Layer-Dependent Interfacial Transport and Optoelectrical Properties of MoS2 on Ultraflat Metals.

Layered materials based on transition-metal dichalcogenides (TMDs) are promising for a wide range of electronic and optoelectronic devices. Realizing such practical applications often requires metal-TMD connections or contacts. Hence, a complete understanding of electronic band alignments and potential barrier heights governing the transport through metal-TMD junctions is critical. However, it is presently unclear how the energy bands of a TMD align while in contact with a metal as a function of the number of layers. In pursuit of removing this knowledge gap, we have performed conductive atomic force microscopy (CAFM) of few-layered (1 to 5 layers) MoS2 immobilized on ultraflat conducting Au surfaces [root-mean-square (rms) surface roughness < 0.2 nm] and indium-tin oxide (ITO) substrates (rms surface roughness < 0.7 nm) forming a vertical metal (CAFM tip)-semiconductor-metal device. We have observed that the current increases with the number of layers up to five layers. By applying Fowler-Nordheim tunneling theory, we have determined the barrier heights for different layers and observed how this barrier decreases as the number of layers increases. Using density functional theory calculations, we successfully demonstrated that the barrier height decreases as the layer number increases. By illuminating TMDs on a transparent ultraflat conducting ITO substrate, we observed a reduction in current when compared to the current measured in the dark, hence demonstrating negative photoconductivity. Our study provides a fundamental understanding of the local electronic and optoelectronic behaviors of the TMD-metal junction, which depends on the numbers of TMD layers and may pave an avenue toward developing nanoscale electronic devices with tailored layer-dependent transport properties.

Photoresponse of Natural van der Waals Heterostructures.

Van der Waals heterostructures consisting of two-dimensional materials offer a platform to obtain materials by design and are very attractive owing to unique electronic states. Research on 2D van der Waals heterostructures (vdWH) has so far been focused on fabricating individually stacked atomically thin unary or binary crystals. Such systems include graphene, hexagonal boron nitride, and members of the transition metal dichalcogenide family. Here we present our experimental study of the optoelectronic properties of a naturally occurring vdWH, known as franckeite, which is a complex layered crystal composed of lead, tin, antimony, iron, and sulfur. We present here that thin film franckeite (60 nm < d < 100 nm) behaves as a narrow band gap semiconductor demonstrating a wide-band photoresponse. We have observed the band-edge transition at ∼1500 nm (∼830 meV) and high external quantum efficiency (EQE ≈ 3%) at room temperature. Laser-power-resolved and temperature-resolved photocurrent measurements reveal that the photocarrier generation and recombination are dominated by continuously distributed trap states within the band gap. To understand wavelength-resolved photocurrent, we also calculated the optical absorption properties via density functional theory. Finally, we have shown that the device has a fast photoresponse with a rise time as fast as ∼1 ms. Our study provides a fundamental understanding of the optoelectronic behavior in a complex naturally occurring vdWH, and may pave an avenue toward developing nanoscale optoelectronic devices with tailored properties.

Electrical Control of near-Field Energy Transfer between Quantum Dots and Two-Dimensional Semiconductors.

We investigate near-field energy transfer between chemically synthesized quantum dots (QDs) and two-dimensional semiconductors. We fabricate devices in which electrostatically gated semiconducting monolayer molybdenum disulfide (MoS2) is placed atop a homogeneous self-assembled layer of core-shell CdSSe QDs. We demonstrate efficient nonradiative Förster resonant energy transfer (FRET) from QDs into MoS2 and prove that modest gate-induced variation in the excitonic absorption of MoS2 leads to large (∼500%) changes in the FRET rate. This in turn allows for up to ∼75% electrical modulation of QD photoluminescence intensity. The hybrid QD/MoS2 devices operate within a small voltage range, allow for continuous modification of the QD photoluminescence intensity, and can be used for selective tuning of QDs emitting in the visible-IR range.

Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy.

The optical response of semiconducting monolayer transition-metal dichalcogenides (TMDCs) is dominated by strongly bound excitons that are stable even at room temperature. However, substrate-related effects such as screening and disorder in currently available specimens mask many anticipated physical phenomena and limit device applications of TMDCs. Here, we demonstrate that that these undesirable effects are strongly suppressed in suspended devices. Extremely robust (photogain > 1,000) and fast (response time < 1 ms) photoresponse allow us to study, for the first time, the formation, binding energies, and dissociation mechanisms of excitons in TMDCs through photocurrent spectroscopy. By analyzing the spectral positions of peaks in the photocurrent and by comparing them with first-principles calculations, we obtain binding energies, band gaps and spin-orbit splitting in monolayer TMDCs. For monolayer MoS2, in particular, we obtain an extremely large binding energy for band-edge excitons, E bind ≥ 570 meV. Along with band-edge excitons, we observe excitons associated with a van Hove singularity of rather unique nature. The analysis of the source-drain voltage dependence of photocurrent spectra reveals exciton dissociation and photoconversion mechanisms in TMDCs.

