our ability to predict future climate. Multi-sensor observations from the A-Train satellite constellation provide valuable observational constraints necessary to reduce uncertainties in model simulations of aerosol direct effects. This study will discuss recent efforts to quantify aerosol direct effects globally and regionally using CloudSat's radiative fluxes and heating rates product. Improving upon previous techniques, this approach leverages the capability of CloudSat and CALIPSO to retrieve vertically resolved estimates of cloud and aerosol properties critical for accurately evaluating the radiative impacts of aerosols. We estimate the global annual mean aerosol direct effect to be -1.9 +/- 0.6 W/m2, which is in better agreement with previously published estimates from global models than previous satellite-based estimates. Detailed comparisons against a fully coupled simulation of the Community Earth System Model, however, reveal that this agreement on the global annual mean masks large regional discrepancies between modeled and observed estimates of aerosol direct effects related to model biases in cloud cover. A low bias in stratocumulus cloud cover over the southeastern Pacific Ocean, for example, leads to an overestimate of the radiative effects of marine aerosols. Stratocumulus clouds over the southeastern Atlantic Ocean can enhance aerosol absorption by 50% allowing aerosol layers to remain self-lofted in an area of subsidence. Aerosol heating is found to peak at 0.6 +/- 0.3 K/day an altitude of 4 km in September when biomass burning reaches a maximum. Finally, the contributions of observed aerosols components are evaluated to estimate the direct radiative forcing of anthropogenic aerosols. Aerosol forcing is computed using satellite-based radiative kernels that describe the sensitivity of shortwave fluxes in response to aerosol optical depth. The direct radiative forcing is estimated to be -0.21 W/m2 with the largest contributions from pollution that is partially offset by a positive forcing from smoke aerosols. The results from these analyses provide new benchmarks on the global radiative effects of aerosols and offer new insights for improving future assessments.
Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report
DOE Office of Scientific and Technical Information (OSTI.GOV)
Cappa, Christopher D; Atkinson, Dean B
The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements ismore » facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?« less
NASA Astrophysics Data System (ADS)
Sun, C.; Lee, B. P.; Huang, D.; Jie Li, Y.; Schurman, M. I.; Louie, P. K. K.; Luk, C.; Chan, C. K.
2016-02-01
Non-refractory submicron aerosol is characterized using an Aerosol Chemical Speciation Monitor (ACSM) in the fall and winter seasons of 2013 on the roadside in an Asian megacity environment in Hong Kong. Organic aerosol (OA), characterized by application of Positive Matrix Factorization (PMF), and sulfate are found to be dominant. Traffic-related organic aerosol shows good correlation with other vehicle-related species, and cooking aerosol displays clear mealtime concentration maxima and association with surface winds from restaurant areas. Contributions of individual species and OA factors to high NR-PM1 are analyzed for hourly data and daily data; while cooking emissions in OA contribute to high hourly concentrations, particularly during mealtimes, secondary organic aerosol components are responsible for episodic events and high day-to-day PM concentrations. Clean periods are either associated with precipitation, which reduces secondary OA with a lesser impact on primary organics, or clean oceanic air masses with reduced long-range transport and better dilution of local pollution. Haze events are connected with increases in contribution of secondary organic aerosol, from 30 to 50 % among total non-refractory organics, and the influence of continental air masses.
NASA Astrophysics Data System (ADS)
Li, Y.; Flanner, M.
2017-12-01
Accelerating surface melt on the Greenland Ice Sheet (GrIS) has led to a doubling of Greenland's contribution to global sea level rise during recent decades. The darkening effect due to black carbon (BC), dust, and other light absorbing impurities (LAI) enhances snow melt by boosting its absorption of solar energy. It is therefore important for coupled aerosol-climate and ice sheet models to include snow darkening effects from LAI, and yet most do not. In this study, we develop an aerosol deposition—snow melt kernel based on the Community Earth System Model (CESM) to investigate changes in melt flux due to variations in the amount and timing of aerosol deposition on the GrIS. The Community Land Model (CLM) component of CESM is driven with a large range of aerosol deposition fluxes to determine non-linear relationships between melt perturbation and deposition amount occurring in different months and location (thereby capturing variations in base state associated with elevation and latitude). The kernel product will include climatological-mean effects and standard deviations associated with interannual variability. Finally, the kernel will allow aerosol deposition fluxes from any global or regional aerosol model to be translated into surface melt perturbations of the GrIS, thus extending the utility of state-of-the-art aerosol models.
Simms, A D; Weston, C F; West, R M; Hall, A S; Batin, P D; Timmis, A; Hemingway, H; Fox, Kaa; Gale, C P
2015-06-01
To examine the association between cumulative missed opportunities for care (CMOC) and mortality in patients with ST-elevation myocardial infarction (STEMI). A cohort study of 112,286 STEMI patients discharged from hospital alive between January 2007 and December 2010, using data from the Myocardial Ischaemia National Audit Project (MINAP). A CMOC score was calculated for each patient and included: pre-hospital ECG, acute use of aspirin, timely reperfusion, prescription at hospital discharge of aspirin, thienopyridine inhibitor, ACE-inhibitor (or equivalent), HMG-CoA reductase inhibitor and β-blocker, and referral for cardiac rehabilitation. Mixed-effects logistic regression models evaluated the effect of CMOC on risk-adjusted 30-day and 1-year mortality (RAMR). 44.5% of patients were ineligible for ≥1 care component. Of patients eligible for all nine components, 50.6% missed ≥1 opportunity. Pre-hospital ECG and timely reperfusion were most frequently missed, predicting further missed care at discharge (pre-hospital ECG incident rate ratio [95% CI]: 1.64 [1.58-1.70]; timely reperfusion 9.94 [9.51-10.40]). Patients ineligible for care had higher RAMR than those eligible for care (30-days: 1.7% vs. 1.1%; 1-year: 8.6% vs. 5.2%), whilst those with no missed care had lower mortality than patients with ≥4 CMOC (30-days: 0.5% vs. 5.4%, adjusted OR (aOR) per CMOC group 1.22, 95% CI: 1.05-1.42; 1-year: 3.2% vs. 22.8%, aOR 1.23, 1.13-1.34). Opportunities for care in STEMI are commonly missed and significantly associated with early and later mortality. Thus, outcomes after STEMI may be improved by greater attention to missed opportunities to eligible care. © The European Society of Cardiology 2014.
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.
Mora, Marco; Braun, Rachel A.; Shingler, Taylor; Sorooshian, Armin
2017-01-01
This paper presents an aerosol characterization study from 2003 to 2015 for the Mexico City Metropolitan Area using remotely sensed aerosol data, ground-based measurements, air mass trajectory modeling, aerosol chemical composition modeling, and reanalysis data for the broader Megalopolis of Central Mexico region. The most extensive biomass burning emissions occur between March and May concurrent with the highest aerosol optical depth, ultraviolet aerosol index, and surface particulate matter (PM) mass concentration values. A notable enhancement in coarse PM levels is observed during vehicular rush hour periods on weekdays versus weekends owing to nonengine-related emissions such as resuspended dust. Among wet deposition species measured, PM2.5, PM10, and PMcoarse (PM10−PM2.5) were best correlated with NH4+, SO42−, and Ca2+, suggesting that the latter three constituents are important components of the aerosol seeding raindrops that eventually deposit to the surface in the study region. Reductions in surface PM mass concentrations were observed in 2014–2015 owing to reduced regional biomass burning as compared to 2003–2013. PMID:28955600
NASA Astrophysics Data System (ADS)
Drewnick, Frank; Hings, Silke S.; Curtius, Joachim; Eerdekens, Gunter; Williams, Jonathan
The chemical composition and chemically resolved size distributions of fine aerosol particles were measured at high time resolution (5 min) with a time-of-flight aerosol mass spectrometer (TOF-AMS) during the New Year's 2005 fireworks in Mainz, central Germany. In addition, particle number concentrations and trace gas concentrations were measured using a condensation particle counter (CPC) and a proton transfer reaction mass spectrometer (PTR-MS). The main non-refractory components of the firework aerosol were potassium, sulfate, total organics and chloride. Increased trace gas mixing ratios of methanol, acetonitrile, acetone and acetaldehyde were observed. Aerosol nitrate and ammonium concentrations were not significantly affected by the fireworks as well as the measured aromatic trace gases. The sub-micron aerosol concentrations peaked about 20 min after midnight with total mass concentrations larger than 600 μg m -3. The trace gas concentrations peaked about 30 min later. Using the sulfur-to-potassium concentration ratio measured in another fireworks aerosol, it was for the first time possible to estimate the relative ionization efficiency of aerosol potassium, measured with the TOF-AMS. Here we found a value of RIE K=2.9.
Proceedings of the 1983 Scientific Conference on Obscuration and Aerosol Research
1984-07-01
Aerosol Measurement Spheroids Laser Pulses Target Signatures Optical Pulses Pulse Propagation Clouds Laser Radiation Transport Analysis...Schematic diagram of apparatus used to make ATR measurements . (a) Top view of components. Solid line is path of laser radiation, broken line is path of...fabricated to measure the extinction properties of these materials for CO2 laser radiation. The selection process and preparation of the
Volatility of organic aerosol and its components in the megacity of Paris
NASA Astrophysics Data System (ADS)
Paciga, Andrea; Karnezi, Eleni; Kostenidou, Evangelia; Hildebrandt, Lea; Psichoudaki, Magda; Engelhart, Gabriella J.; Lee, Byong-Hyoek; Crippa, Monica; Prévôt, André S. H.; Baltensperger, Urs; Pandis, Spyros N.
2016-02-01
Using a mass transfer model and the volatility basis set, we estimate the volatility distribution for the organic aerosol (OA) components during summer and winter in Paris, France as part of the collaborative project MEGAPOLI. The concentrations of the OA components as a function of temperature were measured combining data from a thermodenuder and an aerosol mass spectrometer (AMS) with Positive Matrix Factorization (PMF) analysis. The hydrocarbon-like organic aerosol (HOA) had similar volatility distributions for the summer and winter campaigns with half of the material in the saturation concentration bin of 10 µg m-3 and another 35-40 % consisting of low and extremely low volatility organic compounds (LVOCs with effective saturation concentrations C* of 10-3-0.1 µg m-3 and ELVOCs C* less or equal than 10-4 µg m-3, respectively). The winter cooking OA (COA) was more than an order of magnitude less volatile than the summer COA. The low-volatility oxygenated OA (LV-OOA) factor detected in the summer had the lowest volatility of all the derived factors and consisted almost exclusively of ELVOCs. The volatility for the semi-volatile oxygenated OA (SV-OOA) was significantly higher than that of the LV-OOA, containing both semi-volatile organic components (SVOCs with C* in the 1-100 µg m-3 range) and LVOCs. The oxygenated OA (OOA) factor in winter consisted of SVOCs (45 %), LVOCs (25 %) and ELVOCs (30 %). The volatility of marine OA (MOA) was higher than that of the other factors containing around 60 % SVOCs. The biomass burning OA (BBOA) factor contained components with a wide range of volatilities with significant contributions from both SVOCs (50 %) and LVOCs (30 %). Finally, combining the bulk average O : C ratios and volatility distributions of the various factors, our results are placed into the two-dimensional volatility basis set (2D-VBS) framework. The OA factors cover a broad spectrum of volatilities with no direct link between the average volatility and average O : C of the OA components.
Chang, Howard H.; Wang, Yujie; Hu, Xuefei; Lyapustin, Alexei
2017-01-01
Satellite-retrieved aerosol optical properties have been extensively used to estimate ground-level fine particulate matter (PM2.5) concentrations in support of air pollution health effects research and air quality assessment at the urban to global scales. However, a large proportion, ~70%, of satellite observations of aerosols are missing as a result of cloud-cover, surface brightness, and snow-cover. The resulting PM2.5 estimates could therefore be biased due to this non-random data missingness. Cloud-cover in particular has the potential to impact ground-level PM2.5 concentrations through complex chemical and physical processes. We developed a series of statistical models using the Multi-Angle Implementation of Atmospheric Correction (MAIAC) aerosol product at 1 km resolution with information from the MODIS cloud product and meteorological information to investigate the extent to which cloud parameters and associated meteorological conditions impact ground-level aerosols at two urban sites in the US: Atlanta and San Francisco. We find that changes in temperature, wind speed, relative humidity, planetary boundary layer height, convective available potential energy, precipitation, cloud effective radius, cloud optical depth, and cloud emissivity are associated with changes in PM2.5 concentration and composition, and the changes differ by overpass time and cloud phase as well as between the San Francisco and Atlanta sites. A case-study at the San Francisco site confirmed that accounting for cloud-cover and associated meteorological conditions could substantially alter the spatial distribution of monthly ground-level PM2.5 concentrations. PMID:29057838
NASA Astrophysics Data System (ADS)
Li, X.; Zhang, C.; Li, W.
2017-12-01
Long-term spatiotemporal analysis and modeling of aerosol optical depth (AOD) distribution is of paramount importance to study radiative forcing, climate change, and human health. This study is focused on the trends and variations of AOD over six stations located in United States and China during 2003 to 2015, using satellite-retrieved Moderate Resolution Imaging Spectrometer (MODIS) Collection 6 retrievals and ground measurements derived from Aerosol Robotic NETwork (AERONET). An autoregressive integrated moving average (ARIMA) model is applied to simulate and predict AOD values. The R2, adjusted R2, Root Mean Square Error (RMSE), Mean Absolute Error (MAE), Mean Absolute Percentage Error (MAPE), and Bayesian Information Criterion (BIC) are used as indices to select the best fitted model. Results show that there is a persistent decreasing trend in AOD for both MODIS data and AERONET data over three stations. Monthly and seasonal AOD variations reveal consistent aerosol patterns over stations along mid-latitudes. Regional differences impacted by climatology and land cover types are observed for the selected stations. Statistical validation of time series models indicates that the non-seasonal ARIMA model performs better for AERONET AOD data than for MODIS AOD data over most stations, suggesting the method works better for data with higher quality. By contrast, the seasonal ARIMA model reproduces the seasonal variations of MODIS AOD data much more precisely. Overall, the reasonably predicted results indicate the applicability and feasibility of the stochastic ARIMA modeling technique to forecast future and missing AOD values.
NASA Technical Reports Server (NTRS)
Belle, Jessica H.; Chang, Howard H.; Wang, Yujie; Hu, Xuefei; Lyapustin, Alexei; Liu, Yang
2017-01-01
Satellite-retrieved aerosol optical properties have been extensively used to estimate ground-level fine particulate matter (PM2.5) concentrations in support of air pollution health effects research and air quality assessment at the urban to global scales. However, a large proportion, approximately 70%, of satellite observations of aerosols are missing as a result of cloud-cover, surface brightness, and snow-cover. The resulting PM2.5 estimates could therefore be biased due to this non-random data missingness. Cloud-cover in particular has the potential to impact ground-level PM2.5 concentrations through complex chemical and physical processes. We developed a series of statistical models using the Multi-Angle Implementation of Atmospheric Correction (MAIAC) aerosol product at 1 km resolution with information from the MODIS cloud product and meteorological information to investigate the extent to which cloud parameters and associated meteorological conditions impact ground-level aerosols at two urban sites in the US: Atlanta and San Francisco. We find that changes in temperature, wind speed, relative humidity, planetary boundary layer height, convective available potential energy, precipitation, cloud effective radius, cloud optical depth, and cloud emissivity are associated with changes in PM2.5 concentration and composition, and the changes differ by overpass time and cloud phase as well as between the San Francisco and Atlanta sites. A case-study at the San Francisco site confirmed that accounting for cloud-cover and associated meteorological conditions could substantially alter the spatial distribution of monthly ground-level PM2.5 concentrations.
Belle, Jessica H; Chang, Howard H; Wang, Yujie; Hu, Xuefei; Lyapustin, Alexei; Liu, Yang
2017-10-18
Satellite-retrieved aerosol optical properties have been extensively used to estimate ground-level fine particulate matter (PM 2.5 ) concentrations in support of air pollution health effects research and air quality assessment at the urban to global scales. However, a large proportion, ~70%, of satellite observations of aerosols are missing as a result of cloud-cover, surface brightness, and snow-cover. The resulting PM 2.5 estimates could therefore be biased due to this non-random data missingness. Cloud-cover in particular has the potential to impact ground-level PM 2.5 concentrations through complex chemical and physical processes. We developed a series of statistical models using the Multi-Angle Implementation of Atmospheric Correction (MAIAC) aerosol product at 1 km resolution with information from the MODIS cloud product and meteorological information to investigate the extent to which cloud parameters and associated meteorological conditions impact ground-level aerosols at two urban sites in the US: Atlanta and San Francisco. We find that changes in temperature, wind speed, relative humidity, planetary boundary layer height, convective available potential energy, precipitation, cloud effective radius, cloud optical depth, and cloud emissivity are associated with changes in PM 2.5 concentration and composition, and the changes differ by overpass time and cloud phase as well as between the San Francisco and Atlanta sites. A case-study at the San Francisco site confirmed that accounting for cloud-cover and associated meteorological conditions could substantially alter the spatial distribution of monthly ground-level PM 2.5 concentrations.
Development of global model for atmospheric backscatter at CO2 wavelengths
NASA Technical Reports Server (NTRS)
Kent, G. S.; Wang, P. H.; Farrukh, U.; Deepak, A.; Patterson, E. M.
1985-01-01
The improvement of an understanding of the variation of the aerosol backscattering at 10.6 micron within the free troposphere and the development model to describe this was undertaken. The analysis combines theoretical modeling with the results contained within three independent data sets. The data sets are obtained by the SAGE I/SAM II satellite experiments, the GAMETAG flight series and by direct backscatter measurements. The theoretical work includes use of a bimodal, two component aerosol model, and the study of the microphysical and associated optical changes occurring within an aerosol plume. A consistent picture is obtained, which describes the variation of the aerosol backscattering function in the free troposphere with altitude, latitude, and season. Most data are available and greatest consistency is found inside the Northern Hemisphere.
NASA Astrophysics Data System (ADS)
Miyazaki, Yuzo; Kawamura, Kimitaka; Sawano, Maki
2010-12-01
Size-segregated aerosol samples were collected over the western North Pacific in summer 2008 to investigate marine biological contribution to organic aerosols. The samples were analyzed for organic carbon (OC), water-soluble organic carbon (WSOC), and water-soluble organic compounds including diacids (C2-C9), ω-oxocarboxylic acids, and α-dicarbonyls as well as methanesulfonic acid (MSA). The average concentrations of OC and oxalic acid (C2) were approximately two to three times larger in marine biologically more influenced aerosols, defined by the concentrations of MSA and azelaic acid (C9), than in less influenced aerosols. WSOC, which showed a statistically significant correlation with MSA, accounted for 15-21% of total mass of the components determined in the submicrometer range of biologically more influenced aerosols. These values are comparable to those of water-insoluble organic carbon (WIOC) (˜14-23%), suggesting that organic aerosols in this region are enriched in secondary organic aerosols (SOA) linked to oceanic biological activity. In these aerosols, substantial fractions of C2-C4 diacids were found in the submicrometer size range. Positive correlations of oxalic acid with C3-C5 diacids and glyoxylic acid suggest that secondary production of oxalic acid occurs possibly in the aqueous aerosol phase via the oxidation of longer-chain diacids and glyoxylic acid in the oceanic region with higher biological productivity. We found similar concentration levels and size distributions of methylglyoxal between the two types of aerosols, suggesting that formation of oxalic acid via the oxidation of methylglyoxal from marine isoprene is insignificant in the study region.
