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Acting as a highly nonlinear response to the strong laser field, highharmonic generation (HHG) naturally contains the fingerprints of atomic andelectronic properties of materials. Electronic properties of a solid such asband structure and topology can thus be probed, while the phonon dynamicsduring HHG are often neglected. Here we show that by exploiting the effects ofphonon deformation on HHG, the intrinsic phonon information can be decipheredand direct probing of band- and mode-resolved electron-phonon couplings (EPC)of photoexcited materials is possible. Considering HHG spectroscopy can bevacuum free and unrestricted to electron occupation, this work suggests HHG ispromising for all-optical characterization of EPC in solids, especially forgapped quantum states or materials under high pressure.

Probing Phonon dynamics and Electron-Phonon Coupling by High Harmonic Generation in Solids