Spin Defects Research Articles

Extending radiowave frequency detection range with dressed states of solid-state spin ensembles

Quantum sensors using solid-state spin defects excel in the detection of radiofrequency (RF) fields, serving various applications in communication, ranging, and sensing. For this purpose, pulsed dynamical decoupling (PDD) protocols are typically applied, which enhance sensitivity to RF signals. However, these methods are limited to frequencies of a few megahertz, which poses a challenge for sensing higher frequencies. We introduce an alternative approach based on a continuous dynamical decoupling (CDD) scheme involving dressed states of nitrogen vacancy (NV) ensemble spins driven within a microwave resonator. We compare the CDD methods to established PDD protocols and demonstrate the detection of RF signals up to ~85 MHz, about ten times the current limit imposed by the PDD approach under identical conditions. Implementing the CDD method in a heterodyne/synchronized protocol combines the high-frequency detection with high spectral resolution. This advancement extends to various domains requiring detection in the high frequency (HF) and very high frequency (VHF) ranges of the RF spectrum, including spin sensor-based magnetic resonance spectroscopy at high magnetic fields.

Investigation of PCVSi− defect in 4H–SiC as a candidate for a qubit

Abstract Exploration of spin defects in semiconductors for possible qubits encourages the development of the quantum field. Silicon carbide (SiC) is a suitable platform to carry spin defects, due to its excellent electrical, mechanical and optical properties, together with its convenience for crystallographic growth and doping processes. In this study, a negatively charged phosphorus-vacancy (PCVSi −) defect, consisting of a silicon vacancy and nearby substitution of a phosphorus atom to a carbon atom in 4H–SiC, is investigated by first-principles calculations. This defect is demonstrated to possess a high spin (S = 1) with relatively low formation energy. Computed zero-phonon line energy and zero-field splitting parameters of this defect are close to those of neutral divacancy (VCVSi 0), negatively charged nitrogen-vacancy center (NCVSi −) and some other color centers, which indicate a similarity of both optical and spin properties among them. Moreover, the electron spin coherence time of this defect turns out to be 1.15–1.40 ms. Such a long coherence time provides the defect with reliability for quantum information processing. Our results show that the PCVSi − defect can be a promising candidate for a qubit.

Precision multi-mode microwave spectroscopy of paramagnetic and rare-earth ion spin defects in single crystal calcium tungstate

We present experimental observations of dilute ion spin ensemble defects in a low-loss single crystal cylindrical sample of CaWO4 cooled to 30 mK in temperature. Crystal field perturbations were elucidated by constructing a dielectrically loaded microwave cavity resonator from the crystal. The resonator exhibited numerous whispering gallery modes with high Q-factors of up to 3×107, equivalent to a loss tangent of ∼3×10−8. The low loss allowed precision multi-mode spectroscopy of numerous high Q-factor photon–spin interactions. Measurements between 7 and 22 GHz revealed the presence of Gd3+, Fe3+, and another trace species, inferred to be rare-earth, at concentrations on the order of parts per billion. These findings motivate further exploration of prospective uses of this low-loss dielectric material for applications regarding precision and quantum metrology, as well as tests for beyond standard model physics.

Transition-Metal-Related Quantum Emitters in Wurtzite AlN and GaN.

Transition-metal centers exhibit a paramagnetic ground state in wide-bandgap semiconductors and are promising for nanophotonics and quantum information processing. Specifically, there is a growing interest in discovering prominent paramagnetic spin defects that can be manipulated using optical methods. Here, we investigate the electronic structure and magneto-optical properties of Cr and Mn substitutional centers in wurtzite AlN and GaN. We use state-of-the-art hybrid density functional theory calculations to determine level structure, stability, optical signatures, and magnetic properties of these centers. The excitation energies are calculated using the constrained occupation approach and rigorously verified with the complete active space configuration interaction approach. Our simulations of the photoluminescence spectra indicate that in AlN and in GaN are responsible for the observed narrow quantum emission near 1.2 eV. We compute the zero-field splitting (ZFS) parameters and outline an optical spin polarization protocol for and . Our results demonstrate that these centers are promising candidates for spin qubits.