Aerosols in atmospheric chemistry and biogeochemical cycles of nutrients
NASA Astrophysics Data System (ADS)
Kanakidou, Maria; Myriokefalitakis, Stelios; Tsigaridis, Kostas
2018-06-01
Atmospheric aerosols have complex and variable compositions and properties. While scientific interest is centered on the health and climatic effects of atmospheric aerosols, insufficient attention is given to their involvement in multiphase chemistry that alters their contribution as carriers of nutrients in ecosystems. However, there is experimental proof that the nutrient equilibria of both land and marine ecosystems have been disturbed during the Anthropocene period. This review study first summarizes our current understanding of aerosol chemical processing in the atmosphere as relevant to biogeochemical cycles. Then it binds together results of recent modeling studies based on laboratory and field experiments, focusing on the organic and dust components of aerosols that account for multiphase chemistry, aerosol ageing in the atmosphere, nutrient (N, P, Fe) emissions, atmospheric transport, transformation and deposition. The human-driven contribution to atmospheric deposition of these nutrients, derived by global simulations using past and future anthropogenic emissions of pollutants, is put into perspective with regard to potential changes in nutrient limitations and biodiversity. Atmospheric deposition of nutrients has been suggested to result in human-induced ecosystem limitations with regard to specific nutrients. Such modifications favor the development of certain species against others and affect the overall functioning of ecosystems. Organic forms of nutrients are found to contribute to the atmospheric deposition of the nutrients N, P and Fe by 20%–40%, 35%–45% and 7%–18%, respectively. These have the potential to be key components of the biogeochemical cycles since there is initial proof of their bioavailability to ecosystems. Bioaerosols have been found to make a significant contribution to atmospheric sources of N and P, indicating potentially significant interactions between terrestrial and marine ecosystems. These results deserve further experimental and modeling studies to reduce uncertainties and understand the feedbacks induced by atmospheric deposition of nutrients to ecosystems.
SAS program for quantitative stratigraphic correlation by principal components
Hohn, M.E.
1985-01-01
A SAS program is presented which constructs a composite section of stratigraphic events through principal components analysis. The variables in the analysis are stratigraphic sections and the observational units are range limits of taxa. The program standardizes data in each section, extracts eigenvectors, estimates missing range limits, and computes the composite section from scores of events on the first principal component. Provided is an option of several types of diagnostic plots; these help one to determine conservative range limits or unrealistic estimates of missing values. Inspection of the graphs and eigenvalues allow one to evaluate goodness of fit between the composite and measured data. The program is extended easily to the creation of a rank-order composite. ?? 1985.
Intercontinental Transport of Aerosols: Implication for Regional Air Quality
NASA Technical Reports Server (NTRS)
Chin, Mian; Diehl, Thomas; Ginoux, Paul
2006-01-01
Aerosol particles, also known as PM2.5 (particle diameter less than 2.5 microns) and PM10 (particle diameter less than 10 microns), is one of the key atmospheric components that determine ambient air quality. Current US air quality standards for PM10 (particles with diameter < 10 microns) and PM2.5 (particles with diameter 2.5 microns) are 50 pg/cu m and 15 pg/cu m, respectively. While local and regional emission sources are the main cause of air pollution problems, aerosols can be transported on a hemispheric or global scale. In this study, we use the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to quantify contributions of long-range transport vs. local/regional pollution sources and from natural vs. anthropogenic sources to PM concentrations different regions. In particular, we estimate the hemispheric impact of anthropogenic sulfate aerosols and dust from major source areas on other regions in the world. The GOCART model results are compared with satellite remote sensing and ground-based network measurements of aerosol optical depth and concentrations.
Guilmette, Raymond A; Cheng, Yung Sung
2009-03-01
As part of the Capstone Depleted Uranium (DU) Aerosol Study, the solubility of selected aerosol samples was measured using an accepted in vitro dissolution test system. This static system was employed along with a SUF (synthetic ultrafiltrate) solvent, which is designed to mimic the physiological chemistry of extracellular fluid. Using sequentially obtained solvent samples, the dissolution behavior over a 46-d test period was evaluated by fitting the measurement data to two- or three-component negative exponential functions. These functions were then compared with Type M and S absorption taken from the International Commission on Radiological Protection Publication 66 Human Respiratory Tract Model. The results indicated that there was a substantial variability in solubility of the aerosols, which in part depended on the type of armor being impacted by the DU penetrator and the particle size fraction being tested. Although some trends were suggested, the variability noted leads to uncertainties in predicting the solubility of other DU-based aerosols. Nevertheless, these data provide a useful experimental basis for modeling the intake-dose relationships for inhaled DU aerosols arising from penetrator impact on armored vehicles.
NASA Astrophysics Data System (ADS)
Bruehl, C.; Schallock, J.; Lelieveld, J.; Bingen, C.; Robert, C. E.; Hoepfner, M.; Clarisse, L.
2017-12-01
The atmospheric chemistry - general circulation model EMAC with a modal interactive aerosol module is used to estimate radiative effects of UTLS aerosol for the ENVISAT period 2002 to 2012 in the framework of SPARC/SSIRC. Volcanic SO2 injections by about 230 explosive volcano eruptions are estimated mostly from MIPAS limb observations. For periods of data gaps, injected SO2 is estimated indirectly from extinctions observed by GOMOS. GOMOS extinctions in the UTLS and the seasonal component of radiative forcing can be only reproduced by the model if a comprehensive treatment of desert dust and organic and black carbon is included. Upward transport of particles and gases by the Asian Monsoon appears to contribute importantly. The time series of simulated stratospheric aerosol optical depth and radiative forcing agree with the corresponding quantities derived from different satellite data sets. Comparisons of total aerosol optical depth with IASI show that tropospheric and stratospheric aerosol in the model are consistently and realistically represented.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Liu, Jun; Dedrick, Jeramy; Russell, Lynn M.
Observations of the organic components of the natural aerosol are scarce in Antarctica, which limits our understanding of natural aerosols and their connection to seasonal and spatial patterns of cloud albedo in the region. From November 2015 to December 2016, the ARM West Antarctic Radiation Experiment (AWARE) measured submicron aerosol properties near McMurdo Station at the southern tip of Ross Island. Submicron organic mass (OM), particle number, and cloud condensation nuclei concentrations were higher in summer than other seasons. The measurements included a range of compositions and concentrations that likely reflected both local anthropogenic emissions and natural background sources. We isolated themore » natural organic components by separating a natural factor and a local combustion factor. The natural OM was 150 times higher in summer than in winter. The local anthropogenic emissions were not hygroscopic and had little contribution to the CCN concentrations. Natural sources that included marine sea spray and seabird emissions contributed 56 % OM in summer but only 3 % in winter. The natural OM had high hydroxyl group fraction (55 %), 6 % alkane, and 6 % amine group mass, consistent with marine organic composition. In addition, the Fourier transform infrared (FTIR) spectra showed the natural sources of organic aerosol were characterized by amide group absorption, which may be from seabird populations. Finally, carboxylic acid group contributions were high in summer and associated with natural sources, likely forming by secondary reactions.« less
NASA Astrophysics Data System (ADS)
Disselkamp, R. S.; Barrie, L. A.; Shutthanadan, S.; Cliff, S.; Cahill, T.
2001-12-01
In mid-August, 2001, an aircraft-based air-quality study was performed in the Puget Sound, WA, area entitled PNW2001 (http://www.pnl.gov/pnw2001). The objectives of this field campaign were the following: 1. reveal information about the 3-dimensional distribution of ozone, its gaseous precursors and fine particulate matter during weather conditions favoring air pollution; 2. derive information about the accuracy of urban and biogenic emissions inventories that are used to drive the air quality forecast models; and 3. examine the accuracy of modeled ozone concentration with that observed. In support of these efforts, we collected time-averaged ( { ~}10 minute averages), size-segregated, aerosol composition and mass-loading information using ex post facto analysis techniques of synchrotron x-ray fluorescence (s-XRF), proton induced x-ray emissions(PIXE), proton elastic scattering (PESA), and scanning transmission ion microscopy (STIM). This is the first time these analysis techniques have been used together on samples collected from aircraft using an optimized 3-stage rotating drum impactor. In our presentation, we will discuss the aerosol components in three aerosol size fractions as identified by statistical analysis of multielemental data (including total mass, H, Na, Mg, Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Pb) and relate variations in these components to physical aerosol properties, other gaseous trace constituents and to air mass origin.
Liu, Jun; Dedrick, Jeramy; Russell, Lynn M.; ...
2018-01-18
Observations of the organic components of the natural aerosol are scarce in Antarctica, which limits our understanding of natural aerosols and their connection to seasonal and spatial patterns of cloud albedo in the region. From November 2015 to December 2016, the ARM West Antarctic Radiation Experiment (AWARE) measured submicron aerosol properties near McMurdo Station at the southern tip of Ross Island. Submicron organic mass (OM), particle number, and cloud condensation nuclei concentrations were higher in summer than other seasons. The measurements included a range of compositions and concentrations that likely reflected both local anthropogenic emissions and natural background sources. We isolated themore » natural organic components by separating a natural factor and a local combustion factor. The natural OM was 150 times higher in summer than in winter. The local anthropogenic emissions were not hygroscopic and had little contribution to the CCN concentrations. Natural sources that included marine sea spray and seabird emissions contributed 56 % OM in summer but only 3 % in winter. The natural OM had high hydroxyl group fraction (55 %), 6 % alkane, and 6 % amine group mass, consistent with marine organic composition. In addition, the Fourier transform infrared (FTIR) spectra showed the natural sources of organic aerosol were characterized by amide group absorption, which may be from seabird populations. Finally, carboxylic acid group contributions were high in summer and associated with natural sources, likely forming by secondary reactions.« less
Electronic cigarettes: product characterisation and design considerations.
Brown, Christopher J; Cheng, James M
2014-05-01
To review the available evidence regarding electronic cigarette (e-cigarette) product characterisation and design features in order to understand their potential impact on individual users and on public health. Systematic literature searches in 10 reference databases were conducted through October 2013. A total of 14 articles and documents and 16 patents were included in this analysis. Numerous disposable and reusable e-cigarette product options exist, representing wide variation in product configuration and component functionality. Common e-cigarette components include an aerosol generator, a flow sensor, a battery and a nicotine-containing solution storage area. e-cigarettes currently include many interchangeable parts, enabling users to modify the character of the delivered aerosol and, therefore, the product's 'effectiveness' as a nicotine delivery product. Materials in e-cigarettes may include metals, rubber and ceramics. Some materials may be aerosolised and have adverse health effects. Several studies have described significant performance variability across and within e-cigarette brands. Patent applications include novel product features designed to influence aerosol properties and e-cigarette efficiency at delivering nicotine. Although e-cigarettes share a basic design, engineering variations and user modifications result in differences in nicotine delivery and potential product risks. e-cigarette aerosols may include harmful and potentially harmful constituents. Battery explosions and the risks of exposure to the e-liquid (especially for children) are also concerns. Additional research will enhance the current understanding of basic e-cigarette design and operation, aerosol production and processing, and functionality. A standardised e-cigarette testing regime should be developed to allow product comparisons.
NASA Astrophysics Data System (ADS)
Khoder, M. I.; Hassan, S. K.
Weekday and weekend ambient aerosol samples were collected from the city centre of Cairo, namely "Ramsis" during the summer season of the year 2006, and have been analyzed for water-soluble ionic species. The average concentrations of the total suspended particulate matter (TSP) and their water-soluble components were higher during weekdays than on weekends, indicating that the decreased traffic density on weekends leads to a decrease in the levels of the TSP and their water-soluble ionic species. The average concentrations of the TSP were 454 μg m -3 on weekdays and 298 μg m -3 on weekends. The weekday/weekend concentration ratios were 1.52 for TSP, 1.27 for SO 42-, 1.64 for Cl -, 1.54 for NO 3-, 1.17 for NH 4+, 1.67 for Ca 2+, 1.83 for Na +, 1.75 for K + and 1.73 for Mg 2+. City centre of Cairo has high levels of the TSP and their water-soluble ionic species compared with many polluted cities in the world. Among all of the measured water-soluble components, SO 42- was the most abundant species followed by Ca 2+ on weekdays and weekends. The average mass ratios of NO 3-/SO 42- in the TSP were 0.41 on weekdays and 0.34 on weekends, suggesting that the stationary source emissions were more predominant. The NH 4+/SO 42- molar ratios and its relation with the concentrations of TSP and Ca 2+ during the weekdays and weekends indicate that the chemical form of sulfate and ammonium in aerosol particles varies with TSP and Ca 2+ levels. At high TSP and Ca 2+ levels, and NH 4+/SO 42- molar ratios less than one, SO 42- in aerosol particles may be present as CaSO 4 and (NH 4) 2SO 4·CaSO 4·2H 2O, whereas it is expected to be present as (NH 4) 2SO 4, (NH 4) 2SO 4·CaSO 4·2H 2O and CaSO 4 at low levels of TSP and Ca 2+, and NH 4+/SO 42- molar ratios between 1 and 2. The mean pH values of the TSP were 7.65 on weekdays and 6.97 on weekends, indicating that aerosol particles brought a large amount of crustal species, and might alleviate the tendency of acidification. The relationships between the concentrations of acidic components (NO 3- and SO 42-) and basic components (NH 4+, Ca 2+ and Mg 2+) on weekdays and weekends indicate that the acidity of aerosol particles is neutralized. Ca 2+ and NH 4+ are the most dominant neutralization substances in Cairo atmosphere.
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 (r = 0.53-0.75, p < 0.01) between LO-OOA and odd oxygen (Ox = O3 + NO2), and between MO-OOA and liquid water content in aerosols. BBOA was resolved in spring and autumn, influenced by agricultural biomass burning (e.g., field preparation burnings, straw burning after the harvest). CCOA was only identified in winter due to domestic heating. These results signified that the comprehensive management for biomass burning and coal combustion emissions is needed. High concentrations of chemical components in PM1 in Beijing, especially in winter or in adverse meteorological conditions, suggest that further strengthening the regional emission control of primary particulate and precursors of secondary species is expected.
Cloud Condensation Nuclei Measurements During the First Year of the ORACLES Study
NASA Astrophysics Data System (ADS)
Kacarab, M.; Howell, S. G.; Wood, R.; Redemann, J.; Nenes, A.
2016-12-01
Aerosols have significant impacts on air quality and climate. Their ability to scatter and absorb radiation and to act as cloud condensation nuclei (CCN) plays a very important role in the global climate. Biomass burning organic aerosol (BBOA) can drastically elevate the concentration of CCN in clouds, but the response in droplet number may be strongly suppressed (or even reversed) owing to low supersaturations that may develop from the strong competition of water vapor (Bougiatioti et al. 2016). Understanding and constraining the magnitude of droplet response to biomass burning plumes is an important component of the aerosol-cloud interaction problem. The southeastern Atlantic (SEA) cloud deck provides a unique opportunity to study these cloud-BBOA interactions for marine stratocumulus, as it is overlain by a large, optically thick biomass burning aerosol plume from Southern Africa during the burning season. The interaction between these biomass burning aerosols and the SEA cloud deck is being investigated in the NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) study. The CCN activity of aerosol around the SEA cloud deck and associated biomass burning plume was evaluated during the first year of the ORACLES study with direct measurements of CCN concentration, aerosol size distribution and composition onboard the NASA P-3 aircraft during August and September of 2016. Here we present analysis of the observed CCN activity of the BBOA aerosol in and around the SEA cloud deck and its relationship to aerosol size, chemical composition, and plume mixing and aging. We also evaluate the predicted and observed droplet number sensitivity to the aerosol fluctuations and quantify, using the data, the drivers of droplet number variability (vertical velocity or aerosol properties) as a function of biomass burning plume characteristics.
NASA Technical Reports Server (NTRS)
Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.
2017-01-01
The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.
NASA Astrophysics Data System (ADS)
Khaykin, Sergey M.; Godin-Beekmann, Sophie; Keckhut, Philippe; Hauchecorne, Alain; Jumelet, Julien; Vernier, Jean-Paul; Bourassa, Adam; Degenstein, Doug A.; Rieger, Landon A.; Bingen, Christine; Vanhellemont, Filip; Robert, Charles; DeLand, Matthew; Bhartia, Pawan K.
2017-02-01
The article presents new high-quality continuous stratospheric aerosol observations spanning 1994-2015 at the French Observatoire de Haute-Provence (OHP, 44° N, 6° E) obtained by two independent, regularly maintained lidar systems operating within the Network for Detection of Atmospheric Composition Change (NDACC). Lidar series are compared with global-coverage observations by Stratospheric Aerosol and Gas Experiment (SAGE II), Global Ozone Monitoring by Occultation of Stars (GOMOS), Optical Spectrograph and InfraRed Imaging System (OSIRIS), Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and Ozone Mapping Profiling Suite (OMPS) satellite instruments, altogether covering the time span of OHP lidar measurements. Local OHP and zonal-mean satellite series of stratospheric aerosol optical depth are in excellent agreement, allowing for accurate characterization of stratospheric aerosol evolution and variability at northern midlatitudes during the last 2 decades. The combination of local and global observations is used for a careful separation between volcanically perturbed and quiescent periods. While the volcanic signatures dominate the stratospheric aerosol record, the background aerosol abundance is found to be modulated remotely by the poleward transport of convectively cleansed air from the deep tropics and aerosol-laden air from the Asian monsoon region. The annual cycle of background aerosol at midlatitudes, featuring a minimum during late spring and a maximum during late summer, correlates with that of water vapor from the Aura Microwave Limb Sounder (MLS). Observations covering two volcanically quiescent periods over the last 2 decades provide an indication of a growth in the nonvolcanic component of stratospheric aerosol. A statistically significant factor of 2 increase in nonvolcanic aerosol since 1998, seasonally restricted to late summer and fall, is associated with the influence of the Asian monsoon and growing pollution therein.
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.
Marine Stratocumulus Properties from the FPDR - PDI as a Function of Aerosol during ORACLES
NASA Astrophysics Data System (ADS)
Small Griswold, J. D.; Heikkila, A.
