A molecular dynamics quantum Kramers study of proton transfer in solution

Dimitri Antoniou, Steven D Schwartz

Research output: Contribution to journalArticle

44 Citations (Scopus)

Abstract

We present a quantum study of a proton transfer reaction AH-B⇌A--H+B in liquid methyl chloride, where the AH-B complex corresponds to phenol-amine. We use the same intramolecular potentials that were used in two earlier studies of this system [H. Azzouzz and D. Borgis, J. Chem. Phys. 98, 7361 (1993); S. Hammes-Schiffer and J. C. Tully, J. Chem. Phys. 101, 4657 (1994).] The former study employed a Landau-Zener approach and a molecular dynamics centroid method, while the latter a surface-hopping method. These studies obtained results that differ by an order of magnitude. In the present work, we first performed a molecular dynamics simulation to obtain the spectral density, which was then used as an input to the method we have developed for the study of the quantum Kramers problem [S. D. Schwartz, J. Chem. Phys. 105, 6871 (1996)]. Thus, in this work both the reaction coordinate and the bath are treated quantum mechanically.

Original languageEnglish (US)
Pages (from-to)465-472
Number of pages8
JournalThe Journal of Chemical Physics
Volume110
Issue number1
DOIs
StatePublished - 1999
Externally publishedYes

Fingerprint

Proton transfer
Molecular dynamics
Methyl Chloride
molecular dynamics
methyl chloride
protons
Spectral density
Phenol
phenols
centroids
Amines
baths
amines
Hydrogen
Computer simulation
Liquids
liquids
simulation

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

A molecular dynamics quantum Kramers study of proton transfer in solution. / Antoniou, Dimitri; Schwartz, Steven D.

In: The Journal of Chemical Physics, Vol. 110, No. 1, 1999, p. 465-472.

Research output: Contribution to journalArticle

@article{c4b8bb0171d949f783294e755eecdf9a,
title = "A molecular dynamics quantum Kramers study of proton transfer in solution",
abstract = "We present a quantum study of a proton transfer reaction AH-B⇌A--H+B in liquid methyl chloride, where the AH-B complex corresponds to phenol-amine. We use the same intramolecular potentials that were used in two earlier studies of this system [H. Azzouzz and D. Borgis, J. Chem. Phys. 98, 7361 (1993); S. Hammes-Schiffer and J. C. Tully, J. Chem. Phys. 101, 4657 (1994).] The former study employed a Landau-Zener approach and a molecular dynamics centroid method, while the latter a surface-hopping method. These studies obtained results that differ by an order of magnitude. In the present work, we first performed a molecular dynamics simulation to obtain the spectral density, which was then used as an input to the method we have developed for the study of the quantum Kramers problem [S. D. Schwartz, J. Chem. Phys. 105, 6871 (1996)]. Thus, in this work both the reaction coordinate and the bath are treated quantum mechanically.",
author = "Dimitri Antoniou and Schwartz, {Steven D}",
year = "1999",
doi = "10.1063/1.478107",
language = "English (US)",
volume = "110",
pages = "465--472",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "1",

}

TY - JOUR

T1 - A molecular dynamics quantum Kramers study of proton transfer in solution

AU - Antoniou, Dimitri

AU - Schwartz, Steven D

PY - 1999

Y1 - 1999

N2 - We present a quantum study of a proton transfer reaction AH-B⇌A--H+B in liquid methyl chloride, where the AH-B complex corresponds to phenol-amine. We use the same intramolecular potentials that were used in two earlier studies of this system [H. Azzouzz and D. Borgis, J. Chem. Phys. 98, 7361 (1993); S. Hammes-Schiffer and J. C. Tully, J. Chem. Phys. 101, 4657 (1994).] The former study employed a Landau-Zener approach and a molecular dynamics centroid method, while the latter a surface-hopping method. These studies obtained results that differ by an order of magnitude. In the present work, we first performed a molecular dynamics simulation to obtain the spectral density, which was then used as an input to the method we have developed for the study of the quantum Kramers problem [S. D. Schwartz, J. Chem. Phys. 105, 6871 (1996)]. Thus, in this work both the reaction coordinate and the bath are treated quantum mechanically.

AB - We present a quantum study of a proton transfer reaction AH-B⇌A--H+B in liquid methyl chloride, where the AH-B complex corresponds to phenol-amine. We use the same intramolecular potentials that were used in two earlier studies of this system [H. Azzouzz and D. Borgis, J. Chem. Phys. 98, 7361 (1993); S. Hammes-Schiffer and J. C. Tully, J. Chem. Phys. 101, 4657 (1994).] The former study employed a Landau-Zener approach and a molecular dynamics centroid method, while the latter a surface-hopping method. These studies obtained results that differ by an order of magnitude. In the present work, we first performed a molecular dynamics simulation to obtain the spectral density, which was then used as an input to the method we have developed for the study of the quantum Kramers problem [S. D. Schwartz, J. Chem. Phys. 105, 6871 (1996)]. Thus, in this work both the reaction coordinate and the bath are treated quantum mechanically.

UR - http://www.scopus.com/inward/record.url?scp=0032615369&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0032615369&partnerID=8YFLogxK

U2 - 10.1063/1.478107

DO - 10.1063/1.478107

M3 - Article

VL - 110

SP - 465

EP - 472

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 1

ER -