Engineering Boron Vacancy Defects in Boron Nitride Nanotubes.

Spin defects in hexagonal boron nitride (hBN) are emerging as promising platforms for quantum sensing applications. In particular, the negatively charged boron vacancy (VB-) centers have been engineered in bulk hBN and few-layer hBN flakes, and employed for sensing. Here, we investigate the engineering of VB- spin defects in boron nitride nanotubes (BNNTs). The generated spin defects are distributed along and around the BNNTs. Moreover, in contrast to hBN flakes, the spins in BNNTs exhibit a directional response relative to the direction of a surrounding magnetic field, which is consistent with the tubular geometry. The unique geometry of BNNTs allows for a more controlled and predictable placement of spin defects compared to bulk hBN, paving the way for innovative sensing applications with high spatial resolution and optomechanical studies of spin defects in hBN.

Detecting and Imaging of Magnons at Nanoscale with van der Waals Quantum Sensor

AbstractMagnonic devices are extensively studied for energy‐efficient information processing. High spatial resolution and high accuracy measurement is required to characterize the excitation and distribution of magnons. Here, sensing and imaging of magnons in the magnetic insulator (YIG) is realized with negatively charged boron vacancy () spin defects in 2D hexagonal boron nitride (hBN). Thermal magnon noise is studied through spin relaxometry, illustrating the nanometers proximity of the 2D quantum sensor over a large area. The small probe‐sample standoff distance helps to detect weak signals with diffraction‐limited spatial resolution. The uniform out‐of‐plane symmetry axis of is further utilized to study perpendicular magnetic anisotropy (PMA). It effectively extracts the stray field of microwave‐excited magnons from the direct stripline field. The distributions of propagating and localized magnons in different structures are subsequently imaged and analyzed. The work provides the strategy for utilizing the distinctive advantages of the van der Waals quantum sensor in magnetic imaging. The results will promote the development of magnonic devices for diverse applications.

Quantum Spin Probe of Single Charge Dynamics.

Electronic defects in semiconductors form the basis for emerging quantum technologies, but many defect centers are difficult to access at the single-particle level. 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 the charge populations and dynamics of single substitutional nitrogen spin defects in diamond. By probing their steady-state spin population, read out at the single-defect level with a nearby nitrogen vacancy center, we directly measure the defect ionization-corroborated by first-principles calculations-an effect we do not have access to with traditional coherence-based quantum sensing.

Defect-induced localization of information scrambling in 1D Kitaev model

We discuss one-dimensional(1D) spin compass model or 1D Kitaev model in the presence of local bond defects. Three types of local disorders concerning both bond-nature and bond-strength that occur on kitaev materials have been investigated. Using exact diagonalization, two-point spin-spin structural correlations and four-point Out-of-Time-Order Correlators(OTOC) have been computed for the defective spin chains. The proposed quantities give signatures of these defects in terms of their responses to location and strength of defects. A key observation is that the information scrambling in the OTOC space gets trapped at the defect site giving rise to the phenomena of localization of information scrambling thus making these correlators a suitable diagnostic tool to detect and characterize these defects.

Nanotube spin defects for omnidirectional magnetic field sensing

Optically addressable spin defects in three-dimensional (3D) crystals and two-dimensional (2D) van der Waals (vdW) materials are revolutionizing nanoscale quantum sensing. Spin defects in one-dimensional (1D) vdW nanotubes will provide unique opportunities due to their small sizes in two dimensions and absence of dangling bonds on side walls. However, optically detected magnetic resonance of localized spin defects in a nanotube has not been observed. Here, we report the observation of single spin color centers in boron nitride nanotubes (BNNTs) at room temperature. Our findings suggest that these BNNT spin defects possess a spin S = 1/2 ground state without an intrinsic quantization axis, leading to orientation-independent magnetic field sensing. We harness this unique feature to observe anisotropic magnetization of a 2D magnet in magnetic fields along orthogonal directions, a challenge for conventional spin S = 1 defects such as diamond nitrogen-vacancy centers. Additionally, we develop a method to deterministically transfer a BNNT onto a cantilever and use it to demonstrate scanning probe magnetometry. Further refinement of our approach will enable atomic scale quantum sensing of magnetic fields in any direction.

