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Sample records for aerosol hygroscopic growth

  1. Phase transformation and growth of hygroscopic aerosols

    SciTech Connect

    Tang, I.N.

    1995-09-01

    Ambient aerosols frequently contain large portions of hygroscopic inorganic salts such as chlorides, nitrates, and sulfates 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 the relative humidity of the atmosphere reaches a level specific to the chemical composition of the aerosol particle. Conversely, when the relative humidity decreases and becomes low enough, the saline droplet will evaporate and suddenly crystallize, expelling all its water content. The phase transformation and growth of aerosols play an important role in many atmospheric processes affecting air quality, visibility degradation, and climate changes. In this chapter, an exposition of the underlying thermodynamic principles is given, and recent advances in experimental methods utilizing single-particle levitation are discussed. In addition, pertinent and available thermodynamic data, which are needed for predicting the deliquescence properties of single and multi-component aerosols, are compiled. This chapter is useful to research scientists who are either interested in pursuing further studies of aerosol thermodynamics, or required to model the dynamic behavior of hygroscopic aerosols in a humid environment.

  2. Subarctic atmospheric aerosol composition: 2. Hygroscopic growth properties

    SciTech Connect

    Herich, Hanna; Kammermann, Lukas; Friedman, Beth; Gross, Deborah S.; Weingartner, E.; Lohmann, U.; Spichtinger, Peter; Gysel, Martin; Baltensperger, Urs; Cziczo, Daniel J.

    2009-07-10

    Sub-arctic aerosols were sampled during July 2007 at the Abisko Scientific Research Station Stordalen site in northern Sweden with an instrument setup consisting of a custom-built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) connected in series to a single particle mass spectrometer. Aerosol chemical composition in the form of bipolar single particle mass spectra was determined as a function of hygroscopic growth both in situ and in real time. The HTDMA was deployed at a relative humidity of 82% and particles with a dry mobility diameter of 260 nm were selected. Aerosols from two distinct airmasses were analyzed during the sampling period. Sea salt aerosols were found to be the dominant particle group with the highest hygroscopicity. High intensities of sodium and related peaks in the mass spectra were identified as exclusive markers for large hygroscopic growth. Particles from biomass combustion were found to be the least hygroscopic aerosol category. Species normally considered soluble (e.g., sulfates and nitrates) were found in particles ranging from high to low hygroscopicity. Furthermore, the signal intensities of the peaks related to these species did not correlate with hygroscopicity.

  3. Phase transformation and growth of hygroscopic aerosols

    SciTech Connect

    Tang, I.N.

    1999-11-01

    Ambient aerosols play an important role in many atmospheric processes affecting air quality, visibility degradation, and climatic changes as well. Both natural and anthropogenic sources contribute to the formation of ambient aerosols, which are composed mostly of sulfates, nitrates, and chlorides in either pure or mixed forms. These inorganic salt aerosols are hygroscopic by nature and exhibit the properties of deliquescence and efflorescence in humid air. For pure inorganic salt particles with diameter larger than 0.1 micron, the phase transformation from a solid particle to a saline droplet occurs only when the relative humidity in the surrounding atmosphere reaches a certain critical level corresponding to the water activity of the saturated solution. The droplet size or mass in equilibrium with relative humidity can be calculated in a straightforward manner from thermodynamic considerations. For aqueous droplets 0.1 micron or smaller, the surface curvature effect on vapor pressure becomes important and the Kelvin equation must be used.

  4. 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.

  5. 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

  6. 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.

  7. Aerosol hygroscopic growth parameterization based on a solute specific coefficient

    NASA Astrophysics Data System (ADS)

    Metzger, S.; Steil, B.; Xu, L.; Penner, J. E.; Lelieveld, J.

    2011-09-01

    Water is a main component of atmospheric aerosols and its amount depends on the particle chemical composition. We introduce a new parameterization for the aerosol hygroscopic growth factor (HGF), based on an empirical relation between water activity (aw) and solute molality (μs) through a single solute specific coefficient νi. Three main advantages are: (1) wide applicability, (2) simplicity and (3) analytical nature. (1) Our approach considers the Kelvin effect and covers ideal solutions at large relative humidity (RH), including CCN activation, as well as concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). (2) A single νi coefficient suffices to parameterize the HGF for a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. (3) In contrast to previous methods, our analytical aw parameterization depends not only on a linear correction factor for the solute molality, instead νi also appears in the exponent in form x · ax. According to our findings, νi can be assumed constant for the entire aw range (0-1). Thus, the νi based method is computationally efficient. In this work we focus on single solute solutions, where νi is pre-determined with the bisection method from our analytical equations using RHD measurements and the saturation molality μssat. The computed aerosol HGF and supersaturation (Köhler-theory) compare well with the results of the thermodynamic reference model E-AIM for the key compounds NaCl and (NH4)2SO4 relevant for CCN modeling and calibration studies. The equations introduced here provide the basis of our revised gas-liquid-solid partitioning model, i.e. version 4 of the EQuilibrium Simplified Aerosol Model (EQSAM4), described in a companion paper.

  8. 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.

  9. In-situ determination of atmospheric aerosol composition as a function of hygroscopic growth

    SciTech Connect

    Herich, Hanna; Kammermann, Lukas; Gysel, Martin; Weingartner, E.; Baltensperger, Urs; Lohmann, U.; Cziczo, Daniel J.

    2008-08-30

    An in-situ measurement setup to determine the chemical composition of aerosols as a function of hygroscopicity is presented. This has been done by connecting a custom-built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) and an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS), commercially available from TSI (Model 3800). Single particle bipolar mass spectra from aerosols leaving the HTDMA could thus be obtained as a function of the hygroscopic growth factor. For these studies the HTDMA was set at a relative humidity of 82% and particles with a dry diameter of 260 nm were selected. The setup was first laboratory tested after which field experiments were performed. Two datasets were obtained during wintertime 2007 in Switzerland: the first in the urban Zurich environment and the other at the remote high alpine research station Jungfraujoch (JFJ). In Zurich several thousand mass spectra were obtained in less than two days of sampling due to a high aerosol loading. At the JFJ, due to low particle concentrations in free tropospheric airmasses, a longer sampling period was required. Both in Zurich and at the JFJ two different growth factor modes were observed. Results from these two locations show that most aerosol particles were a mixture of several compounds. A large contribution of organics and combustion species was found in the less hygroscopic growth mode for both locations. Non-combustion refractory material (e.g. metals, mineral dust, and fly ash) was also highly enhanced in the non-hygroscopic particles. Sulfate, normally considered highly soluble, was found to be a constituent in almost all particles independent of their hygroscopic growth factor.

  10. Absorbing aerosols at high relative humidity: linking hygroscopic growth to optical properties

    NASA Astrophysics Data System (ADS)

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

    2012-06-01

    One of the major uncertainties in the understanding of Earth's climate system is the interaction between solar radiation and aerosols in the atmosphere. Aerosols exposed to high humidity will change their chemical, physical, and optical properties due to their increased water content. To model hydrated aerosols, atmospheric chemistry and climate models often use the volume weighted mixing rule to predict the complex refractive index (RI) of aerosols when they interact with high relative humidity, and, in general, assume homogeneous mixing. This study explores the validity of these assumptions. A humidified cavity ring down aerosol spectrometer (CRD-AS) and a tandem hygroscopic DMA (differential mobility analyzer) are used to measure the extinction coefficient and hygroscopic growth factors of humidified aerosols, respectively. The measurements are performed at 80% and 90%RH at wavelengths of 532 nm and 355 nm using size-selected aerosols with different degrees of absorption; from purely scattering to highly absorbing particles. The ratio of the humidified to the dry extinction coefficients (fRHext(%RH, Dry)) is measured and compared to theoretical calculations based on Mie theory. Using the measured hygroscopic growth factors and assuming homogeneous mixing, the expected RIs using the volume weighted mixing rule are compared to the RIs derived from the extinction measurements. We found a weak linear dependence or no dependence of fRH(%RH, Dry) with size for hydrated absorbing aerosols in contrast to the non-monotonically decreasing behavior with size for purely scattering aerosols. No discernible difference could be made between the two wavelengths used. Less than 7% 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. However, for substances with growth factor less than 1.15 the volume weighted mixing rule assumption

  11. Control over hygroscopic growth of saline aqueous aerosol using Pluronic polymer additives.

    PubMed

    Haddrell, Allen E; Hargreaves, Graham; Davies, James F; Reid, Jonathan P

    2013-02-25

    The hygroscopic properties of an aerosol originating from a nebulizer solution can affect the extent of peripheral deposition within the respiratory tract, which in turn affects drug efficacy of drugs delivered to the lungs. Thus, the ability to tailor the degree and rate of hygroscopic growth of an aerosol produced by a nebulizer through modification of the formulation would serve to improve drug efficacy through targeted lung deposition. In this study, the kinetic and thermodynamic hygroscopic properties of sodium chloride aerosol mixed with commercially available Pluronic polymers, specifically F77 and F127, are reported using three complementary single aerosol analysis techniques, specifically aerosol optical tweezers, a double ring electrodynamic balance and a concentric cylinder electrodynamic balance. The F77 polymer is shown to have a predictable effect on the hygroscopic properties of the aerosol: the ability of the droplet to uptake water from the air depends on the solute weight percent of sodium chloride present in a linear dose dependant manner. Unlike the smaller F77, a non-linear relationship was observed for the larger molecular weight F127 polymer, with significant suppression of hygroscopic growth (>50% by mass) for solution aerosol containing even only 1 wt% of the polymer and 99 wt% sodium chloride. The suppression of growth is shown to be consistent with the formation of mixed phase aerosol particles containing hydrophilic inorganic rich domains and hydrophobic polymer rich domains that sequester some of the inorganic component, with the two phases responding to changes in relative humidity independently. This independence of coupling with the gas phase is apparent in both the equilibrium state and the kinetics of water evaporation/condensation. By starting with a saline nebulizer solution with a concentration of F127 ∼10(-2)mM, a 12% reduction in the radius of all aerosol produced at a relative humidity (RH) of 84% is possible. The

  12. Diurnal variations in the hygroscopic growth cycles of ambient aerosol populations

    NASA Astrophysics Data System (ADS)

    Santarpia, Joshua L.; Gasparini, Roberto; Li, Runjun; Collins, Don R.

    2005-02-01

    During August and September of 2002, a relative humidity (RH) scanning tandem differential mobility analyzer system was used to measure the deliquescence/crystallization properties of ambient aerosol populations in southeast Texas. During August, sampling was conducted at a rural site on the Texas A&M campus in College Station, and in September, sampling was conducted at an urban site near the Houston ship channel. Measurements from both sites indicate that there are cyclical changes in the composition of the soluble fraction of the aerosol, which are not strongly linked to the local aerosol source. The observations show that as temperature increases and RH decreases, the hysteresis loop describing the RH dependence of aerosol hygroscopic growth collapses. On the basis of results from other studies that have shown the dominant ions present in aerosols in this region to be ammonium and sulfate, it is proposed that this collapse is due to a decrease in the ammonium to sulfate ratio in the aerosol particles, which coincides with increasing temperature and decreasing RH. This cyclical change in aerosol acidity may influence secondary organic aerosol production and may exaggerate the impact of the aerosol on human health. The compositional changes also result in a daily cycle in crystallization RH that is in phase with that of the ambient RH, which reduces the probability that hygroscopic particles will crystallize in the afternoon when the ambient RH is a minimum.

  13. Photochemical aging of secondary organic aerosols: effects on hygroscopic growth and CCN activation

    NASA Astrophysics Data System (ADS)

    Buchholz, A.; Mentel, Th. F.; Tillmann, R.; Schlosser, E.; Mildenberger, K.; Clauss, T.; Henning, S.; Kiselev, A.; Stratmann, F.

    2009-04-01

    Plant emitted volatile organic carbons (VOCs) are a major precursor of secondary organic aerosols (SOA), an important constituent of atmospheric aerosols. The precursors are oxidized via ozonolysis, photooxidation, or by NO3 and form aerosol particles. Due to further oxidation of the organic matter the composition of the SOA may age with time. This will also change the hygroscopic growth (HG) and cloud condensation nuclei (CCN) activation of the particles. In this study we generated and aged SOA in the SAPHIR chamber at the Research Centre Juelich under near atmospheric conditions: natural sunlight, low precursor and O3 concentrations, and long reaction times. As precursor we used a mixture of 5 monoterpenes (MT) or 5 MT with 2 sesquiterpenes which had been identified as major constituents of plant emissions in previous experiments. Concentrations ranged between 4 and 100 ppb MT and the total reaction time was 36h. HG was measured at RH=10-97% by a Hygroscopic Tandem Differential Analyser (HTDMA, FZ Juelich) and at RH=97-99% by the Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile, IfT Leipzig). The agreement between HTDMA and LACIS-mobile data was generally good. CCN properties were measured with a continuous flow CCN Counter from DMT. SOA particles generated on a sunny day were more hygroscopic and had a lower activation diameter (Dcrit) than SOA formed under cloudy conditions. With aging it became more hygroscopic and Dcrit decreased. Sunlight enhanced this effect. But the change in HG and Dcrit due to aging was less than the difference between SOA generated under different conditions (i.e. sunny or cloudy). We did not observe a dependence of the HG on the precursor concentration.

  14. 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

  15. 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.

  16. Understanding hygroscopic growth and phase transformation of aerosols using single particle Raman spectroscopy in an electrodynamic balance.

    PubMed

    Lee, Alex K Y; Ling, T Y; Chan, Chak K

    2008-01-01

    Hygroscopic growth is one of the most fundamental properties of atmospheric aerosols. By absorbing or evaporating water, an aerosol particle changes its size, morphology, phase, chemical composition and reactivity and other parameters such as its refractive index. These changes affect the fate and the environmental impacts of atmospheric aerosols, including global climate change. The ElectroDynamic Balance (EDB) has been widely accepted as a unique tool for measuring hygroscopic properties and for investigating phase transformation of aerosols via single particle levitation. Coupled with Raman spectroscopy, an EDB/Raman system is a powerful tool that can be used to investigate both physical and chemical changes associated with the hygroscopic properties of individually levitated particles under controlled environments. In this paper, we report the use of an EDB/Raman system to investigate (1) contact ion pairs formation in supersaturated magnesium sulfate solutions; (2) phase transformation in ammonium nitrate/ammonium sulfate mixed particles; (3) hygroscopicity of organically coated inorganic aerosols; and (4) heterogeneous reactions altering the hygroscopicity of organic aerosols.

  17. Impact of aerosol hygroscopic growth on the direct aerosol radiative effect in summer on North China Plain

    NASA Astrophysics Data System (ADS)

    Kuang, Y.; Zhao, C. S.; Tao, J. C.; Bian, Y. X.; Ma, N.

    2016-12-01

    In this paper, relative humidity (RH) profiles and their impacts on the vertical variations of aerosol optical properties and the direct aerosol radiative effect (DARE) have been investigated based on surface measurements from the Haze in China campaign and sounding data from the North China Plain. Among the profiles obtained from July to September in 2008, about half have RHs greater than 80% within the mixed layer. The vertical variations in the aerosol optical properties at ambient RH, including the extinction coefficient (σext), single scattering albedo (SSA) and asymmetry factor (g), are remarkably different from the variations in the dry aerosols and are highly dependent on the RH profiles. Increases of the aerosol optical depth and column-averaged SSA and g due to aerosol water uptake can reach up to 64%, 0.052 and 0.079, respectively. The fractional contribution to the instantaneous DARE at the top of the atmosphere due to aerosol hygroscopic growth reaches 60% in high RH profiles. DARE estimates can be significantly biased if the RH dependence of SSA or g is not considered. We suggest that if their vertical profiles or column-averaged values are absent, then the ambient values of SSA and g at the surface should be used rather than the values of SSA and g obtained from dry aerosols when estimating DAREs.

  18. A Method for Determining Hygroscopic Growth Factor for Organic Aerosols From Vapor Pressure Experiments

    NASA Astrophysics Data System (ADS)

    Rodriguez, L. I.; Tabazadeh, A.; Golden, D. M.; Jacobson, M. Z.

    2008-12-01

    Currently, the tandem differential mobility analyzer (TDMA) is one of the most commonly used instruments to study the hygroscopic behavior of aerosols. The hygroscopic growth factor (HGF), defined as the ratio of the diameter of a spherical particle when it is exposed to humid conditions to that at dry conditions, is typically used to quantify particle water uptake. We present a new formulation to express the HGF of an aerosol particle as a function of water activity (aW) in the aqueous phase. Our approach is based on the fact that 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 as a function of solution concentration and temperature. For the pertinent solutions, we report coefficients resulting from a least square fitting of the water activity data as a function of molality for temperatures from 0 to 30°C. We compared the results obtained using our measured water activities in the HGF formulation with previous studies published, where TDMA is used to directly measure the HGF, for solutes commonly found in atmospheric aerosols. Our results indicate agreement with TDMA studies for common inorganic salts and water-miscible organic particles that are known to deliquesce into aqueous drops at high relative humidity (RH). However, we find a difference for organic particles that show no deliquescence behavior at low RH. For example, one TDMA study measured a HGF of 1.18 for 100 nm phthalic acid particles at 90% RH (aW= 0.9) and 30°C. Our data showed that even an aqueous solution saturated in phthalic acid did not lower the vapor pressure of pure water at 30°C. We propose that the adsorption of a negligible mass of water by a porous particle can lead to an apparent growth in particle size by changing the particle morphology.

  19. Dynamic growth and deposition of hygroscopic aerosols in the nasal airway of a 5-year-old child.

    PubMed

    Kim, Jong Won; Xi, Jinxiang; Si, Xiuhua A

    2013-01-01

    Hygroscopic growth within the human respiratory tract can be significant, which may notably alter the behavior and fate of the inhaled aerosols. The objective of this study is to evaluate the hygroscopic effects upon the transport and deposition of nasally inhaled fine-regime aerosols in children. A physiologically realistic nasal-laryngeal airway model was developed based on magnetic resonance imaging of a 5-year-old boy. Temperature and relative humidity field were simulated using the low Reynolds number k - ε turbulence model and chemical specie transport model under a spectrum of four thermo-humidity conditions. Particle growth and transport were simulated using a well validated Lagrangian tracking model coupled with a user-defined hygroscopic growth module. The subsequent aerosol depositions for the four inhalation scenarios were evaluated on a multiscale basis such as total, subregional, and cellular-level depositions. Results of this study show that a supersaturated humid environment is possible in the nasal turbinate region and can lead to significant condensation growth (d / d(0)  > 10) of nasally inhaled aerosols. Depositions in the nasal airway can also be greatly enhanced by condensation growth with appropriate inhalation temperature and humidity. For subsaturated and mild inhalation conditions, the hygroscopic effects were found to be nonsignificant for total depositions, while exerting a large impact upon localized depositions.

  20. Dynamics of aerosol size during inhalation: hygroscopic growth of commercial nebulizer formulations.

    PubMed

    Haddrell, Allen E; Davies, James F; Miles, Rachael E H; Reid, Jonathan P; Dailey, Lea Ann; Murnane, Darragh

    2014-03-10

    The size of aerosol particles prior to, and during, inhalation influences the site of deposition within the lung. As such, a detailed understanding of the hygroscopic growth of an aerosol during inhalation is necessary to accurately model the deposited dose. In the first part of this study, it is demonstrated that the aerosol produced by a nebulizer, depending on the airflows rates, may experience a (predictable) wide range of relative humidity prior to inhalation and undergo dramatic changes in both size and solute concentration. A series of sensitive single aerosol analysis techniques are then used to make measurements of the relative humidity dependent thermodynamic equilibrium properties of aerosol generated from four common nebulizer formulations. Measurements are also reported of the kinetics of mass transport during the evaporation or condensation of water from the aerosol. Combined, these measurements allow accurate prediction of the temporal response of the aerosol size prior to and during inhalation. Specifically, we compare aerosol composed of pure saline (150 mM sodium chloride solution in ultrapure water) with two commercially available nebulizer products containing relatively low compound doses: Breath®, consisting of a simple salbutamol sulfate solution (5 mg/2.5 mL; 1.7 mM) in saline, and Flixotide® Nebules, consisting of a more complex stabilized fluticasone propionate suspension (0.25 mg/mL; 0.5 mM in saline. A mimic of the commercial product Tobi© (60 mg/mL tobramycin and 2.25 mg/mL NaCl, pH 5.5-6.5) is also studied, which was prepared in house. In all cases, the presence of the pharmaceutical was shown to have a profound effect on the magnitude, and in some cases the rate, of the mass flux of water to and from the aerosol as compared to saline. These findings provide physical chemical evidence supporting observations from human inhalation studies, and suggest that using the growth dynamics of a pure saline aerosol in a lung inhalation model

  1. 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).

  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

    in the mid-IR range (800 to 7000 cm(-1)) also showed no significant changes in either the real or the imaginary parts of the refractive indices for brown carbon aerosol particles when compared to ammonium sulfate. Therefore, changes in the optical properties of ammonium sulfate in the mid-IR spectral range due to reaction with methylglyoxal appear to be insignificant. In addition to these measurements, we have characterized additional physicochemical properties of the brown carbon aerosol particles including hygroscopic growth using a tandem-differential mobility analyzer. Compared to ammonium sulfate, brown carbon aerosol particles are found to have lower deliquescence relative humidity (DRH), efflorescence relative humidity (ERH), and hygroscopic growth at the same relative humidities. Overall, our study provides new details of the optical and physicochemical properties of a class of secondary organic aerosol which may have important implications for atmospheric chemistry and climate.

  3. Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Hodas, Natasha; Zuend, Andreas; Schilling, Katherine; Berkemeier, Thomas; Shiraiwa, Manabu; Flagan, Richard C.; Seinfeld, John H.

    2016-10-01

    Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. However, uncertainty remains regarding the factors that contribute to observations of low hygroscopic growth below water saturation but enhanced cloud condensation nuclei (CCN) activity for a given aerosol population. Utilizing laboratory surrogates for oligomers in atmospheric aerosols, we explore the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors. Measurements of hygroscopic growth under subsaturated conditions and the CCN activity of aerosols comprised of polyethylene glycol (PEG) with average molecular masses ranging from 200 to 10 000 g mol-1 and mixtures of PEG with ammonium sulfate (AS) were conducted. Experimental results are compared to calculations of hygroscopic growth at thermodynamic equilibrium conducted with the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model, and the potential influence of kinetic limitations on observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Particle-phase behavior, including the prevalence of liquid-liquid phase separation (LLPS), was also modeled with AIOMFAC. Under subsaturated relative humidity (RH) conditions, we observed little variability in hygroscopic growth across PEG systems with different molecular masses; however, an increase in CCN activity with increasing PEG molecular mass was observed. This effect is most pronounced for PEG-AS mixtures, and, in fact, an enhancement in CCN activity was observed for the PEG10000-AS mixture as compared to pure AS, as evidenced by a 15 % reduction in critical activation diameter at a supersaturation of 0.8 %. We also

  4. 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.

  5. 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.

  6. Cloud Condensation Nuclei Activity, Droplet Growth Kinetics and Hygroscopicity of Biogenic and Anthropogenic Secondary Organic Aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, Defeng; Buchholz, Angela; Kortner, Birthe; Schlag, Patrick; Rubach, Florian; Hendrik, Fucks; Kiendler-Scharr, Astrid; Tillmann, Ralf; Wahner, Andreas; Hallquist, Mattias; Flores, Michel; Rudich, Yinon; Glasius, Marianne; Kourtchev, Ivan; Kalberer, Markus; Mentel, Thomas

    2015-04-01

    Recent field data and model analysis show that secondary organic aerosol (SOA) formation is enhanced under anthropogenic influences (de Gouw et al. 2005, Spracklen et al. 2011). The interaction of biogenic VOCs (BVOCs) with anthropogenic emissions such as anthropogenic VOCs (AVOCs) could change the particle formation yields and the aerosol properties, as was recently demonstrated (Emanuelsson et al., 2013; Flores et al., 2014). However, the effect of the interaction of BVOCs with AVOCs on cloud condensation nuclei (CCN) activity and hygroscopicity of SOA remains elusive. Characterizing such changes is necessary in order to assess the indirect radiative forcing of biogenic aerosols that form under anthropogenic influence. In this study, we investigated the influence of AVOCs on CCN activation and hygroscopic growth of BSOA. SOA was formed from photooxidation of monoterpenes and aromatics as representatives of BVOCs and AVOCs, respectively. The hygroscopicity and CCN activation of BSOA were studied and compared with that of anthropogenic SOA (ASOA) and the mixture of ASOA and BSOA (ABSOA). We found that ASOA had a significantly higher hygroscopicity than BSOA at similar OH dose, which is attributed to a higher oxidation level of ASOA. While the ASOA fraction had an enhancing effect on the hygroscopicity of ABSOA compared to BSOA, the hygroscopicity of ABSOA cannot be explained by a linear combination of the pure ASOA and BSOA systems, indicating potentially additional non-linear effects such as oligomerization. However, in contrast to hygroscopicity, ASOA showed similar CCN activity as BSOA, in spite of its higher oxidation level. The ASOA fraction did not enhance the CCN activity of ABSOA. The discrepancy between hygroscopicity and CCN activity is discussed. In addition, BSOA, ABSOA and ASOA formed similar droplet size with ammonium sulfate in CCN at a given supersaturation, indicating none of these aerosols had a delay in the water uptake in the supersaturated

  7. 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

  8. Phase state is a limiting factor in hygroscopic growth of secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Virtanen, Annele

    2014-05-01

    Secondary organic aerosol (SOA) particles formed from oxidation products of volatile organic compounds (VOC) form a significant fraction of the total atmospheric particulate matter affecting climate both directly and indirectly. The dependence of hygroscopicity on particle composition is often represented with the single parameter κ, commonly used in global models to describe the hygroscopic properties of atmospheric aerosol particles. The physical phase state of SOA particles affects the partitioning of organic vapors and also may affect the uptake of water vapor and particle activation into cloud droplets. Thus, hygroscopic behaviour of SOA particles is affected by composition (i.e. oxidation state and molecular size) but also by phase of particles. In this study the following three distinct studies were performed: (1) particle bounced fraction (BF) measurements, which are qualitatively related to particle phase, as a function of relative humidity using an Aerosol Bounce Instrument (ABI). We assume that the particles with BF > 0 are solid or semisolid, and that particles with BF = 0 behave mechanically as liquids (2) water uptake measured in the sub-saturated region using hygroscopicity tandem differential mobility analyzer (HTDMA) by measuring the ratio of wet to dry particle diameter following exposure to water vapor at a controlled RH (3) cloud droplet formation in the supersaturated region using a cloud condensation nuclei counter (CCNc). Particle composition and oxidation state was measured with a compact time of flight aerosol mass spectrometer (c-ToF-AMS). In this study we show that at sub-saturation conditions water uptake by SOA particles is restricted due to the kinetic limitations. Diffusion and solubility limitations inhibit water uptake until the humidity is high enough for dissolution to occur. Our studies show that this 'threshold' humidity is dependent on particle composition, oxidation state, and average molecular size. Our laboratory results

  9. Hygroscopic growth of water soluble organic carbon isolated from atmospheric aerosol collected at US national parks and Storm Peak Laboratory

    NASA Astrophysics Data System (ADS)

    Taylor, Nathan F.; Collins, Don R.; Lowenthal, Douglas H.; McCubbin, Ian B.; Gannet Hallar, A.; Samburova, Vera; Zielinska, Barbara; Kumar, Naresh; Mazzoleni, Lynn R.

    2017-02-01

    Due to the atmospheric abundance and chemical complexity of water soluble organic carbon (WSOC), its contribution to the hydration behavior of atmospheric aerosol is both significant and difficult to assess. For the present study, the hygroscopicity and CCN activity of isolated atmospheric WSOC particulate matter was measured without the compounding effects of common, soluble inorganic aerosol constituents. WSOC was extracted with high purity water from daily high-volume PM2.5 filter samples and separated from water soluble inorganic constituents using solid-phase extraction. The WSOC filter extracts were concentrated and combined to provide sufficient mass for continuous generation of the WSOC-only aerosol over the combined measurement time of the tandem differential mobility analyzer and coupled scanning mobility particle sizer-CCN counter used for the analysis. Aerosol samples were taken at Great Smoky Mountains National Park during the summer of 2006 and fall-winter of 2007-2008; Mount Rainier National Park during the summer of 2009; Storm Peak Laboratory (SPL) near Steamboat Springs, Colorado, during the summer of 2010; and Acadia National Park during the summer of 2011. Across all sampling locations and seasons, the hygroscopic growth of WSOC samples at 90 % RH, expressed in terms of the hygroscopicity parameter, κ, ranged from 0.05 to 0.15. Comparisons between the hygroscopicity of WSOC and that of samples containing all soluble materials extracted from the filters implied a significant modification of the hydration behavior of inorganic components, including decreased hysteresis separating efflorescence and deliquescence and enhanced water uptake between 30 and 70 % RH.

  10. 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.

  11. 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.

  12. Hygroscopic growth of atmospheric aerosol particles based on lidar, radiosonde, and in situ measurements: Case studies from the Xinzhou field campaign

    NASA Astrophysics Data System (ADS)

    Lv, Min; Liu, Dong; Li, Zhanqing; Mao, Jietai; Sun, Yele; Wang, Zhenzhu; Wang, Yingjian; Xie, Chenbo

    2017-02-01

    Lidar, radiosonde, and ground-based in situ nephelometer measurements made during an intensive field campaign carried out from July to September 2014 at the Xinzhou meteorological station were used to determine the aerosol hygroscopic growth effect in a cloud-capped, well-mixed boundary layer. Aerosol hygroscopic properties at 355 and 532 nm were examined for two cases with distinct aerosol layers. Lidar-derived maximum enhancement factors in terms of aerosol backscatter coefficient derived using a relative humidity (RH) reference value of 85% were 1.19 at 532 nm and 1.10 at 355 nm for Case I and 2.32 at 532 nm and 1.94 at 355 nm for Case II. To derive the aerosol particle hygroscopic growth factor at specific RH values, the Kasten and Hänel models were used. A comparison of the goodness of fit for the two models showed that the Kasten model performed better. The hygroscopic growth curve for RH>90% was much steeper than that for RH in the range of 85-90%. The slopes of the lidar-derived enhancement factor curve (measured from 85% to 95% RH) and the nephelometer-derived enhancement factor curve (measured from 40% to 62% RH) in Case I show similar trends, which lends confidence to using lidar measurements for studying aerosol particle hygroscopic growth. Data from a ground aerosol chemical speciation monitor showed that the larger values of aerosol hygroscopic enhancement factor in Case II corresponded to greater mass concentrations of sulfate and nitrate in the atmosphere.

  13. 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.

  14. 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.

  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

    decomposition products NH3 and HNO3. The efflorescence threshold of NaCl-BSA particles decreased with increasing BSA dry mass fraction, i.e. the protein inhibited the formation of salt crystals and enhanced the stability of supersaturated solution droplets. The H-TDMA and TEM results indicate that the protein was enriched at the surface of the mixed particles and formed an envelope, which inhibits the access of water vapor to the particle core and leads to kinetic limitations of hygroscopic growth, phase transitions, and microstructural rearrangement processes. Besides these surface and kinetic effects, proteins and comparable organic macromolecules may also influence the thermodynamic properties of the aqueous bulk solution (solubilities, vapor pressures, and chemical equilibria, e.g. for the decomposition and evaporation of NH4NO3. The observed effects should be taken into account in the analysis of data from laboratory experiments and field measurements and in the modelling of aerosol processes involving water vapor and particles with complex composition. They can strongly influence experimental results, and depending on ambient conditions they may also play a significant role in the atmosphere (deliquescence, efflorescence, and CCN activation of particles). In fact, irregular hygroscopic growth curves similar to the ones observed in this study have recently been reported from H-TDMA experiments with water-soluble organics extracted from real air particulate matter and with humic-like substances. The Köhler theory calculations performed with different models demonstrate that the hygroscopic growth of particles composed of inorganic salts and proteins can be efficiently described with a simple volume additivity approach, provided that the correct dry solute mass equivalent diameter and composition are known. A simple parameterisation of the osmotic coefficient has been derived from an osmotic pressure virial equation and appears to be well-suited for proteins and comparable

  16. 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.

  17. Aerosol Number-size Distributions and Hygroscopic Growth in the Marine Boundary Layer during ACE-Asia

    NASA Astrophysics Data System (ADS)

    Covert, D. S.; Coffman, D. J.; Bates, T. S.

    2001-12-01

    As part of the Aerosol Chemistry Experiment-Asia (ACE-Asia), measurements of the physical and hygroscopic properties of aerosol particles were made on the NOAA Research Vessel Ron Brown in the experiment's study area around southern Japan, the Sea of Japan and the Yellow Sea from 30 March through 19 April, 2001 (Day of Year 90 through 109). The number-size distribution from 3 nm to 10 um diameter was measured with a combination of differential mobility analyzers and aerodynamic particle sizers. The system was operated at 55% relative humidity (RH) for consistency with optical measurements and size dependent chemical sampling on the ship. A separate system consisting of three differential mobility analyzers and humidity conditioners measured the change in hydration of the accumulation mode particles from an initial condition of 55% RH to humidities of 20% and 90% RH. The result is a distribution of hygroscopic growth factors at the end RH relative to the initial humidity. The size distributions varied widely depending on the location of the ship, the source of the air mass and the local meteorological conditions. The dominant features included ultrafine particles (less than 20 nm), soil dust particulate mass (greater than 2 um) and Aitken, accumulation mode number and mass (40 to 600 nm). The results are limited to case studies rather than any statistical or time-space average due to the limited data base and the few sources and air mass types encountered in the 21 day period. The results have been analyzed and categorized according to specific air mass trajectories and chemical analysis and are considered representative of those air masses at the marine boundary layer level. Soil dust dominated distributions were observed on days 101 through 103 with volume concentrations of 50 to 100 um3/cm3 and a volume mean diameter of 3 um. High concentrations of ultrafine particles were observed on the later two of these days from early morning through mid-afternoon in spite

  18. 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

  19. The Effect of Temperature on Hygroscopic Growth of Organic Aerosols Over The 273-303K Range as Derived From Bulk Solution Experiments

    NASA Astrophysics Data System (ADS)

    Rodriguez, L. I.; Tabazadeh, A.; Golden, D. M.; Jacobson, M. Z.

    2009-12-01

    Studies have shown that organic matter often constitutes up to 50% by mass of tropospheric aerosols. It is also known that these organics may considerably alter the water uptake properties of aerosol particles. Water uptake of a particle is typically quantified by the hygroscopic growth factor, defined as the ratio of the diameter of a spherical particle when it is exposed to humid conditions to that under dry conditions. In this study, we have assembled an apparatus to measure water activity over aqueous solutions as a function of temperature and solute concentration. We report the experimental precision of our vapor pressure apparatus, obtained by replicating several experiments. Using this apparatus, we studied aqueous solutions of organic compounds representing the categories found in atmospheric aerosols such as simple sugars, diacids, humic materials, and some of their mixtures with inorganic salts. From these measurements, we directly computed the hygroscopic growth factor (HGF) using a formulation that expresses HGF as a function of water activity. Our approach is based on the fact that water activity limits the growth of a particle that can be attributed to water uptake. While most studies report the hygroscopic growth factor of atmospheric aerosols at room temperature (20 - 30°C), we explored the temperature effect on hygroscopic growth of organic aerosols within the 0 - 30°C temperature range. Within experimental error, we found no temperature dependence of the HGF in the 0 - 30°C range, for solutes d-glucose, levoglucosan, succinic acid, phthalic acid, humic acid and Suwanne River fulvic acid. For example, the water activity of an aqueous solution of d-glucose corresponding to a HGF of 1.72 varied by only 1% from 0 to 30°C, well below the experimental error. We report hygroscopic growth curves as a function of temperature and relative humidity for these six organic solutes and some of their mixtures with inorganic salts. Finally, we compare our HGF

  20. 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.

    2004-02-01

    The interaction of aerosol particles composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations (100-300nm particle size range, 298K, 960hPa). 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 sim35% relative humidity (RH) and a hygroscopic diameter increase by up to sim10% 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 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

  1. 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

  2. Hygroscopicity of Early Earth and Titan Laboratory Aerosol Analogs

    NASA Astrophysics Data System (ADS)

    Hasenkopf, C. A.; Beaver, M. R.; Freedman, M. A.; Toon, O. B.; Tolbert, M. A.

    2009-12-01

    We have explored the ability of organic hazes, known to exist in the atmosphere of Titan and postulated to have existed in the Archean Earth atmosphere, to act as cloud condensation nuclei (CCN). These laboratory aerosol analogs are generated via UV-photolysis of early Earth and Titan analog gas mixtures and are designed to mimic the present day atmospheric conditions on Titan and the early Earth atmosphere before the rise of oxygen. Water uptake is observed to occur on the early Earth and Titan aerosol analogs at relative humidities of 80% - 90% via optical growth measurements using cavity ring-down aerosol extinction spectroscopy. We find the optical growth of these aerosols is similar to known slightly-soluble organic acids, such as phthalic and pyromellitic acids. On average, the optical growth of the early Earth analog is slightly larger than the Titan analog. In order to translate our measurements obtained in a subsaturated regime into the CCN ability of these particles, we rely on the hygroscopicity parameter κ, developed by Petters & Kreidenweis (2007). We retrieve κ = 0.17±0.03 and 0.06±0.01 for the early Earth and Titan analogs, respectively. This early Earth analog hygroscopicity value indicates that the aerosol could activate at reasonable water vapor supersaturations. We use previous aerosol mass spectrometry results to correlate the chemical structure of the two types of analog with their hygroscopicity. The hygroscopicity of the early Earth aerosol analog, coupled with the apparent lack of other good CCN during the Archean, helps explain the role of the organic haze in the indirect effect of clouds on the early Earth and indicates that it may have had a significant impact on the hydrological cycle.

  3. Hygroscopic and chemical characterisation of Po Valley aerosol

    NASA Astrophysics Data System (ADS)

    Bialek, J.; Dall Osto, M.; Vaattovaara, P.; Decesari, S.; Ovadnevaite, J.; Laaksonen, A.; O'Dowd, C.

    2014-02-01

    Continental summer-time aerosol in the Italian Po Valley was characterised in terms of hygroscopic properties and the influence of chemical composition therein. Additionally, the ethanol affinity of particles was analysed. The campaign-average minima in hygroscopic growth factors (HGFs, at 90% relative humidity) occurred just before and during sunrise from 03:00 to 06:00 LT (all data are reported in the local time), but, more generally, the hygroscopicity during the whole night is very low, particularly in the smaller particle sizes. The average HGFs recorded during the low HGF period were in a range from 1.18 (for the smallest, 35nm particles) to 1.38 (for the largest, 165 nm particles). During the day, the HGF gradually increased to achieve maximum values in the early afternoon hours 12:00-15:00, reaching 1.32 for 35 nm particles and 1.46 for 165 nm particles. Two contrasting case scenarios were encountered during the measurement period: Case 1 was associated with westerly air flow moving at a moderate pace and Case 2 was associated with more stagnant, slower moving air from the north-easterly sector. Case 1 exhibited weak diurnal temporal patterns, with no distinct maximum or minimum in HGF or chemical composition, and was associated with moderate non-refractory aerosol mass concentrations (for 50% size cut at 1 μ) of the order of 4.5 μg m-3. For Case 1, organics contributed typically 50% of the mass. Case 2 was characterised by >9.5 μg m-3 total non-refractory mass (<1 μ) in the early morning hours (04:00), decreasing to ~3 μg m-3 by late morning (10:00) and exhibited strong diurnal changes in chemical composition, particularly in nitrate mass but also in total organic mass concentrations. Specifically, the concentrations of nitrate peaked at night-time, along with the concentrations of hydrocarbon-like organic aerosol (HOA) and of semi-volatile oxygenated organic aerosol (SV-OOA). In general, organic growth factors (OGFs) followed a trend which was

  4. 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.

