Nitrogen-vacancy Centers Research Articles

Detection of electron spin resonance of a single nitrogen-vacancy center in diamond using the excited-state lifetime

Detection of electron spin resonance of a single nitrogen-vacancy center in diamond using the excited-state lifetime

First-principles study of the Stark shift effect on the zero-phonon line of the NV center in diamond

First-principles study of the Stark shift effect on the zero-phonon line of the NV center in diamond

Simultaneous vector magnetometry based on fluorescence polarization of NV centers ensemble in diamond

The nitrogen-vacancy (NV) centers ensemble has extensive application prospects in vector-magnetic-field measurement due to its accurate and fixed spatial orientations along the crystallographic axes of diamonds. However, to address signals of NV centers along all four axes, a large bias magnetic field sufficient to spectrally separate their resonances is typically inevitable, which may affect the magnetic substance under test and require multiple-frequency microwaves to interrogate signals of the four axes. Here, we demonstrate an NV-based simultaneous vector magnetometer that works at a bias field as low as just separating the resonant peaks of |ms=±1 states and utilizes a single-frequency microwave. By simultaneously detecting the fluorescence at specific optical polarization angles in three orthogonal directions and determining the transformation matrix in advance, all the Cartesian components of the magnetic field under test are distinguished. The experimentally achieved magnetic-field sensitivity is 63 nT/Hz, and the bias field is reduced to around 11 Gauss (still reducible by narrowing the linewidth) in ambient conditions. The proposed methods dramatically reduce the bias field for NV-based simultaneous vector magnetometers and potentially expand their applications in biological science, materials science, and industrial noninvasive detection.

Visualized Axial Localization of Nitrogen-Vacancy Center in Bulk Diamond Assisted by Radially Polarized Beam

Visualized Axial Localization of Nitrogen-Vacancy Center in Bulk Diamond Assisted by Radially Polarized Beam

Single and double quantum transitions in spin-mixed states under photo-excitation

Electronic spins associated with the Nitrogen-Vacancy (NV) center in diamond offer an opportunity to study spin-related phenomena with extremely high sensitivity owing to their high degree of optical polarization. Here, we study both single- and double-quantum transitions (SQT and DQT) in NV centers between spin-mixed states, which arise from magnetic fields that are non-collinear to the NV axis. We demonstrate the amplification of the ESR signal from both these types of transition under laser illumination. We obtain hyperfine-resolved X-band ESR signal as a function of both excitation laser power and misalignment of static magnetic field with the NV axis. This, combined with our analysis using a seven-level model that incorporates thermal polarization and double quantum relaxation, allows us to comprehensively analyze the polarization of NV spins under off-axis fields. Such detailed understanding of spin-mixed states in NV centers under photo-excitation can help greatly in realizing NV-diamond platform’s potential in sensing correlated magnets and biological samples, as well as other emerging applications, such as masing and nuclear hyperpolarization.

Dual-media laser system: Nitrogen vacancy diamond and red semiconductor laser.

Diamond is a potential host material for laser applications due to its exceptional thermal properties, ultrawide bandgap, and color centers, which promise gain across the visible spectrum. More recently, coherent laser methods offer improved sensitivity for magnetometry. However, diamond fabrication is difficult in comparison to other crystalline matrices, and many optical loss channels are not yet understood. Here, we demonstrate a continuous-wave laser threshold as a function of the pump intensity on nitrogen-vacancy (NV) color centers. To achieve this, we constructed a laser cavity with both an NV diamond medium and an intracavity antireflection-coated diode laser. This dual-medium approach compensates intrinsic losses of the cavity by providing a fixed additional gain below threshold of the diode laser. We observe a continuous-wave laser threshold of the laser system and linewidth narrowing with increasing green pump power on the NV centers. Our results are a major development toward coherent approaches to magnetometry.

Luminescent Organic Triplet Diradicals as Optically Addressable Molecular Qubits.

