Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses

TL;DR

This study uses broadband XUV pulses and first-principles calculations to simultaneously measure and reveal a coherent, bidirectional energy exchange between carriers and phonons in photoexcited bismuth, confirming theoretical predictions.

Contribution

It introduces a novel experimental approach combining transient reflectivity and first-principles calculations to directly observe coupled carrier-phonon dynamics in Peierls-distorted materials.

Findings

Revealed anticorrelation between phonon dynamics and carrier temperature.

Validated theoretical predictions of energy exchange in Peierls-distorted bismuth.

Demonstrated real-time, coupled electronic and structural response measurement.

Abstract

In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet to quantify both responses in photoexcited bismuth in a single measurement. With the help of first-principles calculations based on density-functional theory (DFT) and time-dependent DFT, the real-space atomic motion and the temperature of both electrons and holes as a function of time are captured simultaneously, retrieving an anticorrelation between the $A_{1g}$ phonon dynamics and carrier temperature. The results reveal a coherent, bi-directional energy exchange between carriers and phonons, which is a dynamical counterpart of the static Peierls-Jones distortion, providing first-time validation of previous theoretical predictions.