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We demonstrate nearly a microsecond of spin coherence in Er3+ ions doped in cerium dioxide nanocrystal hosts, despite a large gyromagnetic ratio and nanometric proximity of the spin defect to the nanocrystal surface. The long spin coherence is enabled by reducing the dopant density below the instantaneous diffusion limit in a nuclear spin-free host material, reaching the limit of a single erbium spin defect per nanocrystal. We observe a large Orbach energy in a highly symmetric cubic site, further protecting the coherence in a qubit that would otherwise rapidly decohere. Spatially correlated electron spectroscopy measurements reveal the presence of Ce3+ at the nanocrystal surface that likely acts as extraneous paramagnetic spin noise. Even with these factors, defect-embedded nanocrystal hosts show tremendous promise for quantum sensing and quantum communication applications, with multiple avenues, including core-shell fabrication, redox tuning of oxygen vacancies, and organic surfactant modification, available to further enhance their spin coherence and functionality in the future., Comment: 26 pages, 5 figures

Optically interfaced solid-state defects are promising candidates for quantum communication technologies. The ideal defect system would feature bright telecom emission, long-lived spin states, and a scalable material platform, simultaneously. Here, we employ one such system, vanadium (V4+) in silicon carbide (SiC), to establish a potential telecom spin-photon interface within a mature semiconductor host. This demonstration of efficient optical spin polarization and readout facilitates all optical measurements of temperature-dependent spin relaxation times (T1). With this technique, we lower the temperature from about 2K to 100 mK to observe a remarkable four-orders-of-magnitude increase in spin T1 from all measured sites, with site-specific values ranging from 57 ms to above 27 s. Furthermore, we identify the underlying relaxation mechanisms, which involve a two-phonon Orbach process, indicating the opportunity for strain-tuning to enable qubit operation at higher temperatures. These results position V4+ in SiC as a prime candidate for scalable quantum nodes in future quantum networks., Comment: 11 pages, 6 figures

Quantum information technology offers the potential to realize unprecedented computational resources via secure channels capable of distributing entanglement between quantum computers. Diamond, as a host to atom-like defects with optically-accessible spin qubits, is a leading platform to realize quantum memory nodes needed to extend the reach of quantum links. Photonic crystal (PhC) cavities enhance light-matter interaction and are essential ingredients of an efficient interface between spins and photons that are used to store and communicate quantum information respectively. Despite great effort, however, the realization of visible PhC cavities with high quality factor (Q) and design flexibility is challenging in diamond. Here, we demonstrate one- and two-dimensional PhC cavities fabricated in recently developed thin-film diamonds, featuring Q-factors of 1.8x10$^5$ and 1.6x10$^5$, respectively, the highest Qs for visible PhC cavities realized in any material. Importantly, our fabrication process is simple and high-yield, based on conventional planar fabrication techniques, in contrast to previous approaches that rely on complex undercut methods. We also demonstrate fiber-coupled 1D PhC cavities with high photon extraction efficiency, and optical coupling between a single SiV center and such a cavity at 4K achieving a Purcell factor of 13. The demonstrated diamond thin-film photonic platform will improve the performance and scalability of quantum nodes and expand the range of quantum technologies.

Electronic defects in semiconductors form the basis for many emerging quantum technologies. Understanding defect spin and charge dynamics in solid state platforms is crucial to developing these building blocks, but many defect centers are difficult to access at the single-particle level due to the lack of sensitive readout techniques. A method for probing optically inactive spin defects would reveal semiconductor physics at the atomic scale and advance the study of new quantum systems. We exploit the intrinsic correlation between the charge and spin states of defect centers to measure defect charge populations and dynamics through the steady-state spin population, read-out at the single-defect level with a nearby optically active qubit. We directly measure ionization and charge relaxation of single dark defects in diamond, effects we do not have access to with traditional coherence-based quantum sensing. These spin resonance-based methods generalize to other solid state defect systems in relevant materials., Comment: 8 pages, 4 figures

We perform resonant fluorescence lifetime measurements on a nanocavity-coupled erbium ensemble as a function of cavity-laser detuning and pump power. Our measurements reveal an anomalous three-fold suppression of the ensemble Purcell factor at zero cavity detuning and high pump fluence. We capture qualitative aspects of this decay rate suppression using a Tavis-Cummings model of non-interacting spins coupled to a common cavity., Comment: 4 figures

Solid-state atomic defects with optical transitions in the telecommunication bands, potentially in a nuclear spin free environment, are important for applications in fiber-based quantum networks. Erbium ions doped in CeO$_2$ offer such a desired combination. Here we report on the optical homogeneous linewidth and electron spin coherence of Er$^{3+}$ ions doped in CeO$_2$ epitaxial film grown on a Si(111) substrate. The long-lived optical transition near 1530 nm in the environmentally-protected 4f shell of Er$^{3+}$ shows a narrow homogeneous linewidth of 440 kHz with an optical coherence time of 0.72 $\mu$s at 3.6 K. The reduced nuclear spin noise in the host allows for Er$^{3+}$ electron spin polarization at 3.6 K, yielding an electron spin coherence of 0.66 $\mu$s (in the isolated ion limit) and a spin relaxation of 2.5 ms. These findings indicate the potential of Er$^{3+}$:CeO$_2$ film as a valuable platform for quantum networks and communication applications., Comment: 18 pages, 4 figures

The use of trivalent erbium (Er$^{3+}$), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunications devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface makes it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO$_2$) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping control over the Er concentration. Even though the as-grown films are amorphous, after oxygen annealing they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO$_2$. Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (300) of their optical lifetime. Our findings demonstrate a low-temperature, non-destructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories., Comment: 5 figures

