Single Color Centers Research Articles

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.

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.

Kinetics and Quantum Trajectories of Luminescence Intensity of Single Color Centers in Sodium Fluoride Crystals

Kinetics and Quantum Trajectories of Luminescence Intensity of Single Color Centers in Sodium Fluoride Crystals

Single-photon emission from silicon-vacancy color centers in polycrystalline diamond membranes

Single-color centers in thin polycrystalline diamond membranes allow the platform to be used in integrated quantum photonics, hybrid quantum systems, and other complex functional materials. While single-crystal diamond membranes are still technologically challenging to fabricate as they cannot be grown on a non-diamond substrate, free-standing polycrystalline diamond membranes can be conveniently fabricated at large-scale from nanocrystalline diamond seeds on a substrate that can be selectively etched. However, their practical application for quantum photonics is so far limited by crystallographic defects, impurities, graphitic grain boundaries, small grain sizes, scattering loss, and strain. In this paper, we report on a single-photon source based on silicon-vacancy color centers in a polycrystalline diamond membrane. We discuss the spectroscopic approach and quantify the photon statistics, obtaining a g2(0) ≈ 0.04. Our findings hold promise for introducing polycrystalline diamond to quantum photonics and hybrid quantum systems.

Qudit-Based Spectroscopy for Measurement and Control of Nuclear-Spin Qubits in Silicon Carbide.

Nuclear spins with hyperfine coupling to single electron spins are highly valuable quantum bits. Here we probe and characterize the particularly rich nuclear-spin environment around single silicon vacancy color centers (V2) in 4H-SiC. By using the electron spin-3/2 qudit as a four level sensor, we identify several sets of ^{29}Si and ^{13}C nuclear spins through their hyperfine interaction. We extract the major components of their hyperfine coupling via optical detected nuclear magnetic resonance, and assign them to shells in the crystal via the density function theory simulations. We utilize the ground-state level anticrossing of the electron spin for dynamic nuclear polarization and achieve a nuclear-spin polarization of up to 98±6%. We show that this scheme can be used to detect the nuclear magnetic resonance signal of individual spins and demonstrate their coherent control. Our work provides a detailed set of parameters and first steps for future use of SiC as a multiqubit memory and quantum computing platform.

Giant Quantum Electrodynamic Effects on Single SiV Color Centers in Nanosized Diamonds.

Understanding and mastering quantum electrodynamics phenomena is essential to the development of quantum nanophotonics applications. While tailoring of the local vacuum field has been widely used to tune the luminescence rate and directionality of a quantum emitter, its impact on their transition energies is barely investigated and exploited. Fluorescent defects in nanosized diamonds constitute an attractive nanophotonic platform to investigate the Lamb shift of an emitter embedded in a dielectric nanostructure with high refractive index. Using spectral and time-resolved optical spectroscopy of single SiV defects, we unveil blue shifts (up to 80 meV) of their emission lines, which are interpreted from model calculations as giant Lamb shifts. Moreover, evidence for a positive correlation between their fluorescence decay rates and emission line widths is observed, as a signature of modifications not only of the photonic local density of states but also of the phononic one, as the nanodiamond size is decreased. Correlative light-electron microscopy of single SiVs and their host nanodiamonds further supports these findings. These results make nanodiamond-SiVs promising as optically driven spin qubits and quantum light sources tunable through nanoscale tailoring of vacuum-field fluctuations.

