The coherent behavior of the single electron and single nuclear spins of a defect center in diamond and a 13C nucleus in its vicinity, respectively, are investigated. The energy levels associated with the hyperfine coupling of the electron spin of the defect center to the 13C nuclear spin are analyzed. Methods of magnetic resonance together with optical readout of single defect centers have been applied in order to observe the coherent dynamics of the electron and nuclear spins. Long coherence times, in the order of microseconds for electron spins and tens of microseconds for nuclear spins, recommend the studied system as a good experimental approach for implementing a 2-qubit gate.
We demonstrate that the spin decoherence of nitrogen vacancy (NV) centers in diamond can be suppressed by a transverse magnetic field if the electron spin bath is the primary decoherence source. The NV spin coherence, created in "a decoherence-free subspace" is protected by the transverse component of the zero-field splitting, increasing the spin-coherence time about twofold. The decoherence due to the electron spin bath is also suppressed at magnetic fields stronger than ~25 gauss when applied parallel to the NV symmetry axis. Our method can be used to extend the spin-coherence time of simila…
Nitrogen-vacancy (NV) centers in diamond have become an important tool for quantum technologies. All of these applications rely on long coherence times of electron and nuclear spins associated with these centers. Here, we study the energy level anti-crossings of an NV center in diamond coupled to a first-shell 13C nuclear spin in a small static magnetic field. These level anti-crossings occur for specific orientations of the static magnetic field due to the strong non-secular components of the Hamiltonian. At these orientations we observe decoherence-free subspaces, where the electron spin coh…
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…
A First-principles Computational Framework for Quantum Decoherence in Complex Diamond Spin Environments
Sungkyunkwan University（成均馆大学）；Ajou University（亚洲大学）；University of Chicago（芝加哥大学）；Korea Institute of Science and Technology（韩国科学技术院）；Korean Research Institute of Standards and Science（韩国计量科学研究院）；Ulm University（乌尔姆大学）；Korea University of Science and Technology（韩国科学技术院）；Argonne National Laboratory（阿贡国家实验室）
We model the decoherence and dephasing of nitrogen vacancy (NV) centers in diamond due to a noisy paramagnetic bath, with and without the presence of a rf field that couples levels of the ground electronic state manifold, using a simple quantum mechanical model that allows for analytical solutions. The model treats the NV three-level ground state system in the presence of fluctuating magnetic fields that arise from the environment, and that result in decoherence, dephasing and dissipation. We show that all 9 eigenmodes of the three-level system are coupled to each other due to interaction with…
We report on room-temperature coherent manipulation of the spin of a single nitrogen-vacancy center in diamond and a study of its coherence as a function of magnetic field. We use magnetic resonance to induce Rabi nutations, and apply a Hahn spin echo to remove the effect of low-frequency dephasing. A sharp rise in the decoherence rate is observed at magnetic fields where the nitrogen-vacancy center spin couples resonantly to substitutional nitrogen spins via the magnetic dipolar coupling. Finally, we find evidence that away from these energy resonances spin flips of nitrogen electrons are the…
Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single Nitrogen-Vacancy color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3E excited state, which is invaluable for the development of diamond-based quantum information processing.
Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR)…
In this report, the polarization properties of the photoluminescence emitted by single nitrogen-vacancy (NV) color centers in diamond are investigated using resonant excitation at cryogenic temperature. We first underline that the two excited-state orbital branches are associated with two orthogonal transition dipoles. Using selective excitation of one dipole, we then show that the photoluminescence is partially unpolarized owing to fast relaxation between the two orbitals induced by the thermal bath. This result might be important in the context of the realization of indistinguishable single …
The efficiency of collecting photons from optically active defect centres in bulk diamond is greatly reduced by refraction and reflection at the diamond-air interface. We report on the fabrication and measurement of a geometrical solution to the problem; integrated solid immersion lenses (SILs) etched directly into the surface of diamond. An increase of a factor of 10 was observed in the saturated count-rate from a single negatively charged nitrogen-vacancy (NV-) within a 5um diameter SIL compared with NV-s under a planar surface in the same crystal. A factor of 3 reduction in background emiss…
We experimentally demonstrate that the decoherence of a spin by a spin bath can be completely eliminated by fully polarizing the spin bath. We use electron paramagnetic resonance at 240 gigahertz and 8 Tesla to study the spin coherence time $T_2$ of nitrogen-vacancy centers and nitrogen impurities in diamond from room temperature down to 1.3 K. A sharp increase of $T_2$ is observed below the Zeeman energy (11.5 K). The data are well described by a suppression of the flip-flop induced spin bath fluctuations due to thermal spin polarization. $T_2$ saturates at $\sim 250 μs$ below 2 K, where the …
Photon interference among distant quantum emitters is a promising method to generate large scale quantum networks. Interference is best achieved when photons show long coherence times. For the nitrogen-vacancy defect center in diamond we measure the coherence times of photons via optically induced Rabi oscillations. Experiments reveal a close to Fourier transform (i.e. lifetime) limited width of photons emitted even when averaged over minutes. The projected contrast of two-photon interference (0.8) is high enough to envisage the applications in quantum information processing. We report 12 and …
Solid-state quantum registers are exceptional for storing quantum information at room temperature with long coherence time. Nevertheless, practical applications toward quantum supremacy require even longer coherence time to allow for more complex algorithms. In this work we propose a quantum register that lies in a decoherence-free subspace to be implemented with color centers in diamond. The quantum information is encoded in two logical states composed of two nearby nuclear spins, while an electron spin is used as ancilla for initialization and control. Moreover, by tuning an off-axis magneti…
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.
We experimentally demonstrate an approach to scale up quantum devices by harnessing spin defects in the environment of a quantum probe. We follow this approach to identify, locate, and control two electron-nuclear spin defects in the environment of a single nitrogen-vacancy center in diamond. By performing spectroscopy at various orientations of the magnetic field, we extract the unknown parameters of the hyperfine and dipolar interaction tensors, which we use to locate the two spin defects and design control sequences to initialize, manipulate, and readout their quantum state. We finally crea…
We present a combined theoretical and experimental study of solid-state spin decoherence in an electronic spin bath, focusing specifically on ensembles of nitrogen vacancy (NV) color centers in diamond and the associated substitutional nitrogen spin bath. We perform measurements of NV spin free induction decay times $T_2^*$ and spin-echo coherence times $T_2$ in 25 diamond samples with nitrogen concentrations [N] ranging from 0.01 to 300\,ppm. We introduce a microscopic model and perform numerical simulations to quantitatively explain the degradation of both $T_2^*$ and $T_2$ over four orders …
The negatively charged nitrogen-vacancy (NV-) centre in diamond has many exciting applications in quantum nano-metrology, including magnetometry, electrometry, thermometry and piezometry. Indeed, it is possible for a single NV- centre to measure the complete three-dimensional vector of the local electric field or the position of a single fundamental charge in ambient conditions. However, in order to achieve such vector measurements, near complete knowledge of the orientation of the centre's defect structure is required. Here, we demonstrate an optically detected magnetic resonance (ODMR) techn…
Circuit-QED has demonstrated very strong coupling between individual microwave photons trapped in a superconducting coplanar resonator and nearby superconducting qubits. In this work we show how, by designing a novel interconnect, one can strongly connect the superconducting resonator, via a magnetic interaction, to a small number (perhaps single), of electronic spins. By choosing the electronic spin to be within a Nitrogen Vacancy centre in diamond one can perform optical readout, polarization and control of this electron spin using microwave and radio frequency irradiation. More importantly,…