Solid-state electron spin qubits, like the nitrogen-vacancy center in diamond, rely on control sequences of population inversion to enhance sensitivity and improve device coherence. But even for this paradigmatic system, the fundamental limits of population inversion and potential impacts on applications like quantum sensing have not been assessed quantitatively. Here, we perform high accuracy simulations beyond the rotating wave approximation, including explicit unitary simulation of neighboring nuclear spins. Using quantum optimal control, we identify analytical pulses for the control of a qubit subspace within the spin-1 ground state and quantify the relationship between pulse complexity, control duration, and fidelity. We find exponentially increasing amplitude and bandwidth requirements with reduced control duration and further quantify the emergence of non-Markovian effects for multipulse sequences using sub-nanosecond population inversion. From this, we determine that the reduced fidelity and non-Markovianity is due to coherent interactions of the electron spin with the nuclear spin environment. Ultimately, we identify a potentially realizable regime of nanosecond control duration for high-fidelity multipulse sequences. These results provide key insights into the fundamental limits of quantum information processing using electron spin defects in diamond., Comment: 9 pages, 5 figures

Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets-systems with naturally commensurate energies-have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV-NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems., Comment: 14 pages, 4 figures

The nitrogen vacancy (NV) center in diamond, a well-studied, optically active spin defect, is the prototypical system in many state of the art quantum sensing and communication applications. In addition to the enticing properties intrinsic to the NV center, its diamond host's nuclear and electronic spin baths can be leveraged as resources for quantum information, rather than considered solely as sources of decoherence. However, current synthesis approaches result in stochastic defect spin positions, reducing the technology's potential for deterministic control and yield of NV-spin bath systems, as well as scalability and integration with other technologies. Here, we demonstrate the use of theoretical calculations of electronic central spin decoherence as an integral part of an NV-spin bath synthesis workflow, providing a path forward for the quantitative design of NV center-based quantum sensing systems. We use computationally generated coherence data to characterize the properties of single NV center qubits across relevant growth parameters to find general trends in coherence time distributions dependent on spin bath dimensionality and density. We then build a maximum likelihood estimator with our theoretical model, enabling the characterization of a test sample through NV T2* measurements. Finally, we explore the impact of dimensionality on the yield of strongly coupled electron spin systems. The methods presented herein are general and applicable to other qubit platforms that can be appropriately simulated., Comment: 12 pages, 6 figures

Robust spin-photon interfaces in solids are essential components in quantum networking and sensing technologies. Ideally, these interfaces combine a long-lived spin memory, coherent optical transitions, fast and high-fidelity spin manipulation, and straightforward device integration and scaling. The tin-vacancy center (SnV) in diamond is a promising spin-photon interface with desirable optical and spin properties at 1.7 K. However, the SnV spin lacks efficient microwave control and its spin coherence degrades with higher temperature. In this work, we introduce a new platform that overcomes these challenges - SnV centers in uniformly strained thin diamond membranes. The controlled generation of crystal strain introduces orbital mixing that allows microwave control of the spin state with 99.36(9) % gate fidelity and spin coherence protection beyond a millisecond. Moreover, the presence of crystal strain suppresses temperature dependent dephasing processes, leading to a considerable improvement of the coherence time up to 223(10) ${\mu}$s at 4 K, a widely accessible temperature in common cryogenic systems. Critically, the coherence of optical transitions is unaffected by the elevated temperature, exhibiting nearly lifetime-limited optical linewidths. Combined with the compatibility of diamond membranes with device integration, the demonstrated platform is an ideal spin-photon interface for future quantum technologies.

Diamond has superlative material properties for a broad range of quantum and electronic technologies. However, heteroepitaxial growth of single crystal diamond remains limited, impeding integration and evolution of diamond-based technologies. Here, we directly bond single-crystal diamond membranes to a wide variety of materials including silicon, fused silica, sapphire, thermal oxide, and lithium niobate. Our bonding process combines customized membrane synthesis, transfer, and dry surface functionalization, allowing for minimal contamination while providing pathways for near unity yield and scalability. We generate bonded crystalline membranes with thickness as low as 10 nm, sub-nm interfacial regions, and nanometer-scale thickness variability over 200 by 200 $\mu m^2$ areas. We measure spin coherence times $T_2$ for nitrogen-vacancy centers in bonded membranes of up to 623(21) $\mu$s, suitable for advanced quantum applications. We demonstrate multiple methods for integrating high quality factor nanophotonic cavities with the diamond heterostructures, highlighting the platform versatility in quantum photonic applications. Furthermore, we show that our ultra-thin diamond membranes are compatible with total internal reflection fluorescence (TIRF) microscopy, which enables interfacing coherent diamond quantum sensors with living cells while rejecting unwanted background luminescence. The processes demonstrated herein provide a full toolkit to synthesize heterogeneous diamond-based hybrid systems for quantum and electronic technologies., Comment: 64 pages, 25 figures

Single-qubit sensing protocols can be used to measure qubit-bath coupling parameters. However, for sufficiently large coupling, the sensing protocol itself perturbs the bath, which is predicted to result in a characteristic response in the sensing measurements. Here, we observe this bath perturbation, also known as a quantum quench, by preparing the nuclear spin bath of a nitrogen-vacancy (NV) center in polarized initial states and performing phase-resolved spin echo measurements on the NV electron spin. These measurements reveal a time-dependent phase determined by the initial state of the bath. We derive the relationship between sensor phase and Gaussian spin bath polarization, and apply it to reconstruct both the axial and transverse polarization components. Using this insight, we optimize the transfer efficiency of our dynamic nuclear polarization sequence. This technique for directly measuring bath polarization may assist in preparing high-fidelity quantum memory states, improving nanoscale NMR methods, and investigating non-Gaussian quantum baths., Comment: 34 pages, 7 figures

Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects such as erbium suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here we present a scalable approach towards CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of $5\times10^{4}$ and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step towards realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies., Comment: 3 figures

An outstanding hurdle for defect spin qubits in silicon carbide (SiC) is single-shot readout - a deterministic measurement of the quantum state. Here, we demonstrate single-shot readout of single defects in SiC via spin-to-charge conversion, whereby the defect's spin state is mapped onto a long-lived charge state. With this technique, we achieve over 80% readout fidelity without pre- or post-selection, resulting in a high signal-to-noise ratio (SNR) that enables us to measure long spin coherence times. Combined with pulsed dynamical decoupling sequences in an isotopically purified host material, we report single spin T2 > 5s, over two orders of magnitude greater than previously reported in this system. The mapping of these coherent spin states onto single charges unlocks both single-shot readout for scalable quantum nodes and opportunities for electrical readout via integration with semiconductor devices., Comment: 18 pages, 5 figures

Color centers in diamond are widely explored as qubits in quantum technologies. However, challenges remain in the effective and efficient integration of these diamond-hosted qubits in device heterostructures. Here, nanoscale-thick uniform diamond membranes are synthesized via "smart-cut" and isotopically (12C) purified overgrowth. These membranes have tunable thicknesses (demonstrated 50 nm to 250 nm), are deterministically transferable, have bilaterally atomically flat surfaces (Rq <= 0.3 nm), and bulk-diamond-like crystallinity. Color centers are synthesized via both implantation and in-situ overgrowth incorporation. Within 110 nm thick membranes, individual germanium-vacancy (GeV-) centers exhibit stable photoluminescence at 5.4 K and average optical transition linewidths as low as 125 MHz. The room temperature spin coherence of individual nitrogen-vacancy (NV-) centers shows Ramsey spin dephasing times (T2*) and Hahn echo times (T2) as long as 150 us and 400 us, respectively. This platform enables the straightforward integration of diamond membranes that host coherent color centers into quantum technologies., Comment: 50 pages, 13 figures

Noiseless optical components are critical for applications ranging from metrology to quantum communication. Here we characterize several commercial telecom C-band fiber components for parasitic noise using a tunable laser. We observe the spectral signature of trace concentrations of erbium in all devices from the underlying optical crystals including YVO4, LiNbO3, TeO2 and AMTIR glass. Due to the long erbium lifetime, these signals are challenging to mitigate at the single photon level in the telecom range, and suggests the need for higher purity optical crystals., Comment: 5 pages, 3 figures

Optically and magnetically active point defects in semiconductors are interesting platforms for the development of solid-state quantum technologies. Their optical properties are usually probed by measuring photoluminescence spectra, which provide information on excitation energies and on the interaction of electrons with lattice vibrations. We present a combined computational and experimental study of photoluminescence spectra of defects in diamond and SiC, aimed at assessing the validity of theoretical and numerical approximations used in first principles calculations, including the use of the Franck-Condon principle and the displaced harmonic oscillator approximation. We focus on prototypical examples of solid-state qubits, the divacancy centers in SiC and the nitrogen-vacancy in diamond, and we report computed photoluminescence spectra as a function of temperature that are in very good agreement with the measured ones. As expected we find that the use of hybrid functionals leads to more accurate results than semilocal functionals. Interestingly our calculations show that constrained density functional theory (CDFT) and time-dependent hybrid DFT perform equally well in describing the excited state potential energy surface of triplet states; our findings indicate that CDFT, a relatively cheap computational approach, is sufficiently accurate for the calculations of photoluminescence spectra of the defects studied here. Finally, we find that only by correcting for finite-size effects and extrapolating to the dilute limit, one can obtain a good agreement between theory and experiment. Our results provide a detailed validation protocol of first principles calculations of photoluminescence spectra, necessary both for the interpretation of experiments and for robust predictions of the electronic properties of point defects in semiconductors.

Spin defect centers with long quantum coherence times ($T_2$) are key solid-state platforms for a variety of quantum applications. Recently, cluster correlation expansion (CCE) techniques have emerged as a powerful tool to simulate the $T_2$ of defect electron spins in these solid-state systems with good accuracy. Here, based on CCE, we uncover an algebraic expression for $T_2$ generalized for host compounds with dilute nuclear spin baths, which enables a quantitative and comprehensive materials exploration with a near instantaneous estimate of the coherence. We investigate more than 12,000 host compounds at natural isotopic abundance, and find that silicon carbide (SiC), a prominent widegap semiconductor for quantum applications, possesses the longest coherence times among widegap non-chalcogenides. In addition, more than 700 chalcogenides are shown to possess a longer $T_2$ than SiC. We suggest new potential host compounds with promisingly long $T_2$ up to 47 ms, and pave the way to explore unprecedented functional materials for quantum applications., Comment: 24 pages, 4 figures, 1 table

