The Organic Surfactant Pool on Secondary Organic Aerosol Particles
EMSL Project ID
49291
Abstract
Secondary organic aerosol (SOA) particles particles rank among the least understood atmospheric constituents in the climate system. Key questions concern their poorly quantified roles in cloud activation and radiative forcing. Our prior work shows that surface chemistry can help address these questions, given that the particle surface is the first entity encountered by an approaching gas phase species. Motivated by results obtained thus far for trans-beta-isoprene epoxydiol (IEPOX), we will test the following hypothesis across a broader range of possible particle precursor species: partitioning to the particle phase can affect further growth and propensity of an SOA particle to act as a cloud condensation nucleus (CCN) by affecting surface properties that regulate subsequent growth (by acting as a barrier or attractor) and hygroscopicity (by affecting surface tension) through formation of an organic surfactant pool at the SOA particle surface. This hypothesis will be tested by (1) synthesizing deuterated and unlabeled terpenes and their oxidation products in pure form at NU, (2) preparing SOA particles from them at Harvard, (3) making surface- and bulk-specific spectroscopic, chemical, and mechanistic measurements on these particles at Harvard, NU, and PNNL, specifically PNNL's unique SFG spectrometer, its mass spectrometry and NMR capabilities, and its computational resources, and (4) performing computational simulations of surfactant pool candidate compounds for comparison to experiment at Yale.
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
Co-Investigator(s)
Team Members
Related Publications
Be A.G., H. Chase, Y. Liu, M. Upshur, Y. Zhang, A. Tuladhar, and Z.A. Jessamy-Chase, et al. 2019. "Atmospheric ß-Caryophyllene-Derived Ozonolysis Products at Interfaces." ACS Earth and Space Chemistry 3, no. 2:158-169. PNNL-SA-140243. doi:10.1021/acsearthspacechem.8b00156
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 H, S Chen, L Fu, MA Upshur, B Rudshteyn, R Thomson, H Wang, V Batista, and FM Geiger. 2017. "Orientations of Nonlocal Vibrational Modes from Combined Experimental and Theoretical Sum Frequency Spectroscopy." Chemical Physics Letters 683:199-204. doi:10.1016/j.cplett.2017.01.015
Upshur M.A., M. Vega, A.G. Be, H.M. Chase, Y. Zhang, A. Tuladhar, and Z.A. Jessamy-Chase, et al. 2019. "Synthesis and Surface Spectroscopy of alpha-Pinene Isotopologues and Their Corresponding Secondary Organic Material." Chemical Science 10, no. 36:8390-8398. PNNL-SA-143837. doi:10.1039/c9sc02399b