Santamaría-Holek I, Pérez-Madrid A
UMDI-J, Facultad de Ciencias, Universidad Nacional Autónoma de México, Campus Juriquilla, 76230 Querétaro, Mexico.
Departament de Física de la Matèria Condensada, Universitat de Barcelona, 08028 Barcelona, Spain.
J Chem Phys. 2020 Dec 28;153(24):244116. doi: 10.1063/5.0032634.
Understanding and managing the influence that either external forces or non-equilibrated environments may have on chemical processes is essential for the current and future development of theoretical chemistry. One of the central questions to solve is how to generalize the transition state theory in order to make it applicable in far from equilibrium situations. In this sense, here we propose a way to generalize Eyring's equation based on the definition of an effective thermal energy (temperature) emerging from the coupling of both fast and slow dynamic variables analyzed within the generalized Langevin dynamics scheme. This coupling makes the energy distribution of the fast degrees of freedom not equilibrate because they have been enslaved to the dynamics of the corresponding slow degrees. However, the introduction of the effective thermal energy enables us to restore an effective adiabatic separation of timescales leading to a renormalization of the generalized fluctuation-dissipation theorem. Hence, this procedure opens the possibility to deal with systems far away from equilibrium. A significant consequence of our results is that Eyring's equation is generalized to treat systems under the influence of strong external forces.
理解并掌控外力或非平衡环境对化学过程可能产生的影响,对于理论化学的当前及未来发展至关重要。有待解决的核心问题之一是如何推广过渡态理论,使其适用于远离平衡的情形。从这个意义上讲,在此我们基于广义朗之万动力学方案中对快速和慢速动力学变量耦合所产生的有效热能(温度)的定义,提出一种推广艾林方程的方法。这种耦合使得快速自由度的能量分布无法达到平衡,因为它们受限于相应慢速自由度的动力学。然而,有效热能的引入使我们能够恢复有效的绝热时间尺度分离,从而实现广义涨落耗散定理的重整化。因此,该方法为处理远离平衡态的系统开辟了可能性。我们结果的一个重要推论是,艾林方程得到推广,可用于处理受强外力影响的系统。