Magnetic impurities in diamond influence the relaxation properties and thus limit the sensitivity of magnetic, electric, strain, and temperature sensors based on nitrogen-vacancy color centers. Diamond samples may exhibit significant spatial variations in the impurity concentrations hindering the quantitative analysis of relaxation pathways. Here, we present a local measurement technique which can be used to determine the concentration of various species of defects by utilizing double electron-electron resonance. This method will help to improve the understanding of the physics underlying spin relaxation and guide the development of diamond samples, as well as offering protocols for optimized sensing.
In this work we use fluorescence from nitrogen-vacancy defects in diamond to detect and explore other paramagnetic defects in the diamond, such as P1 defects, which are commonly undetectable through optical detection of magnetic resonance in standard conditions. Our method does not require overlap between the defects' resonances and therefore is applicable in a wide region of magnetic fields and frequencies, as verified by excellent fit to theoretical predictions. We propose a depolarization scheme of P1 defects to account for the observed data. To verify our results, we perform cavity-based d…
We study a spin-phononic system where diamond defect centers are interfaced with a quasi-one-dimensional phononic crystal. We show that, a single defect center, coupled to the phonon modes of a phononic crystal waveguide near the band gap, can seed its own phononic cavity mode with an exponentially decaying envelope around the defect center's position. The spin-induced phononic cavity, with a greatly reduced and tunable mode volume, allows coherent phonon-mediated interactions between distant spins with a highly tunable range, enabling access to a variety of long-range interacting spin models.…
In this paper, we study the photoinduced switching of the nitrogen-vacancy (NV) center between two different charge states - negative (NV-) and neutral (NV0) at liquid helium temperature. The conversion of NV- to NV0 on a single defect is experimentally proven and its rate scales quadratically with power under resonant excitation. In addition, we found that resonant excitation of the neutral NV changes the charge state, recovering its negative configuration. This type of conversion significantly improves spectral stability of NV- defect and allows high fidelity initialization of the spin qubit…
We demonstrate coherent control of the optical transition of single Nitrogen-Vacancy defect centers in diamond. On applying short resonant laser pulses, we observe optical Rabi oscillations with a half-period as short as 1 nanosecond, an order of magnitude shorter than the spontaneous emission time. By studying the decay of Rabi oscillations, we find that the decoherence is dominated by laser-induced spectral jumps. By using a low-power probe pulse as a detuning sensor and applying post-selection, we demonstrate that spectral diffusion can be overcome in this system to generate coherent photon…
We propose a fast, scalable all-optical design for arbitrary two-qubit operations for defect qubits in diamond (NV centers) and in silicon carbide, which are promising candidates for room temperature quantum computing. The interaction between qubits is carried out by microcavity photons. The approach uses constructive interference from higher energy excited states activated by optical control. In this approach the cavity mode remains off-resonance with the directly accessible optical transitions used for initialization and readout. All quantum operations are controlled by near-resonant narrow-…
The nitrogen-vacancy color center in diamond has rapidly emerged as an important solid-state system for quantum information processing. While individual spin registers have been used to implement small-scale diamond quantum computing, the realization of a large-scale device requires development of an on-chip quantum bus for transporting information between distant qubits. Here we propose a method for coherent quantum transport of an electron and its spin state between distant NV centers. Transport is achieved by the implementation of spatial stimulated adiabatic Raman passage through the optic…
Wide field-of-view magnetic field microscopy has been realised by probing shifts in optically detected magnetic resonance (ODMR) spectrum of Nitrogen Vacancy (NV) defect centers in diamond. However, these widefield diamond NV magnetometers require few to several minutes of acquisition to get a single magnetic field image, rendering the technique temporally static in it's current form. This limitation prevents application of diamond NV magnetometers to novel imaging of dynamically varying microscale magnetic field processes. Here, we show that the magnetic field imaging frame rate can be signif…
A promising approach for multi-qubit quantum registers is to use optically addressable spins to control multiple dark electron-spin defects in the environment. While recent experiments have observed signatures of coherent interactions with such dark spins, it is an open challenge to realize the individual control required for quantum information processing. Here we demonstrate the initialisation, control and entanglement of individual dark spins associated to multiple P1 centers, which are part of a spin bath surrounding a nitrogen-vacancy center in diamond. We realize projective measurements …
Diamond defect centers are promising solid state magnetometers. Single centers allow for high spatial resolution field imaging but are limited in their magnetic field sensitivity to around 10 nT/Hz^(1/2) at room-temperature. Using defect center ensembles sensitivity can be scaled as N^(1/2) when N is the number of defects. In the present work we use an ensemble of 1e11 defect centers for sensing. By carefully eliminating all noise sources like laser intensity fluctuations, microwave amplitude and phase noise we achieve a photon shot noise limited field sensitivity of 0.9 pT/Hz^(1/2) at room-te…
