The electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties are reviewed. Recent advances in the development of atomically thin layers of van der Waals bonded solids have opened up new possibilities for the exploration of 2D physics as well as for materials for applications. Among them, semiconductor transition metal dichalcogenides, MX2 (M = Mo, W; X = S, Se), have bandgaps in the near-infrared to the visible region, in contrast to the zero bandgap of graphene. In the monolayer limit, these materials have been shown to possess direct bandgaps, a property well suited for photonics and optoelectronics applications. Here, we review the electronic and optical properties and the recent progress in applications of 2D semiconductor transition metal dichalcogenides with emphasis on strong excitonic effects, and spin- and valley-dependent properties.

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides

Semiconductor technology is currently based on the manipulation of electronic charge; however, electrons have additional degrees of freedom, such as spin and valley, that can be used to encode and process information. Over the past several decades, there has been significant progress in manipulating electron spin for semiconductor spintronic devices, motivated by potential spin-based information processing and storage applications. However, experimental progress towards manipulating the valley degree of freedom for potential valleytronic devices has been limited until very recently. We review the latest advances in valleytronics, which have largely been enabled by the isolation of 2D materials (such as graphene and semiconducting transition metal dichalcogenides) that host an easily accessible electronic valley degree of freedom, allowing for dynamic control. The energy extrema of an electronic band are referred to as valleys. In 2D materials, two distinguishable valleys can be used to encode information and explore other valleytronic applications.

Valleytronics in 2D materials

This Review summarizes recent progress of single-photon emitters based on defects in solids and highlights new research directions. The photophysical properties of single-photon emitters and efforts towards scalable system integration are also discussed.

Solid-state single-photon emitters

Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here recent progress in understanding of the excitonic properties in monolayer TMDs is reviewed and future challenges are laid out. Discussed are the consequences of the strong direct and exchange Coulomb interaction, exciton light-matter coupling, and influence of finite carrier and electron-hole pair densities on the exciton properties in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.

Colloquium : Excitons in atomically thin transition metal dichalcogenides

Magnetism, originating from the moving charges and spin of elementary particles, has revolutionized important technologies such as data storage and biomedical imaging, and continues to bring forth new phenomena in emergent materials and reduced dimensions. The recently discovered two-dimensional (2D) magnetic van der Waals crystals provide ideal platforms for understanding 2D magnetism, the control of which has been fueling opportunities for atomically thin, flexible magneto-optic and magnetoelectric devices (such as magnetoresistive memories and spin field-effect transistors). The seamless integration of 2D magnets with dissimilar electronic and photonic materials opens up exciting possibilities for unprecedented properties and functionalities. We review the progress in this area and identify the possible directions for device applications, which may lead to advances in spintronics, sensors, and computing.

Two-dimensional magnetic crystals and emergent heterostructure devices

Zero-dimensional photonic quantum emitters can be realized using defects in the two-dimensional dichalcogenides.

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Optically active quantum dots in monolayer WSe2.

Charge carriers in transition metal dichalcogenides have an extra degree of freedom known as valley pseudospin, which is associated with the shape of the energy bands. Experiments show that this pseudospin can be manipulated using magnetic fields.

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Valley Zeeman effect in elementary optical excitations of monolayer WSe2

Cavity spectroscopy measurements elucidate the Fermi polaron nature of the optical excitations in monolayer transition metal dichalcogenides. The dynamics of a mobile quantum impurity in a degenerate Fermi system is a fundamental problem in many-body physics. The interest in this field has been renewed due to recent ground-breaking experiments with ultracold Fermi gases1,2,3,4,5. Optical creation of an exciton or a polariton in a two-dimensional electron system embedded in a microcavity constitutes a new frontier for this field due to an interplay between cavity coupling favouring ultralow-mass polariton formation6 and exciton–electron interactions leading to polaron or trion formation7,8. Here, we present cavity spectroscopy of gate-tunable monolayer MoSe2 (ref. 9) exhibiting strongly bound trion and polaron resonances, as well as non-perturbative coupling to a single microcavity mode10,11. As the electron density is increased, the oscillator strength determined from the polariton splitting is gradually transferred from the higher-energy repulsive exciton-polaron resonance to the lower-energy attractive exciton-polaron state. Simultaneous observation of polariton formation in both attractive and repulsive branches indicates a new regime of polaron physics where the polariton impurity mass can be much smaller than that of the electrons. Our findings shed new light on optical response of semiconductors in the presence of free carriers by identifying the Fermi polaron nature of excitonic resonances and constitute a first step in investigation of a new class of degenerate Bose–Fermi mixtures12,13.

Fermi polaron-polaritons in charge-tunable atomically thin semiconductors

Semiconductor quantum dots have emerged as promising candidates for implementation of quantum information processing since they allow for a quantum interface between stationary spin qubits and propagating single photons. In the meanwhile, transition metal dichalcogenide (TMD) monolayers have moved to the forefront of solid-state research due to their unique band structure featuring a large band gap with degenerate valleys and non-zero Berry curvature. Here we report the observation of quantum dots in monolayer tungsten-diselenide with an energy that is 20 to 100 meV lower than that of two dimensional excitons. Photon antibunching in second-order photon correlations unequivocally demonstrates the zero-dimensional anharmonic nature of these quantum emitters. The strong anisotropic magnetic response of the spatially localized emission peaks strongly indicates that radiative recombination stems from localized excitons that inherit their electronic properties from the host TMD. The large $\sim$ 1 meV zero-field splitting shows that the quantum dots have singlet ground states and an anisotropic confinement most likely induced by impurities or defects in the host TMD. Electrical control in van der Waals heterostructures and robust spin-valley degree of freedom render TMD quantum dots promising for quantum information processing.

Optically Active Quantum Dots in Monolayer WSe$_2$

For applications exploiting the valley pseudospin degree of freedom in transition metal dichalcogenide monolayers, efficient preparation of electrons or holes in a single valley is essential. Here, we show that a magnetic field of 7 T leads to a near-complete valley polarization of electrons in a MoSe_{2} monolayer with a density 1.6×10^{12}  cm^{-2}; in the absence of exchange interactions favoring single-valley occupancy, a similar degree of valley polarization would have required a pseudospin g factor of 38. To investigate the magnetic response, we use polarization resolved photoluminescence as well as resonant reflection measurements. In the latter, we observe gate voltage dependent transfer of oscillator strength from the exciton to the attractive Fermi polaron: stark differences in the spectrum of the two light helicities provide a confirmation of valley polarization. Our findings suggest an interaction induced giant paramagnetic response of MoSe_{2}, which paves the way for valleytronics applications.

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Meinrad Sidler

Papers

Optically active quantum dots in monolayer WSe2.

Valley Zeeman effect in elementary optical excitations of monolayer WSe2

Fermi polaron-polaritons in charge-tunable atomically thin semiconductors

Optically Active Quantum Dots in Monolayer WSe$_2$

Giant Paramagnetism-Induced Valley Polarization of Electrons in Charge-Tunable Monolayer MoSe 2