Shaping Exciton Dynamics in 2D Semiconductors by Tailored Ultrafast Pulses

Abstract Excitonic resonances in two-dimensional semiconductors play a crucial role in enhancing nonlinear light-matter interactions. However, the influence of resonant dynamics on the time-dependent behavior of these nonlinear effects has received little attention, as optical wave-mixing is commonly assumed to be instantaneous. In this study, we investigate the impact of excited state dynamics on the generation of second and third-order nonlinearities from Monolayer WSe2 in ambient conditions. By shaping a sub-10fs driving pulse to complement the exciton resonant dynamics, we demonstrate a significant enhancement of four-wave-mixing beyond what is achieved using a transform-limited pulse. Conversely, a time-reversed pulse shape leads to destructive quantum interference effects, suppressing nonlinear generation. We apply this technique simultaneously to two successive exciton states, showcasing the selective choice in the resonant state that produces nonlinearity. The ability to control nonlinear carrier dynamics in two-dimensional semiconductors holds promise for remote noninvasive optical manipulation in optoelectronic devices.