Optical Tuning of Exciton and Trion Emissions in Monolayer Phosphorene

Monolayer phosphorene provides a unique two-dimensional (2D) platform to investigate the fundamental dynamics of excitons and trions (charged excitons) in reduced dimensions. However, owing to its high instability, unambiguous identification of monolayer phosphorene has been elusive. Consequently, many important fundamental properties, such as exciton dynamics, remain underexplored. We report a rapid, noninvasive, and highly accurate approach based on optical interferometry to determine the layer number of phosphorene, and confirm the results with reliable photoluminescence measurements. Furthermore, we successfully probed the dynamics of excitons and trions in monolayer phosphorene by controlling the photo-carrier injection in a relatively low excitation power range. Based on our measured optical gap and the previously measured electronic energy gap, we determined the exciton binding energy to be ~0.3 eV for the monolayer phosphorene on SiO2/Si substrate, which agrees well with theoretical predictions. A huge trion binding energy of ~100 meV was first observed in monolayer phosphorene, which is around five times higher than that in transition metal dichalcogenide (TMD) monolayer semiconductor, such as MoS2. The carrier lifetime of exciton emission in monolayer phosphorene was measured to be ~220 ps, which is comparable to those in other 2D TMD semiconductors. Our results open new avenues for exploring fundamental phenomena and novel optoelectronic applications using monolayer phosphorene.

Unambiguous identification of monolayer phosphorene by phase-shifting interferometry

Monolayer phosphorene provides a unique two-dimensional (2D) platform to investigate the fundamental many-body interactions. However, owing to its high instability, unambiguous identification of monolayer phosphorene has been elusive. Consequently, many important fundamental properties, such as exciton dynamics, remain underexplored. We report a rapid, noninvasive, and highly accurate approach based on optical interferometry to determine the layer number of phosphorene, and confirm the results with reliable photoluminescence measurements. Based on the measured optical gap and the calculated electronic energy gap, we determined the exciton binding energy to be ~0.4 eV for the monolayer phosphorene on SiO2/Si substrate, which agrees well with theoretical predictions. Our results open new avenues for exploring fundamental phenomena and novel optoelectronic applications using monolayer phosphorene.

Atomically Thin Optical Lenses and Gratings

Two-dimensional (2D) materials have emerged as promising candidates for miniaturized optoelectronic devices, due to their strong inelastic interactions with light. On the other hand, a miniaturized optical system also requires strong elastic light-matter interactions to control the flow of light. Here, we report giant optical path length (OPL) from a single-layer molybdenum disulfide (MoS2), which is around one order of magnitude larger than that from a single-layer graphene. Using such giant OPL to engineer the phase front of optical beams, we demonstrated, to the best of our knowledge, the worlds thinnest optical lens consisting of a few layers of MoS2 less than 6.3 nm thick. Moreover, we show that MoS2 has much better dielectric response than good conductor (like gold) and other dielectric materials (like Si, SiO2 or graphene). By taking advantage of the giant elastic scattering efficiency in ultra-thin high-index 2D materials, we demonstrated high-efficiency gratings based on a single- or few-layers of MoS2. The capability of manipulating the flow of light in 2D materials opens an exciting avenue towards unprecedented miniaturization of optical components and the integration of advanced optical functionalities.