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Title: Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP)

Abstract

Cloud condensation nuclei (CCN) spectrum and the CCN activated fraction of size-resolved aerosols (SR-CCN) were measured at a rural site on Long Island during the Department of Energy (DOE) aerosol life cycle intensive operational period (ALC-IOP) from 15 July to 15 August 2011. During the last week of the ALC-IOP, the dependence of the activated fraction on aerosol volatility was characterized by sampling downstream of a thermodenuder (TD) operated at temperatures up to 100°C. Here we present aerosol properties, including aerosol total number concentration, CCN spectrum, and the CCN hygroscopicity, for air masses of representative origins during the ALC-IOP. The hygroscopicity of organic species in the aerosol is derived from CCN hygroscopicity and chemical composition. The dependence of organic hygroscopicity on the organic oxidation level (e.g., atomic O:C ratio) agrees well with theoretical predictions and results from previous laboratory and field studies. The derived κorg and O:C ratio first increase as TD temperature increases from 20°C (i.e., ambient temperature) to 50 or 75°C and then decrease as TD temperature further increases to 100°C. The initial increases of O:C and κorg with TD temperature below 50°C are likely due to evaporation of more volatile organics with relatively lower O:C and hygroscopicitymore » such as primary organic aerosol. At the high TD temperatures, the decreases of O:C and κorg indicate that evaporated organics were more oxygenated and had lower molecular weights. These trends are different from previous laboratory experiments and field observations, which reported that organic O:C increased monotonically with increasing TD temperature, whereas κorg decreased with the TD temperature. One possible reason is that previous studies were either focused on laboratory-generated secondary organic aerosol (SOA) or based on field observations at locations more dominated by SOA.« less

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ;
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Atmospheric Radiation Measurement (ARM) Data Center; Washington Univ., St. Louis, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Contributing Org.:
Argonne National Lab. (ANL); Oak Ridge National Lab. (ORNL)
OSTI Identifier:
1818607
Alternate Identifier(s):
OSTI ID: 1820930; OSTI ID: 1837830
Grant/Contract Number:  
SC0007178; FG02-11ER65293; SC0020259; SC0021017
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 21 Journal Issue: 17; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Mei, Fan, Wang, Jian, Zhou, Shan, Zhang, Qi, Collier, Sonya, and Xu, Jianzhong. Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP). Germany: N. p., 2021. Web. doi:10.5194/acp-21-13019-2021.
Mei, Fan, Wang, Jian, Zhou, Shan, Zhang, Qi, Collier, Sonya, & Xu, Jianzhong. Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP). Germany. https://doi.org/10.5194/acp-21-13019-2021
Mei, Fan, Wang, Jian, Zhou, Shan, Zhang, Qi, Collier, Sonya, and Xu, Jianzhong. Thu . "Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP)". Germany. https://doi.org/10.5194/acp-21-13019-2021.
@article{osti_1818607,
title = {Measurement report: Cloud condensation nuclei activity and its variation with organic oxidation level and volatility observed during an aerosol life cycle intensive operational period (ALC-IOP)},
author = {Mei, Fan and Wang, Jian and Zhou, Shan and Zhang, Qi and Collier, Sonya and Xu, Jianzhong},
abstractNote = {Cloud condensation nuclei (CCN) spectrum and the CCN activated fraction of size-resolved aerosols (SR-CCN) were measured at a rural site on Long Island during the Department of Energy (DOE) aerosol life cycle intensive operational period (ALC-IOP) from 15 July to 15 August 2011. During the last week of the ALC-IOP, the dependence of the activated fraction on aerosol volatility was characterized by sampling downstream of a thermodenuder (TD) operated at temperatures up to 100°C. Here we present aerosol properties, including aerosol total number concentration, CCN spectrum, and the CCN hygroscopicity, for air masses of representative origins during the ALC-IOP. The hygroscopicity of organic species in the aerosol is derived from CCN hygroscopicity and chemical composition. The dependence of organic hygroscopicity on the organic oxidation level (e.g., atomic O:C ratio) agrees well with theoretical predictions and results from previous laboratory and field studies. The derived κorg and O:C ratio first increase as TD temperature increases from 20°C (i.e., ambient temperature) to 50 or 75°C and then decrease as TD temperature further increases to 100°C. The initial increases of O:C and κorg with TD temperature below 50°C are likely due to evaporation of more volatile organics with relatively lower O:C and hygroscopicity such as primary organic aerosol. At the high TD temperatures, the decreases of O:C and κorg indicate that evaporated organics were more oxygenated and had lower molecular weights. These trends are different from previous laboratory experiments and field observations, which reported that organic O:C increased monotonically with increasing TD temperature, whereas κorg decreased with the TD temperature. One possible reason is that previous studies were either focused on laboratory-generated secondary organic aerosol (SOA) or based on field observations at locations more dominated by SOA.},
doi = {10.5194/acp-21-13019-2021},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 17,
volume = 21,
place = {Germany},
year = {Thu Sep 02 00:00:00 EDT 2021},
month = {Thu Sep 02 00:00:00 EDT 2021}
}

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