NV centers in diamond: Quantum-chemical modeling

Quantum-chemical modeling is used to study the relationship between the spin states of nitrogen vacancy (NV) centers and their position on a (100) surface or in the bulk of a diamond crystal. The spin density of the NV centers is computed, and the position of the centers on the crystal surface is demonstrated to be energetically more favorable. The (100) surface of diamond crystal is found to affect the geometrical parameters and adsorption properties of NV centers and their spin-density distribution, relative to these properties in the bulk.     

基于金刚石氮-空位色心的精密磁测量

磁是一种重要的物理现象,对其进行精密测量推动了许多科技领域的发展.各类测磁技术,包括霍尔传感器、超导量子干涉仪、自旋磁共振等,都致力于提升空间分辨率和灵敏度.近年来,金刚石中的氮-空位色心广受关注.这一固态单自旋体系具有许多优点,例如易于初始化和读出、可操控、具有较长相干时间等,这使得它不仅在量子信息、量子计算等领域崭露头角,而且在量子精密测量上显现出巨大的应用前景.基于氮-空位色心,利用动力学解耦、关联谱等技术,已实现若干高灵敏度、高分辨率的微观磁共振实验,其中包括纳米尺度乃至单分子、单自旋的核磁共振和电子顺磁共振.氮-空位色心也可以用于微波和射频信号的精密测量.本文对围绕上述主题开展的一系列研究工作进行综述.     

Raman-excited spin coherences in nitrogen-vacancy color centers in diamond

Raman-excited spin coherences were experimentally observed in nitrogen-vacancy (N-V) diamond color centers by means of nondegenerate four-wave mixing and electromagnetically induced transparency. The maximal absorption suppression was found to be 17%, which corresponds to 70% of what is possible given the random geometric orientation of the N-V center in diamond. In the context of quantum computing in solids, this level of transparency represents efficient preparation of quantum bits, as well as the ability to perform arbitrary single-quantum-bit rotations.     

Coupling nitrogen-vacancy centers in diamond to superconducting flux qubits

We propose a method to achieve coherent coupling between nitrogen-vacancy (NV) centers in diamond and superconducting (SC) flux qubits. The resulting coupling can be used to create a coherent interaction between the spin states of distant NV centers mediated by the flux qubit. Furthermore, the magnetic coupling can be used to achieve a coherent transfer of quantum information between the flux qubit and an ensemble of NV centers. This enables a long-term memory for a SC quantum processor and possibly an interface between SC qubits and light.     

Stark shift control of single optical centers in diamond

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.     

Laser-polarization-dependent and magnetically controlled optical bistability in diamond nitrogen-vacancy centers

We explore laser-polarization-dependent and magnetically controlled optical bistability (OB) in an optical ring cavity filled with diamond nitrogen-vacancy (NV) defect centers under optical excitation. The shape of the OB curve can be significantly modified in a new operating regime from the previously studied OB case, namely, by adjusting the intensity of the external magnetic field and the polarization of the control beam. The influences of the intensity of the control beam, the frequency detuning, and the cooperation parameter on the OB behavior are also discussed in detail. These results are useful in real experiments for realizing an all-optical bistate switching or coding element in a solid-state platform.     

Two-photon quantum interference from separate nitrogen vacancy centers in diamond

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 nonresonantly 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 entanglement between remote NV centers and the realization of quantum networks with solid-state spins.     

Photon antibunching in the fluorescence of individual color centers in diamond

We observed photon antibunching in the fluorescent light emitted from a single nitrogen-vacancy center in diamond at room temperature. The possibility of generating triggerable single photons with such a solid-state system is discussed.     

Micron-sized diamond particles containing Ge-V and Si-V color centers

Micron-sized diamond particles containing germanium-vacancy(Ge-V) color centers with a zero-photon line(ZPL)around 602.3 nm are successfully grown using hot filament chemical vapor deposition.The crystal morphology changes from icosahedron to truncated octahedron and decahedron, finally becomes spherical with the growth pressure increase.Due to the chamber containing Si, all diamond particles contain silicon-vacancy(Si-V) color centers.High growth pressure contributes to the formation of Ge-V and Si-V in diamonds.With prolonging growth time, the change in the full width at half maximum(FWHM) of the diamond peak is small, which shows that the concentration of Ge-V and Si-V centers nearly maintains a constant.The FWHM of the Ge-V ZPL is around 4 nm, which is smaller than that reported, suggesting that the Ge-V center has a more perfect structure.Ge-V and Si-V photoluminescence(PL) intensities increase with the prolonging growth time due to the increased diamond content and reduced content of sp~2-bonded carbon and trans-polyacetylene.In summary, increasing the growth pressure and prolonging the growth time are beneficial to enhance the Ge-V and Si-V PL intensities.     

Creation of entangled state between two spaced NV centers in diamond

A method for creating an entangled state between two NV centers in a diamond that do not interact directly with each other is studied. The method is based on the excitation of centers via a half divider (a 50% beamsplitter) with the subsequent coherent inversion of the spin of the excited center and the detection of a photon emitted by the excited center. The parameters of a multimode single-photon pulse that make it possible to achieve a maximally possible excitation of the centers at a given solid angle of the focusing of the light on the center are found. The probability to create an entangled state in relation to the parameters of the initial state of a photon, the turn-on and turn-off times of the microwave pulse and the light focusing solid angle is determined. Optimal values of these parameters that ensure a maximal probability of the entanglement creation are determined.     

