Defects In hBN Research Articles

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.

Purcell-Induced Bright Single Photon Emitters in Hexagonal Boron Nitride.

Single photon emitters (SPEs) in hexagonal boron nitride (hBN) are elementary building blocks for room-temperature on-chip quantum photonic technologies. However, fundamental challenges, such as slow radiative decay and nondeterministic placement of the emitters, limit their full potential. Here, we demonstrate large-area arrays of plasmonic nanoresonators (PNRs) for Purcell-induced room-temperature SPEs by engineering emitter-cavity coupling and enhancing radiative emission. Gold-coated silicon pillars with an alumina spacer enable a 10-fold local-field enhancement in the emission band of native hBN defects. We observe bright SPEs with an average saturated emission rate surpassing 5 million counts per second, an average lifetime of <0.5 ns, and 29% yield. Density functional theory reveals the beneficial role of an alumina spacer between hBN and gold, mitigating the electronic broadening of emission from defects proximal to the metal. Our results offer arrays of bright, heterogeneously integrated single-photon sources, paving the way for robust and scalable quantum information systems.

Atomic and Electronic Structure of Defects in hBN: Enhancing Single-Defect Functionalities.

Defect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their midgap electronic structure and orbital/spin wave function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic midgap states to the well-established photoluminescence response (including single-photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: (1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM and (2) multisite defect complexes exhibiting a ladder of empty and occupied midgap states characterized by distinct spatial geometries. Combining direct probing of midgap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics.

The hBN Defects Database: A Theoretical Compilation of Color Centers in Hexagonal Boron Nitride

The hBN Defects Database: A Theoretical Compilation of Color Centers in Hexagonal Boron Nitride

Atomic Defect Quantification by Lateral Force Microscopy.

Atomic defects in two-dimensional (2D) materials impact electronic and optoelectronic properties, such as doping and single photon emission. An understanding of defect-property relationships is essential for optimizing material performance. However, progress in understanding these critical relationships is hindered by a lack of straightforward approaches for accurate, precise, and reliable defect quantification on the nanoscale, especially for insulating materials. Here, we demonstrate that lateral force microscopy (LFM), a mechanical technique, can observe atomic defects in semiconducting and insulating 2D materials under ambient conditions. We first improve the sensitivity of LFM through consideration of cantilever mechanics. With the improved sensitivity, we use LFM to locate atomic-scale point defects on the surface of bulk MoSe2. By directly comparing LFM and conductive atomic force microscopy (CAFM) measurements on bulk MoSe2, we demonstrate that point defects observed with LFM are atomic defects in the crystal. As a mechanical technique, LFM does not require a conductive pathway, which allows defect characterization on insulating materials, such as hexagonal boron nitride (hBN). We demonstrate the ability to observe intrinsic defects in hBN and defects introduced by annealing. Our demonstration of LFM as a mechanical defect characterization technique applicable to both conductive and insulating 2D materials will enable routine defect-property determination and accelerate materials research.

Identifying Electronic Transitions of Defects in Hexagonal Boron Nitride for Quantum Memories

AbstractA quantum memory is a crucial keystone for enabling large‐scale quantum networks. Applicable to the practical implementation, specific properties, i.e., long storage time, selective efficient coupling with other systems, and a high memory efficiency are desirable. Though many quantum memory systems are developed thus far, none of them can perfectly meet all requirements. This work herein proposes a quantum memory based on color centers in hexagonal boron nitride (hBN), where its performance is evaluated based on a simple theoretical model of suitable defects in a cavity. Employing density functional theory calculations, 257 triplet and 211 singlet spin electronic transitions are investigated. Among these defects, it is found that some defects inherit the Λ electronic structures desirable for a Raman‐type quantum memory and optical transitions can couple with other quantum systems. Further, the required quality factor and bandwidth are examined for each defect to achieve a 95% writing efficiency. Both parameters are influenced by the radiative transition rate in the defect state. In addition, inheriting triplet‐singlet spin multiplicity indicates the possibility of being a quantum sensing, in particular, optically detected magnetic resonance. This work therefore demonstrates the potential usage of hBN defects as a quantum memory in future quantum networks.

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.

Extending the coherence of spin defects in hBN enables advanced qubit control and quantum sensing

Negatively-charged boron vacancy centers ({{V}_{B}}^{-}) in hexagonal Boron Nitride (hBN) are attracting increasing interest since they represent optically-addressable qubits in a van der Waals material. In particular, these spin defects have shown promise as sensors for temperature, pressure, and static magnetic fields. However, their short spin coherence time limits their scope for quantum technology. Here, we apply dynamical decoupling techniques to suppress magnetic noise and extend the spin coherence time by two orders of magnitude, approaching the fundamental T1 relaxation limit. Based on this improvement, we demonstrate advanced spin control and a set of quantum sensing protocols to detect radiofrequency signals with sub-Hz resolution. The corresponding sensitivity is benchmarked against that of state-of-the-art NV-diamond quantum sensors. This work lays the foundation for nanoscale sensing using spin defects in an exfoliable material and opens a promising path to quantum sensors and quantum networks integrated into ultra-thin structures.

