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In this paper we study the dynamics of an ensemble of nitrogen-vacancy centers in diamond when its photoluminescence is detected by means of a widefield imaging system. We develop a seven-level model and use it to simulate the widefield detection of nitrogen-vacancy centers Rabi oscillations. The simulation results are compared with experimental measurements showing a good agreement. In particular, we use the model to explain the asymmetric shape of the detected Rabi oscillations due to an incomplete repolarization of the nitrogen-vacancy center during the pulse sequence implemented for the detection of Rabi oscillations., Comment: 14 pages, 7 figures

Engineering a layer of nitrogen-vacancy (NV) centers on the tip of a diamond anvil creates a multipurpose quantum sensors array for high pressure measurements, especially for probing magnetic and superconducting properties of materials. Expanding this concept above 100 GPa appears to be a substantial challenge. We observe that deviatoric stress on the anvil tip sets a limit at 40-50 GPa for practical magnetic measurements based on optically detected magnetic resonance (ODMR) of NV centers under pressure. We show that this limit can be circumvented up to at least 130 GPa by machining a micropillar on the anvil tip to create a quasi-hydrostatic stress environment for the NV centers. This is quantified using the pressure dependence of the diamond Raman shift, the NV ODMR dependence on applied magnetic field, and NV photoluminescence spectral shift. This paves the way for direct and reliable detection of the Meissner effect in superconductors above 100 GPa, such as super-hydrides., Comment: 5 pages, 4 figures

The spin readout of an ensemble of nitrogen-vacancy (NV) centers in diamond can be realized by a photoconductive detection that is a complementary method to the optical detection of the NV electron spin magnetic resonance. Here, we implement the photoconductive detection through graphitic planar electrodes that collect the photocurrent. Graphitic electrodes are patterned using a xenon Focused-Ion Beam on an Optical-Grade quality diamond crystal containing a nitrogen concentration of ~1 ppm and a NV concentration of a few ppb. Resistance and current-voltage characteristics of the NV-doped diamond junction are investigated tuning the 532 nm pump beam intensity. The junction has an ohmic behavior and under a strong bias field, we observe velocity saturation of the optically-induced carriers in the diamond junction. We perform the photoconductive detection in continuous-wave regime of the magnetic resonance of the NV centers ensemble for a magnetic field applied along the <100> and the <111> direction with a magnitude above 100 mT. This technique enables the realization of all-carbon diamond quantum sensors integrating graphitic microstructures for the electrical readout., Comment: 11 pages, 3 figures, the following article has been submitted to Applied Physics Letters

We investigate the optical properties of silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in nanodiamonds under hydrostatic pressure up to 180 GPa. The nanodiamonds were synthetized by Si or Ge-doped plasma assisted chemical vapor deposition and, for our experiment, pressurized in a diamond anvil cell. Under hydrostatic pressure we observe blue-shifts of the SiV and GeV zero-phonon lines by 17 THz (70 meV) and 78 THz (320 meV), respectively. These measured pressure induced shifts are in good agreement with ab initio calculations that take into account the lattice compression based on the equation of state of diamond and that are extended to the case of the tin-vacancy (SnV) center. This work provides guidance on the use of group-IV-vacancy centers as quantum sensors under extreme pressures that will exploit their specific optical and spin properties induced by their intrinsic inversion-symmetric structure., Comment: 7 pages, 4 figures

The fast development of radio-frequency (RF) technologies increases the need for compact, low consumption and broadband real-time RF spectral analyser. To overcome the electronic bottleneck encountered by electronic solutions, which limits the real time bandwidth to hundreds of MHz, we propose a new approach exploiting the quantum properties of the nitrogen-vacancy (NV) center in diamond. Here we describe a Quantum Diamond Signal Analyser (Q-DiSA) platform and characterize its performances. We successfully detect RF signals over a large tunable frequency range (25 GHz), a wide instantaneous bandwidth (up to 4 GHz), a MHz frequency resolution (down to 1 MHz), a ms temporal resolution and a large dynamic range (40 dB).

The Brownian motion of a particle hotter than its environment is an iconic out-of-equilibrium system. Its study provides valuable insights into nanoscale thermal effects. Notably, it supplies an excellent diagnosis of thermal effects in optically levitated particles, a promising platform for force sensing and quantum physics tests. Thus, understanding the relevant parameters in this effect is critical. In this context, we test the role of particles' shape and material, using optically levitated nanodiamonds hosting NV centers to measure the particles' internal temperature and center-of-mass dynamics. We present a model to assess the nanodiamond internal temperature from its dynamics, adaptable to other particles. We also demonstrate that other mechanisms affect the nanodiamond dynamics and its stability in the trap. Finally, our work, by showing levitating nanodiamonds as an excellent tool for studying nano-thermal effects, opens prospects for increasing the trapping stability of optically levitated particles., Comment: 14 pages with supporting information

