Probing phonon-driven symmetry alterations in graphene via high-harmonic spectroscopy

Abstract: High-harmonic spectroscopy has become an essential ingredient in probing various ultrafast electronic processes in solids with sub-cycle temporal resolution. Despite its immense importance, sensitivity of high-harmonic spectroscopy to phonon dynamics in solids is not well known. This work addresses this critical question and demonstrates the potential of high-harmonic spectroscopy in probing intertwined phonon-electron dynamics in solids. A pump pulse excites in-plane optical phonon modes in monolayer graphene and a circularly polarised pulse is employed to probe the excited phonon dynamics that generates higher-order harmonics. We show that the coherent phonon dynamics alters the dynamical symmetry of graphene with the probe pulse and leads the generations of the symmetry-forbidden harmonics. Moreover, sidebands associated with the prominent harmonic peaks are generated as a result of the coherent dynamics. It is found that the symmetries and the characteristic timescale of the excited phonon mode determine the polarisation and positions of these sidebands. Present work opens an avenue in time-resolved probing of phonon-driven processes and dynamical symmetries in solids with sub-cycle temporal resolution.