scholarly journals Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Ålesund, Svalbard

2014 ◽  
Vol 14 (6) ◽  
pp. 7067-7111 ◽  
Author(s):  
N. Rastak ◽  
S. Silvergren ◽  
P. Zieger ◽  
U. Wideqvist ◽  
J. Ström ◽  
...  
Keyword(s):  
Seasonal Variation ◽  
Water Uptake ◽  
Aerosol Particles ◽  
The Arctic ◽  
Aerosol Size Distribution ◽  
Ambient Atmosphere ◽  
Radiative Effect ◽  
Hygroscopic Growth ◽  
Scattering Coefficients ◽  
Aerosol Scattering

Abstract. In this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m−2) in the Arctic at Ny-Ålesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July, August and September), when small particles (< 100 nm in diameter) dominate the aerosol size distribution. The maximum scattering by dry particles was observed during Arctic haze period (March, April and May) when average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 ± 2.26 (mean ± standard deviation), with lower values during the haze period (March, April, May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE on the surface, with the smallest effect during the haze period (March, April and May) and the highest during late summer and beginning of fall (July, August and September).

scholarly journals Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Ålesund, Svalbard

2014 ◽  
Vol 14 (14) ◽  
pp. 7445-7460 ◽  
Author(s):  
N. Rastak ◽  
S. Silvergren ◽  
P. Zieger ◽  
U. Wideqvist ◽  
J. Ström ◽  
...  
Keyword(s):  
Seasonal Variation ◽  
Water Uptake ◽  
Aerosol Particles ◽  
The Arctic ◽  
Ambient Atmosphere ◽  
Radiative Effect ◽  
Hygroscopic Growth ◽  
Scattering Coefficients ◽  
Aerosol Scattering ◽  
July August September

Abstract. In this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m−2) in the Arctic at Ny-Ålesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, a Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July-August-September), when small particles (< 100 nm in diameter) dominate the aerosol number size distribution. The maximum scattering by dry particles was observed during the Arctic haze period (March-April-May) when the average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 ± 2.26 (mean ± standard deviation), with lower values during the haze period (March-April-May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE at the surface, with the smallest effect during the haze period (March-April-May) and the highest during late summer and beginning of fall (July-August-September).

scholarly journals Effects of relative humidity on aerosol light scattering in the Arctic

2010 ◽  
Vol 10 (8) ◽  
pp. 3875-3890 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
M. Gysel ◽  
J. Ström ◽  
S. Henne ◽  
...  
Keyword(s):  
Standard Deviation ◽  
Light Scattering ◽  
Relative Humidity ◽  
Aerosol Particles ◽  
Aerosol Size Distribution ◽  
Hygroscopic Growth ◽  
Scattering Coefficients ◽  
Dry Conditions ◽  
Hygroscopic Particles

Abstract. Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties – especially the aerosol light scattering – are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH>30–40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time for aerosol particles present in summer and fall in the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σsp(λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions with an average RH<10% (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor f(RH, λ) is the key parameter to describe the RH effect on σsp(λ) and is defined as the RH dependent σsp(RH, λ) divided by the corresponding dry σsp(RHdry, λ). During our campaign the average f(RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of f(RH, λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry measured in-situ scattering coefficients. The RH dependency of the recorded f(RH, λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor g(RH), defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found, on average, g(RH=85%) values to be 1.61±0.12 (mean±standard deviation). No clear seasonal shift of f(RH, λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of f(RH, λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we present a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location.

scholarly journals Effects of relative humidity on aerosol light scattering in the Arctic

2010 ◽  
Vol 10 (2) ◽  
pp. 3659-3698 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
M. Gysel ◽  
J. Ström ◽  
S. Henne ◽  
...  
Keyword(s):  
Standard Deviation ◽  
Light Scattering ◽  
Relative Humidity ◽  
Aerosol Particles ◽  
Aerosol Size Distribution ◽  
Hygroscopic Growth ◽  
Scattering Coefficients ◽  
Dry Conditions ◽  
Hygroscopic Particles

