Ab initio nonadiabatic molecular dynamics investigation on the dynamics of photogenerated spin hole current in Cu-doped MoS2

Fully spin-polarized hole current is theoretically proposed to be generated by photoexcitation in the impurity states of the MoS2 monolayer with sulfur partially substituted by copper. To understand the dynamics of the photogenerated spin hole current, we perform a time-domain ab initio nonadiabatic molecular dynamics investigation with different initial excitation and temperature. First, the spin hole relaxes in a band-by-band manner. Therefore a longer lifetime can be achieved if the initial hole is generated at the lower edge of the impurity bands. Second, the phonon excitation is found to affect the spin hole dynamics significantly. When the temperature is decreased from 100 to 50 K, the hole relaxation across the band gap is strongly suppressed by the phonon bottleneck, which is due to the reduction of the phonon occupations. Our results show that the initial hole generation and phonon excitation are two key factors determining the dynamics of the photogenerated spin hole, which provide insights into the design of optimal spintronic devices.