Search

Emergent strongly-correlated electronic phenomena in atomically-thin transition metal dichalcogenides are an exciting frontier in condensed matter physics, with examples ranging from bilayer superconductivity~\cite{zhao2023evidence} and electronic Wigner crystals~\cite{smolenski2021signatures,zhou2021bilayer} to the ongoing quest for exciton condensation~\cite{wang2019evidence,ma2021strongly,shi2022bilayer}. Here, we experimentally investigate the properties of indirect excitons in naturally-grown MoS$_2$-homobilayer, integrated in a dual-gate device structure allowing independent control of the electron density and out-of-plane electric field. Under conditions when electron tunneling between the layers is negligible~\cite{pisoni2019absence}, upon electron doping the sample, we observe that the two excitons with opposing dipoles hybridize, displaying unusual behavior distinct from both conventional level crossing and anti-crossing. We show that these observations can be explained by static random coupling between the excitons, which increases with electron density and decreases with temperature. We argue that this phenomenon is indicative of a spatially fluctuating order parameter in the form of interlayer electron coherence, a theoretically predicted many-body state~\cite{zheng1997exchange} that has yet to be unambiguously established experimentally outside of the quantum Hall regime~\cite{sarma2008perspectives,spielman2000resonantly,kellogg2004vanishing,kellogg2002observation,spielman2001observation,fertig1989energy,shi2022bilayer}. Implications of our findings for future experiments and quantum optics applications are discussed.

Excitons in transition metal dichalcogenides (TMDs) have emerged as a promising platform for novel applications ranging from optoelectronic devices to quantum optics and solid state quantum simulators. While much progress has been made towards characterizing and controlling excitons in TMDs, manipulating their properties during the course of their lifetime - a key requirement for many optoelectronic device and information processing modalities - remains an outstanding challenge. Here we combine long-lived interlayer excitons in angle-aligned MoSe$_2$/WSe$_2$ heterostructures with fast electrical control to realize dynamical control schemes, in which exciton properties are not predetermined at the time of excitation but can be dynamically manipulated during their lifetime. Leveraging the out-of-plane exciton dipole moment, we use electric fields to demonstrate dynamical control over the exciton emission wavelength. Moreover, employing a patterned gate geometry, we demonstrate rapid local sample doping and toggling of the radiative decay rate through exciton-charge interactions during the exciton lifetime. Spatially mapping the exciton response reveals charge redistribution, offering a novel probe of electronic transport in twisted TMD heterostructures. Our results establish the feasibility of dynamical exciton control schemes, unlocking new directions for exciton-based information processing and optoelectronic devices, and the realization of excitonic phenomena in TMDs., Comment: 37 pages, 4 figures in main text, 6 figures in supplemental materials; (v2) corrected funding acknowledgements

A mirror twin boundary (MTB) in a transition metal dichalcogenide (TMD) monolayer can host one-dimensional electron liquid of a topological nature with tunable interactions. Unfortunately, the electrical characterization of such boundaries has been challenging due to the paucity of samples with large enough size and high quality. Here, we report an epitaxial growth of monolayer molybdenum disulfide (MoS$_2$) bicrystals with well-isolated MTBs that are tens of micrometers long. Conductance measurements of these MTBs exhibit power-law behaviors as a function of temperature and bias voltage up to room temperature, consistent with electrons tunneling into a Luttinger liquid. Transport measurements of two distinct types of MTBs reveal the critical role of the atomic-scale defects. This study demonstrates that MTBs in TMD monolayers provide an exciting new platform for studying the interplay between electronic interactions and topology.

Strongly interacting electronic systems possess rich phase diagrams resulting from the competition between different quantum ground states. A general mechanism that relieves this frustration is the emergence of microemulsion phases, where regions of different phase self-organize across multiple length scales. The experimental characterization of these phases often poses significant challenges, as the long-range Coulomb interaction microscopically mingles the competing states. Here, we use cryogenic reflectance and magneto-optical spectroscopy to observe the signatures of the mixed state between an electronic Wigner crystal and an electron liquid in a MoSe2 monolayer. We find that the transit into this 'microemulsion' state is marked by anomalies in exciton reflectance, spin susceptibility, and Umklapp scattering, establishing it as a distinct phase of electronic matter. Our study of the two-dimensional electronic microemulsion phase elucidates the physics of novel correlated electron states with strong Coulomb interactions.

