Terahertz sum-frequency excitation of coherent optical phonons in the two-dimensional semiconductor WSe2

Driving fundamental excitations via strong light fields is one of the most important issues in solid state physics, which opens up new avenues to control material properties. Two-dimensional materials are fruitful platforms for future semiconductor applications, including opto-electronic and phononic devices, yet the phonon dynamics and nonlinear phonon–phonon coupling remain under-explored. Here, we demonstrate coherent phonon excitation in thin films of the layered two-dimensional semiconductor WSe2 induced by intense and broadband ultrafast terahertz (THz) pulses. We performed THz Kerr effect spectroscopy and observed coherent phonon oscillations assigned to the E2g optical phonon mode. The phonon amplitude displays a quadratic THz field strength dependence, indicating a sum-frequency THz excitation process. Furthermore, pump–probe polarization and crystal orientation relationships, supported by symmetry analysis of the nonlinear susceptibility and Raman tensors, provide helpful insight into nonlinear phonon–phonon interactions and potential coherent control schemes for the manipulation of phonon polarization and material properties in WSe2.