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α -Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity

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Huang, Wei, Saathoff, Harald, Pajunoja, Aki, Shen, Xiaoli, Naumann, Karl-Heinz, Wagner, Robert, Virtanen, Annele, Leisner, Thomas, Mohr, Claudia·2018·Atmospheric Chemistry and Physics
DOI 10.5194/acp-18-2883-2018

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Abstract

Abstract. Chemical composition and viscosity of secondary organic aerosol (SOA) from α-pinene (C10H16) ozonolysis were investigated for low temperature conditions (223 K). Two types of experiments were performed using two simulation chambers at the Karlsruhe Institute of Technology, the Aerosol Preparation and Characterization chamber (APC), and the Aerosol Interaction and Dynamics in the Atmosphere chamber (AIDA). Experiment type 1 simulated SOA formation at upper tropospheric conditions: SOA was generated in the AIDA chamber directly at 223 K, 61 % relative humidity (RH) (experiment termed cold humid, CH), or for comparison at 6 % RH (experiment termed cold dry, CD) conditions. Experiment type 2 simulated SOA uplifting: SOA was formed in the APC chamber at room temperature (296 K), <1 % RH (experiment termed warm dry, WD) or 21 % RH (experiment termed warm humid, WH) conditions, and then partially transferred to the AIDA chamber kept at 223 K, and 61 % RH (WDtoCH) or 30 % RH (WHtoCH), respectively. Precursor concentrations varied between 0.7 and 2.2 ppm α-pinene, and 2.3 and 1.8 ppm ozone for type 1 and type 2 experiments, respectively. Among other instrumentation, a chemical ionization mass spectrometer (CIMS) with filter inlet for gases and aerosols (FIGAERO), deploying I- as reagent ion, was used for SOA chemical composition analysis. For type 1 experiments with lower α-pinene concentration and cold SOA formation temperature (223 K), smaller particles of 100–300 nm vacuum aerodynamic diameter (dva) and higher mass fractions (>40 %) of adducts (molecules with more than 10 carbon atoms) of α-pinene oxidation products were observed. For type 2 experiments with higher α-pinene concentration and warm SOA formation temperature (296 K), larger particles (~500 nm dva) with smaller mass fractions of adducts (<35 %) were produced. We also observed differences (up to 20 ºC) in maximum desorption temperature (Tmax) of individual compounds desorbing from the particles deposited on the FIGAERO Teflon filter for different experiments, indicating that Tmax is not purely a function of a compound's vapor pressure or volatility, but is also influenced by diffusion limitations within the particles (particle viscosity), interactions between particles deposited on the filter (particle matrix), and/or particle mass on the filter. Highest Tmax were observed for SOA under dry conditions and with higher adduct mass fraction; lowest Tmax for SOA under humid conditions and with lowest adduct mass fraction. The observations indicate that particle viscosity may be influenced by intra- and inter-molecular hydrogen bonding between oligomers, and particle water uptake, even under such low temperature conditions. Our results suggest that particle physicochemical properties such as viscosity and oligomer content mutually influence each other, and that variation in Tmax of particle desorptions may provide implications for particle viscosity and particle matrix effects. The differences in particle physicochemical properties observed between our different experiments demonstrate the importance of taking experimental conditions into consideration when interpreting data from laboratory studies or using them as input in climate models.

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    “However, at an even lower temperature of 223 K, Huang et al. (2018) observed increased mass fractions of oligomers in the SOA formed from ɑ-pinene ozonolysis, which was attributed to increased hydrogen bonding in the higher viscosity SOA (compared to SOA formed at 296 K).”
    Background

Metadata

Authors
Huang, W., Saathoff, H., Pajunoja, A., Shen, X., Naumann, K.-H., Wagner, R., Virtanen, A., Leisner, T., & Mohr, C.
Affiliations
  • Karlsruhe Institute of Technology (DE)
  • University of Eastern Finland (FI)
Corresponding author
Mohr, Claudia
ORCID
Venue
Atmospheric Chemistry and Physics
Publisher
Copernicus GmbH
Published
2018-02-28
Volume
18
Issue
4
Pages
2883-2898
ISSN
  • 1680-7316 (ISSN-L)
  • 1680-7324
DOI
10.5194/acp-18-2883-2018
OpenAlex
W2753712924
Cited by
129
References
0
Citations by year
2026: 3 · 2025: 6 · 2024: 10 · 2023: 14 · 2022: 36 · 2021: 32 · 2020: 12 · 2019: 7 · 2018: 9
FWCI
7.31
Type
journal article
Language
en
Open access
Licence
Locations
  • Atmospheric chemistry and physics (publishedVersion, cc-by)
  • Repository KITopen (Karlsruhe Institute of Technology) (submittedVersion, cc-by)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • KITopen (cc-by)
Funders
  • European Research Council (335478)
  • Research Council of Finland (272041)
Topics
  • Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
  • Physical Sciences › Environmental Science › Global and Planetary Change › Atmospheric aerosols and clouds
  • Physical Sciences › Chemical Engineering › Fluid Flow and Transfer Processes › Advanced Combustion Engine Technologies
Keywords
secondary organic aerosol, α-pinene, ozonolysis, low temperature, particle viscosity, chemical composition, oligomerization, particle size distribution, relative humidity, SOA aging, upper troposphere, chemical ionization mass spectrometry, atmospheric oxidation products

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