Revealing emergent magnetic charge in an antiferromagnet with diamond quantum magnetometry.

Whirling topological textures play a key role in exotic phases of magnetic materials and are promising for logic and memory applications. In antiferromagnets, these textures exhibit enhanced stability and faster dynamics with respect to their ferromagnetic counterparts, but they are also difficult to study due to their vanishing net magnetic moment. One technique that meets the demand of highly sensitive vectorial magnetic field sensing with negligible backaction is diamond quantum magnetometry. Here we show that an archetypal antiferromagnet-haematite-hosts a rich tapestry of monopolar, dipolar and quadrupolar emergent magnetic charge distributions. The direct read-out of the previously inaccessible vorticity of an antiferromagnetic spin texture provides the crucial connection to its magnetic charge through a duality relation. Our work defines a paradigmatic class of magnetic systems to explore two-dimensional monopolar physics, and highlights the transformative role that diamond quantum magnetometry could play in exploring emergent phenomena in quantum materials.

A quantum coherent spin in hexagonal boron nitride at ambient conditions.

Solid-state spin-photon interfaces that combine single-photon generation and long-lived spin coherence with scalable device integration-ideally under ambient conditions-hold great promise for the implementation of quantum networks and sensors. Despite rapid progress reported across several candidate systems, those possessing quantum coherent single spins at room temperature remain extremely rare. Here we report quantum coherent control under ambient conditions of a single-photon-emitting defect spin in a layered van der Waals material, namely, hexagonal boron nitride. We identify that the carbon-related defect has a spin-triplet electronic ground-state manifold. We demonstrate that the spin coherence is predominantly governed by coupling to only a few proximal nuclei and is prolonged by decoupling protocols. Our results serve to introduce a new platform to realize a room-temperature spin qubit coupled to a multiqubit quantum register or quantum sensor with nanoscale sample proximity.

Photonic Indistinguishability of the Tin-Vacancy Center in Nanostructured Diamond.

Tin-vacancy centers in diamond are promising spin-photon interfaces owing to their high quantum efficiency, large Debye-Waller factor, and compatibility with photonic nanostructuring. Benchmarking their single-photon indistinguishability is a key challenge for future applications. Here, we report the generation of single photons with 99.7_{-2.5}^{+0.3}% purity and 63(9)% indistinguishability from a resonantly excited tin-vacancy center in a single-mode waveguide. We obtain quantum control of the optical transition with 1.71(1)-ns-long π pulses of 77.1(8)% fidelity and show it is spectrally stable over 100 ms. A modest Purcell enhancement factor of 12 would enhance the indistinguishability to 95%.

Quadrature squeezed photons from a two-level system.

Resonance fluorescence arises from the interaction of an optical field with a two-level system, and has played a fundamental role in the development of quantum optics and its applications. Despite its conceptual simplicity, it entails a wide range of intriguing phenomena, such as the Mollow-triplet emission spectrum, photon antibunching and coherent photon emission. One fundamental aspect of resonance fluorescence--squeezing in the form of reduced quantum fluctuations in the single photon stream from an atom in free space--was predicted more than 30 years ago. However, the requirement to operate in the weak excitation regime, together with the combination of modest oscillator strength of atoms and low collection efficiencies, has continued to necessitate stringent experimental conditions for the observation of squeezing with atoms. Attempts to circumvent these issues had to sacrifice antibunching, owing to either stimulated forward scattering from atomic ensembles or multi-photon transitions inside optical cavities. Here, we use an artificial atom with a large optical dipole enabling 100-fold improvement of the photon detection rate over the natural atom counterpart and reach the necessary conditions for the observation of quadrature squeezing in single resonance-fluorescence photons. By implementing phase-dependent homodyne intensity-correlation detection, we demonstrate that the electric field quadrature variance of resonance fluorescence is three per cent below the fundamental limit set by vacuum fluctuations, while the photon statistics remain antibunched. The presence of squeezing and antibunching simultaneously is a fully non-classical outcome of the wave-particle duality of photons.

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.

Collective Quantum Memory Activated by a Driven Central Spin.

