Journal article


An analysis of nonadiabatic ring-polymer molecular dynamics and its application to vibronic spectra


Publication Details
Author(s): Richardson J, Meyer P, Pleinert MO, Thoss M
Publisher: ELSEVIER SCIENCE BV
Publication year: 2017
Volume: 482
Pages range: 124-134
ISSN: 0301-0104

Abstract

Nonadiabatic ring-polymer molecular dynamics employs the mapping approach to describe nonadiabatic effects within the ring-polymer ansatz. In this paper, it is generalized to allow for the nuclear and electronic degrees of freedom to be described by different numbers of ring-polymer beads. Analysis of the resulting method shows that as the number of electronic mapping variables increases, certain problems associated with the approach are removed, such as the non-unique choice of the mapping Hamiltonian and negative populations leading to inverted potential-energy surfaces. Explicit integration over cyclic variables reduces the sign problem for the initial distribution in the general case. A new application for the simulation of vibronic spectra is described and promising results are presented for a model system. (C) 2016 Elsevier B.V. All rights reserved.



How to cite
APA: Richardson, J., Meyer, P., Pleinert, M.-O., & Thoss, M. (2017). An analysis of nonadiabatic ring-polymer molecular dynamics and its application to vibronic spectra. Chemical Physics, 482, 124-134. https://dx.doi.org/10.1016/j.chemphys.2016.09.036

MLA: Richardson, Jeremy, et al. "An analysis of nonadiabatic ring-polymer molecular dynamics and its application to vibronic spectra." Chemical Physics 482 (2017): 124-134.

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