Wörner Hans Jakob, Arrell Christopher A, Banerji Natalie, Cannizzo Andrea, Chergui Majed, Das Akshaya K, Hamm Peter, Keller Ursula, Kraus Peter M, Liberatore Elisa, Lopez-Tarifa Pablo, Lucchini Matteo, Meuwly Markus, Milne Chris, Moser Jacques-E, Rothlisberger Ursula, Smolentsev Grigory, Teuscher Joël, van Bokhoven Jeroen A, Wenger Oliver
Laboratory of Physical Chemistry, ETH Zürich, Zürich, Switzerland.
Laboratory of Ultrafast Spectroscopy and Lausanne Centre for Ultrafast Science (LACUS), École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland.
Struct Dyn. 2017 Dec 27;4(6):061508. doi: 10.1063/1.4996505. eCollection 2017 Nov.
The transfer of charge at the molecular level plays a fundamental role in many areas of chemistry, physics, biology and materials science. Today, more than 60 years after the seminal work of R. A. Marcus, charge transfer is still a very active field of research. An important recent impetus comes from the ability to resolve ever faster temporal events, down to the attosecond time scale. Such a high temporal resolution now offers the possibility to unravel the most elementary quantum dynamics of both electrons and nuclei that participate in the complex process of charge transfer. This review covers recent research that addresses the following questions. Can we reconstruct the migration of charge across a molecule on the atomic length and electronic time scales? Can we use strong laser fields to control charge migration? Can we temporally resolve and understand intramolecular charge transfer in dissociative ionization of small molecules, in transition-metal complexes and in conjugated polymers? Can we tailor molecular systems towards specific charge-transfer processes? What are the time scales of the elementary steps of charge transfer in liquids and nanoparticles? Important new insights into each of these topics, obtained from state-of-the-art ultrafast spectroscopy and/or theoretical methods, are summarized in this review.
电荷在分子层面的转移在化学、物理、生物学和材料科学的诸多领域都起着基础性作用。如今，在R. A. 马库斯的开创性工作过去60多年后，电荷转移仍是一个非常活跃的研究领域。近期一个重要的推动力来自于能够解析越来越快的时间事件，直至阿秒时间尺度。如此高的时间分辨率现在为揭示参与电荷转移复杂过程的电子和原子核的最基本量子动力学提供了可能。本综述涵盖了近期针对以下问题的研究。我们能否在原子长度和电子时间尺度上重构电荷在分子中的迁移？我们能否利用强激光场来控制电荷迁移？我们能否在时间上分辨并理解小分子、过渡金属配合物和共轭聚合物的解离电离中的分子内电荷转移？我们能否针对特定的电荷转移过程来设计分子系统？液体和纳米颗粒中电荷转移基本步骤的时间尺度是多少？本综述总结了从最新的超快光谱学和/或理论方法中获得的关于上述每个主题的重要新见解。
