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Sample records for aerosol hygroscopicity parameter

  1. Mass-based hygroscopicity parameter interaction model and measurement of atmospheric aerosol water uptake

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Rose, D.; Pöschl, U.

    2013-01-01

    In this study we derive and apply a mass-based hygroscopicity parameter interaction model for efficient description of concentration-dependent water uptake by atmospheric aerosol particles with complex chemical composition. The model approach builds on the single hygroscopicity parameter model of Petters and Kreidenweis (2007). We introduce an observable mass-based hygroscopicity parameter κm which can be deconvoluted into a dilute hygroscopicity parameter (κm0) and additional self- and cross-interaction parameters describing non-ideal solution behavior and concentration dependencies of single- and multi-component systems. For reference aerosol samples of sodium chloride and ammonium sulfate, the κm-interaction model (KIM) captures the experimentally observed concentration and humidity dependence of the hygroscopicity parameter and is in good agreement with an accurate reference model based on the Pitzer ion-interaction approach (Aerosol Inorganic Model, AIM). Experimental results for pure organic particles (malonic acid, levoglucosan) and for mixed organic-inorganic particles (malonic acid - ammonium sulfate) are also well reproduced by KIM, taking into account apparent or equilibrium solubilities for stepwise or gradual deliquescence and efflorescence transitions. The mixed organic-inorganic particles as well as atmospheric aerosol samples exhibit three distinctly different regimes of hygroscopicity: (I) a quasi-eutonic deliquescence & efflorescence regime at low-humidity where substances are just partly dissolved and exist also in a non-dissolved phase, (II) a gradual deliquescence & efflorescence regime at intermediate humidity where different solutes undergo gradual dissolution or solidification in the aqueous phase; and (III) a dilute regime at high humidity where the solutes are fully dissolved approaching their dilute hygroscopicity. For atmospheric aerosol samples collected from boreal rural air and from pristine tropical rainforest air (secondary

  2. Hygroscopic Characteristics of Alkylaminium Carboxylate Aerosols.

    PubMed

    Gomez-Hernandez, Mario; McKeown, Megan; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Lavi, Avi; Rudich, Yinon; Collins, Don R; Zhang, Renyi

    2016-03-01

    The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity for a series of alkylaminium carboxylate aerosols have been measured using a hygroscopicity tandem differential mobility analyzer coupled to a condensation particle counter and a CCN counter. The particles, consisting of the mixtures of mono- (acetic, propanoic, p-toluic, and cis-pinonic acid) and dicarboxylic (oxalic, succinic, malic, adipic, and azelaic acid) acid with alkylamine (mono-, di-, and trimethylamines), represent those commonly found under diverse environmental conditions. The hygroscopicity parameter (κ) of the alkylaminium carboxylate aerosols was derived from the HGF and CCN results and theoretically calculated. The HGF at 90% RH is in the range of 1.3 to 1.8 for alkylaminium monocarboxylates and 1.1 to 2.2 for alkylaminium dicarboxylates, dependent on the molecular functionality (i.e., the carboxylic or OH functional group in organic acids and methyl substitution in alkylamines). The κ value for all alkylaminium carboxylates is in the range of 0.06-1.37 derived from the HGF measurements at 90% RH, 0.05-0.49 derived from the CCN measurements, and 0.22-0.66 theoretically calculated. The measured hygroscopicity of the alkylaminium carboxylates increases with decreasing acid to base ratio. The deliquescence point is apparent for several of the alkylaminium dicarboxylates but not for the alkylaminium monocarboxylates. Our results reveal that alkylaminium carboxylate aerosols exhibit distinct hygroscopic and deliquescent characteristics that are dependent on their molecular functionality, hence regulating their impacts on human health, air quality, and direct and indirect radiative forcing on climate. PMID:26794419

  3. A case study of single hygroscopicity parameter and its link to the functional groups and phase transition for urban aerosols in Taipei City

    NASA Astrophysics Data System (ADS)

    Hung, Hui-Ming; Hsu, Chia-Hung; Lin, Wei-Ting; Chen, Yu-Quan

    2016-05-01

    The hygroscopicity, functional groups and phase transitions of urban aerosol particles in Taipei City were studied using a cloud condensation nuclei counter (CCNc) with a scanning mobility particle sizer (SMPS) and an attenuated total reflectance with infrared (ATR-IR) detection technique. With the assumption of larger particles being activated first, the derived single hygroscopicity parameter (κ) exhibited an increasing trend with particle size, i.e., from 0.022 ± 0.01 at 87 ± 10 nm to 0.13 ± 0.03 at 240 ± 20 nm. The collected size-selected particles were characterized using ATR-IR for the functional groups of alkyl, carbonyl, ammonium, sulfate and nitrate, which showed various size dependence patterns, linked to different formation mechanisms. The hygroscopic response based on the ratio (xW_solute) for sample film of absorption by the enhanced water-stretching peak to that by the selected solute showed a better consistency with pure ammonium sulfate for sub-micron size particles. Based on the derived ammonium sulfate volume fraction from IR analysis, the κ received from CCNc measurements was concluded mainly contributed by ammonium sulfate for sub-micrometer particles. The increasing trend of sodium nitrate absorbance at aerosol diameter ≥1 μm was due to a reaction of nitric acid with sea salt particles. The micrometer sized particles were apparent not only in a significantly higher xW_solute than pure sodium nitrate but also had a deliquescence RH of 69 ± 1%, similar to that of sodium nitrate-sodium chloride mixtures. Overall, the organic species in this study exhibited a low hygroscopicity with less than 0.036 of contribution for the overall κ, and the major hygroscopic material of urban aerosols consisted primarily of ammonium sulfate in the sub-micrometer particles and sodium nitrate with sea salt in the coarse particles.

  4. The impact of marine surface organic enrichment on the measured hygroscopicity parameter of laboratory generated sea-spray aerosols

    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.

  5. The hygroscopicity of indoor aerosol particles

    SciTech Connect

    Wei, L.

    1993-07-01

    A system to study the hygroscopic growth of particle was developed by combining a Tandem Differential Mobility Analyzer (TDMA) with a wetted wall reactor. This system is capable of mimicking the conditions in human respiratory tract, and measuring the particle size change due to the hygroscopic growth. The performance of the system was tested with three kinds of particles of known composition, NaCl, (NH{sub 4}){sub 2}SO{sub 4}, and (NH{sub 4})HS0{sub 4} particles. The hygroscopicity of a variety of common indoor aerosol particles was studied including combustion aerosols (cigarette smoking, cooking, incenses and candles) and consumer spray products such as glass cleaner, general purpose cleaner, hair spray, furniture polish spray, disinfectant, and insect killer. Experiments indicate that most of the indoor aerosols show some hygroscopic growth and only a few materials do not. The magnitude of hygroscopic growth ranges from 20% to 300% depending on the particle size and fraction of water soluble components.

  6. A case study of single hygroscopicity parameter and its link to the functional groups and phase transition for urban aerosols in Taipei City

    NASA Astrophysics Data System (ADS)

    Hung, Hui-Ming; Hsu, Chia-Hung; Lin, Wei-Ting; Chen, Yu-Quan

    2016-05-01

    The hygroscopicity, functional groups and phase transitions of urban aerosol particles in Taipei City were studied using a cloud condensation nuclei counter (CCNc) with a scanning mobility particle sizer (SMPS) and an attenuated total reflectance with infrared (ATR-IR) detection technique. With the assumption of larger particles being activated first, the derived single hygroscopicity parameter (κ) exhibited an increasing trend with particle size, i.e., from 0.022 ± 0.01 at 87 ± 10 nm to 0.13 ± 0.03 at 240 ± 20 nm. The collected size-selected particles were characterized using ATR-IR for the functional groups of alkyl, carbonyl, ammonium, sulfate and nitrate, which showed various size dependence patterns, linked to different formation mechanisms. The hygroscopic response based on the ratio (xW_solute) for sample film of absorption by the enhanced water-stretching peak to that by the selected solute showed a better consistency with pure ammonium sulfate for sub-micron size particles. Based on the derived ammonium sulfate volume fraction from IR analysis, the κ received from CCNc measurements was concluded mainly contributed by ammonium sulfate for sub-micrometer particles. The increasing trend of sodium nitrate absorbance at aerosol diameter ≥1 μm was due to a reaction of nitric acid with sea salt particles. The micrometer sized particles were apparent not only in a significantly higher xW_solute than pure sodium nitrate but also had a deliquescence RH of 69 ± 1%, similar to that of sodium nitrate-sodium chloride mixtures. Overall, the organic species in this study exhibited a low hygroscopicity with less than 0.036 of contribution for the overall κ, and the major hygroscopic material of urban aerosols consisted primarily of ammonium sulfate in the sub-micrometer particles and sodium nitrate with sea salt in the coarse particles.

  7. Hygroscopic growth of urban aerosol particles during the 2009 Mirage-Shanghai Campaign

    NASA Astrophysics Data System (ADS)

    Ye, Xingnan; Tang, Chen; Yin, Zi; Chen, Jianmin; Ma, Zhen; Kong, Lingdong; Yang, Xin; Gao, Wei; Geng, Fuhai

    2013-01-01

    The hygroscopic properties of submicrometer urban aerosol particles were studied during the 2009 Mirage-Shanghai Campaign. The urban aerosols were composed of more-hygroscopic and nearly-hydrophobic particles, together with a trace of less-hygroscopic particles. The mean hygroscopicity parameter κ of the more-hygroscopic mode varied in the range of 0.27-0.39 depending on particle size. The relative abundance of the more-hygroscopic particles at any size was ca. 70%, slightly increasing with particle size. The number fraction of the nearly-hydrophobic particles fluctuated between 0.1 and 0.4 daily, in accordance with traffic emissions and atmospheric diffusion. The results from relative humidity dependence on hygroscopic growth and chemical analysis of fine particles indicated that particulate nitrate formation through the homogenous gas-phase reaction was suppressed under ammonia-deficient atmosphere in summer whereas the equilibrium was broken by more available NH3 during adverse meteorological conditions.

  8. Relating hygroscopicity and composition of organic aerosol particulate matter

    SciTech Connect

    Duplissy, J.; DeCarlo, P. F.; Dommen, J.; Alfarra, M. R.; Metzger, A.; Barmpadimos, I.; Prevot, A. S. H.; Weingartner, E.; Tritscher, T.; Gysel, M.; Aiken, A. C.; Jimenez, J. L.; Canagaratna, M. R.; Worsnop, D. R.; Collins, D. R.; Tomlinson, J.; Baltensperger, U.

    2011-01-01

    A hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f44). m/z 44 is due mostly to the ion fragment CO2+ for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfraujoch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation between the hygroscopicity of OA at subsaturated RH, as given by the hygroscopic growth factor (GF) or "κorg" parameter, and f44 was determined and is given by κorg = 2.2 × f44 - 0.13. This approximation can be further verified and refined as the database for AMS and HTDMA measurements is constantly being expanded around the world. Finally, the use of this approximation could introduce an important simplification in the parameterization of hygroscopicity of OA in atmospheric models, since f44 is correlated with the photochemical age of an air mass.

  9. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    NASA Astrophysics Data System (ADS)

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2015-04-01

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined here as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1-0.15 and 0.9-1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.

  10. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    DOE PAGESBeta

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2015-04-17

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined heremore » as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.« less

  11. Aerosol optical hygroscopicity measurements during the 2010 CARES Campaign

    DOE PAGESBeta

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2014-12-10

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 CARES study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GF) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles, yielding κ = 0.1–0.15 and 0.9–1.0, respectively. Themore » derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.« less

  12. Aerosol optical hygroscopicity measurements during the 2010 CARES Campaign

    NASA Astrophysics Data System (ADS)

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2014-12-01

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 CARES study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GF) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles, yielding κ = 0.1-0.15 and 0.9-1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.

  13. Effect of Aerosol Size and Hygroscopicity on Aerosol Optical Depth in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Brock, Charles; Wagner, Nick; Gordon, Timothy

    2016-04-01

    Aerosol optical depth (AOD) is affected by the size, optical characteristics, and hygroscopicity of particles, confounding attempts to link remote sensing observations of AOD to measured or modeled aerosol mass concentrations. In situ airborne observations of aerosol optical, chemical, microphysical and hygroscopic properties were made in the southeastern United States in the daytime in summer 2013. We use these observations to constrain a simple model that is used to test the sensitivity of AOD to the various measured parameters. As expected, the AOD was found to be most sensitive to aerosol mass concentration and to aerosol water content, which is controlled by aerosol hygroscopicity and the ambient relative humidity. However, AOD was also fairly sensitive to the mean particle diameter and the width of the size distribution. These parameters are often prescribed in global models that use simplified modal parameterizations to describe the aerosol, suggesting that the values chosen could substantially bias the calculated relationship between aerosol mass and optical extinction, AOD, and radiative forcing.

  14. Numerical Model to Characterize the Size Increase of Combination Drug and Hygroscopic Excipient Nanoparticle Aerosols

    PubMed Central

    Longest, P. Worth; Hindle, Michael

    2011-01-01

    Enhanced excipient growth is a newly proposed respiratory delivery strategy in which submicrometer or nanometer particles composed of a drug and hygroscopic excipient are delivered to the airways in order to minimize extrathoracic depositional losses and maximize lung retention. The objective of this study was to develop a validated mathematical model of aerosol size increase for hygroscopic excipients and combination excipient-drug particles and to apply this model to characterize growth under typical respiratory conditions. Compared with in vitro experiments, the droplet growth model accurately predicted the size increase of single component and combination drug and excipient particles. For typical respiratory drug delivery conditions, the model showed that droplet size increase could be effectively correlated with the product of a newly defined hygroscopic parameter and initial volume fractions of the drug and excipient in the particle. A series of growth correlations was then developed that successively included the effects of initial drug and excipient mass loadings, initial aerosol size, and aerosol number concentration. Considering EEG delivery, large diameter growth ratios (2.1–4.6) were observed for a range of hygroscopic excipients combined with both hygroscopic and non-hygroscopic drugs. These diameter growth ratios were achieved at excipient mass loadings of 50% and below and at realistic aerosol number concentrations. The developed correlations were then used for specifying the appropriate initial mass loadings of engineered insulin nanoparticles in order to achieve a predetermined size increase while maximizing drug payload and minimizing the amount of hygroscopic excipient. PMID:21804683

  15. Hygroscopic growth of aerosol particles in the Po Valley

    NASA Astrophysics Data System (ADS)

    Svenningsson, I. B.; Hansson, H.-C.; Wiedensohler, A.; Ogren, J. A.; Noone, K. J.; Hallberg, A.

    1992-11-01

    A Tandem Differential Mobility Analyser (TDMA) was used to study the hygroscopic growth of individual ambient aerosol particles in the Po Valley, Italy. The measurements were made during the GCE fog experiment in November 1989. During fog, the interstitial aerosol (Dp(at ambient relative humidity)<5µm) was sampled. Two modes of particles with different hygroscopic growth were found for 0.030µmhygroscopic mode and 1.1±0.07 for the less-hygroscopic mode. The growth factors and the proportion of the particles that were less hygroscopic varied considerably from day to day, but no significant size dependence was seen. Comparison of growth factors for pure salt particles and the measured growth factors indicates that both hygroscopic modes contain a major insoluble part. The effect of the external mixing of hygroscopic properties on the activation of particles to fog droplets is discussed and the fraction of particles that were activated as a function of particle size is predicted. Comparison with the measured scavenging fraction as a function of particle size shows that the hygroscopic properties of the individual particle are as important as the particle size in determining if it will be activated in a fog.

  16. Comparison of aerosol hygroscopicity and mixing state between winter and summer seasons in Pearl River Delta region, China

    NASA Astrophysics Data System (ADS)

    Jiang, Rongxin; Tan, Haobo; Tang, Lili; Cai, Mingfu; Yin, Yan; Li, Fei; Liu, Li; Xu, Hanbing; Chan, P. W.; Deng, Xuejiao; Wu, Dui

    2016-03-01

    Hygroscopic properties of aerosol particles are important for determining aerosol size distributions, and thus determining scattering and absorption coefficients at ambient atmospheric conditions. In this study, hygroscopic properties of aerosol particles at an urban site in Guangzhou, China, were measured using a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) system during the winter and the summer. The results show that the urban aerosols were composed of more-hygroscopic, less-hygroscopic and non-hygroscopic particles. For less-hygroscopic particles of 40-200 nm in diameter, the hygroscopic parameter κLH was around 0.15. For more-hygroscopic particles, the κMH was from 0.290 to 0.339 with a particle size from 40 to 200 nm. For non-hygroscopic particles, the κNH was about 0.015. It was found that the number fraction of less-hygroscopic particles (NFLH) was correlated with the atmospheric oxidation which can be presented by OC/EC. This paper attributed the larger NFLH in winter to the higher value of OC/EC (3.0). Such conditions may lead to more formation of less-hygroscopic particles. Backward trajectories cluster analysis shows that there is a certain link between air mass origin and aerosol hygroscopicity, but it seems to be independent of the level of pollution. The difference of NFNH indicates that the mixing state of aerosol particles can also be affected by air mass origin. Diurnal variations in aerosol hygroscopic parameters in both seasons show that during daytime, aerosol particles tend to have a low degree of external mixing or quasi-internal mixing, resulting in a higher NFMH and a larger κmean; during nighttime and early mornings, they tend to be mixed externally, resulting in a lower NFMH and a smaller κmean. This can be attributed to atmospheric aging effect and evolution of mixing layer height and implies that soot (non-hygroscopic) particles present to a large extent as internal mixtures by the time they leave the urban

  17. CMAQ validation of optical parameters and PM2.5 based on lidar and sky radiometers: a sensitivity study of optical parameters to hygroscopic aerosols

    NASA Astrophysics Data System (ADS)

    Vladutescu, Daniela Viviana; Garofalo, Erika; Gross, Barry; Moshary, Fred; Ahmed, Samir

    2009-08-01

    With the dramatically climate changing we are facing today atmospheric monitoring is of major importance. Several atmospheric monitoring instruments are used for measuring atmospheric composition, optical coefficients, PM2.5, aerosol optical depth, size distribution, PBL height and many other parameters. However an inexpensive method of determining these parameters is by use of models and one model that depicts the aerosol dynamics in the atmosphere is the Community Multi-scale Air Quality (CMAQ) model. Our paper is focused on converting CMAQ retrieval outputs into optical coefficients that can then be comparing the lidar, AERONET and TEOM measurements performed at City College of the City University of New York . Differences between the full approach and parameterized methods such as the MALM formula used in AIR-NOW are observed and comparisons with AERONET show the full modeling is in general superior to the MALM formula.

  18. Initial size distributions and hygroscopicity of indoor combustion aerosol particles

    SciTech Connect

    Li, W.; Hopke, P.K.

    1993-10-01

    Cigarette smoke, incense smoke, natural gas flames, propane fuel flames, and candle flames are contributors of indoor aerosol particles. To provide a quantitative basis for the modeling of inhaled aerosol deposition pattern, the hygroscopic growth of particles from these five sources as well as the source size distributions were measured. Because the experiments were performed on the bases of particles of single size, it provided not only the averaged particle`s hygroscopic growth of each source, but also the detailed size change for particles of different sizes within the whole size spectrum. The source particle size distribution measurements found that cigarette smoke and incense smoke contained particles in the size range of 100-700 nm, while the natural gas, propane, and candle flames generated particles between 10 and 100 nm. The hygroscopic growth experiments showed that these combustion aerosol particles could grow 10% to 120%, depending on the particle sizes and origins. 18 refs., 15 figs., 3 tabs.

  19. Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

    NASA Astrophysics Data System (ADS)

    Phillips, B.; Dawson, K. W.; Royalty, T. M.; Reed, R. E.; Petters, M.; Meskhidze, N.

    2015-12-01

    Atmospheric aerosols play a central role in many environmental processes by influencing the Earth's radiative balance, tropospheric chemistry, clouds, biogeochemical cycles, and visibility as well as adversely impacting human health. Based on their origin, atmospheric aerosols can be defined as anthropogenic or natural. Recent studies have shown that a large fraction of uncertainty in the radiative effects of anthropogenic aerosols is related to uncertainty in natural—background—aerosols. Marine aerosols are of particular interest due to the abundance of oceans covering the Earth's surface. Despite their importance, limited information is currently available for size- and composition-resolved marine aerosol emission fluxes. Our group has designed and built an instrument for measuring the size- and hygroscopicity-resolved sea spray aerosol fluxes. The instrument was first deployed during spring 2015 at the end of the 560 m pier of the US Army Corps of Engineers' Field Research Facility in Duck, NC. Measurements include 200 nm-sized diameter growth factor (hygroscopicity) distributions, sea spray particle flux measurements, and total sub-micron sized aerosol concentration. Ancillary ocean data includes salinity, pH, sea surface temperature, dissolved oxygen content, and relative fluorescence (proxy for [Chl-a]). Hygroscopicity distribution measurements show two broad peaks, one indicative of organics and sulfates and another suggestive of sea salt. The fraction of 200 nm-sized salt particles having hygroscopicity similar to that of sea-spray aerosol contributes up to ~24% of the distribution on days with high-speed onshore winds and up to ~3% on calm days with winds blowing from the continent. However, the total concentration of sea-spray-like particles originating from offshore versus onshore winds was relatively similar. Changes in the relative contribution of sea-salt to number concentration were caused by a concomitant changes in total aerosol concentration

  20. Vertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, Bernadette; Gysel, Martin; Rubach, Florian; Mentel, Thomas F.; Goger, Brigitta; Poulain, Laurent; Schlag, Patrick; Miettinen, Pasi; Pajunoja, Aki; Virtanen, Annele; Klein Baltink, Henk; Bas Henzing, J. S.; Größ, Johannes; Gobbi, Gian Paolo; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Decesari, Stefano; Facchini, Maria Cristina; Weingartner, Ernest; Baltensperger, Urs

    2016-06-01

    Vertical profiles of the aerosol particles hygroscopic properties, their mixing state as well as chemical composition were measured above northern Italy and the Netherlands. An aerosol mass spectrometer (AMS; for chemical composition) and a white-light humidified optical particle spectrometer (WHOPS; for hygroscopic growth) were deployed on a Zeppelin NT airship within the PEGASOS project. This allowed one to investigate the development of the different layers within the planetary boundary layer (PBL), providing a unique in situ data set for airborne aerosol particles properties in the first kilometre of the atmosphere. Profiles measured during the morning hours on 20 June 2012 in the Po Valley, Italy, showed an increased nitrate fraction at ˜ 100 m above ground level (a.g.l.) coupled with enhanced hygroscopic growth compared to ˜ 700 m a. g. l. This result was derived from both measurements of the aerosol composition and direct measurements of the hygroscopicity, yielding hygroscopicity parameters (κ) of 0.34 ± 0.12 and 0.19 ± 0.07 for 500 nm particles, at ˜ 100 and ˜ 700 m a. g. l., respectively. The difference is attributed to the structure of the PBL at this time of day which featured several independent sub-layers with different types of aerosols. Later in the day the vertical structures disappeared due to the mixing of the layers and similar aerosol particle properties were found at all probed altitudes (mean κ ≈ 0.18 ± 0.07). The aerosol properties observed at the lowest flight level (100 m a. g. l.) were consistent with parallel measurements at a ground site, both in the morning and afternoon. Overall, the aerosol particles were found to be externally mixed, with a prevailing hygroscopic fraction. The flights near Cabauw in the Netherlands in the fully mixed PBL did not feature altitude-dependent characteristics. Particles were also externally mixed and had an even larger hygroscopic fraction compared to the results in Italy. The mean κ from

  1. The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

    PubMed

    Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

    2015-06-24

    Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate. PMID:27162963

  2. The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol

    PubMed Central

    2015-01-01

    Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle–particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle–particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate. PMID:27162963

  3. Water Uptake and Hygroscopic Growth of Organosulfate Aerosol.

    PubMed

    Estillore, Armando D; Hettiyadura, Anusha P S; Qin, Zhen; Leckrone, Erin; Wombacher, Becky; Humphry, Tim; Stone, Elizabeth A; Grassian, Vicki H

    2016-04-19

    Organosulfates (OS) are important components of secondary organic aerosol (SOA) that have been identified in numerous field studies. This class of compounds within SOA can potentially affect aerosol physicochemical properties such as hygroscopicity because of their polar and hydrophilic nature as well as their low volatility. Currently, there is a dearth of information on how aerosol particles that contain OS interact with water vapor in the atmosphere. Herein we report a laboratory investigation on the hygroscopic properties of a structurally diverse set of OS salts at varying relative humidity (RH) using a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA). The OS studied include the potassium salts of glycolic acid sulfate, hydroxyacetone sulfate, 4-hydroxy-2,3-epoxybutane sulfate, and 2-butenediol sulfate and the sodium salts of benzyl sulfate, methyl sulfate, ethyl sulfate, and propyl sulfate. In addition, mixtures of OS and sodium chloride were also studied. The results showed gradual deliquescence of these aerosol particles characterized by continuous uptake and evaporation of water in both hydration and dehydration processes for the OS, while the mixture showed prompt deliquescence and effloresce transitions, albeit at a lower relative humidity relative to pure sodium chloride. Hygroscopic growth of these OS at 85% RH were also fit to parameterized functional forms. This new information provided here has important implications about the atmospheric lifetime, light scattering properties, and the role of OS in cloud formation. Moreover, results of these studies can ultimately serve as a basis for the development and evaluation of thermodynamic models for these compounds in order to consider their impact on the atmosphere. PMID:26967467

  4. Characterization of the Changes in Hygroscopicity of Ambient Organic Aerosol due to Oxidation by Gas Phase OH

    NASA Astrophysics Data System (ADS)

    Wong, J. P.; McWhinney, R. D.; Slowik, J. G.; Abbatt, J.

    2011-12-01

    Despite the ubiquitous nature of organic aerosols and their importance in climate forcing, the influence of chemical processes on their ability to act as cloud condensation nuclei (CCN) in the atmosphere remains uncertain. Changes to the hygroscopicity of ambient organic aerosol due to OH oxidation were explored at a remote forested (Whistler, British Columbia) and an urban (Toronto, Ontario) site. Organic aerosol was exposed to controlled levels of OH radicals in a portable flow tube reactor, the Toronto Photo-Oxidation Tube (TPOT). An Aerodyne Aerosol Mass Spectrometer (AMS) monitored the changes in the chemical composition due to OH-initiated oxidation. The CCN activity of size-selected particles was measured with a DMT Cloud Condensation Nuclei Counter (CCNc) to determine the hygroscopicity parameter, κ. Preliminary results suggest that gas phase OH oxidation increases the degree of oxygenation of organic aerosol, leading to increases in hygroscopicity. These results yield insights into the mechanism by which oxidation affects the hygroscopicity of ambient aerosol of various sources, and to constrain the main aging process that leads to the observation of increasing hygroscopicity with increasing oxidation of organic aerosol.

  5. [Hygroscopic Properties of Aerosol Particles in North Suburb of Nanjing in Spring].

    PubMed

    Xu, Bin; Zhang, Ze-feng; Li, Yan-weil; Qin, Xin; Miao, Qing; Shen, Yan

    2015-06-01

    The hygroscopic properties of submicron aerosol particles have significant effects on spectral distribution, CCN activation, climate forcing, human health and so on. A Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) was utilized to analyze the hygroscopic properties of aerosol particles in the northern suburb of Nanjing during 16 April to 21 May, 2014. At relative humidity (RH) of 90%, for particles with dry diameters 30-230 nm, the probability distribution of GF (GF-PDF) shows a distinct bimodal pattern, with a dominant more-hygroscopic group and a smaller less-hygroscopic group. A contrast analysis between day and night suggests that, aerosol particles during day time have a stronger hygroscopicity and a higher number fraction of more-hygroscopic group than that at night overall. Aerosol particles during night have a higher degree of externally mixed state. Backward trajectory analysis using HYSPLIT mode reveals that, the sampling site is mainly affected by three air masses. For aitken nuclei, northwest continental air masses experience a longer aging process and have a stronger hygroscopicity. For condensation nuclei, east air masses have a stronger hygroscopicity and have a higher number fraction of more-hygroscopic group. Aerosol particles in local air masses have a high number fraction of more-hygroscopic group in the whole diameter range. PMID:26387289

  6. Long term measurements of the estimated hygroscopic enhancement of aerosol optical properties

    NASA Astrophysics Data System (ADS)

    Hervo, Maxime; Sellegri, Karine; Pichon, Jean Marc; Roger, Jean Claude; Laj, Paolo

    2015-04-01

    Water vapour has a major impact on aerosol optical properties, thus on the Radiative Forcing for aerosol-radiation interaction (RFari). However there is few studies measuring this impact over a large period. Optical properties of aerosols were measured at the GAW Puy de Dôme station (1465m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the dry optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the planetary boundary layer height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type and the season. At 90% humidity, the scattering factor enhancement (fsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH= 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type. To our knowledge, these results are one of the first presenting the impact of water vapour on the aerosol optical properties for a long period, and the first for a site at the border between the planetary boundary layer

  7. Estimation of aerosol optical properties considering hygroscopicity and light absorption

    NASA Astrophysics Data System (ADS)

    Jung, Chang Hoon; Lee, Ji Yi; Kim, Yong Pyo

    2015-03-01

    In this study, the influences of water solubility and light absorption on the optical properties of organic aerosols were investigated. A size-resolved model for calculating optical properties was developed by combining thermodynamic hygroscopic growth and aerosol dynamics models. The internal mixtures based on the homogeneous and core-shell mixing were compared. The results showed that the radiative forcing (RF) of Water Soluble Organic Carbon (WSOC) aerosol can be estimated to range from -0.07 to -0.49 W/m2 for core-shell mixing and from -0.09 to -0.47 W/m2 for homogeneous mixing under the simulation conditions (RH = 60%). The light absorption properties of WSOC showed the mass absorption efficiency (MAE) of WSOC can be estimated 0.43-0.5 m2/g, which accounts for 5-10% of the MAE of elemental carbon (EC). The effect on MAE of increasing the imaginary refractive index of WSOC was also calculated, and it was found that increasing the imaginary refractive index by 0.001i enhanced WSOC aerosol absorption by approximately 0.02 m2/g. Finally, the sensitivity test results revealed that changes in the fine mode fraction (FMF) and in the geometric mean diameter of the accumulation mode play important roles in estimating RF during hygroscopic growth.

  8. Aerosol optical properties in the southeastern United States in summer - Part 1: Hygroscopic growth

    NASA Astrophysics Data System (ADS)

    Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.

    2016-04-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made during May-September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at relative humidities (RHs) of ˜ 15, ˜ 70, and ˜ 90 % and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. The calculated enhancement in hydrated aerosol extinction with relative humidity, f(RH), calculated by this method agreed well with the observed f(RH) at ˜ 90 % RH. The dominance of organic aerosol, which comprised 65 ± 10 % of particulate matter with aerodynamic diameter < 1 µm in the planetary boundary layer, resulted in relatively low f(RH) values of 1.43 ± 0.67 at 70 % RH and 2.28 ± 1.05 at 90 % RH. The subsaturated κ-Köhler hygroscopicity parameter κ for the organic fraction of the aerosol must have been < 0.10 to be consistent with 75 % of the observations within uncertainties, with a best estimate of κ = 0.05. This subsaturated κ value for the organic aerosol in the southeastern US is broadly consistent with field studies in rural environments. A new, physically based, single-parameter representation was developed that better described f(RH) than did the widely used gamma power-law approximation.

  9. Vertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, B.; Gysel, M.; Rubach, F.; Mentel, T. F.; Goger, B.; Poulain, L.; Schlag, P.; Miettinen, P.; Pajunoja, A.; Virtanen, A.; Bialek, J.; Klein Baltink, H.; Henzing, J. S.; Größ, J.; Gobbi, G. P.; Wiedensohler, A.; Kiendler-Scharr, A.; O'Dowd, C.; Decesari, S.; Facchini, M. C.; Weingartner, E.; Baltensperger, U.

    2015-03-01

    Airborne measurements of the aerosol hygroscopic and optical properties as well as chemical composition were performed in the Netherlands and northern Italy on board of a Zeppelin NT airship during the PEGASOS field campaigns in 2012. The vertical changes in aerosol properties during the development of the mixing layer were studied. Hygroscopic growth factors (GF) at 95% relative humidity were determined using the white-light humidified optical particles spectrometer (WHOPS) for dry diameters of 300 and 500 nm particles. These measurements were supplemented by an aerosol mass spectrometer (AMS) and an aethalometer providing information on the aerosol chemical composition. Several vertical profiles between 100 and 700 m a.g. were flown just after sunrise close to the San Pietro Capofiume ground station in the Po Valley, Italy. During the early morning hours the lowest layer (newly developing mixing layer) contained a high nitrate fraction (20%) which was coupled with enhanced hygroscopic growth. In the layer above (residual layer) small nitrate fractions of ~ 2% were measured as well as low GFs. After full mixing of the layers, typically around noon and with increased temperature, the nitrate fraction decreased to 2% at all altitudes and led to similar hygroscopicity values as found in the residual layer. These distinct vertical and temporal changes underline the importance of airborne campaigns to study aerosol properties during the development of the mixed layer. The aerosol was externally mixed with 22 and 67% of the 500 nm particles in the range GF < 1.1 and GF > 1.5, respectively. Contributors to the non-hygroscopic mode in the observed size range are most likely mineral dust and biological material. Mean hygroscopicity parameters (κ) were 0.34, 0.19 and 0.18 for particles in the newly forming mixing layer, residual layer and fully mixed layer, respectively. These results agree well with those from chemical analysis which found values of κ = 0.27, 0.21 and 0

  10. Vertical profiles of cloud condensation nuclei, aerosol hygroscopicity, water uptake, and scattering across the United States

    NASA Astrophysics Data System (ADS)

    Lin, J. J.; Bougiatioti, A.; Nenes, A.; Anderson, B. E.; Beyersdorf, A. J.; Brock, C. A.; Gordon, T. D.; Lack, D.; Law, D. C.; Liao, J.; Middlebrook, A. M.; Richardson, M.; Thornhill, K. L., II; Winstead, E.; Wagner, N. L.; Welti, A.; Ziemba, L. D.

    2014-12-01

    The evolutions of vertical distributions of aerosol chemical, microphysical, hygroscopic, and optical properties present fundamental challenges to the understanding of ground-level air quality and radiative transfer, and few datasets exist to date for evaluation of atmospheric models. Data collected from recent NASA and NOAA field campaigns in the California Central Valley (DISCOVER-AQ), southeast United States (SENEX, SEAC4RS) and Texas (DISCOVER-AQ) allow for a unique opportunity to constrain vertical profiles of climate-relevant aerosol properties. This work presents in-situ aircraft measurements of cloud condensation nuclei (CCN) concentration and derivations of aerosol hygroscopicity, water uptake, and light scattering. Aerosol hygroscopicity is derived from CCN and aerosol measurements. Inorganic water uptake is calculated from aerosol composition using ISORROPIA, a chemical thermodynamic model, while organic water uptake is calculated from organic hygroscopicity. Aerosol scattering closure is performed between scattering from water uptake calculations and in-situ scattering measurements.

  11. Hygroscopic, Morphological, and Chemical Properties of Agricultural Aerosols

    NASA Astrophysics Data System (ADS)

    Hiranuma, N.; Brooks, S. D.; Cheek, L.; Thornton, D. C.; Auvermann, B. W.; Littleton, R.

    2007-12-01

    Agricultural fugitive dust is a significant source of localized air pollution in the semi-arid southern Great Plains. In the Texas Panhandle, daily episodes of ground-level fugitive dust emissions from the cattle feedlots are routinely observed in conjunction with increased cattle activity in the late afternoons and early evenings. We conducted a field study to characterize size-selected agricultural aerosols with respect to hygroscopic, morphological, and chemical properties and to attempt to identify any correlations between these properties. To explore the hygroscopic nature of agricultural particles, we have collected size-resolved aerosol samples using a cascade impactor system at a cattle feedlot in the Texas Panhandle and have used the Environmental Scanning Electron Microscope (ESEM) to determine the water uptake by individual particles in those samples as a function of relative humidity. To characterize the size distribution of agricultural aerosols as a function of time, A GRIMM aerosol spectrometer and Sequential Mobility Particle Sizer and Counter (SMPS) measurements were simultaneously performed in an overall size range of 11 nm to 20 µm diameters at a cattle feedlot. Complementary determination of the elemental composition of individual particles was performed using Energy Dispersive X-ray Spectroscopy (EDS). In addition to the EDS analysis, an ammonia scrubber was used to collect ammonia and ammonium in the gas and particulate phases, respectively. The concentration of these species was quantified offline via UV spectrophotometry at 640 nanometers. The results of this study will provide important particulate emission data from a feedyard, needed to improve our understanding of the role of agricultural particulates in local and regional air quality.

  12. Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T. B.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2013-05-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic hygroscopicity parameter, κ*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (forg) are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which predictions of the hygroscopicity parameter are compared against κ*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51% ± 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00-08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour" and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory material not measured

  13. CCN estimates from bulk hygroscopic growth factors of ambient aerosols during the pre-monsoon season over Central Nepal

    NASA Astrophysics Data System (ADS)

    Shrestha, Prabhakar; Barros, Ana P.; Khlystov, Andrei

    2013-03-01

    Aerosol size distribution (ambient and dried) and chemical composition were measured simultaneously using two Scanning Mobility Particle Sizers (SMPSs) and filters during the pre-monsoon season (April-June 2009) at two locations in Central Nepal: Dhulikhel, an urban site in the Kathmandu valley, and Besisahar, a rural village in the Marsyangdi valley. Diameter growth factors (DGF) were estimated using the larger mode (around 100 nm) of the aerosol size distributions. The measured DGF suggest that the aerosols were in metastable state below 80% RH owing to the strong diurnal cycle of relative humidity (RH) at Dhulikhel, while no discernible growth was observed for Besisahar. Assuming ideal behavior of water-soluble organic compounds and using their fraction as determined by water extraction of filters produced the best agreement for a two-component hygroscopic growth model with the observed DGFs. This finding together with the DGF and chemical composition data were used to determine the aerosol bulk hygroscopicity parameter, κ. The κ parameter suggests that aerosols in this region are less hygroscopic than aerosols reported in previous studies from other regions. The estimated κ and the vertically scaled aerosol size distribution were then used to estimate the CCN spectra. These are the first estimates of CCN spectra from ground-based observations for the Central Himalaya region.

  14. The contribution of aerosol hygroscopic growth to the modeled aerosol radiative effect

    NASA Astrophysics Data System (ADS)

    Kokkola, Harri; Kühn, Thomas; Kirkevåg, Alf; Romakkaniemi, Sami; Arola, Antti

    2016-04-01

    The hygroscopic growth of atmospheric aerosols can have a significant effect on the direct radiative effect of atmospheric aerosol. However, there are significant uncertainties concerning how much of the radiative forcing is due to different chemical compounds, especially water. For example, modeled optical depth of water in global aerosol-climate models varies by more than a factor of two. These differences can be attributed to differences in modeled 1) hygroscopicity, 2) ambient relative humidity, and/or 3) aerosol size distribution. In this study, we investigate which of these above-mentioned factors cause the largest variability in the modeled optical depth of water. In order to do this, we have developed a tool that calculates aerosol extinction using interchangeable global 3D data of aerosol composition, relative humidity, and aerosol size distribution fields. This data is obtained from models that have taken part in the open international initiative AeroCom (Aerosol Comparisons between Observations and Models). In addition, we use global 3D data for relative humidity from the Atmospheric Infrared Sounder (AIRS) flying on board NASA's Aqua satellite and the National Centers for Environmental Prediction (NCEP) reanalysis data. These observations are used to evaluate the modeled relative humidity fields. In the first stage of the study, we made a detailed investigation using the aerosol-chemistry-climate model ECHAM-HAMMOZ in which most of the aerosol optical depth is caused by water. Our results show that the model significantly overestimates the relative humidity over the oceans while over land, the overestimation is lower or it is underestimated. Since this overestimation occurs over the oceans, the water optical depth is amplified as the hygroscopic growth is very sensitive to changes in high relative humidities. Over land, error in modeled relative humidity is unlikely to cause significant errors in water optical depth as relative humidities are generally

  15. Multiwavelength In-situ Aerosol Absorption, Scattering, and Hygroscopic Properties During the TEXAQS 2006 Field Campaign: Aerosol Classification and Variability

    NASA Astrophysics Data System (ADS)

    Sierau, B.; Covert, D. S.; Coffman, D. J.; Quinn, P. K.; Bates, T. S.

    2006-12-01

    In-situ, three wavelength-measurements of aerosol scattering and absorption of the regional aerosol near the coast of Texas, i.e. Houston and the Houston ship channel, as well as the Gulf of Mexico were carried out onboard the NOAA research vessel Ronald H. Brown during the 2006 TEXAQS/GoMACCS field campaign in July through September 2006. Aerosol scattering, hemispheric backscattering and absorption-coefficients were measured for particles with diameters dp<10μm and dp<1μm using multiwavelength integrating nephelometers and filter-based absorption photometers (PSAPs) at 60% RH (nephelometers). Light scattering was measured as a function of RH at two additional humidities, (ca. 25%, and 85% RH). Together with the 60% RH data, this enabled determination of the hygroscopic growth curve of scattering. The extensive and intensive optical properties were used to characterize the aerosol in the Houston, TX area and the Coastal Gulf of Mexico region and to provide information critical to understanding the climatic and air quality impacts of those aerosols. Analysis focuses on how these properties change during the chemical processing of sources within the project area and how they are affected by changes in atmospheric relative humidity that accompany transport, diurnal cycles and vertical mixing. The results are relevant to radiation transfer, visibility, air quality, and interpretation of remote sensing data from lidar and satellite. The results will be presented based on a regional classification of the sampled air masses to identify distinct aerosol populations and sources and to show the temporal and spatial variability of the measured parameters. Special emphasize will be given to the physico-chemical properties of aerosols measured during extensive Saharan dust periods encountered during the cruise and several air pollution episodes and industrial plumes. Scattering hygroscopic growth will be analyzed along with the chemical composition of the aerosol and its

  16. Water Activity Limits the Hygroscopic Growth Factor of Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rodriguez, L. I.; Cabrera, J. A.; Golden, D.; Tabazadeh, A.

    2007-12-01

    In this work we study the hygroscopic behavior of organic aerosols, which has important implications for Earth's climate. The hygroscopic growth factor (HGF) is defined as the ratio of the diameter of a spherical particle when it is exposed to dry conditions to that at humid conditions. We present a new formulation to express the HGF of an aerosol particle as a function of water activity (aw) in the aqueous phase. This new formulation matches reported HGFs for common inorganic salts and water-miscible organic particles that are known to deliquesce into aqueous drops at high relative humidities (RH). Many studies use tandem differential mobility analyzers (TDMA) to determine the HGF of organic aerosols. For example, Brooks et al. used a TDMA to measure a HGF of 1.2 for 2 μm phthalic acid (PA) particles at 90% RH (aw= 0.9). However, water activity limits the growth of a particle that can be attributed to water uptake. We have assembled a vapor pressure apparatus to measure aw of aqueous solutions at room temperature. Measured water activities for PA, used in our growth formulation, yield a HGF of ~ 1.0005 for 2 μm PA particles at 90% RH. Comparing our results against Brooks et al. suggests that TDMA experiments may grossly overestimate the HGF of PA particles since water activity limits this growth to below 1.0005. Alternatively, we suggest that the adsorption of a negligible mass of water by a highly porous PA particle can lead to an apparent growth in particle size by changing its morphology. Other studies also use TDMAs to measure HGFs of secondary organic aerosols (SOAs). HGFs reported for SOAs are very similar to PA, suggesting that the observed growth may be due to morphological changes in particle size rather than water uptake as commonly assumed. We built a smog chamber where an organic precursor, such as d-limonene, reacts with nitrogen oxides under UV radiation to produce SOAs. We compare the HGFs for SOAs obtained with our method to those obtained with

  17. Aerosol Nucleation Frequency and Hygroscopicity at a Forested Site in the Southeastern United States

    NASA Astrophysics Data System (ADS)

    O'Halloran, T. L.; Fuentes, J. D.; Collins, D. R.; Cleveland, M. J.

    2007-12-01

    This paper examines how aerosol hygroscopicity and nucleation frequency, measured with a tandem differential mobility analyzer (TDMA) at a rural site in the southeastern United States, vary with air mass source regions and transport pathways. We also examine an observed enhancement in aerosol hygroscopicity during nucleation events. During October through December, 2006, a TDMA was used to measure submicron aerosol size distributions and size-resolved hygroscopicity at a forested site in the southeastern U.S. Measurements were conducted above a mixed deciduous forest at the Virginia Forest Research Facility, a newly operational permanent micrometeorological facility located approximately 20 km east of the foothills of the Blue Ridge Mountains. The site features a 40-m walkup scaffolding tower above a 20-m mixed deciduous forest with excellent fetch, and a climate controlled lab for housing instruments and data acquisition systems. Hygroscopic growth factor distributions were measured for eight dry diameters between 0.013 and 0.400 μm. Cluster analysis of back trajectories was applied to identify characteristic source regions and air mass pathways during the study period. Significant differences were found in the frequency of aerosol nucleation events and hygroscopicity amongst the five distinct pathways identified by the cluster analysis. Nucleation occurred most frequently when fast moving air masses originated from the northern central U.S. and lower central Canada. In these cases existing aerosol surface area was low, and the majority of trajectories passed directly over the Ohio River valley. Hygroscopicity generally increased with increasing dry diameter, except for the largest size bin, which had a slightly lower hygroscopicity than the next smallest size. Two clusters with short, stagnant trajectories contained aerosols with enhanced hygroscopicity at dry diameters less than 0.100 μm. Aerosol hygroscopicity was significantly enhanced, especially at small

  18. Hygroscopic behavior of multicomponent organic aerosols and their internal mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Jing, Bo; Tong, Shengrui; Liu, Qifan; Li, Kun; Wang, Weigang; Zhang, Yunhong; Ge, Maofa

    2016-03-01

    Water-soluble organic compounds (WSOCs) are important components of organics in the atmospheric fine particulate matter. Although WSOCs play an important role in the hygroscopicity of aerosols, knowledge on the water uptake behavior of internally mixed WSOC aerosols remains limited. Here, the hygroscopic properties of single components such as levoglucosan, oxalic acid, malonic acid, succinic acid, phthalic acid, and multicomponent WSOC aerosols mainly involving oxalic acid are investigated with the hygroscopicity tandem differential mobility analyzer (HTDMA). The coexisting hygroscopic species including levoglucosan, malonic acid, and phthalic acid have a strong influence on the hygroscopic growth and phase behavior of oxalic acid, even suppressing its crystallization completely during the drying process. The phase behaviors of oxalic acid/levoglucosan mixed particles are confirmed by infrared spectra. The discrepancies between measured growth factors and predictions from Extended Aerosol Inorganics Model (E-AIM) with the Universal Quasi-Chemical Functional Group Activity Coefficient (UNIFAC) method and Zdanovskii-Stokes-Robinson (ZSR) approach increase at medium and high relative humidity (RH) assuming oxalic acid in a crystalline solid state. For the internal mixture of oxalic acid with levoglucosan or succinic acid, there is enhanced water uptake at high RH compared to the model predictions based on reasonable oxalic acid phase assumption. Organic mixture has more complex effects on the hygroscopicity of ammonium sulfate than single species. Although hygroscopic species such as levoglucosan account for a small fraction in the multicomponent aerosols, they may still strongly influence the hygroscopic behavior of ammonium sulfate by changing the phase state of oxalic acid which plays the role of "intermediate" species. Considering the abundance of oxalic acid in the atmospheric aerosols, its mixtures with hygroscopic species may significantly promote water uptake

  19. Hygroscopic behavior of multicomponent organic aerosols and their internal mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Jing, B.; Tong, S. R.; Liu, Q. F.; Li, K.; Wang, W. G.; Zhang, Y. H.; Ge, M. F.

    2015-08-01

    Water soluble organic compounds (WSOCs) are important components of organics in the atmospheric fine particulate matter. Although WSOCs play an important role in the hygroscopicity of aerosols, water uptake behavior of internally mixed WSOC aerosols remains limited characterization. Here, the hygroscopic properties of single component such as levoglucosan, oxalic acid, malonic acid, succinic acid and phthalic acid and multicomponent WSOC aerosols mainly involving oxalic acid are investigated with the hygroscopicity tandem differential mobility analyzer (HTDMA). The coexisting hygroscopic species including levoglucosan, malonic acid and phthalic acid have strong influence on the hygroscopic growth and phase behavior of oxalic acid, even suppress its crystallization completely. The interactions between oxalic acid and levoglucosan are confirmed by infrared spectra. The discrepancies between measured growth factors and predictions from Extended Aerosol Inorganics Model (E-AIM) with UNIFAC method and Zdanovskii-Stokes-Robinson (ZSR) approach increase at medium and high relative humidity (RH) assuming oxalic acid in a solid state. For the internal mixture of oxalic acid with levoglucosan or succinic acid, there is enhanced water uptake at high RH due to positive chemical interactions between solutes. Organic mixture has more complex effect on the hygroscopicity of ammonium sulfate than single species. Although hygroscopic species such as levoglucosan accounts for a small fraction in the multicomponent aerosols, they may still strongly influence the hygroscopic behavior of ammonium sulfate by changing phase state of oxalic acid which plays the role of "intermediate" species. Considering the abundance of oxalic acid in the atmospheric aerosols, its mixtures with hygroscopic species may significantly promote water uptake under high RH conditions and thus affect the cloud condensation nuclei (CCN) activity, optical properties and chemical reactivity of atmospheric particles.

  20. The white-light humidified optical particle spectrometer (WHOPS) - a novel airborne system to characterize aerosol hygroscopicity

    NASA Astrophysics Data System (ADS)

    Rosati, B.; Wehrle, G.; Gysel, M.; Zieger, P.; Baltensperger, U.; Weingartner, E.

    2015-02-01

    Aerosol particles experience hygroscopic growth at enhanced relative humidity (RH), which leads to changes in their optical properties. We developed the white-light humidified optical particle spectrometer (WHOPS), a new instrument to investigate the particles' hygroscopic growth. Here we present a detailed technical description and characterization of the WHOPS in laboratory and field experiments. The WHOPS consists of a differential mobility analyzer, a humidifier/bypass and a white-light aerosol spectrometer (WELAS) connected in series to provide fast measurements of particle hygroscopicity at subsaturated RH and optical properties on airborne platforms. The WELAS employs a white-light source to minimize ambiguities in the optical particle sizing. In contrast to other hygroscopicity instruments, the WHOPS retrieves information of relatively large particles (i.e., diameter D > 280 nm), therefore investigating the more optically relevant size ranges. The effective index of refraction of the dry particles is retrieved from the optical diameter measured for size-selected aerosol samples with a well-defined dry mobility diameter. The data analysis approach for the optical sizing and retrieval of the index of refraction was extensively tested in laboratory experiments with polystyrene latex size standards and ammonium sulfate particles of different diameters. The hygroscopic growth factor (GF) distribution and aerosol mixing state is inferred from the optical size distribution measured for the size-selected and humidified aerosol sample. Laboratory experiments with pure ammonium sulfate particles revealed good agreement with Köhler theory (mean bias of ~3% and maximal deviation of 8% for GFs at RH = 95%). During first airborne measurements in the Netherlands, GFs (mean value of the GF distribution) at RH = 95% between 1.79 and 2.43 with a median of 2.02 were observed for particles with a dry diameter of 500 nm. This corresponds to hygroscopicity parameters

  1. Physiochemical properties of carbonaceous aerosol from agricultural residue burning: Density, volatility, and hygroscopicity

    NASA Astrophysics Data System (ADS)

    Li, Chunlin; Hu, Yunjie; Chen, Jianmin; Ma, Zhen; Ye, Xingnan; Yang, Xin; Wang, Lin; Wang, Xinming; Mellouki, Abdelwahid

    2016-09-01

    Size-resolved effective density, mixing state, and hygroscopicity of smoke particles from five kinds of agricultural residues burning were characterized using an aerosol chamber system, including a volatility/hygroscopic tandem differential mobility analyzer (V/H-TDMA) combined with an aerosol particle mass analyzer (APM). To profile relationship between the thermodynamic properties and chemical compositions, smoke PM1.0 and PM2.5 were also measured for the water soluble inorganics, mineral elements, and carbonaceous materials like organic carbon (OC) and elemental carbon (EC). Smoke particle has a density of 1.1-1.4 g cm-3, and hygroscopicity parameter (κ) derived from hygroscopic growth factor (GF) of the particles ranges from 0.20 to 0.35. Size- and fuel type-dependence of density and κ are obvious. The integrated effective densities (ρ) and hygroscopicity parameters (κ) both scale with alkali species, which could be parameterized as a function of organic and inorganic mass fraction (forg &finorg) in smoke PM1.0 and PM2.5: ρ-1 =finorg · ρinorg-1 +forg · ρorg-1 and κ =finorg ·κinorg +forg ·κorg . The extrapolated values of ρinorg and ρorg are 2.13 and 1.14 g cm-3 in smoke PM1.0, while the characteristic κ values of organic and inorganic components are about 0.087 and 0.734, which are similar to the bulk density and κ calculated from predefined chemical species and also consistent with those values observed in ambient air. Volatility of smoke particle was quantified as volume fraction remaining (VFR) and mass fraction remaining (MFR). The gradient temperature of V-TDMA was set to be consistent with the splitting temperature in the OC-EC measurement (OC1 and OC2 separated at 150 and 250 °C). Combing the thermogram data and chemical composition of smoke PM1.0, the densities of organic matter (OM1 and OM2 correspond to OC1 and OC2) are estimated as 0.61-0.90 and 0.86-1.13 g cm-3, and the ratios of OM1/OC1 and OM2/OC2 are 1.07 and 1.29 on average

  2. Cloud condensation nuclei activity, droplet growth kinetics, and hygroscopicity of biogenic and anthropogenic secondary organic aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, D. F.; Buchholz, A.; Kortner, B.; Schlag, P.; Rubach, F.; Fuchs, H.; Kiendler-Scharr, A.; Tillmann, R.; Wahner, A.; Watne, Å. K.; Hallquist, M.; Flores, J. M.; Rudich, Y.; Kristensen, K.; Hansen, A. M. K.; Glasius, M.; Kourtchev, I.; Kalberer, M.; Mentel, Th. F.

    2016-02-01

    Interaction of biogenic volatile organic compounds (VOCs) with Anthropogenic VOC (AVOC) affects the physicochemical properties of secondary organic aerosol (SOA). We investigated cloud droplet activation (CCN activity), droplet growth kinetics, and hygroscopicity of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Selected monoterpenes and aromatics were used as representative precursors of BSOA and ASOA, respectively.

    We found that BSOA, ASOA, and ABSOA had similar CCN activity despite the higher oxygen to carbon ratio (O/C) of ASOA compared to BSOA and ABSOA. For individual reaction systems, CCN activity increased with the degree of oxidation. Yet, when considering all different types of SOA together, the hygroscopicity parameter, κCCN, did not correlate with O/C. Droplet growth kinetics of BSOA, ASOA, and ABSOA were comparable to that of (NH4)2SO4, which indicates that there was no delay in the water uptake for these SOA in supersaturated conditions.

    In contrast to CCN activity, the hygroscopicity parameter from a hygroscopic tandem differential mobility analyzer (HTDMA) measurement, κHTDMA, of ASOA was distinctively higher (0.09-0.10) than that of BSOA (0.03-0.06), which was attributed to the higher degree of oxidation of ASOA. The ASOA components in mixed ABSOA enhanced aerosol hygroscopicity. Changing the ASOA fraction by adding biogenic VOC (BVOC) to ASOA or vice versa (AVOC to BSOA) changed the hygroscopicity of aerosol, in line with the change in the degree of oxidation of aerosol. However, the hygroscopicity of ABSOA cannot be described by a simple linear combination of pure BSOA and ASOA systems. This indicates that additional processes, possibly oligomerization, affected the hygroscopicity.

    Closure analysis of CCN and HTDMA data showed κHTDMA was lower than κCCN by 30-70 %. Better closure was achieved for ASOA compared to BSOA. This

  3. Hygroscopicity of aerosol particles and CCN activity of nearly hydrophobic particles in the urban atmosphere over Japan during summer

    NASA Astrophysics Data System (ADS)

    Ogawa, Shuhei; Setoguchi, Yoshitaka; Kawana, Kaori; Nakayama, Tomoki; Ikeda, Yuka; Sawada, Yuuki; Matsumi, Yutaka; Mochida, Michihiro

    2016-06-01

    We investigated the hygroscopicity of 150 nm particles and the number-size distributions and the cloud condensation nuclei (CCN) activity of nearly hydrophobic particles in aerosols over Nagoya, Japan, during summer. We analyzed the correlations between the number concentrations of particles in specific hygroscopic growth factor (g) ranges and the mass concentrations of chemical components. This analysis suggests the association of nearly hydrophobic particles with hydrocarbon-like organic aerosol, elemental carbon and semivolatile oxygenated organic aerosol (SV-OOA), that of less hygroscopic particles with SV-OOA and nitrate and that of more hygroscopic particles with low-volatile oxygenated organic aerosol (LV-OOA) and sulfate. The hygroscopicity parameter (κ) of organics was derived based on the g distributions and chemical composition of 150 nm particles. The κ of the organics correlated positively with the fraction of the total organic mass spectral signal at m/z 44 and the volume fraction of the LV-OOA to the organics, indicating that organics with highly oxygenated structures including carboxylic acid groups contribute to the water uptake. The number-size distributions of the nearly hydrophobic particles with g around 1.0 and 1.1 correlated with the mass concentrations of chemical components. The results show that the chemical composition of the particles with g around 1.0 was different between the Aitken mode and the accumulation mode size ranges. An analysis for a parameter Fmax of the curves fitted to the CCN efficiency spectra of the particles with g around 1.0 suggests that the coating by organics associated with SV-OOA elevated the CCN activity of these particles.

  4. Effects of Organic-Inorganic Interactions on the Hygroscopicity of Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Lienhard, D.; Krieger, U. K.

    2013-12-01

    Aerosol hygroscopicity is an important property affecting size as well as phase transitions and viscosity of soluble or partially soluble particles following changes in ambient relative humidity (RH) and temperature. The effects of hygroscopic particle growth on the water contents and physical states of aerosol phases in turn may significantly affect multiphase chemistry, the direct effect of aerosols on climate, and the ability of specific particles to act as cloud condensation or ice nuclei. The hygroscopic growth of organic-inorganic mixtures in stable or metastable equilibrium with the RH of the surrounding air is governed by chemical thermodynamics and can be described, in principle, by adequate thermodynamic models. Organic-inorganic interactions involving dissolved ionic species in liquid (potentially highly viscous) phases tend to deviate substantially from ideal mixing and can lead to hygroscopicity behaviour deviating from simple linear additivity assumptions at given RH. The latter assumptions are employed in the Zdanovskii-Stokes-Robinson (ZSR) mixing rule, which is typically found to describe hygroscopic mass growth well in the RH range of completely liquid aerosol systems. We present a comparison and discussion of thermodynamic calculations based on the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model and hygroscopic growth factor data from new measurements with an electrodynamic balance (EDB) as well as data from the literature. We focus on the different hygroscopicity features below the full deliquescence RH of multicomponent organic-inorganic systems. Experiments and model calculations are performed for different multicomponent systems showing varying degrees of organic-inorganic miscibility, including liquid-liquid phase separation, hygroscopicity, and hysteresis effects between metastable and stable gas-aerosol equilibria. It is found that depending on the hygroscopicity of the organic aerosol fraction

  5. Hygroscopicity of dicarbonyl-amine secondary organic aerosol products investigated with HTDMA

    NASA Astrophysics Data System (ADS)

    Hawkins, L. N.; de Haan, D. O.

    2010-12-01

    Recent studies have shown the importance of amine-dicarbonyl chemistry as a secondary organic aerosol (SOA) formation pathway, producing imines, imidazoles, and N-containing oligomers. Preliminary work in our group has suggested that some of these products may be surface active. Therefore, the presence of these products may result in important changes to submicron particle hygroscopicity that affect aerosol scattering and cloud condensation nuclei (CCN) activity, especially in regions with significant amine-containing particles. To investigate their hygroscopicity, we have designed a hygroscopicity tandem differential mobility analyzer (HTDMA) system around a 300 L Teflon chamber that allows for longer humidification times needed for some organic aerosol components that are only slightly hygroscopic. This modification provides a range of residence times from 2.5 minutes up to 1 hour, unlike previously published systems that vary from 2-30 seconds. Using the modified hygroscopicity tandem differential mobility analyzer (HTDMA), we have measured the hygroscopic growth factor (HGF) of SOA formed from reactions of glyoxal (and methylglyoxal) with methylamine, ammonium sulfate, and several amino acids. Changes to inorganic aerosol HGF in response to the presence of SOA products are also investigated.

  6. Changes in droplet surface tension affect the observed hygroscopicity of photochemically aged biomass burning aerosol.

    PubMed

    Giordano, Michael R; Short, Daniel Z; Hosseini, Seyedehsan; Lichtenberg, William; Asa-Awuku, Akua A

    2013-10-01

    This study examines the hygroscopic and surface tension properties as a function of photochemical aging of the aerosol emissions from biomass burning. Experiments were conducted in a chamber setting at the UC-Riverside Center for Environmental Research and Technology (CE-CERT) Atmospheric Processes Lab using two biomass fuel sources, manzanita and chamise. Cloud condensation nuclei (CCN) measurements and off-line filter sample analysis were conducted. The water-soluble organic carbon content and surface tension of the extracted filter samples were measured. Surface tension information was then examined with Köhler theory analysis to calculate the hygroscopicity parameter, κ. Laboratory measurement of biomass burning smoke from two chaparral fuels is shown to depress the surface tension of water by 30% or more at organic matter concentrations relevant at droplet activation. Accounting for surface tension depression can lower the calculated κ by a factor of 2. This work provides evidence for surface tension depression in an important aerosol system and may provide closure for differing sub- and supersaturated κ measurements. PMID:23957441

  7. The impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient

    NASA Astrophysics Data System (ADS)

    Tao, Jiangchuan; Zhao, Chunsheng

    2016-04-01

    Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number-size distribution and hygroscopic growth factor (at RH values above 90 %) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty ofω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90 %). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98 % at the height of 1 km increases by 30.4 %, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.

  8. The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

    NASA Astrophysics Data System (ADS)

    Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

    2014-12-01

    Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

  9. Size matters in the water uptake and hygroscopic growth of atmospherically relevant multicomponent aerosol particles.

    PubMed

    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. PMID:25521409

  10. Hygroscopic Properties of Atmospheric Aerosol Measured with an HTDMA in an Urban Background Site in Madrid

    NASA Astrophysics Data System (ADS)

    Alonso-Blanco, E.; Gómez-Moreno, F. J.; Becerril, M.; Coz, E.; Artíñano, B.

    2015-12-01

    The observation of high aerosol hygroscopic growth in Madrid is mainly limited to specific atmospheric conditions, such as local stagnation episodes, which take place in winter time. One of these episodes was identified in December 2014 and the hygroscopic growth factor (GF) measurements obtained in such episode were analysed in order to know the influence of the meteorological conditions on aerosol hygroscopic properties. The prevailing high atmospheric stability triggered an increase of the particle total concentration during the study period, with several peaks that exceeded 4.0 104 particles cm-3, as well as an increase in the inorganic fraction of the aerosol, the NO3- concentration, which in this case corresponded to 25% of the total PM1 non-refractory composition. The aerosol hygroscopic growth distribution was bimodal during the episode, with an average GF around 1.2 for the five dry particle sizes measured and an average GF spread ≥ 0.15. In addition, it is important to note that when a reduction in the concentrations of NO3- is observed, it coincides with a decrease of the GF and its spread. These data suggest, on the one hand, a high degree of external mixing state of the aerosol during the episode and, on the other hand, a notable association between the GF and the inorganic fraction of the aerosol.

  11. Size-dependent hygroscopicity parameter (κ) and chemical composition of secondary organic cloud condensation nuclei

    NASA Astrophysics Data System (ADS)

    Zhao, D. F.; Buchholz, A.; Kortner, B.; Schlag, P.; Rubach, F.; Kiendler-Scharr, A.; Tillmann, R.; Wahner, A.; Flores, J. M.; Rudich, Y.; Watne, À. K.; Hallquist, M.; Wildt, J.; Mentel, Th. F.

    2015-12-01

    Secondary organic aerosol components (SOA) contribute significantly to the activation of cloud condensation nuclei (CCN) in the atmosphere. The CCN activity of internally mixed submicron SOA particles is often parameterized assuming a size-independent single-hygroscopicity parameter κ. In the experiments done in a large atmospheric reactor (SAPHIR, Simulation of Atmospheric PHotochemistry In a large Reaction chamber, Jülich), we consistently observed size-dependent κ and particle composition for SOA from different precursors in the size range of 50 nm-200 nm. Smaller particles had higher κ and a higher degree of oxidation, although all particles were formed from the same reaction mixture. Since decreasing volatility and increasing hygroscopicity often covary with the degree of oxidation, the size dependence of composition and hence of CCN activity can be understood by enrichment of higher oxygenated, low-volatility hygroscopic compounds in smaller particles. Neglecting the size dependence of κ can lead to significant bias in the prediction of the activated fraction of particles during cloud formation.

