Nonlinear absorption dynamics using field-induced surface hopping: zinc porphyrin in water.
Nonlinear absorption dynamics using field-induced surface hopping: zinc porphyrin in water.
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使用场诱导表面跳跃的非线性吸收动力学：水中的锌卟啉
DOI：
10.1002/cphc.201300053
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发表时间：
2013
期刊：
影响因子：
--
通讯作者：
R. Mitrić
中科院分区：
文献类型：
--
作者：
M.I.S. Röhr;J. Petersen;M. Wohlgemuth;V. Bonačić-Koutecký;R. Mitrić
我们希望用我们的场诱导表面跳跃(FISH)方法来模拟强非共振激光诱导的非线性吸收动力学。我们在多态模型系统上对FISH方法和精确的量子动力学模拟进行了系统的比较，并证明FISH方法可以精确地模拟包括多光子电子跃迁在内的非线性激发过程。特别是对模拟双光子跃迁的两种不同方法进行了比较。第一种方法本质上是精确的，涉及到在扩展的激发态流形中求解含时薛定谔方程，而在第二种方法中，只有瞬时填充的非本质态被有效的二次耦合项取代，并且动力学在相当小的态流形中进行。我们通过模拟锌(锌)卟啉在气相和水中的线性和非线性激光驱动动力学，说明我们的方法对复杂分子系统的适用性。为此，FISH方法与量子力学-分子力学方法(QM/MM)相结合，后者通常适用于大类复杂系统。我们的发现是，多光子吸收和动力学增加了锌卟啉在非线性区域，特别是在溶液中的高激发态布居，这为操纵激发态性质，如瞬时吸收动力学和电子弛豫提供了一种手段。
We wish to present the application of our field‐induced surface‐hopping (FISH) method to simulate nonlinear absorption dynamics induced by strong nonresonant laser fields. We provide a systematic comparison of the FISH approach with exact quantum dynamics simulations on a multistate model system and demonstrate that FISH allows for accurate simulations of nonlinear excitation processes including multiphoton electronic transitions. In particular, two different approaches for simulating two‐photon transitions are compared. The first approach is essentially exact and involves the solution of the time‐dependent Schrödinger equation in an extended manifold of excited states, while in the second one only transiently populated nonessential states are replaced by an effective quadratic coupling term, and dynamics is performed in a considerably smaller manifold of states. We illustrate the applicability of our method to complex molecular systems by simulating the linear and nonlinear laser‐driven dynamics in zinc (Zn) porphyrin in the gas phase and in water. For this purpose, the FISH approach is connected with the quantum mechanical‐molecular mechanical approach (QM/MM) which is generally applicable to large classes of complex systems. Our findings that multiphoton absorption and dynamics increase the population of higher excited states of Zn porphyrin in the nonlinear regime, in particular in solution, provides a means for manipulating excited‐state properties, such as transient absorption dynamics and electronic relaxation.
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