Optical-spin interfaces that enable the photoinitialization, coherent microwave manipulation, and optical read-out of ground state spins have been studied extensively in solid-state defects such as diamond nitrogen vacancy (NV) centers and are promising for quantum information science applications. Molecular quantum bits (qubits) offer many advantages over solid-state spin centers through synthetic control of their optical and spin properties and their scalability into well-defined multiqubit arrays. In this work, we report an optical-spin interface in an organic molecular qubit consisting of two luminescent tris(2,4,6-trichlorophenyl)methyl (TTM) radicals connected via the meta-positions of a phenyl linker. The triplet ground state of this system can be photoinitialized in its |T0⟩ state by shelving triplet populations as singlets through spin-selective excited-state intersystem crossing with 80% selectivity from |T+⟩ and |T-⟩. The fluorescence intensity in the triplet manifold is determined by the ground-state polarization, and we show successful optical read-out of the ground-state spin following microwave manipulations by fluorescence-detected magnetic resonance spectroscopy. At 85 K, the lifetime of the polarized ground state is 45 ± 3 μs, and the ground state phase memory time is Tm = 5.9 ± 0.1 μs, which increases to 26.8 ± 1.6 μs at 5 K. These results show that luminescent diradicals with triplet ground states can serve as optically addressable molecular qubits with long spin coherence times, which marks an important step toward the rational design of spin-optical interfaces in organic materials.

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.

Nitrogen-vacancy centers as a self-gauged micro-scale heater and its application for multi-modal sensing

The optical excitation of nitrogen-vacancy (NV) color centers in diamonds mostly results in fluorescence emission. During this process, a portion of the incident energy is transferred to phonon vibration, which heats the diamond crystal. For single NV color centers, the heat generated by the optical cycle is negligible, while for an ensemble of NV defects, the generated heat accumulates rapidly and heats the diamond. The temperature rise is rapid due to the high thermal conductivity of the diamond. In addition to the ability to be heated by light, the NV defect's unique properties also allow for the precise measurement of temperature using optically detected magnetic resonance. Here, we experimentally demonstrate that microcrystalline diamond containing NV center ensembles can be used as a self-gauged microheater. We attached a microcrystal diamond to an optical fiber in an endoscope configuration, evaluated its performance as a self-gauged heater under varied biologically relevant environments, and discussed its potential applications. In addition to the aforementioned capabilities, the NV defect enables the precise measurement of local magnetic fields. This provides a unique multimodal sensor to probe temperature-controlled magnetic phenomena at microscopic scales.

Making Use of Low‐Cost High‐Pressure–High‐Temperature‐Diamond Materials for Industry‐Type Quantum Sensor Device Applications

A cost‐effective approach to provide diamond platelets containing nitrogen vacancy center ensembles (NVs) in the range of ppm is investigated. Industry‐type high‐pressure–high‐temperature‐diamond type 1b containing a high number of interstitial nitrogen in the range of several tens of ppm are used and small diamond platelets (size ≈1 × 1 mm2, thickness ≈300 μm) are prepared by laser cutting and polishing. The nitrogen is converted into NV by means of high‐energy electron irradiation of 10 MeV and annealing at 900 °C. Variations in the irradiation dose between 0.5E18 1/cm2 and 2E18 1/cm2 result in different densities of NV. The diamond platelets are analyzed with regard to their nitrogen concentration and photoluminescence as well as optically detected magnetic resonance is used to investigate the usability for a NV‐based magnetometer. A method to calculate the ratio of negatively to neutrally charged NV (NV−/NV0) is proposed that uses the photoluminescence intensities of the spectrum at 575 and 638 nm, namely, the zero‐phonon lines of NV− and NV0.

Insight into the nitrogen-vacancy center formation in type-Ib diamond by irradiation and annealing approach

Abstract Comprehending the microscopic formation of nitrogen vacancy (NV) centers in nitrogen-doped diamonds is crucial for enhancing the controllable preparation of NV centers and quantum applications. Irradiation followed by annealing simulations for a type-Ib diamond with a 900 ppm concentration of isolated nitrogen is conducted along different orientations and at different annealing temperatures. In these simulations, molecular dynamics (MD) with smoothly connected potential functions are implemented. MD simulations revealed the dynamic formation process of the NV center, which was subsequently verified by first-principles calculations and experiments. The results indicate that vacancies undergo one or multiple migrations by exchanging sites with neighboring atoms. There are three mechanisms for the formation of NV centers: direct irradiation-induced NV formation, irradiation with further annealing to form NV and vacancy migration (VM) during the annealing process. Furthermore, the results show that both VM and NV center formations are affected by orientations. This study clarifies the formation of NV centers across multiple scales and provides a solid foundation for the targeted preparation of NV centers.