  12. Hygroscopic Behavior of Multicomponent Aerosols Involving NaCl and Dicarboxylic Acids.

    PubMed

    Peng, Chao; Jing, Bo; Guo, Yu-Cong; Zhang, Yun-Hong; Ge, Mao-Fa

    2016-02-25

    Atmospheric aerosols are usually complex mixtures of inorganic and organic compounds. The hygroscopicity of mixed particles is closely related to their chemical composition and interactions between components, which is still poorly understood. In this study, the hygroscopic properties of submicron particles composed of NaCl and dicarboxylic acids including oxalic acid (OA), malonic acid (MA), and succinic acid (SA) with various mass ratios are investigated with a hygroscopicity tandem differential mobility analyzer (HTDMA) system. Both the Zdanovskii-Stokes-Robinson (ZSR) method and extended aerosol inorganics model (E-AIM) are applied to predict the water uptake behaviors of sodium chloride/dicarboxylic acid mixtures. For NaCl/OA mixed particles, the measured growth factors were significantly lower than predictions from the model methods, indicating a change in particle composition caused by chloride depletion. The hygroscopic growth of NaCl/MA particles was well described by E-AIM, and that of NaCl/SA particles was dependent upon mixing ratio. Compared with model predictions, it was determined that water uptake of the NaCl/OA mixture could be enhanced and could be closer to the predictions by addition of levoglucosan or malonic acid, which retained water even at low relative humidity (RH), leading to inhibition of HCl evaporation during dehydration. These results demonstrate that the coexisting hygroscopic species have a strong influence on the phase state of particles, thus affecting chemical interactions between inorganic and organic compounds as well as the overall hygroscopicity of mixed particles. PMID:26820230

  13. Relationship between volatility, hygroscopicity, and CCN activity of winter aerosols: Kanpur, Indo-Gangetic Basin

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, Sachchida

    2016-04-01

    Aerosol volatility is one of the key property in deciding their lifetime and fate. The volatile species have the potential to affect SOA estimation, so their characterization and establishment of relationship with mass loading, chemical composition, hygroscopicity and CCN activity is required. A 42 days long winter campaign was conducted in an anthropogenically polluted location (Kanpur, India) where CCN activity of both ambient and thermally treated aerosols was characterized. Enhanced partitioning of semi-volatile molecules into particle phase at higher loading conditions was observed. Unexpectedly, the most oxidized organic factor was observed both least volatile and hygroscopic in nature. Lower

  14. Hygroscopicity of water-soluble organic compounds in atmospheric aerosols: amino acids and biomass burning derived organic species.

    PubMed

    Chan, Man Nin; Choi, Man Yee; Ng, Nga Lee; Chan, Chak K

    2005-03-15

    Amino acids and organic species derived from biomass burning can potentially affect the hygroscopicity and cloud condensation activities of aerosols. The hygroscopicity of seven amino acids (glycine, alanine, serine, glutamine, threonine, arginine, and asparagine) and three organic species most commonly detected in biomass burning aerosols (levoglucosan, mannosan, and galactosan) were measured using an electrodynamic balance. Crystallization was observed in the glycine, alanine, serine, glutamine, and threonine particles upon evaporation of water, while no phase transition was observed in the arginine and asparagine particles even at 5% relative humidity (RH). Water activity data from these aqueous amino acid particles, except arginine and asparagine, was used to revise the interaction parameters in UNIQUAC functional group activity coefficients to give predictions to within 15% of the measurements. Levoglucosan, mannosan, and galactosan particles did not crystallize nor did they deliquesce. They existed as highly concentrated liquid droplets at low RH, suggesting that biomass burning aerosols retain water at low RH. In addition, these particles follow a very similar pattern in hygroscopic growth. A generalized growth law (Gf = (1 - RH/100)-0.095) is proposed for levoglucosan, mannosan, and galactosan particles. PMID:15819209

  15. Hygroscopic behavior of water-soluble matter extracted from biomass burning aerosols collected at a rural site in Tanzania, East Africa

    NASA Astrophysics Data System (ADS)

    Boreddy, S. K. R.; Kawamura, Kimitaka; Mkoma, Stelyus; Fu, Pingqing

    2014-11-01

    In this study, we present the hygroscopic behavior of water-soluble matter (WSM) extracted from biomass burning derived particulate matter 2.5 (PM2.5) aerosols collected at a rural background site in Tanzania during June-August 2011. Hygroscopic growth factors, g(RH), of WSM were measured by hygroscopic tandem differential mobility analyzer (H-TDMA) with an initial dry particle diameter of 100 nm. We observed that the g(RH) of WSM at 90% relative humidity (RH), g(90%)WSM, ranged from 1.10 to 1.47 with an average of 1.25 ± 0.12. The H-TDMA retrieved hygroscopicity parameter of WSM, κWSM, ranged from 0.04 to 0.24 with a mean of 0.11 ± 0.07. We found that the observed g(90%)WSM is positively correlated with PM2.5 mass fractions of K+ (R2 = 0.61), Cl- (0.54), and organic carbon (0.58). Moreover, it well correlates with levoglucosan (0.67) and total diacids (0.76), implying that although the inorganic fraction may be the most important factor to control the hygroscopicity; biomass burning organics play a significant role in the hygroscopicity of Tanzanian aerosols. The lower growth factors obtained over the sampling site are probably due to the formation of less water-soluble potassium oxalate (K2C2O4) or less hygroscopic K2SO4 particles during atmospheric aging. We observed a moderate correlation (R2 = 0.33) between PM2.5 mass fraction of WSOC and g(90%)WSM. The retrieved g(90%)WSOM values ranged from 1.0 to 1.25 with a mean of 1.16 ± 0.05. This study demonstrates that the hygroscopicity of Tanzanian aerosols is largely controlled by the emission of biomass burning products and the subsequent chemical aging during atmospheric transport.

  16. Hygroscopic properties of aerosol formed by oxidation of limonene, α-pinene, and β-pinene

    NASA Astrophysics Data System (ADS)

    Virkkula, Aki; van Dingenen, Rita; Raes, Frank; Hjorth, Jens

    1999-02-01

    The hygroscopic properties of aerosol formed by oxidation of three monoterpenes, limonene, α-pinene, and β-pinene, were measured using a tandem differential mobility analyzer (TDMA). The experiments were performed in the European Photoreactor (EUPHORE) in Valencia, Spain. The experiments included ozonolysis and photooxidation with and without ammonium sulfate seed aerosol. Pure organic particles, formed by oxidation of the terpenes in the absence of the seed aerosol, proved to be slightly hygroscopic. The hygroscopic growth factor (G) was close to 1.10 at relative humidity 84% ± 1%, which is often observed as the G of the less hygroscopic mode of atmospheric aerosol in field measurements. In the experiments with ammonium sulfate seed aerosol G decreased from approximately 1.5 before the start of terpene oxidation to approximately 1.1 as the oxidation products condensed on the particles. G was not proportional to the organic layer thickness but decreased with increasing organic volume fraction. Our analysis shows that in the internally mixed particles, ammonium sulfate and the organic products take up water independently of one another.

  17. Hygroscopic growth of size-resolved, emission-source classified, aerosol particles sampled across the United States

    NASA Astrophysics Data System (ADS)

    Shingler, T.; Crosbie, E. C.; Ziemba, L. D.; Anderson, B. E.; Campuzano Jost, P.; Jimenez, J. L.; Mikoviny, T.; Wisthaler, A.; Sorooshian, A.

    2014-12-01

    The hygroscopic growth of atmospheric aerosol particles is a key air quality parameter, impacting the radiation budget, visibility, and cloud formation. During the DC3 and SEAC4RS field campaigns (>300 total flight hours), measurements were made over 32 US states, Canada, the Pacific Ocean, and the Gulf of Mexico, between the surface and 41,000 feet ASL. The aircraft research payloads included a suite of in-situ aerosol and gas phase instruments. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) and the Langley Aerosol Research Group Experiment (LARGE) humidified nephelometer instrument applied different techniques to measure water uptake by aerosol particles at prescribed relative humidity values. Size-resolved growth factor (GF ≡ Dp,wet/Dp,dry) measurements by the DASH-SP are compared to bulk scattering measurements (f(RH) ≡ σscat,wet/σscat,dry) by the LARGE instrument. Spatial location and volatile organic compound tracers such as isoprene and acetonitrile are used to classify the origin of distinct air masses, including: forest fires, biogenic-emitting forests, agricultural use lands, marine boundary layer, urban, and rural background. Analyses of GF results by air mass origin are reported and results are compared with f(RH) measurements. A parameterization between the f(RH) and GF measurements and its potential uses are discussed.

  18. Hygroscopicity of Amine Secondary Aerosol - Mixtures of Organic and Inorganic Components

    NASA Astrophysics Data System (ADS)

    Tang, X.; Cocker, D. R.; Purvis-Roberts, K.; Asa-Awuku, A. A.

    2012-12-01

    Aliphatic amines are emitted from both biogenic and anthropogenic sources and contribute to the formation of secondary aerosol in reactions with atmospheric radicals. However, the cloud condensation nuclei (CCN) ability of amine aerosol has not been explored yet. Here, we study the hygroscopicity of aerosol formed from three aliphatic amines (trimethylamine, diethylamine and butylamine) in the UCR environmental chamber. Amines can react with NO3, a dominant night time oxidant in acid-base and/or oxidation reactions. The mass fraction of organic and inorganic components of formed aerosol was measured by Particle-into-Liquid Sampler coupled to dual ion chromatographs (PILS-ICs) and Scanning Mobility Particle Sizer (SMPS). CCN counter was used to measure the water-uptake ability of these particles. Significantly high hygroscopicity (κ>0.3) was observed for aerosols formed from diethylamine and butylamine with NO3 radicals, which comprised >40% inorganic salt. Compared with amines oxidized by hydroxyl radicals, the presence of aminium salts formed in acid-base reactions greatly improved CCN activity of NO3-initiated aerosol. The effect of water vapor on the formation of aminium salts and aerosol hygroscopicity was also studied. Our results will significantly impact the estimation and role of amines in atmospheric chemistry and global climate models.

  19. Hygroscopic Properties of Aircraft Engine Exhaust Aerosol Produced From Traditional and Alternative Fuels

    NASA Astrophysics Data System (ADS)

    Moore, R.; Ziemba, L. D.; Beyersdorf, A. J.; Thornhill, K. L.; Winstead, E. L.; Crumeyrolle, S.; Chen, G.; Anderson, B. E.

    2012-12-01

    Aircraft emissions of greenhouse gases and aerosols constitute an important component of anthropogenic climate forcing, of which aerosol-cloud interactions remain poorly understood. It is currently thought that the ability of these aerosols to alter upper tropospheric cirrus cloud properties may produce radiative forcings many times larger than the impact of linear contrails alone and which may partially offset the impact of greenhouse gas emissions from aviation (Burkhardt and Karcher, Nature, 2011). Consequently, it is important to characterize the ability of these engine-emitted aerosol to act as cloud condensation nuclei (CCN) and ice nuclei (IN) to form clouds. While a number of studies in the literature have examined aerosol-cloud interactions for laboratory-generated soot or from aircraft engines burning traditional fuels, limited attention has been given to how switching to alternative jet fuels impacts the ability of engine-emitted aerosols to form clouds. The key to understanding these changes is the aerosol hygroscopicity. To address this need, the second NASA Alternative Aviation Fuel Experiment (AAFEX-II) was conducted in 2011 to examine the aerosol emissions from the NASA DC-8 under a variety of different engine power and fuel type conditions. Five fuel types were considered including traditional JP-8 fuel, synthetic Fischer-Tropsh (FT) fuel , sulfur-doped FT fuel (FTS) , hydrotreated renewable jet (HRJ) fuel, and a 50:50 blend of JP-8 with HRJ. Emissions were sampled from the DC-8 on the airport jetway at a distance of 145 meters downwind of the engine by a comprehensive suite of aerosol instrumentation that provided information on the aerosol concentration, size distribution, soot mass, and CCN activity. Concurrent measurements of carbon dioxide were used to account for plume dilution so that characteristic emissions indices could be determined. It is found that both engine power and fuel type significantly influence the hygroscopic properties of

  20. INFLUENCE OF HYGROSCOPIC GROWTH UPON THE DEPOSITION OF BRONCHODILATOR AEROSOLS IN UPPER HUMAN AIRWAYS

    EPA Science Inventory

    The influence of hygroscopic growth upon the behavior of two bronchodilator drugs in upper airways is studied with an aerosol deposition model. The latter accounts for laryngeal jet impaction and turbulent flow instabilities caused by the larynx in computing particle deposition e...

  1. Application of Aerosol Hygroscopicity Measured at the Atmospheric Radiation Measurement Program's Southern Great Plains Site to Examine Composition and Evolution

    NASA Technical Reports Server (NTRS)

    Gasparini, Roberto; Runjun, Li; Collins, Don R.; Ferrare, Richard A.; Brackett, Vincent G.

    2006-01-01

    A Differential Mobility Analyzer/Tandem Differential Mobility Analyzer (DMA/TDMA) was used to measure submicron aerosol size distributions, hygroscopicity, and occasionally volatility during the May 2003 Aerosol Intensive Operational Period (IOP) at the Central Facility of the Atmospheric Radiation Measurement Program's Southern Great Plains (ARM SGP) site. Hygroscopic growth factor distributions for particles at eight dry diameters ranging from 0.012 micrometers to 0.600 micrometers were measured throughout the study. For a subset of particle sizes, more detailed measurements were occasionally made in which the relative humidity or temperature to which the aerosol was exposed was varied over a wide range. These measurements, in conjunction with backtrajectory clustering, were used to infer aerosol composition and to gain insight into the processes responsible for evolution. The hygroscopic growth of both the smallest and largest particles analyzed was typically less than that of particles with dry diameters of about 0.100 micrometers. It is speculated that condensation of secondary organic aerosol on nucleation mode particles is largely responsible for the minimal hygroscopic growth observed at the smallest sizes considered. Growth factor distributions of the largest particles characterized typically contained a nonhygroscopic mode believed to be composed primarily of dust. A model was developed to characterize the hygroscopic properties of particles within a size distribution mode through analysis of the fixed size hygroscopic growth measurements. The performance of this model was quantified through comparison of the measured fixed size hygroscopic growth factor distributions with those simulated through convolution of the size-resolved concentration contributed by each of the size modes and the mode-resolved hygroscopicity. This transformation from sizeresolved hygroscopicity to mode-resolved hygroscopicity facilitated examination of changes in the hygroscopic

  2. Optical and Physicochemical Properties of Brown Carbon Aerosol: Light Scattering, FTIR Extinction Spectroscopy, and Hygroscopic Growth.

    PubMed

    Tang, Mingjin; Alexander, Jennifer M; Kwon, Deokhyeon; Estillore, Armando D; Laskina, Olga; Young, Mark A; Kleiber, Paul D; Grassian, Vicki H

    2016-06-23

    A great deal of attention has been paid to brown carbon aerosol in the troposphere because it can both scatter and absorb solar radiation, thus affecting the Earth's climate. However, knowledge of the optical and chemical properties of brown carbon aerosol is still limited. In this study, we have investigated different aspects of the optical properties of brown carbon aerosol that have not been previously explored. These properties include extinction spectroscopy in the mid-infrared region and light scattering at two different visible wavelengths, 532 and 402 nm. A proxy for atmospheric brown carbon aerosol was formed from the aqueous reaction of ammonium sulfate with methylglyoxal. The different optical properties were measured as a function of reaction time for a period of up to 19 days. UV/vis absorption experiments of bulk solutions showed that the optical absorption of aqueous brown carbon solution significantly increases as a function of reaction time in the spectral range from 200 to 700 nm. The analysis of the light scattering data, however, showed no significant differences between ammonium sulfate and brown carbon aerosol particles in the measured scattering phase functions, linear polarization profiles, or the derived real parts of the refractive indices at either 532 or 402 nm, even for the longest reaction times with greatest visible extinction. The light scattering experiments are relatively insensitive to the imaginary part of the refractive index, and it was only possible to place an upper limit of k ≤ 0.01 on the imaginary index values. These results suggest that after the reaction with methylglyoxal the single scattering albedo of ammonium sulfate aerosol is significantly reduced but that the light scattering properties including the scattering asymmetry parameter, which is a measure of the relative amount of forward-to-backward scattering, remain essentially unchanged from that of unprocessed ammonium sulfate. The optical extinction properties

  3. Study of aerosol hygroscopic events over the Cabauw experimental site for atmospheric research (CESAR) using the multi-wavelength Raman lidar Caeli

    NASA Astrophysics Data System (ADS)

    Fernández, A. J.; Apituley, A.; Veselovskii, I.; Suvorina, A.; Henzing, J.; Pujadas, M.; Artíñano, B.

    2015-11-01

    This article presents a study of aerosol optical and microphysical properties under different relative humidity (RH) but well mixed layer conditions using optical and microphysical aerosol properties from multi-wavelength (MW) Raman lidar and in-situ aerosol observations collected at the Cabauw Experimental Site for Atmospheric Research (CESAR). Two hygroscopic events are described through 3 backscatter (β) and 2 extinction (α) coefficients which in turn provide intensive parameters such as the backscatter-related Ångström exponent (åβ) and the lidar ratio (LR). Along with it, profiles of RH were inferred from Raman lidar observations and therefore, as a result of varying humidity conditions, a shift on the aerosol optical properties can be described. Thus, it is observed that as RH increases, aerosols uptake water vapour, augment their size and consequently the åβ diminishes whereas the LR increases. The enhancement factor based on the backscatter coefficient at 532 nm, which characterizes the aerosol from hygroscopic standpoint, is also estimated. Finally, microphysical properties that are necessary for aerosol radiative forcing estimates - such as volume, effective radii, refractive index and size distribution, all vertically resolved - are retrieved using the inversion with regularization. Using this method, two hygroscopic events are described in detail.

  4. On aerosol hygroscopicity, cloud condensation nuclei (CCN) spectra and critical supersaturation measured at two remote islands of Korea between 2006 and 2009

    NASA Astrophysics Data System (ADS)

    Kim, J. H.; Yum, S. S.; Shim, S.; Yoon, S.-C.; Hudson, J. G.; Park, J.; Lee, S.-J.

    2011-07-01

    Aerosol size distribution, total concentration (i.e., condensation nuclei (CN) concentration, NCN), cloud condensation nuclei (CCN) concentration (NCCN), hygroscopicity at ~90 % relative humidity (RH) were measured at a background monitoring site at Gosan, Jeju Island, south of the Korea Peninsula in August 2006, April to May 2007 and August to October 2008. Similar measurement took place in August 2009 at another background site (Baengnyeongdo Comprehensive Monitoring Observatory, BCMO) on the island of Baengnyeongdo, off the west coast of the Korean Peninsula. Both islands were found to be influenced by continental sources regardless of season and year. Average values for all of the measured NCCN at 0.2, 0.6 and 1.0 % supersaturations (S), NCN, and geometric mean diameter (Dg) from both islands were in the range of 1043-3051 cm-3, 2076-4360 cm-3, 2713-4694 cm-3, 3890-5117 cm-3 and 81-98 nm, respectively. Although the differences in Dg and NCN were small between Gosan and BCMO, NCCN at various S was much higher at the latter, which is closer to China. Most of the aerosols were internally mixed and no notable differences in hygroscopicity were found between the days of strong pollution influence and the non-pollution days for both islands. During the 2008 and 2009 campaigns, critical supersaturation for cloud nucleation (Sc) for selected particle sizes was measured. Particles of 100 nm diameters had mean Sc of 0.19 ± 0.02 % during 2008 and those of 81 and 110 nm diameters had mean Sc of 0.26 ± 0.07 % and 0.17 ± 0.04 %, respectively, during 2009. Hygroscopicity parameters estimated from the measured Sc were mostly higher than the ones from the measured hygroscopic growth at ~90 % RH. For the 2008 campaign, NCCN at 0.2, 0.6 and 1.0 % S were predicted based on the measured dry particle size distribution and various ways of representing aerosol hygroscopicity. The best closure was obtained when temporally varying and size-resolved hygroscopicity information from

  5. Reconciling Organic Aerosol Volatility, Hygroscopicity, and Oxidation State During the Colorado DISCOVER-AQ Deployment

    NASA Astrophysics Data System (ADS)

    Hite, J. R.; Moore, R.; Martin, R.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.; Nenes, A.

    2014-12-01

    The organic fraction of submicron aerosol can profoundly impact radiative forcing on climate directly, through enhancement of extinction, or indirectly through modulation of cloud formation. Semi-volatile constituents of organic ambient aerosol are of particular interest as their partitioning between the vapor and aerosol phases is not well constrained by current atmospheric models and appears to play an important role in the formation of cloud condensation nuclei (CCN) as suggested by recent research. An experimental setup consisting of a DMT CCN counter and SMPS downstream of a custom-built thermodenuder assembly was deployed during the summer 2014 DISCOVER-AQ field campaign to retrieve simultaneous, size-resolved volatility and hygroscopicity - through the use of scanning mobility CCN analysis (SMCA). Housed in the NASA Langley mobile laboratory, a suite of complimentary measurements were made available onboard including submicron aerosol composition and oxidation state provided by an HR-ToF-AMS, and aerosol optical properties provided by a range of other instruments including an SP2. Air masses sampled from locations across the Central Colorado region include influences from regional aerosol nucleation/growth events, long-range transport of Canadian biomass burning aerosols, cattle feedlot emissions and influences of the Denver urban plume - amidst a backdrop of widespread oil and gas exploration. The analysis focuses on the reconciliation of the retrieved aerosol volatility distributions and corresponding hygroscopicity and oxidation state observations, including the use of AMS factor analysis.

  6. Characterizing the Hygroscopicity of Nascent Sea Spray Aerosol from Synthetic Blooms

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  7. Hygroscopic mixing state of urban aerosol derived from size-resolved cloud condensation nuclei measurements during the MEGAPOLI campaign in Paris

    NASA Astrophysics Data System (ADS)

    Jurányi, Z.; Tritscher, T.; Gysel, M.; Laborde, M.; Gomes, L.; Roberts, G.; Baltensperger, U.; Weingartner, E.

    2013-07-01

    Ambient aerosols are a complex mixture of particles with different physical and chemical properties and consequently distinct hygroscopic behaviour. The hygroscopicity of a particle determines its water uptake at subsaturated relative humidity (RH) and its ability to form a cloud droplet at supersaturated RH. These processes influence Earth's climate and the atmospheric lifetime of the particles. Cloud condensation nuclei (CCN) number size distributions (i.e. CCN number concentrations as a function of dry particle diameter) were measured close to Paris during the MEGAPOLI campaign in January-February 2010, covering 10 different supersaturations (SS = 0.1-1.0%). The time-resolved hygroscopic mixing state with respect to CCN activation was also derived from these measurements. Simultaneously, a hygroscopicity tandem differential mobility analyser (HTDMA) was used to measure the hygroscopic growth factor (ratio of wet to dry mobility diameter) distributions at RH = 90%. The aerosol was highly externally mixed and its mixing state showed significant temporal variability. The average particle hygroscopicity was relatively low at subsaturation (RH = 90%; mean hygroscopicity parameter κ = 0.12-0.27) and increased with increasing dry diameter in the range 35-265 nm. The mean κ value, derived from the CCN measurements at supersaturation, ranged from 0.08 to 0.24 at SS = 1.0-0.1%. Two types of mixing-state resolved hygroscopicity closure studies were performed, comparing the water uptake ability measured below and above saturation. In the first type the CCN counter was connected in series with the HTDMA and and closure was achieved over the whole range of probed dry diameters, growth factors and supersaturations using the κ-parametrization for the water activity and assuming surface tension of pure water in the Köhler theory. In the second closure type we compared hygroscopicity distributions derived from parallel monodisperse CCN measurements and HTDMA measurements

  8. CCN activation and hygroscopic growth measurements of secondary organic aerosols from tree emissions

    NASA Astrophysics Data System (ADS)

    Buchholz, Angela; Mentel, Thomas F.; Kiendler-Scharr, Astrid; Spindler, Christian; Tillmann, Ralf; Kleist, Einhard; Wildt, Juergen

    2010-05-01

    Plant emitted volatile organic compounds (VOCs) are a major precursor of secondary organic aerosols (SOA), an important constituent of atmospheric aerosols. We used the Juelich Plant Atmosphere Chamber (JPAC) at the Research Center Juelich to investigate the microphysical properties of aerosols. SOA particles were produced from the ozonolysis and reaction of OH radicals with the complex VOC mixture emitted from trees typical for the boreal forest. Hygroscopic growth factors (GF) were determined with a humidity tandem differential mobility analyzer (HTDMA) for different particle sizes at RH = 2 - 97%. Cloud condensation nuclei (CCN) activation was measured with a continuous flow CCN counter (DMT). Additionally, the chemical composition, size distribution and number concentration of the particles were measured. The gas phase was monitored with GC-MS and PTR-MS. Changing the emission pattern of the trees changed the measured GF and the diameter of the dry particles that were activated (Dcrit). However, below 80% RH the GF changes are within the range of the measurement error. The GF (RH = 95%) are between 1.11 and 1.19 and the Dcrit(SS = 0.4%) in a range of 93 - 100nm. Koehler theory was applied to achieve closure between CCN activation and GF measurements. The κ parameter according to Petters and Kreidenweis (2007) was calculated for all SS (κ(CCN)) and RH (κ(GF)). The κ(GF) decrease with increasing RH but levels off at RH > 95%. Assuming the surface tension of pure water, κ(GF, RH>95%) would be by a factor of 2 lower than κ(CCN). Closure between the HTDMA and CCN measurement requires the use of either a lower surface tension or a limited solubility of the organic material. Reference: Petters, M. D. and Kreidenweis, S. M. (2007). Atmos. Chem. Phys., 7, 1961-1971.

  9. Hygroscopic Measurements of Aerosol Particles in Colorado during the Discover AQ Campaign 2014

    NASA Astrophysics Data System (ADS)

    Orozco, D.; Delgado, R.; Espinosa, R.; Martins, J. V.; Hoff, R. M.

    2014-12-01

    In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground observations with other optical aerosol measurements such satellite and sunphotometric retrievals of aerosol optical depth and their inversions. In the summer of 2014, the DISCOVER-AQ campaign was held in Colorado, where systematic and concurrent observations of column- integrated surface, and vertically-resolved distributions of aerosols and trace gases relevant to air quality and their evolution during the day were observed. Aerosol optical properties were measured in the UMBC trailer at the city of Golden using a TSI-3563 nephelometer and an in-situ Polarized Imaging Nephelometer (PI-NEPH) designed and built by the LACO group at UMBC. The PI-NEPH measures aerosol phase matrix components in high angular range between 2 and 178 degrees scattering angle at three wavelengths (λ=473, 532 and 671nm). The two measured elements of the phase matrix, intensity (P11) and linear polarization (P12) provide extensive characterization of the scattering properties of the studied aerosol. The scattering coefficient, P11 and P12 were measured under different humidity conditions to obtain the enhancement factor f(RH) and the dependence of P11 and P12 to RH using a humidifier dryer system covering a RH range from 20 to 90%. The ratio between scattering coefficients at high and low humidity in Golden Colorado showed relatively low hygroscopic growth in the aerosol particles f(RH=80%) was 1.27±0.19 for the first three weeks of sampling. According to speciated measurements performed at the UMBC trailer, the predominance of dust and organic aerosols over more hygroscopic nitrate and sulfate in the

  10. Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation.

    PubMed

    Tang, Mingjin; Cziczo, Daniel J; Grassian, Vicki H

    2016-04-13

    Mineral dust aerosol is one of the major types of aerosol present in the troposphere. The molecular level interactions of water vapor with mineral dust are of global significance. Hygroscopicity, light scattering and absorption, heterogneous reactivity and the ability to form clouds are all related to water-dust interactions. In this review article, experimental techniques to probe water interactions with dust and theoretical frameworks to understand these interactions are discussed. A comprehensive overview of laboratory studies of water adsorption, hygroscopicity, cloud condensation, and ice nucleation of fresh and atmspherically aged mineral dust particles is provided. Finally, we relate laboratory studies and theoretical simulations that provide fundemental insights into these processes on the molecular level with field measurements that illustrate the atmospheric significance of these processes. Overall, the details of water interactions with mineral dust are covered from multiple perspectives in this review article. PMID:27015126

  11. Chemical and size effects of hygroscopic aerosols on light scattering coefficients

    NASA Astrophysics Data System (ADS)

    Tang, Ignatius N.

    1996-08-01

    The extensive thermodynamic and optical properties recently reported [Tang and Munkelwitz, 1994a] for sulfate and nitrate solution droplets are incorporated into a visibility model for computing light scattering by hygroscopic aerosols. The following aerosol systems are considered: NH4HSO4, (NH4)2SO4, (NH4)3H(SO4), NaHSO4, Na2SO4, NH4NO3, and NaNO3. In addition, H2SO4 and NaCl are included to represent freshly formed sulfate and background sea-salt aerosols, respectively. Scattering coefficients, based on 1 μg dry salt per cubic meter of air, are calculated as a function of relative humidity for aerosols of various chemical compositions and lognormal size distributions. For a given size distribution the light scattered by aerosol particles per unit dry-salt mass concentration is only weakly dependent on chemical constituents of the hygroscopic sulfate and nitrate aerosols. Sulfuric acid and sodium chloride aerosols, however, are exceptions and scatter light more efficiently than all other inorganic salt aerosols considered in this study. Both internal and external mixtures exhibit similar light-scattering properties. Thus for common sulfate and nitrate aerosols, since the chemical effect is outweighed by the size effect, it follows that observed light scattering by the ambient aerosol can be approximated, within practical measurement uncertainties, by assuming the aerosol being an external mixture. This has a definite advantage for either visibility degradation or climatic impact modeling calculations, because relevant data are now available for external mixtures but only very scarce for internal mixtures.

  12. Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements

    NASA Astrophysics Data System (ADS)

    Bhattu, Deepika; Tripathi, S. N.; Chakraborty, Abhishek

    2016-10-01

    The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ-Kohler theory using size-resolved CCN measurements (κCCN) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements (κAMS) were compared. The accumulation mode particles were found to be more hygroscopic (κCCN = 0.24) than Aitken mode (κCCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm-42 nm with κCCN = 0.13-0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κAMS>κCCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (forg) and κCCN at lower SS explained this behaviour. The decrease in κCCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%. Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the

  13. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    DOE PAGESBeta

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-24

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased duringmore » photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  14. A new experimental approach to study the hygroscopic and optical properties of aerosols: application to ammonium sulfate particles

    NASA Astrophysics Data System (ADS)

    Denjean, C.; Formenti, P.; Picquet-Varrault, B.; Katrib, Y.; Pangui, E.; Zapf, P.; Doussin, J. F.

    2014-01-01

    A new methodology for the determination of the changes due to hygroscopic growth with relative humidity of the number size distribution and optical properties of polydispersed aerosols is described. This method uses the simulation chamber CESAM where the hygroscopic properties of polydispersed aerosol particles can be investigated in situ by exposing them to RH ranging from 0 to 100% for approximately 1 h. In situ humidification is used to provide simultaneous information on the RH-dependence of the particle size and the corresponding scattering coefficient (σscat), and that for the entire size distribution. Optical closure studies, based on integrated nephelometer and aethalometer measurements, Mie scattering calculations and measured particle size distributions, can therefore be performed to yield derived parameters such as the complex refractive index (CRI) at λ = 525 nm. The CRI can also be retrieved in the visible spectrum by combining differential mobility analyzer (DMA) and white light aerosol spectrometer (Palas Welas®) measurements. We have applied this methodology to ammonium sulfate particles, which have well known optical and hygroscopic properties. The CRI obtained from the two methods (1.54-1.57) compared favourably to each other and are also in reasonable agreement with the literature values. The particle's growth was compared to values obtained for one selected size of particles (150 nm) with a H-TDMA and the effect of the residence time for particles humidification was investigated. When the humidification was performed in the chamber for a few minutes, a continuous increase of the ammonium sulfate particle's size and σscat was observed from RH values as low as 30% RH. Comparison of the measured and modelled values based on Köhler and Mie theories shows that layers of water are adsorbed on ammonium sulfate particles below the deliquescence point. In contradiction, the particle's growth reported with H-TDMAs showed a prompt deliquescence of

  15. Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid

    NASA Astrophysics Data System (ADS)

    Ehn, M.; Petäjä, T.; Aufmhoff, H.; Aalto, P.; Hämeri, K.; Arnold, F.; Laaksonen, A.; Kulmala, M.

    2006-10-01

    Freshly formed atmospheric aerosol particles are neither large enough to efficiently scatter incoming solar radiation nor able to act as cloud condensation nuclei. As the particles grow larger, their hygroscopicity determines the limiting size after which they are important in both of the aforementioned processes. The condensing species resulting in growth alter the hygroscopicity of the particles. We have measured hygroscopic growth of aerosol particles present in a boreal forest, along with the very hygroscopic atmospheric trace gas sulfuric acid. The focus was on days with new particle formation by nucleation. The measured hygroscopic growth factors (GF) correlated positively with gaseous phase sulfuric acid concentrations. This correlation had a strong size dependency; the smaller the particle, the more condensing sulfuric acid is bound to alter the GF due to initially smaller mass. In addition, water uptake of nucleation mode particles was monitored during new particle formation events and followed during their growth to Aitken mode sizes. As the modal diameter increased, the solubility of the particles decreased. This indicated that initially more hygroscopic particles transformed into less hygroscopic or even hydrophobic particles. A similar behavior was seen also during days with no particle formation, with GF decreasing during the evenings and increasing during early morning. This can be tentatively explained by day- and nighttime differences in the hygroscopicity of condensable vapors.

  16. Chemical closure study on hygroscopic properties of urban aerosol particles in Sapporo, Japan.

    PubMed

    Aggarwal, Shankar Gopala; Mochida, Michihiro; Kitamori, Yasuyuki; Kawamura, Kimitaka

    2007-10-15

    To assess the link between hygroscopicity of atmospheric particles and the chemical composition, we performed a chemical closure study on the hygroscopicity of organic-inorganic mixed particles nebulized from water extracts of ambient aerosols collected in Sapporo, Japan during summer 2005. The hygroscopicity of 100 nm particles was measured using a hygroscopicity tandem differential mobility analyzer (HTDMA) at 5-95% relative humidity. The chemical analyses of the extracts showed that inorganic salts accounted for 32-84% of the water-soluble fraction and that the remaining was water-soluble organic matter (WSOM). The liquid water content (LWC) of particles was primarily governed by the relative abundance of inorganic salts in particles. The chemical closure with a thermodynamic model did not indicate a significant perturbation of LWC by WSOM at 85% RH with the consideration of the uncertainties estimated. However, a positive perturbation by WSOM was suggested at 50% RH. Individual oxygenated compounds identified using gas chromatography were not abundant enough to substantially increase the LWC at 85% RH. PMID:17993129

  17. Hygroscopicity of internally mixed multi-component aerosol particles of atmospheric relevance

    NASA Astrophysics Data System (ADS)

    Liu, Qifan; Jing, Bo; Peng, Chao; Tong, Shengrui; Wang, Weigang; Ge, Maofa

    2016-01-01

    The hygroscopic properties of two water-soluble organic compounds (WSOCs) relevant to urban haze pollution (phthalic acid and levoglucosan) and their internally mixtures with inorganic salts (ammonium sulfate and ammonium nitrate) are investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA) system. The multi-component particles uptake water gradually in the range 5-90% relative humidity (RH). The experimental results are compared with the thermodynamic model predictions. For most mixtures, Extended Aerosol Inorganic Model (E-AIM) predictions agree well with the measured growth factors. The hygroscopic growth of mixed particles can be well described by the Zdanovskii-Stokes-Robinson (ZSR) relation as long as the mixed particles are completely liquid. ZSR calculations underestimate the water uptake of mixed particles at moderate RH due to the partial dissolution of ammonium sulfate in the organic and ammonium nitrate solution in this RH region. The phase of ammonium nitrate in the initial dry particles changes dramatically with the composition of mixtures. The presence of organics in the mixed particles can inhibit the crystallization of ammonium nitrate during the drying process and results in water uptake at low RH (RH < 60%). These results demonstrate that certain representative WSOCs can substantially influence the hygroscopicity of inorganic salts and overall water uptake of particles.

  18. A humidity controlled Nephelometer system to study the hygroscopic properties of aerosols in the marine environment

    NASA Astrophysics Data System (ADS)

    Vaishya, Aditya; O'Dowd, Colin; Jennings, S. Gerard

    2010-05-01

    A Humidograph system has been designed to study the hygroscopic properties of aerosols for different air-masses and for different seasons in the marine environment. Since ambient marine aerosols are likely to be found in a metastable state, and in accordance with recommendations of WMO/GAW to sample dry aerosol, a drying unit (Nafion based) is placed just after the inlet to dry the aerosols to a relative humidity (RH) < 40% so as not to misinterpret the optical properties of hygroscopic aerosols if they are on the descending branch of the hysteresis curve. The flow after the dryer is split into two, one going to a 3-wavelength TSI-3563 Integrating Nephelometer, and the other to a Gore-Tex based humidifier followed by a single-wavelength TSI-3561 Integrating Nephelometer. The humidifier is used to vary the RH from 40% to 90%. While the TSI-3563 Integrating Nephelometer will operate at RH < 40%, the TSI-3561 Integrating Nephelometer will operate under varying RH conditions. Software developed in LabVIEW is used to control the hardware components and to log the data in a predefined format. Results of the performance of the Humidograph system in the laboratory and at the Mace Head Atmospheric Research Station are presented.

  19. CCN Activity, Hygroscopicity, and Droplet Activation Kinetics of Secondary Organic Aerosol Resulting from the 2010 Gulf Oil Spill

    NASA Astrophysics Data System (ADS)

    Moore, R.; Lathem, T. L.; Cerully, K.; Bahreini, R.; Brock, C. A.; Langridge, J. M.; Middlebrook, A. M.; Nenes, A.; Calnex Science Team

    2010-12-01

    We present an analysis of the hygroscopicity and droplet activation kinetics of cloud condensation nuclei (CCN) sampled onboard the National Oceanic and Atmospheric Administration WP-3D aircraft downwind of the Deepwater Horizon oil spill site on June 8th and 10th, 2010. This set of measurements provides a unique case study for assessing in-situ the impact of fresh, hydrocarbonlike aerosols, which are expected to be formed via gas-to-particle conversion of the semi-volatile vapors released from oil evaporation. Similar hydrocarbon-rich aerosols constitute an important local emissions source in urban areas, but often coexist as an external/partially-internal mixture with more-oxidized, aged organic and sulfate aerosol. The DWH site provides the means to study the hygroscopic properties of these less-oxidized organic aerosols above a cleaner environmental background typical of marine environments in order to better discern their contribution to CCN activity and droplet growth. Measurements were performed with a Droplet Measurement Technologies Streamwise, Thermal-Gradient CCN counter, operating both as a counter (s=0.3%) and as a spectrometer (s=0.2-0.6%) using the newly-developed Scanning Flow CCN Analysis (SFCA) technique [1]. The instrument measures both the number concentration of particles able to nucleate droplets and also their resulting droplet sizes. The measured size information combined with a comprehensive computational fluid dynamics instrument model enables us to determine the rate of water uptake onto the particles and parameterize it in terms of an effective mass transfer coefficient [2], a key parameter needed to predict the number of activated droplets in ambient clouds. Non-refractory aerosol chemical composition was measured with an Aerodyne compact time-of-flight aerosol mass spectrometer. It was observed that the aerosols sampled downwind of the site on both days were composed predominantly of organics with a low degree of oxidation and low

  20. HYGROSCOPIC GROWTH: ITS EFFECT ON AEROSOL THERAPY AND INHALATION TOXICOLOGY

    EPA Science Inventory

    The success of an aerosol therapy protocol is contingent upon a proper quantity of drug being delivered to an appropriate site within the respiratory tract to elicit a therapeutic effect. Likewise, an accurate risk assessment of the threat to human health presented by airborne po...

  1. Aerosol mixing-state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    NASA Astrophysics Data System (ADS)

    Lance, S.; Raatikainen, T.; Onasch, T.; Worsnop, D. R.; Yu, X.-Y.; Alexander, M. L.; Stolzenburg, M. R.; McMurry, P. H.; Smith, J. N.; Nenes, A.

    2012-06-01

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic water uptake coefficient, κ*, for the CCN active aerosol population using both size-resolved HTDMA and size-resolved CCNc measurements. Organic mass fractions, forg, are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which κAMS is inferred and compared against κ*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% ± 0.06%. We also find that at 06:00-08:00 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as internally-mixed. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning "rush hour", and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the AMS

  2. Aerosol mixingstate, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    SciTech Connect

    Lance, Sara; Raatikainen, T.; Onasch, Timothy B.; Worsnop, Douglas R.; Yu, Xiao-Ying; Alexander, M. L.; Stolzenberg, Mark; McMurry, Peter; Smith, James N.; Nenes, Athanasios

    2013-05-15

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. K¨ohler theory is used to evaluate the characteristic water uptake coefficient, k*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions, (forg), are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which kAMS is inferred and compared against k*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased k* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% +/- 0.06%. We also find that at 0600-0800 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as “internally-mixed”. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning “rush hour”, and the entire campaign. We show that k* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for k* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the

  3. Reformulating atmospheric aerosol thermodynamics and hygroscopic growth into fog, haze and clouds

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Lelieveld, J.

    2007-06-01

    Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to consistently include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis - merely based on solute solubilities - to explicitly account for the water mass consumed by hydration. As a result, in chemical and thermodynamical equilibrium the relative humidity (RH) suffices to determine the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and directly links the aerosol hygroscopic growth to fog, haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3) for use in regional and global chemistry-transport and climate models. Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stoichiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as

  4. Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

    NASA Astrophysics Data System (ADS)

    Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

    2013-12-01

    The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles <100 nm generated by means of jets

  5. The effect of low solublility organic acids on the hygroscopicity of sodium halide aerosols

    NASA Astrophysics Data System (ADS)

    Miñambres, L.; Méndez, E.; Sánchez, M. N.; Castaño, F.; Basterretxea, F. J.

    2014-02-01

    In order to accurately assess the influence of fatty acids on the hygroscopic and other physicochemical properties of sea salt aerosols, hexanoic, octanoic or lauric acid together with sodium halide salts (NaCl, NaBr and NaI) have been chosen to be performed in this study. The hygroscopic properties of sodium halide submicrometer particles covered with organic acids have been examined by Fourier-transform infrared spectroscopy in an aerosol flow cell. Covered particles were generated by flowing atomized sodium halide particles (either dry or aqueous) through a heated oven containing the gaseous acid. The obtained results indicate that gaseous organic acids easily nucleate onto dry and aqueous sodium halide particles. On the other hand, Scanning Electron Microscopy (SEM) images indicate that lauric acid coating on NaCl particles makes them to aggregate in small clusters. The hygroscopic behaviour of covered sodium halide particles in deliquescence mode shows different features with the exchange of the halide ion: whereas the organic covering has little effect in NaBr particles, NaCl and NaI covered particles change their deliquescence relative humidities, with different trends observed for each of the acids studied. In efflorescence mode, the overall effect of the organic covering is to retard the loss of water in the particles. It has been observed that the presence of gaseous water in heterogeneously nucleated particles tends to displace the cover of hexanoic acid to energetically stabilize the system.

  6. The effect of low solubility organic acids on the hygroscopicity of sodium halide aerosols

    NASA Astrophysics Data System (ADS)

    Miñambres, L.; Méndez, E.; Sánchez, M. N.; Castaño, F.; Basterretxea, F. J.

    2014-10-01

    In order to accurately assess the influence of fatty acids on the hygroscopic and other physicochemical properties of sea salt aerosols, hexanoic, octanoic or lauric acid together with sodium halide salts (NaCl, NaBr and NaI) have been chosen to be investigated in this study. The hygroscopic properties of sodium halide sub-micrometre particles covered with organic acids have been examined by Fourier-transform infrared spectroscopy in an aerosol flow cell. Covered particles were generated by flowing atomized sodium halide particles (either dry or aqueous) through a heated oven containing the gaseous acid. The obtained results indicate that gaseous organic acids easily nucleate onto dry and aqueous sodium halide particles. On the other hand, scanning electron microscopy (SEM) images indicate that lauric acid coating on NaCl particles makes them to aggregate in small clusters. The hygroscopic behaviour of covered sodium halide particles in deliquescence mode shows different features with the exchange of the halide ion, whereas the organic surfactant has little effect in NaBr particles, NaCl and NaI covered particles experience appreciable shifts in their deliquescence relative humidities, with different trends observed for each of the acids studied. In efflorescence mode, the overall effect of the organic covering is to retard the loss of water in the particles. It has been observed that the presence of gaseous water in heterogeneously nucleated particles tends to displace the cover of hexanoic acid to energetically stabilize the system.

  7. Hygroscopicity Behavior, Activation Properties and Chemical Composition of Atmospheric Aerosol at a Background Site in the Megacity Region of Peking

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Nowak, Andreas; Mildenberger, Katrin; Göbel, Tina; Nekat, Bettina; van Pinxteren, Dominik; Herrmann, Hartmut; Zhao, Chunsheng; Wiedensohler, Alfred; Stratmann, Frank

    2010-05-01

    Large areas of China suffer from heavy air pollution (both gaseous and particulate) caused by strong economic growth in the last two decades. However, knowledge concerning the physical and chemical properties of the resulting aerosol particles populations, and their effects on the optical properties of the atmosphere, is still sparse. In the framework of the investigations presented here, comprehensive measurements concerning aerosol particle hygroscopicity, CCN ability, composition, and optical properties were performed. The investigations are part of the DFG-funded project HaChi (Haze in China) and are conducted in collaboration with the Peking University. A conclusive parameterization of aerosol hygroscopicity and activation data is aimed for, which will then be implemented in a meso-scale model to investigate aerosol-cloud-radiation and precipitation interactions. During two intensive measurements campaigns (March 2009 and July/ August 2009), in-situ aerosol measurements have been performed in an air-conditioned mobile laboratory next to the Wuqing Meteorological Station (39°23'8.53"N, 117°1'25.88"E), which is located between Bejing and Tijanjin and is thereby an ideal background site in a megacity region. The particle number size distribution (TDMPS), the particle optical properties (MAAP and nephelometer) and their hygroscopic properties at high RH (HH-TDMA, LACIS-mobile) were characterized as well as their cloud nucleating properties above supersaturation (DMT-CCNC). 24 h PM1 particle samples were continuously collected over the two campaigns in winter and summer using a DIGITEL high volume sampler (DHA-80). Additionally two 6h size-resolved samples (daytime and night-time) were collected each day applying an 11-stage Berner impactor. The size-selection of HH-TDMA, LACIS and the CCNC was synchronized with the Berner stages. Opening analysis of the winter campaign data showed that the HH-TDMA usually detected a hydrophobic and a hygroscopic mode, i.e., the

  8. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing

    PubMed Central

    Zhang, Renyi; Khalizov, Alexei F.; Pagels, Joakim; Zhang, Dan; Xue, Huaxin; McMurry, Peter H.

    2008-01-01

    The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by ≈10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing. PMID:18645179

  9. Hygroscopic properties of the Paris urban aerosol in relation to its chemical composition

    NASA Astrophysics Data System (ADS)

    Kamilli, K. A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.

    2014-01-01

    Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m-3, e.g., during winter.

  10. Hygroscopic properties of the Paris urban aerosol in relation to its chemical composition

    NASA Astrophysics Data System (ADS)

    Kamilli, K. A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.

    2013-05-01

    Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site LHVP in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m3, e.g. during winter.

  11. Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

    NASA Astrophysics Data System (ADS)

    Ziese, M.; Wex, H.; Nilsson, E.; Salma, I.; Ocskay, R.; Hennig, T.; Massling, A.; Stratmann, F.

    2007-09-01

    The hygroscopic growth and activation of two HULIS and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities up to 99.75%. The critical diameters for activation were measured using LACIS for supersaturations between 2 and 10 per mill. All three samples showed a similar hygroscopic growth behaviour, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini et al., 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from relative humidities larger than 98% up to activation. However it failed for the Aerosol-Water extract.

  12. Hygroscopicity of organic compounds from biomass burning and their influence on the water uptake of mixed organic ammonium sulfate aerosols

    NASA Astrophysics Data System (ADS)

    Lei, T.; Zuend, A.; Wang, W. G.; Zhang, Y. H.; Ge, M. F.

    2014-10-01

    Hygroscopic behavior of organic compounds, including levoglucosan, 4-hydroxybenzoic acid, and humic acid, as well as their effects on the hygroscopic properties of ammonium sulfate (AS) in internally mixed particles are studied by a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds used represent pyrolysis products of wood that are emitted from biomass burning sources. It is found that humic acid aerosol particles only slightly take up water, starting at RH (relative humidity) above ~70%. This is contrasted by the continuous water absorption of levoglucosan aerosol particles in the range 5-90% RH. However, no hygroscopic growth is observed for 4-hydroxybenzoic acid aerosol particles. Predicted water uptake using the ideal solution theory, the AIOMFAC model and the E-AIM (with UNIFAC) model are consistent with measured hygroscopic growth factors of levoglucosan. However, the use of these models without consideration of crystalline organic phases is not appropriate to describe the hygroscopicity of organics that do not exhibit continuous water uptake, such as 4-hydroxybenzoic acid and humic acid. Mixed aerosol particles consisting of ammonium sulfate and levoglucosan, 4-hydroxybenzoic acid, or humic acid with different organic mass fractions, take up a reduced amount of water above 80% RH (above AS deliquescence) relative to pure ammonium sulfate aerosol particles of the same mass. Hygroscopic growth of mixtures of ammonium sulfate and levoglucosan with different organic mass fractions agree well with the predictions of the thermodynamic models. Use of the Zdanovskii-Stokes-Robinson (ZSR) relation and AIOMFAC model lead to good agreement with measured growth factors of mixtures of ammonium sulfate with 4-hydroxybenzoic acid assuming an insoluble organic phase. Deviations of model predictions from the HTDMA measurement are mainly due to the occurrence of a microscopical solid phase restructuring at increased humidity (morphology

  13. Organic component vapor pressures and hygroscopicities of aqueous aerosol measured by optical tweezers.

    PubMed

    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. PMID:25522920

  14. Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)

    NASA Astrophysics Data System (ADS)

    Reutter, P.; Su, H.; Trentmann, J.; Simmel, M.; Rose, D.; Gunthe, S. S.; Wernli, H.; Andreae, M. O.; Pöschl, U.

    2009-09-01

    We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25-20 m s-1) and aerosol particle number concentrations (NCN=200-105 cm-3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10-3 m s-1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (<≈10-4 m s-1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN. (3) An aerosol- and updraft-sensitive regime (transitional regime), which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w. In sensitivity studies we have tested the influence of aerosol particle size distribution and hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05-0.6), we found that NCD depends rather weakly on the actual value of κ

  15. Reformulating atmospheric aerosol thermodynamics and hygroscopic growth into haze and clouds

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Lelieveld, J.

    2007-01-01

    Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis - merely based on solute solubilities. In chemical and thermodynamical equilibrium the relative humidity (RH) determines the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and to directly link the aerosol hygroscopic growth to haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3). Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stochiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as single solute molalities, molal based activities, including activity coefficients for volatile compounds, and deliquescence relative humidities of mixed solutes. Various

  16. Effect of aging on morphology, hygroscopicity, and optical properties of soot aerosol

    NASA Astrophysics Data System (ADS)

    Khalizov, A. F.; Xue, H.; Pagels, J.; McMurry, P. H.; Zhang, R.

    2009-12-01

    Soot from incomplete combustion represents one of the major forms of particulate matter pollution, profoundly impacting human health, air quality, and climate. The direct and indirect radiative effects of soot aerosol depend on particle composition and morphology, which may vary significantly when aerosol is subjected to atmospheric aging. We will present an overview of a comprehensive set of experimental measurements performed in our laboratory at Texas A&M to study the effect of internal mixing with atmospheric species on morphology, hygroscopicity, and optical properties of combustion soot. In our experiments, size-classified soot aerosol was exposed to 0.1 - 1000 ppb (part per billion) mixing ratios of sulfuric acid and dicarboxylic organic acids and resulting changes particle morphology and mixing state under dry and humid conditions were characterized through mass-mobility measurements by aerosol particle mass analyzer (APM) and tandem differential mobility analyzer (TDMA). Light absorption and scattering cross-sections for well-characterized fresh and coated soot aerosol were derived using a cavity ring-down spectrometer and an integrating nephelometer in order to assess the effect of atmospheric processing on the radiative properties of atmospheric soot. Internally mixed soot shows significant changes in particle morphology, increasing with the mass fraction of the coating material and relative humidity. Restructuring was the strongest for aggregates coated by sulfuric and glutaric acids whereas succinic acid coating did not result in observable morphology change. Sulfuric acid - coated particles experienced large hygroscopic growth at sub-saturated conditions and activated to cloud droplets at atmospherically relevant supersaturations. Furthermore, coating and subsequent hygroscopic growth considerably altered the optical properties of soot aerosol, increasing light scattering and absorption cross-sections. We found that irreversible restructuring of soot

  17. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    DOE PAGESBeta

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J. -D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; et al

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water solublemore » fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the

  18. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-03-01

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ∼34% in the accumulation vs. ∼47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ∼70%, while efflorescence occurred at different humidities, i.e., at ∼35% RH for submicron particles vs. ∼50% RH for supermicron particles. This ∼15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ∼0.15 for

  19. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-08-01

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws

  20. Hygroscopic properties of smoke-generated organic aerosol particles emitted in the marine atmosphere

    NASA Astrophysics Data System (ADS)

    Wonaschütz, A.; Coggon, M.; Sorooshian, A.; Modini, R.; Frossard, A. A.; Ahlm, L.; Mülmenstädt, J.; Roberts, G. C.; Russell, L. M.; Dey, S.; Brechtel, F. J.; Seinfeld, J. H.

    2013-10-01

    During the Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE), a plume of organic aerosol was produced by a smoke generator and emitted into the marine atmosphere from aboard the R/V Point Sur. In this study, the hygroscopic properties and the chemical composition of the plume were studied at plume ages between 0 and 4 h in different meteorological conditions. In sunny conditions, the plume particles had very low hygroscopic growth factors (GFs): between 1.05 and 1.09 for 30 nm and between 1.02 and 1.1 for 150 nm dry size at a relative humidity (RH) of 92%, contrasted by an average marine background GF of 1.6. New particles were produced in large quantities (several 10 000 cm-3), which lead to substantially increased cloud condensation nuclei (CCN) concentrations at supersaturations between 0.07 and 0.88%. Ratios of oxygen to carbon (O : C) and water-soluble organic mass (WSOM) increased with plume age: from < 0.001 to 0.2, and from 2.42 to 4.96 μg m-3, respectively, while organic mass fractions decreased slightly (~ 0.97 to ~ 0.94). High-resolution aerosol mass spectrometer (AMS) spectra show that the organic fragment m/z 43 was dominated by C2H3O+ in the small, new particle mode and by C3H7+ in the large particle mode. In the marine background aerosol, GFs for 150 nm particles at 40% RH were found to be enhanced at higher organic mass fractions: an average GF of 1.06 was observed for aerosols with an organic mass fraction of 0.53, and a GF of 1.04 for an organic mass fraction of 0.35.

  1. Aerosol hygroscopicity and CCN activity during the AC3Exp campaign: Implications for CCN parameterization

    NASA Astrophysics Data System (ADS)

    Zhang, Fang; Li, Yanan; Li, Zhanqing

    2015-04-01

    Atmospheric aerosol particles acting as CCN are pivotal elements of the hydrological cycle and climate change. In this study, we measured and characterized NCCN in relatively clean and polluted air during the AC3Exp campaign conducted at Xianghe, China during summer 2013. The aim was to examine CCN activation properties under high aerosol loading conditions in a polluted region and to assess the impacts of particle size and chemical composition on the CCN AR which acts as a proxy of the total number of aerosol particles in the atmosphere. A gradual increase in size-resolved AR with particle diameter suggests that aerosol particles have different hygroscopicities. For particles in the accumulation mode, values of κapa range from 0.31-0.38 under background conditions, which is about 20% higher than that derived under polluted conditions. For particles in the nucleation or Aitken mode, κ range from 0.20-0.34 under both background and polluted conditions. Larger particles were on average more hygroscopic than smaller particles. However, the case is more complex for particles originating from heavy pollution due to the diversity in particle composition and mixing state. The low R2 for the NPO CCN closure test suggests a 30%-40% uncertainty in total NCCN estimation. Using bulk chemical composition data from ACSM measurements, the relationship between bulk AR and the physical and chemical properties of atmospheric aerosols is investigated. Based on a case study, it has been concluded that one cannot use a parameterized formula using only total NCN to estimate total NCCN. Our results showed a possibility of using bulk κchem and f44 in combination with bulk NCN > 100 nm to parameterize CCN number concentrations.

  2. Ambient sulfate aerosol deposition in man: modeling the influence of hygroscopicity.

    PubMed Central

    Martonen, T B; Barnett, A E; Miller, F J

    1985-01-01

    Atmospheric sulfate aerosols [H2SO4, (NH4)2SO4, and NH4HSO4] are of international concern because of their global prevalence and potential irritant or toxic effects on humans. To assess hazards following inhalation exposure, the total dose delivered to the human respiratory tract and its regional distribution must be determined. The mass median aerodynamic diameter of the inhaled aerosol will influence the sites of deposition in the respiratory tract. Atmospheric sulfate aerosols are hygroscopic and will have changing particle sizes and densities as they absorb water vapor in the humid environment of the human respiratory tract. Experimental and theoretical data that describe particle size as a function of temperature and relative humidity were used in computer subroutines of an aerosol deposition model in order to calculate the dose dispersion of H2SO4, (NH4)2SO4, and NH4HSO4 aerosols in man. Different temperature and relative humidity environments that approximately correspond to nasal and oral breathing were studied. The predicted deposition patterns are very different from those of nonhygroscopic aerosols with identical inhaled mass median aerodynamic diameter values. PMID:4076076

  3. Variations in hygroscopic growth of sub- and super-micron sea spray aerosols during a phytoplankton bloom

    NASA Astrophysics Data System (ADS)

    Forestieri, S.; Jayarathne, T. S.; Stone, E. A.; Laskina, O.; Grassian, V. H.; Lee, C.; Sultana, C. M.; Moore, K.; Cornwell, G.; Novak, G.; Bertram, T. H.; Prather, K. A.; Cappa, C. D.

    2014-12-01

    Marine sea spray aerosols (SSA) make up an important portion of natural aerosols (prior to anthropogenic influence) and are therefore important in establishing the baseline for anthropogenic aerosol climate impacts. One way aerosols impact climate is by scattering solar radiation, and how much light is scattered depends upon the size of aerosols. Aerosols grow larger via water uptake and thus scatter more light at elevated relative humidities. This growth depends on composition. SSA can become enriched in organics during phytoplankton blooms, becoming less salty and therefore less hygroscopic. Aerosol hygroscopicity of SSA sampled during an in-lab phytoplankton bloom were measured during the CAICE-IMPACTS 2014 study. SSA were generated via breaking waves in an enclosed 33 m wave channel filled with natural seawater. Aerosol hygroscopicity was characterized by measuring light extinction at 532 nm of dry aerosols and of aerosols humidified to 85% relative humidity using a Cavity Ringdown Spectrometer. These optical growth factors (humidified extinction/dry extinction) were converted to physical growth factors using Mie Theory calculations and aerosol size distributions measured with a scanning electrical mobility spectrometer (SEMS) and an aerodynamic particle sizer (APS). Growth factors for super- and sub-micron SSA were quantified separately through the use of a PM2.5 cyclone or PM1 impactor. The observed SSA growth factors will be linked to SSA and source water chemical composition determined by both offline and online analysis of samples. The SSA bulk growth factors will also be compared with concurrent measurements of the efficiency with which SSA act as cloud condensation nuclei. Observed SSA growth factors will also be compared to offline hygroscopic growth measurements.

  4. Hygroscopic Characteristics of Organic Laden Ambient Aerosols in Yosemite National Park

    NASA Astrophysics Data System (ADS)

    Malm, W. C.; Day, D. E.; Kreidenweis, S. M.; Collett, J. L.; Carrico, C. M.; Lee, T.; Bench, G.; Carrillo, J.

    2003-12-01

    Water absorption by inorganic compounds can be modeled with some degree of certainty; however, water uptake by ambient organic aerosols remains speculative. To improve the understanding of organic hygroscopicity, an aerosol characterization study was conducted at Yosemite National Park, California, starting in July and ending in the first week of September 2002. High time resolution measurement (15-minute time increments) of PM2.5 ionic species (Cl-, SO42-, NO3-, Na+, NH4+, K+, Mg2+, and Ca2+) were measured using PILS (Particle-Into-Liquid-System)/IC (Ion Chromatography). Commercially available annular denuders and a PM2.5 cyclone (URG) were used upstream of the PILS/IC to remove particles greater than 2.5 μm and acidic and basic gases. A dual wavelength aethalometer and an R&P particulate carbon monitor were used to measure carbon on a semi-continuous basis while a DRUM sampler allowed for semi-continuous estimates of concentrations of elements associated with crustal material. Standard IMPROVE type samplers were used to measure 24-hr integrated samples of these same aerosols. Two nephelometers operated in tandem, one dry and the other with a controlled humidity environment, were used to measure f(RH) = bscat(RH)/bscat,dry, where bscat(RH) is the scattering coefficient measured at some relative humidity and bscat,dry is the scattering coefficient measured at RH <10%. The aerosol composition was highly variable in time, with a strong diurnal cycle. Organic carbon mass was observed to be, on the average, 70% of the fine mass with days where its contribution was well over 95% of the mass. Measurements of carbon isotopes revealed the fraction of carbon from biogenic sources to range from approximately 73 to 95%. Water soluble potassium was highly correlated with carbon mass, suggesting the influence of wood smoke. The ionic fraction of the aerosol consisted primarily of ammonium sulfate and in most cases nitrate was in the form of sodium nitrate. Fine soil mass was

  5. Influence of particle-phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2015-05-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle-phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids to phase-separated particles to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40 to 90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids; (2) forcing a single phase but accounting for non-ideal interactions through activity coefficient calculations; and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation of the inorganic and organic components is assumed at all RH values, with water uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  6. Influence of particle phase state on the hygroscopic behavior of mixed organic-inorganic aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Mui, W.; Flagan, R. C.; Seinfeld, J. H.

    2014-12-01

    Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particle phase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids, to phase-separated particles, to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40-90%. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids, (2) forcing a single phase, but accounting for non-ideal interactions through activity coefficient calculations, and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation between the inorganic and organic components is assumed at all RH values, with water-uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquid-liquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrose-containing particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF

  7. AMS Measurements in National Parks of Aerosol Mass, Size and Composition, Comparison with Filter Samples and Correlation with Particle Hygroscopicity and Optical Extinction Properties

    NASA Astrophysics Data System (ADS)

    Alexander, M.; Taylor, N. F.; Collins, D. R.; Kumar, N.; Allen, J.; Newburn, M.; Lowenthal, D. H.; Zielinska, B.

    2011-12-01

    We report a comparison of results from aerosol studies at Great Smoky Mountain National Park (2006), Mt. Rainier National Park (2009) and Acadia National Park (2011), all class I visibility areas associated with IMPROVE (Interagency Monitoring of Protected Visual Environments) sites. This collaborative study was sponsored by the Electric Power Research Institute (EPRI) and was done with the cooperation of the National Park Service and the EPA. The atmospheric aerosol composition in these sites is influenced by a number of anthropogenic as well as biogenic sources, providing a rich environment for fundamental aerosol studies. The primary purpose of these studies was to add state-of-the-art aerosol instrumentation to the standard light extinction and aerosol measurements at the site, used to determine parameters for the IMPROVE light extinction reconstruction equation, adopted by the EPA to estimate light extinction from atmospheric aerosol concentrations and Rayleigh scattering. The combination of these diverse measurements also provides significant insight into fundamental aerosol properties such as aging and radiative forcing. New instrumentation included a quadrupole aerosol mass spectrometer (Aerodyne Q-AMS-Smoky Mountain Study), a high resolution aerosol time-of-flight mass spectrometer (Aerodyne HR-ToF-AMS - Mt. Rainier and Acadia studies) for real time measurements that directly address the relationship between sulfate, nitrate, and OC size and concentration, which is related to cloud and dry gas-to-particle conversion as air masses age during transport, the relationship between WSOC hygroscopic growth and oxygenated organic (OOA) composition, the OCM/OC ratio, and the chemical composition that determines the ambient hygroscopic state. The OCM/OC ratio and organic water uptake was addressed with high-volume and medium volume PM2.5 aerosol samples. Aerosols were collected daily on Teflon coated glass fiber filters (TGFF) in four high-volume PM2.5 samplers

  8. Sensitivity of depositions to the size and hygroscopicity of Cs-bearing aerosols released from the Fukushima nuclear accident

    NASA Astrophysics Data System (ADS)

    Kajino, Mizuo; Adachi, Kouji; Sekiyama, Tsuyoshi; Zaizen, Yuji; Igarashi, Yasuhito

    2014-05-01

    We recently revealed that the microphysical properties of aerosols carrying the radioactive Cs released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) at an early stage (March 14-15, 2011) of the accident could be very different from what we assumed previously: super-micron and non-hygroscopic at the early stage, whereas sub-micron and hygroscopic afterwards (at least later than March 20-22). In the study, two sensitivity simulations with the two different aerosol microphysical properties were conducted using a regional scale meteorology- chemical transport model (NHM-Chem). The impact of the difference was quite significant. 17% (0.001%) of the radioactive Cs fell onto the ground by dry (wet) deposition processes, and the rest was deposited into the ocean or was transported out of the model domain, which is central and northern part of the main land of Japan, under the assumption that Cs-bearing aerosols are non-hygroscopic and super-micron. On the other hand, 5.7% (11.3%) fell onto the ground by dry (wet) deposition, for the cases under the assumption that the Cs-bearing aerosols are hygroscopic and sub-micron. For the accurate simulation of the deposition of radionuclides, knowledge of the aerosol microphysical properties is essential as well as the accuracy of the simulated wind fields and precipitation patterns.

