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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

We detail several scientific and engineering innovations which enable the controlled spalling of 10 - 50 micron thick films of single crystal 4H silicon carbide (4H-SiC) from bulk substrates. 4H-SiC's properties, including high thermal conductivity and a wide bandgap, make it an ideal candidate for high-temperature, high-voltage power electronic devices. Moreover, 4H-SiC has been shown to be an excellent host of solid-state atomic defect qubits for quantum computing and quantum networking. Because 4H-SiC single crystal substrates are expensive (due to long growth times and limited yield), techniques for removal and transfer of bulk-quality films in the tens-of-microns thickness range are highly desirable to allow for substrate reuse and integration of the separated films. In this work we utilize novel approaches for stressor layer thickness control and spalling crack initiation to demonstrate controlled spalling of 4H-SiC, the highest fracture toughness material spalled to date. Additionally, we demonstrate substrate re-use, bonding of the spalled films to carrier substrates, and explore the spin coherence of the spalled films. In preliminary studies we are able to achieve coherent spin control of neutral divacancy ($VV^{0}$) qubit ensembles and measure a quasi-bulk spin $T_{2}$ of 79.7 $\mu$s in such spalled films., Comment: 16 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.

Two dimensional (2D) semiconductors present unique opportunities to intertwine optical and magnetic functionalities and to tune these performances through defects and dopants. In 2D semiconductors, the properties of excitons often vary due to the underlying magnetic order, but the modification of their magnetic properties by excitonic processes remains difficult to achieve. Here, we integrate exciton pumping into a quantum sensing protocol on nitrogen-vacancy centers in diamond to image the optically-induced transient stray fields in few-layer, antiferromagnetic CrCl$_3$. We discover that exciton recombination enhances the in-plane magnetization of the CrCl$_3$ layers, with an outsized effect in the surface monolayers and when the surface is unencapsulated. Concomitantly, time-resolved photoluminescence measurements reveal that a defect-assisted Auger recombination dominates for atomically thin CrCl$_3$ with tightly localized, nearly forbidden excitons and amplified surface-to-volume ratio. These experimental signatures establish the magnetically enhanced state to result from an exciton-activated electron transfer between surface impurities and the spin-polarized conduction band. Density functional theory calculations identify that the mediating impurity state could originate from oxygen adsorbates with spins antiparallel to the magnetization of their host layer. Our work unambiguously demonstrates the tunability of single intrinsic magnetic layers via defect engineering and opens a pathway to dynamically reconfigure these effects in devices through optical control., Comment: 9 pages, 6 figures

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

Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies such as quantum memory, due to the intrinsic spin-photon interface of the rare-earth ion combined with the integration methods available in the solid-state. Erbium-doped cerium oxide (Er:CeO$_2$) is a particularly promising platform for such a quantum memory, as it combines the telecom-wavelength (~1.5 $\mu$m) 4f-4f transition of erbium, a predicted long electron spin coherence time supported by CeO$_2$, and is also near lattice-matched to silicon for heteroepitaxial growth. In this work, we report on the epitaxial growth of Er:CeO$_2$ thin films on silicon using molecular beam epitaxy (MBE), with controlled erbium concentration down to 2 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO$_2$ host structure, and characterize the spin and optical properties of the embedded Er$^{3+}$ ions. In the 2-3 ppm Er regime, we identify EPR linewidths of 245(1) MHz, optical inhomogeneous linewidths of 9.5(2) GHz, optical excited state lifetimes of 3.5(1) ms, and spectral diffusion-limited homogenoeus linewidths as narrow as 4.8(3) MHz in the as-grown material. We test annealing of the Er:CeO$_2$ films up to 900 deg C, which yields modest narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%. We have also studied the variation of the optical properties as a function of Er doping and find that the results are consistent with the trends expected from inter-dopant charge interactions., Comment: 15 pages, 6 figures (including supplemental information)

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

Rare-earth ions (REI) have emerged as an attractive candidate for solid-state qubits, particularly as a quantum memory. Their 4f-4f transitions are shielded by filled 5s and 5p orbitals, offering a degree of protection from external electric fields. Embedded within a thin film oxide host, REIs could enable a qubit platform with significant memory capabilities. Furthermore, a silicon-compatible thin film form factor would enable the use of standard semiconductor fabrication processes to achieve chip-based integrability and scalability for functional quantum networks. Towards this goal, we have carried out optical and microstructural studies of erbium-doped polycrystalline and epitaxial TiO$_2$ thin films on Si (100), r-sapphire, and SrTiO$_3$ (100). We observe that the inhomogeneous optical linewidth of the Er photoluminescence is comparable or better for polycrystalline Er:TiO$_2$(grown on Si) in comparison to single crystal epitaxial films on sapphire or SrTiO$_3$, implying a relative insensitivity to extended defects. We investigated the effect of the film/substrate and film/air interface and found that the inhomogeneous linewidth and spectral diffusion can be significantly improved via bottom buffer and top capping layers of undoped TiO$_2$. Using such approaches, we obtain inhomogeneous linewidths of 5.2 GHz and spectral diffusion of 180 MHz in Er:TiO$_2$ /Si(100) films and have demonstrated the engineerability of quantum-relevant properties in these thin films., Comment: 13 pages, 6 figures; corrects the units for spectral diffusion values (MHz throughout the manuscript instead of GHz(typo) in some places)

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.

