Two-Dimensional Terahertz Spectroscopy of Condensed-Phase Molecular Systems

Abstract

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 frequency 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.

14 pages, 8 figures

References in corpus (6)

• High Kerr nonlinearity of water in THz spectral range
• Analysis of 2D THz-Raman spectroscopy using a non-Markovian Brownian oscillator model with nonlinear system-bath interactions
• 2D THz spectroscopic investigation of ballistic conduction-band electron dynamics in InSb
• Field-Induced Tunneling Ionization and Terahertz-Driven Electron Dynamics in Liquid Water
• The sign of the polarizability anisotropy of polar molecules is obtained faithfully from terahertz Kerr effect
• Feynman Diagram Description of 2D-Raman-THz Spectroscopy Applied to Water

Cited by in corpus (2)

• Field-Induced Electron Generation in Water: Solvation Dynamics and Many-Body Interactions
• Solvated electrons in polar liquids as epsilon-near-zero materials tunable in the terahertz frequency range