Atomically thin semiconductor heterostructures provide a two-dimensional (2D) device platform for creating high densities of cold, controllable excitons. Interlayer excitons (IEs), bound electrons and holes localized to separate 2D quantum well layers, have permanent out-of-plane dipole moments and long lifetimes, allowing their spatial distribution to be tuned on demand. Here, we employ electrostatic gates to trap IEs and control their density. By electrically modulating the IE Stark shift, electron-hole pair concentrations above $2\times10^{12}$ cm$^{-2}$ can be achieved. At this high IE density, we observe an exponentially increasing linewidth broadening indicative of an IE ionization transition, independent of the trap depth. This runaway threshold remains constant at low temperatures, but increases above 20 K, consistent with the quantum dissociation of a degenerate IE gas. Our demonstration of the IE ionization in a tunable electrostatic trap represents an important step towards the realization of dipolar exciton condensates in solid-state optoelectronic devices., Comment: 14 pages, 4 main figures, 1 extended data figure

A key challenge in realizing practical quantum networks for long-distance quantum communication involves robust entanglement between quantum memory nodes connected via fiber optical infrastructure. Here, we demonstrate a two-node quantum network composed of multi-qubit registers based on silicon-vacancy (SiV) centers in nanophotonic diamond cavities integrated with a telecommunication (telecom) fiber network. Remote entanglement is generated via the cavity-enhanced interactions between the SiV's electron spin qubits and optical photons. Serial, heralded spin-photon entangling gate operations with time-bin qubits are used for robust entanglement of separated nodes. Long-lived nuclear spin qubits are used to provide second-long entanglement storage and integrated error detection. By integrating efficient bi-directional quantum frequency conversion of photonic communication qubits to telecom frequencies (1350 nm), we demonstrate entanglement of two nuclear spin memories through 40 km spools of low-loss fiber and a 35 km long fiber loop deployed in the Boston area urban environment, representing an enabling step towards practical quantum repeaters and large-scale quantum networks., Comment: 23 pages, 16 figures

Efficient nanophotonic devices are essential for applications in quantum networking, optical information processing, sensing, and nonlinear optics. Extensive research efforts have focused on integrating two-dimensional (2D) materials into photonic structures, but this integration is often limited by size and material quality. Here, we use hexagonal boron nitride (hBN), a benchmark choice for encapsulating atomically thin materials, as a waveguiding layer while simultaneously improving the optical quality of the embedded films. When combined with photonic inverse design, it becomes a complete nanophotonic platform to interface with optically active 2D materials. Grating couplers and low-loss waveguides provide optical interfacing and routing, tunable cavities provide a large exciton-photon coupling to transition metal dichalcogenides (TMD) monolayers through Purcell enhancement, and metasurfaces enable the efficient detection of TMD dark excitons. This work paves the way for advanced 2D-material nanophotonic structures for classical and quantum nonlinear optics.

Ferroic orders describe spontaneous polarization of spin, charge, and lattice degrees of freedom in materials. Materials featuring multiple ferroic orders, known as multiferroics, play important roles in multi-functional electrical and magnetic device applications. 2D materials with honeycomb lattices offer exciting opportunities to engineer unconventional multiferroicity, where the ferroic orders are driven purely by the orbital degrees of freedom but not electron spin. These include ferro-valleytricity corresponding to the electron valley and ferro-orbital-magnetism supported by quantum geometric effects. Such orbital multiferroics could offer strong valley-magnetic couplings and large responses to external fields-enabling device applications such as multiple-state memory elements, and electric control of valley and magnetic states. Here we report orbital multiferroicity in pentalayer rhombohedral graphene using low temperature magneto-transport measurements. We observed anomalous Hall signals Rxy with an exceptionally large Hall angle (tan{\Theta}H > 0.6) and orbital magnetic hysteresis at hole doping. There are four such states with different valley polarizations and orbital magnetizations, forming a valley-magnetic quartet. By sweeping the gate electric field E we observed a butterfly-shaped hysteresis of Rxy connecting the quartet. This hysteresis indicates a ferro-valleytronic order that couples to the composite field E\cdot B, but not the individual fields. Tuning E would switch each ferroic order independently, and achieve non-volatile switching of them together. Our observations demonstrate a new type of multiferroics and point to electrically tunable ultra-low power valleytronic and magnetic devices.

Practical quantum networks require interfacing quantum memories with existing channels and systems that operate in the telecom band. Here we demonstrate low-noise, bidirectional quantum frequency conversion that enables a solid-state quantum memory to directly interface with telecom-band systems. In particular, we demonstrate conversion of visible-band single photons emitted from a silicon-vacancy (SiV) center in diamond to the telecom O-band, maintaining low noise ($g^2(0)<0.1$) and high indistinguishability ($V=89\pm8\%$). We further demonstrate the utility of this system for quantum networking by converting telecom-band time-bin pulses, sent across a lossy and noisy 50 km deployed fiber link, to the visible band and mapping their quantum states onto a diamond quantum memory with fidelity $\mathcal{F}=87\pm 2.5 \% $. These results demonstrate the viability of SiV quantum memories integrated with telecom-band systems for scalable quantum networking applications., Comment: 9 pages, 5 figures + Supplemental Materials