We excite the gyrotropic mode of a magnetic vortex and observe the resulting effect on the spin state of a nearby nitrogen-vacancy (NV) defect in diamond. Thin permalloy disks fabricated on a diamond sample are magnetized in a vortex state in which the magnetization curls around a central core. The magnetization dynamics of this configuration are described by a discrete spectrum of confined magnon modes, as well as a low-frequency gyrotropic mode in which the vortex core precesses about its equilibrium position. Despite the spin transition frequencies being far-detuned from the modes of the ferromagnet, we observe enhanced relaxation of the NV spin when driving the gyrotropic mode. Moreover, we map the spatial dependence of the interaction between the vortex and the spin by translating the vortex core within the disk with an applied magnetic field, resulting in steplike motion as the vortex is pinned and de-pinned. The strong spin relaxation is observed when the vortex core is within approximately 250 nm of the NV center defect. We attribute this effect to the higher frequencies in the spectrum of the magnetic fringe field arising from the soliton-like nature of the gyrotropic mode when driven with sufficiently large amplitude., Comment: 7 pages, 5 figures

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

This paper demonstrates the first beam resonators fabricated from bulk high purity semi-insulating 4H Silicon Carbide wafers (HPSI 4H-SiC). Our innovations include: (1) Multi-level front-side, back-side inductively coupled plasma-deep reactive ion etching (ICP-DRIE) technology to fabricate thin, low-mass, bending-mode resonators framed by the SiC substrate (2) Laser Doppler Vibrometer (LDV) measurements of mechanical quality factors (Q) > 10,000 with frequencies ranging from 300 kHz to 8MHz and (3) Calculated uniaxial in-plane surface stress 20 MPa at top surface of resonator base when operating at resonance in vacuum., Comment: 4 pages, 5 figures, 1 table. Conference paper for Transducers 2019

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

In this two-part article series we provide a generalized description of the scattering geometry of Bragg coherent diffraction imaging (BCDI) experiments, the shear distortion effects inherent to the resulting three-dimensional (3D) image from current phase retrieval methods and strategies to mitigate this distortion. In this Part I, we derive in general terms the real-space coordinate transformation to correct this shear, which originates in the more fundamental relationship between the representations of mutually conjugate 3D spaces. Such a transformation, applied as a final post-processing step following phase retrieval, is crucial for arriving at an un-distorted and physically meaningful image of the 3D scatterer. As the relevance of BCDI grows in the field of materials characterization, we take this opportunity to generalize the available sparse literature that addresses the geometric theory of BCDI and the subsequent analysis methods. This aspect, specific to coherent Bragg diffraction and absent in two-dimensional transmission CDI experiments, gains particular importance concerning spatially-resolved characterization of 3D crystalline materials in a realiable, non-destructive manner. These articles describe this theory, from the diffraction in Bragg geometry, to the corrections needed to obtain a properly rendered digital image of the 3D scatterer. Part I provides the experimental BCDI communitcy with the theoretical underpinnings of the 3D real-space distortions in the phase-retrieved object, along with the necessary post-retrieval correction method. Part II builds upon the geometric theory developed in Part I with the formalism to correct the shear distortions directly on an orthogonal grid within the phase retrieval algorithm itself, allowing more physically realistic constraints to be applied., Comment: Double-spaced, 31 pages, 4 figures, 1 table, under review

Sensing electric fields with high sensitivity, high spatial resolution and at radio frequencies can be challenging to realize. Recently, point defects in silicon carbide have shown their ability to measure local electric fields by optical charge conversion of their charge state. Here we report the combination of heterodyne detection with charge-based electric field sensing, solving many of the previous limitations of this technique. Owing to the non-linear response of the charge conversion to electric fields, the application of a separate "pump" electric field results in a detection sensitivity as low as 1.1 (V/cm)/$\sqrt{Hz}$, with near-diffraction limited spatial resolution and tunable control of the sensor dynamic range. In addition, we show both incoherent and coherent heterodyne detection, allowing measurements of either unknown random fields or synchronized fields with higher sensitivities. Finally, we demonstrate in-plane vector measurements of the electric field by combining orthogonal pump electric fields. Overall, this work establishes charge-based measurements as highly relevant for solid-state defect sensing., Comment: 7 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

