Dietze Daniel R, Mathies Richard A
Department of Chemistry, University of California in Berkeley, CA, Berkeley, 94720, USA.
Chemphyschem. 2016 May 4;17(9):1224-51. doi: 10.1002/cphc.201600104. Epub 2016 Mar 18.
Femtosecond stimulated Raman spectroscopy (FSRS) is an ultrafast nonlinear optical technique that provides vibrational structural information with high temporal (sub-50 fs) precision and high spectral (10 cm(-1) ) resolution. Since the first full demonstration of its capabilities ≈15 years ago, FSRS has evolved into a mature technique, giving deep insights into chemical and biochemical reaction dynamics that would be inaccessible with any other technique. It is now being routinely applied to virtually all possible photochemical reactions and systems spanning from single molecules in solution to thin films, bulk crystals and macromolecular proteins. This review starts with an historic overview and discusses the theoretical and experimental concepts behind this technology. Emphasis is put on the current state-of-the-art experimental realization and several variations of FSRS that have been developed. The unique capabilities of FSRS are illustrated through a comprehensive presentation of experiments to date followed by prospects.
飞秒受激拉曼光谱（FSRS）是一种超快非线性光学技术，它能以高时间精度（低于50飞秒）和高光谱分辨率（10厘米⁻¹）提供振动结构信息。自约15年前首次全面展示其功能以来，FSRS已发展成为一项成熟的技术，能深入洞察化学和生化反应动力学，而这是其他任何技术都无法实现的。目前，它已被常规应用于几乎所有可能的光化学反应和体系，涵盖从溶液中的单分子到薄膜、块状晶体和大分子蛋白质等。本文综述首先进行历史概述，然后讨论该技术背后的理论和实验概念。重点介绍了当前最先进的实验实现方式以及已开发的FSRS的几种变体。通过全面展示迄今为止的实验及其前景，阐述了FSRS的独特功能。