Local Diagnostics of Spin Defects in Irradiated SiC Schottky Diodes

Local Diagnostics of Spin Defects in Irradiated SiC Schottky Diodes

Laser Beam Induced Charge Collection for Defect Mapping and Spin State Readout in Diamond

Laser Beam Induced Charge Collection for Defect Mapping and Spin State Readout in Diamond

(Invited) Tackling Interface Challenges for Shallow Diamond Color Centers

Spin defects in wide-bandgap semiconductors, such as color centers in diamond, can be highly sensitive to local (nanoscale) changes in magnetic field, temperature, and strain. These solid-state quantum sensors have certain advantages over their atomic counterparts owing to their room-temperature operation without the need for vacuum components and the relative ease of photonic- and RF-component integration. However, near-surface quantum defects exhibit spin decoherence and most of the light emitted is trapped within the bulk crystal due total internal reflection at the interface. In this presentation, I will summarize our recent work towards better understanding and addressing these interface challenges, including the modeling and experimental characterization of radiative emission of near-surface emitters, design of nanophotonic components to improve light extraction, and surface analysis and chemical termination techniques aimed at improving spin coherence of emitters.

Multi-species optically addressable spin defects in a van der Waals material

Optically addressable spin defects hosted in two-dimensional van der Waals materials represent a new frontier for quantum technologies, promising to lead to a new class of ultrathin quantum sensors and simulators. Recently, hexagonal boron nitride (hBN) has been shown to host several types of optically addressable spin defects, thus offering a unique opportunity to simultaneously address and utilise various spin species in a single material. Here we demonstrate an interplay between two separate spin species within a single hBN crystal, namely S = 1 boron vacancy defects and carbon-related electron spins. We reveal the S = 1/2 character of the carbon-related defect and further demonstrate room temperature coherent control and optical readout of both S = 1 and S = 1/2 spin species. By tuning the two spin ensembles into resonance with each other, we observe cross-relaxation indicating strong inter-species dipolar coupling. We then demonstrate magnetic imaging using the S = 1/2 defects and leverage their lack of intrinsic quantization axis to probe the magnetic anisotropy of a test sample. Our results establish hBN as a versatile platform for quantum technologies in a van der Waals host at room temperature.

Developing 3D Models of Atom-Like Defect Spin Memories in Crystals for Quantum Technology Research and Education

Developing 3D Models of Atom-Like Defect Spin Memories in Crystals for Quantum Technology Research and Education

Interplay between charge and spin noise in the near-surface theory of decoherence and relaxation of C3v symmetry qutrit spin-1 centers

Decoherence and relaxation of solid-state defect qutrits near a crystal surface, where they are commonly used as quantum sensors, originate from charge and magnetic field noise. A complete theory requires a formalism for decoherence and relaxation that includes all Hamiltonian terms allowed by the defect's point-group symmetry. This formalism, presented here for the C3v symmetry of a spin-1 defect in a diamond, silicon carbide, or similar host, relies on a Lindblad dynamical equation and clarifies the relative contributions of charge and spin noise to relaxation and decoherence, along with their dependence on the defect spin's depth and resonant frequencies. The calculations agree with the experimental measurements of Sangtawesin [], and corroborate the importance of charge noise. Published by the American Physical Society 2024