Temperature sensors with micro- and nanoscale spatial resolution have long been explored for their potential to investigate the details of physical systems at an unprecedented scale. In particular, the rapid miniaturization of transistor technology, with the associated steep boost in power density, calls for sensors that accurately monitor heating distributions. Here, we report on a simple and scalable fabrication approach, based on directed self-assembly and transfer printing techniques, to construct arrays of nanodiamonds containing temperature sensitive fluorescent spin defects. The nanoparticles are embedded within a low thermal conductivity matrix that allows for repeated use on a wide range of systems with minimal spurious effects. Additionally, we demonstrate access to a wide spectrum of array parameters ranging from sparser single particle arrays to denser devices with approximately 100 % yield and stronger photoluminescence signal, ideal for temperature measurements. With these we experimentally reconstruct the temperature map of an operating coplanar waveguide to confirm the accuracy of these platforms., Comment: 15 pages, 4 figures

We exploit the high-symmetry spin state obtained for equal Rashba and linear Dresselhaus interactions to derive a closed-form expression for the weak localization magnetoconductivity -- the paradigmatic signature of spin-orbit coupling in quantum transport. The small parameter of the theory is the deviation from the symmetry state introduced by the mismatch of the linear terms and by the cubic Dresselhaus term. In this regime, we perform quantum transport experiments in GaAs quantum wells. Top and back gates allow independent tuning of the Rashba and Dresselhaus terms in order to explore the broken-symmetry regime where the formula applies. We present a reliable two-step method to extract all parameters from fits to the new expression, obtaining excellent agreement with recent experiments. This provides experimental confirmation of the new theory, and advances spin-orbit coupling towards a powerful resource in emerging quantum technologies., Comment: 13 pages, 6 figures, supplementary included on arXiv

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

Circularly polarized photons are known to generate a directional helicity-dependent photocurrent in three-dimensional topological insulators at room temperature. Surprisingly, the phenomenon is readily observed at photon energies that excite electrons to states far above the spin-momentum locked Dirac cone and the underlying mechanism for the helicity-dependent photocurrent is still not understood. We resolve the puzzle through a comprehensive study of the helicity-dependent photocurrent in (Bi,Sb)_2Te_3 thin films as a function of the incidence angle of the optical excitation, its wavelength, and the gate-tuned chemical potential. Our observations allow us to unambiguously identify the circular photo-galvanic effect as the dominant mechanism for the helicity-dependent photocurrent. Additionally, we use an analytical calculation to relate the directional nature of the photocurrent to asymmetric optical transitions between the topological surface states and bulk bands. The insights we obtain are important for engineering opto-spintronic devices that rely on optical steering of spin and charge currents.

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)

Many proposed experiments involving topological insulators (TIs) require spatial control over time-reversal symmetry and chemical potential. We demonstrate reconfigurable micron-scale optical control of both magnetization (which breaks time-reversal symmetry) and chemical potential in ferromagnetic thin films of Cr-(Bi,Sb)$_2$Te$_3$ grown on SrTiO$_3$. By optically modulating the coercivity of the films, we write and erase arbitrary patterns in their remanent magnetization, which we then image with Kerr microscopy. Additionally, by optically manipulating a space charge layer in the underlying SrTiO$_3$ substrates, we control the local chemical potential of the films. This optical gating effect allows us to write and erase p-n junctions in the films, which we study with photocurrent microscopy. Both effects are persistent and may be patterned and imaged independently on a few-micron scale. Dynamic optical control over both magnetization and chemical potential of a TI may be useful in efforts to understand and control the edge states predicted at magnetic domain walls in quantum anomalous Hall insulators., Comment: 15 pages, 5 figures

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 Rashba and Dresselhaus spin-orbit (SO) interactions in 2D electron gases act as effective magnetic fields with momentum-dependent directions, which cause spin decay as the spins undergo arbitrary precessions about these randomly-oriented SO fields due to momentum scattering. Theoretically and experimentally, it has been established that by fine-tuning the Rashba $\alpha$ and Dresselhaus $\beta$ couplings to equal $\it{fixed}$ strengths $\alpha=\beta$, the total SO field becomes unidirectional thus rendering the electron spins immune to dephasing due to momentum scattering. A robust persistent spin helix (PSH) has already been experimentally realized at this singular point $\alpha=\beta$. Here we employ the suppression of weak antilocalization as a sensitive detector for matched SO fields together with a technique that allows for independent electrical control over the SO couplings via top gate voltage $V_T$ and back gate voltage $V_B$. We demonstrate for the first time the gate control of $\beta$ and the $\it{continuous\,locking}$ of the SO fields at $\alpha=\beta$, i.e., we are able to vary both $\alpha$ and $\beta$ controllably and continuously with $V_T$ and $V_B$, while keeping them locked at equal strengths. This makes possible a new concept: "stretchable PSHs", i.e., helical spin patterns with continuously variable pitches $P$ over a wide parameter range. The extracted spin-diffusion lengths and decay times as a function of $\alpha/\beta$ show a significant enhancement near $\alpha/\beta=1$. Since within the continuous-locking regime quantum transport is diffusive (2D) for charge while ballistic (1D) for spin and thus amenable to coherent spin control, stretchable PSHs could provide the platform for the much heralded long-distance communication $\sim 8 - 25$ $\mu$m between solid-state spin qubits., Comment: 5 color figures, with supplementary info available on arXiv. arXiv admin note: substantial text overlap with arXiv:1403.3518