Molecular Surface Spectroscopy of Secondary Organic Aerosol Particles
EMSL Project ID
47891
Abstract
This proposal focuses on applying EMSL's high-resolution vibrational spectroscopy (hr-SFG) capabilities (Hongfei Wang), nano-DESI high-resolution mass spectrometry analysis techniques (Julia and Alex Laskin), and high-performance computing clusters to carry out a molecular study of the organic species present at the surfaces of secondary aerosol (SOA) particles. The proposed studies are supported by exciting preliminary results obtained 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. We will: A) Carry out the first surface-specific studies -- and the first vibrational assignments -- of alpha-pinene and its oxidation products, enabled via isotopologues synthesized in homogeneous and pure form, at solid/vapor interfaces;
B) Perform the first study aimed at probing the presence of synthesized reference compounds in synthetic and natural, size-selected SOA particle material; and
C) Test SOA particle formation mechanisms by 'fast-forwarding' through chemical reaction pathways proposed by others.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2015-09-30
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.
Ho J, B Psciuk, H Chase, B Rudshteyn, MA Upshur, L Fu, R Thomson, H Wang, FM Geiger, and V Batista. 2016. "Sum Frequency Generation Spectroscopy and Molecular Dynamics Simulations Reveal A Rotationally Fluid Adsorption State of ?-Pinene on Silica." Journal of Physical Chemistry C 120(23):12578-12589. doi:10. 1021/acs. jpcc. 6b03158
Mifflin AL, LA Velarde Ruiz Esparza, J Ho, B Psciuk, C Negre, CJ Ebben, MA Upshur, Z Lu, B Strick, R Thomson, V Batista, H Wang, and FM Geiger. 2015. "Accurate Lineshapes from Sub-1 cm-1 Resolution Sum Frequency Generation Vibrational Spectroscopy of alpha-Pinene at Room Temperature." Journal of Physical Chemistry A. doi:10.1021/jp510700z
Shrestha M, Y Zhang, MA Upshur, P Liu, SL Blair, H Wang, S Nizkorodov, R Thomson, ST Martin, and FM Geiger. 2014. "On Surface Order and Disorder of ?-Pinene-Derived Secondary Organic Material." Journal of Physical Chemistry A. doi:10.1021/jp510780e