Institut für Reine und Angewandte Chemie, Carl von Ossietzky Universität Oldenburg, Postfach 2503, D-26111 Oldenburg, Germany.
J Chem Phys. 2012 Mar 28;136(12):124118. doi: 10.1063/1.3698289.
In this paper, control of open quantum systems with emphasis on the control of surface photochemical reactions is presented. A quantum system in a condensed phase undergoes strong dissipative processes. From a theoretical viewpoint, it is important to model such processes in a rigorous way. In this work, the description of open quantum systems is realized within the surrogate hamiltonian approach [R. Baer and R. Kosloff, J. Chem. Phys. 106, 8862 (1997)]. An efficient and accurate method to find control fields is optimal control theory (OCT) [W. Zhu, J. Botina, and H. Rabitz, J. Chem. Phys. 108, 1953 (1998); Y. Ohtsuki, G. Turinici, and H. Rabitz, J. Chem. Phys. 120, 5509 (2004)]. To gain control of open quantum systems, the surrogate hamiltonian approach and OCT, with time-dependent targets, are combined. Three open quantum systems are investigated by the combined method, a harmonic oscillator immersed in an ohmic bath, CO adsorbed on a platinum surface, and NO adsorbed on a nickel oxide surface. Throughout this paper, atomic units, i.e., ℏ = m(e) = e = a(0) = 1, have been used unless otherwise stated.
本文主要介绍了开放量子系统的控制，特别是表面光化学反应的控制。凝聚相中的量子系统会经历强烈的耗散过程。从理论角度来看，以严格的方式对这些过程进行建模非常重要。在这项工作中，开放量子系统的描述是通过替代哈密顿方法[R. Baer 和 R. Kosloff, J. Chem. Phys. 106, 8862 (1997)]来实现的。寻找控制场的一种有效且精确的方法是最优控制理论（OCT）[W. Zhu, J. Botina 和 H. Rabitz, J. Chem. Phys. 108, 1953 (1998); Y. Ohtsuki, G. Turinici 和 H. Rabitz, J. Chem. Phys. 120, 5509 (2004)]。为了对开放量子系统进行控制，我们将替代哈密顿方法和 OCT 与时间相关的目标相结合。通过组合方法研究了三个开放量子系统，分别是浸入欧姆浴中的谐振子、CO 吸附在铂表面上和 NO 吸附在氧化镍表面上。在本文中，除非另有说明，否则使用的单位均为原子单位，即 ℏ = m(e) = e = a(0) = 1。