The ability to manipulate entanglement between multiple spatially-separated qubits is essential for quantum information processing. Although nitrogen-vacancy (NV) centers in diamond provide a promising qubit platform, developing scalable two-qubit gates remains a well-known challenge. To this end, magnon-mediated entanglement proposals have attracted attention due to their long-range spin-coherent propagation. Optimal device geometries and gate protocols of such schemes, however, have yet to be determined. Here we predict strong long-distance ($>\mu$m) NV-NV coupling via magnon modes with cooperativities exceeding unity in ferromagnetic bar and waveguide structures. Moreover, we explore and compare on-resonant transduction and off-resonant virtual-magnon exchange protocols, and discuss their suitability for generating or manipulating entangled states at low temperatures ($T\lesssim 150$ mK) under realistic experimental conditions. This work will guide future experiments that aim to entangle spin qubits in solids with magnon excitations., Comment: PRX Quantum in press, 10 pages, 5 figures

Defects with associated electron and nuclear spins in solid-state materials have a long history relevant to quantum information science going back to the first spin echo experiments with silicon dopants in the 1950s. Since the turn of the century, the field has rapidly spread to a vast array of defects and host crystals applicable to quantum communication, sensing, and computing. From simple spin resonance to long-distance remote entanglement, the complexity of working with spin defects is fast advancing, and requires an in-depth understanding of their spin, optical, charge, and material properties in this modern context. This is especially critical for discovering new relevant systems dedicated to specific quantum applications. In this review, we therefore expand upon all the key components with an emphasis on the properties of defects and the host material, on engineering opportunities and other pathways for improvement. Finally, this review aims to be as defect and material agnostic as possible, with some emphasis on optical emitters, providing a broad guideline for the field of solid-state spin defects for quantum information., Comment: 40 pages, 7 figures, 259 references

Optically addressable paramagnetic defects in wide-band-gap semiconductors are promising platforms for quantum communications and sensing. The presence of avoided crossings between the electronic levels of these defects can substantially alter their quantum dynamics and be both detrimental and beneficial for quantum information applications. Avoided crossings give rise to clock transitions, which can significantly improve protection from magnetic noise and favorably increase coherence time. However, the reduced coupling between electronic and nuclear spins at an avoided crossing may be detrimental to applications where nuclear spins act as quantum memories. Here we present a combined theoretical and experimental study of the quantum dynamics of paramagnetic defects interacting with a nuclear spin bath at avoided crossings. We develop a computational approach based on a generalization of the cluster expansion technique, which can account for processes beyond pure dephasing and describe the dynamics of any solid-state spin-qubits near avoided crossings. Using this approach and experimental validation, we determine the change in nature and source of noise at avoided crossings for divacancies in SiC. We find that we can condition the clock transition of the divacancies in SiC on multiple adjacent nuclear spins states. In our experiments, we demonstrate that one can suppress the effects of fluctuating charge impurities with depletion techniques, leading to an increased coherence time at clock transition, limited purely by magnetic noise. Combined with ab-initio predictions of spin Hamiltonian parameters, the proposed theoretical approach paves the way to designing the coherence properties of spin qubits from first principles., Comment: 29 pages, 7 figures

Nuclear spins in the solid state are both a cause of decoherence and a valuable resource for spin qubits. In this work, we demonstrate control of isolated 29Si nuclear spins in silicon carbide (SiC) to create an entangled state between an optically active divacancy spin and a strongly coupled nuclear register. We then show how isotopic engineering of SiC unlocks control of single weakly coupled nuclear spins and present an ab initio method to predict the optimal isotopic fraction which maximizes the number of usable nuclear memories. We bolster these results by reporting high-fidelity electron spin control (F=99.984(1)%), alongside extended coherence times (T2=2.3 ms, T2DD>14.5 ms), and a >40 fold increase in dephasing time (T2*) from isotopic purification. Overall, this work underlines the importance of controlling the nuclear environment in solid-state systems and provides milestone demonstrations that link single photon emitters with nuclear memories in an industrially scalable material., Comment: 25 pages, 5 figures

Decoherence largely limits the physical realization of qubits and its mitigation is critical to quantum science. Here, we construct a robust qubit embedded in a decoherence-protected subspace, obtained by hybridizing an applied microwave drive with the ground-state electron spin of a silicon carbide divacancy defect. The qubit is protected from magnetic, electric, and temperature fluctuations, which account for nearly all relevant decoherence channels in the solid state. This culminates in an increase of the qubit's inhomogeneous dephasing time by over four orders of magnitude (to > 22 milliseconds), while its Hahn-echo coherence time approaches 64 milliseconds. Requiring few key platform-independent components, this result suggests that substantial coherence improvements can be achieved in a wide selection of quantum architectures., Comment: 12 pages, 4 figures

Integrating solid-state quantum emitters with nanophotonic resonators is essential for efficient spin-photon interfacing and optical networking applications. While diamond color centers have proven to be excellent candidates for emerging quantum technologies, their integration with optical resonators remains challenging. Conventional approaches based on etching resonators into diamond often negatively impact color center performance and offer low device yield. Here, we developed an integrated photonics platform based on templated atomic layer deposition of TiO2 on diamond membranes. Our fabrication method yields high-performance nanophotonic devices while avoiding etching wavelength-scale features into diamond. Moreover, this technique generates highly reproducible optical resonances and can be iterated on individual diamond samples, a unique processing advantage. Our approach is suitable for a broad range of both wavelengths and substrates and can enable high-cooperativity interfacing between cavity photons and coherent defects in diamond or silicon carbide, rare earth ions, or other material systems., Comment: 13 pages, 4 figures, 1 table

