First-principles study of electron dynamics of MoS2 under femtosecond laser irradiation from deep ultraviolet to near-infrared wavelengths

Time-dependent density functional theory was employed to investigate the electron dynamics of MoS2 following femtosecond pulse irradiation. The study concerned the effects of laser wavelength, intensities, and polarization and elucidated the ionization mechanisms across the intensity range of 1010–1014 W/cm2. As laser intensity increases, MoS2 irradiated with an infrared (IR) laser (800 nm) deviates from single-photon absorption at lower intensities compared to that subjected to an ultraviolet (UV) laser (266 nm), and nonlinear effects in the current arise at lower intensities for the 800 nm laser. At a wavelength of 266 nm, MoS2 irradiated with an a-axis polarized laser deposited more energy and generated more electron–hole pairs compared to c-axis polarization. Rate equations were used to estimate the total number of excited electrons in MoS2 and the corresponding plasma frequency. Simulation results indicate that the damage threshold of the UV laser is higher than that of the IR laser, which contradicts the experimental results. This outcome suggests that the mechanism of material damage induced by the UV femtosecond laser near the damage threshold is independent of optical breakdown. The findings of this research are significant for enhancing the performance of MoS2-based photodetectors and optimizing their stability and reliability in high-power, short-wavelength laser applications.