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Register a new userEnvironment-insensitive and gate-controllable photocurrent enabled by bandgap engineering of MoS2 junctions
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Two-dimensional (2D) materials are composed of atomically thin crystals with an enormous surface-to-volume ratio, and their physical properties can be easily subjected to the change of the chemical environment. Encapsulation with other layered materials, such as hexagonal boron nitride, is a common practice; however, this approach often requires inextricable fabrication processes. Alternatively, it is intriguing to explore methods to control transport properties in the circumstance of no encapsulated layer. This is very challenging because of the ubiquitous presence of adsorbents, which can lead to charged-impurity scattering sites, charge traps, and recombination centers. Here, we show that the short-circuit photocurrent originated from the built-in electric field at the MoS2 junction is surprisingly insensitive to the gaseous environment over the range from a vacuum of 1X10^(-6) Torr to ambient condition. The environmental insensitivity of the short-circuit photocurrent is attributed to the characteristic of the diffusion current that is associated with the gradient of carrier density. Conversely, the photocurrent with bias exhibits typical persistent photoconductivity and greatly depends on the gaseous environment. The observation of environment-insensitive short-circuit photocurrent demonstrates an alternative method to design device structure for 2D-material-based optoelectronic applications.
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We report the influence of uniaxial tensile mechanical strain in the range 0-2.2% on the phonon spectra and bandstructures of monolayer and bilayer molybdenum disulfide (MoS2) two-dimensional crystals. First, we employ Raman spectroscopy to observe phonon softening with increased strain, breaking the degeneracy in the E Raman mode of MoS2, and extract a Gruneisen parameter of ~1.06. Second, using photoluminescence spectroscopy we measure a decrease in the optical band gap of MoS2 that is roughly linear with strain, ~45 meV% strain for monolayer MoS2 and ~120 meV% strain for bilayer MoS2. Third, we observe a pronounced strain-induced decrease in the photoluminescence intensity of monolayer MoS2 that is indicative of the direct-to-indirect transition of the character of the optical band gap of this material at applied strain of ~1.5%, a value supported by first-principles calculations that include excitonic effects. These observations constitute the first demonstration of strain engineering the band structure in the emergent class of two-dimensional crystals, transition-metal dichalcogenides.
The discovery of graphene has put the spotlight on other layered materials including transition metal dichalcogenites (TMD) as building blocks for novel heterostructures assembled from stacked atomic layers. Molybdenum disulfide, MoS2, a semiconductor in the TMD family, with its remarkable thermal and chemical stability and high mobility, has emerged as a promising candidate for post-silicon applications such as switching, photonics, and flexible electronics. Since these rely on controlling the position of the Fermi energy (EF), it is crucial to understand its dependence on doping and gating. Here we employed scanning tunneling microscopy (STM) and spectroscopy (STS) with gating capabilities to measure the bandgap and the position of EF in MoS2, and to track its evolution with gate voltage. For bulk samples, the measured bandgap (~1.3eV) is comparable to the value obtained by photoluminescence, and the position of EF (~0.35eV) below the conduction band, is consistent with n-doping reported in this material. Using topography together with spectroscopy we traced the source of the n-doping in bulk MoS2 samples to point defects, which we attribute to S vacancies. In contrast, for thin films deposited on SiO2, we found significantly higher levels of n-doping that cannot be attributed to S vacancies. By combining gated STS with transport measurements in a field effect transistor (FET) configuration, we demonstrate that the higher levels of n-doping in thin film samples is due to charge traps at the sample-substrate interface.
The unusual electrical and optical properties of graphene make it a promising candidate for optoelectronic applications. An important, but as yet unexplored aspect is the role of photo-excited hot carriers in charge and energy transport at graphene interfaces. Here, we perform time-resolved (~250 fs) scanning photocurrent microscopy on a tunable graphene pn junction. The ultrafast pump-probe measurements yield a photocurrent response time of ~1.5 ps at room temperature increasing to ~4 ps at 20 K. Combined with the negligible dependence of photocurrent amplitude on environmental temperature this implies that hot carriers rather than phonons dominate energy transport at high frequencies. Gate-dependent pump-probe measurements demonstrate that both thermoelectric and built-in electric field effects contribute to the photocurrent excited by laser pulses. The relative weight of each contribution depends on the junction configuration. A single laser beam excitation also displays multiple polarity-reversals as a function of carrier density, a signature of impact ionization. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (~500 GHz) for potential graphene-based photon detection, sensing, and communication.
The ability to control the size of the electronic bandgap is an integral part of solid-state technology. Atomically-thin two-dimensional crystals offer a new approach for tuning the energies of the electronic states based on the interplay between the environmental sensitivity and unusual strength of the Coulomb interaction in these materials. By engineering the surrounding dielectric environment, we are able to tune the electronic bandgap in monolayers of WS2 and WSe2 by hundreds of meV. We exploit this behavior to present an in-plane dielectric heterostructure with a spatially dependent bandgap, illustrating the feasibility of our approach for the creation of lateral junctions with nanoscale resolution. This successful demonstration of bandgap engineering based on the non-invasive modification of the Coulomb interaction should enable the design of a new class of atomically thin devices to advance the limits of size and functionality for solid-state technologies.
We introduce an always-on, exchange-only qubit made up of three localized semiconductor spins that offers a true sweet spot to fluctuations of the quantum dot energy levels. Both single- and two-qubit gate operations can be performed using only exchange pulses while maintaining this sweet spot. We show how to interconvert this qubit to other three-spin encoded qubits as a new resource for quantum computation and communication.
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