MoS2(1-x) Se2x single-layer films are prepared using a mixture of organic selenium and sulfur precursors as well as a solid molybdenum source. The direct bandgaps are found to scale nearly linearly with composition in the range of 1.87 eV (pure single-layer MoS2 ) to 1.55 eV (pure single-layer MoSe2 ) permitting straightforward bandgap engineering.
Transition metal dichalcogenides (TMDs) have emerged as a new class of two-dimensional materials that are promising for electronics and photonics. To date, optoelectronic measurements in these materials have shown the conventional behavior expected from photoconductors such as a linear or sublinear dependence of the photocurrent on light intensity. Here, we report the observation of a new regime of operation where the photocurrent depends superlinearly on light intensity. We use spatially resolved photocurrent measurements on devices consisting of CVD-grown monolayers of TMD alloys spanning MoS2 to MoSe2 to show the photoconductive nature of the photoresponse, with the photocurrent dominated by recombination and field-induced carrier separation in the channel. Time-dependent photoconductivity measurements show the presence of persistent photoconductivity for the S-rich alloys, while photocurrent measurements at fixed wavelength for devices of different alloy compositions show a systematic decrease of the responsivity with increasing Se content associated with increased linearity of the current-voltage characteristics. A model based on the presence of different types of recombination centers is presented to explain the origin of the superlinear dependence on light intensity, which emerges when the nonequilibrium occupancy of initially empty fast recombination centers becomes comparable to that of slow recombination centers.
Sputtering of MoS2 films of single-layer thickness by low-energy argon ions selectively reduces the sulfur content of the material without significant depletion of molybdenum. X-ray photoelectron spectroscopy shows little modification of the Mo 3d states during this process, suggesting the absence of significant reorganization or damage to the overall structure of the MoS2 film. Accompanying ab initio molecular dynamics simulations find clusters of sulfur vacancies in the top plane of single-layer MoS2 to be structurally stable. Measurements of the photoluminescence at temperatures between 175 and 300 K show quenching of almost 80% for an ~10% decrease in sulfur content.
Lithium niobate is the archetypical ferroelectric material and the substrate of choice for numerous applications including surface acoustic wave radio frequencies devices and integrated optics. It offers a unique combination of substantial piezoelectric and birefringent properties, yet its lack of optical activity and semiconducting transport hamper application in optoelectronics. Here we fabricate and characterize a hybrid MoS2/LiNbO3 acousto-electric device via a scalable route that uses millimetre-scale direct chemical vapour deposition of MoS2 followed by lithographic definition of a field-effect transistor structure on top. The prototypical device exhibits electrical characteristics competitive with MoS2 devices on silicon. Surface acoustic waves excited on the substrate can manipulate and probe the electrical transport in the monolayer device in a contact-free manner. We realize both a sound-driven battery and an acoustic photodetector. Our findings open directions to non-invasive investigation of electrical properties of monolayer films.
MoS 2 is a highly interesting material, which exhibits a crossover from an indirect band gap in the bulk crystal to a direct gap for single layers. Here, we perform a direct comparison between large-area MoS 2 films grown by chemical vapor deposition (CVD) and MoS 2 flakes prepared by mechanical exfoliation from mineral bulk crystal. Raman spectroscopy measurements show differences between the in-plane and out-of-plane phonon mode positions in CVD-grown and exfoliated MoS 2 . Photoluminescence (PL) mapping reveals large regions in the CVD-grown films that emit strong PL at room-temperature, and low-temperature PL scans demonstrate a large spectral shift of the A exciton emission as a function of position. Polarization-resolved PL measurements under near-resonant excitation conditions show a strong circular polarization of the PL, corresponding to a valley polarization.
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