Terahertz-Induced Tunnel Ionization Drives Coherent Raman-Active Phonon in Bismuth

Driving coherent lattice motion with THz pulses has emerged as a novel pathway for achieving dynamic stabilization of exotic phases that are inaccessible in equilibrium quantum materials. In this Letter, we present a previously unexplored mechanism for THz excitation of Raman-active phonons. We show that intense THz pulses centered at 1 THz can excite the Raman-active A1g phonon mode at 2.9 THz in a bismuth film. We rule out the possibilities of the phonon being excited through conventional anharmonic coupling to other modes or via a THz sum frequency process. Instead, we demonstrate that the THz-driven tunnel ionization provides a plausible means of creating a displacive driving force to initiate the phonon oscillations. Our Letter highlights a new mechanism for exciting coherent phonons, offering potential for dynamic control over the electronic and structural properties of semimetals and narrow-band semiconductors on ultrafast timescales.