2016-12-01
Aerosol-cloud interactions in the southeastern Atlantic (SEA) region were investigated during year 1 of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field project in Aug-Sept 2016. This region is of interest due to seasonally persistent marine stratocumulus cloud decks that are an important component of the climate system due to their radiative and hydrologic impacts. The SEA deck is unique due to the interactions between these clouds and transported biomass burning aerosol during the July-October fire season. These biomass burning aerosol play multiple roles in modifying the cloud deck through interactions with radiation as absorbing aerosol and through modifications to cloud microphysical properties as cloud condensation nuclei. This work uses in situcloud data obtained with a Flight Probe Dual Range - Phase Doppler Interferometer (FPDR - PDI), standard aerosol instrumentation on board the NASA P-3, and reanalysis data to investigate Aerosol-Cloud Interactions (ACI). The FPDR - PDI provides unique cloud microphysical observations of individual cloud drop arrivals allowing for the computation of a variety of microphysical cloud properties including individual drop size, cloud drop number concentration, cloud drop size distributions, liquid water content, and cloud thickness. The FPDR - PDI measurement technique also provides droplet spacing and drop velocity information which is used to investigate turbulence and entrainment mixing processes. We use aerosol information such as average background aerosol amount (low, mid, high) and location relative to cloud (above or mixing) to sort FPDR - PDI cloud properties. To control for meteorological co-variances we further sort the data within aerosol categories by lower tropospheric stability, vertical velocity, and surface wind direction. We then determine general marine stratocumulus cloud characteristics under each of the various aerosol categories to investigate ACI in the SEA.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dzepina, K.; Mazzoleni, C.; Fialho, P.
Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.« less
Dzepina, K.; Mazzoleni, C.; Fialho, P.; ...
2015-05-05
Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m -3. On average, organic aerosol components represent the largest mass fraction of the totalmore » measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100–1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.« less
NASA Astrophysics Data System (ADS)
Dzepina, K.; Mazzoleni, C.; Fialho, P.; China, S.; Zhang, B.; Owen, R. C.; Helmig, D.; Hueber, J.; Kumar, S.; Perlinger, J. A.; Kramer, L. J.; Dziobak, M. P.; Ampadu, M. T.; Olsen, S.; Wuebbles, D. J.; Mazzoleni, L. R.
2015-05-01
Free tropospheric aerosol was sampled at the Pico Mountain Observatory located at 2225 m above mean sea level on Pico Island of the Azores archipelago in the North Atlantic. The observatory is located ~ 3900 km east and downwind of North America, which enables studies of free tropospheric air transported over long distances. Aerosol samples collected on filters from June to October 2012 were analyzed to characterize organic carbon, elemental carbon, and inorganic ions. The average ambient concentration of aerosol was 0.9 ± 0.7 μg m-3. On average, organic aerosol components represent the largest mass fraction of the total measured aerosol (60 ± 51%), followed by sulfate (23 ± 28%), nitrate (13 ± 10%), chloride (2 ± 3%), and elemental carbon (2 ± 2%). Water-soluble organic matter (WSOM) extracted from two aerosol samples (9/24 and 9/25) collected consecutively during a pollution event were analyzed using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. Approximately 4000 molecular formulas were assigned to each of the mass spectra in the range of m/z 100-1000. The majority of the assigned molecular formulas had unsaturated structures with CHO and CHNO elemental compositions. FLEXPART retroplume analyses showed the sampled air masses were very aged (average plume age > 12 days). These aged aerosol WSOM compounds had an average O/C ratio of ~ 0.45, which is relatively low compared to O/C ratios of other aged aerosol. The increase in aerosol loading during the measurement period of 9/24 was linked to biomass burning emissions from North America by FLEXPART retroplume analysis and Moderate Resolution Imaging Spectroradiometer (MODIS) fire counts. This was confirmed with biomass burning markers detected in the WSOM and with the morphology and mixing state of particles as determined by scanning electron microscopy. The presence of markers characteristic of aqueous-phase reactions of phenolic species suggests that the aerosol collected at the Pico Mountain Observatory had undergone cloud processing before reaching the site. Finally, the air masses of 9/25 were more aged and influenced by marine emissions, as indicated by the presence of organosulfates and other species characteristic of marine aerosol. The change in the air masses for the two samples was corroborated by the changes in ethane, propane, and ozone, morphology of particles, as well as by the FLEXPART retroplume simulations. This paper presents the first detailed molecular characterization of free tropospheric aged aerosol intercepted at a lower free troposphere remote location and provides evidence of low oxygenation after long-range transport. We hypothesize this is a result of the selective removal of highly aged and polar species during long-range transport, because the aerosol underwent a combination of atmospheric processes during transport facilitating aqueous-phase removal (e.g., clouds processing) and fragmentation (e.g., photolysis) of components.
Kumar, V; Chandra, B P; Sinha, V
2018-01-12
Biomass fires impact global atmospheric chemistry. The reactive compounds emitted and formed due to biomass fires drive ozone and organic aerosol formation, affecting both air quality and climate. Direct hydroxyl (OH) Reactivity measurements quantify total gaseous reactive pollutant loadings and comparison with measured compounds yields the fraction of unmeasured compounds. Here, we quantified the magnitude and composition of total OH reactivity in the north-west Indo-Gangetic Plain. More than 120% increase occurred in total OH reactivity (28 s -1 to 64 s -1 ) and from no missing OH reactivity in the normal summertime air, the missing OH reactivity fraction increased to ~40 % in the post-harvest summertime period influenced by large scale biomass fires highlighting presence of unmeasured compounds. Increased missing OH reactivity between the two summertime periods was associated with increased concentrations of compounds with strong photochemical source such as acetaldehyde, acetone, hydroxyacetone, nitromethane, amides, isocyanic acid and primary emissions of acetonitrile and aromatic compounds. Currently even the most detailed state-of-the art atmospheric chemistry models exclude formamide, acetamide, nitromethane and isocyanic acid and their highly reactive precursor alkylamines (e.g. methylamine, ethylamine, dimethylamine, trimethylamine). For improved understanding of atmospheric chemistry-air quality-climate feedbacks in biomass-fire impacted atmospheric environments, future studies should include these compounds.
Actinic Flux Calculations: A Model Sensitivity Study
NASA Technical Reports Server (NTRS)
Krotkov, Nickolay A.; Flittner, D.; Ahmad, Z.; Herman, J. R.; Einaudi, Franco (Technical Monitor)
2000-01-01
calculate direct and diffuse surface irradiance and actinic flux (downwelling (2p) and total (4p)) for the reference model. Sensitivity analysis has shown that the accuracy of the radiative transfer flux calculations for a unit ETS (i.e. atmospheric transmittance) together with a numerical interpolation technique for the constituents' vertical profiles is better than 1% for SZA less than 70(sub o) and wavelengths longer than 310 nm. The differences increase for shorter wavelengths and larger SZA, due to the differences in pseudo-spherical correction techniques and vertical discretetization among the codes. Our sensitivity study includes variation of ozone cross-sections, ETS spectra and the effects of wavelength shifts between vacuum and air scales. We also investigate the effects of aerosols on the spectral flux components in the UV and visible spectral regions. The "aerosol correction factors" (ACFs) were calculated at discrete wavelengths and different SZAs for each flux component (direct, diffuse, reflected) and prescribed IPMMI aerosol parameters. Finally, the sensitivity study was extended to calculation of selected photolysis rates coefficients.
NASA Astrophysics Data System (ADS)
Schmidt, Susan; Schneider, Johannes; Thomas, Klimach; Stephan, Mertes; Ludwig, Schenk; Udo, Kästner; Frank, Stratmann; Joachim, Curtius; Piotr, Kupiszewski; Ernest, Weingartner; Emanuel, Hammer; Paul, Vochezer; Martin, Schnaiter; Stephan, Borrmann
2014-05-01
In the framework of the DFG (deutsche Forschungsgemeinschaft)-funded research unit INUIT (Ice Nuclei research UnIT) a field campaign at the High Alpine Research Station Jungfraujoch (JFJ, Swiss Alps, Sphinx Laboratory, 3580 m asl; 7°59'2''E, 46°32'53''N) took place in January/February 2013 (INUIT-JFJ 2013). The goal of the measurements was to investigate the chemical composition of ice particle residues (IPR) in ambient air as well as the background aerosol particles. Previous investigations conducted at the JFJ showed that particles consisting of mineral components dominate the ice particle residue number (Kamphus et al., 2008) but also particles consisting of black carbon were found to be enriched in IPR (Mertes et al., 2007; Cozic et al., 2008). Cziczo et al. find out that lead as well is a good ice nucleus and was measured in IPR at previous measurements at the JFJ. During INUIT-JFJ 2013, the IPR were sampled out of mixed-phase clouds by an Ice-CVI (Ice Counterflow Virtual Impactor, Mertes et al., 2007) and an ISI (Ice Selective Inlet, Kupiszewski et al., 2013) and analyzed by the single particle mass spectrometer ALABAMA (Aircraft-based Laser Ablation Aerosol Mass Spectrometer; Brands et al., 2011). Additionally, the ALABAMA was connected to a total aerosol-inlet to investigate the chemical composition of background aerosol particles. During 217 hours of background aerosol measurements we analyzed more than 27000 aerosol particles, which consisted mainly of pure organic components or organics mixed with ammonium, metals or mineral components. During six cloud events with approximately 63 h measurement time we detected 162 IPR sampled by the Ice-CVI. The main part of these IPR were also composed of organic material mixed with other chemical compounds. Additionally, we found particles which consisted of mineral components (approximately 23 %). Sampling mixed-phase cloud through the ISI we measured during four cloud events 34 ice residues in approximately 30 h measurement time. The main part of the chemical compounds of these IPR were also organic material mixed with metals or with mineral compounds. We also found a smaller part of particles which consisted of pure mineral components (about 48 %). Lead was also found in the IPR measured behind Ice-CVI (~14 %) as well as in the background aerosol (~0.04 %). Black carbon particles were only found in the background aerosol. Because of the topography of the JFJ, air masses can reach the station only from the northwestern or southeastern direction (Hammer et al., 2013). Back trajectory calculations show that during our measurements the air masses were dominated mainly by long-distance transport from North America over Great Britain and France. This may explain the lower abundance of mineral dust in the ice residues compared to the previous studies. Brands, M., Kamphus, M., Böttger, T., Schneider, J., Drewnick, F., Roth, A., Curtius, J., Voigt, C., Borbon, A., Beekmann, M., Bourdon, A., Perrin, T. and Borrmann, S. (2011) Aerosol Sci. Technol., 45, 46-64. Cozic, J., Mertes, S., Verheggen, B., Cziczo, D. J., Gallavardin, S. J., Walter, S., Baltensperger, U. and Weingartner, E. (2008) J. Geophys. Res.-Atmos., 113, D15209. Cziczo, D. J., Stetzer. O., Worringen, A., Ebert, M., Weinbruch, S., Kamphus, M., Gallavardin, S. J., Curtius, J., Borrmann, S., Froyd, K. D., Mertes, S., Möhler, O., Lohmann, U. (2009) Nature Geoscience, 2, 333-336 Hammer, E., Bukowiecki, N., Gysel, M., Jurányi, Z., Hoyle, C. R., Vogt, R., Baltensperger, U. and Weingartner, E. (2013) Atmos. Chem. Phys. Discuss., 13, 20419-20462 Kamphus, M., Ettner-Mahl, M., Klimach, T., Drewnick, F, Keller, L., Cziczo, D. J., Mertes, S., Borrmann, S. and Curtius1, J. (2010) Atmos. Chem. Phys., 10, 8077-8095. Kupiszewski, P., Weingartner, E., Färber, R., Gysel, M., Hammer, E., Fuchs, C., Baltensperger, U., Vochezer, P., Schnaiter, M., Linke, C., Toprak, E., Mertes, S., Schneider, J., Schmidt, S. (2013) European Aerosol Conference, Prague. Mertes, S., Verheggen, B., Walter,S., Connolly,P., Ebert, M., Schneider, J., Bower, K. N., Cozic, J., Weinbruch, S., Baltensperger, U. and Weingartner, E. (2007) Aerosol Sci. Technol., 41, 848-864.
International Space Station (ISS)
2001-08-18
Astronaut Patrick G. Forrester works with the the Materials International Space Station Experiment (MISSE) during extravehicular activity (EVA). MISSE would expose 750 material samples for about 18 months and collect information on how different materials weather the space environment The objective of MISSE is to develop early, low-cost, non-intrusive opportunities to conduct critical space exposure tests of space materials and components plarned for use on future spacecraft. The experiment was the first externally mounted experiment conducted on the International Space Station (ISS) and was installed on the outside of the ISS Quest Airlock. MISSE was launched on August 10, 2001 aboard the Space Shuttle Orbiter Discovery.
NASA Astrophysics Data System (ADS)
Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.
2013-10-01
This study investigates the contribution of potential sources to the submicron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). A total of 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by gas chromatography-mass spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by multivariate curve resolution-alternating least squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin and three of secondary OA origin, while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (urban primary organic aerosol, or POA Urban), mainly traffic emissions but also cigarette smoke, contributed 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA at RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation (REG.). Three secondary organic aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO) - i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols - showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, or 16% and 7%, at UB and RS, respectively). By contrast, a SOA biogenic component attributed to α-pinene oxidation (SOA BIO PIN) presented average concentrations of 0.5 μg m-3 at UB (24% of OA) and 0.2 μg m-3 at RS (7%), respectively, suggesting that this SOA component did not impact the two monitoring sites at the same level. A clear anti-correlation was observed between SOA ISO and SOA PIN during nucleation days, surprisingly suggesting that some of the growth of urban freshly nucleating particles may be driven by biogenic α-pinene oxidation products but inhibited by isoprene organic compounds. A third SOA component was formed by a mixture of aged anthropogenic and biogenic secondary organic compounds (SOA Aged) that accumulated under stagnant atmospheric conditions, contributing for 12% to OA at RS (0.4 μg OC m-3) and for 18% at UB (0.4 μg OC m-3). A sixth component, formed by C7-C9 dicarboxylic acids and detected especially during daytime, was called "urban oxygenated organic aerosol" (OOA Urban) due to its high abundance at urban RS (23%; 0.8 μg OCm-3) vs. UB (10%; 0.2 μg OCm-3), with a well-defined daytime maximum. This temporal trend and geographical differentiation suggests that local anthropogenic sources were determining this component. However, the changes of these organic molecules were also influenced by the air mass trajectories, indicating that atmospheric conditions have an influence on this component, although the specific origin on this component remains unclear. It points to a secondary organic component driven by primary urban sources including cooking and traffic (mainly gasoline) activities.
NASA Astrophysics Data System (ADS)
Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.
2013-04-01
This study investigates the contribution of potential sources to the sub-micron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by Gas Chromatography-Mass Spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by Multivariate Curve Resolution-Alternating Least Squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin, three of secondary OA origin while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (Urban primary organic aerosol, Urban POA) contributed for 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA in RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation. Three Secondary Organic Aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO), i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols, showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, 16% and 7%, at UB and RS, respectively). By contrast, a SOA biogenic component attributed to α-pinene oxidation (SOA BIO PIN) presented average concentrations of 0.5 μg m-3 at UB (24% of OA) and 0.2 μg m-3 at RS (7%), respectively, suggesting that this SOA component did not impact the two monitoring site at the same level. A clear anti correlation was observed between SOA ISO and SOA PIN during nucleation days, surprisingly suggesting that some of the growth of urban freshly nucleating particles may be driven by biogenic α-pinene oxidation products but inhibited by isoprene organic compounds. A third SOA component was formed by a mixture of aged anthropogenic and biogenic secondary organic compounds (Aged SOA) that accumulated under stagnant atmospheric conditions, contributing for 12% to OA at RS (0.4 μg OC m-3) and for 18% at UB (0.4 μg OC m-3). A sixth component, formed by C7-C9 dicarboxylic acids and detected especially during daytime, was called "urban oxygenated organic aerosol" (Urban OOA) due to its high abundance in urban RS (23%; 0.8 μg OC m-3) vs. UB (10%; 0.2 μg OC m-3), with a well-defined daytime maximum. This temporal trend and geographical differentiation suggests that local anthropogenic sources were determining this component. However, the changes of these organic molecules were also influenced by the air mass trajectories, indicating that atmospheric conditions had an influence on this component although the specific origin on this component remains unclear. It points to a secondary organic component driven by primary urban sources including cooking and traffic (mainly gasoline) activities.
NASA Astrophysics Data System (ADS)
Tsimpidi, A. P.; Karydis, V. A.; Zavala, M.; Lei, W.; Molina, L. T.; Pandis, S. N.
2007-05-01
Atmospheric aerosols have adverse effects on human health, contribute to the visibility reduction and influence the energy balance of the planet. A three-dimensional chemical transport model (PMCAMx) (Gaydos et al., 2007) is used to simulate the particular matter (PM) mass composition distribution in the Mexico City Metropolitan Area (MCMA). PMCAMx uses the framework of CAMx (ENVIRON, 2002) modelling the processes of horizontal and vertical advection, horizontal and vertical dispersion, wet and dry deposition, and gas-phase chemistry. In addition to the above, PMCAMx includes three detailed aerosol modules: inorganic aerosol growth (Gaydos et al., 2003; Koo et al., 2003a), aqueous-phase chemistry (Fahey and Pandis, 2001), and secondary organic aerosol formation and growth (Koo et al., 2004). The aerosol thermodynamic model ISORROPIA has been improved as it now simulates explicitly the chemistry of Ca, Mg, and K salts and is linked to PMCAMx. The hybrid approach (Koo et al., 2003b) for modelling aerosol dynamics is applied in order to accurately simulate the inorganic components in coarse mode. This approach assumes that the smallest particles are in equilibrium while the condensation/evaporation equation is solved for the larger ones. The new CMU organic aerosol model, which is based on the splitting of the organic aerosol volatility range in discrete bins, is also used. The model predictions are evaluated against the PM and vapour concentration measurements from the MCMA-2003 Campaign (Molina et al., 2007). References Gaydos, T., Pinder, R., Koo, B., Fahey, Κ., Yarwood, G., and Pandis, S. N., (2007). Development and application of a three-dimensional Chemical Transport Model, PMCAMx. Atmospheric Environment, in press. ENVIRON (2002). User's guide to the comprehensive air quality model with extensions (CAMx). Version 3.10. Report prepared by ENVIRON International corporation, Novato, CA Gaydos, T., Koo, B., and Pandis, S. N., (2003). Development and application of an efficient moving sectional approach for the solution of the atmospheric aerosol condensation/evaporation equations. Atmospheric Environment, 37, 3303-3316. Fahey, K. and Pandis, S. N., (2001). Optimizing model performance: variable size resolution in cloud chemistry modelling. Atmospheric Environment 35, 4471-4478. Koo, B., Pandis S. N., and Ansari, A. (2003a). Integrated approaches to modelling the organic and inorganic atmospheric aerosol components. Atmospheric Environment, 37, 4757-4768. Koo, B., Gaydos, T.M., Pandis, S.N., (2003b). Evaluation of the equilibrium, hybrid, and dynamic aerosol modeling approaches. Aerosol Science and Technology 37, 53-64 Molina, L.T., Kolb, C.E., de Foy, B., Lamb, B., Brune, W., Molina, M.J., (2007). Air Quality in North Americas Most Populous City Overview of MCMA-2003 Campaign. Atmos. Chem. Phys. Discuss. 7.
