RESUMO
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.
Assuntos
Dissulfetos/química , Dissulfetos/efeitos da radiação , Eletroquímica/instrumentação , Nanopartículas Metálicas/química , Nanopartículas Metálicas/efeitos da radiação , Molibdênio/química , Molibdênio/efeitos da radiação , Fotoquímica/instrumentação , Ligas/química , Ligas/efeitos da radiação , Cristalização/métodos , Condutividade Elétrica , Desenho de Equipamento , Análise de Falha de Equipamento , Gases/química , Luz , Modelos Lineares , Teste de Materiais , Modelos Químicos , Nanotecnologia/instrumentação , Nanotecnologia/métodos , Doses de RadiaçãoRESUMO
The chemical vapor deposition (CVD) of molybdenum disulfide (MoS2) single-layer films onto periodically poled lithium niobate is possible while maintaining the substrate polarization pattern. The MoS2 growth exhibits a preference for the ferroelectric domains polarized "up" with respect to the surface so that the MoS2 film may be templated by the substrate ferroelectric polarization pattern without the need for further lithography. MoS2 monolayers preserve the surface polarization of the "up" domains, while slightly quenching the surface polarization on the "down" domains as revealed by piezoresponse force microscopy. Electrical transport measurements suggest changes in the dominant carrier for CVD MoS2 under application of an external voltage, depending on the domain orientation of the ferroelectric substrate. Such sensitivity to ferroelectric substrate polarization opens the possibility for ferroelectric nonvolatile gating of transition metal dichalcogenides in scalable devices fabricated free of exfoliation and transfer.
RESUMO
Chemical vapor deposition allows the preparation of few-layer films of MoTe2 in three distinct structural phases depending on the growth quench temperature: 2H, 1T', and 1T. We present experimental and computed Raman spectra for each of the phases and utilize transport measurements to explore the properties of the 1T MoTe2 phase. Density functional theory modeling predicts a (semi-)metallic character. Our experimental 1T films affirm the former, show facile µA-scale source-drain currents, and increase in conductivity with temperature, different from the 1T' phase. Variation of the growth method allows the formation of hybrid films of mixed phases that exhibit susceptibility to gating and significantly increased conductivity.
RESUMO
We used angle-resolved photoemission spectroscopy (ARPES) to map out the band structure of single-layer WSe2. The splitting of the top of the valence band because of spin-orbit coupling is 513 ± 10 meV, in general agreement with theoretical predictions and in the same range as that of bulk WSe2. Overall, our density functional theory (DFT) calculations of the band structure are in excellent agreement with the ARPES results. We have verified that the few discrepancies between theory and experiment are not due to the effect of strain. The differences between the DFT-calculated band structure using local density approximation (LDA) and that using the generalized gradient approximation (GGA), for single-layer WSe2, are caused mainly by differences in the respective charge densities.
RESUMO
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.
RESUMO
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.
RESUMO
We demonstrate bandgap tuning of a single-layer MoS2 film on SiO2/Si via substitution of its sulfur atoms by selenium through a process of gentle sputtering, exposure to a selenium precursor, and annealing. We characterize the substitution process both for S/S and S/Se replacement. Photoluminescence and, in the latter case, X-ray photoelectron spectroscopy provide direct evidence of optical band gap shift and selenium incorporation, respectively. We discuss our experimental observations, including the limit of the achievable bandgap shift, in terms of the role of stress in the film as elucidated by computational studies, based on density functional theory. The resultant films are stable in vacuum, but deteriorate under optical excitation in air.