English

An alternative derivation of ring-polymer molecular dynamics transition-state theory

Chemical Physics 2016-05-06 v2 Quantum Physics

Abstract

In a previous article [J. Chem. Phys. 138, 084108 (2013)], we showed that the t0+t\to 0_+ limit of ring-polymer molecular dynamics (RPMD) rate-theory is also the t0+t\to 0_+ limit of a new type of quantum flux-side time-correlation function, in which the dividing surfaces are invariant to imaginary-time translation; in other words, that RPMD transition-state theory (RPMD-TST) is a t0+t\to 0_+ quantum transition-state theory (QTST). Recently, Jang and Voth [J. Chem. Phys. 144, 084110 (2016)] rederived this quantum t0+t\to 0_+ limit, and claimed that it gives instead the centroid-density approximation. Here we show that the t0+t\to 0_+ limit derived by Jang and Voth is in fact RPMD-TST.

Cite

@article{arxiv.1603.07966,
  title  = {An alternative derivation of ring-polymer molecular dynamics transition-state theory},
  author = {Timothy J. H. Hele and Stuart C. Althorpe},
  journal= {arXiv preprint arXiv:1603.07966},
  year   = {2016}
}