The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led ...to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors, photovoltaic devices and so on. Here, we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light-emitting diodes (LEDs) made by stacking metallic graphene, insulating hexagonal boron nitride and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit an extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further on increasing the number of available 2D crystals and improving their electronic quality.
Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance ...of surface interactions and charging effects requiring new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping of MoS2 with SiO2 and Si(x)N(y), improving mechanical coupling of MoS2 with surrounding dielectrics. We show that the observed PL non-uniformities are related to strong variation in the local electron charging of MoS2 films. In completely encapsulated films, negative charging is enhanced leading to uniform optical properties. Observed great sensitivity of optical characteristics of 2D films to surface interactions has important implications for optoelectronics applications of layered materials.
Highly nonlinear optical materials with strong effective photon-photon interactions are required for ultrafast and quantum optical signal processing circuitry. Here we report strong Kerr-like ...nonlinearities by employing efficient optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe
at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at small photon fluxes due to phase space filling. We find the ratio of trion- to neutral exciton-polariton interaction strength is in the range from 10 to 100 in TMDC materials and that trion-polariton nonlinearity is comparable to that in other polariton systems. The results are in good agreement with a theory accounting for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. Our findings open a way to scalable quantum optics applications with TMDCs.
Integration of quasi-two-dimensional (2D) films of metal–chalcogenides in optical microcavities permits new photonic applications of these materials. Here we present tunable microcavities with ...monolayer MoS2 or few monolayer GaSe films. We observe significant modification of spectral and temporal properties of photoluminescence (PL): PL is emitted in spectrally narrow and wavelength-tunable cavity modes with quality factors up to 7400; a 10-fold PL lifetime shortening is achieved, a consequence of Purcell enhancement of the spontaneous emission rate.
The interaction of an electronic spin with its nuclear environment, an issue known as the central spin problem, has been the subject of considerable attention due to its relevance for spin-based ...quantum computation using semiconductor quantum dots. Independent control of the nuclear spin bath using nuclear magnetic resonance techniques and dynamic nuclear polarization using the central spin itself offer unique possibilities for manipulating the nuclear bath with significant consequences for the coherence and controlled manipulation of the central spin. Here we review some of the recent optical and transport experiments that have explored this central spin problem using semiconductor quantum dots. We focus on the interaction between 10(4)-10(6) nuclear spins and a spin of a single electron or valence-band hole. We also review the experimental techniques as well as the key theoretical ideas and the implications for quantum information science.
Interaction with nuclear spins leads to decoherence and information loss in solid-state electron-spin qubits. One particular, ineradicable source of electron decoherence arises from decoherence of ...the nuclear spin bath, driven by nuclear-nuclear dipolar interactions. Owing to its many-body nature nuclear decoherence is difficult to predict, especially for an important class of strained nanostructures where nuclear quadrupolar effects have a significant but largely unknown impact. Here, we report direct measurement of nuclear spin bath coherence in individual self-assembled InGaAs/GaAs quantum dots: spin-echo coherence times in the range 1.2-4.5 ms are found. Based on these values, we demonstrate that strain-induced quadrupolar interactions make nuclear spin fluctuations much slower compared with lattice-matched GaAs/AlGaAs structures. Our findings demonstrate that quadrupolar effects can potentially be used to engineer optically active III-V semiconductor spin-qubits with a nearly noise-free nuclear spin bath, previously achievable only in nuclear spin-0 semiconductors, where qubit network interconnection and scaling are challenging.
Two-dimensional transition metal dichalcogenides (TMDs) provide a unique possibility to generate and read-out excitonic valley coherence using linearly polarized light, opening the way to valley ...information transfer between distant systems. However, these excitons have short lifetimes (ps) and efficiently lose their valley coherence via the electron-hole exchange interaction. Here, we show that control of these processes can be gained by embedding a monolayer of WSe
in an optical microcavity, forming part-light-part-matter exciton-polaritons. We demonstrate optical initialization of valley coherent polariton populations, exhibiting luminescence with a linear polarization degree up to 3 times higher than displayed by bare excitons. We utilize an external magnetic field alongside selective exciton-cavity-mode detuning to control the polariton valley pseudospin vector rotation, which reaches 45° at B = 8 T. This work provides unique insight into the decoherence mechanisms in TMDs and demonstrates the potential for engineering the valley pseudospin dynamics in monolayer semiconductors embedded in photonic structures.
Strong coupling between light and the fundamental excitations of a two-dimensional electron gas (2DEG) is of foundational importance both to pure physics and to the understanding and development of ...future photonic nanotechnologies1–7. Here we study the relationship between spin polarization of a 2DEG in a monolayer semiconductor, MoSe2, and light–matter interactions modified by a zero-dimensional optical microcavity. We find pronounced spin-susceptibility of the 2DEG to simultaneously enhance and suppress trion-polariton formation in opposite photon helicities. This leads to observation of a giant effective valley Zeeman splitting for trion-polaritons (g-factor of >20), exceeding the purely trionic splitting by over five times. Going further, we observe clear effective optical nonlinearity arising from the highly nonlinear behaviour of the valley-specific strong light–matter coupling regime, and allowing all-optical tuning of the polaritonic Zeeman splitting from 4 meV to >10 meV. Our experiments lay the groundwork for engineering topological phases with true unidirectionality in monolayer semiconductors, accompanied by giant effective photonic nonlinearities rooted in many-body exciton–electron correlations.Researchers show spin-susceptibility in monolayer MoSe2 and demonstrate giant effective valley Zeeman splitting and nonlinearity for trion-polaritons.
Unique structural and optical properties of atomically thin two-dimensional semiconducting transition metal dichalcogenides enable in principle their efficient coupling to photonic cavities having ...the optical mode volume close to or below the diffraction limit. Recently, it has become possible to make all-dielectric nano-cavities with reduced mode volumes and negligible non-radiative losses. Here, we realise low-loss high-refractive-index dielectric gallium phosphide (GaP) nano-antennas with small mode volumes coupled to atomic mono- and bilayers of WSeFormula: see text. We observe a photoluminescence enhancement exceeding 10Formula: see text compared with WSeFormula: see text placed on planar GaP, and trace its origin to a combination of enhancement of the spontaneous emission rate, favourable modification of the photoluminescence directionality and enhanced optical excitation efficiency. A further effect of the coupling is observed in the photoluminescence polarisation dependence and in the Raman scattering signal enhancement exceeding 10Formula: see text. Our findings reveal dielectric nano-antennas as a promising platform for engineering light-matter coupling in two-dimensional semiconductors.
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