Diamond materials are central to an increasing range of advanced technological demonstrations, from high power electronics, to nano-scale quantum bio-imaging with unprecedented sensitivity. However, the full exploitation of diamond for these applications is often limited by the uncontrolled nature of the diamond material surface, which suffers from Fermi-level pinning and hosts a significant density of electro-magnetic noise sources. These issues occur despite the oxide-free and air-stable nature of the diamond crystal surface, which should be an ideal candidate for functionalization and chemi…
Individual, luminescent point defects in solids so called color centers are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: First, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of single-crystal diamond. Second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging bas…
We propose an experiment that would produce and measure a large Aharonov-Casher (A-C) phase in a solid-state system under macroscopic motion. A diamond crystal is mounted on a spinning disk in the presence of a uniform electric field. Internal magnetic states of a single NV defect, replacing interferometer trajectories, are coherently controlled by microwave pulses. The A-C phase shift is manifested as a relative phase, of up to 17 radians, between components of a superposition of magnetic substates, which is two orders of magnitude larger than that measured in any other atom-scale quantum sys…
We report a systematic study of the hyperfine interaction between the electron spin of a single nitrogen-vacancy (NV) defect in diamond and nearby $^{13}$C nuclear spins, by using pulsed electron spin resonance spectroscopy. We isolate a set of discrete values of the hyperfine coupling strength ranging from 14 MHz to 400 kHz and corresponding to $^{13}$C nuclear spins placed at different lattice sites of the diamond matrix. For each lattice site, the hyperfine interaction is further investigated through nuclear spin polarization measurements and by studying the magnetic field dependence of the…
Diamond photonics is an ever growing field of research driven by the prospects of harnessing diamond and its colour centres as suitable hardware for solid-state quantum applications. The last two decades have seen the field been shaped by the nitrogen-vacancy (NV) centre both with breakthrough fundamental physics demonstrations and practical realizations. Recently however, an entire suite of other diamond defects has emerged. They are M V colour centres, where M indicates one of the elements in the IV column of the periodic table Si, Ge, Sn and Pb, and V indicates lattice vacancies, i.e. missi…
We report a magnetic field dependence of fluorescence of diamond single crystals containing NV$^-$ centers. In such spectra, numerous sharp lines are found, which correspond to Level Anti-Crossings (LACs) in coupled spins systems comprising an NV$^-$ center. Theoretical modeling of such "LAC-spectra" enables characterization of paramagnetic defect centers and determination of their magnetic resonance parameters, such as zero-field splitting and hyperfine coupling constants. The outlined method thus enables sensitive detection of paramagnetic impurities in diamond crystals.
The nitrogen-vacancy (NV) defect in diamond is an efficient quantum sensor of randomly fluctuating signals via relaxometry measurements. In particular, the longitudinal spin relaxation of the NV defect accelerates in the presence of magnetic noise with a spectral component at its electron spin resonance frequency. We look into this effect quantitatively by applying a calibrated and tunable magnetic noise on a single NV defect. We show that an increase of the longitudinal spin relaxation rate translates into a reduction of the photoluminescence (PL) signal emitted under continuous optical illum…
We investigate spin and optical properties of individual nitrogen-vacancy centers located within 1-10 nm from the diamond surface. We observe stable defects with a characteristic optically detected magnetic resonance spectrum down to lowest depth. We also find a small, but systematic spectral broadening for defects shallower than about 2 nm. This broadening is consistent with the presence of a surface paramagnetic impurity layer [Tisler et al., ACS Nano 3, 1959 (2009)] largely decoupled by motional averaging. The observation of stable and well-behaved defects very close to the surface is criti…
Measuring local temperature with a spatial resolution on the order of a few nanometers has a wide range of applications from semiconductor industry over material to life sciences. When combined with precision temperature measurement it promises to give excess to small temperature changes caused e.g. by chemical reactions or biochemical processes. However, nanoscale temperature measurements and precision have excluded each other so far owing to the physical processes used for temperature measurement of limited stability of nanoscale probes. Here we experimentally demonstrate a novel nanoscale t…
Laser writing with ultrashort pulses provides a potential route for the manufacture of three-dimensional wires, waveguides and defects within diamond. We present a transmission electron microscopy (TEM) study of the intrinsic structure of the laser modifications and reveal a complex distribution of defects. Electron energy loss spectroscopy (EELS) indicates that the majority of the irradiated region remains as $sp^3$ bonded diamond. Electrically-conductive paths are attributed to the formation of multiple nano-scale, $sp^2$-bonded graphitic wires and a network of strain-relieving micro-cracks.