  5. Hygroscopic and chemical characterisation of Po Valley aerosol

    NASA Astrophysics Data System (ADS)

    Bialek, J.; Dall'Osto, M.; Vaattovaara, P.; Ovadnevaite, J.; Decesari, S.; Laaksonen, A.; O'Dowd, C.

    2013-02-01

    Continental summer-time aerosol in the Italian Po Valley was characterized in terms of hygroscopic properties and the influence of chemical composition therein. The campaign-average minima in hygroscopic growth factors (HGFs) occurred just before and during sunrise from 03:00-06:00, but more generally, the whole night shows very low hygroscopicity, particularly in the smaller particle sizes. The average HGFs increased from 1.18 for the smallest sized particles (35 nm) to 1.38 for the largest sizes (165 nm) for the lowest HGF period while during the day, the HGF gradually increased to achieve maximum values in the early afternoon hours from 12:00-15:00, reaching 1.32 for 35 nm particles and 1.46 for 165 nm particles. Two contrasting case scenarios were encountered during the measurement period: Case 1 was associated with westerly air flow moving at a moderate pace and Case 2 was associated with more stagnant, slower moving air from the north-easterly sector. Case 1 exhibited low diurnal temporal patterns and was associated with moderate non-refractory aerosol mass concentrations (for 50% size cut at 1 μm) of the order of 4.5 μg m-3. For Case 1, organics contributed typically to 50% of the mass. Case 2 was characterized by > 9.5 μg m-3 total mass (< 1 μm) in the early morning hours (04:00), decreasing to ∼ 3 μg m-3 by late morning (10:00) and exhibited strong diurnal changes in chemical composition, particularly in nitrate mass but also in total organic mass concentrations. Organic growth factors (OGFs) exhibited a minimum around 15:00, 1-2 h after the peak in HGF. Particles sized 165 nm exhibited moderate diurnal variability in HGF, ranging from 80% at night to 95% of "more hygroscopic" growth factors (i.e. GF = 1.35-1.9) around noon. The diurnal changes in HGF progressively became enhanced with decreasing particle size, decreasing from 95% "more hygroscopic" growth factor fraction at noon to 10% fraction at midnight, while the "less hygroscopic" growth

  6. Studies of single aerosol particles containing malonic acid, glutaric acid, and their mixtures with sodium chloride. I. Hygroscopic growth.

    PubMed

    Pope, Francis D; Dennis-Smither, Ben J; Griffiths, Paul T; Clegg, Simon L; Cox, R Anthony

    2010-04-29

    We describe a newly constructed electrodynamic balance with which to measure the relative mass of single aerosol particles at varying relative humidity. Measurements of changing mass with respect to the relative humidity allow mass (m) growth factors (m(aqueous)/m(dry)) and diameter (d) growth factors (d(aqueous)/d(dry)) of the aerosol to be determined. Four aerosol types were investigated: malonic acid, glutaric acid, mixtures of malonic acid and sodium chloride, and mixtures of glutaric acid and sodium chloride. The mass growth factors of the malonic acid and glutaric acid aqueous phase aerosols, at 85% relative humidity, were 2.11 +/- 0.08 and 1.73 +/- 0.19, respectively. The mass growth factors of the mixed organic/inorganic aerosols are dependent upon the molar fraction of the individual components. Results are compared with previous laboratory determinations and theoretical predictions.

  7. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    DOE PAGES

    Atkinson, D. B.; Radney, J. G.; Lum, J.; ...

    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

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

    PubMed

    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.

  9. How Important Is Organic Aerosol Hygroscopicity to Aerosol Indirect Forcing?

    SciTech Connect

    Liu, Xiaohong; Wang, Jian

    2010-12-07

    Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation and yield of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR Community Atmospheric Model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (“κ” value) of POA and SOA. Our model simulation indicates that in the present-day condition changing “κ” value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S=0.1% by 40-60% over the POA source regions, while changing “κ” value of SOA by ±50% (from 0.14 to 0.07 and 0.21) changes the CCN within 30%. Changes in the in-cloud droplet number concentrations (CDNC) are within 20% in most locations on the globe with the above changes in “κ” value of POA and SOA. Global annual mean anthropogenic aerosol indirect forcing (AIF) between present-day (PD) and pre-industrial (PI) conditions change by 0.4 W m-2 with the control run of -1.3 W m-2. AIF reduces with the increase hygroscopicity of organic aerosol, indicating the important role of natural organic aerosol in buffering the relative change of CDNC from PI to PD.

  10. 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.

  11. 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

  12. Hygroscopic growth and CCN activity of HULIS from different environments

    NASA Astrophysics Data System (ADS)

    Kristensen, Thomas B.; Wex, Heike; Nekat, Bettina; Nøjgaard, Jacob K.; van Pinxteren, Dominik; Lowenthal, Douglas H.; Mazzoleni, Lynn R.; Dieckmann, Katrin; Bender Koch, Christian; Mentel, Thomas F.; Herrmann, Hartmut; Gannet Hallar, A.; Stratmann, Frank; Bilde, Merete

    2012-11-01

    Humic-like substances (HULIS) constitute a significant fraction of aerosol particles in different environments. Studies of the role of HULIS in hygroscopic growth and cloud condensation nuclei (CCN) activity of aerosol particles are scarce, and results differ significantly. In this work the hygroscopic growth and CCN activity of water extracts (WE) and HULIS extracted from particulate matter (PM) collected at a polluted urban site (Copenhagen, Denmark), a rural site (Melpitz, Germany) and the remote site Storm Peak Laboratory (Colorado, USA) were investigated. Measurements of inorganic ions, elemental carbon, organic carbon and water soluble organic carbon (WSOC) within the PM confirmed that the sources of aerosol particles most likely differed for the three samples. The hygroscopic properties of the filtered WE were characterized by hygroscopicity parameters for subsaturated conditions (κGF) of 0.25, 0.41 and 0.22, and for supersaturated conditions κCCN were 0.23, 0.29 and 0.22 respectively for the urban, rural and remote WE samples. The measured hygroscopic growth and CCN activity were almost identical for the three HULIS samples and could be well represented by κGF = 0.07 and κCCN = 0.08-0.10 respectively. Small amounts of inorganic ions were present in the HULIS samples so the actual values for pure HULIS are expected to be slightly lower (κGF* = 0.04-0.06 and κCCN* = 0.07-0.08). The HULIS samples are thus less hygroscopic compared to most previous studies. To aid direct comparison of hygroscopic properties of HULIS from different studies, we recommend that the fraction of inorganic species in the HULIS samples always is measured and reported.

  13. An alternative method estimating hygroscopic growth factor of aerosol light scattering coefficient: a case study in an urban area of Guangzhou, South China

    NASA Astrophysics Data System (ADS)

    Lin, Z. J.; Zhang, Z. S.; Zhang, L.; Tao, J.; Zhang, R. J.; Cao, J. J.; Zhang, Y. H.

    2014-01-01

    A method was developed to estimate hygroscopic growth factor (f(RH)) of aerosol light scattering coefficient (bsp), making use of the measured size- and chemically-resolved aerosol samples. Regarding this method, chemical composition of the measured aerosol samples were first reconstructed using the equilibrium model ISOPPORIA II. The model reconstructed chemical composition varies with a varying relative humidity (RH) input, which was then employed to calculate bsp and f(RH) of bsp using Mie Model. Further, the RH dependence of f(RH) of bsp (denoted as f(RH) derived from model calculation was empirically fitted with a two-parameter formula. One of the two parameters was set to be a constant for practical applications. For validation, the developed formula of fsp(RH) was applied to correct the long-term records of measured bsp from the values under comparative dry conditions to the ones under ambient RH conditions. Compared with the original bsp data, the f(RH)-corrected bsp had a higher linear correlation with and a smaller discrepancy from the bsp data derived directly from visibility and absorption measurements. The method described in this paper provides an alternative approach to estimate fsp(RH) and has many potential applications.

  14. 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.

  15. An observational study of the hygroscopic properties of aerosols over the Pearl River Delta region

    NASA Astrophysics Data System (ADS)

    Tan, Haobo; Yin, Yan; Gu, Xuesong; Li, Fei; Chan, P. W.; Xu, Hanbing; Deng, Xuejiao; Wan, Qilin

    2013-10-01

    Hygroscopic growth can significantly affect size distribution and activation of aerosol particles, as well as their effects on human health, atmospheric visibility, and climate. In this study, an H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) was utilized to measure hygroscopic growth factor and mixing state of aerosol particles at the CAWNET station in Panyu, Guangzhou, China. A statistical analysis of the results show that, at relative humidity (RH) of 90%, for less-hygroscopic particles of 40-200 nm in diameter, the growth factor (gLH) was around 1.13, while the number fraction (NFLH) varied between 0.41 ± 0.136 and 0.26 ± 0.078; for more-hygroscopic particles, the growth factor (gMH) varied between 1.46 and 1.55 with the average equivalent ammonium sulfate ratio (ɛAS) ranging from 0.63 to 0.68. The differences in ɛAS among particle of different sizes reveal that more-hygroscopic inorganic salts, such as ammonium sulfate and ammonium nitrate, are of more effective condensation growth for Aitken mode particles. A combined analysis of the probability density function of growth factor (Gf-PDF) and simultaneous meteorological data shows that during clean periods with air masses moving from the north, the particles are more likely to have homogeneous chemical composition, while during polluted or pollution accumulation periods, variations in mean number weighted growth factor (gmean) and NFMH become more pronounced, indicating that locally-emitted aerosol particles tend to be in an externally mixed state and contain a certain proportion of less-hygroscopic particles. This study can help improve our understanding of aerosol hygroscopicity and its impact on the atmospheric visibility and environment.

  16. Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

    NASA Astrophysics Data System (ADS)

    Massoli, P.; Lambe, A.; Ahern, A.; Williams, L. R.; Ehn, M.; Mikkila, J.; Canagaratna, M.; Brune, W. H.; Onasch, T. B.; Jayne, J.; Petdjd, T. T.; Kulmala, M. T.; Laaksonen, A.; Kolb, C. E.; Davidovits, P.; Worsnop, D. R.

    2010-12-01

    Laboratory experiments investigated the relationship between degree of oxidation and hygroscopic properties of secondary organic aerosol (SOA) particles. The hygroscopic growth factor (HGF), the CCN activity (κCCN) and the degree of aerosol oxidation (represented by the atomic O:C ratio) were measured for α-pinene, 1,3,5-trimethylbenzene (TMB), m-xylene and α pinene/m-xylene mixture SOA generated via OH radical oxidation in an aerosol flow reactor. Our results show that both HGF and κCCN increase with O:C. The TMB and m-xylene SOA were, respectively, the least and most hygroscopic of the system studied. An average HGF of 1.25 and a κCCN of 0.2 were measured at O:C of 0.65, in agreement with results reported for ambient data. The HGF based κ(κHGF) under predicted the κCCN values of 20 to 50% for all but the TMB SOA. Within the limitations of instrumental capabilities, we define the extent to which the hygroscopic properties of SOA particles can be predicted from their oxidation level and provide parameterizations suitable for interpreting ambient data.

  17. 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

  18. Hygroscopic growth of atmospheric and model humic-like substances

    NASA Astrophysics Data System (ADS)

    Dinar, E.; Taraniuk, I.; Graber, E. R.; Anttila, T.; Mentel, T. F.; Rudich, Y.

    2007-03-01

    The hygroscopic growth (HG) of humic-like substances (HULIS) extracted from smoke and pollution aerosol particles and of Suwannee River fulvic acid (SRFA, bulk and fractions of different molecular weight) was measured by humidity tandem differential mobility analyzer (H-TDMA). By characterizing physical and chemical parameters such as molecular weight, elemental composition, and surface tension, we test the effect of these parameters on particle interactions with water vapor. For molecular weight-fractionated SRFA fractions, the growth factor at 90% relative humidity was generally inversely proportional to the molecular weight. HULIS extracts from ambient particles are more hygroscopic than all the SRFA fractions and exhibit different hygroscopic properties depending on their origin and residence time in the atmosphere. The results point out some dissimilarities between SRFA and aerosol-derived HULIS. The cloud condensation nuclei (CCN) behavior of the studied materials was predicted on the basis of hygroscopic growth using a recently introduced approach of Kreidenweis et al. (2005) and compared to CCN activity measurements on the same samples (Dinar et al., 2006). It is found that the computational approach (Kreidenweis et al., 2005) works reasonably well for SRFA fractions but is limited in use for the HULIS extracts from aerosol particles. The difficulties arise from uncertainties associated with HG measurements at high relative humidity, which leads to large errors in the predicted CCN activity.

  19. 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.

  20. In-cloud measurements highlight the role of aerosol hygroscopicity in cloud droplet formation

    NASA Astrophysics Data System (ADS)

    Väisänen, Olli; Ruuskanen, Antti; Ylisirniö, Arttu; Miettinen, Pasi; Portin, Harri; Hao, Liqing; Leskinen, Ari; Komppula, Mika; Romakkaniemi, Sami; Lehtinen, Kari E. J.; Virtanen, Annele

    2016-08-01

    The relationship between aerosol hygroscopicity and cloud droplet activation was studied at the Puijo measurement station in Kuopio, Finland, during the autumn 2014. The hygroscopic growth of 80, 120 and 150 nm particles was measured at 90 % relative humidity with a hygroscopic tandem differential mobility analyzer. Typically, the growth factor (GF) distributions appeared bimodal with clearly distinguishable peaks around 1.0-1.1 and 1.4-1.6. However, the relative contribution of the two modes appeared highly variable reflecting the probable presence of fresh anthropogenic particle emissions. The hygroscopicity-dependent activation properties were estimated in a case study comprising four separate cloud events with varying characteristics. At 120 and 150 nm, the activation efficiencies within the low- and high-GF modes varied between 0-34 and 57-83 %, respectively, indicating that the less hygroscopic particles remained mostly non-activated, whereas the more hygroscopic mode was predominantly scavenged into cloud droplets. By modifying the measured GF distributions, it was estimated how the cloud droplet concentrations would change if all the particles belonged to the more hygroscopic group. According to κ-Köhler simulations, the cloud droplet concentrations increased up to 70 % when the possible feedback effects on effective peak supersaturation (between 0.16 and 0.29 %) were assumed negligible. This is an indirect but clear illustration of the sensitivity of cloud formation to aerosol chemical composition.

  1. Relationship between aerosol oxidation level and hygroscopic properties of laboratory generated secondary organic aerosol (SOA) particles

    NASA Astrophysics Data System (ADS)

    Massoli, P.; Lambe, A. T.; Ahern, A. T.; Williams, L. R.; Ehn, M.; Mikkilä, J.; Canagaratna, M. R.; Brune, W. H.; Onasch, T. B.; Jayne, J. T.; Petäjä, T.; Kulmala, M.; Laaksonen, A.; Kolb, C. E.; Davidovits, P.; Worsnop, D. R.

    2010-12-01

    Laboratory experiments investigated the relationship between oxidation level and hygroscopic properties of secondary organic aerosol (SOA) particles generated via OH radical oxidation in an aerosol flow reactor. The hygroscopic growth factor at 90% RH (HGF90%), the CCN activity ($\\kappa$ORG,CCN) and the level of oxidation (atomic O:C ratio) of the SOA particles were measured. Both HGF90% and $\\kappa$ORG,CCN increased with O:C; the HGF90% varied linearly with O:C, while $\\kappa$ORG,CCN mostly followed a nonlinear trend. An average HGF90% of 1.25 and $\\kappa$ORG,CCN of 0.19 were measured for O:C of 0.65, in agreement with results reported for ambient data. The $\\kappa$ORG values estimated from the HGF90% ($\\kappa$ORG,HGF) were 20 to 50% lower than paired $\\kappa$ORG,CCN values for all SOA particles except 1,3,5-trimethylbenzene (TMB), the least hygroscopic of the SOA systems. Within the limitations of instrumental capabilities, we show that differences in hygroscopic behavior among the investigated SOA systems may correspond to differences in elemental composition.

  2. Hygroscopic aerosol deposition in the human upper respiratory tract under various thermo-humidity conditions.

    PubMed

    Xi, Jinxiang; Kim, Jongwon; Si, Xiuhua A; Zhou, Yue

    2013-01-01

    The deposition of hygroscopic aerosols is highly complex in nature, which results from a cumulative effect of dynamic particle growth and the real-time size-specific deposition mechanisms. The objective of this study is to evaluate hygroscopic effects on the particle growth, transport, and deposition of nasally inhaled aerosols across a range of 0.2-2.5 μm in an adult image-based nose-throat model. Temperature and relative humidity fields were simulated using the LRN k-ω turbulence model and species transport model under a spectrum of thermo-humidity conditions. Particle growth and transport were simulated using a well validated Lagrangian tracking model coupled with a user-defined hygroscopic growth module. Results of this study indicate that the saturation level and initial particle size are the two major factors that determine the particle growth rate (d/d0), while the effect of inhalation flow rate is found to be not significant. An empirical correlation of condensation growth of nasally inhaled hygroscopic aerosols in adults has been developed based on a variety of thermo-humidity inhalation conditions. Significant elevated nasal depositions of hygroscopic aerosols could be induced by condensation growth for both sub-micrometer and small micrometer particulates. In particular, the deposition of initially 2.5 μm hygroscopic aerosols was observed to be 5-8 times that of inert particles under warm to hot saturated conditions. Results of this study have important implications in exposure assessment in hot humid environments, where much higher risks may be expected compared to normal conditions.

  3. Hygroscopic properties of different aerosol types over the Atlantic and Indian Oceans

    NASA Astrophysics Data System (ADS)

    Maßling, A.; Wiedensohler, A.; Busch, B.; Neusüß, C.; Quinn, P.; Bates, T.; Covert, D.

    2003-09-01

    Hygroscopic properties of atmospheric particles were studied in the marine tropospheric boundary layer over the Atlantic and Indian Oceans during two consecutive field studies: the Aerosols99 cruise (Atlantic Ocean) from 15 January to 20 February 1999, and the INDOEX cruise (Indian Ocean Experiment) from 23 February to 30 March 1999. The hygroscopic properties were compared to optical and chemical properties, such as absorption, chemical inorganic composition, and mass concentration of organic and elemental carbon, to identify the influence of these parameters on hygroscopicity. During the two field studies, four types of aerosol-sampling instruments were used on board the NOAA (National Oceanic and Atmospheric Administration) Research Vessel Ronald H. Brown: Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA), seven-stage cascade impactor, two-stage cascade impactor, and Particle Soot Absorption Photometer (PSAP). The HTDMA was used to determine the hygroscopic properties of atmospheric particles at initial dry sizes (Dp) of 50, 150, and 250 nm and at relative humidities (RH) of 30, 55, 75, and 90%. Simultaneously, a seven-stage cascade impactor of which 3 stages were in the sub-mm size range was used to determine the molar composition of the major inorganic ions such as ammonium and sulfate ions. A two-stage cascade impactor (1 in the sub-mm size range, 1 in the sup-mm size range) was used to determine the mass concentration of organic and elemental carbon. The PSAP was used (at a wavelength of 565 nm) to measure the light absorption coefficient of the aerosol. During the two field studies, air masses of several different origins passed the ship's cruise path. The occurrence of different air masses was classified into special time periods signifying the origin of the observed aerosol. All time periods showed a group of particles with high hygroscopic growth. The measured average hygroscopic growth factors defined by the ratio of dry and wet particle

  4. 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.

  5. Optical and Hygroscopic Studies of Aerosols In Simulated Planetary Atmospheres

    NASA Astrophysics Data System (ADS)

    Hasenkopf, Christa A.

    2011-08-01

    in the UV-Vis than Khare et al. (1984) values. These results may imply that (a) photolysis is not the dominant source of aerosol on Titan, and/or (b) the optical retrievals are dominated by the more absorbing and scattering electric discharge generated aerosol. For the hygroscopicity studies, the optical growth of the early Earth analog at various relative humidities (RH) was measured, as well as a Titan analog for comparison. The retrieved hygroscopic parameter for the early Earth analog indicates that a humidified early Earth aerosol could have contributed to a larger antigreenhouse effect on the early Earth atmosphere than previously modeled with dry aerosol. Such effects would be important in regions where RH is greater than 50% because such high humidities are needed for significant amounts of water to be on the aerosol. The retrieved hygroscopicity parameter also indicates that the particles could activate into cloud droplets at reasonable supersaturations. In regions where the haze was dominant, it is expected that low particle concentrations, once activated into cloud droplets, would create short-lived, optically thin clouds. Such clouds, if predominant on the early Earth, would have a lower albedo than clouds today, thereby warming the planet relative to current day clouds.

  6. Hygroscopic growth of particles nebulized from water-soluble extracts of PM2.5 aerosols over the Bay of Bengal: Influence of heterogeneity in air masses and formation pathways.

    PubMed

    Boreddy, S K R; Kawamura, Kimitaka; Bikkina, Srinivas; Sarin, M M

    2016-02-15

    Hygroscopic properties of water-soluble matter (WSM) extracted from fine-mode aerosols (PM2.5) in the marine atmospheric boundary layer of the Bay of Bengal (BoB) have been investigated during a cruise from 27th December 2008 to 30th January 2009. Hygroscopic growth factors were measured on particles generated from the WSM using an H-TDMA system with an initial dry size of 100 nm in the range of 5-95% relative humidity (RH). The measured hygroscopic growth of WSM at 90% RH, g(90%)WSM, were ranged from 1.11 to 1.74 (mean: 1.43 ± 0.19) over the northern BoB and 1.12 to 1.38 (mean: 1.25 ± 0.09) over the southern BoB. A key finding is that distinct hygroscopic growth factors are associated with the air masses from the Indo-Gangetic plains (IGP), which are clearly distinguishable from those associated with air masses from Southeast Asia (SEA). We found higher (lower) g(90%)WSM over the northern (southern) BoB, which were associated with an IGP (SEA) air masses, probably due the formation of high hygroscopic salts such as (NH4)2SO4. On the other hand, biomass burning influenced SEA air masses confer the low hygroscopic salts such as K2SO4, MgSO4, and organic salts over the southern BoB. Interestingly, mass fractions of water-soluble organic matter (WSOM) showed negative and positive correlations with g(90%)WSM over the northern and southern BoB, respectively, suggesting that the mixing state of organic and inorganic fractions could play a major role on the g(90%)WSM over the BoB. Further, WSOM/SO4(2-) mass ratios suggest that SO4(2-) dominates the g(90%)WSM over the northern BoB whereas WSOM fractions were important over the southern BoB. The present study also suggests that aging process could significantly alter the hygroscopic growth of aerosol particles over the BoB, especially over the southern BoB.

  7. 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.

  8. 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

  9. Hygroscopic properties of different aerosol types over the Atlantic and Indian Oceans

    NASA Astrophysics Data System (ADS)

    Maßling, A.; Wiedensohler, A.; Busch, B.; Neusüß, C.; Quinn, P.; Bates, T.; Covert, D.

    2003-01-01

    time periods signifying the origin of the observed aerosol. All time periods showed a group of particles with high hygroscopic growth. The measured average hygroscopic growth factors ranged from 1.6 to 2.0, depending on the dry particle size and on the type of air mass. Particles with low hygroscopic growth occurred only when continentally influenced air masses arrived at the ship's position. Distinctions in hygroscopic growth of particles of different air masses were more significant for small relative humidities (30% or 55% RH). High concentrations of elemental carbon corresponded with high light absorption coefficients and with the occurrence of less-hygroscopic and nearly hydrophobic particle fractions in the hygroscopic growth distributions. Finally, a solubility model was used to calculate soluble particle volume fractions for air masses of different origin in the Northern and Southern Hemispheres. A key finding is that clean marine air masses that had no land contact for five to six days could clearly be distinguished from polluted air masses that had passed over a continent several days before reaching the ship. This distinction was based on results by taking into account only the hygroscopic characteristics and the solubility of the observed particles.

  10. Hygroscopicity of Black-Carbon-Containing Aerosol in Wildfire Plumes

    NASA Astrophysics Data System (ADS)

    Perring, A. E.; Schwarz, J. P.; Markovic, M. Z.; Fahey, D. W.; Yokelson, R. J.; Jimenez, J. L.; Campuzano Jost, P.; Day, D. A.; Palm, B. B.; Wisthaler, A.; Ziemba, L. D.; Anderson, B. E.; Diskin, G. S.; Huey, L. G.; Gao, R. S.

    2015-12-01

    Water uptake by black carbon (BC) containing aerosol has been quantified in wildfire plumes of varying age (from 1 to ~40 hr old) sampled in North America during the NASA SEAC4RS mission of 2013. Measurements were made in flight using parallel single-particle soot photometers (SP2) that simultaneously detected the BC component of the ambient aerosol ensemble under contrasting humidity conditions. The hygroscopicity parameter, κ, of material internally mixed with BC derived from this data set is consistent with previous estimates of bulk aerosol hygroscopicity from biomass burning sources. We explore the temporal evolution of κ during aging of the Yosemite Rim Fire plume to constrain the rate of conversion of BC-containing aerosol from hydrophobic to hydrophilic modes in these emissions. We also investigate the relationship between κ values for BC-containing particles and the oxidation state and hygroscopicity of the bulk aerosol. These observations have implications for BC transport and removal in biomass burning plumes and provide important constraints on model treatment of BC optical and microphysical properties from wildfire sources in ambient conditions.

  11. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-11-01

    concentration dependence of κm can be described by a simple KIM model equation based on observable mass growth factors and six fit parameters summarizing the combined effects of the dilute intrinsic hygroscopicity and interaction parameters of all involved chemical components. One of the fit parameters represents κm,∞ and can be used to predict CCN activation diameters as a function of water vapor supersaturation. For sodium chloride reference particles as well as for pristine rainforest aerosols consisting mostly of secondary organic matter, we obtained good agreement between the predicted and measured critical diameters of CCN activation. The application of KIM and mass-based measurement techniques shall help to bridge gaps in the current understanding of water uptake by atmospheric aerosols: (1) the gap between hygroscopicity parameters determined by HTDMA (hygroscopicity tandem differential mobility analyzer) or FDHA measurements under sub-saturated conditions and by CCN measurements at water vapor supersaturation, and (2) the gap between the results of simplified single parameter models widely used in atmospheric or climate science and the results of complex multi-parameter ion- and molecule-interaction models frequently used in physical chemistry and thermodynamics (AIM, E-AIM, UNIFAC, AIOMFAC etc.).

  13. 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.

  14. 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.

  15. 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

  16. Combined use of optical and electron microscopic techniques for the measurement of hygroscopic property, chemical composition, and morphology of individual aerosol particles.

    PubMed

    Ahn, Kang-Ho; Kim, Sun-Man; Jung, Hae-Jin; Lee, Mi-Jung; Eom, Hyo-Jin; Maskey, Shila; Ro, Chul-Un

    2010-10-01

    In this work, an analytical method for the characterization of the hygroscopic property, chemical composition, and morphology of individual aerosol particles is introduced. The method, which is based on the combined use of optical and electron microscopic techniques, is simple and easy to apply. An optical microscopic technique was used to perform the visual observation of the phase transformation and hygroscopic growth of aerosol particles on a single particle level. A quantitative energy-dispersive electron probe X-ray microanalysis, named low-Z particle EPMA, was used to perform a quantitative chemical speciation of the same individual particles after the measurement of the hygroscopic property. To validate the analytical methodology, the hygroscopic properties of artificially generated NaCl, KCl, (NH(4))(2)SO(4), and Na(2)SO(4) aerosol particles of micrometer size were investigated. The practical applicability of the analytical method for studying the hygroscopic property, chemical composition, and morphology of ambient aerosol particles is demonstrated.

  17. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-09-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/glutaric acid system; deviations up to 10% in mass growth factor (corresponding to deviations up to 3.5% in size growth factor) are observed for the ammonium sulfate/citric acid 1:1 mixture at 80% RH. We observe even more significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  18. [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.

  19. Hygroscopic behavior of water-soluble matter in marine aerosols over the East China Sea.

    PubMed

    Yan, Yu; Fu, Pingqing; Jing, Bo; Peng, Chao; Boreddy, S K R; Yang, Fan; Wei, Lianfang; Sun, Yele; Wang, Zifa; Ge, Maofa

    2017-02-01

    In this study, we investigated hygroscopic properties of water-soluble matter (WSM) in marine aerosols over the East China Sea, which were collected during a Natural Science Foundation of China (NSFC) sharing cruise in 2014. Hygroscopic growth factors (g) of WSM were measured by a hygroscopicity tandem differential mobility analyzer (H-TDMA) with an initial dry particle mobility diameter of 100nm. The observed g at 90% relative humidity (RH), g(90%)WSM, defined as the ratio of the particle diameter at 90% RH to that at RH<5% (initial dry diameter), ranged from 1.67 to 2.41 (mean±std: 1.99±0.23). The g values were lower than that of seawater (2.1) but comparable with those reported for marine aerosols (1.79-2.08). The H-TDMA retrieved hygroscopicity parameter of WSM, κWSM, ranged from 0.46 to 1.56 (0.88±0.35). The observed g(90%)WSM during the daytime ranged from 1.67 to 2.40 (1.95±0.21) versus 1.71 to 2.41 (2.03±0.26) during the nighttime. κWSM was 0.81±0.32 in the daytime and 0.95±0.40 in the nighttime. The day/night differences of g(90%)WSM and κWSM indicated that nighttime marine aerosols were more hygroscopic than those in daytime, which was likely related to enhanced heterogeneous reaction of ammonium nitrate in nighttime and the higher Cl(-)/Na(+) molar ratios obtained (0.80) in nighttime than those (0.47) in daytime. Inorganic ions accounted for 72-99% of WSM with SO4(2-) being the dominant species, contributing to 47% of the total inorganic ion mass. The declined g(90%) comparing with sea water was likely due to the transport of anthropogenic aerosols, chemical aging of dust particles, the contribution of biomass burning products, and the aerosol hygroscopic growth inhibition of organics.

  20. 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

  1. 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

  2. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    NASA Astrophysics Data System (ADS)

    Asmi, E.; Frey, A.; Virkkula, A.; Ehn, M.; Manninen, H. E.; Timonen, H.; Tolonen-Kivimäki, O.; Aurela, M.; Hillamo, R.; Kulmala, M.

    2009-12-01

    The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  3. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    NASA Astrophysics Data System (ADS)

    Asmi, E.; Frey, A.; Virkkula, A.; Ehn, M.; Manninen, H. E.; Timonen, H.; Tolonen-Kivimäki, O.; Aurela, M.; Hillamo, R.; Kulmala, M.

    2010-05-01

    The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. A non-equilibrium model for the hygroscopic growth and dry deposition of atmospheric particles to water surfaces

    SciTech Connect

    Zufall, M.J.; Davidson, C.I.; Bergin, M.H.

    1995-12-31

    Atmospheric dry deposition may provide a significant contribution of pollutants to a body of water. The rate of dry deposition to water surfaces may be enhanced by the growth of hygroscopic aerosols. Current dry deposition models predict hygroscopic growth by assuming equilibrium between the particles and atmosphere. However, particles larger than 1 mm may not reach their equilibrium size. These models also assume a constant, high (> 99%) relative humidity throughout the laminar flow region several centimeters above the water surface. Relative humidity profiles determined for ocean surfaces show that this is generally not the case, as the relative humidity decreases quickly above the water surface. A hygroscopic growth model is presented that combines more accurate relative humidity profiles with detailed water vapor mass transport. Hygroscopic growth estimates for ammonium nitrate, ammonium sulfate and mixtures of these two salts show that the current deposition models greatly over predict the influence of hygroscopic growth on deposition velocity to water surfaces.

  10. 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.

  11. 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

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

    PubMed

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

    2008-07-29

    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 approximately 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.

  13. Size-resolved aerosol composition and its link to hygroscopicity at a forested site in Colorado

    NASA Astrophysics Data System (ADS)

    Levin, E. J. T.; Prenni, A. J.; Palm, B. B.; Day, D. A.; Campuzano-Jost, P.; Winkler, P. M.; Kreidenweis, S. M.; DeMott, P. J.; Jimenez, J. L.; Smith, J. N.

    2014-03-01

    Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen-Rocky Mountain Biogenic Aerosol Study) campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions were between 70 and 90%. Corresponding aerosol hygroscopicity was observed to be in the range κ = 0.15-0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an aerosol mass spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study, with an assumed value of κorg = 0.13 resulting in the best agreement.

  14. Hygroscopic properties of humic-like organics isolated from atmospheric fine aerosol

    NASA Astrophysics Data System (ADS)

    Gysel, M.; Nyeki, S.; Weingartner, E.; Galambos, I.; Kiss, G.; Baltensperger, U.

    2003-04-01

    Organic species are a major fraction of the fine aerosol mode and it has been suggested that water-soluble organic carbon (WSOC) compounds may play an important role in cloud formation. Fine aerosol samples (diameter D < 1.5 μm) from the continental rural site K-puszta, Hungary, were characterized using a solid phase extraction method. The total water-soluble content (WSC) was composed of 49 % inorganics, 14 % highly water-soluble organics, and 37 % of less soluble organics. The latter, called isolated organic matter (ISOM), is assumed to be mainly composed of humic-like substances. Hygroscopic growth factors (HGF) of nebulised WSC and ISOM extracts, as well as reference substances NRFA and NRHA (fulvic and humic acids), were measured with an H-TDMA. Under increasing RH dry ISOM particles (D{_o} = 100 nm) dissolved in the range RH = 30 - 60 %, followed by continuous growth above this deliquescence transition, resulting in HGFs of D/D{_o} 1.14 at 90 % RH. Particles from WSC extracts exhibited HGFs of D/D{_o} 1.61 at 90 % RH. This is close to the HGF of pure ammonium sulfate (D/D{_o} = 1.69 at 90 % RH), indicating that ISOM contributes significantly to water uptake of mixed WSC particles. Although ISOM is distinctly less hygroscopic than pure inorganic salt particles, its role in the hygroscopic behavior of atmospheric particles is important because of the large abundance and relatively low deliquescence RH. HGFs of NRFA and NRHA were 1.15 and 1.07 at 90 % RH, and deliquescence was at 80 and 90 % RH, respectively. Their hygroscopic behavior was qualitatively similar to ISOM samples, but quantitative differences might be a result of larger average molecular size of the reference substances.

  15. 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.

  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. Role of the volatile fraction of submicron marine aerosol on its hygroscopic properties

    NASA Astrophysics Data System (ADS)

    Sellegri, Karine; Villani, Paolo; Picard, David; Dupuy, Regis; O'Dowd, Colin; Laj, Paolo

    2008-11-01

    The hygroscopic growth factor (HGF) of 85 nm and 20 nm marine aerosol particles was measured during January 2006 for a three-week period within the frame of the EU FP6 project MAP (Marine Aerosol Production) winter campaign at the coastal site of Mace Head, using the TDMA technique. The results are compared to aerosol particles produced in a simulation tank by bubbling air through sea water sampled near the station, and through synthetic sea water (inorganic salts). This simulation is assimilated to primary production. Aitken and mode particles (20 nm) and accumulation mode particles (85 nm) both show HGF of 1.92 and 2.01 for particles generated through bubbling in natural and artificial sea water respectively. In the Aitken mode, the marine particles sampled in the atmosphere shows a monomodal HGF slightly lower than the one measured for sea salt particles artificially produced by bubble bursting in natural sea water (HGF = 1.83). This is also the case for the more hygroscopic mode of accumulation mode particles. In addition, the HGF of 85 nm particles observed in the atmosphere during clean marine sectors exhibits half of its population with a 1.4 HGF. An external mixture of the accumulation mode marine particles indicates a secondary source of this size of particles, a partial processing during transport, or an inhomogeneity of the sea water composition. A gentle 90 °C thermo-desorption results in a significant decrease of the number fraction of moderately hygroscopic (HGF = 1.4) particles in the accumulation mode to the benefit of the seasalt mode, pointing to the presence of semi-volatile compounds with pronounced hydrophobic properties. The thermo-desorption has no effect on the HGF of bubble generated aerosols, neither for synthetic or natural sea water, nor on the atmospheric Aitken mode, indicating that these hydrophobic compounds are secondarily integrated in the particulate phase. No difference between night and day samples is observed on the natural

  18. 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.

  19. 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

  20. 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

  1. On the Physicochemical Processes Controlling Organic Aerosol Hygroscopicity

    NASA Astrophysics Data System (ADS)

    Petters, Sarah Suda

    Aerosol particles in the atmosphere can influence air quality and climate through their interaction with water. Aerosols are an important factor in cloud formation because they serve as cloud condensation nuclei (CCN). Organic compounds contribute a large fraction of the atmospheric aerosol mass but their ability to serve as CCN is less certain relative to inorganic compounds. Limitations of the measurement techniques and theoretical gaps in understanding have prevented agreement between predicted and measured CCN. One way to quantify a compound's CCN activity is by the hygroscopicity parameter, kappa. This dissertation presents research towards constraining the variability of organic aerosol kappa at the process level using three approaches: developing a measurement technique; measuring the dependence of kappa on molecular functional groups; and measuring the effect of surface active molecules on kappa for mixtures. Chapter 2 presents a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) instrument to measure aerosol water uptake at high relative humidity (RH). Measurements up to 99% RH were achieved by improving the precision of aerosol sizing, actively controlling temperature, and calibrating RH between measurements. Osmotic coefficients were obtained within +/-20% for organic aerosols sized between 30 and 200 nanometers. These results may improve water uptake models by providing accurate data at high RH. Chapter 3 presents a study of the sensitivity of kappa to changes in molecular functional group composition for pure compounds. Molecules were synthesized via gas and liquidphase reactions varying the type and location of functional groups, purified by High Performance Liquid Chromatography (HPLC), and routed for CCN measurement. The hydroxyl (-OH) and carbon chain length (-CH2-) changed kappa most, where hydroxyl groups increase kappa and longer carbon chains decrease kappa. This suggests that hydroxyl groups and molecular size dominate the

  2. 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

  3. 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.

  4. 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

  5. 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.

  6. 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.

    2014-05-01

    Hygroscopic behavior of organic compounds, including levoglucosan, 4-hydroxybenzoic acid and humic acid, and 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 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-hydrobenxybenzoic 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 effects), which are not

  7. 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.

  8. Assessment of CCN based on size-resolved hygroscopicity data: Results from urban aerosol measurements in Nagoya, Japan

    NASA Astrophysics Data System (ADS)

    Kawana, K.; Nakayama, T.; Mochida, M.

    2012-12-01

    To assess the number concentrations and the proportion of cloud condensation nuclei (CCN) and the CCN activation diameter (dact) of urban aerosols based on size-resolved hygroscopicity, the atmospheric observation was performed for 10 days at an urban site of Nagoya, Japan in September 2009. The hygroscopic growth factor (HGF) distributions of aerosol particles at 85% RH were measured using a hygroscopicity tandem differential mobility analyzer (HTDMA) system, which consists of two differential mobility analyzers (DMAs) and a condensation particle counter (CPC). The proportion of CCN in the aerosol particles exiting the first DMA of the HTDMA was measured using a CCN counter and a CPC. The number concentrations of CCN (NCCN), the ratio of NCCN to the number concentrations of condensation nuclei (NCN), and dact were predicted from the observed HTDMA data based on k-köhler theory, and they were compared with measured values. Here, measured NCCN is that obtained from the number-size distribution of aerosol particles and the size-resolved NCCN/NCN. The measured dact was obtained from a curve fit to a CCN efficiency spectrum. The dact was predicted using different two methods. Whereas one of the methods to predict dact is based on the mean hygroscopic growth factor (gmean) at each diameter, the other accounts for activation of aerosol particles at each HGF bin. The NCCN and NCCN/NCN were predicted using the latter method only. The predicted NCCN and the predicted NCCN/NCN were, respectively, on average 19% and 15% lower than the measured values. The predicted dact were on average 8% higher than the measured values by both of the methods.

  9. A study of phase transformations in hygroscopic aerosols by Raman spectroscopy

    SciTech Connect

    Tang, I.N.; Fung, K.H.

