Hao Li, Jun-Yu Ou, Behrad Gholipour, JinKyu So, Davide Piccinotti, Vassili Fedotov, Nikitas Papasimakis
We demonstrate experimentally that the distribution of the decay rates of nitrogen-vacancy centers in diamond becomes narrower by over five times for nanodiamonds embedded in thin chalcogenide films.
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We experimentally demonstrate a broadband enhancement of emission from nitrogen vacancy centers in nanodiamonds. The enhancement is achieved by using a multilayer metamaterial with hyperbolic dispersion. The metamaterial is fabricated as a stack of alternating gold and alumina layers. Our approach paves the way towards the construction of efficient single-photon sources as planar on-chip devices.
Nanodiamonds containing luminescent point defects are widely explored for applications in quantum bio-sensing such as nanoscale magnetometry, thermometry, and electrometry. A key challenge in the development of such applications is a large variation in fluorescence properties observed between particles, even when obtained from the same batch or nominally identical fabrication processes. By theoretically modelling the emission of nitrogen-vacancy colour centres in spherical nanoparticles, we are able to show that the fluorescence spectrum varies with the exact position of the emitter within the…
Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence
本研究结合扫描电子显微镜阴极荧光与干涉测量法，利用纳米金刚石氮-空位中心作为量子发射体，首次在纳米分辨率下实验揭示了其与表面等离极化激元耦合产生的Purcell效应及寿命缩短现象。
Fluorescent nanodiamonds are attracting major attention in the field of bio-sensing and biolabeling. In this work we demonstrate a robust approach to surface functionalize individual nanodiamonds with metal-phenolic networks that enhance the photoluminescence from single nitrogen vacancy (NV) centers. We show that single NV centres in the coated nanodiamonds also exhibit shorter lifetimes, opening another channel for high resolution sensing. We propose that the nanodiamond encapsulation suppresses the non-radiative decay pathways of the NV color centers. Our results provide a versatile and ass…
A nitrogen-vacancy (NV$^-$) center in a nanodiamond, levitated in high vacuum, has recently been proposed as a probe for demonstrating mesoscopic center-of-mass superpositions \cite{Scala2013, Zhang2013} and for testing quantum gravity \cite{Albrecht2014}. Here, we study the behavior of optically levitated nanodiamonds containing NV$^-$ centers at sub-atmospheric pressures and show that while they burn in air, this can be prevented by replacing the air with nitrogen. However, in nitrogen the nanodiamonds graphitize below $\approx 10$ mB. Exploiting the Brownian motion of a levitated nanodiamon…
We present the first evidence of nitrogen vacancy (NV) photoluminescence from a nanodiamond suspended in a free-space optical dipole trap at atmospheric pressure. The photoluminescence rates are shown to decrease with increasing trap laser power, but are inconsistent with a thermal quenching process. For a continuous-wave trap, the neutral charge state (NV$^0$) appears to be suppressed. Chopping the trap laser yields higher total count rates and results in a mixture of both NV$^0$ and the negative charge state (NV$^-$).
We have characterized thermal susceptibilities of the spectral band at 740 nm of silicon-vacancy (SiV) centers in Si- and Si,P-doped nanodiamonds over a temperature range from 295 K to 350 K, which is of interest for thermometry in biological systems. Si-doped crystals reveal linear dependence of the SiV zero-phonon line position, width and relative amplitude with susceptibilities of 0.0126(4) nm/K, 0.062(2) nm/K and $-0.037(2)$ K$^{-1}$, respectively. Si,P-doped nanodiamonds show significantly smaller (up to 35 % for the width) susceptibilities and prove control of SiV properties with additio…
Silicon vacancy (SiV) centers in diamonds have emerged as a very promising candidate for quantum emitter due to their narrow emission line resulting in their indistinguishability. While many different quantum emitters have already been used for excitation of various propagating plasmonic modes, the corresponding exploitation of SiV centers remained so far uncharted territory. Here, we report on excitation of surface plasmon modes supported by silver nanowires using SiV centers in nanodiamonds. The coupling of SiV center fluorescence to surface plasmons is observed, when a nanodiamond situated …
Nanodiamonds containing color centers open up many applications in quantum information processing, metrology, and quantum sensing. In particular, silicon vacancy (SiV) centers are prominent candidates as quantum emitters due to their beneficial optical qualities. Here we characterize nanodiamonds produced by a high-pressure high-temperature method without catalyst metals, focusing on two samples with clear SiV signatures. Different growth temperatures and relative content of silicon in the initial compound between the samples altered their nanodiamond size distributions and abundance of SiV ce…
