Light Polarization-Controlled Conversion of Ultrafast Coherent-Incoherent Exciton Dynamics in Few-Layer ReS2

Coherent light-matter interaction can transiently modulate the quantum states of matter under nonresonant laser excitation. This phenomenon, called the optical Stark effect, is one of the promising candidates for realizing ultrafast optical switches. However, the ultrafast modulations induced by the coherent light-matter interactions usually involve unwanted incoherent responses, significantly reducing the overall operation speed. Here, by using ultrafast pump-probe spectroscopy, we suppress the incoherent response and modulate the coherent-to-incoherent ratio in the two-dimensional semiconductor ReS2. We selectively convert the coherent and incoherent responses of an anisotropic exciton state by solely using photon polarizations, improving the control ratio by 3 orders of magnitude. The efficient modulation was enabled by transient superpositions of differential spectra from two nondegenerate exciton states due to the light polarization dependencies. This work provides a valuable contribution toward realizing ideal ultrafast optical switches.