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Title: Lability of secondary organic particulate matter

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [3];  [4];  [5];  [6]; ORCiD logo [7]
  1. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
  2. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences ; University of Macau (China). Department of Civil and Environmental Engineering, Faculty of Science and Technology
  3. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences ; Harvard University, Boston, MA (United States). T. H. Chan School of Public Health
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Sciences and Global Change Division
  6. University of British Columbia, Vancouver, BC (Canada). Department of Chemistry
  7. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences

Accurate simulations of the consenctrations of atmospheric organic particulate matter (PM) are needed for predicting energy flow in the Earth’s climate system. In the past, simulations of organic PM widely assume equilibrium partitioning of semivolatile organic compounds (SVOCs) between the PM and surrounding vapor. Herein, we test this assumption by measuring evaporation rates and associated vapor mass concentration of organic films representative of atmospheric PM. For films representing anthropogenic PM, evaporation rates and vapor mass concentrations increased above a threshold relative humidity (RH), indicating equilibrium partitioning above a transition RH but not below. In contrast for films representing biogenic PM, no threshold was observed, indicating equilibrium partitioning at all RHs. The results suggest that the mass lability of atmospheric organic PM can differ in consequential ways among Earth’s natural biomes, polluted regions, and regions of land-use change, and these differences need to be considered when simulating atmospheric organic PM.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; AC05-76RL01830
OSTI ID:
1377574
Alternate ID(s):
OSTI ID: 1340828
Report Number(s):
PNNL-SA-115585; ark:/13030/qt2cb5j6ng
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 113, Issue 45; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 80 works
Citation information provided by
Web of Science

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Cited By (22)

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition journal January 2018
Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol text January 2019
Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes–Einstein and fractional Stokes–Einstein relations journal January 2019
The viscosity of atmospherically relevant organic particles journal March 2018
Mixing times of organic molecules within secondary organic aerosol particles: a global planetary boundary layer perspective journal January 2017
Optimization of process models for determining volatility distribution and viscosity of organic aerosols from isothermal particle evaporation data journal January 2019
Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol text January 2019
Mixing of secondary organic aerosols versus relative humidity journal October 2016
Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol journal January 2019
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors journal January 2019
Arctic marine secondary organic aerosol contributes significantly to summertime particle size distributions in the Canadian Arctic Archipelago journal January 2019
Global distribution of particle phase state in atmospheric secondary organic aerosols journal April 2017
A review of experimental techniques for aerosol hygroscopicity studies 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
Anthropogenic influences on the physical state of submicron particulate matter over a tropical forest journal January 2017
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
Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter journal October 2018
Temperature-Dependent Viscosity of Organic Materials Characterized by Atomic Force Microscope journal November 2021
Predictions of the glass transition temperature and viscosity of organic aerosols from volatility distributions journal January 2020
Organic aerosol volatility and viscosity in the North China Plain: contrast between summer and winter journal January 2021
Investigation of water adsorption and hygroscopicity of atmospherically relevant particles using a commercial vapor sorption analyzer journal October 2017
Deconvolution of FIGAERO-CIMS thermal desorption profiles using positive matrix factorisation to identify chemical and physical processes during particle evaporation text January 2020