Laser manufacturing of spatial resolution approaching quantum limit

Atomic and close-to-atom scale manufacturing is a promising avenue toward single-photon emitters, single-electron transistors, single-atom memory, and quantum-bit devices for future communication, computation, and sensing applications. Laser manufacturing is outstanding to this end for ease of beam manipulation, batch production, and no requirement for photomasks. It is, however, suffering from optical diffraction limits. Herein, we report a spatial resolution improved to the quantum limit by exploiting a threshold tracing and lock-in method, whereby the two-order gap between atomic point defect complexes and optical diffraction limit is surpassed, and a feature size of <5 nm is realized. The underlying physics is that the uncertainty of local atom thermal motion dominates electron excitation, rather than the power density slope of the incident laser. We show that the colour centre yield in hexagonal boron nitride is transformed from stochastic to deterministic, and the emission from individual sites becomes polychromatic to monochromatic. As a result, single colour centres in the regular array are deterministically created with a unity yield and high positional accuracy, serving as a step forward for integrated quantum technological applications.

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.

Modular chip-integrated photonic control of artificial atoms in diamond waveguides

A central goal in creating long-distance quantum networks and distributed quantum computing is the development of interconnected and individually controlled qubit nodes. Atom-like emitters in diamond have emerged as a leading system for optically networked quantum memories, motivating the development of visible-spectrum, multi-channel photonic integrated circuit (PIC) systems for scalable atom control. However, it has remained an open challenge to realize optical programmability with a qubit layer that can achieve high optical detection probability over many optical channels. Here, we address this problem by introducing a modular architecture of piezoelectrically actuated atom-control PICs (APICs) and artificial atoms embedded in diamond nanostructures designed for high-efficiency free-space collection. The high-speed four-channel APIC is based on a splitting tree mesh with triple-phase shifter Mach–Zehnder interferometers. This design simultaneously achieves optically broadband operation at visible wavelengths, high-fidelity switching (&gt;40dB) at low voltages, submicrosecond modulation timescales (&gt;30MHz), and minimal channel-to-channel crosstalk for repeatable optical pulse carving. Via a reconfigurable free-space interconnect, we use the APIC to address single silicon vacancy color centers in individual diamond waveguides with inverse tapered couplers, achieving efficient single photon detection probabilities (∼15%) and second-order autocorrelation measurements g(2)(0)&lt;0.14 for all channels. The modularity of this distributed APIC–quantum memory system simplifies the quantum control problem, potentially enabling further scaling to thousands of channels.

Polarization study of single color centers in aluminum nitride

Color centers in wide-bandgap semiconductors are a promising class of solid-state quantum light source, many of which operate at room temperature. We examine a family of color centers in aluminum nitride, which emits close to 620 nm. We present a technique to rapidly map an ensemble of these single photon emitters, identifying all emitters, not just those with absorption dipole parallel to the laser polarization. We demonstrate a fast technique to determine their absorption polarization orientation in the c-plane, finding they are uniformly distributed in orientation, in contrast to many other emitters in crystalline materials.

Scalable manufacturing of quantum light emitters in silicon under rapid thermal annealing.

Quantum light sources play a fundamental role in quantum technologies ranging from quantum networking to quantum sensing and computation. The development of these technologies requires scalable platforms, and the recent discovery of quantum light sources in silicon represents an exciting and promising prospect for scalability. The usual process for creating color centers in silicon involves carbon implantation into silicon, followed by rapid thermal annealing. However, the dependence of critical optical properties, such as the inhomogeneous broadening, the density, and the signal-to-background ratio, on centers implantation steps is poorly understood. We investigate the role of rapid thermal annealing on the dynamic of the formation of single color centers in silicon. We find that the density and the inhomogeneous broadening greatly depend on the annealing time. We attribute the observations to nanoscale thermal processes occurring around single centers and leading to local strain fluctuations. Our experimental observation is supported by theoretical modeling based on first principles calculations. The results indicate that annealing is currently the main step limiting the scalable manufacturing of color centers in silicon.

Fabrication of single color centers in sub-50 nm nanodiamonds using ion implantation

Abstract Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV−) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV− centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV− centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV− centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ∼20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.

