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Title: Molecular formula composition of β-caryophyllene ozonolysis SOA formed in humid and dry conditions

Here, we studied the molecular formula composition of six β-caryophyllene SOA samples using ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry under various reaction conditions. The SOA samples were generated in dry or low relative humidity (RH) chamber conditions with or without cyclohexane. All of the studied SOA mass spectra have three distinct clusters of hundreds of negative ions referred to as Group I (100 < m/z < 400), Group II (400 < m/z < 700) and Group III (700 < m/z < 1 000) compounds. C 14-16H 22-28O 2-11, C 28-29H 42-48O 6-16 and C 42-43H 68-70O 14-16 were observed as highly abundant organic compounds in the compound class of Group I, II and III, respectively. The relative intensities of most analytes were higher in humid conditions compared to those in dry conditions, indicating the importance of water-dependent reactions and the catalytic role of water both in the presence and absence of cyclohexane. In addition, molecular formulas with higher average carbon numbers were observed in humid SOA than in dry SOA in the absence of cyclohexane, suggesting a decrease of cleavage reactions in humid condition. This study characterizes β-caryophyllene ozonolysis SOA based on ultrahigh mass resolution and demonstratesmore » the significance of humidity in terms of the molecular distributions and relative abundances of the analytes. We also discuss the possible mechanism for the formation of Group I-III compounds based on the current understanding of SOA formation in the atmosphere.« less
Authors:
 [1] ;  [2] ;  [2] ; ORCiD logo [2] ;  [3]
  1. Michigan Technological Univ., Houghton, MI (United States). Dept. of Chemistry; Univ. of Massachusetts, Amherst, MA (United States). Dept. of Chemistry
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Michigan Technological Univ., Houghton, MI (United States). Dept. of Chemistry; Michigan Technological Univ., Houghton, MI (United States). Atmospheric Science Program
Publication Date:
Report Number(s):
LA-UR-17-28024
Journal ID: ISSN 1352-2310
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Atmospheric Environment (1994)
Additional Journal Information:
Journal Name: Atmospheric Environment (1994); Journal Volume: 154; Journal Issue: C; Journal ID: ISSN 1352-2310
Publisher:
Elsevier
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; Gordon and Betty Moore Foundation; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Analytical Chemistry; Earth Sciences; secondary organic aerosols; beta-caryophyllene; ozonolysis; Smog-chamber; SOA; High resolution mass spectrometry; FT-ICR
OSTI Identifier:
1412872
Alternate Identifier(s):
OSTI ID: 1398733

Kundu, Shuvashish, Fisseha, Rebeka, Putman, Annie L., Rahn, Thomas A., and Mazzoleni, Lynn R.. Molecular formula composition of β-caryophyllene ozonolysis SOA formed in humid and dry conditions. United States: N. p., Web. doi:10.1016/j.atmosenv.2016.12.031.
Kundu, Shuvashish, Fisseha, Rebeka, Putman, Annie L., Rahn, Thomas A., & Mazzoleni, Lynn R.. Molecular formula composition of β-caryophyllene ozonolysis SOA formed in humid and dry conditions. United States. doi:10.1016/j.atmosenv.2016.12.031.
Kundu, Shuvashish, Fisseha, Rebeka, Putman, Annie L., Rahn, Thomas A., and Mazzoleni, Lynn R.. 2016. "Molecular formula composition of β-caryophyllene ozonolysis SOA formed in humid and dry conditions". United States. doi:10.1016/j.atmosenv.2016.12.031. https://www.osti.gov/servlets/purl/1412872.
@article{osti_1412872,
title = {Molecular formula composition of β-caryophyllene ozonolysis SOA formed in humid and dry conditions},
author = {Kundu, Shuvashish and Fisseha, Rebeka and Putman, Annie L. and Rahn, Thomas A. and Mazzoleni, Lynn R.},
abstractNote = {Here, we studied the molecular formula composition of six β-caryophyllene SOA samples using ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry under various reaction conditions. The SOA samples were generated in dry or low relative humidity (RH) chamber conditions with or without cyclohexane. All of the studied SOA mass spectra have three distinct clusters of hundreds of negative ions referred to as Group I (100 < m/z < 400), Group II (400 < m/z < 700) and Group III (700 < m/z < 1 000) compounds. C14-16H22-28O2-11, C28-29H42-48O6-16 and C42-43H68-70O14-16 were observed as highly abundant organic compounds in the compound class of Group I, II and III, respectively. The relative intensities of most analytes were higher in humid conditions compared to those in dry conditions, indicating the importance of water-dependent reactions and the catalytic role of water both in the presence and absence of cyclohexane. In addition, molecular formulas with higher average carbon numbers were observed in humid SOA than in dry SOA in the absence of cyclohexane, suggesting a decrease of cleavage reactions in humid condition. This study characterizes β-caryophyllene ozonolysis SOA based on ultrahigh mass resolution and demonstrates the significance of humidity in terms of the molecular distributions and relative abundances of the analytes. We also discuss the possible mechanism for the formation of Group I-III compounds based on the current understanding of SOA formation in the atmosphere.},
doi = {10.1016/j.atmosenv.2016.12.031},
journal = {Atmospheric Environment (1994)},
number = C,
volume = 154,
place = {United States},
year = {2016},
month = {12}
}