Exciton Brightening in Monolayer Phosphorene via Dimensionality Modification

Abstract: Two-dimensional (2D) monolayer phosphorene, a 2D system with quasi-one-dimensional (quasi-1D) excitons, provides a unique 2D platform for investigating the dynamics of excitons in reduced dimensions and fundamental many-body interactions. However, on the other hand, the quasi-1D excitonic nature can limit the luminescence quantum yield significantly. Here, we report exciton brightening in monolayer phosphorene achieved via the dimensionality modification of excitons from quasi-1D to zero-dimensional (0D), through the transference of monolayer phosphorene samples onto defect-rich oxide substrate deposited by plasma-enhanced chemical vapor deposition (PECVD). The resultant interfacial luminescent local states lead to exciton localization and trigger efficient photon emissions at a new wavelength of ~920 nm. The luminescence quantum yield of 0D-like localized excitons is measured to be at least 33.6 times larger than that of intrinsic quasi-1D free excitons in monolayer phosphorene. This is primarily due to the reduction of non-radiative decay rate and the possibly enhanced radiative recombination probability. Owing to the large trapping energy, this new photon emission from the localized excitons in monolayer phosphorene can be observed at elevated temperature, which contrasts markedly with defect-induced photon emission from transition metal dichalcogenide (TMD) semiconductor monolayers that can only be observed at cryogenic temperatures. Our findings introduce new avenues for the development of novel photonic devices based on monolayer phosphorene, such as near-infrared lighting devices that are operable at elevated temperature. More importantly, 2D phosphorene with quasi-1D free excitons and 0D-like localized excitons provides a unique platform to investigate the fundamental phenomena in the ideal 2D-1D-0D hybrid system.