Detection of a Coherent Excitonic State in the Layered Semiconductor BiI3

The measurement and manipulation of the coherent dynamics of excitonic states constitute a forefront research challenge in semiconductor optics and quantum-coherence-based protocols for optoelectronic technologies. Layered semiconductors have emerged as an ideal platform for the study of exciton dynamics with accessible and technologically relevant energy and time scales. Here, we investigate the subpicosecond exciton dynamics in a van der Waals semiconductor upon quasi-resonant excitation and achieve to single out an incipient coherent excitonic state. Combining broad-band transient reflectance spectroscopy and simulations based on many-body perturbation theory, we reveal a transient enhancement of the excitonic line intensity that originates from photoinduced coherent polarization that is phase-locked with the interacting electromagnetic field. This finding allows us to define the spectral signature of a coherent excitonic state and to experimentally track the dynamical crossover from coherent to incoherent exciton, unlocking the prospective optical control of an exciton population on the intrinsic quantum-coherence time scale.