Quantum interference of resonance fluorescence from Germanium-vacancy color centers in diamond
Disheng Chen, Johannes Froech, Shihao Ru, Hongbing Cai, Naizhou Wang, Giorgio Adamo, John Scott, Fuli Li, Nikolay Zheludev, Igor Aharonovich, Wei-bo Gao
Resonance fluorescence from a quantum emitter is an ideal source to extract indistinguishable photons. By using the cross polarization to suppress the laser scattering, we observed resonance fluorescence from GeV color centers in diamond at cryogenic temperature. The Fourier-transform-limited linewidth emission with $T_2/2T_1\sim0.86$ allows for two-photon interference based on single GeV color center. Under pulsed excitation, the 24 ns separated photons exhibit a Hong-Ou-Mandel visibility of $0.604\pm0.022$, while the continuous-wave excitation leads to a coalescence time window of 1.05 radiative lifetime. Together with single-shot readout of spin states, it paves the way towards building a quantum network with GeV color centers in diamond.
Scalable quantum photonic networks require coherent excitation of quantum emitters. However, many solid-state systems can undergo a transition to a dark shelving state that inhibits the fluorescence. Here we demonstrate that a controlled gating using a weak non-resonant laser, the resonant excitation can be recovered and amplified for single germanium vacancies (GeVs). Employing the gated resonance excitation, we achieve optically stable resonance fluorescence of GeV centers. Our results are pivotal for the deployment of diamond color centers as reliable building blocks for scalable solid stat…
We demonstrate a quantum nanophotonics platform based on germanium-vacancy (GeV) color centers in fiber-coupled diamond nanophotonic waveguides. We show that GeV optical transitions have a high quantum efficiency and are nearly lifetime-broadened in such nanophotonic structures. These properties yield an efficient interface between waveguide photons and a single GeV without the use of a cavity or slow-light waveguide. As a result, a single GeV center reduces waveguide transmission by $18 \pm 1\%$ on resonance in a single pass. We use a nanophotonic interferometer to perform homodyne detection …
The nitrogen-vacancy center in diamond has been explored extensively as a light-matter interface for quantum information applications, however it is limited by low coherent photon emission and spectral instability. Here, we present a promising interface based on an alternate defect with superior optical properties (the germanium-vacancy) coupled to a finesse $\approx11{,}000$ fiber cavity, resulting in a $31^{+11}_{-15}$-fold increase in the spectral density of emission. This work sets the stage for cryogenic experiments, where we predict a measurable increase in the spontaneous emission rate.
Single crystal diamond membranes that host optically active emitters are highly attractive components for integrated quantum nanophotonics. In this work we demonstrate bottom-up synthesis of single crystal diamond membranes containing the germanium vacancy (GeV) color centers. We employ a lift-off technique to generate the membranes and perform chemical vapour deposition in a presence of germanium oxide to realize the insitu doping. Finally, we show that these membranes are suitable for engineering of photonic resonators such as microring cavities with quality factors of 1500. The robust and s…
Nitrogen-Vacancy (NV) centers in diamond have been used in recent years for a wide range of applications, from nano-scale NMR to quantum computation. These applications depend strongly on the efficient readout of the NV center's spin state, which is currently limited. Here we suggest a method of reading the NV center's spin state, using the weak optical transition in the singlet manifold. We numerically calculate the number of photons collected from each spin state using this technique, and show that an order of magnitude enhancement in spin readout signal-to-noise ratio is expected, making si…
Room-temperature fluorescence detection of the nitrogen-vacancy center electronic spin typically has low signal to noise, requiring long experiments to reveal an averaged signal. Here, we present a simple approach to analysis of time-resolved fluorescence data that permits an improvement in measurement precision through signal processing alone. Applying our technique to experimental data reveals an improvement in signal to noise equivalent to a 14% increase in photon collection efficiency. We further explore the dependence of the signal to noise ratio on excitation power, and analyze our resul…
