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The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb-bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe 2 crystals exhibit electric-field-driven coupling with the ground (1s) and excited states (2s) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to 0.73 ± 0.01 enm), high energy tunability (up to ~200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from -4 to +14). Further, we observe the bi- and tri-layer excited state (2s) interlayer excitons and their coupling with the intralayer excitons states (1s and 2s). Our results, in good agreement with a coupled oscillator model with spin (layer)-selectivity and beyond standard density functional theory calculations, promote multilayer 2H-MoSe 2 as a highly tunable platform to explore exciton-exciton interactions with strong light-matter interactions., (© 2024. The Author(s).)

Abstract: Interlayer excitons (IXs), composed of electron and hole states localized in different layers, excel in bilayers composed of atomically thin van der Waals materials such as semiconducting transition-metal dichalcogenides (TMDs) due to drastically enlarged exciton binding energies, exciting spin-valley properties, elongated lifetimes, and large permanent dipoles. The latter allows modification by electric fields and the study of thermalized bosonic quasiparticles, from the single particle level to interacting degenerate dense ensembles. Additionally, the freedom to combine bilayers of different van der Waals materials without lattice or relative twist-angle constraints leads to layer-hybridized and Moiré excitons, which can be widely engineered. This article covers fundamental aspects of IXs, including correlation phenomena as well as the consequence of Moiré superlattices with a strong focus on TMD homo- and heterobilayers., Competing Interests: Conflict of interestThere is no conflict of interest., (© The Author(s) 2024.)

Magnetism in two-dimensional (2D) van der Waals (vdW) materials has recently emerged as one of the most promising areas in condensed matter research, with many exciting emerging properties and significant potential for applications ranging from topological magnonics to low-power spintronics, quantum computing, and optical communications. In the brief time after their discovery, 2D magnets have blossomed into a rich area for investigation, where fundamental concepts in magnetism are challenged by the behavior of spins that can develop at the single layer limit. However, much effort is still needed in multiple fronts before 2D magnets can be routinely used for practical implementations. In this comprehensive review, prominent authors with expertise in complementary fields of 2D magnetism ( i.e. , synthesis, device engineering, magneto-optics, imaging, transport, mechanics, spin excitations, and theory and simulations) have joined together to provide a genome of current knowledge and a guideline for future developments in 2D magnetic materials research.

Moiré patterns with a superlattice potential can be formed by vertically stacking two layered materials with a relative twist or lattice constant mismatch. In transition metal dichalcogenide-based systems, the moiré potential landscape can trap interlayer excitons (IXs) at specific atomic registries. Here, we report that spatially isolated trapped IXs in a molybdenum diselenide/tungsten diselenide heterobilayer device provide a sensitive optical probe of carrier filling in their immediate environment. By mapping the spatial positions of individual trapped IXs, we are able to spectrally track the emitters as the moiré lattice is filled with excess carriers. Upon initial doping of the heterobilayer, neutral trapped IXs form charged IXs (IX trions) uniformly with a binding energy of ~7 meV. Upon further doping, the empty superlattice sites sequentially fill, creating a Coulomb staircase: stepwise changes in the IX trion emission energy due to Coulomb interactions with carriers at nearest-neighbour moiré sites. This non-invasive, highly local technique can complement transport and non-local optical sensing techniques to characterize Coulomb interaction energies, visualize charge correlated states, or probe local disorder in a moiré superlattice., (© 2021. The Author(s).)