  9. Composition and hygroscopicity of aerosol particles at Mt. Lu in South China: Implications for acid precipitation

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Chi, Jianwei; Shi, Zongbo; Wang, Xinfeng; Chen, Bin; Wang, Yan; Li, Tao; Chen, Jianmin; Zhang, Daizhou; Wang, Zifa; Shi, Chune; Liu, Liangke; Wang, Wenxing

    2014-09-01

    Physicochemical properties of aerosol particles were studied at Mt. Lu, an elevated site (115°59‧E, 29°35‧N, 1165 m) within the acid precipitation area. Northeast winds transport copious amounts of air pollutants and water vapor from the Yangtze River Delta into this acid precipitation area. NH4+ and SO42- are the dominant ions in PM2.5 and determine aerosol acidity. Individual particle analysis shows abundant S-rich and metals (i.e. Fe-, Zn-, Mn-, and Pb-rich) particles. Unlike aerosol particles in North China and urban areas, there are little soot and mineral particles at Mt. Lu. Lack of mineral particles contributed to the higher acidity in precipitation in the research area. Nano-sized spherical metal particles were observed to be embedded in 37% of S-rich particles. These metal particles were likely originated from heavy industries and fired-power plants. Hygroscopic experiments show that most particles start to deliquesce at 73-76% but organic coating lowers the particle deliquescence relative humidity (DRH) to 63-73%. The DRHs of these aerosol particles are clearly smaller than that of pure ammonium sulfate particles which is 80%. Since RH in ambient air was relatively high, ranging from 65% to 85% during our study period, most particles at our sampling site were in liquid phase. Our results suggest that liquid phase reactions in aerosol particles may contribute to SO2 to sulfuric acid conversion in the acid precipitation area.

  10. Low hygroscopic scattering enhancement of boreal aerosol and the implications for a columnar optical closure study

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Aalto, P. P.; Aaltonen, V.; Äijälä, M.; Backman, J.; Hong, J.; Komppula, M.; Krejci, R.; Laborde, M.; Lampilahti, J.; de Leeuw, G.; Pfüller, A.; Rosati, B.; Tesche, M.; Tunved, P.; Väänänen, R.; Petäjä, T.

    2015-07-01

    Ambient aerosol particles can take up water and thus change their optical properties depending on the hygroscopicity and the relative humidity (RH) of the surrounding air. Knowledge of the hygroscopicity effect is of crucial importance for radiative forcing calculations and is also needed for the comparison or validation of remote sensing or model results with in situ measurements. Specifically, particle light scattering depends on RH and can be described by the scattering enhancement factor f(RH), which is defined as the particle light scattering coefficient at defined RH divided by its dry value (RH <30-40 %). Here, we present results of an intensive field campaign carried out in summer 2013 at the SMEAR II station at Hyytiälä, Finland. Ground-based and airborne measurements of aerosol optical, chemical and microphysical properties were conducted. The f(RH) measured at ground level by a humidified nephelometer is found to be generally lower (e.g. 1.63±0.22 at RH = 85 % and λ = 525 nm) than observed at other European sites. One reason is the high organic mass fraction of the aerosol encountered at Hyytiälä to which f(RH) is clearly anti-correlated (R2≈0.8). A simplified parametrization of f(RH) based on the measured chemical mass fraction can therefore be derived for this aerosol type. A trajectory analysis revealed that elevated values of f(RH) and the corresponding elevated inorganic mass fraction are partially caused by transported hygroscopic sea spray particles. An optical closure study shows the consistency of the ground-based in situ measurements. Our measurements allow to determine the ambient particle light extinction coefficient using the measured f(RH). By combining the ground-based measurements with intensive aircraft measurements of the particle number size distribution and ambient RH, columnar values of the particle extinction coefficient are determined and compared to columnar measurements of a co-located AERONET sun photometer. The water

  11. Multiwavelength In-situ Aerosol Absorption, Scattering, and Hygroscopic Properties During the TEXAQS 2006 Field Campaign: Aerosol Classification and Variability

    NASA Astrophysics Data System (ADS)

    Sierau, B.; Covert, D. S.; Coffman, D. J.; Quinn, P. K.; Bates, T. S.

    2007-12-01

    In-situ, three wavelength-measurements of optical properties of the aerosol near the coast of Texas, i.e. in the region of Houston and the Houston ship channel, as well as in the Gulf of Mexico were carried out onboard the NOAA research vessel Ronald H. Brown during the 2006 TEXAQS/GoMACCS field campaign in July through September 2006. Aerosol scattering, hemispheric backscattering and absorption-coefficients were measured for particles with diameters dp<10μm and dp<1μm using integrating nephelometers and filter-based absorption photometers (PSAPs) at 60% RH (nephelometers). Submicrometric light scattering coefficient was measured at two additional humidities, ca. 25%, and 85% RH. Together with the 60% RH data, this enabled determination of the effect of aerosol hygroscopic growth on light scattering and an empirical light scattering growth factor. The results are relevant to radiation transfer, visibility, air quality, and interpretation of remote sensing data from lidar and satellite. The extensive and intensive optical properties along with meteorological analysis are used to characterize the aerosol in the Houston, TX region and the Coastal Gulf of Mexico and to provide information critical to understanding the climatic and air quality impacts of those aerosols. Further analysis focuses on the changes that these properties undergo during chemical processing of emissions within the project area and how they are affected by changes in atmospheric relative humidity that accompany transport, diurnal cycles and vertical mixing. The results are classified by source region and flow regime of the sampled air masses to identify distinct aerosol populations. Special emphasis is given to the physico-chemical properties of aerosols measured during two periods when Saharan dust was encountered during the cruise as well as to several air pollution episodes and plumes from industrial complexes. The combination of hygroscopic growth, light scattering and absorption

  12. Airborne characterization of subsaturated aerosol hygroscopicity and dry refractive index from the surface to 6.5 km during the SEAC4RS campaign

    NASA Astrophysics Data System (ADS)

    Shingler, Taylor; Crosbie, Ewan; Ortega, Amber; Shiraiwa, Manabu; Zuend, Andreas; Beyersdorf, Andreas; Ziemba, Luke; Anderson, Bruce; Thornhill, Lee; Perring, Anne E.; Schwarz, Joshua P.; Campazano-Jost, Pedro; Day, Douglas A.; Jimenez, Jose L.; Hair, Johnathan W.; Mikoviny, Tomas; Wisthaler, Armin; Sorooshian, Armin

    2016-04-01

    In situ aerosol particle measurements were conducted during 21 NASA DC-8 flights in the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys field campaign over the United States, Canada, Pacific Ocean, and Gulf of Mexico. For the first time, this study reports rapid, size-resolved hygroscopic growth and real refractive index (RI at 532 nm) data between the surface and upper troposphere in a variety of air masses including wildfires, agricultural fires, biogenic, marine, and urban outflow. The Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe (DASH-SP) quantified size-resolved diameter growth factors (GF = Dp,wet/Dp,dry) that are used to infer the hygroscopicity parameter κ. Thermokinetic simulations were conducted to estimate the impact of partial particle volatilization within the DASH-SP across a range of sampling conditions. Analyses of GF and RI data as a function of air mass origin, dry size, and altitude are reported, in addition to κ values for the inorganic and organic fractions of aerosol. Average RI values are found to be fairly constant (1.52-1.54) for all air mass categories. An algorithm is used to compare size-resolved DASH-SP GF with bulk scattering f(RH = 80%) data obtained from a pair of nephelometers, and the results show that the two can only be reconciled if GF is assumed to decrease with increasing dry size above 400 nm (i.e., beyond the upper bound of DASH-SP measurements). Individual case studies illustrate variations of hygroscopicity as a function of dry size, environmental conditions, altitude, and composition.

  13. Estimation of surface-level PM concentration from satellite observation taking into account the aerosol vertical profiles and hygroscopicity.

    PubMed

    Kim, Kwanchul; Lee, Kwon H; Kim, Ji I; Noh, Youngmin; Shin, Dong H; Shin, Sung K; Lee, Dasom; Kim, Jhoon; Kim, Young J; Song, Chul H

    2016-01-01

    Surface-level PM10 distribution was estimated from the satellite aerosol optical depth (AOD) products, taking the account of vertical profiles and hygroscopicity of aerosols over Jeju, Korea during March 2008 and October 2009. In this study, MODIS AOD data from the Terra and Aqua satellites were corrected with aerosol extinction profiles and relative humidity data. PBLH (Planetary Boundary Layer Height) was determined from MPLNET lidar-derived aerosol extinction coefficient profiles. Through statistical analysis, better agreement in correlation (R = 0.82) between the hourly PM10 concentration and hourly average Sunphotometer AOD was the obtained when vertical fraction method (VFM) considering Haze Layer Height (HLH) and hygroscopic growth factor f(RH) was used. The validity of the derived relationship between satellite AOD and surface PM10 concentration clearly demonstrates that satellite AOD data can be utilized for remote sensing of spatial distribution of regional PM10 concentration. PMID:26421659

  14. The Effects of Mineral Dust on the Hygroscopic and Optical Properties of Inorganic Salt Aerosols

    NASA Astrophysics Data System (ADS)

    Attwood, A. R.; Greenslade, M. E.

    2011-12-01

    Mineral dust particles are a significant fraction of the total aerosol mass, thus they play an important role in the Earth's radiative budget by direct scattering and absorption of radiation. Assessing this impact is complicated by the variability of optical properties resulting from water uptake and changes in chemical composition due to atmospheric mixing. Internal mixtures of montmorillonite, a clay component of mineral dust, with sodium chloride and ammonium sulfate were studied optically using cavity ring down spectroscopy. The effects of the addition of the clay to the optically observed deliquescence relative humidity (DRH) and water uptake of these salts was considered by investigating a series of different salt mass fractions. In most cases, montmorillonite alters the hygroscopic properties and causes the DRH to occur at a lower relative humidity. For ammonium sulfate, optical properties can be approximated by volume weighted mixing rules with some minor deviations around the DRH. For sodium chloride, this approximation is only accurate below the DRH with enhanced water uptake at higher relative humidities. Our results show that salt particles may transition from solid to liquid at a lower relative humidity than is expected based on the salt alone, as observed with changes in optical properties. Further, they contradict current measurements in the literature that suggest little change in the hygroscopic behavior of salts when insoluble mineral dust components are added and should continue to be investigated. Accurate, direct measurements of the effect of the addition of clays to the optical properties of common aerosol species will allow for improvements in the prediction of the aerosol direct effect.

  15. Numerical investigation of the coagulation mixing between dust and hygroscopic aerosol particles and its impacts

    NASA Astrophysics Data System (ADS)

    Tsai, I.-Chun; Chen, Jen-Ping; Lin, Yi-Chiu; Chung-Kuang Chou, Charles; Chen, Wei-Nai

    2015-05-01

    A statistical-numerical aerosol parameterization was incorporated into the Community Multiscale Air Quality modeling system to study the coagulation mixing process focusing on a dust storm event that occurred over East Asia. Simulation results show that the coagulation mixing process tends to decrease aerosol mass, surface area, and number concentrations over the dust source areas. Over the downwind oceanic areas, aerosol concentrations generally increased due to enhanced sedimentation as particles became larger upon coagulation. The mixture process can reduce the overall single-scattering albedo by up to 10% as a result of enhanced core with shell absorption by dust and reduction in the number of scattering particles. The enhanced dry deposition speed also altered the vertical distribution. In addition, the ability of aerosol particles to serve as cloud condensation nuclei (CCN) increased from around 107 m-3 to above 109 m-3 over downwind areas because a large amount of mineral dust particles became effective CCN with solute coating, except over the highly polluted areas where multiple collections of hygroscopic particles by dust in effect reduced CCN number. This CCN effect is much stronger for coagulation mixing than by the uptake of sulfuric acid gas on dust, although the nitric acid gas uptake was not investigated. The ability of dust particles to serve as ice nuclei may decrease or increase at low or high subzero temperatures, respectively, due to the switching from deposition nucleation to immersion freezing or haze freezing.

  16. Airborne measurements of hygroscopicity and mixing state of aerosols in the planetary boundary layer during the PEGASOS campaigns

    NASA Astrophysics Data System (ADS)

    Rosati, Bernadette; Weingartner, Ernest; Gysel, Martin; Rubach, Florian; Mentel, Thomas; Baltensperger, Urs

    2014-05-01

    Aerosols interact directly with the incident solar radiation by scattering or absorbing the light. The optical properties of an aerosol particle can strongly be altered at enhanced relative humidity (RH). Depending on the particle's chemical composition, it can experience hygroscopic growth, leading to a change in size and index of refraction compared to the dry particle (Zieger et al., 2011). Besides, aerosols can exist in different mixing states which are usually divided into internal and external mixtures. If all particles of a certain size have the same chemical composition, they are described as internally mixed, whereas if particles of equal size have different chemical composition, they are defined as externally mixed. Depending on the mixture the hygroscopic behavior will change: internally mixed aerosols will grow uniformly with increasing RH, while the different substances in external mixtures will experience different growing behaviors leading to a mode-splitting or broadened size distribution. Laboratory studies are commonly performed at dry conditions but it is known that temperature and RH as well as chemical composition are changing with altitude (Morgan et al., 2010). This further leads to the conclusion that the in-situ measurements of optical properties at different heights are crucial for climate forcing calculations. Within the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) the white- light humidified optical particle spectrometer (WHOPS) was developed and installed on the Zeppelin to investigate changes of light scattering with regard to water uptake and altitude. This instrument firstly selects a dry monodisperse aerosol by its electrical mobility and then exposes it to a well-defined RH (typically 95%). Alternately, the dry and humidified particles are measured in a white-light optical particle spectrometer (WELAS). In this way it is possible to infer the effective index of refraction of the dry particles, their hygroscopic

  17. Comparative analysis of hygroscopic properties of atmospheric aerosols at ZOTTO Siberian background station during summer and winter campaigns of 2011

    NASA Astrophysics Data System (ADS)

    Ryshkevich, T. I.; Mironov, G. N.; Mironova, S. Yu.; Vlasenko, S. S.; Chi, X.; Andreae, M. O.; Mikhailov, E. F.

    2015-09-01

    The results of measurements of hygroscopic properties and chemical analysis of atmospheric aerosol samples collected from June 10 to 20 and December 15 to 25, 2011, at the ZOTTO background stations (60.8° N, 89.35° E) in Central Siberia are presented. The sorption properties of aerosols are studied with the help of a differential analyzer of absorbed water mass in the relative humidity range of 5 to 99%. It has been found that the hygroscopic growth factor of aerosol particles collected during the winter campaign is on average 45% higher than that of the aerosol collected in the summer campaign, which leads to a 40% decrease in the critical supersaturation threshold of cloud activation of particles. The measurement data are analyzed and parameterized using a new approach that takes into account the concentration effects in the particle—water vapor system at low humidities. Based on the chemical analysis, the content of water-soluble substances in the winter sample is 2.5 times higher than in the summer sample. Here, the amount of sulfates and nitrates increases 20 and 88 times, respectively. A trajectory analysis of air mass motion shows that the increased content of inorganic ions in aerosols for the winter sample is caused by long-range transport of pollutants from industrial areas of Siberia. This difference in the chemical composition is the main source of the observed difference in hygroscopic and condensation properties of the aerosol particles.

  18. Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

    NASA Astrophysics Data System (ADS)

    Ziese, M.; Wex, H.; Nilsson, E.; Salma, I.; Ocskay, R.; Hennig, T.; Massling, A.; Stratmann, F.

    2008-03-01

    The hygroscopic growth and activation of two HULIS (HUmic LIke Substance) and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator) together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer). Hygroscopic growth was determined for relative humidities (RHs) up to 99.75%. The critical diameters for activation were measured for supersaturations between 0.2 and 1%. All three samples showed a similar hygroscopic growth behavior, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a) and the Szyszkowski-equation (Szyszkowski, 1908; Facchini, 1999) were used for parameterizing the Raoult and the Kelvin (surface tension) terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from RHs larger than 98% up to activation. It was also shown to work well with data on HULIS taken from literature. Here, different atmospheric life-times and/or different sources for the different samples showed up in different coefficients for the parameterization. However, the parameterization did not work out well for the Aerosol-Water-Extract.

  19. Hygroscopicity and CCN activity of atmospheric aerosol particles and their relation to organics: Characteristics of urban aerosols in Nagoya, Japan

    NASA Astrophysics Data System (ADS)

    Kawana, Kaori; Nakayama, Tomoki; Mochida, Michihiro

    2016-04-01

    The size-resolved distributions of hygroscopic growth factor g and the ratios of cloud condensation nuclei (CCN) to condensation nuclei of atmospheric aerosols were investigated in Nagoya, Japan. The average of the distributions of g at 85% relative humidity was bimodal. The size-resolved mean κ derived from g showed an increasing trend with diameter: 0.17-0.33 at 24-359 nm. The κ values calculated from CCN activation curves were 37% higher than those derived from g. Only 9% of the 37% difference is explained by the difference in the κ of inorganics under subsaturated and supersaturated conditions, suggesting a contribution of organics to the remaining 28% difference. The size-averaged κ of organics (κorg) was calculated as 0.14 and 0.19 by two different methods. The number fractions of CCN predicted from the hygroscopicity data over the range of 24-359 nm are loosely consistent with those observed if the size- and time-averaged g is applied to all particles (differences: -30% to +10%). This consistency improves if size- and time-resolved g and g distribution are used (differences: -19% to -3%). Whereas the number fractions of CCN predicted from the composition data are greatly underestimated if organics are assumed to be insoluble (differences: -64% to -45%), they are more consistent if κorg of 0.14 or 0.19 is applied (differences: -10% to +14%). The results demonstrate the importance of the dependence of the g of particles on time and particle size and the hygroscopicity of organics for CCN number concentrations in the urban atmosphere.

  20. Accurate Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative Humidity.

    PubMed

    Rovelli, Grazia; Miles, Rachael E H; Reid, Jonathan P; Clegg, Simon L

    2016-06-30

    Using a comparative evaporation kinetics approach, we describe a new and accurate method for determining the equilibrium hygroscopic growth of aerosol droplets. The time-evolving size of an aqueous droplet, as it evaporates to a steady size and composition that is in equilibrium with the gas phase relative humidity, is used to determine the time-dependent mass flux of water, yielding information on the vapor pressure of water above the droplet surface at every instant in time. Accurate characterization of the gas phase relative humidity is provided from a control measurement of the evaporation profile of a droplet of know equilibrium properties, either a pure water droplet or a sodium chloride droplet. In combination, and by comparison with simulations that account for both the heat and mass transport governing the droplet evaporation kinetics, these measurements allow accurate retrieval of the equilibrium properties of the solution droplet (i.e., the variations with water activity in the mass fraction of solute, diameter growth factor, osmotic coefficient or number of water molecules per solute molecule). Hygroscopicity measurements can be made over a wide range in water activity (from >0.99 to, in principle, <0.05) on time scales of <10 s for droplets containing involatile or volatile solutes. The approach is benchmarked for binary and ternary inorganic solution aerosols with typical uncertainties in water activity of <±0.2% at water activities >0.9 and ∼±1% below 80% RH, and maximum uncertainties in diameter growth factor of ±0.7%. For all of the inorganic systems examined, the time-dependent data are consistent with large values of the mass accommodation (or evaporation) coefficient (>0.1). PMID:27285052

  1. Effect of hygroscopic growth on the aerosol light-scattering coefficient: A review of measurements, techniques and error sources

    NASA Astrophysics Data System (ADS)

    Titos, G.; Cazorla, A.; Zieger, P.; Andrews, E.; Lyamani, H.; Granados-Muñoz, M. J.; Olmo, F. J.; Alados-Arboledas, L.

    2016-09-01

    Knowledge of the scattering enhancement factor, f(RH), is important for an accurate description of direct aerosol radiative forcing. This factor is defined as the ratio between the scattering coefficient at enhanced relative humidity, RH, to a reference (dry) scattering coefficient. Here, we review the different experimental designs used to measure the scattering coefficient at dry and humidified conditions as well as the procedures followed to analyze the measurements. Several empirical parameterizations for the relationship between f(RH) and RH have been proposed in the literature. These parameterizations have been reviewed and tested using experimental data representative of different hygroscopic growth behavior and a new parameterization is presented. The potential sources of error in f(RH) are discussed. A Monte Carlo method is used to investigate the overall measurement uncertainty, which is found to be around 20-40% for moderately hygroscopic aerosols. The main factors contributing to this uncertainty are the uncertainty in RH measurement, the dry reference state and the nephelometer uncertainty. A literature survey of nephelometry-based f(RH) measurements is presented as a function of aerosol type. In general, the highest f(RH) values were measured in clean marine environments, with pollution having a major influence on f(RH). Dust aerosol tended to have the lowest reported hygroscopicity of any of the aerosol types studied. Major open questions and suggestions for future research priorities are outlined.

  2. Chemical and hygroscopic properties of aerosol organics at Storm Peak Laboratory

    NASA Astrophysics Data System (ADS)

    Hallar, A. Gannet; Lowenthal, Douglas H.; Clegg, Simon L.; Samburova, Vera; Taylor, Nathan; Mazzoleni, Lynn R.; Zielinska, Barbara K.; Kristensen, Thomas B.; Chirokova, Galina; McCubbin, Ian B.; Dodson, Craig; Collins, Don

    2013-05-01

    A combined field and laboratory study was conducted to improve our understanding of the chemical and hygroscopic properties of organic compounds in aerosols sampled in the background continental atmosphere. PM2.5 (particles with aerodynamic diameters smaller than 2.5 µm) aerosols were collected from 24 June to 28 July 2010 at Storm Peak Laboratory (SPL) in the Park Range of northwestern Colorado. New particle formation (NPF) was frequent at SPL during this campaign, and the samples were not influenced by regional dust storms. Filter samples were analyzed for organic carbon (OC) and elemental carbon (EC), water soluble OC (WSOC), major inorganic ions, and detailed organic speciation. WSOC was isolated from inorganic ions using solid phase absorbents. Hygroscopic growth factors (GFs) and cloud condensation nucleus (CCN) activity of the WSOC were measured in the laboratory. Organic compounds compose the majority (average of 64% with a standard deviation (SD) of 9%) of the mass of measured species and WSOC accounted for an average of 89% (with a SD of 21%) of OC mass. Daily samples were composited according to back trajectories. On average, organic acids, sugars, and sugar alcohols accounted for 12.5 ± 6.2% (average ± SD) of WSOC. Based on the composition of these compounds and that of high molecular weight compounds identified using ultra high resolution mass spectrometry, the organic mass to OC ratio of the WSOC is estimated to be 2.04. The average hygroscopic GFs at RH = 80% (GF80) were 1.10 ± 0.03 for particles derived from isolated WSOC and 1.27 ± 0.03 for particles derived from the total water-soluble material (WSM). CCN activity followed a similar pattern. The critical diameters at a super-saturation of 0.35% were 0.072 ± 0.009 and 0.094 ± 0.006 µm for particles derived from WSM and isolated WSOC, respectively. These GF results compare favorably with estimates from thermodynamic models, which explicitly relate the water activity (RH) to concentration for

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  4. Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods

    NASA Astrophysics Data System (ADS)

    Meier, J.; Wehner, B.; Massling, A.; Birmili, W.; Nowak, A.; Gnauk, T.; Brüggemann, E.; Herrmann, H.; Min, H.; Wiedensohler, A.

    2009-03-01

    This paper presents hygroscopicity measurements of aerosol particles in the urban atmosphere of Beijing carried out in January 2005. Therefore, three different methods were used: 1) Combining Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements; 2) Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) technique; 3) Calculating hygroscopic growth factors on the basis of a solubility model quantified by Micro Orifice Uniform Deposit Impactor (MOUDI) samples. Particle number size distributions from H-DMPS and TDMPS were evaluated to derive size-resolved descriptive hygroscopic growth factors (DHGF) of 30-400 nm particles at relative humidities (RH) of 55%, 77% and 90%. The atmospheric particles in Beijing were rather hydrophobic, with a maximum growth factor in the accumulation mode around 1.40 (±0.03) at 90% RH. The descriptive hygroscopic growth factors decreased significantly towards the lower measurement limit (1.04 (±0.15) at Dp=30 nm). A good agreement was found between the DHGFs and the H-TDMA-derived hygroscopic growth factors in the accumulation mode (100-400 nm), the DHGFs underestimated the values from the H-TDMA in the Aitken mode (<100 nm) by up to 0.1 at 90% RH. The calculation of hygroscopic growth factors based on the measured chemical composition showed that different modes of combining the inorganic ions caused a variation in growth factor of 0.1 at 90% RH. The solubility model was able to reproduce the size-dependent trend in the growth factor found by the other methods. In two cases of ion-dominated aerosol, the composition-derived growth factors tended to agree (±0.05) or underestimate (up to 0.1) the values measured by the other two methods. In the case of the organic-dominated aerosol, the reverse was true, with an overestimation of up to 0.2. The results shed light on the real experimental and methodological uncertainties that are still connected with the

  5. On aerosol hygroscopicity, cloud condensation nuclei (CCN) spectra and critical supersaturation measured at two remote islands of Korea between 2006 and 2009

    NASA Astrophysics Data System (ADS)

    Kim, J. H.; Yum, S. S.; Shim, S.; Yoon, S.-C.; Hudson, J. G.; Park, J.; Lee, S.-J.

    2011-12-01

    Aerosol size distribution, total concentration (i.e. condensation nuclei (CN) concentration, NCN), cloud condensation nuclei (CCN) concentration (NCCN), hygroscopicity at ~90% relative humidity (RH) were measured at a background monitoring site at Gosan, Jeju Island, south of the Korean Peninsula in August 2006, April to May 2007 and August to October 2008. Similar measurements took place in August 2009 at another background site (Baengnyeongdo Comprehensive Monitoring Observatory, BCMO) on the island of Baengnyeongdo, off the west coast of the Korean Peninsula. Both islands were found to be influenced by continental sources regardless of season and year. Average values for all of the measured NCCN at 0.2, 0.6 and 1.0% supersaturations (S), NCN, and geometric mean diameter (Dg) from both islands were in the range of 1043-3051 cm-3, 2076-4360 cm-3, 2713-4694 cm-3, 3890-5117 cm-3 and 81-98 nm, respectively. Although the differences in Dg and NCN were small between Gosan and BCMO, NCCN at various S was much higher at the latter, which is closer to China. Most of the aerosols were internally mixed and no notable differences in hygroscopicity were found between the days of strong pollution influence and the non-pollution days for both islands. During the 2008 and 2009 campaigns, critical supersaturation for CCN nucleation (Sc) for selected particle sizes was measured. Particles of 100 nm diameters had mean Sc of 0.19 ± 0.02% during 2008 and those of 81 and 110 nm diameters had mean Sc of 0.26 ± 0.07% and 0.17 ± 0.04%, respectively, during 2009. The values of the hygroscopicity parameter (κ), estimated from measured Sc, were mostly higher than the κ values obtained from the measured hygroscopic growth at ~90% RH. For the 2008 campaign, NCCN at 0.2, 0.6 and 1.0% S were predicted based on measured dry particle size distributions and various ways of representing particle hygroscopicity. The best closure was obtained when temporally varying and size

  6. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    SciTech Connect

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    The atmosphere is composed of a complex mixture of gases and suspended microscopic aerosol particles. The ability of these particles to take up water (hygroscopicity) and to act as nuclei for cloud droplet formation significantly impacts aerosol light scattering and absorption, and cloud formation, thereby influencing air quality, visibility, and climate in important ways. A substantial, yet poorly characterized component of the atmospheric aerosol is organic matter. Its major sources are direct emissions from combustion processes, which are referred to as primary organic aerosol (POA), or in situ processes in which volatile organic compounds (VOCs) are oxidized in the atmosphere to low volatility reaction products that subsequent condense to form particles that are referred to as secondary organic aerosol (SOA). POA and VOCs are emitted to the atmosphere from both anthropogenic and natural (biogenic) sources. The overall goal of this experimental research project was to conduct laboratory studies under simulated atmospheric conditions to investigate the effects of the chemical composition of organic aerosol particles on their hygroscopicity and cloud condensation nucleation (CCN) activity, in order to develop quantitative relationships that could be used to more accurately incorporate aerosol-cloud interactions into regional and global atmospheric models. More specifically, the project aimed to determine the products, mechanisms, and rates of chemical reactions involved in the processing of organic aerosol particles by atmospheric oxidants and to investigate the relationships between the chemical composition of organic particles (as represented by molecule sizes and the specific functional groups that are present) and the hygroscopicity and CCN activity of oxidized POA and SOA formed from the oxidation of the major classes of anthropogenic and biogenic VOCs that are emitted to the atmosphere, as well as model hydrocarbons. The general approach for this project was

  7. Comparison Between Lidar and Nephelometer Measurements of Aerosol Hygroscopicity at the Southern Great Plains Atmospheric Radiation Measurement Site

    NASA Technical Reports Server (NTRS)

    Pahlow, M.; Feingold, G.; Jefferson, A.; Andrews, E.; Ogren, J. A.; Wang, J.; Lee, Y.-N.; Ferrare, R. A.

    2004-01-01

    Aerosol hygroscopicity has a significant effect on radiative properties of aerosols. Here a lidar method, applicable to cloud-capped, well-mixed atmospheric boundary layers, is employed to determine the hygroscopic growth factor f(RH) under unperturbed, ambient atmospheric conditions. The data used for the analysis were collected under a wide range of atmospheric aerosol levels during both routine measurement periods and during the intensive operations period (IOP) in May 2003 at the Southern Great Plains (SGP) Climate Research Facility in Oklahoma, USA, as part of the Atmospheric Radiation Measurement (ARM) program. There is a good correlation (approx. 0.7) between a lidar-derived growth factor (measured over the range 85% RH to 96% RH) with a nephelometer-derived growth factor measured over the RH range 40% to 85%. For these RH ranges, the slope of the lidar-derived growth factor is much steeper than that of the nephelometer-derived growth factor, reflecting the rapid increase in particle size with increasing RH. The results are corroborated by aerosol model calculations of lidar and nephelometer equivalent f(RH) based on in situ aerosol size and composition measurements during the IOP. It is suggested that the lidar method can provide useful measurements of the dependence of aerosol optical properties on relative humidity, and under conditions closer to saturation than can currently be achieved with humidified nephelometers.

  8. Hygroscopic and Chemical Properties of Aerosols collected near a Copper Smelter: Implications for Public and Environmental Health

    PubMed Central

    Sorooshian, Armin; Csavina, Janae; Shingler, Taylor; Dey, Stephen; Brechtel, Fred J.; Sáez, A. Eduardo; Betterton, Eric A.

    2012-01-01

    Particulate matter emissions near active copper smelters and mine tailings in the southwestern United States pose a potential threat to nearby environments owing to toxic species that can be inhaled and deposited in various regions of the body depending on the composition and size of the particles, which are linked by particle hygroscopic properties. This study reports the first simultaneous measurements of size-resolved chemical and hygroscopic properties of particles next to an active copper smelter and mine tailings by the towns of Hayden and Winkelman in southern Arizona. Size-resolved particulate matter samples collected near an active copper smelter were examined with inductively coupled plasma mass spectrometry, ion chromatography, and a humidified tandem differential mobility analyzer. Aerosol particles collected at the measurement site are enriched in metals and metalloids (e.g. arsenic, lead, and cadmium) and water-uptake measurements of aqueous extracts of collected samples indicate that the particle diameter range of particles most enriched with these species (0.18–0.55 µm) overlaps with the most hygroscopic mode at a relative humidity of 90% (0.10–0.32 µm). These measurements have implications for public health, microphysical effects of aerosols, and regional impacts owing to the transport and deposition of contaminated aerosol particles. PMID:22852879

  9. Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods

    NASA Astrophysics Data System (ADS)

    Meier, J.; Wehner, B.; Massling, A.; Birmili, W.; Nowak, A.; Gnauk, T.; Brüggemann, E.; Herrmann, H.; Min, H.; Wiedensohler, A.

    2009-09-01

    The hygroscopic properties of atmospheric aerosols are highly relevant for the quantification of radiative effects in the atmosphere, but also of interest for the assessment of particle health effects upon inhalation. This article reports measurements of aerosol particle hygroscopicity in the highly polluted urban atmosphere of Beijing, China in January 2005. The meteorological conditions corresponded to a relatively cold and dry atmosphere. Three different methods were used: 1) A combination of Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements, 2) A Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), and 3) A simplistic solubility model fed by chemical particle composition determined from Micro Orifice Uniform Deposit Impactor (MOUDI) samples. From the H-DMPS and TDMPS particle number size distributions, a size-resolved descriptive hygroscopic growth factor (DHGF) was determined for the relative humidities (RH) 55%, 77% and 90%, and particle diameters between 30 and 400 nm. In Beijing, the highest DHGFs were observed for accumulation mode particles, 1.40 (±0.03) at 90% RH. DHGF decreased significantly with particle size, reaching 1.04 (±0.15) at 30 nm. H-TDMA data also suggest a decrease in growth factor towards the biggest particles investigated (350 nm), associated with an increasing fraction of nearly hydrophobic particles. The agreement between the H-DMPS/TDMPS and H-TDMA methods was satisfactory in the accumulation mode size range (100-400 nm). In the Aitken mode range (<100 nm), the H-DMPS/TDMPS method yielded growth factors lower by up to 0.1 at 90% RH. The application of the solubility model based on measured chemical composition clearly reproduced the size-dependent trend in hygroscopic particle growth observed by the other methods. In the case of aerosol dominated by inorganic ions, the composition-derived growth factors tended to agree (± 0.05) or underestimate (up to

  10. Size Resolved measurements of aerosol hygroscopicity and mixing state during Green Ocean Amazon (GoAmazon) 2014

    NASA Astrophysics Data System (ADS)

    Thalman, R. M.; Artaxo, P.; Campuzano Jost, P.; Barbosa, H. M.; Day, D. A.; de Sá, S. S.; Hu, W.; Jimenez, J. L.; Kuang, C.; Palm, B. B.; Krüger, M. L.; Manzi, A. O.; Martin, S. T.; Poeschl, U.; Sedlacek, A. J., III; Senum, G.; Souza, R. A. F. D.; Springston, S. R.; Alexander, M. L.; Watson, T. B.; Wang, J.

    2014-12-01

    Measurements of size-resolved cloud condensation nucleai (CCN) spectra were performed at the T3 site of the Green Ocean Amazon (GoAmazon) field project located near Manacapuru, Brazil during 2014. The T3 site is a receptor site for both polluted urban down-wind (Manaus, BR a city of several million 70 km up wind) and background (Amazon rainforest) air-masses and can provide a contrast between clean and polluted conditions. Particle hygroscopicity (kappa) and mixing state were calculated from the particle activation spectrum measured by size selecting aerosols and exposing them to a wide range of supersaturation in the CCN counter (Droplet Measurement Technologies Continuous-Flow Streamwise Thermal Gradient CCN Chamber). The supersaturation was varied between 0.07 and 1.1% by changing a combination of both total flow rate and temperature gradient in the CCN counter. Measured spectra were examined for air masses with different level of influence from Manaus plume. Particle hygroscopicity generally peaked near noon local time which was broadly consistent with the trend in aerosol sulfate. The average kappa values during the first intensive operation period were 0.14±0.05, 0.14±0.04 and 0.16±0.06 for 75, 112 and 171 nm particles respectively. Evaluation of particle hygroscopicity and dispersion (mixing state) will be presented with respect to size and level of pollution.

  11. Aging of secondary organic aerosol from small aromatic VOCs. Changes in chemical composition, mass yield, volatility and hygroscopicity

    DOE PAGESBeta

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2014-12-12

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form and transform SOA from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx. The effects of chemical aging on organic aerosol (OA) composition, mass yield, volatility and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state OSC) and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSmore » C ranged from -0.29 to 0.45 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  12. Relating the hygroscopic properties of submicron aerosol to both gas- and particle-phase chemical composition in a boreal forest environment

    NASA Astrophysics Data System (ADS)

    Hong, J.; Kim, J.; Nieminen, T.; Duplissy, J.; Ehn, M.; Äijälä, M.; Hao, L. Q.; Nie, W.; Sarnela, N.; Prisle, N. L.; Kulmala, M.; Virtanen, A.; Petäjä, T.; Kerminen, V.-M.

    2015-10-01

    Measurements of the hygroscopicity of 15-145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-Aerosols-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a high-resolution aerosol mass spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (O : C ratio) of the organic matter in the particle phase. Using an O : C dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii-Stokes-Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics concentration (ELVOC) and the HGF of particles of any size.

  13. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    SciTech Connect

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J. -D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode.

    The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments.

    The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was

  14. Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulphate

    NASA Astrophysics Data System (ADS)

    Badger, C. L.; George, I.; Griffiths, P. T.; Braban, C. F.; Cox, R. A.; Abbatt, J. P. D.

    2006-03-01

    The phase transitions and hygroscopic growth of two humic acid aerosols (Aldrich sodium salt and Leonardite Standard (IHSS)) and their mixtures with ammonium sulphate have been investigated using a combination of two techniques, Fourier transform infra-red (FTIR) spectroscopy and tandem differential mobility analysis (TDMA). A growth factor of 1.16 at 85% relative humidity (RH) was found for the Aldrich humic acid which can be regarded as an upper limit for growth factors of humic-like substances (HULIS) found in atmospheric aerosol and is significantly smaller than that of typical atmospheric inorganics. We find that the humic acid aerosols exhibit water uptake over all relative humidities with no apparent phase changes, suggesting that these aerosols readily form supersaturated droplets. In the mixed particles, the humic acid component decreases the deliquescence relative humidity (DRH) and increases the efflorescence relative humidity (ERH) of the ammonium sulphate component, and there is some degree of water uptake prior to ammonium sulphate deliquescence. In addition, at low RH, the FTIR spectra show that the ammonium is present in a different chemical environment in the mixed aerosols than in crystalline ammonium sulphate, perhaps existing as a complex with the humic materials. The growth factors of the mixed aerosols are intermediate between those of the single-component aerosols and can be predicted assuming that the inorganic and organic fractions take up water independently.

  15. Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulphate

    NASA Astrophysics Data System (ADS)

    Badger, C. L.; George, I.; Griffiths, P. T.; Braban, C. F.; Cox, R. A.; Abbatt, J. P. D.

    2005-10-01

    The phase transitions and hygroscopic growth of two humic acid aerosols (Aldrich sodium salt and Leonardite Standard (IHSS)) and their mixtures with ammonium sulphate have been investigated using a combination of two techniques, Fourier transform infra-red (FTIR) spectroscopy and tandem differential mobility analysis (TDMA). A growth factor of 1.16 at 85% relative humdity (RH) was found for the Aldrich humic acid which can be regarded as an upper limit for growth factors of humic-like substances (HULIS) found in atmospheric aerosol and is significantly smaller than that of typical atmospheric inorganics. We find that the humic acid aerosols exhibit water uptake over all relative humidites with no apparent phase changes, suggesting that these aerosols readily form supersaturated droplets. In the mixed particles, the humic acid component decreases the deliquescence relative humidity (DRH) and increases the efflorescence relative humidity (ERH) of the ammonium sulphate component, and there is some degree of water uptake prior to ammonium sulphate deliquescence. In addition, at low RH, the FTIR spectra show that the ammonium is present in a different chemical environment in the mixed aerosols than in crystalline ammonium sulphate, perhaps existing as a complex with the humic materials. The growth factors of the mixed aerosols are intermediate between those of the single component aerosols and can be predicted assuming that the inorganic and organic fractions take up water independently.

  16. Study of Aerosol Liquid Water Content based on Hygroscopicity Measurements at High Relative Humidity in the North China Plain

    NASA Astrophysics Data System (ADS)

    Bian, Y.; Zhao, C.

    2013-12-01

    Aerosol has significant effects on direct/indirect climate forcing, visibility, tropospheric chemistry and human health. Water can represent an extensive proportion of the mass of aerosol particles, and can also serve as a medium for aqueous-phase reactions in such particulate matter. In this study, a new method is proposed to estimate the aerosol liquid water content at high relative humidity, based on aerosol hygroscopic growth factors, particle number size distribution and relative humidity measured during the Haze in China (HaChi) campaign of July-August, 2009. The aerosol liquid water content estimated by this method is compared to the results calculated by a thermodynamic equilibrium model (ISORROPIA II). The calculation results from these two methods agree well at high relative humidity above 60% with the correlation coefficient of 0.9658. At relative humidity lower than 60%, the thermodynamic equilibrium model underestimates the aerosol liquid water content. The discrepancy is mainly caused by the ISORROPIA II model, which considers only limited chemical species. The mean and maximum value of aerosol liquid water content during July-August, 2009 in the North China Plain reached 1.69×10^{-4}g/m^3 and 9.71×10^{-4}g/m^3, respectively. Aerosol liquid water content is highly related to the relative humidity. There exists a distinct diurnal variation of the aerosol liquid water content, with lower values during daytime and higher ones during night time. The contribution to the aerosol liquid water content from the accumulation mode is dominating among all the aerosol particle modes.

  17. Relating the hygroscopic properties of submicron aerosol to both gas- and particle-phase chemical composition in a boreal forest environment

    NASA Astrophysics Data System (ADS)

    Hong, J.; Kim, J.; Nieminen, T.; Duplissy, J.; Ehn, M.; Äijälä, M.; Hao, L.; Nie, W.; Sarnela, N.; Prisle, N. L.; Kulmala, M.; Virtanen, A.; Petäjä, T.; Kerminen, V.-M.

    2015-06-01

    Measurements of the hygroscopicity of 15-145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-AeroSOIs-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a High-Resolution Aerosol Mass Spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (O : C ratio) of the organic matter in the particle phase. Using an O : C dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii-Stokes-Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more there was sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics (ELVOCs) concentration and the HGF of particles of any size.

  18. Relating hygroscopicity and optical properties to chemical composition and structure of secondary organic aerosol particles generated from the ozonolysis of α-pinene

    NASA Astrophysics Data System (ADS)

    Denjean, C.; Formenti, P.; Picquet-Varrault, B.; Pangui, E.; Zapf, P.; Katrib, Y.; Giorio, C.; Tapparo, A.; Monod, A.; Temime-Roussel, B.; Decorse, P.; Mangeney, C.; Doussin, J. F.

    2015-03-01

    Secondary organic aerosol (SOA) were generated from the ozonolysis of α-pinene in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber. The SOA formation and aging were studied by following their optical, hygroscopic and chemical properties. The optical properties were investigated by determining the particle complex refractive index (CRI). The hygroscopicity was quantified by measuring the effect of relative humidity (RH) on the particle size (size growth factor, GF) and on the scattering coefficient (scattering growth factor, f(RH)). The oxygen to carbon atomic ratios (O : C) of the particle surface and bulk were used as a sensitive parameter to correlate the changes in hygroscopic and optical properties of the SOA composition during their formation and aging in CESAM. The real CRI at 525 nm wavelength decreased from 1.43-1.60 (±0.02) to 1.32-1.38 (±0.02) during the SOA formation. The decrease in the real CRI correlated to the O : C decrease from 0.68 (±0.20) to 0.55 (±0.16). In contrast, the GF remained roughly constant over the reaction time, with values of 1.02-1.07 (±0.02) at 90% (±4.2%) RH. Simultaneous measurements of O : C of the particle surface revealed that the SOA was not composed of a homogeneous mixture, but contained less oxidised species at the surface which may limit water absorption. In addition, an apparent change in both mobility diameter and scattering coefficient with increasing RH from 0 to 30% was observed for SOA after 14 h of reaction. We postulate that this change could be due to a change in the viscosity of the SOA from a predominantly glassy state to a predominantly liquid state.

  19. Hygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: implications for regional direct radiative forcing under clean and polluted conditions

    NASA Astrophysics Data System (ADS)

    Stock, M.; Cheng, Y. F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.

    2011-05-01

    This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70-80 %, up to 50-70 % of the calculated visibility reduction was

  20. Hygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: implications for regional direct radiative forcing under clean and polluted conditions

    NASA Astrophysics Data System (ADS)

    Stock, M.; Cheng, Y. F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.

    2010-11-01

    This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer - Aerodynamic Particle Sizer (H-DMA-APS). Like in several studies before, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The hygroscopic particle growth factors at 90% RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. All data recorded between 12 August and 20 October, 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp ≥ 150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in more continentally influenced air masses. Particle size distributions and hygroscopic growth factors were employed to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its daytime values around 70-80% in summer, up to 50-70% of the calculated visibility

  1. Aerosol Activity and Hygroscopicity Combined with Lidar Data in the Urban Atmosphere of Athens, Greece in the Frame of the HYGRA_CD Campaign

    NASA Astrophysics Data System (ADS)

    Bougiatioti, Aikaterini; Papayannis, Alexandros; Vratolis, Stergios; Argyrouli, Athina; Mihalopoulos, Nikolaos; Tsagkaraki, Maria; Nenes, Athanasios; Eleftheriadis, Konstantinos

    2016-06-01

    Measurements of cloud condensation nuclei (CCN) concentrations between 0.2-1.0% supersaturation and aerosol size distribution were performed at an urban background site of Athens during HygrA-CD. The site is affected by local and long-range transported emissions as portrayed by the external mixing of the particles, as the larger ones appear to be more hygroscopic and more CCN-active than smaller ones. Activation fractions at all supersaturations exhibit a diurnal variability with minimum values around noon, which are considerably lower than unity. This reinforces the conclusion that the aerosol is mostly externally mixed between "fresher", less hygroscopic components with more aged, CCN active constituents.

  2. Measurements of the evaporation and hygroscopic response of single fine-mode aerosol particles using a Bessel beam optical trap.

    PubMed

    Cotterell, Michael I; Mason, Bernard J; Carruthers, Antonia E; Walker, Jim S; Orr-Ewing, Andrew J; Reid, Jonathan P

    2014-02-01

    A single horizontally-propagating zeroth order Bessel laser beam with a counter-propagating gas flow was used to confine single fine-mode aerosol particles over extended periods of time, during which process measurements were performed. Particle sizes were measured by the analysis of the angular variation of light scattered at 532 nm by a particle in the Bessel beam, using either a probe beam at 405 nm or 633 nm. The vapour pressures of glycerol and 1,2,6-hexanetriol particles were determined to be 7.5 ± 2.6 mPa and 0.20 ± 0.02 mPa respectively. The lower volatility of hexanetriol allowed better definition of the trapping environment relative humidity profile over the measurement time period, thus higher precision measurements were obtained compared to those for glycerol. The size evolution of a hexanetriol particle, as well as its refractive index at wavelengths 532 nm and 405 nm, were determined by modelling its position along the Bessel beam propagation length while collecting phase functions with the 405 nm probe beam. Measurements of the hygroscopic growth of sodium chloride and ammonium sulfate have been performed on particles as small as 350 nm in radius, with growth curves well described by widely used equilibrium state models. These are the smallest particles for which single-particle hygroscopicity has been measured and represent the first measurements of hygroscopicity on fine mode and near-accumulation mode aerosols, the size regimes bearing the most atmospheric relevance in terms of loading, light extinction and scattering. Finally, the technique is contrasted with other single particle and ensemble methods, and limitations are assessed. PMID:24346588

  3. Characterization of solvent-extractable organics in urban aerosols based on mass spectrum analysis and hygroscopic growth measurement.

    PubMed

    Mihara, Toshiyuki; Mochida, Michihiro

    2011-11-01

    To characterize atmospheric particulate organics with respect to polarity, aerosol samples collected on filters in the urban area of Nagoya, Japan, in 2009 were extracted using water, methanol, and ethyl acetate. The extracts were atomized and analyzed using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a hygroscopicity tandem differential mobility analyzer. The atmospheric concentrations of the extracted organics were determined using phthalic acid as a reference material. Comparison of the organic carbon concentrations measured using a carbon analyzer and the HR-ToF-AMS suggests that organics extracted with water (WSOM) and ethyl acetate (EASOM) or those extracted with methanol (MSOM) comprise the greater part of total organics. The oxygen-carbon ratios (O/C) of the extracted organics varied: 0.51-0.75 (WSOM), 0.37-0.48 (MSOM), and 0.27-0.33 (EASOM). In the ion-group analysis, WSOM, MSOM, and EASOM were clearly characterized by the different fractions of the CH and CO(2) groups. On the basis of the hygroscopic growth measurements of the extracts, κ of organics at 90% relative humidity (κ(org)) were estimated. Positive correlation of κ(org) with O/C (r 0.70) was found for MSOM and EASOM, but no clear correlation was found for WSOM. PMID:21877700

  4. Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

    NASA Astrophysics Data System (ADS)

    Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

    2014-12-01

    The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

  5. In-Situ Measurements of Aerosol Optical and Hygroscopic Properties at the Look Rock Site during SOAS 2013

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Zimmermann, K.; Bertram, T. H.; Corrigan, A. L.; Guzman, J. M.; Russell, L. M.; Budisulistiorini, S.; Li, X.; Surratt, J. D.; Hicks, W.; Bairai, S. T.; Cappa, C. D.

    2013-12-01

    One of the main goals of the Southern Oxidant and Aerosol Study (SOAS) is to characterize the climate-relevant properties of aerosols over the southeastern United States at the interface of biogenic and anthropogenic emissions. As part of the SOAS campaign, the UCD cavity ringdown/photoacoustic spectrometer was deployed to make in-situ measurements of aerosol light extinction, absorption and sub-saturated hygroscopicity at the Look Rock site (LRK) in the Great Smoky Mountains National Park, TN from June 1 to July 15, 2013. The site is influenced by substantial biogenic emissions with varying impacts from anthropogenic pollutants, allowing for direct examination of the optical and hygroscopic properties of anthropogenic-influenced biogenic secondary organic aerosols (SOA). During the experiment period, the average dry aerosol extinction (Bext), absorption (Babs) coefficients and single scattering albedo (SSA) at 532 nm were 30.3 × 16.5 Mm-1, 1.12 × 0.78 Mm-1 and 0.96 × 0.06. The Babs at 532 nm was well correlated (r2 = 0.79) with the refractory black carbon (rBC) number concentration determined by a single particle soot spectrometer (SP2). The absorption by black carbon (BC), brown carbon (BrC) and the absorption enhancement due to the 'lensing' effect were quantified by comparing the Babs of ambient and thermo-denuded aerosols at 405 nm and 532 nm. The optical sub-saturated hygroscopic growth factor was derived from extinction and particle size distribution measurements at dry and elevated relative humidity. In addition, to explore the extent to which ammonia mediated chemistry leads to BrC formation, as suggested in recent laboratory studies(1,2), we performed an NH3 perturbation experiment in-situ for 1 week during the study, in which ambient aerosols were exposed to approximately 100 ppb NH3 with a residence time of ~ 3hr. The broader implications of these observational data at LRK will be discussed in the context of the concurrent gas and aerosol chemical

  6. Long term measurements of optical properties and their hygroscopic enhancement

    NASA Astrophysics Data System (ADS)

    Hervo, M.; Sellegri, K.; Pichon, J. M.; Roger, J. C.; Laj, P.

    2014-11-01

    Optical properties of aerosols were measured from the GAW Puy de Dôme station (1465 m) over a seven year period (2006-2012). The impact of hygroscopicity on aerosol optical properties was calculated over a two year period (2010-2011). The analysis of the spatial and temporal variability of the optical properties showed that while no long term trend was found, a clear seasonal and diurnal variation was observed on the extensive parameters (scattering, absorption). Scattering and absorption coefficients were highest during the warm season and daytime, in concordance with the seasonality and diurnal variation of the PBL height reaching the site. Intensive parameters (single scattering albedo, asymmetry factor, refractive index) did not show such a strong diurnal variability, but still indicated different values depending on the season. Both extensive and intensive optical parameters were sensitive to the air mass origin. A strong impact of hygroscopicity on aerosol optical properties was calculated, mainly on aerosol scattering, with a dependence on the aerosol type. At 90% humidity, the scattering factor enhancement (fσsca) was more than 4.4 for oceanic aerosol that have mixed with a pollution plume. Consequently, the aerosol radiative forcing was estimated to be 2.8 times higher at RH = 90% and 1.75 times higher at ambient RH when hygroscopic growth of the aerosol was considered. The hygroscopicity enhancement factor of the scattering coefficient was parameterized as a function of humidity and air mass type.

  7. Investigating hygroscopic behavior and phase separation of organic/inorganic mixed phase aerosol particles with FTIR spectroscopy

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Cziczo, D. J.

    2013-12-01

    Atmospheric aerosol particles can be composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have very well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. For example, the deliquescence relative humidity of pure ammonium sulfate is about 80% and its efflorescence point is about 35%. This behavior of ammonium sulfate is important to atmospheric chemistry because some reactions, such as the hydrolysis of nitrogen pentoxide, occur on aqueous but not crystalline surfaces. Deliquescence and efflorescence of simple inorganic salt particles have been investigated by a variety of methods, such as IR spectroscopy, tandem mobility analysis and electrodynamic balance. Field measurements have shown that atmospheric aerosol are not typically a single inorganic salt, instead they often contain organic as well as inorganic species. Mixed inorganic/organic aerosol particles, while abundant in the atmosphere, have not been studied as extensively. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. This project investigates the deliquescence and efflorescence points, phase separation and ability to exchange gas-phase components of mixed organic and inorganic aerosol using a flow tube coupled with FTIR spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O:C ratios, including glycerol, 1,2,6-hexanetriol, 1,4-butanediol and 1,5-pentanediol have been investigated. This project aims to study gas-phase exchange in these aerosol systems to determine if exchange is impacted when phase separation occurs.

  8. In-cloud processes of methacrolein under simulated conditions - Part 3: Hygroscopic and volatility properties of the formed secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Michaud, V.; El Haddad, I.; Liu, Yao; Sellegri, K.; Laj, P.; Villani, P.; Picard, D.; Marchand, N.; Monod, A.

    2009-07-01

    The hygroscopic and volatility properties of secondary organic aerosol (SOA) produced from the nebulization of solutions after aqueous phase photooxidation of methacrolein was experimentally studied in a laboratory, using a Volatility-Hygroscopicity Tandem DMA (VHTDMA). The obtained SOA were 80% 100°C-volatile after 5 h of reaction and only 20% 100°C-volatile after 22 h of reaction. The Hygroscopic Growth Factor (HGF) of the SOA produced from the nebulization of solutions after aqueous-phase photooxidation of methacrolein is 1.34-1.43, which is significantly higher than the HGF of SOA formed by gas-phase photooxidation of terpenes, usually found almost hydrophobic. These hygroscopic properties were confirmed for SOA formed by the nebulization of the same solutions where NaCl was added. The hygroscopic properties of the cloud droplet residuals decrease with the reaction time, in parallel with the formation of more refractory compounds. This decrease was mainly attributed to the 250°C-refractive fraction (presumably representative of the highest molecular weight compounds), which evolved from moderately hygroscopic (HGF of 1.52) to less hygroscopic (HGF of 1.36). Oligomerization is suggested as a process responsible for the decrease of both volatility and hygroscopicity with time. The NaCl seeded experiments enabled us to show that 19±4 mg L-1 of SOA was produced after 9.5 h of reaction and 41±9 mg L-1 after 22 h of in-cloud reaction. Because more and more SOA is formed as the reaction time increases, our results show that the reaction products formed during the aqueous-phase OH-oxidation of methacrolein may play a major role in the properties of residual particles upon the droplet's evaporation. Therefore, the specific physical properties of SOA produced during cloud processes should be taken into account for a global estimation of SOA and their atmospheric impacts.

  9. Hygroscopic growth of water-soluble matter extracted from remote marine aerosols over the western North Pacific: Influence of pollutants transported from East Asia.

    PubMed

    Boreddy, S K R; Kawamura, K

    2016-07-01

    We examined the hygroscopic properties of water-soluble matter (WSM) nebulized from water extracts of total suspended particles (TSP) collected at Chichijima Island in the western North Pacific during January to September 2003. The hygroscopic growth factor g(RH) of the aerosol particles was measured using a hygroscopic tandem differential mobility analyzer (HTDMA) with an initial dry particle diameter of 100nm and relative humidity (RH) of 5-95%. The measured growth factor at 90% RH, g(90%), ranged from 1.51 to 2.14 (mean: 1.76±0.15), significantly lower than that of sea salts (2.1), probably owing to the heterogeneous reactions associated with chloride depletion in sea-salt particles and water-soluble organic matter (WSOM). The g(90%) maximized in summer and minimized in spring. The decrease in spring was most likely explained by the formation of less hygroscopic salts or particles via organometallic reactions during the long-range transport of Asian dust. Cl(-) and Na(+) dominate the mass fractions of WSM, followed by nss-SO4(2-) and WSOM. Based on regression analysis, we confirmed that g(90%) at Chichijima Island largely increased due to the dominant sea spray; however, atmospheric processes associated with chloride depletion in sea salts and WSOM often suppressed g(90%). Furthermore, we explored the deviation (average: 18%) between the measured and predicted g(90%) by comparing measured and model growth factors. The present study demonstrates that long-range atmospheric transport of anthropogenic pollutants (SO2, NOx, organics, etc.) and the interactions with sea-salt particles often suppress the hygroscopic growth of marine aerosols over the western North Pacific, affecting the remote background conditions. The present study also suggests that the HCl liberation leads to the formation of less hygroscopic aerosols over the western North Pacific during long-range transport. PMID:27016676

  10. Hygroscopic properties and extinction of aerosol particles at ambient relative humidity in South-Eastern China

    NASA Astrophysics Data System (ADS)

    Eichler, H.; Cheng, Y. F.; Birmili, W.; Nowak, A.; Wiedensohler, A.; Brüggemann, E.; Gnauk, T.; Herrmann, H.; Althausen, D.; Ansmann, A.; Engelmann, R.; Tesche, M.; Wendisch, M.; Zhang, Y. H.; Hu, M.; Liu, S.; Zeng, L. M.

    During the "Program of Regional Integrated Experiments of Air Quality over Pearl River Delta 2004 (PRIDE-PRD2004)" hygroscopic properties of particles in the diameter range 22 nm to 10μm were determined. For that purpose, a Humidifying Differential Mobility Particle Sizer (H-DMPS) and a Micro-Orifice Uniform Deposition Impactor (MOUDI) were operated. The derived size-dependent particle hygroscopic growth factors were interpolated to ambient relative humidity (RH) and used to calculate the particle number size distributions (PNSDs) at ambient conditions. A comparison between the modeled particle extinction coefficients (σ) and those observed with a Raman lidar was made. It is shown that the particle extinction coefficient ( σext) at ambient RH can be properly estimated with Mie-model calculations based on the in situ physico-chemical measurements of dry and humidified PNSD and chemical composition.

  11. L-Leucine as an excipient against moisture on in vitro aerosolization performances of highly hygroscopic spray-dried powders.

    PubMed

    Li, Liang; Sun, Siping; Parumasivam, Thaigarajan; Denman, John A; Gengenbach, Thomas; Tang, Patricia; Mao, Shirui; Chan, Hak-Kim

    2016-05-01

    L-Leucine (LL) has been widely used to enhance the dispersion performance of powders for inhalation. LL can also protect powders against moisture, but this effect is much less studied. The aim of this study was to investigate whether LL could prevent moisture-induced deterioration in in vitro aerosolization performances of highly hygroscopic spray-dried powders. Disodium cromoglycate (DSCG) was chosen as a model drug and different amounts of LL (2-40% w/w) were added to the formulation, with the aim to explore the relationship between powder dispersion, moisture protection and physicochemical properties of the powders. The powder formulations were prepared by spray drying of aqueous solutions containing known concentrations of DSCG and LL. The particle sizes were measured by laser diffraction. The physicochemical properties of fine particles were characterized by X-ray powder diffraction (XRD), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), and dynamic vapor sorption (DVS). The surface morphology and chemistry of fine particles were analyzed by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS). In vitro aerosolization performances were evaluated by a next generation impactor (NGI) after the powders were stored at 60% or 75% relative humidity (RH), and 25°C for 24h. Spray-dried (SD) DSCG powders were amorphous and absorbed 30-45% (w/w) water at 70-80% RH, resulting in deterioration in the aerosolization performance of the powders. LL did not decrease the water uptake of DSCG powders, but it could significantly reduce the effect of moisture on aerosolization performances. This is due to enrichment of crystalline LL on the surface of the composite particles. The effect was directly related to the percentage of LL coverage on the surface of particles. Formulations having 61-73% (molar percent) of LL on the particle surface (which correspond to 10-20% (w

  12. Parameter sensitivity study of Arctic aerosol vertical distribution in CAM5

    NASA Astrophysics Data System (ADS)

    Jiao, C.; Flanner, M.

    2015-12-01

    Arctic surface temperature response to light-absorbing aerosols (black carbon, brown carbon and dust) depends strongly on their vertical distributions. Improving model simulations of three dimensional aerosol fields in the remote Arctic region will therefore lead to improved projections of the climate change caused by aerosol emissions. In this study, we investigate how different physical parameterizations in the Community Atmosphere Model version 5 (CAM5) influence the simulated vertical distribution of Arctic aerosols. We design experiments to test the sensitivity of the simulated aerosol fields to perturbations of selected aerosol process-related parameters in the Modal Aerosol Module with seven lognormal modes (MAM7), such as those govern aerosol aging, in-cloud and below-cloud scavenging, aerosol hygroscopicity and so on. The simulations are compared with observed aerosol vertical distributions and total optical depth to assess model performance and quantify uncertainties associated with these model parameterizations. Observations applied here include Arctic aircraft measurements of black carbon and sulfate vertical profiles, along with Aerosol Robotic Network (AERONET) optical depth measurements. We also assess the utility of using High Spectral Resolution Lidar (HSRL) measurements from the ARM Barrow site to infer vertical profiles of aerosol extinction. The sensitivity study explored here will provide guidance for optimizing global aerosol simulations.

  13. Influence of biomass burning on CCN number and hygroscopicity during summertime in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Bougiatioti, A.; Bezantakos, S.; Stavroulas, I.; Kalivitis, N.; Kokkalis, P.; Biskos, G.; Mihalopoulos, N.; Papayannis, A.; Nenes, A.

    2015-08-01

    This study investigates the CCN activity and hygroscopic properties of particles influenced by biomass burning in the eastern Mediterranean. 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 cloud condensation nuclei (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 hygroscopicity parameter, κ, for all particle sizes. The reason, however, for this decrease was not the same for all size modes; smaller particle sizes appeared to be richer in less hygroscopic, less CCN-active components due to coagulation processes while larger particles become less hygroscopic during the biomass burning events due to condensation of less hygroscopic gaseous compounds. In addition, smaller particles 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 aging and retained high levels of CCN activity. These conclusions are further supported by the observed mixing state determined by the HTDMA measurements. ACSM measurements indicate that the bulk composition reflects the hygroscopicity and chemical nature of the largest particles and a large fraction of the CCN concentrations sampled. Based on Positive Matrix Factorization (PMF) analysis of the organic ACSM spectra, CCN concentrations follow a similar trend with the BBOA component, with enhancements of CCN in biomass burning plumes ranging between 65 and 150 %, for supersaturations ranging between 0.2 and 0.7 %. Using multilinear regression, we determine the

  14. Absorbing aerosols at high relative humidity: closure between hygroscopic growth and optical properties

    NASA Astrophysics Data System (ADS)

    Flores, J. M.; Bar-Or, R. Z.; Bluvshtein, N.; Abo-Riziq, A.; Kostinski, A.; Borrmann, S.; Koren, I.; Rudich, Y.

    2012-01-01

    The extinction coefficient and growth factor of humidified aerosols, at 80% and 90% RH, and at 532 nm and 355 nm wavelengths were measured for size-selected particles for ammonium sulfate, IHSS Pahokee peat (a lightly absorbing humic-like substance proxy), nigrosine (a black dye to model highly absorbing substances), and a mixture of AS and nigrosine. The ratio of the humidified extinction coefficients to the dry (fRHext(%RH, Dry)) was explored. The measured fRHext(%RH, Dry) was compared to theoretical calculations based on Mie theory, using the measured growth factors and assuming homogeneous mixing. The expected complex refractive indices (RIs) using the volume weighted mixing rule were compared to the RIs derived from the extinction measurements. Moreover, the differences between assuming a core-shell structure or a homogeneous mixing of the substances is examined. The laboratory results were used as a basis to model the change in the total extinction, the single scattering albedo (ω), and the asymmetry parameter (g) in the twilight zone of clouds at 355 nm and 532 nm. We found slightly linear to no dependency of fRH(%RH, Dry) with size for absorbing substances in contrast to the decreasing exponential behavior with size for purely scattering substances. However, no discernable difference could be made between the two wavelengths used. Less than 5% differences were found between the real parts of the complex refractive indices derived and those calculated using the volume weighted mixing rule, and the imaginary parts had up to a 20% difference. Moreover, for substances with growth factor less than 1.15 there was, in average, less than 5% difference between the extinction efficiencies calculated using a core-shell model and assuming homogeneous mixing for size parameters less than 2.5. For x>2.5 the differences were greater causing and overestimation of the extinction efficiency (Qext) values if homogenous mixing was assume instead of a core-shell structure. The

  15. Interaction of aerosol particles composed of protein and salts with water vapor: hygroscopic growth and microstructural rearrangement

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Niessner, R.; Pöschl, U.

    2003-09-01

    The interaction of aerosol particles in the 100-200 nm size range composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor at ambient temperature and pressure (25°C, 1 atm) has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations. BSA was chosen as a well-defined model substance for proteins and other macromolecular compounds, which constitute a large fraction of the water-soluble organic component of air particulate matter. Pure BSA particles exhibited deliquescence and efflorescence transitions at ~35% relative humidity (RH) and a hygroscopic diameter increase by up to ~10% at 95% RH in good agreement with model calculations based on a simple parameterisation of the osmotic coefficient. Pure NaCl particles were converted from near-cubic to near-spherical or polyhedral shape upon interaction with water vapor at relative humidities below the deliquescence threshold (partial surface dissolution and recrystallisation), and the diameters of pure NH4NO3 particles decreased by up to 10% due to chemical decomposition and evaporation. Mixed NaCl-BSA and NH4NO3-BSA particles interacting with water vapor exhibited mobility equivalent diameter reductions of up to 20%, depending on particle generation, conditioning, size, and chemical composition (BSA dry mass fraction 10-90%). These observations can be explained by formation of porous agglomerates (envelope void fractions up to 50%) due to ion-protein interactions and electric charge effects on the one hand, and by compaction of the agglomerate structure due to capillary condensation effects on the other. The size of NH4NO3-BSA particles was apparently also influenced by volatilisation of NH4NO3, but not as much as for pure salt particles, i.e. the protein inhibited the decomposition of NH4NO3 or the evaporation of the

  16. Reduction in biomass burning aerosol light absorption upon humidification: Roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

    SciTech Connect

    lewis, Kristen A.; Arnott, W. P.; Moosmuller, H.; Chakrabarti, Raj; Carrico, Christian M.; Kreidenweis, Sonia M.; Day, Derek E.; Malm, William C.; Laskin, Alexander; Jimenez, Jose L.; Ulbrich, Ingrid M.; Huffman, John A.; Onasch, Timothy B.; Trimborn, Achim; Liu, Li; Mishchenko, M.