    1995-12-31

    Atmospheric aerosol particles are composed mostly of hygroscopic inorganic salts. These aerosols play an important role in many atmospheric processes which affect local air quality, visibility degradation, and the global climate as well. Indeed, hygroscopic aerosols as metastable supersaturated solution droplets are routinely observed in laboratories. Here, we report first spectroscopic evidence that new metastable solid states form from hygroscopic aerosol particles. Levitated single particles undergo hydration and crystallization in calibrated humidity environment. Laser Raman and Mie scattering techniques are used to probe the chemical and physical state of the microparticle before and after phase transformation. The formation of these states is not predicted from bulk-phase thermodynamics. In some cases, the resulting metastable state is entirely unknown heretofore. We also present new solid/solution and solid/solid phase transitions which occur exclusively in microparticles.

  10. 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.

  11. Direct measurements of the optical cross sections and refractive indices of individual volatile and hygroscopic aerosol particles.

    PubMed

    Mason, B J; Cotterell, M I; Preston, T C; Orr-Ewing, A J; Reid, J P

    2015-06-04

    We present measurements of the evolving extinction cross sections of individual aerosol particles (spanning 700-2500 nm in radius) during the evaporation of volatile components or hygroscopic growth using a combination of a single particle trap formed from a Bessel light beam and cavity ring-down spectroscopy. For single component organic aerosol droplets of 1,2,6-hexanetriol, polyethylene glycol 400, and glycerol, the slow evaporation of the organic component (over time scales of 1000 to 10,000 s) leads to a time-varying size and extinction cross section that can be used to estimate the refractive index of the droplet. Measurements on binary aqueous-inorganic aerosol droplets containing one of the inorganic solutes ammonium bisulfate, ammonium sulfate, sodium nitrate, or sodium chloride (over time scales of 1000 to 15,000 s) under conditions of changing relative humidity show that extinction cross-section measurements are consistent with expectations from accepted models for the variation in droplet refractive index with hygroscopic growth. In addition, we use these systems to establish an experimental protocol for future single particle extinction measurements. The advantages of mapping out the evolving light extinction cross-section of an individual particle over extended time frames accompanied by hygroscopic cycling or component evaporation are discussed.

  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.; 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.

  13. Hygroscopic growth and deliquescence of NaCl nanoparticles coated with surfactant AOT.

    PubMed

    Alshawa, Ahmad; Dopfer, Otto; Harmon, Christopher W; Nizkorodov, Sergey A; Underwood, Joelle S

    2009-07-02

    Aerosolized nanoparticles of NaCl coated with variable amounts of surfactant AOT were generated by electrospraying AOT/NaCl aqueous solutions, followed by neutralizing and drying the resulting particles. A tandem differential mobility analyzer was used to select a narrow size distribution of particles with mobility equivalent diameters below 20 nm and monitor their hygroscopic growth as a function of relative humidity. Effects of the particle size and relative amount of surfactant on the hygroscopic growth of NaCl were studied. For pure NaCl nanoparticles, the deliquescence relative humidity (DRH) increased as the particle size was decreased, in full agreement with previous measurements. Below the DRH the NaCl nanoparticles had an equivalent of one-four monolayers of water adsorbed on the surface. The addition of a sub-monolayer AOT coating reduced the DRH and suppressed the hygroscopic growth of the NaCl core. At AOT coverage levels exceeding one monolayer, a clear deliquescence transition was no longer discernible. The Zdanovskii-Stokes-Robinson (ZSR) model failed to predict the observed growth factors of mixed AOT/NaCl nanoparticles reflecting a large contribution of the interfacial interactions between NaCl and AOT to the total free energy of the particles. There were indications that AOT/NaCl nanoparticles prepared by the electrospray aerosol source were enhanced in the relative mass fraction of AOT in comparison with the solution from which they were electrosprayed.

  14. Profiling aerosol optical, microphysical and hygroscopic properties in ambient conditions by combining in situ and remote sensing

    NASA Astrophysics Data System (ADS)

    Tsekeri, Alexandra; Amiridis, Vassilis; Marenco, Franco; Nenes, Athanasios; Marinou, Eleni; Solomos, Stavros; Rosenberg, Phil; Trembath, Jamie; Nott, Graeme J.; Allan, James; Le Breton, Michael; Bacak, Asan; Coe, Hugh; Percival, Carl; Mihalopoulos, Nikolaos

    2017-01-01

    We present the In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) that combines airborne in situ and lidar remote sensing data to retrieve vertical profiles of ambient aerosol optical, microphysical and hygroscopic properties, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. Here we apply the algorithm on data collected from the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft during the ACEMED campaign in the Eastern Mediterranean. Vertical profiles of aerosol microphysical properties have been derived successfully for an aged smoke plume near the city of Thessaloniki with aerosol optical depth of ˜ 0.4 at 532 nm, single scattering albedos of ˜ 0.9-0.95 at 550 nm and typical lidar ratios for smoke of ˜ 60-80 sr at 532 nm. IRRA retrieves highly hydrated particles above land, with 55 and 80 % water volume content for ambient relative humidity of 80 and 90 %, respectively. The proposed methodology is highly advantageous for aerosol characterization in humid conditions and can find valuable applications in aerosol-cloud interaction schemes. Moreover, it can be used for the validation of active space-borne sensors, as is demonstrated here for the case of CALIPSO.

  15. Impact of mixing state and hygroscopicity on CCN activity of biomass burning aerosol in Amazonia

    NASA Astrophysics Data System (ADS)

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

    2017-02-01

    Smoke aerosols prevail throughout Amazonia because of widespread biomass burning during the dry season, and external mixing, low variability in the particle size distribution and low particle hygroscopicity are typical. There can be profound effects on cloud properties. This study uses an adiabatic cloud model to simulate the activation of smoke particles as cloud condensation nuclei (CCN) for three hypothetical case studies, chosen as to resemble biomass burning aerosol observations in Amazonia. The relative importance of variability in hygroscopicity, mixing state, and activation kinetics for the activated fraction and maximum supersaturation is assessed. For a population with κp = 0.04, an overestimation of the cloud droplet number concentration Nd for the three selected case studies between 22.4 ± 1.4 and 54.3 ± 3.7 % was obtained when assuming a hygroscopicity parameter κp = 0.20. Assuming internal mixing of the aerosol population led to overestimations of up to 20 % of Nd when a group of particles with medium hygroscopicity was present in the externally mixed population cases. However, the overestimations were below 10 % for external mixtures between very low and low-hygroscopicity particles, as seems to be the case for Amazon smoke particles. Kinetic limitations were significant for medium- and high-hygroscopicity particles, and much lower for very low and low-hygroscopicity particles. When particles were assumed to be at equilibrium and to respond instantly to changes in the air parcel supersaturation, the overestimation of the droplet concentration was up to ˜ 100 % in internally mixed populations, and up to ˜ 250 % in externally mixed ones, being larger for the higher values of hygroscopicity. In addition, a perceptible delay between the times when maximum supersaturation and maximum aerosol activated fraction are reached was noticed and, for aerosol populations with effective hygroscopicity κpeff higher than a certain threshold value, the delay in

  16. 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.

  17. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

    NASA Astrophysics Data System (ADS)

    Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

    2008-03-01

    Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

  18. Hygroscopic growth and cloud droplet activation of xanthan gum as a proxy for marine hydrogels

    NASA Astrophysics Data System (ADS)

    Dawson, K. W.; Petters, M. D.; Meskhidze, N.; Petters, S. Suda; Kreidenweis, S. M.

    2016-10-01

    Knowledge of the physical characteristics and chemical composition of marine organic aerosols is needed for the quantification of their effects on cloud microphysical processes and solar radiative transfer. Here we use xanthan gum (XG)—a bacterial biopolymer—as a proxy for marine hydrogels. Measurements were performed for pure XG particles and mixtures of XG with sodium chloride, calcium nitrate, and calcium carbonate. The aerosol hygroscopicity parameter (κ) is derived from hygroscopic growth factor measurements (κgf) at variable water activity (aw) and from cloud condensation nuclei activation efficiency (κccn). The Zdanovskii, Stokes, and Robinson (ZSR) hygroscopicity parameter derived for multicomponent systems (κmix, sol) is used to compare measurements of κgf and κccn. Pure XG shows close agreement of κgf (at aw = 0.9) and κccn of 0.09 and 0.10, respectively. Adding salts to the system results in deviations of κgf (at aw = 0.9) from κccn. The measured κgf and ZSR-derived hygroscopicity parameter (κmix, sol) values for different solutions show close agreement at aw > 0.9, while κgf is lower in comparison to κmix, sol at aw < 0.9. The differences between predicted κmix, sol and measured κgf and κccn values are explained by the effects of hydration and presence of salt ions on the structure of the polymer networks. Results from this study imply that at supersaturations of 0.1 and 0.5%, the presence of 30% sea salt by mass can reduce the activation diameter of pure primary marine organic aerosols from 257 to 156 nm and from 87 to 53 nm, respectively.

  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. Will Aerosol Hygroscopicity Change with Biodiesel, Renewable Diesel Fuels and Emission Control Technologies?

    PubMed

    Vu, Diep; Short, Daniel; Karavalakis, Georgios; Durbin, Thomas D; Asa-Awuku, Akua

    2017-02-07

    The use of biodiesel and renewable diesel fuels in compression ignition engines and aftertreatment technologies may affect vehicle exhaust emissions. In this study two 2012 light-duty vehicles equipped with direct injection diesel engines, diesel oxidation catalyst (DOC), diesel particulate filter (DPF), and selective catalytic reduction (SCR) were tested on a chassis dynamometer. One vehicle was tested over the Federal Test Procedure (FTP) cycle on seven biodiesel and renewable diesel fuel blends. Both vehicles were exercised over double Environmental Protection Agency (EPA) Highway fuel economy test (HWFET) cycles on ultralow sulfur diesel (ULSD) and a soy-based biodiesel blend to investigate the aerosol hygroscopicity during the regeneration of the DPF. Overall, the apparent hygroscopicity of emissions during nonregeneration events is consistently low (κ < 0.1) for all fuels over the FTP cycle. Aerosol emitted during filter regeneration is significantly more CCN active and hygroscopic; average κ values range from 0.242 to 0.439 and are as high as 0.843. Regardless of fuel, the current classification of "fresh" tailpipe emissions as nonhygroscopic remains true during nonregeneration operation. However, aftertreatment technologies such as DPF, will produce significantly more hygroscopic particles during regeneration. To our knowledge, this is the first study to show a significant enhancement of hygroscopic materials emitted during DPF regeneration of on-road diesel vehicles. As such, the contribution of regeneration emissions from a growing fleet of diesel vehicles will be important.

  1. 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

  2. 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

  3. Calculation of aerosol optical properties under different assumptions on mixing state, refractive index, density and hygroscopicity: uncertainties and importance of representation of aerosol mixing state

    NASA Astrophysics Data System (ADS)

    Curci, Gabriele

    2015-04-01

    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. We used the FlexAOD post-processing tool to calculate the optical properties (aerosol optical depth (AOD), single scattering albedo (SSA) and asymmetry parameter (g)) from chemistry-transport model aerosol profiles, using a wide range of assumptions on aerosol chemical and physical properties. We calculated that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. We then tested simple parameterizations of the aerosol mixing state, expressed as a function of the aerosol aging, and verified that they may be helpful in reducing the uncertainty when comparing simulations with AERONET retrievals.

  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, 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.

  5. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2017-02-01

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

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

    DOE PAGES

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; ...

    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

  8. Surface organic monolayers control the hygroscopic growth of submicrometer particles at high relative humidity.

    PubMed

    Ruehl, Christopher R; Wilson, Kevin R

    2014-06-05

    Although many organic molecules commonly found in the atmosphere are known to be surface-active in macroscopic aqueous solutions, the impact of surface partitioning of organic molecules to a microscopic aqueous droplet interface remains unclear. Here we measure the droplet size formed, at a relative humidity (∼99.9%) just below saturation, on submicrometer particles containing an ammonium sulfate core and an organic layer of a model compound of varying thickness. The 12 model organic compounds are a series of dicarboxylic acids (C3 to C10), cis-pinonic, oleic, lauric, and myristic acids, which represent a broad range in solubility from miscible (malonic acid) to insoluble. The variation in droplet size with increasing organic aerosol fraction cannot be explained by assuming the organic material is dissolved in the bulk droplet. Instead, the wet droplet diameters exhibit a complex and nonlinear dependence on organic aerosol volume fraction, leading to hygroscopic growth that is in some cases smaller and in others larger than that predicted by bulk solubility alone. For palmitic and stearic acid, small droplets at or below the detection limit of the instrument are observed, indicating significant kinetic limitations for water uptake, which are consistent with mass accommodation coefficients on the order of 10(-4). A model based on the two-dimensional van der Waals equation of state is used to explain the complex droplet growth with organic aerosol fraction and dry diameter. The model suggests that mono- and dicarboxylic acids with limited water solubility partition to the droplet surface and reduce surface tension only after a two-dimensional condensed monolayer is formed. Two relatively soluble compounds, malonic and glutaric acid, also appear to form surface phases, which increase hygroscopicity. There is a clear alternation in the threshold for droplet growth observed for odd and even carbon number diacids, which is explained in the model by differences in the

  9. Hygroscopic Measurements of Aerosol Particles in the San Joaquin Valley California during the DRAGON and Discover AQ Campaign 2013

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

    In the ambient atmosphere, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH). 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 observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth. The DISCOVER-AQ campaign is focused in improving the interpretation and relation between satellite observations and surface conditions related to air quality. In the winter of 2013, this campaign was held in the San Joaquin Valley, California, 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. Different instruments such as particulate samplers, lidars, meteorological stations and airborne passive and active monitoring were coordinated to measure the aerosol structure of the San Joaquin Valley in a simultaneous fashion. A novel humidifier-dryer system for a TSI 3563 Nephelometer was implemented in the Penn State University NATIVE trailer located in Porterville California 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. Measurements in Porterville California reached dry scattering coefficient readings greater than 300Mm-1 at 550nm indicating the presence of a large amount of particles in the region. However, the ratio between scattering coefficients at high and low humidity, called the enhancement factor f

  10. 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

    2014-02-07

    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.

  11. 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.

  12. 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.

  13. 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

  14. 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

  15. Quantifying the Hygroscopic Growth of Individual Submicrometer Particles with Atomic Force Microscopy.

    PubMed

    Morris, Holly S; Estillore, Armando D; Laskina, Olga; Grassian, Vicki H; Tivanski, Alexei V

    2016-04-05

    The water uptake behavior of atmospheric aerosol dictates their climate effects. In many studies, aerosol particles are deposited onto solid substrates to measure water uptake; however, the effects of the substrate are not well understood. Furthermore, in some cases, methods used to analyze and quantify water uptake of substrate deposited particles use a two-dimensional (2D) analysis to monitor growth by following changes in the particle diameter with relative humidity (RH). However, this 2D analysis assumes that the droplet grows equally in all directions. If particle growth is not isotropic in height and diameter, this assumption can cause inaccuracies when quantifying hygroscopic growth factors (GFs), where GF for a for a spherical particle is defined as the ratio of the particle diameter at a particular relative humidity divided by the dry particle diameter (typically about 5% RH). However, as shown here, anisotropic growth can occur in some cases. In these cases, a three-dimensional (3D) analysis of the growth is needed. This study introduces a way to quantify the hygroscopic growth of substrate deposited particles composed of model systems relevant to atmospheric aerosols using atomic force microscopy (AFM), which gives information on both the particle height and area and thus a three-dimensional view of each particle. In this study, we compare GFs of submicrometer sized particles composed of single component sodium chloride (NaCl) and malonic acid (MA), as well as binary mixtures of NaCl and MA, and NaCl and nonanoic acid (NA) determined by AFM using area (2D) equivalent diameters, similar to conventional microscopy methods, to GFs determined using volume (3D) equivalent diameter. We also compare these values to GFs determined by a hygroscopic tandem differential mobility analyzer (HTDMA; substrate free, 3D method). It was found that utilizing volume equivalent diameter for quantifying GFs with AFM agreed well with those determined by substrate-free HTDMA

  16. 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

  17. Hygroscopic Behavior of Ambient Aerosols at an Anthropogenically Perturbed Continental U.S.A. Site, Bondville, Illinois.

    NASA Astrophysics Data System (ADS)

    Kus, P.; Rood, M. J.; Ogren, J.; Quinn, P.; Covert, D. S.

    2002-12-01

    The dependence of ambient aerosols' light scattering coefficient on controlled relative humidity (RH) conditions was measured for ambient aerosol at the Bondville Aerosol Research Site (BEARS), located in east-central Illinois, USA. The measurements were made with a controlled RH nephelometry system between 1995 and 2000. The fact that an aerosol's hygroscopic growth is one of the most important parameters in estimating an aerosol's ability to cause radiative forcing makes it important to characterize that property at relevant locations on a regional scale. Total and hemispheric back scattering coefficients were measured by two nephelometers operating in series as a function of wavelength of light (450, 550, and 700 nm), controlled RH, and upper particle diameter (Dp) of 1 and 10 μm. In addition, gravimetric and inorganic ion composition of the sub-micrometer diameter particles were determined using filter samples. Particle size distributions were measured by a combined system of Differential Mobility Analyzer (DMA) and Aerodynamic Particle Sizer (APS) during a 20-day intensive field campaign. Hygroscopic growth factor (f(RH=82%)) is expressed as the ratio of the scattering coefficient at 82% RH to the scattering at a reference RH (RH<40%). The measured f(RH) values exhibited both deliquescent and monotonic types of growth and were fitted to two different nonlinear equations depending on the type of observed growth. The value of f(RH=82%) at 550 nm was 1.84 +/- 0.43 for sub-micrometer and almost the same with 1.83 +/- 0.42 for super-micrometer aerosols. Higher f(RH) values were associated with the periods where the scattering was dominated by sub-micrometer diameter particles. Deliquescent type of growth was observed 20% of the time. The f(RH) values were higher for aerosol exhibiting deliquescent growth by 8%, which is statistically significant. Available air mass trajectories revealed that the highest f(RH) values were observed when the air mass reaching the

  18. 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

  19. 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

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

    DOE PAGES

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; ...

    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

  1. 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

  2. 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

  3. Comparison of experimental and modeled absorption enhancement by black carbon (BC) cored polydisperse aerosols under hygroscopic conditions.

    PubMed

    Shamjad, P M; Tripathi, S N; Aggarwal, S G; Mishra, S K; Joshi, Manish; Khan, Arshad; Sapra, B K; Ram, Kirpa

    2012-08-07

    The quantification of the radiative impacts of light absorbing ambient black carbon (BC) particles strongly depends on accurate measurements of BC mass concentration and absorption coefficient (β(abs)). In this study, an experiment has been conducted to quantify the influence of hygroscopic growth of ambient particles on light absorption. Using the hygroscopic growth factor (i.e., Zdanovskii-Stokes-Robinson (ZSR) approach), a model has been developed to predict the chemical composition of particles based on measurements, and the absorption and scattering coefficients are derived using a core-shell assumption with light extinction estimates based on Mie theory. The estimated optical properties agree within 7% for absorption coefficient and 30% for scattering coefficient with that of measured values. The enhancement of absorption is found to vary according to the thickness of the shell and BC mass, with a maximum of 2.3 for a shell thickness of 18 nm for the particles. The findings of this study underline the importance of considering aerosol-mixing states while calculating their radiative forcing.

  4. Shapes of internally mixed hygroscopic aerosol particles after deliquescence, and their effect on light scattering

    NASA Astrophysics Data System (ADS)

    Adachi, Kouji; Freney, Evelyn J.; Buseck, Peter R.

    2011-07-01

    Hygroscopic aerosol particles change the magnitude of light scattering through condensation and evaporation of water vapor. We collected aerosol particles from two megacities and observed the particle shapes at various values of relative humidity (RH) using an environmental cell within a transmission electron microscope. Many Mexico City samples had sulfate particles that were embedded within weakly hygroscopic organic aerosol, whereas the Los Angeles samples mainly consisted of externally mixed sulfate particles. For the Mexico City samples, when the RH was increased in the microscope, only the sulfate parts deliquesced, but the entire particle did not become spherical, i.e., particles containing deliquescent phases do not necessarily become spherical upon deliquescence. This result conflicts with the assumption used in many models, i.e., that deliquesced particles become spherical. Using a discrete-dipole approximation to calculate light scattering of simulated particles that resemble the observed ones, we show that, for particles >1.0 μm, the spherical-shape assumption used in Mie theory underestimates the light scattering by ˜50%, with the exact value depending on the sizes and relative volumes of the constituent phases.

  5. 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.

  6. Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles

    NASA Astrophysics Data System (ADS)

    Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

    2017-02-01

    While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles.

  7. Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles

    PubMed Central

    Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

    2017-01-01

    While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles. PMID:28240258

  8. Hygroscopic properties of potassium chloride and its internal mixtures with organic compounds relevant to biomass burning aerosol particles.

    PubMed

    Jing, Bo; Peng, Chao; Wang, Yidan; Liu, Qifan; Tong, Shengrui; Zhang, Yunhong; Ge, Maofa

    2017-02-27

    While water uptake of aerosols exerts considerable impacts on climate, the effects of aerosol composition and potential interactions between species on hygroscopicity of atmospheric particles have not been fully characterized. The water uptake behaviors of potassium chloride and its internal mixtures with water soluble organic compounds (WSOCs) related to biomass burning aerosols including oxalic acid, levoglucosan and humic acid at different mass ratios were investigated using a hygroscopicity tandem differential mobility analyzer (HTDMA). Deliquescence points of KCl/organic mixtures were observed to occur at lower RH values and over a broader RH range eventually disappearing at high organic mass fractions. This leads to substantial under-prediction of water uptake at intermediate RH. Large discrepancies for water content between model predictions and measurements were observed for KCl aerosols with 75 wt% oxalic acid content, which is likely due to the formation of less hygroscopic potassium oxalate from interactions between KCl and oxalic acid without taken into account in the model methods. Our results also indicate strong influence of levoglucosan on hygroscopic behaviors of multicomponent mixed particles. These findings are important in further understanding the role of interactions between WSOCs and inorganic salt on hygroscopic behaviors and environmental effects of atmospheric particles.

  9. 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.

  10. 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.

  11. Influence of collecting substrates on the characterization of hygroscopic properties of inorganic aerosol particles.

    PubMed

    Eom, Hyo-Jin; Gupta, Dhrubajyoti; Li, Xue; Jung, Hae-Jin; Kim, Hyekyeong; Ro, Chul-Un

    2014-03-04

    The influence of six collecting substrates with different physical properties on the hygroscopicity measurement of inorganic aerosol particle surrogates and the potential applications of these substrates were examined experimentally. Laboratory-generated single salt particles, such as NaCl, KCl, and (NH4)2SO4, 1-5 μm in size, were deposited on transmission electron microscopy grids (TEM grids), parafilm-M, Al foil, Ag foil, silicon wafer, and cover glass. The particle hygroscopic properties were examined by optical microscopy. Contact angle measurements showed that parafilm-M is hydrophobic, and cover glass, silicon wafer, Al foil, and Ag foil substrates are hydrophilic. The observed deliquescence relative humidity (DRH) values for NaCl, KCl, and (NH4)2SO4 on the TEM grids and parafilm-M substrates agreed well with the literature values, whereas the DRHs obtained on the hydrophilic substrates were consistently ∼1-2% lower, compared to those on the hydrophobic substrates. The water layer adsorbed on the salt crystals prior to deliquescence increases the Gibb's free energy of the salt crystal-substrate system compared to the free energy of the salt droplet-substrate system, which in turn reduces the DRHs. The hydrophilic nature of the substrate does not affect the measured efflorescence RH (ERH) values. However, the Cl(-) or SO4(2-) ions in aqueous salt droplets seem to have reacted with Ag foil to form AgCl or Ag2SO4, respectively, which in turn acts as seeds for the heterogeneous nucleation of the original salts, leading to higher ERHs. The TEM grids were found to be most suitable for the hygroscopic measurements of individual inorganic aerosol particles by optical microscopy and when multiple analytical techniques, such as scanning electron microscopy-energy dispersive X-ray spectroscopy, TEM-EDX, and/or Raman microspectrometry, are applied to the same individual particles.

  12. 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.

  13. 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.

  14. 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.

  15. 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

  16. 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

  17. 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.

    2015-02-01

    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 by a humidified nephelometer is found to be significantly lower (1.53±0.24 at RH = 85% and λ=450 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 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 direct measurements of a co-located AERONET Sun photometer. The water uptake is found to be of minor importance for the column averaged properties due to the low particle hygroscopicity and the low RH during the

  18. Hygroscopic properties of urban aerosols and their cloud condensation nuclei activities measured in Seoul during the MAPS-Seoul campaign

    NASA Astrophysics Data System (ADS)

    Kim, Najin; Park, Minsu; Yum, Seong Soo; Park, Jong Sung; Song, In Ho; Shin, Hye Jung; Ahn, Joon Young; Kwak, Kyung-Hwan; Kim, Hwajin; Bae, Gwi-Nam; Lee, Gangwoong

    2017-03-01

    Aerosol physical properties, chemical compositions, hygroscopicity and cloud condensation nuclei (CCN) activities were measured in Seoul, the highly populated capital city of Korea, during the Megacity Air Pollution Studies (MAPS-Seoul) campaign, in May-June 2015. The average aerosol concentration for particle diameters >10 nm was 11787 ± 7421 cm-3 with dominant peaks at morning rush hours and in the afternoon due to frequent new particle formation (NPF) events. The average CCN concentration was 4075 ± 1812 cm-3 at 0.6% supersaturation, with little diurnal variation. The average hygroscopicity parameter (κ) value determined using a humidified tandem differential mobility analyzer (HTDMA) ranged 0.17-0.27 for a range of particle diameters (30-150 nm). The κ values derived using the aerosol mass spectrometer (AMS) data with three different methods were 0.32-0.34, significantly higher than those from HTDMA due to the uncertainties in the hygroscopicity values of different chemical compositions, especially organics and black carbon. Factors affecting the aerosol hygroscopicity seemed to be traffic and chemical processes during the NPF events. The CCN concentration predicted based on HTDMA κ data showed very good agreement with the measured one. Because of the overestimation of κ, CCN closure with the predicted CCN concentration based on AMS κ data over-predicted CCN concentration although the linear correlation between measured and predicted CCN concentration was still very good.

  19. At-Sea Evaluation of the Obscuration Characteristics of a Hygroscopic Aerosol Smoke Produced by the CY85A Pyrotechnic

    DTIC Science & Technology

    1983-12-01

    and IiWIU* by block nmber) Salty Dog Obscuration .2Hygroscopic aerosol Extinction ISmoke Pyrotechnically Generated ’For the past six years, Calapan, in...Extinction Characteristics for Salty Dog , NWC 29 and NWC 78 Pyrotechnics,", Calspan Report No. 6663-M-l, 40 pp, Calspan Corporation, Buffalo, NY 14225. 4

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

    NASA Astrophysics Data System (ADS)

    Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

    2009-11-01

    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 were 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 revealed 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 lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) 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.

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

    NASA Astrophysics Data System (ADS)

    Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

    2009-07-01

    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.

  2. 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.

  3. 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.

  4. 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%.

  5. Ambient observations of hygroscopic growth factor and f(RH) below 1: Case studies from surface and airborne measurements

    NASA Astrophysics Data System (ADS)

    Shingler, Taylor; Sorooshian, Armin; Ortega, Amber; Crosbie, Ewan; Wonaschütz, Anna; Perring, Anne E.; Beyersdorf, Andreas; Ziemba, Luke; Jimenez, Jose L.; Campuzano-Jost, Pedro; Mikoviny, Tomas; Wisthaler, Armin; Russell, Lynn M.

    2016-11-01

    This study reports a detailed set of ambient observations of optical/physical shrinking of particles from exposure to water vapor with consistency across different instruments and regions. Data have been utilized from (i) a shipboard humidified tandem differential mobility analyzer during the Eastern Pacific Emitted Aerosol Cloud Experiment in 2011, (ii) multiple instruments on the NASA DC-8 research aircraft during the Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys in 2013, and (iii) the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe during ambient measurements in Tucson, Arizona, during summer 2014 and winter 2015. Hygroscopic growth factor (ratio of humidified-to-dry diameter, GF = Dp,wet/Dp,dry) and f(RH) (ratio of humidified-to-dry scattering coefficients) values below 1 were observed across the range of relative humidity (RH) investigated (75-95%). A commonality of observations of GF and f(RH) below 1 in these experiments was the presence of particles enriched with carbonaceous matter, especially from biomass burning. Evidence of externally mixed aerosol, and thus multiple GFs with at least one GF < 1, was observed concurrently with f(RH) < 1 during smoke periods. Possible mechanisms responsible for observed shrinkage are discussed and include particle restructuring, volatilization effects, and refractive index modifications due to aqueous processing resulting in optical size modification. To further investigate ambient observations of GFs and f(RH) values less than 1, it is recommended to add an optional prehumidification bypass module to hygroscopicity instruments, to preemptively collapse particles prior to controlled RH measurements.

  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. Aerosol Hygroscopicity in the Marine Atmosphere: a Closure Study Using High- Resolution, Size-Resolved AMS and Multiple-RH DASH-SP Data

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Sorooshian, A.; Murphy, S.; Flagan, R. C.; Seinfeld, J. H.

    2008-12-01

    We have conducted the first closure study to couple high-resolution aerosol mass spectrometer (AMS) composition data with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) measurements from the differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). These data were collected off the coast of Central California during seven of the 16 flights carried out during the MASE-II field campaign in July 2007. Two of the seven flights were conducted in airmasses that originated over the continental United States. These flights exhibited elevated organic volume fractions (VForganic =~0.46 ± 0.22, as opposed to 0.24 ± 0.18 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61 ± 0.14 at 92%RH, as compared with 1.91 ± 0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53 ± 0.10 at 85%, compared with 1.58 ± 0.08 for all other flights, and no measurable GF suppression at low RH (1.31 ± 0.06 at 74%, compared with 1.31 ± 0.07 for all other flights). Organic loadings were slightly elevated in above-cloud aerosols, as compared with below-cloud aerosols, and corresponded to a similar trend of significantly suppressed GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided excellent agreement with DASH-SP measurements (R2 = 0.79). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.20, 1.43, and 1.46 at 74, 85, and 92% RH, respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids, and correspond to a highly oxidized, presumably water-soluble, organic fraction (O:C = 0.92 ± 0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is VForganic, indicating that a simple emperical model

  8. Aerosol hygroscopicity in the marine atmosphere: a closure study using high-resolution, size-resolved AMS and multiple-RH DASH-SP data

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Sorooshian, A.; Murphy, S. M.; Flagan, R. C.; Seinfeld, J. H.

    2008-09-01

    We have conducted the first closure study to couple high-resolution aerosol mass spectrometer (AMS) composition data with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) measurements from the differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). These data were collected off the coast of Central California during seven of the 16 flights carried out during the MASE-II field campaign in July 2007. Two of the seven flights were conducted in airmasses that originated over the continental United States. These flights exhibited elevated organic volume fractions (VForganic=0.46±0.22, as opposed to 0.24±0.18 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92% RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for all other flights, and no measurable GF suppression at low RH (1.31±0.06 at 74%, compared with 1.31±0.07 for all other flights). Organic loadings were slightly elevated in above-cloud aerosols, as compared with below-cloud aerosols, and corresponded to a similar trend of significantly suppressed GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided excellent agreement with DASH-SP measurements (R2=0.79). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.20, 1.43, and 1.46 at 74, 85, and 92% RH, respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids, and correspond to a highly oxidized, presumably water-soluble, organic fraction (O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is VForganic, indicating that a simple emperical model relating GF, RH, and

  9. Phase, morphology, and hygroscopicity of mixed oleic acid/sodium chloride/water aerosol particles before and after ozonolysis.

    PubMed

    Dennis-Smither, Benjamin J; Hanford, Kate L; Kwamena, Nana-Owusua A; Miles, Rachael E H; Reid, Jonathan P

    2012-06-21

    Aerosol optical tweezers are used to probe the phase, morphology, and hygroscopicity of single aerosol particles consisting of an inorganic component, sodium chloride, and a water insoluble organic component, oleic acid. Coagulation of oleic acid aerosol with an optically trapped aqueous sodium chloride droplet leads to formation of a phase-separated particle with two partially engulfed liquid phases. The dependence of the phase and morphology of the trapped particle with variation in relative humidity (RH) is investigated by cavity enhanced Raman spectroscopy over the RH range <5% to >95%. The efflorescence and deliquescence behavior of the inorganic component is shown to be unaffected by the presence of the organic phase. Whereas efflorescence occurs promptly (<1 s), the deliquescence process requires both dissolution of the inorganic component and the adoption of an equilibrium morphology for the resulting two phase particle, occurring on a time-scale of <20 s. Comparative measurements of the hygroscopicity of mixed aqueous sodium chloride/oleic acid droplets with undoped aqueous sodium chloride droplets show that the oleic acid does not impact on the equilibration partitioning of water between the inorganic component and the gas phase or the time response of evaporation/condensation. The oxidative aging of the particles through reaction with ozone is shown to increase the hygroscopicity of the organic component.

  10. Hygroscopic and chemical properties of aerosols collected near a copper smelter: implications for public and environmental health.

    PubMed

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

    2012-09-04

    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 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.

  11. 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

  12. 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

  13. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, H.; Cheng, Y.; Ma, N.; Wang, Z.; Wang, X.; Pöhlker, M.; Nillius, B.; Wiedensohler, A.; Pöschl, U.

    2015-09-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to understand aerosol-cloud interactions and their climate impact. It can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach is also applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  14. A broad supersaturation scanning (BS2) approach for rapid measurement of aerosol particle hygroscopicity and cloud condensation nuclei activity

    NASA Astrophysics Data System (ADS)

    Su, Hang; Cheng, Yafang; Ma, Nan; Wang, Zhibin; Wang, Xiaoxiang; Pöhlker, Mira L.; Nillius, Björn; Wiedensohler, Alfred; Pöschl, Ulrich

    2016-10-01

    The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to the understanding of aerosol-cloud interactions and their impact on climate. They can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach may also be applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for aircraft and long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

  15. 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.

  16. From hygroscopic aerosols to cloud droplets: The HygrA-CD campaign in the Athens basin - An overview.

    PubMed

    Papayannis, A; Argyrouli, A; Bougiatioti, A; Remoundaki, E; Vratolis, S; Nenes, A; Solomos, S; Komppula, M; Giannakaki, E; Kalogiros, J; Banks, R; Eleftheriadis, K; Mantas, E; Diapouli, E; Tzanis, C G; Kazadzis, S; Binietoglou, I; Labzovskii, L; Vande Hey, J; Zerefos, C S

    2017-01-01

    The international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD), organized in the Greater Athens Area (GAA), Greece from 15 May to 22 June 2014, aimed to study the physico-chemical properties of aerosols and their impact on the formation of clouds in the convective Planetary Boundary Layer (PBL). We found that under continental (W-NW-N) and Etesian (NE) synoptic wind flow and with a deep moist PBL (~2-2.5km height), mixed hygroscopic (anthropogenic, biomass burning and marine) particles arrive over the GAA, and contribute to the formation of convective non-precipitating PBL clouds (of ~16-20μm mean diameter) with vertical extent up to 500m. Under these conditions, high updraft velocities (1-2ms(-1)) and cloud condensation nuclei (CCN) concentrations (~2000cm(-3) at 1% supersaturation), generated clouds with an estimated cloud droplet number of ~600cm(-3). Under Saharan wind flow conditions (S-SW) a shallow PBL (<1-1.2km height) develops, leading to much higher CCN concentrations (~3500-5000cm(-3) at 1% supersaturation) near the ground; updraft velocities, however, were significantly lower, with an estimated maximum cloud droplet number of ~200cm(-3) and without observed significant PBL cloud formation. The largest contribution to cloud droplet number variance is attributed to the updraft velocity variability, followed by variances in aerosol number concentration.

  17. Real-Time Investigation of Chemical Compositions and Hygroscopic Properties of Aerosols Generated from NaCl and Malonic Acid Mixture Solutions Using in Situ Raman Microspectrometry.

    PubMed

    Li, Xue; Gupta, Dhrubajyoti; Lee, Jisoo; Park, Geonhee; Ro, Chul-Un

    2017-01-03

    Recently, ambient sea spray aerosols (SSAs) have been reported to undergo reactions with dicarboxylic acids (DCAs). Several studies have examined the hygroscopic behavior and chemical reactivity of aerosols generated from NaCl-DCA mixture solutions, but the results have varied, especially for the NaCl-malonic acid (NaCl-MA) mixture system. In this work, in situ Raman microspectrometry (RMS) was used to simultaneously monitor the change in chemical composition, size, and phase as a function of the relative humidity, for individual aerosols generated from NaCl-MA solutions, during two hygroscopic measurement cycles, which were performed first through the dehydration process, followed by a humidification process, in each cycle. In situ RMS analysis for the aerosols showed that the chemical reaction between NaCl and MA occurred rapidly in the time scale of 1 h and considerably in the aqueous phase, mostly during the first dehydration process, and the chemical reaction occurs more rapidly when MA is more enriched in the aerosols. For example, the reaction between NaCl and MA for aerosols generated from solutions of NaCl:MA = 2:1 and 1:2 occurred by 81% and 100% at RH = 42% and 45%, respectively, during the first dehydration process. The aerosols generated from the solution of NaCl:MA = 2:1 revealed single efflorescence and deliquescence transitions repeatedly during two hygroscopic cycles. The aerosols from NaCl:MA = 1:1 and 1:2 solutions showed just an efflorescence transition during the first dehydration process and no efflorescence and deliquescence transition during the hygroscopic cycles, respectively. The observed different hygroscopic behavior was due to the different contents of NaCl, MA, and monosodium malonate in the aerosols, which were monitored real-time by in situ RMS.

  18. 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

  19. Direct comparison of the hygroscopic properties of ammonium sulfate and sodium chloride aerosol at relative humidities approaching saturation.

    PubMed

    Walker, Jim S; Wills, Jon B; Reid, Jonathan P; Wang, Liangyu; Topping, David O; Butler, Jason R; Zhang, Yun-Hong

    2010-12-09

    Holographic optical tweezers are used to make comparative measurements of the hygroscopic properties of single component aqueous aerosol containing sodium chloride and ammonium sulfate over a range of relative humidity from 84% to 96%. The change in RH over the course of the experiment is monitored precisely using a sodium chloride probe droplet with accuracy better than ±0.09%. The measurements are used to assess the accuracy of thermodynamic treatments of the relationship between water activity and solute mass fraction with particular attention focused on the dilute solute limit approaching saturation vapor pressure. The consistency of the frequently used Clegg-Brimblecombe-Wexler (CBW) treatment for predicting the hygroscopic properties of sodium chloride and ammonium sulfate aerosol is confirmed. Measurements of the equilibrium size of ammonium sulfate aerosol are found to agree with predictions to within an uncertainty of ±0.2%. Given the accuracy of treating equilibrium composition, the inconsistencies highlighted in recent calibration measurements of critical supersaturations of sodium chloride and ammonium sulfate aerosol cannot be attributed to uncertainties associated with the thermodynamic predictions and must have an alternative origin. It is concluded that the CBW treatment can allow the critical supersaturation to be estimated for sodium chloride and ammonium sulfate aerosol with an accuracy of better than ±0.002% in RH. This corresponds to an uncertainty of ≤1% in the critical supersaturation for typical supersaturations of 0.2% and above. This supports the view that these systems can be used to accurately calibrate instruments that measure cloud condensation nuclei concentrations at selected supersaturations. These measurements represent the first study in which the equilibrium properties of two particles of chemically distinct composition have been compared simultaneously and directly alongside each other in the same environment.

  20. 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.

  1. 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.

  2. 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.