Rhombohedral stacked multilayer graphene is an ideal platform to search for correlated electron phenomena, due to its pair of flat bands touching at zero energy and further tunability by an electric field. Furthermore, its valley-dependent Berry phase at zero energy points to possible topological states when the pseudospin symmetry is broken by electron correlation. However, experimental explorations of these opportunities are very limited so far, due to a lack of devices with optimized layer numbers and configurations. Here we present electron transport measurements of hBN-encapsulated pentalayer graphene at down to 100 milli-Kelvin. We observed a correlated insulating state with >MOhm resistance at zero charge density and zero displacement field, where the tight-binding calculation predicts a metallic ground state. By increasing the displacement field, we observed a Chern insulator state with C = -5 and two other states with C = -3 at a low magnetic field of ~1 Tesla. At high displacement fields and charge densities, we observed isospin-polarized quarter- and half-metals. Therefore, rhombohedral-stacked pentalayer graphene is the first graphene system to exhibit two different types of Fermi-surface instabilities: driven by a pair of flat bands touching at zero energy, and by the Stoner mechanism in a single flat band. Our results demonstrate a new direction to explore intertwined electron correlation and topology phenomena in natural graphitic materials without the need of moir\'e superlattice engineering.

Dynamical decoupling techniques constitute an integral part of many quantum sensing platforms, often leading to orders-of-magnitude improvements in coherence time and sensitivity. Most AC sensing sequences involve a periodic echo-like structure, in which the target signal is synchronized with the echo period. We show that for strongly interacting systems, this construction leads to a fundamental sensitivity limit associated with imperfect interaction decoupling. We present a simple physical picture demonstrating the origin of this limitation, and further formalize these considerations in terms of concise higher-order decoupling rules. We then show how these limitations can be surpassed by identifying a novel sequence building block, in which the signal period matches twice the echo period. Using these decoupling rules and the resulting sequence building block, we experimentally demonstrate significant improvements in dynamical decoupling timescales and magnetic field sensitivity, opening the door for new applications in quantum sensing and quantum many-body physics., Comment: 5 pages, 3 figures, see accompanying paper "Higher-Order Methods for Hamiltonian Engineering Pulse Sequence Design" for details on Hamiltonian engineering techniques

Understanding the microscopic mechanisms of thermalization in closed quantum systems is among the key challenges in modern quantum many-body physics. We demonstrate a method to probe local thermalization in a large-scale many-body system by exploiting its inherent disorder, and use this to uncover the thermalization mechanisms in a three-dimensional, dipolar-interacting spin system with tunable interactions. Utilizing advanced Hamiltonian engineering techniques to explore a range of spin Hamiltonians, we observe a striking change in the characteristic shape and timescale of local correlation decay as we vary the engineered exchange anisotropy. We show that these observations originate from the system's intrinsic many-body dynamics and reveal the signatures of conservation laws within localized clusters of spins, which do not readily manifest using global probes. Our method provides an exquisite lens into the tunable nature of local thermalization dynamics, and enables detailed studies of scrambling, thermalization and hydrodynamics in strongly-interacting quantum systems., Comment: 6 pages, 4 figures main text

Long-distance quantum communication and networking require quantum memory nodes with efficient optical interfaces and long memory times. We report the realization of an integrated two-qubit network node based on silicon-vacancy centers (SiVs) in diamond nanophotonic cavities. Our qubit register consists of the SiV electron spin acting as a communication qubit and the strongly coupled 29Si nuclear spin acting as a memory qubit with a quantum memory time exceeding two seconds. By using a highly strained SiV with suppressed electron spin-phonon interactions, we realize electron-photon entangling gates at elevated temperatures up to 1.5 K and nucleus-photon entangling gates up to 4.3 K. Finally, we demonstrate efficient error detection in nuclear spin-photon gates by using the electron spin as a flag qubit, making this platform a promising candidate for scalable quantum repeaters., Comment: 24 pages, 19 figures

We demonstrate quantum logic enhanced sensitivity for a macroscopic ensemble of solid-state, hybrid two-qubit sensors. We achieve a factor of 30 improvement in signal-to-noise ratio, translating to a sensitivity enhancement exceeding an order of magnitude. Using the electronic spins of nitrogen vacancy (NV) centers in diamond as sensors, we leverage the on-site nitrogen nuclear spins of the NV centers as memory qubits, in combination with homogeneous bias and control fields, ensuring that all of the ${\sim}10^9$ two-qubit sensors are sufficiently identical to permit global control of the NV ensemble spin states. We find quantum logic sensitivity enhancement for multiple measurement protocols with varying optimal sensing intervals, including XY8 dynamical decoupling and correlation spectroscopy, using a synthetic AC magnetic field. The results are independent of the nature of the target signal and broadly applicable to metrology using NV centers and other solid-state ensembles. This work provides a benchmark for macroscopic ensembles of quantum sensors that employ quantum logic or quantum error correction algorithms for enhanced sensitivity., Comment: 7 pages, 5 figures; Supplemental: 4 pages, 3 figures

An efficient, scalable source of shaped single photons that can be directly integrated with optical fiber networks and quantum memories is at the heart of many protocols in quantum information science. We demonstrate a deterministic source of arbitrarily temporally shaped single-photon pulses with high efficiency (detection efficiency = 14.9%) and purity ($g^{(2)}(0) = 0.0168$) and streams of up to 11 consecutively detected single photons using a silicon-vacancy center in a highly directional fiber-integrated diamond nanophotonic cavity. Combined with previously demonstrated spin-photon entangling gates, this system enables on-demand generation of streams of correlated photons such as cluster states and could be used as a resource for robust transmission and processing of quantum information.

