Spin Defects Research Articles

Control of an Environmental Spin Defect beyond the Coherence Limit of a Central Spin

Electronic spin defects in the environment of an optically active spin can be used to increase the size and hence the performance of solid-state quantum registers, especially for applications in quantum metrology and quantum communication. Previous works on multiqubit electronic spin registers in the environment of a nitrogen-vacancy (NV) center in diamond have only included spins directly coupled to the NV. As this direct coupling is limited by the central spin coherence time, it significantly restricts the maximum attainable size of the register. To address this problem, we present a scalable approach to increase the size of electronic spin registers. Our approach exploits a weakly coupled probe spin together with double-resonance control sequences to mediate the transfer of spin polarization between the central NV spin and an environmental spin that is not directly coupled to it. We experimentally realize this approach to demonstrate the detection and coherent control of an unknown electronic spin outside the coherence limit of a central NV. Our work paves the way for engineering larger quantum spin registers with the potential to advance nanoscale sensing, enable correlated noise spectroscopy for error correction, and facilitate the realization of spin-chain quantum wires for quantum communication. Published by the American Physical Society 2024

Defects in layered boron nitride grown by Metal Organic Vapor Phase Epitaxy: luminescence and positron annihilation studies

Defects in two-dimensional boron nitride (BN) are candidates for a manifold of applications, for example, as single-photon emitters or optically addressable spin defects. However, the topic has proven to be complex and despite extensive research efforts, knowledge on midgap defects and their signature in photoluminescence (PL) remains fragmentary. Mass production of high-quality layered BN by Metal Organic Vapor Phase Epitaxy (MOVPE) is possible and effective, thus understanding the conditions of formation and identifying defects that arise in the material grown by this method is extremely important. Here, we present an analysis of the influence of the MOVPE growth conditions of layered BN on the occurrence of specific structural defects. PL spectra in the visible range were analysed involving the Huang-Rhys theory implemented in the fitting procedure for polycrystalline samples grown under various conditions. Such an approach allowed us to separate bands from individual entities. Two bands at 1.57 eV and 2.6 eV with phonon replicas were observed. The three additional bands are characterized by a broad emission centered at 1.38 eV, 1.9 eV and 2.24 eV. Further properties, including an analysis of the surface morphology, the impact of annealing and laser bleaching on the PL spectra and Positron Annihilation Spectroscopy (PAS) were considered to draw conclusions about the nature of the examined defects. The PAS analysis correlated with the PL of the BN layers allows us to classify the studied samples in terms of the concentrations of boron vacancies and their complexes. Based on the obtained results, we propose that the rich family of PL bands observed in various sp2-BN layers is associated with different defect complexes build of boron vacancies (VB), boron antisite defects (BN), substitutional carbon defects (CB, CN) and their donor-acceptor pairs. The main value of this paper is the transfer of knowledge gained about defects and the corresponding luminescent bands to characterize high-quality continuous epitaxial sp2-BN layers. The presented results constitute an important step toward the deterministic manipulation of defect concentrations in two-dimensional boron nitride, which opens up new pathways for future optoelectronic device application.

Integrated Manipulation and Addressing of Spin Defect in Diamond.

Scalable and addressable integrated manipulation of qubits is crucial for practical quantum information applications. Different waveguides have been used to transport the optical and electrical driving pulses, which are usually required for qubit manipulation. However, the separated multifields may limit the compactness and efficiency of manipulation and introduce unwanted perturbation. Here, we develop a tapered fiber-nanowire-electrode hybrid structure to realize integrated optical and microwave manipulation of solid-state spins at nanoscale. Visible light and microwave driving pulses are simultaneously transported and concentrated along an Ag nanowire. Studied with spin defects in diamond, the results show that the different driving fields are aligned with high accuracy. The spatially selective spin manipulation is realized. And the frequency-scanning optically detected magnetic resonance (ODMR) of spin qubits is measured, illustrating the potential for portable quantum sensing. Our work provides a new scheme for developing compact, miniaturized quantum sensors and quantum information processing devices.

Quantum Vibronic Effects on the Excitation Energies of the Nitrogen-Vacancy Center in Diamond.

