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.
We employ the technique of optical detection of magnetic resonance to study dipolar interaction in diamond between nitrogen-vacancy color centers of different crystallographic orientations and substitutional nitrogen defects. We demonstrate optical measurements of resonant spin flips-flips (second Larmor line), and flip-flops between different spin ensembles in diamond. In addition, the strain coupling between the nitrogen-vacancy color centers and bulk acoustic modes is studied using optical detection. Our findings may help optimizing cross polarization protocols, which, in turn, may allow im…
Generation of local magnetic field at the nanoscale is desired for many applications such as spin-qubit-based quantum memories. However, this is a challenge due to the slow decay of static magnetic fields. Here, we demonstrate photonic spin density (PSD) induced effective static magnetic field for an ensemble of nitrogen-vacancy (NV) centers in bulk diamond. This locally induced magnetic field is a result of coherent interaction between the optical excitation and the NV centers. We demonstrate an optically induced spin rotation on the Bloch sphere exceeding 10 degrees which has potential appli…
Raman excited spin coherences were experimentally observed in N-V diamond color centers via nondegenerate four-wave mixing (NDFWM) and electromagnetically induced transparency (EIT). 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 the efficient preparation of quantum bits (qubits), as well as ability to perform arbitrary single qubit rotations.
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…
We investigate nuclear spin hyperpolarization from nitrogen vacancy centers in isotopically enriched diamonds with $^{13}$C concentrations up to 100%. $^{13}$C enrichment leads to hyperfine structure of the nitrogen vacancy electron spin resonance spectrum and as a result the spectrum of dynamic nuclear polarization. We show that strongly-coupled $^{13}$C spins in the first shell surrounding a nitrogen vacancy center generate resolved hyperfine splittings, but do not act as an intermediary in the transfer of hyperpolarization of bulk nuclear spins. High levels of $^{13}$C enrichment are desira…
We use single-spin resonant spectroscopy to study the spin structure in the orbital excited-state of a diamond nitrogen-vacancy center at room temperature. We find that the excited state spin levels have a zero-field splitting that is approximately half of the value of the ground state levels, a g-factor similar to the ground state value, and a hyperfine splitting ~20x larger than in the ground state. In addition, the width of the resonances reflects the electronic lifetime in the excited state. We also show that the spin-splitting can significantly differ between NV centers, likely due to the…
The novel aspect of the centre (NV-) in diamond is the high degree of spin polarisation achieved through optical illumination. In this paper it is shown that the spin polarisation occurs as a consequence of an electron-vibration interaction combined with spin-orbit interaction, and an electronic model involving these interactions is developed to account for the observed polarisation.
We present an experimental and theoretical study of the optically detected magnetic resonance signals for ensembles of negatively charged nitrogen-vacancy (NV) centers in 13C isotopically enriched single-crystal diamond. We observe four broad transition peaks with superimposed sharp features at zero magnetic field and study their dependence on applied magnetic field. A theoretical model that reproduces all qualitative features of these spectra is developed. Understanding the magnetic-resonance spectra of NV centers in isotopically enriched diamond is important for emerging applications in nucl…
Nitrogen-vacancy (NV) centers in diamond are considered sensors for detecting magnetic fields. Pulsed optically detected magnetic resonance (ODMR) is typically used to detect AC magnetic fields; however, this technique can only be implemented after careful calibration that involves aligning an external static magnetic field, measuring continuous-wave (CW) ODMR, determining the Rabi frequency, and setting the microwave phase. In contrast, CW-ODMR can be simply implemented by continuous application of green CW laser and a microwave filed. In this letter, we report a method that uses NV centers a…
The nitrogen-vacancy (N-V) center in diamond is a widely-used platform for quantum information processing and metrology. The electron-spin state of N-V center could be initialized and readout optically, and manipulated by resonate microwave fields. In this work, we analyze the dependence of electron-spin initialization on widths of laser pulses. We build a numerical model to simulate this process and verify the simulation results in experiment. Both simulations and experiments reveal a fact that shorter laser pulses are helpful to the electron-spin polarization. We therefore propose to use ext…
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…
The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the t…
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…
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.
