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

Journal article


Publication Details

Author(s): Richardson J, Meyer P, Pleinert MO, Thoss M
Journal: Chemical Physics
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.



FAU Authors / FAU Editors

Pleinert, Marc-Oliver
Professur für Experimentalphysik
Richardson, Jeremy Dr.
Professur für Theoretische Physik mit dem Schwerpunkt Elektronentransport in Molekülen
Thoss, Michael Prof. Dr.
Professur für Theoretische Physik mit dem Schwerpunkt Elektronentransport in Molekülen


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.

BibTeX: 

Last updated on 2018-19-04 at 04:16