Transition Path Theory (TPT) provides a rigorous framework to investigate the dynamics of rare thermally activated transitions. In this theory, a central role is played by the forward committor function q+(x), which provides the ideal reaction coordinate. Furthermore, the reactive dynamics and kinetics are fully characterized in terms of two time-independent scalar and vector distributions. In this work, we develop a scheme which enables all these ingredients of TPT to be efficiently computed using the short non-equilibrium trajectories generated by means of a specific combination of enhanced path sampling techniques. In particular, first we further extend the recently introduced self-consistent path sampling algorithm in order to compute the committor q+(x). Next, we show how this result can be exploited in order to define efficient algorithms which enable us to directly sample the transition path ensemble.

Bartolucci, G., Orioli, S., Faccioli, P. (2018). Transition path theory from biased simulations. THE JOURNAL OF CHEMICAL PHYSICS, 149(7) [10.1063/1.5027253].

Transition path theory from biased simulations

Faccioli, P.
2018

Abstract

Transition Path Theory (TPT) provides a rigorous framework to investigate the dynamics of rare thermally activated transitions. In this theory, a central role is played by the forward committor function q+(x), which provides the ideal reaction coordinate. Furthermore, the reactive dynamics and kinetics are fully characterized in terms of two time-independent scalar and vector distributions. In this work, we develop a scheme which enables all these ingredients of TPT to be efficiently computed using the short non-equilibrium trajectories generated by means of a specific combination of enhanced path sampling techniques. In particular, first we further extend the recently introduced self-consistent path sampling algorithm in order to compute the committor q+(x). Next, we show how this result can be exploited in order to define efficient algorithms which enable us to directly sample the transition path ensemble.
Articolo in rivista - Articolo scientifico
Physics and Astronomy (all); Physical and Theoretical Chemistry
English
2018
149
7
072336
none
Bartolucci, G., Orioli, S., Faccioli, P. (2018). Transition path theory from biased simulations. THE JOURNAL OF CHEMICAL PHYSICS, 149(7) [10.1063/1.5027253].
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/10281/405617
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