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Transition metal dichalcogenides (TMDCs) have attracted significant attention for optoelectronic, photovoltaic and photoelectrochemical applications. The properties of TMDCs are highly dependent on the number of stacked atomic layers, which is usually counted post-fabrication, using a combination of optical methods and atomic force microscopy (AFM) height measurements. Here, we use photoluminescence spectroscopy and three different AFM methods to demonstrate significant discrepancies in height measurements of exfoliated MoSe$_2$ flakes on SiO$_2$ depending on the method used. We highlight that overlooking effects from electrostatic forces, contaminants and surface binding can be misleading when measuring the height of a MoSe$_2$ flake. These factors must be taken into account as a part of the protocol for counting TMDC layers.
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Interfacing atomically thin van der Waals semiconductors with magnetic substrates enables additional control on their intrinsic valley degree of freedom and provides a promising platform for the development of novel valleytronic devices for information processing and storage. Here we study circularly polarized photoluminescence in heterostructures of monolayer MoSe$_2$ and thin films of ferrimagnetic bismuth iron garnet. We observe strong emission from charged excitons with negative valley polarization, which switches sign with increasing temperature, and demonstrate contrasting response to left and right circularly polarized excitation, associated with finite out-of-plane magnetization in the substrate. We propose a theoretical model accounting for magnetization-induced imbalance of charge carriers in the two valleys of MoSe$_2$, as well as for valley-switching scattering from B to A excitons and fast formation of trions with extended valley relaxation times, which shows excellent agreement with the experimental data. Our results provide new insights into valley physics in 2D semiconductors interfaced with magnetic substrates.
Nanoplasmonic systems combined with optically-active two-dimensional materials provide intriguing opportunities to explore and control light-matter interactions at extreme sub-wavelength lengthscales approaching the exciton Bohr radius. Here, we present room- and cryogenic-temperature investigations of light-matter interactions between an MoSe$_2$ monolayer and individual lithographically defined gold dipole nanoantennas having sub-10 nm feed gaps. By progressively tuning the nanoantenna size, their dipolar resonance is tuned relative to the A-exciton transition in a proximal MoSe$_2$ monolayer achieving a total tuning of $sim 130;mathrm{meV}$. Differential reflectance measurements performed on $> 100$ structures reveal an apparent avoided crossing between exciton and dipolar mode and an exciton-plasmon coupling constant of $g= 55;mathrm{meV}$, representing $g/(hbaromega_X)geq3%$ of the transition energy. This places our hybrid system in the intermediate-coupling regime where spectra exhibit a characteristic Fano-like shape, indicative of the interplay between pronounced light-matter coupling and significant damping. We also demonstrate active control of the optical response by varying the polarization of the excitation light to programmably suppress coupling to the dipole mode. We further study the emerging optical signatures of the monolayer localized at dipole nanoantennas at $10;mathrm{K}$. Our findings represent a key step towards realizing non-linear photonic devices based on 2D materials with potential for low-energy and ultrafast performance.
Excitons in atomically-thin semiconductors interact very strongly with electromagnetic radiation and are necessarily close to a surface. Here, we exploit the deep-subwavelength confinement of surface plasmon polaritons (SPPs) at the edge of a metal-insulator-metal plasmonic waveguide and their proximity of 2D excitons in an adjacent atomically thin semiconductor to build an ultra-compact photodetector. When subject to far-field excitation we show that excitons are created throughout the dielectric gap region of our waveguide and converted to free carriers primarily at the anode of our device. In the near-field regime, strongly confined SPPs are launched, routed and detected in a 20nm narrow region at the interface between the waveguide and the monolayer semiconductor. This leads to an ultra-compact active detector region of only ~0.03$mu m ^2$ that absorbs 86% of the propagating energy in the SPP. Due to the electromagnetic character of the SPPs, the spectral response is essentially identical to the far-field regime, exhibiting strong resonances close to the exciton energies. While most of our experiments are performed on monolayer thick MoSe$_2$, the photocurrent-per-layer increases super linearly in multilayer devices due to the suppression of radiative exciton recombination. These results demonstrate an integrated device for nanoscale routing and detection of light with the potential for on-chip integration at technologically relevant, few-nanometer length scales.
Neutral and charged excitons (trions) in atomically-thin materials offer important capabilities for photonics, from ultrafast photodetectors to highly-efficient light-emitting diodes and lasers. Recent studies of van der Waals (vdW) heterostructures comprised of dissimilar monolayer materials have uncovered a wealth of optical phenomena that are predominantly governed by interlayer interactions. Here, we examine the optical properties in NbSe$_2$ - MoSe$_2$ vdW heterostructures, which provide an important model system to study metal-semiconductor interfaces, a common element in optoelectronics. Through low-temperature photoluminescence (PL) microscopy we discover a sharp emission feature, L1, that is localized at the NbSe$_2$-capped regions of MoSe$_2$. L1 is observed at energies below the commonly-studied MoSe$_2$ excitons and trions, and exhibits temperature- and power-dependent PL consistent with exciton localization in a confining potential. Remarkably, L1 is very robust not just in different samples, but also under a variety of fabrication processes. Using first-principles calculations we reveal that the confinement potential required for exciton localization naturally arises from the in-plane band bending due to the changes in the electron affinity between pristine MoSe$_2$ and NbSe$_2$ - MoSe$_2$ heterostructure. We discuss the implications of our studies for atomically-thin optoelectronics devices with atomically-sharp interfaces and tunable electronic structures.
Semiconductors require stable doping for applications in transistors, optoelectronics, and thermoelectrics. However, this has been challenging for two-dimensional (2D) materials, where existing approaches are either incompatible with conventional semiconductor processing or introduce time-dependent, hysteretic behavior. Here we show that low temperature (< 200$^circ$ C) sub-stoichiometric AlO$_x$ provides a stable n-doping layer for monolayer MoS$_2$, compatible with circuit integration. This approach achieves carrier densities > 2x10$^{13}$ 1/cm$^2$, sheet resistance as low as ~7 kOhm/sq, and good contact resistance ~480 Ohm.um in transistors from monolayer MoS$_2$ grown by chemical vapor deposition. We also reach record current density of nearly 700 uA/um (>110 MA/cm$^2$) in this three-atom-thick semiconductor while preserving transistor on/off current ratio > $10^6$. The maximum current is ultimately limited by self-heating and could exceed 1 mA/um with better device heat sinking. With their 0.1 nA/um off-current, such doped MoS$_2$ devices approach several low-power transistor metrics required by the international technology roadmap
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