The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiamond coupled to a 1D photonic crystal cavity. We assess the Purcell enhancement via three independent measurement techniques and perform autocorrelation measurements at elevated excitation powers in confocal microscopy. Employing a three-level model allows us to extract the setup efficiency, individual transition rates and thus the internal quantum efficiency of our system. Combining our results, we find that the enhancement of the radiative decay rate via the Purcell effect results in an internal quantum efficiency of 90 % for cavity-coupled NV centers. Our findings will facilitate the realization of nano-scale single photon sources with near-unity internal quantum efficiencies operating at high repetition rates.
We demonstrate cooling of ultrathin fiber tapers coupled with nitrogen vacancy (NV) centers in nanodiamonds to cryogenic temperatures. Nanodiamonds containing multiple NV centers are deposited on the subwavelength 480-nm-diameter nanofiber region of fiber tapers. The fiber tapers are successfully cooled to 9 K using our home-built mounting holder and an optimized cooling speed. The fluorescence from the nanodiamond NV centers is efficiently channeled into a single guided mode and shows characteristic sharp zero-phonon lines of both neutral and negatively charged NV centers. The present nanofib…
Nanodiamonds containing nitrogen-vacancy (NV) centers offer a versatile platform for sensing applications spanning from nanomagnetism to in-vivo monitoring of cellular processes. In many cases, however, weak optical signals and poor contrast demand long acquisition times that prevent the measurement of environmental dynamics. Here, we demonstrate the ability to perform fast, high-contrast optical measurements of charge distributions in ensembles of NV centers in nanodiamonds and use the technique to improve the spin readout signal-to-noise ratio through spin-to-charge conversion. A study of 38…
Nanodiamonds containing nitrogen vacancy (NV-) centers show promise for a number of emerging applications including targeted in vivo imaging and generating nuclear spin hyperpolarization for enhanced NMR spectroscopy and imaging. Here, we develop a detailed understanding of the magnetic resonance behavior of NV- centers in an ensemble of nanodiamonds with random crystal orientations. Two-dimensional optically detected magnetic resonance spectroscopy reveals the distribution of energy levels, spin populations, and transition probabilities that give rise to a complex spectrum. We identify overto…
Here we report the size reduction and effects on nitrogen-vacancy centres in nanodiamonds by air oxidation using a combined atomic force and confocal microscope. The average height reduction of individual crystals as measured by atomic force microscopy was 10.6 nm/h at 600 °C air oxidation at atmospheric pressure. The oxidation process modified the surface including removal of non-diamond carbon and organic material which also led to a decrease in background fluorescence. During the course of the nanodiamond size reduction, we observed the annihilation of nitrogen-vacancy centres which provide…
Thanks to their versatility, nitrogen-vacancy (NV) centers in nanodiamonds have been widely adopted as nanoscale sensors. However, their sensitivities are limited by their short coherence times relative to NVs in bulk diamond. A more complete understanding of the origins of decoherence in nanodiamonds is critical to improving their performance. Here we present measurements of fast spin relaxation on qutrit transitions between the energy eigenstates composed of the $m_s = \pm1$ states of the NV$^-$ electronic ground state in $\sim40$-nm nanodiamonds under ambient conditions. For frequency split…
We report on sensing stability of nanodiamond (ND) quantum sensors in various pH aqueous buffer solutions for the two detection schemes of quantum decoherence spectroscopy and thermometry. The electron spin properties of single nitrogen-vacancy (NV) centers in 25-nm-sized NDs have been characterized by a spin-measurement compatible perfusion (SMCP) chamber where observing the same individual NDs in different buffer solutions is possible. With this system, we have determined the stability of the NV quantum sensors during the pH change from 4 to 11 as the fluctuations of +- 12% and +- 0.2 MHz fo…
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…
We propose a scheme to realize universal quantum gates between nitrogen-vacancy (NV) centers in an optically trapped nanodiamond, through uniform magnetic field induced coupling between the NV centers and the torsional mode of the levitated nanodiamond. The gates are tolerant to the thermal noise of the torsional mode. By combining the scheme with dynamical decoupling technology, it is found that the high fidelity quantum gates are possible for the present experimental conditions. The proposed scheme is useful for NV-center-based quantum network and distributed quantum computation
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 …
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confir…
The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen-vacancy centre in diamond - a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen-vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of …
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…
Here we propose and analyse in detail protocols that can achieve rapid hyperpolarization of 13C nuclear spins in randomly oriented ensembles of nanodiamonds at room temperature. Our protocols exploit a combination of optical polarization of electron spins in nitrogen-vacancy centers and the transfer of this polarization to 13C nuclei by means of microwave control to overcome the severe challenges that are posed by the random orientation of the nanodiamonds and their nitrogen-vacancy centers. Specifically, these random orientations result in exceedingly large energy variations of the electron s…
The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that the SiV center in nanodiamond exhibits a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range of approximatly 730 nm to 742 nm and broad linewidths between 5 nm and 17 nm, whereas the second group comprises a…
We experimentally demonstrate the integration of silicon-vacancy centers in nanodiamonds (SiV-NDs) with an optical nanofiber (ONF). We grow SiV-NDs on seed NDs dispersed on a quartz substrate using a microwave plasma-assisted chemical vapor deposition method. First, we search and characterize SiV-NDs on a quartz substrate using an inverted confocal microscope and an atomic force microscope (AFM). Subsequently, we pick up SiV-NDs from the quartz substrate and deposit them on the surface of a free-standing ONF using the AFM tip. The fluorescence emission spectrum, photon count rate, and intensit…
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$^-$).
