Lifetime limited optical excitation lines of single nitrogen vacancy (NV) defect centers in diamond have been observed at liquid helium temperature. They display unprecedented spectral stability over many seconds and excitation cycles. Spectral tuning of the spin selective optical resonances was performed via the application of an external electric field (i.e. the Stark shift). A rich variety of Stark shifts were observed including linear as well as quadratic components. The ability to tune the excitation lines of single NV centers has potential applications in quantum information processing.
Quantum emitters in diamond are leading optically-accessible solid-state qubits. Among these, Group IV-vacancy defect centers have attracted great interest as coherent and stable optical interfaces to long-lived spin states. Theory indicates that their inversion symmetry provides first-order insensitivity to stray electric fields, a common limitation for optical coherence in any host material. Here we experimentally quantify this electric field dependence via an external electric field applied to individual tin-vacancy (SnV) centers in diamond. These measurements reveal that the permanent elec…
We review the electronic level structure of the nitrogen-vacancy in diamond and some common experimental techniques to study its optical properties at low temperatures. We then summarize several recent experiments and advances in using nitrogen-vacancy centers for quantum optics.
The optical coupling of guided modes in a GaP waveguide to nitrogen-vacancy (NV) centers in diamond is demonstrated. The electric field penetration into diamond and the loss of the guided mode are measured. The results indicate that the GaP-diamond system could be useful for realizing coupled microcavity-NV devices for quantum information processing in diamond.
Color centers in diamond are versatile solid state atomic-like systems suitable for quantum technological applications. In particular, the negatively charged silicon vacancy center (SiV) can exhibit a narrow photoluminescence (PL) line and lifetime-limited linewidth in bulk diamonds at cryogenic temperature. We present a low-temperature study of chemical vapour deposition (CVD)-grown diamond nano-pyramids containing SiV centers. The PL spectra feature a bulk-like zero-phonon line with ensembles of SiV centers, with a linewidth below 10 GHz which demonstrates very low crystal strain for such a …
We have observed photon antibunching in the fluorescence light emitted from a single N-V center in diamond at room temperature. The possibility of generating triggerable single photons with such a solide state system is discussed
Quantum memories for optical and microwave photons provide key functionalities in quantum processing and communications. Here we propose a protocol well adapted to solid state ensemble based memories coupled to cavities. It is called Stark Echo Modulation Memory (SEMM), and allows large storage bandwidths and low noise. This is achieved in a echo like sequence combined with phase shifts induced by small electric fields through the linear Stark effect. We investigated the protocol for rare earth nuclear spins and found a high suppression of unwanted collective emissions that is compatible with …
We report the narrow inhomogeneous distribution of the zero-phonon line from tin-vacancy (SnV) centers in diamond and the overlap of spectra from multiple separated SnV centers. Photoluminescence excitation spectroscopy measurements at a cryogenic temperature showed that SnV centers exhibit stable fluorescence and linewidths close to the Fourier transform-limited linewidth. The inhomogeneous distribution was as low as ~4 GHz, which enabled the observation of Sn isotope-dependent resonant frequencies. Owing to the narrow inhomogeneous distribution, we observed multiple SnV centers showing ident…
Diamond based quantum technology is a fast emerging field with both scientific and technological importance. With the growing knowledge and experience concerning diamond based quantum systems, comes an increased demand for performance. Quantum optimal control (QOC) provides a direct solution to a number of existing challenges as well as a basis for proposed future applications. Together with a swift review of QOC strategies, quantum sensing and other relevant quantum technology applications of nitrogen-vacancy (NV) centers in diamond, we give the necessary background to summarize recent advanc…
We present a scheme to generate entangled photons using the NV centers in diamond. We show how the long-lived nuclear spin in diamond can mediate entanglement between multiple photons thereby increasing the length of entangled photon string. With the proposed scheme one could generate both n-photon GHZ and cluster states. We present an experimental scheme realizing the same and estimating the rate of entanglement generation both in the presence and absence of a cavity.
We investigate correlations between fluorescence photons emitted by single N-V centers in diamond with respect to the optical excitation power. The autocorrelation function shows clear photon antibunching at short times, proving the uniqueness of the emitting center. We also report on a photon bunching effect, which involves a trapping level. An analysis using rate-equations for the populations of the N-V center levels shows the intensity dependence of the rate equation coefficients.
