Direct Patterning of Optoelectronic Nanostructures Using Encapsulated Layered Transition Metal Dichalcogenides.

Direct top-down nanopatterning of semiconductors is a powerful tool for engineering properties of optoelectronic devices. Translating this approach to two-dimensional semiconductors such as monolayer transition metal dichalcogenides (TMDs) is challenging because of both the small scales required for confinement and the degradation of electronic and optical properties caused by high-energy and high-dose electron radiation used for high-resolution top-down direct electron beam patterning. We show that encapsulating a TMD monolayer with hexagonal boron nitride preserves the narrow exciton linewidths and emission intensity typical in such heterostructures after electron beam lithography, allowing direct patterning of functional optical monolayer nanostructures on scales of a few tens of nanometers. We leverage this fabrication method to study size-dependent effects on nanodot arrays of MoS2 and MoSe2 as well as laterally confined electrical transport devices, demonstrating the potential of top-down lithography for nanoscale TMD optoelectronics.

Valley-selective optical Stark effect of exciton-polaritons in a monolayer semiconductor.

Selective breaking of degenerate energy levels is a well-known tool for coherent manipulation of spin states. Though most simply achieved with magnetic fields, polarization-sensitive optical methods provide high-speed alternatives. Exploiting the optical selection rules of transition metal dichalcogenide monolayers, the optical Stark effect allows for ultrafast manipulation of valley-coherent excitons. Compared to excitons in these materials, microcavity exciton-polaritons offer a promising alternative for valley manipulation, with longer lifetimes, enhanced valley coherence, and operation across wider temperature ranges. Here, we show valley-selective control of polariton energies in WS2 using the optical Stark effect, extending coherent valley manipulation to the hybrid light-matter regime. Ultrafast pump-probe measurements reveal polariton spectra with strong polarization contrast originating from valley-selective energy shifts. This demonstration of valley degeneracy breaking at picosecond timescales establishes a method for coherent control of valley phenomena in exciton-polaritons.

Electrical Control of Circular Photogalvanic Spin-Valley Photocurrent in a Monolayer Semiconductor.

In a monolayer transition metal dichalcogenide (TMDC) that lacks structural inversion symmetry, spin degeneracy is lifted by strong spin-orbit coupling, and a distinctive spin-valley locking allows for the creation of valley-locked spin-polarized carriers with a circularly polarized optical excitation. When excited carriers also have net in-plane momentum, spin-polarized photocurrents can be generated at ambient temperature without magnetic fields or materials. The behavior of these spin-polarized photocurrents in monolayer TMDC remains largely unexplored. In this work, we demonstrate the tuning of spin-valley photocurrent generated from the circularly polarized photogalvanic effect in monolayer MoS2, including magnitude and polarization degree, by purely electric means at room temperature. The magnitude of spin-polarized photocurrent can be modulated up to 45 times larger, and the polarization degree of the total photocurrent can be tuned significantly (here from 0.5 to 16.6%) by gate control. Combined with the atomic thickness and wafer-scale growth capabilities of monolayer TMDC, the efficient electrical tuning of spin-valley photocurrent suggests a pathway to achieve spin-logic processing by local gate architectures in monolayer opto-spintronic devices.

Size-tunable Lateral Confinement in Monolayer Semiconductors.

Three-dimensional confinement allows semiconductor quantum dots to exhibit size-tunable electronic and optical properties that enable a wide range of opto-electronic applications from displays, solar cells and bio-medical imaging to single-electron devices. Additional modalities such as spin and valley properties in monolayer transition metal dichalcogenides provide further degrees of freedom requisite for information processing and spintronics. In nanostructures, however, spatial confinement can cause hybridization that inhibits the robustness of these emergent properties. Here, we show that laterally-confined excitons in monolayer MoS2 nanodots can be created through top-down nanopatterning with controlled size tunability. Unlike chemically-exfoliated monolayer nanoparticles, the lithographically patterned monolayer semiconductor nanodots down to a radius of 15 nm exhibit the same valley polarization as in a continuous monolayer sheet. The inherited bulk spin and valley properties, the size dependence of excitonic energies, and the ability to fabricate MoS2 nanostructures using semiconductor-compatible processing suggest that monolayer semiconductor nanodots have potential to be multimodal building blocks of integrated optoelectronics and spintronics systems.

Coherent optical non-reciprocity in axisymmetric resonators.

We describe an approach to optical non-reciprocity that exploits the local helicity of evanescent electric fields in axisymmetric resonators. By interfacing an optical cavity to helicity-sensitive transitions, such as Zeeman levels in a quantum dot, light transmission through a waveguide becomes direction-dependent when the state degeneracy is lifted. Using a linearized quantum master equation, we analyze the configurations that exhibit non-reciprocity, and we show that reasonable parameters from existing cavity QED experiments are sufficient to demonstrate a coherent non-reciprocal optical isolator operating at the level of a single photon.