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 conversion of lower volatility components into the detected higher volatility compounds.« less
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 conversion of lower volatility components into the detected higher volatility compounds.« less
Imputation of missing data in time series for air pollutants
NASA Astrophysics Data System (ADS)
Junger, W. L.; Ponce de Leon, A.
2015-02-01
Missing data are major concerns in epidemiological studies of the health effects of environmental air pollutants. This article presents an imputation-based method that is suitable for multivariate time series data, which uses the EM algorithm under the assumption of normal distribution. Different approaches are considered for filtering the temporal component. A simulation study was performed to assess validity and performance of proposed method in comparison with some frequently used methods. Simulations showed that when the amount of missing data was as low as 5%, the complete data analysis yielded satisfactory results regardless of the generating mechanism of the missing data, whereas the validity began to degenerate when the proportion of missing values exceeded 10%. The proposed imputation method exhibited good accuracy and precision in different settings with respect to the patterns of missing observations. Most of the imputations obtained valid results, even under missing not at random. The methods proposed in this study are implemented as a package called mtsdi for the statistical software system R.
Spacecraft intercept guidance using zero effort miss steering
NASA Astrophysics Data System (ADS)
Newman, Brett
The suitability of proportional navigation, or an equivalent zero effort miss formulation, for spacecraft intercepts during midcourse guidance, followed by a ballistic coast to the endgame, is addressed. The problem is formulated in terms of relative motion in a general 3D framework. The proposed guidance law for the commanded thrust vector orientation consists of the sum of two terms: (1) along the line of sight unit direction and (2) along the zero effort miss component perpendicular to the line of sight and proportional to the miss itself and a guidance gain. If the guidance law is to be suitable for longer range targeting applications with significant ballistic coasting after burnout, determination of the zero effort miss must account for the different gravitational accelerations experienced by each vehicle. The proposed miss determination techniques employ approximations for the true differential gravity effect. Theoretical results are applied to a numerical engagement scenario and the resulting performance is evaluated in terms of the miss distances determined from nonlinear simulation.
Top-of-atmosphere radiative forcing affected by brown carbon in the upper troposphere
NASA Astrophysics Data System (ADS)
Zhang, Yuzhong; Forrister, Haviland; Liu, Jiumeng; Dibb, Jack; Anderson, Bruce; Schwarz, Joshua P.; Perring, Anne E.; Jimenez, Jose L.; Campuzano-Jost, Pedro; Wang, Yuhang; Nenes, Athanasios; Weber, Rodney J.
2017-07-01
Carbonaceous aerosols affect the global radiative balance by absorbing and scattering radiation, which leads to warming or cooling of the atmosphere, respectively. Black carbon is the main light-absorbing component. A portion of the organic aerosol known as brown carbon also absorbs light. The climate sensitivity to absorbing aerosols rapidly increases with altitude, but brown carbon measurements are limited in the upper troposphere. Here we present aircraft observations of vertical aerosol distributions over the continental United States in May and June 2012 to show that light-absorbing brown carbon is prevalent in the troposphere, and absorbs more short-wavelength radiation than black carbon at altitudes between 5 and 12 km. We find that brown carbon is transported to these altitudes by deep convection, and that in-cloud heterogeneous processing may produce brown carbon. Radiative transfer calculations suggest that brown carbon accounts for about 24% of combined black and brown carbon warming effect at the tropopause. Roughly two-thirds of the estimated brown carbon forcing occurs above 5 km, although most brown carbon is found below 5 km. The highest radiative absorption occurred during an event that ingested a wildfire plume. We conclude that high-altitude brown carbon from biomass burning is an unappreciated component of climate forcing.
NASA Astrophysics Data System (ADS)
Helin, Aku; Sietiö, Outi-Maaria; Heinonsalo, Jussi; Bäck, Jaana; Riekkola, Marja-Liisa; Parshintsev, Jevgeni
2017-11-01
Primary biological aerosol particles (PBAPs) are ubiquitous in the atmosphere and constitute ˜ 30 % of atmospheric aerosol particle mass in sizes > 1 µm. PBAP components, such as bacteria, fungi and pollen, may affect the climate by acting as cloud-active particles, thus having an effect on cloud and precipitation formation processes. In this study, size-segregated aerosol samples (< 1.0, 1-2.5, 2.5-10 and > 10 µm) were collected in boreal forest (Hyytiälä, Finland) during a 9-month period covering all seasons and analysed for free amino acids (FAAs), DNA concentration and microorganism (bacteria, Pseudomonas and fungi). Measurements were performed using tandem mass spectrometry, spectrophotometry and qPCR, respectively. Meteorological parameters and statistical analysis were used to study their atmospheric implication for results. Distinct annual patterns of PBAP components were observed, late spring and autumn being seasons of dominant occurrence. Elevated abundances of FAAs and bacteria were observed during the local pollen season, whereas fungi were observed at the highest level during autumn. Meteorological parameters such as air and soil temperature, radiation and rainfall were observed to possess a close relationship with PBAP abundances on an annual scale.
NASA Astrophysics Data System (ADS)
Ripoll, A.; Minguillón, M. C.; Pey, J.; Jimenez, J. L.; Day, D. A.; Sosedova, Y.; Canonaco, F.; Prévôt, A. S. H.; Querol, X.; Alastuey, A.
2015-03-01
Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011-April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM1 components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Additional research is needed to characterize the sources and processes of SOA formation at remote sites.
Ripoll, Anna; Minguillon, M. C.; Pey, J.; ...
2015-03-16
Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM 1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM 1 components are attributed to variations in evolution of the planetary boundarymore » layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM 1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM 1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Furthermore, additional research is needed to characterize the sources and processes of SOA formation at remote sites.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ripoll, Anna; Minguillon, M. C.; Pey, J.
Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM 1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM 1 components are attributed to variations in evolution of the planetary boundarymore » layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM 1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM 1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Furthermore, additional research is needed to characterize the sources and processes of SOA formation at remote sites.« less
Age Changes in the Missing-Letter Effect Revisited
ERIC Educational Resources Information Center
Saint-Aubin, J.; Klein, R.M.; Landry, T.
2005-01-01
When participants search for a target letter while reading, they make more omissions if the target letter is embedded in frequent function words than in less frequent content words. Reflecting developmental changes in component language and literacy skills, the size of this effect increases with age. With adults, the missing-letter effect is due…
77 FR 28328 - Airworthiness Directives; Sikorsky Aircraft Corporation Helicopters
Federal Register 2010, 2011, 2012, 2013, 2014
2012-05-14
... loose or missing fastener, a crack, damage, or corrosion and adding an internal doubler to the aft shear... proposed actions are intended to detect a loose or missing fastener, a crack, damage, or corrosion on the T... inspection of the T/R pylon ``components and structure for obvious damage, cracks, corrosion, and security...
NASA Astrophysics Data System (ADS)
Quaas, J.; Ming, Y.; Menon, S.; Takemura, T.; Wang, M.; Penner, J. E.; Gettelman, A.; Lohmann, U.; Bellouin, N.; Boucher, O.; Sayer, A. M.; Thomas, G. E.; McComiskey, A.; Feingold, G.; Hoose, C.; Kristjánsson, J. E.; Liu, X.; Balkanski, Y.; Donner, L. J.; Ginoux, P. A.; Stier, P.; Grandey, B.; Feichter, J.; Sednev, I.; Bauer, S. E.; Koch, D.; Grainger, R. G.; Kirkevåg, A.; Iversen, T.; Seland, Ø.; Easter, R.; Ghan, S. J.; Rasch, P. J.; Morrison, H.; Lamarque, J.-F.; Iacono, M. J.; Kinne, S.; Schulz, M.
2009-11-01
Aerosol indirect effects continue to constitute one of the most important uncertainties for anthropogenic climate perturbations. Within the international AEROCOM initiative, the representation of aerosol-cloud-radiation interactions in ten different general circulation models (GCMs) is evaluated using three satellite datasets. The focus is on stratiform liquid water clouds since most GCMs do not include ice nucleation effects, and none of the model explicitly parameterises aerosol effects on convective clouds. We compute statistical relationships between aerosol optical depth (τa) and various cloud and radiation quantities in a manner that is consistent between the models and the satellite data. It is found that the model-simulated influence of aerosols on cloud droplet number concentration (Nd) compares relatively well to the satellite data at least over the ocean. The relationship between τa and liquid water path is simulated much too strongly by the models. This suggests that the implementation of the second aerosol indirect effect mainly in terms of an autoconversion parameterisation has to be revisited in the GCMs. A positive relationship between total cloud fraction (fcld) and τa as found in the satellite data is simulated by the majority of the models, albeit less strongly than that in the satellite data in most of them. In a discussion of the hypotheses proposed in the literature to explain the satellite-derived strong fcld-τa relationship, our results indicate that none can be identified as a unique explanation. Relationships similar to the ones found in satellite data between τa and cloud top temperature or outgoing long-wave radiation (OLR) are simulated by only a few GCMs. The GCMs that simulate a negative OLR-τa relationship show a strong positive correlation between τa and fcld. The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of τa, and parameterisation assumptions such as a lower bound on Nd. Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of -1.5±0.5 Wm-2. In an alternative approach, the radiative flux perturbation due to anthropogenic aerosols can be broken down into a component over the cloud-free portion of the globe (approximately the aerosol direct effect) and a component over the cloudy portion of the globe (approximately the aerosol indirect effect). An estimate obtained by scaling these simulated clear- and cloudy-sky forcings with estimates of anthropogenic τa and satellite-retrieved Nd-τa regression slopes, respectively, yields a global, annual-mean aerosol direct effect estimate of -0.4±0.2 Wm-2 and a cloudy-sky (aerosol indirect effect) estimate of -0.7±0.5 Wm-2, with a total estimate of -1.2±0.4 Wm-2.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Quaas, Johannes; Ming, Yi; Menon, Surabi
2010-03-12
Aerosol indirect effects continue to constitute one of the most important uncertainties for anthropogenic climate perturbations. Within the international AEROCOM initiative, the representation of aerosol-cloud-radiation interactions in ten different general circulation models (GCMs) is evaluated using three satellite datasets. The focus is on stratiform liquid water clouds since most GCMs do not include ice nucleation effects, and none of the model explicitly parameterises aerosol effects on convective clouds. We compute statistical relationships between aerosol optical depth ({tau}{sub a}) and various cloud and radiation quantities in a manner that is consistent between the models and the satellite data. It is foundmore » that the model-simulated influence of aerosols on cloud droplet number concentration (N{sub d}) compares relatively well to the satellite data at least over the ocean. The relationship between {tau}{sub a} and liquid water path is simulated much too strongly by the models. This suggests that the implementation of the second aerosol indirect effect mainly in terms of an autoconversion parameterisation has to be revisited in the GCMs. A positive relationship between total cloud fraction (f{sub cld}) and {tau}{sub a} as found in the satellite data is simulated by the majority of the models, albeit less strongly than that in the satellite data in most of them. In a discussion of the hypotheses proposed in the literature to explain the satellite-derived strong f{sub cld} - {tau}{sub a} relationship, our results indicate that none can be identified as a unique explanation. Relationships similar to the ones found in satellite data between {tau}{sub a} and cloud top temperature or outgoing long-wave radiation (OLR) are simulated by only a few GCMs. The GCMs that simulate a negative OLR - {tau}{sub a} relationship show a strong positive correlation between {tau}{sub a} and f{sub cld} The short-wave total aerosol radiative forcing as simulated by the GCMs is strongly influenced by the simulated anthropogenic fraction of {tau}{sub a}, and parameterization assumptions such as a lower bound on N{sub d}. Nevertheless, the strengths of the statistical relationships are good predictors for the aerosol forcings in the models. An estimate of the total short-wave aerosol forcing inferred from the combination of these predictors for the modelled forcings with the satellite-derived statistical relationships yields a global annual mean value of -1.5 {+-} 0.5 Wm{sup -2}. In an alternative approach, the radiative flux perturbation due to anthropogenic aerosols can be broken down into a component over the cloud-free portion of the globe (approximately the aerosol direct effect) and a component over the cloudy portion of the globe (approximately the aerosol indirect effect). An estimate obtained by scaling these simulated clear- and cloudy-sky forcings with estimates of anthropogenic {tau}{sub a} and satellite-retrieved Nd - {tau}{sub a} regression slopes, respectively, yields a global, annual-mean aerosol direct effect estimate of -0.4 {+-} 0.2 Wm{sup -2} and a cloudy-sky (aerosol indirect effect) estimate of -0.7 {+-} 0.5 Wm{sup -2}, with a total estimate of -1.2 {+-} 0.4 Wm{sup -2}.« less
NASA Astrophysics Data System (ADS)
Bikkina, Srinivas; Kawamura, Kimitaka; Miyazaki, Yuzo; Fu, Pingqing
2014-05-01
Atmospheric dicarboxylic acids (DCA) are a ubiquitous water-soluble component of secondary organic aerosols (SOA), which can act as cloud condensation nuclei (CCN), affecting the Earth's climate. Despite the high abundances of oxalic acid and related compounds in the marine aerosols, there is no consensus on what controls their distributions over the open ocean. Marine biological productivity could play a role in the production of DCA, but there is no substantial evidence to support this hypothesis. Here we present latitudinal distributions of DCA, oxoacids and α-dicarbonyls in the marine aerosols from the remote Pacific. Their concentrations were found several times higher in more biologically influenced aerosols (MBA) than less biologically influenced aerosols. We propose isoprene and unsaturated fatty acids as sources of DCA as inferred from significantly higher abundances of isoprene-SOA tracers and azelaic acid in MBA. These results have implications toward the reassessment of climate forcing feedbacks of marine-derived SOA.
Fluorescent water-soluble organic aerosols in the High Arctic atmosphere
Fu, Pingqing; Kawamura, Kimitaka; Chen, Jing; Qin, Mingyue; Ren, Lujie; Sun, Yele; Wang, Zifa; Barrie, Leonard A.; Tachibana, Eri; Ding, Aijun; Yamashita, Youhei
2015-01-01
Organic aerosols are ubiquitous in the earth’s atmosphere. They have been extensively studied in urban, rural and marine environments. However, little is known about the fluorescence properties of water-soluble organic carbon (WSOC) or their transport to and distribution in the polar regions. Here, we present evidence that fluorescent WSOC is a substantial component of High Arctic aerosols. The ratios of fluorescence intensity of protein-like peak to humic-like peak generally increased from dark winter to early summer, indicating an enhanced contribution of protein-like organics from the ocean to Arctic aerosols after the polar sunrise. Such a seasonal pattern is in agreement with an increase of stable carbon isotope ratios of total carbon (δ13CTC) from −26.8‰ to −22.5‰. Our results suggest that Arctic aerosols are derived from a combination of the long-range transport of terrestrial organics and local sea-to-air emission of marine organics, with an estimated contribution from the latter of 8.7–77% (mean 45%). PMID:25920042
Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming
NASA Technical Reports Server (NTRS)
Hofmann, David J.
1993-01-01
The paper examines the tropospheric aerosol record obtained over the period 1971 to 1990, during which high-altitude balloons with optical particle counters were launched at Laramie, Wyoming, in a long-term study of the stratospheric sulfate aerosol layer. All aerosol particle size ranges display pronounced seasonal variations, with the condensation nuclei concentration and the optically active component showing a summer maximum throughout the troposphere. Mass estimates, assuming spherical sulfate particles, indicate an average column mass between altitudes of 2.5 and 10 km of about 4 and 16 mg/sq m in winter and summer, respectively. Calculated optical depths vary between 0.01 and 0.04 from winter to summer; the estimated mass scattering cross section is about 3 sq m/g throughout the troposphere. There is evidence for a decreasing trend of 1.6-1.8 percent/yr in the optically active tropospheric aerosol over the past 20 yr, which may be related to a similar reduction in SO2 emission in the U.S. over this period.
An Overview of the GEOS-5 Aerosol Reanalysis
NASA Technical Reports Server (NTRS)
da Silva, Arlindo; Colarco, Peter Richard; Damenov, Anton Spasov; Buchard-Marchant, Virginie; Randles, Cynthia A.; Gupta, Pawan
2011-01-01
GEOS-5 is the latest version of the NASA Global Modeling and Assimilation Office (GMAO) earth system model. GEOS-5 contains components for atmospheric circulation and composition (including data assimilation), ocean circulation and biogeochemistry, and land surface processes. In addition to traditional meteorological parameters, GEOS-5 includes modules representing the atmospheric composition, most notably aerosols and tropospheric/stratospheric chemical constituents, taking explicit account of the impact of these constituents on the radiative processes of the atmosphere. MERRA is a NASA meteorological reanalysis for the satellite era (1979-present) using GEOS-5. This project focuses on historical analyses of the hydrological cycle on a broad range of weather and climate time scales. As a first step towards an integrated Earth System Analysis (IESA), the GMAO is extending MERRA with reanalyses for other components of the earth system: land, ocean, bio-geochemistry and atmospheric constituents. In this talk we will present results from the MERRA-driven aerosol reanalysis covering the Aqua period (2003-present). The assimilation of Aerosol Optical Depth (AOD) in GEOS-5 involves very careful cloud screening and homogenization of the observing system by means of a Neural Net scheme that translates MODIS radiances into AERONET calibrated AOD. These measurements are further quality controlled using an adaptive buddy check scheme, and assimilated using the Local Displacement Ensemble (LDE) methodology. For this reanalysis, GEOS-5 runs at a nominal 50km horizontal resolution with 72 vertical layers (top at approx. 8Skm). GEOS-5 is driven by daily biomass burning emissions derived from MODIS fire radiative power retrievals. We will present a summary of our efforts to validate such dataset. The GEOS-5 assimilated aerosol fields are first validated by comparison to independent in-situ measurements (AERONET and PM2.5 surface concentrations). In order to asses aerosol absorption on a global scale, we perform a detailed radiative transfer calculation to simulate the UV aerosol index, comparing our results to OMI measurements. By simulating aerosol attenuated backscatter, we use CALIPSO measurements to evaluate the vertical structure of our aerosol estimates, in particular in regions where we have larger discrepancies with OMI. Finally, the consistency of our AOD estimates with estimates from MISR, MODIS/Deep Blue, OMI and PARASOL will be briefly discussed.