  3. Aerosol hygroscopicity in the marine atmosphere: a closure study using high-time-resolution, multiple-RH DASH-SP and size-resolved C-ToF-AMS data

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Sorooshian, A.; Murphy, S. M.; Flagan, R. C.; Seinfeld, J. H.

    2009-04-01

    We have conducted the first airborne hygroscopic growth closure study to utilize data from an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) coupled with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) measurements from the differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP). These data were collected off the coast of Central California during seven of the 16 flights carried out during the MASE-II field campaign in July 2007. Two of the seven flights were conducted in airmasses characterized by continental origin. These flights exhibited elevated organic volume fractions (VForganic=0.56±0.19, as opposed to 0.39±0.20 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92% RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for all other flights), and no measurable GF suppression at low RH (1.31±0.06 at 74%, compared with 1.31±0.07 for all other flights). Organic loadings were slightly elevated in above-cloud aerosols, as compared with below-cloud aerosols, and corresponded to a similar trend of significantly suppressed GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided good agreement with DASH-SP measurements (R2=0.78). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.22, 1.45, and 1.48 at 74, 85, and 92% RH, respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids, and correspond to a highly oxidized, presumably water-soluble, organic fraction (mission-averaged O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is VForganic, indicating

  4. CCN spectra, hygroscopicity, and droplet activation kinetics of secondary organic aerosol resulting from the 2010 Deepwater Horizon oil spill.

    PubMed

    Moore, Richard H; Raatikainen, Tomi; Langridge, Justin M; Bahreini, Roya; Brock, Charles A; Holloway, John S; Lack, Daniel A; Middlebrook, Ann M; Perring, Anne E; Schwarz, Joshua P; Spackman, J Ryan; Nenes, Athanasios

    2012-03-20

    Secondary organic aerosol (SOA) resulting from the oxidation of organic species emitted by the Deepwater Horizon oil spill were sampled during two survey flights conducted by a National Oceanic and Atmospheric Administration WP-3D aircraft in June 2010. A new technique for fast measurements of cloud condensation nuclei (CCN) supersaturation spectra called Scanning Flow CCN Analysis was deployed for the first time on an airborne platform. Retrieved CCN spectra show that most particles act as CCN above (0.3 ± 0.05)% supersaturation, which increased to (0.4 ± 0.1)% supersaturation for the most organic-rich aerosol sampled. The aerosol hygroscopicity parameter, κ, was inferred from both measurements of CCN activity and from humidified-particle light extinction, and varied from 0.05 to 0.10 within the emissions plumes. However, κ values were lower than expected from chemical composition measurements, indicating a degree of external mixing or size-dependent chemistry, which was reconciled assuming bimodal, size-dependent composition. The CCN droplet effective water uptake coefficient, γ(cond), was inferred from the data using a comprehensive instrument model, and no significant delay in droplet activation kinetics from the presence of organics was observed, despite a large fraction of hydrocarbon-like SOA present in the aerosol.

  5. Hygroscopicity and optical properties of alkylaminium sulfates.

    PubMed

    Hu, Dawei; Li, Chunlin; Chen, Hui; Chen, Jianmin; Ye, Xingnan; Li, Ling; Yang, Xin; Wang, Xinming; Mellouki, Abdelwahid; Hu, Zhongyang

    2014-01-01

    The hygroscopicity and optical properties of alkylaminium sulfates (AASs) were investigated using a hygroscopicity tandem differential mobility analyzer coupled to a cavity ring-down spectrometer and a nephelometer. AAS particles do not exhibit a deliquescence phenomenon and show a monotonic increase in diameter as the relative humidity (RH) ascends. Hygroscopic growth factors (GFs) for 40, 100 and 150 nm alkylaminium sulfate particles do not show an apparent Kelvin effect when RH is less than 45%, whereas GFs of the salt aerosols increase with initial particle size when RH is higher than 45%. Calculation using the Zdanovskii-Stokes-Robinson mixing rule suggests that hygroscopic growth of triethylaminium sulfate-ammonium sulfate mixtures is non-deliquescent, occurring at very low RH, implying that the displacement of ammonia by amine will significantly enhance the hygroscopicity of (NH4)2SO4 aerosols. In addition, light extinction of AAS particles is a combined effect of both scattering and absorption under dry conditions, but is dominated by scattering under wet conditions.

  6. 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

  7. 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.

  8. Long-term observations of cloud condensation nuclei in the Amazon rain forest - Part 1: Aerosol size distribution, hygroscopicity, and new model parametrizations for CCN prediction

    NASA Astrophysics Data System (ADS)

    Pöhlker, Mira L.; Pöhlker, Christopher; Ditas, Florian; Klimach, Thomas; Hrabe de Angelis, Isabella; Araújo, Alessandro; Brito, Joel; Carbone, Samara; Cheng, Yafang; Chi, Xuguang; Ditz, Reiner; Gunthe, Sachin S.; Kesselmeier, Jürgen; Könemann, Tobias; Lavrič, Jošt V.; Martin, Scot T.; Mikhailov, Eugene; Moran-Zuloaga, Daniel; Rose, Diana; Saturno, Jorge; Su, Hang; Thalman, Ryan; Walter, David; Wang, Jian; Wolff, Stefan; Barbosa, Henrique M. J.; Artaxo, Paulo; Andreae, Meinrat O.; Pöschl, Ulrich

    2016-12-01

    Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014-February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.

  9. 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.

  10. 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.

  11. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  13. Hygroscopic growth and deliquescence of NaCl nanoparticles mixed with surfactant SDS.

    PubMed

    Harmon, Christopher W; Grimm, Ronald L; McIntire, Theresa M; Peterson, Mark D; Njegic, Bosiljka; Angel, Vanessa M; Alshawa, Ahmad; Underwood, Joelle S; Tobias, Douglas J; Gerber, R Benny; Gordon, Mark S; Hemminger, John C; Nizkorodov, Sergey A

    2010-02-25

    Several complementary experimental and theoretical methodologies were used to explore water uptake on sodium chloride (NaCl) particles containing varying amounts of sodium dodecyl sulfate (SDS) to elucidate the interaction of water with well-defined, environmentally relevant surfaces. Experiments probed the hygroscopic growth of mixed SDS/NaCl nanoparticles that were generated by electrospraying aqueous 2 g/L solutions containing SDS and NaCl with relative NaCl/SDS weight fractions of 0, 5, 11, 23, or 50 wt/wt %. Particles with mobility-equivalent diameters of 14.0(+/-0.2) nm were size selected and their hygroscopic growth was monitored by a tandem nano-differential mobility analyzer as a function of relative humidity (RH). Nanoparticles generated from 0 and 5 wt/wt % solutions deliquesced abruptly at 79.1(+/-1.0)% RH. Both of these nanoparticle compositions had 3.1(+/-0.5) monolayers of adsorbed surface water prior to deliquescing and showed good agreement with the Brunauer-Emmett-Teller and the Frenkel-Halsey-Hill isotherms. Above the deliquescence point, the growth curves could be qualitatively described by Kohler theory after appropriately accounting for the effect of the particle shape on mobility. The SDS/NaCl nanoparticles with larger SDS fractions displayed gradual deliquescence at a RH that was significantly lower than 79.1%. All compositions of SDS/NaCl nanoparticles had monotonically suppressed mobility growth factors (GF(m)) with increasing fractions of SDS in the electrosprayed solutions. The Zdanovskii-Stokes-Robinson model was used to estimate the actual fractions of SDS and NaCl in the nanoparticles; it suggested the nanoparticles were enhanced in SDS relative to their electrospray solution concentrations. X-ray photoelectron spectroscopy (XPS), FTIR, and AFM were consistent with SDS forming first a monolayer and then a crystalline phase around the NaCl core. Molecular dynamics simulations of water vapor interacting with SDS/NaCl slabs showed that

  14. 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.

  15. 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

  16. Size-resolved respiratory-tract deposition of fine and ultrafine hydrophobic and hygroscopic aerosol particles during rest and exercise.

    PubMed

    Löndahl, Jakob; Massling, Andreas; Pagels, Joakim; Swietlicki, Erik; Vaclavik, Elvira; Loft, Steffen

    2007-02-01

    Airborne ultrafine particles (diameter <100 nm) are ubiquitous in the environment and have been associated with adverse health effects. The respiratory-tract deposition of these particles is fundamentally influenced by their hygroscopicity: their ability to grow by condensation of water in the humid respiratory system. Ambient particles are typically hygroscopic, to varying degrees. This article investigates the influence of hygroscopicity, exercise level, gender, and intersubject variability on size-dependent deposition of fine and ultrafine particles during spontaneous breathing. Using a novel and well-characterized setup, respiratory-tract deposition in the range 12-320 nm has been measured for 29 healthy adults (20 men, 9 women). Each subject completed four sessions: rest and light exercise on an ergometer bicycle while inhaling both hydrophobic (diethylhexylsebacate) and hygroscopic (NaCl) particles. The deposited fraction (DF) based on dry diameters was two to four times higher for the hydrophobic ultrafine particles than for the hygroscopic. The DF of hygroscopic ultrafine particles could be estimated by calculating their equilibrium size at 99.5% relative humidity. The differences in average DF due to exercise level and gender were essentially less than 0.03. However, the minute ventilation increased fourfold during exercise and was 18-46% higher for the men than for the women. Consequently the deposited dose of particles was fourfold higher during exercise and considerably increased for the male subjects. Some individuals consistently had a high DF in all four sessions. As an example, the results show that an average person exposed to 100-nm hydrophobic particles during exercise will receive a 16 times higher dose than a relaxed person exposed to an equal amount of hygroscopic (NaCl) particles.

  17. 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.

    2014-12-01

    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 ten 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 two-stage efflorescence transitions: 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

  18. 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

  19. 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.

  20. Cloud condensation nuclei in polluted air and biomass burning smoke: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

    Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate, but their abundance, properties and sources are highly variable and not well known. We have measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign on 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; 20-300 nm) were recorded at water vapor supersaturations (S) in the range of 0.07% to 1.27%. Depending on S, the dry CCN activation diameters were in the range of 30-200 nm, corresponding to effective hygroscopicity parameters kappa in the range of 0.1-0.5. The hygroscopicity of particles in the accumulation size range was generally higher than that of particles in the nucleation and Aitken size range. The campaign average value of kappa for all aerosol particles across the investigated size range was 0.3, which equals the average value of kappa for other continental locations. During a strong local biomass burning event, the activation diameters increased by ~10% and the average value of kappa 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, which indicates substantial proportions 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 (N_CCN,S) ranged from 1100 cm-3 at S=0.07% to 16 000 cm-3 at S=1.27%, representing ~7% to ~85% of the total aerosol particle number concentration. Based on the measurement data, we have tested different model approaches (power laws and kappa-Köhler model) for the approximation/prediction of N_CCN,S as a function of water vapor supersaturation, aerosol particle number

  1. 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

  2. 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.

  3. Influence of the external mixing state of atmospheric aerosol on derived CCN number concentrations

    NASA Astrophysics Data System (ADS)

    Wex, H.; McFiggans, G.; Henning, S.; Stratmann, F.

    2010-05-01

    We derived the range of particle hygroscopicities ($\\kappa$) that occurs in the atmosphere, based on literature data of measured hygroscopic growth or based on chemical composition. The derived $\\kappa$-values show that the atmospheric aerosol often is an external mixture with respect to hygroscopicity. Mean $\\kappa$ were derived for urban, rural, and marine aerosols for the different hygroscopic modes. Using these $\\kappa$ and exemplary particle number size distributions for the different aerosols, the number concentration of cloud condensation nuclei (NCCN) was derived for two cases, (1) accounting for the less hygroscopic fraction of particles and (2) assuming all particles to have $\\kappa$ of the more hygroscopic mode. NCCN derived from measured particle hygroscopicity is overestimated for case (2). Overestimation of NCCN is largest for fresh continental aerosol and less pronounced for marine aerosol. With $\\kappa$ derived from bulk aerosol composition data, only the hygroscopicity of more soluble aerosol particles is captured. Bulk or even size-resolved composition data will be insufficient to predict NCCN under many conditions unless independent information about particle mixing state is available.

  4. Aerosol growth in Titan's ionosphere.

    PubMed

    Lavvas, Panayotis; Yelle, Roger V; Koskinen, Tommi; Bazin, Axel; Vuitton, Véronique; Vigren, Erik; Galand, Marina; Wellbrock, Anne; Coates, Andrew J; Wahlund, Jan-Erik; Crary, Frank J; Snowden, Darci

    2013-02-19

    Photochemically produced aerosols are common among the atmospheres of our solar system and beyond. Observations and models have shown that photochemical aerosols have direct consequences on atmospheric properties as well as important astrobiological ramifications, but the mechanisms involved in their formation remain unclear. Here we show that the formation of aerosols in Titan's upper atmosphere is directly related to ion processes, and we provide a complete interpretation of observed mass spectra by the Cassini instruments from small to large masses. Because all planetary atmospheres possess ionospheres, we anticipate that the mechanisms identified here will be efficient in other environments as well, modulated by the chemical complexity of each atmosphere.

  5. 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.

  6. 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.

  7. 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.

    2008-09-01

    Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate, but their abundance, properties and sources are highly variable and not well known. We have measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign on 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; 20 300 nm) were recorded at water vapor supersaturations (S) in the range of 0.07% to 1.27%. Depending on S, the dry CCN activation diameters were in the range of 30 200 nm, corresponding to effective hygroscopicity parameters κ in the range of 0.1 0.5. The hygroscopicity of particles in the accumulation size range was generally higher than that of particles in the nucleation and Aitken size range. The campaign average value of κ for all aerosol particles across the investigated size range was 0.3, which equals the average value of κ for other continental locations. During a strong local biomass burning event, the activation diameters increased by ~10% and 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, which indicates substantial proportions 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 1100 cm-3 at S=0.07% to 16 000 cm-3 at S=1.27%, representing ~7% to ~85% of the total aerosol particle number concentration. Based on the measurement data, we have tested different model approaches (power laws and κ-Köhler model) for the approximation/prediction of NCCN,S as a function of water vapor supersaturation, aerosol particle number concentration, size

  8. 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

  9. 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...

  10. Investigations of Physicochemical Properties of Size-Resolved, Subsaturated, Atmospheric Aerosol Particles: Instrument Development, Field Measurements, and Data Analysis

    NASA Astrophysics Data System (ADS)

    Shingler, Taylor

    Aerosol particle properties and their impact on air quality, clouds, and the hydrologic cycle remain a critically important factor for the understanding of our atmosphere. Particle hygroscopic growth leads to impacts on direct and indirect radiative forcing properties, the likelihood for particles to act as cloud condensation nuclei, and aerosol-cloud interactions. Current instruments measuring hygroscopic growth have a number of limitations, lacking either the ability to measure size-resolved particles or process samples at a fast enough resolution to be suitable for airborne deployment. Advanced in-situ airborne particle retrieval and measurements of aerosol hygroscopic growth and scattering properties are analyzed and discussed. To improve the analysis of cloud nuclei particles, an updated counterflow virtual impact inlet was characterized and deployed during the 2011 E-PEACE field campaign. Theoretical and laboratory based cut size diameters were determined and validated against data collected from an airborne platform. In pursuit of higher quality aerosol particle hygroscopicity measurements, a newer instrument, the differential aerosol sizing and hygroscopicity probe (DASH-SP) has been developed in the recent past and only flown on a handful of campaigns. It has been proven to provide quality, rapid, size-resolved hygroscopic growth factor data, but was further improved into a smaller form factor making it easier for deployment on airborne platforms. It was flown during the 2013 SEAC4RS field campaign and the data was analyzed to composite air mass based hygroscopicity and refractive index (real portion only) statistics. Additionally, a comparison of bulk and size-resolved hygroscopic growth measurements was conducted. Significant findings include a potential particle size bias on bulk scattering measurements as well as a narrow range of ambient real portion of refractive index values. An investigation into the first reported ambient hygroscopicity

  11. 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

  12. Aerosol activation: parameterised versus explicit calculation for global models

    NASA Astrophysics Data System (ADS)

    Tost, H.; Pringle, K.; Metzger, S.; Lelieveld, J.

    2009-04-01

    A key process in studies of the aerosol indirect effects on clouds is the activation of particles into droplets at 100% relative humidity. To model this process in cloud, meteorological and climate models is a difficult undertaking because of the wide range of scales involved. The chemical composition of the atmospheric aerosol, originating from both air pollution and natural sources, substantially impacts the aerosol water uptake and growth due to its hygroscopicity. In this study a comparison of aerosol activation, using state-of-the-art aerosol activation parameterisations, and explicit activation due to hygroscopic growth is performed.For that purpose we apply the GMXe aerosol model - treating both dynamic and thermodynamic aerosol properties - within the EMAC (ECHAM5/MESSy Atmospheric chemistry, an atmospheric chemistry general circulation) model. This new aerosol model can explicitely calculate the water uptake of aerosols due to hygroscopicity, allowing the growth of aerosol particles into the regimes of cloud droplets in case of sufficient water vapour availability. Global model simulations using both activation schemes will be presented and compared, elucidating the advantages of each approach.

  13. 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.

  14. Hygroscopic Growth of Self-Assembled Layered Surfactant Molecules at the Interface between Air and Organic Salts

    SciTech Connect

    Shin, Yongsoon; Wang, Li Q.; Fryxell, Glen E.; Exarhos, Gregory J.; Lu, Yunfeng

    2003-12-15

    In this paper, we report a self-assembly of surfactant molecules at the interface of air/hygroscopic quaternary ammonium salts such as tetrabutylammonium acetate (TBAAc), tetrabutylammonium bromide (TBAB), and tetrabutylammonium nitrate (TBAN), where they show different hygroscopicity, TBAAc > TBAB TBAN. Homogeneously dissolved surfactants rearrange themselves when they contact air due to high moisture adsorption behavior of such organic salts. Highly ordered lamellar phases with different lattice spacings have been observed when surfactants with long alkyl chains were used. Alkylammonium halides form monolayers, while neutral alkylamines forms bilayers based upon basal spacings of their X-ray diffraction patterns. The change in basal spacings in lamellar patterns, the alkyl chain conformation of surfactants, and H-bonding property of neutral amine surfactants are discussed in detail.

  15. Relationship between CCN activation properties and oxidation level of aerosol organics observed during recent field studies

    NASA Astrophysics Data System (ADS)

    Mei, F.; Zhang, Q.; Xu, J.; Setyan, A.; Hayes, P. L.; Ortega, A. M.; Allan, J. D.; Taylor, J.; Jimenez, J.; Wang, J.

    2011-12-01

    Organic compounds are an important component of atmospheric aerosol, and can contribute upward of ~90% of total fine aerosol mass. Atmospheric aerosols often consist of hundreds of organic species, and their hygroscopicities are not well understood. This incomplete understanding limits our ability to accurately simulate aerosol cloud condensation nuclei (CCN) spectrum and therefore the aerosol indirect effects, which remain the most uncertain components in forcing of climate change over the industrial period. In this study, the hygroscopicity of aerosol organics characterized during three recent field campaigns, CalNex-LA (Pasadena, California), CARES (Cool, CA), and Aerosol lifecycle IOP (Upton, NY), is presented. Hygroscopicity of aerosol particles, which were mixtures of both inorganic and organic species, is first determined from the size-resolved activation efficiency spectrum. Based on measured aerosol chemical composition, the hygroscopicity of organics is then derived from the particle hygroscopicity by subtracting the contribution of inorganic species, whose hygroscopicities are well understood. During the three field studies, organic aerosols were characterized within a number of representative air masses, including urban plumes and those dominated by biogenic emissions. Aerosol organics measured by HR-ToF-AMS exhibit various degrees of photochemical aging, with the atomic O:C ratio ranges from ~0.35 to ~0.65. The hygroscopicity of organics is well correlated with its O:C ratio, increasing from 0.07 at the O:C ratio of 0.35 to 0.16 at the O:C ratio of 0.65. This suggests that to the first order, a simple, semi-empirical parameterization of organic aerosol hygroscopicity based on oxidation level can be developed for global models. While the measurements show that aerosol organics can substantially influence the droplet growth kinetics by modifying particle critical supersaturation, size-classified organic particles exhibit essentially identical growth

  16. Effects of seed aerosols on the growth of secondary organic aerosols from the photooxidation of toluene.

    PubMed

    Hao, Li-qing; Wang, Zhen-ya; Huang, Ming-qiang; Fang, Li; Zhang, Wei-jun

    2007-01-01

    Hydroxyl radical (.OH)-initiated photooxidation reaction of toluene was carried out in a self-made smog chamber. Four individual seed aerosols such as ammonium sulfate, ammonium nitrate, sodium silicate and calcium chloride, were introduced into the chamber to assess their influence on the growth of secondary organic aerosols (SOA). It was found that the low concentration of seed aerosols might lead to high concentration of SOA particles. Seed aerosols would promote rates of SOA formation at the start of the reaction and inhibit its formation rate with prolonging the reaction time. In the case of ca. 9000 pt/cm3 seed aerosol load, the addition of sodium silicate induced a same effect on the SOA formation as ammonium nitrate. The influence of the four individual seed aerosols on the generation of SOA decreased in the order of calcium chloride>sodium silicate and ammonium nitrate>ammonium sulfate.

  17. 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

  18. Investigation of the hygroscopic growth of self-assembled layers of N-alkyl-N-methylpyrrolidinium bromides at the interface between air and organic salt

    SciTech Connect

    Shin, Yongsoon; Baker, Gary A.; Wang, Li Q.; Exarhos, Gregory J.

    2008-04-01

    We report on the hygroscopic growth of self-assembled lamellae, composed of N-alkyl-N-methylpyrrolidinium bromide (CnMPB; n = 10, 12, 14, 16, 18) surfactant molecules, spontaneously formed at the interface between ambient air and the low-melting organic salt tetrabutylammonium acetate (TBAAc). The organization process to form well-defined hygroscopic bilayer patterns at the air/TBAAc interface was investigated using a combination of time-dependent X-ray diffraction (XRD) and carbon-13 cross-polarization magic angle spinning nuclear magnetic resonance (13C CP/MAS NMR) spectroscopy. CnMPB surfactants containing the highest alkyl chain lengths studied (n = 16, 18) formed highly ordered, fully-interdigitated bilayer patterns with an all-trans conformation of interior methylene carbons. In contrast, CnMPB surfactants with shorter alkane chains (n = 10, 12, 14) in this series formed less-ordered bilayer arrangements with mixed trans/gauche aliphatic character. The lamellar patterns became increasingly ordered with longer exposure to humid air at the air/salt interface.

  19. 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

  20. Simultaneous Measurements of Individual Ambient Particles Size, Composition, Effective Density, and Hygroscopicity

    SciTech Connect

    Zelenyuk, Alla; Imre, Dan G.; Han, J.; Oatis, Susan

    2008-03-01

    The interaction between atmospheric particles and water vapor impacts directly and significantly the effect that these particles exert on the atmosphere. The hygroscopicity of individual particles, which is a quantitative measure of their response to changes in relative humidity, is related to their internal compositions. To properly include atmospheric aerosols in any model requires knowledge of the relationship between particle size, composition and hygroscopicity. Here we demonstrate the capability to conduct in real-time the simultaneous measurements of individual ambient particle hygroscopic growth factors, densities and compositions using a hydrated tandem differential mobility analyzer that is coupled to an ultra-sensitive single particle mass spectrometer. We use as an example the class of particles that are composed of sulfate mixed with oxygenated organics to illustrate how such multidimensional single particle characterization can be used to yield quantitative information about the composition of individual particles. We show that the data provide the relative concentrations of organics and sulfates, the density of the two fractions and particle hygroscopicity.

  1. 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.

  2. Experimental and theoretical investigation of nucleation and growth of atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Zhao, Jun

    Aerosol particles have profound impacts on human health, atmospheric radiation, and cloud microphysics and these impacts are strongly dependent on particle sizes. However, formation and growth of atmospheric particles are currently not well understood. In this work, laboratory and theoretical studies have been performed to investigate the formation and growth of atmospheric particles. The first two parts of the dissertation are a laboratory investigation of new particle formation and growth, and a theoretical study of atmospheric molecular complexes and clusters. The nucleation rate was considerably enhanced in the presence of cis-pinonic acid and ammonia. The composition of the critical cluster was estimated from the dependence of the nucleation rate on the precursor concentration and the time evolution of the clusters was then simulated using molecular dynamic simulations. Results from quantum chemical calculations and quantum theory of atoms in molecules (QTAIM) reveal that formation of strong hydrogen bonding between an organic acid and sulfuric acid is likely responsible for a reduction of the nucleation barrier by modifying the hydrophobic properties of the organic acid and allowing further addition of hydrophilic species (e.g., H2SO4, H2O, and possibly NH 3) to the hydrophilic side of the clusters. This promotes growth of the nascent cluster to overcome the nucleation barrier and thus enhances the nucleation in the atmosphere. The last part of this dissertation is the laboratory investigation of heterogeneous interactions of atmospheric carbonyls with sulfuric acid. Direct measurement has been performed to investigate the heterogeneous uptake of atmospheric carbonyls on sulfuric acid. Important parameters have been obtained from the time-dependent or time-independent uptake profiles. The results indicated that the acid-catalyzed reactions of larger aldehydes (e.g. octanal and 2, 4-hexadienal) in sulfuric acid solution were attributed to aldol condensation in

  3. Aerosol growth in Titan’s ionosphere

    PubMed Central

    Lavvas, Panayotis; Yelle, Roger V.; Koskinen, Tommi; Bazin, Axel; Vuitton, Véronique; Vigren, Erik; Galand, Marina; Wellbrock, Anne; Coates, Andrew J.; Wahlund, Jan-Erik; Crary, Frank J.; Snowden, Darci

    2013-01-01

    Photochemically produced aerosols are common among the atmospheres of our solar system and beyond. Observations and models have shown that photochemical aerosols have direct consequences on atmospheric properties as well as important astrobiological ramifications, but the mechanisms involved in their formation remain unclear. Here we show that the formation of aerosols in Titan’s upper atmosphere is directly related to ion processes, and we provide a complete interpretation of observed mass spectra by the Cassini instruments from small to large masses. Because all planetary atmospheres possess ionospheres, we anticipate that the mechanisms identified here will be efficient in other environments as well, modulated by the chemical complexity of each atmosphere. PMID:23382231

  4. 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.

  5. Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles

    NASA Astrophysics Data System (ADS)

    Meyer, N. K.; Duplissy, J.; Gysel, M.; Metzger, A.; Dommen, J.; Weingartner, E.; Alfarra, M. R.; Prevot, A. S. H.; Fletcher, C.; Good, N.; McFiggans, G.; Jonsson, Â. M.; Hallquist, M.; Baltensperger, U.; Ristovski, Z. D.

    2009-01-01

    The volatile and hygroscopic properties of ammonium sulphate seeded and unseeded secondary organic aerosol (SOA) derived from the photo-oxidation of atmospherically relevant concentrations of α-pinene were studied. The seed particles were electrospray generated ammonium sulphate ((NH4)2SO4) having diameters of approximately 33 nm with a quasi-mono-disperse size distribution (geometric standard deviation σg=1.3). The volatile and hygroscopic properties of both seeded and unseeded SOA were simultaneously measured with a VH-TDMA (volatility - hygroscopicity tandem differential mobility analyzer). VH-TDMA measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF) factor for increased volatilisation temperatures such that the more volatile compounds appear to be more hygroscopic. This is opposite to the expected preferential evaporation of more volatile but less hygroscopic material, but could also be due to enhanced oligomerisation occurring at the higher temperature in the thermodenuder. In addition, HGF measurements of seeded SOA were measured as a function of time at two relative humidities, below (RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH) of the pure ammonium sulphate seeds. As these measurements were conducted during the onset phase of photo-oxidation, during particle growth, they enabled us to find the dependence of the HGF as a function of the volume fraction of the SOA coating. HGF's measured at RH of 85% showed a continuous decrease as the SOA coating thickness increased. The measured growth factors show good agreements with ZSR predictions indicating that, at these RH values, there are only minor solute-solute interactions. At 75% RH, as the SOA fraction increased, a rapid increase in the HGF was observed indicating that an increasing fraction of the (NH4)2SO4 is subject to a phase transition, going into solution, with an increasing volume fraction of SOA. To our knowledge this is the first time that SOA derived

  6. Plume Mechanics and Aerosol Growth Processes.

    DTIC Science & Technology

    1987-07-01

    UNIT ELEMENT NO. NO NO ACCESSION NO %. Aberdeen Proving Ground, MD 21010-5423 II 11 TITLE (include Security Classification) Plume Mechanics and...formulation and a finite element sc hem e ......... ..................... 192 c. Diffusion of aerosols in laminar flow in a cylindrical tube...The principal elements are the liquid oil and carrier gas metering systems, the oil vaporizer, coaxial jet system, and the sampling and aerosol

  7. Formation and growth of photochemical aerosols in Titan's atmosphere

    NASA Astrophysics Data System (ADS)

    Cabane, M.; Chassefiere, E.; Israel, Guy

    1992-04-01

    Recent development in the understanding of the morphology of haze aerosols in Titan's atmosphere, aggregate particles, and their associated optical properties are considered in the flight of a microphysical model of aerosols. Two different phases of the formation process are identified: initial growth of aerosols near the formation altitude by accretion of very small elementary particles; and (2) settling during which particles of about the same size stock together, leading to the formation of aggregates which contain some tens to several hundred monomers. The first phase leads to the formation of nearly spherical 'monomers' (radius approximately equal to 0.05 micrometers). An eulerian microphysical model is used. It is shown that the monomer radius is extremely sensitive to the altitude where aerosols are created. The formation altitude of aerosols is found to lie in the range from 350 to 400 km.

  8. The utilization of physisorption analyzer for studying the hygroscopic properties of atmospheric relevant particles.

    PubMed

    Ma, Qingxin; Liu, Yongchun; He, Hong

    2010-04-01

    The hygroscopic behavior of atmospheric aerosols has a significant effect on the global climate change. In this study, a physisorption analyzer was used to measure the water adsorption capacity of Al(2)O(3), NaCl, NH(4)NO(3), and (NH(4))(2)SO(4) particles at 273.6 K. Qualitative and quantitative information about water adsorption on these particles was obtained with changing the temperature and/or relative humidity (RH). Uptake of water on Al(2)O(3) showed a type-II BET adsorption isotherm with the monolayer formed at approximately 18% relative humidity (RH). The hygroscopic properties of NaCl, (NH(4))(2)SO(4), and NH(4)NO(3), including the deliquescence relative humidities (DRH), the temperature dependence of the DRH for NH(4)NO(3), and the growth factors of NaCl and (NH(4))(2)SO(4) were determined. All these results were in good agreement with the results obtained by other methods and/or theoretical prediction with a deviation less than 2%. For NaCl, the water adsorption amount increase rate exhibits three stages (<30% RH, approximately 30%-65% RH, and >65% RH) in the predeliquescence process and monolayer thin film water was formed at about 30% RH. It demonstrated that this instrument was practicable for studying the hygroscopic behavior of both soluble and insoluble but wettable atmospheric nonviolate aerosol particles.

  9. Hygroscopic Growth of Self-Assembled Layered Surfactant Molecules at the Interface between Air and Organic Salts

    SciTech Connect

    Shin, Yongsoon; Wang, Li Q.; Fryxell, Glen E.; Exarhos, Gregory J.

    2005-04-01

    We report here a self-assembly of surfactant molecules at the interface of air/hygroscopic quaternary ammonium salts, tetrabutylammonium acetate (TBAAc). Homogeneously dissolved surfactant molecules at 100 C self-assemble upon contacting air due to high moisture adsorption behavior of the organic salt when cooling down. Highly ordered lamellar phases with different lattice spacings have been observed when surfactants with various lengths of alkyl chains were used. CnTMAB/TBAAc systems showed all trans conformation of interior methylene carbons and interdigited bilayers with an average CH2 increment of 0.119nm, while CnNH2/TBAAc systems showed trans/gauche mixed conformations of interior methylene carbons and bilayers with an average CH2 increment of 0.247nm. CnNH2s in CnNH2/TBAAc formed bilayers through water-mediated intermolecular hydrogen bonds with a water layer thickness of 0.51-0.61nm. In CnTAB/TBAAc, as the head group of CnTAB is bigger, the interdigited bilayer thickness (d-spacing) is smaller because their bigger head groups accommodate enough space for alkyl tails to come in between them.

  10. Caribbean coral growth influenced by anthropogenic aerosol emissions

    NASA Astrophysics Data System (ADS)

    Kwiatkowski, Lester; Cox, Peter M.; Economou, Theo; Halloran, Paul R.; Mumby, Peter J.; Booth, Ben B. B.; Carilli, Jessica; Guzman, Hector M.

    2013-05-01

    Coral growth rates are highly dependent on environmental variables such as sea surface temperature and solar irradiance. Multi-decadal variability in coral growth rates has been documented throughout the Caribbean over the past 150-200 years, and linked to variations in Atlantic sea surface temperatures. Multi-decadal variability in sea surface temperatures in the North Atlantic, in turn, has been linked to volcanic and anthropogenic aerosol forcing. Here, we examine the drivers of changes in coral growth rates in the western Caribbean between 1880 and 2000, using previously published coral growth chronologies from two sites in the region, and a numerical model. Changes in coral growth rates over this period coincided with variations in sea surface temperature and incoming short-wave radiation. Our model simulations show that variations in the concentration of anthropogenic aerosols caused variations in sea surface temperature and incoming radiation in the second half of the twentieth century. Before this, variations in volcanic aerosols may have played a more important role. With the exception of extreme mass bleaching events, we suggest that neither climate change from greenhouse-gas emissions nor ocean acidification is necessarily the driver of multi-decadal variations in growth rates at some Caribbean locations. Rather, the cause may be regional climate change due to volcanic and anthropogenic aerosol emissions.

  11. Nucleation and Growth of Stratospheric Aerosols

    DTIC Science & Technology

    1981-01-01

    phase constituents can be removed from partici- pating in further homogeneous reaction mechanisms. Furthermore, although no definitive evidence currently...during periods of large volcanic eruptions sulfate aerosol is generated by an in situ oxidation mechanism rather than by simple input of tephra from the...reach a peak concentration. Tephra are known to settle out relatively rapidly, and it must be concluded that this increase in sulfate concentration is

  12. Transformation from hydrophobic to hygroscopic diesel soot particles by photochemical aging

    NASA Astrophysics Data System (ADS)

    Tritscher, T.; Juranyi, Z.; Martin, M.; Chirico, R.; Heringa, M.; Gysel, M.; Sierau, B.; Decarlo, P. F.; Dommen, J.; Prevot, A. S.; Weingartner, E.; Baltensperger, U.

    2010-12-01

    Combustion emissions are a complex mixture of black carbon (BC), organics, and other compounds in the gas and particle phase. In global climate modeling BC is categorized in hydrophobic and hydrophilic, but the fraction of particles in each category is quite difficult to quantify. A particle is called hydrophobic, if it is non-wettable and therefore cannot act as cloud condensation nuclei (CCN). Hydrophilic particles are hygroscopic, if they can take up water at elevated RH. The hygroscopicity and the CCN activation of diesel exhaust particles were measured during experiments at the PSI smog chamber with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) at 95% relative humidity (RH), which measures diameter growth factors (GF), the ratio of the wet (d(RH)) and the dry diameter (d0), and with a Cloud Condensation Nuclei Counter (CCNC) at RH > 100%. Diesel exhaust from different passenger cars was introduced via heated injection system into the chamber. Fresh soot (BC and primary organic aerosol (POA)) is known to form nm-size fractal aggregates. These primary soot particles were coated with secondary organic aerosol (SOA) mass after lights were turned on. The figure conceptually illustrates the observed findings. Fresh soot particles are hydrophobic as they do not activate as cloud droplets even at high supersaturations like non-hygroscopic but wettable particles do. SOA coating appears on the soot aggregates after photochemical aging was started. Slightly aged particles were found to be CCN-active and thus they are hydrophilic. However, the GF of the H-TDMA was <1, indicating a shrinking of these particles. This restructuring was confirmed with a pre-humidifier, which makes the particles compact and less fractal in front of the H-TDMA. Continued aging of diesel exhaust leads to CCN-active particles with a GF >1, indicating the hygroscopicity of these particles. Our measurements show that photochemical aging with SOA formation can change a hydrophobic

  13. Atmospheric pressure flow reactor / aerosol mass spectrometer studies of tropospheric aerosol nucleat and growth kinetics. Final report, June, 2001

    SciTech Connect

    Worsnop, Douglas R.

    2001-06-01

    The objective of this program was to determine the mechanisms and rates of growth and transformation and growth processes that control secondary aerosol particles in both the clear and polluted troposphere. The experimental plan coupled an aerosol mass spectrometer (AMS) with a chemical ionization mass spectrometer to provide simultaneous measurement of condensed and particle phases. The first task investigated the kinetics of tropospheric particle growth and transformation by measuring vapor accretion to particles (uptake coefficients, including mass accommodation coefficients and heterogeneous reaction rate coefficients). Other work initiated investigation of aerosol nucleation processes by monitoring the appearance of submicron particles with the AMS as a function of precursor gas concentrations. Three projects were investigated during the program: (1) Ozonolysis of oleic acid aerosols as model of chemical reactivity of secondary organic aerosol; (2) Activation of soot particles by measurement deliquescence in the presence of sulfuric acid and water vapor; (3) Controlled nucleation and growth of sulfuric acid aerosols.

  14. Modeling global organic aerosol formation and growth

    NASA Astrophysics Data System (ADS)

    Tsimpidi, Alexandra; Karydis, Vlasios; Pandis, Spyros; Lelieveld, Jos

    2014-05-01

    A computationally efficient framework for the description of organic aerosol (OA)-gas partitioning and chemical aging has been developed and implemented into the EMAC atmospheric chemistry-climate model. This model simulates the formation of primary (POA) and secondary organic aerosols (SOA) from semi-volatile (SVOC), intermediate-volatile (IVOC) and volatile organic compounds (VOC). POA are divided in two groups with saturation concentrations at 298 K 0.1, 10, 1000, 100000 µg m-3: OA from fossil fuel combustion and biomass burning. The first 2 surrogate species from each group represent the SVOC while the other surrogate species represent the IVOC. Photochemical reactions that change the volatility of the organics in the gas phase are taken into account. The oxidation products from each group of precursors (SVOC, IVOC, and VOC) are lumped into an additional set of oxidized surrogate species (S-SOA, I-SOA, and V-SOA, respectively) in order to track their source of origin. This model is used to i) estimate the relative contributions of SOA and POA to total OA, ii) determine how SOA concentrations are affected by biogenic and anthropogenic emissions, and iii) evaluate the effect of photochemical aging and long-range transport on OA budget over specific regions.

  15. Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and un-seeded SOA particles

    NASA Astrophysics Data System (ADS)

    Meyer, N. K.; Duplissy, J.; Gysel, M.; Metzger, A.; Dommen, J.; Weingartner, E.; Alfarra, M. R.; Fletcher, C.; Good, N.; McFiggans, G.; Jonsson, Ã. M.; Hallquist, M.; Baltensperger, U.; Ristovski, Z. D.