Techniques to mold the flow of light on subwavelength scales enable fundamentally new optical systems and device applications. The realization of programmable, active optical systems with fast, tunable components is among the outstanding challenges in the field. Here, we experimentally demonstrate a few-pixel beam steering device based on electrostatic gate control of excitons in an atomically thin semiconductor with strong light-matter interactions. By combining the high reflectivity of a MoSe2 monolayer with a graphene split-gate geometry, we shape the wavefront phase profile to achieve continuously tunable beam deflection with a range of 10$^\circ$, two-dimensional beam steering, and switching times down to 1.6 nanoseconds. Our approach opens the door for a new class of atomically thin optical systems, such as rapidly switchable beam arrays and quantum metasurfaces operating at their fundamental thickness limit.

Solid-state quantum emitters are promising candidates for the realization of quantum networks, owing to their long-lived spin memories, high-fidelity local operations, and optical connectivity for long-range entanglement. However, due to differences in local environment, solid-state emitters typically feature a range of distinct transition frequencies, which makes it challenging to create optically mediated entanglement between arbitrary emitter pairs. We propose and demonstrate an efficient method for entangling emitters with optical transitions separated by many linewidths. In our approach, electro-optic modulators enable a single photon to herald a parity measurement on a pair of spin qubits. We experimentally demonstrate the protocol using two silicon-vacancy center sin a diamond nanophotonic cavity, with optical transitions separated by 7.4 GHz. Working with distinguishable emitters allows for individual qubit addressing and readout, enabling parallel control and entanglement of both co-located and spatially separated emitters, a key step towards scaling up quantum information processing systems, Comment: 6 pages and 3 figures. Supplementary material, 13 pages and 13 figures, is available at the end of the manuscript

Monolayers of transition metal dichalcogenides (TMDs) have recently emerged as a promising optoelectronic platform. To leverage their full potential, however, it is important to understand and engineer the properties of the different exciton species that exist in these monolayers, as well as to control their transport through the material. A promising approach relies on engineering strain landscapes in atomically thin semiconductors that excitons navigate. In WSe$_2$ monolayers, for example, localized strain has been used to control the emission wavelength of excitons, induce exciton funneling and conversion, and even realize single-photon sources and quantum dots. Before these phenomena can be fully leveraged for applications, including quantum information processing, the details of excitons' interaction with the strain landscape must be well understood. To address this, we have developed a cryogenic technique capable of probing the dynamics of both bright and dark excitons in nanoscale strain landscapes in TMDs. In our approach, a nanosculpted tapered optical fiber is used to simultaneously generate strain and probe the near-field optical response of WSe$_2$ monolayers at 5 K. When the monolayer is pushed by the fiber, its lowest energy photoluminescence (PL) peaks red shift by as much as 390 meV, (corresponding to 20% of the bandgap of an unstrained WSe$_2$ monolayer). The red-shifting peaks are polarized perpendicularly to the WSe$_2$ plane and have long rising times (10 ps) and lifetimes (52 ps), indicating that they originate from nominally spin-forbidden dark excitons. Taken together, these observations indicate that dark excitons are funneled to the high-strain regions during their long lifetime and are the principal participants in drift and diffusion at cryogenic temperatures. Our work elucidates the important role that dark excitons play in locally strained WSe$_2$., Comment: 19 pages, 4 figures

Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Transition metal dichalcogenides (TMDs), with their large spin-orbit coupling, have been of special interest for valleytronic applications for their coupling of circularly polarized light to excitons with selective valley and spin$^{1-4}$. In atomically thin MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructures, the unique atomic registry of vdW layers provides a quasi-angular momentum to interlayer excitons$^{5,6}$, enabling emission from otherwise dark spin triplet excitons. Here, we report electrically tunable spin singlet and triplet exciton emission from atomically aligned TMD heterostructures. We confirm the spin configurations of the light-emitting excitons employing magnetic fields to measure effective exciton g-factors. The interlayer tunneling current across the TMD vdW heterostructure enables the electrical generation of singlet and triplet exciton emission in this atomically thin PN junction. We demonstrate electrically tunability between the singlet and triplet excitons that are generated by charge injection. Atomically thin TMD heterostructure light emitting diodes thus enables a route for optoelectronic devices that can configure spin and valley quantum states independently by controlling the atomic stacking registry., Comment: Extended work of previous study: arXiv:1912.07678

