Probing the Vibrational Coherences of Organic Atmospheric Aerosol Systems
EMSL Project ID
48842
Abstract
This proposal focuses on applying EMSL’s sub-1cm-1-resolution vibrational spectroscopy (hr-SFG) capabilities (Hongfei Wang), solid state NMR spectroscopy (Nancy Washton), nano-DESI high-resolution mass spectrometry analysis techniques (Julia and Alex Laskin), and high-performance computing clusters to improve our molecular-scale understanding of the organic species that are present within and at the surfaces of secondary aerosol (SOA) particles. The proposed studies described herein are supported by new insights that were recently published with data collected at EMSL’s hr-SFG spectrometer in the group of Hongfei Wang, in Victor Batista’s computational chemistry group at Yale University, in the laboratories of Franz Geiger (SFG) and Regan Thomson (organic synthesis) at Northwestern University, and in Scot Martin’s environmental chamber and flow tube at Harvard University. As part of this proposed project, we will use PNNL’s facilities to test SOA particle properties and formation mechanisms by ‘fast-forwarding’ through chemical reaction pathways proposed by others. Specifically, we will:
A) Analyze the vibrational surface and bulk responses of SOA particle material prepared from the dark ozonolysis of unlabeled and isotope-labeled terpene precursors such as alpha-pinene;
B) Determine the chemical composition and molecular structure of said labeled and unlabeled SOA particle material using solid-state NMR and mass spectrometric responses; and
C) Compare the results to those obtained from synthesized reference compounds, as well as field-derived and size-resolved SOA particles samples from GoAmazon2014/5.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2015-10-01
End Date
2016-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Chase HM, J Ho, MA Upshur, R Thomson, V Batista, and FM Geiger. 2017. "Unanticipated Stickiness of alpha-Pinene." Journal of Physical Chemistry A 121(17):3239–3246. doi:10.1021/acs.jpca.6b12653
Chase HM, Upshur MA, Ho J, Strick BL, Psciuk B, Rudshteyn B, Ebben CJ, Fu L, Wang HF, Zhang Y, Martin ST, Thomson RJ, Batista VS, Geiger FM. Counterfactual-Enabled Molecular Spectroscopy of Alpha-Pinene and its Deuterated Isotopologues. Poster presented at: 63rd Pacific Conference on Spectroscopy and Dynamics; 2016 Jan 28-31; Alisomar, CA.
Geiger FM. 2015. "Toward the Identification of Molecular Constituents Associated with the Surfaces of Isoprene-Derived Secondary Organic Aerosol (SOA) Particles." Presented by Geiger, Franz (Invited Speaker) at American Chemical Society National Meeting, Denver, CO on March 22, 2015.