NASA Astrophysics Data System (ADS)
Giorgiana Galon-Negru, Alina; Iulian Olariu, Romeo; Arsene, Cecilia
2018-04-01
This study assesses the effects of particle size and season on the content of the major inorganic and organic aerosol ionic components in the Iasi urban area, north-eastern Romania. Continuous measurements were carried out over 2016 using a cascade Dekati low-pressure impactor (DLPI) performing aerosol size classification in 13 specific fractions over the 0.0276-9.94 µm size range. Fine-particulate Cl-, NO3-, NH4+, and K+ exhibited clear minima during the warm season and clear maxima over the cold season, mainly due to trends in emission sources, changes in the mixing layer depth and specific meteorological conditions. Fine-particulate SO42- did not show much variation with respect to seasons. Particulate NH4+ and NO3- ions were identified as critical parameters controlling aerosol chemistry in the area, and their measured concentrations in fine-mode (PM2.5) aerosols were found to be in reasonable good agreement with modelled values for winter but not for summer. The likely reason is that NH4NO3 aerosols are lost due to volatility over the warm season. We found that NH4+ in PM2.5 is primarily associated with SO42- and NO3- but not with Cl-. Actually, indirect ISORROPIA-II estimations showed that the atmosphere in the Iasi area might be ammonia rich during both the cold and warm seasons, enabling enough NH3 to be present to neutralize H2SO4, HNO3, and HCl acidic components and to generate fine-particulate ammonium salts, in the form of (NH4)2SO4, NH4NO3, and NH4Cl. ISORROPIA-II runs allowed us to estimate that over the warm season ˜ 35 % of the total analysed samples had very strongly acidic pH (0-3), a fraction that rose to ˜ 43 % over the cold season. Moreover, while in the cold season the acidity is mainly accounted for by inorganic acids, in the warm ones there is an important contribution by other compounds, possibly organic. Indeed, changes in aerosol acidity would most likely impact the gas-particle partitioning of semi-volatile organic acids. Overall, we estimate that within the aerosol mass concentration the ionic mass brings a contribution as high as 40.6 %, with the rest still being unaccounted for.
An overview of geoengineering of climate using stratospheric sulphate aerosols
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rasch, Philip J.; Tilmes, S.; Turco, Richard P.
2010-01-01
We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changesmore » in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of ‘acid rain’ that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy reaching the surface, and this may influence ecosystems. The impact of geoengineering on these components of the Earth system has not yet been studied. Representations for the formation, evolution and removal of aerosol and distribution of particle size are still very crude, and more work will be needed to gain confidence in our understanding of the deliberate production of this class of aerosols and their role in the climate system.« less
An overview of geoengineering of climate using stratospheric sulphate aerosols.
Rasch, Philip J; Tilmes, Simone; Turco, Richard P; Robock, Alan; Oman, Luke; Chen, Chih-Chieh; Stenchikov, Georgiy L; Garcia, Rolando R
2008-11-13
We provide an overview of geoengineering by stratospheric sulphate aerosols. The state of understanding about this topic as of early 2008 is reviewed, summarizing the past 30 years of work in the area, highlighting some very recent studies using climate models, and discussing methods used to deliver sulphur species to the stratosphere. The studies reviewed here suggest that sulphate aerosols can counteract the globally averaged temperature increase associated with increasing greenhouse gases, and reduce changes to some other components of the Earth system. There are likely to be remaining regional climate changes after geoengineering, with some regions experiencing significant changes in temperature or precipitation. The aerosols also serve as surfaces for heterogeneous chemistry resulting in increased ozone depletion. The delivery of sulphur species to the stratosphere in a way that will produce particles of the right size is shown to be a complex and potentially very difficult task. Two simple delivery scenarios are explored, but similar exercises will be needed for other suggested delivery mechanisms. While the introduction of the geoengineering source of sulphate aerosol will perturb the sulphur cycle of the stratosphere signicantly, it is a small perturbation to the total (stratosphere and troposphere) sulphur cycle. The geoengineering source would thus be a small contributor to the total global source of 'acid rain' that could be compensated for through improved pollution control of anthropogenic tropospheric sources. Some areas of research remain unexplored. Although ozone may be depleted, with a consequent increase to solar ultraviolet-B (UVB) energy reaching the surface and a potential impact on health and biological populations, the aerosols will also scatter and attenuate this part of the energy spectrum, and this may compensate the UVB enhancement associated with ozone depletion. The aerosol will also change the ratio of diffuse to direct energy reaching the surface, and this may influence ecosystems. The impact of geoengineering on these components of the Earth system has not yet been studied. Representations for the formation, evolution and removal of aerosol and distribution of particle size are still very crude, and more work will be needed to gain confidence in our understanding of the deliberate production of this class of aerosols and their role in the climate system.
Chu, Biwu; Liggio, John; Liu, Yongchun; He, Hong; Takekawa, Hideto; Li, Shao-Meng; Hao, Jiming
2017-01-01
The organic component is the most abundant fraction of atmospheric submicron particles, while the formation mechanisms of secondary organic aerosol (SOA) are not fully understood. The effects of sulfate seed aerosols on SOA formation were investigated with a series of experiments carried out using a 9 m3 smog chamber. The presence of FeSO4 or Fe2(SO4)3 seed aerosols decreased SOA yields and increased oxidation levels in both ozonolysis and OH-oxidation of α-pinene compared to that in the presence of ZnSO4 or (NH4)2SO4. These findings were explained by metal-mediated aerosol-phase oxidation of organics: reactive radicals were generated on FeSO4 or Fe2(SO4)3 seed aerosols and reacted further with the organic mass. This effect would help to explain the high O/C ratios of organics in ambient particles that thus far cannot be reproduced in laboratory and model studies. In addition, the gap in the SOA yields between experiments with different seed aerosols was more significant in OH-oxidation experiments compared to ozonolysis experiments, while the gap in estimated O/C ratios was less obvious. This may have resulted from the different chemical compositions and oxidation levels of the SOA generated in the two systems, which affect the branching ratio of functionalization and fragmentation during aerosol oxidation. PMID:28059151
Chu, Biwu; Liggio, John; Liu, Yongchun; He, Hong; Takekawa, Hideto; Li, Shao-Meng; Hao, Jiming
2017-01-06
The organic component is the most abundant fraction of atmospheric submicron particles, while the formation mechanisms of secondary organic aerosol (SOA) are not fully understood. The effects of sulfate seed aerosols on SOA formation were investigated with a series of experiments carried out using a 9 m 3 smog chamber. The presence of FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols decreased SOA yields and increased oxidation levels in both ozonolysis and OH-oxidation of α-pinene compared to that in the presence of ZnSO 4 or (NH 4 ) 2 SO 4 . These findings were explained by metal-mediated aerosol-phase oxidation of organics: reactive radicals were generated on FeSO 4 or Fe 2 (SO 4 ) 3 seed aerosols and reacted further with the organic mass. This effect would help to explain the high O/C ratios of organics in ambient particles that thus far cannot be reproduced in laboratory and model studies. In addition, the gap in the SOA yields between experiments with different seed aerosols was more significant in OH-oxidation experiments compared to ozonolysis experiments, while the gap in estimated O/C ratios was less obvious. This may have resulted from the different chemical compositions and oxidation levels of the SOA generated in the two systems, which affect the branching ratio of functionalization and fragmentation during aerosol oxidation.
Direct Aerosol Forcing Uncertainty
Mccomiskey, Allison
2008-01-15
Understanding sources of uncertainty in aerosol direct radiative forcing (DRF), the difference in a given radiative flux component with and without aerosol, is essential to quantifying changes in Earth's radiation budget. We examine the uncertainty in DRF due to measurement uncertainty in the quantities on which it depends: aerosol optical depth, single scattering albedo, asymmetry parameter, solar geometry, and surface albedo. Direct radiative forcing at the top of the atmosphere and at the surface as well as sensitivities, the changes in DRF in response to unit changes in individual aerosol or surface properties, are calculated at three locations representing distinct aerosol types and radiative environments. The uncertainty in DRF associated with a given property is computed as the product of the sensitivity and typical measurement uncertainty in the respective aerosol or surface property. Sensitivity and uncertainty values permit estimation of total uncertainty in calculated DRF and identification of properties that most limit accuracy in estimating forcing. Total uncertainties in modeled local diurnally averaged forcing range from 0.2 to 1.3 W m-2 (42 to 20%) depending on location (from tropical to polar sites), solar zenith angle, surface reflectance, aerosol type, and aerosol optical depth. The largest contributor to total uncertainty in DRF is usually single scattering albedo; however decreasing measurement uncertainties for any property would increase accuracy in DRF. Comparison of two radiative transfer models suggests the contribution of modeling error is small compared to the total uncertainty although comparable to uncertainty arising from some individual properties.
Carbonaceous Aerosol Characterization during 2016 KOR-US 2016
NASA Astrophysics Data System (ADS)
Rodriguez, B.; Santos, G. M.; Sanchez, D.; Jeong, D.; Czimczik, C. I.; Kim, S.
2017-12-01
Atmospheric carbonaceous aerosols are a major component of fine particulate matter and assume important roles in Earth's climate and human health. Because atmospheric carbonaceous aerosols exist as a continuum ranging from small, light-scattering organic carbon (OC), to highly-condensed, light-absorbing elemental carbon (EC) they have contrasting effects on interaction with incoming and outgoing radiation, cloud formation, and snow/ice albedo. By strengthening our understanding of the relative contribution and sources of OC and EC we will be able to further describe aerosol formation and mixing at the regional level. To understand the relative anthropogenic and biogenic contributions to carbonaceous aerosol, 12 PM10 aerosols samples were collected on quartz fiber filters at the Mt. Taewha Research Forest in South Korea during the KORUS-AQ 2016 campaign over periods of 24-48 hours with a high-volume air sampler. Analysis of bulk C and N concentrations and absorption properties of filter extracts interspersed with HYSPLIT model results indicated that continental outflow across the Yellow Sea in enriched in bulk nitrogen loading and enhanced bulk absorptive properties of the aerosols. Bulk radiocarbon analysis also indicated enriched values in all samples indicating contamination from a nuclear power plant or the combustion of biomedical waste nearby. Here, we aim to investigate further the chemical characterization of VOCs adsorbed unto the aerosol through TD-GC-TOFMS. With this dataset we aim to determine the relative contribution of anthropogenic and biogenic aerosols by utilizing specific chemical tracers for source apportionment.
NASA Technical Reports Server (NTRS)
Gorzelska, K.; Talbot, R. W.; Klemm, K.; Lefer, B.; Klemm, O.; Gregory, G. L.; Anderson, B.; Barrie, L. A.
1994-01-01
Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.
Occurrence of pristine aerosol environments on a polluted planet
Hamilton, Douglas S.; Lee, Lindsay A.; Pringle, Kirsty J.; Reddington, Carly L.; Spracklen, Dominick V.; Carslaw, Kenneth S.
2014-01-01
Natural aerosols define a preindustrial baseline state from which the magnitude of anthropogenic aerosol effects on climate are calculated and are a major component of the large uncertainty in anthropogenic aerosol−cloud radiative forcing. This uncertainty would be reduced if aerosol environments unperturbed by air pollution could be studied in the present-day atmosphere, but the pervasiveness of air pollution makes identification of unperturbed regions difficult. Here, we use global model simulations to define unperturbed aerosol regions in terms of two measures that compare 1750 and 2000 conditions—the number of days with similar aerosol concentrations and the similarity of the aerosol response to perturbations in model processes and emissions. The analysis shows that the aerosol system in many present-day environments looks and behaves like it did in the preindustrial era. On a global annual mean, unperturbed aerosol regions cover 12% of the Earth (16% of the ocean surface and 2% of the land surface). There is a strong seasonal variation in unperturbed regions of between 4% in August and 27% in January, with the most persistent conditions occurring over the equatorial Pacific. About 90% of unperturbed regions occur in the Southern Hemisphere, but in the Northern Hemisphere, unperturbed conditions are transient and spatially patchy. In cloudy regions with a radiative forcing relative to 1750, model results suggest that unperturbed aerosol conditions could still occur on a small number of days per month. However, these environments are mostly in the Southern Hemisphere, potentially limiting the usefulness in reducing Northern Hemisphere forcing uncertainty. PMID:25512511
Optical extinction of highly porous aerosol following atmospheric freeze drying
NASA Astrophysics Data System (ADS)
Adler, Gabriela; Haspel, Carynelisa; Moise, Tamar; Rudich, Yinon
2014-06-01
Porous glassy particles are a potentially significant but unexplored component of atmospheric aerosol that can form by aerosol processing through the ice phase of high convective clouds. The optical properties of porous glassy aerosols formed from a freeze-dry cycle simulating freezing and sublimation of ice particles were measured using a cavity ring down aerosol spectrometer (CRD-AS) at 532 nm and 355 nm wavelength. The measured extinction efficiency was significantly reduced for porous organic and mixed organic-ammonium sulfate particles as compared to the extinction efficiency of the homogeneous aerosol of the same composition prior to the freeze-drying process. A number of theoretical approaches for modeling the optical extinction of porous aerosols were explored. These include effective medium approximations, extended effective medium approximations, multilayer concentric sphere models, Rayleigh-Debye-Gans theory, and the discrete dipole approximation. Though such approaches are commonly used to describe porous particles in astrophysical and atmospheric contexts, in the current study, these approaches predicted an even lower extinction than the measured one. Rather, the best representation of the measured extinction was obtained with an effective refractive index retrieved from a fit to Mie scattering theory assuming spherical particles with a fixed void content. The single-scattering albedo of the porous glassy aerosols was derived using this effective refractive index and was found to be lower than that of the corresponding homogeneous aerosol, indicating stronger relative absorption at the wavelengths measured. The reduced extinction and increased absorption may be of significance in assessing direct, indirect, and semidirect forcing in regions where porous aerosols are expected to be prevalent.
NASA Astrophysics Data System (ADS)
D'Ambro, Emma L.; Lee, Ben H.; Liu, Jiumeng; Shilling, John E.; Gaston, Cassandra J.; Lopez-Hilfiker, Felipe D.; Schobesberger, Siegfried; Zaveri, Rahul A.; Mohr, Claudia; Lutz, Anna; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.; Rivera-Rios, Jean C.; Keutsch, Frank N.; Thornton, Joel A.
2017-01-01
We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation in an environmental simulation chamber at a variety of oxidant conditions and using dry neutral seed particles to suppress acid-catalyzed multiphase chemistry. A high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and Aerosols (FIGAERO) allowed for simultaneous online sampling of the gas and particle composition. Under high-HO2 and low-NO conditions, highly oxygenated (O : C ≥ 1) C5 compounds were major components (˜ 50 %) of SOA. The SOA composition and effective volatility evolved both as a function of time and as a function of input NO concentrations. Organic nitrates increased in both the gas and particle phases as input NO increased, but the dominant non-nitrate particle-phase components monotonically decreased. We use comparisons of measured and predicted gas-particle partitioning of individual components to assess the validity of literature-based group-contribution methods for estimating saturation vapor concentrations. While there is evidence for equilibrium partitioning being achieved on the chamber residence timescale (5.2 h) for some individual components, significant errors in group-contribution methods are revealed. In addition, > 30 % of the SOA mass, detected as low-molecular-weight semivolatile compounds, cannot be reconciled with equilibrium partitioning. These compounds desorb from the FIGAERO at unexpectedly high temperatures given their molecular composition, which is indicative of thermal decomposition of effectively lower-volatility components such as larger molecular weight oligomers.
NASA Astrophysics Data System (ADS)
Ben Salah, Ahmed; Ragot, Nicolas; Paquet, Thierry
2013-01-01
The French National Library (BnF*) has launched many mass digitization projects in order to give access to its collection. The indexation of digital documents on Gallica (digital library of the BnF) is done through their textual content obtained thanks to service providers that use Optical Character Recognition softwares (OCR). OCR softwares have become increasingly complex systems composed of several subsystems dedicated to the analysis and the recognition of the elements in a page. However, the reliability of these systems is always an issue at stake. Indeed, in some cases, we can find errors in OCR outputs that occur because of an accumulation of several errors at different levels in the OCR process. One of the frequent errors in OCR outputs is the missed text components. The presence of such errors may lead to severe defects in digital libraries. In this paper, we investigate the detection of missed text components to control the OCR results from the collections of the French National Library. Our verification approach uses local information inside the pages based on Radon transform descriptors and Local Binary Patterns descriptors (LBP) coupled with OCR results to control their consistency. The experimental results show that our method detects 84.15% of the missed textual components, by comparing the OCR ALTO files outputs (produced by the service providers) to the images of the document.
Using MODIS Cloud Regimes to Sort Diagnostic Signals of Aerosol-Cloud-Precipitation Interactions
Oreopoulos, Lazaros; Cho, Nayeong; Lee, Dongmin
2018-01-01
Coincident multi-year measurements of aerosol, cloud, precipitation and radiation at near-global scales are analyzed to diagnose their apparent relationships as suggestive of interactions previously proposed based on theoretical, observational, and model constructs. Specifically, we examine whether differences in aerosol loading in separate observations go along with consistently different precipitation, cloud properties, and cloud radiative effects. Our analysis uses a cloud regime (CR) framework to dissect and sort the results. The CRs come from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor and are defined as distinct groups of cloud systems with similar co-variations of cloud top pressure and cloud optical thickness. Aerosol optical depth used as proxy for aerosol loading comes from two sources, MODIS observations, and the MERRA-2 re-analysis, and its variability is defined with respect to local seasonal climatologies. The choice of aerosol dataset impacts our results substantially. We also find that the responses of the marine and continental component of a CR are frequently quite disparate. Overall, CRs dominated by warm clouds tend to exhibit less ambiguous signals, but also have more uncertainty with regard to precipitation changes. Finally, we find weak, but occasionally systematic co-variations of select meteorological indicators and aerosol, which serves as a sober reminder that ascribing changes in cloud and cloud-affected variables solely to aerosol variations is precarious. PMID:29651373
Using MODIS Cloud Regimes to Sort Diagnostic Signals of Aerosol-Cloud-Precipitation Interactions.
Oreopoulos, Lazaros; Cho, Nayeong; Lee, Dongmin
2017-05-27
Coincident multi-year measurements of aerosol, cloud, precipitation and radiation at near-global scales are analyzed to diagnose their apparent relationships as suggestive of interactions previously proposed based on theoretical, observational, and model constructs. Specifically, we examine whether differences in aerosol loading in separate observations go along with consistently different precipitation, cloud properties, and cloud radiative effects. Our analysis uses a cloud regime (CR) framework to dissect and sort the results. The CRs come from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor and are defined as distinct groups of cloud systems with similar co-variations of cloud top pressure and cloud optical thickness. Aerosol optical depth used as proxy for aerosol loading comes from two sources, MODIS observations, and the MERRA-2 re-analysis, and its variability is defined with respect to local seasonal climatologies. The choice of aerosol dataset impacts our results substantially. We also find that the responses of the marine and continental component of a CR are frequently quite disparate. Overall, CRs dominated by warm clouds tend to exhibit less ambiguous signals, but also have more uncertainty with regard to precipitation changes. Finally, we find weak, but occasionally systematic co-variations of select meteorological indicators and aerosol, which serves as a sober reminder that ascribing changes in cloud and cloud-affected variables solely to aerosol variations is precarious.
