Random Walks on Lattices. Influence of Competing Reaction Centers on Diffusion-Controlled Processes

TL;DR

This paper investigates how competing reaction centers influence diffusion-controlled reactions on lattices, analyzing mean walklengths and reaction efficiencies in different dimensions and scenarios using theoretical and simulation methods.

Contribution

It introduces a comprehensive model for diffusion-reaction processes with competing reactions, including finite size corrections and the two-walker problem, expanding understanding of reaction efficiencies.

Findings

Mean walklength is smaller in 3D than 2D for similar lattice sizes.

Increasing trapping probability s reduces differences between 2D and 3D systems.

Reaction efficiency increases with higher trapping probability s.

Abstract

We study diffusion-reaction processes on periodic square planar lattices and simple cubic (sc) lattices. Considered first is a single diffusing reactant undergoing an irreversible reaction upon first encounter with a stationary co-reactant ["one-walker (1W) problem"]. We then generalize this scenario to allow for a competing reaction, i.e., instantaneous trapping of the diffusing reactant with probability $s$ at any vacant site before interacting with a (stationary) co-reactant at a target site. We determine the mean walklength of the diffusing reactant until irreversible reaction occurs. We use generating functions and the theory of finite Markov processes, as well as MC simulations. To investigate the dependence of walklength on lattice size we compute the first, finite size corrections to the Green function of the sc lattice, and provide a Pad\'e approximation for this quantity. Finally, we consider the case where both reactant and co-reactant undergo synchronous nearest-neighbor displacements ["two-walker (2W) problem"]. In this case, reactant and co-reactant can individually be trapped with probability $s$ at any vacant lattice site, or can undergo an irreversible reaction on first encounter at any site. When $s=0$ we find that, both for the 1W and the 2W problem, for lattices with (approximately) the same number of sites, the mean walklength is smaller (and hence the reaction efficiency greater) in $d=3$ than in $d=2$. Increasing $s$ tends to reduce differences in system dimensionality, and distinctions between the 1W problem and the 2W problem. Our model provides a good starting point to develop studies on the efficiency of apparently diverse diffusion-reaction processes, such as diffusion on a partially poisoned catalytic substrate or photosynthetic trapping of excitations.