Coupling a qubit coherently to an ensemble is the basis for collective quantum memories. A single driven electron in a quantum dot can deterministically excite low-energy collective modes of a nuclear spin ensemble in the presence of lattice strain. We propose to gate a quantum state transfer between this central electron and these low-energy excitations-spin waves-in the presence of a strong magnetic field, where the nuclear coherence time is long. We develop a microscopic theory capable of calculating the exact time evolution of the strained electron-nuclear system. With this, we evaluate the operation of quantum state storage and show that fidelities up to 90% can be reached with a modest nuclear polarization of only 50%. These findings demonstrate that strain-enabled nuclear spin waves are a highly suitable candidate for quantum memory.

All-Optical Control of the Silicon-Vacancy Spin in Diamond at Millikelvin Temperatures.

The silicon-vacancy center in diamond offers attractive opportunities in quantum photonics due to its favorable optical properties and optically addressable electronic spin. Here, we combine both to achieve all-optical coherent control of its spin states. We utilize this method to explore spin dephasing effects in an impurity-rich sample beyond the limit of phonon-induced decoherence: Employing Ramsey and Hahn-echo techniques at temperatures down to 40 mK we identify resonant coupling to a substitutional nitrogen spin bath as limiting decoherence source for the electron spin.

Demonstration of a Coherent Electronic Spin Cluster in Diamond.

An obstacle for spin-based quantum sensors is magnetic noise due to proximal spins. However, a cluster of such spins can become an asset, if it can be controlled. Here, we polarize and readout a cluster of three nitrogen electron spins coupled to a single nitrogen-vacancy spin in diamond. We further achieve sub-nm localization of the cluster spins. Finally, we demonstrate coherent spin exchange between the species by simultaneous dressing of the nitrogen-vacancy and the nitrogen states. These results establish the feasibility of environment-assisted sensing and quantum simulations with diamond spins.

Observing bulk diamond spin coherence in high-purity nanodiamonds.

Nitrogen-vacancy (NV) centres in diamond are attractive for research straddling quantum information science, nanoscale magnetometry and thermometry. Whereas ultrapure bulk diamond NVs sustain the longest spin coherence times among optically accessible spins, nanodiamond NVs exhibit persistently poor spin coherence. Here we introduce high-purity nanodiamonds accommodating record-long NV coherence times, >60 µs, observed through universal dynamical decoupling. We show that the main contribution to decoherence comes from nearby nitrogen impurities rather than surface states. We protect the NV spin free precession, essential to d.c. magnetometry, by driving solely these impurities into the motional narrowing regime. This extends the NV free induction decay time from 440 ns, longer than that in type Ib bulk diamond, to 1.27 µs, which is comparable to that in type IIa (impurity-free) diamond. These properties allow the simultaneous exploitation of both high sensitivity and nanometre resolution in diamond-based emergent quantum technologies.

All-optical formation of coherent dark states of silicon-vacancy spins in diamond.

Spin impurities in diamond can be versatile tools for a wide range of solid-state-based quantum technologies, but finding spin impurities that offer sufficient quality in both photonic and spin properties remains a challenge for this pursuit. The silicon-vacancy center has recently attracted much interest because of its spin-accessible optical transitions and the quality of its optical spectrum. Complementing these properties, spin coherence is essential for the suitability of this center as a spin-photon quantum interface. Here, we report all-optical generation of coherent superpositions of spin states in the ground state of a negatively charged silicon-vacancy center using coherent population trapping. Our measurements reveal a characteristic spin coherence time, T2*, exceeding 45 nanoseconds at 4 K. We further investigate the role of phonon-mediated coupling between orbital states as a source of irreversible decoherence. Our results indicate the feasibility of all-optical coherent control of silicon-vacancy spins using ultrafast laser pulses.

Electronic structure of the silicon vacancy color center in diamond.

