A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio

Zhang, Xuan; Krechmer, Jordan E.; Groessl, Michael; Xu, Wen; Graf, Stephan; Cubison, Michael; Jayne, John T.; Jimenez, Jose L.; Worsnop, Douglas R.; Canagaratna, Manjula R.

doi:10.5194/acp-16-12945-2016

Title: A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio

Journal Article · Wed Oct 19 00:00:00 EDT 2016 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-16-12945-2016· OSTI ID:1360106

Zhang, Xuan ^[1];

^[2]; Groessl, Michael ^[3]; Xu, Wen ^[1]; Graf, Stephan ^[3]; Cubison, Michael ^[3]; Jayne, John T. ^[1]; Jimenez, Jose L. ^[2]; Worsnop, Douglas R. ^[1]; Canagaratna, Manjula R. ^[1]

Aerodyne Research Inc., Billerica, MA (United States)
Univ. of Colorado, Boulder, CO (United States); Cooperative Institute for Research in Environmental Sciences, Boulder, CO (United States)
TOFWERK, Thun (Switzerland)

Here, a new metric is introduced for representing the molecular signature of atmospherically relevant organic compounds, the collision cross section (Ω), a quantity that is related to the structure and geometry of molecules and is derived from ion mobility measurements. By combination with the mass-to-charge ratio (m/z), a two-dimensional Ω – m/z space is developed to facilitate the comprehensive investigation of the complex organic mixtures. A unique distribution pattern of chemical classes, characterized by functional groups including amine, alcohol, carbonyl, carboxylic acid, ester, and organic sulfate, is developed on the 2-D Ω – m/z space. Species of the same chemical class, despite variations in the molecular structures, tend to situate as a narrow band on the space and follow a trend line. Reactions involving changes in functionalization and fragmentation can be represented by the directionalities along or across these trend lines, thus allowing for the interpretation of atmospheric transformation mechanisms of organic species. The characteristics of trend lines for a variety of functionalities that are commonly present in the atmosphere can be predicted by the core model simulations, which provide a useful tool to identify the chemical class to which an unknown species belongs on the Ω – m/z space. Within the band produced by each chemical class on the space, molecular structural assignment can be achieved by utilizing collision-induced dissociation as well as by comparing the measured collision cross sections in the context of those obtained via molecular dynamics simulations.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0011105

OSTI ID:: 1360106

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 16, Issue 20; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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