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 effects of local strain, which provides a pathway to control over the spin Hamiltonian and may be useful for quantum information processing.
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.
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 study the resonant optical transitions of a single nitrogen-vacancy (NV) center that is coherently dressed by a strong mechanical drive. Using a gigahertz-frequency diamond mechanical resonator that is strain-coupled to an NV center's orbital states, we demonstrate coherent Raman sidebands out to the ninth order and orbital-phonon interactions that mix the two excited-state orbital branches. These interactions are spectroscopically revealed through a multi-phonon Rabi splitting of the orbital branches which scales as a function of resonator driving amplitude, and is successfully reproduced …
The ability to manipulate nano-particles at the nano-scale is critical for the development of active quantum systems. This paper presents a new technique to manipulate diamond nano-crystals at the nano-scale using a scanning electron microscope, nano-manipulator and custom tapered optical fibre probes. The manipulation of a ~ 300 nm diamond crystal, containing a single nitrogen-vacancy centre, onto the endface of an optical fibre is demonstrated. The emission properties of the single photon source post manipulation are in excellent agreement with those observed on the original substrate.
Fast quantum spin manipulation is needed to design spin-based quantum logic gates and other quantum applications. Here, we construct exact evolution operator of the nitrogen-vacancy-center (NV) spin in diamond under external magnetic fields and investigate the nonadiabatic geometric phases, both cyclic and non-cyclic, in these fast-manipulated NV spin systems. It is believed that the nonadiabatic geometric phases can be measured in future experiments and these fast quantum manipulations can be useful in designing spin-based quantum applications.
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…
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.
Precise coherent control of the individual electronic spins associated with atom-like impurities in the solid state is essential for applications in quantum information processing and quantum metrology. We demonstrate all-optical initialization, fast coherent manipulation, and readout of the electronic spin of the negatively charged nitrogen-vacancy (NV$^-$) center in diamond at T$\sim$7K. We then present the observation of a novel double-dark resonance in the spectroscopy of an individual NV center. These techniques open the door for new applications ranging from robust manipulation of spin s…
As a potential candidate for quantum computation and metrology, the nitrogen vacancy (NV)center in diamond presented both challenges and opportunities resulted from charge state conversion. By utilizing different lasers for the photon-induced charge state conversion, we achieved the sub-diffraction charge state manipulation. The charge state depletion (CSD) microscopy resolution was improved to 4.1 nm by optimizing the laser pulse sequences. Subsequently, the electron spin state dynamics of adjacent NV centers were selectively detected via the CSD. The experimental results demonstrated that th…
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.
The nitrogen-vacancy (NV) center spin represents an appealing candidate for quantum information processing. Besides the widely used microwave control, its coherent manipulation may also be achieved using laser as mediated by the excited energy levels. Nevertheless, the multiple levels of the excited state of NV center spin make the coherent transition process become complex and may affect the fidelity of coherent manipulation. Here, we adopt the strategy of optimal quantum control to accelerate coherent state transfer in the ground state manifold of NV center spin using laser. The results demo…
Isolated nuclear spins offer a promising building block for quantum information processing systems, but their weak interactions often impede preparation, control, and detection. Hyperfine coupling to a proximal electronic spin can enhance each of these processes. Using the electronic spin of the nitrogen-vacancy center as an intermediary, we demonstrate robust initialization, single-qubit manipulation, and direct optical readout of 13C, 15N, and 14N nuclear spins in diamond. These results pave the way for nitrogen nuclear spin based quantum information architectures in diamond.
We investigate bright fluorescence of nitrogen (NV)- and silicon-vacancy color centers in pyramidal, single crystal diamond tips which are commercially available as atomic force microscope probes. We coherently manipulate NV electronic spin ensembles with $T_2 = 7.7(3)\,μ$s. Color center lifetimes in different tip heights indicate effective refractive index effects and quenching. Using numerical simulations, we verify enhanced photon rates from emitters close to the pyramid apex; a situation promising for scanning probe sensing.
We investigate the possibilities to realize light extraction from single crystal diamond (SCD) nanopillars. This was achieved by dedicated 519 nm laser-induced spin-state initiation of negatively charged nitrogen vacancies (NV-). For the first time, we present possibility to perform effective spin-readout of NV(-)s that were naturally generated by the growth process during chemical vapor deposition (CVD) synthesis within SCD without any post-growth implantation strategies. Applied diamond was neither implanted with 14N+, nor was the CVD synthesized SCD annealed, making the presence of nitrogen…
We demonstrate a magnetometry technique using nitrogen-vacancy centres in diamond which makes use of coherent two-photon transitions. We find that the sensitivity to magnetic fields can be significantly improved in isotopically purified diamond. Furthermore, the long-term stability of magnetic field measurements is significantly enhanced, thereby reducing the minimum detectable long-term field variations for both quasi-static and periodic fields. The method is useful both for sensing applications and as a spin qubit manipulation technique.
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.