    2008-05-01

    The volatile and hygroscopic properties of ammonium sulphate seeded and un-seeded secondary organic aerosol (SOA) derived from the photo-oxidation of atmospherically relevant concentrations of α-pinene were studied. The seed particles were electrospray generated ammonium sulphate ((NH4)2SO4) having diameters of approximately 33 nm with a quasi-mono-disperse size distribution (geometric standard deviation σg=1.3). The volatile and hygroscopic properties of both seeded and unseeded SOA were simultaneously measured with a VH-TDMA (volatility - hygroscopicity tandem differential mobility analyzer). VH-TDMA measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF) factor for increased volatilisation temperatures such that the more volatile compounds appear to be more hygroscopic. This is opposite to the expected preferential evaporation of more volatile but less hygroscopic material, but could also be due to enhanced oligomerisation occurring at the higher temperature in the thermodenuder. In addition, HGF measurements of seeded SOA were measured as a function of time at two relative humidities, below (RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH) of the pure ammonium sulphate seeds. As these measurements were conducted during the onset phase of photo-oxidation, during particle growth, they enabled us to find the dependence of the HGF as a function of the volume fraction of the SOA coating. HGF's measured at RH of 85% showed a continuous decrease as the SOA coating thickness increased. The measured growth factors show good agreements with ZSR predictions indicating that, at these RH values, there are only minor solute-solute interactions. At 75% RH, as the SOA fraction increased, a rapid increase in the HGF was observed indicating that an increasing fraction of the (NH4)2SO4 is subject to a phase transition, going into solution, with an increasing volume fraction of SOA. To our knowledge this is the first time that SOA derived

  16. Timescale for hygroscopic conversion of calcite mineral particles through heterogeneous reaction with nitric acid.

    PubMed

    Sullivan, Ryan C; Moore, Meagan J K; Petters, Markus D; Kreidenweis, Sonia M; Roberts, Greg C; Prather, Kimberly A

    2009-09-28

    Atmospheric heterogeneous reactions can potentially change the hygroscopicity of atmospheric aerosols as they undergo chemical aging processes in the atmosphere. A particle's hygroscopicity influences its cloud condensation nuclei (CCN) properties with potential impacts on cloud formation and climate. In this study, size-selected calcite mineral particles were reacted with controlled amounts of nitric acid vapour over a wide range of relative humidities in an aerosol flow tube to study the conversion of insoluble and thus apparently non-hygroscopic calcium carbonate into soluble and hygroscopic calcium nitrate. The rate of hygroscopic change particles undergo during a heterogeneous reaction is derived from experimental measurements for the first time. The chemistry of the reacted particles was determined using an ultrafine aerosol time-of-flight mass spectrometer (UF-ATOFMS) while the particles' hygroscopicity was determined through measuring CCN activation curves fit to a single parameter of hygroscopicity, kappa. The reaction is rapid, corresponding to atmospheric timescales of hours. At low to moderate HNO3 exposures, the increase in the hygroscopicity of the particles is a linear function of the HNO3(g) exposure. The experimentally observed conversion rate was used to constrain a simple but accurate kinetic model. This model predicts that calcite particles will be rapidly converted into hygroscopic particles (kappa>0.1) within 4 h for low HNO3 mixing ratios (10 pptv) and in less than 3 min for 1000 pptv HNO3. This suggests that the hygroscopic conversion of the calcite component of atmospheric mineral dust aerosol will be controlled by the availability of nitric acid and similar reactants, and not by the atmospheric residence time.

  17. 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

  18. Aerosol-induced mechanisms for cumulus congestus growth

    NASA Astrophysics Data System (ADS)

    Sheffield, Amanda M.; Saleeby, Stephen M.; Heever, Susan C.

    2015-09-01

    Tropical convection has been observed to contain three cloud modes, the middle of which is cumulus congestus clouds. Congestus clouds act to moisten the tropical atmosphere, may be mixed-phase, and on occasion surpass the freezing level inversion from where they may develop into deeper convection. This study investigates the impacts of enhanced aerosol concentrations on the growth of congestus clouds produced in idealized cloud-resolving model simulations run under a state of radiative convective equilibrium (RCE). High-resolution, long-duration simulations were completed using the Regional Atmospheric Modeling System (RAMS). Aerosol concentrations between 2 and 4 km above ground level were varied from clean to polluted conditions in order to represent the advection of Saharan dust over the Atlantic Ocean. The congestus populations within each aerosol simulation are statistically analyzed using 10 days of model output after the simulation reaches RCE. Results indicate that congestus in more polluted conditions produce greater amounts of cloud water and ice mass, enhanced updraft strengths, and an increase in the number of congestus cloud tops that extend above the freezing level. Enhanced vapor depositional growth on the populations of more numerous, smaller cloud droplets in the polluted conditions, and the subsequent increase in latent heat release in the warm phase regions of the cloud, is found to be important factors in convective invigoration of these cloud systems. Aerosol feedbacks associated with cold pools and condensate loading also influence the updraft strength and act in opposition to the warm phase invigoration processes.

  19. Aerosol growth in Titan's ionosphere through particle charging

    NASA Astrophysics Data System (ADS)

    Lavvas, P.; Yelle, R. V.; Koskinen, T.; Bazin, A.; Vuitton, V.; Vigren, E.; Galand, M. F.; Wellbrock, A.; Coates, A. J.; Wahlund, J.; Crary, F.; Snowden, D. S.

    2012-12-01

    Observations of Titan's lower thermosphere and ionosphere by Cassini instruments demonstrate the presence of large mass negative ions of a few thousand amu, and the presence of positive ions up to a few hundred amu [1,2]. The mechanisms though responsible for the production of these large ions have so far remained elusive. A recent Titan flyby that probed deeper layers of Titan's thermosphere than usual, revealed a discrepancy in the observed positive ion and electron density, with the electron density lower than the abundance required to satisfy charge balance [3]. The remaining electron density was found in the form of the large mass negative ions. Aerosols can be charged on interaction with electrons and ions, while this charge can affect the particle coagulation, thus, their subsequent growth. Given the above observations we investigate here the potential role of aerosols in Titan's ionosphere and how this interaction affects the aerosol evolution. This investigation is performed with the use of a model that couples between the ionospheric photochemical evolution and the microphysical growth of aerosols in a self-consistent approach. Our results show that particle charging has an important role in the ionosphere. Most of the produced particles in the ionosphere attain a negative charge. Thus, they act as a sink for the free electrons with the remaining free electron densities consistent with the recent Cassini observations. Being negatively charged, the particles repel each other reducing in this way the coagulation rates and the growth of the aerosols. On the other hand, the negatively charged particles attract the abundant positive ions, which results to enhanced collisions between them. The mass added to the particles by the ions leads to an increase in their size and an increase in the resulting mass flux of the aerosols. Our simulated mass per charge spectra provide excellent fits to the observed positive and negative ion spectra from the Cassini Plasma

  20. Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

    NASA Astrophysics Data System (ADS)

    Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

    2016-10-01

    Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

  1. Final Report "Nucleation and Growth of Atmospheric Aerosols" DOE Grant No. DE-FG02-98ER62556

    SciTech Connect

    McMurry, Peter H.; Eisele, Fred L.

    2005-06-02

    Research that was supported by this contract has contributed substantially to progress in our understanding of new particle formation in the atmosphere. Objectives included the development of new measurement methods, the application of those new instrument systems in atmospheric field studies, and the interpretation of results from those studies. We developed the "Nano TDMA" to measure the hygroscopicity and volatility of 4-20 nm particles. We used this instrument system to characterize properties of atmospheric particles in the Atlanta atmosphere in July/August 2002 as well as to study properties of diesel exhaust particles. We also developed the thermal desorption chemical ionization mass spectrometer (TDCIMS) to measure the chemical composition of nanoparticles as small as 7 nm with a time resolution of 10-20 minutes. The TDCIMS is currently the only instrument that can perform such measurements. Atmospheric field measurements were carried out in Atlanta (July/August 2002; we refer to this as the ANARChE study) and in Boulder, CO (2003/04). In the ANARChE study we measured, for the first time, the composition of freshly nucleated particles as small as 7 nm using the TDCIMS. The ANARChE study also included the first nano-TDMA measurements of the volatility and hygroscopicity of freshly nucleated particles as small as 4 nm. Other parameters that were measured included particle size distributions (3 nm-2 µm), and sulfuric acid and ammonia concentrations. Key discoveries from the ANARChE study are: (1) freshly nucleated particles in Atlanta consist primarily of ammonium and sulfate; evidence for significant amounts of other species such as organics and nitrates was not found; (2) new particle formation occurs when rates of cluster loss to preexisting particles are small compared to rates of lost to the next larger cluster size by growth; a dimensionless parameter L describes the ratio of these rates, and measurements showed that new particle formation was always

  2. 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

  3. Aerosol-Cloud-Radiation Interactions in Atmospheric Forecast Models

    DTIC Science & Technology

    2008-09-30

    succinic and adipic acids show no growth. Airborne measurements of hygroscopic growth factors of ship exhaust aerosol during the 2007 Marine Stratus...presented for several organic acids . Oxalic, malonic, glutaric, and glyoxylic acids grow gradually with increasing relative humidity up to 94%, while...respectively. These values agree with previously reported values for water-soluble organics such as dicarboxylic and multifunctional acids , and correspond

  4. Organic Aerosol Nucleation and Growth at the CERN CLOUD chamber

    NASA Astrophysics Data System (ADS)

    Tröstl, Jasmin; Lethipalo, Katrianne; Bianchi, Federico; Sipilä, Mikko; Nieminen, Tuomo; Wagner, Robert; Frege, Carla; Simon, Mario; Weingartner, Ernest; Gysel, Martin; Dommen, Josef; Baltensperger, Urs

    2014-05-01

    It is well known that atmospheric aerosols influence the climate by changing Earth's radiation balance (IPCC 2007 and 2013). Recent models have shown (Merikanto et al. 2009) that aerosol nucleation is one of the biggest sources of low level cloud condensation nuclei. Still, aerosol nucleation and growth are not fully understood. The driving force of nucleation and growth is sulfuric acid. However ambient nucleation and growth rates cannot be explained by solely sulfuric acid as precursor. Recent studies have shown that only traces of precursors like ammonia and dimethylamine enhance the nucleation rates dramatically (Kirkby et al. 2011, Almeida et al., 2013). Thus the role of different aerosol precursor needs to be studied not only in ambient but also in very well controlled chamber experiments. The CLOUD (Cosmics Leaving OUtdoor Droplets) experiment enables conducting experiments very close to atmospheric conditions and with a very low contaminant background. The latest CLOUD experiments focus on the role of organics in aerosol nucleation and growth. For this purpose, numerous experiments with alpha-pinene have been conducted at the CERN CLOUD chamber. Several state-of-the-art instruments were used to cover the whole complexity of the experiment. Chamber conditions were set to 40% relative humidity and 5° C. Atmospheric concentrations of SO2, O3, HONO, H2O and alpha-pinene were injected to the chamber. Different oxidation conditions were used, yielding different levels of oxidized organics: (1) OH radicals, (2) Ozone with the OH scavenger H2 (pure ozonolysis) and (3) both. SO2 was injected to allow for sulfuric acid production. Optical UV fibers were used to enable photochemical reactions. A high field cage (30 kV) can be turned on to remove all charged particles in the chamber to enable completely neutral conditions. Comparing neutral conditions to the beam conditions using CERN's proton synchrotron, the fraction of ion-induced nucleation can be studied. Using

  5. AN ASSESSMENT OF HYGROSCOPIC GROWTH FACTORS FOR AEROSOLS IN THE SURFACE BOUNDARY LAYER FOR COMPUTING DIRECT RADIATIVE FORCING. (R825248)

    EPA Science Inventory

    The perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Concl...

  6. 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.

  7. Temporal Variation of Aerosol Properties at a Rural Continental Site and Study of Aerosol Evolution through Growth Law Analysis

    NASA Technical Reports Server (NTRS)

    Wang, Jian; Collins, Don; Covert, David; Elleman, Robert; Ferrare, Richard A.; Gasparini, Roberto; Jonsson, Haflidi; Ogren, John; Sheridan, Patrick; Tsay, Si-Chee

    2006-01-01

    Aerosol size distributions were measured by a Scanning Mobility Particle Sizer (SMPS) onboard the CIRPAS Twin Otter aircraft during 16 flights at the Southern Great Plains (SGP) site in northern central Oklahoma as part of the Aerosol Intensive Operation period in May, 2003. During the same period a second SMPS was deployed at a surface station and provided continuous measurements. Combined with trace gas measurements at the SGP site and back-trajectory analysis, the aerosol size distributions provided insights into the sources of aerosols observed at the SGP site. High particle concentrations, observed mostly during daytime, were well correlated with the sulfur dioxide (SO2) mixing ratios, suggesting nucleation involving sulfuric acid is likely the main source of newly formed particles at the SGP. Aerosols within plumes originating from wildfires in Central America were measured at the surface site. Vertically compact aerosol layers, which can be traced back to forest fires in East Asia, were intercepted at altitudes over 3000 meters. Analyses of size dependent particle growth rates for four periods during which high cloud coverage was observed indicate growth dominated by volume controlled reactions. Sulfate accounts for 50% to 72% of the increase in aerosol volume concentration; the rest of the volume concentration increase was likely due to secondary organic species. The growth law analyses and meteorological conditions indicate that the sulfate was produced mainly through aqueous oxidation of SO2 in clouds droplets and hydrated aerosol particles.

  8. Nucleation and growth processes of atmospheric aerosols and clouds

    SciTech Connect

    Schwartz, S.E.; McGraw, R.L.

    1995-11-01

    This project seeks to gain enhanced understanding of the rate of formation and growth of new particles and of cloud droplets as a function of pertinent controlling atmospheric variables, thereby permitting accurate representation of these processes in climate models. Aerosol size distributions are shaped by complex nucleation and growth and mixing processes that are difficult to represent in models, due to the need to accurately represent the evaporation/growth kinetics for each of the billions of discrete cluster sizes in the growth sequence, ranging from molecular clusters to particles of radius of several tenths of a micrometer or greater. A potentially very powerful means of solving this problem may be given by the method of moments (MOM), which tracks the time dependence of just the lower-order radial moments of the size distribution without requiring knowledge of the distribution itself.

  9. Estimating aerosol light-scattering enhancement from dry aerosol optical properties at different sites

    NASA Astrophysics Data System (ADS)

    Titos, Gloria; Jefferson, Anne; Sheridan, Patrick; Andrews, Elisabeth; Lyamani, Hassan; Ogren, John; Alados-Arboledas, Lucas

    2014-05-01

    Microphysical and optical properties of aerosol particles are strongly dependent on the relative humidity (RH). 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. The scattering enhancement factor, f(RH), is defined as the ratio of the scattering coefficient at a high and reference RH. 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 explore the relationship between aerosol light-scattering enhancement and dry aerosol optical properties such as the single scattering albedo (SSA) and the scattering Ångström exponent (SAE) at multiple sites around the world. The measurements used in this study were conducted by the US Department of Energy at sites where different aerosol types predominate (pristine marine, polluted marine, dust dominated, agricultural and forest environments, among others). In all cases, the scattering enhancement decreases as the SSA decreases, that is, as the contribution of absorbing particles increases. On the other hand, for marine influenced environments the scattering enhancement clearly increases as the contribution of coarse particles increases (SAE decreases), evidence of the influence of hygroscopic coarse sea salt particles. For other aerosol types the relationship between f(RH) and SAE is not so straightforward. Combining all datasets, f(RH) was found to exponentially increase with SSA with a high correlation coefficient.

  10. Water absorption by secondary organic aerosol and its effect on inorganic aerosol behavior

    SciTech Connect

    Ansari, A.S.; Pandis, S.N.

    2000-01-01

    The hygroscopic nature of atmospheric aerosol has generally been associated with its inorganic fraction. In this study, a group contribution method is used to predict the water absorption of secondary organic aerosol (SOA). Compared against growth measurements of mixed inorganic-organic particles, this method appears to provide a first-order approximation in predicting SOA water absorption. The growth of common SOA species is predicted to be significantly less than common atmospheric inorganic salts such as (NH{sub 4}){sub 2}SO{sub 4} and NaCl. Using this group contribution method as a tool in predicting SOA water absorption, an integrated modeling approach is developed combining available SOA and inorganic aerosol models to predict overall aerosol behavior. The effect of SOA on water absorption and nitrate partitioning between the gas and aerosol phases is determined. On average, it appears that SOA accounts for approximately 7% of total aerosol water and increases aerosol nitrate concentrations by approximately 10%. At high relative humidity and low SOA mass fractions, the role of SOA in nitrate partitioning and its contribution to total aerosol water is negligible. However, the water absorption of SOA appears to be less sensitive to changes in relative humidity than that of inorganic species, and thus at low relative humidity and high SOA mass fraction concentrations, SOA is predicted to account for approximately 20% of total aerosol water and a 50% increase in aerosol nitrate concentrations. These findings could improve the results of modeling studies where aerosol nitrate has often been underpredicted.

  11. 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.

  12. Simultaneous Measurement of Size, Composition, Hygroscopicity, and Density of Single Ambient Particles

    NASA Astrophysics Data System (ADS)

    Zelenyuk, A.; Imre, D. G.; Han, J.; Oatis, S.

    2003-12-01

    The holly grail in aerosol climate interaction is a roadmap that takes one from emissions of aerosol and aerosol precursors through aerosol transformations, to optical and cloud effects and finally to climate impacts. A critical element on this path must be the behavior of aerosol as a function of atmospheric relative humidity, which in turn requires an understanding of the correlation between aerosol composition and hygroscopicity. For single component particles this problem is tractable and reasonably understood. But, the vast majority of particles in the real atmosphere are internal mixtures of hygroscopic salts, organic acids and or bases, long chain hydrocarbons, soot, mineral dust and the list go on. Hundreds of organic compounds with highly varying hygroscopicities can be found in single particles. It would be unrealistic to expect global climate models to include and track each of these compounds. A similar problem faces the experimental world, where measuring the size, detailed molecular composition and hygroscopicity of individual particles although, in principle possible, is impractical. Single particle mass spectroscopy can be used to classify particles as organics mixed with sulfate, for example. Or in some cases pinpoint the class of some of the organics found in the mixture. But it cannot yield a quantitative measure of relative amounts. In an attempt to address this issue we have developed the method to measure simultaneously hygroscopicity, size, and composition of individual ambient particles. However, the data from Long Island NY, where the vast majority of particles were internally mixed sulfate with organics, the correlation between composition and hygroscopicity was rather weak. This is due to the fact that single-laser single particle mass spectra cannot quantitatively measure the ratio of organics to sulfates. In contrast, we found a very clear correlation between hygroscopicity and particle density for a given class of particles. In this

  13. Influences of relative humidity on aerosol optical properties and aerosol radiative forcing during ACE-Asia

    NASA Astrophysics Data System (ADS)

    Yoon, Soon-Chang; Kim, Jiyoung

    In situ measurements at Gosan, South Korea, and onboard C-130 aircraft during ACE-Asia were analyzed to investigate the influence of relative humidity (RH) on aerosol optical properties and radiative forcing. The temporal variation of aerosol chemical composition at the Gosan super-site was highly dependent on the air mass transport pathways and source region. RH in the springtime over East Asia were distributed with very high spatial and temporal variation. The RH profile onboard C-130 aircraft measurements exhibits a mixed layer height of about 2 km. Aerosol scattering coefficient ( σsp) under ambient RH was greatly enhanced as compared with that at dry RH (RH<40%). From the aerosol optical and radiative transfer modeling studies, we found that the extinction and scattering coefficients are greatly enhanced with RH. Single scattering albedo with RH is also sensitively changed in the longer wavelength. Asymmetry parameter ( g) is gradually increased with RH although g decreases with wavelength at a given RH. Aerosol optical depth (AOD) at 550 nm and RH of 50% increased to factors 1.24, 1.51, 2.16, and 3.20 at different RH levels 70, 80, 90, and 95%, respectively. Diurnal-averaged aerosol radiative forcings for surface, TOA, and atmosphere were increased with RH because AOD was increased with RH due to hygroscopic growth of aerosol particles. This result implies that the hygroscopic growth due to water-soluble or hydrophilic particles in the lower troposphere may significantly modify the magnitude of aerosol radiative forcing both at the surface and TOA. However, the diurnal-averaged radiative forcing efficiencies at the surface, TOA, and atmosphere were decreased with increasing RH. The decrease of the forcing efficiency with RH results from the fact that increasing rate of aerosol optical depth with RH is greater than the increasing rate of aerosol radiative forcing with RH.

  14. Measuring Mass-Based Hygroscopicity of Atmospheric Particles through in situ Imaging

    SciTech Connect

    Piens, Dominique` Y.; Kelly, Stephen T.; Harder, Tristan; Petters, Markus D.; O'Brien, Rachel; 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 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 determined for 158 particles broadly agreed with those of the humidified particles, indicating the potential to infer the 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 submicron atmospheric particles.

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

    SciTech Connect

    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 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. As a result, these methods offer unique quantitative capabilities to characterize and correlate the hygroscopicity and chemistry of individual submicrometer atmospheric particles.

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

    DOE PAGES

    Piens, Dominique S.; Kelly, Stephen T.; Harder, Tristan H.; ...

    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

  17. 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

  18. Aerosol-nutrient-induced picoplankton growth in Lake Tahoe

    NASA Astrophysics Data System (ADS)

    Mackey, Katherine R. M.; Hunter, Deborah; Fischer, Emily V.; Jiang, Yilun; Allen, Brant; Chen, Ying; Liston, Anne; Reuter, John; Schladow, Geoff; Paytan, Adina

    2013-07-01

    Tahoe is an oligotrophic lake appreciated for its transparent waters, yet the Lake's clarity has been declining for several decades due in part to eutrophication. At the same time, a shift from nitrogen (N) toward phosphorus (P) limitation of phytoplankton has occurred that could be due to atmospheric deposition of nutrients with high N:P ratios. Atmospheric particle samples collected during 2005-2006 had a mean soluble N:P ratio of 192:1, well above the Redfield ratio of 16:1 typically required by phytoplankton. Samples collected during the Angora Fire that occurred in 2007 were particularly enriched in N relative to P, with a mean ratio >2800:1. A bioassay incubation experiment was conducted using locally collected atmospheric total suspended particulate (TSP) matter. TSP samples with high ammonium (NH4+) and low P content favored the growth of picoplankton (cells <3 µm) and opportunistic filamentous cyanobacteria, whereas larger nanophytoplankton (cells 3-20 µm) were better competitors when more P was available. Picoplankton growth can increase primary productivity without causing a large increase in chlorophyll (chl a) or biomass. Aerosol-nutrient-induced picoplankton growth (together with shifts in grazing dynamics and stratification trends) may contribute to the uncoupling between primary productivity, chl a, and biomass that has been observed in Lake Tahoe in the last several decades and, in particular, following the Wheeler and Angora Fires. The chemical composition of aerosols has a marked impact on ecosystem dynamics in Lake Tahoe with potential consequences to lake productivity and microbial community dynamics.

  19. Relative humidity impact on aerosol parameters in a Paris suburban area

    NASA Astrophysics Data System (ADS)

    Randriamiarisoa, H.; Chazette, P.; Couvert, P.; Sanak, J.; Mégie, G.

    2006-05-01

    Measurements of relative humidity (RH) and aerosol parameters (scattering cross section, size distributions and chemical composition), performed in ambient atmospheric conditions, have been used to study the influence of relative humidity on aerosol properties. The data were acquired in a suburban area south of Paris, between 18 and 24 July 2000, in the framework of the "Etude et Simulation de la Qualité de l'air en Ile-de-France" (ESQUIF) program. According to the origin of the air masses arriving over the Paris area, the aerosol hygroscopicity is more or less pronounced. The aerosol chemical composition data were used as input of a thermodynamic model to simulate the variation of the aerosol water mass content with ambient RH and to determine the main inorganic salt compounds. The coupling of observations and modelling reveals the presence of deliquescence processes with hysteresis phenomenon in the hygroscopic growth cycle. Based on the Hänel model, parameterisations of the scattering cross section, the modal radius of the accumulation mode of the size distribution and the aerosol water mass content, as a function of increasing RH, have been assessed. For the first time, a crosscheck of these parameterisations has been performed and shows that the hygroscopic behaviour of the accumulation mode can be coherently characterized by combined optical, size distribution and chemical measurements.

  20. Relative humidity impact on aerosol parameters in a Paris suburban area

    NASA Astrophysics Data System (ADS)

    Randriamiarisoa, H.; Chazette, P.; Couvert, P.; Sanak, J.; Mégie, G.

    2005-09-01

    Measurements of relative humidity (RH) and aerosol parameters (scattering cross section, size distributions and chemical composition), performed in ambient atmospheric conditions, have been used to study the influence of relative humidity on aerosol properties. The data were acquired in a suburban area south of Paris, between 18 and 24 July 2000, in the framework of the ''Etude et Simulation de la Qualité de l'air en Ile-de-France'' (ESQUIF) program. According to the origin of the air masses arriving over the Paris area, the aerosol hygroscopicity is more or less pronounced. The aerosol chemical composition data were used as input of a thermodynamic model to simulate the variation of the aerosol water mass content with ambient RH and to determine the main inorganic salt compounds. The coupling of observations and modelling reveals the presence of deliquescence processes with hysteresis phenomenon in the hygroscopic growth cycle. Based on the Hänel model, parameterisations of the scattering cross section, the modal radius of the accumulation mode of the size distribution and the aerosol water mass content, as a function of increasing RH, have been assessed. For the first time, a crosscheck of these parameterisations has been performed and shows that the hygroscopic behaviour of the accumulation mode can be coherently characterized by combined optical, size distribution and chemical measurements.

  1. Aerosols

    Atmospheric Science Data Center

    2013-04-17

    ... article title:  Aerosols over Central and Eastern Europe     View Larger Image ... last weeks of March 2003, widespread aerosol pollution over Europe was detected by several satellite-borne instruments. The Multi-angle ...

  2. Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: Sensitivity to background aerosol and meteorology

    NASA Astrophysics Data System (ADS)

    Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

    2011-12-01

    New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the effective downwind plume aerosol emissions can be greatly modified by both meteorological and background aerosol conditions. In general, new particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

  3. Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

    NASA Astrophysics Data System (ADS)

    Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

    2012-01-01

    New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

  4. Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

    NASA Astrophysics Data System (ADS)

    Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

    2011-09-01

    New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10 s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

  5. 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

  6. 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

  7. AEROSOL GROWTH IN A STEADY-STATE, CONTINUOUS FLOW CHAMBER: APPLICATION TO STUDIES OF SECONDARY AEROSOL FORMATION

    EPA Science Inventory

    An analytical solution for the steady-state aerosol size distribution achieved in a steady-state, continuous flow chamber is derived, where particle growth is occurring by gas-to-particle conversion and particle loss is occurring by deposition to the walls of the chamber. The s...

  8. Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires

    NASA Astrophysics Data System (ADS)

    Mallet, Marc D.; Cravigan, Luke T.; Milic, Andelija; Alroe, Joel; Ristovski, Zoran D.; Ward, Jason; Keywood, Melita; Williams, Leah R.; Selleck, Paul; Miljevic, Branka

    2017-03-01

    The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm-3 when frequent and close fires were burning - up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ = 0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to ˜ 100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large

  9. Performance of combination drug and hygroscopic excipient submicrometer particles from a softmist inhaler in a characteristic model of the airways.

    PubMed

    Longest, P Worth; Tian, Geng; Li, Xiang; Son, Yoen-Ju; Hindle, Michael

    2012-12-01

    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 computational fluid dynamic (CFD) simulations. The airway model included a characteristic mouth-throat (MT) and upper tracheobronchial (TB) region through the third bifurcation 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.

  10. [Ecological effect of hygroscopic and condensate water on biological soil crusts in Shapotou region of China].

    PubMed

    Pan, Yan-Xia; Wang, Xin-Ping; Zhang, Ya-Feng; Hu, Rui

    2013-03-01

    By the method of field experiment combined with laboratory analysis, this paper studied the ecological significance of hygroscopic and condensate water on the biological soil crusts in the vegetation sand-fixing area in Shapotou region of China. In the study area, 90% of hygroscopic and condensate water was within the 3 cm soil depth, which didn' t affect the surface soil water content. The hygroscopic and condensate water generated at night involved in the exchange process of soil surface water and atmosphere water vapor, made up the loss of soil water due to the evaporation during the day, and made the surface soil water not reduced rapidly. The amount of the generated hygroscopic and condensate water had a positive correlation with the chlorophyll content of biological soil crusts, indicating that the hygroscopic and condensate water could improve the growth activity of the biological soil crusts, and thus, benefit the biomass accumulation of the crusts.

  11. Cloud forming potential of oligomers relevant to secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Xu, Wen; Guo, Song; Gomez-Hernandez, Mario; Zamora, Misti L.; Secrest, Jeremiah; Marrero-Ortiz, Wilmarie; Zhang, Annie L.; Collins, Don R.; Zhang, Renyi

    2014-09-01

    The hygroscopic growth factor (HGF) and cloud condensation nuclei (CCN) activity are measured for surrogates that mimic atmospherically relevant oligomers, including glyoxal trimer dihydrate, methyl glyoxal trimer dihydrate, sucrose, methyl glyoxal mixtures with sulfuric acid and glycolic acid, and 2,4-hexandienal mixtures with sulfuric acid and glycolic acid. For the single-component aerosols, the measured HGF ranges from 1.3 to 1.4 at a relative humidity of 90%, and the hygroscopicity parameter (κ) is in the range of 0.06 to 0.19 on the basis of the measured CCN activity and 0.13 to 0.22 on the basis of the measured HGF, compared to the calculated values of 0.08 to 0.16. Large differences exist in the κ values derived using the measured HGF and CCN data for the multi-component aerosols. Our results reveal that, in contrast to the oxidation process, oligomerization decreases particle hygroscopicity and CCN activity and provides guidance for analyzing the organic species in ambient aerosols.

  12. Nonequilibrium Atmospheric Secondary Organic Aerosol Formation and Growth

    SciTech Connect

    Perraud, Veronique M.; Bruns, Emily A.; Ezell, Michael J.; Johnson, Stanley N.; Yu, Yong; Alexander, M. L.; Zelenyuk, Alla; Imre, D.; Chang, W. L.; Dabdub, Donald; Pankow, James F.; Finlayson-Pitts, Barbara J.

    2012-02-21

    Airborne particles play a critical role in air quality, human health effects, visibility and climate. Secondary organic aerosols (SOA) account for a significant portion of total airborne particles. They are formed in reactions of organic gases that produce low volatility and semi-volatile organic compounds (SVOCs). Current atmospheric models assume that SOA are liquids into which SVOCs undergo equilibrium partitioning and grow the particles. However a large discrepancy between model predictions and field measurements of SOA is commonly observed. We report here laboratory studies of the oxidation of a-pinene by ozone and nitrate radicals and show that particle composition is actually consistent with a kinetically determined growth mechanism, and not with equilibrium partitioning between the gas phase and liquid particles. If this is indeed a general phenomenon in air, the formulation of atmospheric SOA models will have to be revised to reflect this new paradigm. This will have significant impacts on quantifying the role of SOA in air quality, visibility, and climate.

  13. Some optical properties of smoke aerosol in Indonesia and tropical Australia

    NASA Astrophysics Data System (ADS)

    Gras, J. L.; Jensen, J. B.; Okada, K.; Ikegami, M.; Zaizen, Y.; Makino, Y.

    Aerosol light-scattering coefficient at 530 nm and its hygroscopic growth were determined in biomass-burning smoke in the lower atmosphere over Kalimantan and northern Australia during the 1997 dry-season fires. Both in and away from plumes, light-scattering was considerably greater in the Indonesian region and hygroscopic growth in scattering was also consistently greater. The relative increase in scattering, from 20% to 80% relative humidity, was typically 1.37 in northern Australian and 1.65 in Kalimantan. Limited aerosol light absorption data indicate relatively small absorption in the Indonesian smoke. In part these differences can be explained by different combustion phases, mixed flaming and smoldering in the Australian savanna fires compared with predominantly smoldering in Indonesia, although these and other concurrent measurements suggest that underground peat combustion may have made a significant contribution to the Indonesian smoke.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  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. 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.

  17. Condensational growth and trace species scavenging in stratospheric sulfuric acid/water aerosol droplets

    NASA Technical Reports Server (NTRS)

    Tompson, Robert V., Jr.

    1991-01-01

    Stratospheric aerosols play a significant role in the environment. The composition of aerosols is believed to be a liquid solution of sulfuric acid and water with numerous trace species. Of these trace species, ozone in particular was recognized as being very important in its role of shielding the environment from harmful ultraviolet radiation. Also among the trace species are HCl and ClONO2, the so called chlorine reservoir species and various oxides of nitrogen. The quantity of stratospheric aerosol and its particle size distribution determines, to a large degree, the chemistry present in the stratosphere. Aerosols experience 3 types of growth: nucleation, condensation, and coagulation. The application of condensation investigations to the specific problem of stratospheric aerosols is discussed.

  18. 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

  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. What Can We Learn From Laboratory Studies of Inorganic Sea Spray Aerosol?

    NASA Astrophysics Data System (ADS)

    Salter, M. E.; Zieger, P.; Acosta Navarro, J. C.; Grythe, H.; Kirkevag, A.; Rosati, B.; Riipinen, I.; Nilsson, E. D.

    2015-12-01

    Since 2013 we have been operating a temperature-controlled plunging-jet sea spray aerosol chamber at Stockholm University using inorganic artificial seawater. Using size-resolved measurements of the foam bubbles responsible for the aerosol production we were able to show that it is changes to these foam bubbles which drive the observed changes in aerosol production and size distribution as water temperature changes (Salter et al., 2014). Further, by combining size-resolved measurements of aerosol production as a function of water temperature with measurements of air entrainment by the plunging-jet we have developed a temperature-dependent sea spray source function for deployment in large-scale models (Salter et al., 2015). We have also studied the hygroscopicity, morphology, and chemical composition of the inorganic sea spray aerosol produced in the chamber. The sea spray aerosol generated from artificial seawater exhibited lower hygroscopic growth than both pure NaCl and output from the E-AIM aerosol thermodynamics model when all relevant inorganic ions in the sea salt were included. Results from sensitivity tests using a large-scale earth system model suggest that the lower hygroscopicity observed in our laboratory measurements has important implications for calculations of the radiative balance of the Earth. In addition, size-dependent chemical fractionation of several inorganic ions was observed relative to the artificial seawater with potentially important implications for the chemistry of the marine boundary layer. Each of these studies suggest that there is still much to be learned from rigorous experiments using inorganic seawater proxies. Salter et al., (2014), On the seawater temperature dependence of the sea spray aerosol generated by a continuous plunging jet. J. Geophys. Res. Atmos., 119, 9052-9072, doi: 10.1002/2013JD021376 Salter et al., (2015), An empirically derived inorganic sea spray source function incorporating sea surface temperature. Atmos

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

    NASA Technical Reports Server (NTRS)

    Russell, P. B.; Bergstrom, Robert W.; Schmid, B.; Livingston, J. M.

    2000-01-01

    We estimate the impact of North Atlantic aerosols on the net short-wave flux at the tropopause by combining satellite-derived aerosol optical depth (AOD) maps with model aerosol properties determined via closure analyses in TARFOX and ACE 2. We exclude African dust, primarily by restricting latitudes to 25-60 N. The analyses use in situ aerosol composition measurements and air- and ship-borne sun-photometer measurements of AOD spectra. The aerosol model yields computed flux sensitivities (dFlux/dAOD) that agree with measurements by airborne flux radiometers in TARFOX. Its midvisible single-scattering albedo is 0.9. which is in the range obtained from in situ measurements of scattering and absorption in both TARFOX and ACE 2. Combining satellite-derived AOD maps with the aerosol model yields maps of 24-hour average net radiative flux changes. For simultaneous AVHRR, radiance measurements exceeded the sunphotometer AODs by about 0.04. However. shipboard sunphotometer and AVHRR AODs agreed Within 0.02 for data acquired during satellite overflights on two other days. We discuss attempts to demonstrate column closure within the MBL by comparing shipboard sunphotometer AODs and values calculated from simultaneous shipboard in-situ aerosol size distribution measurements. These comparisons were mostly unsuccessful, but they illustrate the difficulties inherent in this type of closure analysis. Specifically, AODs derived from near-surface in-situ size distribution measurements are extremely sensitive to the assumed hygroscopic growth model that itself requires an assumption of particle composition as a function of height and size, to the radiosonde-measured relative humidity, and to the vertical profile of particle number. We investigate further the effects of hygroscopic particle growth within the MBL by using shipboard lidar aerosol backscatter profiles together with the sunphotometer AOD.

  2. Seasonality of Aerosols the Southeastern United States

    NASA Astrophysics Data System (ADS)

    Ford, B. J.; Heald, C. L.

    2012-12-01

    Previous studies have suggested that increases in atmospheric aerosols of biogenic origin may have caused regional cooling over the southeastern United States in recent decades. Understanding the sources and behaviors of these aerosols is important for determining their role in a changing climate and managing their air quality impacts. In this study, we investigate the strong seasonality in aerosol optical depth (AOD) observed by MODIS, MISR, and CALIOP instruments over the southeastern United States and show that this is not simulated by a chemical transport model (GEOS-Chem). However, the model does reproduce surface PM 2.5 concentrations in the region as reported by the IMPROVE and Southeastern Aerosol Research and Characterization (SEARCH) networks, as well as the muted seasonality of these concentrations. In addition, these surface measurements show that organic aerosol makes up a small fraction of total PM 2.5 and has relatively little seasonality, which calls into question the importance of biogenic aerosol as a driver for climate change in the region. Sounding profiles and ground observations of relative humidity suggest that the magnitude of seasonality in AOD cannot be explained by seasonal differences in the hygroscopic growth of aerosols. CALIOP measurements of the vertical profile of aerosol extinction confirm that the likely reconciliation of the differences in seasonality between the surface PM 2.5 and AOD observations is the formation of aerosol aloft, a process not captured by the model. These findings provide initial insights for the Southern Oxidant and Aerosol Study (SOAS) campaign in 2013 which aims to investigate the anthropogenic influence on biogenic aerosol formation in the Southeastern US and elucidate the impact on regional climate and air quality.

  3. 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.

  4. Condensational Growth of Combination Drug-Excipient Submicrometer Particles for Targeted High Efficiency Pulmonary Delivery: Comparison of CFD Predictions with Experimental Results

    PubMed Central

    Hindle, Michael

    2011-01-01

    Purpose The objective of this study was to investigate the hygroscopic growth of combination drug and excipient submicrometer aerosols for respiratory drug delivery using in vitro experiments and a newly developed computational fluid dynamics (CFD) model. Methods Submicrometer combination drug and excipient particles were generated experimentally using both the capillary aerosol generator and the Respimat inhaler. Aerosol hygroscopic growth was evaluated in vitro and with CFD in a coiled tube geometry designed to provide residence times and thermodynamic conditions consistent with the airways. Results The in vitro results and CFD predictions both indicated that the initially submicrometer particles increased in mean size to a range of 1.6–2.5 µm for the 50:50 combination of a non-hygroscopic drug (budesonide) and different hygroscopic excipients. CFD results matched the in vitro predictions to within 10% and highlighted gradual and steady size increase of the droplets, which will be effective for minimizing extrathoracic deposition and producing deposition deep within the respiratory tract. Conclusions Enhanced excipient growth (EEG) appears to provide an effective technique to increase pharmaceutical aerosol size, and the developed CFD model will provide a powerful design tool for optimizing this technique to produce high efficiency pulmonary delivery. PMID:21948458

  5. Early growth dynamical implications for the steerability of stratospheric solar radiation management via sulfur aerosol particles

    NASA Astrophysics Data System (ADS)

    Benduhn, François; Schallock, Jennifer; Lawrence, Mark G.

    2016-09-01

    Aerosol growth dynamics may have implications for the steerability of stratospheric solar radiation management via sulfur particles. This paper derives a set of critical initial growth conditions that are analyzed as a function of two key parameters: the initial concentration of the injected sulfuric acid and its dilution rate with the surrounding air. Based upon this analysis, early aerosol growth dynamical regimes may be defined and classified in terms of their likelihood to serve as candidates for the controlled generation of a radiatively effective aerosol. Our results indicate that the regime that fulfills all critical conditions would require that airplane turbines be used to provide sufficient turbulence. The regime's parameter space is narrow and related to steep gradients, thus pointing to potential fine tuning requirements. More research, development, and testing would be required to refine our findings and determine their global-scale implications.