We investigated the impact of quantum vibronic coupling on the electronic properties of solid-state spin defects using stochastic methods and first-principles molecular dynamics with a quantum thermostat. Focusing on the negatively charged nitrogen-vacancy center in diamond as an exemplary case, we found a significant dynamic Jahn-Teller splitting of the doubly degenerate single-particle levels within the diamond's band gap, even at 0 K, with a magnitude exceeding 180 meV. This pronounced splitting leads to substantial renormalizations of these levels and, subsequently, of the vertical excitation energies of the doubly degenerate singlet and triplet excited states. Our findings underscore the pressing need to incorporate quantum vibronic effects into first-principles calculations, particularly when comparing computed vertical excitation energies with experimental data. Our study also reveals the efficiency of stochastic thermal line sampling for studying phonon renormalizations of solid-state spin defects.

High frequency magnetometry with an ensemble of spin qubits in hexagonal boron nitride

Sensors based on spin qubits in 2D crystals offer the prospect of nanoscale proximities between sensor and source, which could provide access to otherwise inaccessible signals. For AC magnetometry, the sensitivity and frequency range are typically limited by the noise spectrum, which determines the qubit coherence time. We address this using phase modulated continuous concatenated dynamic decoupling, which extends the coherence time towards the T1 limit at room temperature and enables tuneable narrowband AC magnetometry. Using an ensemble of negatively charged boron vacancies in hexagonal boron nitride, we detect out-of-plane AC fields in the range of ~ 10 − 150 MHz, and in-plane fields within ± 150 MHz of the electron spin resonance. We measure an AC magnetic field sensitivity of sim 1,mu {{{rm{T}}}}/sqrt{{{{rm{Hz}}}}} at ~ 2.5 GHz, for a sensor volume of ~ 0.1 μm3. This work establishes the viability of spin defects in 2D materials for high frequency magnetometry, with wide-ranging applications across science and technology.

Isotope engineering for spin defects in van der Waals materials.

Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ([Formula: see text]) in hexagonal boron nitride (hBN), we grow isotopically purified h10B15N crystals. Compared to [Formula: see text] in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded [Formula: see text] spin transitions as well as extended coherence time T2 and relaxation time T1. For quantum sensing, [Formula: see text] centers in our h10B15Nsamples exhibit a factor of 4 (2) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the [Formula: see text] hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor 15Nnuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

Photonic Spin Hopfions and Monopole Loops.

Spin textures with various topological orders are of great theoretical and practical interest. Hopfion, a spin texture characterized by a three-dimensional topological order was recently realized in electronic spin systems. Here, we show that monochromatic light can be structured such that its photonic spin exhibits a hopfion texture in the three-dimensional real space. We also provide ways to construct spin textures of arbitrary Hopf charges. When extending the system to four dimensions by introducing a parameter dimension, a new type of topological defect in the form of a monopole loop in photonic spin is encountered. Each point on the loop is a topological spin defect in three dimensions, and the loop itself carries quantized Hopf charges. Such photonic spin texture and defect may find application in control and sensing of nanoparticles, and optical generation of topological texture in motions of particles or fluids.

First-Principles Investigation of Near-Surface Divacancies in Silicon Carbide.

The realization of quantum sensors using spin defects in semiconductors requires a thorough understanding of the physical properties of the defects in the proximity of surfaces. We report a study of the divacancy (VSiVC) in 3C-SiC, a promising material for quantum applications, as a function of surface reconstruction and termination with -H, -OH, -F and oxygen groups. We show that a VSiVC close to hydrogen-terminated (2 × 1) surfaces is a robust spin-defect with a triplet ground state and no surface states in the band gap and with small variations of many of its physical properties relative to the bulk, including the zero-phonon line and zero-field splitting. However, the Debye-Waller factor decreases in the vicinity of the surface and our calculations indicate it may be improved by strain-engineering. Overall our results show that the VSiVC close to SiC surfaces is a promising spin defect for quantum applications, similar to its bulk counterpart.