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 …
We investigate phonon induced electronic dynamics in the ground and excited states of the negatively charged silicon-vacancy ($\mathrm{SiV}^-$) centre in diamond. Optical transition line widths, transition wavelength and excited state lifetimes are measured for the temperature range 4-350 K. The ground state orbital relaxation rates are measured using time-resolved fluorescence techniques. A microscopic model of the thermal broadening in the excited and ground states of the $\mathrm{SiV}^-$ centre is developed. A vibronic process involving single-phonon transitions is found to determine orbita…
A collapse and revival shape of Rabi oscillations of a single Nitrogen-Vacancy (NV) center electron spin has been observed in diamond at room temperature. Because of hyperfine interaction between the host 14N nuclear spin and NV center electron spin, different orientation of the 14N nuclear spin leads to a triplet splitting of the transition between the ground ms=0 and excited states ms=1. Microwave can excite the three transitions equally to induce three independent nutations and the shape of Rabi oscillations is a combination of the three nutations. This result provides an innovative view of…
A detailed study of the photophysical properties of several novel color centers in chemical vapor deposition diamond is presented. These emitters show narrow luminescence lines in the near infra-red. Single photon emission was verified with continuous and pulsed excitation with emission rates at saturation in the MHz regime, whilst direct lifetime measurements reveal excited state lifetimes ranging from 1-14 ns. In addition, a number of quantum emitters demonstrate two level behavior with no bunching present in the second order correlation function. An improved method of evaluating the quantum…
We describe an all-optical scheme for spin manipulation in the ground-state triplet of the negatively charged nitrogen-vacancy (NV) center in diamond. Virtual optical excitation from the 3A_2 ground state into the 3E excited state allows for spin rotations by virtue of the spin-spin interaction in the two-fold orbitally degenerate excited state. We derive an effective Hamiltonian for optically induced spin-flip transitions within the ground state spin triplet due to off-resonant optical pumping. Furthermore, we investigate the spin qubit formed by the Zeeman sub-levels with spin projection m_S…
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 …
We report a versatile method to efficiently polarize single nuclear spins in diamond, which is based on optical pumping of a single NV color center and mediated by a level-anti crossing in its excited state. A nuclear spin polarization higher than 98% is achieved at room temperature for the 15N nuclear spin associated to the NV center, corresponding to $μ$K effective nuclear spin temperature. We then show simultaneous deterministic initialization of two nuclear spins (13C and 15N) in close vicinity to a NV defect. Such robust control of nuclear spin states is a key ingredient for further scali…
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…
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…
Generating robust entanglement among solid-state spins is key for applications in quantum information processing and precision sensing. We show here a dissipative approach to generate such entanglement among the hyperfine coupled electron nuclear spins using the rapid optical decay of electronic excited states. The combined dark state interference effects of the optical and microwave driving fields in the presence of spontaneous emission from the short-lived excited state leads to a dissipative formation of an entangled steady state. We show that the dissipative entanglement is generated for a…
We report polarization of a dense nuclear-spin ensemble in diamond and its dependence on magnetic field and temperature. The polarization method is based on the transfer of electron spin polarization of negatively charged nitrogen vacancy color centers to the nuclear spins via the excited-state level anti-crossing of the center. We polarize 90% of the 14N nuclear spins within the NV centers, and 70% of the proximal 13C nuclear spins with hyperfine interaction strength of 13-14 MHz. Magnetic-field dependence of the polarization reveals sharp decrease in polarization at specific field values cor…
We studied the dynamic nuclear spin polarization of nitrogen in negatively charged nitrogen-vacancy (NV) centers in diamond both experimentally and theoretically over a wide range of magnetic fields from 0 to 1100 G covering both the excited-state level anti-crossing and the ground-state level anti-crossing magnetic field regions. Special attention was paid to the less studied ground-state level anti-crossing region. The nuclear spin polarization was inferred from measurements of the optically detected magnetic resonance signal. These measurements show that a very large (up to $96 \pm 2\%$) nu…
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.
