Intrinsic temporal and spectral mixing in time-resolved terahertz spectroscopy

TL;DR

This paper reveals that ultrafast optical-pump terahertz-probe measurements exhibit complex time-frequency features due to intrinsic mixing effects, which can be misinterpreted as coherent responses, and provides a theoretical and experimental analysis of these phenomena.

Contribution

It introduces a systematic understanding of intrinsic temporal and spectral mixing effects in time-resolved terahertz spectroscopy through experiments, simulations, and extended response theory.

Findings

Unexpected early-time features in 2D THz maps explained by intrinsic mixing.

Finite-difference time-domain simulations reproduce observed features.

Extended non-equilibrium response theory accounts for systematic effects.

Abstract

In an ultrafast optical-pump terahertz-probe measurement, the photoinduced material response can be modulated on a timescale shorter than the extent of the THz pulse. In this situation, the measured time-frequency response deviates from a simple time-dependent linear response. When full two-dimensional time-frequency maps are measured, this yields complex features that can be incorrectly assigned to a photoexcited coherent response. We investigate this experimentally via the measured response of photoexcited SnSe, whereby photoinduced phase change dynamics lead to ultrafast changes of the charge carrier and lattice optical conductivity response. Two-dimensional time-frequency THz transmission maps subsequently show unexpected time-frequency features at early pump-probe delay times. These features are reproduced in both finite-difference time-domain simulations of the THz experiment and in an extension of non-equilibrium response function theory, demonstrating their systematic origin. This work improves the understanding of systematic effects in high time resolution optical-pump THz-probe spectroscopy, and explores the conditions in which they are likely to appear.