Coherent Erbium Spin Defects in Colloidal Nanocrystal Hosts.

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, which 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.

Nanocavity-Mediated Purcell Enhancement of Er in TiO2 Thin Films Grown via Atomic Layer Deposition.

The use of trivalent erbium (Er3+), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunication 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 make 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 (TiO2) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping controls 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 TiO2. 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, nondestructive, 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.

Magnon-mediated qubit coupling determined via dissipation measurements.

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.

Deterministic nanoscale quantum spin-defect implantation and diffraction strain imaging.

Local crystallographic features negatively affect quantum spin defects by changing the local electrostatic environment, often resulting in degraded or varied qubit optical and coherence properties. Few tools exist that enable the deterministic synthesis and study of such intricate systems on the nano-scale, making defect-to-defect strain environment quantification difficult. In this paper, we highlight state-of-the-art capabilities from the U.S. Department of Energy's Nanoscale Science Research Centers that directly address these shortcomings. Specifically, we demonstrate how complementary capabilities of nano-implantation and nano-diffraction can be used to demonstrate the quantum relevant, spatially deterministic creation of neutral divacancy centers in 4H silicon carbide, while investigating and characterizing these systems on the≤25nmscale with strain sensitivities on the order of1×10-6,relevant to defect formation dynamics. This work lays the foundation for ongoing studies into the dynamics and deterministic formation of low strain homogeneous quantum relevant spin defects in the solid state.

Purcell Enhancement of Erbium Ions in TiO2 on Silicon Nanocavities.

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. Moreover, 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 toward 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 × 104 and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step toward realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies.

Generalized scaling of spin qubit coherence in over 12,000 host materials.

SignificanceAtomic defects in solid-state materials are promising candidates as quantum bits, or qubits. New materials are actively being investigated as hosts for new defect qubits; however, there are no unifying guidelines that can quantitatively predict qubit performance in a new material. One of the most critical property of qubits is their quantum coherence. While cluster correlation expansion (CCE) techniques are useful to simulate the coherence of electron spins in defects, they are computationally expensive to investigate broad classes of stable materials. Using CCE simulations, we reveal a general scaling relation between the electron spin coherence time and the properties of qubit host materials that enables rapid and quantitative exploration of new materials hosting spin defects.

Five-second coherence of a single spin with single-shot readout in silicon carbide.

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 postselection, resulting in a high signal-to-noise ratio 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 > 5 seconds, 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.

Tunable and Transferable Diamond Membranes for Integrated Quantum Technologies.

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 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 line widths 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 and 400 µs, respectively. This platform enables the straightforward integration of diamond membranes that host coherent color centers into quantum technologies.

Tunable Cr4+ Molecular Color Centers.

The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. Here, we demonstrate that the electronic structure that enables optical-spin initialization and readout for S = 1, Cr(aryl)4, where aryl = 2,4-dimethylphenyl (1), o-tolyl (2), and 2,3-dimethylphenyl (3), is readily translated into Cr(alkyl)4 compounds, where alkyl = 2,2,2-triphenylethyl (4), (trimethylsilyl)methyl (5), and cyclohexyl (6). The small ground state zero field splitting values (<5 GHz) for 1-6 allowed for coherent spin manipulation at X-band microwave frequency, enabling temperature-, concentration-, and orientation-dependent investigations of the spin dynamics. Electronic absorption and emission spectroscopy confirmed the desired electronic structures for 4-6, which exhibit photoluminescence from 897 to 923 nm, while theoretical calculations elucidated the varied bonding interactions of the aryl and alkyl Cr4+ compounds. The combined experimental and theoretical comparison of Cr(aryl)4 and Cr(alkyl)4 systems illustrates the impact of the ligand field on both the ground state spin structure and excited state manifold, laying the groundwork for the design of structurally precise optically addressable molecular qubits.

Parasitic erbium photoluminescence in commercial telecom fiber optical components.

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 amorphous material transmitting infrared radiation 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.

Trigonal Bipyramidal V3+ Complex as an Optically Addressable Molecular Qubit Candidate.

Synthetic chemistry enables a bottom-up approach to quantum information science, where atoms can be deterministically positioned in a quantum bit or qubit. Two key requirements to realize quantum technologies are qubit initialization and read-out. By imbuing molecular spins with optical initialization and readout mechanisms, analogous to solid-state defects, molecules could be integrated into existing quantum infrastructure. To mimic the electronic structure of optically addressable defect sites, we designed the spin-triplet, V3+ complex, (C6F5)3trenVCNtBu (1). We measured the static spin properties as well as the spin coherence time of 1 demonstrating coherent control of this spin qubit with a 240 GHz electron paramagnetic resonance spectrometer powered by a free electron laser. We found that 1 exhibited narrow, near-infrared photoluminescence (PL) from a spin-singlet excited state. Using variable magnetic field PL spectroscopy, we resolved emission into each of the ground-state spin sublevels, a crucial component for spin-selective optical initialization and readout. This work demonstrates that trigonally symmetric, heteroleptic V3+ complexes are candidates for optical spin addressability.