Микроспектроскопия единичных центров окраски в щелочно-галоидных кристаллах

Single color centers in the LiF crystal were studied by confocal fluorescence microscopy with analysis and statistical processing of the time dependences of their fluorescence intensity. The possibility of identifying quantum systems whose selection by luminescence excitation (absorption) spectra, luminescence spectra, and luminescence decay time is difficult due to their overlap or due to the coincidence of the corresponding characteristics of different centers is shown. An additional identification feature in this case is the flicker frequency and other characteristics of the time dependences of the luminescence intensity. The efficiency of the method is demonstrated by the example of two color centers of different nature (F2 and F3, stabilized by an impurity–vacancy dipole) in a lithium fluoride crystal.

Microscopic Study of Optically Stable Coherent Color Centers in Diamond Generated by High-Temperature Annealing

Single color centers in solid have emerged as promising physical platforms for quantum information science. Creating these centers with excellent quantum properties is a key foundation for further technological developments. In particular, the microscopic understanding of the spin-bath environments is the key to engineer color centers for quantum control. In this work, we propose and demonstrate a distinct high-temperature annealing (HTA) approach for creating high-quality nitrogen vacancy (N-V) centers in implantation-free diamonds. Simultaneously using the created N-V centers as probes for their local environment we verify that no damage is microscopically induced by the HTA. Nearly all single N-V centers created in ultralow-nitrogen-concentration membranes possess stable and Fourier-transform-limited optical spectra. Furthermore, HTA strongly reduces noise sources naturally grown in ensemble samples, and leads to more than threefold improvements of decoherence time and sensitivity. We also verify that the vacancy activation and defect reformation, especially H3 and P1 centers, can explain the reconfiguration between spin baths and color centers. This distinct approach will become a powerful tool in vacancy-based quantum technology.

Quantum Interference of Resonance Fluorescence from Germanium-Vacancy Color Centers in Diamond

Resonance fluorescence from a quantum emitter is an ideal source to extract indistinguishable photons. By using the cross-polarization to suppress the laser scattering, we observed resonance fluorescence from GeV color centers in diamond at cryogenic temperature. The Fourier-transform-limited line width emission with T2/2T1 ∼ 0.86 allows for two-photon interference based on single GeV color center. Under pulsed excitation, the separated photons exhibit a Hong-Ou-Mandel quantum interference above classical limit, whereas the continuous-wave excitation leads to a coalescence time window of 1.05 radiative lifetime. In addition, we demonstrated a single-shot readout of spin states with a fidelity of 74%. Our experiments lay down the foundation for building a quantum network with GeV color centers in diamond.

Resonant and phonon-assisted ultrafast coherent control of a single hBN color center

Single-photon emitters in solid-state systems are important building blocks for scalable quantum technologies. Recently, quantum light emitters have been discovered in the wide-gap van der Waals insulator hexagonal boron nitride (hBN). These color centers have attracted considerable attention due to their quantum performance at elevated temperatures and wide range of transition energies. Here, we demonstrate coherent state manipulation of a single hBN color center with ultrafast laser pulses and investigate in our joint experiment–theory study the coupling between the electronic system and phonons. We demonstrate that coherent control can be performed not only resonantly on the optical transition giving access to the decoherence but also phonon-assisted, which reveals the internal phonon quantum dynamics. In the case of optical phonons, we measure their decoherence, stemming in part from their anharmonic decay. Dephasing induced by the creation of acoustic phonons manifests as a rapid decrease in the coherent control signal when traveling phonon wave packets are emitted. Furthermore, we demonstrate that the quantum superposition between a phonon-assisted process and resonant excitation causes ultrafast oscillations of the coherent control signal. Our results pave the way for ultrafast phonon quantum state control on the nanoscale and open up a new promising perspective for hybrid quantum technologies.

Optical and Spin Properties of NV Center Ensembles in Diamond Nano-Pillars.