Graphene transistor as a probe for streaming potential.

We explore the dependence of electrical transport in a graphene field effect transistor (GraFET) on the flow of water/sodium chloride electrolyte within the immediate vicinity of that transistor. We find large and reproducible shifts in the charge neutrality point of GraFETs that are dependent on the liquid velocity and the ion concentration. We show that these shifts are consistent with the variation of the local electrochemical potential of the liquid next to graphene that are caused by the fluid flow (streaming potential). Furthermore, we utilize the sensitivity of electrical transport in GraFETs to the parameters of the fluid flow to demonstrate graphene-based mass flow and ionic concentration sensing. We successfully detect a flow as small as ∼70 nL/min and detect a change in the ionic concentration as small as ∼40 nM.

Probing charge scattering mechanisms in suspended graphene by varying its dielectric environment.

Graphene with high carrier mobility µ is required both for graphene-based electronic devices and for the investigation of the fundamental properties of Dirac fermions. An attractive approach to increase the mobility is to place graphene in an environment with high static dielectric constant κ that would screen the electric field due to the charged impurities present near graphene's surface. Here we investigate the effect of the dielectric environment of graphene and study electrical transport in multi-terminal graphene devices suspended in liquids with κ ranging from 1.9 to 33. For non-polar liquids (κ<5), we observe a rapid increase of µ(κ), with room-temperature mobility reaching ~60,000 cm(2) Vs(-1) for devices in anisole (κ = 4.3). We associate this trend with dielectric screening of charged impurities adsorbed on graphene. We observe much lower mobility µ~20,000 cm(2) Vs(-1) for devices in polar liquids (κ ≥ 18) and explain it by additional scattering caused by ions present in such liquids.

A nanoscale Ti∕GaAs metal-semiconductor hybrid sensor for room temperature light detection.

We report an individually addressable Ti∕GaAs metal-semiconductor hybrid optical nanosensor with positive photoresistance and a sensitivity that increases as the device dimensions shrink. The underlying physics relates to the crossover from ballistic to diffusive transport of the photoinduced carriers and the geometric enhancement of the effect associated with a Schottky-barrier-coupled parallel metal shunt layer. For a 250 nm device under 633 nm illumination we observe a specific detectivity of D(*)=5.06×10(11) cm √Hz∕W with a dynamic response of 40 dB.

Fluidic measurement of electric field sensitivity of Ti-GaAs Schottky junction gated field effect biosensors.

We report the electric field and pH sensitivity of fluid gated metal-semiconductor hybrid (MSH) Schottky structures consisting of a Titanium layer on n-type GaAs. Compared to standard field-effect sensors, the MSH Schottky structures are 21 times more sensitive to electric field of -46.6 V/cm and show about six times larger resistance change as pH of the solution is decreased from 8.17 to 5.54. The potential change at the fluidic gate and passivation layer interface by bias voltages and pH are mirrored by the metal shunt, resulting in larger depletion widths under the Schottky junction and resistance change as compared to sensors with no Schottky junction. 2D numerical simulation results are in good agreement with the measured data and suggest thinner mesa with lower doping density can further increase device sensitivity.

Dimensional crossover and weak localization in a 90 nm n-GaAs thin film.

We report on the magnetotransport in a 90 nm thick n-type GaAs epitaxial thin film in the weak localization (WL) regime. Low temperature (T

Extraordinary electroconductance in metal-semiconductor hybrid structures.

We report the phenomenon of extraordinary electroconductance in microscopic metal-semiconductor hybrid structures fabricated from GaAs epitaxial layer and a Ti thin film shunt. Four-lead Van der Pauw structures show a gain of 5.2% in electroconductance under +2.5 kVcm with zero shunt bias. The increase in the sample conductance results from the thermionic field emission of electrons and the geometrical amplification. A model provides good agreement with the experimental data and clearly demonstrates the geometry dependence of the field effect in extraordinary electroconductance (EEC). The differences between EEC devices and field effect transistors, such as junction field effect transistor (FET) and Schottky barrier gate FET, are discussed.

Drastic reduction of shot noise in semiconductor superlattices.

We have found experimentally that the shot noise of the tunneling current I through an undoped semiconductor superlattice is reduced with respect to the Poissonian noise value 2eI, and that the noise approaches 1/3 of that value in superlattices whose quantum wells are strongly coupled. On the other hand, when the coupling is weak or when a strong electric field is applied to the superlattice, the noise becomes Poissonian. Although our results are qualitatively consistent with existing theories for one-dimensional multibarrier structures, the theories cannot account for the dependence of the noise on superlattice parameters that we have observed.