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 report sensitive detection of the nuclear quadrupolar interaction of the 14N nuclear spin of the nitrogen-vacancy (NV) center using the electron spin echo envelope modulation technique. We applied a weak transverse magnetic field to the spin system so that certain forbidden transitions became weakly allowed due to second-order effects involving the nonsecular terms of the hyperfine interaction. The weak transitions cause modulation of the electron spin-echo signal, and a theoretical analysis suggests that the modulation frequency is primarily determined by the nuclear quadrupolar frequency;…
We study features in the optically detected magnetic resonance (ODMR) signals associated with negatively charged nitrogen-vacancy (NV) centers coupled to other paramagnetic impurities in diamond. Our results are important for understanding ODMR line shapes and for optimization of devices based on NV centers. We determine the origins of several side features to the unperturbed NV magnetic resonance by studying their magnetic field and microwave power dependences. Side resonances separated by around 130 MHz are due to hyperfine coupling between NV centers and nearest-neighbor C-13 nuclear spins.…
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…
The application of magnetic resonance (MR) spectroscopy at progressively smaller length scales may eventually permit "chemical imaging" of spins at the surfaces of materials and biological complexes. In particular, the negatively charged nitrogen-vacancy (NV-) centre in diamond has been exploited as an optical transducer for nanoscale nuclear magnetic resonance. However, the spectra of detected spins are generally broadened by their interaction with proximate paramagnetic NV- centres through coherent and incoherent mechanisms. Here we demonstrate a detection technique that can resolve the spec…
Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV0 centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign the…
The sensitivity of Magnetic Resonance Imaging (MRI) depends strongly on nuclear spin polarisation and, motivated by this observation, dynamical nuclear spin polarisation has recently been applied to enhance MRI protocols (Kurhanewicz, J., et al., Neoplasia 13, 81 (2011)). Nuclear spins associated with the 13 C carbon isotope (nuclear spin I = 1/2) in diamond possess uniquely long spin lattice relaxation times (Reynhardt, E.C. and G.L. High, Prog. in Nuc. Mag. Res. Sp. 38, 37 (2011)) If they are present in diamond nanocrystals, especially when strongly polarised, they form a promising contrast …
Diamond membrane devices containing optically coherent nitrogen-vacancy (NV) centers are key to enable novel cryogenic experiments such as optical ground-state cooling of hybrid spin-mechanical systems and efficient entanglement distribution in quantum networks. Here, we report on the fabrication of a (3.4 $\pm$ 0.2) μm thin, smooth (surface roughness r$_q$ < 0.4 nm over an area of 20 μm by 30 μm diamond membrane containing individually resolvable, narrow linewidth (< 100 MHz) NV centers. We fabricate this sample via a combination of high energy electron irradiation, high temperature annealing…
Pulsed laser excitation causes the luminescence of Nitrogen Vacancy centers in diamond to unexpectedly decrease with increasing pulse energy. This decrease is observed in both the negatively charged and neutral centers and is caused by shortening of the luminescence lifetimes of the centers of both types. In darkness, the luminescence does not show any recovery on a time scale of 10 microseconds but as little as three low-intensity pulses can return the luminescence to its previous, brighter state. An external magnetic field reduces the magnitude of the effect. A possible mechanism for these p…
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 …
Efficient and reversible optical to microwave coherent transducers are required to enable entanglement transfer between superconducting qubits and light for quantum networks. Rare-earth-doped crystals that possess narrow optical and spin transitions are a promising way to implement these devices. Current approaches use ground-state electron spin transitions that have coherence lifetimes ($T_2$) often limited by spin flip-flop processes and/or spectral diffusion, even at very low temperatures. Here, we investigate spin coherence in an optically excited state of an Er$^{3+}$:Y$_2$SiO$_5$ crystal…
We discuss the recent proposal by Thommen and Mandel (Phys. Rev. Lett. {\bf 96}, 053601 (2006)) for electromagnetically induced negative refraction. Although the main conclusion of the paper -- the possibility to achieve negative refraction in an experimentally accessible atomic scheme -- remains valid, we show that the weak-excitation approximation used is invalid in the parameter regime studied and leads to quantitatively incorrect predictions. We show that negative refraction is always accompanied by absorption rather than by gain, and that the maximum value of the refraction-absorption rat…
We report bulk, room-temperature hyperpolarization of 13C nuclear spins observed via high-field nuclear magnetic resonance (NMR). The hyperpolarization is achieved by optical pumping (OP) of nitrogen vacancy defect centers in diamond accompanied by dynamic nuclear polarization (DNP). The technique harnesses the large optically-induced spin polarization of NV- centers at room temperature, which is many orders of magnitude greater than thermal equilibrium polarization and typically achievable only at sub-Kelvin temperatures. Transfer of the spin polarization to the 13C nuclear spins is accomplis…
The optical transition linewidth and emission polarization of single nitrogen-vacancy (NV) centers are measured from 5 K to room temperature. Inter-excited state population relaxation is shown to broaden the zero-phonon line and both the relaxation and linewidth are found to follow a T^5 dependence for T up to 100 K. This dependence indicates that the dynamic Jahn-Teller effect is the dominant dephasing mechanism for the NV optical transitions at low temperatures.
