Department of Physics and Astronomy, Hunter College of the City University of New York, 695 Park Avenue, New York, New York 10065, USA.
Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science and Department of Physics, Luruper Chaussee 149, 22761 Hamburg, Germany.
Phys Rev Lett. 2019 Aug 23;123(8):083201. doi: 10.1103/PhysRevLett.123.083201.
We find and analyze the exact time-dependent potential energy surface driving the proton motion for a model of cavity-induced suppression of proton-coupled electron transfer. We show how, in contrast to the polaritonic surfaces, its features directly correlate to the proton dynamics and we discuss cavity modifications of its structure responsible for the suppression. The results highlight the interplay between nonadiabatic effects from coupling to photons and coupling to electrons and suggest caution is needed when applying traditional dynamics methods based on polaritonic surfaces.
我们找到了并分析了一个模型中驱动质子运动的确切的时变势能表面，该模型为空腔诱导质子耦合电子转移抑制。我们展示了与极化子表面相反，其特征如何直接与质子动力学相关联，并讨论了空腔对其结构的修饰如何导致抑制。结果突出了与耦合到光子和电子的非绝热效应之间的相互作用，并建议在应用基于极化子表面的传统动力学方法时需要谨慎。