Fluorescent nanodiamonds (NDs) are crystal defect-based light-emitting nanoparticles that can be applied to quantum information science and quantum sensing. Of particular interest are nitrogen vacancy (NV) centers that allow optical access to their coherently controllable electron spin systems, leading to spin-photon quantum devices and nanoscale sensing of various physical parameters. However, the NV spin coherence time (T2) in NDs has been limited to one or two orders of magnitude shorter than those in bulk diamonds owing to the complicated surface effect that decoheres the NV spin systems. …
Realising controlled quantum dynamics via the magnetic interactions between colour centers in diamond remains a challenge despite recent demonstrations for nanometer separated pairs. Here we propose to use the intrinsic acoustical phonons in diamond as a data bus for accomplishing this task. We show that for nanodiamonds the electron-phonon coupling can take significant values that together with mode frequencies in the THz range, can serve as a resource for conditional gate operations. Based on these results we analyze how to use this phonon-induced interaction for constructing quantum gates a…
We introduce an advanced material system for the production and spectroscopy of single silicon vacancy (SiV) color centers in diamond. We use microwave plasma chemical vapor deposition to synthesize heteroepitaxial nanodiamonds of approx. 160 nm in lateral size with a thickness of approx. 75 nm. These oriented 'nanoislands' combine the enhanced fluorescence extraction from subwavelength sized nanodiamonds with defined crystal orientation. The investigated SiV centers display narrow zero-phonon-lines down to 0.7 nm in the wavelength range 730-750 nm. We investigate in detail the phonon-coupling…
Single silicon vacancy (SiV) color centers in diamond have recently shown the ability for high brightness, narrow bandwidth, room temperature single photon emission. This work develops a model describing the three level population dynamics of single SiV centers in diamond nanocrystals on iridium surfaces including an intensity dependent de-shelving process. Furthermore, we investigate the brightness and photostability of single centers and find maximum single photon rates of 6.2 Mcps under continuous excitation. We investigate the collection efficiency of the fluorescence and estimate quantum …
We present a study of the charge state conversion of single nitrogen-vacancy (NV) defects hosted in nanodiamonds (NDs). We first show that the proportion of negatively-charged NV$^{-}$ defects, with respect to its neutral counterpart NV$^{0}$, decreases with the size of the ND. We then propose a simple model based on a layer of electron traps located at the ND surface which is in good agreement with the recorded statistics. By using thermal oxidation to remove the shell of amorphous carbon around the NDs, we demonstrate a significant increase of the proportion of NV$^{-}$ defects in 10-nm NDs.…
Powered by the mutual developments in instrumentation, materials andtheoretical descriptions, sensing and imaging capabilities of quantum emitters insolids have significantly increased in the past two decades. Quantum emitters insolids, whose properties resemble those of atoms and ions, provide alternative waysto probing natural and artificial nanoscopic systems with minimum disturbance andultimate spatial resolution. Among those emerging quantum emitters, the nitrogen-vacancy (NV) color center in diamond is an outstanding example due to its intrinsicproperties at room temperature (highly-lumi…
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. …
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…
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 investigate the optical properties of silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in nanodiamonds under hydrostatic pressure up to 180 GPa. The nanodiamonds were synthetized by Si or Ge-doped plasma assisted chemical vapor deposition and, for our experiment, pressurized in a diamond anvil cell. Under hydrostatic pressure we observe blue-shifts of the SiV and GeV zero-phonon lines by 17 THz (70 meV) and 78 THz (320 meV), respectively. These measured pressure induced shifts are in good agreement with ab initio calculations that take into account the lattice compression bas…