Nitrogen-vacancy (NV) color centers in diamond are excellent quantum sensors possessing high sensitivity and nano-scale spatial resolution. Their integration in photonic structures is often desired, since it leads to an increased photon emission and also allows the realization of solid-state quantum technology architectures. Here, we report the fabrication of diamond nano-pillars with diameters up to 1000 nm by electron beam lithography and inductively coupled plasma reactive ion etching in nitrogen-rich diamonds (type Ib) with [100] and [111] crystal orientations. The NV centers were created by keV-He ion bombardment and subsequent annealing, and we estimate an average number of NVs per pillar to be 4300 ± 300 and 520 ± 120 for the [100] and [111] samples, respectively. Lifetime measurements of the NVs’ excited state showed two time constants with average values of τ1 ≈ 2 ns and τ2 ≈ 8 ns, which are shorter as compared to a single color center in a bulk crystal (τ ≈ 10 ns). This is probably due to a coupling between the NVs as well as due to interaction with bombardment-induced defects and substitutional nitrogen (P1 centers). Optically detected magnetic resonance measurements revealed a contrast of about 5% and average coherence and relaxation times of T2 [100] = 420 ± 40 ns, T2 [111] = 560 ± 50 ns, and T1 [100] = 162 ± 11 μs, T1 [111] = 174 ± 24 μs. These pillars could find an application for scanning probe magnetic field imaging.

Narrow-linewidth diamond single-photon sources prepared via femtosecond laser

Nitrogen-vacancy (NV) color centers in diamonds with narrow optical linewidths are commonly used as solid-state single-photon sources that emit indistinguishable photons. However, NV color centers prepared using ion implantation typically have large optical linewidths of over 100 MHz. Herein, we used the femtosecond laser direct writing (FsLDW) technique to prepare single NV color centers in diamond with a narrow optical linewidth of 13.05 ± 0.2 MHz and a long decoherence time of 445 ± 27.6 μs. In addition, the density functional theory was adopted to establish calculation models and illustrate why single NV color centers prepared by FsLDW have narrower linewidths compared to those of the ion implantation method. Thus, this study provides an effective reference for the preparation of narrow-linewidth single-color centers in diamonds and other wide-gap crystals.

Theoretical calculation of fiber cavity coupling silicon carbide membrance

Single spin color centers in solid materials are one of the promising candidates for quantum information processing, and attract a great deal of interest. Nowadays, single spin color centers in silicon carbide, such as divacancies and silicon vacancies have been developed rapidly, because they not only have similar properties of the NV centers in diamond, but also possess infrared fluorescence that is more favorable for transmission in optical fiber. However, these centers possess week fluorescence with broad spectrum, which prevents some key technologies from being put into practical application, such as quantum key distribution, photon-spin entanglement, spin-spin entanglement and quantum sensing. Therefore, optical resonator is very suitable for coupling centers to filter their spectrum and enhance the fluorescence by Purcell effect. It is very advantageous to use the fiber end face as cavity mirrors, thereby the fiber can provide small cavity volume corresponding to a large enhancement in spin color centers, and collect the fluorescence in cavity simultaneously, which has no extra loss in comparison with other collection methods. In this work, the properties and performance of fiber Fabry-Perot cavity coupling silicon carbide membrane are mainly studied through theoretical calculation. Firstly, some parameters are optimized such as membrane roughness and mirror reflection by calculating the mode of the fiber cavity and enhancing the color centers coupling into the cavity, then analyzing the properties of different modes in cavity, the enhancement effect on cavity coupling color centers, and other relevant factors affecting the cavity coupling color centers. Next, the influences of dominated factor and vibration on the properties of the cavity, the enhancement and outcoupling of centers coupled into the cavity are investigated, and finally the optimal outcoupling efficiency corresponding to different vibration intensities is obtained. These results give direct guidance for the further experimental design and direction for optimization of the fiber cavity coupling color centers.

Optical coupling between a single tin-vacancy center and a photonic crystal cavity in diamond

16-fold enhancement of spontaneous emission rate of a single new color center in diamond is achieved using a high-quality factor photonic crystal nanocavity for efficient spin-photon interfaces.