    2009-11-27

    Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

  17. Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

    SciTech Connect

    Ziemann, Paul J.; Kreidenweis, Sonia M.; Petters, Markus D.

    2013-06-30

    The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

  18. Aerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Brock, C. A.; Wagner, N. L.; Anderson, B. E.; Beyersdorf, A.; Campuzano-Jost, P.; Day, D. A.; Diskin, G. S.; Gordon, T. D.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Markovic, M.; Middlebrook, A. M.; Perring, A. E.; Richardson, M. S.; Schwarz, J. P.; Welti, A.; Ziemba, L. D.; Murphy, D. M.

    2015-11-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013. Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0-4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation of these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry-climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ~ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental airmasses in which an accumulation mode between 0.1-0.5 μm diameter dominates aerosol extinction.

  19. Aerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Welti, Andre; Ziemba, Luke D.; Murphy, Daniel M.

    2016-04-01

    Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0-4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry-climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ˜ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1-0.5 µm diameter dominates aerosol extinction.

  20. Competing effects of viscosity and surface-tension depression on the hygroscopicity and CCN activity of laboratory surrogates for oligomers in atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Hodas, N.; Zuend, A.; Shiraiwa, M.; Flagan, R. C.; Seinfeld, J.; Schilling, K.; Berkemeier, T.

    2015-12-01

    The presence of oligomers in biomass burning aerosol, as well as secondary organic aerosol derived from other sources, influences particle viscosity and can introduce kinetic limitations to water uptake. This, in turn, impacts aerosol optical properties and the efficiency with which these particles serve as cloud condensation nuclei (CCN). To explore the influence of organic-component viscosity on aerosol hygroscopicity, the water-uptake behavior of aerosol systems comprised of polyethylene glycol (PEG) and mixtures of PEG and ammonium sulfate (AS) was measured under sub- and supersaturated relative humidity (RH) conditions. Experiments were conducted with systems containing PEG with average molecular weights ranging from 200 to 10,000 g/mol, corresponding to a range in viscosity of 0.004 - 4.5 Pa s under dry conditions. While evidence suggests that viscous aerosol components can suppress water uptake at RH < 90%, under supersaturated conditions (with respect to RH), an increase in CCN activity with increasing PEG molecular weight was observed. We attribute this to an increase in the efficiency with which PEG serves as a surfactant with increasing molecular weight. This effect is most pronounced for PEG-AS mixtures and, in fact, a modest increase in CCN activity is observed for the PEG 10,000-AS mixture as compared to pure AS, as evidenced by a 4% reduction in critical activation diameter. Experimental results are compared with calculations of hygroscopic growth at thermodynamic equilibrium using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients model and the potential influence of kinetic limitations to observed water uptake is further explored with the Kinetic Multi-Layer Model of Gas-Particle Interactions. Results suggest the competing effects of organic-component viscosity and surface-tension depression may lead to RH-dependent differences in hygroscopicity for oligomers and other surface-active compounds present in atmospheric

  1. Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China - Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

    Rose, D.; Nowak, A.; Achtert, P.; Wiedensohler, A.; Hu, M.; Shao, M.; Zhang, Y.; Andreae, M. O.; Pöschl, U.

    2010-04-01

    Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1-30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20-290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≍0.1-0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity - most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm-3 at S=0.068% to 16 000 cm-3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from

  2. Vapour pressures and hygroscopicity of semi-volatile organic components in ternary organic/inorganic/water aerosol droplet trapped by aerosol optical tweezers

    NASA Astrophysics Data System (ADS)

    Cai, Chen; Zhang, Yunhong

    2016-04-01

    Knowledge of the vapour pressures of semi-volatile organic compounds is of critical importance in determining their partitioning behaviour into atmospheric aerosol. Quantifying the gas/particle partitioning of organic compounds is of great importance since at present published results of the vapour pressures of compounds of interest (typically with vapour pressures lower than 0.01 Pa) can be different by several orders of magnitude and influences on SVOCs evaporation from participation of inorganic compounds remains unclear. In this study we present a new method for the retrieval of SVOCs vapour pressures from single aerosol droplets in an aerosol optical tweezers system. Measurements of the concentration of SVOC (derived from experimentally determined RI) and radius of SVOC aqueous droplets are correlated in an expression derived from the Maxwell gas phase diffusion equation for the determination of vapour pressure. ( ) dmi-= 4π dr3Conc + dConcir3 = 4πrMiDi,gas-(p ‑ p) dt 3 dt i dt RT i,∞ i,r Relationship between r dr/dt (nm2s‑1) and r2dConcentration/dt (nm2gL‑1s‑1) is presented, in which the slope is derived for determination of hygroscopic line whilst the axis intercept can be determined to estimate vapour pressure. Briefly the method relies on the levitation of a droplet (3-7 μm radius) in an aerosol optical tweezers system. In this system the droplet acts as a microcavity and the size and refractive index of the particle can be extracted by using Mie theory to fit the positions of the "whispering gallery modes" in the cavity enhanced Raman spectroscopy fingerprint. The vapour pressure can then be extracted from the correlation between the rate of change of particle radius with the rate of change of composition (refractive index, n). We will show that information about the hygroscopicity of the particle and how this changes as the particle evaporates can also be determined from the changing slopes of these plots.

  3. The Global Ozone and Aerosol Profiles and Aerosol Hygroscopic Effect and Absorption Optical Depth (GOA2HEAD) Network Initiative

    NASA Astrophysics Data System (ADS)

    Gao, R. S.; Elkins, J. W.; Frost, G. J.; McComiskey, A. C.; Murphy, D. M.; Ogren, J. A.; Petropavlovskikh, I. V.; Rosenlof, K. H.

    2014-12-01

    Inverse modeling using measurements of ozone (O3) and aerosol is a powerful tool for deriving pollutant emissions. Because they have relatively long lifetimes, O3 and aerosol are transported over large distances. Frequent and globally spaced vertical profiles rather than ground-based measurements alone are therefore highly desired. Three requirements necessary for a successful global monitoring program are: Low equipment cost, low operation cost, and reliable measurements of known uncertainty. Conventional profiling using aircraft provides excellent data, but is cost prohibitive on a large scale. Here we describe a new platform and instruments meeting all three global monitoring requirements. The platform consists of a small balloon and an auto-homing glider. The glider is released from the balloon at about 5 km altitude, returning the light instrument package to the launch location, and allowing for consistent recovery of the payload. Atmospheric profiling can be performed either during ascent or descent (or both) depending on measurement requirements. We will present the specifications for two instrument packages currently under development. The first measures O3, RH, p, T, dry aerosol particle number and size distribution, and aerosol optical depth. The second measures dry aerosol particle number and size distribution, and aerosol absorption coefficient. Other potential instrument packages and the desired spatial/temporal resolution for the GOA2HEAD monitoring initiative will also be discussed.

  4. DOSIMETRY MODEL FOR HYGROSCOPIC SULFATE AEROSOLS IN SELECTED TEMPERATURE AND RELATIVE HUMIDITY PATTERNS

    EPA Science Inventory

    Sulfate aerosols (NH4HSO4,(NH4)2SO4 and H2SO4) are of international health effects concern because of their global prevalence and potential irritant or toxic effects on human health. To assess hazards following inhalation exposure, the total dose delivered to the human respirator...

  5. Aerosol water parameterisation: a single parameter framework

    NASA Astrophysics Data System (ADS)

    Metzger, Swen; Steil, Benedikt; Abdelkader, Mohamed; Klingmüller, Klaus; Xu, Li; Penner, Joyce E.; Fountoukis, Christos; Nenes, Athanasios; Lelieveld, Jos

    2016-06-01

    We introduce a framework to efficiently parameterise the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute-specific coefficient was introduced in Metzger et al. (2012) to accurately parameterise the single solution hygroscopic growth, considering the Kelvin effect - accounting for the water uptake of concentrated nanometer-sized particles up to dilute solutions, i.e. from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler theory). Here we extend the νi parameterisation from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II and ISORROPIA II models as well as textbook examples. We apply our parameterisation in the EQuilibrium Simplified Aerosol Model V4 (EQSAM4clim) for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show (i) that the νi approach enables one to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that ammonium sulfate mixtures can be solved with a simple method, e.g. pure ammonium nitrate and mixed ammonium nitrate and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

  6. Aerosol water parameterization: a single parameter framework

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Steil, B.; Abdelkader, M.; Klingmüller, K.; Xu, L.; Penner, J. E.; Fountoukis, C.; Nenes, A.; Lelieveld, J.

    2015-11-01

    We introduce a framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute specific coefficient was introduced in Metzger et al. (2012) to accurately parameterize the single solution hygroscopic growth, considering the Kelvin effect - accounting for the water uptake of concentrated nanometer sized particles up to dilute solutions, i.e., from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler-theory). Here we extend the νi-parameterization from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II, ISORROPIA II models as well as textbook examples. We apply our parameterization in EQSAM4clim, the EQuilibrium Simplified Aerosol Model V4 for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show: (i) that the νi-approach enables to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that, e.g., pure ammonium nitrate and mixed ammonium nitrate - ammonium sulfate mixtures can be solved with a simple method, and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

  7. Discontinuous hygroscopic growth of an aqueous surfactant/salt aerosol particle levitated in an electrodynamic balance

    NASA Astrophysics Data System (ADS)

    Soonsin, V.; Krieger, U. K.; Peter, T.

    2010-12-01

    Organic compounds are a major fraction of tropospheric aerosol. The organic fraction is usually internally mixed with inorganic salts. Surface-active organic matter or surfactants, enriched in the oceanic surface layer and transferred to the atmosphere by bubble-bursting processes, are the most likely candidates to contribute the observed organic fraction in sea salt aerosol [1, 2]. If the organic substance is a surfactant, it will lower the surface tension. In addition aggregates of the organic monomers, called micelles, will form if the concentration of the organic exceeds a certain limit (critical micelle concentration). These aggregates do have different morphology (spheres or globular or rod like micelles, or spherical bilayer vesicles etc.) and size, depending on the nature of the organic molecule, its concentration and the concentration of inorganic salts [3]. These aggregate may promote solubilisation of organic compounds in aqueous atmospheric aerosol. We performed measurements of ternary aqueous solution particles consisting of tetraethylene glycol monooctyl ether (C8E4) as organic surfactant and sodium chloride (NaCl) as inorganic salt and water (H2O) using single levitated aerosol particles in an electrodynamic balance. The particles can be stored contact-free in a temperature and humidity controlled chamber and optical resonance spectroscopy is used to monitor radius change [4]. Mie resonance spectra of ternary droplets show discontinuous growth with increasing relative humidity (RH) and also discontinuous shrinkage with decreasing relative humidity. We observe this behavior at temperatures and RHs at which the salt is completely deliquesced and the concentration of the organic surfactant is larger than the critical micelle concentration. Independent measurements of particle mass show also discontinuous water uptake. We speculate that this discontinuous, step-like, growth is caused by disaggregation of a micelle needed to conserve the monolayer of

  8. Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach

    NASA Astrophysics Data System (ADS)

    Hartmann, Markus; Heim, Lars-Oliver; Ebert, Martin; Weinbruch, Stephan; Kandler, Konrad

    2015-04-01

    Hygroscopic properties of large aerosol particles using the example of aged Saharan mineral dust - a semi-automated electron microscopy approach Markus Hartmann(1), Lars-Oliver Heim(2), Martin Ebert(1), Stephan Weinbruch(1), Konrad Kandler(1) The Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) took place at Barbados from June 10 to July 15 2013. During this period, dust was frequently transported from Africa across the Atlantic Ocean toward the Caribbean. In this study, we investigate the atmospheric aging of the dust aerosol based on its hygroscopicity. Aerosol samples were collected ground-based at Ragged Point (13°9'54.4"N, 59°25'55.7"W) with a single round jet cascade impactor on nickel-substrates. The particles from the stage with a 50% efficiency cutoff size of 1 µm were analyzed with an Environmental Scanning Electron Microscope (ESEM) equipped with an energy-dispersive X-ray detector (EDX) and a cooling stage. In an initial automated run, information on particle size and chemical composition for elements heavier than carbon were gathered. Afterwards, electron microscope images of the same sample areas as before were taken during a stepwise increase of relative humidities (between 50 % and 92%), so that the hygroscopic growth of the droplets could be directly observed. The observed hygroscopic growth can be correlated to the chemical composition of the respective particles. For the automated analysis of several hundred images of droplets an image processing algorithm in Python was developed. The algorithm is based on histogram equalization and watershed segmentation. Since SEM images can only deliver two-dimensional information, but the hygroscopic growth factor usually refers to the volume of a drop, Atomic Force Microscopy (AFM) was used to derive an empirical function for the drop volume depending on the apparent drop diameter in the electron images. Aside from the mineral dust, composed of mostly silicates and

  9. Aerosol hygroscopicity and its impact on atmospheric visibility and radiative forcing in Guangzhou during the 2006 PRIDE-PRD campaign

    NASA Astrophysics Data System (ADS)

    Liu, Xingang; Zhang, Yuanhang; Cheng, Yafang; Hu, Min; Han, Tingting

    2012-12-01

    The objective of this study is to quantify the relation of aerosol chemical compositions and optical properties, and to assess the impact of relative humidity (RH) on atmospheric visibility and aerosol direct radiative forcing (ADRF). Mass concentration and size distribution of aerosol chemical compositions as well as aerosol optical properties were concurrently measured at Guangzhou urban site during the PRD (Pearl River Delta) campaign from 1 to 31 July, 2006. Gaseous pollutant NO2 and meteorological parameter were simultaneously monitored. Compared with its dry condition, atmospheric ambient extinction coefficient σext(RH) averagely increased about 51% and atmospheric visibility deceased about 35%, among which RH played an important role on the optical properties of water soluble inorganic salts. (NH4)2SO4 is the most important component responsible for visibility degradation at Guangzhou. In addition, the asymmetry factor g increased from 0.64 to 0.74 with the up-scatter fraction β decreasing from 0.24 to 0.19 when RH increasing from 40% to 90%. At 80% RH, the ADRF increased about 280% compared to that at dry condition and it averagely increased about 100% during the campaign under ambient conditions. It can be inferred that aerosol water content is a key factor and could not be ignored in assessing the role of aerosols in visibility impairment and radiative forcing, especially in the regions with high RH.

  10. AEROSOL OPTICAL PROPERTIES AND BIOGENIC SOA: EFFECT ON HYGROSCOPIC PROPERTIES AND LIGHT ABSORPTION

    EPA Science Inventory

    This study will provide a comprehensive characterization of optical properties of biogenic SOA and their sensitivity to anthropogenic influence. Several parameters critical for climate modeling, such as absorption cross-section, single scattering albedo and sensitivity to R...

  11. Hygroscopic Properties of Oxidation Products of Terpenes

    NASA Astrophysics Data System (ADS)

    Lodhi, N. A.; Mozurkewich, M.

    2009-05-01

    To understand the hygroscopic growth factor (HGF) of secondary organic aerosol (SOA) formed by the oxidation of terpenes, a series of seeded and nucleation experiments were conducted at the York University smog chamber facility. Oxidation of terpenes by OH was carried out in a dry chamber (RH˜5%). In nucleation experiments particles formed were pure organic and their hygroscopic growth factor was measured as function of relative humidity by using a tandem differential mobility analyzer (HTDMA). Humidograms of these particles don't show any deliquescence or efflorescence. Humidograms of pure organic particles formed by the oxidation products of β-pinene show slight but smooth take up of water while particles formed by α-pinene and δ3-carene exhibit very little or no water uptake. Experimental results were fitted with an empirical equation and the hygroscopicity parameter for the particles formed by β-pinene was found to be 0.019±0.009. To examine the interaction of organic and inorganic phases, monodisperse ammonium sulfate seed particles injected into the smog chamber were allowed to undergo condensational growth due to partitioning of terpenes oxidation products from the gas phase. Humidograms of seeded particles show both smooth hygroscopic growth and deliquescence. These experimental results were fitted with a numerical model that accounts for water uptake by both phases and for the gradual dissolution of ammonium sulfate. The results show that volume additivity is a reasonable approximation for this system and that HTDMA results can be inverted to obtain the organic hygroscopicity parameter and the relative amounts of organic and inorganic material

  12. Optical measurement of medical aerosol media parameters

    NASA Astrophysics Data System (ADS)

    Sharkany, Josif P.; Zhytov, Nikolay B.; Sichka, Mikhail J.; Lemko, Ivan S.; Pintye, Josif L.; Chonka, Yaroslav V.

    2000-07-01

    The problem of aerosol media parameters measurements are presented in the work and these media are used for the treatment of the patients with bronchial asthma moreover we show the results of the development and the concentration and dispersity of the particles for the long-term monitoring under such conditions when the aggressive surroundings are available. The system for concentration measurements is developed, which consists of two identical photometers permitting to carry out the measurements of the transmission changes and the light dispersion depending on the concentration of the particles. The given system permits to take into account the error, connected with the deposition of the salt particles on the optical windows and the mirrors in the course of the long-term monitoring. For the controlling of the dispersity of the aggressive media aerosols the optical system is developed and used for the non-stop analysis of the Fure-spectra of the aerosols which deposit on the lavsan film. The registration of the information is performed with the help of the rule of the photoreceivers or CCD-chamber which are located in the Fure- plane. With the help of the developed optical system the measurements of the concentration and dispersity of the rock-salt aerosols were made in the medical mines of Solotvino (Ukraine) and in the artificial chambers of the aerosol therapy.

  13. Aerosol Hygroscopicity Measured in Pristine and Polluted Conditions During the First Year of the GoAmazon 2014/15 Experiment

    NASA Astrophysics Data System (ADS)

    Barbosa, H. M.; Krüger, M. L.; Thalman, R.; Wang, J.; Pauliquevis, T.; Brito, J.; Poeschl, U.; Andreae, M. O.; Martin, S. T.; Artaxo, P.

    2015-12-01

    The effects of aerosol particles on cloud microphysical properties, cloud cover, precipitation, and regional climate are an important aspect of the climate system. The Amazon region is particularly susceptible to changes in number-diameter distributions of the atmospheric particle population because of the low background concentrations and high water vapor levels, indicating a regime of cloud properties that is highly sensitive to aerosol microphysics. This natural regime, different from most other continental areas worldwide, is expected to be perturbed by the interaction of the Manaus urban plume with the natural the natural environment. Studying the effects of this interaction on the cloud and aerosol life cycle is the main objective of the Green Ocean Amazon (GoAmazon) campaign taking place around Manaus-Brazil from January 2014 to December 2015. In this paper we compare the particle hygroscopicity calculated from measurements of size-resolved cloud condensation nuclei performed at three ground sites during the first year of the GoAmazon 2014/15 experiment. Site T3 is about 70 km downwind from Manaus experiencing urban polluted and background conditions; site T2 is just across the Rio Negro from Manaus and CCN measurements were performed there only from 15 August 2014 to 30 Jan 2015; and T0, at the Amazon Tall Tower Observatory (ATTO), is a pristine site about 200 km upwind from Manaus. Our results indicate a lower hygroscopicity under polluted conditions (mean kappa values around 0.14 to 0.16) than under clean conditions (mean kappa around 0.2 to 0.3). At the clean site, it was possible to identify peaks of large sea salt particles with organic coating, while small particles seems to be purely organic. The activation fraction and hygroscopicity will be compared and discussed as a function of particle size. The mean kappa at ATTO is 0.17+-0.05 (mean of June and September) when there is no impact from long range transport from Africa or fresh soot emissions

  14. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-01-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  15. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-09-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  16. Characterization of marine boundary layer aerosol from North Atlantic and European sources: Physical and chemical properties and climate forcing parameters

    NASA Astrophysics Data System (ADS)

    Dusek, Ulrike

    This thesis focuses on aerosol properties measured in Southwestern Portugal during the second Aerosol Characterization Experiment. Fundamental aerosol physical properties such as particle size distribution and hygroscopic properties are related to possible sources and aerosol transformation processes. From these fundamental properties we derive aerosol properties that are important for aerosol forcing of climate. First, a new method for calculating CCN spectra is proposed in this work and tested using sensitivity studies and comparisons to direct measurements. The measured and calculated CCN spectra differ on average by 30%, which at small supersaturations is similar to the measurement uncertainties. Second, aerosol number to volume ratios (R) are calculated and the fact that values of R are relatively constrained is explained based on observed correlations between size distribution parameters. Third, a simple parameterization of the humidity dependence of the submicron aerosol scattering coefficient has been derived, depending only on a volume weighted average diameter growth factor and the volume mean diameter of the dry size distribution. One set of empirical parameters can be used to parameterize all aerosol types characterized during the ACE-2 measurement period. Aerosol physical properties and climate forcing parameters in the North-East Atlantic Ocean were clearly affected by pollution outbreaks from Europe. The submicron particle volume increased by a factor of 5 in polluted conditions, the light scattering coefficient of dry particles increased on average by a factor of up to 10, CCN concentrations at supersaturations of 0.2% increased by a factor of 3--5. The aerosol fundamental properties vary often strongly with air mass history, but also show short-term variability that often has a characteristic diurnal scale. The number concentration of fine particles below 50nm and the particle hygroscopic growth factors are mostly dominated by diurnal processes

  17. Aerosol Observing System (AOS) Handbook

    SciTech Connect

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  18. Climate Engineering with Stratospheric Aerosols and Associated Engineering Parameters

    SciTech Connect

    Kravitz, Benjamin S.

    2013-02-12

    Climate engineering with stratospheric aerosols, an idea inspired by large volcaniceruptions, could cool the Earth’s surface and thus alleviate some of the predicted dangerous impacts of anthropogenic climate change. However, the effectiveness of climate engineering to achieve a particular climate goal, and any associated side effects, depend on certain aerosol parameters and how the aerosols are deployed in the stratosphere. Through the examples of sulfate and black carbon aerosols, this paper examines "engineering" parameters-aerosol composition, aerosol size, and spatial and temporal variations in deployment-for stratospheric climate engineering. The effects of climate engineering are sensitive to these parameters, suggesting that a particle could be found ordesigned to achieve specific desired climate outcomes. This prospect opens the possibility for discussion of societal goals for climate engineering.

  19. How Does a Raindrop Grow?: Precipitation in natural clouds may develop from ice crystals or from large hygroscopic aerosols.

    PubMed

    Braham, R R

    1959-01-16

    On the basis of presently available data, combined with present-day knowledge of the physics and chemistry of cloud particle development, it is possible to make the following generalizations about the mode of precipitation in natural clouds. 1) The all-water mechanism begins to operate as soon as a parcel of cloud air is formed and continues to operate throughout the life of the cloud. The ice-crystal mechanism, on the other hand, can begin to operate only after the top of the cloud has reached levels where ice nuclei can be effective (about -15 degrees C). Some clouds never reach this height; any precipitation from them must be through the all-water mechanism. In cold climates and at high levels in the atmosphere, the cloud bases may be very close to this critical temperature. In the tropics, approximately 25,000 feet separate the bases of low clouds from the natural ice level. 2) The number of large hygroscopic nuclei in maritime air over tropical oceans is entirely adequate to rain-out any cloud with a base below about 10,000 feet, provided the cloud duration and cloud depth is sufficient for the precipitation process to operate. Extensive trajectories over land will decrease the number of sea-salt particles, both because of sedimentation and removal in rain. Measurements show an order-of-magnitude decrease in the number of large particles as maritime air moves from the Gulf of Mexico to the vicinity of St. Louis, during the summer months. Measurements in Arizona and New Mexico show even smaller chloride concentrations, presumably because of the long overland trajectories required in reaching these areas. The maritime particles lost in overland trajectories apparently are more than replaced by particles of land origin. The latter are usually of mixed composition and are less favorable for the formation of outsized solution droplets. 3) Ice nuclei, required for the formation of ice crystals and for droplet freezing, are rather rare at temperatures higher than

  20. Hygroscopic properties of NaCl and NaNO3 mixture particles as reacted inorganic sea-salt aerosol surrogates

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Kim, H.; Park, G.; Li, X.; Eom, H.-J.; Ro, C.-U.

    2015-03-01

    NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NOx/HNO3, so internally mixed NaCl and NaNO3 aerosol particles can co-exist over a wide range of mixing ratios. Laboratory-generated, micrometer-sized NaCl and NaNO3 mixture particles at 10 mixing ratios (mole fractions of NaCl (XNaCl) = 0.1 to 0.9) were examined systematically to observe their hygroscopic behavior, derive experimental phase diagrams for deliquescence and efflorescence, and understand the efflorescence mechanism. During the humidifying process, aerosol particles with the eutonic composition (XNaCl = 0.38) showed only one phase transition at their mutual deliquescence relative humidity (MDRH) of 67.9 (±0.5)% On the other hand, particles with other mixing ratios showed two distinct deliquescence transitions; i.e., the eutonic component dissolved at MDRH, and the remainder in the solid phase dissolved completely at their DRHs depending on the mixing ratios, resulting in a phase diagram composed of four different phases, as predicted thermodynamically. During the dehydration process, NaCl-rich particles (XNaCl > 0.38) showed a two stage efflorescence transition: the first stage was purely driven by the homogeneous nucleation of NaCl and the second stage at the mutual efflorescence RH (MERH) of the eutonic components, with values in the range of 30.0-35.5%. Interestingly, aerosol particles with the eutonic composition (XNaCl = 0.38) also showed two-stage efflorescence, with NaCl crystallizing first followed by heterogeneous nucleation of the remaining NaNO3 on the NaCl seeds. NaNO3-rich particles (XNaCl ≤ 0.3) underwent single-stage efflorescence transitions at ERHs progressively lower than the MERH because of the homogeneous nucleation of NaCl and the almost simultaneous heterogeneous nucleation of NaNO3 on the NaCl seeds. SEM/EDX elemental mapping indicated that the effloresced NaCl-NaNO3 particles at all mixing ratios were composed of a homogeneously

  1. Hygroscopic behavior of NaCl-MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidifying process

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Eom, H.-J.; Cho, H.-R.; Ro, C.-U.

    2015-07-01

    NaCl and MgCl2 are the two major constituents of seawater, so NaCl-MgCl2 mixture particles can be a better representative of sea-spray aerosols (SSAs) than pure NaCl. However, there have been very few hygroscopic studies of pure MgCl2 and NaCl-MgCl2 mixture aerosol particles despite the MgCl2 moiety playing a major role in the hygroscopic behavior of nascent SSAs. Laboratory-generated pure MgCl2 and NaCl-MgCl2 mixture aerosol particles with 12 mixing ratios (0.01 ≤ mole fraction of NaCl (XNaCl) ≤ 0.9) were examined systematically by optical microscopy, in-situ Raman microspectrometry (RMS), and scanning electron microscopy/energy dispersive X-ray spectrometry (SEM/EDX) elemental X-ray mapping to observe their hygroscopic behavior, derive the experimental phase diagrams, and obtain the chemical micro-structures. Dry-deposited MgCl2·6H2O particles exhibited a deliquescence relative humidity (DRH) of ∼ 33.0 % and an efflorescence RH (ERH) of 10.8-9.1 %, whereas the nebulized pure MgCl2 and MgCl2-dominant particles of XNaCl = 0.026 (eutonic) and 0.01 showed single-stage transitions at DRH of ∼ 15.9 % and ERH of 10.1-3.2 %. The characteristic OH-stretching Raman signatures indicated the crystallization of MgCl2·4H2O at low RHs, suggesting that the kinetic barrier to MgCl2·6H2O crystallization is not overcome in the timescale of the dehydration measurements. The NaCl-MgCl2 mixture particles of 0.05 ≤ XNaCl ≤ 0.9 generally showed two-stage deliquescence: first at the mutual DRH (MDRH) of ~ 15.9 %; and second with the complete dissolution of NaCl at the second DRHs depending on the mixing ratios, resulting in a phase diagram composed of three distinct phases. During dehydration, most particles of 0.05 ≤ XNaCl ≤ 0.9 exhibited two-stage efflorescence: first, by the homogeneous nucleation of NaCl; and second, at mutual ERH (MERH) of ∼ 10.4-2.9 %, by the crystallization of the MgCl2·4H2O moiety, also resulting in three distinct phases. Interestingly

  2. Hygroscopic behavior of NaCl-MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidification

    NASA Astrophysics Data System (ADS)

    Gupta, D.; Eom, H.-J.; Cho, H.-R.; Ro, C.-U.

    2015-10-01

    As Na+, Mg2+, and Cl- are major ionic constituents of seawater, NaCl-MgCl2 mixture particles might represent sea-spray aerosols (SSAs) better than pure NaCl. However, there have been very few hygroscopic studies of pure MgCl2 and NaCl-MgCl2 mixture aerosol particles despite the MgCl2 moiety playing a major role in the hygroscopic behavior of nascent SSAs. Laboratory-generated pure MgCl2 and NaCl-MgCl2 mixture aerosol particles with 12 mixing ratios (0.01 ≤ mole fraction of NaCl (XNaCl) ≤ 0.9) were examined systematically by optical microscopy (OM), in situ Raman micro-spectrometry (RMS), and scanning electron microscopy/energy dispersive X-ray spectrometry (SEM/EDX) elemental X-ray mapping to observe their hygroscopic behavior, derive the experimental phase diagrams, and obtain the chemical micro-structures. Dry-deposited MgCl2 ⋅ 6H2O particles exhibited a deliquescence relative humidity (DRH) of ~ 33.0 % and an efflorescence RH (ERH) of 10.8-9.1 %, whereas the nebulized pure MgCl2 and MgCl2-dominant particles of XNaCl = 0.026 (eutonic) and 0.01 showed single-stage transitions at DRH of ~ 15.9 % and ERH of 10.1-3.2 %. The characteristic OH-stretching Raman signatures indicated the crystallization of MgCl2 ⋅ 4H2O at low relative humidities (RHs), suggesting that the kinetic barrier to MgCl2 ⋅ 6H2O crystallization is not overcome in the timescale of the dehydration measurements. The NaCl-MgCl2 mixture particles of 0.05 ≤ XNaCl ≤ 0.9 generally showed two-stage deliquescence: first at the mutual DRH (MDRH) of ~ 15.9 %; and second with the complete dissolution of NaCl at the second DRHs depending on the mixing ratios, resulting in a phase diagram composed of three distinct phases. During dehydration, most particles of 0.05 ≤ XNaCl ≤ 0.9 exhibited two-stage efflorescence: first, by the homogeneous nucleation of NaCl; and second, at mutual ERH (MERH) of ~ 10.4-2.9 %, by the crystallization of the MgCl2 ⋅ 4H2O moiety, also resulting in three

  3. NOVEL MEASUREMENTS OF VOLATILITY- AND POLARITY-SEPARATED ORGANIC AEROSOL COMPOSITION AND ASSOCIATED HYGROSCOPICITY TO INVESTIGATE THE INFLUENCE OF MIXED ANTHROPOGENIC-BIOGENIC EMISSIONS ON ATMOSPHERIC AGING PROCESSES

    EPA Science Inventory

    Through the proposed study, novel measurements of compositional and hygroscopic changes during SOA formation and transformation under various mixtures of biogenic- anthropogenic sources will be obser\\led: 1) under unperturbed conditions, allowing meteorology to deliver vari...

  4. In-cloud processes of methacrolein under simulated conditions - Part 3: Hygroscopic and volatility properties of the formed Secondary Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Michaud, V.; El Haddad, I.; Liu, Y.; Sellegri, K.; Laj, P.; Villani, P.; Picard, D.; Marchand, N.; Monod, A.

    2009-03-01

    The hygroscopic and volatility properties of SOA produced from the nebulization of solutions after aqueous phase photooxidation of methacrolein was experimentally studied in laboratory, using a Volatility-Hygroscopicity Tandem DMA (VHTDMA). The obtained SOA were 80% 100°C-volatile after 5 h of reaction and only 20% 100°C-volatile after 22 h of reaction. The Hygroscopic Growth Factor (HGF) of the SOA produced from the nebulization of solutions after aqueous-phase photooxidation of methacrolein is 1.34-1.43, which is significantly higher than the HGF of SOA formed by gas-phase phtooxidation of terpenes, usually found nearly hydrophobic. These hygroscopic properties were confirmed for SOA formed by the nebulization of the same solutions where NaCl was added. The hygroscopic properties of the cloud droplet residuals decrease with the reaction time, in parallel with the formation of more refractory compounds. This decrease was mainly attributed to the 250°C-refractive fraction (presumably representative of the highest molecular weigh compounds), evolved from moderately hygroscopic (HGF of 1.52) to less hygroscopic (HGF of 1.36). Oligomerization is suggested as a process responsible for the decrease of both volatility and hygroscopicity with time. The NaCl seeded experiments enabled us to show that 19±4 mg L-1 of SOA was produced after 9.5 h of reaction and 41±9 mg L-1 after 22 h of in-cloud reaction. Because more and more SOA is formed as the reaction time increases, our results show that the reaction products formed during the aqueous-phase OH-oxidation of methacrolein may play a major role in the properties of residual particles upon droplet's evaporation. Therefore, the specific physical properties of SOA produced during cloud processes should be taken into account for a global estimation of SOA and their atmospheric impacts.

  5. Hygroscopic Growth and Activation of Particles containing Algea-Exudate

    NASA Astrophysics Data System (ADS)

    Wex, Heike; Fuentes, Elena; Tsagkogeorgas, Georgios; Voigtländer, Jens; Clauss, Tina; Kiselev, Alexei; Green, David; Coe, Hugh; McFiggans, Gordon; Stratmann, Frank

    2010-05-01

    ). For particles containing also algae-exudate, however, the concentration dependent non-ideal behaviour was quenched, resulting in a quasi ideal solution behavior. Such solutions could be described by a single-parameter representation for all water-vapour saturations at which measurements had been done (from 0.8 up to supersaturation). References: Fuentes, E., H. Coe, D. Green, G. De Leeuw, and G. McFiggans (2009), Laboratory-generated primary marine aerosol via bubble-bursting and atomization, Aerosol Meas. Tech. Discuss., 2, 2281-2320. O'Dowd, C. D., and G. de Leeuw (2007), Marine aerosol production: A review of the current knowledge, Phil. Trans. R. Soc. A, 365(1856), 1753-1774, doi:1710.1098/rsta.2007.2043. Niedermeier, D., H. Wex, J. Voigtländer, F. Stratmann, E. Brüggemann, A. Kiselev, H. Henk, and J. Heintzenberg (2008), LACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation, Atmos. Chem. Phys., 8, 579-590. Randall, D. A., Coakley, J. A., Fairall, C. W., Kropfli, R. A., and Lenschow, D. H. (1984) Outlook for research on subtropical marine stratiform clouds, Bull. Am. Meteor. Soc., 65, 1290-1301, 1984. Roberts, G., and A. Nenes (2005), A continuous-flow streamwise thermal-gradient CCN chamber for atmospheric measurements, Aerosol Sci. Technol., 39, 206-221. Stratmann, F., A. Kiselev, S. Wurzler, M. Wendisch, J. Heintzenberg, R. J. Charlson, K. Diehl, H. Wex, and S. Schmidt (2004), Laboratory studies and numerical simulations of cloud droplet formation under realistic super-saturation conditions, J. Atmos. Oceanic Technol., 21, 876-887. Wex, H., T. Hennig, I. Salma, R. Ocskay, A. Kiselev, S. Henning, A. Massling, A. Wiedensohler, and F. Stratmann (2007), Hygroscopic growth and measured and modeled critical super-saturations of an atmospheric HULIS sample, Geophys. Res. Lett., 34(L02818), doi:10.1029/2006GL028260.

  6. Influence of semi-volatile species on particle hygroscopic growth

    NASA Astrophysics Data System (ADS)

    Villani, P.; Sellegri, K.; Monier, M.; Laj, P.

    2009-01-01

    The hygroscopic properties of aerosol particles are often related to their content of soluble material, on the basis of the Kohler theory. Recent studies, however, seem to indicate that the role of aerosol particle semi-volatile fraction properties has been underestimated. In this study, we use a novel method based on a Tandem Differential Mobility Analyser (TDMA) system combining particle volatilization and humidification conditioning (VH-TDMA) to test the effect of the gentle volatilization of a small fraction of the atmospheric particles on the particle hygroscopic growth in several environments (urban to remote). Results show that the particle hygroscopic properties can either be enhanced or decreased after thermal conditioning of the particle at moderate temperatures (50 to 110°C). The hygroscopic growth factor changes induced by volatilization indicate that some volatile compounds, although present at low concentrations, drastically influence the hygroscopic growth of particles in the way that can not be predicted by the Kohler theory at equilibrium.

  7. Multi-Parameter Aerosol Scattering Sensor

    NASA Technical Reports Server (NTRS)

    Greenberg, Paul S.; Fischer, David G.

    2011-01-01

    This work relates to the development of sensors that measure specific aerosol properties. These properties are in the form of integrated moment distributions, i.e., total surface area, total mass, etc., or mathematical combinations of these moment distributions. Specifically, the innovation involves two fundamental features: a computational tool to design and optimize such sensors and the embodiment of these sensors in actual practice. The measurement of aerosol properties is a problem of general interest. Applications include, but are not limited to, environmental monitoring, assessment of human respiratory health, fire detection, emission characterization and control, and pollutant monitoring. The objectives for sensor development include increased accuracy and/or dynamic range, the inclusion in a single sensor of the ability to measure multiple aerosol properties, and developing an overall physical package that is rugged, compact, and low in power consumption, so as to enable deployment in harsh or confined field applications, and as distributed sensor networks. Existing instruments for this purpose include scattering photometers, direct-reading mass instruments, Beta absorption devices, differential mobility analyzers, and gravitational samplers. The family of sensors reported here is predicated on the interaction of light and matter; specifically, the scattering of light from distributions of aerosol particles. The particular arrangement of the sensor, e.g. the wavelength(s) of incident radiation, the number and location of optical detectors, etc., can be derived so as to optimize the sensor response to aerosol properties of practical interest. A key feature of the design is the potential embodiment as an extremely compact, integrated microsensor package. This is of fundamental importance, as it enables numerous previously inaccessible applications. The embodiment of these sensors is inherently low maintenance and high reliability by design. The novel and

  8. Spatio-temporal variations in aerosol optical and cloud parameters over Southern India retrieved from MODIS satellite data

    NASA Astrophysics Data System (ADS)

    Balakrishnaiah, G.; Raghavendra kumar, K.; Suresh Kumar Reddy, B.; Rama Gopal, K.; Reddy, R. R.; Reddy, L. S. S.; Swamulu, C.; Nazeer Ahammed, Y.; Narasimhulu, K.; KrishnaMoorthy, K.; Suresh Babu, S.

    2012-02-01

    Remote sensing of global aerosols has generated a great scientific interest in a variety of applications related to global warming and climate change. The spatial and temporal variations in aerosol particles over Southern India were described in the present study and the impact of these variations on various optical properties of clouds, using Moderate Resolution Imaging Spectroradiometer (MODIS) data retrieved from the Terra satellite. High mean Aerosol Optical Depth (AOD) values were observed in almost all regions during the summer season, whereas in Pune, Visakhapatnam and Hyderabad, high AOD values were noticed during the monsoon season. The Ångström exponent that increases with AOD is opposite to what would be the case if swelling of particles due to hygroscopic growth near cloudy areas played a major role in the MODIS data. We then analyzed the relationships between AOD and four other cloud parameters, namely water vapor (WV), cloud fraction (CF), cloud top temperature (CTT) and cloud top pressure (CTP). Regional correlation maps and time series plots for aerosol (AOD) and cloud parameters were produced to provide a better understanding of aerosol-cloud interaction. The correlation between AOD and CF was greater than 0.51 in Visakhapatnam, 0.45 in Thiruvanantapuram, 0.42 in Pune and whereas in Bangalore, Hyderabad and Anantapur, it is 0.17, 0.39 and 0.12, respectively. The analyses showed strong positive correlations between AOD and WV for all cities investigated. The correlation between AOD and CF was positive for all selected cities. AOD showed a negative correlation with CTP and CTT in Southern Indian regions.

  9. Biomass-burning impact on CCN number, hygroscopicity and cloud formation during summertime in the eastern Mediterranean

    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

  10. Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime

    NASA Astrophysics Data System (ADS)

    Wu, Z. J.; Zheng, J.; Shang, D. J.; Du, Z. F.; Wu, Y. S.; Zeng, L. M.; Wiedensohler, A.; Hu, M.

    2016-02-01

    Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16 ± 0.07, 0.19 ± 0.06, 0.22 ± 0.06, 0.26 ± 0.07, and 0.28 ± 0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF > 1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m-3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.

  11. Raman lidar observations of particle hygroscopicity during COPS

    NASA Astrophysics Data System (ADS)

    Stelitano, D.; Di Girolamo, P.; Summa, D.

    2012-04-01

    The characterization of particle hygroscopicity has primary importance for climate monitoring and prediction. Model studies have demonstrated that relative humidity (RH) has a critical influence on aerosol climate forcing. The relationship between aerosol backscattering and relative humidity has been investigated in numerous studies (among others, Pahlow et al., 2006; Wulfmeyer and Feingold, 2000; Veselovskii et al., 2009). Hygroscopic properties of aerosols influence particle size distribution and refractive index and hence their radiative effects. Aerosol particles tend to grow at large relative humidity values as a result of their hygroscopicity. Raman lidars with aerosol, water vapour and temperature measurement capability are potentially attractive tools for studying aerosol hygroscopicity as in fact they can provide continuous altitude-resolved measurements of particle optical, size and microphysical properties, as well as relative humidity, without perturbing the aerosols or their environment. Specifically, the University of Basilicata Raman lidar system (BASIL) considered for the present study, has the capability to perform all-lidar measurements of relative humidity based on the application of both the rotational and the vibrational Raman lidar techniques in the UV. BASIL was operational in Achern (Black Forest, Lat: 48.64 ° N, Long: 8.06 ° E, Elev.: 140 m) between 25 May and 30 August 2007 in the framework of the Convective and Orographically-induced Precipitation Study (COPS). During COPS, BASIL collected more than 500 hours of measurements, distributed over 58 measurement days and 34 intensive observation periods (IOPs). The present analysis is focused on selected case studies characterized by the presence of different aerosol types with different hygroscopic behaviour. The observed behaviour, dependent upon aerosol composition, may range from hygrophobic to strongly hygroscopic. Results from the different case studies will be illustrated and

  12. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions.

    PubMed

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J

    2009-09-28

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter kappa. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived kappa values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and approximately 3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had kappa approximately 0.003. The kaolinite samples were less hygroscopic and had kappa=0.001. SD (kappa=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (kappa=0.007) and ATD (kappa=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which

  13. Hygroscopicity of materials internally mixed with black carbon measured in Tokyo

    NASA Astrophysics Data System (ADS)

    Ohata, Sho; Schwarz, Joshua P.; Moteki, Nobuhiro; Koike, Makoto; Takami, Akinori; Kondo, Yutaka

    2016-01-01

    Black carbon (BC) aerosols become internally mixed with non-BC compounds (BC coatings) during aging in the atmosphere. In this study, we measured the hygroscopicity parameter κ on a single-particle basis for both BC-coating materials (κBC-coat) and BC-free particles (κBC-free) in the urban atmosphere of Tokyo, using a single-particle soot photometer (SP2). In our measurement system, dry ambient particles were first mass selected by an aerosol particle mass analyzer, then humidified, and then passed to the SP2 for detection of their refractory BC mass content and optical diameter. A quadrupole aerosol mass spectrometer was also employed to interpret the hygroscopicity data. During the observation period, the measured κBC-coat generally agreed with κBC-free to within ±25% and was usually in typical range for inorganic and organic aerosols. These results indicate that BC-coating materials and BC-free particles in Tokyo usually had similar chemical compositions, internal mixtures of inorganic and organic compounds, even in a source region. However, occasionally κBC-coat was much higher than κBC-free values, when the mass concentrations of BC and organic aerosols were poorly correlated. This indicates external mixing of BC-containing and BC-free particles from different sources. These findings improve our understanding of the cloud condensation nuclei activity of BC-containing particles, which strongly influences their wet removal, and optical properties in the ambient air.

  14. Parameterization of the Cloud Nucleating Activity of Fresh, Aged, and Internally-Mixed Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Kreidenweis, S.; Petters, M.; Demott, P.; Prenni, A.; Ziemann, P.

    2006-12-01

    Carbonaceous particle types affect global climate, visibility, and human health, but their primary and secondary sources, sinks, and tropospheric lifetimes are highly uncertain. The size and hygroscopicity of particles, and in particular their activity as cloud condensation nuclei (CCN), plays a large role in determining their atmospheric impacts and lifetimes. However, hygroscopicity is difficult to parameterize for many organic species for which no thermodynamic data exist, and for complex, multicomponent aerosols of undefined composition. We propose a simple method to describe the relationship between dry particle diameter and CCN activity using a single hygroscopicity parameter, κ. We derive values of κ from fitting of experimental CCN-activity data from the literature and from recent experiments, including oxidation-aged organic particles and secondary organic aerosols. Values of κ are between 0.5 and 2 for highly-CCN- active salts such as sodium chloride, between 0.01 and 0.5 for slightly to very hygroscopic organic aerosols such as those produced in biomass burning and as secondary organic aerosols, and 0 for nonhygroscopic components. The hygroscopicity of internal mixtures can be calculated as a volume fraction weighted average of the hygroscopicity parameters of the individual species comprising the mixture. Aging of aerosol, understood as changes in hygroscopicity due to condensation of hydrophilic species, coagulation of aerosol populations, or heterogeneous chemical reactions, are described conveniently by changes in κ. Our studies show that oxidative aging that proceeds by addition of functional groups to the CHx carbon backbone leads to only small changes in κ, and thus the process alone is inefficient at rendering small, initially- hydrophobic primary organic particles capable of being scavenged by cloud-drop nucleation. Other processes, such as coagulation and condensation, control the rate of hydrophobic-to-hydrophilic conversion of primary

  15. Aqueous Phase Photo-Oxidation of Succinic Acid: Changes in Hygroscopic Properties and Reaction Products

    NASA Astrophysics Data System (ADS)

    Hudson, P. K.; Ninokawa, A.; Hofstra, J.; de Lijser, P.

    2013-12-01

    Atmospheric aerosol particles have been identified as important factors in understanding climate change. The extent to which aerosols affect climate is determined, in part, by hygroscopic properties which can change as a result of atmospheric processing. Dicarboxylic acids, components of atmospheric aerosol, have a wide range of hygroscopic properties and can undergo oxidation and photolysis reactions in the atmosphere. In this study, the hygroscopic properties of succinic acid aerosol, a non-hygroscopic four carbon dicarboxylic acid, were measured with a humidified tandem differential mobility analyzer (HTDMA) and compared to reaction products resulting from the aqueous phase photo-oxidation reaction of hydrogen peroxide and succinic acid. Reaction products were determined and quantified using gas chromatography-flame ionization detection (GC-FID) and GC-mass spectrometry (GC-MS) as a function of hydrogen peroxide:succinic acid concentration ratio and photolysis time. Although reaction products include larger non-hygroscopic dicarboxylic acids (e.g. adipic acid) and smaller hygroscopic dicarboxylic acids (e.g. malonic and oxalic acids), comparison of hygroscopic growth curves to Zdanovskii-Stokes-Robinson (ZSR) predictions suggests that the hygroscopic properties of many of the product mixtures are largely independent of the hygroscopicity of the individual components. This study provides a framework for future investigations to fully understand and predict the role of chemical reactions in altering atmospheric conditions that affect climate.

  16. Hygroscopicity of mineral dust particles: Roles of chemical mixing state and hygroscopic conversion timescale

    NASA Astrophysics Data System (ADS)

    Sullivan, R. C.; Moore, M. J.; Petters, M. D.; Laskin, A.; Roberts, G. C.; Kreidenweis, S. M.; Prather, K. A.

    2009-05-01

    Our laboratory investigations of mineral dust particle hygroscopicity are motivated by field observations of the atmospheric processing of dust. During ACE-Asia we observed sulphate and nitrate to be strongly segregated from each other in individual aged Asian dust particles. CCN activation curves of pure calcium minerals as proxies for fresh (calcium carbonate) and aged (calcium sulphate, nitrate, chloride) dust indicate that this mixing state would cause a large fraction of aged dust particles to remain poor warm cloud nucleation potential, contrary to previous assumptions. The enrichment of oxalic acid in calcium-rich dust particles could have similar effects due to the formation of insoluble calcium oxalate. Soluble calcium nitrate and chloride reaction products are hygroscopic and will transform mineral dust into excellent CCN. Generating insoluble mineral particles wet by atomization produced particles with much higher hygroscopicity then when resuspended dry. The atomized particles are likely composed of dissolved residuals and do not properly reflect the chemistry of dry mineral powders. Aerosol flow tube experiments were employed to study the conversion of calcium carbonate into calcium nitrate via heterogeneous reaction with nitric acid, with simultaneous measurements of the reacted particles' chemistry and hygroscopicity. The timescale for this hygroscopic conversion was found to occur on the order of a few hours under tropospheric conditions. This implies that the conversion of non-hygroscopic calcite- containing dust into hygroscopic particles will be controlled by the availability of nitric acid, and not by the atmospheric residence time. Results from recent investigations of the effect of secondary coatings on the ice nucleation properties of dust particles will also be presented. The cloud formation potential of aged dust particles depends on both the quantity and form of the secondary species that have reacted or mixed with the dust. These results

  17. Continuous Measurement of Particle Hygroscopicity as a Function of Diameter

    NASA Astrophysics Data System (ADS)

    Brock, C. A.; Anderson, B. E.; Ziemba, L. D.; Thornhill, K. L.; Moore, R.; Beyersdorf, A. J.; Winstead, E. L.; Crumeyrolle, S.; Wagner, N.; Langridge, J. M.; Richardson, M.; Lack, D. A.; Law, D. C.; Shingler, T.; Sorooshian, A.

    2012-12-01

    An ultra-high sensitivity aerosol spectrometer (UHSAS, Droplet Measurement Technologies, Boulder, CO, USA) has been substantially modified to humidify the aerosol sample stream. The size distribution of deliquesced particles at humidities as high as 95% is measured. By combining a Mie model of instrument response with measurements of dry and wet size distributions, the hygroscopic growth factor as a function of particle diameter can be estimated. By operating a second, well-calibrated dry UHSAS simultaneously with the humidified UHSAS, the size-dependent particle hygroscopicity can be determined continuously, which is particularly useful for airborne sampling where rapid time response is required. The technique has been applied to laboratory particles of inorganic salts and of polystyrene latex, and to mixed sulfate/organic particles and dense forest fire smoke measured on an aircraft during the Deep Convective Clouds and Chemistry (DC3) project. Results will be compared with measurements of aerosol extinction at different RH values and of hygroscopic growth made with a differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). Initial evaluations of changes in hygroscopicity due to processing in convective clouds will be presented. Limitations of the technique, such as the effects of external mixtures and insoluble components, will be discussed.

  18. Cloud Forming Potential of Aminium Carboxylate Aerosols

    NASA Astrophysics Data System (ADS)

    Gomez Hernandez, M. E.; McKeown, M.; Taylor, N.; Collins, D. R.; Lavi, A.; Rudich, Y.; Zhang, R.

    2014-12-01

    Atmospheric aerosols affect visibility, air quality, human health, climate, and in particular the aerosol direct and indirect forcings represent the largest uncertainty in climate projections. In this paper, we present laboratory measurements of the hygroscopic growth factors (HGf) and cloud condensation nuclei (CCN) activity of a series of aminium carboxylate salt aerosols, utilizing a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) coupled to a Condensation Particle Counter (CPC) and a CCN counter. HGf measurements were conducted for size-selected aerosols with diameters ranging from 46 nm to 151 nm and at relative humidity (RH%) values ranging from 10 to 90%. In addition, we have calculated the CCN activation diameters for the aminium carboxylate aerosols and derived the hygroscopicity parameter (k or kappa) values for all species using three methods, i.e., the mixing rule approximation, HGf, and CCN results. Our results show that variations in the ratio of acid to base directly affect the activation diameter, HGf, and (k) values of the aminium carboxylate aerosols. Atmospheric implications of the variations in the chemical composition of aminium carboxylate aerosols on their cloud forming potential will be discussed.

  19. Hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Wu, Z. J.; Nowak, A.; Poulain, L.; Herrmann, H.; Wiedensohler, A.

    2011-03-01

    The hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their effects on ammonium sulfate was investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA). No hygroscopic growth is observed for sodium oxalate, while ammonium oxalate shows slight growth (growth factor = 1.05 at 90%). The growth factors at 90% RH for sodium acetate, sodium malonate, sodium succinate, sodium tartrate, ammonium tartrate, sodium pyruvate, sodium maleate, and humic acid sodium salt are 1.79, 1.78, 1.69, 1.54, 1.29, 1.70, 1.78, and 1.19, respectively. The mixtures of organic salts with ammonium sulfate, which are prepared simulating the atmospheric aerosols, are determined. A clear shift in DRH of mixture to lower RH is observed with increasing organic mass fraction. Above RH = 80%, the humidograms of the different mixtures are quite close to that of pure ammonium sulfate. Köhler theory is used to predict the effective hygroscopicity parameter, κ, for mixtures at 90% RH. The results show that Köhler theory underestimated kappa for mixtures without considering the water solubility of ammonium oxalate. However, if the water solubility of ammonium oxalate is taken into account, the results show a much better agreement with those derived from H-TDMA measurements.

  20. Influence of semi-volatile species on particle hygroscopic growth

    NASA Astrophysics Data System (ADS)

    Villani, Paolo; Sellegri, Karine; Monier, Marie; Laj, Paolo

    2013-11-01

    In this study, we use a Tandem Differential Mobility Analyser (TDMA) system combining particle volatilization and humidification conditioning (VH-TDMA) to test the effect of the gentle volatilization of a small fraction of the atmospheric particles on the particle hygroscopic growth in several environments (urban to remote). We first give an overview of the Hygroscopic Growth Factors (HGF) in these various environments, showing that in most of them, aerosol particles are externally mixed. We then show that the particle hygroscopicity can either be increased or decreased after thermal conditioning of the particle at moderate temperatures (50-110 °C). The hygroscopic growth factor changes induced by volatilization indicate that some volatile compounds, although present at low concentrations, can significantly influence the hygroscopic growth of particles in a way that can most of time be theoretically explained if simplified assumptions are used. However, simplified assumptions occasionally fail over several hours to explain hygroscopic changes, kinetic/surface effects observed at remote environments are suspected to be important.

  1. Changes of hygroscopicity and morphology during ageing of diesel soot

    NASA Astrophysics Data System (ADS)

    Tritscher, Torsten; Jurányi, Zsófia; Martin, Maria; Chirico, Roberto; Gysel, Martin; Heringa, Maarten F.; DeCarlo, Peter F.; Sierau, Berko; Prévôt, André S. H.; Weingartner, Ernest; Baltensperger, Urs

    2011-07-01

    Soot particles are an important component of atmospheric aerosol and their interaction with water is important for their climate effects. The hygroscopicity of fresh and photochemically aged soot and secondary organic aerosol (SOA) from diesel passenger car emissions was studied under atmospherically relevant conditions in a smog chamber at sub-and supersaturation of water vapor. Fresh soot particles show no significant hygroscopic growth nor cloud condensation nucleus (CCN) activity. Ageing by condensation of SOA formed by photooxidation of the volatile organic carbon (VOC) emission leads to increased water uptake and CCN activity as well as to a compaction of the initially non-spherical soot particles when exposed to high relative humidity (RH). It is important to consider the latter effect for the interpretation of mobility based measurements. The vehicle with oxidation catalyst (EURO3) emits much fewer VOCs than the vehicle without after-treatment (EURO2). Consequently, more SOA is formed for the latter, resulting in more pronounced effects on particle hygroscopicity and CCN activity. Nevertheless, the aged soot particles did not reach the hygroscopicity of pure SOA particles formed from diesel VOC emissions, which are similarly hygroscopic (0.06 < κH - TDMA < 0.12 and 0.09 < κCCN < 0.14) as SOA from other precursor gases investigated in previous studies.

  2. The optical properties of hygroscopic soot aggregates with water coating

    NASA Astrophysics Data System (ADS)

    Wu, Yu; Cheng, Tianhai; Zheng, Lijuan

    2014-05-01

    Anthropogenic aerosols, such as soot, have modified the Earth's radiation balance by scattering and absorbing solar and long-wave radiative transmission, which have largely influenced the global climate change since the industrial era. Based on transmission electron microscope images (TEM), soot particles are shown as the complex, fractal-like aggregate structures. In humid atmospheric environments, these soot aggregates tend to acquire a water coating, which introduces further complexity to the problem of determining the optical properties of the aggregates. The hygroscopic growth of soot aggregates is important for the aging of these absorbing aerosols, which can significantly influence the optical properties of these kinds of soot particles. In this paper, according to the specific volume fractions of soot core in the water coated soot particle, the monomers of fractal soot aggregates are modeled as semi-external mixtures (physical contact) with constant radius of soot core and variable size of water coating. The single scattering properties of these hygroscopic soot particles, such as scattering matrices, the cross sections of extinction, absorption and scattering, single scattering albedo (SSA), and asymmetry parameter (ASY), are calculated using the numerically exact superposition T-matrix method. The morphological effects are compared with different monomer numbers and fractal dimensions of the soot aggregates, as well as different size of water coating for these concentric spherical monomers. The results have shown that SSA, cross sections of extinction and absorption are increased for soot aggregates with thicker weakly absorbing coating on the monomers. It is found that the SSA of aged soot aggregates with hygroscopic grown are remarkably (~50% for volume fraction of soot aggregates is 0.5, at 0.670μm) larger than fresh soot particles without the consideration of water coating, due to the size of water coating and the morphological features, such as the

  3. Hygroscopicity and composition of Alaskan Arctic CCN during April 2008

    NASA Astrophysics Data System (ADS)

    Moore, R. H.; Bahreini, R.; Brock, C. A.; Froyd, K. D.; Cozic, J.; Holloway, J. S.; Middlebrook, A. M.; Murphy, D. M.; Nenes, A.

    2011-08-01

    We present a comprehensive characterization of cloud condensation nuclei (CCN) sampled in the Alaskan Arctic during the 2008 Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project, a component of the POLARCAT and International Polar Year (IPY) initiatives. Four distinct air mass types were sampled including relatively pristine Arctic background conditions as well as biomass burning and anthropogenic pollution plumes. Despite differences in chemical composition, inferred aerosol hygroscopicities were fairly invariant and ranged from κ = 0.1-0.3 over the atmospherically-relevant range of water vapor supersaturations studied. Analysis of the individual mass spectral m/z 43 and 44 peaks from an aerosol mass spectrometer show the organic aerosols sampled to be well-oxygenated, consistent with with long-range transport and aerosol aging processes. However, inferred hygroscopicities are less than would be predicted based on previous parameterizations of biogenic oxygenated organic aerosol, suggesting an upper limit on organic aerosol hygroscopicity above which κ is less sensitive to the O:C ratio. Most Arctic aerosol act as CCN above 0.1 % supersaturation, although the data suggest the presence of an externally-mixed, non-CCN-active mode comprising approximately 0-20 % of the aerosol number. CCN closure was assessed using measured size distributions, bulk chemical composition measurements, and assumed aerosol mixing states; CCN predictions tended toward overprediction, with the best agreement (± 0-20 %) obtained by assuming the aerosol to be externally-mixed with soluble organics. Closure also varied with CCN concentration, and the best agreement was found for CCN concentrations above 100 cm-3 with a 1.5- to 3-fold overprediction at lower concentrations.

  4. Experimentally measured morphology of biomass burning aerosol and its impacts on CCN ability

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Espinoza, C.; Asa-Awuku, A.

    2015-02-01

    This study examines the morphological properties of freshly emitted and atmospherically aged aerosols from biomass burning. The impacts of particle morphology assumptions on hygroscopic predictions are examined. Chamber experiments were conducted at the University of California, Riverside, Center for Environmental Research and Technology (CE-CERT) atmospheric processes lab using two biomass fuel sources: manzanita and chamise. Morphological data was obtained through the use of an aerosol particle mass analyzer (APM), scanning mobility particle sizer (SMPS) system and transmission electron microscope (TEM). Data from these instruments was used to calculate both a dynamic shape factor and a fractal-like dimension for the biomass burning emissions. This data was then used with κ-Köhler theory to adjust the calculated hygroscopicity for experimentally determined morphological characteristics of the aerosol. Laboratory measurement of biomass burning aerosol from two chaparral fuels show that particles are nonspherical with dynamic shape factors greater than 1.15 for aerosol sizes relevant to cloud condensation nuclei (CCN) activation. Accounting for particle morphology can shift the hygroscopicity parameter by 0.15 or more. To our knowledge, this work provides the first laboratory chamber measurements of morphological characteristics for biomass burning cloud condensation nuclei and provides experimental particle shape evidence to support the variation in reported hygroscopicities of the complex aerosol.

  5. Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

    NASA Astrophysics Data System (ADS)

    Kim, J.; Ahlm, L.; Yli-Juuti, T.; Lawler, M.; Keskinen, H.; Tröstl, J.; Schobesberger, S.; Duplissy, J.; Amorim, A.; Bianchi, F.; Donahue, N. M.; Flagan, R. C.; Hakala, J.; Heinritzi, M.; Jokinen, T.; Kürten, A.; Laaksonen, A.; Lehtipalo, K.; Miettinen, P.; Petäjä, T.; Rissanen, M. P.; Rondo, L.; Sengupta, K.; Simon, M.; Tomé, A.; Williamson, C.; Wimmer, D.; Winkler, P. M.; Ehrhart, S.; Ye, P.; Kirkby, J.; Curtius, J.; Baltensperger, U.; Kulmala, M.; Lehtinen, K. E. J.; Smith, J. N.; Riipinen, I.; Virtanen, A.

    2016-01-01

    Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm-3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (κDMAS ˜ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid-imethylamine experiments increased with increasing particle size. The κ values of particles in the presence of

  6. Hygroscopicity and composition of Alaskan Arctic CCN during April 2008

    NASA Astrophysics Data System (ADS)

    Moore, R. H.; Bahreini, R.; Brock, C. A.; Froyd, K. D.; Cozic, J.; Holloway, J. S.; Middlebrook, A. M.; Murphy, D. M.; Nenes, A.

    2011-11-01

    We present a comprehensive characterization of cloud condensation nuclei (CCN) sampled in the Alaskan Arctic during the 2008 Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project, a component of the POLARCAT and International Polar Year (IPY) initiatives. Four distinct air mass types were sampled including a cleaner Arctic background and a relatively pristine sea ice boundary layer as well as biomass burning and anthropogenic pollution plumes. Despite differences in chemical composition, inferred aerosol hygroscopicities were fairly invariant and ranged from κ = 0.1-0.3 over the atmospherically-relevant range of water vapor supersaturations studied. Organic aerosols sampled were found to be well-oxygenated, consistent with long-range transport and aerosol aging processes. However, inferred hygroscopicities are less than would be predicted based on previous parameterizations of biogenic oxygenated organic aerosol, suggesting an upper limit on organic aerosol hygroscopicity above which κ is less sensitive to the O:C ratio. Most Arctic aerosols act as CCN above 0.1 % supersaturation, although the data suggest the presence of an externally-mixed, non-CCN-active mode comprising approximately 0-20% of the aerosol number. CCN closure was assessed using measured size distributions, bulk chemical composition, and assumed aerosol mixing states; CCN predictions tended toward overprediction, with the best agreement (±0-20 %) obtained by assuming the aerosol to be externally-mixed with soluble organics. Closure also varied with CCN concentration, and the best agreement was found for CCN concentrations above 100 cm-3 with a 1.5- to 3-fold overprediction at lower concentrations.

  7. Characterization of particle hygroscopicity by Raman lidar: Selected case studies from the convective and orographically-induced precipitation study

    NASA Astrophysics Data System (ADS)

    Stelitano, Dario; Di Girolamo, Paolo; Summa, Donato

    2013-05-01

    The characterization of particle hygroscopicity has primary importance for climate monitoring and prediction. Model studies have demonstrated that relative humidity (RH) has a critical influence on aerosol climate forcing. Hygroscopic properties of aerosols influence particle size distribution and refractive index and hence their radiative effects. Aerosol particles tend to grow at large relative humidity values as a result of their hygroscopicity. Raman lidars with aerosol, water vapor and temperature measurement capability are potentially attractive tools for studying aerosol hygroscopicity as in fact they can provide continuous altitude-resolved measurements of particle optical, size and microphysical properties, as well as relative humidity, without perturbing the aerosols or their environment. Specifically, the University of Basilicata Raman lidar system (BASIL) considered for the present study, has the capability to perform all-lidar measurements of relative humidity based on the application of both the rotational and the vibrational Raman lidar techniques in the UV. BASIL was operational in Achern (Black Forest, Lat: 48.64° N, Long: 8.06° E, Elev.: 140 m) between 25 May and 30 August 2007 in the framework of the Convective and Orographically-induced Precipitation Study (COPS). The present analysis is focused on selected case studies characterized by the presence of different aerosol types with different hygroscopic behavior. The observed behavior, dependent upon aerosol composition, may range from hygrophobic to strongly hygroscopic.

  8. Multiple scattering in cloud layers; some results. [emphasizing aerosol parameters on global basis

    NASA Technical Reports Server (NTRS)

    Vandehulst, H. C.