Two-Photon Interference from Silicon-Vacancy Centers in Remote Nanodiamonds
本研究展示了远程纳米金刚石中两个硅空位中心的双光子干涉，Hong-Ou-Mandel效率达61%，为混合量子技术提供了新途径。
Nitrogen-Vacancy Color Centers in Nanodiamonds as Reference Single-Photon Emitters
针对单量子发射体缺乏参考标准的问题，本文提出含单个 NV⁻ 色心的纳米金刚石，并通过跨实验室重测验证其可作为稳定可靠的单光子发射参考标准。
Strongly Coupled Spins of Silicon-Vacancy Centers Inside a Nanodiamond with Sub-Megahertz Linewidth
本研究考察纳米金刚石中带负电硅空位中心的自旋环境，实现电子自旋强耦合且退相干率低于1 MHz，并展示构建多自旋量子存储器寄存器的潜力。
Nanoscale thermometry is paramount to study primary processes of heat transfer in solids and is a subject of hot debate in cell biology. Here we report ultrafast temperature sensing using all-optical thermometry exploiting synthetic nanodiamonds with silicon-vacancy (SiV) centres embedded at a high concentration. Using multi-parametric analysis of photoluminescence (PL) of these centres, we have achieved an intrinsic noise floor of about 10 mK Hz$^{-1/2}$, which is a thousand-fold increase in the readout speed in comparison to the current record values demonstrated with all-optical methods of …
Spectral diffusion is the phenomenon of random jumps in the emission wavelength of narrow lines. This phenomenon is a major hurdle for applications of solid state quantum emitters like quantum dots, molecules or diamond defect centers in an integrated quantum optical technology. Here, we provide further insight into the underlying processes of spectral diffusion of the zero phonon line of single nitrogen vacancy centers in nanodiamonds by using a novel method based on photon correlation interferometry. The method works although the spectral diffusion rate is several orders of magnitude higher …
Nanodiamonds containing negatively charged nitrogen vacancy centres (${\text{NV}}^{-}$) have applications as localized sensors in biological material and have been proposed as a platform to probe the macroscopic limits of spatial superposition and the quantum nature of gravity. A key requirement for these applications is to obtain nanodiamonds containing ${\text{NV}}^{-}$ with long spin coherence times. Using milling to fabricate nanodiamonds processes the full 3D volume of the bulk material at once, unlike etching, but has, up to now, limited ${\text{NV}}^{-}$ spin coherence times. Here, we u…
Using an optical tweezers apparatus, we demonstrate three-dimensional control of nanodiamonds in solution with simultaneous readout of ground-state electron-spin resonance (ESR) transitions in an ensemble of diamond nitrogen-vacancy (NV) color centers. Despite the motion and random orientation of NV centers suspended in the optical trap, we observe distinct peaks in the measured ESR spectra qualitatively similar to the same measurement in bulk. Accounting for the random dynamics, we model the ESR spectra observed in an externally applied magnetic field to enable d.c. magnetometry in solution. …
Ultrafast emission rates obtained from quantum emitters coupled to plasmonic nanoantennas have recently opened fundamentally new possibilities in quantum information and sensing applications. Plasmonic nanoantennas greatly improve the brightness of quantum emitters by dramatically shortening their fluorescence lifetimes. Gap plasmonic nanocavities that support strongly confined modes are of particular interest for such applications. We demonstrate single-photon emission from nitrogen-vacancy (NV) centers in nanodiamonds coupled to nanosized gap plasmonic cavities with internal mode volumes abo…
We demonstrate an optical far-field super-resolution microscopy using array of nitrogen vacancy centers in bulk diamond as near-field optical probes. The local optical field, which transmits through the nanostructures on the diamond surface, is measured by detecting the charge state conversion of nitrogen vacancy center. And the locating of nitrogen vacancy center with spatial resolution of 6.1 nm is realized with the charge state depletion nanoscopy. The nanostructures on the surface of diamond are then imaged with resolution below optical diffraction limit. The results offer an approach to b…
A nanodiamond (ND) hosting nitrogen-vacancy (NV) color centers is attached on the apex of an optical tip for near-field microscopy. Its fluorescence is used to launch surface plasmon-polaritons (SPPs) in a thin polycrystalline gold film. It is shown that the quantum nature of the initial source of light is preserved after conversion to SPPs. This opens the way to a deterministic quantum plasmonics, where single SPPs can be injected at well-defined positions in a plasmonic device produced by top-down approaches.
