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

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 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,more » 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 ≈ 0.15) and a Colorado boreal forest (κv ≈ 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 partly 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 time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.« less

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [3]; ORCiD logo [3];  [2];  [2];  [4];  [5];  [6]
+ Show Author Affiliations
  1. Max Planck Institute for Chemistry, Mainz (Germany); St. Petersburg State Univ., St. Petersburg (Russia)
  2. St. Petersburg State Univ., St. Petersburg (Russia)
  3. Max Planck Institute for Chemistry, Mainz (Germany)
  4. Max Planck Institute for Intelligent Systems, Stuttgart (Germany)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Max Plank Institute for Chemistry, Mainz (Germany)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1209326
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics Discussions (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics Discussions (Online); Journal Volume: 15; Journal Issue: 6; Journal ID: ISSN 1680-7375
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

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., and Andreae, M. O. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign. United States: N. p., 2015. Web. doi:10.5194/acpd-15-7837-2015.
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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. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign. United States. https://doi.org/10.5194/acpd-15-7837-2015
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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., and Andreae, M. O. Mon . "Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign". United States. https://doi.org/10.5194/acpd-15-7837-2015. https://www.osti.gov/servlets/purl/1209326.
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@article{osti_1209326,
title = {Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign},
author = {Mikhailov, E. F. and Mironov, G. N. and Pöhlker, C. and Chi, X. and Krüger, M. L. and Shiraiwa, M. and Förster, J. -D. and Pöschl, U. and Vlasenko, S. S. and Ryshkevich, T. I. and Weigand, M. and Kilcoyne, A. L. D. and Andreae, M. O.},
abstractNote = {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 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 ≈ 0.15) and a Colorado boreal forest (κv ≈ 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 partly 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 time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.},
doi = {10.5194/acpd-15-7837-2015},
journal = {Atmospheric Chemistry and Physics Discussions (Online)},
number = 6,
volume = 15,
place = {United States},
year = {Mon Mar 16 00:00:00 EDT 2015},
month = {Mon Mar 16 00:00:00 EDT 2015}
}
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Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid
posted_content, October 2006

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