Quantum emitters in aluminum nitride induced by heavy ion irradiation

The integration of solid-state single-photon sources with foundry-compatible photonic platforms is crucial for practical and scalable quantum photonic applications. This study explores aluminum nitride (AlN) as a material with properties highly suitable for integrated on-chip photonics and the ability to host defect-center related single-photon emitters. We have conducted a comprehensive analysis of the creation of single-photon emitters in AlN, utilizing heavy ion irradiation and thermal annealing techniques. Subsequently, we have performed a detailed analysis of their photophysical properties. Guided by theoretical predictions, we assessed the potential of Zirconium (Zr) ions to create optically addressable spin defects and employed Krypton (Kr) ions as an alternative to target lattice defects without inducing chemical doping effects. With a 532 nm excitation wavelength, we found that single-photon emitters induced by ion irradiation were primarily associated with vacancy-type defects in the AlN lattice for both Zr and Kr ions. The density of these emitters increased with ion fluence, and there was an optimal value that resulted in a high density of emitters with low AlN background fluorescence. Under a shorter excitation wavelength of 405 nm, Zr-irradiated AlN exhibited isolated point-like emitters with fluorescence in the spectral range theoretically predicted for spin-defects. However, similar defects emitting in the same spectral range were also observed in AlN irradiated with Kr ions as well as in as-grown AlN with intrinsic defects. This result is supportive of the earlier theoretical predictions, but at the same time highlights the difficulties in identifying the sought-after quantum emitters with interesting properties related to the incorporation of Zr ions into the AlN lattice by fluorescence alone. The results of this study largely contribute to the field of creating quantum emitters in AlN by ion irradiation and direct future studies emphasizing the need for spatially localized Zr implantation and testing for specific spin properties.

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.

Performance optimization of FeSiCr/ZnO soft magnetic composites by highly orientation and domain wall engineering

The power loss and permeability of soft magnetic composite (SMC) might be improved by surface modification and magnetic field orientation of flake particles. The oriented ZnO-modified flaky FeSiCr SMCs were produced under the magnetic field. The orienting mechanism of flake powder under a magnetic field produced by Helmholtz coils was investigated using torque model analysis. After surface modification, the permeability and power loss of ZnO-modified flaky FeSiCr SMCs could reach 63 and 421.29 kW/m3(at 50 mT, 100 kHz), respectively. The three-dimensional loss separation results demonstrate that spin rotation mechanism, defects, and dislocations of ZnO modification from theory and experiment may be responsible for the enhanced soft magnetic characteristics.

Manipulating carbon related spin defects in boron nitride by changing the MOCVD growth temperature

A common solution for precise magnetic field sensing is to employ spin-active defects in semiconductors, with the NV center in diamond as a prominent example. However, the three-dimensional nature of diamond limits the obtainable proximity of the defect to the sample. Two-dimensional boron nitride, which can host spin-active defects, can be used to overcome those limitations. In this work, we study spin properties of sp2-bonded boron nitride layers grown using Metal Organic Chemical Vapor Deposition at temperatures ranging from 700 °C to 1200 °C. With Electron Spin Resonance (ESR) we show that our layers exhibit spin properties, which we ascribe to carbon related defects. Supported by photoluminescence and Fourier-transform infrared spectroscopy, we distinguish three different regimes: (i) growth at low temperatures with no ESR signal, (ii) growth at intermediate temperatures with a strong ESR signal and a large number of spin defects, (iii) growth at high temperatures with a weaker ESR signal and a lower number of spin defects. The observed effects can be further enhanced by an additional annealing step. Our studies demonstrate wafer-scale boron nitride that intrinsically hosts spin defects without any ion or neutron irradiation, which may be employed in spin memories or magnetic field detectors.

Discovery of atomic clock-like spin defects in simple oxides from first principles

Virtually noiseless due to the scarcity of spinful nuclei in the lattice, simple oxides hold promise as hosts of solid-state spin qubits. However, no suitable spin defect has yet been found in these systems. Using high-throughput first-principles calculations, we predict spin defects in calcium oxide with electronic properties remarkably similar to those of the NV center in diamond. These defects are charged complexes where a dopant atom — Sb, Bi, or I — occupies the volume vacated by adjacent cation and anion vacancies. The predicted zero phonon line shows that the Bi complex emits in the telecommunication range, and the computed many-body energy levels suggest a viable optical cycle required for qubit initialization. Notably, the high-spin nucleus of each dopant strongly couples to the electron spin, leading to many controllable quantum levels and the emergence of atomic clock-like transitions that are well protected from environmental noise. Specifically, the Hanh-echo coherence time increases beyond seconds at the clock-like transition in the defect with 209Bi. Our results pave the way to designing quantum states with long coherence times in simple oxides, making them attractive platforms for quantum technologies.