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.

arXiv comment14 pages, 8 figures

References in corpus (11)

• Sub-cycle control of terahertz high-harmonic generation by dynamical Bloch oscillations
• Two-dimensional terahertz magnetic resonance spectroscopy of collective spin waves
• Electric field correlation measurements on the electromagnetic vacuum state
• 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
• Nonlinear TeraHertz Coherent Excitation of Vibrational Modes of Liquids
• Feynman Diagram Description of 2D-Raman-THz Spectroscopy Applied to Water
• The sign of the polarizability anisotropy of polar molecules is obtained faithfully from terahertz Kerr effect
• Dynamic Kerr effect responses in the Terahertz-range

Cited by in corpus (11)

• Two-dimensional THz spectroscopy of nonlinear phononics in the topological insulator ${\mathrm{MnBi}}_2{\mathrm{Te}}_4$
• Enantiodetection of chiral molecules via two-dimensional spectroscopy
• A many-body approach to transport in quantum systems: From the transient regime to the stationary state
• Probing Inhomogeneous Cuprate Superconductivity by Terahertz Josephson Echo Spectroscopy
• 400 kHz repetition rate THz-TDS with 24 mW of average power driven by a compact industrial Yb-laser
• Principles of 2D terahertz spectroscopy of collective excitations: the case of Josephson plasmons in layered superconductors
• Field-Induced Electron Generation in Water: Solvation Dynamics and Many-Body Interactions
• Excitation-Dependent Features and Artifacts in 2-D Terahertz Spectroscopy
• Unlocking Quantum Control and Multi-Order Correlations via Terahertz Two-Dimensional Coherent Spectroscopy
• Solvated electrons in polar liquids as epsilon-near-zero materials tunable in the terahertz frequency range
• Coherent two-dimensional THz magnetic resonance spectroscopies for molecular magnets: Analysis of Dzyaloshinskii-Moriya interaction