Scanning diamond magnetometers based on the optically detected magnetic resonance of the nitrogen-vacancy centre offer very high sensitivity and non-invasive imaging capabilities when the stray fields emanating from ultrathin magnetic materials are sufficiently low (< 10 mT). Beyond this low-field regime, the optical signal quenches and a quantitative measurement is challenging. While the field-dependent NV photoluminescence can still provide qualitative information on magnetic morphology, this operation regime remains unexplored particularly for surface magnetisation larger than $\sim$ 3 mA. Here, we introduce a multi-angle reconstruction technique (MARe) that captures the full nanoscale domain morphology in all magnetic-field regimes leading to NV photoluminescence quench. To demonstrate this, we use [Ir/Co/Pt]$_{14}$ multilayer films with surface magnetisation an order of magnitude larger than previous reports. Our approach brings non-invasive nanoscale magnetic field imaging capability to the study of a wider pool of magnetic materials and phenomena.

We report the possibility to simultaneously perform wide-field nitrogen-vacancy (NV) diamond magnetic microscopy and synchrotron X-ray diffraction (XRD) measurements at high pressure. NV color centers are created on the culet of a diamond anvil which is integrated in a diamond anvil cell for static compression of the sample. The optically detected spin resonance of the NV centers is used to map the stray magnetic field produced by the sample magnetization. Using this combined scheme, the magnetic and structural behaviors can be simultaneously measured. As a proof-of-principle, we record the correlated {\alpha}-Fe to {\epsilon}-Fe structural and magnetic transitions of iron that occur here between 15 and 20 GPa at 300 K., Comment: 12 pages, 4 figures

We report the experimental study of the temperature-dependence of the longitudinal spin relaxation time $T_1$ of single Nitrogen-Vacancy (NV) centers hosted in nanodiamonds. To determine the relaxation mechanisms at stake, measurements of the $T_1$ relaxation time are performed for a set of individual NV centers both at room and cryogenic temperatures. The results are consistant with a temperature-dependent relaxation process which is attributed to a thermally-activated magnetic noise produced by paramagnetic impurities lying on the nanodiamond surface. These results confirm the existence of surface-induced spin relaxation processes occurring in nanodiamonds, which are relevant for future developments of sensitive nanoscale NV-based quantum sensors.

Pressure is a unique tool to tune the interplay between structural, electronic and magnetic interactions. It leads to remarkable properties of materials such as recent temperature records in superconductivity. Advanced magnetic measurements under very high pressure in the Diamond Anvil Cell (DAC) use synchrotron approaches but these are lacking a formal link to the macroscopic magnetic properties. We report an alternative method consisting in optical magnetometry based on nitrogen-vacancy (NV) centers created at the surface of a diamond anvil. We illustrate the method by two measurements realized at room and low temperature respectively: the pressure evolution of the magnetization of an iron bead up to 30 GPa showing the iron ferromagnetic collapse and the detection of the superconducting transition of MgB2 at 7 GPa., Comment: 15 pages, 4 figures

We propose an hybrid laser system consisting of a semiconductor external cavity laser associated to an intra-cavity diamond etalon doped with nitrogen-vacancy color centers. We consider laser emission tuned to the infrared absorption line that is enhanced under the magnetic field dependent nitrogen-vacancy electron spin resonance and show that this architecture leads to a compact solid-state magnetometer that can be operated at room-temperature. The sensitivity to the magnetic field limited by the photon shot-noise of the output laser beam is estimated to be around $250~\mathrm{fT/\sqrt{Hz}}$. Unlike usual NV center infrared magnetometry, this method would not require an external frequency stabilized laser. Since the proposed system relies on the competition between the laser threshold and an intracavity absorption, such laser-based optical sensor could be easily adapted to a broad variety of physical systems.

We present a novel technique based on an ensemble of Nitrogen-Vacancy (NV) centers in diamond to perform Magnetic Current Imaging (MCI) on an Integrated Circuit (IC). NV centers in diamond allow measuring the three components of the magnetic fields generated by a mA range current in an IC structure over a field of 50 x 200 {\mu}m^2 with sub-micron resolution. Vector measurements allow using a more robust algorithm than those used for MCI using Giant Magneto Resistance (GMR) or Superconducting Quantum Interference Device (SQUID) sensors and it is opening new current reconstruction prospects. Calculated MCI from these measurements shows a very good agreement with theoretical current path. Acquisition time is around 10 sec, which is much faster than scanning measurements using SQUID or GMR. The experimental set-up relies on a standard optical microscope, and the measurements can be performed at room temperature and atmospheric pressure. These early experiments, not optimized for IC, show that NV centers in diamond could become a real alternative for MCI in IC., Comment: 7 pages, 4 figures

The creation of nitrogen-vacancy centres in diamond is nowadays well controlled using nitrogen implantation and annealing. Although the high-resolution placement of NV centres has been demonstrated using either collimation through pierced AFM tips or masks with apertures made by electron beam lithography, a targeted implantation into pre-defined structures in diamond may not be achieved using these techniques. We show that a beam of nitrogen ions can be focused to approximately 100 nm using focused ion beam (FIB) technology. The nitrogen ion beam is produced using an electron cyclotron resonance (ECR) plasma source. Combined with a scanning electron microscope, the nitrogen-FIB offers new possibilities for the targeted creation of single defects in diamond. This maskless technology is suitable for example for the creation of optical centres in the cavities of photonic crystals or in diamond tips for scanning magnetometry. Finally, we further show that by changing the gas source from nitrogen to xenon, standard FIB milling capabilities are also available within the same tool.

