Monolayer (1L) transition metal dichalcogenides (TMDs) are two-dimensional direct-bandgap semiconductors with promising applications of quantum light emitters. Recent studies have shown that intrinsically low quantum yields (QYs) of 1L-TMDs can be greatly improved by chemical treatments. However, nonradiative exciton−exciton annihilation (EEA) appears to significantly limit light emission of 1L-TMDs at a nominal density of photoexcited excitons due to strong Coulomb interaction. Here we show that the EEA rate constant (γ) can be reduced by laser irradiation treatment in mechanically exfoliated monolayer tungsten disulfide (1L-WS 2 ), causing significantly improved light emission at the saturating optical pumping level. Time-resolved photoluminescence (PL) measurements showed that γ reduced from 0.66 ± 0.15 cm 2 /s to 0.20 ± 0.05 cm 2 /s simply using our laser irradiation. The laser-irradiated region exhibited lower PL response at low excitation levels, however at the high excitation level displayed 3× higher PL intensity and QY than the region without laser treatment. The shorter PL lifetime and lower PL response at low excitation levels suggested that laser irradiation increased the density of sulfur vacancies of 1L-WS 2 , but we attribute these induced defects, adsorbed by oxygen in air, to the origin for reduced EEA by hindering exciton diffusion. Our laser irradiation was likewise effective for reducing EEA and increasing PL of chemically treated 1L-WS 2 with a high QY, exhibiting the general applicability of our method. Our results suggest that exciton−exciton interaction in 1L-TMDs may be conveniently controlled by the laser treatment, which may lead to unsaturated exciton emission at high excitation levels.
Vertically stacked van der Waals (vdW) heterostructures have been suggested as a robust platform for studying interfacial phenomena and related electric/optoelectronic devices. While the interlayer Coulomb interaction mediated by the vdW coupling has been extensively studied for carrier recombination processes in a diode transport, its correlation with the interlayer tunneling transport has not been elucidated. Here, a contrast is reported between tunneling and drift photocurrents tailored by the interlayer coupling strength in MoSe /MoS hetero-bilayers (HBs). The interfacial coupling modulated by thermal annealing is identified by the interlayer phonon coupling in Raman spectra and the emerging interlayer exciton peak in photoluminescence spectra. In strongly coupled HBs, positive photocurrents are observed owing to the inelastic band-to-band tunneling assisted by interlayer excitons that prevail over exciton recombinations. By contrast, weakly coupled HBs exhibit a negative photovoltaic diode behavior, manifested as a drift current without interlayer excitonic emissions. This study sheds light on tailoring the tunneling transport for numerous optoelectronic HB devices.
Structural phase transitions in layered two-dimensional (2D) materials are of significant interest owing to their ability to exist in multiple metastable states with distinctive properties. However, phase transition in bulk MoS2 by nondestructive electron infusion has not yet been realized. In this study, we report the 2H to 1T′ phase transition and in-between intermediates in bulk MoS2 using MoS2/[Ca2N]+·e– heterostructures, in which kinetic free electrons were directly injected into MoS2. We observed various phases in MoS2 ranging from heavily doped 2H to a distorted lattice state and then on to a complete 1T′ state. Snapshots of the multiphase transition were captured by extraordinary Raman shift and bandgap reduction and were further elucidated by theoretical calculations. We also observed a weakening in interlayer coupling in the vicinity of the metallic regime, which led to an unusually strong photoluminescence emission, suggesting light-efficient bulk MoS2. Our results thus suggest the optoelectronic applications that can fully utilize the multiphase transition of bulk 2D materials.
Spatially heterogeneous effects of bis(trifluoromethane)sulfonimide (TFSI) and benzyl viologen (BV) treatment on the optical properties of triangular monolayer tungsten disulfides are investigated by nanoscale spectral imaging.
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