A solid-state system combining a stable spin degree of freedom with an efficient optical interface is highly desirable as an element for integrated quantum optical and quantum information systems. We demonstrate a bright color center in diamond with excellent optical properties and controllable electronic spin states. Specifically, we carry out detailed optical spectroscopy of a Germanium Vacancy (GeV) color center demonstrating optical spectral stability. Using an external magnetic field to lift the electronic spin degeneracy, we explore the spin degree of freedom as a controllable qubit. Spi…
Solid-state quantum emitters, such as artificially engineered quantum dots or naturally occurring defects in solids, are being investigated for applications ranging from quantum information science and optoelectronics to biomedical imaging. Recently, these same systems have also been studied from the perspective of nanoscale metrology. In this letter we study the near-field optical properties of a diamond nanocrystal hosting a single nitrogen vacancy center. We find that the nitrogen vacancy center is a sensitive probe of the surrounding electromagnetic mode structure. We exploit this sensitiv…
We introduce an advanced material system for the production and spectroscopy of single silicon vacancy (SiV) color centers in diamond. We use microwave plasma chemical vapor deposition to synthesize heteroepitaxial nanodiamonds of approx. 160 nm in lateral size with a thickness of approx. 75 nm. These oriented 'nanoislands' combine the enhanced fluorescence extraction from subwavelength sized nanodiamonds with defined crystal orientation. The investigated SiV centers display narrow zero-phonon-lines down to 0.7 nm in the wavelength range 730-750 nm. We investigate in detail the phonon-coupling…
The nitrogen-vacancy colour centre in diamond is emerging as one of the most important solid-state quantum systems. It has applications to fields including high-precision sensing, quantum computing, single photon communication, metrology, nanoscale magnetic imaging and biosensing. For all of these applications, a high quantum yield of emitted photons is desirable. However, diamond samples engineered to have high densities of nitrogen-vacancy centres show levels of brightness varying significantly within single batches, or even within the same sample. Here we show that nearby nitrogen impuritie…
Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration six-fold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature and the coherence time T2 can be reached to around 17.1 μs. Furthermore, investigation of fluor…
Optical microcavities are a powerful tool to enhance spontaneous emission of individual quantum emitters. However, the broad emission spectra encountered in the solid state at room temperature limit the influence of a cavity, and call for ultra-small mode volume. We demonstrate Purcell-enhanced single photon emission from nitrogen-vacancy (NV) centers in nanodiamonds coupled to a tunable fiber-based microcavity with a mode volume down to $1.0\,λ^{3}$. We record cavity-enhanced fluorescence images and study several single emitters with one cavity. The Purcell effect is evidenced by enhanced flu…
Tin-vacancy (SnV) color centers were created in diamond by ion implantation and subsequent high temperature annealing up to 2100 °C at 7.7 GPa. The first-principles calculation suggests that the large atom of tin can be incorporated into the diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The SnV center shows a sharp zero phonon line at 619 nm at room temperature. This line splits into four peaks at cryogenic temperatures with a larger ground state splitting of ~850 GHz than those of color centers based on oth…
We demonstrate real-time magnetometry by detecting fluorescence from a nitrogen vacancy center in the setting of coherent population trapping and by estimating magnetic field from the time series of the observed photon counts, which are correlated with the underlying field. The proof-of-principle experiment uses an external time-varying magnetic field that follows an Ornstein-Uhlenbeck (OU) process. By taking into consideration the statistical properties of the OU process, a Bayesian inference-based estimator can effectively update dynamical information of the field in real time with the detec…
We introduce a microwave-assisted spectroscopy technique to determine the relative concentrations of nitrogen vacancy (NV) centers in diamond that are negatively-charged (NV${}^-$) and neutrally-charged (NV${}^0$), and present its application to studying spin-dependent ionization in NV ensembles and enhancing NV-magnetometer sensitivity. Our technique is based on selectively modulating the NV${}^-$ fluorescence with a spin-state-resonant microwave drive to isolate, in-situ, the spectral shape of the NV${}^-$ and NV${}^0$ contributions to an NV-ensemble sample's fluorescence. As well as serving…
