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Optical Tuning of Exciton and Trion Emissions in Monolayer Phosphorene

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 Added by Yuerui Lu
 Publication date 2015
  fields Physics
and research's language is English




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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.



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Monolayer transition metal dichalcogenides (TMDs) are direct gap semiconductors emerging promising applications in diverse optoelectronic devices. To improve performance, recent investigations have been systematically focused on the tuning of their optical properties. However, an all-optical approach with the reversible feature is still a challenge. Here we demonstrate the tunability of the photoluminescence (PL) properties of monolayer WS2 via laser irradiation. The modulation of PL intensity, as well as the conversion between neutral exciton and charged trion have been readily and reversibly achieved by using different laser power densities. We attribute the reversible manipulation to the laser-assisted adsorption and desorption of gas molecules, which will deplete or release free electrons from the surface of WS2 and thus modify its PL properties. This all-optical manipulation, with advantages of reversibility, quantitative control, and high spatial resolution, suggests promising applications of TMDs monolayers in optoelectronic and nanophotonic applications, such as optical data storage, micropatterning, and display.
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.
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