  6. Updating CMAQ secondary organic aerosol properties relevant for aerosol water interactions

    EPA Science Inventory

    Properties of secondary organic aerosol (SOA) compounds in CMAQ are updated with state-of-the-science estimates from structure activity relationships to provide consistency among volatility, molecular weight, degree of oxygenation, and solubility/hygroscopicity. These updated pro...

  7. 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

  8. Scanning supersaturation condensation particle counter applied as a nano-CCN counter for size-resolved analysis of the hygroscopicity and chemical composition of nanoparticles

    NASA Astrophysics Data System (ADS)

    Wang, Z.; Su, H.; Wang, X.; Ma, N.; Wiedensohler, A.; Poschl, U.; Cheng, Y.

    2015-05-01

    Knowledge about the chemical composition of aerosol particles is essential to understand their formation and evolution in the atmosphere. Due to analytical limitations, however, relatively little information is available for sub-10 nm particles. We present the design of a nano-cloud condensation nuclei counter (nano-CCNC) for measuring size-resolved hygroscopicity and inferring chemical composition of sub-10 nm aerosol particles. We extend the use of counting efficiency spectra from a water-based condensation particle counter (CPC) and link it to the analysis of CCN activation spectra, which provides a theoretical basis for the application of a scanning supersaturation CPC (SS-CPC) as a nano-CCNC. Measurement procedures and data analysis methods are demonstrated through laboratory experiments with monodisperse particles of diameter down to 2.5 nm, where sodium chloride, ammonium sulfate, sucrose and tungsten oxide can be easily discriminated by different characteristic supersaturations of water droplet formation. A near-linear relationship between hygroscopicity parameter κ and organic mass fraction is also found for sucrose-ammonium sulfate mixtures. The design is not limited to the water CPC, but also applies to CPCs with other working fluids (e.g. butanol, perfluorotributylamine). We suggest that a combination of SS-CPCs with multiple working fluids may provide further insight into the chemical composition of nanoparticles and the role of organic and inorganic compounds in the initial steps of atmospheric new particle formation and growth.

  9. 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

  10. Implementation of the Missing Aerosol Physics into LLNL IMPACT

    SciTech Connect

    Chuang, C

    2005-02-09

    In recent assessments of climate forcing, the Intergovernmental Panel on Climate Change lists aerosol as one o f the most important anthropogenic agents that influence climate. Atmospheric aerosols directly affect the radiative fluxes at the surface and top of the Earth's atmosphere by scattering and/or absorbing radiation. Further, aerosols indirectly change cloud microphysical properties (such as cloud drop effective radius) that also affect the radiative fluxes. However, the estimate of the magnitude of aerosol climatic effect varies widely, and aerosol/cloud interactions remain one of the most uncertain aspects of climate models today. The Atmospheric Sciences Division has formulated a plan to enhance and expand our modeling expertise in aerosol/cloud/climate interactions. Under previous LDRD support, we successfully developed a computationally efficient version of IMPACT to simulate aerosol climatology. This new version contains a compact chemical mechanism for the prediction of sulfate and also predicts the distributions of organic carbon (OC), black carbon (BC), dust, and sea salt. Furthermore, we implemented a radiation package into IMPACT to calculate the radiative forcing and heating/cooling rates by aerosols. This accomplishment built the foundation of our currently funded projects under the NASA Global Modeling and Analysis Program as well as the DOE Atmospheric Radiation Program. Despite the fact that our research is being recognized as an important effort to quantify the effects of anthropogenic aerosols on climate, the major shortcoming of our previous simulations on aerosol climatic effects is the over simplification of spatial and temporal variations of aerosol size distributions that are shaped by complicated nucleation, growth, transport and removal processes. Virtually all properties of atmospheric aerosols and clouds depend strongly on aerosol size distribution. Moreover, molecular processing on aerosol surfaces alters the hygroscopic

  11. Formation and growth of indoor air aerosol particles as a result of D-limonene oxidation

    NASA Astrophysics Data System (ADS)

    Vartiainen, E.; Kulmala, M.; Ruuskanen, T. M.; Taipale, R.; Rinne, J.; Vehkamäki, H.

    Oxidation of D-limonene, which is a common monoterpene, can lead to new aerosol particle formation in indoor environments. Thus, products containing D-limonene, such as citrus fruits, air refresheners, household cleaning agents, and waxes, can act as indoor air aerosol particle sources. We released D-limonene into the room air by peeling oranges and measured the concentration of aerosol particles of three different size ranges. In addition, we measured the concentration of D-limonene, the oxidant, and the concentration of ozone, the oxidizing gas. Based on the measurements we calculated the growth rate of the small aerosol particles, which were 3-10 nm in diameter, to be about 6300nmh-1, and the losses of the aerosol particles that were due to the coagulation and condensation processes. From these, we further approximated the concentration of the condensable vapour and its source rate and then calculated the formation rate of the small aerosol particles. For the final result, we calculated the nucleation rate and the maximum number of molecules in a critical cluster. The nucleation rate was in the order of 105cm-3s-1 and the number of molecules in a critical-sized cluster became 1.2. The results were in agreement with the activation theory.

  12. Modeling aerosol growth by aqueous chemistry in nonprecipitating stratiform cloud

    SciTech Connect

    Ovchinnikov, Mikhail; Easter, Richard C.

    2010-07-29

    A new microphysics module based on a two-dimensional (2D) joint size distribution function representing both interstitial and cloud particles is developed and applied to studying aerosol processing in non-precipitating stratocumulus clouds. The module is implemented in a three-dimensional dynamical framework of a large-eddy simulation (LES) model and in a trajectory ensemble model (TEM). Both models are used to study the modification of sulfate aerosol by the activation - aqueous chemistry - resuspension cycle in shallow marine stratocumulus clouds. The effect of particle mixing and different size-distribution representations on modeled aerosol processing are studied in a comparison of the LES and TEM simulations with the identical microphysics treatment exposes and a comparison of TEM simulations with a 2D fixed and moving bin microphysics. Particle mixing which is represented in LES and neglected in the TEM leads to the mean relative per particle dry mass change in the TEM simulations being about 30% lower than in analogous subsample of LES domain. Particles in the final LES spectrum are mixed in from different “parcels”, some of which have experienced longer in-cloud residence times than the TEM parcels, all of which originated in the subcloud layer, have. The mean relative per particle dry mass change differs by 14% between TEM simulations with fixed and moving bin microphysics. Finally, the TEM model with the moving bin microphysics is used to evaluate assumptions about liquid water mass partitioning among activated cloud condensation nuclei (CCN) of different dry sizes. These assumptions are used in large-scale models to map the bulk aqueous chemistry sulfate production, which is largely proportional to the liquid water mass, to the changes in aerosol size distribution. It is shown that the commonly used assumptions that the droplet mass is independent of CCN size or that the droplet mass is proportional to the CCN size to the third power do not perform

  13. Using Aerocom Results to Constrain Black Carbon, Sulphate and Total Direct Aerosol Radiative Forcing and Their Uncertainties

    NASA Astrophysics Data System (ADS)

    Samset, B. H.; Myhre, G.

    2014-12-01

    Aerosols affect the global radiative balance, and hence the climate, through a multitude of processes. However, even the direct interaction of aerosols with incoming sunlight is at present insufficiently constrained. Here we compare the output of 15 recent aerosol climate models (AeroCom Phase II), both column averaged and vertically resolved. Through a simple MonteCarlo approach, we show that the model based total anthropogenic aerosol direct radiative forcing (DRF) uncertainty may be underestimated. Constraining modelled vertical profiles of black carbon (BC) concentration to aircraft measurements in remote regions, we further show that recent BC DRF estimates may be biased high. A short modelled BC lifetime is indicated as a necessary, though not sufficient, requirement for reproducing measurements. Finally, modeled sulphate aerosol DRF is discussed in the context of differences in representation of humidity and hygroscopic growth in the models.

  14. Impacts of oxidation aging on secondary organic aerosol formation, particle growth rate, cloud condensation nuclei abundance, and aerosol climate forcing

    NASA Astrophysics Data System (ADS)

    Yu, F.; Luo, G.

    2014-12-01

    Particle composition measurements indicate that organic aerosol (OA) makes up ~20-90% of submicron particulate mass and secondary OA (SOA) accounts for a large fraction (~ 72 ±21%) of these OA masses at many locations around the globe. The volatility changes of secondary organic gases (SOG) associated with oxidation aging as well as the contribution of highly oxidized low volatile SOG (LV-SOG) to the condensational growth of secondary particles have been found to be important in laboratory and field measurements but are poorly represented in global models. A novel scheme to extend the widely used two-product SOA formation model, by adding a third product arising from the oxidation aging (i.e., LV-SOG) and considering the dynamic transfer of mass from higher to lower volatile products, has been developed and implemented into a global chemical transport model (GEOS-Chem) and a community atmosphere model (CESM-CAM5). The scheme requires only minor changes to the existing two-product SOA formation model and is computationally efficient. With the oxidation rate constrained by laboratory measurements, we show that the new scheme predicts a much higher SOA mass concentrations, improving the agreement with aerosol mass spectrometer SOA measurements. The kinetic condensation of LV-SOG on ultrafine particles, simulated by a size-resolved (sectional) advanced particle microphysics (APM) model incorporated into in GEOS-Chem and CAM5, increases the particle growth rate substantially and improves the agreement of simulated cloud condensation nuclei (CCN) concentrations with observations. Based on GEOS-Chem-APM simulations, the new SOA formation scheme increases global mean low troposphere SOA mass concentration by ~130% and CCN abundance by ~ 15%, and optical depth of secondary particles and coated black carbon and primary organic carbon particles by ~10%. As a result, aerosol radiative cooling effect (direct + first indirect) is enhanced by -0.9 W/m2, with large spatial

  15. Aerosol optical depth increase in partly cloudy conditions

    NASA Astrophysics Data System (ADS)

    Chand, Duli; Wood, Robert; Ghan, Steven J.; Wang, Minghuai; Ovchinnikov, Mikhail; Rasch, Philip J.; Miller, Steven; Schichtel, Bret; Moore, Tom

    2012-09-01

    Remote sensing observations of aerosol from surface and satellite instruments are extensively used for atmospheric and climate research. From passive sensors, the apparent cloud-free atmosphere in the vicinity of clouds often appears to be brighter than further away from the clouds, leading to an increase in the retrieved aerosol optical depth (τ). Mechanisms contributing to this enhancement or increase, including contamination by undetected clouds, hygroscopic growth of aerosol particles, and meteorological conditions, have been debated in recent literature, but the extent to which each of these factors influence the observed enhancement (Δτ) is poorly known. Here we used 11 years of daily global observations at 10 × 10 km2 resolution from the MODIS on the NASA Terra satellite to quantify τ as a function of cloud fraction (CF). Our analysis reveals that, averaged over the globe, the clear sky τ is enhanced by Δτ = 0.05 in cloudy conditions (CF = 0.8-0.9). This enhancement in Δτ corresponds to relative enhancement of 25% in cloudy conditions (CF = 0.8-0.9) compared with relatively clear conditions (CF = 0.1-0.2). Unlike the absolute enhancement Δτ, the relative increase in τis rather consistent in all seasons and is 25-35% in the subtropics and 15-25% at mid and higher latitudes. Using a simple Gaussian probability density function model to connect cloud cover and the distribution of relative humidity, we argue that much of the enhancement is consistent with aerosol hygroscopic growth in the humid environment surrounding clouds. Consideration of these cloud-dependentτeffects will facilitate understanding aerosol-cloud interactions and reduce the uncertainty in estimates of aerosol radiative forcing by global climate models.

  16. Aerosol optical depth increase in partly cloudy conditions

    SciTech Connect

    Chand, Duli; Wood, R.; Ghan, Steven J.; Wang, Minghuai; Ovchinnikov, Mikhail; Rasch, Philip J.; Miller, Steven D.; Schichtel, Bret; Moore, Tom

    2012-09-14

    Remote sensing observations of aerosol from surface and satellite instruments are extensively used for atmospheric and climate research. From passive sensors, the apparent cloud-free atmosphere in the vicinity of clouds often appears to be brighter then further away from the clouds, leading to an enhancement in the retrieved aerosol optical depth. Mechanisms contributing to this enhancement, including contamination by undetected clouds, hygroscopic growth of aerosol particles, and meteorological conditions, have been debated in recent literature, but an extent to which each of these factors influence the observed enhancement is poorly known. Here we used 11 years of daily global observations at 10x10 km2 resolution from the MODIS on the NASA Terra satellite to quantify as a function of cloud fraction (CF). Our analysis reveals that, averaged over the globe, the clear sky is enhanced by ? = 0.05 which corresponds to relative enhancements of 25% in cloudy conditions (CF=0.8-0.9) compared with relatively clear conditions (CF=0.1-0.2). Unlike the absolute enhancement ?, the relative increase in ? is rather consistent in all seasons and is 25-35% in the subtropics and 15-25% at mid and higher latitudes. Using a simple Gaussian probability density function model to connect cloud cover and the distribution of relative humidity, we argue that much of the enhancement is consistent with aerosol hygroscopic growth in the humid environment surrounding clouds. Consideration of these cloud-dependent effects will facilitate understanding aerosol-cloud interactions and reduce the uncertainty in estimates of aerosol radiative forcing by global climate models.

  17. Seasonal heterogeneity in aerosol types over Dibrugarh-North-Eastern India

    NASA Astrophysics Data System (ADS)

    Pathak, Binita; Bhuyan, Pradip Kumar; Gogoi, Mukunda; Bhuyan, Kalyan

    2012-02-01

    Columnar aerosol properties retrieved from Multi-Wavelength solar Radiometer (MWR) measurements during the period 2001-2010 over Dibrugarh (27.3°N, 94.6°E, 111 m amsl), North-Eastern India are analyzed to identify the types of aerosols in the atmospheric column. Highest Aerosol optical depth (AOD) characterizes the pre-monsoon (March-May), while lowest AOD has been observed during the post-monsoon (Oct-Nov) season. The Ångström exponent (α) indicates predominance of fine aerosols during post-monsoon and winter (Dec-Feb) and dominance of coarse mode in pre-monsoon and monsoon (June-Sept). NOAA HYSPLIT back trajectory analysis suggests that the seasonal heterogeneity in aerosol characteristics can be attributed to the varying contribution from different source regions. Using the relationship between AOD 500 and α, the aerosols can be classified into five main types viz. continental average (CA), marine continental average (MCA), urban/industrial and biomass burning (UB) and desert dust (DD) while the remaining cases are considered as unidentified or mixed type (MT). These aerosol types exhibit seasonal heterogeneity in their contribution depending upon variability in sources. In winter, local production contributes to observed appreciable CA aerosol type, while highest percentage of UB type is attributed to both local and transported aerosols. On the other hand, transported UB and DD types play a significant role in the pre-monsoon season. Post-monsoon season is indicative of background continental average aerosol condition with a significant contribution from CA and MCA aerosols. Monsoon aerosols couldn't be distinguished properly due to different particle growth processes like humidification, hygroscopic growth etc. and hence MT aerosol type is predominant in this season. This is the first ever attempt to classify aerosols over this environment.

  18. Heterogeneous photochemistry of imidazole-2-carboxaldehyde: HO2 radical formation and aerosol growth

    NASA Astrophysics Data System (ADS)

    González Palacios, Laura; Corral Arroyo, Pablo; Aregahegn, Kifle Z.; Steimer, Sarah S.; Bartels-Rausch, Thorsten; Nozière, Barbara; George, Christian; Ammann, Markus; Volkamer, Rainer

    2016-09-01

    The multiphase chemistry of glyoxal is a source of secondary organic aerosol (SOA), including its light-absorbing product imidazole-2-carboxaldehyde (IC). IC is a photosensitizer that can contribute to additional aerosol ageing and growth when its excited triplet state oxidizes hydrocarbons (reactive uptake) via H-transfer chemistry. We have conducted a series of photochemical coated-wall flow tube (CWFT) experiments using films of IC and citric acid (CA), an organic proxy and H donor in the condensed phase. The formation rate of gas-phase HO2 radicals (PHO2) was measured indirectly by converting gas-phase NO into NO2. We report on experiments that relied on measurements of NO2 formation, NO loss and HONO formation. PHO2 was found to be a linear function of (1) the [IC] × [CA] concentration product and (2) the photon actinic flux. Additionally, (3) a more complex function of relative humidity (25 % < RH < 63 %) and of (4) the O2 / N2 ratio (15 % < O2 / N2 < 56 %) was observed, most likely indicating competing effects of dilution, HO2 mobility and losses in the film. The maximum PHO2 was observed at 25-55 % RH and at ambient O2 / N2. The HO2 radicals form in the condensed phase when excited IC triplet states are reduced by H transfer from a donor, CA in our system, and subsequently react with O2 to regenerate IC, leading to a catalytic cycle. OH does not appear to be formed as a primary product but is produced from the reaction of NO with HO2 in the gas phase. Further, seed aerosols containing IC and ammonium sulfate were exposed to gas-phase limonene and NOx in aerosol flow tube experiments, confirming significant PHO2 from aerosol surfaces. Our results indicate a potentially relevant contribution of triplet state photochemistry for gas-phase HO2 production, aerosol growth and ageing in the atmosphere.

  19. Aerosol production and growth in the marine boundary layer

    NASA Astrophysics Data System (ADS)

    Russell, Lynn M.; Pandis, Spyros N.; Seinfeld, John H.

    1994-10-01

    The dependence of cloud condensation nuclei (CCN) production on the marine dimethylsulfide (DMS) flux is modeled with a dynamic description of the gas, aerosol, and aqueous phase processes in a closed air parcel. The results support the conclusion reached in previous work with a steady state model that an approximately linear dependence exists between CCN concentration and DMS flux under typical remote marine conditions. This linearity does not hold for low DMS fluxes (the threshold is typically near 2.5 micromol/sq m/day) because the sea-salt particles heterogeneously convert the available SO2 to sulfate inhibiting the creation of new particles. The conditions under which this linear relationship holds are investigated by a series of sensitivity studies, focusing particular attention on the impact of the timing and frequency of cloud events. We consider the regimes of the model's semiempirical parameters, showing that the uncertainty associated with two such parameters, namely, the nucleation rate scaling factor and the sulfuric acid accommodation coefficient, is sufficient to change the predicted CCN production due to DMS from over 300/cu cm/day to none. This sensitivity accounts for most of the range of results predicted by previous models of the DMS-CCN system.

  20. Cassini CAPS-ELS observations of carbon-based anions and aerosol growth in Titan's ionosphere

    NASA Astrophysics Data System (ADS)

    Desai, Ravindra; Coates, Andrew; Wellbrock, Anne; Kataria, Dhiren; Jones, Geraint; Lewis, Gethyn; Waite, J.

    2016-06-01

    Cassini observations of Titans ionosphere revealed an atmosphere rich in positively charged ions with masses up to > 350 amu and negatively charged ions and aerosols with mass over charge ratios as high as 13,800 amu/q. The detection of negatively charged molecules by the Cassini CAPS Electron Spectrometer (CAPS-ELS) was particularly surprising and showed how the synthesis of large aerosol-size particles takes place at altitudes much greater than previously thought. Here, we present further analysis into this CAPS-ELS dataset, through an enhanced understanding of the instrument's response function. In previous studies the intrinsic E/E energy resolution of the instrument did not allow specific species to be identified and the detections were classified into broad mass ranges. In this study we use an updated fitting procedure to show how the ELS mass spectrum can be resolved into specific peaks at multiples of carbon-based anions up to > 100 amu/q. The negatively charged ions and aerosols in Titans ionosphere increase in mass with decreasing altitude, the lightest species being observed close to Titan's exobase of ˜1,450km and heaviest species observed at altitudes < 950km. We identify key stages in this apparent growth process and report on key intermediaries which appear to trigger the rapid growth of the larger aerosol-size particles.

  1. Hexagonal ice stability and growth in the presence of glyoxal and secondary organic aerosols.

    PubMed

    Daskalakis, Vangelis; Hadjicharalambous, Marios

    2014-09-07

    The presence of ice dominates the microphysics of formation of high altitude cirrus and polar stratospheric clouds, as well as the maturity of thunderstorms. We report on the hexagonal (1h) ice stability and growth in binary as well as multi-compound aerosols in atmospherically relevant conformations. The ubiquitous atmospheric trace gas glyoxal along with secondary organic aerosol (SOA) also in the presence of CO2 interacts with large ice 1h crystals of 1300-2000 water molecules. The crystals are subjected to phase transitions under superheating and supercooling conditions by Molecular Dynamics (MD) simulations. Density Functional Theory (DFT) based geometry optimization and vibrational frequency analysis are also employed for a smaller ice 1h cell of 12 water molecules. The interaction of the latter with each organic molecule reveals the extent of the mechanical stress exerted on the ordered ice structure. Full hydration of glyoxal promotes ice 1h stability and growth in wet aerosols, while partial hydration or full oxidation exerts a destabilizing effect on the ice 1h lattice. This behavior is associated with the ability of each organic phase to match the order of the ice 1h crystal. We propose that aqueous chemistry in wet aerosols may also have a strong effect on the microphysics of cloud formation.

  2. 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

  3. 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

  4. 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.

  5. Topochemical diffusion-reaction-convection dynamics in vapor-to-particle aerosol nucleation and growth

    NASA Astrophysics Data System (ADS)

    Thompson, Stephen; Shipman, Patrick D.

    2013-05-01

    We report on patterns and oscillations observed in topochemically organized vapor-toparticle experimental systems involving aerosol nucleation and growth processes in which NH3 reacts with HCl, HNO3, H2SO4, and CH3COOH. Mathematical models of these systems in comparison with experiments allow us to estimate parameters such as kinetic constants and nucleation thresholds. The patterns are strongly influenced by charging, hydration, and turbulence driven by exothermicity.

  6. Morphological characterization of soot aerosol particles during LACIS Experiment in November (LExNo)

    NASA Astrophysics Data System (ADS)

    Kiselev, A.; Wennrich, C.; Stratmann, F.; Wex, H.; Henning, S.; Mentel, T. F.; Kiendler-Scharr, A.; Schneider, J.; Walter, S.; Lieberwirth, I.

    2010-06-01

    Combined mobility and aerodynamic measurements were used to characterize the morphology of soot particles in an experimental campaign on the hygroscopic growth and activation of an artificial biomass burning aerosol. A custom-made, single-stage low-pressure impactor and two aerosol mass spectrometers (AMS) operating in the free molecular regime were used to measure the vacuum aerodynamic diameter of mobility-selected artificial soot particles that were produced in a spark discharge generator and then modified by condensation of ammonium hydrogen sulfate or levoglucosan as a coating to change their hydroscopic activity. Transmission electron microscope images revealed a relationship between the electrical mobility diameter and the diameter of the enveloping sphere, thus enabling evaluation of the effective density of soot agglomerates. A fractal description of the morphology of the soot aggregates allowed for evaluation of the average mass of the hygroscopic material per particle. The average mass of the hygroscopic material per particle was also measured directly with the two AMS instruments, and the agreement between the two methods was found satisfactory. This tandem approach allows detection of small changes in the particle effective density and morphology caused by condensation of organic material.

  7. Hygroscopic properties of Amazonian biomass burning and European background HULIS and investigation of their effects on surface tension with two models linking H-TDMA to CCNC data

    NASA Astrophysics Data System (ADS)

    Fors, E. O.; Rissler, J.; Massling, A.; Svenningsson, B.; Andreae, M. O.; Dusek, U.; Frank, G. P.; Hoffer, A.; Bilde, M.; Kiss, G.; Janitsek, S.; Henning, S.; Facchini, M. C.; Decesari, S.; Swietlicki, E.

    2010-06-01

    HUmic-LIke Substances (HULIS) have been identified as major contributors to the organic carbon in atmospheric aerosol. The term "HULIS" is used to describe the organic material found in aerosol particles that resembles the humic organic material in rivers and sea water and in soils. In this study, two sets of filter samples from atmospheric aerosols were collected at different sites. One set of samples was collected at the K-puszta rural site in Hungary, about 80 km SE of Budapest, and a second was collected at a site in Rondônia, Amazonia, Brazil, during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) biomass burning season experiment. HULIS were extracted from the samples and their hygroscopic properties were studied using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) at relative humidity (RH) <100%, and a cloud condensation nucleus counter (CCNC) at RH >100%. The H-TDMA measurements were carried out at a dry diameter of 100 nm and for RH ranging from 30 to 98%. At 90% RH the HULIS samples showed diameter growth factors between 1.04 and 1.07, reaching values of 1.4 at 98% RH. The cloud nucleating properties of the two sets of aerosol samples were analysed using two types of thermal static cloud condensation nucleus counters. Two different parameterization models were applied to investigate the potential effect of HULIS surface activity, both yielding similar results. For the K-puszta winter HULIS sample, the surface tension at the point of activation was estimated to be lowered by between 34% (47.7 mN/m) and 31% (50.3 mN/m) for dry sizes between 50 and 120 nm in comparison to pure water. A moderate lowering was also observed for the entire water soluble aerosol sample, including both organic and inorganic compounds, where the surface tension was decreased by between 2% (71.2 mN/m) and 13% (63.3 mN/m).

  8. Chemical and physical properties of biomass burning aerosols and their CCN activity: A case study in Beijing, China.

    PubMed

    Wu, Zhijun; Zheng, Jing; Wang, Yu; Shang, Dongjie; Du, Zhoufei; Zhang, Yuanhang; Hu, Min

    2017-02-01

    Biomass burning emits large amounts of both trace gases and particles into the atmosphere. It plays a profound role in regional air quality and climate change. In the present study, an intensive campaign was carried out at an urban site in Beijing, China, in June 2014, which covered the winter wheat harvest season over the North China Plain (NCP). Meanwhile, two evident biomass-burning events were observed. A clear burst in ultrafine particles (below 100nm in diameter, PM1) and subsequent particle growth took place during the events. With the growth of the ultrafine particles, the organic fraction of PM1 increased significantly. The ratio of oxygen to carbon (O:C), which had an average value of 0.23±0.04, did not show an obvious enhancement, indicating that a significant chemical aging process of the biomass-burning aerosols was not observed during the course of events. This finding might have been due to the fact that the biomass-burning events occurred in the late afternoon and grew during the nighttime, which is associated with a low atmospheric oxidation capacity. On average, organics and black carbon (BC) were dominant in the biomass-burning aerosols, accounting for 60±10% and 18±3% of PM1. The high organic and BC fractions led to a significant suppression of particle hygroscopicity. Comparisons among hygroscopicity tandem differential mobility analyzer (HTDMA)-derived, cloud condensation nuclei counter (CCNc)-derived, and aerosol mass spectrometer-based hygroscopicity parameter (κ) values were consistent. The mean κ values of biomass-burning aerosols derived from both HTDMA and CCNc measurements were approximately 0.1, regardless of the particle size, indicating that the biomass-burning aerosols were less active. The burst in particle count during the biomass-burning events resulted in an increased number of cloud condensation nuclei (CCN) at supersaturation (SS)=0.2-0.8%.

  9. Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

    NASA Astrophysics Data System (ADS)

    Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

    2012-04-01

    New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

  10. COMMIT in 7-SEAS/BASELInE: Operation of and Observations from a Novel, Mobile Laboratory for Measuring In-Situ Properties of Aerosols and Gases

    NASA Technical Reports Server (NTRS)

    Pantina, Peter; Tsay, Si-Chee; Hsiao, Ta-Chih; Loftus, Adrian M.; Kuo, Ferret; Ou-Yang, Chang-Feng; Sayer, Andrew M.; Wang, Shen-Hsiang; Lin, Neng-Huei; Hsu, N. Christina; Janjai, Serm; Chantara, Somporn; Nguyen, Anh X.

    2016-01-01

    Trace gases and aerosols (particularly biomass-burning aerosols) have important implications for air quality and climate studies in Southeast Asia (SEA). This paper describes the purpose, operation, and datasets collected from NASA Goddard Space Flight Center's (NASA/GSFC) Chemical, Optical, and Microphysical Measurements of In-situ Troposphere (COMMIT) laboratory, a mobile platform designed to measure trace gases and optical/microphysical properties of naturally occurring and anthropogenic aerosols. More importantly, the laboratory houses a specialized humidification system to characterize hygroscopic growth/enhancement, a behavior that affects aerosol properties and cloud-aerosol interactions and is generally underrepresented in the current literature. A summary of the trace gas and optical/microphysical measurements is provided, along with additional detail and analysis of data collected from the hygroscopic system during the 2015 Seven South-East Asian Studies (7-SEAS) field campaign. The results suggest that data from the platform are reliable and will complement future studies of aerosols and air quality in SEA and other regions of interest.

  11. Properties of jet engine combustion particles during the PartEmis experiment: Hygroscopicity at subsaturated conditions

    NASA Astrophysics Data System (ADS)

    Gysel, M.; Nyeki, S.; Weingartner, E.; Baltensperger, U.; Giebl, H.; Hitzenberger, R.; Petzold, A.; Wilson, C. W.

    2003-06-01

    Hygroscopic properties of combustion particles were measured online with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) during PartEmis jet engine combustor experiments. The combustor was operated at old and modern cruise conditions with fuel sulfur contents (FSC) of 50, 410 and 1270 μg g-1, and hygroscopic growth factors (HGF) of particles with different dry diameters were investigated at relative humidities RH <= 95%. HGFs increased strongly with increasing FSC (HGF[95% RH, 50 nm, modern cruise] = 1.01 and 1.16 for low and high FSC, respectively), and decreased with increasing particle size at fixed FSC, whereas no significant difference was detected between old and modern cruise. HGFs agreed well with a two-parameter theoretical model which provided an estimate of the sulfuric acid content of dry particles, indicating a nearly linear dependence on FSC.

  12. 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... Devices § 884.4260 Hygroscopic Laminaria cervical dilator. (a) Identification. A hygroscopic Laminaria cervical dilator is a device designed to dilate (stretch open) the cervical os by cervical insertion of...

  13. 21 CFR 884.4260 - Hygroscopic Laminaria cervical dilator.

    Code of Federal Regulations, 2012 CFR

    2012-04-01

    ... 21 Food and Drugs 8 2012-04-01 2012-04-01 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...

  14. 21 CFR 884.4260 - Hygroscopic Laminaria cervical dilator.

    Code of Federal Regulations, 2014 CFR

    2014-04-01

    ... 21 Food and Drugs 8 2014-04-01 2014-04-01 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...

  15. 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...

  16. 21 CFR 884.4260 - Hygroscopic Laminaria cervical dilator.

    Code of Federal Regulations, 2013 CFR

    2013-04-01

    ... 21 Food and Drugs 8 2013-04-01 2013-04-01 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. Modeling of growth and evaporation effects on the extinction of 1.0-micron solar radiation traversing stratospheric sulfuric acid aerosols

    NASA Technical Reports Server (NTRS)

    Yue, G. K.; Deepak, A.

    1981-01-01

    The effects of growth and evaporation of stratospheric sulfuric acid aerosols on the extinction of solar radiation traversing such an aerosol medium are reported for the case of 1.0-micron solar radiation. Modeling results show that aerosol extinction is not very sensitive to the change of ambient water vapor concentration, but is sensitive to ambient temperature changes, especially at low ambient temperatures and high ambient water vapor concentration. A clarification is given of the effects of initial aerosol size distribution and composition on the change of aerosol extinction due to growth and evaporation processes. It is shown that experiments designed to observe solar radiation extinction of aerosols may also be applied to the determination of observed changes in aerosol optical properties, environmental parameters, or the physical and optical characteristics of sulfate aerosols.

  18. Measurements of submicron aerosols at the California-Mexico border during the Cal-Mex 2010 field campaign

    NASA Astrophysics Data System (ADS)

    Levy, Misti E.; Zhang, Renyi; Zheng, Jun; Tan, Haobo; Wang, Yuan; Molina, Luisa T.; Takahama, S.; Russell, L. M.; Li, Guohui

    2014-05-01

    We present measurements of submicron aerosols in Tijuana, Mexico during the Cal-Mex 2010 field campaign. A suite of aerosol instrumentations were deployed, including a hygroscopic-volatility tandem differential mobility analyzer (HV-TDMA), aerosol particle mass analyzer (APM), condensation particle counter (CPC), cavity ring-down spectrometer (CRDS), and nephelometer to measure the aerosol size distributions, effective density, hygroscopic growth factors (HGF), volatility growth factors (VGF), and optical properties. The average mass concentration of PM0.6 is 10.39 ± 7.61 μg m-3, and the derived average black carbon (BC) mass concentration is 2.87 ± 2.65 μg m-3. There is little new particle formation or particle growth during the day, and the mass loading is dominated by organic aerosols and BC, which on average are 37% and 27% of PM1.0, respectively. For four particle sizes of 46, 81, 151, and 240 nm, the measured particle effective density, HGFs, and VGFs exhibit distinct diurnal trends and size-dependence. For smaller particles (46 and 81 nm), the effective density distribution is unimodal during the day and night, signifying an internally mixed aerosol composition. In contrast, larger particles (151 and 240 nm) exhibit a bi-modal effective density distribution during the daytime, indicating an external mixture of fresh BC and organic aerosols, but a unimodal distribution during the night, corresponding to an internal mixture of BC and organic aerosols. The smaller particles show a noticeable diurnal trend in the effective density distribution, with the highest effective density (1.70 g cm-3) occurring shortly after midnight and the lowest value (0.90 g cm-3) occurring during the afternoon, corresponding most likely to primary organic aerosols and BC, respectively. Both HGFs and VGFs measured are strongly size-dependent. HGFs increase with increasing particle size, indicating that the largest particles are more hygroscopic. VGFs decrease with increasing

  19. CCN activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

    Tang, X.; Price, D.; Praske, E.; Vu, D.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-01-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3), contains less volatile compounds than the primary aliphatic amine (BA) aerosol. TMA + N2O5 form semi-volatile organics in low RH conditions that have κ ~ 0.20, indicative of slightly soluble organic material. As RH increases, several inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. Higher CCN activity (κ > 0.3) was also observed for humid BA+N2O5 aerosols compared with dry aerosol (κ ~ 0.2), as a result of the formation of inorganic salts such as NH4NO3 and butylamine nitrate (C4H11N · HNO3). Compared with TMA, BA+N2O5 reactions produce more volatile aerosols. The BA+N2O5 aerosol products under humid experiments were found to be very sensitive to the temperature within the stream-wise continuous flow thermal gradient CCN counter. The CCN counter, when set above a 21 °C temperature difference, evaporates BA+N2O5 aerosol formed at RH ≥ 30%; κ ranges from 0.4 to 0.7 and is dependent on the instrument supersaturation (ss) settings. The aerosol behaves non-ideally, hence simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems κ ranges from 0.2 < κ < 0.7. This work indicates that

  20. Formation and Growth of New Organic Aerosol Particles over the Deepwater Horizon Oil Spill

    NASA Astrophysics Data System (ADS)

    Brock, C. A.; Murphy, D. M.; Bahreini, R.; Middlebrook, A. M.; De Gouw, J. A.

    2011-12-01

    Aerosol size distributions were measured in June 2010 downwind of the surface oil slick produced by the Deepwater Horizon oil spill in the Gulf of Mexico. Rapid condensation of partially oxidized hydrocarbons was responsible for formation of a plume of secondary organic aerosol downwind of the spill region. New particles were nucleated upwind of the freshest surface oil but downwind of oil that surfaced less than 100 hours previously. These new particles grew by condensation at rates of ~20 nm hr-1; preexisting accumulation mode particles grew by ~10 nm hr-1. The gas-phase concentration of a condensing species necessary to support the observed growth rate assuming irreversible adsorption with unit accommodation coefficient is estimated to be ~0.04-0.09 μg m-3 (~3-8 pptv). The ratio of growth rates for newly formed particles to accumulation mode particles was consistent within error limits with irreversible condensation. Because new particle formation did not occur in areas away from the <100 hr-old oil slick, these results indicate that the oxidation products of VOC species, probably C14-C16 compounds, were directly involved in the growth of the new particles. While a unique and extreme environment, the oil spill plume provides insight into similar processes that may occur in urban and industrial areas where petrochemical products are produced and consumed.

  1. 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.

  2. RELATIONSHIP BETWEEN MEASURED WATER VAPOR GROWTH AND CHEMISTRY OF ATMOSPHERIC AEROSOL FOR GRAND CANYON, ARIZONA, IN WINTER 1990.

    EPA Science Inventory

    Size-resolved aerosol growth measurements (growth = moist particle diameter/dry particle diameter) and chemical composition monitoring were conducted during a 3 month period in the winter of 1990 at the South Rim of Grand Canyon National Park, AZ as part of the Navajo Generating ...

  3. Fog Induced Aerosol Modification Observed by AERONET, Including Occurrences During Major Air Pollution Events

    NASA Astrophysics Data System (ADS)

    Eck, T. F.; Holben, B. N.; Reid, J. S.; Giles, D. M.; Rivas, M.; Singh, R. P.; Tripathi, S. N.; Bruegge, C. J.; Li, Z.; Platnick, S. E.; Arnold, T.; Ferrare, R. A.; Hostetler, C. A.; Burton, S. P.; Kim, J.; Kim, Y. J.; Sinyuk, A.; Dubovik, O.; Arola, A. T.; Schafer, J.; Artaxo, P.; Smirnov, A.; Chen, H.; Goloub, P.

    2015-12-01

    The modification of aerosol optical properties due to interaction with fog is examined from measurements made by sun/sky radiometers at several AERONET sites. Retrieved total column volume size distributions for cases identified as aerosol modified by fog often show very a large 'middle mode' submicron radius (~0.4 to 0.5 microns), which is typically seen as a component of a bimodal sub-micron distribution. These middle mode sized particles are often called cloud-processed or residual aerosol. This bimodal accumulation mode distribution may be due to one mode (the larger one) from fog-processed aerosol and the other from interstitial aerosol, or possibly from two different aerosol species (differing chemical composition) with differing hygroscopic growth factors. The size of the fine mode particles from AERONET retrieved for these cases exceeds the size of sub-micron sized particles retrieved for nearly all other aerosol types, suggesting significant modification of aerosols within the fog or cloud environment. In-situ measured aerosol size distributions made during other fog events are compared to the AERONET retrievals, and show close agreement in the residual mode particle size. Almucantar retrievals are analyzed from the Kanpur site in the Indo-Gangetic Plain in India (fog in January), Beijing (fog in winter), Fresno, CA in the San Joaquin Valley (fog in winter), South Korea (Yellow Sea fog in spring), Arica on the northern coast of Chile (stratocumulus), and several other sites with aerosol observations made after fog dissipated. Additionally, several major air pollution events are discussed where extremely high aerosol concentrations were measured at the surface and during which fog also occurred, resulting in the detection very large fine mode aerosols (residual mode) from AERONET retrievals in some of these events. Low wind speeds that occurred during these events were conducive to both pollutant accumulation and also fog formation. The presence of fog then

  4. Study of aerosol optical properties at Kunming in southwest China and long-range transport of biomass burning aerosols from North Burma

    NASA Astrophysics Data System (ADS)

    Zhu, J.; Xia, X.; Che, H.; Wang, J.; Zhang, J.; Duan, Y.

    2016-03-01

    Seasonal variation of aerosol optical properties and dominant aerosol types at Kunming (KM), an urban site in southwest China, is characterized. Substantial influences of the hygroscopic growth and long-range transport of biomass burning (BB) aerosols on aerosol optical properties at KM are revealed. These results are derived from a detailed analysis of (a) aerosol optical properties (e.g. aerosol optical depth (AOD), columnar water vapor (CWV), single scattering albedo (SSA) and size distribution) retrieved from sunphotometer measurements during March 2012-August 2013, (b) satellite AOD and active fire products, (c) the attenuated backscatter profiles from the space-born lidar, and (d) the back-trajectories. The mean AOD440nm and extinction Angstrom exponent (EAE440 - 870) at KM are 0.42 ± 0.32 and 1.25 ± 0.35, respectively. Seasonally, high AOD440nm (0.51 ± 0.34), low EAE440 - 870 (1.06 ± 0.34) and high CWV (4.25 ± 0.97 cm) during the wet season (May - October) contrast with their counterparts 0.17 ± 0.11, 1.40 ± 0.31 and 1.91 ± 0.37 cm during the major dry season (November-February) and 0.53 ± 0.29, 1.39 ± 0.19, and 2.66 ± 0.44 cm in the late dry season (March-April). These contrasts between wet and major dry season, together with the finding that the fine mode radius increases significantly with AOD during the wet season, suggest the importance of the aerosol hygroscopic growth in regulating the seasonal variation of aerosol properties. BB and Urban/Industrial (UI) aerosols are two major aerosol types. Back trajectory analysis shows that airflows on clean days during the major dry season are often from west of KM where the AOD is low. In contrast, air masses on polluted days are from west (in late dry season) and east (in wet season) of KM where the AOD is often large. BB air mass is found mostly originated from North Burma where BB aerosols are lifted upward to 5 km and then subsequently transported to southwest China via prevailing westerly winds.