Current induced hidden states in Josephson junctions

Josephson junctions enable dissipation-less electrical current through metals and insulators below a critical current. Despite being central to quantum technology based on superconducting quantum bits and fundamental research into self-conjugate quasiparticles, the spatial distribution of super current flow at the junction and its predicted evolution with current bias and external magnetic field remain experimentally elusive. Revealing the hidden current flow, featureless in electrical resistance, helps understanding unconventional phenomena such as the nonreciprocal critical current, i.e., Josephson diode effect. Here we introduce a platform to visualize super current flow at the nanoscale. Utilizing a scanning magnetometer based on nitrogen vacancy centers in diamond, we uncover competing ground states electrically switchable within the zero-resistance regime. The competition results from the superconducting phase re-configuration induced by the Josephson current and kinetic inductance of thin-film superconductors. We further identify a new mechanism for the Josephson diode effect involving the Josephson current-induced phase. The nanoscale super current flow emerges as a new experimental observable for elucidating unconventional superconductivity, and optimizing quantum computation and energy-efficient devices.

Charge and Spin Dynamics and Destabilization of Shallow Nitrogen-Vacancy Centers under UV and Blue Excitation.

Shallow nitrogen-vacancy (NV) centers in diamond offer opportunities to study photochemical reactions, including photogeneration of radical pairs, at the single-molecule regime. A prerequisite is a detailed understanding of charge and spin dynamics of NVs exposed to the short-wavelength light required to excite chemical species. Here, we investigate the charge and spin dynamics of shallow NVs under 445 and 375 nm illumination. With blue excitation, charge-state preparation is power-dependent, and modest spin initialization fidelity is observed. Under UV excitation, charge-state preparation is power-independent and no spin polarization is observed. Aging of NVs under prolonged UV exposure manifests in a reduced charge stability and spin contrast. We attribute this aging to modified local charge environments of near-surface NVs and identify distinct electronic traps only accessible at short wavelengths. Finally, we evaluate the prospects of NVs to probe photogenerated radical pairs based on measured sensitivities and outline possible sensing schemes.

First-principles calculations of optical and positron annihilation properties of NV center in 3C-SiC

We studied the optical and positron annihilation properties of NCVSi in 3C-SiC using first-principles calculations. We found that the charge-state transition and the spin-conserving optical transition levels are very close to each other. In order to distinguish between the NV center and intrinsic defect, we calculate in detail the defect formation energies, temperature-dependent positron lifetimes, and electron-positron momentum distribution of these defects in 3C-SiC. We suggest that using positrons technique alone is insufficiently sensitive in identifying the charge-states of NCVSi, necessitating the use of additional characterization methods to address this issue.

Microscale fiber-integrated vector magnetometer with on-tip field biasing using N - V ensembles in diamond microcrystals

In quantum sensing of magnetic fields, ensembles of nitrogen-vacancy centers in diamond offer high sensitivity, high bandwidth and outstanding spatial resolution while operating in harsh environments. Moreover, the orientation of defect centers along four crystal axes forms an intrinsic coordinate system, enabling vector magnetometry within a single diamond crystal. While most vector magnetometers rely on a known bias magnetic field for full recovery of three-dimensional (3D) field information, employing external 3D Helmholtz coils or permanent magnets results in bulky, laboratory-bound setups, impeding miniaturization of the device. Here, a novel approach is presented that utilizes a fiber-integrated microscale coil at the fiber tip to generate a localized uniaxial magnetic field. The same fiber-tip coil is used in parallel for spin control by combining dc and microwave signals in a bias tee. To implement vector magnetometry using a uniaxial bias field, the orientation of the diamond crystal is preselected and then fully characterized by rotating a static magnetic field in three planes of rotation. The measurement of vector magnetic fields in the full solid angle is demonstrated with a shot-noise-limited sensitivity of 19.4nT/Hz1/2 and microscale spatial resolution while achieving a fiber sensor head cross section of less than 1mm2. Published by the American Physical Society 2024

Photonic-Cavity-Enhanced Laser Writing of Color Centers in Diamond.

Color centers in diamond have widespread utility in quantum technologies, but their creation process remains stochastic in nature. Deterministic creation of color centers in device-ready diamond platforms can improve the yield, scalability, and integration. Recent work using pulsed laser excitation has shown impressive progress in deterministically creating defects in bulk diamond. Here, we extend this laser-writing process into nanophotonic devices etched into diamond membranes, including nanopillars and photonic resonators with writing and subsequent readout occurring in situ at cryogenic temperatures. We demonstrate the optically driven creation of carbon vacancy (GR1) and nitrogen vacancy (NV) centers in diamond nanopillars and observe enhanced photoluminescence collection from them. We also fabricate bullseye resonators and leverage their cavity modes to locally amplify the laser-writing field, yielding defect creation with picojoule write-pulse energies 100 times lower than those typically used in bulk diamond demonstrations.

