Unlocking Quantum Control and Multi-Order Correlations via Terahertz Two-Dimensional Coherent Spectroscopy

TL;DR

Terahertz two-dimensional coherent spectroscopy (THz-2DCS) is a powerful emerging technique that enables detailed probing, visualization, and control of quantum materials' ultrafast, nonequilibrium dynamics and multi-order correlations, revealing hidden excitations and collective modes.

Contribution

This review highlights recent advances in THz-2DCS, demonstrating its capabilities in exploring and manipulating quantum material properties beyond traditional methods.

Findings

Probing nonequilibrium superconductivity and topological phases.

Detecting exotic collective modes and excitations.

Advancing THz-2DCS instrumentation for future applications.

Abstract

Terahertz two-dimensional coherent spectroscopy (THz-2DCS) is transforming our ability to probe, visualize, and control quantum materials far from equilibrium. This emerging technique brings multi-dimensional resolution to the ultrafast dynamics of nonequilibrium phases of matter, enabling new capabilities demanding precise coherent control and measurement of many-body dynamics and multi-order correlations. By mapping complex excitations across time and frequency dimensions, THz-2DCS delivers coherence tomography of driven quantum matter, thus revealing hidden excitation pathways, measuring higher order nonlinear response functions, disentangling various quantum pathways, capturing collective modes on ultrafast timescales and at terahertz frequencies. These experimental features frequently remain obscured in traditional single particle measurements, ultrafast spectroscopy techniques, and equilibrium-based probes. This Review traces the early development of THz-2DCS and showcases significant recent progress in leveraging this technique to probe and manipulate quantum material properties, including nonequilibrium superconductivity, nonlinear magnonics, dynamical topological phases, and the detection of novel excitations and exotic collective modes with potential technological impact. Looking forward, we identify critical opportunities in advancing THz-2DCS instrumentation and experimental strategies that are shaping future applications in THz optoelectronics, quantum information processing, and sensing.