Influence of neutron irradiation on X-ray diffraction, Raman spectrum and photoluminescence from pyrolytic and hot-pressed hexagonal boron nitride

Hexagonal boron nitride (hBN) is considered as an ideal semiconductor material for solid-state neutron detector, owing to its large neutron scattering section because of the low atomic number of B and excellent physical properties. Here we study the influence of neutron irradiation on crystal structure and on intermediate energy state (IMES) levels induced by the presence of impurities and defects in hBN. Large-size and thick pyrolytic and hot-pressed hBN (PBN and HBN) samples, which can be directly applied for neutron detector devices, are prepared and bombarded by neutrons with different irradiation fluences. The SEM and TEM are used to observe the sample difference of PBN and HBN. X-ray diffraction and Raman spectroscopy are applied to examine the influence of neutron irradiation on lattice structures along different crystal directions of PBN and HBN samples. Photoluminescence (PL) is employed to study the effect of neutron irradiation on IMESs in these samples. We find that the neutron irradiation does not alter the in-plane lattice structures of both PBN and HBN samples, but it can release the inter-layer tensions induced by sample growth of the PBN samples. Interestingly and surprisingly, the neutron irradiation does not affect the IMES levels responsible for PL generation, where PL is attributed mainly from phonon-assisted radiative electron-hole coupling for both PBN and HBN samples. Furthermore, the results indicate that the neutron irradiation can weaken the effective carrier-phonon coupling and exciton transitions in PBN and HBN samples. Overall, both PBN and HBN samples show some degree of the resistance to neutron irradiation in terms of these basic physical properties. The interesting and important findings from this work can help us to gain an in-depth understanding of the influence of neutron irradiation on basic physical properties of hBN materials. These effects can be taken into account when designing and applying the hBN materials for neutron detectors.

Annealing of blue quantum emitters in carbon-doped hexagonal boron nitride

Reliable methods to create quantum emitters in hexagonal boron nitride (hBN) are highly sought after for scalable applications in quantum photonic devices. Specifically, recent efforts have focused on defects in hBN with a zero phonon line at 2.8 eV (436 nm). Here, we employ carbon-doped hBN crystals that were irradiated by an electron beam to generate these emitters and perform annealing treatments to investigate the stability of the emitters. We find that the blue emitters are stable up to ∼800 °C. However, upon annealing to 1000 °C, the emitters disappear, and a family of other emitters appears in the region of hBN that had been irradiated by an electron beam. Our findings contribute to the understanding of emitter species and emitter formation in hBN.

Coupling spin defects in hexagonal boron nitride to a microwave cavity

Optically addressable spin defects in hexagonal boron nitride (hBN) have become a promising platform for quantum sensing. While sensitivity of these defects is limited by their interactions with the spin environment in hBN, inefficient microwave delivery can further reduce their sensitivity. Here, we design and fabricate a microwave double arc resonator for efficient transferring of the microwave field at 3.8 GHz. The spin transitions in the ground state of VB− are coupled to the frequency of the microwave cavity, which result in enhanced optically detected magnetic resonance (ODMR) contrast. In addition, the linewidth of the ODMR signal further reduces, achieving a magnetic field sensitivity as low as 42.4 μT/√Hz. Our robust and scalable device engineering is promising for future employment of spin defects in hBN for quantum sensing.

Magnetic Field Sensitivity Optimization of Negatively Charged Boron Vacancy Defects in hBN.

AbstractOptically active spin defects in hexagonal boron nitride (hBN) have recently emerged as compelling quantum sensors hosted by a two dimensional (2D) material. The photodynamics and sensitivity of spin defects are governed by their level structure and associated transition rates. These are, however, poorly understood for spin defects in hBN. Here, optical and microwave pump‐probe measurements are used to characterize the relaxation dynamics of the negatively charged boron vacancy (VB−)—the most widely‐studied spin defect in hBN. A 5‐level model is used to deduce transition rates that give rise to spin‐dependent VB− photoluminescence, and the lifetime of the VB− intersystem crossing metastable state. The obtained rates are used to simulate the magnetic field sensitivity of VB− defects and demonstrate high resolution imaging of the magnetic field generated by a single magnetic particle using optimal sensing parameters predicted by the model. The results reveal the rates that underpin VB− photodynamics, which is important for both a fundamental understanding of the VB− as a spin‐photon interface and for achieving optimal sensitivity in quantum sensing applications.