Physical and Optical/Radiative Properties of Arctic Aerosols: Potential Effects on Arctic Climate
NASA Technical Reports Server (NTRS)
Pueschel, R. F.; Kinne, S. A.; Gore, Warren J. (Technical Monitor)
1994-01-01
We have determined the abundance of light-scattering sulfuric acid (H2SO4/H2O) and light-absorbing black carbon aerosol (BCA) in Spring 1992 in the Arctic atmosphere by airborne in situ sampling with impactors, and measured particle sizes and morphologies by scanning electron microscopy. The mass of BCA in the Arctic troposphere is one percent of the total aerosol, reduced to one part in 104 in the stratosphere. A Mie algorithm permits the calculation of the optical properties of the various aerosol components, and an algorithm developed by Ackerman and Toon and modified to serve our needs lets us calculate the optical effects of the black carbon aerosol that is mixed internally with the sulfuric acid aerosol. It follows that the effect of internally-mixed BCA on the aerosol scattering and absorption properties depends on its location within the droplet. BCA concentrated near the droplet surface has a greater effect on absorption of solar radiation than does the same amount of BCA located near its center. Single scatter albedos of the combined system are omega(sub 0)=1.0 in the post-Pinatubo Arctic stratosphere, and as low as 0.94 in the troposphere. The aerosol has the potential to regionally warm the Arctic earth-atmosphere system, because of the high surface albedo of the snow-covered Arctic.
NASA Astrophysics Data System (ADS)
Cao, F.; Zhang, Y.; Kawamura, K.
2015-12-01
To better characterize the sources of fine particulate matter (i.e. PM2.5) in Sanjiang Plain, Northeast China, aerosol chemical composition such total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied as well as stable carbon isotopic composition (δ13C) of TC. Intensively open biomass burning episodes were identified from late September to early October by satellite fire and aerosol optical depth maps. During the biomass burning episodes, concentrations of PM2.5, OC, EC, and WSOC increased by a factor of 4-12 compared to non-biomass-burning periods. Non-sea-salt potassium is strongly correlated with PM2.5, OC, EC and WSOC, suggesting an important contribution of biomass burning emission. The enrichment in both the non-sea-salt potassium and chlorine is significantly larger than other inorganic species, indicating that biomass burning aerosols in Sanjiang Plain is mostly fresh and less aged. In addition, WSOC to OC ratio is relatively lower compared to that reported in biomass burning aerosols in tropical regions, supporting that biomass burning aerosols in Sanjiang Plain is mostly primary and secondary organic aerosols is not significant. A lower average δ13C value (-26.2‰) is found for the biomass-burning aerosols, suggesting a dominant contribution from combustion of C3 plants in the studied region.
NASA Astrophysics Data System (ADS)
Cohen, J. B.; Lan, R.; Lin, C.; Ng, D. H. L.; Lim, A.
2017-12-01
A multi-instrument, inverse modeling approach, is employed to identify and quantify large-scale global biomass urban aerosol emissions profiles. The approach uses MISR, MODIS, OMI and MOPITT, with data from 2006 to 2016, to generate spatial and temporal loads, as well as some information about composition. The method is able to identify regions impacted by stable urban sources, changing urban sources, intense fires, and linear-combinations. Subsequent quantification is a unified field, leading to a less biased profile, with the result not requiring arbitrary scaling to match long-term means. Additionally, the result reasonably reproduces inter and intra annual variation. Both meso-scale (WRF-CHEM) and global (MIT-AERO, multi-mode, multi-mixing state aerosol model) models of aerosol transport, chemistry, and physics, are used to generate resulting 4D aerosol fields. Comparisons with CALIOP, AERONET, and surface chemical and aerosol networks, provide unbiased confirmation, while column and vertical loadings provide additional feedback. There are three significant results. First, there is a reduction in sources over existing urban areas in East Asia. Second, there is an increase in sources over new urban areas in South, South East, and East Asia. Third, that there is an increase in fire sources in South and South East Asia. There are other initial findings relevant to the global tropics, which have not been as deeply investigated. The results improve the model match with both the mean and variation, which is essential if we hope to understand seasonal extremes. The results also quantify impacts of both local and long-range sources. This is of extreme urgency, in particular in developing nations, where there are considerable contributions from long-range or otherwise unknown sources, that impact hundreds of millions of people throughout Asia. It is hoped that the approach provided here can help us to make critical decisions about total sources, as well as point out the many missing scientific and analytical issues still required to address.
Effect of Heterogeneous Chemical Reactions on the Köhler Activation of Aqueous Organic Aerosols.
Djikaev, Yuri S; Ruckenstein, Eli
2018-05-03
We study some thermodynamic aspects of the activation of aqueous organic aerosols into cloud droplets considering the aerosols to consist of liquid solution of water and hydrophilic and hydrophobic organic compounds, taking into account the presence of reactive species in the air. The hydrophobic (surfactant) organic molecules on the surface of such an aerosol can be processed by chemical reactions with some atmospheric species; this affects the hygroscopicity of the aerosol and hence its ability to become a cloud droplet either via nucleation or via Köhler activation. The most probable pathway of such processing involves atmospheric hydroxyl radicals that abstract hydrogen atoms from hydrophobic organic molecules located on the aerosol surface (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). These two reactions play a crucial role in the enhancement of the Köhler activation of the aerosol and its evolution into a cloud droplet. Taking them and a third reaction (next in the multistep chain of relevant heterogeneous reactions) into account, one can derive an explicit expression for the free energy of formation of a four-component aqueous droplet on a ternary aqueous organic aerosol as a function of four independent variables of state of a droplet. The results of numerical calculations suggest that the formation of cloud droplets on such (aqueous hydrophilic/hydrophobic organic) aerosols is most likely to occur as a Köhler activation-like process rather than via nucleation. The model allows one to determine the threshold parameters of the system necessary for the Köhler activation of such aerosols, which are predicted to be very sensitive to the equilibrium constant of the chain of three heterogeneous reactions involved in the chemical aging of aerosols.
NASA Technical Reports Server (NTRS)
Tao, W.-K.; Li, X.; Khain, A.; Mastsui, T.; Lang, S.; Simpson, J.
2007-01-01
Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 20011. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds NRC [2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path and the "semi-direct" effect on cloud coverage. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect, is even more complex, especially for mixed-phase convective clouds. ln this paper, a cloud-resolving model (CRM) with detailed spectral-bin microphysics was used to examine the effect of aerosols on three different deep convective cloud systems that developed in different geographic locations: South Florida, Oklahoma and the Central Pacific. In all three cases, rain reaches the ground earlier for the low CCN (clean) case. Rain suppression is also evident in all three cases with high CCN (dirty) case. However, this suppression only occurs during the first hour of the simulations. During the mature stages of the simulations, the effects of increasing aerosol concentration range from rain suppression in the Oklahoma case, to almost no effect in the Florida case, to rain enhancement in the Pacific case. These results show the complexity of aerosol interactions with convection.
The Sensitivity of SeaWiFS Ocean Color Retrievals to Aerosol Amount and Type
NASA Technical Reports Server (NTRS)
Kahn, Ralph A.; Sayer, Andrew M.; Ahmad, Ziauddin; Franz, Bryan A.
2016-01-01
As atmospheric reflectance dominates top-of-the-atmosphere radiance over ocean, atmospheric correction is a critical component of ocean color retrievals. This paper explores the operational Sea-viewing Wide Field-of-View Sensor (SeaWiFS) algorithm atmospheric correction with approximately 13 000 coincident surface-based aerosol measurements. Aerosol optical depth at 440 nm (AOD(sub 440)) is overestimated for AOD below approximately 0.1-0.15 and is increasingly underestimated at higher AOD; also, single-scattering albedo (SSA) appears overestimated when the actual value less than approximately 0.96.AOD(sub 440) and its spectral slope tend to be overestimated preferentially for coarse-mode particles. Sensitivity analysis shows that changes in these factors lead to systematic differences in derived ocean water-leaving reflectance (Rrs) at 440 nm. The standard SeaWiFS algorithm compensates for AOD anomalies in the presence of nonabsorbing, medium-size-dominated aerosols. However, at low AOD and with absorbing aerosols, in situ observations and previous case studies demonstrate that retrieved Rrs is sensitive to spectral AOD and possibly also SSA anomalies. Stratifying the dataset by aerosol-type proxies shows the dependence of the AOD anomaly and resulting Rrs patterns on aerosol type, though the correlation with the SSA anomaly is too subtle to be quantified with these data. Retrieved chlorophyll-a concentrations (Chl) are affected in a complex way by Rrs differences, and these effects occur preferentially at high and low Chl values. Absorbing aerosol effects are likely to be most important over biologically productive waters near coasts and along major aerosol transport pathways. These results suggest that future ocean color spacecraft missions aiming to cover the range of naturally occurring and anthropogenic aerosols, especially at wavelengths shorter than 440 nm, will require better aerosol amount and type constraints.
NASA Astrophysics Data System (ADS)
Singh, Atinderpal; Srivastava, Rohit; Rastogi, Neeraj; Singh, Darshan
2016-02-01
The current study focuses on the assessment of model simulated optical and radiative properties of aerosols incorporating the measured chemical composition of aerosol samples collected at Patiala during October, 2011-February, 2012. Monthly average mass concentration of PM2.5, elemental carbon (EC), primary organic carbon (POC), water-soluble (WS) and insoluble (INS) aerosols ranged from 120 to 192, 6.2 to 7.2, 20 to 39, 59 to 111 and 35 to 90 μg m-3, respectively. Mass concentration of different components of aerosols was further used for the assessment of optical properties derived from Optical Properties of Aerosols and Clouds (OPAC) model simulations. Microtops based measured aerosol optical depth (AOD500) ranged from 0.47 to 0.62 showing maximum value during November and December, and minimum during February. Ångström exponent (α380-870) remained high (>0.90) throughout the study period except in February (0.74), suggesting predominance of fine mode particles over the study region. The observed ratio of scattering to absorbing aerosols was incorporated in OPAC model simulations and single scattering albedo (SSA at 500 nm) so obtained ranged between 0.80 and 0.92 with relatively low values during the period of extensive biomass burning. In the present study, SBDART based estimated values of aerosol radiative forcing (ARF) at the surface (SRF) and top of the atmosphere (TOA) ranged from -31 to -66 Wm-2 and -2 to -18 W m-2 respectively. The atmospheric ARF, ranged between + 18 and + 58 Wm-2 resulting in the atmospheric heating rate between 0.5 and 1.6 K day-1. These results signify the role of scattering and absorbing aerosols in affecting the magnitude of aerosol forcing.
Missing Value Imputation Approach for Mass Spectrometry-based Metabolomics Data.
Wei, Runmin; Wang, Jingye; Su, Mingming; Jia, Erik; Chen, Shaoqiu; Chen, Tianlu; Ni, Yan
2018-01-12
Missing values exist widely in mass-spectrometry (MS) based metabolomics data. Various methods have been applied for handling missing values, but the selection can significantly affect following data analyses. Typically, there are three types of missing values, missing not at random (MNAR), missing at random (MAR), and missing completely at random (MCAR). Our study comprehensively compared eight imputation methods (zero, half minimum (HM), mean, median, random forest (RF), singular value decomposition (SVD), k-nearest neighbors (kNN), and quantile regression imputation of left-censored data (QRILC)) for different types of missing values using four metabolomics datasets. Normalized root mean squared error (NRMSE) and NRMSE-based sum of ranks (SOR) were applied to evaluate imputation accuracy. Principal component analysis (PCA)/partial least squares (PLS)-Procrustes analysis were used to evaluate the overall sample distribution. Student's t-test followed by correlation analysis was conducted to evaluate the effects on univariate statistics. Our findings demonstrated that RF performed the best for MCAR/MAR and QRILC was the favored one for left-censored MNAR. Finally, we proposed a comprehensive strategy and developed a public-accessible web-tool for the application of missing value imputation in metabolomics ( https://metabolomics.cc.hawaii.edu/software/MetImp/ ).
NASA Astrophysics Data System (ADS)
Alexander, B.; Park, R. J.
2006-12-01
The oxygen isotopic composition of sulfate aerosols (Δ17O ~ δ&&17O 0.5*δ18O) reflects the relative importance of different photochemical oxidation pathways in the atmosphere. Simulated isotopic variability in a global chemical transport model (GEOS-Chem) shows good agreement with observations in oceanic [Alexander et al., 2005] and some continental sites. However, a large discrepancy exists between modeled and measured isotopic composition in the high northern latitudes, reflecting an incomplete understanding of the sulfur budget in this region. Recent oxygen isotope measurements of sulfate aerosols collected at Alert, Canada suggest that transition metal catalyzed oxidation of SO2 by O2 in the aqueous-phase is significant during winter [Mc Cabe et al.,2006]. Global chemistry models ignore this oxidation pathway because it is believed to be important only regionally, and because of the large uncertainties in atmospheric metal concentrations and oxidation states. We have incorporated Fe(III) and Mn(II) catalyzed oxidation of S(IV) (S(IV) = SO2·H2O + HSO3- + SO32-) by O2 into the GEOS-Chem model using the McCabe et al. [2006] isotope measurements as a constraint. We will examine the importance of this oxidation pathway for the sulfur budget in the Arctic, and on the global scale. Preliminary results suggest that, during winter, up to 75% of aerosol sulfate at Alert forms via the metal catalysis pathway. The addition of this chemical pathway decreases the SO2 burden in the Arctic (north of 60°N) by 40% due to an increase in the oxidation rate. The comparison of large-scale sulfate aerosol models study (COSAM) showed that on average, models over-predict SO2 mixing ratios by factors of 2 or more [Barrie et al., 2001]. This "missing" S(IV) oxidation pathway can partially explain this discrepancy.
Salvatore, Stefania; Bramness, Jørgen G; Røislien, Jo
2016-07-12
Wastewater-based epidemiology (WBE) is a novel approach in drug use epidemiology which aims to monitor the extent of use of various drugs in a community. In this study, we investigate functional principal component analysis (FPCA) as a tool for analysing WBE data and compare it to traditional principal component analysis (PCA) and to wavelet principal component analysis (WPCA) which is more flexible temporally. We analysed temporal wastewater data from 42 European cities collected daily over one week in March 2013. The main temporal features of ecstasy (MDMA) were extracted using FPCA using both Fourier and B-spline basis functions with three different smoothing parameters, along with PCA and WPCA with different mother wavelets and shrinkage rules. The stability of FPCA was explored through bootstrapping and analysis of sensitivity to missing data. The first three principal components (PCs), functional principal components (FPCs) and wavelet principal components (WPCs) explained 87.5-99.6 % of the temporal variation between cities, depending on the choice of basis and smoothing. The extracted temporal features from PCA, FPCA and WPCA were consistent. FPCA using Fourier basis and common-optimal smoothing was the most stable and least sensitive to missing data. FPCA is a flexible and analytically tractable method for analysing temporal changes in wastewater data, and is robust to missing data. WPCA did not reveal any rapid temporal changes in the data not captured by FPCA. Overall the results suggest FPCA with Fourier basis functions and common-optimal smoothing parameter as the most accurate approach when analysing WBE data.
A New Black Carbon Sensor for Dense Air Quality Monitoring Networks
Caubel, Julien J.; Cados, Troy E.; Kirchstetter, Thomas W.
2018-01-01
Low-cost air pollution sensors are emerging and increasingly being deployed in densely distributed wireless networks that provide more spatial resolution than is typical in traditional monitoring of ambient air quality. However, a low-cost option to measure black carbon (BC)—a major component of particulate matter pollution associated with adverse human health risks—is missing. This paper presents a new BC sensor designed to fill this gap, the Aerosol Black Carbon Detector (ABCD), which incorporates a compact weatherproof enclosure, solar-powered rechargeable battery, and cellular communication to enable long-term, remote operation. This paper also demonstrates a data processing methodology that reduces the ABCD’s sensitivity to ambient temperature fluctuations, and therefore improves measurement performance in unconditioned operating environments (e.g., outdoors). A fleet of over 100 ABCDs was operated outdoors in collocation with a commercial BC instrument (Magee Scientific, Model AE33) housed inside a regulatory air quality monitoring station. The measurement performance of the 105 ABCDs is comparable to the AE33. The fleet-average precision and accuracy, expressed in terms of mean absolute percentage error, are 9.2 ± 0.8% (relative to the fleet average data) and 24.6 ± 0.9% (relative to the AE33 data), respectively (fleet-average ± 90% confidence interval). PMID:29494528
A New Black Carbon Sensor for Dense Air Quality Monitoring Networks.
Caubel, Julien J; Cados, Troy E; Kirchstetter, Thomas W
2018-03-01
Low-cost air pollution sensors are emerging and increasingly being deployed in densely distributed wireless networks that provide more spatial resolution than is typical in traditional monitoring of ambient air quality. However, a low-cost option to measure black carbon (BC)-a major component of particulate matter pollution associated with adverse human health risks-is missing. This paper presents a new BC sensor designed to fill this gap, the Aerosol Black Carbon Detector (ABCD), which incorporates a compact weatherproof enclosure, solar-powered rechargeable battery, and cellular communication to enable long-term, remote operation. This paper also demonstrates a data processing methodology that reduces the ABCD's sensitivity to ambient temperature fluctuations, and therefore improves measurement performance in unconditioned operating environments (e.g., outdoors). A fleet of over 100 ABCDs was operated outdoors in collocation with a commercial BC instrument (Magee Scientific, Model AE33) housed inside a regulatory air quality monitoring station. The measurement performance of the 105 ABCDs is comparable to the AE33. The fleet-average precision and accuracy, expressed in terms of mean absolute percentage error, are 9.2 ± 0.8% (relative to the fleet average data) and 24.6 ± 0.9% (relative to the AE33 data), respectively (fleet-average ± 90% confidence interval).
Organic and inorganic decomposition products from the thermal desorption of atmospheric particles
NASA Astrophysics Data System (ADS)
Williams, B. J.; Zhang, Y.; Zuo, X.; Martinez, R. E.; Walker, M. J.; Kreisberg, N. M.; Goldstein, A. H.; Docherty, K. S.; Jimenez, J. L.
