Stochastic wave packet approach to nonadiabatic scattering of diatomic molecules from metals.
Stochastic wave packet approach to nonadiabatic scattering of diatomic molecules from metals.
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DOI：
10.1063/1.5092698
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发表时间：
2019-05
期刊：
影响因子：
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通讯作者：
T. Serwatka;J. Tremblay
中科院分区：
文献类型：
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作者：
T. Serwatka;J. Tremblay
在这篇文章中，我们提出了一个量子动力学方法来研究垂直入射下双原子分子从金属表面的非弹性散射。耗散动力学服从随机薛定谔方程，该方程将系统的时间演化描述为分段确定性过程。分子的振动自由度和金属电子之间的能量交换表示使用运营商在张量积的形式，这是耦合通过从一阶微扰理论计算的非谐跃迁率。全维观测值是通过平均超过模拟在4D中，包括内部拉伸，到表面的距离，和方向角，在不同的表面网站。应用该方法研究了NO在Au（111）表面的振动激发态散射，揭示了NO量子化能量弛豫的重要通道。
In this contribution, we present a quantum dynamical approach to study inelastic scattering of diatomic molecules from metal surfaces at normal incidence. The dissipative dynamics obeys a stochastic Schrödinger equation describing the time-evolution of the system as a piecewise deterministic process. Energy exchange between the molecular vibrational degrees of freedom and the metal electrons is represented using operators in tensor product form, which are coupled via anharmonic transition rates calculated from first-order perturbation theory. Full dimensional observables are obtained by averaging over simulations in 4D-including the internal stretch, the distance to the surface, and the orientation angles-at different surface sites. The method is applied to the state-resolved scattering of vibrationally excited NO from Au(111), revealing important channels for quantized energy relaxation.