Abstract. Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties – especially the aerosol light scattering – are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH<30–40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time of aerosol particles present in summer and fall at the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σsp(λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor f(RH,λ) is the key parameter to describe the RH effect on σsp(λ) and is defined as the RH dependent σsp(RH,λ) divided by the corresponding dry σsp(RHdry,λ). During our campaign the average f(RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of f(RH,λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry measured in-situ scattering coefficients. The RH dependency of the recorded f(RH,λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor g, defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found on average for g values of 1.61±0.12 (mean ± standard deviation). No clear seasonal shift of f(RH,λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of f(RH,λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we give a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location.

scholarly journals Tandem configuration of differential mobility and centrifugal particle mass analysers for investigating aerosol hygroscopic properties

2017 ◽  
Vol 10 (3) ◽  
pp. 1269-1280 ◽  
Author(s):  
Sergey S. Vlasenko ◽  
Hang Su ◽  
Ulrich Pöschl ◽  
Meinrat O. Andreae ◽  
Eugene F. Mikhailov
Keyword(s):  
Water Uptake ◽  
Aerosol Particles ◽  
Interaction Model ◽  
Growth Curves ◽  
Particle Mass ◽  
Submicron Particles ◽  
Hygroscopic Growth ◽  
Differential Mobility ◽  
Hygroscopic Properties ◽  
Modal Mass

Abstract. A tandem arrangement of Differential Mobility Analyser and Humidified Centrifugal Particle Mass Analyser (DMA-HCPMA) was developed to measure the deliquescence and efflorescence thresholds and the water uptake of submicron particles over the relative humidity (RH) range from 10 to 95 %. The hygroscopic growth curves obtained for ammonium sulfate and sodium chloride test aerosols are consistent with thermodynamic model predictions and literature data. The DMA-HCPMA system was applied to measure the hygroscopic properties of urban aerosol particles, and the kappa mass interaction model (KIM) was used to characterize and parameterize the concentration-dependent water uptake observed in the 50–95 % RH range. For DMA-selected 160 nm dry particles (modal mass of 3.5 fg), we obtained a volume-based hygroscopicity parameter, κv ≈  0.2, which is consistent with literature data for freshly emitted urban aerosols.Overall, our results show that the DMA-HCPMA system can be used to measure size-resolved mass growth factors of atmospheric aerosol particles upon hydration and dehydration up to 95 % RH. Direct measurements of particle mass avoid the typical complications associated with the commonly used mobility-diameter-based HTDMA technique (mainly due to poorly defined or unknown morphology and density).

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

2015 ◽  
Vol 15 (15) ◽  
pp. 8847-8869 ◽  
Author(s):  
E. F. Mikhailov ◽  
G. N. Mironov ◽  
C. Pöhlker ◽  
X. Chi ◽  
M. L. Krüger ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Water Uptake ◽  
Aerosol Particles ◽  
Organic Coating ◽  
Water Soluble ◽  
Submicron Particles ◽  
Hygroscopic Growth ◽  
Accumulation Mode ◽  
Hygroscopic Properties ◽  
Coarse Mode

Abstract. 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) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κv,ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv &amp;approx; 0.15) and a Colorado mountain forest (κv &amp;approx; 0.16 ). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv,p. The obtained κv,p values overestimate the experimental FDHA-KIM-derived κv,ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (> 300 nm) and supermicron aerosol particles possess core–shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall, the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second timescales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.

scholarly journals The rate of equilibration of viscous aerosol particles

2016 ◽  
Vol 16 (8) ◽  
pp. 5299-5313 ◽  
Author(s):  
Simon O'Meara ◽  
David O. Topping ◽  
Gordon McFiggans
Keyword(s):  
Diffusion Coefficient ◽  
Diffusion Coefficients ◽  
Aerosol Particles ◽  
Volatile Component ◽  
Water Soluble ◽  
Ambient Atmosphere ◽  
Equilibration Time ◽  
Hygroscopic Growth ◽  
Research Activity ◽  
Model Framework

Abstract. The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1–90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1  ×  10−25 m2 s−1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