Optically detected magnetic resonance (ODMR) is a way to characterize the NV centers. Recently, a remarkably sharp dip was observed in the ODMR with a high-density ensemble of NV centers, and this was reproduced by a theoretical model in [Zhu et al., Nature Communications 5, 3424 (2014)], showing that the dip is a consequence of the spin-1 properties of the NV centers. Here, we present much more details of analysis to show how this model can be applied to investigate the properties of the NV centers. By using our model, we have reproduced the ODMR with and without applied magnetic fields. Also…
In this paper cross-relaxation between nitrogen-vacancy (NV) centers and substitutional nitrogen in a diamond crystal was studied. It was demonstrated that optically detected magnetic resonance signals (ODMR) can be used to measure these signals successfully. The ODMR were detected at axial magnetic field values around 51.2~mT in a diamond sample with a relatively high (200~ppm) nitrogen concentration. We observed transitions that involve magnetic sublevels that are split by the hyperfine interaction. Microwaves in the frequency ranges from 1.3 GHz to 1.6 GHz ($m_S=0\longrightarrow m_S=-1$ NV …
We investigate the real-time estimation protocols for the frequency shift of optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in nanodiamonds (NDs). Efficiently integrating multipoint ODMR measurements and ND particle tracking into fluorescence microscopy has recently demonstrated stable monitoring of the temperature inside living animals. We analyze the multipoint ODMR measurement techniques (3-, 4-, and 6-point methods) in detail and quantify the amount of measurement artifact owing to several systematic errors derived from instrumental errors of experimental har…
We present a general theory for using an optically pumped diamond nitrogen-vacancy center as a tunable, non-equilibrium bath to control a variety of nuclear spin dynamics (such as dephasing, relaxation, squeezing, polarization, etc.) and the nuclear spin noise. It opens a new avenue towards engineering the dissipative and collective nuclear spin evolution and solves an open problem brought up by the $^{13}$C nuclear spin noise suppression experiment [E. Togan \textit{et al}., Nature 478, 497 (2011)].
