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Register a new userUnambiguous identification of monolayer phosphorene by phase-shifting interferometry
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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.
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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.
The two-dimensional semiconductor phosphorene has attracted extensive research interests for potential applications in optoelectronics, spintronics, catalysis, sensors, and energy conversion. To harness phosphorenes potential requires a better understanding of how intrinsic defects control carrier concentration, character, and mobility. Using density-functional theory and a charge correction scheme to account for the appropriate boundary conditions, we conduct a comprehensive study of the effect of structure on the formation energy, electronic structure, and charge transition level of the charged vacancy point defects in phosphorene. We predict that the neutral vacancy exhibits a 9-5 ring structure with a formation energy of 1.7 eV and transitions to a negatively charged state at a Fermi level 1.04 eV above the valence band maximum. The corresponding optical charge transitions display sizeable Frank-Condon shifts with a large Stokes shift of 0.3 eV. Phosphorene vacancies should become negatively charged in n-doped phosphorene, which would passivate the dopants and reduce the charge carrier concentration and mobility.
There have been continuous efforts to seek for novel functional two-dimensional semiconductors with high performance for future applications in nanoelectronics and optoelectronics. In this work, we introduce a successful experimental approach to fabricate monolayer phosphorene by mechanical cleavage and the following Ar+ plasma thinning process. The thickness of phosphorene is unambiguously determined by optical contrast combined with atomic force microscope (AFM). Raman spectroscopy is used to characterize the pristine and plasma-treated samples. The Raman frequency of A2g mode stiffens, and the intensity ratio of A2g to A1g modes shows monotonic discrete increase with the decrease of phosphorene thickness down to monolayer. All those phenomena can be used to identify the thickness of this novel two-dimensional semiconductor efficiently. This work for monolayer phosphorene fabrication and thickness determination will facilitates the research of 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.
In the current extensive studies of transition metal dichalcogenides (TMDCs), compared to hexagonal layered materials, like graphene, hBN and MoS2, low symmetry layered 2D crystals showed great potential for applications in anisotropic devices. Rhenium diselenide (ReSe2) has the bulk space group P1 and belongs to triclinic crystal system with a deformed cadmium iodide type structure. Here we unambiguously determined monolayer and its vertical orientation of rhenium diselenide membrane with an individual electron diffraction pattern, which could be applicable to low symmetry crystal systems, including both triclinic and monoclinic lattices, as long as their third unit-cell basis vector is not perpendicular to basal plane. Atomically resolved image from probe corrected annular dark field scanning transmission electron microscope (ADF-STEM) was employed to validate layer number. Finally, experimental results were well explained by kinematical electron diffraction theory and corresponding simulations.
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