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 describe a technique for fabricating micro- and nano-structures incorporating fluorescent defects in diamond with a positional accuracy in the hundreds of nanometers. Using confocal fluorescence microscopy and focused ion beam (FIB) etching we first locate a suitable defect with respect to registration marks on the diamond surface and then etch a structure using these coordinates. We demonstrate the technique here by etching an 8 micron diameter hemisphere positioned such that a single negatively charged nitrogen-vacancy defect lies at its origin. This type of structure increases the photon…
Saturable absorption in defect-rich diamond nanophotonics
Institute for Quantum Science and Technology, University of Calgary（卡尔加里大学量子科学与技术研究所）；Department of Physics, University of Alberta（阿尔伯塔大学物理系）；National Research Council of Canada, Quantum and Nanotechnology Research Centre（加拿大国家研究委员会量子与纳米技术研究中心）
We demonstrate the tunable enhancement of the zero phonon line of a single nitrogen-vacancy color center in diamond at cryogenic temperature. An open cavity fabricated using focused ion beam milling provides mode volumes as small as 1.24 $μ$m$^3$. In-situ tuning of the cavity resonance is achieved with piezoelectric actuators. At optimal coupling of the full open cavity the signal from individual zero phonon line transitions is enhanced by about a factor of 10 and the overall emission rate of the NV$^-$ center is increased by 40% compared with that measured from the same center in the absence …
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…
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.…
Silicon-vacancy and tin-vacancy defects in diamond are of interest as alternative qubits to the NV center due to their superior optical properties. While the availability of optical transitions in these defects is one of their assets, high-fidelity optical coherent control has not been demonstrated. Here, we design novel optical control schemes tailored to these defects. We evaluate the performance of arbitrary single-qubit rotations of the electron spin qubit both in the absence and presence of an external magnetic field, by taking into account both coherent and incoherent errors. We find tha…
Fabrication of single nickel-nitrogen (NE8) defect centers in diamond by chemical vapor deposition is demonstrated. Under continuous-wave 745 nm laser excitation single defects were induced to emit single photon pulses at 797 nm with a linewidth of 1.5 nm at room temperature. Photon antibunching of single centers was demonstrated using a Hanbury-Brown and Twiss interferometer. Confocal images revealed approximately 10^6 optically active sites/cm^2 in the synthesized films. The fabrication of an NE8 based single photon source in synthetic diamond is important for fiber based quantum cryptograph…
Understanding and mitigating decoherence is a key challenge for quantum science and technology. The main source of decoherence for solid-state spin systems is the uncontrolled spin bath environment. Here, we demonstrate quantum control of a mesoscopic spin bath in diamond at room temperature that is composed of electron spins of substitutional nitrogen impurities. The resulting spin bath dynamics are probed using a single nitrogen-vacancy (NV) centre electron spin as a magnetic field sensor. We exploit the spin bath control to dynamically suppress dephasing of the NV spin by the spin bath. Fur…
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 report a study of the 3E excited-state structure of single nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model of the excited-state structure is developed and shows excellent agreement with experimental observations. Besides, we show that the two orbital branches associated with the 3E excited-state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of d…
Optically active solid-state spin defects have the potential to become a versatile resource for quantum information processing applications. Nitrogen-vacancy defect centers (NV) in diamond act as quantum memories and can be interfaced by coherent photons as demonstrated in entanglement protocols. However, in particular in diamond nanostructures, the effect of spectral diffusion leads to optical decoherence hindering entanglement generation. In this work, we present strategies to significantly reduce the electric noise in diamond nanostructures. We demonstrate single NVs in nanopillars exhibiti…
Engineering single atomic defects into wide bandgap materials has become an attractive field in recent years due to emerging applications such as solid-state quantum bits and sensors. The simplest atomic-scale defect is the lattice vacancy which is often a constituent part of more complex defects such as the nitrogen-vacancy (NV) centre in diamond, therefore an understanding of the formation mechanisms and precision engineering of vacancies is desirable. We present a theoretical and experimental study into the ultra-fast laser generation of vacancy-interstitial pairs (Frenkel defects) in diamo…
The silicon-vacancy center in diamond offers attractive opportunities in quantum photonics due to its favorable optical properties and optically addressable electronic spin. Here, we combine both to achieve all-optical coherent control of its spin states. We utilize this method to explore spin dephasing effects in an impurity-rich sample beyond the limit of phonon-induced decoherence: Employing Ramsey and Hahn-echo techniques at 12mK base temperature we identify resonant coupling to a substitutional nitrogen spin bath as the limiting decoherence source for the electron spin.