Nitrogen-vacancy (NV) centers in diamonds are interesting due to their remarkable characteristics that are well suited to applications in quantum-information processing and magnetic field sensing, as well as representing stable fluorescent sources. Multiple NV centers in nanodiamonds (NDs) are especially useful as biological fluorophores due to their chemical neutrality, brightness and room-temperature photostability. Furthermore, NDs containing multiple NV centers also have potential in high-precision magnetic field and temperature sensing. Coupling NV centers to propagating surface plasmon p…
We show a marked reduction in the emission from nitrogen-vacancy (NV) color centers in single crystal diamond due to exposure of the diamond to hydrogen plasmas ranging from 700°C to 1000°C. Significant fluorescence reduction was observed beneath the exposed surface to at least 80mm depth after ~10 minutes, and did not recover after post-annealing in vacuum for seven hours at 1100°C. We attribute the fluorescence reduction to the formation of NVH centers by the plasma induced diffusion of hydrogen. These results have important implications for the formation of nitrogen-vacancy centers for quan…
We demonstrate cooling of ultrathin fiber tapers coupled with nitrogen vacancy (NV) centers in nanodiamonds to cryogenic temperatures. Nanodiamonds containing multiple NV centers are deposited on the subwavelength 480-nm-diameter nanofiber region of fiber tapers. The fiber tapers are successfully cooled to 9 K using our home-built mounting holder and an optimized cooling speed. The fluorescence from the nanodiamond NV centers is efficiently channeled into a single guided mode and shows characteristic sharp zero-phonon lines of both neutral and negatively charged NV centers. The present nanofib…
Hyperfine spectroscopy and fast, all-optical arbitrary state initialization and readout of a single, ten-level ${}^{73}$Ge vacancy nuclear spin qudit in diamond
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…
In this Letter, we proposed and experimentally demonstrated a method to detect vector magnetic field with a single nitrogen vacancy (NV) center in diamond. The magnetic field in parallel with the axis of the NV center can be obtained by detecting the electron Zeeman shift, while the Larmor precession of an ancillary nuclear spin close to the NV center can be used to measure the field perpendicular to the axis. Experimentally, both the Zeeman shift and Larmor precession can be measured through the fluorescence from the NV center. By applying additional calibrated magnetic fields, complete infor…
We demonstrate fluorescence thermometry techniques with sensitivities approaching 10 mK Hz^(-1/2) based on the spin-dependent photoluminescence of nitrogen vacancy (NV) centers in diamond. These techniques use dynamical decoupling protocols to convert thermally induced shifts in the NV center's spin resonance frequencies into large changes in its fluorescence. By mitigating interactions with nearby nuclear spins and facilitating selective thermal measurements, these protocols enhance the spin coherence times accessible for thermometry by 45x, corresponding to a 7x improvement in the NV center'…
We report on the use of a single NV center to probe fluctuating AC magnetic fields. Using engineered currents to induce random changes in the field amplitude and phase, we show that stochastic fluctuations reduce the NV center sensitivity and, in general, make the NV response field-dependent. We also introduce two modalities to determine the field spectral composition, unknown a priori in a practical application. One strategy capitalizes on the generation of AC-field-induced coherence 'revivals', while the other approach uses the time-tagged fluorescence intensity record from successive NV obs…
Surface plasmon polaritons (SPPs) are locally excited at silver surfaces using (~100) nm-sized nanodiamonds (NDs) with multiple nitrogen-vacancy (NV) centers (~400). The fluorescence from an externally illuminated (at 532 nm) ND and from nearby NDs, which are not illuminated but produce out-of-plane scattering of SPPs excited by the illuminated ND, exhibit distinctly different wavelength spectra, showing short-wavelength filtering due to the SPP propagation loss. The results indicate that NDs with multiple NV centers can be used as efficient sub-wavelength SPP sources in planar integrated plas…