The coupling between defects in diamond and a superconducting microwave resonator is studied in the nonlinear regime. Both negatively charged nitrogen-vacancy and P1 defects are explored. The measured cavity mode response exhibits strong nonlinearity near a spin resonance. Data is compared with theoretical predictions and a good agreement is obtained in a wide range of externally controlled parameters. The nonlinear effect under study in the current paper is expected to play a role in any cavity-based magnetic resonance imaging technique and to impose a fundamental limit upon its sensitivity.
Atomic-size spin defects in solids are unique quantum systems. Most applications require nanometer positioning accuracy, which is typically achieved by low energy ion implantation. So far, a drawback of this technique is the significant residual implantation-induced damage to the lattice, which strongly degrades the performance of spins in quantum applications. In this letter we show that the charge state of implantation-induced defects drastically influences the formation of lattice defects during thermal annealing. We demonstrate that charging of vacancies localized at e.g. individual nitrog…
Control over the charge states of color centers in solids is necessary in order to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-bandgap semiconductors are complex, and much remains unknown. Here, we utilize single shot charge state readout of an individual nitrogen-vacancy (NV) center to probe charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many microns away. With this method, we study the optica…
Color centers in diamond have emerged as leading solid-state artificial atoms for a range of quantum technologies, from quantum sensing to quantum networks. Concerted research activities are now underway to identify new color centers that combine stable spin and optical properties of the nitrogen vacancy (NV$^-$) with the spectral stability of the silicon vacancy (SiV$^-$) centers in diamond, with recent research identifying other group IV color centers with superior properties. In this Letter, we investigate a new class of diamond quantum emitters from first principles, the group III color ce…
There has been rapidly growing interest in hybrid quantum devices involving a solid-state spin and a macroscopic mechanical oscillator. Such hybrid devices create exciting opportunities to mediate interactions between disparate qubits and to explore the quantum regime of macroscopic mechanical objects. In particular, a system consisting of the nitrogen-vacancy defect center in diamond coupled to a high quality factor mechanical oscillator is an appealing candidate for such a hybrid quantum device, as it utilizes the highly coherent and versatile spin properties of the defect center. In this pa…
We use the electronic spin of a single Nitrogen-Vacancy (NV) defect in diamond to observe the real-time evolution of neighboring single nuclear spins under ambient conditions. Using a diamond sample with a natural abundance of $^{13}$C isotopes, we first demonstrate high fidelity initialization and single-shot readout of an individual $^{13}$C nuclear spin. By including the intrinsic $^{14}$N nuclear spin of the NV defect in the quantum register, we then report the simultaneous observation of quantum jumps linked to both nuclear spin species, providing an efficient initialization of the two qu…
Coherently coupled pairs or multimers of nitrogen-vacancy defect electron spins in diamond have many promising applications especially in quantum information processing (QIP) but also in nanoscale sensing applications. Scalable registers of spin qubits are essential to the progress of QIP. Ion implantation is the only known technique able to produce defect pairs close enough to allow spin coupling via dipolar interaction. Although several competing methods have been proposed to increase the resulting resolution of ion implantation, the reliable creation of working registers is still to be demo…
Dynamic nuclear spin polarization (DNP) mediated by paramagnetic point defects in semiconductors is a key resource for both initializing nuclear quantum memories and producing nuclear hyperpolarization. DNP is therefore an important process in the field of quantum-information processing, sensitivity-enhanced nuclear magnetic resonance, and nuclear-spin-based spintronics. DNP based on optical pumping of point defects has been demonstrated by using the electron spin of nitrogen-vacancy (NV) center in diamond, and more recently, by using divacancy and related defect spins in hexagonal silicon car…
Fluorescent defects in non-cytotoxic diamond nanoparticles are candidates for qubits in quantum computing, optical labels in biomedical imaging and sensors in magnetometry. For each application these defects need to be optically and thermodynamically stable, and included in individual particles at suitable concentrations (singly or in large numbers). In this letter, we combine simulations, theory and experiment to provide the first comprehensive and generic prediction of the size, temperature and nitrogen-concentration dependent stability of optically active NV defects in nanodiamonds.
