Strong Local-Field Enhancement of the Nonlinear Soft-Mode Response in a Molecular Crystal

The nonlinear response of soft-mode excitations in polycrystalline acetylsalicylic acid (aspirin) is studied with two-dimensional terahertz spectroscopy. We demonstrate that the correlation of CH3 rotational modes with collective oscillations of pi electrons drives the system into the nonperturbative regime of light-matter interaction, even for a moderate strength of the THz driving field on the order of 50 kV/cm. Nonlinear absorption around 1.1 THz leads to a blueshifted coherent emission at 1.7 THz, revealing the dynamic breakup of the strong electron-phonon correlations. The observed behavior is reproduced by theoretical calculations including dynamic local-field correlations.