Characteristics of interacting carbon-antisite-vacancies in 4H silicon carbide

Spin defects in semiconductors have demonstrated promising electronic structures for potential applications in quantum computing and sensing. Among various proposed quantum byte systems, spin defects in silicon carbide have attracted significant attention due to several advantages they offer over other options. In this study, we investigate carbon-antisite-vacancy defects in 4H silicon carbide through ab initio density functional theory calculations. With the HSE06 functionals, the ab initio computation can predict much more accurate electronic structures. However, the corresponding computational cost is high, especially for supercells consisting of several hundreds of atoms. In this investigation, the carbon-antisite-vacancy defect is studied by using a high-performance computing cluster, with a specific focus on supercells that encompass two such defects. The extension of a single carbon-antisite-vacancy defect is depicted by referring to the spin density distribution. Different defect types show similar spin density patterns. Based on the single defect characteristics, supercells with paired carbon-antisite-vacancy defects are created. It is found that the binding energy can reach 2 eV for overlapping defects. In the case of insignificant overlap of the corresponding single defects, the ground state magnetic moment is 4 µB, accompanied by a negligible binding energy. However, if there is a significant overlap of the spin density, the magnetic moment changes to 2 µB. These findings can serve as helpful references for the study of spin defects in 4H silicon carbide, particularly in the potential carbon-antisite-vacancy application research.

Excited State Properties of Point Defects in Semiconductors and Insulators Investigated with Time-Dependent Density Functional Theory.

We present a formulation of spin-conserving and spin-flip hybrid time-dependent density functional theory (TDDFT), including the calculation of analytical forces, which allows for efficient calculations of excited state properties of solid-state systems with hundreds to thousands of atoms. We discuss an implementation on both GPU- and CPU-based architectures along with several acceleration techniques. We then apply our formulation to the study of several point defects in semiconductors and insulators, specifically the negatively charged nitrogen-vacancy and neutral silicon-vacancy centers in diamond, the neutral divacancy center in 4H silicon carbide, and the neutral oxygen-vacancy center in magnesium oxide. Our results highlight the importance of taking into account structural relaxations in excited states in order to interpret and predict optical absorption and emission mechanisms in spin defects.

Widefield Diamond Quantum Sensing with Neuromorphic Vision Sensors.

Despite increasing interest in developing ultrasensitive widefield diamond magnetometry for various applications, achieving high temporal resolution and sensitivity simultaneously remains a key challenge. This is largely due to the transfer and processing of massive amounts of data from the frame-based sensor to capture the widefield fluorescence intensity of spin defects in diamonds. In this study, a neuromorphic vision sensor to encode the changes of fluorescence intensity into spikes in the optically detected magnetic resonance (ODMR) measurements is adopted, closely resembling the operation of the human vision system, which leads to highly compressed data volume and reduced latency. It also results in a vast dynamic range, high temporal resolution, and exceptional signal-to-background ratio. After a thorough theoretical evaluation, the experiment with an off-the-shelf event camera demonstrated a 13× improvement in temporal resolution with comparable precision of detecting ODMR resonance frequencies compared with the state-of-the-art highly specialized frame-based approach. It is successfully deploy this technology in monitoring dynamically modulated laser heating of gold nanoparticles coated on a diamond surface, a recognizably difficult task using existing approaches. The current development provides new insights for high-precision and low-latency widefield quantum sensing, with possibilities for integration with emerging memory devices to realize more intelligent quantum sensors.

High-Throughput Search for Triplet Point Defects with Narrow Emission Lines in 2D Materials.

We employ a first-principles computational workflow to screen for optically accessible, high-spin point defects in wide band gap, two-dimensional (2D) crystals. Starting from an initial set of 5388 point defects, comprising both native and extrinsic, single and double defects in ten previously synthesized 2D host materials, we identify 596 defects with a triplet ground state. For these defects, we calculate the defect formation energy, hyperfine (HF) coupling, and zero-field splitting (ZFS) tensors. For 39 triplet transitions exhibiting particularly low Huang-Rhys factors, we calculate the full photoluminescence (PL) spectrum. Our approach reveals many spin defects with narrow PL line shapes and emission frequencies covering a broad spectral range. Most of the defects are hosted in hexagonal BN (hBN), which we ascribe to its high stiffness, but some are also found in MgI2, MoS2, MgBr2 and CaI2. As specific examples, we propose the defects vSMoS0 and NiSMoS0 in MoS2 as interesting candidates with potential applications to magnetic field sensors and quantum information technology.

