Two-dimensional (2D) transition metal dichalcogenides have emerged as a promising material system for optoelectronic applications, but their primary figure of merit, the room-temperature photoluminescence quantum yield (QY), is extremely low. The prototypical 2D material molybdenum disulfide (MoS2) is reported to have a maximum QY of 0.6%, which indicates a considerable defect density. Here we report on an air-stable, solution-based chemical treatment by an organic superacid, which uniformly enhances the photoluminescence and minority carrier lifetime of MoS2 monolayers by more than two orders of magnitude. The treatment eliminates defect-mediated nonradiative recombination, thus resulting in a final QY of more than 95%, with a longest-observed lifetime of 10.8 ± 0.6 nanoseconds. Our ability to obtain optoelectronic monolayers with near-perfect properties opens the door for the development of highly efficient light-emitting diodes, lasers, and solar cells based on 2D materials.

Monolayer molybdenum disulfide (MoS 2 ) has attracted tremendous attention due to its promising applications in high-performance field-effect transistors, phototransistors, spintronic devices and nonlinear optics. The enhanced photoluminescence effect in monolayer MoS 2 was discovered and, as a strong tool, was employed for strain and defect analysis in MoS 2 . Recently, large-size monolayer MoS 2 has been produced by chemical vapour deposition, but has not yet been fully explored. Here we systematically characterize chemical vapour deposition-grown MoS 2 by photoluminescence spectroscopy and mapping and demonstrate non-uniform strain in single-crystalline monolayer MoS 2 and strain-induced bandgap engineering. We also evaluate the effective strain transferred from polymer substrates to MoS 2 by three-dimensional finite element analysis. Furthermore, our work demonstrates that photoluminescence mapping can be used as a non-contact approach for quick identification of grain boundaries in MoS 2 .

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Defects in conventional semiconductors substantially lower the photoluminescence (PL)quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional (2D) transition metal dichalcogenides (TMDCs), such as monolayer MoS2, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic by electrostatic doping, without any chemical passivation. Surprisingly, neutral exciton recombination is entirely radiative even in the presence of a high native defect density. This finding enables TMDC monolayers for optoelectronic device applications as the stringent requirement of low defect density is eased.Multiparticle Coulomb interactions are particularly pronounced in transition metal dichalcogenide (TMDC) monolayers, leading to a multitude of recombination pathways, each associated with the different quasiparticles produced by these interactions (1). The recombination rate of excitons formed by photogenerated carriers (2, 3), depends nonlinearly on the concentration. Because excitons interact with background charge to form trions (4-8), the Fermi level also controls the dominant recombination pathway. Thus, both the background carrier concentration and the generation rate must be tuned to investigate the complete effect of multiparticle interactions on TMDC photoluminescence (PL) quantum yield (QY).In this work, we simultaneously altered the photocarrier generation rate (G) by varying the incident pump power, and the total charge concentration (electron and hole population densities; N and P) by varying the back-gate voltage (Vg) in a capacitor structure (Fig. 1A). Surprisingly, we found that all neutral excitons recombine radiatively in as-processed monolayers of MoS2, resulting in near-unity QY at low generation rates. This high QY occurred despite a reported high

Two-dimensional (2D) materials, particularly black phosphorus (bP), have demonstrated themselves to be excellent candidates for high-performance infrared photodetectors and transistors. However, high-quality bP can be obtained only via mechanical exfoliation from high-temperature- and high-pressure-grown bulk crystals and degrades rapidly when exposed to ambient conditions. Here, we report solution-synthesized and air-stable quasi-2D tellurium (Te) nanoflakes for short-wave infrared (SWIR) photodetectors. We perform comprehensive optical characterization via polarization-resolved transmission and reflection measurements and report the absorbance and complex refractive index of Te crystals. It is found that this material is an indirect semiconductor with a band gap of 0.31 eV. From temperature-dependent electrical measurements, we confirm this band-gap value and find that 12 nm thick Te nanoflakes show high hole mobilities of 450 and 1430 cm V s at 300 and 77 K, respectively. Finally, we demonstrate that despite its indirect band gap, Te can be utilized for high-performance SWIR photodetectors by employing optical cavity substrates consisting of Au/AlO to dramatically increase the absorption in the semiconductor. By changing the thickness of the AlO cavity, the peak responsivity of Te photoconductors can be tuned from 1.4 μm (13 A/W) to 2.4 μm (8 A/W) with a cutoff wavelength of 3.4 μm, fully capturing the SWIR band. An optimized room-temperature specific detectivity ( D*) of 2 × 10 cm Hz W is obtained at a wavelength of 1.7 μm.

Optoelectronic devices based on two-dimensional (2D) materials have shown tremendous promise over the past few years; however, there are still numerous challenges that need to be overcome to enable their application in devices. These include improving their poor photoluminescence (PL) quantum yield (QY) as well as better understanding of exciton-based recombination kinetics. Recently, we developed a chemical treatment technique using an organic superacid, bis(trifluoromethane)sulfonimide (TFSI), which was shown to improve the quantum yield in MoS2 from less than 1% to over 95%. Here, we perform detailed steady-state and transient optical characterization on some of the most heavily studied direct bandgap 2D materials, specifically WS2, MoS2, WSe2, and MoSe2, over a large pump dynamic range to study the recombination mechanisms present in these materials. We then explore the effects of TFSI treatment on the PL QY and recombination kinetics for each case. Our results suggest that sulfur-based 2D materials are amenable to repair/passivation by TFSI, while the mechanism is thus far ineffective on selenium based systems. We also show that biexcitonic recombination is the dominant nonradiative pathway in these materials and that the kinetics for TFSI treated MoS2 and WS2 can be described using a simple two parameter model.

Gold-mediated exfoliation of ultralarge optoelectronically perfect monolayers with lateral dimensions up to ≈500 μm is reported. Electrical, optical, and X-ray photo-electron spectroscopy characterization show that the quality of the gold-exfoliated flakes is similar to that of tape-exfoliated flakes. Large-area flakes allow manufacturing of large-area mono-layer transition metal dichalcogenide electronics.

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here we present a two-step low pressure vapor-assisted solution process to grow high quality homogeneous CH 3 NH 3 PbI 3-x Br x perovskite films over the full band gap range of 1.6 eV to 2.