Surface Optical Rectification from Layered MoS₂ Crystal by THz Time-Domain Surface Emission Spectroscopy

Surface optical rectification was observed from the layered semiconductor molybdenum disulfide (MoS₂) crystal via terahertz (THz) time-domain surface emission spectroscopy under linearly polarized femtosecond laser excitation. The radiated THz amplitude of MoS₂ has a linear dependence on ever-increasing pump fluence and thus quadratic with the pump electric field, which discriminates from the surface Dember field induced THz radiation in InAs and the transient photocurrent-induced THz generation in graphite. Theoretical analysis based on space symmetry of MoS₂ crystal suggests that the underlying mechanism of THz radiation is surface optical rectification under the reflection configuration. This is consistent with the experimental results according to the radiated THz amplitude dependences on azimuthal and incident polarization angles. We also demonstrated the damage threshold of MoS₂ due to microscopic bond breaking under the femtosecond laser irradiation, which can be monitored via THz time-domain emission spectroscopy and Raman spectroscopy.