Pump Pulse Bandwidth-Activated Nonlinear Phononic Coupling in CdWO4_4

To control structure-function relationships in solids with light, we must harness the shape of the potential energy surface, as expressed in anharmonic coupling coefficients. We use two-dimensional terahertz (THz) spectroscopy to identify trilinear coupling between sets of vibrational modes in CdWO$_4$. It is generally understood that efficient trilinear coupling occurs when the frequencies of two coupled modes add or subtract to the frequency of the third mode. Interestingly, we observe that this condition is not necessary: the THz driving-pulse itself can activate the coupling by contributing broad frequency content to the initial motion of the excited modes. Understanding that the bandwidth of the driving force can activate energy-flow pathways has broad implications for coherent control of collective modes using intense THz light pulses.Comment: 27 Pages, 15 Figure