Concentration fluctuations in nonisothermal reaction-diffusion systems

J Chem Phys. 2007 Jul 21;127(3):034501. doi: 10.1063/1.2746326.

Abstract

In this paper a simple reaction-diffusion system, namely a binary fluid mixture with an association-dissociation reaction between the two components, is considered. Fluctuations at hydrodynamic spatiotemporal scales when a temperature gradient is present in this chemically reacting system are studied. First, fluctuating hydrodynamics when the system is in global equilibrium (isothermal) is reviewed. Comparing the two cases, an enhancement of the intensity of concentration fluctuations in the presence of a temperature gradient is predicted. The nonequilibrium concentration fluctuations are spatially long ranged, with an intensity depending on the wave number q. The intensity exhibits a crossover from a proportional, variantq(-4) to a proportional, variantq(-2) behavior depending on whether the corresponding wavelength is smaller or larger than the penetration depth of the reacting mixture. This opens a possibility to distinguish between diffusion- or activation-controlled regimes of the reaction by measuring these fluctuations. In addition, the possible observation of these fluctuations in nonequilibrium molecular dynamics simulations is considered.