2015-12-01
Atmospheric aerosol composition is often analyzed using thermal desorption techniques to evaporate samples and deliver organic or inorganic molecules to various designs of detectors for identification and quantification. The organic aerosol (OA) fraction is composed of thousands of individual compounds, some with nitrogen- and sulfur-containing functionality, and often contains oligomeric material, much of which may be susceptible to decomposition upon heating. Here we analyze thermal decomposition products as measured by a thermal desorption aerosol gas chromatograph (TAG) capable of separating thermal decomposition products from thermally stable molecules. The TAG impacts particles onto a collection and thermal desorption (CTD) cell, and upon completion of sample collection, heats and transfers the sample in a helium flow up to 310 °C. Desorbed molecules are refocused at the head of a GC column that is held at 45 °C and any volatile decomposition products pass directly through the column and into an electron impact quadrupole mass spectrometer (MS). Analysis of the sample introduction (thermal decomposition) period reveals contributions of NO+ (m/z 30), NO2+ (m/z 46), SO+ (m/z 48), and SO2+ (m/z 64), derived from either inorganic or organic particle-phase nitrate and sulfate. CO2+ (m/z 44) makes up a major component of the decomposition signal, along with smaller contributions from other organic components that vary with the type of aerosol contributing to the signal (e.g., m/z 53, 82 observed here for isoprene-derived secondary OA). All of these ions are important for ambient aerosol analyzed with the aerosol mass spectrometer (AMS), suggesting similarity of the thermal desorption processes in both instruments. Ambient observations of these decomposition products compared to organic, nitrate, and sulfate mass concentrations measured by an AMS reveal good correlation, with improved correlations for OA when compared to the AMS oxygenated OA (OOA) component. TAG signal found in the traditional compound elution time period reveals higher correlations with AMS hydrocarbon-like OA (HOA) combined with the fraction of OOA that is less oxygenated. Potential to quantify nitrate and sulfate aerosol mass concentrations using the TAG system is explored through analysis of ammonium sulfate and ammonium nitrate standards. While chemical standards display a linear response in the TAG system, re-desorptions of the CTD cell following ambient sample analysis shows some signal carryover on sulfate and organics, and new desorption methods should be developed to improve throughput. Future standards should be composed of complex organic/inorganic mixtures, similar to what is found in the atmosphere, and perhaps will more accurately account for any aerosol mixture effects on compositional quantification.
Organic and inorganic decomposition products from the thermal desorption of atmospheric particles
NASA Astrophysics Data System (ADS)
Williams, Brent J.; Zhang, Yaping; Zuo, Xiaochen; Martinez, Raul E.; Walker, Michael J.; Kreisberg, Nathan M.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.
2016-04-01
Atmospheric aerosol composition is often analyzed using thermal desorption techniques to evaporate samples and deliver organic or inorganic molecules to various designs of detectors for identification and quantification. The organic aerosol (OA) fraction is composed of thousands of individual compounds, some with nitrogen- and sulfur-containing functionality and, often contains oligomeric material, much of which may be susceptible to decomposition upon heating. Here we analyze thermal decomposition products as measured by a thermal desorption aerosol gas chromatograph (TAG) capable of separating thermal decomposition products from thermally stable molecules. The TAG impacts particles onto a collection and thermal desorption (CTD) cell, and upon completion of sample collection, heats and transfers the sample in a helium flow up to 310 °C. Desorbed molecules are refocused at the head of a gas chromatography column that is held at 45 °C and any volatile decomposition products pass directly through the column and into an electron impact quadrupole mass spectrometer. Analysis of the sample introduction (thermal decomposition) period reveals contributions of NO+ (m/z 30), NO2+ (m/z 46), SO+ (m/z 48), and SO2+ (m/z 64), derived from either inorganic or organic particle-phase nitrate and sulfate. CO2+ (m/z 44) makes up a major component of the decomposition signal, along with smaller contributions from other organic components that vary with the type of aerosol contributing to the signal (e.g., m/z 53, 82 observed here for isoprene-derived secondary OA). All of these ions are important for ambient aerosol analyzed with the aerosol mass spectrometer (AMS), suggesting similarity of the thermal desorption processes in both instruments. Ambient observations of these decomposition products compared to organic, nitrate, and sulfate mass concentrations measured by an AMS reveal good correlation, with improved correlations for OA when compared to the AMS oxygenated OA (OOA) component. TAG signal found in the traditional compound elution time period reveals higher correlations with AMS hydrocarbon-like OA (HOA) combined with the fraction of OOA that is less oxygenated. Potential to quantify nitrate and sulfate aerosol mass concentrations using the TAG system is explored through analysis of ammonium sulfate and ammonium nitrate standards. While chemical standards display a linear response in the TAG system, redesorptions of the CTD cell following ambient sample analysis show some signal carryover on sulfate and organics, and new desorption methods should be developed to improve throughput. Future standards should be composed of complex organic/inorganic mixtures, similar to what is found in the atmosphere, and perhaps will more accurately account for any aerosol mixture effects on compositional quantification.
Organic and inorganic decomposition products from the thermal desorption of atmospheric particles
Williams, Brent J.; Zhang, Yaping; Zuo, Xiaochen; ...
2016-04-11
Here, atmospheric aerosol composition is often analyzed using thermal desorption techniques to evaporate samples and deliver organic or inorganic molecules to various designs of detectors for identification and quantification. The organic aerosol (OA) fraction is composed of thousands of individual compounds, some with nitrogen- and sulfur-containing functionality and, often contains oligomeric material, much of which may be susceptible to decomposition upon heating. Here we analyze thermal decomposition products as measured by a thermal desorption aerosol gas chromatograph (TAG) capable of separating thermal decomposition products from thermally stable molecules. The TAG impacts particles onto a collection and thermal desorption (CTD) cell, and upon completionmore » of sample collection, heats and transfers the sample in a helium flow up to 310 °C. Desorbed molecules are refocused at the head of a gas chromatography column that is held at 45 °C and any volatile decomposition products pass directly through the column and into an electron impact quadrupole mass spectrometer. Analysis of the sample introduction (thermal decomposition) period reveals contributions of NO + ( m/z 30), NO 2 + ( m/z 46), SO + ( m/z 48), and SO 2 + ( m/z 64), derived from either inorganic or organic particle-phase nitrate and sulfate. CO 2 + ( m/z 44) makes up a major component of the decomposition signal, along with smaller contributions from other organic components that vary with the type of aerosol contributing to the signal (e.g., m/z 53, 82 observed here for isoprene-derived secondary OA). All of these ions are important for ambient aerosol analyzed with the aerosol mass spectrometer (AMS), suggesting similarity of the thermal desorption processes in both instruments. Ambient observations of these decomposition products compared to organic, nitrate, and sulfate mass concentrations measured by an AMS reveal good correlation, with improved correlations for OA when compared to the AMS oxygenated OA (OOA) component. TAG signal found in the traditional compound elution time period reveals higher correlations with AMS hydrocarbon-like OA (HOA) combined with the fraction of OOA that is less oxygenated. Potential to quantify nitrate and sulfate aerosol mass concentrations using the TAG system is explored through analysis of ammonium sulfate and ammonium nitrate standards. While chemical standards display a linear response in the TAG system, redesorptions of the CTD cell following ambient sample analysis show some signal carryover on sulfate and organics, and new desorption methods should be developed to improve throughput. Future standards should be composed of complex organic/inorganic mixtures, similar to what is found in the atmosphere, and perhaps will more accurately account for any aerosol mixture effects on compositional quantification.« less
NASA Astrophysics Data System (ADS)
Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J. C.; Sodeau, J. R.; Healy, R. M.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; O'Dowd, C. D.
2009-12-01
As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the NE Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Black carbon concentrations in polluted air were between 300-400 ng m-3, and in clean marine air were less than 50 ng m-3. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were highest in marine tropical air - even higher than in continental air. MSA was present at twice the concentrations of previously-reported concentrations at the same location and the same season. Both continental and marine air exhibited aerosol GFs significantly less than ammonium sulphate and even less in terms of sea salt aerosol pointing to a significant organic contribution to all air mass aerosol properties.
NASA Astrophysics Data System (ADS)
Schill, S.; Novak, G.; Zimmermann, K.; Bertram, T. H.
2014-12-01
The ocean serves as a major source for atmospheric aerosol particles, yet the chemicophysical properties of sea spray aerosol to date are not well characterized. Understanding the transfer of organic compounds, present in the sea surface microlayer (SSML), to sea-spray particles and their resulting impact on cloud formation is important for predicting aerosol impact on climate in remote marine environments. Here, we present a series of laboratory experiments designed to probe the fractionation of select organic molecules during wave breaking. We use a representative set of organic mimics (e.g. sterols, sugars, lipids, proteins, fatty acids) to test a recent physically based model of organic enrichment in sea-spray aerosol [Burrows et al., 2014] that is based on Langmuir absorption equilibria. Experiments were conducted in the UCSD Marine Aerosol Reference Tank (MART) permitting accurate representation of wave breaking processes in the laboratory. We report kappa values for the resulting sea-spray aerosols and compare them to a predictions made using Kappa-Köhler Theory driven by a linear combination of the pure component kappa values. Hygroscopicity determinations made using the model systems are discussed within the context of measurements of CCN activity made using natural, coastal water.
Antarctic polar stratospheric aerosols: The roles of nitrates, chlorides and sulfates
NASA Technical Reports Server (NTRS)
Pueschel, R. F.; Snetsinger, K. G.; Goodman, J. K.; Ferry, G. V.; Oberbeck, V. R.; Verma, S.; Fong, W.
1988-01-01
Nitric and hydrochloric acids have been postulated to condense in the winter polar stratosphere to become an important component of polar stratospheric clouds. One implication is that the removal of NO(y) from the gas phase by this mechanism allows high Cl(x) concentrations to react with O3, because the formation of ClNO3 is inhibited. Contributions of NO3 and Cl to the stratospheric aerosol were determined during the 1987 Airborne Antarctic Ozone Experiment by testing for the presence of nitrates and chlorides in the condensed phase. Aerosol particles were collected on four 500 micron diameter gold wires, each pretreated differently to give results that were specific to certain physical and chemical aerosol properties. One wire was carbon-coated for concentration and size analyses by scanning electron microscopy; X-ray energy dispersive analyses permitted the detection of S and Cl in individual particles. Three more wires were coated with Nitron, barium chloride and silver nitrate, respectively, to detect nitrate, sulfate and chloride in aerosol particles. All three ions, viz., sulfates, nitrates and chlorides were detected in the Antarctic stratospheric aerosol. In terms of number concentrations, the aerosol was dominated by sulfates, followed by chlorides and nitrates. An inverse linear regression can be established between nitrate concentrations and ozone mixing ratio, and between temperature and nitrates.
Aerosol indirect effect on tropospheric ozone via lightning
NASA Astrophysics Data System (ADS)
Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.
2012-12-01
Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications for understanding past and projecting future tropospheric O3 forcing as well as wildfire changes and call for integrated investigations of the coupled aerosol-cloud-chemistry system.
NASA Astrophysics Data System (ADS)
Yorks, J. E.; McGill, M. J.; Nowottnick, E. P.
2015-12-01
Plumes from hazardous events, such as ash from volcanic eruptions and smoke from wildfires, can have a profound impact on the climate system, human health and the economy. Global aerosol transport models are very useful for tracking hazardous plumes and predicting the transport of these plumes. However aerosol vertical distributions and optical properties are a major weakness of global aerosol transport models, yet a key component of tracking and forecasting smoke and ash. The Cloud-Aerosol Transport System (CATS) is an elastic backscatter lidar designed to provide vertical profiles of clouds and aerosols while also demonstrating new in-space technologies for future Earth Science missions. CATS has been operating on the Japanese Experiment Module - Exposed Facility (JEM-EF) of the International Space Station (ISS) since early February 2015. The ISS orbit provides more comprehensive coverage of the tropics and mid-latitudes than sun-synchronous orbiting sensors, with nearly a three-day repeat cycle. The ISS orbit also provides CATS with excellent coverage over the primary aerosol transport tracks, mid-latitude storm tracks, and tropical convection. Data from CATS is used to derive properties of clouds and aerosols including: layer height, layer thickness, backscatter, optical depth, extinction, and depolarization-based discrimination of particle type. The measurements of atmospheric clouds and aerosols provided by the CATS payload have demonstrated several science benefits. CATS provides near-real-time observations of cloud and aerosol vertical distributions that can be used as inputs to global models. The infrastructure of the ISS allows CATS data to be captured, transmitted, and received at the CATS ground station within several minutes of data collection. The CATS backscatter and vertical feature mask are part of a customized near real time (NRT) product that the CATS processing team produces within 6 hours of collection. The continuous near real time CATS data availability is an extraordinary capability and permits vertical profiles of aerosols to flow directly into any aerosol transport model.
NASA Technical Reports Server (NTRS)
Miller, Mark A.; Reynolds, R. M.; Bartholomew, Mary Jane
2001-01-01
The aerosol scattering component of the total radiance measured at the detectors of ocean color satellites is determined with atmospheric correction algorithms. These algorithms are based on aerosol optical thickness measurements made in two channels that lie in the near-infrared portion of the electromagnetic spectrum. The aerosol properties in the near-infrared region are used because there is no significant contribution to the satellite-measured radiance from the underlying ocean surface in that spectral region. In the visible wavelength bands, the spectrum of radiation scattered from the turbid atmosphere is convolved with the spectrum of radiation scattered from the surface layers of the ocean. The radiance contribution made by aerosols in the visible bands is determined from the near-infrared measurements through the use of aerosol models and radiation transfer codes. Selection of appropriate aerosol models from the near-infrared measurements is a fundamental challenge. There are several challenges with respect to the development, improvement, and evaluation of satellite ocean-color atmospheric correction algorithms. A common thread among these challenges is the lack of over-ocean aerosol data. Until recently, one of the most important limitations has been the lack of techniques and instruments to make aerosol measurements at sea. There has been steady progress in this area over the past five years, and there are several new and promising devices and techniques for data collection. The development of new instruments and the collection of more aerosol data from over the world's oceans have brought the realization that aerosol measurements that can be directly compared with aerosol measurements from ocean color satellite measurements are difficult to obtain. There are two problems that limit these types of comparisons: the cloudiness of the atmosphere over the world's oceans and the limitations of the techniques and instruments used to collect aerosol data from ships. To address the latter, we have developed a new type of shipboard sun photometer.
Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes During Boreal Spring and Summer
NASA Technical Reports Server (NTRS)
Lau, William K. M.; Kim, M. K.; Kim, K. M.; Chin, Mian
2005-01-01
Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface tempera- cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.
Energy-based and process-based constraints on aerosol-climate interaction
NASA Astrophysics Data System (ADS)
Suzuki, K.; Sato, Y.; Takemura, T.; Michibata, T.; Goto, D.; Oikawa, E.
2017-12-01
Recent advance in both satellite observations and global modeling provides us with a novel opportunity to investigate the long-standing aerosol-climate interaction issue at a fundamental process level, particularly with a combined use of them. In this presentation, we will highlight our recent progress in understanding the aerosol-cloud-precipitation interaction and its implication for global climate with a synergistic use of a state-of-the-art global climate model (MIROC), a global cloud-resolving model (NICAM) and recent satellite observations (A-Train). In particular, we explore two different aspects of the aerosol-climate interaction issue, i.e. (i) the global energy balance perspective with its modulation due to aerosols and (ii) the process-level characteristics of the aerosol-induced perturbations to cloud and precipitation. For the former, climate model simulations are used to quantify how components of global energy budget are modulated by the aerosol forcing. The moist processes are shown to be a critical pathway that links the forcing efficacy and the hydrologic sensitivity arising from aerosol perturbations. Effects of scattering (e.g. sulfate) and absorbing (e.g. black carbon) aerosols are compared in this context to highlight their distinctively different impacts on climate and hydrologic cycle. The aerosol-induced modulation of moist processes is also investigated in the context of the second aspect above to facilitate recent arguments on possible overestimates of the aerosol-cloud interaction in climate models. Our recent simulations with NICAM are shown to highlight how diverse responses of cloud to aerosol perturbation, which have been failed to represent in traditional climate models, are reproduced by the high-resolution global model with sophisticated cloud microphysics. We will discuss implications of these findings for a linkage between the two aspects above to aid advance process-based understandings of the aerosol-climate interaction and also to mitigate a "dichotomy" recently found by the authors between the two aspects in the context of the climate projection.
Effects of Aerosol on Atmospheric Dynamics and Hydrologic Processes during Boreal Spring and Summer
NASA Technical Reports Server (NTRS)
Lau, William K. M.; Kim, M. K.; Chin, Mian; Kim, K. M.
2005-01-01
Global and regional climate impacts of present-day aerosol loading during boreal spring are investigated using the NASA finite volume General Circulation Model (fvGCM). Three-dimensional distributions of loadings of five species of tropospheric aerosols, i.e., sulfate, black carbon, organic carbon, soil dust, and sea salt are prescribed from outputs of the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The aerosol loadings are used to calculate the extinction coefficient, single scattering albedo, and asymmetric factor at eleven spectral wavelengths in the radiative transfer code. We find that aerosol-radiative forcing during boreal spring excites a wavetrain-like pattern in tropospheric temperature and geopotential height that emanates from Northern Africa, through Eurasia, to northeastern Pacific. Associated with the teleconnection is strong surface cooling over regions with large aerosol loading, i.e., China, India, and Africa. Low-to-mid tropospheric heating due to shortwave absorption is found in regions with large loading of dust (Northern Africa, and central East Asia), and black carbon (South and East Asia). In addition pronounced surface cooling is found over the Caspian Sea and warming over Eurasian and northeastern Asia, where aerosol loadings are relatively low. These warming and cooling are components of teleconnection pattern produced primarily by atmospheric heating from absorbing aerosols, i.e., dust from North Africa and.black carbon from South and East Asia. Effects of aerosols on atmospheric hydrologic cycle in the Asian monsoon region are also investigated. Results show that absorbing aerosols, i.e., black carbon and dust, induce large-scale upper-level heating anomaly over the Tibetan Plateau in April and May, ushering in an early onset of the Indian summer monsoon. Absorbing aerosols also enhance lower-level heating and anomalous ascent over northern India, intensifying the Indian monsoon. Overall, the aerosol-induced large-scale surface temperature cooling leads to a reduction of monsoon rainfall over the East Asia continent, and adjacent oceanic regions.
A scattering methodology for droplet sizing of e-cigarette aerosols.