Color centers in diamond are a promising platform for quantum technologies, and understanding their interactions with the environment is crucial for these applications. We report a study of spin- lattice relaxation (T1) of the neutral charge state of the silicon vacancy center in diamond. Above 20 K, T1 decreases rapidly with a temperature dependence characteristic of an Orbach process, and is strongly anisotropic with respect to magnetic field orientation. As the angle of the magnetic field is rotated relative to the symmetry axis of the defect, T1 is reduced by over three orders of magnitude…
Quantum computing is an attractive and multidisciplinary field, which became a focus for experimental and theoretical research during last decade. Among other systems, like ions in traps or superconducting circuits, solid-states based qubits are considered to be promising candidates for first experimental tests of quantum hardware. Here we report recent progress in quantum information processing with point defect in diamond. Qubits are defined as single spin states (electron or nuclear). This allows exploring long coherence time (up to seconds for nuclear spins at cryogenic temperatures). In a…
Quantum emitters are an integral component for a broad range of quantum technologies including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single photon generation and photon mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vac…
We present direct imaging of the emission pattern of individual chromium-based single photon emitters in diamond and measure their quantum efficiency. By imaging the excited state transition dipole intensity distribution in the back focal plane of high numerical aperture objective, we determined that the emission dipole is oriented nearly orthogonal to the diamond-air interface. Employing ion implantation techniques, the emitters were engineered with various proximities from the diamond-air interface. By comparing the decay rates from the single chromium emitters at different depths in the dia…
In diamond, the mechanical vibration induced strain can lead to interaction between the mechanical mode and the nitrogen-vecancy (NV) centers. In this work, we propose to utilize the strain induced coupling for the quantum non-demolition (QND) single phonon measurement and memory in diamond. The single phonon in a diamond mechanical resonator can be perfectly absorbed and emitted by the NV centers ensemble (NVE) with adiabatically tuning the microwave driving. An optical laser drives the NVE to the excited states, which have much larger coupling strength to the mechanical mode. By adiabaticall…
The nitrogen-vacancy defect center (NV center) is a promising candidate for quantum information processing due to the possibility of coherent manipulation of individual spins in the absence of the cryogenic requirement. We report a room-temperature implementation of the Deutsch-Jozsa algorithm by encoding both a qubit and an auxiliary state in the electron spin of a single NV center. By thus exploiting the specific S=1 character of the spin system, we demonstrate how even scarce quantum resources can be used for test-bed experiments on the way towards a large-scale quantum computing architectu…
Colour centres in diamond have emerged as versatile tools for solid-state quantum technologies ranging from quantum information to metrology, where the nitrogen-vacancy centre is the most studied to-date. Recently, this toolbox has expanded to include different materials for their nanofabrication opportunities, and novel colour centres to realize more efficient spin-photon quantum interfaces. Of these, the silicon-vacancy centre stands out with ultrabright single photon emission predominantly into the desirable zero-phonon line. The challenge for utilizing this centre is to realise the hithert…
We investigate the magnetic field dependent photo-physics of individual Nitrogen-Vacancy (NV) color centers in diamond under cryogenic conditions. At distinct magnetic fields, we observe significant reductions in the NV photoluminescence rate, which indicate a marked decrease in the optical readout efficiency of the NV's ground state spin. We assign these dips to excited state level anti-crossings, which occur at magnetic fields that strongly depend on the effective, local strain environment of the NV center. Our results offer new insights into the structure of the NVs' excited states and a ne…
We propose fast phase-gates of single nuclear spins interacting with single electron spins. The gate operation utilizes geometric phase shifts of the electron spin induced by fast/slow rotating fields; the path difference depending on nuclear spin states enables nuclear phase shifts. The gate time is inversely proportional to the frequency of the slow rotating field. As an example, we use nitrogen-vacancy centers in diamond, and show the phase-gate time orders of magnitude shorter than previously reported. We also show the robustness of the gate against decoherence and systematic errors.
Precise characterization of a hyperfine interaction is a prerequisite for high fidelity manipulations of electron and nuclear spins belonging to a hybrid qubit register in diamond. Here, we demonstrate a novel scheme for determining a hyperfine interaction, using single-quantum and zero-quantum Ramsey fringes, by applying it to the system of a Nitrogen Vacancy (NV) center and a $^{13}$C nuclear spin in the 1$^{\mathrm{st}}$ shell. The zero-quantum Ramsey fringe, analogous to the quantum beat in a $Λ$-type level structure, particularly enhances the measurement precision for non-secular hyperfin…
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 (…
Strong light-matter interactions are critical for quantum technologies based on light, such as memories or nonlinear interactions. Solid state materials will be particularly important for such applications, because of the relative ease of fabrication of components. Silicon vacancy centers (SiV) in diamond feature especially narrow inhomogeneous spectral lines, which are rare in solid materials. Here, we demonstrate resonant coherent manipulation, stimulated Raman adiabatic passage, and strong light-matter interaction via four-wave mixing of a weak signal field in an ensemble of SiV centers.
Nitrogen vacancy (NV) centers in diamond are promising elemental blocks for quantum optics [1, 2], spin-based quantum information processing [3, 4], and high-resolution sensing [5-13]. Yet, fully exploiting these capabilities of single NV centers requires strategies to accurately manipulate them. Here, we use optical tweezers as a tool to achieve deterministic trapping and 3D spatial manipulation of individual nano-diamonds hosting a single NV spin. Remarkably, we find the NV axis is nearly fixed inside the trap and can be controlled in-situ, by adjusting the polarization of the trapping light…
Precise knowledge of a quantum system's Hamiltonian is a critical pre-requisite for its use in many quantum information technologies. Here, we report a method for the precise characterization of the non-secular part of the excited-state Hamiltonian of an electronic-nuclear spin system in diamond. The method relies on the investigation of the dynamic nuclear polarization mediated by the electronic spin, which is currently exploited as a primary tool for initializing nuclear qubits and performing enhanced nuclear magnetic resonance. By measuring the temporal evolution of the population of the gr…
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 …
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…
The emerging field of quantum acoustics explores interactions between acoustic waves and artificial atoms and their applications in quantum information processing. In this experimental study, we demonstrate the coupling between a surface acoustic wave (SAW) and an electron spin in diamond by taking advantage of the strong strain coupling of the excited states of a nitrogen vacancy center, while avoiding the short lifetime of these states. The SAW-spin coupling takes place through a lamda-type three-level system where two ground spin states couple to a common excited state through a phonon-assi…
