No abstract

Two-dimensional transition metal dichalcogenides are promising candidates for ultrathin optoelectronic devices due to their high absorption coefficients and intrinsically passivated surfaces. To maintain these near-perfect surfaces, recent research has focused on fabricating contacts that limit Fermi-level pinning at the metal-semiconductor interface. Here, we develop a new, simple procedure for transferring metal contacts that does not require aligned lithography. Using this technique, we fabricate vertical Schottky-junction WS2 solar cells, with Ag and Au as asymmetric work function contacts. Under laser illumination, we observe rectifying behavior and open-circuit voltage above 500 mV in devices with transferred contacts, in contrast to resistive behavior and open-circuit voltage below 15 mV in devices with evaporated contacts. One-sun measurements and device simulation results indicate that this metal transfer process could enable high specific power vertical Schottky-junction transition metal dichalcogenide photovoltaics, and we anticipate that this technique will lead to advances for two-dimensional devices more broadly.

Light sails propelled by radiation pressure from high-power lasers have the potential to achieve relativistic spaceflight. In order to propel a spacecraft to relativistic speeds, an ultrathin, gram-sized light sail will need to be stably accelerated by lasers with ∼MW/cm intensities operating in the near-infrared spectral range. Such a laser-driven sail requires multiband electromagnetic functionality: it must simultaneously exhibit very low absorptivity in the (Doppler-broadened) laser beam spectrum in the near-infrared and high emissivity in the mid-infrared for efficient radiative cooling. These engineering challenges present an opportunity for nanophotonic design. Here, we show that designed thin-film heterostructures could become multifunctional building-block elements of the light sail, due to their ability to achieve substantial reflectivity while maintaining low absorption in the near-infrared, significant emissivity in the mid-infrared, and a very low mass. For a light sail carrying a payload, we propose a relevant figure of merit-the reflectivity adjusted area density-that can capture the trade-off between sail mass and reflectivity, independent of other quantities such as the incident beam power, phased array size, or the payload mass. Furthermore, we present designs for effective thermal management via radiative cooling and compare propulsion efficiencies for several candidate materials, using a general approach that could apply to a broad range of high-power laser propulsion problems.

Monolayer transition-metal dichalcogenides (TMDCs) in the 2H-phase are promising semiconductors for opto-valleytronic and opto-spintronic applications because of their strong spin-valley coupling. Here, we report detailed studies of opto-valleytronic properties of heterogeneous domains in CVD-grown monolayer WS2 single crystals. By illuminating WS2 with off-resonance circularly polarized light and measuring the resulting spatially resolved circularly polarized emission (P circ), we find significantly large circular polarization (P circ up to 60% and 45% for α- and β-domains, respectively) already at 300 K, which increases to nearly 90% in the α-domains at 80 K. Studies of spatially resolved photoluminescence (PL) spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, Kelvin-probe force microscopy, and conductive atomic force microscopy reveal direct correlation among the PL intensity, defect densities, and chemical potential, with the α-domains showing lower defect densities and a smaller work function by 0.13 eV than the β-domains. This work function difference indicates the occurrence of type-two band alignments between the α- and β-domains. We adapt a classical model to explain how electronically active defects may serve as nonradiative recombination centers and find good agreement between experiments and the model. Scanning tunneling microscopic/spectroscopic (STM/STS) studies provide further evidence for tungsten vacancies (WVs) being the primary defects responsible for the suppressed PL and circular polarization in WS2. These results therefore suggest a pathway to control the opto-valleytronic properties of TMDCs by means of defect engineering.

A power-dependent relative photoluminescence measurement method is developed for double-heterostructures composed of III-V semiconductors. Analyzing the data yields insight into the radiative efficiency of the absorbing layer as a function of laser intensity. Four GaAs samples of different thicknesses are characterized, and the measured data are corrected for dependencies of carrier concentration and photon recycling. This correction procedure is described and discussed in detail in order to determine the material's Shockley-Read-Hall lifetime as a function of excitation intensity. The procedure assumes 100% internal radiative efficiency under the highest injection conditions, and we show this leads to less than 0.5% uncertainty. The resulting GaAs material demonstrates a 5.7 ± 0.5 ns nonradiative lifetime across all samples of similar doping (2–3 × 1017 cm−3) for an injected excess carrier concentration below 4 × 1012 cm−3. This increases considerably up to longer than 1 μs under high injection levels due to a trap saturation effect. The method is also shown to give insight into bulk and interface recombination.