A Wigner crystal, a regular electron lattice arising from strong correlation effects, is one of the earliest predicted collective electronic states. This many-body state exhibits quantum and classical phase transitions and has been proposed as a basis for quantum information processing applications. In semiconductor platforms, two-dimensional Wigner crystals have been observed under magnetic field or moir\'e-based lattice potential where the electron kinetic energy is strongly suppressed. Here, we report bilayer Wigner crystal formation without a magnetic or confinement field in atomically thin MoSe$_2$ bilayers separated by hexagonal boron nitride. We observe optical signatures of robust correlated insulating states formed at symmetric (1:1) and asymmetric (4:1 and 7:1) electron doping of the two MoSe$_2$ layers at cryogenic temperatures. We attribute these features to the bilayer Wigner crystals formed from two commensurate triangular electron lattices in each layer, stabilized via inter-layer interaction. These bilayer Wigner crystal phases are remarkably stable and undergo quantum and thermal melting transitions above a critical electron density of up to $6 \times10^{12}$ cm$^{-2}$ and at temperatures of ~40 K. Our results demonstrate that atomically thin semiconductors provide a promising new platform for realizing strongly correlated electronic states, probing their electronic and magnetic phase transitions, and developing novel applications in quantum electronics and optoelectronics., Comment: 4 figures

Optically-probed nitrogen-vacancy (NV) quantum defects in diamond can detect nuclear magnetic resonance (NMR) signals with high-spectral resolution from micron-scale sample volumes of about 10 picoliters. However, a key challenge for NV-NMR is detecting samples at millimolar concentrations. Here, we demonstrate an improvement in NV-NMR proton concentration sensitivity of about $10^5$ over thermal polarization by hyperpolarizing sample proton spins through signal amplification by reversible exchange (SABRE), enabling micron-scale NMR of small molecule sample concentrations as low as 1 millimolar in picoliter volumes. The SABRE-enhanced NV-NMR technique may enable detection and chemical analysis of low concentration molecules and their dynamics in complex micron-scale systems such as single-cells., Comment: 5 pages, 4 figures

Understanding the coordination of cell division timing is one of the outstanding questions in the field of developmental biology. One active control parameter of the cell cycle duration is temperature, as it can accelerate or decelerate the rate of biochemical reactions. However, controlled experiments at the cellular-scale are challenging due to the limited availability of biocompatible temperature sensors as well as the lack of practical methods to systematically control local temperatures and cellular dynamics. Here, we demonstrate a method to probe and control the cell division timing in Caenorhabditis elegans embryos using a combination of local laser heating and nanoscale thermometry. Local infrared laser illumination produces a temperature gradient across the embryo, which is precisely measured by in-vivo nanoscale thermometry using quantum defects in nanodiamonds. These techniques enable selective, controlled acceleration of the cell divisions, even enabling an inversion of division order at the two cell stage. Our data suggest that the cell cycle timing asynchrony of the early embryonic development in C. elegans is determined independently by individual cells rather than via cell-to-cell communication. Our method can be used to control the development of multicellular organisms and to provide insights into the regulation of cell division timings as a consequence of local perturbations., Comment: 6+6 pages, 4+9 figures

Structural engineering of van der Waals heterostructures via stacking and twisting has recently been used to create moir\'e superlattices, enabling the realization of new optical and electronic properties in solid-state systems. In particular, moir\'e lattices in twisted bilayers of transition metal dichalcogenides (TMDs) have been shown to lead to exciton trapping, host Mott insulating and superconducting states, and act as unique Hubbard systems whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures also feature atomic reconstruction and domain formation. Unfortunately, due to the nanoscale sizes (~10 nm) of typical moir\'e domains, the effects of atomic reconstruction on the electronic and excitonic properties of these heterostructures could not be investigated systematically and have often been ignored. Here, we use near-0$^o$ twist angle MoSe$_2$/MoSe$_2$ bilayers with large rhombohedral AB/BA domains to directly probe excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane (z) electric dipole moments in opposite directions. The dipole orientation of ground-state $\Gamma$-K interlayer excitons (X$_{I,1}$) can be flipped with electric fields, while higher-energy K-K interlayer excitons (X$_{I,2}$) undergo field-asymmetric hybridization with intralayer K-K excitons (X$_0$). Our study reveals the profound impacts of crystal symmetry on TMD excitons and points to new avenues for realizing topologically nontrivial systems, exotic metasurfaces, collective excitonic phases, and quantum emitter arrays via domain-pattern engineering., Comment: 29 pages, 4 figures in main text, 6 figures in supplementary information

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe$_2$/WSe$_2$ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than three orders of magnitude via electrostatic doping, enabling switching of the DOCP from ~80% in the n-doped regime to <5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom., Comment: 31 pages, 4 figures in main text, 5 figures in supplemental materials

Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular momentum to interlayer excitons, enabling emission from otherwise dark spin-triplet excitons. Employing magnetic field, we show that photons emitted by triplet and singlet excitons in the same valley have opposite chirality. We also measure effective exciton g-factors, presenting direct and quantitative evidence of triplet interlayer excitons. We further demonstrate gate tuning of the relative photoluminescence intensity between singlet and triplet charged excitons. Electrically controlled emission between singlet and triplet excitons enables a route for optoelectronic devices that can configure excitonic chiral, spin, and valley quantum states.