Solid state quantum emitters with spin registers are promising platforms for quantum communication, yet few emit in the narrow telecom band necessary for low-loss fiber networks. Here we create and isolate near-surface single vanadium dopants in silicon carbide (SiC) with stable and narrow emission in the O-band (1278-1388 nm), with brightness allowing cavity-free detection in a wafer-scale CMOS-compatible material. In vanadium ensembles, we characterize the complex d1 orbital physics in all five available sites in 4H-SiC and 6H-SiC. The optical transitions are sensitive to mass shifts from local silicon and carbon isotopes, enabling optically resolved nuclear spin registers. Optically detected magnetic resonance in the ground and excited orbital states reveals a variety of hyperfine interactions with the vanadium nuclear spin and clock transitions for quantum memories. Finally, we demonstrate coherent quantum control of the spin state. These results provide a path for telecom emitters in the solid-state for quantum applications., Comment: 16 pages, 4 figures

Spin defects in silicon carbide have exceptional electron spin coherence with a near-infrared spin-photon interface in a material amenable to modern semiconductor fabrication. Leveraging these advantages, we successfully integrate highly coherent single neutral divacancy spins in commercially available p-i-n structures and fabricate diodes to modulate the local electrical environment of the defects. These devices enable deterministic charge state control and broad Stark shift tuning exceeding 850 GHz. Surprisingly, we show that charge depletion results in a narrowing of the optical linewidths by over 50 fold, approaching the lifetime limit. These results demonstrate a method for mitigating the ubiquitous problem of spectral diffusion in solid-state emitters by engineering the electrical environment while utilizing classical semiconductor devices to control scalable spin-based quantum systems., Comment: 20 pages, 5 figures

Interfacing solid-state defect electron spins to other quantum systems is an ongoing challenge. The ground-state spin's weak coupling to its environment bestows excellent coherence properties, but also limits desired drive fields. The excited-state orbitals of these electrons, however, can exhibit stronger coupling to phononic and electric fields. Here, we demonstrate electrically driven coherent quantum interference in the optical transition of single, basally oriented divacancies in commercially available 4H silicon carbide. By applying microwave frequency electric fields, we coherently drive the divacancy's excited-state orbitals and induce Landau-Zener-Stuckelberg interference fringes in the resonant optical absorption spectrum. Additionally, we find remarkably coherent optical and spin subsystems enabled by the basal divacancy's symmetry. These properties establish divacancies as strong candidates for quantum communication and hybrid system applications, where simultaneous control over optical and spin degrees of freedom is paramount., Comment: 17 pages, 4 figures

The detection of photocurrents is central to understanding and harnessing the interaction of light with matter. Although widely used, transport-based detection averages over spatial distributions and can suffer from low photocarrier collection efficiency. Here, we introduce a contact-free method to spatially resolve local photocurrent densities using a proximal quantum magnetometer. We interface monolayer MoS2 with a near-surface ensemble of nitrogen-vacancy centers in diamond and map the generated photothermal current distribution through its magnetic field profile. By synchronizing the photoexcitation with dynamical decoupling of the sensor spin, we extend the sensor's quantum coherence and achieve sensitivities to alternating current densities as small as 20 nA per micron. Our spatiotemporal measurements reveal that the photocurrent circulates as vortices, manifesting the Nernst effect, and rises with a timescale indicative of the system's thermal properties. Our method establishes an unprecedented probe for optoelectronic phenomena, ideally suited to the emerging class of two-dimensional materials, and stimulates applications towards large-area photodetectors and stick-on sources of magnetic fields for quantum control., Comment: 19 pages, 4 figures

Hybrid spin-mechanical systems provide a platform for integrating quantum registers and transducers. Efficient creation and control of such systems require a comprehensive understanding of the individual spin and mechanical components as well as their mutual interactions. Point defects in silicon carbide (SiC) offer long-lived, optically addressable spin registers in a wafer-scale material with low acoustic losses, making them natural candidates for integration with high quality factor mechanical resonators. Here, we show Gaussian focusing of a surface acoustic wave in SiC, characterized by a novel stroboscopic X-ray diffraction imaging technique, which delivers direct, strain amplitude information at nanoscale spatial resolution. Using ab initio calculations, we provide a more complete picture of spin-strain coupling for various defects in SiC with C3v symmetry. This reveals the importance of shear for future device engineering and enhanced spin-mechanical coupling. We demonstrate all-optical detection of acoustic paramagnetic resonance without microwave magnetic fields, relevant to sensing applications. Finally, we show mechanically driven Autler-Townes splittings and magnetically forbidden Rabi oscillations. These results offer a basis for full strain control of three-level spin systems., Comment: 17 pages, 4 figures

Neutrally charged divacancies in silicon carbide (SiC) are paramagnetic color centers whose long coherence times and near-telecom operating wavelengths make them promising for scalable quantum communication technologies compatible with existing fiber optic networks. However, local strain inhomogeneity can randomly perturb their optical transition frequencies, which degrades the indistinguishability of photons emitted from separate defects, and hinders their coupling to optical cavities. Here we show that electric fields can be used to tune the optical transition frequencies of single neutral divacancy defects in 4H-SiC over a range of several GHz via the DC Stark effect. The same technique can also control the charge state of the defect on microsecond timescales, which we use to stabilize unstable or non-neutral divacancies into their neutral charge state. Using fluorescence-based charge state detection, we show both 975 nm and 1130 nm excitation can prepare its neutral charge state with near unity efficiency., Comment: 12 pages, 4 figures