With the ability to transfer and process quantum information, large-scale quantum networks will enable a suite of fundamentally new applications, from quantum communications to distributed sensing, metrology, and computing. This perspective reviews requirements for quantum network nodes and color centers in diamond as suitable node candidates. We give a brief overview of state-of-the-art quantum network experiments employing color centers in diamond, and discuss future research directions, focusing in particular on the control and coherence of qubits that distribute and store entangled states,…
We propose an approach for an optical qubit rotation in the negatively charged nitrogen-vacancy (NV) center in diamond. The qubit is encoded in the ground degenerate states at the relatively low temperature limit. The basic idea of the rotation procedure is the non-Abelian geometric phase in an adiabatic passage, which is produced by the nonadiabatic transition between the two degenerate dark states. The feasibility is based on the success of modeling the NV center as an excited-doublet four-level atom.
Magnetometry with nitrogen-vacancy color centers in diamond has gained significant interest among researchers in recent years. Absolute knowledge of the three-dimensional orientation of the magnetic field is necessary for many applications. Conventional magnetometry measurements are usually performed with NV ensembles in a bulk diamond with a thin NV layer or a scanning probe in the form of a diamond tip, which requires a smooth sample surface and proximity of the probing device, often limiting the sensing capabilities. Here, we present a method for determining the three-dimensional orientatio…
The limitation of simultaneous measurements of noncommuting observables can be eliminated when the measured particle is maximally entangled with a quantum memory. We present a proposal for testing this quantum-memory-assisted entropic uncertainty relation in a single nitrogen-vacancy (N-V) center in diamond only by local electronic measurements. As an application, this entropic uncertainty relation is used to witness entanglement between the electron and nuclear spins of the N-V center, which is close to the reach of currently available technology.
An ensemble of nitrogen-vacancy (NV) centers in diamond is a fascinating candidate to realize a sensitive magnetic field sensor. In particular, since the axes of the NV centers are distributed along four directions, a collection of measurement data from NV centers with different axes provides information on the vector components of a magnetic field. However, in the conventional approach, the low measurement contrast of NV centers limits the sensitivity of vector magnetic field sensing. Recently, to overcome this problem, multi-frequency control of the NV centers has been proposed. The key idea…
We report a new method to determine the orientation of individual nitrogen-vacancy (NV) centers in a bulk diamond and use them to realize a calibration-free vector magnetometer with nanoscale resolution. Optical vortex beam is used for optical excitation and scanning the NV center in a [111]-oriented diamond. The scanning fluorescence patterns of NV center with different orientations are completely different. Thus, the orientation information on each NV center in the lattice can be known directly without any calibration process. Further, we use three differently oriented NV centers to form a m…
Precise control over the position of a single quantum object is important for many experiments in quantum science and nanotechnology. We report on a technique for high-accuracy positioning of individual diamond nanocrystals. The positioning is done with a home-built nanomanipulator under real-time scanning electron imaging, yielding an accuracy of a few nanometers. This technique is applied to pick up, move and position a single NV defect center contained in a diamond nanocrystal. We verify that the unique optical and spin properties of the NV center are conserved by the positioning process.
