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Title: Effect of varying experimental conditions on the viscosity of α-pinene derived secondary organic material

Journal Article · · Atmospheric Chemistry and Physics (Online)
 [1];  [2];  [3];  [1];  [3];  [1];  [3];  [4];  [1]
  1. Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
  2. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences
  3. Leibniz Inst. for Tropospheric Research, Leipzig (Germany)
  4. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences and Dept. of Earth and Planetary Sciences

Knowledge of the viscosity of particles containing secondary organic material (SOM) is useful for predicting reaction rates and diffusion in SOM particles. In this study we investigate the viscosity of SOM particles as a function of relative humidity and SOM particle mass concentration, during SOM synthesis. The SOM was generated via the ozonolysis of α-pinene at < 5 % relative humidity (RH). Experiments were carried out using the poke-and-flow technique, which measures the experimental flow time (τexp, flow) of SOM after poking the material with a needle. In the first set of experiments, we show that τexp, flow increased by a factor of 3600 as the RH increased from < 0.5 RH to 50 % RH, for SOM with a production mass concentration of 121 µg m-3. Based on simulations, the viscosities of the particles were between 6 × 105 and 5 × 107 Pa s at < 0.5 % RH and between 3 × 102 and 9 × 103 Pa s at 50 % RH. In the second set of experiments we show that under dry conditions τexp, flow decreased by a factor of 45 as the production mass concentration increased from 121 to 14 000 µg m-3. From simulations of the poke-and-flow experiments, the viscosity of SOM with a production mass concentration of 14 000 µg m-3 was determined to be between 4 × 104 and 1.5 × 106 Pa s compared to between 6 × 105 and 5 × 107 Pa s for SOM with a production mass concentration of 121 µg m-3. The results can be rationalized by a dependence of the chemical composition of SOM on production conditions. Lastly, these results emphasize the shifting characteristics of SOM, not just with RH and precursor type, but also with the production conditions, and suggest that production mass concentration and the RH at which the viscosity was determined should be considered both when comparing laboratory results and when extrapolating these results to the atmosphere.

Research Organization:
Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemistry
Sponsoring Organization:
National Science Foundation (NSF); USDOE
OSTI ID:
1375407
Journal Information:
Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 10 Vol. 16; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
United States
Language:
English

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Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol journal June 2017
Temperature- and Humidity-Dependent Phase States of Secondary Organic Aerosols journal January 2019
The viscosity of atmospherically relevant organic particles journal March 2018
Amorphous phase state diagrams and viscosity of ternary aqueous organic/organic and inorganic/organic mixtures journal January 2018
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Perspectives on the Future of Ice Nucleation Research: Research Needs and Unanswered Questions Identified from Two International Workshops journal July 2017
Perspectives on the Future of Ice Nucleation Research: Research Needs and Unanswered Questions Identified from Two International Workshops text January 2017
Mixing times of organic molecules within secondary organic aerosol particles: a global planetary boundary layer perspective journal January 2017
Diffusion coefficients of organic molecules in sucrose–water solutions and comparison with Stokes–Einstein predictions journal January 2017
The effect of hydroxyl functional groups and molar mass on the viscosity of non-crystalline organic and organic–water particles journal January 2017
Influence of relative humidity on the heterogeneous oxidation of secondary organic aerosol journal January 2018
Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition journal January 2018
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors journal January 2019
Viscosities, diffusion coefficients, and mixing times of intrinsic fluorescent organic molecules in brown limonene secondary organic aerosol and tests of the Stokes–Einstein equation journal January 2019
Viscosity of erythritol and erythritol–water particles as a function of water activity: new results and an intercomparison of techniques for measuring the viscosity of particles journal January 2018