Efficient on-chip integration of single-photon emitters imposes a major bottleneck for applications of photonic integrated circuits in quantum technologies. Resonantly excited solid-state emitters are emerging as near-optimal quantum light sources, if not for the lack of scalability of current devices. Current integration approaches rely on cost-inefficient individual emitter placement in photonic integrated circuits, rendering applications impossible. A promising scalable platform is based on two-dimensional (2D) semiconductors. However, resonant excitation and single-photon emission of waveguide-coupled 2D emitters have proven to be elusive. Here, we show a scalable approach using a silicon nitride photonic waveguide to simultaneously strain-localize single-photon emitters from a tungsten diselenide (WSe 2 ) monolayer and to couple them into a waveguide mode. We demonstrate the guiding of single photons in the photonic circuit by measuring second-order autocorrelation of g (2) (0) = 0.150 ± 0.093 and perform on-chip resonant excitation, yielding a g (2) (0) = 0.377 ± 0.081. Our results are an important step to enable coherent control of quantum states and multiplexing of high-quality single photons in a scalable photonic quantum circuit., Competing Interests: The authors declare no competing financial interest., (© 2021 The Authors. Published by American Chemical Society.)

We characterize the coherent dynamics of a two-level quantum emitter driven by a pair of symmetrically detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum emission, enabling background-free photon extraction from the emitter. While excitation is not possible without spectral overlap between the exciting pulse and the quantum emitter transition for ideal two-level systems due to cancellation of the accumulated pulse area, we find that any additional interactions that interfere with cancellation of the accumulated pulse area may lead to a finite stationary population inversion. Our spectroscopic results of a solid-state two-level system show that, while coupling to lattice vibrations helps to improve the inversion efficiency up to 50% under symmetric driving, coherent population control and a larger amount of inversion are possible using asymmetric dichromatic excitation, which we achieve by adjusting the ratio of the intensities between the red- and blue-detuned pulses. Our measured results, supported by simulations using a real-time path-integral method, offer a new perspective toward realizing efficient, background-free photon generation and extraction.

Photon antibunching, a hallmark of quantum light, has been observed in the correlations of light from isolated atomic and atomic-like solid-state systems. Two-dimensional semiconductor heterostructures offer a unique method to create a quantum light source: Moiré trapping potentials for excitons are predicted to create arrays of quantum emitters. While signatures of moiré-trapped excitons have been observed, their quantum nature has yet to be confirmed. Here, we report photon antibunching from single moiré-trapped interlayer excitons in a heterobilayer. Via magneto-optical spectroscopy, we demonstrate that the discrete anharmonic spectra arise from bound band-edge electron-hole pairs trapped in moiré potentials. Last, we exploit the large permanent dipole of interlayer excitons to achieve large direct current (DC) Stark tuning up to 40 meV. Our results confirm the quantum nature of moiré-confined excitons and open opportunities to investigate their inhomogeneity and interactions between the emitters or energetically tune single emitters into resonance with cavity modes., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution License 4.0 (CC BY).)

Van der Waals heterostructures offer attractive opportunities to design quantum materials. For instance, transition metal dichalcogenides (TMDs) possess three quantum degrees of freedom: spin, valley index and layer index. Furthermore, twisted TMD heterobilayers can form moiré patterns that modulate the electronic band structure according to the atomic registry, leading to spatial confinement of interlayer excitons (IXs). Here we report the observation of spin-layer locking of IXs trapped in moiré potentials formed in a heterostructure of bilayer 2H-MoSe 2 and monolayer WSe 2 . The phenomenon of locked electron spin and layer index leads to two quantum-confined IX species with distinct spin-layer-valley configurations. Furthermore, we observe that the atomic registries of the moiré trapping sites in the three layers are intrinsically locked together due to the 2H-type stacking characteristic of bilayer TMDs. These results identify the layer index as a useful degree of freedom to engineer tunable few-level quantum systems in two-dimensional heterostructures.

