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.
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.
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.
The various decay mechanisms of excitons in cuprous oxide (Cu 2 O) are highly sensitive to defects which can relax selection rules. Here we report cryogenic hyperspectral imaging of exciton luminescence from cuprous oxide crystals grown via the floating zone method showing the samples have few defects. Some locations, however, show strain splitting of the 1s orthoexciton triplet polariton luminescence. Strain is reduced by annealing. In addition, annealing causes annihilation of oxygen and copper vacancies, which leads to a negative correlation between luminescence of unlike vacancies.
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.
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