Layered materials as a platform for quantum technologies.

Layered materials are taking centre stage in the ever-increasing research effort to develop material platforms for quantum technologies. We are at the dawn of the era of layered quantum materials. Their optical, electronic, magnetic, thermal and mechanical properties make them attractive for most aspects of this global pursuit. Layered materials have already shown potential as scalable components, including quantum light sources, photon detectors and nanoscale sensors, and have enabled research of new phases of matter within the broader field of quantum simulations. In this Review we discuss opportunities and challenges faced by layered materials within the landscape of material platforms for quantum technologies. In particular, we focus on applications that rely on light-matter interfaces.

Identification of Exciton Complexes in Charge-Tunable Janus WSeS Monolayers.

Janus transition-metal dichalcogenide monolayers are artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>18 meV) spectra obfuscating their specific excitonic origin. Here, we identify the neutral and the negatively charged inter- and intravalley exciton transitions in Janus WSeS monolayers with ∼6 meV optical line widths. We integrate Janus monolayers into vertical heterostructures, allowing doping control. Magneto-optic measurements indicate that monolayer WSeS has a direct bandgap at the K points. Our results pave the way for applications such as nanoscale sensing, which relies on resolving excitonic energy shifts, and the development of Janus-based optoelectronic devices, which requires charge-state control and integration into vertical heterostructures.

Reaching the Excitonic Limit in 2D Janus Monolayers by In Situ Deterministic Growth.

Named after the two-faced Roman god of transitions, transition metal dichalcogenide (TMD) Janus monolayers have two different chalcogen surfaces, inherently breaking the out-of-plane mirror symmetry. The broken mirror symmetry and the resulting potential gradient lead to the emergence of quantum properties such as the Rashba effect and the formation of dipolar excitons. Experimental access to these quantum properties, however, hinges on the ability to produce high-quality 2D Janus monolayers. Here, these results introduce a holistic 2D Janus synthesis technique that allows real-time monitoring of the growth process. This prototype chamber integrates in situ spectroscopy, offering fundamental insights into the structural evolution and growth kinetics, that allow the evaluation and optimization of the quality of Janus monolayers. The versatility of this method is demonstrated by synthesizing and monitoring the conversion of SWSe, SNbSe, and SMoSe Janus monolayers. Deterministic conversion and real-time data collection further aid in conversion of exfoliated TMDs to Janus monolayers and unparalleled exciton linewidth values are reached, compared to the current best standard. The results offer an insight into the process kinetics and aid in the development of new Janus monolayers with high optical quality, which is much needed to access their exotic properties.

Transform-Limited Photons From a Coherent Tin-Vacancy Spin in Diamond.

Solid-state quantum emitters that couple coherent optical transitions to long-lived spin qubits are essential for quantum networks. Here we report on the spin and optical properties of individual tin-vacancy (SnV) centers in diamond nanostructures. Through cryogenic magneto-optical and spin spectroscopy, we verify the inversion-symmetric electronic structure of the SnV, identify spin-conserving and spin-flipping transitions, characterize transition linewidths, measure electron spin lifetimes, and evaluate the spin dephasing time. We find that the optical transitions are consistent with the radiative lifetime limit even in nanofabricated structures. The spin lifetime is phonon limited with an exponential temperature scaling leading to T_{1}>10 ms, and the coherence time, T_{2}^{*} reaches the nuclear spin-bath limit upon cooling to 2.9 K. These spin properties exceed those of other inversion-symmetric color centers for which similar values require millikelvin temperatures. With a combination of coherent optical transitions and long spin coherence without dilution refrigeration, the SnV is a promising candidate for feasable and scalable quantum networking applications.

Charge-tuneable biexciton complexes in monolayer WSe2.

Monolayer transition metal dichalcogenides have strong Coulomb-mediated many-body interactions. Theoretical studies have predicted the existence of numerous multi-particle excitonic states. Two-particle excitons and three-particle trions have been identified by their optical signatures. However, more complex states such as biexcitons have been elusive due to limited spectral quality of the optical emission. Here, we report direct evidence of two biexciton complexes in monolayer tungsten diselenide: the four-particle neutral biexciton and the five-particle negatively charged biexciton. We distinguish these states by power-dependent photoluminescence and demonstrate full electrical switching between them. We determine the band states of the elementary particles comprising the biexcitons through magneto-optical spectroscopy. We also resolve a splitting of 2.5 meV for the neutral biexciton, which we attribute to the fine structure, providing reference for subsequent studies. Our results unveil the nature of multi-exciton complexes in transitionmetal dichalcogenides and offer direct routes towards deterministic control in many-body quantum phenomena.

Large-scale quantum-emitter arrays in atomically thin semiconductors.

Quantum light emitters have been observed in atomically thin layers of transition metal dichalcogenides. However, they are found at random locations within the host material and usually in low densities, hindering experiments aiming to investigate this new class of emitters. Here, we create deterministic arrays of hundreds of quantum emitters in tungsten diselenide and tungsten disulphide monolayers, emitting across a range of wavelengths in the visible spectrum (610-680 nm and 740-820 nm), with a greater spectral stability than their randomly occurring counterparts. This is achieved by depositing monolayers onto silica substrates nanopatterned with arrays of 150-nm-diameter pillars ranging from 60 to 190 nm in height. The nanopillars create localized deformations in the material resulting in the quantum confinement of excitons. Our method may enable the placement of emitters in photonic structures such as optical waveguides in a scalable way, where precise and accurate positioning is paramount.