Pratte, Pascal; Cosandey, Stéphane; Goujon-Ginglinger, Catherine
2016-10-01
Knowledge of the droplet size distribution of inhalable aerosols is important to predict aerosol deposition yield at various respiratory tract locations in human. Optical methodologies are usually preferred over the multi-stage cascade impactor for high-throughput measurements of aerosol particle/droplet size distributions. Evaluate the Laser Aerosol Spectrometer technology based on Polystyrene Sphere Latex (PSL) calibration curve applied for the experimental determination of droplet size distributions in the diameter range typical of commercial e-cigarette aerosols (147-1361 nm). This calibration procedure was tested for a TSI Laser Aerosol Spectrometer (LAS) operating at a wavelength of 633 nm and assessed against model di-ethyl-hexyl-sebacat (DEHS) droplets and e-cigarette aerosols. The PSL size response was measured, and intra- and between-day standard deviations calculated. DEHS droplet sizes were underestimated by 15-20% by the LAS when the PSL calibration curve was used; however, the intra- and between-day relative standard deviations were < 3%. This bias is attributed to the fact that the index of refraction of PSL calibrated particles is different in comparison to test aerosols. This 15-20% does not include the droplet evaporation component, which may reduce droplet size prior a measurement is performed. Aerosol concentration was measured accurately with a maximum uncertainty of 20%. Count median diameters and mass median aerodynamic diameters of selected e-cigarette aerosols ranged from 130-191 nm to 225-293 nm, respectively, similar to published values. The LAS instrument can be used to measure e-cigarette aerosol droplet size distributions with a bias underestimating the expected value by 15-20% when using a precise PSL calibration curve. Controlled variability of DEHS size measurements can be achieved with the LAS system; however, this method can only be applied to test aerosols having a refractive index close to that of PSL particles used for calibration.
Cheng, Tianhai; Wu, Yu; Chen, Hao
2014-06-30
Light absorbing carbon aerosols play a substantial role in climate change through radiative forcing, which is the dominant absorber of solar radiation. Radiative properties of light absorbing carbon aerosols are strongly dependent on the morphological factors and the mixing mechanism of black carbon with other aerosol components. This study focuses on the morphological effects on the optical properties of internally mixed light absorbing carbon aerosols using the numerically exact superposition T-matrix method. Three types aerosols with different aging status such as freshly emitted BC particles, thinly coated light absorbing carbon aerosols, heavily coated light absorbing carbon aerosols are studied. Our study showed that morphological factors change with the aging of internally mixed light absorbing carbon aerosols to result in a dramatic change in their optical properties. The absorption properties of light absorbing carbon aerosols can be enhanced approximately a factor of 2 at 0.67 um, and these enhancements depend on the morphological factors. A larger shell/core diameter ratio of volume-equivalent shell-core spheres (S/C), which indicates the degree of coating, leads to stronger absorption. The enhancement of absorption properties accompanies a greater enhancement of scattering properties, which is reflected in an increase in single scattering albedo (SSA). The enhancement of single scattering albedo due to the morphological effects can reach a factor of 3.75 at 0.67 μm. The asymmetry parameter has a similar yet smaller enhancement. Moreover, the corresponding optical properties of shell-and-core model determined by using Lorenz -Mie solutions are presented for comparison. We found that the optical properties of internally mixed light absorbing carbon aerosol can differ fundamentally from those calculated for the Mie theory shell-and-core model, particularly for thinly coated light absorbing carbon aerosols. Our studies indicate that the complex morphology of internally mixed light absorbing carbon aerosols must be explicitly considered in climate radiation balance.
Quantifying the sensitivity of aerosol optical depths retrieved from MSG SEVIRI to a priori data
NASA Astrophysics Data System (ADS)
Bulgin, C. E.; Palmer, P. I.; Merchant, C. J.; Siddans, R.; Poulsen, C.; Grainger, R. G.; Thomas, G.; Carboni, E.; McConnell, C.; Highwood, E.
2009-12-01
Radiative forcing contributions from aerosol direct and indirect effects remain one of the most uncertain components of the climate system. Satellite observations of aerosol optical properties offer important constraints on atmospheric aerosols but their sensitivity to prior assumptions must be better characterized before they are used effectively to reduce uncertainty in aerosol radiative forcing. We assess the sensitivity of the Oxford-RAL Aerosol and Cloud (ORAC) optimal estimation retrieval of aerosol optical depth (AOD) from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) to a priori aerosol data. SEVIRI is a geostationary satellite instrument centred over Africa and the neighbouring Atlantic Ocean, routinely sampling desert dust and biomass burning outflow from Africa. We quantify the uncertainty in SEVIRI AOD retrievals in the presence of desert dust by comparing retrievals that use prior information from the Optical Properties of Aerosol and Cloud (OPAC) database, with those that use measured aerosol properties during the Dust Outflow and Deposition to the Ocean (DODO) aircraft campaign (August, 2006). We also assess the sensitivity of retrieved AODs to changes in solar zenith angle, and the vertical profile of aerosol effective radius and extinction coefficient input into the retrieval forward model. Currently the ORAC retrieval scheme retrieves AODs for five aerosol types (desert dust, biomass burning, maritime, urban and continental) and chooses the most appropriate AOD based on the cost functions. We generate an improved prior aerosol speciation database for SEVIRI based on a statistical analysis of a Saharan Dust Index (SDI) determined using variances of different brightness temperatures, and organic and black carbon tracers from the GEOS-Chem chemistry transport model. This database is described as a function of season and time of day. We quantify the difference in AODs between those chosen based on prior information from the SDI and GEOS-Chem and those chosen based on the smallest cost function.
International Space Station (ISS)
2001-08-17
Backdropped by a sunrise, the newly installed Materials International Space Station Experiment (MISSE) is visible on this image. MISSE would expose 750 material samples for about 18 months and collect information on how different materials weather the space environment. The objective of MISSE is to develop early, low-cost, non-intrusive opportunities to conduct critical space exposure tests of space materials and components plarned for use on future spacecraft. The experiment was the first externally mounted experiment conducted on the International Space Station (ISS) and was installed on the outside of the ISS Quest Airlock during extravehicular activity (EVA) of the STS-105 mission. MISSE was launched on August 10, 2001 aboard the Space Shuttle Orbiter Discovery.
Kipling, Zak; Stier, Philip; Johnson, Colin E.; ...
2016-02-26
The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3–UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficientlymore » coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3–UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN > 3 nm), while the profiles of larger particles (e.g. CN > 100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. Here, we also show that the processes that affect the AOD-normalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions.« less
Yeh, Hsu-Chi; Chen, Bean T.; Cheng, Yung-Sung; Newton, George J.
1988-08-30
A virtual impactor having improved efficiency and low wall losses in which a core of clean air is inserted into the aerosol flow while aerosol flow is maintained adjacent inner wall surfaces of the focusing portion of the impactor. The flow rate of the core and the length of the throat of the impactor's collection probe, as well as the dimensional relationships of other components of the impactor adjacent the separation region of the impactor, are selected to optimize separation efficiency.
NASA Astrophysics Data System (ADS)
Kaiser, Christopher; Hendricks, Johannes; Righi, Mattia; Jöckel, Patrick
2016-04-01
The reliability of aerosol radiative forcing estimates from climate models depends on the accuracy of simulated global aerosol distribution and composition, as well as on the models' representation of the aerosol-cloud and aerosol-radiation interactions. To help improve on previous modeling studies, we recently developed the new aerosol microphysics submodel MADE3 that explicitly tracks particle mixing state in the Aitken, accumulation, and coarse mode size ranges. We implemented MADE3 into the global atmospheric chemistry general circulation model EMAC and evaluated it by comparison of simulated aerosol properties to observations. Compared properties include continental near-surface aerosol component concentrations and size distributions, continental and marine aerosol vertical profiles, and nearly global aerosol optical depth. Recent studies have shown the specific importance of aerosol vertical profiles for determination of the aerosol radiative forcing. Therefore, our focus here is on the evaluation of simulated vertical profiles. The observational data is taken from campaigns between 1990 and 2011 over the Pacific Ocean, over North and South America, and over Europe. The datasets include black carbon and total aerosol mass mixing ratios, as well as aerosol particle number concentrations. Compared to other models, EMAC with MADE3 yields good agreement with the observations - despite a general high bias of the simulated mass mixing ratio profiles. However, BC concentrations are generally overestimated by many models in the upper troposphere. With MADE3 in EMAC, we find better agreement of the simulated BC profiles with HIPPO data than the multi-model average of the models that took part in the AeroCom project. There is an interesting difference between the profiles from individual campaigns and more "climatological" datasets. For instance, compared to spatially and temporally localized campaigns, the model simulates a more continuous decline in both total aerosol and black carbon mass mixing ratio with altitude than found in the observations. In contrast, measured profiles from the HIPPO project are qualitatively captured well. Similar conclusions hold for the comparison of simulated and measured aerosol particle number concentrations. On the one hand, these results exemplify the difficulty in evaluating the representativeness of the simulated global climatological state of the aerosol by means of comparison with individually measured vertical profiles. On the other hand, it highlights the value of aircraft campaigns with large spatial and temporal coverage for model evaluation.
PM2.5 ORGANIC COMPOSITION FROM SEVERAL SITES IN THE UNITED STATES
Organic constituents make up an important component of fine particulate matter (PM2.5) in ambient environments. While part of the composition of organic aerosol results from emissions of primary sources, an additional component appears to come from gas-to-particle conversion o...
Configuration and Assessment of the GISS ModelE2 Contributions to the CMIP5 Archive
NASA Technical Reports Server (NTRS)
Schmidt, Gavin A.; Kelley, Max; Nazarenko, Larissa; Ruedy, Reto; Russell, Gary L.; Aleinov, Igor; Bauer, Mike; Bauer, Susanne E.; Bhat, Maharaj K.; Bleck, Rainer;
2014-01-01
We present a description of the ModelE2 version of the Goddard Institute for Space Studies (GISS) General Circulation Model (GCM) and the configurations used in the simulations performed for the Coupled Model Intercomparison Project Phase 5 (CMIP5). We use six variations related to the treatment of the atmospheric composition, the calculation of aerosol indirect effects, and ocean model component. Specifically, we test the difference between atmospheric models that have noninteractive composition, where radiatively important aerosols and ozone are prescribed from precomputed decadal averages, and interactive versions where atmospheric chemistry and aerosols are calculated given decadally varying emissions. The impact of the first aerosol indirect effect on clouds is either specified using a simple tuning, or parameterized using a cloud microphysics scheme. We also use two dynamic ocean components: the Russell and HYbrid Coordinate Ocean Model (HYCOM) which differ significantly in their basic formulations and grid. Results are presented for the climatological means over the satellite era (1980-2004) taken from transient simulations starting from the preindustrial (1850) driven by estimates of appropriate forcings over the 20th Century. Differences in base climate and variability related to the choice of ocean model are large, indicating an important structural uncertainty. The impact of interactive atmospheric composition on the climatology is relatively small except in regions such as the lower stratosphere, where ozone plays an important role, and the tropics, where aerosol changes affect the hydrological cycle and cloud cover. While key improvements over previous versions of the model are evident, these are not uniform across all metrics.
Morin, Jean-Paul; Hasson, Virginie; Fall, Mamadou; Papaioanou, Eleni; Preterre, David; Gouriou, Frantz; Keravec, Veronika; Konstandopoulos, Athanasios; Dionnet, Frédéric
2008-06-01
Diesel engine emission aerosol-induced toxicity patterns were compared using both in vitro (organotypic cultures of lung tissue) and in vivo experimentations mimicking the inhalation situation with continuous aerosol flow exposure designs. Using liquid media resuspended diesel particles, we show that toxic response pattern is influenced by the presence of tensioactive agent in the medium which alter particle-borne pollutant bioavailability. Using continuous aerosol exposure in vitro, we show that with high sulfur fuel (300ppm) in the absence of oxidation catalysis, particulate matter was the main toxic component triggering DNA damage and systemic inflammation, while a very limited oxidant stress was evidenced. In contrast, with ultra-low sulfur fuel in the presence of strong diesel oxidation catalysis, the specific role of particulate matter is no longer evidenced and the gas phase then becomes the major component triggering strong oxidant stress, increased NO(2) being the most probable trigger. In vivo, plasma tumor necrosis factor alpha (TNFalpha), lung superoxide dismutase (SOD), catalase and glutathione peroxidase (GPx) activity levels varied in agreement with in vitro observations. Diesel emission treatment with oxycat provokes a marked systemic oxidant stress. Again NO(2) proved to account for a major part of these impacts. In conclusion, similar anti-oxidant responses were observed in in vitro and in vivo experiments after diesel emission aerosol continuous flow exposures. The lung slice organotypic culture model-exposed complex aerosol appears to be a very valuable alternative to in vivo inhalation toxicology experimentations in rodents.
Missing Data Treatments at the Second Level of Hierarchical Linear Models
ERIC Educational Resources Information Center
St. Clair, Suzanne W.
2011-01-01
The current study evaluated the performance of traditional versus modern MDTs in the estimation of fixed-effects and variance components for data missing at the second level of an hierarchical linear model (HLM) model across 24 different study conditions. Variables manipulated in the analysis included, (a) number of Level-2 variables with missing…
Aerosol radiative forcing from GEO satellite data over land surfaces
NASA Astrophysics Data System (ADS)
Costa, Maria J.; Silva, Ana M.
2005-10-01
Aerosols direct and indirect effects on the Earth's climate are widely recognized but have yet to be adequately quantified. Difficulties arise due to the very high spatial and temporal variability of aerosols, which is a major cause of uncertainties in radiative forcing studies. The effective monitoring of the global aerosol distribution is only made possible by satellite monitoring and this is the reason why the interest in aerosol observations from satellite passive radiometers is steadily increasing. From the point of view of the study of land surfaces, the atmosphere with its constituents represents an obscurant whose effects should be as much as possible eliminated, being this process sometimes referred to as atmospheric correction. In absence of clouds and using spectral intervals where gas absorption can be avoided to a great extent, only the aerosol effect remains to be corrected. The monitoring of the aerosol particles present in the atmosphere is then crucial to succeed in doing an accurate atmospheric correction, otherwise the surface properties may be inadequately characterised. However, the atmospheric correction over land surfaces turns out to be a difficult task since surface reflection competes with the atmospheric component of the signal. On the other hand, a single mean pre-established aerosol characterisation would not be sufficient for this purpose due to very high spatial and temporal variability of aerosols and their unpredictability, especially what concerns particulary intense "events" such as biomass burning and forest fires, desert dust episodes and volcanic eruptions. In this context, an operational methodology has been developed at the University of Evora - Evora Geophysics Centre (CGE), in the framework of the Satellite Application Facility for Land Surface Analysis - Land SAF, to derive an Aerosol Product from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) data, flying on the Geostationary (GEO) satellite system Meteosat-8. The aerosol characterization obtained is used to calculate the fluxes and estimate the aerosol radiative forcing at the top of the atmosphere. The methodology along with the results of the aerosol properties and radiative forcing using SEVIRI images is presented. The aerosol optical thickness results are compared with ground-based measurements from the Aerosol Robotic NETwork (AERONET), to assess the accuracy of the methodology presented.
NASA Astrophysics Data System (ADS)
Trainic, M.
2013-12-01
Phytoplankton blooms are responsible for about 50% of the global photosynthesis, thus are a key component of the major nutrient cycles in the ocean. These blooms can be a significant source for flux of volatiles and aerosols, affecting physical chemical processes in the atmosphere. One of the most widely distributed and abundant phytoplankton species in the oceans is the coccolithophore Emiliania huxleyi. In this research, we explore the influence of the different stages of E. huxleyi bloom on the emission of primary aerosols. For this purpose, we conducted a series of controlled lab experiments to measure aerosol emissions during the growth of E. huxleyi. The cultures were grown in a specially designed growth chamber, and the aerosols were generated in a bubbling system. We collected the emitted aerosol particles on filters, and conducted a series of analysis. Scanning electron microscopy (SEM) analysis of the aerosols emitted from E.huxleyi 1216 cultures demonstrate emission of CaCO3 platelets from their exoskeleton into the air, while coccolithophores cells were absent. The results suggest that while healthy coccolithophore cells are too heavy to aerosolize, during cell lysis the coccoliths shed from the coccolithophore cells are emitted into the atmosphere. Therefore, aerosol production during bloom demise may be greater than from healthy E.huxleyi populations. We also investigated the size distribution of the aerosols at various stages of E. huxleyi growth. The presence of calcified cells greatly effects the size distribution of the emitted aerosol population. This work motivated us to explore aerosols emitted during E. huxleyi spring bloom, in a laboratory we constructed onboard the R/V Knorr research vessel, as part of the North Atlantic Virus Infection of Coccolithophore Expedition (June-July 2012). These results have far-reaching implications on the effect of E. huxleyi bloom dynamics on aerosol properties. We not only show that the E. huxleyi calcite shells are emitted as aerosols, but also that aerosol type and therefore chemical composition, microphysical and optical properties depend on the stage of the bloom growth. Unraveling the atmospheric signature of algal bloom dynamics in the ocean will provide novel insights into its ecological and climatic roles.
NASA Astrophysics Data System (ADS)
Artaxo, P.; Barbosa, H. M.; Brito, J.; Carbone, S.; Fiorese, C.; Andre, B.; Rizzo, L. V.; Ditas, F.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Holanda, B. A.; Wang, J.; Souza, R. A. F. D.; Machado, L.; Andreae, M. O.; Martin, S. T.
2016-12-01
The GoAmazon 2014/15 experiment (Observations and Modeling of the Green Ocean Amazon) was a great opportunity to study how urbanization can change aerosol properties under pristine conditions in a tropical rain forest. The experiment took place from January 2014 to December 2015 in the vicinity of Manaus, Brazil, where several sampling stations were operated. Natural biogenic aerosol properties were studied in 3 sampling stations upwind of Manaus (ATTO (T0a), ZF2 (T0z) and EMBRAPA (T0e)). Urban impacted aerosols were analysed in two downwind sampling stations at Tiwa (T2) and Manacapuru (T3). Properties analysed were size distribution, scattering and absorption, composition, vertical profiles and others. Remote sensing measurements were done using AERONET and MODIS, while extensive ground based measurements were done in all sampling stations. Remote sensing measurements shows important changes in aerosol optical depth (AOD), especially in the aerosol absorption component. It was also observed a reduction in cloud droplet size downwind of Manaus for liquid phase clouds. Changes in particle number and size were also very significant, that reflected in changes in the aerosol radiative forcing (RF) before and after Manaus plume. In the dry season, an average RF of -24 w/m² was observed upwind, while -17 w/m² was observed downwind, due to large scale biomass burning aerosols. Single scattering albedo (SSA) at 550 nm changed from a high value of 0.96 upwind to 0.84 downwind due to the increase in absorbing aerosols in the wet season. In the dry season, SSA at 550nm changed from 0.95 to 0.87. Aerosol composition showed a large dominance of organic aerosols for all sites, accounting for 65-75% of PM1 non refractory aerosol. Most of these were secondary organic aerosol (SOA), with very low sulfate and nitrate concentrations. The influence of the Manaus plume on aerosol properties was more intense during the wet season, because in the dry season a significant amount of large scale biomass burning aerosol was observed for all GoAmazon 2014/15 sites.