A First Principle Model of Differential Ion Mobility: the Effect of Ion-Solvent Clustering
- 21 November 2019
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Society for Mass Spectrometry
- Vol. 30 (12), 2711-2725
- https://doi.org/10.1007/s13361-019-02340-1
Abstract
The use of differential mobility spectrometry (DMS) as a separation tool prior to mass analysis has increased in popularity over the years. However, the fundamental principles behind the difference between high- and low-field mobility is still a matter of debate—especially regarding the strong impact of solvent molecules added to the gas phase in chemically modified DMS environments. In this contribution, we aim to present a thorough model for the determination of the ion mobility over a wide range of field strengths and subsequent calculation of DMS dispersion plots. Our model relies on first principle calculations only, incorporating the modeling of the “hard-sphere” mobility, the change in CCS with field strength, and the degree of clustering of solvent molecules to the ion. We show that all three factors have to be taken into account to qualitatively predict dispersion plots. In particular, type A behavior (i.e., strong clustering) in DMS can only be explained by a significant change of the mean cluster size with field strengths. The fact that our model correctly predicts trends between differently strong binding solvents, as well as the solvent concentration and the background gas temperature, highlights the importance of clustering for differential mobility.Keywords
Funding Information
- Natural Sciences and Engineering Research Council of Canada (Discovery Grant)
- Deutscher Akademischer Austauschdienst
- Early Researcher Award
- Compute Canada
This publication has 63 references indexed in Scilit:
- Systematic Ion Source Parameter Assessment by Automated Determination of the Distribution of Ion Acceptance (DIA) Using APLIJournal of the American Society for Mass Spectrometry, 2019
- Fundamentals of ion mobility spectrometryCurrent Opinion in Chemical Biology, 2018
- Uniform Moment Theory for Charged Particle Motion in Gases. 2. Second ApproximationJournal of Statistical Physics, 2016
- Atmospheric Pressure Ion Source Development: Experimental Validation of Simulated Ion Trajectories within Complex Flow and Electrical FieldsJournal of the American Society for Mass Spectrometry, 2013
- Uniform Moment Theory for Charged Particle Motion in GasesJournal of the American Society for Mass Spectrometry, 2012
- Ion mobility spectrometry‐mass spectrometry (IMS‐MS) of small molecules: Separating and assigning structures to ionsMass Spectrometry Reviews, 2012
- Simulation of Ion Motion at Atmospheric Pressure: Particle Tracing Versus Electrokinetic FlowJournal of the American Society for Mass Spectrometry, 2011
- Ion Mobility SpectrometryPublished by Taylor & Francis Ltd ,2005
- Velocity distribution functions and transport coefficients of atomic ions in atomic gases by a Gram—Charlier approachChemical Physics, 1994
- Transport Properties of Ions in GasesPublished by Wiley ,1988