An ensemble of nitrogen-vacancy (NV) centers in diamond is an attractive device to detect small magnetic fields. In particular, by exploiting the fact that the NV center can be aligned along one of four different axes due to symmetry, it is possible to extract information concerning vector magnetic fields. However, in the conventional scheme, low readout contrasts of the NV centers significantly decrease the sensitivity of the vector magnetic field sensing. Here, we propose a way to improve the sensitivity of the vector magnetic field sensing of the NV centers using multi-frequency control. Si…
We propose an efficient scheme for a coherent quantum interface between microwave and optical photons using nitrogen-vacancy (NV) centers in diamond. In this setup, an NV center ensemble is simultaneously coupled to an optical and a microwave cavity. We show that, by using the collective spin excitation modes as an intermediary, quantum states can be transferred between the microwave cavity and the optical cavity through either a double-swap scheme or a dark-state protocol. This hybrid quantum interface may provide interesting applications in single microwave photon detections or quantum infor…
Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi…
We study spectroscopy of negatively charged nitrogen-vacancy center in diamond at high temperatures under high vacuum conditions. Spin resonances are studied using optical detection of magnetic resonance (ODMR), and optical spectroscopy is employed to study radiative transitions. Upon increasing the temperature the intensity of radiative decay in visible and infra-red decreased. In addition, the ODMR resonance frequencies were decreased, and the phonon line emission shifted to higher wavelengths. Fitting the measured intensity of photo-luminescence with the theoretical predictions of the Mott-…
Observation of Shear Strain in Ion-Implanted Diamond Substrate and Diamond Nanophotonic Structures
Indian Institute of Technology Bombay（印度理工学院孟买分校）；Center for Research in Nano Technology and Science, Indian Institute of Technology Bombay（印度理工学院纳米科技与科学研究中心）；Solid State Physics Laboratory（固体物理实验室）；School of Physical Sciences, UM-DAE Centre for Excellence in Basic Sciences, University of Mumbai（孟买大学基础科学卓越中心物理学院）
The development of materials processing techniques for optical diamond nanostructures containing a single color center is an important problem in quantum science and technology. In this work, we present the combination of ion implantation and top-down diamond nanofabrication in two scenarios: diamond nanopillars and diamond nanowires. The first device consists of a 'shallow' implant (~20nm) to generate Nitrogen-vacancy (NV) color centers near the top surface of the diamond crystal. Individual NV centers are then isolated mechanically by dry etching a regular array of nanopillars in the diamond…
Optical coupling of nitrogen vacancy centers in single-crystal diamond to an on-chip microcavity is demonstrated. The microcavity is fabricated from a hybrid gallium phosphide and diamond material system, and supports whispering gallery mode resonances with spectrometer resolution limited Q > 25000.
Two dimensional electronic spectroscopy and transient grating measurements were performed, for the first time, on nitrogen-vacancy centers in diamond. These measurements reveal energy transfer and vibrational pathways with consequences for spin coherence.
We report coherent interactions within an ensemble of silicon-vacancy color centers in diamond. The interactions are ascribed to resonant dipole-dipole coupling. Further, we demonstrate control over resonant center pairs by using a driving optical pulse to induce collective, interaction-enabled Rabi-oscillations in the ensemble. Non-resonant center pairs do not undergo collective oscillations.
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…
Integrating atomic quantum memories based on color centers in diamond with on-chip photonic devices would enable entanglement distribution over long distances. However, efforts towards integration have been challenging because color centers can be highly sensitive to their environment, and their properties degrade in nanofabricated structures. Here, we describe a heterogeneously integrated, on-chip, III-V diamond platform designed for neutral silicon vacancy (SiV0) centers in diamond that circumvents the need for etching the diamond substrate. Through evanescent coupling to SiV0 centers near t…
We propose the integrable N-dimensional Calogero-Coulomb-Stark and two-center Calogero-Coulomb systems and construct their constants of motion via the Dunkl operators. Their Schrödinger equations decouple in parabolic and elliptic coordinates into the set of three differential equations like for the Coulomb-Stark and two-center Coulomb problems. The Calogero term preserves the energy levels, but changes their degrees of degeneracy.
We demonstrate coupling of the zero-phonon line of individual nitrogen-vacancy centers and the modes of microring resonators fabricated in single-crystal diamond. A zero-phonon line enhancement exceeding ten-fold is estimated from lifetime measurements at cryogenic temperatures. The devices are fabricated using standard semiconductor techniques and off-the-shelf materials, thus enabling integrated diamond photonics.
Nitrogen-vacancy (NV) centers in diamond can be used for nanoscale sensing with atomic resolution and sensitivity; however, it has been observed that their properties degrade as they approach the diamond surface. Here we report that in addition to degraded spin coherence, NV centers within nanometers of the surface can also exhibit decreased fluorescence contrast for optically detected electron spin resonance (OD-ESR). We demonstrate that this decreased OD-ESR contrast arises from charge state dynamics of the NV center, and that it is strongly surface-dependent, indicating that surface enginee…
We present measurements of the Electronic Spin Resonance (ESR) of Nitrogen Vacancy (NV) centers in diamonds that are levitating in a ring Paul trap under vacuum. We observe ESR spectra of NV centers embedded in micron-sized diamonds at vacuum pressures down to $2\times 10^{-1}$ mbar, limited by the green laser heating of the diamond. We also observe the NV photoluminescence at vacuum pressures down to $10^{-2}$ mbar and discuss the steps required to control the NV spin under ultra-high vacuum.