The optical and electronic properties of van der Waals (vdW) heterostructures depend strongly on the atomic stacking order of the constituent layers. This is exemplified by periodic variation of the local atomic registry, known as moire patterns, giving rise to superconductivity and ferromagnetism in twisted bilayer graphene and novel exciton states in transition metal dichalcogenides (TMD) heterobilayers. However, the presence of the nanometer-scale moire superlattices is typically deduced indirectly, because conventional imaging techniques, such as transmission electron microscopy (TEM), require special sample preparation that is incompatible with most optical and transport measurements. Here, we demonstrate a method that uses a secondary electron microscope to directly image the local stacking order in fully hexagonal boron nitride (hBN) encapsulated, gated vdW heterostructure devices on standard Si-substrates. Using this method, we demonstrate imaging of reconstructed moire patterns in stacked TMDs, ABC/ABA stacking order in graphene multilayers, and AB/BA boundaries in bilayer graphene. Furthermore, we show that the technique is non-destructive, thus unlocking the possibility of directly correlating local stacking order with optical and electronic properties, crucial to the development of vdW heterostructure devices with precisely controlled functionality.

Moir\'e superlattices in twisted van der Waals materials constitute a promising platform for engineering electronic and optical properties. However, a major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate the local moir\'e structure with optical properties. By using a recently developed scanning electron microscopy technique to image twisted WSe$_2$/WSe$_2$ bilayers, we directly correlate increasing moir\'e periodicity with the emergence of two distinct exciton species. These can be tuned individually through electrostatic gating, and feature different valley coherence properties. Our observations can be understood as resulting from an array of two intralayer exciton species residing in alternating locations in the superlattice, and illuminate the influence of the moir\'e potential on lateral exciton motion. They open up new avenues for controlling exciton arrays in twisted TMDs, with applications in quantum optoelectronics and explorations of novel many body systems., Comment: 25 pages, 4 figures in main text, 4 figures in supplementary materials

The ability to communicate quantum information over long distances is of central importance in quantum science and engineering. For example, it enables secure quantum key distribution (QKD) relying on fundamental principles that prohibit the "cloning" of unknown quantum states. While QKD is being successfully deployed, its range is currently limited by photon losses and cannot be extended using straightforward measure-and-repeat strategies without compromising its unconditional security. Alternatively, quantum repeaters, which utilize intermediate quantum memory nodes and error correction techniques, can extend the range of quantum channels. However, their implementation remains an outstanding challenge, requiring a combination of efficient and high-fidelity quantum memories, gate operations, and measurements. Here we report the experimental realization of memory-enhanced quantum communication. We use a single solid-state spin memory integrated in a nanophotonic diamond resonator to implement asynchronous Bell-state measurements. This enables a four-fold increase in the secret key rate of measurement device independent (MDI)-QKD over the loss-equivalent direct-transmission method while operating megahertz clock rates. Our results represent a significant step towards practical quantum repeaters and large-scale quantum networks., Comment: 6 pages and 4 figures. Supplementary material, 9 pages and 5 figures, is available at the end of the manuscript

Quantum metrology makes use of coherent superpositions to detect weak signals. While in principle the sensitivity can be improved by increasing the density of sensing particles, in practice this improvement is severely hindered by interactions between them. Using a dense ensemble of interacting electronic spins in diamond, we demonstrate a novel approach to quantum metrology. It is based on a new method of robust quantum control, which allows us to simultaneously eliminate the undesired effects associated with spin-spin interactions, disorder and control imperfections, enabling a five-fold enhancement in coherence time compared to conventional control sequences. Combined with optimal initialization and readout protocols, this allows us to break the limit for AC magnetic field sensing imposed by interactions, opening a promising avenue for the development of solid-state ensemble magnetometers with unprecedented sensitivity., Comment: 7 + 34 pages, 4 + 10 figures. V2: Improved sensitivity number and presentation

The growth of single crystals of MoS2 and WS2 by materials transport through a liquid salt flux made from a low melting mixture of NaCl and CsCl is described. The crystals are characterized by single crystal X-ray diffraction, which reveals that they are 2H-MoS2 with a small percentage (about 3%) of 3R intergrowths. The 2H-WS2 crystals display less than 1% of 3R intergrowths. Photoluminescence spectra of exfoliated monolayers suggest that MoS2 grown by this method has superior crystallinity in comparison to commercially-available MoS2 crystals., Comment: 24 pages, 8 figures. SI: 4 tables

We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photonic density of states in a controllable and reversible fashion, we show that both the absorption and emission properties of the excitons can be dynamically modulated. This electromechanical control over exciton dynamics in a mechanically flexible, atomically thin semiconductor opens up new avenues in cavity quantum optomechanics, nonlinear quantum optics, and topological photonics., Comment: accepted version

Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral interlayer excitons across the whole sample that can be controlled by excitation power and gate electrodes. We also realize the drift motion of charged interlayer excitons using Ohmic-contacted devices. The electrical generation and control of excitons provides a new route for realizing quantum manipulation of bosonic composite particles with complete electrical tunability.