Effect of environmental screening and strain on optoelectronic properties of two-dimensional quantum defects

Point defects in hexagonal boron nitride (hBN) are promising candidates as single-photon emitters (SPEs) in nanophotonics and quantum information applications. The precise control of SPEs requires in-depth understanding of their optoelectronic properties. However, how the surrounding environment of host materials, including the number of layers, substrates, and strain, influences SPEs has not been fully understood. In this work, we study the dielectric screening effect due to the number of layers and substrates, and the strain effect on the optical properties of carbon dimer and nitrogen vacancy defects in hBN from first-principles many-body perturbation theory. We report that environmental screening causes a lowering of the quasiparticle gap and exciton binding energy, leading to nearly constant optical excitation energy and exciton radiative lifetime. We explain the results with an analytical model starting from the Bethe–Salpeter equation Hamiltonian with Wannier basis. We also show that optical properties of quantum defects are largely tunable by strain with highly anisotropic response, in good agreement with experimental measurements. Our work clarifies the effect of environmental screening and strain on optoelectronic properties of quantum defects in two-dimensional insulators, facilitating future applications of SPEs and spin qubits in low-dimensional systems.

Quantum Key Distribution Using a Quantum Emitter in Hexagonal Boron Nitride

AbstractQuantum key distribution (QKD) is considered the most immediate application to be widely implemented among a variety of potential quantum technologies. QKD enables sharing secret keys between distant users by using photons as information carriers. An ongoing endeavor is to implement these protocols in practice in a robust, and compact manner so as to be efficiently deployable in a range of real‐world scenarios. Single photon sources (SPS) in solid‐state materials are prime candidates in this respect. This article demonstrates a room temperature, discrete‐variable quantum key distribution system using a bright single photon source in hexagonal‐boron nitride, operating in free‐space. Employing an easily interchangeable photon source system, keys with one million bits length, and a secret key of approximately 70000 bits, at a quantum bit error rate of 6%, with ε‐security of 10−10 are generated. This study demonstrates the first proof of concept finite‐key BB84 QKD system realized with hBN defects.

Coherent dynamics of strongly interacting electronic spin defects in hexagonal boron nitride

Optically active spin defects in van der Waals materials are promising platforms for modern quantum technologies. Here we investigate the coherent dynamics of strongly interacting ensembles of negatively charged boron-vacancy ({{{{{{{{rm{V}}}}}}}}}_{{{{{{{{rm{B}}}}}}}}}^{-}) centers in hexagonal boron nitride (hBN) with varying defect density. By employing advanced dynamical decoupling sequences to selectively isolate different dephasing sources, we observe more than 5-fold improvement in the measured coherence times across all hBN samples. Crucially, we identify that the many-body interaction within the {{{{{{{{rm{V}}}}}}}}}_{{{{{{{{rm{B}}}}}}}}}^{-} ensemble plays a substantial role in the coherent dynamics, which is then used to directly estimate the concentration of {{{{{{{{rm{V}}}}}}}}}_{{{{{{{{rm{B}}}}}}}}}^{-}. We find that at high ion implantation dosage, only a small portion of the created boron vacancy defects are in the desired negatively charged state. Finally, we investigate the spin response of {{{{{{{{rm{V}}}}}}}}}_{{{{{{{{rm{B}}}}}}}}}^{-} to the local charged defects induced electric field signals, and estimate its ground state transverse electric field susceptibility. Our results provide new insights on the spin and charge properties of {{{{{{{{rm{V}}}}}}}}}_{{{{{{{{rm{B}}}}}}}}}^{-}, which are important for future use of defects in hBN as quantum sensors and simulators.

Spin Defects in hBN assisted by Metallic Nanotrenches for Quantum Sensing.

The omnipresence of hexagonal boron nitride (hBN) in devices embedding two-dimensional materials has prompted it as the most sought after platform to implement quantum sensing due to its testing while operating capability. The negatively charged boron vacancy (VB-) in hBN plays a prominent role, as it can be easily generated while its spin population can be initialized and read out by optical means at room-temperature. But the lower quantum yield hinders its widespread use as an integrated quantum sensor. Here, we demonstrate an emission enhancement amounting to 400 by nanotrench arrays compatible with coplanar waveguide (CPW) electrodes employed for spin-state detection. By monitoring the reflectance spectrum of the resonators as additional layers of hBN are transferred, we have optimized the overall hBN/nanotrench optical response, maximizing thereby the luminescence enhancement. Based on these finely tuned heterostructures, we achieved an enhanced DC magnetic field sensitivity as high as 6 × 10-5 T/Hz1/2.

