Molecular Insights into Gas–Particle Partitioning and Viscosity of Atmospheric Brown CarbonClick to copy article linkArticle link copied!
- Qiaorong XieQiaorong XieDepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Qiaorong Xie
- Nealan G. A. GerrebosNealan G. A. GerrebosDepartment of Chemistry, University of British Columbia, Vancouver, V6T 1Z1 BC, CanadaMore by Nealan G. A. Gerrebos
- Diego Calderon-ArrietaDiego Calderon-ArrietaDepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Diego Calderon-Arrieta
- Isaac S. MortonIsaac S. MortonDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Isaac S. Morton
- Emily R. HalpernEmily R. HalpernDepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Emily R. Halpern
- Chunlin LiChunlin LiCollege of Environmental Science and Engineering, Tongji University, Shanghai 200072, ChinaMore by Chunlin Li
- Mei Fei ZengMei Fei ZengDepartment of Chemistry, University of British Columbia, Vancouver, V6T 1Z1 BC, CanadaMore by Mei Fei Zeng
- Allan K. BertramAllan K. BertramDepartment of Chemistry, University of British Columbia, Vancouver, V6T 1Z1 BC, CanadaMore by Allan K. Bertram
- Yinon RudichYinon RudichDepartment of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, IsraelMore by Yinon Rudich
- Alexander Laskin*Alexander Laskin*Email: [email protected]Department of Chemistry and Department of Earth, Atmospheric, and Planetary Sciences, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Alexander Laskin
Abstract
Biomass burning organic aerosol (BBOA), containing brown carbon chromophores, plays a critical role in atmospheric chemistry and climate forcing. However, the effects of evaporation on BBOA volatility and viscosity under different environmental conditions remain poorly understood. This study focuses on the molecular characterization of laboratory-generated BBOA proxies from wood pyrolysis emissions. The initial mixture, “pyrolysis oil (PO1)”, was progressively evaporated to produce more concentrated mixtures (PO1.33, PO2, and PO3) with volume reduction factors of 1.33, 2, and 3, respectively. Chemical speciation and volatility were investigated using temperature-programmed desorption combined with direct analysis in real-time ionization and high-resolution mass spectrometry (TPD-DART-HRMS). This novel approach quantified saturation vapor pressures and enthalpies of individual species, enabling the construction of volatility basis set distributions and the quantification of gas–particle partitioning. Viscosity estimates, validated by poke-flow experiments, showed a significant increase with evaporation, slowing particle-phase diffusion and extending equilibration times. These findings suggest that highly viscous tar ball particles in aged biomass burning emissions form as semivolatile components evaporate. The study highlights the importance of evaporation processes in shaping BBOA properties, underscoring the need to incorporate these factors into atmospheric models for better predictions of BBOA aging and its environmental impact.
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This article is cited by 6 publications.
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- Markus Ammann. Concluding remarks: Atmospheric chemistry in cold environments. Faraday Discussions 2025, 258 , 597-613. https://doi.org/10.1039/D5FD00042D
- Yafeng Gou, Mingjie Xie, Jing Chen. The phase state and viscosity of organic aerosol and related impacts on atmospheric physicochemical processes: A review. Atmospheric Environment 2025, 343 , 120985. https://doi.org/10.1016/j.atmosenv.2024.120985
- Qiaorong Xie, Alexander Laskin. Molecular characterization of atmospheric organic aerosols: Contemporary applications of high-resolution mass spectrometry. TrAC Trends in Analytical Chemistry 2024, 181 , 117986. https://doi.org/10.1016/j.trac.2024.117986
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