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.

Transition metal dichalcogenides (TMDCs) have been extensively explored for applications in electronic and optoelectronic devices due to their unique material properties. However, the presence of large contact resistances is still a fundamental challenge in the field. In this work, we study defect engineering by using a mild plasma treatment (He or H2) as an approach to reduce the contact resistance to WSe2. Material characterization by X-ray photoelectron spectroscopy, photoluminescence, and Kelvin probe force microscopy confirm defect-induced n-doping, up to degenerate level, which is attributed to the creation of anion (Se) vacancies. The plasma treatment is adopted in the fabrication process flow of WSe2 n-type metal-oxide-semiconductor field-effect transistors to selectively create anion vacancies at the metal contact regions. Due to lowering the metal contact resistance, improvements in the device performance metrics such as a 20× improvement in ON current and a nearly ideal subthreshold swing value of 66 mV/dec are observed. This work demonstrates that defect engineering at the contact regions can be utilized as a reliable scheme to realize high-performance electronic and optoelectronic TMDC devices.

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Molybdenum disulfide (MoS2) has been widely examined as a catalyst containing no precious metals for the hydrogen evolution reaction (HER); however, these examinations have utilized synthesized MoS2 because the pristine MoS2 mineral is known to be a poor catalyst. The fundamental challenge with pristine MoS2 is the inert HER activity of the predominant (0001) basal surface plane. In order to achieve high HER performance with pristine MoS2, it is essential to activate the basal plane. Here, we report a general thermal process in which the basal plane is texturized to increase the density of HER-active edge sites. This texturization is achieved through a simple thermal annealing procedure in a hydrogen environment, removing sulfur from the MoS2 surface to form edge sites. As a result, the process generates high HER catalytic performance in pristine MoS2 across various morphologies such as the bulk mineral, films composed of micron-scale flakes, and even films of a commercially available spray of nanoflake MoS2. The lowest overpotential (η) observed for these samples was η = 170 mV to obtain 10 mA/cm(2) of HER current density.

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