Defects in silicon carbide (SiC) have emerged as a favorable platform for optically-active spin-based quantum technologies. Spin qubits exist in specific charge states of these defects, where the ability to control these states can provide enhanced spin-dependent readout and long-term charge stability of the qubits. We investigate this charge state control for two major spin qubits in 4H-SiC, the divacancy (VV) and silicon vacancy (Vsi), obtaining bidirectional optical charge conversion between the bright and dark states of these defects. We measure increased photoluminescence from VV ensembles by up to three orders of magnitude using near-ultraviolet excitation, depending on the substrate, and without degrading the electron spin coherence time. This charge conversion remains stable for hours at cryogenic temperatures, allowing spatial and persistent patterning of the relative charge state populations. We develop a comprehensive model of the defects and optical processes involved, offering a strong basis to improve material design and to develop quantum applications in SiC., Comment: 10 pages, figures

Although geometric phases in quantum evolution were historically overlooked, their active control now stimulates strategies for constructing robust quantum technologies. Here, we demonstrate arbitrary single-qubit holonomic gates from a single cycle of non-adiabatic evolution, eliminating the need to concatenate two separate cycles. Our method varies the amplitude, phase, and detuning of a two-tone optical field to control the non-Abelian geometric phase acquired by a nitrogen-vacancy center in diamond over a coherent excitation cycle. We demonstrate the enhanced robustness of detuned gates to excited-state decoherence and provide insights for optimizing fast holonomic control in dissipative quantum systems., Comment: Minor revisions to main text (6 pages); added supplementary material (7 pages)

The divacancies in SiC are a family of paramagnetic defects that show promise for quantum communication technologies due to their long-lived electron spin coherence and their optical addressability at near-telecom wavelengths. Nonetheless, a mechanism for high-fidelity spin-to-photon conversion, which is a crucial prerequisite for such technologies, has not yet been demonstrated. Here we demonstrate a high-fidelity spin-to-photon interface in isolated divacancies in epitaxial films of 3C-SiC and 4H-SiC. Our data show that divacancies in 4H-SiC have minimal undesirable spin-mixing, and that the optical linewidths in our current sample are already similar to those of recent remote entanglement demonstrations in other systems. Moreover, we find that 3C-SiC divacancies have millisecond Hahn-echo spin coherence time, which is among the longest measured in a naturally isotopic solid. The presence of defects with these properties in a commercial semiconductor that can be heteroepitaxially grown as a thin film on shows promise for future quantum networks based on SiC defects., Comment: 26 pages, 4 figures

The nitrogen-vacancy (NV) center in diamond has been extensively studied in recent years for its remarkable quantum coherence properties that make it an ideal candidate for room temperature quantum computing and quantum sensing schemes. However, these schemes rely on spin-spin dipolar interactions, which require the NV centers to be within a few nanometers from each other while still separately addressable, or to be in close proximity of the diamond surface, where their coherence properties significantly degrade. Here we demonstrate a method for overcoming these limitations using a hybrid yttrium iron garnet (YIG)-nanodiamond quantum system constructed with the help of directed assembly and transfer printing techniques. We show that YIG spin-waves can amplify the oscillating field of a microwave source by more than two orders of magnitude and efficiently mediate its coherent interactions with an NV center ensemble. These results demonstrate that spin-waves in ferromagnets can be used as quantum buses for enhanced, long-range qubit interactions, paving the way to ultra-efficient manipulation and coupling of solid state defects in hybrid quantum networks and sensing devices., Comment: 7 pages, 4 figures

Spins bound to point defects are increasingly viewed as an important resource for solid-state implementations of quantum information technologies. In particular, there is a growing interest in the identification of new classes of defect spin that can be controlled optically. Here we demonstrate ensemble optical spin polarization and optically detected magnetic resonance (ODMR) of the S = 1 electronic ground state of chromium (Cr4+) impurities in silicon carbide (SiC) and gallium nitride (GaN). Spin polarization is made possible by the narrow optical linewidths of these ensembles (< 8.5 GHz), which are similar in magnitude to the ground state zero-field spin splitting energies of the ions at liquid helium temperatures. We therefore are able to optically resolve individual spin sublevels within the ensembles at low magnetic fields using resonant excitation from a cavity-stabilized, narrow-linewidth laser. Additionally, these near-infrared emitters possess exceptionally weak phonon sidebands, ensuring that > 73% of the overall optical emission is contained with the defects zero-phonon lines. These characteristics make this semiconductor-based, transition metal impurity system a promising target for further study in the ongoing effort to integrate optically active quantum states within common optoelectronic materials., Comment: 13 pages, 4 figures

Adiabatic evolutions find widespread utility in applications to quantum state engineering, geometric quantum computation, and quantum simulation. Although offering robustness to experimental imperfections, adiabatic processes are susceptible to decoherence due to their long evolution time. A general strategy termed "shortcuts to adiabaticity" (STA) aims to remedy this vulnerability by designing fast dynamics to reproduce the results of slow, adiabatic evolutions. Here, we implement a novel STA technique known as "superadiabatic transitionless driving" (SATD) to speed up stimulated Raman adiabatic passage (STIRAP) in a solid-state lambda ({\Lambda}) system. Utilizing optical transitions to a dissipative excited state in the nitrogen-vacancy (NV) center in diamond, we demonstrate the accelerated performance of different shortcut trajectories for population transfer and for the initialization and transfer of coherent superpositions. We reveal that SATD protocols exhibit robustness to dissipation and experimental uncertainty, and can be optimized when these effects are present. These results motivate STA as a promising tool for controlling open quantum systems comprising individual or hybrid nanomechanical, superconducting, and photonic elements in the solid state., Comment: 20 pages, 4 figures