The nitrogen vacancy (NV) center in diamond exhibits spin-dependent fluorescence and long spin coherence times under ambient conditions, enabling applications in quantum information processing and sensing. NV centers near the surface can have strong interactions with external materials and spins, enabling new forms of nanoscale spectroscopy. However, NV spin coherence degrades within 100 nanometers of the surface, suggesting that diamond surfaces are plagued with ubiquitous defects. Prior work on characterizing near-surface noise has primarily relied on using NV centers themselves as probes; while this has the advantage of exquisite sensitivity, it provides only indirect information about the origin of the noise. Here we demonstrate that surface spectroscopy methods and single spin measurements can be used as complementary diagnostics to understand sources of noise. We find that surface morphology is crucial for realizing reproducible chemical termination, and use these insights to achieve a highly ordered, oxygen-terminated surface with suppressed noise. We observe NV centers within 10 nm of the surface with coherence times extended by an order of magnitude.

Nuclear magnetic resonance (NMR) spectroscopy is a widely used tool for chemical analysis and molecular structure identification. Because it typically relies on the weak magnetic fields produced by a small thermal nuclear spin polarization, NMR suffers from poor molecule-number sensitivity compared to other analytical techniques. Recently, a new class of NMR sensors based on optically-probed nitrogen-vacancy (NV) quantum defects in diamond have allowed molecular spectroscopy from sample volumes several orders of magnitude smaller than the most sensitive inductive detectors. To date, however, NV-NMR spectrometers have only been able to observe signals from pure, highly concentrated samples. To overcome this limitation, we introduce a technique that combines picoliter-scale NV-NMR with fully integrated Overhauser dynamic nuclear polarization (DNP) to perform high-resolution spectroscopy on a variety of small molecules in dilute solution, with femtomole sensitivity. Our technique advances mass-limited NMR spectroscopy for drug and natural product discovery, catalysis research, and single cell studies.

Photon-mediated interactions between quantum systems are essential for realizing quantum networks and scalable quantum information processing. We demonstrate such interactions between pairs of silicon-vacancy (SiV) color centers strongly coupled to a diamond nanophotonic cavity. When the optical transitions of the two color centers are tuned into resonance, the coupling to the common cavity mode results in a coherent interaction between them, leading to spectrally-resolved superradiant and subradiant states. We use the electronic spin degrees of freedom of the SiV centers to control these optically-mediated interactions. Our experiments pave the way for implementation of cavity-mediated quantum gates between spin qubits and for realization of scalable quantum network nodes., Comment: 8 pages and 4 figures. Supplementary Material, 23 pages and 9 figures, available as an ancillary file

We demonstrate a synchronized readout (SR) technique for spectrally selective detection of oscillating magnetic fields with sub-millihertz resolution, using coherent manipulation of solid state spins. The SR technique is implemented in a sensitive magnetometer (~50 picotesla/Hz^(1/2)) based on nitrogen vacancy (NV) centers in diamond, and used to detect nuclear magnetic resonance (NMR) signals from liquid-state samples. We obtain NMR spectral resolution ~3 Hz, which is nearly two orders of magnitude narrower than previously demonstrated with NV based techniques, using a sample volume of ~1 picoliter. This is the first application of NV-detected NMR to sense Boltzmann-polarized nuclear spin magnetization, and the first to observe chemical shifts and J-couplings.

Transition metal dichalcogenide monolayers are promising candidates for exploring new electronic and optical phenomena and for realizing atomically thin optoelectronic devices. They host tightly bound electron-hole pairs (excitons) that can be efficiently excited by resonant light fields. Here, we demonstrate that a single monolayer of molybdenum diselenide (MoSe2) can dramatically modify light transmission near the excitonic resonance, acting as an electrically switchable mirror that reflects up to 85% of incident light at cryogenic temperatures. This high reflectance is a direct consequence of the excellent coherence properties of excitons in this atomically thin semiconductor, encapsulated by hexagonal boron nitride. Furthermore, we show that the MoSe2 monolayer exhibits power- and wavelength-dependent nonlinearities that stem from exciton-based lattice heating in the case of continuous-wave excitation and exciton-exciton interactions when fast, pulsed laser excitation is used. These observations open up new possibilities for studying quantum nonlinear optical phenomena and topological photonics, and for miniaturizing optical devices., Comment: 4 figures