Van der Waals materials offer a wide range of atomic layers with unique properties that can be easily combined to engineer novel electronic and photonic devices. A missing ingredient of the van der Waals platform is a two-dimensional crystal with naturally occurring out-of-plane luminescent dipole orientation. Here we measure the far-field photoluminescence intensity distribution of bulk InSe and two-dimensional InSe, WSe 2 and MoSe 2 . We demonstrate, with the support of ab-initio calculations, that layered InSe flakes sustain luminescent excitons with an intrinsic out-of-plane orientation, in contrast with the in-plane orientation of dipoles we find in two-dimensional WSe 2 and MoSe 2 at room-temperature. These results, combined with the high tunability of the optical response and outstanding transport properties, position layered InSe as a promising semiconductor for novel optoelectronic devices, in particular for hybrid integrated photonic chips which exploit the out-of-plane dipole orientation.

Gate-tunable quantum-mechanical tunnelling of particles between a quantum confined state and a nearby Fermi reservoir of delocalized states has underpinned many advances in spintronics and solid-state quantum optics. The prototypical example is a semiconductor quantum dot separated from a gated contact by a tunnel barrier. This enables Coulomb blockade, the phenomenon whereby electrons or holes can be loaded one-by-one into a quantum dot 1,2 . Depending on the tunnel-coupling strength 3,4 , this capability facilitates single spin quantum bits 1,2,5 or coherent many-body interactions between the confined spin and the Fermi reservoir 6,7 . Van der Waals (vdW) heterostructures, in which a wide range of unique atomic layers can easily be combined, offer novel prospects to engineer coherent quantum confined spins 8,9 , tunnel barriers down to the atomic limit 10 or a Fermi reservoir beyond the conventional flat density of states 11 . However, gate-control of vdW nanostructures 12-16 at the single particle level is needed to unlock their potential. Here we report Coulomb blockade in a vdW heterostructure consisting of a transition metal dichalcogenide quantum dot coupled to a graphene contact through an atomically thin hexagonal boron nitride (hBN) tunnel barrier. Thanks to a tunable Fermi reservoir, we can deterministically load either a single electron or a single hole into the quantum dot. We observe hybrid excitons, composed of localized quantum dot states and delocalized continuum states, arising from ultra-strong spin-conserving tunnel coupling through the atomically thin tunnel barrier. Probing the charged excitons in applied magnetic fields, we observe large gyromagnetic ratios (∼8). Our results establish a foundation for engineering next-generation devices to investigate either novel regimes of Kondo physics or isolated quantum bits in a vdW heterostructure platform.

The particular optical and electronic properties recently reported for 2D InSe depict this 2D material as being very versatile for future electronic and optoelectronic devices with tunable and optimized functionalities. For its fundamental study and the development of practical applications, rapid and accurate identification methods of atomically thin InSe are essential. Here, we demonstrate an enhancement of the optical contrast between InSe nanosheets and the underlying SiO 2 /Si substrate by illuminating with a 40 nm wide bandpass filter centered at 500 nm. Moreover, we study the optical contrast of 2D InSe on transparent substrates. Our results suggest that a good optical contrast is achieved for transparent substrates with low real refractive indices such as LiF or a viscoelastic polydimethylsiloxane stamp. In this case, an optimum optical contrast would be achieved by using a bandpass filter centered at 450 nm. These results can be very useful for speeding up the continuously growing research on 2D InSe and its applications.

Manipulating properties of matter at the nanoscale is the essence of nanotechnology, which has enabled the realization of quantum dots, nanotubes, metamaterials, and two-dimensional materials with tailored electronic and optical properties. Two-dimensional semiconductors have revealed promising perspectives in nanotechnology. However, the tunability of their physical properties is challenging for semiconductors studied until now. Here we show the ability of morphological manipulation strategies, such as nanotexturing or, at the limit, important surface roughness, to enhance light absorption and the luminescent response of atomically thin indium selenide nanosheets. Besides, quantum-size confinement effects make this two-dimensional semiconductor to exhibit one of the largest band gap tunability ranges observed in a two-dimensional semiconductor: from infrared, in bulk material, to visible wavelengths, at the single layer. These results are relevant for the design of new optoelectronic devices, including heterostructures of two-dimensional materials with optimized band gap functionalities and in-plane heterojunctions with minimal junction defect density.