  5. Laboratory study on the hygroscopic behavior of external and internal C2-C4 dicarboxylic acid-NaCl mixtures.

    PubMed

    Ma, Qingxin; Ma, Jinzhu; Liu, Chang; Lai, Chengyue; He, Hong

    2013-09-17

    Atmospheric aerosol is usually found to be a mixture of various inorganic and organic components in field measurements, whereas the effect of this mixing state on the hygroscopicity of aerosol particles has remained unknown. In this study, the hygroscopic behavior of mixtures of C2-C4 dicarboxylic acids and NaCl was investigated. For both externally and internally mixed malonic acid-NaCl and succinic acid-NaCl particles, correlation between water content and chemical composition was observed and the water content of these mixtures at relative humidity (RH) above 80% can be well predicted by the Zdanovskii-Stokes-Robinson (ZSR) method. In contrast, a nonlinear relation between the total water content of the mixtures and the water content of each chemical composition separately was found for oxalic acid-NaCl mixtures. Compared to the values predicted by the ZSR method, the dissolution of oxalic acid in external mixtures resulted in an increase in the total water content, whereas the formation of less hygroscopic disodium oxalate in internal mixtures led to a significant decrease in the total water content. Furthermore, we found that the hygroscopicity of the sodium dicarboxylate plays a critical role in determining the aqueous chemistry of dicarboxylic acid-NaCl mixtures during the humidifying and dehumidifying process. It was also found that the hydration of oxalic acid and the deliquescence of NaCl did not change in external oxalic acid-NaCl mixtures. The deliquescence relative humidity (DRHs) for both malonic acid and NaCl decreased in both external and internal mixtures. These results could help in understanding the conversion processes of dicarboxylic acids to dicarboxylate salts, as well as the substitution of Cl by oxalate in the atmosphere. It was demonstrated that the effect of coexisting components on the hygroscopic behavior of mixed aerosols should not be neglected.

  6. Effect of humidity and particle hygroscopicity on the mass loading capacity of high efficiency particulate air (HEPA) filters

    SciTech Connect

    Gupta, A.; Biswas, P. ); Monson, P.R. ); Novick, V.J. )

    1993-07-01

    The effect of humidity, particle hygroscopicity, and size on the mass loading capacity of glass fiber high efficiency particulate air filters was studied. Above the deliquescent point, the pressure drop across the filter increased nonlinearly with areal loading density (mass collected/filtration area) of a NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or nonhygroscopic particle mass loadings. The specific cake resistance K[sub 2] was computed for different test conditions and used as a measure of the mass loading capacity. K[sub 2] was found to decrease with increasing humidity for nonhygroscopic aluminum oxide particles and for 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) was derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the nonhygroscopic 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. 17 refs., 6 figs., 3 tabs.

  7. A comprehensive evaluation of water uptake on atmospherically relevant mineral surfaces: DRIFT spectroscopy, thermogravimetric analysis and aerosol growth measurements

    NASA Astrophysics Data System (ADS)

    Gustafsson, R. J.; Orlov, A.; Badger, C. L.; Griffiths, P. T.; Cox, R. A.; Lambert, R. M.

    2005-08-01

    The hygroscopicity of mineral aerosol samples has been examined by three independent methods: diffuse reflectance infrared Fourier transform spectroscopy, thermogravimetric analysis and differential mobility analysis. All three methods allow an evaluation of the water coverage of two samples, CaCO3 and Arizona Test dust, as a function of relative humidity. For the first time, a correlation between absolute gravimetric measurements and the other two (indirect) methods has been established. Water uptake isotherms were reliably determined for both solids which at 298 K and 80% relative humidity exhibited similar coverages of ~4 monolayers. However, the behaviour at low relative humidity was markedly different in the two cases, with Arizona Test Dust showing a substantially higher affinity for water in the contact layer. This is understandable in terms of the chemical composition of these two materials. The mobility analysis results are in good accord with field observations and with our own spectroscopic and gravimetric measurements. These findings are of value for an improved understanding of atmospheric chemical processes.

  8. A comprehensive evaluation of water uptake on atmospherically relevant mineral surfaces: DRIFT spectroscopy, thermogravimetric analysis and aerosol growth measurements

    NASA Astrophysics Data System (ADS)

    Gustafsson, R. J.; Orlov, A.; Badger, C. L.; Griffiths, P. T.; Cox, R. A.; Lambert, R. M.

    2005-12-01

    The hygroscopicity of mineral aerosol samples has been examined by three independent methods: diffuse reflectance infrared Fourier transform spectroscopy, thermogravimetric analysis and differential mobility analysis. All three methods allow an evaluation of the water coverage of two samples, CaCO3 and Arizona Test dust, as a function of relative humidity. For the first time, a correlation between absolute gravimetric measurements and the other two (indirect) methods has been established. Water uptake isotherms were reliably determined for both solids which at 298 K and 80% relative humidity exhibited similar coverages of ~4 monolayers. However, the behaviour at low relative humidity was markedly different in the two cases, with Arizona Test Dust showing a substantially higher affinity for water in the contact layer. This is understandable in terms of the chemical composition of these two materials. The mobility analysis results are in good accord with field observations and with our own spectroscopic and gravimetric measurements. These findings are of value for an understanding of atmospheric chemical processes.

  9. Cloud condensation nuclei (CCN) activity of aliphatic amine secondary aerosol

    NASA Astrophysics Data System (ADS)

    Tang, X.; Price, D.; Praske, E.; Vu, D. N.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-06-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g., hydroxyl radical and nitrate radical). The particle can contain both secondary organic aerosol (SOA) and inorganic salts. The ratio of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ, ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3) contains less volatile compounds than the primary aliphatic amine (BA) aerosol. As relative humidity (RH) increases, inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. The humid BA + N2O5 aerosol products were found to be very sensitive to the temperature at which the measurements were made within the streamwise continuous-flow thermal gradient CCN counter; κ ranges from 0.4 to 0.7 dependent on the instrument supersaturation (ss) settings. The variance of the measured aerosol κ values indicates that simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems' κ ranges within 0.2 < κ < 0.7. This work indicates that aerosols formed via nighttime reactions with amines are likely to produce hygroscopic and volatile aerosol, whereas photochemical reactions with OH produce secondary organic aerosol of lower CCN activity. The contributions of semivolatile secondary organic and inorganic material from aliphatic amines must be considered for accurate hygroscopicity and CCN predictions from aliphatic amine systems.

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

    NASA Astrophysics Data System (ADS)

    Orozco, Daniel

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

  11. CCN activity of Amazonian aerosols during GoAmazon 2014/5

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    During the Green Ocean Amazon (GoAmazon) 2014/5 campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 70-km downwind of the city of Manaus (pop. 2 million) from March 12, 2014 to March 3, 2015. Air masses arriving at the T3 site ranged from near natural conditions to strongly impacted by urban pollution and/or biomass burning. Particle hygroscopicity and chemical mixing state were derived from the size resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol was then calculated from the particle hygroscopicity and composition concurrently measured by an Aerosol Mass Spectrometer (AMS) or an Aerosol Chemical Speciation Monitor (ACSM). On average, particle hygroscopicity increased with increasing particle diameter, mainly due to an increasing sulfate volume fraction. The diel variations of particle hygroscopicity, mixing state, and organic hygroscopicity were strongly influenced by a combination of emissions, photochemical oxidation, and the development of boundary layer. The diel variations are examined for different air masses during both wet and dry seasons. The impact of urban pollution and biomass burning on both organic and particle hygroscopicities will be presented. The organic hygroscopicity is investigated against its sources and the oxidation levels (e.g., O:C atomic ratio) for improved understanding of its variations and parameterizations in global models.

  12. 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.

  13. 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.

  14. Hygroscopic properties of magnetic recording tape

    NASA Technical Reports Server (NTRS)

    Cuddihy, E. F.

    1976-01-01

    Relative humidity has been recognized as an important environmental factor in many head-tape interface phenomena such as headwear, friction, staining, and tape shed. Accordingly, the relative humidity is usually specified in many applications of tape use, especially when tape recorders are enclosed in hermetically sealed cases. Normally, the relative humidity is believed regulated by humidification of the fill gas to the specification relative humidity. This study demonstrates that the internal relative humidity in a sealed case is completely controlled by the time-dpendence of the hygroscopic properties of the pack of magnetic recording tape. Differences are found in the hygroscopic properties of the same brand of tape, which apparently result from aging, and which may have an effect on the long-term humidity-regulating behavior in a sealed case, and on the occurrence of head-tape interface phenomena from the long-term use of the tape. Results are presented on the basic hygroscopic properties of magnetic tape, its humidity-regulating behavior in a sealed case, and a theoretical commentary on the relative humidity dependence of head-wear by tape, is included.

  15. Cloud activation properties of organic aerosols observed at an urban site during CalNex-LA

    NASA Astrophysics Data System (ADS)

    Mei, F.; Hayes, P. L.; Ortega, A. M.; Jimenez, J.; Wang, J.

    2010-12-01

    hygroscopicity (κ, Petters and Kreidenweis, 2007, ACP) derived from the size-resolved CCN measurements ranges from 0.2 to 0.3 under the range of measured supersaturations. The derived particle κ increases with increasing particle diameter, which is consistent with observed decrease in organics volume fraction as particle size increases from 100 nm to 300 nm. Based on the particle hygroscopicity and aerosol chemical composition, the organics hygroscopicity (κOrg) was derived as 0.18±0.06, in agreement with κ of organics with the same O:C ratio reported in earlier studies (Chang et al. 2010 ACP; Duplissy et.al 2010 ACPD). Whereas organics strongly influence particle critical supersaturation, size-classified organic particles exhibit similar growth kinetics when compared to (NH4)2SO4 particles with the same critical supersaturation, suggesting aerosol organics observed during CalNex do not inhibit droplet growth through reducing the mass accommodation coefficient of water vapor.

  16. 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

  17. Phase, composition and growth mechanism for secondary organic aerosol from the ozonolysis of α-cedrene

    NASA Astrophysics Data System (ADS)

    Zhao, Y.; Wingen, L. M.; Perraud, V.; Finlayson-Pitts, B. J.

    2015-12-01

    Sesquiterpenes are an important class of biogenic volatile organic compounds (BVOCs) and have a high secondary organic aerosol (SOA) forming potential. However, SOA formation from sesquiterpene oxidation has received less attention compared to other BVOCs such as monoterpenes, and the underlying mechanisms remain poorly understood. In this work, we present a comprehensive experimental investigation of the ozonolysis of α-cedrene both in a glass flow reactor (27-44 s reaction times) and in static Teflon chambers (30-60 min reaction times). The SOA was collected by impaction or filters, followed by analysis using attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR) and electrospray ionization mass spectrometry (ESI-MS), or measured on line using direct analysis in real time (DART-MS) and aerosol mass spectrometry (AMS). The slow evaporation of 2-ethylhexyl nitrate that was incorporated into the SOA during its formation and growth gives an estimated diffusion coefficient of 3 × 10-15 cm2 s-1 and shows that SOA is a highly viscous semi-solid. Possible structures of four newly observed low molecular weight (MW ≤ 300 Da) reaction products with higher oxygen content than those previously reported were identified. High molecular weight (HMW) products formed in the early stages of the oxidation have structures consistent with aldol condensation products, peroxyhemiacetals, and esters. The size-dependent distributions of HMW products in the SOA, as well as the effects of stabilized Criegee intermediate (SCI) scavengers on HMW products and particle formation, confirm that HMW products and reactions of Criegee intermediates play a crucial role in early stages of particle formation. Our studies provide new insights into mechanisms of SOA formation and growth in α-cedrene ozonolysis and the important role of sesquiterpenes in new particle formation as suggested by field measurements.

  18. Phase, composition, and growth mechanism for secondary organic aerosol from the ozonolysis of α-cedrene

    NASA Astrophysics Data System (ADS)

    Zhao, Yue; Wingen, Lisa M.; Perraud, Véronique; Finlayson-Pitts, Barbara J.

    2016-03-01

    Sesquiterpenes are an important class of biogenic volatile organic compounds (BVOCs) and have a high secondary organic aerosol (SOA) forming potential. However, SOA formation from sesquiterpene oxidation has received less attention compared to other BVOCs such as monoterpenes, and the underlying mechanisms remain poorly understood. In this work, we present a comprehensive experimental investigation of the ozonolysis of α-cedrene both in a glass flow reactor (27-44 s reaction times) and in static Teflon chambers (30-60 min reaction times). The SOA was collected by impaction or filters, followed by analysis using attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy and electrospray ionization mass spectrometry (ESI-MS), or measured online using direct analysis in real-time mass spectrometry (DART-MS) and aerosol mass spectrometry (AMS). The slow evaporation of 2-ethylhexyl nitrate that was incorporated into the SOA during its formation and growth gives an estimated diffusion coefficient of 3 × 10-15 cm2 s-1 and shows that SOA is a highly viscous semisolid. Possible structures of four newly observed low molecular weight (MW ≤ 300 Da) reaction products with higher oxygen content than those previously reported were identified. High molecular weight (HMW) products formed in the early stages of the oxidation have structures consistent with aldol condensation products, peroxyhemiacetals, and esters. The size-dependent distributions of HMW products in the SOA, as well as the effects of stabilized Criegee intermediate (SCI) scavengers on HMW products and particle formation, confirm that HMW products and reactions of SCI play a crucial role in early stages of particle formation. Our studies provide new insights into mechanisms of SOA formation and growth in α-cedrene ozonolysis and the important role of sesquiterpenes in new particle formation as suggested by field measurements.

  19. Aerosol-CFD modelling of ultrafine and black carbon particle emission, dilution, and growth near roadways

    NASA Astrophysics Data System (ADS)

    Huang, L.; Gong, S. L.; Gordon, M.; Liggio, J.; Staebler, R. M.; Stroud, C. A.; Lu, G.; Mihele, C.; Brook, J. R.; Jia, C. Q.

    2014-05-01

    Many studies have shown that on-road vehicle emissions are the dominant source of ultrafine particles (UFP; diameter < 100 nm) in urban areas and near-roadway environments. In order to advance our knowledge on the complex interactions and competition among atmospheric dilution, dispersion and dynamics of UFPs, an aerosol dynamics-CFD coupled model is developed and validated against field measurements. A unique approach of applying periodic boundary conditions is proposed to model pollutant dispersion and dynamics in one unified domain from the tailpipe level to the ambient near-road environment. This approach significantly reduces the size of the computational domain, and therefore, allows fast simulation of multiple scenarios. The model is validated against measured turbulent kinetic energy (TKE) and pollution gradients near a major highway. Through a model sensitivity analysis, the relative importance of individual aerosol dynamical processes on the total particle number concentration (N) and particle number-size distribution (PSD) near a highway is investigated. The results demonstrate that (1) coagulation has a negligible effect on N and particle growth, (2) binary homogeneous nucleation (BHN) of H2SO4-H2O is likely responsible for elevated N closest to the road, (3) N and particle growth are very sensitive to the condensation of semi-volatile organics (SVOCs), particle dry deposition, and the interaction between these processes. The results also indicate that, without the proper treatment of atmospheric boundary layer (i.e. its wind profile and turbulence quantities), the nucleation rate would be underestimated by a factor of 5 in the vehicle wake region due to overestimated mixing. Therefore, introducing ABL conditions to activity-based emission models may potentially improve their performance in estimating UFP traffic emissions.

  20. Sensitivity of scattering and absorbing aerosol direct radiative forcing to physical climate factors

    NASA Astrophysics Data System (ADS)

    Ocko, Ilissa B.; Ramaswamy, V.; Ginoux, Paul; Ming, Yi; Horowitz, Larry W.

    2012-10-01

    The direct radiative forcing of the climate system includes effects due to scattering and absorbing aerosols. This study explores how important physical climate characteristics contribute to the magnitudes of the direct radiative forcings (DRF) from anthropogenic sulfate, black carbon, and organic carbon. For this purpose, we employ the GFDL CM2.1 global climate model, which has reasonable aerosol concentrations and reconstruction of twentieth-century climate change. Sulfate and carbonaceous aerosols constitute the most important anthropogenic aerosol perturbations to the climate system and provide striking contrasts between primarily scattering (sulfate and organic carbon) and primarily absorbing (black carbon) species. The quantitative roles of cloud coverage, surface albedo, and relative humidity in governing the sign and magnitude of all-sky top-of-atmosphere (TOA) forcings are examined. Clouds reduce the global mean sulfate TOA DRF by almost 50%, reduce the global mean organic carbon TOA DRF by more than 30%, and increase the global mean black carbon TOA DRF by almost 80%. Sulfate forcing is increased by over 50% as a result of hygroscopic growth, while high-albedo surfaces are found to have only a minor (less than 10%) impact on all global mean forcings. Although the radiative forcing magnitudes are subject to uncertainties in the state of mixing of the aerosol species, it is clear that fundamental physical climate characteristics play a large role in governing aerosol direct radiative forcing magnitudes.

  1. Synergetic formation of secondary inorganic and organic aerosol: effect of SO2 and NH3 on particle formation and growth

    NASA Astrophysics Data System (ADS)

    Chu, Biwu; Zhang, Xiao; Liu, Yongchun; He, Hong; Sun, Yele; Jiang, Jingkun; Li, Junhua; Hao, Jiming

    2016-11-01

    The effects of SO2 and NH3 on secondary organic aerosol formation have rarely been investigated together, while the interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain. Here we studied the effects of SO2 and NH3 on secondary aerosol formation in the photooxidation system of toluene/NOx in the presence or absence of Al2O3 seed aerosols in a 2 m3 smog chamber. The presence of SO2 increased new particle formation and particle growth significantly, regardless of whether NH3 was present. Sulfate, organic aerosol, nitrate, and ammonium were all found to increase linearly with increasing SO2 concentrations. The increases in these four species were more obvious under NH3-rich conditions, and the generation of nitrate, ammonium, and organic aerosol increased more significantly than sulfate with respect to SO2 concentration, while sulfate was the most sensitive species under NH3-poor conditions. The synergistic effects between SO2 and NH3 in the heterogeneous process contributed greatly to secondary aerosol formation. Specifically, the generation of NH4NO3 was found to be highly dependent on the surface area concentration of suspended particles, and increased most significantly with SO2 concentration among the four species under NH3-rich conditions. Meanwhile, the absorbed NH3 might provide a liquid surface layer for the absorption and subsequent reaction of SO2 and organic products and, therefore, enhance sulfate and secondary organic aerosol (SOA) formation. This effect mainly occurred in the heterogeneous process and resulted in a significantly higher growth rate of seed aerosols compared to without NH3. By applying positive matrix factorisation (PMF) analysis to the AMS data, two factors were identified for the generated SOA. One factor, assigned to less-oxidised organic aerosol and some oligomers, increased with increasing SO2 under NH3-poor conditions, mainly due to the well-known acid catalytic effect of

  2. Characterizing the Vertical Distribution of Aerosols Over the ARM SGP Site

    SciTech Connect

    Richard Ferrare, Connor Flynn, David Turner

    2009-05-05

    This project focused on: 1) evaluating the performance of the DOE ARM SGP Raman lidar system in measuring profiles of water vapor and aerosols, and 2) the use of the Raman lidar measurements of aerosol and water vapor profiles for assessing the vertical distribution of aerosols and water vapor simulated by global transport models and examining diurnal variability of aerosols and water vapor. The highest aerosol extinction was generally observed close to the surface during the nighttime just prior to sunrise. The high values of aerosol extinction are most likely associated with increased scattering by hygroscopic aerosols, since the corresponding average relative humidity values were above 70%. After sunrise, relative humidity and aerosol extinction below 500 m decreased with the growth in the daytime convective boundary layer. The largest aerosol extinction for altitudes above 1 km occurred during the early afternoon most likely as a result of the increase in relative humidity. The water vapor mixing ratio profiles generally showed smaller variations with altitude between day and night. We also compared simultaneous measurements of relative humidity, aerosol extinction, and aerosol optical thickness derived from the ARM SGP Raman lidar and in situ instruments on board a small aircraft flown routinely over the ARM SGP site. In contrast, the differences between the CARL and IAP aerosol extinction measurements are considerably larger. Aerosol extinction derived from the IAP measurements is, on average, about 30-40% less than values derived from the Raman lidar. The reasons for this difference are not clear, but may be related to the corrections for supermicron scattering and relative humidity that were applied to the IAP data. The investigators on this project helped to set up a major field mission (2003 Aerosol IOP) over the DOE ARM SGP site. One of the goals of the mission was to further evaluate the aerosol and water vapor retrievals from this lidar system

  3. Multi-peak accumulation and coarse modes observed from AERONET retrieved aerosol volume size distribution in Beijing

    NASA Astrophysics Data System (ADS)

    Zhang, Ying; Li, Zhengqiang; Zhang, Yuhuan; Chen, Yu; Cuesta, Juan; Ma, Yan

    2016-08-01

    We present characteristic peaks of atmospheric columnar aerosol volume size distribution retrieved from the AErosol RObotic NETwork (AERONET) ground-based Sun-sky radiometer observation, and their correlations with aerosol optical properties and meteorological conditions in Beijing over 2013. The results show that the aerosol volume particle size distribution (VPSD) can be decomposed into up to four characteristic peaks, located in accumulation and coarse modes, respectively. The mean center radii of extra peaks in accumulation and coarse modes locate around 0.28 (±0.09) to 0.38 (±0.11) and 1.25 (±0.56) to 1.47 (±0.30) μm, respectively. The multi-peak size distributions are found in different aerosol loading conditions, with the mean aerosol optical depth (440 nm) of 0.58, 0.49, 1.18 and 1.04 for 2-, 3-I/II and 4-peak VPSD types, while the correspondingly mean relative humidity values are 58, 54, 72 and 67 %, respectively. The results also show the significant increase (from 0.25 to 0.40 μm) of the mean extra peak median radius in the accumulation mode for the 3-peak-II cases, which agrees with aerosol hygroscopic growth related to relative humidity and/or cloud or fog processing.

  4. Fog-induced variations in aerosol optical and physical properties over the Indo-Gangetic Basin and impact to aerosol radiative forcing

    NASA Astrophysics Data System (ADS)

    Das, S. K.; Jayaraman, A.; Misra, A.

    2008-06-01

    A detailed study on the changes in aerosol physical and optical properties during fog events were made in December 2004 at Hissar (29.13° N, 75.70° E), a city located in the Indo-Gangetic basin. The visible aerosol optical depth was relatively low (0.3) during the initial days, which, however, increased (0.86) as the month progressed. The increasing aerosol amount, the decreasing surface temperature and a higher relative humidity condition were found favoring the formation of fog. The fog event is also found to alter the aerosol size distribution. An increase in the number concentration of the nucleation mode (radius<0.1 μm) particles, along with a decrease in the mode radius showed the formation of freshly nucleated aerosols. In the case of accumulation mode (0.1 μmhygroscopic and coagulation growth of particles. The observed aerosol optical depth spectra are model fitted to infer the aerosol components which are further used to compute the aerosol radiative forcing. The top of the atmosphere forcing is found to increase during foggy days due to large backscattering of radiation back to space. It is also shown that during foggy days, as the day progresses the RH value decreases, which reduces the forcing value while the increasing solar elevation increases the forcing value. Thus the fog event which prolongs longer into the daytime has a stronger effect on the diurnally averaged aerosol radiative forcing than those events which are confined only to the early morning hours.

  5. Uncertainties of simulated aerosol optical properties induced by assumptions on aerosol physical and chemical properties: An AQMEII-2 perspective

    NASA Astrophysics Data System (ADS)

    Curci, G.; Hogrefe, C.; Bianconi, R.; Im, U.; Balzarini, A.; Baró, R.; Brunner, D.; Forkel, R.; Giordano, L.; Hirtl, M.; Honzak, L.; Jiménez-Guerrero, P.; Knote, C.; Langer, M.; Makar, P. A.; Pirovano, G.; Pérez, J. L.; San José, R.; Syrakov, D.; Tuccella, P.; Werhahn, J.; Wolke, R.; Žabkar, R.; Zhang, J.; Galmarini, S.

    2015-08-01

    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 intercomparison, we used the bulk mass profiles of aerosol chemical species sampled over the locations of AERONET stations across Europe and North America to calculate the aerosol optical properties under a range of common assumptions for all models. Several simulations with parameters perturbed within a range of observed values are carried out for July 2010 and compared in order to infer the assumptions that have the largest impact on the calculated aerosol optical properties. We calculate that the most important factor of uncertainty is the assumption about the mixing state, for which we estimate an uncertainty of 30-35% on the simulated aerosol optical depth (AOD) and single scattering albedo (SSA). The choice of the core composition in the core-shell representation is of minor importance for calculation of AOD, while it is critical for the SSA. The uncertainty introduced by the choice of mixing state choice on the calculation of the asymmetry parameter is the order of 10%. Other factors of uncertainty tested here have a maximum average impact of 10% each on calculated AOD, and an impact of a few percent on SSA and g. It is thus recommended to focus further research on a more accurate representation of the aerosol mixing state in models, in order to have a less uncertain simulation of the related optical properties.

  6. oVOC production from tropospheric alkyne oxidation and contribution to aerosol formation and growth

    NASA Astrophysics Data System (ADS)

    Goodall, Iain

    2013-04-01

    Ethyne (C2H2) is one of the simplest volatile organic compounds (VOC) and is predominantly emitted via anthropogenic processes and reacts with nitrogen oxides (NOx) in the presence of sunlight to form tropospheric ozone (O3). The dominant oxidation product of ethyne is the dicarbonyl species glyoxal (CHOCHO), which is thought to be a significant contributor to secondary organic aerosol (SOA) formation via irreversible oligomerisation reactions upon the surface of hydrated aerosol particulates and within cloud droplets. A series of chamber experiments were performed at the EUPHORE facility (Valencia, Spain) to study the atmospheric oxidation of ethyne, to determine oxidation product yields and to monitor SOA formation and growth by dicarbonyl oligomerisation. A Proton Transfer Reaction-Time of Flight- Mass Spectrometer (PTR-ToF-MS) was deployed by the University of Leicester to monitor precursor decay and the subsequent evolution of any gas-phase oxidised volatile organic compounds (oVOC). This was further complemented by a Broadband Cavity Enhanced Absorption Spectrometer (BBCEAS) for specific dicarbonyl and NO2 measurements. Aqueous extracts of chamber SOA were taken from filters collected during the experiments and subsequently analysed offline. The work explores the yields of low molecular weight products of ethyne oxidation for light and dark reactions, with varying levels of NOx and OH. Novel experiments were performed under atmospherically relevant conditions utilising natural lighting rather than artificial lighting. Reaction yields have been assessed with the aim of contributing to the ethyne and glyoxal mechanisms in the Master Chemical Mechanism (MCM; http://mcm.leeds.ac.uk/MCM), and have been compared with previously reported values determined from experiments performed under artificial lighting conditions.

  7. Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Martin, S. T.; Koop, T.; Pöschl, U.

    2009-12-01

    Interactions with water are crucial for the properties, transformation and climate effects of atmospheric aerosols. Here we present a conceptual framework for the interaction of amorphous aerosol particles with water vapor, outlining characteristic features and differences in comparison to crystalline particles. We used a hygroscopicity tandem differential mobility analyzer (H-TDMA) to characterize the hydration and dehydration of crystalline ammonium sulfate, amorphous oxalic acid and amorphous levoglucosan particles (diameter ~100 nm, relative humidity 5-95% at 298 K). The experimental data and accompanying Köhler model calculations provide new insights into particle microstructure, surface adsorption, bulk absorption, phase transitions and hygroscopic growth. The results of these and related investigations lead to the following conclusions: (1) Many organic substances, including carboxylic acids, carbohydrates and proteins, tend to form amorphous rather than crystalline phases upon drying of aqueous solution droplets. Depending on viscosity and microstructure, the amorphous phases can be classified as glasses, rubbers, gels or viscous liquids. (2) Amorphous organic substances tend to absorb water vapor and undergo gradual deliquescence and hygroscopic growth at lower relative humidity than their crystalline counterparts. (3) In the course of hydration and dehydration, certain organic substances can form rubber- or gel-like structures (supramolecular networks) and undergo transitions between swollen and collapsed network structures. (4) Organic gels or (semi-)solid amorphous shells (glassy, rubbery, ultra-viscous) with low molecular diffusivity can kinetically limit the uptake and release of water and may influence the hygroscopic growth and activation of aerosol particles as cloud condensation nuclei (CCN) and ice nuclei (IN). Moreover, (semi-)solid amorphous phases may influence the uptake of gaseous photo-oxidants and the chemical transformation and aging of

  8. Aerosol characteristics in Phimai, Thailand determined by continuous observation with a polarization sensitive Mie-Raman lidar and a sky radiometer

    NASA Astrophysics Data System (ADS)

    Sugimoto, Nobuo; Shimizu, Atsushi; Nishizawa, Tomoaki; Matsui, Ichiro; Jin, Yoshitaka; Khatri, Pradeep; Irie, Hitoshi; Takamura, Tamio; Aoki, Kazuma; Thana, Boossarasiri

    2015-06-01

    Distributions and optical characteristics of aerosols were continuously observed with a polarization-sensitive (532 nm), Mie-scattering (532 and 1064 nm) and Raman-scattering (607 nm) lidar and a sky radiometer in Phimai, Thailand. Polarization lidar measurements indicated that high concentration plumes of spherical aerosols considered as biomass burning smoke were often observed in the dry season. Plumes of non-spherical aerosols considered as long-range transported soil dust from Africa, the Middle East, or Northeast Asia were occasionally observed. Furthermore, low-concentration non-spherical aerosols were almost always observed in the atmospheric mixing layer. Extinction coefficient profiles of spherical aerosols and non-spherical dust exhibited different diurnal variations, and spherical aerosols including smoke were distributed in higher altitudes in the mixing layer and residual layer. The difference can be explained by hygroscopic growth of smoke particles and buoyancy of the smoke. Analysis of seasonal variations of optical properties derived from the Raman lidar and the sky radiometer confirmed that the lidar ratio, aerosol optical depth, and Angstrom exponent were higher in the dry season (October-May) and lower in the wet season (June-September). The single scattering albedo was lower in the dry season. These seasonal variations are explained by frequent biomass burning in the dry season consistent with previous studies in Southeast Asian region. At the same time, the present work confirmed that soil dust was a major aerosol component in Phimai, Thailand.

  9. Aircraft- and ground-based assessment of the CCN-AOD relationship and implications on model analysis of ACI and underlying aerosol processes

    NASA Astrophysics Data System (ADS)

    Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Lathem, T. L.; Redemann, J.; Jefferson, A.; Wood, R.

    2014-12-01

    Contrary to common assumptions in satellite-based modeling of aerosol-cloud interactions, ∂logCCN/∂logAOD is less than unity, i.e., the number concentration of cloud condensation nuclei (CCN) less than doubles as aerosol optical depth (AOD) doubles. This can be explained by omnipresent aerosol processes. Condensation, coagulation and cloud processing, for example, generally make particles scatter more light while hardly increasing their number. This paper reports on the relationship in local air masses between CCN concentration, aerosol size distribution and light extinction observed from aircraft and the ground at diverse locations. The CCN-to-local-extinction relationship, when averaged over ~1 km distance and sorted by the wavelength dependence of extinction, varies approximately by a factor of 2, reflecting the variability in aerosol intensive properties. This, together with retrieval uncertainties and the variability in aerosol spatio-temporal distribution and hygroscopic growth, challenges satellite-based CCN estimates. However, the large differences in estimated CCN may correspond to a considerably lower uncertainty in cloud drop number concentration (CDNC), given the sublinear response of CDNC to CCN. Overall, our findings from airborne and ground-based observations call for model-based reexamination of aerosol-cloud interactions and underlying aerosol processes.

  10. Variability of Solar Radiation under Cloud-Free Skies in China: The Role of Aerosols

    SciTech Connect

    Qian, Yun; Wang, Weiguo; Leung, Lai R.; Kaiser, Dale P.

    2007-06-21

    Analysis of long-term surface solar radiation and relative humidity data reveals that much of China experienced significant decreases in global solar radiation and increases in diffuse solar radiation under cloud-free skies from 1961 to 1992. Also, 1992 marked a point of transition in the trends observed for both global solar radiation (from significant decreasing to slight increasing) and diffuse radiation (from significant increasing to slight decreasing). We suggest that continuously increasing aerosol loading from emission of pollutants is responsible for the reduced global solar radiation and increased diffuse radiation in cloud-free skies from 1961 to 1992. We speculate that a decrease in relative humidity observed since 1992 may have reduced the absorption of solar radiation by atmospheric water vapor, and decreased the scattering and extinction efficiency of particles by weakening the hygroscopic growth of aerosols, despite the concurrent increasing trend in the emission of pollutants.

  11. Adsorptive uptake of water by semisolid secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Pajunoja, Aki; Lambe, Andrew T.; Hakala, Jani; Rastak, Narges; Cummings, Molly J.; Brogan, James F.; Hao, Liqing; Paramonov, Mikhail; Hong, Juan; Prisle, Nønne L.; Malila, Jussi; Romakkaniemi, Sami; Lehtinen, Kari E. J.; Laaksonen, Ari; Kulmala, Markku; Massoli, Paola; Onasch, Timothy B.; Donahue, Neil M.; Riipinen, Ilona; Davidovits, Paul; Worsnop, Douglas R.; Petäjä, Tuukka; Virtanen, Annele

    2015-04-01

    Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcing—highlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.

  12. On the contribution of organics to the North East Atlantic aerosol number concentration

    NASA Astrophysics Data System (ADS)

    Bialek, Jakub; Dall'Osto, Manuel; Monahan, Ciaran; Beddows, David; O'Dowd, Colin

    2012-12-01

    k-means statistical-cluster analysis of submicron aerosol size distributions is combined with coincident humidity tandem differential mobility analyser data, leading to five unique aerosol categories for hygroscopic growth factors (HGFs): low sea-salt background marine, high sea-salt background marine, coastal nucleation, open ocean nucleation and anthropogenically influenced scenarios. When considering only marine conditions, and generic aerosol species associated with this environment (e.g. non-sea-salt sulfate, sea-salt, partly soluble organic matter and water insoluble organic matter), the two-year annual average contribution to aerosol number concentration from the different generic species was made up as follows: 46% (30-54%) of partially modified ammonium sulfate particles; 23% (11-40%) of partially modified sea-salt; and the remaining 31% (25-35%) contribution attributed to two distinct organic species as evidenced by different, but low, HGFs. The analysis reveals that on annual timescales, ˜30% of the submicron marine aerosol number concentration is sourced from predominantly organic aerosol while 60% of the anthropogenic aerosol number is predominantly organic. Coastal nucleation events show the highest contribution of the lowest HGF mode (1.19), although this contribution is more likely to be influenced by inorganic iodine oxides. While organic mass internally mixed with inorganic salts will lower the activation potential of these mixed aerosol types, thereby potentially reducing the concentration of cloud condensation nuclei (CCN), pure organic water soluble particles are still likely to be activated into cloud droplets, thereby increasing the concentration of CCN. A combination of dynamics and aerosol concentrations will determine which effect will prevail under given conditions.

  13. The Pasadena Aerosol Characterization Observatory (PACO): chemical and physical analysis of the Western Los Angeles Basin aerosol

    NASA Astrophysics Data System (ADS)

    Hersey, S. P.; Craven, J. S.; Schilling, K. A.; Metcalf, A. R.; Sorooshian, A.; Chan, M. N.; Flagan, R. C.; Seinfeld, J. H.

    2011-02-01

    dominated by organics. Particulate NH4NO3 and (NH4)2SO4 appear to be NH3-limited in regimes I and II, but a significant excess of particulate NH4+ in the hot, dry regime III suggests less marine SO42- and the presence of organic amines. Positive Matrix Factorization (PMF) analysis of C-ToF-AMS data resolved three factors, corresponding to a hydrocarbon-like OA (HOA), semivolatile OOA (SV-OOA), and low-volatility OOA (LV-OOA). HOA appears to be a periodic plume source, while SV-OOA exhibits a strong diurnal pattern correlating with ozone. Peaks in SV-OOA concentration correspond to peaks in DMA number concentration and the appearance of a fine organic mode. LV-OOA appears to be an aged accumulation mode constituent that may be associated with aqueous-phase processing, correlating strongly with sulfate and representing the dominant background organic component. Filter analysis revealed a complex mixture of species during periods dominated by SV-OOA and LV-OOA, with LV-OOA periods characterized by shorter-chain dicarboxylic acids (higher O:C ratio), as well as appreciable amounts of nitrate- and sulfate-substituted organics. Phthalic acid was ubiquitous in filter samples, suggesting that PAH photochemistry may be an important SOA pathway in Los Angeles. Water uptake characteristics indicate that hygroscopicity is largely controlled by organic mass fraction (OMF). The hygroscopicity parameter κ averaged 0.31 ± 0.08, approaching 0.5 at low OMF and 0.1 at high OMF, with increasing OMF suppressing hygroscopic growth and increasing critical dry diameter for CCN activation (Dd). Finally, PACO will provide context for results forthcoming from the CalNex field campaign, which involved ground sampling in Pasadena during the spring and summer of 2010.

  14. Ambient measurements of chemical and physical properties of organic aerosols: Insights into formation, growth, and heterogeneous chemistry

    NASA Astrophysics Data System (ADS)

    Ziemba, Luke D.

    Organic aerosols are a ubiquitous component of the troposphere, from heavily polluted cities to the remote Arctic. In Chapters II, III, and V of this dissertation, the formation of organic aerosol through observations of ambient size distributions is addressed. Chapter IV presents a new pathway for the formation of nitrous acid (HONO) in the urban atmosphere. In Chapter II, the size-resolved chemical composition of sub-micron aerosol was measured at a suburban forested site in North Carolina. Two events were identified in which particle growth, presumably by gas-to-particle conversion, was dominated by accumulation of organic aerosol mass. Growth rates between 1.2 nm hr-1 and 4.9 nm hr-1 were observed. Using a mass-spectral deconvolution method coupled with linear regression analysis, the sub-micron organic aerosol mass observed during the campaign, and during events, was determined to have been influenced by both local and regional secondary processes with only a minor influence from combustion sources. In Chapter III, the chemical characteristics of sub-10-micron aerosol were explored as a function of ambient particle size at a coastal and inland site in New England. Average organic carbon (OC) concentrations of 4.9 microg C m-3 and 3.4 microg C m-3 were observed at the coastal site at the Isles of Shoals (IOS) and at the slightly inland site at Thompson Farm (TF), respectively. An average of 84 and 72% of OC was found to be water-soluble at IOS and TF, respectively. Size distributions indicate that the formation of dicarboxylic acids, especially oxalic acid, is driven by aqueous-phase reactions. A chemical fingerprint analysis suggests that all water-soluble OC at IOS resembles secondary organic aerosol (SOA), while WSOC at TF appears to result from mixed sources. In Chapter IV, a newly identified formation pathway for nitrous acid (HONO) is presented. HONO is an important precursor to hydroxyl radicals in the troposphere and thus contributes to the oxidative

  15. Aerosol nucleation and growth in the TTL, due to tropical convection, during the ACTIVE campaign

    NASA Astrophysics Data System (ADS)

    Waddicor, D.; Vaughan, G.; Choularton, T.

