Communication: A full solution of the annihilation reaction A B → based on time-subordination

David A. Benson*, Diogo Bolster, Amir Paster

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

The connection between the governing equations of chemical reaction and the underlying stochastic processes of particle collision and transformation have been developed previously along two end-member conditions: perfectly mixed and maximally diffusion-limited. The complete governing equation recognizes that in the perfectly mixed case, the particle (i.e., molecular or macro-particle) number state evolution is Markovian, but that spatial self-organization of reactants decreases the probability of reactant pairs finding themselves co-located. This decreased probability manifests itself as a subordination of the clock time: as reactant concentrations become spatially variable (unmixed), the time required for reactants to find each other increases and the random operational time that particles spend in the active reaction process is less than the clock time. For example, in the system A + B → ø, a simple approximate calculation for the return time of a Brownian motion to a moving boundary allows a calculation of the operational time density, and the total solution is a subordination integral of the perfectly-mixed solution with a modified inverse Gaussian subordinator. The system transitions from the well-mixed solution to the asymptotic diffusion-limited solution that decays as t-d4 in d-dimensions.

Original languageEnglish
Article number131101
JournalJournal of Chemical Physics
Volume138
Issue number13
DOIs
StatePublished - 7 Apr 2013
Externally publishedYes

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