The identification of new solid-state defect qubit candidates in widely used semiconductors has the potential to enable the use of nanofabricated devices for enhanced qubit measurement and control operations. In particular, the recent discovery of optically active spin states in silicon carbide thin films offers a scalable route for incorporating defect qubits into on-chip photonic devices. Here we demonstrate the use of 3C silicon carbide photonic crystal cavities for enhanced excitation of color center defect spin ensembles in order to increase measured photoluminescence signal count rates, optically detected magnetic resonance signal intensities, and optical spin initialization rates. We observe up to a factor of 30 increase in the photoluminescence and ODMR signals from Ky5 color centers excited by cavity resonant excitation and increase the rate of ground-state spin initialization by approximately a factor of two. Furthermore, we show that the small excitation mode volume and enhanced excitation and collection efficiencies provided by the structures can be used to study inhomogeneous broadening in defect qubit ensembles. These results highlight some of the benefits that nanofabricated devices offer for engineering the local photonic environment of color center defect qubits to enable applications in quantum information and sensing., Comment: 8 pages, 4 figures

The phase relation between quantum states represents an essential resource for the storage and processing of quantum information. While quantum phases are commonly controlled dynamically by tuning energetic interactions, utilizing geometric phases that accumulate during cyclic evolution may offer superior robustness to noise. To date, demonstrations of geometric phase control in solid-state systems rely on microwave fields that have limited spatial resolution. Here, we demonstrate an all-optical method based on stimulated Raman adiabatic passage to accumulate a geometric phase, the Berry phase, in an individual nitrogen-vacancy (NV) center in diamond. Using diffraction-limited laser light, we guide the NV center's spin along loops on the Bloch sphere to enclose arbitrary Berry phase and characterize these trajectories through time-resolved state tomography. We investigate the limits of this control due to loss of adiabiaticity and decoherence, as well as its robustness to noise intentionally introduced into the experimental control parameters, finding its resilience to be independent of the amount of Berry phase enclosed. These techniques set the foundation for optical geometric manipulation in future implementations of photonic networks of solid state qubits linked and controlled by light., Comment: 18 pages, 5 figures

We demonstrate optically pumped dynamic nuclear polarization of 29-Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H- and 6H-SiC. The 99 +/- 1% degree of polarization at room temperature corresponds to an effective nuclear temperature of 5 microKelvin. By combining ab initio theory with the experimental identification of the color centers' optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging., Comment: 21 pages including supplementary information; four figures in main text and one table

The elimination of defects from SiC has facilitated its move to the forefront of the optoelectronics and power-electronics industries. Nonetheless, because the electronic states of SiC defects can have sharp optical and spin transitions, they are increasingly recognized as a valuable resource for quantum-information and nanoscale-sensing applications. Here, we show that individual electron spin states in highly purified monocrystalline 4H-SiC can be isolated and coherently controlled. Bound to neutral divacancy defects, these states exhibit exceptionally long ensemble Hahn-echo spin coherence, exceeding 1 ms. Coherent control of single spins in a material amenable to advanced growth and microfabrication techniques is an exciting route to wafer-scale quantum technologies., Comment: 11 pages, 3 figures

We demonstrate three-dimensional localization of a single nitrogen-vacancy (NV) center in diamond by combining nitrogen doping during growth with a post-growth 12C implantation technique that facilitates vacancy formation in the crystal. We show that the NV density can be controlled by the implantation dose without necessitating increase of the nitrogen incorporation. By implanting a large 12C dose through nanoscale apertures, we can localize an individual NV center within a volume of (~180 nm)**3 at a deterministic position while reproducibly preserving a coherence time (T2) > 300 {\mu}s. Our approach enables integration of NV centers into diamond nanostructures to realize scalable spin-sensing devices as well as coherent spin coupling mediated by photons and phonons., Comment: 21 pages, 3 figures

The recent discovery of color centers with optically addressable spin states in 3C silicon carbide (SiC) similar to the negatively charged nitrogen vacancy center in diamond has the potential to enable the integration of defect qubits into established wafer scale device architectures for quantum information and sensing applications. Here we demonstrate the design, fabrication, and characterization of photonic crystal cavities in 3C SiC films with incorporated ensembles of color centers and quality factor (Q) to mode volume ratios similar to those achieved in diamond. Simulations show that optimized H1 and L3 structures exhibit Q as high as 45,000 and mode volumes of approximately $(\lambda/n)^{3}$. We utilize the internal color centers as a source of broadband excitation to characterize fabricated structures with resonances tuned to the color center zero phonon line and observe Q in the range of 900-1,500 with narrowband photoluminescence collection enhanced by up to a factor of 10. By comparing the Q factors observed for different geometries with finite-difference time-domain simulations, we find evidence that nonvertical sidewalls are likely the dominant source of discrepancies between our simulated and measured Q factors. These results indicate that defect qubits in 3C SiC thin films show clear promise as a simple, scalable platform for interfacing defect qubits with photonic, optoelectronic, and optomechanical devices., Comment: 12 pages, 3 figures, 1 table

The electron spins of semiconductor defects can have complex interactions with their host, particularly in polar materials like SiC where electrical and mechanical variables are intertwined. By combining pulsed spin resonance with ab-initio simulations, we show that spin-spin interactions within SiC neutral divacancies give rise to spin states with an enhanced Stark effect, sub-10**-6 strain sensitivity, and highly spin-dependent photoluminescence with intensity contrasts of 15-36%. These results establish SiC color centers as compelling systems for sensing nanoscale fields., Comment: 10 pages, 4 figures, 1 table