    2009-04-01

    The Aerosol and Chemical Transport In tropical convection (ACTIVE) campaign took place between October 2005 and February 2006. This investigation involved the sampling of deep convective storms that occur in the Tropics; the campaign was based in Darwin, Northern Territory, Australia - the latter half of the campaign coincided with the monsoon season. A range of scientific equipment was used to sample the inflow and outflow air from these storms; of particular importance were the NERC Dornier (low-level) and ARA Egrett (high-level outflow) aircraft. The Dornier held a range of aerosol, particle and chemical detectors for the purpose of analysing the planetary boundary layer (PBL), in the vicinity of tropical convection. The Egrett contained detection instrumentation for a range of sizes of aerosol and cloud particles (2 Condensation Particle Counters (CPC), CAPS, CIP, CPI) in the storm outflow. This allowed a quantifiable measurement to be made of the effect of deep tropical convection on the aerosol population in the Tropical Tropopause Layer (TTL). The ACTIVE campaign found that there were large numbers of aerosol particles in the 10 - 100 nm (up to 25,000 /cm3 STP) and 100 - 1000 nm (up to 600 /cm3) size ranges. These values, in many instances, surpassed those found in the PBL. The higher levels of aerosol found in the TTL compared to the PBL could indicate that aerosol nucleation was occurring in the TTL as a direct result of convective activity. Furthermore, the Egrett aircraft found distinct boundaries between the high levels of aerosol, which were found in cloud free regions, and very low numbers of aerosol, which were found in the cloudy regions (storm anvil). The air masses were determined, from back trajectories, to have been through convective uplift and were formerly part of the anvil cloud. The cloudy regions would have contained high levels of entrapped precursor gases. Reduced nucleation and cloud particle scavenging of aerosol and gases would give a

  16. Measurements of the hygroscopic and deliquescence properties of organic compounds of different solubilities in water and their relationship with cloud condensation nuclei activities.

    PubMed

    Chan, Man Nin; Kreidenweis, Sonia M; Chan, Chak K

    2008-05-15

    The initial phase (solid or aqueous droplet) of aerosol particles prior to activation is among the critical factors in determining their cloud condensation nuclei (CCN) activity. Single-particle levitation in an electrodynamic balance (EDB)was used to measure the phase transitions and hygroscopic properties of aerosol particles of 11 organic compounds with different solubilities (10(-1) to 102 g solute/100 g water). We use these data and other literature data to relate the CCN activity and hygroscopicity of organic compounds with different solubilities. The EDB data show that glyoxylic acid, 4-methylphthalic acid, monosaccharides (fructose and mannose), and disaccharides (maltose and lactose) did not crystallize and existed as metastable droplets at low relative humidity (RH). Hygroscopic data from this work and in the literature support earlier studies showing that the CCN activities of compounds with solubilities down to the order of 10(-1) g solute/100 g water can be predicted by standard Köhler theory with the assumption of complete dissolution of the solute at activation. We also demonstrate the use of evaporation data (or efflorescence data), which provides information on the water contents of metastable solutions below the compound deliquescence RH that can be extrapolated to higher dilutions, to predict the CCN activity of organic particles, particularly for sparingly soluble organic compounds that do not deliquesce at RH achievable in the EDB and in the hygroscopic tandem differential mobility analyzer.

  17. Cloud and Aerosol Characterization During CAEsAR 2014

    NASA Astrophysics Data System (ADS)

    Zieger, P.; Tesche, M.; Krejci, R.; Baumgardner, D.; Walther, A.; Rosati, B.; Widequist, U.; Tunved, P.; O'Connor, E.; Ström, J.

    2015-12-01

    The Cloud and Aerosol Experiment at Åre (CAEsAR 2014) campaign took place from June to October 2014 at Mt. Åreskutan, Sweden, a remote mountain site in Northern Sweden. The campaign was designed to study the physical and chemical properties of clouds and aerosols under orographic forcing. A unique and comprehensive set-up allowed an in-situ characterization of both constituents at a mountain top station at 1200 m a.s.l. including instruments to measure cloud droplet size distribution, meteorological parameters, cloud residual properties (using a counterflow virtual impactor inlet), cloud water composition and various aerosol chemical and microphysical properties (e.g. size, optical and hygroscopic properties). At the same time, a remote sensing site was installed below the mountain site at 420 m a.s.l. in the immediate vicinity (< 3 km horizontally), with vertical profiling from an aerosol lidar, winds and turbulence from a scanning Doppler lidar, a Sun photometer measuring aerosol columnar optical properties, and a precipitation sampler taking rain water for chemical analysis. In addition, regular radiosoundings were performed from the valley. Here, we present the results of this intensive campaign which includes approx. 900 hours of in-cloud sampling. Various unique cloud features were frequently observed such as dynamically-driven droplet growth, bimodal droplet distributions, and the activation of particles down to approx. 20 nm in dry particle diameter. During the campaign, a forest fire smoke plume was transported over the site with measureable impacts on the cloud properties. This data will be used to constrain cloud and aerosol models, as well as to validate satellite retrievals. A first comparison to VIIRS and MODIS satellite retrievals will also be shown.

  18. Influence of Slightly Soluble Organics on Aerosol Activation

    SciTech Connect

    Abdul-Razzak, Hayder; Ghan, Steven J.

    2005-03-22

    This paper examines the effects of slightly soluble organics on aerosol activation in a parcel of air rising adiabatically. Slightly soluble organics can affect aerosol activation by three mechanisms: lowering surface tension, altering the bulk hygroscopicity, and delaying the growth of particles due to their lower solubilities. Here, we address the third mechanism by simulating the activation process of aerosol particles modeled using a single lognormal size distribution and consisting of an internal uniform chemical mixture of adipic acid (representing slightly soluble organics having extremely low solubility) and ammonium sulfate. The simulations were carried out using measured solubility of adipic acid spanning a wide range of physical and dynamical parameters. The same conditions were re-simulated but assuming fully soluble aerosols. Results of the simulations show that although that the low solubility of the adipic acid alters Köhler curves and increases critical supersaturation of the smaller particles (Köhler curves of the larger particles are not effected since these particles are completely dissolved at the initial supersaturation of zero), it has minimal to no effect on the parcel’s supersaturation except for particles consisting of more than 95% adipic acid. Accordingly, since aerosols in realistic atmospheric conditions do not contain more than 90% organics, we conclude that it is not necessary to retune the parameterization of aerosol activation previously developed and modified to address the other two mechanisms. The slightly soluble organics can thus be assumed to be fully soluble for the purpose of predicting the fraction of activation and the maximum supersaturation with negligible error.

  19. Hygroscopic and phase separation properties of ammonium sulfate/organic/water ternary solutions

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Proud, S. R.; Seppalainen, S. S.; Cziczo, D. J.

    2015-03-01

    Atmospheric aerosol particles are often partially or completely composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. 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 aerosols are not typically pure inorganic salt, instead they often also contain organic species. There is ample evidence from laboratory studies that suggests that mixed particles exist in a phase-separated state, with an aqueous inorganic core and organic shell. Although phase separation has not been measured in situ, there is no reason it would not also take place in the atmosphere. Many recent studies have focused on microscopy techniques that require deposition of the aerosol on a glass slide, possibly changing its surface properties. Here, we investigate 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 1,4-butanediol, glycerol, 1,2,6-hexanetriol, 1,2-hexanediol, and 1,5-pentanediol have been investigated. Those constituents correspond to materials found in the atmosphere in great abundance, and therefore, particles prepared in this study should mimic atmospheric mixed phase aerosol particles. The results of this study tend to be in agreement with previous microscopy experiments, with several key differences, which possibly reveal a size-dependent effect on phase separation in organic/inorganic aerosol particles.

  20. Influence of atmospheric relative humidity on ultraviolet flux and aerosol direct radiative forcing: Observation and simulation

    NASA Astrophysics Data System (ADS)

    Xia, Dong; Chen, Ling; Chen, Huizhong; Luo, Xuyu; Deng, Tao

    2016-08-01

    The atmospheric aerosols can absorb moisture from the environment due to their hydrophilicity and thus affect atmospheric radiation fluxes. In this article, the ultraviolet radiation and relative humidity (RH) data from ground observations and a radiative transfer model were used to examine the influence of RH on ultraviolet radiation flux and aerosol direct radiative forcing under the clear-sky conditions. The results show that RH has a significant influence on ultraviolet radiation because of aerosol hygroscopicity. The relationship between attenuation rate and RH can be fitted logarithmically and all of the R2 of the 4 sets of samples are high, i.e. 0.87, 0.96, 0.9, and 0.9, respectively. When the RH is 60%, 70%, 80% and 90%, the mean aerosol direct radiative forcing in ultraviolet is -4.22W m-2, -4.5W m-2, -4.82W m-2 and -5.4W m-2, respectively. For the selected polluted air samples the growth factor for computing aerosol direct radiative forcing in the ultraviolet for the RH of 80% varies from 1.19 to 1.53, with an average of 1.31.

  1. Estimation of atmospheric aerosol composition from ground-based remote sensing measurements of Sun-sky radiometer

    NASA Astrophysics Data System (ADS)

    Xie, Y. S.; Li, Z. Q.; Zhang, Y. X.; Zhang, Y.; Li, D. H.; Li, K. T.; Xu, H.; Zhang, Y.; Wang, Y. Q.; Chen, X. F.; Schauer, J. J.; Bergin, M.

    2017-01-01

    Remote sensing provides aerosol loading information, but to address climate and air quality model validation, there are additional needs to acquire aerosol composition information. In this study, a comprehensive aerosol composition model is established to quantify black carbon (BC), brown carbon (BrC), mineral dust (DU), particulate organic matters, ammonium sulfate like (AS), sea salt, and aerosol water uptake. We develop forward modeling of aerosol components, including microphysical parameters (real and imaginary refractive indices, volume fraction ratio of fine to coarse mode, and sphericity) and hygroscopic growth models, and propose an optimization scheme to estimate the components. The uncertainties caused by input parameters are also assessed. Sun-sky radiometer measurements and meteorological data obtained during a campaign in Huairou, Beijing, are processed to estimate aerosol components, which are further compared with synchronous in situ chemical measurements. The results show generally good consistencies between remotely estimated and measured components (e.g., correlation coefficients for BC, BrC, AS, and PM2.5 lie in about 0.8-0.9). The comparisons between modeled and observed microphysical parameters also show good agreements, with the exception of sphericity, which is likely caused by high uncertainties of this parameter. Sensitivity studies show that BC and BrC are highly sensitive to imaginary refractive index, while DU is strongly correlated to both volume size and sphericity. The performance of composition retrieval is expected to be improved when the sphericity uncertainty is significantly reduced.

  2. Chemical characterization of submicron aerosol and particle growth events at a national background site (3295 m a.s.l.) on the Tibetan Plateau

    NASA Astrophysics Data System (ADS)

    Du, W.; Sun, Y. L.; Xu, Y. S.; Jiang, Q.; Wang, Q. Q.; Yang, W.; Wang, F.; Bai, Z. P.; Zhao, X. D.; Yang, Y. C.

    2015-09-01

    Atmospheric aerosols exert highly uncertain impacts on radiative forcing and also have detrimental effects on human health. While aerosol particles are widely characterized in megacities in China, aerosol composition, sources and particle growth in rural areas in the Tibetan Plateau remain less understood. Here we present the results from an autumn study that was conducted from 5 September to 15 October 2013 at a national background monitoring station (3295 m a.s.l.) in the Tibetan Plateau. The submicron aerosol composition and particle number size distributions were measured in situ with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) and a Scanning Mobility Particle Sizer (SMPS). The average mass concentration of submicron aerosol (PM1) is 11.4 μg m-3 (range: 1.0-78.4 μg m-3) for the entire study, which is much lower than observed at urban and rural sites in eastern China. Organics dominated PM1, accounting for 43 % on average, followed by sulfate (28 %) and ammonium (11 %). Positive Matrix Factorization analysis of ACSM organic aerosol (OA) mass spectra identified an oxygenated OA (OOA) and a biomass burning OA (BBOA). The OOA dominated OA composition, accounting for 85 % on average, 17 % of which was inferred from aged BBOA. The BBOA contributed a considerable fraction of OA (15 %) due to the burning of cow dung and straw in September. New particle formation and growth events were frequently observed (80 % of time) throughout the study. The average particle growth rate is 2.0 nm h-1 (range: 0.8-3.2 nm h-1). By linking the evolution of particle number size distribution to aerosol composition, we found an elevated contribution of organics during particle growth periods and also a positive relationship between the growth rate and the fraction of OOA in OA, which potentially indicates an important role of organics in particle growth in the Tibetan Plateau.

  3. Investigation the optical and radiative properties of aerosol vertical profile of boundary layer by lidar and ground based measurements

    NASA Astrophysics Data System (ADS)

    Chen, W.; Chou, C.; Lin, P.; Wang, S.

    2011-12-01

    The planetary boundary layer is the air layer near the ground directly affected by diurnal heat, moisture, aerosol, and cloud transfer to or from the surface. In the daytime solar radiation heats the surface, initiating thermal instability or convection. Whereas, the scattering and absorption of aerosols or clouds might decrease the surface radiation or heat atmosphere which induce feedbacks such as the enhanced stratification and change in relative humidity in the boundary layer. This study is aimed to understand the possible radiative effect of aerosols basing on ground based aerosol measurements and lidar installed in National Taiwan University in Taipei. The optical and radiative properties of aerosols are dominated by aerosol composition, particle size, hygroscopicity property, and shape. In this study, aerosol instruments including integrating nephelometer, open air nephelometer, aethalometer are applied to investigate the relationship between aerosol hygroscopicity properties and aerosol types. The aerosol hygroscopicity properties are further applied to investigate the effect of relative humidity on aerosol vertical profiles measured by a dual-wavelength and depolarization lidar. The possible radiative effect of aerosols are approached by vertical atmospheric extinction profiles measured by lidar. Calculated atmospheric and aerosol heating effects was compared with vertical meteorological parameters measured by radiosonde. The result shows light-absorbing aerosol has the potential to affect the stability of planetary boundary layer.

  4. 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.

  5. [Aerosol optical properties during different air-pollution episodes over Beijing].

    PubMed

    Shi, Chan-Zhen; Yu, Xing-Na; Zhou, Bin; Xiang, Lei; Nie, Hao-Hao

    2013-11-01

    Based on the 2005-2011 data from Aerosol Robotic Network (AERONET), this study conducted analysis on aerosol optical properties over Beijing during different air-pollution episodes (biomass burning, CNY firework, dust storm). The aerosol optical depth (AOD) showed notable increases in the air-pollution episodes while the AOD (at 440 nm) during dust storm was 4. 91, 4. 07 and 2.65 times higher as background, biomass burning and firework aerosols. AOD along with Angstrom exponent (alpha) can be used to determine the aerosol types. The dust aerosol had the highest AOD and the lowest alpha. The alpha value of firework (1.09) was smaller than biomass burning (1.21) and background (1.27), indicating that coarse particles were dominant in the former type. Higher AOD of burnings (than background) can be attributed to the optical extinction capability of black carbon aerosol. The single scattering albedo (SSA) was insensitive to wavelength. The SSA value of dust (0.934) was higher than background (0.878), biomass burning (0.921) and firework (0.905). Additionally, the extremely large SSA of burnings here maybe was caused by the aging smoke, hygroscopic growth and so on. The peak radius of aerosol volume size distributions were 0.1-0.2 microm and 2.24 -3.85 microm in clear and polluted conditions. The value of volume concentration ratio between coarse and fine particles was in the order of clear background (1.04), biomass burning (1.10), CNY firework (1.91) and dust storm (4.96) episode.

  6. 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.

  7. 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.

  8. Size dependence of phase transitions in aerosol nanoparticles

    NASA Astrophysics Data System (ADS)

    Cheng, Yafang; Su, Hang; Koop, Thomas; Mikhailov, Eugene; Pöschl, Ulrich

    2015-04-01

    Phase transitions of nanoparticles are of fundamental importance in atmospheric sciences. Current understanding is insufficient to explain observations at the nano-scale. In particular, discrepancies exist between observations and model predictions of deliquescence and efflorescence transitions and the hygroscopic growth of salt nanoparticles. Here we show that these discrepancies can be resolved by consideration of particle size effects with consistent thermodynamic data. We present a new method for the determination of water and solute activities and interfacial energies in highly supersaturated aqueous solution droplets. Our analysis reveals that particle size can strongly alter the characteristic concentration of phase separation in mixed systems, resembling the influence of temperature. Due to similar effects, atmospheric secondary organic aerosol particles at room temperature are expected to be always liquid at diameters below ~20 nm. We thus propose and demonstrate that particle size should be included as an additional dimension in the equilibrium phase diagram of aerosol nanoparticles. Reference: Cheng, Y. et al. Size dependence of phase transitions in aerosol nanoparticles. Nature Communications. 5:5923 doi: 10.1038/ncomms6850 (2015).

  9. Vertical distribution of ambient aerosol extinctive properties during haze and haze-free periods based on the Micro-Pulse Lidar observation in Shanghai.

    PubMed

    Liu, Qiong; He, Qianshan; Fang, Sihua; Guang, Ying; Ma, Chengyu; Chen, Yonghang; Kang, Yanming; Pan, Hu; Zhang, Hua; Yao, Yifeng

    2017-01-01

    Ambient aerosols make a significant contribution to the environment and climate through their optical properties. In this study, the aerosol extinction coefficient and Aerosol optical depth (AOD) retrieved using the Fernald Method from the ground-based Micro-Pulse Lidar (MPL) were used to investigate the characteristics of aerosols during haze and haze-free periods in Shanghai. There were 216 haze days including 145 dry haze days, 39 damp haze days and 32days of both dry and damp haze in Shanghai from March 2009 to February 2010. During the haze periods, aerosols were concentrated mainly below 600m resulting in the most severe pollution layer in Shanghai. In contrast to the aerosol optical properties during haze-free periods, aerosol extinction coefficients and AOD were larger in the lower altitude (below 1km) during haze periods. The lowest 1km contributed 53-72% of the Aerosol optical depth (AOD) below 6km for the haze periods and <41% of that for the haze-free periods except summer. According to the analysis of influencing factors, although atmospheric convection was strong in summer which led to reduce the extinction, the highest occurrence of haze with relatively low aerosol extinction most of time was in summer, which resulted from the factors such as higher relative humidity, temperature and more solar radiation causing hygroscopic growth of particles and formation of secondary aerosols; in spring and autumn, there was less haze occurrences because the boundary layer was relatively higher, which allowed pollutants to diffuse more easily, but spring was the second most frequency season of haze due to frequent dust transport from the north; in winter high concentrations of particles and low boundary layer height were not beneficial to the diffusion of pollutants near the surface and caused haze occurrence rather high with high aerosol extinction.

  10. Hygroscopic Properties and Respiratory System Deposition Behavior of Particulate Matter Emitted By Mining and Smelting Operations.

    PubMed

    Youn, Jong-Sang; Csavina, Janae; Rine, Kyle P; Shingler, Taylor; Taylor, Mark Patrick; Sáez, A Eduardo; Betterton, Eric A; Sorooshian, Armin

    2016-11-01

    This study examines size-resolved physicochemical data for particles sampled near mining and smelting operations and a background urban site in Arizona with a focus on how hygroscopic growth impacts particle deposition behavior. Particles with aerodynamic diameters between 0.056-18 μm were collected at three sites: (i) an active smelter operation in Hayden, AZ, (ii) a legacy mining site with extensive mine tailings in Iron King, AZ, and (iii) an urban site, inner-city Tucson, AZ. Mass size distributions of As and Pb exhibit bimodal profiles with a dominant peak between 0.32 and 0.56 μm and a smaller mode in the coarse range (>3 μm). The hygroscopicity profile did not exhibit the same peaks owing to dependence on other chemical constituents. Submicrometer particles were generally more hygroscopic than supermicrometer ones at all three sites with finite water-uptake ability at all sites and particle sizes examined. Model calculations at a relative humidity of 99.5% reveal significant respiratory system particle deposition enhancements at sizes with the largest concentrations of toxic contaminants. Between dry diameters of 0.32 and 0.56 μm, for instance, ICRP and MPPD models predict deposition fraction enhancements of 171%-261% and 33%-63%, respectively, at the three sites.

  11. Hygroscopic Properties and Respiratory System Deposition Behavior of Particulate Matter Emitted By Mining and Smelting Operations

    PubMed Central

    Youn, Jong-sang; Csavina, Janae; Rine, Kyle P.; Shingler, Taylor; Taylor, Mark Patrick; Sáez, A. Eduardo; Betterton, Eric A.; Sorooshian, Armin

    2016-01-01

    This study examines size-resolved physicochemical data for particles sampled near mining and smelting operations and a background urban site in Arizona with a focus on how hygroscopic growth impacts particle deposition behavior. Particles with aerodynamic diameters between 0.056 – 18 μm were collected at three sites: (i) an active smelter operation in Hayden, AZ, (ii) a legacy mining site with extensive mine tailings in Iron King, AZ, and (iii) an urban site, inner-city Tucson, AZ. Mass size distributions of As and Pb exhibit bimodal profiles with a dominant peak between 0.32-0.56 μm and a smaller mode in the coarse range (> 3 μm). The hygroscopicity profile did not exhibit the same peaks owing to dependence on other chemical constituents. Sub-micrometer particles were generally more hygroscopic than super-micrometer ones at all three sites with finite water-uptake ability at all sites and particle sizes examined. Model calculations at a relative humidity of 99.5% reveal significant respiratory system particle deposition enhancements at sizes with the largest concentrations of toxic contaminants. Between dry diameters of 0.32 and 0.56 μm, for instance, ICRP and MPPD models predict deposition fraction enhancements of 171%-261% and 33%-63%, respectively, at the three sites. PMID:27700056

  12. Efficient Nose-to-Lung (N2L) Aerosol Delivery with a Dry Powder Inhaler

    PubMed Central

    Golshahi, Laleh; Behara, Srinivas R.B.; Tian, Geng; Farkas, Dale R.; Hindle, Michael

    2015-01-01

    Abstract Purpose: Delivering aerosols to the lungs through the nasal route has a number of advantages, but its use has been limited by high depositional loss in the extrathoracic airways. The objective of this study was to evaluate the nose-to-lung (N2L) delivery of excipient enhanced growth (EEG) formulation aerosols generated with a new inline dry powder inhaler (DPI). The device was also adapted to enable aerosol delivery to a patient simultaneously receiving respiratory support from high flow nasal cannula (HFNC) therapy. Methods: The inhaler delivered the antibiotic ciprofloxacin, which was formulated as submicrometer combination particles containing a hygroscopic excipient prepared by spray-drying. Nose-to-lung delivery was assessed using in vitro and computational fluid dynamics (CFD) methods in an airway model that continued through the upper tracheobronchial region. Results: The best performing device contained a 2.3 mm flow control orifice and a 3D rod array with a 3-4-3 rod pattern. Based on in vitro experiments, the emitted dose from the streamlined nasal cannula had a fine particle fraction <5 μm of 95.9% and mass median aerodynamic diameter of 1.4 μm, which was considered ideal for nose-to-lung EEG delivery. With the 2.3-343 device, condensational growth in the airways increased the aerosol size to 2.5–2.7 μm and extrathoracic deposition was <10%. CFD results closely matched the in vitro experiments and predicted that nasal deposition was <2%. Conclusions: The developed DPI produced high efficiency aerosolization with significant size increase of the aerosol within the airways that can be used to enable nose-to-lung delivery and aerosol administration during HFNC therapy. PMID:25192072

  13. 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

  14. 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).

  15. Structural and hygroscopic changes of soot during heterogeneous reaction with O(3).

    PubMed

    Liu, Yongchun; Liu, Chang; Ma, Jinzhu; Ma, Qingxin; He, Hong

    2010-09-28

    Soot aerosols are ubiquitous in the atmosphere and play an important role in global and regional radiative balance and climate. Their environmental impact, however, greatly depends on their structure, composition, particle size, and morphology. In this study, the structural changes of a model soot (Printex U) during a heterogeneous reaction with 80 ppm O(3) at 298 K were investigated using in situ Raman spectroscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and transmission electron microscopy (TEM). Hygroscopic changes due to heterogeneous reaction with O(3) were also studied by water sorption analyzer. The consumption of amorphous carbon (D3 band) and disordered graphitic lattice (D4 band) of soot by ozonization was confirmed by the decrease in the full widths at half maximum and their relative integrated intensities (percentages of integrated areas). Oxygen containing surface species including ketone, lactone, and anhydride were also observed in Raman and IR spectra of ozonized soot. The ozonized soot showed more compacted aggregates with a smaller average diameter of primary particles (29.9 +/- 7.7 nm) and a larger fractal dimension (1.81 +/- 0.08) when compared with fresh soot (36.9 +/- 9.4 nm, and 1.61 +/- 0.10). The ozonization reaction leads to an enhancement of hygroscopicity of soot due to the decrease in particle diameter and the formation of oxygen containing surface species.

  16. 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.

  17. 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.

  18. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect

    Davidovits, Paul

    2015-10-20

    Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

  19. Final Report: "Collaborative Project. Understanding the Chemical Processes That Affect Growth Rates of Freshly Nucleated Particles"

    SciTech Connect

    Smith, James N.; McMurry, Peter H.

    2015-11-12

    This final technical report describes our research activities that have, as the ultimate goal, the development of a model that explains growth rates of freshly nucleated particles. The research activities, which combine field observations with laboratory experiments, explore the relationship between concentrations of gas-phase species that contribute to growth and the rates at which those species are taken up. We also describe measurements of the chemical composition of freshly nucleated particles in a variety of locales, as well as properties (especially hygroscopicity) that influence their effects on climate. Our measurements include a self-organized, DOE-ARM funded project at the Southern Great Plains site, the New Particle Formation Study (NPFS), which took place during spring 2013. NPFS data are available to the research community on the ARM data archive, providing a unique suite observations of trace gas and aerosols that are associated with the formation and growth of atmospheric aerosol particles.

  20. 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.

  1. 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.

  2. Hygroscopic and phase transition properties of alkyl aminium sulfates at low relative humidities.

    PubMed

    Chu, Yangxi; Sauerwein, Meike; Chan, Chak K

    2015-08-14

    Alkyl aminium sulfates (AASs) can affect the physicochemical properties of atmospheric aerosols such as hygroscopicity. Previous laboratory experiments have shown that the water content in AAS bulk solutions is higher than in aqueous ammonium sulfate solution in the range of 60-95% relative humidity (RH). Furthermore, amine was found to evaporate from the solution during the preparation of AASs from the parent amine and sulfuric acid solutions. Here we report the hygroscopicities of deposited particles of four AASs at different aminium-to-sulfate molar ratios (A/Ss) in the range of <3-90% RH using air-flow cells coupled with in situ micro-Raman spectroscopy. Normalized integrated areas of O-H stretching peaks in the Raman spectra were converted to water-to-solute molar ratios (WSRs) at various RH values. Evaporation of amine was also observed in most cases and the exact A/Ss of sample particles or solutions were determined by ion chromatography. Mono-methylaminium sulfate (MMAS) and mono-ethylaminium sulfate (MEAS) particles were stable at A/S = 2.0, but di-methylaminium sulfate (DMAS) and tri-methylaminium sulfate (TMAS) suffered from DMA and TMA evaporation and eventually equilibrated to the A/S of 1.5 and 1.0, respectively. At these stable compositions MMAS and MEAS exhibited phase transitions in the super-saturation region, while DMAS and TMAS showed a continuous and reversible water uptake. Besides, an approach to estimate the hygroscopicities of DMAS and TMAS particles at an initial A/S larger than that of the stable compositions was presented. In the range of 60-95% RH, the WSRs of all the studied AAS particles were consistent with a previous study based on experimental values and the extended Zdanovskii-Stokes-Robinson equation. In general, all the studied AASs were more hygroscopic than their corresponding ammonium counterparts within the studied RH range and evaporation of amine needs to be corrected in studying unstable AAS particles.

  3. Structural Change of Aerosol Particle Aggregates with Exposure to Elevated Relative Humidity.

    PubMed

    Montgomery, James F; Rogak, Steven N; Green, Sheldon I; You, Yuan; Bertram, Allan K

    2015-10-20

    Structural changes of aggregates composed of inorganic salts exposed to relative humidity (RH) between 0 and 80% after formation at selected RH between 0 and 60% were investigated using a tandem differential mobility analyzer (TDMA) and fluorescence microscopy. The TDMA was used to measure a shift in peak mobility diameter for 100-700 nm aggregates of hygroscopic aerosol particles composed of NaCl, Na2SO4, (NH4)2SO4, and nonhygroscopic Al2O3 as the RH was increased. Aggregates of hygroscopic particles were found to shrink when exposed to RH greater than that during the aggregation process. The degree of aggregate restructuring is greater for larger aggregates and greater increases in RH. Growth factors (GF) calculated from mobility diameter measurements as low as 0.77 were seen for NaCl before deliquescence. The GF subsequently increased to 1.23 at 80% RH, indicating growth after deliquescence. Exposure to RH lower than that experienced during aggregation did not result in structural changes. Fluorescent microscopy confirmed that aggregates formed on wire surfaces undergo an irreversible change in structure when exposed to elevated RH. Analysis of 2D movement of aggregates shows a displacement of 5-13% compared to projected length of initial aggregate from a wire surface. Surface tension due to water adsorption within the aggregate structure is a potential cause of the structural changes.

  4. Hygroscopic and phase separation properties of ammonium sulfate/organics/water ternary solutions

    NASA Astrophysics Data System (ADS)

    Zawadowicz, M. A.; Proud, S. R.; Seppalainen, S. S.; Cziczo, D. J.

    2015-08-01

    Atmospheric aerosol particles are often partially or completely composed of inorganic salts, such as ammonium sulfate and sodium chloride, and therefore exhibit hygroscopic properties. Many inorganic salts have well-defined deliquescence and efflorescence points at which they take up and lose water, respectively. Field measurements have shown that atmospheric aerosols are not typically pure inorganic salt, instead, they often also contain organic species. There is ample evidence from laboratory studies that suggests that mixed particles exist in a phase-separated state, with an aqueous inorganic core and organic shell. Although phase separation has not been measured in situ, there is no reason it would not also take place in the atmosphere. Here, we investigate 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 (Fourier transform infrared) spectroscopy. Ammonium sulfate aerosol mixed with organic polyols with different O : C ratios, including 1,4-butanediol, glycerol, 1,2,6-hexanetriol, 1,2-hexanediol, and 1,5-pentanediol have been investigated. Those constituents correspond to materials found in the atmosphere in great abundance and, therefore, particles prepared in this study should mimic atmospheric mixed-phase aerosol particles. Some results of this study tend to be in agreement with previous microscopy experiments, but others, such as phase separation properties of 1,2,6-hexanetriol, do not agree with previous work. Because the particles studied in this experiment are of a smaller size than those used in microscopy studies, the discrepancies found could be a size-related effect.

  5. Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

    NASA Astrophysics Data System (ADS)

    Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J. C.; Sodeau, J. R.; Healy, R. M.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; O'Dowd, C. D.

    2009-12-01

    As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the NE Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Black carbon concentrations in polluted air were between 300-400 ng m-3, and in clean marine air were less than 50 ng m-3. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water

  6. Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

    NASA Astrophysics Data System (ADS)

    Dall'Osto, M.; Ceburnis, D.; Martucci, G.; Bialek, J.; Dupuy, R.; Jennings, S. G.; Berresheim, H.; Wenger, J.; Healy, R.; Facchini, M. C.; Rinaldi, M.; Giulianelli, L.; Finessi, E.; Worsnop, D.; Ehn, M.; Mikkilä, J.; Kulmala, M.; O'Dowd, C. D.

    2010-09-01

    As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm-3, while background marine air aerosol concentrations were between 400-600 cm-3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm-3, was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were

  7. Characteristics of aerosolized ice forming marine biogenic particles

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.

    Ice particles are ubiquitous in the atmosphere existing as the sole constituents of glaciated cirrus clouds or coexisting with supercooled liquid droplets in mixed-phase clouds. Aerosol particles serving as heterogeneous ice nuclei for ice crystal formation impact the global radiative balance by modification of cloud radiative properties, and thus climate. Atmospheric ice formation is not a well understood process and represents great uncertainty for climate prediction. The oceans which cover the majority of the earth's surface host nearly half the total global primary productivity and contribute to the greatest aerosol production by mass. However, the effect of biological activity on particle aerosolization, particle composition, and ice nucleation is not well established. This dissertation investigates the link between marine biological activity, aerosol particle production, physical/chemical particle characteristics, and ice nucleation under controlled laboratory conditions. Dry and humidified aerosol size distributions of particles from bursting bubbles generated by plunging water jets and aeration through frits in a seawater mesocosm containing bacteria and/or phytoplankton cultures, were measured as a function of biological activity. Total particle production significantly increases primarily due to enhanced aerosolization of particles ≤100 nm in diameter attributable to the presence and growth of phytoplankton. Furthermore, hygroscopicity measurements indicate primary organic material associated with the sea salt particles, providing additional evidence for the importance of marine biological activity for ocean derived aerosol composition. Ice nucleation experiments show that these organic rich particles nucleate ice efficiently in the immersion and deposition modes, which underscores their importance in mixed-phase and cirrus cloud formation processes. In separate ice nucleation experiments employing pure cultures of Thalassiosira pseudonana, Nannochloris

  8. On the growth of nitric and sulfuric acid aerosol particles under stratospheric conditions

    NASA Technical Reports Server (NTRS)

    Hamill, Patrick; Turco, R. P.; Toon, O. B.

    1988-01-01

    A theory for the formation of frozen aerosol particles in the Antarctic stratosphere was developed and applied to the formation of polar stratospheric clouds. The theory suggests that the condensed ice particles are composed primarily of nitric acid and water, with small admixtures of sulfuric and hydrochloric acids in solid solution. The proposed particle formation mechanism is in agreement with the magnitude and seasonal behavior of the optical extinction observed in the winter polar stratosphere.

  9. The Role of Aerosols in Cloud Growth, Suppression, and Precipitation: Yoram Kaufman and his Contributions

    NASA Technical Reports Server (NTRS)

    King, Michael D.

    2006-01-01

    Aerosol particles are produced in the earth's atmosphere through both natural as well as manmade processes, and contribute profoundly to the (i) formation and characteristics of clouds, (ii) lifetime of clouds, (iii) optical and microphysical properties of clouds, (iv) human health through effects on air quality and the size of particulates as well as vectors for transport of pathogens, (v) climate response and feedbacks, (vi) precipitation, and (vii) harmful algal blooms. Without aerosol particles in the Earth's atmosphere, there would be no fogs, no clouds, ,no mists, and probably no rain, as noted as far back as 1880 by Scottish physicist John Aitken. With the modern development of instrumentation, both groundbased, airborne, and satellite-based, much progress has been made in linkng phenomena and processes together, and putting regional air quality characteristics and hypothesized cloud response into closer scrutiny and linkages. In h s presentation I will summarize the wide ranging contributions that Yoram Kaufman has made in ground-based (AERONET), aircraft field campaigns (such as SCAR-B and TARFOX), and, especially, satellite remote sensing (Landsat, MODIS, POLDER) to shed new light on this broad ranging and interdisciplinary field of cloud-aerosol-precipitation interactions.

  10. Formation and Growth of Sulfate Aerosols in the Presence of Hydrocarbons: Results from the 2013 Summer Oil Sands FOSSILs Field Campaign, Alberta, Canada

    NASA Astrophysics Data System (ADS)

    Amiri, N.; Ghahremaninezhad, R.; Rempillo, O. T.; Norman, A. L.

    2014-12-01

    Sulfur dioxide oxidation and the effect of oxidation products in formation and growth of aerosols have been studied widely. Despite this, significant gaps still exist in understanding the role of organic matter in SO2 oxidation. Organic molecules, such as Criegee radicals originating from biogenic sources, are expected to be important for SO2 oxidation in addition to organic molecules of anthropogenic origin. A study of SO2 and aerosol sulfate downwind of the oil sands region was conducted as part of the FOSSILS campaign in the summer of 2013 to better understand aerosol growth from SO2 oxidation in the presence of hydrocarbons and the distribution of sulfate in size-segregated aerosols. Hydrocarbons present in the atmosphere during the sampling campaign, collected using evacuated canisters, were characterized using a pre-concentration trap coupled to a GC-FID. The results from this campaign will be explored to determine SO2 oxidation pathways and the effects of oxidation products to aerosol formation and growth.

  11. Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2, and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

    NASA Technical Reports Server (NTRS)

    Livingston, John M.; Kapustin, Vladimir N.; Schmid, Beat; Russell, Philip B.; Quinn, Patricia K.; Bates, Timothy S.; Durkee, Philip A.; Smith, Peter J.; Freudenthaler, Volker; Wiegner, Matthias

    2000-01-01

    Analyses of aerosol optical depth (AOD) and columnar water vapor (CWV) measurements acquired with NASA Ames Research Center's six-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V (research vehicle) Professor Vodyanitskiy during the second Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA (National Oceanographic and Atmospheric Administration)-14/AVHRR (Advanced Very High Resolution Radiometer) satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering measured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from

  12. Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2 and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

    NASA Technical Reports Server (NTRS)

    Livingston, John M.; Kapustin, Vladimir N.; Schmid, Beat; Russell, Philip B.; Quinn, Patricia K.; Bates, Timothy S.; Durkee, Philip A.; Smith, Peter J.; Freudenthaler, Volker; Wiegner, Matthias; Covert, Dave S.; Gasso, Santiago; Hegg, Dean; Collins, Donald R.; Flagan, Richard C.; Seinfeld, John H.; Vitale, Vito; Tomasi, Claudio

    2000-01-01

    Analyses of aerosol optical depth (AOD) and colurnmn water vapor (CWV) measurements acquired with NASA Ames Research Center's 6-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V Professor Vodyanitskiy during the 2nd Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA-14/AVHRR satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering mearured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from radiosonde measurements during 8 soundings on 7 days and also with values calculated from measurements taken on 10 July with

  13. [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.

  14. Impact of volcanic ash plume aerosol on cloud microphysics

    NASA Astrophysics Data System (ADS)

    Martucci, G.; Ovadnevaite, J.; Ceburnis, D.; Berresheim, H.; Varghese, S.; Martin, D.; Flanagan, R.; O'Dowd, C. D.

    2012-03-01

    This study focuses on the dispersion of the Eyjafjallajökull volcanic ash plume over the west of Ireland, at the Mace Head Supersite, and its influence on cloud formation and microphysics during one significant event spanning May 16th and May 17th, 2010. Ground-based remote sensing of cloud microphysics was performed using a K a-band Doppler cloud RADAR, a LIDAR-ceilometer and a multi-channel microwave-radiometer combined with the synergistic analysis scheme SYRSOC ( Synergistic Remote Sensing Of Cloud). For this case study of volcanic aerosol interaction with clouds, cloud droplet number concentration (CDNC), liquid water content (LWC), and droplet effective radius ( reff) and the relative dispersion were retrieved. A unique cloud type formed over Mace Head characterized by layer-averaged maximum, mean and standard deviation values of the CDNC, reff and LWC: Nmax = 948 cm -3, N¯=297cm, σ=250cm, reff max = 35.5 μm, r¯=4.8μm, σ=4.4μm, LWC=0.23gm, LWC¯=0.055gm, σ=0.054gm, respectively. The high CDNC, for marine clean air, were associated with large accumulation mode diameter (395 nm) and a hygroscopic growth factor consistent with sulphuric acid aerosol, despite being almost exclusively internally mixed in submicron sizes. Additionally, the Condensation Nuclei (CN, d > 10 nm) to Cloud Condensation Nuclei (CCN) ratio, CCN:CN ˜1 at the moderately low supersaturat