High Harmonic Spectroscopy Probes Lattice Dynamics

The probing of coherent lattice vibrations in solids has been conventionally carried out using time-resolved transient spectroscopy where only the relative oscillation amplitude can be obtained. Using time-resolved X-ray techniques, absolute electron-phonon coupling strength could be extracted. However, the complexity of such an experiment renders it impossible to be carried out in conventional laboratories. Here we demonstrate that the electron-phonon, anharmonic phonon-phonon coupling, and their relaxation dynamics can be probed in real-time using high-harmonic spectroscopy. Our technique is background-free and has extreme sensitivity directly in the energy domain. In combination with the optical deformation potential calculated from density functional perturbation theory and the absolute energy modulation depth, our measurement reveals the maximum displacement of neighboring oxygen atoms in α-quartz crystal to tens of picometers in real space. By employing a straightforward and robust time-windowed Gabor analysis for the phonon-modulated high-harmonic spectrum, we successfully observe channel-resolved four-phonon scattering processes in such highly nonlinear interactions. Our work opens a new realm for accurate measurement of coherent phonons and their scattering dynamics, which allows for potential benchmarking ab-initio calculations in solids