    1974-01-01

    Theoretical methods are discussed for calculating radiative effects of aerosols. Experimental determination is emphasized for relevant aerosol parameters on a global basis to arrive at realistic estimates of heating and cooling. Internal radiation fields in very thin and very thick slabs are reviewed. Phase functions, polarization, emission by internal sources, and path length distribution are also considered.

  9. Simultaneous Retrieval of Multiple Aerosol Parameters Using a Multi-Angular Approach

    NASA Technical Reports Server (NTRS)

    Kuo, K. S.; Weger, R. C.; Welch, R. M.

    1997-01-01

    Atmospheric aerosol particles, both natural and anthropogenic, are important to the earth's radiative balance through their direct and indirect effects. They scatter the incoming solar radiation (direct effect) and modify the shortwave reflective properties of clouds by acting as cloud condensation nuclei (indirect effect). Although it has been suggested that aerosols exert a net cooling influence on climate, this effect has received less attention than the radiative forcing due to clouds and greenhouse gases. In order to understand the role that aerosols play in a changing climate, detailed and accurate observations are a prerequisite. The retrieval of aerosol optical properties by satellite remote sensing has proven to be a difficult task. The difficulty results mainly from the tenuous nature and variable composition of aerosols. To date, with single-angle satellite observations, we can only retrieve reliably against dark backgrounds, such as over oceans and dense vegetation. Even then, assumptions must be made concerning the chemical composition of aerosols. The best hope we have for aerosol retrievals over bright backgrounds are observations from multiple angles, such as those provided by the MISR and POLDER instruments. In this investigation we examine the feasibility of simultaneous retrieval of multiple aerosol optical parameters using reflectances from a typical set of twelve angles observed by the French POLDER instrument. The retrieved aerosol optical parameters consist of asymmetry factor, single scattering albedo, surface albedo, and optical thickness.

  10. Retrieval of integral parameters of tropospheric aerosol from two-wavelength lidar sounding

    NASA Astrophysics Data System (ADS)

    Korshunov, V. A.

    2007-10-01

    A scheme of interpreting the data of two-wavelength lidar sounding is proposed. The scheme is based on functional relationships between the lidar ratios and between some integral characteristics of aerosol and the ratio of the backscattering coefficients at the sounding wavelengths. The AERONET data, results of contact aerosol measurements and multiwavelength lidar sounding, and the OPAC aerosol model are used to find these functional relationships, which are statistical in character. Analysis of data is made separately for continental, dust, oceanic, and smoke aerosols. Backscattering for mineral aerosol fractions are calculated for a model of randomly oriented spheroids. A numerical experiment shows that the errors in determining a number of integral parameters of aerosol (extinction coefficient, characteristic radius of particles, volume concentrations) that are due to the statistical straggling of lidar ratios and other specified integral characteristics are no greater than 32% if the optical thickness of the sounding layer is no greater than 1.

  11. Scattering directionality parameters of fractal black carbon aerosols and comparison with the Henyey-Greenstein approximation.

    PubMed

    Pandey, Apoorva; Chakrabarty, Rajan K

    2016-07-15

    Current radiation transfer schemes employ the Henyey-Greenstein (HG) phase function to connect three single parameter representations of aerosol scattering directionality-the hemispherical upscatter fraction (β), the backscatter fraction (b), and the asymmetry parameter (g). The HG phase function does not account for particle morphology, which could lead to significant errors. In this Letter, we compute these single parameters for fractal black carbon (BC) aerosols using the numerically exact superposition T-matrix method. The variations in β, g, and b as a function of aerosol morphology are examined. Corrected empirical relationships connecting these parameters are proposed. We find that the HG phase function could introduce up to a 35% error in β and g estimates. Interestingly, these errors are suppressed by the large mass absorption cross-sections of BC aerosols in radiative transfer calculations and contribute to ≤8% error in direct forcing efficiencies. PMID:27420533

  12. Water uptake of multicomponent organic mixtures and their influence on hygroscopicity of inorganic salts.

    PubMed

    Wang, Yuanyuan; Jing, Bo; Guo, Yucong; Li, Junling; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

    2016-07-01

    The hygroscopic behaviors of atmospherically relevant multicomponent water soluble organic compounds (WSOCs) and their effects on ammonium sulfate (AS) and sodium chloride were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA) in the relative humidity (RH) range of 5%-90%. The measured hygroscopic growth was compared with predictions from the Extended-Aerosol Inorganics Model (E-AIM) and Zdanovskii-Stokes-Robinson (ZSR) method. The equal mass multicomponent WSOCs mixture containing levoglucosan, succinic acid, phthalic acid and humic acid showed gradual water uptake without obvious phase change over the whole RH range. It was found that the organic content played an important role in the water uptake of mixed particles. When organic content was dominant in the mixture (75%), the measured hygroscopic growth was higher than predictions from the E-AIM or ZSR relation, especially under high RH conditions. For mass fractions of organics not larger than 50%, the hygroscopic growth of mixtures was in good agreement with model predictions. The influence of interactions between inorganic and organic components on the hygroscopicity of mixed particles was related to the salt type and organic content. These results could contribute to understanding of the hygroscopic behaviors of multicomponent aerosol particles. PMID:27372129

  13. Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in Situ Imaging.

    PubMed

    Piens, Dominique S; Kelly, Stephen T; Harder, Tristan H; Petters, Markus D; O'Brien, Rachel E; Wang, Bingbing; Teske, Ken; Dowell, Pat; Laskin, Alexander; Gilles, Mary K

    2016-05-17

    Quantifying how atmospheric particles interact with water vapor is critical for understanding the effects of aerosols on climate. We present a novel method to measure the mass-based hygroscopicity of particles while characterizing their elemental and carbon functional group compositions. Since mass-based hygroscopicity is insensitive to particle geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, which can have irregular morphologies. Combining scanning electron microscopy with energy dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) analysis, and in situ STXM humidification experiments, this method was validated using laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental composition of 15 complex atmospheric particles were analyzed by leveraging quantification of C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl content. The mixing state of 158 other particles from the sample broadly agreed with those of the humidified particles, indicating the potential to infer atmospheric hygroscopic behavior from a selected subset of particles. These methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles. PMID:27088454

  14. Measuring mass-based hygroscopicity of atmospheric particles through in situ imaging

    DOE PAGESBeta

    Piens, Dominique S.; Kelly, Stephen T.; Harder, Tristan H.; Petters, Markus D.; O’Brien, Rachel E.; Wang, Bingbing; Teske, Ken; Dowell, Pat; Laskin, Alexander; Gilles, Mary K.

    2016-04-18

    Quantifying how atmospheric particles interact with water vapor is critical for understanding the effects of aerosols on climate. We present a novel method to measure the mass-based hygroscopicity of particles while characterizing their elemental and carbon functional group compositions. Since mass-based hygroscopicity is insensitive to particle geometry, it is advantageous for probing the hygroscopic behavior of atmospheric particles, which can have irregular morphologies. Combining scanning electron microscopy with energy dispersive X-ray analysis (SEM/EDX), scanning transmission X-ray microscopy (STXM) analysis, and in situ STXM humidification experiments, this method was validated using laboratory-generated, atmospherically relevant particles. Then, the hygroscopicity and elemental compositionmore » of 15 complex atmospheric particles were analyzed by leveraging quantification of C, N, and O from STXM, and complementary elemental quantification from SEM/EDX. We found three types of hygroscopic responses, and correlated high hygroscopicity with Na and Cl content. The mixing state of 158 other particles from the sample broadly agreed with those of the humidified particles, indicating the potential to infer atmospheric hygroscopic behavior from a selected subset of particles. As a result, these methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles.« less

  15. MISR Level 2 Aerosol parameters (MIL2ASAE_V2)

    NASA Technical Reports Server (NTRS)

    Diner, David J. (Principal Investigator)

    The Aerosol data contain aerosol optical depth, aerosol physical model, ancillary meteorological data, and related parameters. The aerosol data include tropospheric aerosol optical depth, Angstrom exponent and single scattering albedo on 17.6 km centers, aerosol mixture identifier and retrieval residuals, and ancillary data including assumed ozone optical depth and retrieval flags. For complete information about the aerosol mixtures, the user will need to order the MISR Aerosol Climatology Product (MIANACP) to obtain Aerosol Physical and Optical Properties (APOP) and the Mixture files. The Mixture files list up to 3 component models used in each mixture, with their relative compositional fractions, and includes ancillary information such as single scattering albedo. The APOP gives detailed information for the component particle models. [Location=GLOBAL] [Temporal_Coverage: Start_Date=2000-02-24; Stop_Date=] [Spatial_Coverage: Southernmost_Latitude=-90; Northernmost_Latitude=90; Westernmost_Longitude=-180; Easternmost_Longitude=180] [Data_Resolution: Latitude_Resolution=1.1 km - 17.6 km; Longitude_Resolution=1.1 km - 17.6 km; Horizontal_Resolution_Range=1 km - < 10 km or approximately .01 degree - < .09 degree; Temporal_Resolution=about 15 orbits/day; Temporal_Resolution_Range=Daily - < Weekly, Daily - < Weekly].

  16. Urban and rural aerosol characterization of summer smog events during the PIPAPO field campaign in Milan, Italy

    NASA Astrophysics Data System (ADS)

    Baltensperger, U.; Streit, N.; Weingartner, E.; Nyeki, S.; PréVôT, A. S. H.; van Dingenen, R.; Virkkula, A.; Putaud, J.-P.; Even, A.; ten Brink, H.; Blatter, A.; Neftel, A.; GäGgeler, H. W.

    2002-11-01

    A comprehensive range of aerosol parameters was measured at an urban and a rural site in the Milan, Italy metropolitan region during summer smog events in summer 1998. Measurements were performed as part of the Pianura Padana Produzione di Ozono (PIPAPO) field campaign to determine the sensitivity of O3 production to NOX and volatile organic carbon concentrations at several ground stations. Primary aerosol parameters (i.e., direct emissions) such as aerosol black carbon showed a distinct diurnal variation with maxima at about 0000 and 0800 central European summer time (CEST), in contrast to secondary aerosol parameters such as sulfate and nitrate. Aerosol number size distributions were measured under ambient conditions as well as after conditioning with volatility and hygroscopicity systems. A mode at d = 20-30 nm in the number concentration was found at 0800 CEST and exhibited high volatility at 110°C (˜80% volume lost upon heating) but no hygroscopic behavior. Based on these measurements, small particles (d < 40 nm) are thought to consist mainly of hydrophobic particulate organic matter, rather than soot or H2SO4 aerosols. Two distinct hygroscopic modes with average growth factors d/d0 ˜ 1.02 and 1.21-1.28 were found for particles with dry (relative humidity of <30%) diameters d0 = 50-200 nm. Submicrometer aerosols exhibited lower volatility at the rural than at the urban site, which is attributed to additional particulate mass produced by secondary particle formation.

  17. Urban and rural aerosol characterization of summer smog events during the PIPAPO field campaign in Milan, Italy

    NASA Astrophysics Data System (ADS)

    Baltensperger, U.; Streit, N.; Weingartner, E.; Nyeki, S.; Prévôt, A. S. H.; Van Dingenen, R.; Virkkula, A.; Putaud, J.-P.; Even, A.; ten Brink, H.; Blatter, A.; Neftel, A.; Gäggeler, H. W.

    2002-10-01

    A comprehensive range of aerosol parameters was measured at an urban and a rural site in the Milan, Italy metropolitan region during summer smog events in summer 1998. Measurements were performed as part of the Pianura Padana Produzione di Ozono (PIPAPO) field campaign to determine the sensitivity of O3 production to NOX and volatile organic carbon concentrations at several ground stations. Primary aerosol parameters (i.e., direct emissions) such as aerosol black carbon showed a distinct diurnal variation with maxima at about 0000 and 0800 central European summer time (CEST), in contrast to secondary aerosol parameters such as sulfate and nitrate. Aerosol number size distributions were measured under ambient conditions as well as after conditioning with volatility and hygroscopicity systems. A mode at d = 20-30 nm in the number concentration was found at 0800 CEST and exhibited high volatility at 110°C (~80% volume lost upon heating) but no hygroscopic behavior. Based on these measurements, small particles (d < 40 nm) are thought to consist mainly of hydrophobic particulate organic matter, rather than soot or H2SO4 aerosols. Two distinct hygroscopic modes with average growth factors d/d0 ~ 1.02 and 1.21-1.28 were found for particles with dry (relative humidity of <30%) diameters d0 = 50-200 nm. Submicrometer aerosols exhibited lower volatility at the rural than at the urban site, which is attributed to additional particulate mass produced by secondary particle formation.

  18. Simultaneous Retrieval of Multiple Aerosol Parameters Using a Multi-Angular Approach

    NASA Technical Reports Server (NTRS)

    Kuo, K.-S.; Weger, R. C.; Welch, R. M.

    1997-01-01

    Atmospheric aerosol particles, both natural and anthropogenic, are important to the earth's radiative balance through their direct and indirect effects. They scatter the incoming solar radiation (direct effect) and modify the shortwave reflective properties of clouds by acting as cloud condensation nuclei (indirect effect). Although it has been suggested that aerosols exert a net cooling influence on climate, this effect has received less attention than the radiative forcing due to clouds and greenhouse gases. In order to understand the role that aerosols play in a changing climate, detailed and accurate observations are a prerequisite. The retrieval of aerosol optical properties by satellite remote sensing has proven to be a difficult task. The difficulty results mainly from the tenuous nature and variable composition of aerosols. To date, with single-angle satellite observations, we can only retrieve reliably against dark backgrounds, such as over oceans and dense vegetation. Even then, assumptions must be made concerning the chemical composition of aerosols. In this investigation we examine the feasibility of simultaneous retrieval of multiple aerosol optical parameters using reflectances from a typical set of twelve angles observed by the French POLDER instrument. The retrieved aerosol optical parameters consist of asymmetry factor, single scattering albedo, surface albedo, and optical thickness.

  19. Potential of polarization lidar to provide profiles of CCN- and INP-relevant aerosol parameters

    NASA Astrophysics Data System (ADS)

    Mamouri, R. E.; Ansmann, A.

    2015-12-01

    We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of number concentrations of aerosol particles with radius > 50 nm (APC50, reservoir of favorable CCN) and with radius > 250 nm (APC250, reservoir of favorable INP), as well as profiles of the aerosol particle surface area concentration (ASC, used in INP parameterization) can be retrieved from lidar-derived aerosol extinction coefficients (AEC) with relative uncertainties of a factor of around 2 (APC50), and of about 25-50 % (APC250, ASC). Of key importance is the potential of polarization lidar to identify mineral dust particles and to distinguish and separate the aerosol properties of basic aerosol types such as mineral dust and continental pollution (haze, smoke). We investigate the relationship between AEC and APC50, APC250, and ASC for the main lidar wavelengths of 355, 532 and 1064 nm and main aerosol types (dust, pollution, marine). Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures of continental pollution, mineral dust, and marine aerosol. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple relationship between APC50 and the CCN-reservoir particles (APCCCN) and published INP parameterization schemes (with APC250 and ASC as input) we finally compute APCCCN and INP concentration profiles. We apply the full methodology to a lidar observation of a heavy dust outbreak crossing Cyprus with dust up to 8 km height and to a case during which anthropogenic pollution dominated.

  20. Aerosol Single-Scattering Albedo and Asymmetry Parameter from MFRSR Observations during the ARM Aerosol IOP 2003

    SciTech Connect

    Kassianov, Evgueni I.; Flynn, Connor J.; Ackerman, Thomas P.; Barnard, James C.

    2007-06-15

    Multi-filter Rotating Shadowband Radiometers (MFRSRs) provide routine measurements of the aerosol optical depth ( << OLE Object: Microsoft Equation 3.0 >> ) at six wavelengths (0.415, 0.5, 0.615, 0.673, 0.870 and 0.94  << OLE Object: Picture (Metafile) >> ). The single-scattering albedo ( << OLE Object: Microsoft Equation 3.0 >> ) is typically estimated from the MFRSR measurements by assuming the asymmetry parameter ( << OLE Object: Microsoft Equation 3.0 >> ). In most instances, however, it is not easy to set an appropriate value of << OLE Object: Microsoft Equation 3.0 >> due to its strong temporal and spatial variability. Here, we introduce and validate an updated version of our retrieval technique that allows one to estimate simultaneously << OLE Object: Microsoft Equation 3.0 >> and << OLE Object: Microsoft Equation 3.0 >> for different types of aerosol. We use the aerosol and radiative properties obtained during the Atmospheric Science Program (ARM) Aerosol Intensive Operational Period (IOP) to validate our retrieval in two ways. First, the MFRSR-retrieved optical properties are compared with those obtained from independent surface, Aerosol Robotic Network (AERONET) and aircraft measurements. The MFRSR-retrieved optical properties are in reasonable agreement with these independent measurements. Second, we perform radiative closure experiments using the MFRSR-retrieved optical properties. The calculated broadband values of the direct and diffuse fluxes are comparable (~ 5 << OLE Object: Microsoft Equation 3.0 >> ) to those obtained from measurements.

  1. Retrieval of Aerosol Parameters from Continuous H24 Lidar-Ceilometer Measurements

    NASA Astrophysics Data System (ADS)

    Dionisi, D.; Barnaba, F.; Costabile, F.; Di Liberto, L.; Gobbi, G. P.; Wille, H.

    2016-06-01

    Ceilometer technology is increasingly applied to the monitoring and the characterization of tropospheric aerosols. In this work, a method to estimate some key aerosol parameters (extinction coefficient, surface area concentration and volume concentration) from ceilometer measurements is presented. A numerical model has been set up to derive a mean functional relationships between backscatter and the above mentioned parameters based on a large set of simulated aerosol optical properties. A good agreement was found between the modeled backscatter and extinction coefficients and the ones measured by the EARLINET Raman lidars. The developed methodology has then been applied to the measurements acquired by a prototype Polarization Lidar-Ceilometer (PLC). This PLC instrument was developed within the EC- LIFE+ project "DIAPASON" as an upgrade of the commercial, single-channel Jenoptik CHM15k system. The PLC run continuously (h24) close to Rome (Italy) for a whole year (2013-2014). Retrievals of the aerosol backscatter coefficient at 1064 nm and of the relevant aerosol properties were performed using the proposed methodology. This information, coupled to some key aerosol type identification made possible by the depolarization channel, allowed a year-round characterization of the aerosol field at this site. Examples are given to show how this technology coupled to appropriate data inversion methods is potentially useful in the operational monitoring of parameters of air quality and meteorological interest.

  2. Aerosol measurements at a high-elevation site: composition, size, and cloud condensation nuclei activity

    SciTech Connect

    Friedman, Beth; Zelenyuk, Alla; Beranek, Josef; Kulkarni, Gourihar R.; Pekour, Mikhail S.; Hallar, Anna G.; McCubbin, Ian; Thornton, Joel A.; Cziczo, D. J.

    2013-12-09

    We present measurements of CCN concentrations and associated aerosol composition and size properties at a high-elevation research site in March 2011. CCN closure and aerosol hygroscopicity were assessed using simplified assumptions of bulk aerosol properties as well as a new method utilizing single particle composition and size to assess the importance of particle mixing state in CCN activation. Free troposphere analysis found no significant difference between the CCN activity of free tropospheric aerosol and boundary layer aerosol at this location. Closure results indicate that using only size and number information leads to adequate prediction, in the majority of cases within 50%, of CCN concentrations, while incorporating the hygroscopicity parameters of the individual aerosol components measured by single particle mass spectrometry adds to the agreement, in most cases within 20%, between predicted and measured CCN concentrations. For high-elevation continental sites, with largely aged aerosol and low amounts of local area emissions, a lack of chemical knowledge and hygroscopicity may not hinder models in predicting CCN concentrations. At sites influenced by fresh emissions or more heterogeneous particle types, single particle composition information may be more useful in predicting CCN concentrations and understanding the importance of particle mixing state on CCN activation.

  3. Ambient Observations of Sub-1.0 Hygroscopic Growth Factor and f(RH) Values: Case Studies from Surface and Airborne Measurements

    NASA Astrophysics Data System (ADS)

    Ortega, A. M.; Shingler, T.; Crosbie, E.; Wonaschutz, A.; Froyd, K. D.; Adler, G.; Gao, R. S.; Schwarz, J. P.; Perring, A. E.; Brock, C. A.; Beyersdorf, A. J.; Ziemba, L. D.; Jimenez, J. L.; Campuzano Jost, P.; Wisthaler, A.; Sorooshian, A.

    2015-12-01

    Hygroscopic growth occurs when particles take up water vapor and grow when exposed to elevated relative humidity (RH), and is controlled largely by chemical composition. Previous laboratory studies of biomass burning and combustion particles observed particle size shrinkage as soot aerosols, especially those with coatings, were exposed to increasing RH levels, which resulted in sub-1.0 hygroscopicity parameter values (i.e., ratio of humidified-to-dry diameter g(RH) and ratio of humidified-to-dry scattering coefficients f(RH)). To investigate the potential for sub-1.0 hygroscopicity in ambient aerosol, we utilized data from (i) a ship-board HTDMA during E-PEACE 2011, (ii) multiple instruments on the DC8 during SEAC4RS-2013, as well as (iii) the DASH-SP during measurement intensives in Summer 2014 and Winter 2015 in Tucson, Arizona. Suppressed hygroscopicity, including sub-1.0 g(RH), was observed during smoke-influenced periods in SEAC4RS, episodic events in the winter season in Arizona, and smoke-influenced air during E-PEACE. Across the range of RH investigated (75-95%), sub-1.0 g(RH) was lowest at the highest RH values probed (~95%). These sub-1.0 g(RH) observations are consistent with elevated black carbon and organic aerosol concentration in both E-PEACE and SEAC4RS. Collocated measurements during SEAC4RS indicate elevated spikes in black carbon concentrations are coincident with both sub-1.0 f(RH) and g(RH) observations, as well as elevated organic aerosol- and gas-phase fire tracers such as AMS f60 and PTR-MS acetonitrile concentration. This is the first set of ambient observations of sub-1.0 hygroscopicity factors g(RH) and f(RH), with consistency across different instruments, regions, and platforms. Although particle restructuring has been demonstrated in laboratory experiments, field observations are complex as soot coating, secondary chemistry, and heterogeneous processing can occur on the same time scale as measurements. This work motivates continued

  4. A Multi-Parameter Aerosol Classification Method and its Application to Retrievals from Spaceborne Polarimetry

    NASA Astrophysics Data System (ADS)

    Russell, P. B.; Kacenelenbogen, M. S.; Livingston, J. M.; Hasekamp, O. P.; Burton, S. P.; Schuster, G. L.; Johnson, M. S.; Knobelspiesse, K. D.; Redemann, J.; Ramachandran, S.; Holben, B. N.

    2014-12-01

    Classifying observed aerosols into types (e.g., urban-industrial, biomass burning, mineral dust, maritime) helps to understand aerosol sources, transformations, effects, and feedback mechanisms; to improve accuracy of satellite retrievals; and to quantify aerosol radiative impacts on climate. The number of aerosol parameters retrieved from spaceborne sensors has been growing, from the initial aerosol optical depth (AOD) at one or a few wavelengths to a list that now includes AOD, complex refractive index, single scattering albedo (SSA), and depolarization of backscatter, each at several wavelengths, plus several particle size and shape parameters. Making optimal use of these varied data products requires objective, multi-dimensional analysis methods. We describe such a method, which makes explicit use of uncertainties in input parameters. It treats an N-parameter retrieved data point and its N-dimensional uncertainty as an extended data point, E. It then uses a modified Mahalanobis distance, DEC, to assign an observation to the class (cluster) C that has minimum DEC from the point. We use parameters retrieved from the Aerosol Robotic Network (AERONET) to define seven prespecified clusters (pure dust, polluted dust, urban-industrial/developed economy, urban-industrial/developing economy, dark biomass smoke, light biomass smoke, pure marine), and we demonstrate application of the method to a 5-year record of retrievals from the spaceborne POLDER-3 (Polarization and Directionality of the Earth's Reflectances) polarimeter over the island of Crete, Greece. Results show changes of aerosol type at this location in the eastern Mediterranean Sea, which is influenced by a wide variety of aerosol sources.

  5. Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions

    SciTech Connect

    Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, E.; Lohmann, U.; Baltensperger, Urs; Cziczo, Daniel J.

    2009-11-01

    Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of particular interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation with respect to liquid water similar to atmospheric conditions. In this study the sub-saturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols was determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were used. Aerosols were generated both with a wet and a dry disperser and the water uptake was parameterized via the hygroscopicity parameter, κ. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived κ values between 0.00 and 0.02. The latter value can be idealized as a particle consisting of 96.7% (by volume) insoluble material and ~3.3% ammonium sulfate. Pure clay aerosols were found to be generally less hygroscopic than real desert dust particles. All illite and montmorillonite samples had κ~0.003, kaolinites were least hygroscopic and had κ=0.001. SD (κ=0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (κ=0.007) and ATD (κ=0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles while immersed in an aqueous medium during atomization, thus indicating that specification of the generation method is critically important when presenting such data. Any atmospheric processing of

  6. Retrieval of aerosol parameters from the oxygen A band in the presence of chlorophyll fluorescence

    NASA Astrophysics Data System (ADS)

    Sanders, A. F. J.; de Haan, J. F.

    2013-10-01

    We have investigated the precision of retrieved aerosol parameters for a generic aerosol retrieval algorithm over vegetated land using the O2 A band. Chlorophyll fluorescence is taken into account in the forward model. Fluorescence emissions are modeled as isotropic contributions to the upwelling radiance field at the surface and they are retrieved along with aerosol parameters. Precision is calculated by propagating measurement errors and a priori errors, including model parameter errors, using the forward model's derivatives. Measurement errors consist of noise and calibration errors. The model parameter errors considered are related to the single scattering albedo, surface pressure and temperature profile. We assume that measurement noise is dominated by shot noise; thus, results apply to grating spectrometers in particular. We describe precision for various atmospheric states, observation geometries and spectral resolutions of the instrument in a number of retrieval simulations. These precision levels can be compared with user requirements. A comparison of precision estimates with the literature and an analysis of the dependence on the a priori error in the fluorescence emission indicate that aerosol parameters can be retrieved in the presence of chlorophyll fluorescence: if fluorescence is present, fluorescence emissions should be included in the state vector to avoid biases in retrieved aerosol parameters.

  7. Measurement of the Hygroscopicity and Wet Removal of Black-Carbon-Containing Particles in the Urban Atmosphere of Tokyo

    NASA Astrophysics Data System (ADS)

    Ohata, Sho; Moteki, Nobuhiro; Mori, Tatsuhiro; Koike, Makoto; Schwarz, Joshua; Takami, Akinori; Kondo, Yutaka

    2015-04-01

    Megacities are very large, concentrated anthropogenic sources of black carbon (BC) aerosols. Freshly emitted BC particles inside megacities affect local air quality and regional and global climate. The microphysical properties (e.g., number size distribution, coating thickness, and hygroscopicity) of atmospheric BC-containing particles are important because their efficiency of wet removal from the atmosphere can be highly dependent on these properties. In this study, we developed a method for independent measurement of the hygroscopicity of BC-free and BC-containing particles, and then applied it to the ambient observation in the urban atmosphere of Tokyo. A single particle soot photometer (SP2) was modified as a humidified-SP2, which quantifies the BC-core mass (BC content within a BC-containing particle) and optical diameter of individual aerosol particles, under controlled relative humidity (RH), by detecting both the laser-induced incandescence emitted and laser light scattered from each particle (Schwarz et al., 2014, Journal of Aerosol Science). Measurements of growth factor (GF) and hygroscopicity parameter κ for BC-free and BC-containing particles can be achieved by combining an aerosol particle mass analyzer with the newly developed humidified-SP2. This method was tested in the laboratory and then employed in ambient observations in summer 2014. The ambient measurements were made while also measuring number size distribution of BC cores in rainwater with a nebulizer-SP2 system. Throughout the observation period, for BC-containing particles with a dry diameter of about 200 nm, the particles with smaller BC fractions tended to represent greater water uptake, and the number fraction of the less hygroscopic (GF < 1.2 at 85% RH) BC-containing particles was more than 70% of the total BC-containing particles. The measured average number size distribution of BC cores in rainwater was larger than that in the surface air before precipitation began, and the

  8. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-12-01

    Organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments; however their hygroscopic properties remain uncharacterised. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesised and used for simultaneous measurements with a hygroscopicity tandem differential mobility analyser (H-TDMA) and a cloud condensation nuclei counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry diameter for all chemical compositions investigated, indicating that κH-TDMA depends on particle diameter and/or surface effects; however, it is not clear if this trend is statistically significant. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical particle diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w / w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ

  9. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Raatikainen, T.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2015-06-01

    Even though organosulfates have been observed as constituents of atmospheric aerosols in a wide range of environments spanning from the subtropics to the high Arctic, their hygroscopic properties have not been investigated prior to this study. Here, limonene-derived organosulfates with a molecular weight of 250 Da (L-OS 250) were synthesized and used for simultaneous measurements with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Cloud Condensation Nuclei Counter (CCNC) to determine the hygroscopicity parameter, κ, for pure L-OS 250 and mixtures of L-OS 250 with ammonium sulfate (AS) over a wide range of humidity conditions. The κ values derived from measurements with H-TDMA decreased with increasing particle dry size for all chemical compositions investigated, indicating size dependency and/or surface effects. For pure L-OS 250, κ was found to increase with increasing relative humidity, indicating dilution/solubility effects to be significant. Discrepancies in κ between the sub- and supersaturated measurements were observed for L-OS 250, whereas κ of AS and mixed L-OS 250/AS were similar. This discrepancy was primarily ascribed to limited dissolution of L-OS 250 at subsaturated conditions. In general, hygroscopic growth factor, critical activation diameter and κ for the mixed L-OS 250/AS particles converged towards the values of pure AS for mixtures with ≥ 20 % w/w AS. Surface tension measurements of bulk aqueous L-OS 250/AS solutions showed that L-OS 250 was indeed surface active, as expected from its molecular structure, decreasing the surface tension of solutions with 24 % from the pure water-value at a L-OS 250 concentration of 0.0025 mol L-1. Based on these surface tension measurements, we present the first concentration-dependent parametrisation of surface tension for aqueous L-OS 250, which was implemented to different process-level models of L-OS 250 hygroscopicity and CCN activation. The values of κ obtained from the

  10. Classification of Aerosol Retrievals from Spaceborne Polarimetry Using a Multi-Parameter Algorithm

    NASA Astrophysics Data System (ADS)

    Russell, P. B.; Kacenelenbogen, M. S.; Livingston, J. M.; Hasekamp, O.; Burton, S. P.; Schuster, G. L.; Redemann, J.; Ramachandran, S.; Holben, B. N.

    2013-12-01

    In this presentation we demonstrate application of a new aerosol classification algorithm to retrievals from the POLDER-3 polarimeter on the PARASOL spacecraft. Motivation and method: Since the development of global aerosol measurements by satellites and AERONET, classification of observed aerosols into several types (e,g., urban-industrial, biomass burning, mineral dust, maritime, and various subtypes or mixtures of these) has proven useful to: understanding aerosol sources, transformations, effects, and feedback mechanisms; improving accuracy of satellite retrievals; and quantifying assessments of aerosol radiative impacts on climate. With ongoing improvements in satellite measurement capability, the number of aerosol parameters retrieved from spaceborne sensors has been growing, from the initial aerosol optical depth at one or a few wavelengths to a list that now includes complex refractive index, single scattering albedo (SSA), and depolarization of backscatter, each at several wavelengths; wavelength dependences of extinction, scattering, absorption, SSA, and backscatter; and several particle size and shape parameters. Making optimal use of these varied data products requires objective, multi-dimensional analysis methods. We describe such a method, which uses a modified Mahalanobis distance to quantify how far a data point described by N aerosol parameters is from each of several prespecified classes. The method makes explicit use of uncertainties in input parameters, treating a point and its N-dimensional uncertainty as an extended data point or pseudo-cluster E. It then uses a modified Mahalanobis distance, DEC, to assign that observation to the class (cluster) C that has minimum DEC from the point (equivalently, the class to which the point has maximum probability of belonging). The method also uses Wilks' overall lambda to indicate how well the input data lend themselves to separation into classes and Wilks' partial lambda to indicate the relative

  11. Hygroscopic properties of volcanic ash

    NASA Astrophysics Data System (ADS)

    Lathem, T. L.; Kumar, P.; Nenes, A.; Dufek, J.; Sokolik, I. N.; Trail, M.; Russell, A.

    2011-06-01

    Limited observational data exists on the physical interactions between volcanic ash particles and water vapor; yet it is thought that these interactions can strongly impact the microphysical evolution of ash, with implications for its atmospheric lifetime and transport, as well as formation of water and ice clouds. In this study, we investigate for the first time, the hygroscopic properties of ultra-fine volcanic ash (<125 μm diameter) from the eruptions of Mt. St. Helens in 1980, El Chichón in 1982, Tungurahua in 2006, Chaitén in 2008, Mt. Redoubt in 2009, and Eyjafjallajökull in 2010. The hygroscopicity of the ash particles is quantified by their ability to uptake water and nucleate into cloud drops under controlled levels of water vapor supersaturation. Evidence presented strongly suggests that ash uptakes water efficiently via adsorption and a simple parameterization of ash hygroscopicity is developed for use in ash plume and atmospheric models.

  12. Potential of polarization lidar to provide profiles of CCN- and INP-relevant aerosol parameters

    NASA Astrophysics Data System (ADS)

    Mamouri, Rodanthi-Elisavet; Ansmann, Albert

    2016-05-01

    We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of particle number concentrations n50, dry considering dry aerosol particles with radius > 50 nm (reservoir of CCN in the case of marine and continental non-desert aerosols), n100, dry (particles with dry radius > 100 nm, reservoir of desert dust CCN), and of n250, dry (particles with dry radius > 250 nm, reservoir of favorable INP), as well as profiles of the particle surface area concentration sdry (used in INP parameterizations) can be retrieved from lidar-derived aerosol extinction coefficients σ with relative uncertainties of a factor of 1.5-2 in the case of n50, dry and n100, dry and of about 25-50 % in the case of n250, dry and sdry. Of key importance is the potential of polarization lidar to distinguish and separate the optical properties of desert aerosols from non-desert aerosol such as continental and marine particles. We investigate the relationship between σ, measured at ambient atmospheric conditions, and n50, dry for marine and continental aerosols, n100, dry for desert dust particles, and n250, dry and sdry for three aerosol types (desert, non-desert continental, marine) and for the main lidar wavelengths of 355, 532, and 1064 nm. Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple CCN parameterization (with n50, dry or n100, dry as input) and available INP parameterization schemes (with n250, dry and sdry as input) we finally compute

  13. Hygroscopic growth and droplet activation of soot particles: uncoated, succinic or sulfuric acid coated

    NASA Astrophysics Data System (ADS)

    Henning, S.; Ziese, M.; Kiselev, A.; Saathoff, H.; Möhler, O.; Mentel, T. F.; Buchholz, A.; Spindler, C.; Michaud, V.; Monier, M.; Sellegri, K.; Stratmann, F.

    2011-10-01

    The hygroscopic growth and droplet activation of uncoated soot particles and such coated with succinic acid and sulfuric acid were investigated during the IN-11 campaign at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility. A GFG-1000 soot generator applying nitrogen, respectively argon as carrier gas and a miniCAST soot generator were utilized to generate soot particles. Different organic carbon (OC) to black carbon (BC) ratios were adjusted for the CAST-soot by varying the fuel to air ratio. The hygroscopic growth was investigated by means of the mobile Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile) and two different Hygroscopicity Tandem Differential Mobility Analyzers (HTDMA, VHTDMA). Two Cloud Condensation Nucleus Counter (CCNC) were applied to measure the activation of the particles. For the untreated soot particles neither hygroscopic growth nor activation was observed, with exception of a partial activation of GFG-soot generated with argon as carrier gas. Coatings of succinic acid lead to a detectable hygroscopic growth of GFG-soot and enhanced the activated fraction of GFG- (carrier gas: argon) and CAST-soot, whereas no hygroscopic growth of the coated CAST-soot was found. Sulfuric acid coatings lead to an OC-content dependent hygroscopic growth of CAST-soot. Such a dependence was not observed for activation measurements. Coating with sulfuric acid decreased the amount of Polycyclic Aromatic Hydrocarbons (PAH), which were detected by AMS-measurements in the CAST-soot, and increased the amount of substances with lower molecular weight than the initial PAHs. We assume, that these reaction products increased the hygroscopicity of the coated particles in addition to the coating substance itself.

  14. Hygroscopic growth and droplet activation of soot particles: uncoated, succinic or sulfuric acid coated

    NASA Astrophysics Data System (ADS)

    Henning, S.; Ziese, M.; Kiselev, A.; Saathoff, H.; Möhler, O.; Mentel, T. F.; Buchholz, A.; Spindler, C.; Michaud, V.; Monier, M.; Sellegri, K.; Stratmann, F.

    2012-05-01

    The hygroscopic growth and droplet activation of uncoated soot particles and such coated with succinic acid and sulfuric acid were investigated during the IN-11 campaign at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility. A GFG-1000 soot generator applying either nitrogen or argon as carrier gas and a miniCAST soot generator were utilized to generate soot particles. Different organic carbon (OC) to black carbon (BC) ratios were adjusted for the CAST-soot by varying the fuel to air ratio. The hygroscopic growth was investigated by means of the mobile Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile) and two different Hygroscopicity Tandem Differential Mobility Analyzers (HTDMA, VHTDMA). Two Cloud Condensation Nucleus Counter (CCNC) were applied to measure the activation of the particles. For the untreated soot particles neither hygroscopic growth nor activation was observed at a supersaturation of 1%, with exception of a partial activation of GFG-soot generated with argon as carrier gas. Coatings of succinic acid lead to a detectable hygroscopic growth of GFG-soot and enhanced the activated fraction of GFG- (carrier gas: argon) and CAST-soot, whereas no hygroscopic growth of the coated CAST-soot was found. Sulfuric acid coatings led to an OC-content dependent hygroscopic growth of CAST-soot. Such a dependence was not observed for activation measurements. Coating with sulfuric acid decreased the amount of Polycyclic Aromatic Hydrocarbons (PAH), which were detected by AMS-measurements in the CAST-soot, and increased the amount of substances with lower molecular weight than the initial PAHs. We assume that these reaction products increased the hygroscopicity of the coated particles in addition to the coating substance itself.

  15. Atmospheric aerosol optical parameters, deep convective clouds and hail occurence - a correlation study

    NASA Astrophysics Data System (ADS)

    Talianu, Camelia; Andrei, Simona; Toanca, Florica; Stefan, Sabina

    2016-04-01

    Among the severe weather phenomena, whose frequency has increased during the past two decades, hail represents a major threat not only for agriculture but also for other economical fields. Generally, hail are produced in deep convective clouds, developed in an unstable environment. Recent studies have emphasized that besides the state of the atmosphere, the atmospheric composition is also very important. The presence of fine aerosols in atmosphere could have a high impact on nucleation processes, initiating the occurrence of cloud droplets, ice crystals and possibly the occurrence of graupel and/or hail. The presence of aerosols in the atmosphere, correlated with specific atmospheric conditions, could be predictors of the occurrence of hail events. The atmospheric investigation using multiwavelength Lidar systems can offer relevant information regarding the presence of aerosols, identified using their optical properties, and can distinguish between spherical and non-spherical shape, and liquid and solid phase of these aerosols. The aim of this study is to analyse the correlations between the presence and the properties of aerosols in atmosphere, and the production of hail events in a convective environment, using extensive and intensive optical parameters computed from lidar and ceilometer aerosols measurements. From these correlations, we try to evaluate if these aerosols can be taken into consideration as predictors for hail formation. The study has been carried out in Magurele - Romania (44.35N, 26.03E, 93m ASL) using two collocated remote sensing systems: a Raman Lidar (RALI) placed at the Romanian Atmospheric 3D Observatory and a ceilometer CL31 placed at the nearby Faculty of Physics, University of Bucharest. To evaluate the atmospheric conditions, radio sounding and satellite images were used. The period analysed was May 1st - July 15th, 2015, as the May - July period is climatologically favorable for deep convection events. Two hail events have been

  16. Variability of CCN Activation Behaviour of Aerosol Particles in the Marine Boundary Layer of the Northern and Southern Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Henning, Silvia; Dieckmann, Katrin; Hartmann, Susan; Schäfer, Michael; Wu, Zhijun; Merkel, Maik; Wiedensohler, Alfred; Stratmann, Frank

    2013-04-01

    The variability of cloud condensation nucleus (CCN) activation behaviour and total CCN number concentrations was investigated during three ship cruises. Measurements were performed in a mobile laboratory on the German research vessel FS Polarstern cruising between Cape Town and Bremerhaven (April / May and October / November 2011) as well as between Punta Arenas and Bremerhaven (April / May 2012). CCN size distributions were measured for supersaturations between 0.1% and 0.4% using a Cloud Condensation Nucleus Counter (DMT, USA). Aerosol particle and CCN total number concentrations as well as the hygroscopicity parameter κ (Petters and Kreidenweis, 2007) were determined. Furthermore, size distribution data were collected. The hygroscopicity parameter κ featured a high variability during the cruises, with a median κ-value of 0.52 ± 0.26. The κ-values are depended on air mass origin; and are as expected mainly dominated by marine influences, but also long range transport of aerosol particles was detected. In the Celtic Sea, κ was found to be lower than that of clean marine aerosol particles (0.72 ± 0.24; Pringle et al., 2010) with κ-values ~0.2, possibly influenced by anthropogenic emissions from Europe. Close to the West African coast particle hygroscopicity was found to be influenced by the Saharan dust plume, resulting in low κ-values ~0.25. Petters, M.D. and S.M. Kreidenweis (2007), A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. and Phys., 7, 1961-1971. Pringle, K.J., H. Tost, A. Pozzer, U. Pöschl, and J. Lelieveld (2010), Global distribution of the effective aerosol hygroscopicity parameter for CCN activation, Atmos. Chem. Phys., 10, 5241-5255.

  17. USE OF CONTINUOUS MEASUREMENTS OF INTEGRAL AEROSOL PARAMETERS TO ESTIMATE PARTICLE SURFACE AREA

    EPA Science Inventory

    This study was undertaken because of interest in using particle surface area as an indicator for studies of the health effects of particulate matter. First, we wished to determine the integral parameter of the size distribution measured by the electrical aerosol detector. Secon...

  18. The influence of fog parameters on aerosol depletion measured in the KAEVER experiments

    SciTech Connect

    Poss, G.; Weber, D.; Fritsche, B.

    1995-12-31

    The release of radioactive aerosols in the environment is one of the most serious hazards in case of an accident in nuclear power plant. Many efforts have been made in the past in numerous experimental programs like NSPP, DEMONA, VANAM, LACE, MARVIKEN, others are still underway to improve the knowledge of the aerosol behavior and depletion in a reactor containment in order to estimate the possible source term and to validate computer codes. In the German single compartment KAEVER facility the influence of size distribution, morphology, composition and solubility on the aerosol behavior is investigated. One of the more specific items is to learn about {open_quotes}wet depletion{close_quotes} means, the aerosol depletion behavior in condensing atmospheres. There are no experiments known where the fog parameters like droplet size distribution, volume concentration, respectively airborne liquid water content have been measured in- and on-line explicitly. To the authors knowledge the use of the Battelle FASP photometer, which was developed especially for this reason, for the first time gives insight in condensation behavior under accident typical thermal hydraulic conditions. It delivers a basis for code validation in terms of a real comparison of measurements and calculations. The paper presents results from {open_quotes}wet depletion{close_quotes} aerosol experiments demonstrating how depletion velocity depends on the fog parameters and where obviously critical fog parameter seem to change the regime from a {open_quotes}pseudo dry depletion{close_quotes} at a relative humidity of 100% but quasi no or very low airborne liquid water content to a real {open_quotes}wet depletion{close_quotes} under the presence of fogs with varying densities. Characteristics are outlined how soluble and insoluble particles as well as aerosol mixtures behave under condensing conditions.

  19. Remote Sensing of Aerosol and Marine Parameters in Coastal Environments Using Polarized RT Simulations to Analyze OLCI Measurements

    NASA Astrophysics Data System (ADS)

    Stamnes, Knut; Stamnes, Snorre; Li, Wei; Fan, Yongzhen; Chen, Nan; Tanikawa, Tomo; Stamnes, Jakob J.

    2015-12-01

    A study was conducted to investigate whether imager-type spectroradiometer instruments like MODIS, currently flying on board the Aqua and Terra satellites, or MERIS, which flew on board Envisat, or OLCI, to be flown on board Sentinel 3, could detect absorbing aerosols if they could measure the Q Stokes parameter in addition to the total radiance I . Accurate radiative transfer calculations to produce synthetic data together with an optimal estimation inversion scheme was used to retrieve 3 aerosol parameters: aerosol optical depth, fraction of absorbing aerosols, and aerosol location. It was found that knowledge of I was generally insufficient to retrieve all 3 aerosol parameters, whereas knowledge of I and Q made it possible.

  20. DEPOSITION OF SULFATE ACID AEROSOLS IN THE DEVELOPING HUMAN LUNG

    EPA Science Inventory

    Computations of aerosol deposition as affected by (i) aerosol hygroscopicity, (ii) human age, and (iii) respiratory intensity are accomplished using a validated mathematical model. he interactive effects are very complicated but systematic. ew general observations can be made; ra...

  1. Long-term (2001-2012) observation of the modeled hygroscopic growth factor of remote marine TSP aerosols over the western North Pacific: impact of long-range transport of pollutants and their mixing states.

    PubMed

    Boreddy, S K R; Kawamura, Kimitaka; Haque, Md Mozammel

    2015-11-21

    In order to assess the seasonal and annual variability of long-range transported anthropogenic pollutants from East Asia and their effect on the hygroscopicity and precipitation process over the western North Pacific, we conducted long-term calculations of bulk hygroscopicity, g(90%)ZSR, based on the ZSR model using chemical composition data from 2001-2012 at Chichijima Island. We found that sea-salts (Na(+) and Cl(-)) are the major mass fraction (65%) of the total water-soluble matter followed by SO4(2-) (20%) and WSOM (6%). The seasonal variation of g(90%)ZSR was high in summer to autumn and low in winter to spring months, probably due to the influence of the long-range transport of anthropogenic SO4(2-), dust, and organics from East Asia and their interaction with sea-salts through heterogeneous reactions. On the other hand, annual variations of g(90%)ZSR showed a decrease from 2001 to 2006 and then an increase from 2007 to 2012. Interestingly, the annual variations in SO4(2-) mass fractions showed an increase from 2001 to 2006 and then a decrease from 2007 to 2012, demonstrating that SO4(2-) seriously suppresses the hygroscopic growth of sea-salt particles over the western North Pacific. This is further supported by the strong negative correlation between SO4(2-) and g(90%)ZSR. Based on the MODIS satellite data, the present study demonstrates that long-range transported anthropogenic pollutants from East Asia to the North Pacific can act as efficient cloud condensation nuclei but significantly suppress the precipitation by reducing the size of cloud droplets over the western North Pacific. PMID:26473178

  2. A novel technique for estimating aerosol optical thickness trends using meteorological parameters

    NASA Astrophysics Data System (ADS)

    Emetere, Moses E.; Akinyemi, M. L.; Akin-Ojo, O.

    2016-02-01

    Estimating aerosol optical thickness (AOT) over regions can be tasking if satellite data set over such region is very scanty. Therefore a technique whose application captures real-time events is most appropriate for adequate monitoring of risk indicators. A new technique i.e. arithmetic translation of pictorial model (ATOPM) was developed. The ATOPM deals with the use mathematical expression to compute other meteorological parameters obtained from satellite or ground data set. Six locations within 335 × 230 Km2 area of a selected portion of Nigeria were chosen and analyzed -using the meteorological data set (1999-2012) and MATLAB. The research affirms the use of some parameters (e.g. minimum temperature, cloud cover, relative humidity and rainfall) to estimate the aerosol optical thickness. The objective of the paper was satisfied via the use of other meteorological parameters to estimate AOT when the satellite data set over an area is scanty.

  3. MELCOR 1. 8. 1 assessment: LACE aerosol experiment LA4

    SciTech Connect

    Kmetyk, L.N.

    1991-09-01

    The MELCOR code has been used to simulate LACE aerosol experiment LA4. In this test, the behavior of single- and double-component, hygroscopic and nonhygroscopic, aerosols in a condensing environment was monitored. Results are compared to experimental data, and to CONTAIN calculations. Sensitivity studies have been done on time step effects and machine dependencies; thermal/hydraulic parameters such as condensation on heat structures and on pool surface, and radiation heat transfer; and aerosol parameters such as number of MAEROS components and sections assumed, the degree to which plated aerosols are washed off heat structures by condensate film draining, and the effect of non-default values for shape factors and diameter limits. 9 refs., 50 figs., 13 tabs.

  4. Comparison of one-parameter and two-parameter models of aerosol extinction for experimental data of the arid zone of Kazakhstan

    NASA Astrophysics Data System (ADS)

    Shchelkanov, N. N.

    2015-11-01

    Comparison of four aerosol models is carried out: two one-parameter models for a ground layer of the arid zone of Kazakhstan, two-parameter model for horizontal paths and two-parameter model for horizontal and slant paths. It is shown that the models obtained using the new methods for construction of linear regression and separation of the components allow physically correct retrieval of not only the values of the aerosol extinction coefficients, but also their root mean square deviations.

  5. Simulation of the interannual variations of aerosols in China: role of variations in meteorological parameters

    NASA Astrophysics Data System (ADS)

    Mu, Q.; Liao, H.

    2014-09-01

    We used the nested grid version of the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to examine the interannual variations (IAVs) of aerosols over heavily polluted regions in China for years 2004-2012. The role of variations in meteorological parameters was quantified by a simulation with fixed anthropogenic emissions at year 2006 levels and changes in meteorological parameters over 2004-2012. Simulated PM2.5 (particles with a diameter of 2.5 μm or less) aerosol concentrations exhibited large IAVs in North China (NC; 32-42° N, 110-120° E), with regionally averaged absolute percent departure from the mean (APDM) values of 17, 14, 14, and 11% in December-January-February (DJF), March-April-May (MAM), June-July-August (JJA), and September-October-November (SON), respectively. Over South China (SC; 22-32° N, 110-120° E), the IAVs in PM2.5 were found to be the largest in JJA, with the regional mean APDM values of 14% in JJA and of about 9% in other seasons. The concentrations of PM2.5 over the Sichuan Basin (SCB; 27-33° N, 102-110° E) were simulated to have the smallest IAVs among the polluted regions examined in this work, with APDM values of 8-9% in all seasons. All aerosol species (sulfate, nitrate, ammonium, black carbon, and organic carbon) were simulated to have the largest IAVs over NC in DJF, corresponding to the large variations in meteorological parameters over NC in this season. Process analyses were performed to identify the key meteorological parameters that determined the IAVs of different aerosol species in different regions. While the variations in temperature and specific humidity, which influenced the gas-phase formation of sulfate, jointly determined the IAVs of sulfate over NC in both DJF and JJA, wind (or convergence of wind) in DJF and precipitation in JJA were the dominant meteorological factors to influence IAVs of sulfate over SC and the SCB. The IAVs in temperature and specific humidity

  6. THERMOPHORESIS AND ITS THERMAL PARAMETERS FOR AEROSOL COLLECTION

    SciTech Connect

    Huang, Z.; Apte, M.; Gundel, L.

    2007-01-01

    The particle collection effi ciency of a prototype environmental tobacco smoke (ETS) sampler based on the use of thermophoresis is determined by optimizing the operational voltage that determines its thermal gradient. This sampler’s heating element was made of three sets of thermophoretic (TP) wires 25μm in diameter suspended across a channel cut in a printed circuit board and mounted with collection surfaces on both sides. The separation between the heating element and the room temperature collection surface was determined in a numerical simulation based on the Brock-Talbot model. Other thermal parameters of this TP ETS sampler were predicted by the Brock-Talbot model for TP deposition. From the normalized results the optimal collection ratio was expressed in terms of operational voltage and fi lter mass. Prior to the Brock-Talbot model simulation for this sampler, 1.0V was used arbitrarily. The operational voltage was raised to 3.0V, and the collection effi ciency was increased by a factor of fi ve for both theory and experiment.

  7. Thermophoresis and Its Thermal Parameters for Aerosol Collection

    SciTech Connect

    Huang, Z.; Apte, Michael; Gundel, Lara

    2007-08-01

    The particle collection efficiency of a prototype environmental tobacco smoke (ETS) sampler based on the use of thermophoresis is determined by optimizing the operational voltage that determines its thermal gradient. This sampler's heating element was made of three sets of thermophoretic (TP) wires 25mu m in diameter suspended across a channel cut in a printed circuit board and mounted with collection surfaces on both sides. The separation between the heating element and the room temperature collection surface was determined in a numerical simulation based on the Brock-Talbot model. Other thermal parameters of this TP ETS sampler were predicted by the Brock-Talbot model for TP deposition. From the normalized results the optimal collection ratio was expressed in terms of operational voltage and fi lter mass. Prior to the Brock-Talbot model simulation for this sampler, 1.0V was used arbitrarily. The operational voltage was raised to 3.0V, and the collection effi ciency was increased by a factor of fi ve for both theory and experiment.

  8. The single scattering properties of hygroscopic soot aggregates with water coated monomers

    NASA Astrophysics Data System (ADS)

    YU, W.; Tianhai, C.; Hao, C.; Lijuan, Z.

    2013-12-01

    Anthropogenic aerosols, such as soot, have modified the Earth's radiation balance by scattering and absorbing solar and long-wave radiative transmission, which have largely influenced the global climate change since the industrial era. Based on transmission electron microscope images (TEM), soot particles are shown as the complex, fractal-like aggregate structures. In humid atmospheric environments, these soot aggregates tend to acquire a water coating, which introduces further complexity to the problem of determining the optical properties of the aggregates. The hygroscopic growth of soot aggregates is important for the aging of these absorbing aerosols, which can significantly influence the optical properties of these kinds of soot particles. In this paper, according to the specific volume fractions of soot core in the water coated soot particle, the monomers of fractal soot aggregates are modeled as semi-external mixtures (physical contact) with constant radius of soot core and variable size of water coating. The single scattering properties of these hygroscopic soot particles, such as phase function, the cross sections of extinction, absorption and scatting, single scattering albedo (SSA), and asymmetry parameter (ASY), are calculated using the numerically exact superposition T-matrix method. The morphological effects are compared with different monomer numbers and fractal dimension of the soot aggregates, as well as different size of water coating for these spherical monomers. The results have shown that the extinction and absorption cross sections are decreased for the soot aggregates with more thick water coating on monomers, but the single scattering albedo is increased for the larger water coating. It is found that the SSA of aged soot aggregates with hygroscopic grown are remarkably (~50% for volume fraction of soot aggregates is 0.5) larger than fresh soot particles without the consideration of water coating, due to the size of water coating and the

  9. Microscopy and Spectroscopy Techniques to Guide Parameters for Modeling Mineral Dust Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Veghte, D. P.; Moore, J. E.; Jensen, L.; Freedman, M. A.

    2013-12-01

    Mineral dust aerosol particles are the second largest emission by mass into the atmosphere and contribute to the largest uncertainty in radiative forcing. Due to the variation in size, composition, and shape, caused by physical and chemical processing, uncertainty exists as to whether mineral dust causes a net warming or cooling effect. We have used Cavity Ring-Down Aerosol Extinction Spectroscopy (CRD-AES), Scanning Electron Microscopy (SEM), and Transmission Electron Microscopy (TEM) to measure extinction cross sections and morphologies of size-selected, non-absorbing and absorbing mineral dust aerosol particles. We have found that microscopy is essential for characterizing the polydispersity of the size selection of non-spherical particles. Through the combined use of CRD-AES, microscopy, and computation (Mie theory and Discreet Dipole Approximation), we have determined the effect of shape on the optical properties of additional species including clay minerals, quartz, and hematite in the sub-micron regime. Our results have shown that calcite can be treated as polydisperse spheres while quartz and hematite need additional modeling parameters to account for their irregularity. Size selection of clay minerals cannot be performed due to their irregular shape, but microscopy techniques can be used to better quantify the particle aspect ratio. Our results demonstrate a new method that can be used to extend cavity ring-down spectroscopy for the measurement of the optical properties of non-spherical particles. This characterization will lead to better aerosol extinction parameters for modeling aerosol optical properties in climate models and satellite retrieval algorithms.

  10. Aerosol and Surface Parameter Retrievals for a Multi-Angle, Multiband Spectrometer

    NASA Technical Reports Server (NTRS)

    Broderick, Daniel

    2012-01-01

    This software retrieves the surface and atmosphere parameters of multi-angle, multiband spectra. The synthetic spectra are generated by applying the modified Rahman-Pinty-Verstraete Bidirectional Reflectance Distribution Function (BRDF) model, and a single-scattering dominated atmosphere model to surface reflectance data from Multiangle Imaging SpectroRadiometer (MISR). The aerosol physical model uses a single scattering approximation using Rayleigh scattering molecules, and Henyey-Greenstein aerosols. The surface and atmosphere parameters of the models are retrieved using the Lavenberg-Marquardt algorithm. The software can retrieve the surface and atmosphere parameters with two different scales. The surface parameters are retrieved pixel-by-pixel while the atmosphere parameters are retrieved for a group of pixels where the same atmosphere model parameters are applied. This two-scale approach allows one to select the natural scale of the atmosphere properties relative to surface properties. The software also takes advantage of an intelligent initial condition given by the solution of the neighbor pixels.

  11. CCN activation and efficiency of nucleation and impaction removal process of biomass burning aerosols in Brazil: preliminary results.

    NASA Astrophysics Data System (ADS)

    Sánchez Gácita, Madeleine; Longo, Karla M.; Freitas, Saulo R.; Martin, Scot T.

    2015-04-01

    The biomass burning activity constitutes an important source of aerosols and trace gases to the atmosphere globally. In South America, during the dry season, aerosols prevenient from biomass burning are typically transported to long distances from its sources before being removed though contributing significantly to the aerosol budget on a continental scale. The uncertainties in the magnitude of the impacts on the hydrological cycle, the radiation budget and the biogeochemical cycles on a continental scale are still noteworthy. The still unknowns on the efficiency of biomass burning aerosol to act as cloud condensation nuclei (CCN) and the effectiveness of the nucleation and impaction scavenging mechanisms in removing them from the atmosphere contribute to such uncertainties. In the present work, the explicit modelling of the early stages of cloud development using a parcel model for the typical conditions of the dry season and dry-to-wet transition periods in Amazonia allowed an estimation of the efficiency of nucleation scavenging process and the ability of South American biomass burning aerosol to act as CCN. Additionally, the impaction scavenging was simulated for the same aerosol population following a method based on the widely used concept of the efficiency of collision between a raindrop and an aerosol particle. DMPS and H-TDMA data available in the literature for biomass burning aerosol population in the region indicated the presence of a nearly hydrophobic fraction (on average, with specific hygroscopic parameter κ=0.04, and relative abundance of 73 %) and nearly hygroscopic fraction (κ=0.13, 27 %), externally mixed. The hygroscopic parameters and relative abundances of each hygroscopic group, as well as the weighted average specific hygroscopic parameter for the entire population κ=0.06, were used in calculations of aerosol activation and population mass and number concentration scavenged by nucleation. Results from both groups of simulations are

  12. Hygroscopicity Evaluation of Halide Scintillators

    SciTech Connect

    Zhuravleva, M; Stand, L; Wei, H; Hobbs, C. L.; Boatner, Lynn A; Ramey, Joanne Oxendine; Burger, Arnold; Rowe, E; Bhattacharya, P.; Tupitsyn, E; Melcher, Charles L

    2014-01-01

    A collaborative study of relative hygroscopicity of anhydrous halide scintillators grown at various laboratories is presented. We have developed a technique to evaluate moisture sensitivity of both raw materials and grown crystals, in which the moisture absorption rate is measured using a gravimetric analysis. Degradation of the scintillation performance was investigated by recording gamma-ray spectra and monitoring the photopeak position, count rate and energy resolution. The accompanying physical degradation of the samples exposed to ambient atmosphere was photographically recorded as well. The results were compared with ben

  13. Hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Wu, Z. J.; Nowak, A.; Poulain, L.; Herrmann, H.; Wiedensohler, A.

    2011-12-01

    The hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their effects on ammonium sulfate were investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA). No hygroscopic growth is observed for disodium oxalate, while ammonium oxalate shows slight growth (growth factor = 1.05 at 90%). The growth factors at 90% RH for sodium acetate, disodium malonate, disodium succinate, disodium tartrate, diammonium tartrate, sodium pyruvate, disodium maleate, and humic acid sodium salt are 1.79, 1.78, 1.69, 1.54, 1.29, 1.70, 1.78, and 1.19, respectively. The hygroscopic growth of mixtures of organic salts with ammonium sulfate, which are prepared as surrogates of atmospheric aerosols, was determined. A clear shift in deliquescence relative humidity to lower RH with increasing organic mass fraction was observed for these mixtures. Above 80% RH, the contribution to water uptake by the organic salts was close to that of ammonium sulfate for the majority of investigated compounds. The observed hygroscopic growth of the mixed particles at RH above the deliquescence relative humidity of ammonium sulfate agreed well with that predicted using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule. Mixtures of ammonium sulfate with organic salts are more hygroscopic than mixtures with organic acids, indicating that neutralization by gas-phase ammonia and/or association with cations of dicarbonxylic acids may enhance the hygroscopicity of the atmospheric particles.

  14. Emulation of a complex global aerosol model to quantify sensitivity to uncertain parameters

    NASA Astrophysics Data System (ADS)

    Lee, L. A.; Carslaw, K. S.; Pringle, K. J.; Mann, G. W.; Spracklen, D. V.

    2011-12-01

    Sensitivity analysis of atmospheric models is necessary to identify the processes that lead to uncertainty in model predictions, to help understand model diversity through comparison of driving processes, and to prioritise research. Assessing the effect of parameter uncertainty in complex models is challenging and often limited by CPU constraints. Here we present a cost-effective application of variance-based sensitivity analysis to quantify the sensitivity of a 3-D global aerosol model to uncertain parameters. A Gaussian process emulator is used to estimate the model output across multi-dimensional parameter space, using information from a small number of model runs at points chosen using a Latin hypercube space-filling design. Gaussian process emulation is a Bayesian approach that uses information from the model runs along with some prior assumptions about the model behaviour to predict model output everywhere in the uncertainty space. We use the Gaussian process emulator to calculate the percentage of expected output variance explained by uncertainty in global aerosol model parameters and their interactions. To demonstrate the technique, we show examples of cloud condensation nuclei (CCN) sensitivity to 8 model parameters in polluted and remote marine environments as a function of altitude. In the polluted environment 95 % of the variance of CCN concentration is described by uncertainty in the 8 parameters (excluding their interaction effects) and is dominated by the uncertainty in the sulphur emissions, which explains 80 % of the variance. However, in the remote region parameter interaction effects become important, accounting for up to 40 % of the total variance. Some parameters are shown to have a negligible individual effect but a substantial interaction effect. Such sensitivities would not be detected in the commonly used single parameter perturbation experiments, which would therefore underpredict total uncertainty. Gaussian process emulation is shown to

  15. Emulation of a complex global aerosol model to quantify sensitivity to uncertain parameters

    NASA Astrophysics Data System (ADS)

    Lee, L. A.; Carslaw, K. S.; Pringle, K.; Mann, G. W.; Spracklen, D. V.

    2011-07-01

    Sensitivity analysis of atmospheric models is necessary to identify the processes that lead to uncertainty in model predictions, to help understand model diversity, and to prioritise research. Assessing the effect of parameter uncertainty in complex models is challenging and often limited by CPU constraints. Here we present a cost-effective application of variance-based sensitivity analysis to quantify the sensitivity of a 3-D global aerosol model to uncertain parameters. A Gaussian process emulator is used to estimate the model output across multi-dimensional parameter space using information from a small number of model runs at points chosen using a Latin hypercube space-filling design. Gaussian process emulation is a Bayesian approach that uses information from the model runs along with some prior assumptions about the model behaviour to predict model output everywhere in the uncertainty space. We use the Gaussian process emulator to calculate the percentage of expected output variance explained by uncertainty in global aerosol model parameters and their interactions. To demonstrate the technique, we show examples of cloud condensation nuclei (CCN) sensitivity to 8 model parameters in polluted and remote marine environments as a function of altitude. In the polluted environment 95 % of the variance of CCN concentration is described by uncertainty in the 8 parameters (excluding their interaction effects) and is dominated by the uncertainty in the sulphur emissions, which explains 80 % of the variance. However, in the remote region parameter interaction effects become important, accounting for up to 40 % of the total variance. Some parameters are shown to have a negligible individual effect but a substantial interaction effect. Such sensitivities would not be detected in the commonly used single parameter perturbation experiments, which would therefore underpredict total uncertainty. Gaussian process emulation is shown to be an efficient and useful technique for

  16. Aerosol optical properties and their relationship with meteorological parameters during wintertime in Delhi, India

    NASA Astrophysics Data System (ADS)

    Tiwari, S.; Pandithurai, G.; Attri, S. D.; Srivastava, A. K.; Soni, V. K.; Bisht, D. S.; Anil Kumar, V.; Srivastava, Manoj K.