Transition metal dichalcogenide (TMD) monolayers are direct bandgap semiconductors that feature tightly bound excitons, strong spin-orbit coupling, and spin-valley degrees of freedom. Depending on the spin configuration of the electron-hole pairs, intra-valley excitons of TMD monolayers can be either optically bright or dark. Dark excitons involve nominally spin-forbidden optical transitions with zero in-plane transition dipole moment, making their detection with conventional far-field optical techniques challenging. Here, we introduce a new method for probing the optical properties of two-dimensional (2D) materials via near-field coupling to surface plasmon polaritons (SPPs), which selectively enhances optical transitions with dipole moments normal to the 2D plane. We utilize this method to directly detect dark excitons in monolayer TMDs. When a WSe2 monolayer is placed on top of a single-crystal silver film, its emission into near-field-coupled SPPs displays new spectral features whose energies and dipole orientations are consistent with dark neutral and charged excitons. The SPP-based near-field spectroscopy significantly enhances experimental capabilities for probing and manipulating exciton dynamics of atomically thin materials., Comment: 4 figures

We demonstrate a quantum nanophotonics platform based on germanium-vacancy (GeV) color centers in fiber-coupled diamond nanophotonic waveguides. We show that GeV optical transitions have a high quantum efficiency and are nearly lifetime-broadened in such nanophotonic structures. These properties yield an efficient interface between waveguide photons and a single GeV without the use of a cavity or slow-light waveguide. As a result, a single GeV center reduces waveguide transmission by $18 \pm 1\%$ on resonance in a single pass. We use a nanophotonic interferometer to perform homodyne detection of GeV resonance fluorescence. By probing the photon statistics of the output field, we demonstrate that the GeV-waveguide system is nonlinear at the single-photon level., Comment: 5 pages and 5 figures. Supplemental Material, 4 pages and 1 figure, available as an ancillary file

Efficient interfaces between photons and quantum emitters form the basis for quantum networks and enable nonlinear optical devices operating at the single-photon level. We demonstrate an integrated platform for scalable quantum nanophotonics based on silicon-vacancy (SiV) color centers coupled to nanoscale diamond devices. By placing SiV centers inside diamond photonic crystal cavities, we realize a quantum-optical switch controlled by a single color center. We control the switch using SiV metastable orbital states and verify optical switching at the single-photon level by using photon correlation measurements. We use Raman transitions to realize a single-photon source with a tunable frequency and bandwidth in a diamond waveguide. Finally, we create entanglement between two SiV centers by detecting indistinguishable Raman photons emitted into a single waveguide. Entanglement is verified using a novel superradiant feature observed in photon correlation measurements, paving the way for the realization of quantum networks., Comment: 15 pages and 5 figures. Supplementary Material, 36 pages and 10 figures, available as an ancillary file

We demonstrate a robust experimental method for determining the depth of individual shallow Nitrogen-Vacancy (NV) centers in diamond with $\sim1$ nm uncertainty. We use a confocal microscope to observe single NV centers and detect the proton nuclear magnetic resonance (NMR) signal produced by objective immersion oil, which has well understood nuclear spin properties, on the diamond surface. We determine the NV center depth by analyzing the NV NMR data using a model that describes the interaction of a single NV center with the statistically-polarized proton spin bath. We repeat this procedure for a large number of individual, shallow NV centers and compare the resulting NV depths to the mean value expected from simulations of the ion implantation process used to create the NV centers, with reasonable agreement.

We demonstrate a method of magnetic resonance imaging with single nuclear-spin sensitivity under ambient conditions. It employs a network of isolated electronic-spin quantum bits (qubits) that act as quantum reporters on the surface of high purity diamond. The reporter spins are localized with nanometer-scale uncertainty, and their quantum state is coherently manipulated and measured optically via a proximal nitrogen-vacancy (NV) color center located a few nanometers below the diamond surface. The quantum reporter network is then used for sensing, coherent coupling and imaging individual proton spins on the diamond surface with angstrom resolution. This approach may enable direct structural imaging of complex molecules that cannot be accessed from bulk studies. It realizes a new platform for probing novel materials, monitoring chemical reactions, and manipulation of complex systems on surfaces at a quantum level.

Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are well-established techniques that provide valuable information in a diverse set of disciplines but are currently limited to macroscopic sample volumes. Here we demonstrate nanoscale NMR spectroscopy and imaging under ambient conditions of samples containing multiple nuclear species, using nitrogen-vacancy (NV) colour centres in diamond as sensors. With single, shallow NV centres in a diamond chip and samples placed on the diamond surface, we perform NMR spectroscopy and one-dimensional MRI on few-nanometre-sized samples containing $^1$H and $^{19}$F nuclei. Alternatively, we employ a high-density NV layer near the surface of a diamond chip to demonstrate wide-field optical NMR spectroscopy of nanoscale samples containing $^1$H, $^{19}$F, and $^{31}$P nuclei, as well as multi-species two-dimensional optical MRI with sub-micron resolution. For all diamond samples exposed to air, we identify a ubiquitous $^1$H NMR signal, consistent with a $\sim 1$ nm layer of adsorbed hydrocarbons or water on the diamond surface and below any sample placed on the diamond. This work lays the foundation for nanoscale NMR and MRI applications such as studies of single proteins and functional biological imaging with subcellular resolution, as well as characterization of thin films with sub-nanometre resolution.