Ensembles of negatively charged nitrogen vacancy centers (NV-) in diamond have been proposed for sensing of magnetic fields and paramagnetic agents, and as a source of spin-order for the hyperpolarization of nuclei in magnetic resonance applications. To this end, strongly fluorescent nanodiamonds represent promising materials, with large surface areas and dense ensembles of NV-. However, surface effects tend to favor the less useful neutral form, the NV0 centers. Here, we study the fluorescence properties and optically detected magnetic resonance (ODMR) of NV- centers as a function of laser po…
Enhanced Spectral Density of a Single Germanium Vacancy Center in a Nanodiamond by Cavity-Integration
本文利用原子力显微镜纳米操控将含单个GeV$^-$色心的纳米金刚石集成到高精细度法布里-珀罗微腔中，实现48倍光谱密度增强，为高效自旋-光子平台奠定基础。
Molecular imaging refers to a class of noninvasive biomedical imaging techniques with the sensitivity and specificity to image biochemical variations in-vivo. An ideal molecular imaging technique visualizes a biochemical target according to a range of criteria, including high spatial and temporal resolution, high contrast relative to non-targeted tissues, depth-independent penetration into tissue, lack of harm to the organism under study, and low cost. Because no existing molecular imaging modality is ideal for all purposes, new imaging approaches are needed. Here we demonstrate a novel molecu…
We present the results of work on a hybrid material composed of a tellurite glass rod doped with nanodiamonds containing nitrogen-vacancy-nitrogen and paramagnetic nitrogen-vacancy color centers. The reported results include details on tellurite glass and cane fabrication, confocal and wide-field imaging of the nanodiamond distribution in their volume, as well as on the spectroscopic characterization of their fluorescence and Optically Detected Magnetic Resonance measurements of magnetic fields and temperatures. Magnetic fields up to 50 G were examined with a sensitivity of 10$^{-5}$ T Hz$^{-1…
Nanoscale graphitization and defect evolution in silicon-vacancy center-containing nanodiamonds under high-pressure high-temperature annealing
该研究通过原位同步辐射X射线衍射确定了含SiV色心的纳米金刚石高温高压退火的石墨化阈值，建立了规避石墨化的工艺窗口，改善了其光学响应以用于量子技术。
Coherent exchange of single photons is at the heart of applied Quantum Optics. The negatively-charged silicon vacancy center in diamond is among most promising sources for coherent single photons. Its large Debye-Waller factor, short lifetime and extraordinary spectral stability is unique in the field of solid-state single photon sources. However, the excitation and detection of individual centers requires high numerical aperture optics which, combined with the need for cryogenic temperatures, puts technical overhead on experimental realizations. Here, we investigate a hybrid quantum photonics…
Nitrogen-vacancy (NV) centers in diamonds are interesting due to their remarkable characteristics that are well suited to applications in quantum-information processing and magnetic field sensing, as well as representing stable fluorescent sources. Multiple NV centers in nanodiamonds (NDs) are especially useful as biological fluorophores due to their chemical neutrality, brightness and room-temperature photostability. Furthermore, NDs containing multiple NV centers also have potential in high-precision magnetic field and temperature sensing. Coupling NV centers to propagating surface plasmon p…
Using a nanomanipulation technique a nanodiamond with a single nitrogen vacancy center is placed directly on the surface of a gallium phosphide photonic crystal cavity. A Purcell-enhancement of the fluorescence emission at the zero phonon line (ZPL) by a factor of 12.1 is observed. The ZPL coupling is a first crucial step towards future diamond-based integrated quantum optical devices.
The zero-phonon transition rate of a nitrogen-vacancy center is enhanced by a factor of ~70 by coupling to a photonic crystal resonator fabricated in monocrystalline diamond using standard semiconductor fabrication techniques. Photon correlation measurements on the spectrally filtered zero-phonon line show antibunching, a signature that the collected photoluminescence is emitted primarily by a single nitrogen-vacancy center. The linewidth of the coupled nitrogen-vacancy center and the spectral diffusion are characterized using high-resolution photoluminescence and photoluminescence excitation …
Nitrogen-Vacancy Emission from Nanodiamond: Size, Depth, and Surroundings
研究揭示纳米金刚石中氮空位发射受尺寸、深度和周围环境影响，提出混合模型整合电磁模拟与量子光学理论，推动量子发射器光物理的理解。
Optically levitated nanodiamonds with nitrogen-vacancy centers promise a high-quality hybrid spin-optomechanical system. However, the trapped nanodiamond absorbs energy form laser beams and causes thermal damage in vacuum. We propose to solve the problem by trapping a composite particle (a nanodiamond core coated with a less absorptive silica shell) at the center of strongly focused doughnut-shaped laser beams. Systematical study on the trapping stability, heat absorption, and oscillation frequency concludes that the azimuthally polarized Gaussian beam and the linearly polarized Laguerre-Gauss…
Levitated nanodiamonds containing nitrogen vacancy centres in high vacuum are a potential test bed for numerous phenomena in fundamental physics. However, experiments so far have been limited to low vacuum due to heating arising from optical absorption of the trapping laser. We show that milling pure diamond creates nanodiamonds that do not heat up as the optical intensity is raised above 700 GW/m$^2$ below 5 mbar of pressure. This advance now means that the level of attainable vacuum for nanodiamonds in optical dipole traps is no longer temperature limited.