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

2016 ◽  
Author(s):  
Natasha Hodas ◽  
Andreas Zuend ◽  
Katherine Schilling ◽  
Thomas Berkemeier ◽  
Manabu Shiraiwa ◽  
...  
Keyword(s):  
Molecular Mass ◽  
Water Uptake ◽  
Atmospheric Aerosols ◽  
Water Saturation ◽  
Cloud Condensation Nuclei ◽  
Ambient Atmosphere ◽  
Hygroscopic Growth ◽  
Water Diffusivity ◽  
Molecular Masses ◽  
Ccn Activity

Abstract. Organic oligomers and other organic high molecular mass compounds are potential sources of viscous atmospheric aerosol components, which may inhibit the mass transport of water and 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 investigate the influence of particle viscosity on water-uptake behavior, measurements of hygroscopic growth under subsaturated relative humidity (RH) conditions and of the CCN activity of laboratory surrogates for oligomers in atmospheric aerosols were conducted with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe and a CCN counter, respectively. In order to explore variability in water-uptake behavior across aerosol systems with differing viscosities, experiments were conducted for particles comprised of polyethylene glycol (PEG) with average molecular masses of 200, 1,000, and 10,000 g/mol, as well as mixtures of these PEG oligomers with ammonium sulfate (AS). Experimental results were compared with 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 to observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Under subsaturated 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 latter finding is attributed to an increase in the efficiency of PEG as a surfactant with increasing molecular mass. This effect is most pronounced for PEG-AS mixtures, and a modest enhancement in CCN activity was observed for the PEG10,000-AS mixture as compared to pure AS, as evidenced by a 8 % reduction in critical activation diameter at a supersaturation of 0.6 %. The supplementation of experimental observations with the AIOMFAC-based model results and estimations of water diffusivity in PEG suggests that apparent discontinuities in hygroscopicity above and below water saturation can be attributed, at least in part, to a combination of RH-dependent differences in the sensitivity of water uptake behavior to non-ideal interactions and to surface tension effects. There was no evidence that kinetic limitations to water uptake due to the presence of viscous aerosol components influenced hygroscopic growth. This work provides insight into the factors likely to be contributing to discontinuities in aerosol water-uptake behavior below and above water saturation (e.g., low hygroscopic growth at subsaturated RHs, but enhanced CCN activity for a given aerosol population) that have been observed previously in the ambient atmosphere.

scholarly journals Tandem configuration of differential mobility and centrifugal particle mass analyzers for investigating aerosol hygroscopic properties

2016 ◽  
Author(s):  
Sergey S. Vlasenko ◽  
Hang Su ◽  
Ulrich Pöschl ◽  
Meinrat O. Andreae ◽  
Eugene F. Mikhailov
Keyword(s):  
Water Uptake ◽  
Aerosol Particles ◽  
Interaction Model ◽  
Particle Morphology ◽  
Particle Mass ◽  
Submicron Particles ◽  
Mass Analyzer ◽  
Hygroscopic Growth ◽  
Differential Mobility ◽  
Hygroscopic Properties

Abstract. A tandem arrangement of Differential Mobility Analyzer and Humidified Centrifugal Particle Mass Analyzer (DMA-HCPMA) was developed to measure the deliquescence and efflorescence thresholds and the water uptake of submicron particles over the relative humidity (RH) range from 10 % to 95 %. The hygroscopic growth curves obtained for Ammonium sulfate and sodium chloride test aerosols are consistent with thermodynamic model predictions and literature data. The DMA-HCPMA system was applied to measure the hygroscopic properties of urban aerosol particles, and the kappa mass interaction model (KIM) was used to characterize and parameterize the concentration-dependent water uptake observed in the 50–95 % RH range. For DMA-selected 160 nm dry particles (mass of 3.5 fg), we obtained a volume-based hygroscopicity parameter κv &amp;approx; 0.2, which is consistent with literature data for freshly emitted urban aerosols. Overall, our results show that the DMA-HCPMA system can be used to measure size-resolved mass growth factors of atmospheric aerosol particles upon hydration and dehydration up to 95 % RH. The direct measurements of humidified particle mass allow avoiding complications that occur in the commonly used mobility-diameter-based HTDMA technique due to poorly defined particle morphology and density.