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 study the spin and orbital dynamics of single nitrogen-vacancy (NV) centers in diamond between room temperature and 700 K. We find that the ability to optically address and coherently control single spins above room temperature is limited by nonradiative processes that quench the NV center's fluorescence-based spin readout between 550 and 700 K. Combined with electronic structure calculations, our measurements indicate that the energy difference between the 3E and 1A1 electronic states is approximately 0.8 eV. We also demonstrate that the inhomogeneous spin lifetime (T2*) is temperature ind…
Monolithic integration of quantum emitters in nanoscale plasmonic circuitry requires low-loss plasmonic configurations capable of confining light well below the diffraction limit. We demonstrate on-chip remote excitation of nanodiamond-embedded single quantum emitters by plasmonic modes of dielectric ridges atop colloidal silver crystals. The nanodiamonds are produced to incorporate single germanium-vacancy (GeV) centers, providing bright, spectrally narrow and stable single-photon sources suitable for highly integrated circuits. Using electron-beam lithography with hydrogen silsesquioxane (HS…
We present a method relying on shortcuts to adiabaticity to achieve quantum detection of high frequency signals at the nanoscale in a robust manner. More specifically, our protocol delivers tailored amplitudes and frequencies for control fields that, firstly, enable the coupling of the sensor with high-frequency signals and, secondly, minimise errors that would otherwise spoil the detection process. To exemplify the method, we particularise to detection of signals emitted by fast-rotating nuclear spins with nitrogen vacancy center quantum sensors. However, our protocol is straightforwardly app…
Individual, luminescent point defects in solids so called color centers are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: First, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of single-crystal diamond. Second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging bas…
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.
Ultrafast emission rates obtained from quantum emitters coupled to plasmonic nanoantennas have recently opened fundamentally new possibilities in quantum information and sensing applications. Plasmonic nanoantennas greatly improve the brightness of quantum emitters by dramatically shortening their fluorescence lifetimes. Gap plasmonic nanocavities that support strongly confined modes are of particular interest for such applications. We demonstrate single-photon emission from nitrogen-vacancy (NV) centers in nanodiamonds coupled to nanosized gap plasmonic cavities with internal mode volumes abo…
We study the effect of strain on the physical properties of the nitrogen antisite-vacancy pair in hexagonal boron nitride ($h$-BN), a color center that may be employed as a quantum bit in a two-dimensional material. With group theory and ab-initio analysis we show that strong electron-phonon coupling plays a key role in the optical activation of this color center. We find a giant shift on the zero-phonon-line (ZPL) emission of the nitrogen antisite-vacancy pair defect upon applying strain that is typical of $h$-BN samples. Our results provide a plausible explanation for the experimental observ…
We report the narrow inhomogeneous distribution of the zero-phonon line from tin-vacancy (SnV) centers in diamond and the overlap of spectra from multiple separated SnV centers. Photoluminescence excitation spectroscopy measurements at a cryogenic temperature showed that SnV centers exhibit stable fluorescence and linewidths close to the Fourier transform-limited linewidth. The inhomogeneous distribution was as low as ~4 GHz, which enabled the observation of Sn isotope-dependent resonant frequencies. Owing to the narrow inhomogeneous distribution, we observed multiple SnV centers showing ident…
We experimentally demonstrate the integration of silicon-vacancy centers in nanodiamonds (SiV-NDs) with an optical nanofiber (ONF). We grow SiV-NDs on seed NDs dispersed on a quartz substrate using a microwave plasma-assisted chemical vapor deposition method. First, we search and characterize SiV-NDs on a quartz substrate using an inverted confocal microscope and an atomic force microscope (AFM). Subsequently, we pick up SiV-NDs from the quartz substrate and deposit them on the surface of a free-standing ONF using the AFM tip. The fluorescence emission spectrum, photon count rate, and intensit…
We demonstrate magnetometry by detection of the spin state of high-density nitrogen-vacancy ensembles in diamond using optical absorption at 1042 nm. With this technique, measurement contrast, and collection efficiency can approach unity, leading to an increase in magnetic sensitivity compared to the more common method of collecting red fluorescence. Working at 75 K with a sensor with effective volume $50 \times 50 \times 300$ microns^3, we project photon shot-noise limited sensitivity of 5 pT in one second of acquisition and bandwidth from dc to a few megahertz. Operation in a gradiometer con…