Under ambient conditions, spin impurities in solid-state systems are found in thermally-mixed states and are optically "dark", i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright", i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a dressed-state, double-resonance scheme to transfer polarization from bright NV electronic spins to dark substitutional-Nitrogen (P1) elect…
We investigate optically detected magnetic resonance signals from an ensemble of nitrogen-vacancy centers in diamond. The signals are measured for different light powers and microwave powers, and the contrast and linewidth of the magnetic-resonance signals are extracted. For a wide range of experimental settings of the microwave and light powers, the linewidth decreases with increasing light power, and more than a factor of two "light narrowing" is observed.Furthermore, we identify that spin-spin interaction between nitrogen-vacancy centers and substitutional nitrogen atoms in the diamond lead…
The spin coherence time of $^{151}$Eu$^{3+}$ which substitutes the yttrium at site 1 in Y$_2$SiO$_5$ crystal has been extended to 6 hours in a recent work [\textit{Nature} \textbf{517}, 177 (2015)]. To make this long-lived spin coherence useful for optical quantum memory applications, we experimentally characterize the hyperfine interaction of the optically-excited state $^5$D$_0$ using Raman-heterodyne-detected nuclear magnetic resonance. The effective spin Hamiltonians for excited and ground state are fitted based on the experimental spectra obtained in 200 magnetic fields with various orien…
Spins in solids are an ideal candidate to act as a memory and interface with superconducting qubits due to their long coherence times. We spectroscopically investigate erbium-167-doped yttrium orthosilicate as a possible microwave-addressed memory employing its microwave frequency transitions that occur without applying an external magnetic field. We obtain coherence times of 380 $μ$s in a ground state spin transition and 1.48 ms in an excited state spin transition. This is 28 times longer compared to previous zero field measurements, as well as 200 times longer than a previous microwave memor…
Single color centers in solid have emerged as promising physical platforms for quantum information science. Creating these centers with excellent quantum properties is a key foundation for further technological developments. In particular, the microscopic understanding of the spin bath environments is the key to engineer color centers for quantum control. In this work, we propose and demonstrate a distinct high-temperature annealing (HTA) approach for creating high-quality nitrogen vacancy (NV) centers in implantation-free diamonds. Simultaneously using the created NV centers as probes for the…
We propose that an optically excited heavy hole in a quantum dot can drive the surrounding nuclear spins into a quiescent collective state, leading to significantly prolonged coherence time for the electron spin qubit. This provides a general paradigm to combat decoherence by environmental control without involving the active qubit in quantum information processing. It also serves as a unified solution to some open problems brought about by two recent experiments [X. Xu et al., Nature 459, 1105 (2009) and C. Latta et al., Nature Phys. 5, 758 (2009)].
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…
Optically-Induced Modulation and Programming of Diamond Photonic Cavities
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL)（洛桑联邦理工学院物理研究所）；Center of Quantum Science and Engineering, Swiss Federal Institute of Technology Lausanne (EPFL)（洛桑联邦理工学院量子科学与工程中心）；Photonics Research Group, Department of Information Technology (INTEC), Ghent University - IMEC（根特大学信息技朮系光子研究组（与IMEC联合））；University of Stuttgart（斯图加特大学）
Ensembles of erbium dopants can realize quantum memories and frequency converters that operate in the minimal-loss wavelength band of fiber optical communication. Their operation requires the initialization, coherent control and readout of the electronic spin state. In this work, we use a split-ring microwave resonator to demonstrate such control in both the ground and optically excited state. The presented techniques can also be applied to other combinations of dopant and host, and may facilitate the development of new quantum memory protocols and sensing schemes.
The nitrogen-vacancy (NV) center in diamond is supposed to be a building block for quantum computing and nanometer scale metrology at ambient conditions. Therefore, precise knowledge of its quantum states is crucial. Here, we experimentally show that under usual operating conditions the NV exists in an equilibrium of two charge states (70% in the expected negative (NV-) and 30% in the neutral one (NV0)). Projective quantum non-demolition measurement of the nitrogen nuclear spin enables the detection even of the additional, optically inactive state. The nuclear spin can be coherently driven als…
Fluorescent defects in non-cytotoxic diamond nanoparticles are candidates for qubits in quantum computing, optical labels in biomedical imaging and sensors in magnetometry. For each application these defects need to be optically and thermodynamically stable, and included in individual particles at suitable concentrations (singly or in large numbers). In this letter, we combine simulations, theory and experiment to provide the first comprehensive and generic prediction of the size, temperature and nitrogen-concentration dependent stability of optically active NV defects in nanodiamonds.
We investigate spin-dependent decay and intersystem crossing in the optical cycle of single negatively-charged nitrogen-vacancy (NV) centres in diamond. We use spin control and pulsed optical excitation to extract both the spin-resolved lifetimes of the excited states and the degree of optically-induced spin polarization. By optically exciting the centre with a series of picosecond pulses, we determine the spin-flip probabilities per optical cycle, as well as the spin-dependent probability for intersystem crossing. This information, together with the indepedently measured decay rate of singlet…