Oxygen-vacancy defect in 4H-SiC as a near-infrared emitter: An ab initio study

Optically active spin defects in semiconductors can serve as spin-to-photon interfaces, key components in quantum technologies. Silicon carbide (SiC) is a promising host of spin defects thanks to its wide bandgap and well-established crystal growth and device technologies. In this study, we investigated the oxygen-vacancy complexes as potential spin defects in SiC by means of ab initio calculations. We found that the OCVSi defect has a substantially low formation energy compared with its counterpart, OSiVC, regardless of the Fermi level position. The OCVSi defect is stable in its neutral charge state with a high-spin ground state (S = 1) within a wide energy range near the midgap energy. The zero-phonon line (ZPL) of the OCVSi0 defect lies in the near-infrared regime, 1.11–1.24 eV (1004–1117 nm). The radiative lifetime for the ZPL transition of the defect in kk configuration is fairly short (12.5 ns). Furthermore, the estimated Debye–Waller factor for the optical transition is 13.4%, indicating a large weight of ZPL in the photoluminescence spectrum. All together, we conclude that the OCVSi0 defect possesses desirable spin and optical properties and thus is potentially attractive as a quantum bit.

Fabrication and quantum sensing of spin defects in silicon carbide

In the past decade, color centers in silicon carbide (SiC) have emerged as promising platforms for various quantum information technologies. There are three main types of color centers in SiC: silicon-vacancy centers, divacancy centers, and nitrogen-vacancy centers. Their spin states can be polarized by laser and controlled by microwave. These spin defects have been applied in quantum photonics, quantum information processing, quantum networks, and quantum sensing. In this review, we first provide a brief overview of the progress in single-color center fabrications for the three types of spin defects, which form the foundation of color center-based quantum technology. We then discuss the achievements in various quantum sensing, such as magnetic field, electric field, temperature, strain, and pressure. Finally, we summarize the current state of fabrications and quantum sensing of spin defects in SiC and provide an outlook for future developments.

Engineering the formation of spin-defects from first principles

The full realization of spin qubits for quantum technologies relies on the ability to control and design the formation processes of spin defects in semiconductors and insulators. We present a computational protocol to investigate the synthesis of point-defects at the atomistic level, and we apply it to the study of a promising spin-qubit in silicon carbide, the divacancy (VV). Our strategy combines electronic structure calculations based on density functional theory and enhanced sampling techniques coupled with first principles molecular dynamics. We predict the optimal annealing temperatures for the formation of VVs at high temperature and show how to engineer the Fermi level of the material to optimize the defect’s yield for several polytypes of silicon carbide. Our results are in excellent agreement with available experimental data and provide novel atomistic insights into point defect formation and annihilation processes as a function of temperature.

Isotopic Control of the Boron-Vacancy Spin Defect in Hexagonal Boron Nitride.

We report on electron spin resonance (ESR) spectroscopy of boron-vacancy (V_{B}^{-}) centers hosted in isotopically engineered hexagonal boron nitride (hBN) crystals. We first show that isotopic purification of hBN with ^{15}N yields a simplified and well-resolved hyperfine structure of V_{B}^{-} centers, while purification with ^{10}B leads to narrower ESR linewidths. These results establish isotopically purified h^{10}B^{15}N crystals as the optimal host material for future use of V_{B}^{-} spin defects in quantum technologies. Capitalizing on these findings, we then demonstrate optically induced polarization of ^{15}N nuclei in h^{10}B^{15}N, whose mechanism relies on electron-nuclear spin mixing in the V_{B}^{-} ground state. This work opens up new prospects for future developments of spin-based quantum sensors and simulators on a two-dimensional material platform.

Optically Active Spin Defects in Few-Layer Thick Hexagonal Boron Nitride.