We presented a high-sensitivity temperature detection using an implanted single Nitrogen-Vacancy center array in diamond. The high-order Thermal Carr-Purcell-Meiboom-Gill (TCPMG) method was performed on the implanted single nitrogen vacancy (NV) center in diamond in a static magnetic field. We demonstrated that under small detunings for the two driving microwave frequencies, the oscillation frequency of the induced fluorescence of the NV center equals approximately to the average of the detunings of the two driving fields. On basis of the conclusion, the zero-field splitting D for the NV cente…
We theoretically analyse the cooling dynamics of a high-Q mode of a mechanical resonator, when the structure is also an optical cavity and is coupled with a NV center. The NV center is driven by a laser and interacts with the cavity photon field and with the strain field of the mechanical oscillator, while radiation pressure couples mechanical resonator and cavity field. Starting from the full master equation we derive the rate equation for the mechanical resonator's motion, whose coefficients depend on the system parameters and on the noise sources. We then determine the cooling regime, the c…
The charge state dynamics of the nitrogen-vacancy (NV) center in diamond play a key role in a wide range of applications, yet remain imperfectly understood. Using single ps-pulses and pulse pairs, we quantitatively investigate the charge dynamics associated with excitation and fluorescence depletion of a single NV center. Our pulsed excitation approach permits significant modeling simplifications, and allows us to extract relative rates of excitation, stimulated emission, ionization, and recombination under 531 nm and 766 nm illumination. By varying the duration between paired pulses, we can a…
We employ a fiber-based optical microcavity with high finesse to study the enhancement of phonon sideband fluorescence of nitrogen-vacancy centers in nanodiamonds. Harnessing the full tunability and open access of the resonator, we explicitly demonstrate the scaling laws of the Purcell enhancement by varying both the mode volume and the quality factor over a large range. While changes in the emission lifetime remain small in the regime of a broadband emitter, we observe an increase of the emission spectral density by up to a factor of 300. This gives a direct measure of the Purcell factor that…
Single silicon vacancy (SiV) color centers in diamond have recently shown the ability for high brightness, narrow bandwidth, room temperature single photon emission. This work develops a model describing the three level population dynamics of single SiV centers in diamond nanocrystals on iridium surfaces including an intensity dependent de-shelving process. Furthermore, we investigate the brightness and photostability of single centers and find maximum single photon rates of 6.2 Mcps under continuous excitation. We investigate the collection efficiency of the fluorescence and estimate quantum …
Ensembles of nitrogen-vacancy centers in diamond are a highly promising platform for high-sensitivity magnetometry, whose efficacy is often based on efficiently generating and monitoring magnetic-field dependent infrared fluorescence. Here we report on an increased sensing efficiency with the use of a 532-nm resonant confocal cavity and a microwave resonator antenna for measuring the local magnetic noise density using the intrinsic nitrogen-vacancy concentration of a chemical-vapor deposited single-crystal diamond. We measure a near-shot-noise-limited magnetic noise floor of 200 pT/$\sqrt{\tex…
In this work, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6 ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This work paves the way towards realization of building blocks of quantum hardware with an efficie…
Magnetic sensing and imaging instruments are important tools in biological and material sciences. There is an increasing demand for attaining higher sensitivity and spatial resolution, with implementations using a single qubit offering potential improvements in both directions. In this article we describe a scanning magnetometer based on the nitrogen-vacancy center in diamond as the sensor. By means of a quantum-assisted readout scheme together with advances in photon collection efficiency, our device exhibits an enhancement in signal to noise ratio of close to an order of magnitude compared t…
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…