The negatively-charged nitrogen-vacancy (NV) center in diamond is at the frontier of quantum nano-metrology and bio-sensing. Recent attention has focused on the application of high-sensitivity thermometry using the spin resonances of NV centers in nano-diamond to sub-cellular biological and biomedical research. Here, we report a comprehensive investigation of the thermal properties of the center's spin resonances and demonstrate an alternate all-optical NV thermometry technique that exploits the temperature dependence of the center's optical Debye-Waller factor.
We propose a novel source of non-classical light consisting of plasmonic aperture with single-crystal diamond containing a single Nitrogen-Vacancy (NV) color center. Theoretical calculations of optimal structures show that these devices can simultaneously enhance optical pumping by a factor of 7, spontaneous emission rates by Fp ~ 50 (Purcell factor), and offer collection efficiencies up to 40%. These excitation and collection enhancements occur over a broad range of wavelengths (~30nm), and are independently tunable with device geometry, across the excitation (~530nm) and emission (~600-800nm…
The spin dynamics of the diamond NV$^{-}$ center turns out to be similar to that of the chemical compass responsible for avian magnetoreception. We present a simulation framework based on quantum master equation for the former that is based upon the Radical Pair model of the latter. We show that this framework captures all the experimentally studied behavior of the NV$^{-}$ center spin system and can therefore be a predictive modeling tool.
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 …
Resonantly enhanced emission from the zero phonon line of a diamond nitrogen-vacancy (NV) center in single crystal diamond is demonstrated experimentally using a hybrid whispering gallery mode nanocavity. A 900 nm diameter ring nanocavity formed from gallium phosphide, whose sidewalls extend into a diamond substrate, is tuned onto resonance at low-temperature with the zero phonon line of a negatively charged NV center implanted near the diamond surface. When the nanocavity is on resonance, the zero phonon line intensity is enhanced by approximately an order of magnitude, and the spontaneous em…
We report on the observation of quantum interference of the emission from two separate nitrogen vacancy (NV) centers in diamond. Taking advantage of optically induced spin polarization in combination with polarization filtering, we isolate a single transition within the zero-phonon line of the non-resonantly excited NV centers. The time-resolved two-photon interference contrast of this filtered emission reaches 66%. Furthermore, we observe quantum interference from dissimilar NV centers tuned into resonance through the dc Stark effect. These results pave the way towards measurement-based entan…
Applications of negatively charged nitrogen-vacancy center in diamond exploit the center's unique optical and spin properties, which at ambient temperature, are predominately governed by electron-phonon interactions. Here, we investigate these interactions at ambient and elevated temperatures by observing the motional narrowing of the center's excited state spin resonances. We determine that the center's Jahn-Teller dynamics are much slower than currently believed and identify the vital role of symmetric phonon modes. Our results have pronounced implications for center's diverse applications (…
The ST1 center is a point defect in diamond with bright fluorescence and a mechanism for optical spin initialization and readout. The center has impressive potential for applications in diamond quantum computing as a quantum bus to a register of nuclear spins. This is because it has an exceptionally high readout contrast and, unlike the well-known nitrogen-vacancy center, it does not have a ground state electronic spin that decoheres the nuclear spins. However, its chemical structure is unknown and there are large gaps in our understanding of its properties. We present the discovery of ST1 cen…
The diamond nitrogen-vacancy (NV) center is a leading platform for quantum information science due to its optical addressability and room-temperature spin coherence. However, measurements of the NV center's spin state typically require averaging over many cycles to overcome noise. Here, we review several approaches to improve the readout performance and highlight future avenues of research that could enable single-shot electron-spin readout at room temperature.
Color centers in diamond represent a promising platform for developing solid-state single-photon sources and spin-photon interfaces as building blocks for photonics-based quantum technologies. However, although they exhibit a combination of features that make them so attractive, they also suffer from limited control in their emission properties, such as brightness, directionality, and polarization to cite a few. In this paper we present implementations and the experimental investigation of planar Yagi-Uda antennas in diamond, demonstrating highly efficient light extraction and directional emis…
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 …
Fluoride crystals doped with rare-earth ions (REI) and pair centers in diamond for fast ($10^{-9}\rm{s}$) quantum computers (FQC) are proposed. As specific systems for REI doping, we propose $Ca_{1-x}Sr_{x}F_{2}$ crystals and their analogues. The $^{4}f$-states with different total orbital angular moments of these ions serve as two-level systems (qubits). Suitable REIs are proposed as well. It is established that the pair $SiV$ and $GeV$ centers in diamond are promising systems for fast optical quantum computers operating at elevated temperatures.