Enhanced Plasmonic Trapping and Fluorescent Emission of Nitrogen-Vacancy Nanodiamonds Using a High-Efficiency Nanofocusing Device.

Fluorescent nanodiamonds (FNDs) with nitrogen-vacancy centers are pivotal for advancing quantum photonics and imaging through deterministic quantum state manipulation. However, deterministic integration of quantum emitters into photonic devices remains a challenge due to the need for high coupling efficiency and Purcell enhancement. We report a deterministic FND-integrated nanofocusing device achieved by assembling FNDs at a plasmonic waveguide tip through plasmonic-enhanced optical trapping. This technique not only increases the emission rate by 58.6 times compared to isolated FNDs but also preferentially directs radiation into the waveguide at a rate 5.3 times higher than that into free space, achieving an exceptional figure-of-merit of ∼3000 for efficient energy transfer. Our findings represent a significant step toward deterministic integration in quantum imaging and communication, opening new avenues for quantum technology advancements.

Controlled lateral positioning of NV centres in diamond by CVD overgrowth

A challenge to this day in the development of diamond devices for quantum applications is the laterally defined and closely spaced positioning of nitrogen-vacancy centres with exceptional coherence properties. Here, we demonstrate a maskless, implantation-free method for the controlled in-plane positioning of NV centres using a combination of focused ion beam (FIB) milling, plasma etching and nitrogen-doped diamond growth. The Ga+ ion beam milling resulted in 1 μm × 1 μm cavities with depths of up to 450 nm, each cavity exhibiting the four [111]-oriented diamond facets after pure hydrogen plasma treatment and a depth of 700 nm. Low-methane, nitrogen-doped chemical vapour deposition (CVD) overgrowth resulted in in situ formation of oriented NV ensembles, exclusively perpendicular to the {111}-planes.

Probing the electronic ground state of the nitrogen-vacancy center in nanodiamonds at room temperature

The color centers in diamonds are promising candidates in the context of quantum information science, quantum computation, and spin-based quantum sensors due to their spin-dependent optical transitions. The manipulation and optical readout of electronic spin state is measured using a technique known as optically detected magnetic resonance (ODMR). Here, we discuss the indigenous development of ODMR setup to coherently manipulate and precise readout of spin state of nitrogen-vacancy centers (NV) in nanodiamond at room-temperature. The study involves the confocal mapping of an ensemble of NV centers to measure spin state-dependent optical transition by applying an optical excitation and microwave field simultaneously. The spin state control appears as a dip at 2.87 GHz in the measured emission intensity spectra as a function of microwave frequency. An ODMR contrast of 3.4 % is achieved at the NV center emission maximum of 660 nm and an inhomogeneous dephasing time of 0.03 microseconds. We find an inherent small split in the ODMR dip which is induced by local strain in nanodiamonds. The split becomes stronger while applying an external magnetic field, which forms the basis of NV center-based magnetometry. The results are useful for spin-based microwave-optical quantum transducers, quantum sensing, and quantum memory devices.

Thresholdless coherence in a superradiant laser

Lasing threshold in the conventional lasers is the minimum input power required to initiate laser oscillation. It has been widely accepted that the conventional laser threshold occurring around a unity intracavity photon number can be eliminated in the input-output curve by making the so-called β parameter approach unity. The recent experiments, however, have revealed that even in this case the photon statistics still undergo a transition from coherent to thermal statistics when the intracavity mean photon number is decreased below unity. Since the coherent output is only available above the diminished threshold, the long-sought promise of thresholdless lasers to produce always coherent light has become questionable. Here, we present an always-coherent thresholdless laser based on superradiance by two-level atoms in a quantum superposition state with the same phase traversing a high-Q cavity. Superradiant lasing was observed without the conventional lasing threshold around the unity photon number and the photon statistics remained near coherent even below it. The coherence was improved by reducing the coupling constant as well as the excited-state amplitude in the superposition state. Our results pave a way toward always-coherent thresholdless lasers with more practical media such as quantum dots, nitrogen-vacancy centers and doped ions in crystals.