Two-dimensional terahertz spectroscopy of condensed-phase molecular systems.
Two-dimensional terahertz spectroscopy of condensed-phase molecular systems.
复制标题
DOI：
10.1063/5.0046664
复制
发表时间：
2021-03
期刊：
影响因子：
--
通讯作者：
K. Reimann;M. Woerner;T. Elsaesser
中科院分区：
文献类型：
--
作者：
K. Reimann;M. Woerner;T. Elsaesser
非线性太赫兹(THz)光谱学依赖于物质与电场幅度高达兆伏特/厘米(mV/cm)的短周期太赫兹脉冲的相互作用。在凝聚相分子系统中，与分子内和分子间振动等低频基元激发的共振相互作用和非共振场驱动过程都是相关的。二维太赫兹(2D-THz)光谱是跟踪非平衡过程和激发动力学来解释潜在相互作用和分子耦合的关键方法。本文讨论了2D-THz光谱学的主要概念，并用最新的结果说明了它们的发展现状。后者包括分子晶体中振动激发的响应，直至光-物质相互作用和场驱动电离过程的非微扰区域，以及液态水中的电子传输。
Nonlinear terahertz (THz) spectroscopy relies on the interaction of matter with few-cycle THz pulses of electric field amplitudes up to megavolts/centimeter (MV/cm). In condensed-phase molecular systems, both resonant interactions with elementary excitations at low frequencies such as intra- and intermolecular vibrations and nonresonant field-driven processes are relevant. Two-dimensional THz (2D-THz) spectroscopy is a key method for following nonequilibrium processes and dynamics of excitations to decipher the underlying interactions and molecular couplings. This article addresses the state of the art in 2D-THz spectroscopy by discussing the main concepts and illustrating them with recent results. The latter include the response of vibrational excitations in molecular crystals up to the nonperturbative regime of light-matter interaction and field-driven ionization processes and electron transport in liquid water.