Identifying the source of ice nucleating particles in biomass burning aerosol, and the effect of chemical aging and freeze-drying on their freezing properties
EMSL Project ID
49241
Abstract
The nanoscale surface features that create efficient ice active sites on atmospheric particles that control heterogeneous ice nucleation remain largely unknown. Cloud glaciation induced by these ice nucleating particles has significant impacts on the evolution of cloud structure and microphysics, optical properties, and the onset and intensity of precipitation. Our incomplete understanding of the physicochemical particle properties that dictate heterogeneous ice nucleation ability results in large uncertainties in our ability to accurately understand and predict the effects of aerosol particles on clouds and climate change. How ice nucleation properties evolve as particles experience physical and chemical aging during atmospheric transport is an especially enigmatic yet critically important process.Biomass burning particles have recently been identified as a surprisingly strong source of ice nucleating particles, though the specific particle compositions and surface properties that contain ice active sites in this complex combustion aerosol are not yet understood. Recent experiments at Carnegie Mellon University (CMU) have found that photochemical aging of biomass burning aerosol (BBA) in a large chamber reactor caused a significant increase in the freezing temperature of droplets containing BBA compared to the unaged particles. We suspect the oxidation of soot surfaces to be the cause of this enhancement in freezing activity, but the comprehensive and sophisticated single-particle analysis resources and expertise only available at EMSL are required to thoroughly investigate this hypothesis. We also suspect that the creation of highly porous soot particles through "freeze drying" induced by ice nucleation may significantly alter the BBA's ice nucleation properties for subsequent ice nucleation events. We do not possess the sophisticated instrumentation nor the expertise at CMU to perform the necessary comprehensive particle analysis to address the stated hypotheses.
BBA particles collected on Nuclepore polycarbonate filters, and Cu TEM grids and silicon wafer substrates will be sent to EMSL for detailed multi-dimensional spectromicropscopic analysis. BBA particles for analysis will be collected from the chamber reactor before and after simulated atmospheric aging, and ice-active BBA particles contained in frozen droplets will also be selected for analysis. High size resolution of particle composition, carbon oxidation state, particle morphology, and surface physicochemical properties will be obtained using environmental scanning electron microscopy (ESEM) with EDX compositional analysis, and focused ion beam (FIB) analysis of particle internal structure, transmission electron microscopy (TEM) with EELS analysis of surface composition, Raman microscopy for chemical composition, and nano-SIMS for high size resolution measurements of atomic and molecular surface composition. The comprehensive offline analysis of particle physicochemical properties achieved using EMSL resources will be combined with the online particle composition analysis obtained during chamber aging at CMU, and CMU's measurements of the aerosol's immersion and contact freezing properties. This integrated dataset will produce first of its kind parameterizations describing the relationship between ice nucleation properties, particle composition, and chemical aging of biomass burning aerosol, in unprecedented detail. These descriptions will significantly improve the predictions of aerosol-cloud-climate-precipitation interactions obtained from sophisticated atmospheric chemical transport, cloud, and climate models developed through DOE's Atmospheric System Research program, for an increasingly important global source of atmospheric aerosol particles.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Bailey B. Bowers, Lydia G. Jahl, Leif G. Jahn, Ryan C. Sullivan. 2021. "Morphology of Organic Carbon Coatings on Biomass-Burning Particles and Their Role in Reactive Gas Uptake." ACS Earth and Space Chemistry 5 (9):2184-2195. 10.1021/acsearthspacechem.1c00237
Bailey B. Bowers, Lydia G. Jahl, Leif G. Jahn, Ryan C. Sullivan, Joel A. Thornton. 2021. "Response of the Reaction Probability of N2O5 with Authentic Biomass-Burning Aerosol to High Relative Humidity." ACS Earth and Space Chemistry 5 (10):2587-2598. 10.1021/acsearthspacechem.1c00227
Bailey B. Bowers, Thomas A. Brubaker, Kerrigan P. Cain, William D. Fahy, Sara Graves, Lydia G. Jahl, Leif G. Jahn, Michael J. Polen, Ryan C. Sullivan. 2021. "Atmospheric aging enhances the ice nucleation ability of biomass-burning aerosol." Science Advances 7 (9) 10.1126/sciadv.abd3440
Garret D. Bland, Bailey B. Bowers, Lydia G. Jahl, Leif G. Jahn, Luke W. Monroe, Ryan C. Sullivan. 2020. "Metallic and Crustal Elements in Biomass-Burning Aerosol and Ash: Prevalence, Significance, and Similarity to Soil Particles." ACS Earth and Space Chemistry 5 (1):136-148. 10.1021/acsearthspacechem.0c00191
Thomas A. Brubaker, Lydia G. Jahl, Leif G. Jahn, Michael J. Polen, Joshua Somers, Ryan C. Sullivan. 2020. "Biomass combustion produces ice-active minerals in biomass-burning aerosol and bottom ash." Proceedings of the National Academy of Sciences 117 (36):21928-21937. 10.1073/pnas.1922128117