    2015-02-01

    In situ and columnar measurements of aerosol optical properties (AOPs) [Aerosol optical depth (AOD), Angstrom Exponent (AE), Aerosol scattering (σscat) and absorption (σabs) coefficients and single scattering albedo (SSA)] along with soot particles (Black carbon: BC) and fine particles (PM2.5: d ≤ 2.5) were continuously measured at an urban site in Delhi, India during winter period (December 2011 to March 2012). Average values of AOD, σscat, σabs, and SSA at 500 nm; and AE for the observation period were found to be 0.95 ± 0.32, 1027.36 ± 797.1 Mm- 1, 85.95 ± 73.2 Mm- 1 and 0.93 ± 0.03; and 0.94 ± 0.19, respectively. Higher values of σscat and σabs were occurred in the month of December (1857 and 148 Mm- 1) while relatively lower values of σscat (585 Mm- 1) and σabs (44 Mm- 1) were occurred in March and February respectively. SSA, however, was higher during January (0.94) and lower in March (0.89). The mass concentration of PM2.5 and BC were 195.34 ± 157.99 and 10.11 ± 8.83 μg m- 3 respectively during study period. Bimodal distributions were observed in σscat and σabs coefficients during 0800 and 0900 h LT (traffic rush hours) and at 2200 and 2300 h LT (low boundary layer conditions) with lower values during daytime between 1500 and 1700 h LT, respectively. The σscat peak in morning may be attributed to large emissions of aerosol in the traffic rush hours and production of secondary aerosols with increasing solar radiation and temperature. During study period, the σscat (mean) coefficient was 13% lower during daytime as compared to nighttime. An interesting feature was seen in monthly analysis of σscat in between day and nighttime which was 18% and 22% higher in December and January in nighttime however ~ 4% lower during February and March; it is due to effect of local meteorology. The impact of meteorological parameters such as wind speed (WS), wind direction (WD), visibility (VIS) and mixed layer depths (MLDs) on AOPs along with fine and

  17. Retrieval of aerosol parameters from multiwavelength lidar: investigation of the underlying inverse mathematical problem.

    PubMed

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

    2016-03-20

    We present an investigation of some important mathematical and numerical features related to the retrieval of microphysical parameters [complex refractive index, single-scattering albedo, effective radius, total number, surface area, and volume concentrations] of ambient aerosol particles using multiwavelength Raman or high-spectral-resolution lidar. Using simple examples, we prove the non-uniqueness of an inverse solution to be the major source of the retrieval difficulties. Some theoretically possible ways of partially compensating for these difficulties are offered. For instance, an increase in the variety of input data via combination of lidar and certain passive remote sensing instruments will be helpful to reduce the error of estimation of the complex refractive index. We also demonstrate a significant interference between Aitken and accumulation aerosol modes in our inversion algorithm, and confirm that the solutions can be better constrained by limiting the particle radii. Applying a combination of an analytical approach and numerical simulations, we explain the statistical behavior of the microphysical size parameters. We reveal and clarify why the total surface area concentration is consistent even in the presence of non-unique solution sets and is on average the most stable parameter to be estimated, as long as at least one extinction optical coefficient is employed. We find that for selected particle size distributions, the total surface area and volume concentrations can be quickly retrieved with fair precision using only single extinction coefficients in a simple arithmetical relationship. PMID:27140552

  18. The effects of hygroscopicity of fossil fuel BC on mixed-phase and cirrus ice clouds

    NASA Astrophysics Data System (ADS)

    Yun, Y.; Penner, J. E.

    2010-12-01

    Fossil fuel burning BC aerosols are often emitted together with sulfate, which coats the surface of these BC particles and changes their hygroscopicity. The ice forming capability of the fossil fuel burning BC can differ widely as a result of the amount of soluble coating on their surface. Due to the abundance of fossil fuel burning BC particles, a small change in their activated fraction can produce a large difference in their climate forcing. To better quantify the role of fossil fuel burning BC in climate change, a 3-BC (hydrophobic, hydrophilic and hygroscopic BC) scheme is developed to replace the 1-BC scheme in a coupled climate and aerosol transport model (CAM-IMPACT). The new scheme explicitly calculates the condensation and coagulation of sulfate on BC particles and keeps track of their coating in the 3-BC states. The hygroscopicity of BC is determined by the layers of sulfate coating on their surface according to criteria developed in laboratory observations. The ice formation scheme in mixed-phase and cirrus clouds is also updated to treat the 3 hygroscopicity BC groups separately according to their different ice freezing capabilities. This paper will report the climate forcing associated with the new BC scheme as well as comparison with observations.

  19. On the Water Uptake and CCN Activation of Tropospheric Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Rastak, Narges; Pajunoja, Aki; Acosta Navarro, Juan-Camilo; Leong, Yu Jun; Cerully, Kate M.; Nenes, Athanasios; Kirkevåg, Alf; Topping, David; Virtanen, Annele; Riipinen, Ilona

    2016-04-01

    Aerosol particles introduce high uncertainties to radiative climate forcing. If exposed to a given relative humidity (RH), aerosol particles containing soluble material can absorb water and grow in size (hygroscopic growth). If RH is increased further beyond supersaturation (RH >100%) the particles can act as cloud condensation nuclei (CCN). Aerosol particles interactions with water vapour determine to a large extent their influence on climate. Organic aerosols (OA) contribute a large fraction (20-90%) of atmospheric submicron particulate mass, on the other hand they often consist of thousands of compounds with different properties. One of these properties is solubility, which affects the hygroscopic growth and cloud condensation nucleus (CCN) activation of the organic particles. We investigate the hygroscopic behaviour of complex organic aerosols accounting for the distribution of solubilities present in these mixtures. We use the SPARC method to estimate the solubility distributions of isoprene (IP) and monoterpene (MT) SOA based on their chemical composition, as predicted by the Master Chemical Mechanism (MCM). Combining these solubility distributions with the adsorption theory along with the non-ideal behaviour of organic mixtures, we predict the expected hygroscopic growth factors (HGFs), CCN activation behaviour and the related hygroscopicity parameters kappa for these mixtures. The predictions are compared to laboratory measurements as well as field data from MT- and IP-dominated measurement sites. The predicted solubility distributions do a good job in explaining the water uptake of these two mixture types at high relative humidities (RH around 90%), as well as their CCN activation - including the potential differences between the kappa values derived from HGF vs. CCN data. At lower relative humidities, however, the observed water uptake is higher than predicted on solubility alone, particularly for the MT-derived SOA. The data from the low RHs are further

  20. Characteristics of aerosol and meteorological parameters during major dust storm events (2005 - 2010) over Beijing, China

    NASA Astrophysics Data System (ADS)

    Zheng, Sheng; Cao, Chunxiang; Singh, Ramesh

    Multi satellite sensors are capable in monitoring dust storm, its path and changes in atmospheric parameters. The present paper discusses aerosol optical properties and meteorological parameters during major dust storm events (2005-2010) over Beijing, China. The back trajectory model shows that the dust is transported from the Inner Mongolia and Mongolia to Beijing. High aerosol optical depth (AOD) and low Ångström exponent (AE) values are observed during dusty days, the average AOD (675 nm) and AE (440-870 nm) during dusty days are 2.33 and 0.06, respectively. The aerosol size distribution (ASD) in coarse mode shows a large increase in the volume during dusty days. The single scattering albedo (SSA) increases with higher wavelength on dusty days, and higher compared to non-dusty days, indicating the presence of high scattering particles due to dust storm events. Characteristics of particles during dusty and non-dusty days are also supported by the real and imaginary parts of refractive index (RI). High air pollution index (API) during dusty days represent poor air quality is a serious health hazard at the time of dust events. The CO volume mixing ratio (COVMR) from Atmospheric Infrared Sounder (AIRS) shows decrease on the ground on dusty days, while the relative humidity (RH) and H _{2}0 mass mixing ratio (H _{2}OMMR) enhance. In addition, due to the dust storm in 2005, enhanced level of water vapor (WV) using Moderate Resolution Imaging Spectroradiometer (MODIS) data is observed in and around Beijing over the dust storms track.

  1. Hygroscopic properties and cloud condensation nuclei activation of limonene-derived organosulfates and their mixtures with ammonium sulfate

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Hong, J.; Kristensen, K.; Ylisirniö, A.; Virtanen, A.; Petäjä, T.; Glasius, M.; Prisle, N. L.

    2014-12-01

    Atmospheric aerosols have the ability to act as cloud condensation nuclei (CCN), initiating the formation of clouds and hereby influencing the climate system. The ability of aerosols to act as CCN is believed to depend on particle size and chemical composition. Organosulfates (OS), e.g sulfate esters, have been observed as constituents of secondary organic aerosols in numerous atmospheric environments, even as far as the Arctic, where OS have been found to comprise 7-15% of total organic matter and 9-11% of submicron organic matter in two independent studies. However, the properties of particulate OS have not yet been investigated. Here limonene derived OS were synthesized and the hygroscopic properties of these OS and their mixtures with ammonium sulfate (AS) were examined through a series of laboratory experiments. Laboratory generated particles of limonene-derived OS and AS were analysed using a unique set-up splitting the particle flow between a Hygroscopicity Tandem Differential Mobility Analyzer and a Cloud Condensation Nuclei counter, enabling simultaneous measurements of hygroscopic growth and CCN activation. Limonene-derived OS were chosen as study components, since monoterpenes (including limonene) have been identified as important precursors of OS in field samples as well as in smog chamber experiments. AS was used as a representative of the inorganic fraction in atmospheric aerosols. The preliminary results show that limonene-derived OS exhibit weak hygroscopic growth as well as CCN activation potential, however, not as strong as AS. For the organic-inorganic mixtures, it was observed that AS dominated the hygroscopic properties over the limonene-derived OS and became dictating for the measured values of hygroscopic growth and CCN activation, when the mass fraction of AS reached 20% or above. The results will be discussed further and supplementary measurements of OS surface tension and water activity will be presented.

  2. Influence of water uptake on the aerosol particle light scattering at remote sites (Invited)

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Fierz-Schmidhauser, R.; Baltensperger, U.; Weingartner, E.

    2013-12-01

    Since ambient aerosol particles experience hygroscopic growth at enhanced relative humidity (RH), their microphysical and optical properties - especially the aerosol light scattering - are also strongly dependent on RH. The knowledge of this RH effect is of importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements because in the field aerosol in-situ measurements are often performed under dry conditions. The scattering enhancement factor f(RH,λ) is the key parameter to describe this effect of water uptake on the particle light scattering. It is defined as the particle light scattering coefficient σ(RH) at a certain RH and wavelength λ divided by its dry value. Here, we will present results from two remote sites: the Jungfraujoch located at 3580 m a.s.l. in the Swiss Alps and from Zeppelin station located at 78.5°N in the Arctic (Fierz-Schmidhauser et al., 2010; Zieger et al., 2010). Various aerosol optical and microphysical parameters were recorded at these sites using in-situ and remote sensing techniques. The scattering enhancement varied largely from very low values of f(RH=85%,λ=550 nm) around 1.28 for mineral dust transported to the Jungfraujoch to 3.41 for pristine Arctic aerosol. Compensating effects of size and hygroscopicity were observed in the Arctic, i.e. small but less hygroscopic particles eventually had the same magnitude in f(RH) as large but more hygroscopic particles like sea salt. Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f(RH). The f(RH)-values from the two remote sites will also be related to values measured at other maritime, rural, and continental sites in Europe (Zieger et al., 2013). Active and passive remote sensing techniques were used to study the vertical distribution of aerosol optical properties around Jungfraujoch. Part of these in-situ measured parameters, together with the RH-dependent σ(RH) were used to

  3. Size-resolved aerosol water uptake and cloud condensation nuclei measurements as measured above a Southeast Asian rainforest during OP3

    NASA Astrophysics Data System (ADS)

    Irwin, M.; Robinson, N.; Allan, J. D.; Coe, H.; McFiggans, G.

    2011-11-01

    The influence of the properties of fine particles on the formation of clouds and precipitation in the tropical atmosphere is of primary importance to their impacts on radiative forcing and the hydrological cycle. Measurements of aerosol number size distribution, hygroscopicity in both sub- and supersaturated regimes and composition were taken between March and July 2008 in the tropical rainforest in Borneo, Malaysia, marking the first study of this type in an Asian tropical rainforest. Hygroscopic growth factors (GF) at 90 % relative humidity (RH) for the dry diameter range D0 = 32-258 nm, supersaturated water uptake behaviour for the dry diameter range D0 = 45-300 nm and aerosol chemical composition were simultaneously measured using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA), a Droplet Measurement Technologies Cloud Condensation Nuclei counter (CCNc) and an Aerodyne Aerosol Mass Spectrometer (AMS) respectively. The hygroscopicity parameter κ was derived from both CCNc and HTDMA measurements, with the resulting values of κ ranging from 0.05-0.37, and 0.17-0.37, respectively. Although the total range of κ values is in good agreement, there are inconsistencies between CCNc and HTDMA derived κ values at different dry diameters. Results from a study with similar methodology performed in the Amazon rainforest report values for κ within a similar range to those reported in this work, indicating that the aerosol as measured from both sites shows similar hygroscopic properties. However, the derived number of cloud condensation nuclei (NCCN) were much higher in the present experiment than the Amazon, resulting in part from the increased total particle number concentrations observed in the Bornean rainforest. This contrast between the two environments may be of substantial importance in describing the impacts of particles in the tropical atmosphere.

  4. Hygroscopic growth and activation of uncoated and coated soot particles and their relation to ice nucleation

    NASA Astrophysics Data System (ADS)

    Ziese, M.; Henning, S.; Mildenberger, K.; Stratmann, F.; Möhler, O.; Benz, S.; Buchholz, A.; Mentel, Th.; Aida/Lacis-Mobile-Team

    2009-04-01

    Measurements of the hygroscopic growth (HTDMA, LACIS-mobile), activation behavior (DMT-CCNC) - scope of this paper - and ice nucleation (AIDA chamber) were performed to estimate the cloud-forming potential of pure and coated soot particles. Globally, soot particles contribute up to 2.5 % to the atmospheric aerosol. In the framework of the investigations described here, soot particles were generated either applying a graphite-spark-generator (GFG1000) or a flame-soot-generator (Mini-CAST). With respect to the hygroscopic growth and activation behavior, the influences of the carrier-gas (GFG-soot), the OC-content (CAST-soot) and of different coating materials were investigated. Differences in the hygroscopic growth and activation behavior of GFG generated soot particles were found for the two carrier-gases considered. If nitrogen was used, neither hygroscopic growth nor activation were observed. In contrast, when argon was used, particles featured a slight hygroscopic growth and were easier to activate. Hygroscopic growth increases with decreasing OC-content of the CAST-soot, up to growth factor 1.04 at 98.4 % relative humidity. Lower OC-contents also result in the particles being activated more easily. Coating with sulfuric acid enhances the hygroscopic growth and activation behavior of CAST-soot for different OC-contents. If the soot (GFG & CAST) was coated with dicarboxylic acids (oxalic and succinic acid), no enhancement of hygroscopic growth and activation was observed. This is most likely due to evaporation of the coating material. In comparison to the hygroscopic growth and activation behavior, the same trends were observed in the ice-nucleation behavior. That is, the more active a particle is as cloud condensation nuclei, the better it functions as ice nuclei. GFG-soot with argon as carrier-gas acts as a better ice nuclei than GFG-soot with nitrogen. For the CAST-soot the ice-nucleation activity decreases with increasing OC-content. Coating with sulfuric acid

  5. Influence of functional groups on organic aerosol cloud condensation nucleus activity.

    PubMed

    Suda, Sarah R; Petters, Markus D; Yeh, Geoffrey K; Strollo, Christen; Matsunaga, Aiko; Faulhaber, Annelise; Ziemann, Paul J; Prenni, Anthony J; Carrico, Christian M; Sullivan, Ryan C; Kreidenweis, Sonia M

    2014-09-01

    Organic aerosols in the atmosphere are composed of a wide variety of species, reflecting the multitude of sources and growth processes of these particles. Especially challenging is predicting how these particles act as cloud condensation nuclei (CCN). Previous studies have characterized the CCN efficiency for organic compounds in terms of a hygroscopicity parameter, κ. Here we extend these studies by systematically testing the influence of the number and location of molecular functional groups on the hygroscopicity of organic aerosols. Organic compounds synthesized via gas-phase and liquid-phase reactions were characterized by high-performance liquid chromatography coupled with scanning flow CCN analysis and thermal desorption particle beam mass spectrometry. These experiments quantified changes in κ with the addition of one or more functional groups to otherwise similar molecules. The increase in κ per group decreased in the following order: hydroxyl ≫ carboxyl > hydroperoxide > nitrate ≫ methylene (where nitrate and methylene produced negative effects, and hydroperoxide and nitrate groups produced the smallest absolute effects). Our results contribute to a mechanistic understanding of chemical aging and will help guide input and parametrization choices in models relying on simplified treatments such as the atomic oxygen:carbon ratio to predict the evolution of organic aerosol hygroscopicity. PMID:25118824

  6. Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

    NASA Astrophysics Data System (ADS)

    Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

    2016-07-01

    The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a "simulated radiance" product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land-ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers.This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled.In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model subgrid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to

  7. Influence Of Relative Humidity On Light Scattering Measurements Of Aerosols Using A Humidifier-Dryer Nephelometer

    NASA Astrophysics Data System (ADS)

    Orozco, D.; Delgado, R.; Hoff, R. M.

    2012-12-01

    Atmospheric aerosols influence the Earth's radiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence the Earth's radiation budget by modifying the microphysical and radiative properties, as well as the water content and lifetime of clouds. In atmosphere conditions, aerosol particles experience hygroscopic growth due to the relative humidity (RH) influence. Wet aerosols particles are larger than their dry equivalents, therefore they scatter more light. Quantitative knowledge of the RH effect and its influence on the light scattering coefficient on aerosol particles is of substantial importance when comparing ground based observation with other optical aerosol measurements techniques such satellite retrieval and photometry as well as for climate forcing calculations. A humidifier-dryer system for a TSI 3563 Nephelometer was designed and built in order to measure the scattering coefficient σsp(λ) at three different wavelengths (λ=440, 550 and 700nm) in a RH range from 30 to 95%. The system was assembled by combining Nafion tubes to humidify and dry the aerosols and stepping motor valves to control the flow and the amount of humidity entering to the Nephelometer. Regular measurements at UMBC (University Of Maryland, Baltimore County) with ambient and lab-generated aerosols have been taking place to study the hygroscopic properties of the aerosols in the region. The aerosols have been humidified as high as 95.4% and the measured σsp(λ) were on average more than two times greater than those at low RH. Another important parameter used to evaluate the hygroscopic properties of aerosols is the enhancement factor f(λ,RH) which is defined as the σsp(λ,RH) at any specified RH divided by the dry σsp(λ,DRY). Initial results indicates that the enhancement factor for ambient aerosols in the region is f(550,94%) =1.35. Enhancement

  8. Effects of design parameters and puff topography on heating coil temperature and mainstream aerosols in electronic cigarettes

    NASA Astrophysics Data System (ADS)

    Zhao, Tongke; Shu, Shi; Guo, Qiuju; Zhu, Yifang

    2016-06-01

    Emissions from electronic cigarettes (ECs) may contribute to both indoor and outdoor air pollution and the number of users is increasing rapidly. ECs operate based on the evaporation of e-liquid by a high-temperature heating coil. Both puff topography and design parameters can affect this evaporation process. In this study, both mainstream aerosols and heating coil temperature were measured concurrently to study the effects of design parameters and puff topography. The heating coil temperatures and mainstream aerosols varied over a wide range across different brands and within same brand. The peak heating coil temperature and the count median diameter (CMD) of EC aerosols increased with a longer puff duration and a lower puff flow rate. The particle number concentration was positively associated with the puff duration and puff flow rate. These results provide a better understanding of how EC emissions are affected by design parameters and puff topography and emphasize the urgent need to better regulate EC products.

  9. Size-spectra of trace elements in urban aerosol particles by instrumental neutron activation analysis

    SciTech Connect

    Ondov, J.M.; Divita, F. Jr.; Suarez, A.

    1994-12-31

    Knowledge of composition and size of atmospheric aerosol particles is needed to elucidate their sources, atmospheric transformation processes, contributions to visibility reduction, and respiratory and environmental deposition. In a previous communication, we described size spectra and hygroscopic growth of arsenic, selenium, antimony, and zinc in College Park, Maryland, an urban, nonindustrial area located near Washington, D.C., wherein, concentrations of these elements are influenced largely by sulfate-containing aerosol transported from the Ohio River valley region, more than 200 km west of the area, and local coal utility plants and incinerators located 20 to 50 km from the sampling site. At College Park, mass median aerodynamic diameters (mmad) versus relative humidity (RH) data for these elements fell along different curves for samples influenced by local and distant aerosols; i.e., the curve for distant sources lay below the curve for local sources, at larger mmads for the same RH. In this paper we discuss size spectra, distribution parameters, and hygroscopic growth of aerosol particles bearing trace elements in aerosol collected in Camden, New Jersey, a heavily industrial area in which major sources, including an antimony roaster and municipal incinerator, lie in close proximity (i.e., 5 to 15 km) to the site.

  10. Aerosol light-scattering enhancement due to water uptake during TCAP campaign

    NASA Astrophysics Data System (ADS)

    Titos, G.; Jefferson, A.; Sheridan, P. J.; Andrews, E.; Lyamani, H.; Alados-Arboledas, L.; Ogren, J. A.

    2014-02-01

    Aerosol optical properties were measured by the DOE/ARM (US Department of Energy Atmospheric Radiation Measurements) Program Mobile Facility in the framework of the Two-Column Aerosol Project (TCAP) deployed at Cape Cod, Massachusetts, for a~one year period (from summer 2012 to summer 2013). Measured optical properties included aerosol light-absorption coefficient (σap) at low relative humidity (RH) and aerosol light-scattering coefficient (σsp) at low and at RH values varying from 30 to 85%, approximately. Calculated variables included the single scattering albedo (SSA), the scattering Ångström exponent (SAE) and the scattering enhancement factor (f(RH)). Over the period of measurement, f(RH = 80%) had a mean value of 1.9 ± 0.3 and 1.8 ± 0.4 in the PM10 and PM1 fractions, respectively. Higher f(RH = 80%) values were observed for wind directions from 0-180° (marine sector) together with high SSA and low SAE values. The wind sector from 225 to 315° was identified as an anthropogenically-influenced sector, and it was characterized by smaller, darker and less hygroscopic aerosols. For the marine sector, f(RH = 80%) was 2.2 compared with a value of 1.8 obtained for the anthropogenically-influenced sector. The air-mass backward trajectory analysis agreed well with the wind sector analysis. It shows low cluster to cluster variability except for air-masses coming from the Atlantic Ocean that showed higher hygroscopicity. Knowledge of the effect of RH on aerosol optical properties is of great importance for climate forcing calculations and for comparison of in-situ measurements with satellite and remote sensing retrievals. In this sense, predictive capability of f(RH) for use in climate models would be enhanced if other aerosol parameters could be used as proxies to estimate hygroscopic growth. Toward this goal, we propose an exponential equation that successfully estimates aerosol hygroscopicity as a function of SSA at Cape Cod. Further work is needed to determine

  11. Aerosol light-scattering enhancement due to water uptake during the TCAP campaign

    NASA Astrophysics Data System (ADS)

    Titos, G.; Jefferson, A.; Sheridan, P. J.; Andrews, E.; Lyamani, H.; Alados-Arboledas, L.; Ogren, J. A.

    2014-07-01

    Aerosol optical properties were measured by the DOE/ARM (US Department of Energy Atmospheric Radiation Measurements) Program Mobile Facility during the Two-Column Aerosol Project (TCAP) campaign deployed at Cape Cod, Massachusetts, for a 1-year period (from summer 2012 to summer 2013). Measured optical properties included aerosol light-absorption coefficient (σap) at low relative humidity (RH) and aerosol light-scattering coefficient (σsp) at low and at RH values varying from 30 to 85%, approximately. Calculated variables included the single scattering albedo (SSA), the scattering Ångström exponent (SAE) and the scattering enhancement factor (f(RH)). Over the period of measurement, f(RH = 80%) had a mean value of 1.9 ± 0.3 and 1.8 ± 0.4 in the PM10 and PM1 fractions, respectively. Higher f(RH = 80%) values were observed for wind directions from 0 to 180° (marine sector) together with high SSA and low SAE values. The wind sector from 225 to 315° was identified as an anthropogenically influenced sector, and it was characterized by smaller, darker and less hygroscopic aerosols. For the marine sector, f(RH = 80%) was 2.2 compared with a value of 1.8 obtained for the anthropogenically influenced sector. The air-mass backward trajectory analysis agreed well with the wind sector analysis. It shows low cluster to cluster variability except for air masses coming from the Atlantic Ocean that showed higher hygroscopicity. Knowledge of the effect of RH on aerosol optical properties is of great importance for climate forcing calculations and for comparison of in situ measurements with satellite and remote sensing retrievals. In this sense, predictive capability of f(RH) for use in climate models would be enhanced if other aerosol parameters could be used as proxies to estimate hygroscopic growth. Toward this goal, we propose an exponential equation that successfully estimates aerosol hygroscopicity as a function of SSA at Cape Cod. Further work is needed to determine if

  12. Measurements of physical and chemical properties of urban aerosols and their CCN activities in Seoul during the KORUS-AQ pre-campaign

    NASA Astrophysics Data System (ADS)

    Kim, N.; Yum, S. S.; Park, M.; Shin, H. J.; Bae, G. N.; Kwak, K. H.; Park, J. S.; Park, S. M.; Ahn, J.

    2015-12-01

    Interest in cloud condensation nuclei (CCN) has been increasing for the last few decades due to their first order effects on radiative and microphysical properties of clouds. Particularly, scientific understanding of CCN from anthropogenic sources becomes important because it is now considered that large uncertainties in climate change predictions stem from insufficient understanding of CCN. CCN activity is influenced by size and chemical component of aerosols. The KORUS-AQ campaign, jointly organized by National Institute of Environmental Research (NIER) of Korea and National Aeronautics and Space Administration (NASA) aims at understanding various aspects of air quality problem in Korea and will be held in spring, 2016. In preparation for this campaign, pre-campaign was held during May 18-June 13, 2015, in Seoul where numerous local anthropogenic sources exist and influence of Chinese continental outflow directly affects. Here we present some of the important results from the pre-campaign. Chemical properties of aerosols were measured with AMS. Aerosol and CCN number concentrations, aerosol size distribution and aerosol hygroscopic growth factor were measured by CPC, CCN counter, SMPS and H-TDMA, respectively. Average diurnal variation of aerosol number concentration showed three dominant peaks at around 0600_UTC and morning and evening rush hours. Each peak seemed to have different characteristics and therefore detailed analyses of physical and chemical properties of aerosols during the peaks as well as during some special events will be made. The hygroscopicity parameter, kappa, will be estimated by examining CCN activity, H-TDMA measured hygroscopic growth factor and mixing rule of aerosol chemical components, and the result will be compared as well.

  13. Demonstration of Aerosol Property Profiling by Multi-wavelength Lidar Under Varying Relative Humidity Conditions

    NASA Technical Reports Server (NTRS)

    Whiteman, D.N.; Veselovskii, I.; Kolgotin, A.; Korenskii, M.; Andrews, E.

    2008-01-01

    The feasibility of using a multi-wavelength Mie-Raman lidar based on a tripled Nd:YAG laser for profiling aerosol physical parameters in the planetary boundary layer (PBL) under varying conditions of relative humidity (RH) is studied. The lidar quantifies three aerosol backscattering and two extinction coefficients and from these optical data the particle parameters such as concentration, size and complex refractive index are retrieved through inversion with regularization. The column-integrated, lidar-derived parameters are compared with results from the AERONET sun photometer. The lidar and sun photometer agree well in the characterization of the fine mode parameters, however the lidar shows less sensitivity to coarse mode. The lidar results reveal a strong dependence of particle properties on RH. The height regions with enhanced RH are characterized by an increase of backscattering and extinction coefficient and a decrease in the Angstrom exponent coinciding with an increase in the particle size. We present data selection techniques useful for selecting cases that can support the calculation of hygroscopic growth parameters using lidar. Hygroscopic growth factors calculated using these techniques agree with expectations despite the lack of co-located radiosonde data. Despite this limitation, the results demonstrate the potential of multi-wavelength Raman lidar technique for study of aerosol humidification process.

  14. Crop Burning in the North and Northwestern Parts in India and Its Impact on Air Quality and Aerosol Parameters

    NASA Astrophysics Data System (ADS)

    Chauhan, A.

    2015-12-01

    Crop burning in the North and Northwestern parts of India started sometime in 1986 when the farmers started using mechanized forming. During October-November and April-May crop residues are burnt which is a serious health threat to people living in the areas and also it impacts climate of the northern parts of India including Himalayan region. Detailed analysis of satellite data, MODIS, AIRS and OMI AURA have been carried out to study aerosol and meteorological parameters near the source of biomass burning and also at far region. During crop burning period, pronounced changes in the aerosol and meteorological parameters are observed at different pressure levels. The emissions from the crop burning are spread in the Indo-Gangetic plains from west-east, over the Himalayan region and over the central parts of India depending upon the wind direction and wind speed. The air quality changes anomalously affecting the visibility and aerosol parameters. The emissions from crop burning mixes with the local emissions (vehicular and industrial sources) affecting the trace gas concentrations and aerosol optical parameters as a result dense haze fog and smog are observed during burning period. Long range transport of emissions from crop burning over India and its various climatic and health consequences will be presented.

  15. 21 CFR 884.4260 - Hygroscopic Laminaria cervical dilator.

    Code of Federal Regulations, 2010 CFR

    2010-04-01

    ... 21 Food and Drugs 8 2010-04-01 2010-04-01 false Hygroscopic Laminaria cervical dilator. 884.4260 Section 884.4260 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES... Devices § 884.4260 Hygroscopic Laminaria cervical dilator. (a) Identification. A hygroscopic...

  16. 21 CFR 884.4260 - Hygroscopic Laminaria cervical dilator.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... 21 Food and Drugs 8 2011-04-01 2011-04-01 false Hygroscopic Laminaria cervical dilator. 884.4260 Section 884.4260 Food and Drugs FOOD AND DRUG ADMINISTRATION, DEPARTMENT OF HEALTH AND HUMAN SERVICES... Devices § 884.4260 Hygroscopic Laminaria cervical dilator. (a) Identification. A hygroscopic...

  17. Direct radiative effect by multicomponent aerosol over China

    SciTech Connect

    Huang, Xin; Song, Yu; Zhao, Chun; Cai, Xuhui; Zhang, Hongsheng; Zhu, Tong

    2015-05-01

    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 SO2, 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 PM10 and its components, and 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.

  18. Hygroscopic properties of ultrafine particles at an urban site in northern Japan during the summer of 2011

    NASA Astrophysics Data System (ADS)

    Jung, Jinsang; Kawamura, Kimitaka

    2013-04-01

    To investigate the hygroscopic property of ultrafine particles, hygroscopic growth factors [g(RH)] of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. Hygroscopic growth factors at 85% RH [g(85%)] of freshly formed nucleation mode particles ranged from 1.11 to 1.28 with an average of 1.16 ± 0.06. These values are similar to those of secondary organic aerosols, suggesting that low volatile organic vapors are important to the growth of nucleated clusters into quasi-stable aerosol particles larger than 3 nm. Higher g(85%) values (range: 1.21-1.31, AVG: 1.27 ± 0.04) were obtained for grown Aitken mode nucleated particles. This result may indicate that the growth of freshly formed nucleation mode particles to the Aitken mode particles at the urban site can be attributed to condensation not only of low volatility organic vapors but also of highly water-soluble inorganic compounds like sulfuric acid. Diel variations in the number concentrations of less-hygroscopic particles [g(85%) <1.05] were similar to those in NO concentrations, suggesting that less-hygroscopic particles are mainly produced by local anthropogenic emissions such as traffic. Higher g(85%) values (1.27 ± 0.05) were obtained at a dry particle diameter of 120 nm when the air masses originated from downwind areas of the Asian continent, whereas lower g(85%) values (1.19 ± 0.06) were obtained when clean marine air masses arrived in the urban site. These results indicate that the hygroscopic property of large Aitken and small accumulation mode particles (80-165 nm) are highly influenced by the long-range transport of atmospheric particles.

  19. Long-term visibility data in the UK - how does visibility vary with meteorological and pollutant parameters?

    NASA Astrophysics Data System (ADS)

    Singh, Ajit; Bloss, William J.; Pope, Francis D.

    2016-04-01

    Poor visibility can be an indicator of poor air quality. Moreover, degradation in visibility can be hazardous to human safety; for example, low visibility can lead to accidents particularly during winter when fogs are prevalent. The present quantitative analysis attempts to explain the influence of aerosol concentration and composition, and meteorology on long-term UK visibility. We use visibility data from eight UK meteorological stations which have been running since the 1950s. The site locations include urban, rural and marine environments. Overall, most stations show a long term trend of visibility increase, which is indicative of reductions in aerosol pollution, especially in urban areas. Additionally, results at all sites show a very clear dependence on relative humidity, indicating the importance of aerosol hygroscopicity on the ability of aerosols to scatter radiation and hence impact upon visibility. The dependence of visibility on other meteorological parameters (e.g. relative humidity, air temperature, wind speed & direction) is also investigated. To explain the long term visibility trends and their dependence on meteorological conditions, a light extinction model was constructed incorporating the concentrations and composition of historic aerosol. The lack of historic aerosol size distributions and aerosol composition data, which determine hygroscopicity and refractive index, leads to an under-constrained model. Aerosol measurements from the last 10 years are used to constrain these model parameters, and hence their historical variation can be estimated; sensitivity analyses are used to estimate errors for the time period before regular aerosol measurements are available. A good agreement is observed between modelled and measured visibility. This work has generated a unique 60 year data set with which to understand how aerosol concentration and composition has varied over the UK. The model is applicable and easily transferrable to other data sets

  20. 60 years of visibility data in the UK - how does visibility vary with meteorological and pollutant parameters?

    NASA Astrophysics Data System (ADS)

    Singh, A.; Bloss, W.; Pope, F.

    2015-12-01

    Reduced visibility can be an indicator of poor air quality. Moreover, degradation in visibility can be hazardous to human safety; for example, low visibility can lead to accidents particularly during the winter season when fogs are prevalent. Here, we explore the combined influence of aerosol characteristics and meteorology on long-term visibility. We use visibility data from eight meteorological stations, situated in the UK, which have been running since the 1950s. The site locations include urban, rural and marine environments. Most stations show a long term trend of visibility increase, which is indicative of reductions in aerosol pollution, especially in urban areas. Additionally, results at all sites show a very clear dependence on relative humidity, indicating the importance of aerosol hygroscopicity on the ability of aerosols to scatter radiation and hence impact upon visibility. The dependence of visibility on other meteorological parameters (e.g. wind speed, wind direction) is also investigated. To explain the long term visibility trends and their dependence on meteorological conditions, a light extinction model was constructed incorporating the concentrations and composition of historic aerosol. The lack of historic aerosol size distributions and aerosol composition data, which determine hygroscopicity and refractive index, leads to an under-constrained model. Aerosol measurements from the last 10 years are used to constrain these model parameters, and hence their historical variation can be estimated; sensitivity analyses are used to estimate errors for the time period before regular aerosol measurements are available. This work has generated a unique 60 year data set with which to understand how aerosol concentration and composition has varied over the UK. The model is applicable and easily transferrable to other data sets worldwide. Hence, different clean air legislation can be assessed for its effectiveness in reducing aerosol pollution. The

  1. Key parameters controlling OH-initiated formation of secondary organic aerosol in the aqueous phase (aqSOA)

    NASA Astrophysics Data System (ADS)

    Ervens, Barbara; Sorooshian, Armin; Lim, Yong B.; Turpin, Barbara J.

    2014-04-01

    Secondary organic aerosol formation in the aqueous phase of cloud droplets and aerosol particles (aqSOA) might contribute substantially to the total SOA burden and help to explain discrepancies between observed and predicted SOA properties. In order to implement aqSOA formation in models, key processes controlling formation within the multiphase system have to be identified. We explore parameters affecting phase transfer and OH(aq)-initiated aqSOA formation as a function of OH(aq) availability. Box model results suggest OH(aq)-limited photochemical aqSOA formation in cloud water even if aqueous OH(aq) sources are present. This limitation manifests itself as an apparent surface dependence of aqSOA formation. We estimate chemical OH(aq) production fluxes, necessary to establish thermodynamic equilibrium between the phases (based on Henry's law constants) for both cloud and aqueous particles. Estimates show that no (currently known) OH(aq) source in cloud water can remove this limitation, whereas in aerosol water, it might be feasible. Ambient organic mass (oxalate) measurements in stratocumulus clouds as a function of cloud drop surface area and liquid water content exhibit trends similar to model results. These findings support the use of parameterizations of cloud-aqSOA using effective droplet radius rather than liquid water volume or drop surface area. Sensitivity studies suggest that future laboratory studies should explore aqSOA yields in multiphase systems as a function of these parameters and at atmospherically relevant OH(aq) levels. Since aerosol-aqSOA formation significantly depends on OH(aq) availability, parameterizations might be less straightforward, and oxidant (OH) sources within aerosol water emerge as one of the major uncertainties in aerosol-aqSOA formation.

  2. Characteristics of aerosol optical properties and meteorological parameters during three major dust events (2005-2010) over Beijing, China

    NASA Astrophysics Data System (ADS)

    Cao, Chunxiang; Zheng, Sheng; Singh, Ramesh P.

    2014-12-01

    Multi-satellite sensors are capable of monitoring transport and characteristics of dust storms and changes in atmospheric parameters along their transport. The present paper discusses aerosol optical properties and meteorological parameters during major dust storm events occurred in the period 2005-2010 over Beijing, China. The back trajectory model shows that the dust is transported from the Inner Mongolia and Mongolia arid regions to Beijing. High aerosol optical depth (AOD) at the wavelength 675 nm and low Ångström exponent (AE) values in the wavelength 440-870 nm are observed during dusty days. The aerosol size distribution (ASD) in coarse mode shows a large increase in the volume during dusty days. The single scattering albedo (SSA) increases with higher wavelength on dusty days, and is generally found to be higher compared to the days prior to and after the dust events, indicating the presence of high concentrations of scattering particles due to dust storm events. The physico-chemical properties of aerosols during dusty and non dusty days show distinct characteristics as reflected from the changes in the real and imaginary parts of refractive index (RI). In addition, the CO volume mixing ratio (COVMR) from Atmospheric Infrared Sounder (AIRS) shows a pronounced decrease on dusty days, while the H2O mass mixing ratio (H2OMMR) shows enhanced signal. Furthermore, enhanced level of water vapor (WV) using Moderate Resolution Imaging Spectroradiometer (MODIS) data is also observed in and around Beijing over the dust storms track.

  3. Aerosol and Cloud-Nucleating Particle Observations during an Atmospheric River Event

    NASA Astrophysics Data System (ADS)

    DeMott, P. J.; McCluskey, C. S.; Petters, M.; Suski, K. J.; Levin, E. J.; Hill, T. C. J.; Atwood, S. A.; Schill, G. P.; Rocci, K.; Boose, Y.; Martin, A.; Cornwell, G.; Al-Mashat, H.; Moore, K.; Prather, K. A.; Rothfuss, N.; Taylor, H.; Leung, L. R.; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; Creamean, J.; White, A. B.; Kreidenweis, S. M.

    2015-12-01

    The multi-agency CalWater 2015 project occurred over North Central CA and the Eastern Pacific during January to March 2015 (Spackman et al., this session). The goals of the campaign were to document the structure of atmospheric rivers (ARs) that deliver much of the water vapor associated with major winter storms along the U.S. West Coast and to investigate the modulating effect of aerosols on precipitation. Aerosol sources that may influence orographic cloud properties for air lifted over the mountains in California in winter include pollution, biomass burning, soil dusts and marine aerosols, but their roles will also be influenced by transport, vertical stratification, and scavenging processes. We present results from a comprehensive study of aerosol distributions, compositions, and cloud nucleating properties during an intense winter storm during February 2015, including data from an NSF-supported measurement site at Bodega Bay, from the DOE-ARM Cloud Aerosol Precipitation Experiment that included sampling on the NOAA RV Ron Brown offshore and the G-1 aircraft over ocean and land, and with context provided by other NOAA aircraft and remote sensing facilities. With a special focus on the coastal site, we discuss changes in aerosol distributions, aerosol hygroscopicity, and number concentrations of fluorescent particles, cloud condensation nuclei (CCN), and ice nucleating particles (INPs) during the AR event. We compare with periods preceding and following the event. For example, total aerosol number and surface area concentrations at below 0.5 μm diameter decreased from typical values of a few thousand cm-3 and 100 μm2 cm-3, respectively, to a few hundred cm-3 and 10 μm2cm-3 at Bodega Bay during the AR event. CCN concentrations were similarly lower, but hygroscopicity parameter (kappa) increased from typical values of 0.2 to values > 0.5 during the AR.INP and fluorescent particle number concentrations were generally lower during the AR event than at any other

  4. A study of aerosol optical properties using a lightweight optical particle spectrometer and sun photometer from an unmanned aerial system

    NASA Astrophysics Data System (ADS)

    Telg, H.; Murphy, D. M.; Bates, T. S.; Johnson, J. E.; Gao, R. S.

    2015-12-01

    A miniaturized printed optical particle spectrometer (POPS) and sun photometer (miniSASP) have been developed recently for unmanned aerial systems (UAS) and balloon applications. Here we present the first scientific data recorded by the POPS and miniSASP from a Manta UAS during a field campaign on Svalbard, Norway, in April 2015. As part of a payload composed of five different aerosol instruments (absorption photometer, condensation particle counter, filter sampler, miniSASP and POPS) we collected particle size distributions, the optical depth (OD) and the sky brightness from 0 to 3000 m altitude. The complementary measurement approaches of the miniSASP and POPS allow us to calculate aerosol optical properties such as the aerosol optical depth and the angstrom exponent or the asymmetry parameter independently. We discuss deviation between results with respect to aerosol properties, e.g. hygroscopicity and absorption, as well as instrumental limitations.

  5. Optical and radiative-transfer properties of mixed atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Degheidy, A. R.; Sallah, M.; Elgarayhi, A.; Shaaban, S. M.

    2015-04-01

    The optical and radiative-transfer properties of mixed atmospheric aerosols have been investigated. The aerosol medium is considered as a plane-parallel anisotropic scattering medium with diffusive reflecting boundaries and containing an internal radiation source. The basic components are defined by their complex refractive index, a lognormal size distribution and humidity dependence in hygroscopic particles. The aerosol particles are assumed to be spherical, so the scattering parameters in the form of single scattering albedo, asymmetry factor, scattering, absorption, extinction efficiencies and linear anisotropic coefficient are calculated using the Mie theory. The calculations have been performed for individual aerosol particles, internal and external mixing media. Radiation transfer problem through the considered aerosol medium has been solved in terms of the solution of the corresponding source-free problem with simple boundary conditions. For the solution of the source-free problem, the Variational Pomraning-Eddington technique has been employed. The variation of the radiative-transfer properties (partial radiative fluxes at the medium boundaries) have been calculated and represented graphically for the different aerosols with their different mixing states. A comparison of the obtained results versus available published data has been performed and a very good agreement was observed.

  6. Size-resolved aerosol water uptake and cloud condensation nuclei measurements as measured above a Southeast Asian rainforest during OP3

    NASA Astrophysics Data System (ADS)

    Irwin, M.; Robinson, N.; Allan, J. D.; Coe, H.; McFiggans, G.

    2011-01-01

    The influence of the properties of fine particles on the formation of clouds and precipitation in the tropical atmosphere is of primary importance to their impacts on radiative forcing and the hydrological cycle. Measurements of aerosol number size distribution, hygroscopicity in both sub- and supersaturated regimes and composition were taken between March and July 2008 in the tropical rainforest in Borneo, Malaysia, marking the first study of this type in an Asian tropical rainforest. Hygroscopic growth factors (GF) at 90% relative humidity (RH) for the dry diameter range D0=32-258 nm, supersaturated water uptake behaviour for the dry diameter range D0=20-300 nm and aerosol chemical composition were simultaneously measured using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA), a Droplet Measurement Technologies Cloud Condensation Nuclei counter (CCNc) and an Aerodyne Aerosol Mass Spectrometer (AMS), respectively. The derived hygroscopicty parameter κ ranged from between 0.05-0.37 for the supersaturation range 0.11-0.73% compared to those between 0.17-0.37 for measurements performed at a relative humidity of 90%. In contrast, results from a study with similar methodology performed in the Amazon basin report more similar values for κ, indicating that the aerosol as measured from both sites shows similar hygroscopic properties. However, the derived number of cloud condensation nuclei (NCCN) were much higher than those measured in the Amazon, due to the higher particle number concentrations in the rainforests of Borneo. This first contrast between the two environments may be of substantial importance in describing the impacts of particles in the tropical atmosphere.

  7. Large differences in aerosol optical properties over the north-west Atlantic Ocean during the TCAP field campaign

    NASA Astrophysics Data System (ADS)

    Chand, D.; Berg, L. K.; Comstock, J. M.; Fast, J. D.; Flynn, C. J.; Hubbe, J. M.; Kassianov, E.; Mei, F.; Pekour, M. S.; Schmid, B.; Sedlacek, A. J., III; Tomlinson, J. M.; Shilling, J. E.; Wilson, J. M.; Zelenyuk, A.; Berkowitz, C. M.

    2014-12-01

    Aerosol radiative forcing is an important parameter in the Earth's radiation budget and can be an important driver of atmospheric circulation and the hydrological cycle. Accurate estimation of aerosol radiative forcing requires measurement of both the extensive and intensive optical properties of aerosols. While the intensive optical properties are independent of aerosol mass or number, they are critical inputs when calculating radiative forcing with applications to climate research, satellite remote sensing and model validations. The key aerosol intensive properties that need to be evaluated include single scattering albedo (SSA), the angstrom exponent, the asymmetry parameter, the radiative forcing efficiency, and the hygroscopic scattering factor. We report here on values of these variables over the Cape Cod and nearby northwest Atlantic Ocean during the Two Column Aerosol Project (TCAP). The average SSA shows a distinct profile having higher SSA values below the top of well-mixed residual layer (RL) and lower SSA above it. Aerosol in the free troposphere (FT) were found to have less spectral dependence in their optical properties, lower back scatter fraction and higher hygroscopic growth relative to aerosols found in the RL. Analysis of individual particle composition suggests that that ratio of aged to fresh aerosol numbers in the FT is 70% higher compared to aerosols measured in the RL, and that smoke from biomass burning contributed ~10% to this number. Single particle analysis also reveals that the fraction and variability of coated black carbon (BC) aerosol is higher in the FT relative to that measured in the residual layer. The daily radiative forcing efficiency of these aerosols in the FT is factor 2 higher than below RL. Seven years (2007-2013) of CALIPSO satellite observations show that the mean altitude of the top of smoke layers (~3.3 km) consistent with these in situ observations from TCAP. Overall, the long term CALIPSO observations characterizes

  8. Importance of relative humidity in the oxidative ageing of organic aerosols: case study of the ozonolysis of maleic acid aerosol

    NASA Astrophysics Data System (ADS)

    Gallimore, P. J.; Achakulwisut, P.; Pope, F. D.; Davies, J. F.; Spring, D. R.; Kalberer, M.

    2011-12-01

    Many important atmospheric aerosol processes depend on the chemical composition of the aerosol, e.g. water uptake and particle cloud interactions. Atmospheric ageing processes, such as oxidation reactions, significantly and continuously change the chemical composition of aerosol particles throughout their lifetime. These ageing processes are often poorly understood. In this study we utilize an aerosol flow tube set up and an ultra-high resolution mass spectrometer to explore the effect of relative humidity (RH) in the range of <5-90% on the ozonolysis of maleic acid aerosol which is employed as model organic aerosol system. Due to the slow reaction kinetics relatively high ozone concentrations of 160-200 ppm were used to achieve an appreciable degree of oxidation of maleic acid. The effect of oxidative ageing on the hygroscopicity of maleic acid particles is also investigated using an electrodynamic balance and thermodynamic modelling. RH has a profound effect on the oxidation of maleic acid particles. Very little oxidation is observed at RH < 50% and the only observed reaction products are glyoxylic acid and formic acid. In comparison, when RH > 50% there are about 15 oxidation products identified. This increased oxidation was observed even when the particles were exposed to high humidities long after a low RH ozonolysis reaction. This result might have negative implications for the use of water as an extraction solvent for the analysis of oxidized organic aerosols. These humidity-dependent differences in the composition of the ozonolyzed aerosol demonstrate that water is both a key reactant in the oxidation scheme and a determinant of particle phase and hence diffusivity. The measured chemical composition of the processed aerosol is used to model the hygroscopic growth, which compares favourably with water uptake results from the electrodynamic balance measurements. A reaction mechanism is presented which takes into account the RH dependent observations. This

  9. Size segregated water uptake of the urban submicrometer aerosol in Beijing

    NASA Astrophysics Data System (ADS)

    Massling, A.; Stock, M.; Wehner, B.; Wu, Z. J.; Hu, M.; Brüggemann, E.; Gnauk, T.; Herrmann, H.; Wiedensohler, A.

    Physical and chemical properties of submicrometer aerosol particles were measured in summer 2004 (June/July) and winter 2005 (January/February) in Beijing, Peoples Republic of China, using a Twin-Differential Mobility Particle Sizer (T-DMPS), a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA), and a Micro Orifice Uniform Deposit Impactor (MOUDI). Particle number-size distributions were measured in the diameter range Dp = 3-800 nm and hygroscopic properties were determined at initial dry particle diameters of Dp j ( j = 30, 50, 80, 150, 250, and 350 nm) at a relative humidity (RH) of 90%. Hygroscopic properties were compared with chemical analyses of aerosol samples taken with the MOUDI. Based on the hygroscopicity data, the total hygroscopic particle volume was modeled, including dependence on dry particle size, season and level of pollution using a simple approach. Overall, the chemical analysis showed ammonium sulfate to be the major inorganic component of the urban submicrometer aerosol in Beijing along with relatively high fractions of elemental carbon (10-25%) and organic matter (15-60%) depending on particle size and season. The hygroscopic growth distributions (H-TDMA) subdivided the aerosol population into three different groups of particles with varying growth factors depending on dry particle size, namely nearly hydrophobic (growth factor = 0.96-1.07), less hygroscopic (1.06-1.29) and more hygroscopic (1.26-1.62). Hydrophobic particle fractions indicating freshly emitted soot/carbonaceous particles varied between 10 and 32% depending on dry particle size and season. During heavily polluted times, a decreasing number of hydrophobic particle fractions indicated that the urban submicrometer aerosol in Beijing was highly influenced by more aged aerosol transported from the industrial regions around Beijing containing sulfate as a major component. Based on model calculations, the urban submicrometer aerosol in Beijing showed strong compositional

  10. Parameters influencing the aerosol capture performance of the Submerged-Bed Scrubber

    SciTech Connect

    Ruecker, C.M.; Scott, P.A.

    1987-04-01

    The Submerged-Bed Scrubber (SBS) is a novel air cleaning device that has been investigated by Pacific Northwest Laboratory (PNL) for scrubbing off gases from liquid-fed ceramic melters used to vitrify high-level waste (HLW). The concept for the SBS was originally conceived at Hanford for emergency venting of a reactor containment building. The SBS was adapted for use as a quenching scrubber at PNL because it can cool the hot melter off gas as well as remove over 90% of the airborne particles, thus meeting the minimum particulate decontamination factor (DF) of 10 required of a primary scrubber. The experiments in this study showed that the submicron aerosol DF for the SBS can exceed 100 under certain conditions. A conventional device, the ejector-venturi scrubber (EVS), has been previously used in this application. The EVS also adequately cools the hot gases from the melter while exhibiting aerosol removal DFs in the range of 5 to 30. In addition to achieving higher DFs than the EVS, however, the SBS has the advantage of being a passive system, better suited to the remote environment of an HLW processing system. The objective of this study was to characterize the performance of the SBS and to improve the aerosol capture efficiency by modifying the operating procedure or the design. A partial factorial experimental matrix was completed to determine the main effects of aerosol solubility, inlet off-gas temperature, inlet off-gas flow rate, steam-to-air ratio, bed diameter and packing diameter on the particulate removal efficiency of the SBS. Several additional experiments were conducted to measure the influence of the inlet aerosol concentration and scrubbing-water concentration on aerosol-removal performance. 33 refs., 17 figs., 14 tabs.

  11. Hygroscopic chemicals and the formation of advection warm fog: A numerical simulation

    NASA Technical Reports Server (NTRS)

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

    1978-01-01

    The formation of advection fog is closely associated with the characteristics of the aerosol particles, including the chemical composition, mass of the nuclei, particle size, and concentration. Both macrophysical and microphysical processes are considered. In the macrophysical model, the evolution of wind components, water vapor content, liquid water content and potential temperature under the influences of vertical turbulent diffusion, turbulent momentum, and turbulent energy transfers are taken into account. In the microphysical model, the supersaturation effect is incorporated with the surface tension and hygroscopic material solution.

  12. Observation of aerosol parameters at Saga using GOSAT product validation lidar

    NASA Astrophysics Data System (ADS)

    Takubo, Shoichiro; Okumura, Hiroshi; Kawasaki, Takeru; Abdullah, Indra Nugraha; Uchino, Osamu; Morino, Isamu; Yokota, Tatsuya; Nagai, Tomohiro; Sakai, Tetsu; Maki, Takashi; Arai, Kohei

    2012-11-01

    Greenhouse gases Observation SATellite (GOSAT) was launched to enable the precise monitoring of the density of carbon dioxide by combining global observation data sent from space with data obtained on land, and with simulation models. In addition, observation of methane, another greenhouse gas, has been considered. For validation of GOSAT data products, ground-base observation with Fourier Transform Spectrometer (FTS), aerosol lidar and ozone-DIAL (DIfferencial Absorption Lidar) at Saga University, JAPAN has been continued since March, 2011. In this article, observation results obtained from aerosol lidar are reported.

  13. Does the long-range transport of African mineral dust across the Atlantic enhance their hygroscopicity?

    NASA Astrophysics Data System (ADS)

    Denjean, Cyrielle; Caquineau, Sandrine; Desboeufs, Karine; Laurent, Benoit; Quiñones Rosado, Mariana; Vallejo, Pamela; Mayol-Bracero, Olga; Formenti, Paola

    2015-04-01

    Influence of mineral dust on radiation balance is largely dependent on their ability to interact with water. While fresh mineral dusts are highly hydrophobic, various transformation processes (coagulation, heterogeneous chemical reaction) can modify the dust physical and chemical properties during long-range transport, which, in turn, can change the dust hygroscopic properties. The model predictions of the radiative effect by mineral dust still suffer of the lack of certainty of dust hygroscopic properties, and their temporal evolution during long-range transport. We present the first direct surface measurements of the hygroscopicity of Saharan dust after long-range transport over the Atlantic Ocean, their relationship with chemical composition, their influence on particle size and shape and implications for optical properties. Particles were collected during the DUST Aging and TransporT from Africa to the Caribbean (Dust-AttaCk) campaign at the Cape San Juan Puerto Rico station in June-July 2012. Environmental scanning electron microscopy (ESEM) was used to analyze the size, shape, chemical composition and hygroscopic properties of individual particles. At different levels of concentrations in summertime, the coarse mode of atmospheric aerosols in Puerto Rico is dominated by Saharan mineral dust. Most of aged dust particles survived atmospheric transport intact with no observed internal mixture with other species and did not show hygroscopic growth up to 94% relative humidity. This is certainly due to the fact that in summertime dust is mostly transported above the marine boundary layer. A minor portion of mineral dust (approximately 19-28% by number) were involved in atmospheric heterogeneous reactions with acidic gases (likely SO2 and HCl) and sea salt aggregation. While sulfate- and chloride-coated dust remained extremely hydrophobic, dust particles in internal mixing with NaCl underwent profound changes in their hygroscopicity, therefore in size and shape. We

  14. Simulating aerosols over Arabian Peninsula with CHIMERE: Sensitivity to soil, surface parameters and anthropogenic emission inventories

    NASA Astrophysics Data System (ADS)

    Beegum, S. Naseema; Gherboudj, Imen; Chaouch, Naira; Couvidat, Florian; Menut, Laurent; Ghedira, Hosni

    2016-03-01

    A three dimensional chemistry transport model, CHIMERE, was used to simulate the aerosol optical depths (AOD) over the Arabian Peninsula desert with an offline coupling of Weather Research and Forecasting (WRF) model. The simulations were undertaken with: (i) different horizontal and vertical configurations, (ii) new datasets derived for soil/surface properties, and (iii) EDGAR-HTAP anthropogenic emissions inventories. The model performance evaluations were assessed: (i) qualitatively using MODIS (Moderate-Resolution Imaging Spectroradiometer) deep blue (DB) AOD data for the two local dust events of August 6th and 23rd (2013), and (ii) quantitatively using AERONET (Aerosol Robotic Network) AOD observations, CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) aerosol extinction profiles, and AOD simulations from various forecast models. The model results were observed to be highly sensitive to erodibility and aerodynamic surface roughness length. The use of new datasets on soil erodibility, derived from the MODIS reflectance, and aerodynamic surface roughness length (z0), derived from the ERA-Interim datasets, significantly improved the simulation results. Simulations with the global EDGAR-HTAP anthropogenic emission inventories brought the simulated AOD values closer to the observations. Performance testing of the adapted model for the Arabian Peninsula domain with improved datasets showed good agreement between AERONET AOD measurements and CHIMERE simulations, where the correlation coefficient (R) is 0.6. Higher values of the correlation coefficients and slopes were observed for the dusty periods compared to the non-dusty periods.

  15. Long-term measurements of aerosol optical parameters in Athens, Greece

    NASA Astrophysics Data System (ADS)

    Paraskevopoulou, Despoina; Liakakou, Eleni; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

    2015-04-01

    Aerosol chemical composition was studied in conjunction with its optical properties in the area of Athens Greece. For this purpose, sampling of fine aerosol fraction (PM2,5) took place on a daily basis from August 2010 to April 2013 at an urban background location. The samples are subsequently analyzed for their content in organic (OC) and elemental carbon (EC), major ions and trace metals, resulting in the exercise of chemical mass closure. In parallel, the optical properties of aerosols are recorded using a nephelometer and a particle soot absorption photometer (PSAP), leading to the calculation of scattering (σscat) and absorption (σabs) coefficients, respectively; while single scattering albedo (SSA) and mass scattering and absorption efficiencies are thereinafter calculated. Daily σscat values provide an average of 30.1±3.9 Μm-1 while, the average of σabs is 5.2±1.4 Μm-1. The seasonal cycle of σscat presents maximum during summer and in November, due to long-range transport of aerosol from continental Europe and dust transfer from Africa, respectively. The estimated mass absorption efficiency of EC is estimated to be 8.3±0.2 m2 g-1 for the whole studied period, while the corresponding estimated mass scattering efficiency of PM2.5 is 1.7±0.1 m2 g-1 and does not affected by the presence of dust. The average SSA equals to 0.87±0.11 for the three-year period. On a seasonal basis, SSA presents maximum values during summer that is consistent with the reduction of EC - the main absorbing specie. Finally, the reconstruction of scattering coefficients was performed taking into consideration the measured chemistry of fine aerosol.

  16. The effect of organic aerosol material on aerosol reactivity towards ozone

    NASA Astrophysics Data System (ADS)

    Batenburg, Anneke; Gaston, Cassandra; Thornton, Joel; Virtanen, Annele

    2015-04-01

    After aerosol particles are formed or emitted into the atmosphere, heterogeneous reactions with gaseous oxidants cause them to 'age'. Aging can change aerosol properties, such as the hygroscopicity, which is an important parameter in how the particles scatter radiation and form clouds. Conversely, heterogeneous reactions on aerosol particles play a significant role in the cycles of various atmospheric trace gases. Organic compounds, a large part of the total global aerosol matter, can exist in liquid or amorphous (semi)solid physical phases. Different groups have shown that reactions with ozone (O3) can be limited by bulk diffusion in organic aerosol, particularly in viscous, (semi)solid materials, and that organic coatings alter the surface interactions between gas and aerosol particles. We aim to better understand and quantify how the viscosity and phase of organic aerosol matter affect gas-particle interactions. We have chosen the reaction of O3 with particles composed of a potassium iodide (KI) core and a variable organic coating as a model system. The reaction is studied in an aerosol flow reactor that consists of a laminar flow tube and a movable, axial injector for the injection of O3. The aerosol-containing air is inserted at the tube's top. The interaction length (and therefore time), between the particles and the O3 can be varied by moving the injector. Alternatively, the production of aerosol particles can be modulated. The remaining O3 concentration is monitored from the bottom of the tube and particle concentrations are measured simultaneously, which allows us to calculate the reactive uptake coefficient γ. We performed exploratory experiments with internally mixed KI and polyethylene glycol (PEG) particles at the University of Washington (UW) in a setup with a residence time around 50 s. Aerosol particles were generated in an atomizer from solutions with varying concentrations of KI and PEG and inserted into the flow tube after they were diluted and

  17. Thirty month variability of aerosol pulse dispersion and conventional lung function parameters in healthy middle aged smokers and nonsmokers.

    PubMed

    Siekmeier, R; Schiller-Scotland, C F; Stahlhofen, W

    1996-11-01

    Chronic cigarette consumption is a generally accepted reason for the development of chronic obstructive pulmonary disease (COPD). COPD correlates to histomorphological parameters of lung structure as well as pulmonary function tests (PFT). COPD related changes affect PFT determined by conventional methods (bodyplethysmography, spirometry) as well as parameters of convective gas mixing. This study evaluates the diagnostic potential of a non-invasive aerosol method for the discrimination between healthy smokers and nonsmokers in comparison to conventional PFT. The aerosol method is based on the inhalation of small aerosol pulses suspended in particle free air and determines their changes during the breathing maneuver. Changes of aerosol pulse parameters (APP) are used to describe the convective component of gas mixing during ventilation. PFT and APP were determined in 40 healthy subjects (nonsmoker: 51.1 +/- 1.5 years; smoker: 49.6 +/- 1.5 years, 39.1 +/- 2.2 pack years) before and after a time interval of 30 months. Conventional PFT in smokers and nonsmokers showed no relevant differences between the values at the beginning and the end of the observation period. Thirty months later, at the end of the observation interval, a very similar behavior of the APP was obtained, which strongly confirmed the prior observed differences between smokers and nonsmokers. The data suggest that cigarette smoke-induced variations of lung function are also detectable in clinically asymptomatic smokers. Even in cases of normal PFT, most APP are able to discriminate between healthy smokers and nonsmokers. Since PFT showed only minor differences between both groups, it is indicated that APP are superior to PFT in the detection of early disturbances of lung ventilation in healthy smokers. Mean values of PFT and APP in smokers and nonsmokers showed a high reproducibility of the data obtained at the beginning of the study as well as at the end of the observation period. The data of our

  18. 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.

  19. Simulation of the aerosol effect on the microphysical properties of shallow stratocumulus clouds over East Asia using a bin-based meso-scale cloud model

    NASA Astrophysics Data System (ADS)

    Choi, I.-J.; Iguchi, T.; Kim, S.-W.; Yoon, S.-C.; Nakajima, T.

    2010-10-01

    A bin-based meso-scale cloud model has been employed to explore the aerosol influence on the cloud microphysical properties and precipitation efficiency of shallow stratocumulus in East Asia in March 2005. We newly constructed aerosol size distributions and hygroscopicity parameters for five aerosol species that reproduced observed aerosol and cloud condensation nuclei (CCN) number concentrations in the target period, and thereby used in model simulation of the cloud microphysical properties and precipitation efficiency. It is found that the simulated results were satisfactorily close to the satellite-based observation. Significant effects of aerosols as well as of the meteorological condition were found in the simulated cloud properties and precipitation as confirmed by comparing maritime and polluted aerosol cases and by a sensitivity test with interchanging the aerosol conditions for two cases. Cloud droplets in the polluted condition tended to exhibit relatively narrower cloud drop spectral widths with a bias toward smaller droplet sizes than those in maritime condition, supporting the dispersion effect. The polluted aerosol condition also had a tendency of thinner and higher cloud layers than maritime aerosol condition under relatively humid meteorological condition, possibly due to enhanced updraft. In our cases, vertical structures of cloud droplet number and size were affected predominantly by the change in aerosol conditions, whereas in the structures of liquid water content and cloud fraction were influenced by both meteorological and aerosol conditions. Aerosol change made little differences in cloud liquid water, vertical cloud structure, and updraft/downdraft velocities between the maritime and polluted conditions under dry atmospheric condition. Quantitative evaluations of the sensitivity factor between aerosol and cloud parameters revealed a large sensitivity values in the target area compared to the previously reported values, indicating the strong

  20. Study of the CCN formation as a function of aerosol components

    NASA Astrophysics Data System (ADS)

    Fanourgakis, George S.; Myriokefalitakis, Stelios; Kanakidou, Maria

    2016-04-01

    Understanding the role of aerosols in Earth's climate through direct and indirect effects has attracted a lot of attention over the last years. Due to the chemical complexity of aerosols along with the variety of the primary emissions sources and the conversions from gas to particle in atmosphere, accurate predictions for the aerosols impact on a regional and global scale still remains a challenging problem. In this study, we examine the relative contribution of directly emitted particles in the atmosphere (primary particles) and particles formed from gas-to-particle conversion (secondary particles) to the global aerosols and to the cloud condensation nuclei (CCN) formation. The Chemistry Transport Model v4.0 (TM4-ECPL) coupled with an extended version of the aerosol micro-physics model M7, which describes microphysical processes (nucleation, coagulation, condensation of gas-phase species) for sulfate, black carbon, organic carbon sea salt, dust and various secondary organic aerosols, is here used. A systematic analysis on the CCN production as a function of the aerosol chemical composition is performed. The sensitivity of the results to physical parameters that affect the CCN formation and cannot be accurately determined, such as hygroscopicity, is investigated based on a detailed sensitivity analysis. This work has been supported by the European FP7 collaborative project BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding).

  1. Comparison of Asian aerosol's radiative effect in Seoul and Gosan, Korea

    NASA Astrophysics Data System (ADS)

    Yoon, S.; Lee, S.; Choi, I.

