Preprints
https://doi.org/10.5194/egusphere-2023-1821
https://doi.org/10.5194/egusphere-2023-1821
05 Sep 2023
 | 05 Sep 2023

Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and remote environments

Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr

Abstract. The apparent volatility of atmospheric organic aerosol (OA) particles is determined by their chemical composition and environmental conditions (e.g., ambient temperature). A quantitative, experimental assessment of volatility and the respective importance of these two factors remains challenging, especially in ambient measurements. We present molecular composition and volatility of oxygenated OA (OOA) particles in different rural, urban, and remote environments across the globe (including Chacaltaya, Bolivia; Alabama, U.S.; Hyytiälä, Finland; Stuttgart and Karlsruhe, Germany; and Delhi, India) based on deployments of a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO-CIMS). We find on average larger carbon numbers (nC) and lower oxygen-to-carbon (O:C) ratios at the urban sites (nC: 9.8±0.7; O:C: 0.76±0.03; average ± 1 standard deviation), compared to the rural (nC: 8.8±0.6; O:C: 0.80±0.05) and remote mountain stations (nC: 8.1±0.8; O:C: 0.91±0.07), indicative of different emission sources and chemistry. Compounds containing only carbon, hydrogen, and oxygen atoms (CHO) contribute highest to the total OOA mass at the rural sites (79.9±5.2 %), in accordance with their proximity to forested areas (66.2±5.5 % at the mountain sites and 72.6±4.3 % at the urban sites). The largest contribution of nitrogen-containing compounds (CHON) are found at the urban stations (27.1±4.3 %), consistent with their higher NOx levels. Besides, we parametrize OOA volatility (saturation mass concentrations, Csat) using molecular composition information and compare it with the bulk apparent volatility derived from thermal desorption of the OOA particles within the FIGAERO. We find differences in Csat values of up to ~3 orders of magnitude, and variation in thermal desorption profiles (thermograms) across different locations and systems. From our study, we draw the general conclusion that environmental conditions (e.g., ambient temperature) do not directly affect OOA apparent volatility, but rather indirectly by influencing the sources and chemistry of the environment and thus the chemical composition. The comprehensive global dataset provides results that show the complex thermodynamics and chemistry of OOA and their changes during its lifetime in the atmosphere, and that generally the chemical description of OOA suffices to predict its apparent volatility, at least qualitatively. Our study thus provides new insights that will help guide choices of e.g. descriptions of OOA volatility in different model frameworks which has been previously simplified due to challenges to measure and represent it in models.

Journal article(s) based on this preprint

28 Feb 2024
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024,https://doi.org/10.5194/acp-24-2607-2024, 2024
Short summary
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-1821', Anonymous Referee #1, 02 Oct 2023
  • RC2: 'Comment on egusphere-2023-1821', Anonymous Referee #2, 04 Oct 2023
  • AC1: 'Response to all referee comments on egusphere-2023-1821', Wei Huang, 21 Dec 2023

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-1821', Anonymous Referee #1, 02 Oct 2023
  • RC2: 'Comment on egusphere-2023-1821', Anonymous Referee #2, 04 Oct 2023
  • AC1: 'Response to all referee comments on egusphere-2023-1821', Wei Huang, 21 Dec 2023

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by Wei Huang on behalf of the Authors (21 Dec 2023)  Author's response   Author's tracked changes   Manuscript 
ED: Referee Nomination & Report Request started (29 Dec 2023) by Joachim Curtius
RR by Anonymous Referee #1 (04 Jan 2024)
RR by Anonymous Referee #2 (09 Jan 2024)
ED: Publish subject to technical corrections (09 Jan 2024) by Joachim Curtius
AR by Wei Huang on behalf of the Authors (10 Jan 2024)  Manuscript 

Journal article(s) based on this preprint

28 Feb 2024
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024,https://doi.org/10.5194/acp-24-2607-2024, 2024
Short summary
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr

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Latest update: 28 Feb 2024
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Short summary
We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and remote environments across the globe. We did a comprehensive investigation of the relationship between chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.