We demonstrate fluorescence thermometry techniques with sensitivities approaching 10 mK Hz^(-1/2) based on the spin-dependent photoluminescence of nitrogen vacancy (NV) centers in diamond. These techniques use dynamical decoupling protocols to convert thermally induced shifts in the NV center's spin resonance frequencies into large changes in its fluorescence. By mitigating interactions with nearby nuclear spins and facilitating selective thermal measurements, these protocols enhance the spin coherence times accessible for thermometry by 45x, corresponding to a 7x improvement in the NV center's temperature sensitivity. Moreover, we demonstrate these techniques can be applied over a broad temperature range and in both finite and near-zero magnetic field environments. This versatility suggests that the quantum coherence of single spins could be practically leveraged for sensitive thermometry in a wide variety of biological and microscale systems., Comment: 14 pages, 4 figures Proc. Natl. Acad. Sci. USA, online early edition (2013)

The study of individual quantum systems in solids, for use as quantum bits (qubits) and probes of decoherence, requires protocols for their initialization, unitary manipulation, and readout. In many solid-state quantum systems, these operations rely on disparate techniques that can vary widely depending on the particular qubit structure. One such qubit, the nitrogen-vacancy (NV) center spin in diamond, can be initialized and read out through its special spin selective intersystem crossing, while microwave electron spin resonance (ESR) techniques provide unitary spin rotations. Instead, we demonstrate an alternative, fully optical approach to these control protocols in an NV center that does not rely on its intersystem crossing. By tuning an NV center to an excited-state spin anticrossing at cryogenic temperatures, we use coherent population trapping and stimulated Raman techniques to realize initialization, readout, and unitary manipulation of a single spin. Each of these techniques can be directly performed along any arbitrarily-chosen quantum basis, removing the need for extra control steps to map the spin to and from a preferred basis. Combining these protocols, we perform measurements of the NV center's spin coherence, a demonstration of this full optical control. Consisting solely of optical pulses, these techniques enable control within a smaller footprint and within photonic networks. Likewise, this approach obviates the need for both ESR manipulation and spin addressability through the intersystem crossing. This method could therefore be applied to a wide range of potential solid-state qubits, including those which currently lack a means to be addressed., Comment: 14 pages, 5 figures with an additional 25 pages of supporting material with 14 figures

We demonstrate nanometer-precision depth control of nitrogen-vacancy (NV) center creation near the surface of synthetic diamond using an in situ nitrogen delta-doping technique during plasma-enhanced chemical vapor deposition. Despite their proximity to the surface, doped NV centers with depths (d) ranging from 5 - 100 nm display long spin coherence times, T2 > 100 \mus at d = 5 nm and T2 > 600 \mus at d \geq 50 nm. The consistently long spin coherence observed in such shallow NV centers enables applications such as atomic-scale external spin sensing and hybrid quantum architectures., Comment: 14 pages, 4 figures, 11 pages of additional supplementary material

Using an optical tweezers apparatus, we demonstrate three-dimensional control of nanodiamonds in solution with simultaneous readout of ground-state electron-spin resonance (ESR) transitions in an ensemble of diamond nitrogen-vacancy (NV) color centers. Despite the motion and random orientation of NV centers suspended in the optical trap, we observe distinct peaks in the measured ESR spectra qualitatively similar to the same measurement in bulk. Accounting for the random dynamics, we model the ESR spectra observed in an externally applied magnetic field to enable d.c. magnetometry in solution. We estimate the d.c. magnetic field sensitivity based on variations in ESR line shapes to be ~50 microTesla/Hz^1/2. This technique may provide a pathway for spin-based magnetic, electric, and thermal sensing in fluidic environments and biophysical systems inaccessible to existing scanning probe techniques., Comment: 29 pages, 13 figures for manuscript and supporting information

Fabrication of devices designed to fully harness the unique properties of quantum mechanics through their coupling to quantum bits (qubits) is a prominent goal in the field of quantum information processing (QIP). Among various qubit candidates, nitrogen vacancy (NV) centers in diamond have recently emerged as an outstanding platform for room temperature QIP. However, formidable challenges still remain in processing diamond and in the fabrication of thin diamond membranes, which are necessary for planar photonic device engineering. Here we demonstrate epitaxial growth of single crystal diamond membranes using a conventional microwave chemical vapor deposition (CVD) technique. The grown membranes, only a few hundred nanometers thick, show bright luminescence, excellent Raman signature and good NV center electronic spin coherence times. Microdisk cavities fabricated from these membranes exhibit quality factors of up to 3000, overlapping with NV center emission. Our methodology offers a scalable approach for diamond device fabrication for photonics, spintronics, optomechanics and sensing applications., Comment: Copyright rights with a scientific journal

We demonstrate a technique to nanofabricate nitrogen vacancy (NV) centers in diamond based on broad-beam nitrogen implantation through apertures in electron beam lithography resist. This method enables high-throughput nanofabrication of single NV centers on sub-100 nm length scales. Secondary ion mass spectroscopy (SIMS) measurements facilitate depth profiling of the implanted nitrogen to provide three-dimensional characterization of the NV center spatial distribution. Measurements of NV center coherence with on-chip coplanar waveguides suggest a pathway for incorporating this scalable nanofabrication technique in future quantum applications., Comment: This paper has been withdrawn by the authors. 14 pages, 3 figures; Posting has been removed due to editorial request from ACS Nano Letters; This version has been removed by arXiv admin because it contains an inappropriate withdrawal notice