Optical coupling enables intermediate- and long-range interactions between distant quantum emitters. Such interaction may be the basic element in bottom-up approaches of coupled spin systems or for integrated quantum photonics and quantum plasmonics. Here, we prepare nanodiamonds carrying single, negatively-charged silicon-vacancy centers for evanescent optical coupling with access to all degrees of freedom by means of atomic force nanomanipulation. The color centers feature excellent optical properties, comparable to silicon-vacancy centers in bulk diamond, resulting in a resolvable fine stru…
Interferometry with massive particles may have the potential to explore the limitations of standard quantum mechanics in particular where it concerns its boundary with general relativity and the yet to be developed theory of quantum gravity. This development is hindered considerably by the lack of experimental evidence and testable predictions. Analyzing effects that appear to be common to many of such theories, such as a modification of the energy dispersion and of the canonical commutation relation within the standard framework of quantum mechanics, has been proposed as a possible way forwar…
There is significant interest in potential experimental tests of macroscopic quantum effects, both to test potential modifications to quantum theory and to probe the quantum nature of gravity. A proposed platform with which to generate the required macroscopic quantum spatial superposition is a nanodiamond containing a negatively charged nitrogen vacancy (${\text{NV}}^{-}$) centre. In this review, methods to fabricate nanodiamonds containing ${\text{NV}}^{-}$ suitable for these quantum applications are discussed. The proposed probes of the macroscopic limits of quantum theory are presented alo…
Nitrogen-vacancy centres (NVs) in diamond are attractive for research straddling quantum information science and nanoscale magnetometry and thermometry. While ultrapure bulk diamond NVs sustain the longest spin coherence times among optically accessible spins, nanodiamond NVs display persistently poor spin coherence. Here we introduce high-purity nanodiamonds accommodating record-long NV coherence times, >60 us, observed via universal dynamical decoupling. We show that the main contribution to decoherence comes from nearby nitrogen impurities rather than surface states. We protect the NV spin …
We theoretically show that the dipole force of an ensemble of quantum emitters embedded in a dielectric nanosphere can be exploited to achieve near-field optical levitation. The key ingredient is that the polarizability from the ensemble of embedded quantum emitters can be larger than the bulk polarizability of the sphere, thereby enabling the use of repulsive optical potentials and consequently the levitation using optical near-fields. In levitated cavity quantum optomechanics, this could be used to boost the single-photon coupling by combining larger polarizability to mass ratio, larger fiel…
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.
Quantum state readout is a key component of quantum technologies, including applications in sensing, computation, and secure communication. Readout fidelity can be enhanced by repeating readouts. However, the number of repeated readouts is limited by measurement backaction, which changes the quantum state that is measured. This detrimental effect can be overcome by storing the quantum state in an ancilla qubit, chosen to be robust against measurement backaction and to allow error correction. Here, we protect the electronic-spin state of a diamond nitrogen-vacancy center from measurement backac…
We propose a method to generate and detect large quantum superposition states and arbitrary Fock states for the oscillational mode of an optically levitated nanocrystal diamond. The nonlinear interaction required for the generation of non-Gaussian quantum states is enabled through the spin-mechanical coupling with a built-in nitrogen-vacancy center inside the nanodiamond. The proposed method allows the generation of large superpositions of nanoparticles with millions of atoms and the observation of the associated spatial quantum interference under reasonable experimental conditions.
We present the development of an optically detected magnetic resonance (ODMR) system, which enables us to perform the ODMR measurements of a single defect in solids at high frequencies and high magnetic fields. Using the high-frequency and high-field ODMR system, we demonstrate 115 GHz continuous-wave and pulsed ODMR measurements of a single nitrogen-vacancy (NV) center in a diamond crystal at the magnetic field of 4.2 Tesla as well as investigation of field dependence ($0-8$ Tesla) of the longitudinal relaxation time ($T_1$) of NV centers in nanodiamonds.
