A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio
Abstract
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.more »
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1360106
- Grant/Contract Number:
- SC0011105
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Atmospheric Chemistry and Physics (Online)
- Additional Journal Information:
- Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 16; Journal Issue: 20; Journal ID: ISSN 1680-7324
- Publisher:
- European Geosciences Union
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhang, Xuan, Krechmer, Jordan E., Groessl, Michael, Xu, Wen, Graf, Stephan, Cubison, Michael, Jayne, John T., Jimenez, Jose L., Worsnop, Douglas R., and Canagaratna, Manjula R. A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio. United States: N. p., 2016.
Web. doi:10.5194/acp-16-12945-2016.
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. A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio. United States. https://doi.org/10.5194/acp-16-12945-2016
Zhang, Xuan, Krechmer, Jordan E., Groessl, Michael, Xu, Wen, Graf, Stephan, Cubison, Michael, Jayne, John T., Jimenez, Jose L., Worsnop, Douglas R., and Canagaratna, Manjula R. Wed .
"A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio". United States. https://doi.org/10.5194/acp-16-12945-2016. https://www.osti.gov/servlets/purl/1360106.
@article{osti_1360106,
title = {A novel framework for molecular characterization of atmospherically relevant organic compounds based on collision cross section and mass-to-charge ratio},
author = {Zhang, Xuan and Krechmer, Jordan E. and Groessl, Michael and Xu, Wen and Graf, Stephan and Cubison, Michael and Jayne, John T. and Jimenez, Jose L. and Worsnop, Douglas R. and Canagaratna, Manjula R.},
abstractNote = {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.},
doi = {10.5194/acp-16-12945-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 20,
volume = 16,
place = {United States},
year = {Wed Oct 19 00:00:00 EDT 2016},
month = {Wed Oct 19 00:00:00 EDT 2016}
}
Web of Science
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