The negatively charged silicon vacancy (SiV) color center in diamond has recently proven its suitability for bright and stable single photon emission. However, its electronic structure so far has remained elusive. We here explore the electronic structure by exposing single SiV defects to a magnetic field where the Zeeman effect lifts the degeneracy of magnetic sublevels. The similar responses of single centers and a SiV ensemble in a low strain reference sample prove our ability to fabricate almost perfect single SiVs, revealing the true nature of the defect's electronic properties. We model the electronic states using a group-theoretical approach yielding a good agreement with the experimental observations. Furthermore, the model correctly predicts polarization measurements on single SiV centers and explains recently discovered spin selective excitation of SiV defects.

The Defects Genome of Janus Transition Metal Dichalcogenides.

2D Janus Transition Metal Dichalcogenides (TMDs) have attracted much interest due to their exciting quantum properties arising from their unique two-faced structure, broken-mirror symmetry, and consequent colossal polarization field within the monolayer. While efforts are made to achieve high-quality Janus monolayers, the existing methods rely on highly energetic processes that introduce unwanted grain-boundary and point defects with still unexplored effects on the material's structural and excitonic properties Through high-resolution scanning transmission electron microscopy (HRSTEM), density functional theory (DFT), and optical spectroscopy measurements; this work introduces the most encountered and energetically stable point defects. It establishes their impact on the material's optical properties. HRSTEM studies show that the most energetically stable point defects are single (VS and VSe) and double chalcogen vacancy (VS -VSe), interstitial defects (Mi), and metal impurities (MW) and establish their structural characteristics. DFT further establishes their formation energies and related localized bands within the forbidden band. Cryogenic excitonic studies on h-BN-encapsulated Janus monolayers offer a clear correlation between these structural defects and observed emission features, which closely align with the results of the theory. The overall results introduce the defect genome of Janus TMDs as an essential guideline for assessing their structural quality and device properties.

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.

Simultaneous Nanorheometry and Nanothermometry Using Intracellular Diamond Quantum Sensors.

The viscoelasticity of the cytoplasm plays a critical role in cell morphology, cell division, and intracellular transport. Viscoelasticity is also interconnected with other biophysical properties, such as temperature, which is known to influence cellular bioenergetics. Probing the connections between intracellular temperature and cytoplasmic viscoelasticity provides an exciting opportunity for the study of biological phenomena, such as metabolism and disease progression. The small length scales and transient nature of changes in these parameters combined with their complex interdependencies pose a challenge for biosensing tools, which are often limited to a single readout modality. Here, we present a dual-mode quantum sensor capable of performing simultaneous nanoscale thermometry and rheometry in dynamic cellular environments. We use nitrogen-vacancy centers in diamond nanocrystals as biocompatible sensors for in vitro measurements. We combine subdiffraction resolution single-particle tracking in a fluidic environment with optically detected magnetic resonance spectroscopy to perform simultaneous sensing of viscoelasticity and temperature. We use our sensor to demonstrate probing of the temperature-dependent viscoelasticity in complex media at the nanoscale. We then investigate the interplay between intracellular forces and the cytoplasmic rheology in live cells. Finally, we identify different rheological regimes and reveal evidence of active trafficking and details of the nanoscale viscoelasticity of the cytoplasm.

Imaging Nucleation and Propagation of Pinned Domains in Few-Layer Fe5-xGeTe2.

Engineering nontrivial spin textures in magnetic van der Waals materials is highly desirable for spintronic applications based on hybrid heterostructures. The recent observation of labyrinth and bubble domains in the near room-temperature ferromagnet Fe5-xGeTe2 down to a bilayer thickness was thus a significant advancement toward van der Waals-based many-body physics. However, the physical mechanism responsible for stabilizing these domains remains unclear and requires further investigation. Here, we combine cryogenic scanning diamond quantum magnetometry and field reversal techniques to elucidate the high-field propagation and nucleation of bubble domains in trilayer Fe5-xGeTe2. We provide evidence of pinning-induced nucleation of magnetic bubbles and further show an unexpectedly high layer-dependent coercive field. These measurements can be easily extended to a wide range of magnetic materials to provide valuable nanoscale insight into domain processes critical for spintronic applications.

Intrinsic giant magnetoresistance due to exchange-bias-type effects at the surface of single-crystalline NiS2 nanoflakes.