scholarly journals Effect of mixing structure on the water uptake of mixtures of ammonium sulfate and phthalic acid particles

2021 ◽  
Vol 21 (3) ◽  
pp. 2179-2190
Author(s):  
Weigang Wang ◽  
Ting Lei ◽  
Andreas Zuend ◽  
Hang Su ◽  
Yafang Cheng ◽  
...  
Keyword(s):  
Growth Factor ◽  
Relative Humidity ◽  
Water Uptake ◽  
Phthalic Acid ◽  
Aerosol Particles ◽  
Core Shell ◽  
Hygroscopic Growth ◽  
The Core ◽  
Mass Fractions ◽  
Mixing States

Abstract. Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. There are, however, few current studies on the mixing structure effects on aerosol hygroscopicity. Here, we investigated the hygroscopicity of ammonium sulfate / phthalic acid (AS / PA) aerosol particles with different mass fractions of PA in different mixing states in terms of initial particle generation. Firstly, the effect of PA coatings on the hygroscopic behavior of the core-shell-generated mixtures of AS with PA was studied using a coating hygroscopicity tandem differential mobility analyzer (coating HTDMA). The slow increase in the hygroscopic growth factor of core-shell-generated particles is observed with increasing thickness of the coating PA prior to the deliquescence relative humidity (DRH) of AS. At relative humidity (RH) above 80 %, a decrease in the hygroscopic growth factor of particles occurs as the thickness of the PA shell increases, which indicates that the increase of PA mass fractions leads to a reduction of the overall core-shell-generated particle hygroscopicity. In addition, the use of the Zdanovskii–Stokes–Robinson (ZSR) relation leads to the underestimation of the measured growth factors of core-shell-generated particles without consideration of the morphological effect of core-shell-generated particles, especially at higher RH. Secondly, in the case of the AS / PA initially well-mixed particles, a shift of the DRH of AS (∼80 %, Tang and Munkelwitz, 1994) to lower RH is observed due to the presence of PA in the initially well-mixed particles. The predicted hygroscopic growth factor using the ZSR relation is consistent with the measured hygroscopic growth factor of the initially well-mixed particles. Moreover, we compared and discussed the influence of mixing states on the water uptake of AS / PA aerosol particles. It is found that the hygroscopic growth factor of the core-shell-generated particles is slightly higher than that of the initially well-mixed particles with the same mass fractions of PA at RH above 80 %. The observation of AS / PA particles may contribute to a growing field of knowledge regarding the influence of coating properties and mixing structure on water uptake.

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

2014 ◽  
Vol 14 (20) ◽  
pp. 11165-11183 ◽  
Author(s):  
T. Lei ◽  
A. Zuend ◽  
W. G. Wang ◽  
Y. H. Zhang ◽  
M. F. Ge
Keyword(s):  
Growth Factors ◽  
Humic Acid ◽  
Ammonium Sulfate ◽  
Organic Compounds ◽  
Water Uptake ◽  
Biomass Burning ◽  
Aerosol Particles ◽  
Hydroxybenzoic Acid ◽  
Hygroscopic Growth ◽  
Mass Fractions

Abstract. 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 effects), which are not considered in the models. Hygroscopic growth factors of mixed particles containing humic acid are well reproduced by the ZSR relation. Lastly, the organic surrogate compounds represent a selection of some of the most abundant pyrolysis products of biomass burning. The hygroscopic growths of mixtures of the organic surrogate compounds with ammonium sulfate with increasing organics mass fraction representing ambient conditions from the wet to the dry seasonal period in the Amazon basin, exhibit significant water uptake prior to the deliquescence of ammonium sulfate. The measured water absorptions of mixtures of several organic surrogate compounds (including levoglucosan) with ammonium sulfate are close to those of binary mixtures of levoglucosan with ammonium sulfate, indicating that levoglucosan constitutes a major contribution to the aerosol water uptake prior to (and beyond) the deliquescence of ammonium sulfate. Hence, certain hygroscopic organic surrogate compounds can substantially affect the deliquescence point of ammonium sulfate and overall particle water uptake.

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