Dynamics between reactants and products are often mediated by a rate-determining barrier and an associated dividing surface leading to the transition state theory rate. This framework is challenged when the barrier is time-dependent because its motion can give rise to recrossings across the fixed dividing surface. A non-recrossing time-dependent dividing surface can nevertheless be attached to the TS trajectory resulting in recrossing-free dynamics. We extend the formalism—constructed using Lagrangian Descriptors—to systems with additional bath degrees of freedom. The propagation of reactant ensembles provides a numerical demonstration that our dividing surface is recrossing-free and leads to exact TST rates.
Description
Obtaining time-dependent multi-dimensional dividing surfaces using Lagrangian descriptors - ScienceDirect
%0 Journal Article
%1 FELDMAIER2017194
%A Feldmaier, Matthias
%A Junginger, Andrej
%A Main, Jörg
%A Wunner, Günter
%A Hernandez, Rigoberto
%D 2017
%J Chemical Physics Letters
%K main_itp1
%P 194 - 199
%R https://doi.org/10.1016/j.cplett.2017.09.008
%T Obtaining time-dependent multi-dimensional dividing surfaces using Lagrangian descriptors
%U http://www.sciencedirect.com/science/article/pii/S0009261417308412
%V 687
%X Dynamics between reactants and products are often mediated by a rate-determining barrier and an associated dividing surface leading to the transition state theory rate. This framework is challenged when the barrier is time-dependent because its motion can give rise to recrossings across the fixed dividing surface. A non-recrossing time-dependent dividing surface can nevertheless be attached to the TS trajectory resulting in recrossing-free dynamics. We extend the formalism—constructed using Lagrangian Descriptors—to systems with additional bath degrees of freedom. The propagation of reactant ensembles provides a numerical demonstration that our dividing surface is recrossing-free and leads to exact TST rates.
@article{FELDMAIER2017194,
abstract = {Dynamics between reactants and products are often mediated by a rate-determining barrier and an associated dividing surface leading to the transition state theory rate. This framework is challenged when the barrier is time-dependent because its motion can give rise to recrossings across the fixed dividing surface. A non-recrossing time-dependent dividing surface can nevertheless be attached to the TS trajectory resulting in recrossing-free dynamics. We extend the formalism—constructed using Lagrangian Descriptors—to systems with additional bath degrees of freedom. The propagation of reactant ensembles provides a numerical demonstration that our dividing surface is recrossing-free and leads to exact TST rates.},
added-at = {2018-12-04T23:32:40.000+0100},
author = {Feldmaier, Matthias and Junginger, Andrej and Main, Jörg and Wunner, Günter and Hernandez, Rigoberto},
biburl = {https://puma.ub.uni-stuttgart.de/bibtex/2d27ac9deddbc822e462b9c75b2dd4337/rbardak},
description = {Obtaining time-dependent multi-dimensional dividing surfaces using Lagrangian descriptors - ScienceDirect},
doi = {https://doi.org/10.1016/j.cplett.2017.09.008},
interhash = {4369748260c720984f860419d9d04135},
intrahash = {d27ac9deddbc822e462b9c75b2dd4337},
issn = {0009-2614},
journal = {Chemical Physics Letters},
keywords = {main_itp1},
pages = {194 - 199},
timestamp = {2018-12-04T22:32:40.000+0100},
title = {Obtaining time-dependent multi-dimensional dividing surfaces using Lagrangian descriptors},
url = {http://www.sciencedirect.com/science/article/pii/S0009261417308412},
volume = 687,
year = 2017
}