The coexistence of different properties in the same material often results in exciting physical effects. At low temperatures, the pyrite transition-metal disulphide NiS2 hosts both antiferromagnetic and weak ferromagnetic orders, along with surface metallicity dominating its electronic transport. The interplay between such a complex magnetic structure and surface-dominated conduction in NiS2, however, is still not understood. A possible reason for this limited understanding is that NiS2 has been available primarily in bulk single-crystal form, which makes it difficult to perform studies combining magnetometry and transport measurements with high spatial resolution. Here, NiS2 nanoflakes are produced via mechanical cleaving and exfoliation of NiS2 single crystals and their properties are studied on a local (micron-size) scale. Strongly field-asymmetric magnetotransport features are found at low temperatures, which resemble those of more complex magnetic thin film heterostructures. Using nitrogen vacancy magnetometry, these magnetotransport features are related to exchange-bias-type effects between ferromagnetic and antiferromagnetic regions forming near step edges at the nanoflake surface. Nanoflakes with bigger steps exhibit giant magnetoresistance, which suggests a strong influence of magnetic spin textures at the NiS2 surface on its electronic transport. These findings pave the way for the application of NiS2 nanoflakes in van der Waals heterostructures for low-temperature spintronics and superconducting spintronics.

Ideal refocusing of an optically active spin qubit under strong hyperfine interactions.

Combining highly coherent spin control with efficient light-matter coupling offers great opportunities for quantum communication and computing. Optically active semiconductor quantum dots have unparalleled photonic properties but also modest spin coherence limited by their resident nuclei. The nuclear inhomogeneity has thus far bound all dynamical decoupling measurements to a few microseconds. Here, we eliminate this inhomogeneity using lattice-matched GaAs-AlGaAs quantum dot devices and demonstrate dynamical decoupling of the electron spin qubit beyond 0.113(3) ms. Leveraging the 99.30(5)% visibility of our optical π-pulse gates, we use up to Nπ = 81 decoupling pulses and find a coherence time scaling of [Formula: see text]. This scaling manifests an ideal refocusing of strong interactions between the electron and the nuclear spin ensemble, free of extrinsic noise, which holds the promise of lifetime-limited spin coherence. Our findings demonstrate that the most punishing material science challenge for such quantum dot devices has a remedy and constitute the basis for highly coherent spin-photon 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.

Subnatural linewidth single photons from a quantum dot.

The observation of quantum-dot resonance fluorescence enabled a new solid-state approach to generating single photons with a bandwidth approaching the natural linewidth of a quantum-dot transition. Here, we operate in the small Rabi frequency limit of resonance fluorescence--the Heitler regime--to generate subnatural linewidth and high-coherence quantum light from a single quantum dot. The measured single-photon coherence is 30 times longer than the lifetime of the quantum-dot transition, and the single photons exhibit a linewidth which is inherited from the excitation laser. In contrast, intensity-correlation measurements reveal that this photon source maintains a high degree of antibunching behavior on the order of the transition lifetime with vanishing two-photon scattering probability. Generating decoherence-free phase-locked single photons from multiple quantum systems will be feasible with our approach.

Room-temperature optically detected magnetic resonance of single defects in hexagonal boron nitride.

Optically addressable solid-state spins are important platforms for quantum technologies, such as repeaters and sensors. Spins in two-dimensional materials offer an advantage, as the reduced dimensionality enables feasible on-chip integration into devices. Here, we report room-temperature optically detected magnetic resonance (ODMR) from single carbon-related defects in hexagonal boron nitride with up to 100 times stronger contrast than the ensemble average. We identify two distinct bunching timescales in the second-order intensity-correlation measurements for ODMR-active defects, but only one for those without an ODMR response. We also observe either positive or negative ODMR signal for each defect. Based on kinematic models, we relate this bipolarity to highly tuneable internal optical rates. Finally, we resolve an ODMR fine structure in the form of an angle-dependent doublet resonance, indicative of weak but finite zero-field splitting. Our results offer a promising route towards realising a room-temperature spin-photon quantum interface in hexagonal boron nitride.