QM/MM studies of gas-liquid collisional energy transfer

Xiaohu Li, George C Schatz

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Abstract

In this manuscript we describe a molecular dynamics method that has recently been developed to model collisional energy transfer in collisions of hyperthermal gas-phase molecules with ionic liquid surfaces. This method is based on a quantum mechanics/molecular mechanics (QM/MM) partitioning in which electronic structure methods are used to determine forces for the hyperthermal gaseous molecule and molecules in the liquid which it directly interacts with during the first 10 ps of the collision process, while empirical potentials are used for atoms in the liquid that are not directly involved in interacting with the gaseous molecule. Collisions of the gaseous molecule with the liquid surface are simulated using molecular dynamics methods, and from this it is possible to determine energy transfer associated with the gas-surface collision, including scattering of the molecule from the liquid that leads to energy and momentum transfer, and trapping of the gas molecule in the liquid. We illustrate this approach with an application to the collision of hyperthermal CO2 with two ionic liquid surfaces: [bmim][BF4] and [bmim][Tf2N]. The results are used to model recent experimental studies, and our analysis includes an examination of rotational and angular distributions associated with the CO2 scattering, and the translational diffusion and vibrational relaxation of the trapped CO2.

Original languageEnglish
Title of host publicationTheory and Applications in Computational Chemistry
Subtitle of host publicationThe First Decade of the Second Millennium, International Congress TACC-2012
PublisherAmerican Institute of Physics Inc.
Pages131-138
Number of pages8
Volume1456
ISBN (Electronic)9780735410572
DOIs
Publication statusPublished - 2012
EventInternational Congress in Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, TACC 2012 - Pavia, Italy
Duration: Sep 2 2012Sep 7 2012

Other

OtherInternational Congress in Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, TACC 2012
CountryItaly
CityPavia
Period9/2/129/7/12

Fingerprint

quantum mechanics
energy transfer
liquids
gases
liquid surfaces
molecules
collisions
molecular dynamics
molecular relaxation
scattering
momentum transfer
angular distribution
examination
trapping
vapor phases
electronic structure
atoms

Keywords

  • collisional energy transfer
  • diffusion
  • energy transfer
  • hyperthermal
  • Ionic liquid
  • molecular dynamics
  • QM/MM

ASJC Scopus subject areas

  • Physics and Astronomy(all)

Cite this

Li, X., & Schatz, G. C. (2012). QM/MM studies of gas-liquid collisional energy transfer. In Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, International Congress TACC-2012 (Vol. 1456, pp. 131-138). American Institute of Physics Inc.. https://doi.org/10.1063/1.4730652

QM/MM studies of gas-liquid collisional energy transfer. / Li, Xiaohu; Schatz, George C.

Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, International Congress TACC-2012. Vol. 1456 American Institute of Physics Inc., 2012. p. 131-138.

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Li, X & Schatz, GC 2012, QM/MM studies of gas-liquid collisional energy transfer. in Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, International Congress TACC-2012. vol. 1456, American Institute of Physics Inc., pp. 131-138, International Congress in Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, TACC 2012, Pavia, Italy, 9/2/12. https://doi.org/10.1063/1.4730652
Li X, Schatz GC. QM/MM studies of gas-liquid collisional energy transfer. In Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, International Congress TACC-2012. Vol. 1456. American Institute of Physics Inc. 2012. p. 131-138 https://doi.org/10.1063/1.4730652
Li, Xiaohu ; Schatz, George C. / QM/MM studies of gas-liquid collisional energy transfer. Theory and Applications in Computational Chemistry: The First Decade of the Second Millennium, International Congress TACC-2012. Vol. 1456 American Institute of Physics Inc., 2012. pp. 131-138
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