Entanglement and control of single nuclear spins in isotopically engineered silicon carbide.

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 that 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 (Hahn-echo T2 = 2.3 ms, dynamical decoupling T2DD > 14.5 ms), and a >40-fold increase in Ramsey spin dephasing time (T2*) from isotopic purification. Overall, this work underlines the importance of controlling the nuclear environment in solid-state systems and links single photon emitters with nuclear registers in an industrially scalable material.

Universal coherence protection in a solid-state spin qubit.

Decoherence limits the physical realization of qubits, and its mitigation is critical for the development of quantum science and technology. We construct a robust qubit embedded in a decoherence-protected subspace, obtained by applying microwave dressing to a clock transition of the ground-state electron spin of a silicon carbide divacancy defect. The qubit is universally 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 more than 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.

Vanadium spin qubits as telecom quantum emitters in silicon carbide.

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, with brightness allowing cavity-free detection in a wafer-scale material. In vanadium ensembles, we characterize the complex d 1 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. Last, we demonstrate coherent quantum control of the spin state. These results provide a path for telecom emitters in the solid state for quantum applications.

High-Q Nanophotonic Resonators on Diamond Membranes using Templated Atomic Layer Deposition of TiO2.

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.

Purcell Enhancement of a Single Silicon Carbide Color Center with Coherent Spin Control.

Silicon carbide has recently been developed as a platform for optically addressable spin defects. In particular, the neutral divacancy in the 4H polytype displays an optically addressable spin-1 ground state and near-infrared optical emission. Here, we present the Purcell enhancement of a single neutral divacancy coupled to a photonic crystal cavity. We utilize a combination of nanolithographic techniques and a dopant-selective photoelectrochemical etch to produce suspended cavities with quality factors exceeding 5000. Subsequent coupling to a single divacancy leads to a Purcell factor of ∼50, which manifests as increased photoluminescence into the zero-phonon line and a shortened excited-state lifetime. Additionally, we measure coherent control of the divacancy ground-state spin inside the cavity nanostructure and demonstrate extended coherence through dynamical decoupling. This spin-cavity system represents an advance toward scalable long-distance entanglement protocols using silicon carbide that require the interference of indistinguishable photons from spatially separated single qubits.

Electrical and optical control of single spins integrated in scalable semiconductor devices.

Spin defects in silicon carbide have the advantage of exceptional electron spin coherence combined with a near-infrared spin-photon interface, all in a material amenable to modern semiconductor fabrication. Leveraging these advantages, we integrated highly coherent single neutral divacancy spins in commercially available p-i-n structures and fabricated diodes to modulate the local electrical environment of the defects. These devices enable deterministic charge-state control and broad Stark-shift tuning exceeding 850 gigahertz. We show that charge depletion results in a narrowing of the optical linewidths by more than 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 using classical semiconductor devices to control scalable, spin-based quantum systems.

Stabilization of point-defect spin qubits by quantum wells.

Defect-based quantum systems in wide bandgap semiconductors are strong candidates for scalable quantum-information technologies. However, these systems are often complicated by charge-state instabilities and interference by phonons, which can diminish spin-initialization fidelities and limit room-temperature operation. Here, we identify a pathway around these drawbacks by showing that an engineered quantum well can stabilize the charge state of a qubit. Using density-functional theory and experimental synchrotron X-ray diffraction studies, we construct a model for previously unattributed point defect centers in silicon carbide as a near-stacking fault axial divacancy and show how this model explains these defects' robustness against photoionization and room temperature stability. These results provide a materials-based solution to the optical instability of color centers in semiconductors, paving the way for the development of robust single-photon sources and spin qubits.

Electrically driven optical interferometry with spins in silicon carbide.

Interfacing solid-state defect electron spins to other quantum systems is an ongoing challenge. The ground-state spin's weak coupling to its environment not only 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-Stückelberg interference fringes in the resonant optical absorption spectrum. In addition, 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.

Microscale-Resolution Thermal Mapping Using a Flexible Platform of Patterned Quantum Sensors.

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 its 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 constructing 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, with the potential for quantum computing applications, to denser devices with 98 ± 0.8% yield and stronger photoluminescence signals, ideal for temperature measurements. With these, we experimentally reconstruct the temperature map of an operating coplanar waveguide to confirm the accuracy of these platforms.