Using the spin properties of nitrogen-vacancy (NV) centers in levitated diamond, we characterize the absorption of single nanodiamonds. We first calibrate the thermometry response of the NV centers embedded in our nanodiamonds. Then, using this calibration, we estimate the absorption cross-section of single levitated nanodiamonds. We show that this absorption is extrinsic and dominated by volumic effects. Our work opens the way to diamond materials optimization for levitation quantum experiments. It also demonstrates optical levitation as a unique platform to characterize material thermal prop…
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…
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.
This paper presents a method for determination of the size distribution for diamond nanocrystals containing luminescent nitrogen-vacancy (NV) centers using the luminescence intensity only. We also revise the basic photo physical properties of NV centers and conclude that the luminescence quantum yield of such centers is significantly smaller than the frequently stated 100\%. The yield can be as low as 5\% for centers embedded in nanocrystals and depends on their shape and the refractive index of the surrounding medium. The paper also addresses the value of the absorption cross-section of NV ce…
Near transform-limited single photon sources are required for perfect photon indistinguishability in quantum networks. Having such sources in nanodiamonds is particularly important since it can enable engineering hybrid quantum photonic systems. In this letter, we report the generation of optically stable, nearly transform-limited single silicon vacancy emitters in nanodiamonds. Lines as narrow as 325 MHz are reported, which is comparable to the lifetime limited linewidth. Moreover, the emitters exhibit minimal spectrum diffusion and absolute photostability, even if pumped well above saturatio…
In this study, we analyze the operational process of nanodiamond (ND) quantum thermometry based on wide-field detection of optically detected magnetic resonance (ODMR) of nitrogen vacancy centers, and compare its performance with that of confocal ODMR detection. We found that (1) the thermometry results are significantly affected by the shape and size of the camera region of interest (ROI) surrounding the target NDs and that (2) by properly managing the ROI and acquisition parameters of the camera, a temperature precision comparable to confocal detection in living cells can be obtained by wide…
Due to its superior coherent and optical properties at room temperature, the nitrogen-vacancy (N-V ) center in diamond has become a promising quantum probe for nanoscale quantum sensing. However, the application of N-V containing nanodiamonds to quantum sensing suffers from their relatively poor spin coherence times. Here we demonstrate energy efficient protection of N-V spin coherence in nanodiamonds using concatenated continuous dynamical decoupling, which exhibits excellent performance with less stringent microwave power requirement. When applied to nanodiamonds in living cells we are able …
We demonstrate an all-optical thermometer based on an ensemble of silicon-vacancy centers (SiVs) in diamond by utilizing a temperature dependent shift of the SiV optical zero-phonon line transition frequency, $Δλ/ΔT= 6.8\,\mathrm{GHz/K}$. Using SiVs in bulk diamond, we achieve $70\,\mathrm{mK}$ precision at room temperature with a sensitivity of $360\,\mathrm{mK/\sqrt{Hz}}$. Finally, we use SiVs in $200\,\mathrm{nm}$ nanodiamonds as local temperature probes with $521\,\mathrm{ mK/\sqrt{Hz}}$ sensitivity. These results open up new possibilities for nanoscale thermometry in biology, chemistry, a…
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…
Monolithic integration of quantum emitters in nanoscale plasmonic circuitry requires low-loss plasmonic configurations capable of confining light well below the diffraction limit. We demonstrate on-chip remote excitation of nanodiamond-embedded single quantum emitters by plasmonic modes of dielectric ridges atop colloidal silver crystals. The nanodiamonds are produced to incorporate single germanium-vacancy (GeV) centers, providing bright, spectrally narrow and stable single-photon sources suitable for highly integrated circuits. Using electron-beam lithography with hydrogen silsesquioxane (HS…
Materials and Spin Characteristics of Nanodiamonds Partially Covered with Amino Groups and Embedded with Nitrogen-Vacancy Color Centers
HUN-REN Wigner Research Centre for Physics（匈牙利科学院维格纳物理研究中心）；Budapest University of Technology and Economics（布达佩斯技术与经济大学）；Institute of Technical Physics and Materials Science, HUN-REN Centre for Energy Research（匈牙利科学院能源研究中心技术物理与材料科学研究所）
