Gated reactions in discrete time and space

Yuval Scher, Shlomi Reuveni

Research output: Contribution to journalArticlepeer-review

Abstract

How much time does it take for two molecules to react? If a reaction occurs upon contact, the answer to this question boils down to the classic first-passage time problem: find the time it takes for the two molecules to meet. However, this is not always the case as molecules switch stochastically between reactive and non-reactive states. The reaction is then said to be "gated"by the internal states of the molecules involved, which could have a dramatic influence on kinetics. A unified, continuous-time, approach to gated reactions on networks was presented in a recent paper [Scher and Reuveni, Phys. Rev. Lett. 127, 018301 (2021)]. Here, we build on this recent advancement and develop an analogous discrete-time version of the theory. Similar to continuous-time, we employ a renewal approach to show that the gated reaction time can always be expressed in terms of the corresponding ungated first-passage and return times, which yields formulas for the generating function of the gated reaction-time distribution and its corresponding mean and variance. In cases where the mean reaction time diverges, we show that the long-time asymptotics of the gated problem is inherited from its ungated counterpart. However, when molecules spend most of their time non-reactive, an interim regime of slower power-law decay emerges prior to the terminal asymptotics. The discretization of time also gives rise to resonances and anti-resonances, which were absent from the continuous-time picture. These features are illustrated using two case studies that also demonstrate how the general approach presented herein greatly simplifies the analysis of gated reactions.

Original languageEnglish
Article number234112
JournalJournal of Chemical Physics
Volume155
Issue number23
DOIs
StatePublished - 21 Dec 2021

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