Creation and repair of luminescence defects in hexagonal boron nitride by irradiation and annealing for optical neutron detection

Hexagonal boron nitride (hBN) is promising for applications in neutron detection and quantum sensing. Here we created spin-dependent luminescence defects in hBN using 50 keV helium ion beam. The irradiated hBN flakes with a dose around 2 × 1014–1 × 1015/cm2 have the maximum photoluminescence (PL) intensity. The PL spectra are in the range of 700–1000 nm with a peak around 818 nm at 297 K after irradiation with a dose of less than 2 × 1014/cm2, which can be eliminated by high temperature annealing at 1097 K due to defects repair according to Raman spectra. However, the PL peaks exhibit a redshift from 818 nm to 830 nm when the irradiation dose is no less than 1 × 1015/cm2. Combining with constrained density functional theory calculations, it is found that high dose irradiation can cause local lattice swelling and further induce the redshift of PL spectra by 12 nm/0.33% strain. Furthermore, we proposal a novel optical neutron detection method by recording the intensity and position of PL signal of luminescence defects induced by neutron-10B nuclear reaction daughter particles. This work would be helpful to create luminescence defects in hBN for quantum sensing, and develop a novel neutron detector.

Laser Direct Writing of Visible Spin Defects in Hexagonal Boron Nitride for Applications in Spin-Based Technologies

Optically addressable spins in two-dimensional hexagonal boron nitride (hBN) attract widespread attention for their potential advantages in on-chip quantum devices, such as quantum sensors and quantum networks. A variety of spin defects have been found in hBN, but no convenient and deterministic generation methods have been reported for other defects except the negatively charged boron vacancy (VB−). Here we report that by using femtosecond laser direct writing technology, we can deterministically create spin defect ensembles with spectral range from 550 to 800 nm on nanoscale hBN flakes. Positive single-peak optically detected magnetic resonance (ODMR) signals are detected in the presence of a magnetic field perpendicular to the substrate, and the contrast can reach 0.8%. With the appropriate thickness of hBN flakes, substrate, and femtosecond laser pulse energy, we can deterministically and efficiently generate a bright spin defect array. Our results provide a convenient deterministic method to create spin defects in hBN, which will motivate more endeavors for future research and applications of spin-based technologies such as a quantum magnetometer array.

Discretized hexagonal boron nitride quantum emitters and their chemical interconversion

Quantum emitters in two-dimensional hexagonal boron nitride (hBN) are of significant interest because of their unique photophysical properties, such as single-photon emission at room temperature, and promising applications in quantum computing and communications. The photoemission from hBN defects covers a wide range of emission energies but identifying and modulating the properties of specific emitters remain challenging due to uncontrolled formation of hBN defects. In this study, more than 2000 spectra are collected consisting of single, isolated zero-phonon lines (ZPLs) between 1.59 and 2.25 eV from diverse sample types. Most of ZPLs are organized into seven discretized emission energies. All emitters exhibit a range of lifetimes from 1 to 6 ns, and phonon sidebands offset by the dominant lattice phonon in hBN near 1370 cm−1. Two chemical processing schemes are developed based on water and boric acid etching that generate or preferentially interconvert specific emitters, respectively. The identification and chemical interconversion of these discretized emitters should significantly advance the understanding of solid-state chemistry and photophysics of hBN quantum emission.

Reflective dielectric cavity enhanced emission from hexagonal boron nitride spin defect arrays.

Among the various kinds of spin defects in hexagonal boron nitride (hBN), the negatively charged boron vacancy (VB-) spin defect that can be site-specifically generated is undoubtedly a potential candidate for quantum sensing, but its low quantum efficiency restricts its practical applications. Here, we demonstrate a robust enhancement structure called reflective dielectric cavity (RDC) with advantages including easy on-chip integration, convenient processing, low cost and suitable broad-spectrum enhancement for VB- defects. In the experiment, we used a metal reflective layer under the hBN flakes, filled with a transition dielectric layer in the middle, and adjusted the thickness of the dielectric layer to achieve the best coupling between RDC and spin defects in hBN. A remarkable 11-fold enhancement in the fluorescence intensity of VB- spin defects in hBN flakes can be achieved. By designing the metal layer into a waveguide structure, high-contrast optically detected magnetic resonance (ODMR) signal (∼21%) can be obtained. The oxide layer of the RDC can be used as the integrated material to implement secondary processing of micro-nano photonic devices, which means that it can be combined with other enhancement structures to achieve stronger enhancement. This work has guiding significance for realizing the on-chip integration of spin defects in two-dimensional materials.