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Van der Waals heterostructures are synthetic quantum materials composed of stacks of atomically thin two-dimensional (2D) layers. Because the electrons in the atomically thin 2D layers are exposed to layer-to-layer coupling, the properties of van der Waals heterostructures are defined not only by the constituent monolayers, but also by the interactions between the layers. Many fascinating electrical, optical and magnetic properties have recently been reported in different types of van der Waals heterostructures. In this Review, we focus on unique excited-state dynamics in transition metal dichalcogenide (TMDC) heterostructures. TMDC monolayers are the most widely studied 2D semiconductors, featuring prominent exciton states and accessibility to the valley degree of freedom. Many TMDC heterostructures are characterized by a staggered band alignment. This band alignment has profound effects on the evolution of the excited states in heterostructures, including ultrafast charge transfer between the layers, the formation of interlayer excitons, and the existence of long-lived spin and valley polarization in resident carriers. Here we review recent experimental and theoretical efforts to elucidate electron dynamics in TMDC heterostructures, extending from timescales of femtoseconds to microseconds, and comment on the relevance of these effects for potential applications in optoelectronic, valleytronic and spintronic devices.

Interlayer excitons (ILXs) — electron–hole pairs bound across two atomically thin layered semiconductors — have emerged as attractive platforms to study exciton condensation 1 – 4 , single-photon emission and other quantum information applications 5 – 7 . Yet, despite extensive optical spectroscopic investigations 8 – 12 , critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, in a WSe 2 /MoS 2 heterostructure, we captured images of the time-resolved and momentum-resolved distribution of both of the particles that bind to form the ILX: the electron and the hole. We thereby obtain a direct measurement of both the ILX diameter of around 5.2 nm, comparable with the moiré-unit-cell length of 6.1 nm, and the localization of its centre of mass. Surprisingly, this large ILX is found pinned to a region of only 1.8 nm diameter within the moiré cell, smaller than the size of the exciton itself. This high degree of localization of the ILX is backed by Bethe–Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, allowing the formation of extended arrays of localized excitations for quantum technology. Imaging the electron and hole that bind to form interlayer excitons in a 2D moiré material enables direct measurement of its diameter and indicates the localization of its centre of mass.

Optical parametric oscillators (OPOs) have emerged as highly versatile platforms for signal processing, machine learning, and all-optical computation. In particular, integrated photonic circuits have demonstrated an efficient and scalable route to build OPO networks through time-multiplexing. However, for tasks requiring massive parallelism with low latency, spatial multiplexing with vertical micro-cavities is a more natural approach to overcome the shoreline density limits of edge-emitting photonics. To this end, we propose an approach to realizing vertical micro-cavity OPOs (VCOPOs) leveraging recent developments in micro-optical fabrication techniques. We consider thin film LiNbO3-filled dielectric micro-cavities as a case study, but the approach taken here is readily extended to any χ(2) nonlinear medium. Based on conservative industrial fabrication tolerances, we predict a minimal foot-print of ca. 5×5μm2, while achieving oscillation thresholds in the microwatts range. Advanced fabrication methods open a path toward sub-µW oscillation threshold, with a ratio of single-photon non-linear coupling rate to dissipation rate g/κ>5%. We propose a theoretical framework for the classical and quantum operation of two dimensional arrays of VCOPOs, and discuss potential applications such as surface emitting devices, spatially multi-mode parametric amplifiers and squeezers, as well as optical simulators of classical and quantum Hamiltonians.

Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically accessed and manipulated for quantum information processing. Here, we integrate MoS2 with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface Mie modes, the intensity and lifetime of the emission of neutral excitons, trions and defect bound excitons can be enhanced, while the spectral shape can be modified. Additionally, we demonstrate the symmetric enhancement of the degree-of-polarization (DOP) of neutral exciton and trions via valley-resolved PL measurements, and find that the DOP can be as high as 24% for exciton emission and 34% for trion emission at 100K. These results can be understood by analyzing the near-field impact of metasurface resonators on both the chiral absorption of MoS2 emitters as well as the enhanced emission from the Purcell effect. Combining Si-compatible photonic design with large-scale (mm-scale) 2D materials integration, our work makes an important step towards on-chip valleytronic applications approaching room-temperature operation.