    2007-05-01

    Seasonal variations of aerosol optical properties as well as their direct radiative effects were investigated using the ground-based aerosol measurements and an optical model calculation in Seoul, a mega city, and Gosan, a background rural island, Korea. From the yearly AERONET dataset, our analysis of seasonal and monthly cycle of aerosol optical depth (AOD) shows that AODs in Seoul are higher than those in Gosan because of the higher concentrations of water soluble ions in Seoul. Especially, seasonal AOD differences of both sites becomes maximum in Summer due to the synoptic meteorological patterns and hygroscopic growth of anthropogenic aerosols. OPAC (Optical Properties of Aerosol and Clouds) model and Fu-Liou RTM (Radiative Transfer Model) were employed for the evaluation of aerosol direct radiative forcing (ADRF) at surface and top of the atmosphere (TOA). A method of determining the values of aerosol optical properties as input parameters was utilized for the ADRF calculation from the AERONET dataset. In each season, the mean ADRF in Seoul turned out to be larger than that of Gosan. The ADRF in Gosan from RTM calculation was compared with the ground-based radiation measurements during the ACE-Asia IOP in 2001 and the ABC-EAREX2005 IOP in 2005. In addition, ADRF contributions by chemical compositions were compared in this study between Seoul and Gosan.

  2. Evaluation of aerosol indirect radiative effects on climate in the EMAC model

    NASA Astrophysics Data System (ADS)

    Chang, Dong Yeong; Tost, Holger; Steil, Benedikt; Lelieveld, Jos

    2013-04-01

    Anthropogenic aerosol particles directly and indirectly influence cloud properties and the Earth's radiative energy budget. Several studies have estimated the effects on climate using global circulation models (GCMs), indicating large differences between different models and large uncertainty ranges. These are mostly attributed to different cloud microphysical process parameterizations and uncertainties in the representation of aerosols. Without detailed cloud microphysical processes, using empirical relations between aerosol number or mass and cloud droplet number potentially even large discrepancies may arise. In the present study, a mechanistic aerosol activation scheme, based on double moment cloud microphysics, is used to compute aerosol indirect radiative and cloud effects in the EMAC model. Aerosol activation is linked to the cloud droplet nucleation processes in warm clouds, accounting for the number, size, and chemical composition of particles under ambient meteorological conditions. This approach uses a combination of empirical and semi-empirical parameters to represent aerosol water uptake and hygroscopic growth into cloud droplets. To evaluate the performance of our approach satellite datasets are used; for example, total cloud fraction from MODIS data and cloud radiative forcing at the top of atmosphere from CERES EBAF data.

  3. Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: an AQMEII-2 perspective

    EPA Science Inventory

    The calculation of aerosol optical properties from aerosol mass is a process subject to uncertainty related to necessary assumptions on the treatment of the chemical species mixing state, density, refractive index, and hygroscopic growth. In the framework of the AQMEII-2 model in...

  4. Effects of relative humidity on aerosol light scattering: results from different European sites

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Fierz-Schmidhauser, R.; Weingartner, E.; Baltensperger, U.

    2013-04-01

    The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σsp) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l., Ny-Ålesund, located on Spitsbergen in the Arctic, Mace Head, a coastal site in Ireland, Cabauw, a rural site in the Netherlands and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f(RH,λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σsp(RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f(RH) largely varied at the five sites starting from very low values of f(RH = 85%,λ = 550 nm) around 1.28 for mineral dust to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch due to the absence of sea salt. Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f(RH). Both parameters are also needed to successfully predict f(RH). Finally, the measurement results were compared to the widely used aerosol model OPAC (Hess et al., 1998). Significant discrepancies were seen especially at intermediate RH ranges, which were mainly attributed to inappropriate implemented hygroscopic growth within OPAC. Replacement of the hygroscopic growth with recent literature values showed a clear improvement of the OPAC model.

  5. Effects of relative humidity on aerosol light scattering: results from different European sites

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Fierz-Schmidhauser, R.; Weingartner, E.; Baltensperger, U.

    2013-11-01

    The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σsp) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l.; Ny-Ålesund, located on Spitsbergen in the Arctic; Mace Head, a coastal site in Ireland; Cabauw, a rural site in the Netherlands; and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f(RH, λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σsp(RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f(RH) at the five sites varied widely, starting at very low values of f(RH = 85%, λ = 550 nm) around 1.28 for mineral dust, and reaching up to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch (due to the absence of sea salt). Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f(RH). Both parameters are also needed to successfully predict f(RH). Finally, the measurement results were compared to the widely used aerosol model, OPAC (Hess et al., 1998). Significant discrepancies were seen, especially at intermediate RH ranges; these were mainly attributed to inappropriate implementation of hygroscopic growth in the OPAC model. Replacement of the hygroscopic growth with values from the recent literature resulted in a clear improvement of the OPAC model.

  6. The Importance of Water Uptake by Aerosols in the Climate Change Problem

    NASA Astrophysics Data System (ADS)

    Ramaswamy, V.; Ginoux, P.; Randles, C.; Schwarzkopf, M. D.

    2007-12-01

    It is well understood that aerosol species have and are continuing to play a central role in the radiative forcing of the climate system. While the role of single-scattering properties of aerosols on climate is generally well- recognized, a key factor that governs the aerosol optical property viz., the hygroscopic growth has received insufficient attention particularly in terms of its role in the climatic impacts due to aerosols. A sensitivity investigation is performed that quantitatively highlights the consequence of the growth of sea-salt-organic carbon mixtures for radiative forcing. Next, we employ the GFDL coupled atmosphere-ocean model to study specifically the aerosol radiative forcing and climate response arising due to the hygroscopic features of sulfate aerosols as they have increased from preindustrial to present-day. We make use of observations of optical depth and surface concentrations to evaluate the reliability of the simulated hygroscopic growth. Regional climate responses in Europe, Asia and Africa are examined, with a focus on temperature, hydrological cycle and surface energy budgets. The importance of hygroscopicity in the climate change problem is put in perspective by comparing the climatic effects with those due to aerosol absorption as well as with those caused by the infrared-absorbing long- lived greenhouse gases. Further, we explore the climate consequence arising from the scenarios of the future emissions of aerosols and the associated hygroscopicity effects.

  7. Seasonal behavior of PM2.5 deliquescence, crystallization, and hygroscopic growth in the Po Valley (Milan): Implications for remote sensing applications

    NASA Astrophysics Data System (ADS)

    D'Angelo, Luca; Rovelli, Grazia; Casati, Marco; Sangiorgi, Giorgia; Perrone, Maria Grazia; Bolzacchini, Ezio; Ferrero, Luca

    2016-07-01

    Atmospheric aerosols deliquescence and crystallization relative humidity (DRH and CRH) are rarely measured compared to the worldwide number of hygroscopicity measurements; this feature comes from the lack of an efficient method able to capture the whole complexity of chemical composition of aerosols. Despite this, the knowledge of both DRH and CRH are crucial for a correct parameterization of the aerosol hygroscopic growth used in different applications, among which the remote sensing is very important. In this paper, a newly developed technique (direct current conductance method) was applied in an aerosol chamber to Milan PM2.5 samples, to identify aerosol DRH and CRH both during winter and summer. These results were compared with those independently obtained by gravimetric measurements conducted in the chamber using a microbalance. Microbalance data allowed also the determination of the mass hygroscopic growth factor on the collected PM2.5 samples. Results evidenced first a good agreement between the two methods (RMSE = 2.7% and 2.3% for DRH and CRH, respectively). Collected data evidenced the hysteresis behavior of ambient particles and variability in both DRH and CRH between the two seasons. Summer samples showed higher DRH and CRH (on average 71.4 ± 1.0% RH and 62.6 ± 1.2% RH, respectively) than the winter ones (on average 55.2 ± 0.7% RH and 46.9 ± 0.6% RH). This behavior was related to the higher content of sulfates during the summer season. Conversely, the mass hygroscopic growth factor at 90% RH was higher for winter samples (2.76 ± 0.06) with respect to the summer ones (1.91 ± 0.11). Since hysteresis behavior affects optical properties of aerosols, when RH conditions are within the loop, the hygroscopic growth factor could be assigned in a wrong way. Thus, the growth factor was calculated within the hysteresis loop for both upper and lower branches: results showed that difference in hygroscopic growth factor could reach up the 24%.

  8. Intercomparison of aerosol optical parameters from WALI and R-MAN510 aerosol Raman lidars in the framework of HyMeX campaign

    NASA Astrophysics Data System (ADS)

    Boytard, Mai-Lan; Royer, Philippe; Chazette, Patrick; Shang, Xiaoxia; Marnas, Fabien; Totems, Julien; Bizard, Anthony; Bennai, Baya; Sauvage, Laurent

    2013-04-01

    The HyMeX program (Hydrological cycle in Mediterranean eXperiment) aims at improving our understanding of hydrological cycle in the Mediterranen and at a better quantification and forecast of high-impact weather events in numerical weather prediction models. The first Special Observation Period (SOP1) took place in September/October 2012. During this period two aerosol Raman lidars have been deployed at Menorca Island (Spain) : one Water-vapor and Aerosol Raman LIdar (WALI) operated by LSCE/CEA (Laboratoire des Sciences du Climat et de l'Environnement/Commissariat à l'Energie Atomique) and one aerosol Raman and dual-polarization lidar (R-Man510) developed and commercialized by LEOSPHERE company. Both lidars have been continuously running during the campaign and have provided information on aerosol and cloud optical properties under various atmospheric conditions (maritime background aerosols, dust events, cirrus clouds...). We will present here the results of intercomparisons between R-Man510, and WALI aerosol lidar systems and collocated sunphotometer measurements. Limitations and uncertainties on the retrieval of extinction coefficients, depolarization ratio, aerosol optical depths and detection of atmospheric structures (planetary boundary layer height, aerosol/cloud layers) will be discussed according atmospheric conditions. The results will also be compared with theoretical uncertainty assessed with direct/inverse model of lidar profiles.

  9. Study of Hygroscopic Properties of Aminium Sulfate Particles Using Micro-Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Chu, Y.; Sauerwein, M.; Chan, C. K.

    2014-12-01

    As one of the organic nitrogen species, amines are alkaline compounds ubiquitously detected in the atmosphere. Amines have been found to have the potential to enhance atmospheric new particle formation via forming aminium sulfate salts as much as 1000-fold when compared with ammonia, albeit at relatively low atmospheric contents (Almeida et al., 2013). Hygroscopicity of aminium sulfate particles can affect their cloud condensation nuclei (CCN) activity, light scattering or absorption and reactivity in the atmosphere. However, aerosol thermodynamic models such as Extended Aerosol Thermodynamics Model (E-AIM) assume that aminium ions behave similarly to ammonium ions, thus resulting in inaccuracy in predictinghygroscopicity of such compounds. In this study, Micro-Raman spectroscopy was applied to investigate the hygroscopicity of mono-methylaminium sulfate (MMAS), di-methylaminium sulfate (DMAS), tri-methylaminium sulfate (TMAS) and mono-ethylaminium sulfate (MEAS) particles. Since amine can evaporate from stock solutions, Ion Chromatography was used to determine aminium-to-sulfate ion molar ratio (A/S) of studied particles. Results were compared with literature data (Clegg et al., 2013). Due to amine evaporation upon mixing, A/S of stock solutions for particle generation can be below 2.0. In fact, initial A/S were 1.59, 1.91, 1.33 and 2.00 of MMAS, DMAS, TMAS and MEAS particles respectively. Ultimately A/S decreased to 1.5 and 1.0 for DMAS and TMAS, suggesting di-methylamine (DMA) and tri-methylamine (TMA) evaporated from corresponding particles. A/S of MMAS and MEAS kept relatively constant during the relative humidity (RH) cycle in hygroscopic measurements. Unlike (NH4)2SO4, all studied aminium sulfate particles can take up water at low RH. MMAS and MEAS particles underwent phase transition at around 45% and 20% RH respectively, while particles of other aminium sulfates showed continuous hygroscopic trends. References: Almeida, J. et al., 2013. Nature 502, 359

  10. Results of the South African Cloud-Seeding Experiments Using Hygroscopic Flares.

    NASA Astrophysics Data System (ADS)

    Mather, G. K.; Terblanche, D. E.; Steffens, F. E.; Fletcher, L.

    1997-11-01

    Learjet and the results of the randomized experiment, both of which are supported by numerical condensation-coalescence calculations. There are also indications that the hygroscopic seeding may have an impact upon the dynamics of the treated storms, lengthening their lifetimes by strengthening the coupling of the updraft-downdraft storm propagation mechanism.The apparent sensitivity of rainfall in convective clouds to the aerosol concentration, size, and chemical content may have climatic implications. Higher concentrations of small aerosols produced by pollution, biomass burning, etc., could adversely affect the efficiency of the rainfall process. The negative consequences of this effect would be magnified in regions that depend upon convective storms to provide the bulk of their annual rainfall.

  11. Sources and evolution of cloud-active aerosol in California's Sierra Nevada Mountains

    NASA Astrophysics Data System (ADS)

    Roberts, G. C.; Corrigan, C.; Noblitt, S.; Creamean, J.; Collins, D. B.; Cahill, J. F.; Prather, K. A.; Collett, J. L.; Henry, C.

    2011-12-01

    To assess the sources of cloud-active aerosol and their influence on the hydrological cycle in California, the CalWater Experiment took place in winter 2011 in the foothills of the Sierra Nevada Mountains. During this experiment, we coupled the capabilities of demonstrated miniaturized instrumentation - cloud condensation nuclei (CCN), water condensation nuclei (WCN) and microchip capillary electrophoresis (MCE) - to provide direct chemical measurements of cloud active aerosols. Ion concentrations of CCN droplets attribute the anthropogenic, marine and secondary organic contributions to cloud-active aerosols. Detailed spectra from an Aerosol-Time-of-Flight Mass Spectrometer provide additional information on the sources of aerosol. Storm fronts and changes in atmospheric boundary layer brought aerosol and anions associated with Central Valley pollution to the field site with CCN concentrations reaching several thousand cm-3. Hygroscopicity parameters indicate aging of the organic fraction during aerosol transport from the Central Valley to the mountains. Otherwise, CCN concentrations were low when high pressure systems prevented boundary layer development and intrusion of the Central Valley pollution to the site. MCE results show that nitrates and sulfates comprise most of the fraction of the aerosol anion mass (PM1). During the passage of storm fronts, which transported pollution from the Central Valley upslope, nitrate concentrations peaked at several μ g m-3. Low supersaturation CCN concentrations coincide with increases in aerosol nitrate, which suggests that nitrate has a role in cloud formation of giant CCN and, furthermore, in precipitation processes in the Sierra Nevada. CCN spectra show large variations depending on the aerosol sources and sometimes exhibit bi-modal distributions with minima at 0.3% Sc -- similar to the so-called 'Hoppel minima' associated to number size distributions. During these bi-modal events, sulfate also increases supporting the

  12. Radiative impact of atmospheric aerosols and clouds

    NASA Astrophysics Data System (ADS)

    Wong, Jeff

    1998-11-01

    The effect of aerosols and clouds on Earth's shortwave radiation budget is studied in this thesis. An expression for the global annual mean radiative forcing due to sulfate aerosols is extended for absorbing aerosols using a two-stream approximation. This expression depends on the backscattering fraction of the aerosol which varies with the effective radius of the aerosol size distribution. This variation leads to a factor of 2.0 variation in the radiative forcing of slightly absorbing aerosols. Water vapor condenses onto hygroscopic aerosols which results in a change in size and a change in the concentration of the chemical components of the aerosol. The original Köhler equation accurately describes the equilibrium size of a hygroscopic aerosol. Use of the modified Köhler equation leads to errors due to its thermodynamically inconsistent nature. On a global annual average, the direct radiative forcing of hygroscopic sulfate aerosol is -0.69 W m-2. Over highly polluted regions, the local radiative forcing can be as high as -7 W m-2 which is comparable to the forcing due to increased greenhouse gas concentrations. Using a plane-parallel model, an analytical expression is derived for the cloud radiative forcing ratio which is used as a measure of enhanced shortwave radiation absorption of clouds. With this model, high values of this ratio can be achieved by thick clouds with absorptances of approximately 0.3. High values of the ratio can also be obtained with low level clouds if the transmittance of the atmosphere above the cloud is reduced to approximately 0.8. This can be achieved by a high concentration of strongly absorbing aerosols.

  13. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    DOE PAGESBeta

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-14

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed tomore » OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions

  14. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    DOE PAGESBeta

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-06

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH andmore » O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  15. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging

  16. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-01

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical

  17. Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments

    NASA Astrophysics Data System (ADS)

    Kim, J.; Ahlm, L.; Yli-Juuti, T.; Lawler, M.; Keskinen, H.; Tröstl, J.; Schobesberger, S.; Duplissy, J.; Amorim, A.; Bianchi, F.; Donahue, N. M.; Flagan, R. C.; Hakala, J.; Heinritzi, M.; Jokinen, T.; Kürten, A.; Laaksonen, A.; Lehtipalo, K.; Miettinen, P.; Petäjä, T.; Rissanen, M. P.; Rondo, L.; Sengupta, K.; Simon, M.; Tomé, A.; Williamson, C.; Wimmer, D.; Winkler, P. M.; Ehrhart, S.; Ye, P.; Kirkby, J.; Curtius, J.; Kulmala, M.; Lehtinen, K. E. J.; Smith, J. N.; Riipinen, I.; Virtanen, A.

    2015-07-01

    Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In particular, when the concentrations of sulfuric acid was 5.1 × 106 molecules cm-3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (κDMAS ~ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were

  18. Impact of the March 2009 dust event in Saudi Arabia on aerosol optical properties, meteorological parameters, sky temperature and emissivity

    NASA Astrophysics Data System (ADS)

    Maghrabi, A.; Alharbi, B.; Tapper, N.

    2011-04-01

    On 10th March 2009 a widespread and severe dust storm event that lasted several hours struck Riyadh, and represented one of the most intense dust storms experienced in Saudi Arabia in the last two decades. This short-lived storm caused widespread and heavy dust deposition, zero visibility and total airport shutdown, as well as extensive damage to buildings, vehicles, power poles and trees across the city of Riyadh. Changes in Meteorological parameters, aerosol optical depth (AOD), Angstrom exponent α, infrared (IR) sky temperature and atmospheric emissivity were investigated before, during, and after the storm. The analysis showed significant changes in all of the above parameters due to this event. Shortly after the storm arrived, air pressure rapidly increased by 4 hPa, temperature decreased by 6 °C, relative humidly increased from 10% to 30%, the wind direction became northerly and the wind speed increased to a maximum of 30 m s -1. AOD at 550 nm increased from 0.396 to 1.71. The Angstrom exponent α rapidly decreased from 0.192 to -0.078. The mean AOD at 550 nm on the day of the storm was 0.953 higher than during the previous clear day, while α was -0.049 in comparison with 0.323 during the previous day. Theoretical simulations using SMART software showed remarkable changes in both spectral and broadband solar radiation components. The global and direct radiation components decreased by 42% and 68%, respectively, and the diffuse components increased by 44% in comparison with the previous clear day. IR sky temperatures and sky emissivity increased by 24 °C and 0.3, respectively, 2 h after the arrival of the storm. The effect of aerosol loading by the storm on IR atmospheric emission was investigated using MODTRAN software. It was found that the effect of aerosols caused an increase of the atmospheric emission in the atmospheric window (8-14 μm) such that the window emissions resembled those of a blackbody and the atmospheric window was almost closed.

  19. Influence of atmospheric parameters on vertical profiles and horizontal transport of aerosols generated in the surf zone

    NASA Astrophysics Data System (ADS)

    Kusmierczyk-Michulec, J.; Tedeschi, G.; Van Eijk, A. M. J.; Piazzola, J.

    2013-10-01

    The vertical and horizontal transport of aerosols generated over the surf zone is discussed. Experimental data were collected during the second campaign of the Surf Zone Aerosol Experiment that took place in Duck NC (USA) in November 2007. The Empirical Orthogonal Function (EOF) method was used to analyze the vertical concentration gradients, and allowed separating the surf aerosols from aerosols advected from elsewhere. The numerical Marine Aerosol Concentration Model (MACMod) supported the analysis by confirming that the concentration gradients are more pronounced under stable conditions and that aerosol plumes are then more confined to the surface. The model also confirmed the experimental observations made during two boat runs along the offshore wind vector that surf-generated aerosols are efficiently advected out to sea over several tens of kilometers.

  20. Parametric study of the cyclic behaviour of a hygroscopic matrix in a desiccant airflow system

    NASA Astrophysics Data System (ADS)

    Ruivo, C. R.; Costa, J. J.; Figueiredo, A. R.

    2011-09-01

    The study of the transport phenomena in desiccant airflow systems has been addressed in numerous research works, some of them concerning combined processes of cooling, dehumidification and energy recovery. In this paper a detailed numerical model is used to simulate the behaviour of a parallel-plate channel, cyclically exposed to two airflows with different inlet conditions, the plate being composed by a substrate and a desiccant porous layer. The modelled channel is considered to be representative of a real channel of a hygroscopic matrix that is operating at steady state regime, like it occurs in desiccant or enthalpy rotors. The numerical results are treated in order to represent the global behaviour of the hygroscopic rotor under steady state conditions. Results of a parametric study are presented as maps of isovalues of the heat and mass transfer rates and of the outlet states of both airflows, considering channels of distinct wall thickness, of different thickness of the desiccant and the subtract layers, together with wide ranges of the rotation speed and of the wheel partition. The mapped results presented provide an overview of the operation characteristics of hygroscopic rotors, allowing a quick determination of the optimum range of values for relevant parameters, such as the rotation speed and the wheel partition. The model is thus an interesting tool for design and manufacture purposes of enthalpy and desiccant wheels.

  1. Laboratory investigations of mixed organic/inorganic particles: Ice nucleation and optical hygroscopic growth

    NASA Astrophysics Data System (ADS)

    Beaver, Melinda R.

    The interactions of ambient aerosol particles with the atmosphere influence global climate and local visibility. Many of these atmospheric interactions are determined by the chemical composition of the aerosol particles. Ice nucleation in the upper troposphere is influenced and modified by the presence of anthropogenic aerosol particles. Also, interactions between particles and solar radiation are influenced by hygroscopic growth upon humidification. This thesis contains laboratory investigations into the role organic compounds play in ice nucleation and optical hygroscopic growth. Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10) and ketones (C 3 and C9) on ice nucleation in sulfuric acid aerosols. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. The physical properties of the organic compounds (primarily the solubility and melting point) were found to play a dominant role in determining the inferred mode of nucleation (homogenous or heterogeneous) and the specific freezing temperatures observed. Overall, very soluble, low-melting organics, such as acetone and propanal, caused a decrease in aerosol ice nucleation temperatures when compared with aqueous sulfuric acid aerosol. In contrast, sulfuric acid particles exposed to organic compounds of eight carbons and greater, of much lower solubility and higher melting temperatures, nucleate ice at temperatures above aqueous sulfuric acid aerosols. Organic compounds of intermediate carbon chain length, C4-C7, (of intermediate solubility and melting temperatures) nucleated ice at the same temperature as aqueous sulfuric acid aerosols. Light extinction by atmospheric particles is strongly dependent on the size, chemical composition, and water content of the aerosol. Since light extinction by particles directly impacts climate and visibility, measurements of

  2. Neural network radiative transfer solvers for the generation of high resolution solar irradiance spectra parameterized by cloud and aerosol parameters

    NASA Astrophysics Data System (ADS)

    Taylor, M.; Kosmopoulos, P. G.; Kazadzis, S.; Keramitsoglou, I.; Kiranoudis, C. T.

    2016-01-01

    This paper reports on the development of a neural network (NN) model for instantaneous and accurate estimation of solar radiation spectra and budgets geared toward satellite cloud data using a ≈2.4 M record, high-spectral resolution look up table (LUT) generated with the radiative transfer model libRadtran. Two NN solvers, one for clear sky conditions dominated by aerosol and one for cloudy skies, were trained on a normally-distributed and multiparametric subset of the LUT that spans a very broad class of atmospheric and meteorological conditions as inputs with corresponding high resolution solar irradiance target spectra as outputs. The NN solvers were tested by feeding them with a large (10 K record) "off-grid" random subset of the LUT spanning the training data space, and then comparing simulated outputs with target values provided by the LUT. The NN solvers demonstrated a capability to interpolate accurately over the entire multiparametric space. Once trained, the NN solvers allow for high-speed estimation of solar radiation spectra with high spectral resolution (1 nm) and for a quantification of the effect of aerosol and cloud optical parameters on the solar radiation budget without the need for a massive database. The cloudy sky NN solver was applied to high spatial resolution (54 K pixel) cloud data extracted from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) onboard the geostationary Meteosat Second Generation 3 (MSG3) satellite and demonstrated that coherent maps of spectrally-integrated global horizontal irradiance at this resolution can be produced on the order of 1 min.

  3. A Study of Cloud Processing of Organic Aerosols Using Models and CHAPS Data

    SciTech Connect

    Ervens, Barbara

    2012-01-17

    The main theme of our work has been the identification of parameters that mostly affect the formation and modification of aerosol particles and their interaction with water vapor. Our detailed process model studies led to simplifications/parameterizations of these effects that bridge detailed aerosol information from laboratory and field studies and the need for computationally efficient expressions in complex atmospheric models. One focus of our studies has been organic aerosol mass that is formed in the atmosphere by physical and/or chemical processes (secondary organic aerosol, SOA) and represents a large fraction of atmospheric particulate matter. Most current models only describe SOA formation by condensation of low volatility (or semivolatile) gas phase products and neglect processes in the aqueous phase of particles or cloud droplets that differently affect aerosol size and vertical distribution and chemical composition (hygroscopicity). We developed and applied models of aqueous phase SOA formation in cloud droplets and aerosol particles (aqSOA). Placing our model results into the context of laboratory, model and field studies suggests a potentially significant contribution of aqSOA to the global organic mass loading. The second focus of our work has been the analysis of ambient data of particles that might act as cloud condensation nuclei (CCN) at different locations and emission scenarios. Our model studies showed that the description of particle chemical composition and mixing state can often be greatly simplified, in particular in aged aerosol. While over the past years many CCN studies have been successful performed by using such simplified composition/mixing state assumptions, much more uncertainty exists in aerosol-cloud interactions in cold clouds (ice or mixed-phase). Therefore we extended our parcel model that describes warm cloud formation by ice microphysics and explored microphysical parameters that determine the phase state and lifetime of

  4. DEPOSITION PATTERNS OF AEROSOLIZED DRUGS WITHIN HUMAN LUNGS: EFFECTS OF VENTILATORY PARAMETERS

    EPA Science Inventory

    An analytical model is used to study the effects of ventilatory parameters on particle deposition patterns within the human lung. ased upon fluid dynamics considerations (Reynolds numbers), an original method of partitioning the lung is presented. he model is validated by compari...

  5. Impact of Particle Generation Method on the Apparent Hygroscopicity of Insoluble Mineral Particles

    SciTech Connect

    Sullivan, Ryan; Moore, Meagan J.; Petters, Markus D.; Kreidenweis, Sonia M.; Qafoku, Odeta; Laskin, Alexander; Roberts, Greg C.; Prather, Kimberly A.

    2010-07-28

    Atmospheric mineral dust particles represent a major component of tropospheric aerosol mass and provide a reactive surface for heterogeneous reactions with trace atmospheric gases (Dentener et al. 1996).Heterogeneous processes alter the chemical balance of the atmosphere and also modify the physicochemical properties of mineral dust particles (Bauer et al. 2004). Organic and inorganic vapors can react with or partition to dust particles and alter their chemical composition (Al-Hosney et al. 2005; Laskin et al. 2005a, 2005b; Liu et al. 2008; Sullivan et al. 2007, 2009a; Sullivan and Prather 2007; Usher et al. 2003). Calcite (CaCO3) is one of the most reactive components of mineral dust, readily reacting with acidic gases. The fraction of CaCO3 in total dust mineralogy displays large variations between desert regions and other regions of the world as well as between individual mineral particles (Claquin et al. 1999; Jeong 2008; Laskin et al. 2005b; Sullivan et al. 2007). Through reactions with acidic gases CaCO3 can be converted to soluble hygroscopic products including CaCl2 and Ca(NO3)2, and sparingly soluble, non-hygroscopic products including CaSO4 and CaC2O4 (Krueger et al. 2004; Liu et al. 2008; Sullivan et al. 2009a, 2009b).

  6. Comparison of Hygroscopicity, Volatility, and Mixing State of Submicrometer Particles between Cruises over the Arctic Ocean and the Pacific Ocean.

    PubMed

    Kim, Gibaek; Cho, Hee-Joo; Seo, Arom; Kim, Dohyung; Gim, Yeontae; Lee, Bang Yong; Yoon, Young Jun; Park, Kihong

    2015-10-20

    Ship-borne measurements of ambient aerosols were conducted during an 11 937 km cruise over the Arctic Ocean (cruise 1) and the Pacific Ocean (cruise 2). A frequent nucleation event was observed during cruise 1 under marine influence, and the abundant organic matter resulting from the strong biological activity in the ocean could contribute to the formation of new particles and their growth to a detectable size. Concentrations of particle mass and black carbon increased with increasing continental influence from polluted areas. During cruise 1, multiple peaks of hygroscopic growth factor (HGF) of 1.1-1.2, 1.4, and 1.6 were found, and higher amounts of volatile organic species existed in the particles compared to that during cruise 2, which is consistent with the greater availability of volatile organic species caused by the strong oceanic biological activity (cruise 1). Internal mixtures of volatile and nonhygroscopic organic species, nonvolatile and less-hygroscopic organic species, and nonvolatile and hygroscopic nss-sulfate with varying fractions can be assumed to constitute the submicrometer particles. On the basis of elemental composition and morphology, the submicrometer particles were classified into C-rich mixture, S-rich mixture, C/S-rich mixture, Na-rich mixture, C/P-rich mixture, and mineral-rich mixture. Consistently, the fraction of biological particles (i.e., P-containing particles) increased when the ship traveled along a strongly biologically active area. PMID:26389581

  7. Hygroscopic Properties of Internally Mixed Particles Composed of NaCl and Water-Soluble Organic Acids

    SciTech Connect

    Ghorai, Suman; Wang, Bingbing; Tivanski, Alexei V.; Laskin, Alexander

    2014-02-18

    Atmospheric aging of naturally emitted marine aerosol often leads to formation of internally mixed particles composed of sea salts and water soluble organic compounds of anthropogenic origin. Mixing of sea salt and organic components has profound effects on the evolving chemical composition and hygroscopic properties of the resulted particles, which are poorly understood. Here, we have studied chemical composition and hygroscopic properties of laboratory generated NaCl particles mixed with malonic acid (MA) and glutaric acid (GA) at different molar ratios using micro-FTIR spectroscopy and X-ray elemental microanalysis.Hygroscopic properties of inte rnally mixed NaCl and organic acid particles were distinctly different from pure components and varied significantly with the type and amount of organic compound present. Experimental results were in a good agreement with the AIM modeling calculations of gas/liquid/solid partitioning in studied systems. X-ray elemental microanalysis of particles showed that Cl/Na ratio decreased with increasing organic acid component in the particles with MA yielding lower ratios relative to GA. We attribute the depletion of chloride to the formation of Na-malonate and Na-glutarate salts resulted by HCl evaporation from dehydrating particles.

  8. Hygroscopic properties of internally mixed particles composed of NaCl and water-soluble organic acids.

    PubMed

    Ghorai, Suman; Wang, Bingbing; Tivanski, Alexei; Laskin, Alexander

    2014-02-18

    Atmospheric aging of naturally emitted marine aerosol often leads to formation of internally mixed particles composed of sea salts and water-soluble organic compounds of anthropogenic origin. Mixing of sea salt and organic components has profound effects on the evolving chemical composition and hygroscopic properties of the resulted particles, which are poorly understood. Here, we have studied chemical composition and hygroscopic properties of laboratory generated NaCl particles mixed with malonic acid (MA) and glutaric acid (GA) at different molar ratios using micro-FTIR spectroscopy, atomic force microscopy, and X-ray elemental microanalysis. Hygroscopic properties of internally mixed NaCl and organic acid particles were distinctly different from pure components and varied significantly with the type and amount of organic compound present. Experimental results were in a good agreement with the AIM modeling calculations of gas/liquid/solid partitioning in studied systems. X-ray elemental microanalysis of particles showed that Cl/Na ratio decreased with increasing organic acid component in the particles with MA yielding lower ratios relative to GA. We attribute the depletion of chloride to the formation of sodium malonate and sodium glutarate salts resulted by HCl evaporation from dehydrating particles. PMID:24437520

  9. Hygroscopic weight gain of pollen grains from Juniperus species

    NASA Astrophysics Data System (ADS)

    Bunderson, Landon D.; Levetin, Estelle

    2015-05-01

    Juniperus pollen is highly allergenic and is produced in large quantities across Texas, Oklahoma, and New Mexico. The pollen negatively affects human populations adjacent to the trees, and since it can be transported hundreds of kilometers by the wind, it also affects people who are far from the source. Predicting and tracking long-distance transport of pollen is difficult and complex. One parameter that has been understudied is the hygroscopic weight gain of pollen. It is believed that juniper pollen gains weight as humidity increases which could affect settling rate of pollen and thus affect pollen transport. This study was undertaken to examine how changes in relative humidity affect pollen weight, diameter, and settling rate. Juniperus ashei, Juniperus monosperma, and Juniperus pinchotii pollen were applied to greased microscope slides and placed in incubation chambers under a range of temperature and humidity levels. Pollen on slides were weighed using an analytical balance at 2- and 6-h intervals. The size of the pollen was also measured in order to calculate settling rate using Stokes' Law. All pollen types gained weight as humidity increased. The greatest settling rate increase was exhibited by J. pinchotii which increased by 24 %.

  10. Hygroscopic weight gain of pollen grains from Juniperus species.

    PubMed

    Bunderson, Landon D; Levetin, Estelle

    2015-05-01

    Juniperus pollen is highly allergenic and is produced in large quantities across Texas, Oklahoma, and New Mexico. The pollen negatively affects human populations adjacent to the trees, and since it can be transported hundreds of kilometers by the wind, it also affects people who are far from the source. Predicting and tracking long-distance transport of pollen is difficult and complex. One parameter that has been understudied is the hygroscopic weight gain of pollen. It is believed that juniper pollen gains weight as humidity increases which could affect settling rate of pollen and thus affect pollen transport. This study was undertaken to examine how changes in relative humidity affect pollen weight, diameter, and settling rate. Juniperus ashei, Juniperus monosperma, and Juniperus pinchotii pollen were applied to greased microscope slides and placed in incubation chambers under a range of temperature and humidity levels. Pollen on slides were weighed using an analytical balance at 2- and 6-h intervals. The size of the pollen was also measured in order to calculate settling rate using Stokes' Law. All pollen types gained weight as humidity increased. The greatest settling rate increase was exhibited by J. pinchotii which increased by 24 %. PMID:25008113

  11. Use of Observation-Based Aerosol Fields for Detailed Cloud-Scale Modeling Studies

    NASA Astrophysics Data System (ADS)

    Fridlind, A. M.; Vogelmann, A. M.; Ackerman, A. S.; Endo, S.

    2014-12-01

    Within the realm of detailed large-eddy simulation studies with size-resolved microphysics, substantial uncertainties exist regarding the ability of any given model to accurately reproduce basic aspects of cloud microphysics that interact with ambient aerosol properties, such as precipitation formation and evolution. Modeling studies intended to reproduce specific observed cloud fields must also to some degree simplify the complexity of aerosol conditions, and usually lack sufficient measurements to well constrain the most relevant aerosol properties. Here we describe derivation and use of spatiotemporally varying fields of multi-modal aerosol size distributions for 60-hour simulations of boundary-layer clouds observed over Oklahoma during the RACORO campaign. Cases include forced as well as freely convecting shallow clouds, and some warm precipitation. We investigate the sensitivity of simulations to observation-derived aerosol inputs, including hygroscopicity parameter and size distribution properties. Sensitivity is examined in the context of the ability of the simulations to accurately reproduce relevant macrophysical and microphysical cloud properties observed, including droplet size dispersion.

  12. The dependence of aerosol light-scattering on RH over the Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Hegg, D. A.; Covert, D. S.; Crahan, K.; Jonssen, H.

    2002-04-01

    Measurements of the relative humidity dependence of aerosol light scattering are reported from three experimental venues over the Pacific Ocean. The measurement platform utilized was the CIRPAS Twin Otter aircraft. Results are compared with previous measurements at other locales and with theoretical models. The relatively low values of hygroscopicity obtained in marine air are consistent with a substantial organic component to the aerosol.

  13. Carbonaceous Aerosols and Radiative Effects Study (CARES), g1-aircraft, sedlacek sp2

    DOE Data Explorer

    Sedlacek, Art

    2011-08-30

    The primary objective of the Carbonaceous Aerosol and Radiative Effects Study (CARES) in 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume.

  14. Evolution of Organic Aerosols in the Atmosphere

    NASA Astrophysics Data System (ADS)

    Jimenez, J. L.; Canagaratna, M. R.; Donahue, N. M.; Prevot, A. S. H.; Zhang, Q.; Kroll, J. H.; DeCarlo, P. F.; Allan, J. D.; Coe, H.; Ng, N. L.; Aiken, A. C.; Docherty, K. S.; Ulbrich, I. M.; Grieshop, A. P.; Robinson, A. L.; Duplissy, J.; Smith, J. D.; Wilson, K. R.; Lanz, V. A.; Hueglin, C.; Sun, Y. L.; Tian, J.; Laaksonen, A.; Raatikainen, T.; Rautiainen, J.; Vaattovaara, P.; Ehn, M.; Kulmala, M.; Tomlinson, J. M.; Collins, D. R.; Cubison, M. J.; Dunlea, J.; Huffman, J. A.; Onasch, T. B.; Alfarra, M. R.; Williams, P. I.; Bower, K.; Kondo, Y.; Schneider, J.; Drewnick, F.; Borrmann, S.; Weimer, S.; Demerjian, K.; Salcedo, D.; Cottrell, L.; Griffin, R.; Takami, A.; Miyoshi, T.; Hatakeyama, S.; Shimono, A.; Sun, J. Y.; Zhang, Y. M.; Dzepina, K.; Kimmel, J. R.; Sueper, D.; Jayne, J. T.; Herndon, S. C.; Trimborn, A. M.; Williams, L. R.; Wood, E. C.; Middlebrook, A. M.; Kolb, C. E.; Baltensperger, U.; Worsnop, D. R.

    2009-12-01

    Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

  15. Atmospheric aerosols parameters behavior and its association with meteorological activities variables over western Indian tropical semi-urban site i.e., Udaipur

    NASA Astrophysics Data System (ADS)

    Vyas, B. M.; Saxenna, Abhishek; Panwar, Chhagan

    2016-05-01

    The present study has been focused to the identify the role of meteorological processes on changing the monthly variation of AOD at 550nm, Angstrom Exponent Coefficient (AEC, 440/670nm) and Cloud Effective Radius (CER, μm) measured during January, 2005 to December 2013 over western Indian location i.e., Udaipur (24.6° N, 73.7° E, 560 m amsl). The monthly variation of AOD 550nm, AEC and during entire study period have shown the strong combined influence of different local surface meteorological parameters in varying amplitude with different nature. The higher values of wind speed, ambient surface temperature, planetary boundary layer, and favorable wind direction coming from desert and oceanic region (W and SW) may be recognize as some of possible factor to exhibit the higher aerosols loading of bigger aerosol size particles in pre-monsoon. These meteorological factors seem also to be plausible responsible factors for drastically reducing the cloud effective radius in pre-monsoon season. In contrary to this, in winter, lower atmospheric aerosols burden and more abundance of fine size particles along with increasing the CER sizes also seem to be influenced and governed by the adverse nature of meteorological conditions such lowering the PBL, T, WS as well as with air pollutants transportation by wind from the N and NE region, of high aerosols loading of fine size particles as anthropogenic aerosols located far away to the observing site.

  16. Gas/Aerosol partitioning: a simplified method for global modeling

    NASA Astrophysics Data System (ADS)

    Metzger, S. M.

    2000-09-01

    The main focus of this thesis is the development of a simplified method to routinely calculate gas/aerosol partitioning of multicomponent aerosols and aerosol associated water within global atmospheric chemistry and climate models. Atmospheric aerosols are usually multicomponent mixtures, partly composed of acids (e.g. H2SO4, HNO3), their salts (e.g. (NH4)2SO4, NH4NO3, respectively), and water. Because these acids and salts are highly hygroscopic, water, that is associated with aerosols in humid environments, often exceeds the total dry aerosol mass. Both the total dry aerosol mass and the aerosol associated water are important for the role of atmospheric aerosols in climate change simulations. Still, multicomponent aerosols are not yet routinely calculated within global atmospheric chemistry or climate models. The reason is that these particles, especially volatile aerosol compounds, require a complex and computationally expensive thermodynamical treatment. For instance, the aerosol associated water depends on the composition of the aerosol, which is determined by the gas/liquid/solid partitioning, in turn strongly dependent on temperature, relative humidity, and the presence of pre-existing aerosol particles. Based on thermodynamical relations such a simplified method has been derived. This method is based on the assumptions generally made by the modeling of multicomponent aerosols, but uses an alternative approach for the calculation of the aerosol activity and activity coefficients. This alternative approach relates activity coefficients to the ambient relative humidity, according to the vapor pressure reduction and the generalization of Raoult s law. This relationship, or simplification, is a consequence of the assumption that the aerosol composition and the aerosol associated water are in thermodynamic equilibrium with the ambient relative humidity, which determines the solute activity and, hence, activity coefficients of a multicomponent aerosol mixture

  17. Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect

    SciTech Connect

    Wang, J. X.; Lee, Y.- N.; Daum, Peter H.; Jayne, John T.; Alexander, M. L.

    2008-11-03

    Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/ Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.2% supersaturation to those predicted based on size distribution and chemical composition using K¨ohler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization.

  18. [Investigation of Aerosol Mixed State and CCN Activity in Nanjing].

    PubMed

    Zhu, Lin; Ma, Yan; Zheng, Jun; Li, Shi-zheng; Wang, Li-peng

    2016-04-15

    During 11-18 September 2014, the size-resolved aerosol Cloud Condensation Nuclei (CCN) activity and mixing state were measured using Cloud Condensation Nuclei Counter (CCNC), Aerosol Particle Mass (APM) and Scanning Mobility Particle Sizer (SMPS). The results showed that aerosols mainly existed as an internal mixture. For 76, 111, 138 and 181 nm particles, black carbon (BC) accounted for 5.4%, 10%, l0.7% and 6.7% of the particle mass, but as high as 51%, 57%, 70% and 59% of the particle number concentrations, respectively, suggesting that BC was a type of important condensation nuclei in the atmosphere and made significant contributions to particle numbers. The occasionally observed external mixtures were mainly present in 111 and 138 nm particles. The critical supersaturation was 0.25%, 0.13%, 0.06% and 0.015% for 76, 111, 138 and 181 nm particles, respectively. Precipitation and haze had significant effects on the particle CCN activity. The hygroscopicity parameter K was 0.37, 0.29 and 0.39 in rainy, clear and hazy days, respectively. Particle density and CCN activity were impacted by chemical compositions. Compared with clear days, higher contents of inorganic salts and lower contents of organics were found on hazy days, accompanied by lower particle density and higher CCN activity. PMID:27548938

  19. Aerosol-cloud interactions studied with the chemistry-climate model EMAC

    NASA Astrophysics Data System (ADS)

    Chang, D. Y.; Tost, H.; Steil, B.; Lelieveld, J.

    2014-08-01

    This study uses the EMAC atmospheric chemistry-climate model to simulate cloud properties and estimate cloud radiative effects induced by aerosols. We have tested two prognostic cloud droplet nucleation parameterizations, i.e., the standard STN (osmotic coefficient model) and hybrid (HYB, replacing the osmotic coefficient by the κ hygroscopicity parameter) schemes to calculate aerosol hygroscopicity and critical supersaturation, and consider aerosol-cloud feedbacks with a focus on warm clouds. Both prognostic schemes (STN and HYB) account for aerosol number, size and composition effects on droplet nucleation, and are tested in combination with two different cloud cover parameterizations, i.e., a relative humidity threshold and a statistical cloud cover scheme (RH-CLC and ST-CLC). The use of either STN and HYB leads to very different cloud radiative effects, particularly over the continents. The STN scheme predicts highly effective CCN activation in warm clouds and hazes/fogs near the surface. The enhanced CCN activity increases the cloud albedo effect of aerosols and cools the Earth's surface. The cooler surface enhances the hydrostatic stability of the lower continental troposphere and thereby reduces convection and convective precipitation. In contrast, the HYB simulations calculate lower, more realistic CCN activation and consequent cloud albedo effect, leading to relatively stronger convection and high cloud formation. The enhanced high clouds increase greenhouse warming and moderate the cooling effect of the low clouds. With respect to the cloud radiative effects, the statistical ST-CLC scheme shows much higher sensitivity to aerosol-cloud coupling for all continental regions than the RH-CLC threshold scheme, most pronounced for low clouds but also for high clouds. Simulations of the short wave cloud radiative effect at the top of the atmosphere in ST-CLC are a factor of 2-8 more sensitive to aerosol coupling than the RH-CLC configurations. The long wave

  20. Arrange and average algorithm for the retrieval of aerosol microphysical parameters from HSRL-2. Comparison with in-situ measurements during DISCOVER-AQ California and Texas (2013)

    NASA Astrophysics Data System (ADS)

    Chemyakin, E.; Sawamura, P.; Mueller, D.; Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Scarino, A. J.; Hair, J. W.; Berkoff, T.; Cook, A. L.; Harper, D. B.; Seaman, S. T.

    2015-12-01

    Although aerosols are only a fairly minor constituent of Earth's atmosphere they are able to affect its radiative energy balance significantly. Light detection and ranging (lidar) instruments have the potential to play a crucial role in atmospheric research as only these instruments provide information about aerosol properties at a high vertical resolution. We are exploring different algorithmic approaches to retrieve microphysical properties of aerosols using lidar. Almost two decades ago we started with inversion techniques based on Tikhonov's regularization that became a reference point for the improvement of retrieval capabilities of inversion algorithms. Recently we began examining the potential of the "arrange and average" scheme, which relies on a look-up table of optical and microphysical aerosol properties. The future combination of these two different inversion schemes may help us to improve the accuracy of the microphysical data products.The novel arrange and average algorithm was applied to retrieve aerosol optical and microphysical parameters using NASA Langley Research Center (LaRC) High Spectral Resolution Lidar (HSRL-2) data. HSRL-2 is the first airborne HSRL system that is able to provide advanced datasets consisting of backscatter coefficients at 355, 532, and 1064 nm, and extinction coefficients at 355 and 532 nm as input information for aerosol microphysical retrievals. HSRL-2 was deployed on-board NASA LaRC's King Air aircraft during the Deriving Information on Surface Conditions from Column and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaigns over the California Central Valley and Houston. Vertical profiles of aerosol optical properties and size distributions were obtained from in-situ instruments on-board the NASA's P-3B aircraft. As HSRL-2 flew along the same flight track of the P-3B, synergistic measurements and retrievals were obtained by these two independent platforms. We will present an

  1. Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems

    NASA Astrophysics Data System (ADS)

    Massling, A.; Niedermaier, N.; Hennig, T.; Fors, E.; Swietlicki, E.; Ehn, M.; Hämeri, K.; Villani, P.; Laj, P.; Good, N.; McFiggans, G.; Wiedensohler, A.

    2010-02-01

    The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyzers (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonize H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulfate particles or an external mixture of ammonium sulfate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. With regard to RH uncertainties, the H-TDMA systems showed deviations up to 4.5% RH from the set point at RH=90% investigating the hygroscopic growth of ammonium sulfate particles and comparing the results with theory. The evaluation of number fractions investigating an externally mixed aerosol delivered differences up to +/-8% in calculated number fraction for one and the same aerosol type. We analysed the datasets of the different H-TDMAs with one fitting routine to investigate differences caused by the different data evaluation procedures. The results showed that the differences were reduced from +12/-13% to +8/-6%. We can conclude here that a common data evaluation procedure to determine the number fraction of externally mixed aerosols will improve the comparability of H-TDMA measurements. We finally recommend, to ensure a good calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the RH control unit and the second DMA and to monitor those temperatures as accurately as 0.2 °C. For a correct determination of external

  2. [Surgical hygroscopic bandages for amputations, secreting wounds and diabetes foot].

    PubMed

    Topolav, J; Kirov, G; Markov, G; Girov, K; Nedkov, P; Georgieva, A

    2010-01-01

    The authors adopt in clinical practice using of sterile hygroscopic wound dressings 'pampers type'. They use these dressings in 113 patients. The appropriate patients are these with limbs amputations, diabetic foot, suppurative and plenty secreting deep wounds, atonite and decubital wounds. The dressings are sterilised using paraformaldehyde sterilization which do not injure the synthetic materials. The hygroscopic dressings are non- allergic and are well tolerated by the patients. Using these dressings facilitate the medical team work and help to reduce the contamination of the hospital linen and the patients coverlet. They help for accelerating the wound healing process. They are also economic effective by reducing the amount of used dressing material. PMID:21972719

  3. Evolution of aerosol and CCN properties on the Antarctic Peninsula and Southern Ocean during the spring and summer seasons.

    NASA Astrophysics Data System (ADS)

    Corrigan, C.; Roberts, G.; Grant, G.

    2014-12-01

    The Southern Ocean has been identified as one of the key regions that need aerosol measurements to improve our models of global climate change. The Portable AERosol Observing System (PAEROS) was deployed in an extended field campaign to measure CCN and aerosols in Antarctica and the Southern Ocean from October 2013 to mid-March 2014. PAEROS is a lightweight, man-portable instrument package developed at the Scripps Institution of Oceanography for the purpose of collecting autonomous measurements of aerosol and cloud condensation nuclei (CCN) properties in remote and challenging environments. The initial phase involved the PAEROS package sampling onboard the R/V Gould during the five-day transit of the Drake Passage between Punta Arenas, Chile and Palmer Station on the Antarctic Peninsula. Upon arrival at Palmer Station, PAEROS was transferred to land and installed on top of a hill about 500 m from the main buildings. For five months, aerosol and CCN number concentrations, size distributions, black carbon concentrations, solar fluxes, and meteorological parameters were continuously measured at Palmer Station. The experiment covered most of an austral spring and summer cycle, during which time the sea ice retreated and biological activity flourished along the Antarctic Peninsula. While crossing the Drake Passage, a distinct gradient in aerosol concentrations was observed with increasing distance from South America. At Palmer Station, the total aerosol concentrations showed a seasonal cycle with lowest concentration in air masses originating from the Antarctic continent and highest number concentrations coming from the ocean during the peak of biological activity. Chlorophyll concentrations are routinely measured at Palmer Station and showed peak activity in the month of January 2014. Total aerosol and CCN concentrations increased in late spring (November) as the sea ice recedes from Palmer Station, probably a result of being closer to sea spray and biological activity

  4. Organic aerosol effects on fog droplet spectra

    NASA Astrophysics Data System (ADS)

    Ming, Yi; Russell, Lynn M.

    2004-05-01

    Organic aerosol alters cloud and fog properties through surface tension and solubility effects. This study characterizes the role of organic compounds in affecting fog droplet number concentration by initializing and comparing detailed particle microphysical simulations with two field campaigns in the Po Valley. The size distribution and chemical composition of aerosol were based on the measurements made in the Po Valley Fog Experiments in 1989 and 1998-1999. Two types of aerosol with different hygroscopicity were considered: the less hygroscopic particles, composed mainly of organic compounds, and the more hygroscopic particles, composed mainly of inorganic salts. The organic fraction of aerosol mass was explicitly modeled as a mixture of seven soluble compounds [, 2001] by employing a functional group-based thermodynamic model [, 2002]. Condensable gases in the vapor phase included nitric acid, sulfuric acid, and ammonia. The maximum supersaturation in the simulation is 0.030% and is comparable to the calculation by [1992] inferred from measured residual particle fractions. The minimum activation diameters of the less and more hygroscopic particles are 0.49 μm and 0.40 μm, respectively. The predicted residual particle fractions are in agreement with measurements. The organic components of aerosol account for 34% of the droplet residual particle mass and change the average droplet number concentration by -10-6%, depending on the lowering of droplet surface tension and the interactions among dissolving ions. The hygroscopic growth of particles due to the presence of water-soluble organic compounds enhances the condensation of nitric acid and ammonia due to the increased surface area, resulting in a 9% increase in the average droplet number concentration. Assuming ideal behavior of aqueous solutions of water-soluble organic compounds overestimates the hygroscopic growth of particles and increases droplet numbers by 6%. The results are sensitive to microphysical

  5. Observations of aerosol light scattering, absorption, and particle morphology changes as a function of relative humidity

    NASA Astrophysics Data System (ADS)

    Arnott, W. P.; Lewis, K.; Paredes-Miranda, G.; Winter, S.; Day, D.; Chakrabarty, R.; Moosmuller, H.; Jimenez, J. L.; Ulbrich, I.; Huffman, A.; Onasch, T.; Trimborn, A.; Kreidenweis, S.; Carrico, C.; Wold, C.; Lincoln, E.; Freeborn, P.; Hao, W.; McMeeking, G.

    2006-12-01

    A very interesting case of smoke aerosol with very low single scattering albedo, yet very large hygroscopic growth for scattering is presented. Several samples of chamise (Adenostoma fasciculatum), a common and often dominant species in California chaparral, were recently burned at the USFS Fire Science Laboratory in Missoula Montana, and aerosol optics and chemistry were observed, along with humidity-dependent light scattering, absorption, and particle morphology. Photoacoustic measurements of light absorption by two instruments at 870 nm, one on the dry channel, one on the humidified channel, showed strong reduction of aerosol light absorption with RH above 65 percent, and yet a strong increase in light scattering was observed both at 870 nm and 550 nm with nephelometers. Multispectral measurements of aerosol light absorption indicated an Angstrom coefficient for absorption near unity for the aerosols from chamise combustion. It is argued that the hygroscopic growth of scattering is due to uptake of water by the sulfur bearing aerosol. Furthermore, the reduction of aerosol light absorption is argued to be due to the collapse of chain aggregate aerosol as the RH increases wherein the interior of aerosol does no longer contribute to absorption. Implications for biomass burning in general are that humidity processing of aerosols from this source and others like it tends to substantially increase its single scattering albedo, probably in a non-reversible manner. The chemical pathway to hygroscopicity will be addressed.

  6. Performance of Combination Drug and Hygroscopic Excipient Submicrometer Particles from a Softmist Inhaler in a Characteristic Model of the Airways

    PubMed Central

    Longest, P. Worth; Tian, Geng; Li, Xiang; Son, Yoen-Ju; Hindle, Michael

    2012-01-01

    Excipient enhanced growth (EEG) of inhaled submicrometer pharmaceutical aerosols is a recently proposed method intended to significantly reduce extrathoracic deposition and improve lung delivery. The objective of this study was to evaluate the size increase of combination drug and hygroscopic excipient particles in a characteristic model of the airways during inhalation using both in vitro experiments and CFD simulations. The airway model included a characteristic mouth-throat (MT) and upper tracheobronchial (TB) region through the third bifurcation (B3) and was enclosed in a chamber geometry used to simulate the thermodynamic conditions of the lungs. Both in vitro results and CFD simulations were in close agreement and indicated that EEG delivery of combination submicrometer particles could nearly eliminate MT deposition for inhaled pharmaceutical aerosols. Compared with current inhalers, the proposed delivery approach represents a 1–2 order of magnitude reduction in MT deposition. Transient inhalation was found to influence the final size of the aerosol based on changes in residence times and relative humidity values. Aerosol sizes following EEG when exiting the chamber (2.75–4.61 μm) for all cases of initial submicrometer combination particles were equivalent to or larger than many conventional pharmaceutical aerosols that frequently have MMADs in the range of 2–3 μm. PMID:22820981

  7. Satellite retrieval of aerosol microphysical and optical parameters using neural networks: a new methodology applied to the Sahara desert dust peak

    NASA Astrophysics Data System (ADS)

    Taylor, M.; Kazadzis, S.; Tsekeri, A.; Gkikas, A.; Amiridis, V.

    2014-09-01

    In order to exploit the full-earth viewing potential of satellite instruments to globally characterise aerosols, new algorithms are required to deduce key microphysical parameters like the particle size distribution and optical parameters associated with scattering and absorption from space remote sensing data. Here, a methodology based on neural networks is developed to retrieve such parameters from satellite inputs and to validate them with ground-based remote sensing data. For key combinations of input variables available from the MODerate resolution Imaging Spectro-radiometer (MODIS) and the Ozone Measuring Instrument (OMI) Level 3 data sets, a grid of 100 feed-forward neural network architectures is produced, each having a different number of neurons and training proportion. The networks are trained with principal components accounting for 98% of the variance of the inputs together with principal components formed from 38 AErosol RObotic NETwork (AERONET) Level 2.0 (Version 2) retrieved parameters as outputs. Daily averaged, co-located and synchronous data drawn from a cluster of AERONET sites centred on the peak of dust extinction in Northern Africa is used for network training and validation, and the optimal network architecture for each input parameter combination is identified with reference to the lowest mean squared error. The trained networks are then fed with unseen data at the coastal dust site Dakar to test their simulation performance. A neural network (NN), trained with co-located and synchronous satellite inputs comprising three aerosol optical depth measurements at 470, 550 and 660 nm, plus the columnar water vapour (from MODIS) and the modelled absorption aerosol optical depth at 500 nm (from OMI), was able to simultaneously retrieve the daily averaged size distribution, the coarse mode volume, the imaginary part of the complex refractive index, and the spectral single scattering albedo - with moderate precision: correlation coefficients in the

  8. Estimation of aerosol optical depth and additional atmospheric parameters for the calculation of apparent reflectance from radiance measured by the Airborne Visible/Infrared Imaging Spectrometer

    NASA Technical Reports Server (NTRS)

    Green, Robert O.; Conel, James E.; Roberts, Dar A.

    1993-01-01

    The Airborne Visible/Infrared Imaging Spectrometer (AVIRIS) measures spatial images of the total upwelling spectral radiance from 400 to 2500 nm through 10 nm spectral channels. Quantitative research and application objectives for surface investigations require inversion of the measured radiance of surface reflectance or surface leaving radiance. To calculate apparent surface reflectance, estimates of atmospheric water vapor abundance, cirrus cloud effects, surface pressure elevation, and aerosol optical depth are required. Algorithms for the estimation of these atmospheric parameters from the AVIRIS data themselves are described. From these atmospheric parameters we show an example of the calculation of apparent surface reflectance from the AVIRIS-measured radiance using a radiative transfer code.

  9. Inter-comparison of CALIPSO and CloudSat retrieved profiles of aerosol and cloud microphysical parameters with aircraft profiles over a tropical region

    NASA Astrophysics Data System (ADS)

    Padmakumari, B.; Harikishan, G.; Maheskumar, R. S.

    2016-05-01

    Satellites play a major role in understanding the spatial and vertical distribution of aerosols and cloud microphysical parameters over a large area. However, the inherent limitations in satellite retrievals can be improved through inter-comparisons with airborne platforms. Over the Indian sub-continent, the vertical profiles retrieved from space-borne lidar such as CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) on board the satellite CALIPSO and Cloud Profiling Radar (CPR) on board the satellite CloudSat were inter- compared with the aircraft observations conducted during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX). In the absence of high clouds, both aircraft and CALIOP showed similar features of aerosol layering and water-ice cloud signatures. As CALIOP could not penetrate the thick clouds, the aerosol information below the cloud is missed. While the aircraft could measure high concentrations below the cloud base and above the low clouds in the presence of high clouds. The aircraft derived liquid water content (LWC) and droplet effective radii (Re) showed steady increase from cloud base to cloud top with a variable cloud droplet number concentration (CDNC). While the CloudSat derived LWC, CDNC and Re showed increase from the cloud top to cloud base in contradiction to the aircraft measurements. The CloudSat profiles are underestimated as compared to the corresponding aircraft profiles. Validation of satellite retrieved vertical profiles with aircraft measurements is very much essential over the tropics to improve the retrieval algorithms and to constrain the uncertainties in the regional cloud parameterization schemes.

  10. Hygrosopicity measurements of aerosol particles in the San Joaquin Valley, CA, Baltimore, MD, and Golden, CO

    NASA Astrophysics Data System (ADS)

    Orozco, Daniel; Beyersdorf, A. J.; Ziemba, L. D.; Berkoff, T.; Zhang, Q.; Delgado, R.; Hennigan, C. J.; Thornhill, K. L.; Young, D. E.; Parworth, C.; Kim, H.; Hoff, R. M.

    2016-06-01

    Aerosol hygroscopicity was investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (σscat) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (10 January to 6 February 2013), Baltimore, MD (3-30 July 2013), and Golden, CO (12 July to 10 August 2014). Observations in Porterville and Golden were part of the NASA-sponsored Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality project. The measured σscat under varying RH in the three sites was combined with ground aerosol extinction, PM2.5 mass concentrations, and particle composition measurements and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of σscat(RH) at a certain RH divided by σscat at a dry value, was used to evaluate the aerosol hygroscopicity. Particles in Porterville showed low average f(RH = 80%) (1.42) which was attributed to the high carbonaceous loading in the region where residential biomass burning and traffic emissions contribute heavily to air pollution. In Baltimore, the high average f(RH = 80%) (2.06) was attributed to the large contribution of SO42- in the region. The lowest water uptake was observed in Golden, with an average f(RH = 80%) = 1.24 where organic carbon dominated the particle loading. Different empirical fits were evaluated using the f(RH) data. The widely used Kasten (gamma) model was found least satisfactory, as it overestimates f(RH) for RH < 75%. A better empirical fit with two power law curve fitting parameters c and k was found to replicate f(RH) accurately from the three sites. The relationship between the organic carbon mass and the species that are affected by RH and f(RH) was also studied and categorized.

  11. Cloud Formation Potential of Biomass Burning Aerosol Surrogate-Particles Chemically Aged by OH

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Thalman, R. M.; Wang, J.; Li, Z. Q.; Knopf, D. A.

    2014-12-01

    Heterogeneous or multiphase reactions between trace gases such as OH and atmospheric aerosol can influence physicochemical properties of the particles including composition, morphology and lifetime. In this work, the cloud condensation nuclei (CCN) activity of laboratory-generated biomass burning aerosol (BBA) exposed to OH radicals is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type and OH exposure ([OH]×time) using a CCN counter coupled to a custom-built aerosol flow reactor (AFR). The composition of particles collected by a micro-orifice uniform deposit impactor (MOUDI) first subjected to different OH exposures is analyzed by Raman and scanning transmission X-ray microscopy coupled with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative compounds found in BBA that have different hygroscopicity, chemical functionalities, and reactivity with OH radicals. BBA surrogate-particles are generated following atomization of aqueous solutions with mass ratios LEV:MNC:KS of 1:0:0, 0:1:0, 0:0:1, 1:1:0, 0:1:1, 1:0:1, 1:1:1, and 1:0.03:0.3. OH radicals are generated in the AFR following photolysis of O3 in the presence of H2O using a variable intensity ultra-violet (UV) lamp, which allows equivalent atmospheric OH exposures from days to weeks. In addition, we investigate how κ changes i) in response to varying [O3] with and without OH, and ii) at a fixed OH exposure while varying RH. The impact of OH exposure on the CCN activity of BBA will be presented and its atmospheric implications will be discussed.

  12. Hygroscopic properties of newly formed ultrafine particles at an urban site surrounded by deciduous forest (Sapporo, northern Japan) during the summer of 2011

    NASA Astrophysics Data System (ADS)

    Jung, J.; Kawamura, K.

    2014-07-01

    To investigate the hygroscopic properties of ultrafine particles during new particle formation events, the hygroscopic growth factors of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. The hygroscopic growth factor at 85 % relative humidity [g(85%)] of freshly formed nucleation mode particles was 1.11 to 1.28 (average: 1.16 ± 0.06) at a dry particle diameter (Dp) centered on 20 nm, which is equivalent to 1.17 to 1.35 (1.23 ± 0.06) at a dry Dp centered on 100 nm after considering the Kelvin effect. These values are comparable with those of secondary organic aerosols, suggesting that low-volatility organic vapors are important to the burst of nucleation mode particles. The equivalent g(85%) at a dry Dp of 100 nm for nucleated particles that have grown to Aitken mode sizes (1.24 to 1.34; average: 1.30 ± 0.04) were slightly higher than those of newly formed nucleation mode particles, suggesting that the growth of freshly formed nucleation mode particles to the Aitken mode size can be subjected to condensation of not only low-volatility organic vapors, but also water-soluble inorganic species. Based on this result, and previous measurement of radiocarbon in aerosols, we suggest that the burst of nucleation mode particles and their subsequent growth were highly affected by biogenic organic emissions at this measurement site, which is surrounded by deciduous forest. Gradual increases in mode diameter after the burst of nucleation mode particles were observed under southerly wind conditions, with a dominant contribution of intermediately hygroscopic particles. However, sharp increases in mode diameter were observed when the wind direction shifted to northwesterly or northeasterly, with a sharp increase in the highly hygroscopic particle fraction of the Aitken mode particles, indicating that the hygroscopic growth factor of newly formed particles is perturbed by the local winds that deliver

  13. Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions: Part 1 - general equations, parameters, and terminology

    NASA Astrophysics Data System (ADS)

    Pöschl, U.; Rudich, Y.; Ammann, M.

    2005-04-01

    Aerosols and clouds play central roles in atmospheric chemistry and physics, climate, air pollution, and public health. The mechanistic understanding and predictability of aerosol and cloud properties, interactions, transformations, and effects are, however, still very limited. This is due not only to the limited availability of measurement data, but also to the limited applicability and compatibility of model formalisms used for the analysis, interpretation, and description of heterogeneous and multiphase processes. To support the investigation and elucidation of atmospheric aerosol and cloud surface chemistry and gas-particle interactions, we present a comprehensive kinetic model framework with consistent and unambiguous terminology and universally applicable rate equations and parameters. It allows to describe mass transport and chemical reactions at the gas-particle interface and to link aerosol and cloud surface processes with gas phase and particle bulk processes in systems with multiple chemical components and competing physicochemical processes. The key elements and essential aspects of the presented framework are: a simple and descriptive double-layer surface model (sorption layer and quasi-static layer); straightforward flux-based mass balance and rate equations; clear separation of mass transport and chemical reactions; well-defined rate parameters (uptake and accommodation coefficients, reaction and transport rate coefficients); clear distinction between gas phase, gas-surface, and surface-bulk transport (gas phase diffusion correction, surface and bulk accommodation); clear distinction between gas-surface, surface layer, and surface-bulk reactions (Langmuir-Hinshelwood and Eley-Rideal mechanisms); mechanistic description of concentration and time dependencies; flexible inclusion/omission of chemical species and physicochemical processes; flexible convolution/deconvolution of species and processes; and full compatibility with traditional resistor model

  14. Water uptake by organic aerosol and its influence on gas/particle partitioning of secondary organic aerosol in the United States

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu H.; Mahmud, Abdullah; Barsanti, Kelley C.; Asher, William E.; Pankow, James F.; Kleeman, Michael J.

