Chemical Physics Theory Group, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
Center for Nonlinear Phenomena and Complex Systems, Université Libre de Bruxelles (ULB), Code Postal 231, Campus Plaine, B-1050 Brussels, Belgium.
J Chem Phys. 2018 Jul 14;149(2):024904. doi: 10.1063/1.5029344.
Janus motors with chemically active and inactive hemispheres can operate only under nonequilibrium conditions where detailed balance is broken by fluxes of chemical species that establish a nonequilibrium state. A microscopic model for reversible reactive collisions on a Janus motor surface is constructed and shown to satisfy detailed balance. The model is used to study Janus particle reactive dynamics in systems at equilibrium where generalized chemical rate laws that include time-dependent rate coefficients with power-law behavior are shown to describe reaction rates. While maintaining reversible reactions on the Janus catalytic hemisphere, the system is then driven into a nonequilibrium steady state by fluxes of chemical species that control the chemical affinity. The statistical properties of the self-propelled Janus motor in this nonequilibrium steady state are investigated and compared with the predictions of a fluctuating thermodynamics theory. The model has utility beyond the examples presented here, since it allows one to explore various aspects of nonequilibrium fluctuations in systems with self-diffusiophoretic motors from a microscopic perspective.
具有化学活性和非活性半球的 Janus 马达只能在非平衡条件下运行，在这种条件下，化学物质的通量打破了详细平衡，从而建立了非平衡状态。构建了一个用于 Janus 马达表面可逆反应碰撞的微观模型，并证明其满足详细平衡。该模型用于研究平衡系统中 Janus 粒子的反应动力学，其中包括具有幂律行为的时变速率系数的广义化学速率定律，用于描述反应速率。在保持 Janus 催化半球上的可逆反应的同时，通过控制化学亲和力的化学物质通量将系统驱动到非平衡稳态。研究了这个非平衡稳态中自推进 Janus 马达的统计特性，并与涨落热力学理论的预测进行了比较。该模型具有超出本文所提出的示例的用途，因为它允许从微观角度探索具有自扩散马达的系统中非平衡涨落的各个方面。
