Probing Lattice Dynamics in Real-Space and Real-Time

TL;DR

This paper demonstrates how high-harmonic spectroscopy can probe coherent lattice vibrations and their effects on electronic responses in solids with ultrafast, atomic-scale resolution, offering an alternative to traditional diffraction methods.

Contribution

It introduces a novel application of high-harmonic spectroscopy to investigate lattice dynamics in real-space and real-time, achieving atomic-scale spatiotemporal resolution.

Findings

Coherent excitation of phonons in graphene produces sidebands in harmonic spectra.

HHS can characterize phonon mode properties like energy, polarization, and chirality.

Results agree with time-resolved diffuse x-ray scattering measurements.

Abstract

The coherent lattice vibrations significantly impact physical and chemical processes in solids, such as heat transfer, displacive phase transitions, and thermal conductivity. Thus, probing lattice dynamics in real-space and real-time is essential for understanding ubiquitous phenomena in solids. High-harmonic spectroscopy (HHS) has emerged as a preferred technique for investigating static and dynamic properties of solids on ultrafast timescales. Yet, despite these accomplishments, the applicability of HHS to probe the influence of coherent lattice vibrations on electronic responses has remained unexplored. In this thesis, we explore the impact of coherent lattice dynamics on attosecond electronic responses in solids using HHS. We observe that coherent excitation of the in-plane phonon mode in graphene results in sidebands in the harmonic spectrum, separated by the frequency of the excited phonon mode. Additionally, we demonstrate the capability of HHS to characterize energy, polarization, phase difference, and the "chirality" of phonon modes. This thesis offers an avenue to probe phonon-driven processes in solids with sub-cycle temporal resolution. In the later segment, our focus shifts toward probing coherent lattice dynamics in real-space and real-time. We demonstrate that inelastic scattering techniques, combined with theoretical analysis, yield comparable results to those from time-resolved diffraction and imaging measurements within pump-probe configurations. Our findings exhibit excellent agreement with results from a time-resolved diffuse x-ray scattering experiment. Our proposed method serves as an alternative to time-resolved diffraction and imaging methods for probing lattice dynamics in real-space and real-time with atomic-scale spatiotemporal resolution.