Statistical analysis of micro-luminescence maps of implanted optical centers in diamond

We report on an approach to determine the number of optical emitters based on establishing the proper relationship between the statistics of implanted ions and the signal from optical centers (e.g. photoluminescence) collected at different points in the sample. Knowing the number of implanted ions, one can estimate the probability for an ion to create an optical center—the conversion efficiency. The micro-luminescence mapping and statistical analyses were performed on a model Xe optical center in diamond and the conversion efficiency was estimated to be about 30%.     

Coupling of nitrogen-vacancy centers to photonic crystal cavities in monocrystalline diamond

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 spectroscopy.     

Quantum interference of single photons from remote nitrogen-vacancy centers in diamond

We demonstrate quantum interference between indistinguishable photons emitted by two nitrogen-vacancy centers in distinct diamond samples separated by two meters. Macroscopic solid immersion lenses are used to enhance photon collection efficiency. Quantum interference is verified by measuring a value of the second-order cross-correlation function g((2))(0)=0.35±0.04<0.5. In addition, optical transition frequencies of two separated nitrogen-vacancy centers are tuned into resonance with each other by applying external electric fields. An extension of the present approach to generate entanglement of remote solid-state qubits is discussed.     

Interpretation of perturbed angular distribution results for19F implanted into diamond

Perturbed Angular Distribution measurements have been made on natural diamond using recoil implanted fluorine ions as probes. Two distinct lattice sites for fluorine in diamond were found. Site identifications prompted by theoretical cluster calculations are presented. The PAD data are well described by a texture theory, though the origin of the texture effects is presently not known.     

Photo-induced creation of nitrogen-related color centers in diamond nanocrystals under femtosecond illumination

Diamond nanocrystals deposited on a dielectric mirror at the focus of a microscope objective have been illuminated by femtosecond laser pulses. We have observed the photo-creation of color centers, under peak power corresponding to an intensity of about . In a nanocrystal initially containing a single Nitrogen Vacancy (NV) center, femtosecond illumination resulted in the transformation of this center into another one with different spectral features. These features are tentatively attributed to the neutral form NV⁰. This irreversible transformation goes together with the photocreation of other unstable color centers at the laser focus. Such behavior under femtosecond laser illumination place some limitations on the use of sub-picosecond pulses to trigger single photon emission from a single NV center in diamond nanocrystal.     

Quantum repeater based on NV + 13C color centers in diamond

We suggest a specific way to realize the quantum repeater protocol based on NV + ¹³C defects in diamond and feasible with present techniques. Numerical simulation shows the efficiency of the considered realization in respect of both fidelity of final entangled state and time of its creation, under the condition of using small Rabi frequencies and resonant-only operational pulses. The text was submitted by the authors in English.     

Photoluminescence of SiV centers in CVD diamond particles with specific crystallographic planes

We prepared the isolated micrometer-sized diamond particles without seeding on the substrate in hot filament chemical vapor deposition. The diamond particles with specific crystallographic planes and strong silicon-vacancy(SiV) photoluminescence(PL) have been prepared by adjusting the growth pressure. As the growth pressure increases from 2.5 to 3.5 kPa,the diamond particles transit from composite planes of {100} and {111} to only smooth {111} planes. The {111}-faceted diamond particles present better crystal quality and stronger normalized intensity of SiV PL with a narrower bandwidth of 5 nm. Raman depth profiles show that the SiV centers are more likely to be formed on the near-surface areas of the diamond particles, which have poorer crystal quality and greater lattice stress than the inner areas. Complex lattice stress environment in the near-surface areas broadens the bandwidth of SiV PL peak. These results provide a feasible method to prepare diamond particles with specific crystallographic planes and stronger SiV PL.     

Dependence of nitrogen vacancy color centers on nitrogen concentration in synthetic diamond

Crystallization of diamond with different nitrogen concentrations was carried out with a FeNiCo-C system at pressure of 6.5 GPa. As the nitrogen concentration in diamond increased, the color of the synthesized diamond crystals changed from colorless to yellow and finally to atrovirens (a dark green). All the Raman peaks for the obtained crystals were located at about 1330 cm^-1 and contained only the sp³ hybrid diamond phase. Based on Fourier transform infrared results, the nitrogen concentration of the colorless diamond was < 1 ppm and absorption peaks corresponding to nitrogen impurities were not detected. However, the C-center nitrogen concentration of the atrovirens diamond reached 1030 ppm and the value of A-center nitrogen was approximately 180 ppm with a characteristic absorption peak at 1282 cm^-1. Furthermore, neither the NV⁰ nor the NV^- optical color center existed in diamond crystal with nitrogen impurities of less than 1 ppm by photoluminescence measurement. However, Ni-related centers located at 695 nm and 793.6 nm were observed in colorless diamond. The NE8 color center at 793.6 nm has more potential for application than the common NV centers. NV⁰ and NV^- optical color centers coexist in diamond without any additives in the synthesis system. Importantly, only the NV^- color center was noticed in diamond with a higher nitrogen concentration, which maximized optimization of the NV^-/NV⁰ ratio in the diamond structure. This study has provided a new way to prepare diamond containing only NV^- optical color centers.