The prototype of a quantum random number generator is a single photon which impinges onto a beam splitter and is then detected by single photon detectors at one of the two output paths. Prior to detection, the photon is in a quantum mechanical superposition state of the two possible outcomes with - ideally - equal amplitudes until its position is determined by measurement. When the two output modes are observed by a single photon detector, the generated clicks can be interpreted as ones and zeros - and a raw random bit stream is obtained. Here we implement such a random bit generator based on …
Dense ensembles of nitrogen vacancy (NV) centers in diamond are of interest for various applications including magnetometry, masers, hyperpolarization and quantum memory. All of the applications above may benefit from a non-linear response of the ensemble, and hence multiphoton processes are of importance. We study an enhancement of the NV ensemble multiphoton response due to coupling to a superconducting cavity or to an ensemble of Nitrogen 14 substitutional defects (P1). In the latter case, the increased NV sensitivity allowed us to probe the P1 hyperfine splitting. As an example of an appli…
Using a recently developed quantum embedding theory, we present first principles calculations of strongly correlated states of spin defects in diamond. Within this theory, effective Hamiltonians are constructed, which can be solved by classical and quantum computers; the latter promise a much more favorable scaling as a function of system size than the former. In particular, we report a study of the neutral group-IV vacancy complexes in diamond, and we discuss their strongly-correlated spin-singlet and spin-triplet excited states. Our results provide valuable predictions for experiments aimed …
A technique has been developed for depositing diamond crystals on the endfaces of optical fibers and capturing the fluorescence generated by optically active defects in the diamond into the fiber. This letter details the diamond growth on optical fibers and transmission of fluorescence through the fiber from the nitrogen-vacancy (N-V) color center in diamond. Control of the concentration of defects incorporated during the chemical vapor deposition (CVD) growth process is also demonstrated. These are the first critical steps in developing a fiber coupled single photon source based on optically …
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…
Defect cavities in 3D photonic crystal can trap and store light in the smallest volumes allowable in dielectric materials, enhancing non-linearities and cavity QED effects. Here, we study inverse rod-connected diamond (RCD) crystals containing point defect cavities using plane-wave expansion and finite-difference time domain methods. By optimizing the dimensions of the crystal, wide photonic band gaps are obtained. Mid-bandgap resonances can then be engineered by introducing point defects in the crystal. We investigate a variety of single spherical defects at different locations in the unit ce…
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-…
Optically-driven Rabi oscillations of single electron spins in a diamond nitrogen vacancy center are realized with two Raman-resonant optical pulses that are detuned from the respective dipole optical transitions. The Rabi oscillations are nuclear-spin selective and are robust against rapid decoherence of the underlying optical transitions, opening the door to generating phonon-mediated spin entanglement in an optically-driven spin-phonon system. A direct comparison between the Rabi oscillations and simulated Raman adiabatic passage along with a detailed theoretical analysis provide a wealth o…
Electrically-active defects have a significant impact on the performance of electronic devices based on wide band-gap materials such as diamond. This issue is ubiquitous in diamond science and technology, since the presence of charge traps in the active regions of different classes of diamond-based devices (detectors, power diodes, transistors) can significantly affect their performances, due to the formation of space charge, memory effects and the degradation of the electronic response associated with radiation damage. Among the most common defects in diamond, the nitrogen-vacancy (NV) center…
Operating reconfigurable quantum circuits with single photon sources is a key goal of photonic quantum information science and technology. We use an integrated waveguide device comprising of directional couplers and a reconfigurable thermal phase controller to manipulate single photons emitted from a chromium related colour centre in diamond. Observation of both a wave-like interference pattern and particle-like sub-Poissionian autocorrelation functions demonstrates coherent manipulation of single photons emitted from the chromium related centre and verifies wave particle duality.
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…
