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A new metric is introduced for representing the molecular signature ofatmospherically relevant organic compounds, the collision cross section(Ω), a quantity that is related to the structure andgeometry of molecules and is derived from ion mobility measurements. Bycombination with the mass-to-charge ratio (m∕z), a two-dimensionalΩ − m∕z space is developed to facilitate the comprehensiveinvestigation of the complex organic mixtures. A unique distribution patternof chemical classes, characterized by functional groups including amine,alcohol, carbonyl, carboxylic acid, ester, and organic sulfate, is developedon the 2-D Ω − m∕z space. Species of the same chemical class,despite variations in the molecular structures, tend to situate as a narrowband on the space and follow a trend line. Reactions involving changes infunctionalization and fragmentation can be represented by thedirectionalities along or across these trend lines, thus allowing for theinterpretation of atmospheric transformation mechanisms of organic species.The characteristics of trend lines for a variety of functionalities that arecommonly present in the atmosphere can be predicted by the core modelsimulations, which provide a useful tool to identify the chemical class towhich an unknown species belongs on the Ω − m∕z space. Withinthe band produced by each chemical class on the space, molecular structuralassignment can be achieved by utilizing collision-induced dissociation aswell as by comparing the measured collision cross sections in the context ofthose obtained via molecular dynamics simulations

atmospheric chemistry and physics

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