The ability to induce, observe and control quantum coherent interactions in room temperature, electrically driven optoelectronic devices is of outmost significance for advancing quantum science and engineering towards practical applications. We demonstrate here a quantum interference phenomena, Ramsey fringes, in an inhomogeneously broadened InAs/InP quantum dot (QD) ensemble in the form of a 1.5 mm long optical amplifier operating at room temperature. Observation of Ramsey fringes in semiconductor QD was previously achieved only at cryogenic temperatures and only in isolated single dot systems. A high-resolution pump probe scheme where both pulses are characterized by cross frequency resolved optical gating (X-FROG) reveals a clear oscillatory behavior both in the amplitude and the instantaneous frequency of the probe pulse with a period that equals one optical cycle at operational wavelength. Using nominal input delays of 600 to 900 fs and scanning the separation around each delay in 1 fs steps, we map the evolution of the material de-coherence and extract a coherence time. Moreover we notice a unique phenomenon, which can not be observed in single dot systems, that the temporal position of the output probe pulse also oscillates with the same periodicity but with a quarter cycle delay relative to the intensity variations. This delay is the time domain manifestation of coupling between the real and imaginary parts of the complex susceptibility.

We study the interplay between coherent light-matter interactions and non-resonant pulse propagation effects when ultra-short pulses propagate in room-temperature quantum-dot (QD) semiconductor optical amplifiers (SOAs). The signatures observed on a pulse envelope after propagating in a transparent SOA, when coherent Rabi-oscillations are absent, highlight the contribution of two-photon absorption (TPA), and its accompanying Kerr-like effect, as well as of linear dispersion, to the modification of the pulse complex electric field profile. These effects are incorporated into our previously developed finite-difference time-domain comprehensive model that describes the interaction between the pulses and the QD SOA. The present, generalized, model is used to investigate the combined effect of coherent and non-resonant phenomena in the gain and absorption regimes of the QD SOA. It confirms that in the QD SOA we examined, linear dispersion in the presence of the Kerr-like effect causes pulse compression, which counteracts the pulse peak suppression due to TPA, and also modifies the patterns which the coherent Rabi-oscillations imprint on the pulse envelope under both gain and absorption conditions. The inclusion of these effects leads to a better fit with experiments and to a better understanding of the interplay among the various mechanisms so as to be able to better analyze more complex future experiments of coherent light-matter interaction induced by short pulses propagating along an SOA.

Quantum coherent light-matter interactions have been at the forefront of scientific interest since the fundamental predictions of Einstein and the later work of Rabi. Direct observation of quantum coherent interactions entails probing the electronic wavefunction which requires that the electronic state of the matter does not de-phase during the measurement, a condition that can be satisfied by lengthening the coherence time or by shortening the observation time. The short de-phasing time in semiconductors has dictated that all coherent effects reported to date have been recorded directly only at cryogenic temperatures. Here we report on the first direct electronic wavefunction probing in a room-temperature semiconductor. Employing an ultrafast characterization scheme we have demonstrated Rabi oscillations and self-induced transparency in an electrically driven, room-temperature semiconductor laser amplifier, revealing the most intimate details of the light-matter interactions seen to date. The ability to employ quantum effects in solid-state media, which operate at elevated temperatures, will finally bring true quantum mechanical concepts into the realm of practical devices.

We demonstrate the Ramsey analogous experiment known as coherent control, taking place along an electrically-driven semiconductor optical amplifier operating at room temperature.

Interlayer excitons (ILXs) - electron-hole pairs bound across two atomically thin layered semiconductors - have emerged as attractive platforms to study exciton condensation, single-photon emission and other quantum-information applications. Yet, despite extensive optical spectroscopic investigations, critical information about their size, valley configuration and the influence of the moiré potential remains unknown. Here, we captured images of the time- and momentum-resolved distribution of both the electron and the hole that bind to form the ILX in a WSe2/MoS2 heterostructure. We thereby obtain a direct measurement of the interlayer exciton diameter of ~5.4 nm, comparable to the moiré unit-cell length of 6.1 nm. Surprisingly, this large ILX is well localized within the moiré cell to a region of only 1.8 nm - smaller than the size of the exciton itself. This high degree of localization of the interlayer exciton is backed by Bethe-Salpeter equation calculations and demonstrates that the ILX can be localized within small moiré unit cells. Unlike large moiré cells, these are uniform over large regions, thus allowing the formation of extended arrays of localized excitations for quantum technology.

We demonstrate the ability to control quantum coherent Rabi-oscillations in a room-temperature quantum dot semiconductor optical amplifier (SOA) by shaping the light pulses that trigger them. The experiments described here show that when the excitation is resonant with the short wavelength slope of the SOA gain spectrum, a linear frequency chirp affects its ability to trigger Rabi-oscillations within the SOA: A negative chirp inhibits Rabi-oscillations whereas a positive chirp can enhance them, relative to the interaction of a transform limited pulse. The experiments are confirmed by a numerical calculation that models the propagation of the experimentally shaped pulses through the SOA.