A fully integrated quantum optical technology requires active quantum systems incorporated into resonant optical microstructures and inter-connected in three dimensions via photonic wires. Nitrogen vacancy-centres (NV-centres) in diamond which are excellent photostable room temperature single-photon emitters are ideal candidates for that purpose. Extensive research efforts to couple NV-centres to photonic structures such as optical microresonators, microcavities, and waveguides have been pursued. Strategies for integration range from top-down fabrication via etching of diamond membranes to sop…
We present a beam-directed chemical technique for controlling the charge states of near-surface luminescence centers in semiconductors. Specifically, we fluorinate the surface of H-terminated diamond by electron beam irradiation in the presence of NF3 vapor. The fluorination treatment acts as a local chemical switch that alters the charge state of nitrogen-vacancy luminescence centers from the neutral to the negative state. The electron beam fluorination process is highly localized and can be used to control the emission spectrum of individual nanodiamonds and surface regions scanned by the el…
The photoluminescence of nitrogen-vacancy (NV) centers in diamond nanoparticles exhibits specific properties as compared to NV centers in bulk diamond. For instance large fluctuations of lifetime and brightness from particle to particle have been reported. It has also been observed that for nanocrystals much smaller than the mean luminescence wavelength, the particle size sets a lower threshold for resolution in Stimulated Emission Depletion (STED) microscopy. We show that all these features can be quantitatively understood by realizing that the absorption-emission of light by the NV center is…
Electron spins of diamond nitrogen-vacancy (NV) centers are important quantum resources for nanoscale sensing and quantum information. Combining NV spins with levitated optomechanical resonators will provide a hybrid quantum system for novel applications. Here we optically levitate a nanodiamond and demonstrate electron spin control of its built-in NV centers in low vacuum. We observe that the strength of electron spin resonance (ESR) is enhanced when the air pressure is reduced. To better understand this system, we investigate the effects of trap power and measure the absolute internal temper…
We describe and experimentally demonstrate a technique for deterministic coupling between a photonic crystal (PC) nanocavity and single emitters. The technique is based on in-situ scanning of a PC cavity over a sample and allows the positioning of the cavity over a desired emitter with nanoscale resolution. The power of the technique, which we term a Scanning Cavity Microscope (SCM), is demonstrated by coupling the PC nanocavity to a single nitrogen vacancy (NV) center in diamond, an emitter system that provides optically accessible electron and nuclear spin qubits.
Nitrogen-vacancy centers in diamond are attractive as quantum sensors owing to their remarkable optical and spin properties under ambient conditions. Here we experimentally demonstrated a hybrid fiber-based thermometer coupled with nitrogen-vacancy center ensemble and a permanent magnet, where the temperature sensitivity was improved by converting the temperature variation to the magnetic field change based on the thermal-demagnetization of the permanent magnet. We have achieved both large temperature working range (room temperature to 373 K) and millikelvin sensitivity (1.6 mK/sqrt(Hz)), near…
Surface plasmon polaritons (SPPs) are locally excited at silver surfaces using (~100) nm-sized nanodiamonds (NDs) with multiple nitrogen-vacancy (NV) centers (~400). The fluorescence from an externally illuminated (at 532 nm) ND and from nearby NDs, which are not illuminated but produce out-of-plane scattering of SPPs excited by the illuminated ND, exhibit distinctly different wavelength spectra, showing short-wavelength filtering due to the SPP propagation loss. The results indicate that NDs with multiple NV centers can be used as efficient sub-wavelength SPP sources in planar integrated plas…
Optically detected magnetic resonance of nitrogen-vacancy centers in diamond using two-photon excitation
本研究利用双光子激发技术在室温下观测钻石中氮-空位中心的基态光学检测磁共振，实现了对NV中心分布的成像，并首次展示了双光子激发下的ODMR轨迹，为快速三维量子传感和成像提供了新工具。
Template-Assisted Self Assembly of Fluorescent Nanodiamonds for Scalable Quantum Technologies
提出一种毛细管驱动的模板辅助自组装方法，实现直径低于50 nm的纳米金刚石在毫米级区域的精确有序排列，并基于200余个样品的统计测量揭示了NV中心性质与尺寸无关，为量子器件集成奠定基础。
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