    2016-03-01

    Organic aerosol (OA) is at least partly hygroscopic, i.e., water partitions into the organic phase to a degree determined by the relative humidity (RH), the organic chemical composition, and the particle size. This organic-phase water increases the aerosol mass and provides a larger absorbing matrix while decreasing its mean molecular weight, which can encourage additional condensation of semi-volatile organic compounds. Most regional and global atmospheric models account for water uptake by inorganic salts but do not explicitly account for organic-phase water and its subsequent impact on gas/particle partitioning of semi-volatile OA. In this work, we incorporated the organic-phase water model described by Pankow et al. (2015) into the UCD/CIT air quality model to simulate water uptake by OA and assessed its influence on total OA mass concentrations. The model was run for one summer month over two distinct regions: South Coast Air Basin (SoCAB) surrounding Los Angeles, California and the eastern United States (US). In SoCAB where the OA was dominated by non-hygroscopic primary OA (POA), there was very little organic-phase water uptake (0.1-0.2 μg m-3) and consequently very little enhancement (or growth) in total OA concentrations (OA + organic-phase water): a 3% increase in total OA mass was predicted for a 0.1 increase in relative humidity. In contrast, in the eastern US where secondary OA (SOA) from biogenic sources dominated the OA, substantial organic-phase water uptake and enhancement in total OA concentrations was predicted, even in urban locations. On average, the model predicted a 20% growth in total OA mass for a 0.1 increase in relative humidity; the growth was equivalent to a 250 nm particle with a hygroscopicity parameter (κ) of 0.15. Further, for the same relative humidity, the exact extent of organic-phase water uptake and total OA enhancement was found to be dependent on the particle mixing state. When the source-oriented mixing state of aerosols

  15. Satellite retrieval of aerosol microphysical and optical parameters using neural networks: a new methodology applied to the Sahara desert dust peak

    NASA Astrophysics Data System (ADS)

    Taylor, M.; Kazadzis, S.; Tsekeri, A.; Gkikas, A.; Amiridis, V.

    2013-12-01

    In order to exploit the full-Earth viewing potential of satellite instruments to globally characterise aerosols, new algorithms are required to deduce key microphysical parameters like the particle size distribution and optical parameters associated with scattering and absorption from space remote sensing data. Here, a methodology based on neural networks is developed to retrieve such parameters from satellite inputs and to validate them with ground-based remote sensing data. For key combinations of input variables available from MODIS and OMI Level 3 datasets, a grid of 100 feed-forward neural network architectures is produced, each having a different number of neurons and training proportion. The networks are trained with principal components accounting for 98% of the variance of the inputs together with principal components formed from 38 AERONET Level 2.0 (Version 2) retrieved parameters as outputs. Daily-averaged, co-located and synchronous data drawn from a cluster of AERONET sites centred on the peak of dust extinction in Northern Africa is used for network training and validation, and the optimal network architecture for each input parameter combination is identified with reference to the lowest mean squared error. The trained networks are then fed with unseen data at the coastal dust site Dakar to test their simulation performance. A NN, trained with co-located and synchronous satellite inputs comprising three aerosol optical depth measurements at 470, 500 and 660 nm, plus the columnar water vapour (from MODIS) and the modelled absorption aerosol optical depth at 500 nm (from OMI), was able to simultaneously retrieve the daily-averaged size distribution, the coarse mode volume, the imaginary part of the complex refractive index, and the spectral single scattering albedo - with moderate precision: correlation coefficients in the range 0.368 ≤ R ≤ 0.514. The network failed to recover the spectral behaviour of the real part of the complex refractive index

  16. Properties of jet engine combustion particles during the PartEmis experiment. Hygroscopic growth at supersaturated conditions

    NASA Astrophysics Data System (ADS)

    Hitzenberger, R.; Giebl, H.; Petzold, A.; Gysel, M.; Nyeki, S.; Weingartner, E.; Baltensperger, U.; Wilson, C. W.

    2003-07-01

    During the EU Project PartEmis, the microphysical properties of aircraft combustion aerosol were investigated. This study is focused on the ability of exhaust aerosols to act as cloud condensation nuclei (CCN). The combustor was operated at two different conditions representing old and modern aircraft engine technology. CCN concentrations were measured with the University of Vienna CCN counter [ Giebl et al., 2002] at supersaturations around 0.7%. The activation ratio (fraction of CCN in total aerosol) depended on the fuel sulphur content (FSC) and also on the operation conditions. CCN/CN ratios increased from 0.93 through 1.43 to 5.15 . 10-3 (old cruise conditions) and 0.67 through 3.04 to 7.94 . 10-3 (modern cruise conditions) when FSC increased from 50 through 410 to1270 μg/g. The activation behaviour was modelled using classical theories and with a semi-empirical model [ Gysel et al., 2003] based on measured hygroscopicity of the aerosol under subsaturated conditions, which gave the best agreement.

  17. Aerosols and environmental pollution

    NASA Astrophysics Data System (ADS)

    Colbeck, Ian; Lazaridis, Mihalis

    2010-02-01

    The number of publications on atmospheric aerosols has dramatically increased in recent years. This review, predominantly from a European perspective, summarizes the current state of knowledge of the role played by aerosols in environmental pollution and, in addition, highlights gaps in our current knowledge. Aerosol particles are ubiquitous in the Earth’s atmosphere and are central to many environmental issues; ranging from the Earth’s radiative budget to human health. Aerosol size distribution and chemical composition are crucial parameters that determine their dynamics in the atmosphere. Sources of aerosols are both anthropogenic and natural ranging from vehicular emissions to dust resuspension. Ambient concentrations of aerosols are elevated in urban areas with lower values at rural sites. A comprehensive understanding of aerosol ambient characteristics requires a combination of measurements and modeling tools. Legislation for ambient aerosols has been introduced at national and international levels aiming to protect human health and the environment.

  18. The Influence of topography on formation characteristics of hygroscopic and condensate water in Shapotou

    NASA Astrophysics Data System (ADS)

    Pan, Yanxia; Li, Xinrong; Hui, Rong; Zhao, Yang

    2016-04-01

    The formation characteristics of hygroscopic and condensate water for different topographic positions were observed using the PVC pipes manual weighing and CPM method in the typical mobile dunes fixed by straw checkerboard barriers in Shapotou. The results indicated that the formation amounts and duration of hygroscopic and condensate water show moderate spatial heterogeneity at the influence of topography. The formation amounts of hygroscopic and condensate water at different aspects conform to the classical convection model, in which the hygroscopic and condensate water amounts are highest at hollow, and windward aspect gets more water than leeward aspect, the hygroscopic and condensate water amounts at different aspects are expressed as: hollow>Western-faced aspect>Northern-faced aspect>hilltop>Southern-faced aspect>Eastern-faced aspect. The hygroscopic and condensate water amounts at different slope positions for every aspect are as follows: the foot of slope>middle slope>hilltop. A negatively linear correlation is got between slope angles and hygroscopic and condensate water amounts, hygroscopic and condensate water amounts decrease gradually along with the increase of slope angles, the amounts of hygroscopic and condensate water at the vertical aspect are only half of horizontal aspect, which indicated topography were important influence factors for the formation of the hygroscopic and condensate water in arid area.

  19. Characterization of Ambient Black Carbon Aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, R.; Levy, M. E.; Zheng, J.; Molina, L. T.

    2013-12-01

    Because of the strong absorption over a broad range of the electromagnetic spectra, black carbon (BC) is a key short-lived climate forcer, which contributes significantly to climate change by direct radiative forcing and is the second most important component causing global warming after carbon dioxide. The impact of BC on the radiative forcing of the Earth-Atmosphere system is highly dependent of the particle properties. In this presentation, emphasis will be placed on characterizing BC containing aerosols in at the California-Mexico border to obtain a greater understanding of the atmospheric aging and properties of ambient BC aerosols. A comprehensive set of directly measured aerosol properties, including the particle size distribution, effective density, hygroscopicity, volatility, and several optical properties, will be discussed to quantify the mixing state and composition of ambient particles. In Tijuana, Mexico, submicron aerosols are strongly influenced by vehicle emissions; subsequently, the BC concentration in Tijuana is considerably higher than most US cities with an average BC concentration of 2.71 × 2.65 g cm-3. BC accounts for 24.75 % × 9.44 of the total submicron concentration on average, but periodically accounts for over 50%. This high concentration of BC strongly influences many observed aerosol properties such as single scattering albedo, hygroscopicity, effective density, and volatility.

  20. Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China during summertime

    NASA Astrophysics Data System (ADS)

    Wu, Z. J.; Zheng, J.; Shang, D. J.; Du, Z. F.; Wu, Y. S.; Zeng, L. M.; Wiedensohler, A.; Hu, M.

    2015-04-01

    Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the median hygroscopicity parameters (κ) of 50, 100, 150, 200, and 250 nm particles are respectively 0.15, 0.19, 0.22, 0.27, and 0.29, showing an increasing trend with increasing particle size. When PM2.5 mass concentration is greater than 50 μg m-3, the fractions of the hydrophilic mode for 150, 250, 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high time-resolution size-resolved chemical composition derived from AMS measurement on a basis of ZSR mixing rule. An empirical relationship between κ of organic fraction (κorg) and oxygen to carbon ratio (O : C) (κorg= 0.08·O : C+0.02) is obtained. During new particle formation event associating with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particle with the same sizes during non-NPF periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example 250 nm particle) was observed. Such transformations can modify the state of mixture of pre-exiting particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.

  1. A simple parameterization of aerosol emissions in RAMS

    NASA Astrophysics Data System (ADS)

    Letcher, Theodore

    model. Furthermore, SA formation is greatly reduced during the winter months due to the lack of naturally produced organic VOC's. Because of these reasons, it was felt that neglecting SOA within the model was the best course of action. The actual parameterization uses a prescribed source map to add aerosol to the model at two vertical levels that surround an arbitrary height decided by the user. To best represent the real-world, the WRF Chemistry model was run using the National Emissions Inventory (NEI2005) to represent anthropogenic emissions and the Model Emissions of Gases and Aerosols from Nature (MEGAN) to represent natural contributions to aerosol. WRF Chemistry was run for one hour, after which the aerosol output along with the hygroscopicity parameter (κ) were saved into a data file that had the capacity to be interpolated to an arbitrary grid used in RAMS. The comparison of this parameterization to observations collected at Mesa Verde National Park (MVNP) during the Inhibition of Snowfall from Pollution Aerosol (ISPA-III) field campaign yielded promising results. The model was able to simulate the variability in near surface aerosol concentration with reasonable accuracy, though with a general low bias. Furthermore, this model compared much better to the observations than did the WRF Chemistry model using a fraction of the computational expense. This emissions scheme was able to show reasonable solutions regarding the aerosol concentrations and can therefore be used to provide an estimate of the seasonal impact of increased CCN on water resources in Western Colorado with relatively low computational expense.

  2. Observations of relative humidity effects on aerosol light scattering in the Yangtze River Delta of China

    NASA Astrophysics Data System (ADS)

    Zhang, L.; Sun, J. Y.; Shen, X. J.; Zhang, Y. M.; Che, H.; Ma, Q. L.; Zhang, Y. W.; Zhang, X. Y.; Ogren, J. A.

    2015-07-01

    Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ~ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f(85 %)), backscattering coefficient (fb(85 %)), and hemispheric backscatter fraction (fβ(85 %)) were 1.58 ± 0.12, 1.25 ± 0.07, and 0.79 ± 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM1 was found to be a main factor determining the magnitude of f(RH). The highest values of f(RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO3- in fine particles was strongly correlated with f(85 %), which suggests that NO3- played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.

  3. A case study of Asian dust storm particles: chemical composition, reactivity to SO2 and hygroscopic properties.

    PubMed

    Ma, Qingxin; Liu, Yongchun; Liu, Chang; Ma, Jinzhu; He, Hong

    2012-01-01

    Mineral dust comprises a great fraction of the global aerosol loading, but remains the largest uncertainty in predictions of the future climate due to its complexity in composition and physico-chemical properties. In this work, a case study characterizing Asian dust storm particles was conducted by multiple analysis methods, including SEM-EDS, XPS, FT-IR, BET, TPD/mass and Knudsen cell/mass. The morphology, elemental fraction, source distribution, true uptake coefficient for SO2, and hygroscopic behavior were studied. The major components of Asian dust storm particles are aluminosilicate, SiO2 and CaCO3, with organic compounds and inorganic nitrate coated on the surface. It has a low reactivity towards SO2 with a true uptake coefficient, 5.767 x 10(-6), which limits the conversion of SO2 to sulfate during dust storm periods. The low reactivity also means that the heterogeneous reactions of SO2 in both dry and humid air conditions have little effect on the hygroscopic behavior of the dust particles. PMID:22783615

  4. The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore-Washington, D.C. region

    NASA Astrophysics Data System (ADS)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2016-01-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type - such as composition, size, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

  5. Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions - Part 1: General equations, parameters, and terminology

    NASA Astrophysics Data System (ADS)

    Pöschl, U.; Rudich, Y.; Ammann, M.

    2007-12-01

    Aerosols and clouds play central roles in atmospheric chemistry and physics, climate, air pollution, and public health. The mechanistic understanding and predictability of aerosol and cloud properties, interactions, transformations, and effects are, however, still very limited. This is due not only to the limited availability of measurement data, but also to the limited applicability and compatibility of model formalisms used for the analysis, interpretation, and description of heterogeneous and multiphase processes. To support the investigation and elucidation of atmospheric aerosol and cloud surface chemistry and gas-particle interactions, we present a comprehensive kinetic model framework with consistent and unambiguous terminology and universally applicable rate equations and parameters. It enables a detailed description of mass transport and chemical reactions at the gas-particle interface, and it allows linking aerosol and cloud surface processes with gas phase and particle bulk processes in systems with multiple chemical components and competing physicochemical processes. The key elements and essential aspects of the presented framework are: a simple and descriptive double-layer surface model (sorption layer and quasi-static layer); straightforward flux-based mass balance and rate equations; clear separation of mass transport and chemical reactions; well-defined and consistent rate parameters (uptake and accommodation coefficients, reaction and transport rate coefficients); clear distinction between gas phase, gas-surface, and surface-bulk transport (gas phase diffusion, surface and bulk accommodation); clear distinction between gas-surface, surface layer, and surface-bulk reactions (Langmuir-Hinshelwood and Eley-Rideal mechanisms); mechanistic description of concentration and time dependences (transient and steady-state conditions); flexible addition of unlimited numbers of chemical species and physicochemical processes; optional aggregation or resolution

  6. Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems

    NASA Astrophysics Data System (ADS)

    Massling, A.; Niedermeier, N.; Hennig, T.; Fors, E. O.; Swietlicki, E.; Ehn, M.; Hämeri, K.; Villani, P.; Laj, P.; Good, N.; McFiggans, G.; Wiedensohler, A.

    2011-03-01

    The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/-13% to +8/-6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 °C. For the correct determination of external mixtures

  7. The regime of aerosol asymmetry parameter over Europe, the Mediterranean and the Middle East based on MODIS satellite data: evaluation against surface AERONET measurements

    NASA Astrophysics Data System (ADS)

    Korras-Carraca, M. B.; Hatzianastassiou, N.; Matsoukas, C.; Gkikas, A.; Papadimas, C. D.

    2015-11-01

    Atmospheric particulates are a significant forcing agent for the radiative energy budget of the Earth-atmosphere system. The particulates' interaction with radiation, which defines their climate effect, is strongly dependent on their optical properties. In the present work, we study one of the most important optical properties of aerosols, the asymmetry parameter (gaer), over sea surfaces of the region comprising North Africa, the Arabian Peninsula, Europe, and the Mediterranean Basin. These areas are of great interest, because of the variety of aerosol types they host, both anthropogenic and natural. Using satellite data from the collection 051 of MODIS (Moderate Resolution Imaging Spectroradiometer, Terra and Aqua), we investigate the spatiotemporal characteristics of the asymmetry parameter. We generally find significant spatial variability, with larger values over regions dominated by larger size particles, e.g., outside the Atlantic coasts of northwestern Africa, where desert-dust outflow takes place. The gaer values tend to decrease with increasing wavelength, especially over areas dominated by small particulates. The intra-annual variability is found to be small in desert-dust areas, with maximum values during summer, while in all other areas larger values are reported during the cold season and smaller during the warm. Significant intra-annual and inter-annual variability is observed around the Black Sea. However, the inter-annual trends of gaer are found to be generally small. Although satellite data have the advantage of broad geographical coverage, they have to be validated against reliable surface measurements. Therefore, we compare satellite-measured values with gaer values measured at 69 stations of the global surface AERONET (Aerosol Robotic Network), located within our region of interest. This way, we provide some insight on the quality and reliability of MODIS data. We report generally better agreement at the wavelength of 860 nm (correlation

  8. The regime of aerosol asymmetry parameter over Europe, Mediterranean and Middle East based on MODIS satellite data: evaluation against surface AERONET measurements

    NASA Astrophysics Data System (ADS)

    Korras-Carraca, M. B.; Hatzianastassiou, N.; Matsoukas, C.; Gkikas, A.; Papadimas, C. D.

    2014-09-01

    Atmospheric particulates are a significant forcing agent for the radiative energy budget of the Earth-atmosphere system. The particulates' interaction with radiation, which defines their climate effect, is strongly dependent on their optical properties. In the present work, we study one of the most important optical properties of aerosols, the asymmetry parameter (gaer), in the region comprised of North Africa, the Arabian peninsula, Europe, and the Mediterranean basin. These areas are of great interest, because of the variety of aerosol types they host, both anthropogenic and natural. Using satellite data from the collection 051 of MODIS (MODerate resolution Imaging Spectroradiometer, Terra and Aqua), we investigate the spatio-temporal characteristics of the asymmetry parameter. We generally find significant spatial variability, with larger values over regions dominated by larger size particles, e.g. outside the Atlantic coasts of north-western Africa, where desert-dust outflow is taking place. The gaer values tend to decrease with increasing wavelength, especially over areas dominated by small particulates. The intra-annual variability is found to be small in desert-dust areas, with maximum values during summer, while in all other areas larger values are reported during the cold season and smaller during the warm. Significant intra-annual and inter-annual variability is observed around the Black Sea. However, the inter-annual trends of gaer are found to be generally small. Although satellite data have the advantage of broad geographical coverage, they have to be validated against reliable surface measurements. Therefore, we compare satellite-based values with gaer values measured at 69 stations of the global surface network AERONET (Aerosol Robotic Network), located within our region of interest. This way, we provide some insight on the quality and reliability of MODIS data. We report generally better agreement at the wavelength of 870 nm (correlation coefficient

  9. The Effect Of Organic Surfactants On The Properties Of Common Hygroscopic Particles: Effective Densities, Reactivity And Water Evaporation Of Surfactant Coated Particles

    NASA Astrophysics Data System (ADS)

    Cuadrarodriguez, L.; Zelenyuk, A.; Imre, D.; Ellison, B.

    2006-12-01

    Measurements of atmospheric aerosol compositions routinely show that organic compounds account for a very large fraction of the particle mass. The organic compounds that make up this aerosol mass represent a wide range of molecules with a variety of properties. Many of the particles are composed of hygroscopic salts like sulfates, nitrates and sea-salt internally mixed with organics. While the properties of the hygroscopic salts are known, the effect of the organic compounds on the microphysical and chemical properties which include CCN activity is not clear. .One particularly interesting class of internally mixed particles is composed of aqueous salts solutions that are coated with organic surfactants which are molecules with long aliphatic chain and a water soluble end. Because these molecules tend to coat the particles' surfaces, a monolayer might be sufficient to drastically alter their hygroscopic properties, their CCN activity, and reactivity. The aliphatic chains, being exposed to the oxidizing atmosphere are expected to be transformed through heterogeneous chemistry, yielding complex products with mixed properties. We will report the results from a series of observations on ammonium sulfate, sodium chloride and sea salt particles coated with three types of surfactant molecules: sodium lauryl sulfate, sodium oleate and laurtrimonium chloride. We have been able to measure the effective densities of internally mixed particles with a range of surfactant concentration that start below a monolayer and extend all the way to particles composed of pure surfactant. For many of the measurements the data reveal a rather complex picture that cannot be simply interpreted in terms of the known pure-compound densities. For unsaturated hydrocarbons we observed and quantified the effect of oxidation by ozone on particle size, effective density and individual particle mass spectral signatures. One of the more important properties of these surfactants is that they can form a

  10. Aerosol characterization with lidar methods

    NASA Astrophysics Data System (ADS)

    Sugimoto, Nobuo; Nishizawa, Tomoaki; Shimizu, Atsushi; Matsui, Ichiro

    2014-08-01

    Aerosol component analysis methods for characterizing aerosols were developed for various types of lidars including polarization-sensitive Mie scattering lidars, multi-wavelength Raman scattering lidars, and multi-wavelength highspectral- resolution lidars. From the multi-parameter lidar data, the extinction coefficients for four aerosol components can be derived. The microphysical parameters such as single scattering albedo and effective radius can be also estimated from the derived aerosol component distributions.

  11. Remote continental aerosol characteristics in the Rocky Mountains of Colorado and Wyoming

    NASA Astrophysics Data System (ADS)

    Levin, Ezra J. T.

    number concentrations were correlated with the frequency of events typical of new particle formation. Measured sub-micron organic mass fractions were between 70 -- 90% during the summer months, when new particle formation events were most frequent, suggesting the importance of organic species in the nucleation or growth process, or both. Aerosol composition derived from hygroscopicity measurements indicate organic mass fractions of 50 - 60% for particles with diameters larger than 0.15 mum during the winter. The composition of smaller diameter particles appeared to be organic dominated year-round. High organic mass fractions led to low values of aerosol hygroscopicity, described using the kappa parameter. Over the entire year-long BEACHON study, kappa had an average value of 0.16 +/- 0.08, similar to values determined during biologically active periods in tropical and boreal forests, and lower than the commonly assumed value of kappacontinental = 0.3. There was also an observed increase in kappa with size, due to external mixing of the fine mode aerosol. Incorrect representations of kappa or its size dependence led to erroneous values of calculated CCN concentrations, especially for supersaturation values less than 0.3%. At higher supersaturations, most of the measured variability in CCN concentrations was captured by changes in total measured aerosol number concentrations. While data from the three measurement sites were generally well correlated, indicating similarities in seasonal cycles and in total number concentrations, there were some variations between measurements made at different sites and during different years that may be partly due to the effects of local emissions. The averaged data provide reasonable, observationally-based parameters for modeling of aerosol number size distributions and corresponding CCN concentrations. Field observations clearly indicated the episodic influence of wildfire smoke on particle number concentrations and compositions. However

  12. A Sensitivity Study of Radiative Fluxes at the Top of Atmosphere to Cloud-Microphysics and Aerosol Parameters in the Community Atmosphere Model CAM5

    SciTech Connect

    Zhao, Chun; Liu, Xiaohong; Qian, Yun; Yoon, Jin-Ho; Hou, Zhangshuan; Lin, Guang; McFarlane, Sally A.; Wang, Hailong; Yang, Ben; Ma, Po-Lun; Yan, Huiping; Bao, Jie

    2013-11-08

    In this study, we investigated the sensitivity of net radiative fluxes (FNET) at the top of atmosphere (TOA) to 16 selected uncertain parameters mainly related to the cloud microphysics and aerosol schemes in the Community Atmosphere Model version 5 (CAM5). We adopted a quasi-Monte Carlo (QMC) sampling approach to effectively explore the high dimensional parameter space. The output response variables (e.g., FNET) were simulated using CAM5 for each parameter set, and then evaluated using generalized linear model analysis. In response to the perturbations of these 16 parameters, the CAM5-simulated global annual mean FNET ranges from -9.8 to 3.5 W m-2 compared to the CAM5-simulated FNET of 1.9 W m-2 with the default parameter values. Variance-based sensitivity analysis was conducted to show the relative contributions of individual parameter perturbation to the global FNET variance. The results indicate that the changes in the global mean FNET are dominated by those of cloud forcing (CF) within the parameter ranges being investigated. The size threshold parameter related to auto-conversion of cloud ice to snow is confirmed as one of the most influential parameters for FNET in the CAM5 simulation. The strong heterogeneous geographic distribution of FNET variation shows parameters have a clear localized effect over regions where they are acting. However, some parameters also have non-local impacts on FNET variance. Although external factors, such as perturbations of anthropogenic and natural emissions, largely affect FNET variations at the regional scale, their impact is weaker than that of model internal parameters in terms of simulating global mean FNET in this study. The interactions among the 16 selected parameters contribute a relatively small portion of the total FNET variations over most regions of the globe. This study helps us better understand the CAM5 model behavior associated with parameter uncertainties, which will aid the next step of reducing model

  13. Pathophysiological and disease constraints on aerosol delivery

    SciTech Connect

    Gerrity, T.R.

    1989-01-01

    The dose of inhaled particles to the respiratory tract depends upon many factors. These factors include the size of the particles, the pattern of breathing (flow and tidal volume), the physical properties of the articles (hygroscopic or non-hygroscopic), anatomy of the respiratory tract, and the pathophysiologic status of the respiratory tract. In addition to these factors, which are primarily related to the deposition of particles, the rate of particle clearance from the respiratory tract also influences the dose of particles. The paper is a review of the various factors influencing dose of inhaled particles to the respiratory tract. The emphasis of the paper is on therapeutic aerosol particles, though the principals discussed also apply to toxic particles as well. An important area of consideration is the influence of disease on the delivery of particle dose. From the point of view of toxic particles this is important when considering potential susceptible populations.

  14. Using artificial neural networks to retrieve the aerosol type from multi-spectral lidar data

    NASA Astrophysics Data System (ADS)

    Nicolae, Doina; Belegante, Livio; Talianu, Camelia; Vasilescu, Jeni

    2015-04-01

    Aerosols can influence the microphysical and macrophysical properties of clouds and hence impact the energy balance, precipitation and the hydrological cycle. They have different scattering and absorption properties depending on their origin, therefore measured optical properties can be used to retrieve their physical properties, as well as to estimate their chemical composition. Due to the measurement limitations (spectral, uncertainties, range) and high variability of the aerosol properties with environmental conditions (including mixing during transport), the identification of the aerosol type from lidar data is still not solved. However, ground, airborne and space-based lidars provide more and more observations to be exploited. Since 2000, EARLINET collected more than 20,000 aerosol vertical profiles under various meteorological conditions, concerning local or long-range transport of aerosols in the free troposphere. This paper describes the basic algorithm for aerosol typing from optical data using the benefits of artificial neural networks. A relevant database was built to provide sufficient training cases for the neural network, consisting of synthetic and measured aerosol properties. Synthetic aerosols were simulated starting from the microphysical properties of basic components, internally mixed in various proportions. The algorithm combines the GADS database (Global Aerosol DataSet) to OPAC model (Optical Properties of Aerosol and Clouds) and T-Matrix code in order to compute, in an iterative way, the intensive optical properties of each aerosol type. Both pure and mixed aerosol types were considered, as well as their particular non-sphericity and hygroscopicity. Real aerosol cases were picked up from the ESA-CALIPSO database, as well as EARLINET datasets. Specific selection criteria were applied to identify cases with accurate optical data and validated sources. Cross-check of the synthetic versus measured aerosol intensive parameters was performed in

  15. Intercomparison of observations and model aerosol parameters during two Saharan dust events over the southern United Kingdom

    NASA Astrophysics Data System (ADS)

    Buxmann, Joelle; Adam, Mariana; Ordonez, Carlos; Tilbee, Marie; Smyth, Tim; Claxton, Bernard; Sugier, Jacqueline; Agnew, Paul

    2015-04-01

    Saharan desert dust lifted by convection over the hot desert surface can reach high altitudes and be transported over great distances. In the UK, Saharan dust episodes occur several times a year, usually during the spring. Dust lifted by cyclonic circulation is often blown into the Atlantic and transported to the UK. This can result in a rapid degradation of air quality due to the increase in the levels of particulate matter (PM). The ability to model the transport and deposition of dust remains an important challenge in order to characterize different pollution events. We present a comparison of observed Aerosol Optical Depth (AOD) with modelled AOD from the Met Office Air Quality Unified Model (AQUM), performed for two dust events in March 2014 (at 380nm, 440nm, 870nm and 1020nm). The observations are derived from five sun photometers located in the southern UK at Exeter, Cardington, Bayfordbury, Chilbolton, and Plymouth. Correlations are investigated between model column integrated PM2.5 and PM10, and observed fine and coarse mode AOD from AERONET. Vertical profiles of attenuated backscatter and extinction from the Jenoptik Nimbus ceilometers part of the Met Office Laser Cloud Base Recorder (LCBR) network are investigated as well (see also session AS3.17/GI2.2 Lidar and Applications). The Met Office air quality model AQUM is an on-line meteorology, chemistry and aerosol modelling system. It runs at a resolution of 12km over a domain covering the UK and north-western Europe. Atmospheric composition modelling employs two-way coupling between aerosol and chemistry evolution, with explicit modelling of sulphate, nitrate, black carbon, organic carbon, biomass burning and wind-blown mineral dust aerosol components. Both the model and observations show an increase in AOD during the first period from 12 -13 March 2014. For example AOD levels of up to 0.52 for the 380nm channel were recorded by the sun photometer in Exeter. This is relatively high compared to average

  16. Aerosol composition and variability in the Baltimore-Washington, DC region

    NASA Astrophysics Data System (ADS)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2015-08-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type, such as composition, size and hygroscopicity, and to the surrounding atmosphere, such as temperature, relative humidity (RH) and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in-situ atmospheric profiling in the Baltimore, MD-Washington, DC region was performed during fourteen flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 49 %) due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of ammonium sulfate increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity causing an increase in the water content of the aerosol. Conversely, low aerosol loading days had lower ammonium sulfate and higher black carbon contributions causing lower single scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km decreasing to 35 ng m-3

  17. Aerosol typing - key information from aerosol studies

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  18. Tracking sources of severe haze episodes and their physicochemical and hygroscopic properties under Asian continental outflow: Long-range transport pollution, postharvest biomass burning, and Asian dust

    NASA Astrophysics Data System (ADS)

    Jung, Jinsang; Kim, Young J.

    2011-01-01

    Aerosol physicochemical and hygroscopic properties were measured from 12 October to 21 November 2005 at a downwind area of the Asian continental outflow (Gwangju, Korea) to characterize severe haze episodes. Using optically measured elemental carbon (EC) at 660 nm (Opt.EC) and 880 nm (BC) wavelengths and Mie theory, it was estimated that the higher BC/Opt.EC ratio during the cloudy day of the long-range transport (LTP) period was mainly due to EC particle growth from in-cloud processing with secondary aerosols such as sulfate and organic aerosols. Single scattering albedo (SSA) of biomass burning (BB) aerosol increased sharply from 0.89 to 0.94 under a relative humidity >70%, suggesting that organic aerosols emitted from rice straw burning contained high amounts of hydrophilic compounds. The contribution of aerosol water content to the total light extinction coefficient (bext) was determined as 51.4% and 68.4% during the BB and BB + LTP periods, respectively, indicating that the haze episodes were highly enhanced by an increase in aerosol water content. The Asian dust event was characterized by the highest SSA (0.92 ± 0.02), the lowest mass scattering efficiency of fine particles (2.5 ± 1.0 m2 g-1), and the lowest hygroscopic nature (humidity-dependent light scattering enhancement factor, f(80%), which is defined by the ratio of light scattering coefficient at 80% relative humidity to that at dry condition, = ˜1.37). Based on the Ångström exponent (α) values observed at the source region of the Asian continent and the downwind area of South Korea during the BB + LTP period, it was found that the α value of urban aerosols decreased ˜11% for 1-2 days of the transport, probably due to the increase in particle size through water uptake. Increasing rates of surface PM10 mass concentrations at western coastal areas of the South Korean peninsula were in the range 2.4-14.4 μgm-3 h-1 at the beginning of the BB + LTP period (24 October 2005, 0700-2300 LT). Based on

  19. Effective Expansion: Balance between Shrinkage and Hygroscopic Expansion.

    PubMed

    Suiter, E A; Watson, L E; Tantbirojn, D; Lou, J S B; Versluis, A

    2016-05-01

    The purpose of this study was to investigate the relationship between hygroscopic expansion and polymerization shrinkage for compensation of polymerization shrinkage stresses in a restored tooth. One resin-modified glass-ionomer (RMGI) (Ketac Nano, 3M ESPE), 2 compomers (Dyract, Dentsply; Compoglass, Ivoclar), and a universal resin-based composite (Esthet•X HD, Dentsply) were tested. Volumetric change after polymerization ("total shrinkage") and during 4 wk of water storage at 37°C was measured using an optical method (n= 10). Post-gel shrinkage was measured during polymerization using a strain gauge method (n= 10). Extracted human molars with large mesio-occluso-distal slot preparations were restored with the tested restorative materials. Tooth surfaces at baseline (preparation), after restoration, and during 4 wk of 37°C water storage were scanned with an optical scanner to determine cuspal flexure (n= 8). Occlusal interface integrity was measured using dye penetration. Data were analyzed using analysis of variance and post hoc tests (significance level 0.05). All tested materials shrunk after polymerization. RMGI had the highest total shrinkage (4.65%) but lowest post-gel shrinkage (0.35%). Shrinkage values dropped significantly during storage in water but had not completely compensated polymerization shrinkage after 4 wk. All restored teeth initially exhibited inward (negative) cuspal flexure due to polymerization shrinkage. Cuspal flexure with the RMGI restoration was significantly less (-6.4 µm) than with the other materials (-12.1 to -14.1 µm). After 1 d, cuspal flexure reversed to +5.0 µm cuspal expansion with the RMGI and increased to +9.3 µm at 4 wk. After 4 wk, hygroscopic expansion compensated cuspal flexure in a compomer (Compoglass) and reduced flexure with Dyract and resin-based composite. Marginal integrity (93.7% intact restoration wall) was best for the Compoglass restorations and lowest (73.1%) for the RMGI restorations. Hygroscopic

  20. Aerosol Properties over the Eastern North Pacific based on Measurements from the MAGIC Field Campaign

    NASA Astrophysics Data System (ADS)

    Lewis, E. R.; Senum, G.; Springston, S. R.; Kuang, C.

    2015-12-01

    The MAGIC field campaign, funded and operated by the ARM (Atmospheric Radiation Measurement) Climate Research Facility of the US Department of Energy, occurred between September 2012 and October, 2013 aboard the Horizon Lines cargo container ship Spirit making regular trips between Los Angeles, CA and Honolulu, HI. Along this route, which lies very near the GPCI (GCSS Pacific Cross-section Intercomparison) transect, the predominant cloud regime changes from stratocumulus near the California coast to trade-wind cumulus near Hawaii. The transition between these two regimes is poorly understood and not accurately represented in models. The goal of MAGIC was to acquire statistic of this transition and thus improve its representation in models by making repeated transects through this region and measuring properties of clouds and precipitation, aerosols, radiation, and atmospheric structure. To achieve these goals, the Second ARM Mobile Facility (AMF2) was deployed on the Horizon Spirit as it ran its regular route between Los Angeles and Honolulu. AMF2 consists of three 20-foot SeaTainers and includes three radars and other instruments to measure properties of clouds and precipitation; the Aerosol Observing System (AOS), which has a suite of instruments to measure properties of aerosols; and other instruments to measure radiation, meteorological quantities, and sea surface temperature. Two technicians accompanied the AMF2, and scientists rode the ship as observers. MAGIC made nearly 20 round trips between Los Angeles and Honolulu (and thus nearly 40 excursions through the stratocumulus-to-cumulus transition) and spent 200 days at sea, collecting an unprecedented data set. Aerosol properties measured with the AOS include number concentration and size distribution, CCN activity, hygroscopic growth, and light-scattering and absorption. Additionally, more than one hundred filter samples were collected. Aerosol properties and their spatial and temporal behavior are discussed

  1. Aerosol physicochemical properties and implications for visibility during an intense haze episode during winter in Beijing

    NASA Astrophysics Data System (ADS)

    Wang, Y. H.; Liu, Z. R.; Zhang, J. K.; Hu, B.; Ji, D. S.; Yu, Y. C.; Wang, Y. S.

    2015-03-01

    The evolution of physical, chemical and optical properties of urban aerosol particles was characterized during an extreme haze episode in Beijing, PRC, from 24 through 31 January 2013 based on in situ measurements. The average mass concentrations of PM1, PM2.5 and PM10 were 99 ± 67 μg m-3 (average ± SD), 188 ± 128 μg m-3 and 265 ± 157 μg m-3, respectively. A significant increase in PM1-2.5 fraction was observed during the most heavily polluted period. The average scattering coefficient at 550 nm was 877 ± 624 Mm-1. An increasing relative amount of coarse particles can be deduced from the variations of backscattering ratios, asymmetry parameter and scattering Ångström exponent. Particle number-size distributions between 14 and 2500 nm diameter showed high number concentrations, particularly in the nucleation mode and accumulation mode. Size-resolved chemical composition of submicron aerosol from a high-resolution time-of-flight aerosol mass spectrometer showed that the mass concentrations of organic, sulfate, nitrate, ammonium and chlorine mainly resided on particles between 500 and 800 nm (vacuum diameter), and nitrate and ammonium contributed greatly to particle growth during the heavily polluted day (28 January). Increasing relative humidity and stable synoptic conditions on 28 January combined with heavy pollution on 28 January, leading to enhanced water uptake by the hygroscopic submicron particles and formation of secondary aerosol, which might be the main reasons for the severity of the haze episode. Light-scattering apportionment showed that organic, sulfate, ammonium nitrate and ammonium chloride compounds contributed to light-scattering fractions of 54, 24, 12 and 10%, respectively. This study indicated that the organic component in submicron aerosol played an important role in visibility degradation during the haze episode in Beijing.

  2. Measurements and Modeling of Aerosol Absorption and Single Scattering Albedo at Ambient Relative Hum

    NASA Technical Reports Server (NTRS)

    Redemann, J.; Russell, P. B.; Hamill, P.

    2000-01-01

    Uncertainties in the aerosol single scattering albedo have been identified to be an important source of errors in current large-scale model estimates of the direct aerosol radiative forcing of climate. A number of investigators have obtained estimates of the single scattering albedo from a variety of remote sensing and in situ measurements during aerosol field experiments. During the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX, 1996) for example, estimates of the aerosol single scattering albedo were obtained (1) as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from independently measured aerosol properties; (2) from estimates of the aerosol complex index of refraction derived using a combination of airborne sunphotometer, lidar backscatter and in situ size distribution measurements; and (3) from airborne measurements of aerosol scattering and absorption using nephelometers and absorption photometers. In this paper, we briefly compare the results of the latter two methods for two TARFOX case studies, since those techniques provide height-resolved information about the aerosol single scattering albedo. Estimates of the aerosol single scattering albedo from nephelometer and absorption photometer measurements require knowledge of the scattering and absorption humidification (i.e., the increase in these properties in response to an increase in ambient relative humidity), since both measurements are usually carried out at a relative humidity different from the ambient atmosphere. In principle, the scattering humidification factor can be measured, but there is currently no technique widely available to measure the absorption of an aerosol sample as a function of relative humidity. Frequently, for lack of better knowledge, the absorption humidification is assumed to be unity (meaning that there is no change in aerosol absorption due to an increase in ambient relative humidity). This

  3. [AOD and angstrom parameters of aerosols observed by the Chinese sun hazemeter network from August to December 2004].

    PubMed

    Wang, Yue-si; Xin, Jin-yuan; Li, Zhan-qing; Wang, Pu-cai; Wang, Shi-gong; Wen, Tian-xue; Sun, Yang

    2006-09-01

    Atmospheric aerosol optical depth (AOD(lamda=500 nm)), Angstrom turbidity coefficient (beta) and Angstrom wavelength exponent (alpha) are obtained using the CERN sun hazemeter network from Aug to Dec, 2004. The results are as follows: At the Tibetan Plateau, Haibei and Lhasa, the mean of AOD is 0.09, 0.12; the mean of beta is 0.05, 0.13; the mean of a is 1.09, 0.06, respectively. At the Northeast of China, Hailun and Sanjiang, the mean of AOD is 0.14, 0.15; the mean of beta is 0.04, 0.06; the mean of a is 2.32, 1.58, respectively. At the desert region of North China, e.g., Fukang, Shapotou and Eerduosi, the range of averaged AOD is from 0.17 to 0.32; the range of averaged beta is from 0.09 to 0.19; the range of averaged a is from 0.68.to 1.28. At the forest areas, e.g. Changbai Mountain, Beijing forest and Xishuangbanna, the range of averaged AOD is from 0.19 to 0.42; the range of averaged beta is from 0.12 to 0.19; the range of averaged a is from 1.11 to 1.25. At agriculture areas, e.g. Shenyang, Fengqiu, Taoyuan and Yanting, the range of averaged AOD is from 0.34 to 0.68; the range of averaged beta is from 0.18 to 0.38; the range of averaged a is from 0.97 to 1.39. At the littoral areas and the lake of East China, e.g. Jiaozhou Bay, Shanghai City and Tai Lake, the range of averaged AOD is from 0.49 to 0.68; the range of averaged beta is from 0.21 to 0.29; the range of averaged a is from 1.24 to 1.37. At the inland cities, Beijing City and Lanzhou City, the mean of AOD is 0.47, 0.81; the mean of beta is 0.20, 0.45; the mean of a is 1.66, 0.89, respectively. The variations of aerosol properties at nineteen stations are explained in the paper. PMID:17117619

  4. Dependence of Aerosol Light Absorption and Single-Scattering Albedo On Ambient Relative Humidity for Sulfate Aerosols with Black Carbon Cores

    NASA Technical Reports Server (NTRS)

    Redemann, Jens; Russell, Philip B.; Hamill, Patrick

    2001-01-01

    Atmospheric aerosols frequently contain hygroscopic sulfate species and black carbon (soot) inclusions. In this paper we report results of a modeling study to determine the change in aerosol absorption due to increases in ambient relative humidity (RH), for three common sulfate species, assuming that the soot mass fraction is present as a single concentric core within each particle. Because of the lack of detailed knowledge about various input parameters to models describing internally mixed aerosol particle optics, we focus on results that were aimed at determining the maximum effect that particle humidification may have on aerosol light absorption. In the wavelength range from 450 to 750 nm, maximum absorption humidification factors (ratio of wet to 'dry=30% RH' absorption) for single aerosol particles are found to be as large as 1.75 when the RH changes from 30 to 99.5%. Upon lesser humidification from 30 to 80% RH, absorption humidification for single particles is only as much as 1.2, even for the most favorable combination of initial ('dry') soot mass fraction and particle size. Integrated over monomodal lognormal particle size distributions, maximum absorption humidification factors range between 1.07 and 1.15 for humidification from 30 to 80% and between 1.1 and 1.35 for humidification from 30 to 95% RH for all species considered. The largest humidification factors at a wavelength of 450 nm are obtained for 'dry' particle size distributions that peak at a radius of 0.05 microns, while the absorption humidification factors at 700 nm are largest for 'dry' size distributions that are dominated by particles in the radius range of 0.06 to 0.08 microns. Single-scattering albedo estimates at ambient conditions are often based on absorption measurements at low RH (approx. 30%) and the assumption that aerosol absorption does not change upon humidification (i.e., absorption humidification equal to unity). Our modeling study suggests that this assumption alone can

  5. Anti-hygroscopic effect of dextrans in herbal formulations.

    PubMed

    Tong, Henry H Y; Wong, Sammas Y S; Law, Marcus W L; Chu, Kevin K W; Chow, Albert H L

    2008-11-01

    Equilibrium moisture sorptions of two dried aqueous herbal extracts and their mixtures with dextrans of various molecular weights were investigated as a function of relative humidity at ambient temperature, and the data were analyzed by both the Guggenheim-Anderson-deBoer (GAB) and Brunauer-Emmett-Teller (BET) equations. Glass transition temperatures (T(g)) of the samples were measured by differential scanning calorimetry, and their dependence on the moisture contents of the extracts was analyzed by the linear, Fox and expanded Gordon-Taylor mathematical models. All dextran-extract mixtures exhibited single T(g) values, indicating that they existed as single homogeneous phases. The BET equation was found adequate for description of the moisture sorption isotherms for all samples. The dextrans appeared to reduce the hygroscopicity of the herbal extracts solely by a dilution effect. The observed increase in T(g) and accompanying decrease in tackiness of the herbal extracts in the presence of dextrans may be explained by the ability of dextrans to restrict the molecular mobility of simple sugars and to counteract the plasticizing effect of water in the extracts. The expanded Gordon-Taylor equation has proved useful in predicting the T(g) of hygroscopic amorphous herbal mixtures. PMID:18706495

  6. The chemical composition of fine ambient aerosol particles in the Beijing area

    NASA Astrophysics Data System (ADS)

    Nekat, Bettina; van Pinxteren, Dominik; Iinuma, Yoshiteru; Gnauk, Thomas; Müller, Konrad; Herrmann, Hartmut

    2010-05-01

    The strong economical growth in China during the last few decades led to heavy air pollution caused by significantly increased particle emissions. The aerosol particles affect not only the regional air quality and visibility, but can also influence cloud formation processes and the radiative balance of the atmosphere by their optical and microphysical properties. The ability to act as Cloud Condensation Nuclei (CCN) is related to microphysical properties like the hygroscopic growth or the cloud droplet activation. The chemical composition of CCN plays an important role on these properties and varies strongly with the particle size and the time of day. Hygroscopic or surface active substances can increase the hygroscopicity and lower the surface tension of the particle liquid phase, respectively. The presence of such compounds may result in faster cloud droplet activation by faster water uptake. The DFG project HaChi (Haze in China) aimed at studying physical and chemical parameters of urban aerosol particles in the Beijing area in order to associate the chemical composition of aerosol particles with their ability to act as CCN. To this end, two measurement campaigns were performed at the Wuqing National Ordinary Meteorological Observing Station, which is a background site near Beijing. The winter campaign was realized in March 2009 and the summer campaign took place from mid July 2009 to mid August 2009. Fine particles with an aerodynamic diameter smaller than or equal 1 μm were continuously sampled for 24h over the two campaigns using a DIGITEL high volume sampler (DHA-80). The present contribution presents and discusses the results of the chemical characterization of the DIGITEL filters samples. The filters were analyzed for the mass concentration, inorganic ions and carbon sum parameters like elemental (EC), organic (OC) and water soluble organic carbon (WSOC). The WSOC fraction was further characterized for hygroscopic substances like low molecular

  7. Evolution of Organic Aerosols in the Atmosphere.

    SciTech Connect

    Jimenez, J. L.; Canagaratna, M. R.; Donahue, N. M.; Prevot, A. S. H.; Zhang, Qi; Kroll, Jesse H.; DeCarlo, Peter F.; Allan, James D.; Coe, H.; Ng, N. L.; Aiken, Allison; Docherty, Kenneth S.; Ulbrich, Ingrid M.; Grieshop, A. P.; Robinson, A. L.; Duplissy, J.; Smith, J. D.; Wilson, K. R.; Lanz, V. A.; Hueglin, C.; Sun, Y. L.; Tian, J.; Laaksonen, A.; Raatikainen, T.; Rautiainen, J.; Vaattovaara, P.; Ehn, M.; Kulmala, M.; Tomlinson, Jason M.; Collins, Donald R.; Cubison, Michael J.; Dunlea, E. J.; Huffman, John A.; Onasch, Timothy B.; Alfarra, M. R.; Williams, Paul I.; Bower, K.; Kondo, Yutaka; Schneider, J.; Drewnick, F.; Borrmann, S.; Weimer, S.; Demerjian, K.; Salcedo, D.; Cottrell, L.; Griffin, Robert; Takami, A.; Miyoshi, T.; Hatakeyama, S.; Shimono, A.; Sun, J. Y.; Zhang, Y. M.; Dzepina, K.; Kimmel, Joel; Sueper, D.; Jayne, J. T.; Herndon, Scott C.; Trimborn, Achim; Williams, L. R.; Wood, Ezra C.; Middlebrook, A. M.; Kolb, C. E.; Baltensperger, Urs; Worsnop, Douglas R.

    2009-12-11

    Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework that describes the atmospheric evolution of OA and is constrained and motivated by new, high time resolution, experimental characterizations of their composition, volatility, and oxidation state. OA and OA-precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of large amounts of oxygenated organic aerosol (OOA) mass that has comparable concentrations to sulfate aerosol over the Northern Hemisphere. Our new model framework captures the dynamic aging behavior observed in the atmosphere and the laboratory and can serve as a basis for improving parameterizations in regional and global models.

  8. Some Algorithms For Simulating Size-resolved Aerosol Dynamics Models

    NASA Astrophysics Data System (ADS)

    Debry, E.; Sportisse, B.

    The objective of this presentation is to show some algorithms used to solve aerosol dynamics in 3D dispersion models. INTRODUCTION The gas phase pollution has been widely studied and some models are now available . The situation is quite different with respect to atmospheric aerosols . However at- mospheric particulate matter significantly influences atmospheric properties such as radiative balance, cloud formation, gas pollutants concentrations ( gas to particle con- version ), and has an impact on man health. As aerosols properties ( optical, hygroscopic, noxiousness ) depend mainly on their size, it appears important to be able to follow the aerosol ( or particle ) size distribution (PSD) during time. This former is modified by physical processes as coagulation, condensation or evaporation, nucleation and removal. Aerosol dynamics is usually modelized by the well-known General Dynamics Equation (GDE) [1]. MODELS Several models already exist to solve this equation. Multi-modal models are widely used [2] [3] because of the few parameters needed, but the GDE is solved only on its moments and the PSD is assumed to remain in a log-normal form. On the contrary, size-resolved models implies a discretization of the aerosol size spec- trum into several bins and to solve the GDE within each one. This step can be per- formed either by resolving each process separately ( splitting ), for example coagula- tion can be resolved by the well-known "size-binning" algorithms [4] and condensa- tion leads to an advection equation on the PSD [5], or by coupling all processes, what the finite elements [6] and stochastic methods [7] allows. Stochastic algorithms may not be competitive compared to deterministic ones with respect to the computation time, but they provide reference solutions useful to validate more operational codes on realistic cases, as analytic solutions of the GDE exist only for academic cases. REFERENCES [1] Seinfeld, J.H. and Pandis,S.N. Atmospheric chemistry and

  9. Rapid changes in biomass burning aerosols by atmospheric oxidation

    NASA Astrophysics Data System (ADS)

    Vakkari, Ville; Kerminen, Veli-Matti; Beukes, Johan Paul; Tiitta, Petri; Zyl, Pieter G.; Josipovic, Miroslav; Venter, Andrew D.; Jaars, Kerneels; Worsnop, Douglas R.; Kulmala, Markku; Laakso, Lauri

    2014-04-01

    Primary and secondary aerosol particles originating from biomass burning contribute significantly to the atmospheric aerosol budget and thereby to both direct and indirect radiative forcing. Based on detailed measurements of a large number of biomass burning plumes of variable age in southern Africa, we show that the size distribution, chemical composition, single-scattering albedo, and hygroscopicity of biomass burning particles change considerably during the first 2-4 h of their atmospheric transport. These changes, driven by atmospheric oxidation and subsequent secondary aerosol formation, may reach a factor of 6 for the aerosol scattering coefficient and a factor >10 for the cloud condensation nuclei concentration. Since the observed changes take place over the spatial and temporal scales that are neither covered by emission inventories nor captured by large-scale model simulations, the findings reported here point out a significant gap in our understanding on the climatic effects of biomass burning aerosols.

  10. Technical study of some major parameters influencing the performance of an aerosol delivery equipment suitable for calves.

    PubMed

    Genicot, B; Peckova, M; Close, R; Lindsey, J K; Lambert, P; Lekeux, P

    1994-01-01

    Aerosol delivery equipment, suitable for the treatment of bovine respiratory dysfunctions and including 2 parallelly positioned jet nebulizers, was studied in depth in order to determine the optimal working conditions in the field. Indeed, some factors might reasonably alter the performance of this equipment. Among these factors, the influences of the parallel position of jet nebulizers (in order to accommodate the breathing requirements of the cattle and achieve a rapid treatment), of the long feed pipe delivering compressed air (in order to keep the animal away from the compressor unit), and finally of the ambient temperature were studied, this equipment being essentially used during the winter season. This equipment could accommodate the breathing needs of cattle weighing up to 225 kg if a pressure of 600 kPa was developed upstream to the nebulizers. The rate of atomization was significantly reduced when working at ambient air temperatures (272.25 K < T < 274.65 K) close to those encountered in winter. This was especially true when pressure upstream to the nebulizers did not exceed 500 kPa. The immersion of the feed pipe for compressed air in hot water led to an increase in the rate of atomization without raising evaporative water losses, and reduced the drop in temperature in the nebulizer solution. Finally, the rate of atomization significantly increased when the face mask including the nebulizers was maintained so that the nebulizers were in a vertical position or at an angle not less than 60 degrees with respect to the ground. PMID:7951349

  11. Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008

    NASA Astrophysics Data System (ADS)

    Lathem, T. L.; Beyersdorf, A. J.; Thornhill, K. L.; Winstead, E. L.; Cubison, M. J.; Hecobian, A.; Jimenez, J. L.; Weber, R. J.; Anderson, B. E.; Nenes, A.

    2013-03-01

    The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50-85° N and 40-130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66-94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08-0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (ɛWSOM), with a κ = 0.12, such that κorg = 0.12ɛWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine

  12. Aerosol phase transformation in the atmosphere

    SciTech Connect

    Tang, I.N.; Munkelwitz, H.R.

    1992-09-01

    Ambient aerosols are frequently composed of hygroscopic inorganic salts such as chlorides, sulfates and nitrates in either pure or mixed forms. Such inorganic salt aerosols exhibit the properties of deliquescence and efflorescence in air. The phase transformation from a solid particle to a saline droplet usually occurs spontaneously when atmospheric relative humidity reaches a level specific to the chemical composition of the aerosol particle. Conversely, when relative humidity decreases and becomes low enough, a saline droplet will evaporate and suddenly crystallize, expelling all its water content. Information on the composition and temperature dependence of these properties is required in mathematical models for describing the dynamic and transport behavior of ambient aerosols. Experiments are carried out in the temperature range 5--35{degrees}C, using single particles individually suspended in an electrodynamic cell that can be evacuated and back filled with water vapor. The phase transformation of the aerosol particle is monitored by laser light scattering and the relative humidity at the transition point is determined by directly measuring the water vapor pressure in the cell. Results are obtained for particles containing either a single salt or a preselected mixture of NaCl, KCl, NaNO{sub 3}, Na{sub 2}SO{sub 4} and (NH{sub 4}){sub 2}SO{sub 4}, which are common constituents of ambient aerosols. A theoretical model on the composition and temperature dependence of the deliquescence properties is developed for single and two-salt aerosol systems.

  13. Automated Measurements of Ambient Aerosol Chemical Composition and its Dry and Wet Size Distributions at Pittsburgh Supersite

    NASA Astrophysics Data System (ADS)

    Khlystov, A. Y.; Stanier, C.; Chun, W.; Vayenas, D.; Mandiro, M.; Pandis, S. N.

    2001-12-01

    Ambient aerosol particles change size with changes in ambient relative humidity. The magnitude of the size change depends on the hygroscopic properties of the particles, which is determined by their chemical composition. Hygroscopic properties of particles influence many environmentally important aerosol qualities, such as light scattering and partitioning between the gas and particle phases of semivolitile compounds. Studying the hygroscopic growth of ambient particles is thus of paramount importance. The highroscopic growth of ambient particles and their chemical composition are measured continuously within the Pittsburgh Air Quality Study (EPA supersite program). The hygroscopic size changes are measured using an automated system built for this study. The system consists of two Scanning Mobility Particle Sizers (SMPS, TSI Inc.) and an Aerodynamic Particle Sizer (APS, TSI Inc.). The three instruments measure aerosol size distribution between 5 nanometers and 10 micrometers in diameter. The inlets of the instruments and the sheath air lines of the SMPS systems are equipped with computer controlled valves that direct air through Nafion dryers (PermaPure Inc.) or bypass them. The Nafion dryers are drying the air stream below 40% RH at which point ambient particles are expected to lose most or all water and thus be virtually dry. To avoid changes in relative humidity and evaporation of volatile particles due to temperature differences the system is kept at ambient temperature. The system measures alternatively dry (below 40% RH) and wet (actual ambient RH) aerosol size distributions every 6 minutes. The hygroscopic growth observed with the size-spectrometer system is compared with theoretic predictions based on the chemical composition of aerosol particles. A modified semi-continuous Steam-Jet Aerosol Collector provides the total available budget (particles and gas) of water-soluble species, which is used as an input to the thermodynamic model. The model calculates

  14. Control of binder viscosity and hygroscopicity on particle aggregation efficiency

    NASA Astrophysics Data System (ADS)

    Mueller, Sebastian B.; Kueppers, Ulrich; Ayris, Paul M.; Jacob, Michael; Delmelle, Pierre; Dingwell, Donald B.

    2016-04-01

    In the course of explosive volcanic eruptions, large amounts of ash are released into the atmosphere and may subsequently pose a threat to infrastructure, such as aviation industry. Ash plume forecasting is therefore a crucial tool for volcanic hazard mitigation but may be significantly affected by aggregation, altering the aerodynamic properties of particles. Models struggle with the implementation of aggregation since external conditions promoting aggregation have not been completely understood; in a previous study we have shown the rapid generation of ash aggregates through liquid bonding via the use of fluidization bed technology and further defined humidity and temperature ranges necessary to trigger aggregation. Salt (NaCl) was required for the recovery of stable aggregates, acting as a cementation agent and granting aggregate cohesion. A numerical model was used to explain the physics behind particle aggregation mechanisms and further predicted a dependency of aggregation efficiency on liquid binder viscosity. In this study we proof the effect of viscosity on particle aggregation. HCl and H2SO4 solutions were diluted to various concentrations resulting in viscosities between 1 and 2 mPas. Phonolitic and rhyolitic ash samples as well as soda-lime glass beads (serving as analogue material) were fluidized in the ProCell Lab® of Glatt Ingenieurtechnik GmbH and treated with the acids via a bottom-spray technique. Chemically driven interaction between acid liquids and surfaces of the three used materials led to crystal precipitation. Salt crystals (e.g. NaCl) have been confirmed through scanning electron microscopy (SEM) and leachate analysis. Both volcanic ash samples as well as the glass beads showed a clear dependency of aggregation efficiency on viscosity of the sprayed HCl solution. Spraying H2SO4 provoked a collapse of the fluidized bed and no aggregation has been observed. This is accounted by the high hygroscopicity of H2SO4. Dissolving CaCl2 (known to be

  15. The regime of aerosol asymmetry parameter and Angstrom exponent over Europe, Mediterranean and Middle East based on MODIS satellite data. Intercomparison of MODIS-Aqua C051 and C006 retrievals

    NASA Astrophysics Data System (ADS)

    Korras-Carraca, Marios Bruno; Hatzianastassiou, Nikolaos; Matsoukas, Christos; Gkikas, Antonis; Papadimas, Christos; Sayers, Andy

    2015-04-01

    Atmospheric aerosols, both natural and anthropogenic, can cause climate change through their direct, indirect, and semi-direct effects on the radiative energy budget of the Earth-atmosphere system. In the present work, we study two of the most important optical properties of aerosols, the asymmetry parameter (gaer) and the Angstrom exponent (α). Both gaer and α are related with aerosol size, which is a very important parameter for climate and human health. The study region comprises North Africa, the Arabian peninsula, Europe, and the Mediterranean basin. These areas are of great interest, because of the variety of aerosol types they host, both anthropogenic and natural. Urban, industrial or biomass-burning aerosols are usually fine, while desert dust or sea-salt are basically coarse, making thus possible the establishment of a relationship between the type and the size of aerosols. Using satellite data from the collection 051 of MODIS (MODerate resolution Imaging Spectroradiometer, Aqua), we investigate the spatio-temporal characteristics of the asymmetry parameter and Angstrom exponent. We generally find significant spatial variability, with larger gaer values over regions dominated by larger size particles, e.g. outside the Atlantic coasts of north-western Africa, where desert-dust outflow is taking place. The gaer values tend to decrease with increasing wavelength, especially over areas dominated by small particulates. The intra-annual variability is found to be small in desert-dust areas, with maximum values during summer, while in all other areas larger values are reported during the cold season and smaller during the warm. Significant intra-annual and inter-annual variability is observed around the Black Sea. However, the inter-annual trends of gaer are found to be generally small. The geographical distributions for α (given for the pair of wavelengths 550-865 nm) affirm the conclusions drawn from the asymmetry parameter as regards the aerosol size over

  16. Anisotropically functionalized carbon nanotube array based hygroscopic scaffolds.

    PubMed

    Ozden, Sehmus; Ge, Liehui; Narayanan, Tharangattu N; Hart, Amelia H C; Yang, Hyunseung; Sridhar, Srividya; Vajtai, Robert; Ajayan, Pulickel M

    2014-07-01

    Creating ordered microstructures with hydrophobic and hydrophilic moieties that enable the collection and storage of small water droplets from the atmosphere, mimicking structures that exist in insects, such as the Stenocara beetle, which live in environments with limited amounts of water. Inspired by this approach, vertically aligned multiwalled carbon nanotube forests (NTFs) are asymmetrically end-functionalized to create hygroscopic scaffolds for water harvesting and storage from atmospheric air. One side of the NTF is made hydrophilic, which captures water from the atmosphere, and the other side is made superhydrophobic, which prevents water from escaping and the forest from collapsing. To understand how water penetrates into the NTF, the fundamentals of water/NTF surface interaction are discussed. PMID:24896731

  17. Inhibition of Condensation Frosting by Arrays of Hygroscopic Antifreeze Drops.

    PubMed

    Sun, Xiaoda; Damle, Viraj G; Uppal, Aastha; Linder, Rubin; Chandrashekar, Sriram; Mohan, Ajay R; Rykaczewski, Konrad

    2015-12-29

    The formation of frost and ice can have negative impacts on travel and a variety of industrial processes and is typically addressed by dispensing antifreeze substances such as salts and glycols. Despite the popularity of this anti-icing approach, some of the intricate underlying physical mechanisms are just being unraveled. For example, recent studies have shown that in addition to suppressing ice formation within its own volume, an individual salt saturated water microdroplet forms a region of inhibited condensation and condensation frosting (RIC) in its surrounding area. This occurs because salt saturated water, like most antifreeze substances, is hygroscopic and has water vapor pressure at its surface lower than water saturation pressure at the substrate. Here, we demonstrate that for macroscopic drops of propylene glycol and salt saturated water, the absolute RIC size can remain essentially unchanged for several hours. Utilizing this observation, we demonstrate that frost formation can be completely inhibited in-between microscopic and macroscopic arrays of propylene glycol and salt saturated water drops with spacing (S) smaller than twice the radius of the RIC (δ). Furthermore, by characterizing condensation frosting dynamics around various hygroscopic drop arrays, we demonstrate that they can delay complete frosting over of the samples 1.6 to 10 times longer than films of the liquids with equivalent volume. The significant delay in onset of ice nucleation achieved by dispensing propylene glycol in drops rather than in films is likely due to uniform dilution of the drops driven by thermocapillary flow. This transport mode is absent in the films, leading to faster dilution, and with that facilitated homogeneous nucleation, near the liquid-air interface. PMID:26651017

  18. Hygroscopic salts and the potential for life on Mars.

    PubMed

    Davila, Alfonso F; Duport, Luis Gago; Melchiorri, Riccardo; Jänchen, Jochen; Valea, Sergio; de Los Rios, Asunción; Fairén, Alberto G; Möhlmann, Diedrich; McKay, Christopher P; Ascaso, Carmen; Wierzchos, Jacek

    2010-01-01

    Hygroscopic salts have been detected in soils in the northern latitudes of Mars, and widespread chloride-bearing evaporitic deposits have been detected in the southern highlands. The deliquescence of hygroscopic minerals such as chloride salts could provide a local and transient source of liquid water that would be available for microorganisms on the surface. This is known to occur in the Atacama Desert, where massive halite evaporites have become a habitat for photosynthetic and heterotrophic microorganisms that take advantage of the deliquescence of the salt at certain relative humidity (RH) levels. We modeled the climate conditions (RH and temperature) in a region on Mars with chloride-bearing evaporites, and modeled the evolution of the water activity (a(w)) of the deliquescence solutions of three possible chloride salts (sodium chloride, calcium chloride, and magnesium chloride) as a function of temperature. We also studied the water absorption properties of the same salts as a function of RH. Our climate model results show that the RH in the region with chloride-bearing deposits on Mars often reaches the deliquescence points of all three salts, and the temperature reaches levels above their eutectic points seasonally, in the course of a martian year. The a(w) of the deliquescence solutions increases with decreasing temperature due mainly to the precipitation of unstable phases, which removes ions from the solution. The deliquescence of sodium chloride results in transient solutions with a(w) compatible with growth of terrestrial microorganisms down to 252 K, whereas for calcium chloride and magnesium chloride it results in solutions with a(w) below the known limits for growth at all temperatures. However, taking the limits of a(w) used to define special regions on Mars, the deliquescence of calcium chloride deposits would allow for the propagation of terrestrial microorganisms at temperatures between 265 and 253 K, and for metabolic activity (no growth) at