Excitons are quasi-particles composed of electron–hole
pairs
through Coulomb interaction. Due to the atomic-thin thickness, they
are tightly bound in monolayer transition metal dichalcogenides (TMDs)
and dominate their optical properties. The capability to manipulate
the excitonic behavior can significantly influence the photon emission
or carrier transport performance of TMD-based devices. However, on-demand
and region-selective manipulation of the excitonic states in a reversible
manner remains challenging so far. Herein, harnessing the coordinated
effect of femtosecond-laser-driven atomic defect generation, interfacial
electron transfer, and surface molecular desorption/adsorption, we
develop an all-optical approach to manipulate the charge states of
excitons in monolayer molybdenum disulfide (MoS2). Through
steering the laser beam, we demonstrate reconfigurable optical encoding
of the excitonic charge states (between neutral and negative states)
on a single MoS2 flake. Our technique can be extended to
other TMDs materials, which will guide the design of all-optical and
reconfigurable TMD-based optoelectronic and nanophotonic devices.