Magnetometry and magnetic imaging with nitrogen-vacancy (NV) defects in diamond rely on the optical detection of electron spin resonance (ESR). However, this technique is inherently limited to magnetic fields that are weak enough to avoid electron spin mixing. Here we focus on the high off-axis magnetic field regime for which spin mixing alters the NV defect spin dynamics. We first study in a quantitative manner the dependence of the NV defect optical properties on the magnetic field vector B. Magnetic-field-dependent time-resolved photoluminescence (PL) measurements are compared to a seven-le…
Wide-field magnetometry can be realized by imaging the optically-detected magnetic resonance of diamond nitrogen vacancy (NV) center ensembles. However, NV ensemble inhomogeneities significantly limit the magnetic-field sensitivity of these measurements. We demonstrate a double-double quantum (DDQ) driving technique to facilitate wide-field magnetic imaging of dynamic magnetic fields at a micron scale. DDQ imaging employs four-tone radio frequency pulses to suppress inhomogeneity-induced variations of the NV resonant response. As a proof-of-principle, we use the DDQ technique to image the dc m…
The isolated electronic spin system of the Nitrogen-Vacancy (NV) centre in diamond offers unique possibilities to be employed as a nanoscale sensor for detection and imaging of weak magnetic fields. Magnetic imaging with nanometric resolution and field detection capabilities in the nanotesla range are enabled by the atomic-size and exceptionally long spin-coherence times of this naturally occurring defect. The exciting perspectives that ensue from these characteristics have triggered vivid experimental activities in the emerging field of "NV magnetometry". It is the purpose of this article to …
An unusual variety of impact-related diamond from the Popigai impact structure - yakutites - is characterized by complementary methods including optical microscopy, X-ray diffraction, radiography and tomography, infra-red, Raman and luminescence spectroscopy providing structural information at widely different scales. It is shown that relatively large graphite aggregates may be transformed to diamond with preservation of many morphological features. Spectroscopic and X-ray diffraction data indicate that the yakutite matrix represents bulk nanocrystalline diamond. For the first time, features o…
The nitrogen-vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV-) or neutral (NV0), with photo induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination in dependence of the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and o…
Diamond-based microelectromechanical systems (MEMS) enable direct coupling between the quantum states of nitrogen-vacancy (NV) centers and the phonon modes of a mechanical resonator. One example, diamond high-overtone bulk acoustic resonators (HBARs), feature an integrated piezoelectric transducer and support high-quality factor resonance modes into the GHz frequency range. The acoustic modes allow mechanical manipulation of deeply embedded NV centers with long spin and orbital coherence times. Unfortunately, the spin-phonon coupling rate is limited by the large resonator size, $>100~μ$m, and …
Imaging heat transport in suspended diamond nanostructures with integrated spin defect thermometers
Swiss Federal Institute of Technology Lausanne (EPFL)（洛桑联邦理工学院）；PROUD SA（PROUD公司）；Istituto Nazionale di Ricerca Metrologica (INRiM)（意大利国家计量研究所）；University of Stuttgart（斯图加特大学）
Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon vacancy centers in diamond (SiV) offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times make them very promising candidates for qubits. Here, we have developed arrays of nanopillars containing single SiV centers with high yield, and we demonstr…
We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spi…
We present two applications of a single nitrogen vacancy center in a nanodiamond as quantum probe for plasmonic nanostructures. Coupling to the nanostructures is achieved in a highly controlled manner by picking up a pre-characterized nanocrystal with an atomic force microscope and placing it at the desired position. Local launching of single excitations into a nanowire with a spatial control of few nanometers is demonstrated. Further, a two dimensional map of the electromagnetic environment of a plasmonic bowtie antenna was derived, resembling an ultimate limit of fluorescence lifetime nanosc…
Magnetic field sensing, with its recent advances, is emerging as a viable alternative to measure functional activity of single neurons in the brain by sensing action potential associated magnetic fields (APMFs). Measurement of APMFs of large axons of worms have been possible due to their size. In the mammalian brain, axon sizes, their numbers and routes, restricts using such functional imaging methods. With segmented model of mammalian pyramidal neurons, we show that the APMF of intra-axonal currents in the axon hillock are two orders of magnitude larger than other neuronal locations. Expected…
In this work we investigated the time behavior of the polarization of bulk 13C nuclei in diamond above the thermal equilibrium. This nonthermal nuclear hyperpolarization is achieved by cross relaxation between two nitrogen related paramagnetic defect species in diamond in combination with optical pumping. The decay of the hyperpolarization at four different magnetic fields is measured. Furthermore, we use the comparison with conventional nuclear resonance measurements to identify the involved distances of the nuclear spin with respect to the defects and therefore the coupling strengths. Also, …
Diamond is a promising material for the development of emerging applications in quantum optics, quantum information and quantum sensing. The fabrication and characterization of novel luminescent defects with suitable opto-physical properties is therefore of primary importance for further advances in these research fields. In this work we report on the investigation in the formation of photoluminescent (PL) defects upon MeV He implantation in diamond. Such color centers, previously reported only in electroluminescence and cathodoluminescence regime, exhibited two sharp emission lines at 536.5 n…
First-principles density functional theory methods are used to investigate the structure, energetics, and vibrational motions of the neutral vacancy defect in diamond. The measured optical absorption spectrum demonstrates that the tetrahedral $T_d$ point group symmetry of pristine diamond is maintained when a vacancy defect is present. This is shown to arise from the presence of a dynamic Jahn-Teller distortion that is stabilised by large vibrational anharmonicity. Our calculations further demonstrate that the dynamic Jahn-Teller-distorted structure of $T_d$ symmetry is lower in energy than th…