Optically active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this Letter, we first demonstrate that the electron spin resonance frequencies of boron vacancy centers (V_{B}^{-}) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of V_{B}^{-} centers with the hBN thickness with a focus on (i)the zero-field splitting parameters, (ii)the optically induced spin polarization rate and (iii)the longitudinal spin relaxation time. This Letter provides important insights into the properties of V_{B}^{-} centers embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

Highly Coherent Nitrogen‐Vacancy Centers in Diamond via Rational High‐Pressure and High‐Temperature Synthesis and Treatment

AbstractThe high‐pressure and high‐temperature (HPHT) diamonds with well‐controlled defects and low stress offer an ideal host substrate for the fields of quantum information science; however, fabrication of quantum‐grade HPHT diamonds remains a pressing challenge. Here, a major advance in generating highly coherent nitrogen‐vacancy (NV) centers, a promising spin defect in diamonds, via tailored HPHT synthesis and postgrown annealing treatment is reported. The resulting well‐dispersed single NV− centers in type‐IIa diamonds exhibit long spin coherence times comparable to that of the reported chemical vapor deposition diamonds. Moreover, high‐density NV− ensembles in 〈100〉‐grown type‐Ib diamonds with superb zero‐phonon lines considerably sharper than those of native NV− centers in as‐grown diamonds, together with low splitting of resonances are produced. These findings demonstrate a superior synthesis and optimization protocol for creating high‐quality NV− centers avoiding lattice damage in diamond to meet the stringent requirements for a wide range of emerging quantum technologies.

Multilevel Encoding Physically Unclonable Functions Based on The Multispecies Structure in Diamonds

AbstractThe multilevel encoding (MLE) scheme is an effective method for improving the anticounterfeiting encryption capabilities of physically unclonable functions (PUFs). However, owing to the correlation between encoding layers, the encoding capacity (EC) is difficult to improve by orders of magnitude. Herein, four noncorrelated structures in the diamond crystal structure (carbon–carbon single bond, defect luminescence structures, spin structures, and electron energy distribution structures) are considered for MLE. First, the microdiamonds containing nitrogen‐vacancy (NV) color centers are embedded into polydimethylsiloxane (PDMS) to fabricate PUFs. Using an optical imaging system, four codable images of four noncorrelated structures are read. The noncorrelation of the four‐level encoding structure is verified by calculating the Hamming distance (0.496 ± 0.02). The results show that EC exponentially improves to 24×10 000/(100 pixels)2. Furthermore, the encoding method based on the energy level does not depend on physical structure parameters, such as the size and position of the spin structure. Thus, it is protected from structural modeling attacks, resulting in high security. Moreover, PUF labels based on PDMS flexible substrates can be employed for various flexible applications. In the proposed scheme, the information is encrypted by a four‐level two‐dimensional (2D) barcode and decoded by self‐developed PUF authentication software. The proposed scheme presents a way for developing next‐generation PUFs with super‐high EC.

Diamond MEMS: From Classical to Quantum

AbstractDiamond has numerous outstanding properties in mechanics, physics, chemistry, electronics, thermodynamics, and spintronics for either classic micro/nanoelectromechanical systems (MEMS/NEMS) devices or hybrid quantum MEMS/NEMS systems. The extremely high mechanical strength and the ultra‐wide bandgap energy enable the development of mechanically and thermally robust MEMS/NEMS sensors and switches, while the long coherence time of spin defects center enables the reading out through optical methods, precise quantum sensing, and quantum information processing. In this paper, the development of diamond‐based MEMS/NEMS from the viewpoints of classic devices to quantum systems are reviewed. The fabrication process and the classic applications of diamond MEMS/NEMS devices are first described, including those from micro‐crystalline, nano‐crystalline/ultranano‐crystalline, and single‐crystalline diamonds. Then, the physical properties of nitrogen‐vacancy defect center, as well as the application referred to the hybrid system composed of MEMS structures and nitrogen‐vacancy centers embedded, strain–spin interaction, and diamond‐based optomechanics are introduced. Finally, a conclusion and outlook are presented. It is expected that diamond MEMS/NEMS is not only an ideal platform for high‐performance and high‐reliability advanced classic MEMS devices but also for quantum sensing, information, and exploring the fundamentals of quantum mechanics.