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凝聚相中分子动力学的飞秒量子控制

Femtosecond quantum control of molecular dynamics in the condensed phase.

作者信息

Nuernberger Patrick, Vogt Gerhard, Brixner Tobias, Gerber Gustav

机构信息

Universität Würzburg, Physikalisches Institut, Am Hubland, 97074 Würzburg, Germany.

出版信息

Phys Chem Chem Phys. 2007 May 28;9(20):2470-97. doi: 10.1039/b618760a. Epub 2007 Mar 13.

Abstract

We review the progress in controlling quantum dynamical processes in the condensed phase with femtosecond laser pulses. Due to its high particle density the condensed phase has both high relevance and appeal for chemical synthesis. Thus, in recent years different methods have been developed to manipulate the dynamics of condensed-phase systems by changing one or multiple laser pulse parameters. Single-parameter control is often achieved by variation of the excitation pulse's wavelength, its linear chirp or its temporal subpulse separation in case of pulse sequences. Multiparameter control schemes are more flexible and provide a much larger parameter space for an optimal solution. This is realized in adaptive femtosecond quantum control, in which the optimal solution is iteratively obtained through the combination of an experimental feedback signal and an automated learning algorithm. Several experiments are presented that illustrate the different control concepts and highlight their broad applicability. These fascinating achievements show the continuous progress on the way towards the control of complex quantum reactions in the condensed phase.

摘要

我们回顾了利用飞秒激光脉冲控制凝聚相量子动力学过程的进展。由于凝聚相具有高粒子密度,因此对于化学合成具有高度相关性和吸引力。因此,近年来已开发出不同方法,通过改变一个或多个激光脉冲参数来操纵凝聚相系统的动力学。单参数控制通常通过改变激发脉冲的波长、线性啁啾或在脉冲序列情况下改变其时间子脉冲间隔来实现。多参数控制方案更灵活,为最优解提供了大得多的参数空间。这在自适应飞秒量子控制中得以实现,其中通过实验反馈信号和自动学习算法的结合迭代获得最优解。文中给出了几个实验,这些实验说明了不同的控制概念,并突出了它们的广泛适用性。这些引人入胜的成果展示了在控制凝聚相中复杂量子反应的道路上取得的持续进展。

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