Ultrafast shift current dynamics in WS₂ monolayer

The shift current effect, in materials lacking inversion symmetry, may potentially allow the performance of photovoltaics to surpass the Shockley-Queisser limit for traditional p-n junction-based photovoltaics. Although the shift-current effect has been studied from first principles via second-order perturbation theory, an understanding of the dynamics of hot carriers is still lacking. We investigate the dynamics of the shift current in monolayer WS2 via real-time propagation time-dependent density functional theory (rt-TDDFT). We find that the shift current can be generated within 10-20 fs after turning on the lights, and dissipates within approximately a few tens of femtoseconds after turning off the lights. This property can be used for ultrafast photon detection. This work provides an important step toward understanding the dynamics of shift-current effects, which is crucial for device applications.