The practical implementation of many quantum technologies relies on the development of robust and bright single photon sources that operate at room temperature. The negatively charged silicon-vacancy (SiV-) color center in diamond is a possible candidate for such a single photon source. However, due to the high refraction index mismatch to air, color centers in diamond typically exhibit low photon out-coupling. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion effic…
Diamond nitrogen-vacancy (NV) center magnetometry has recently received considerable interest from researchers in the fields of applied physics and sensors. The purpose of this review is to analyze the principle, sensitivity, technical development potential, and application prospect of the diamond NV center magnetometry. This review briefly introduces the physical characteristics of NV centers, summarizes basic principles of the NV center magnetometer, analyzes the theoretical sensitivity, and discusses the impact of technical noise on the NV center magnetometer. Furthermore, the most critical…
We report on wide-field optically detected magnetic resonance imaging of nitrogen-vacancy centers (NVs) in type IIa polycrystalline diamond. These studies reveal a heterogeneous crystalline environment that produces a varied density of NV centers, including preferential orientation within some individual crystal grains, but preserves long spin coherence times. Using the native NVs as nanoscale sensors, we introduce a 3-dimensional strain imaging technique with high sensitivity ( $< 10^{-5}$ Hz$^{-1/2}$) and diffraction-limited resolution across a wide field of view.
Using pulsed photoionization the coherent spin manipulation and echo formation of ensembles of NV- centers in diamond are detected electrically realizing contrasts of up to 17 %. The underlying spin-dependent ionization dynamics are investigated experimentally and compared to Monte-Carlo simulations. This allows the identification of the conditions optimizing contrast and sensitivity which compare favorably with respect to optical detection.
Group-IV color centers in diamond have garnered great interest for their potential as optically active solid-state spin qubits. Future utilization of such emitters requires the development of precise site-controlled emitter generation techniques that are compatible with high-quality nanophotonic devices. This task is more challenging for color centers with large group-IV impurity atoms, which are otherwise promising because of their predicted long spin coherence times without a dilution refrigerator. For example, when applied to the negatively charged tin-vacancy (SnV$^-$) center, conventional…
Phosphorus-doped diamond is relevant for applications in sensing, optoelectronics and quantum photonics, since the unique optical properties of color centers in diamond can be combined with the n-type conductivity attained by the inclusion of phosphorus. Here, we investigate the photoluminescence signal of the nitrogen-vacancy and silicon-vacancy color centers in phosphorus-doped diamond as a function of temperature starting from ambient conditions up to about 100$^\circ$ Celsius, focusing on the zero-phonon line (ZPL). We find that the wavelength and width of the ZPL of the two color centers …
Data-Driven Review and Machine Learning Prediction of Diamond Vacancy Center Synthesis
University of Aveiro（阿威罗大学）；Intelligent Systems Associate Laboratory (LASI)（智能系统联合实验室）；Instituto de Engenharia de Sistemas e Computadores - Microssistemas e Nanotecnologia（系统工程与计算机研究所-微系统与纳米技术）；IPFN, Instituto Superior Técnico, University of Lisbon（里斯本大学高等理工学院物理核研究组）；DECN, Instituto Superior Técnico, University of Lisbon（里斯本大学高等理工学院化学工程与工艺系）；Trent University（特伦特大学）
We theoretically investigate spin decoherence of a single nitrogen-vacancy (NV) center in diamond. Using the spin coherent state P-representation method, coherence evolution of the NV center surrounded by nitrogen electron spins (N) is simulated. We find that spin decoherence time as well as free-induction decay of the NV center depend on the spatial configuration of N spins. Both the spin decoherence rate (1/T2) and dephasing rate (1/T2*) of the NV center increase linearly with the concentration of the N spins. Using the P-representation method, we also demonstrate extracting noise spectrum o…
