Theory of reversible diffusion-influenced reactions with non-Markovian dissociation in two space dimensions

摘要

We investigate the reversible diffusion-influenced reaction of an isolated pair in the presence of a non-Markovian generalization of the backreaction boundary condition in two space dimensions. Following earlier work by Agmon and Weiss, we consider residence time probability densities that decay slower than an exponential and that are characterized by a single parameter 0 < σ ⩽ 1. We calculate an exact expression for a Green's function of the two-dimensional diffusion equation subject to a non-Markovian backreaction boundary condition that is valid for arbitrary σ and for all times. We use the obtained expression to derive the survival probability for the initially unbound pair and we calculate an exact expression for the probability S(t|*) that the initially bound particle is unbound. Finally, we obtain an approximate solution for long times. In particular, we show that the ultimate fate of the bound state is complete dissociation, as in the Markovian case. However, the limiting value is approached quite differently: Instead of a ∼t⁻¹ decay, we obtain 1 − S(t|*) ∼ t^−σln t. The derived expressions should be relevant for a better understanding of reversible membrane-bound reactions in cell biology.