We propose to use an optical cavity to enhance the sensitivity of magnetometers relying on the detection of the spin state of high-density nitrogen-vacancy ensembles in diamond using infrared optical absorption. The role of the cavity is to obtain a contrast in the absorption-detected magnetic resonance approaching unity at room temperature. We project an increase in the photon shot-noise limited sensitivity of two orders of magnitude in comparison with a single-pass approach. Optical losses can limit the enhancement to one order of magnitude which could still enable room temperature operation. Finally, the optical cavity also allows to use smaller pumping power when it is designed to be resonant at both the pump and the signal wavelength.

We study both theoretically and experimentally the free induction decay (FID) of the electron spin associated with a single nitrogen-vacancy defect in high purity diamond, where the main source of decoherence is the hyperfine interaction with a bath of $^{13}$C nuclear spins. In particular, we report a systematic study of the FID signal as a function of the strength of a magnetic field oriented along the symmetry axis of the defect. On average, an increment of the coherence time by a factor of $\sqrt{5/2}$ is observed at high magnetic field in diamond samples with a natural abundance of $^{13}$C nuclear spins, in agreement with numerical simulations and theoretical studies. Further theoretical analysis shows that this enhancement is independent of the concentration of nuclear spin impurities. By dividing the nuclear spin bath into shells and cones, we theoretically identify which nuclear spins are responsible for the observed dynamics., Comment: 16 pages, 7 figures

We present both theoretical and experimental results on fluorescence of single defect centers in diamond nanocrystals embedded in a planar dielectric microcavity. From a theoretical point of view, we show that the overall fluorescence collection efficiency using moderate numerical aperture microscope objective can be enhanced by using a low quality factor microcavity. This could be used in particular for low temperature applications where the numerical aperture of collection microscope objectives is limited due to the experimental constraints. We experimentally investigate the control of the fluorescence spectrum of the emitted light from a single center. We show the simultaneous narrowing of the room temperature broadband emission spectrum and the increase of the fluorescence spectral density., Comment: 22 pages, 10 figures

The controlled and coherent manipulation of individual quantum systems is a fundamental key for the development of quantum information processing. The nitrogen-vacancy (NV) color center in diamond is a promising system since its photoluminescence is perfectly stable at room temperature and its electron spin can be optically read-out at the individual level. We review here the experiments currently realized in our laboratory, concerning the use of single NV color center as single photon source and the coherent magnetic manipulation of the electron spin associated to a single NV color center. Furthermore, we demonstrate a nanoscopy experiment based on saturation absorption effect, which allows to optically pin-point single NV color center at a sub-? resolution. This opens a possibility to independently address two or multiple magnetically-coupled single NV color centers, which is a necessary step toward the realization of a diamond-based quantum computer., Comment: 8 pages

We investigate the electron spin resonance of an ensemble of Nitrogen-Vacancy (NV) color centers in a bulk diamond crystal. The four possible orientations of the NV-center in the lattice lead to different dependences on the magnitude and the orientation of an external static magnetic field. Experimental results obtained with a continuous microwave excitation are in good agreement with simulations. In addition, we observe that the average radiative lifetime of the NV color center is also modified when the external magnetic field is applied. This variation is explained by the mixing between mS = 0 and mS = $\pm$1 spin states of the NV-center with different radiative lifetimes, due to magnetic coupling. These results are of interest for a broad range of applications, such as spin-resonance-based magnetometry with a high-density ensemble of NV-centers, Comment: 14 pages, published on Applied Physics Letters journal

Individual color centers in diamond are promising for near-term quantum technologies including quantum key distribution and metrology. Here we show fabrication of a new color center which has photophysical properties surpassing those of the two main-stay centers, namely the nitrogen vacancy and NE8 centers. The new center is fabricated using focused ion beam implantation of nickel into isolated chemical vapor deposited diamond micro-crystals. Room temperature photoluminescence studies reveal a narrow emission in the near infrared region centered at 768 nm with a lifetime as short as 2 ns. Its focused ion beam compatibility opens the prospect to fabrication with nanometer resolution and realization of integrated quantum photonic devices. Preliminary investigations suggest that this center arises from an as-yet uncharacterized nickel-silicon complex.

We report an experimental test of complementarity using clock-triggered single-photon pulses emitted by an individual N-V color center in a diamond nanocrystal. The single photons are sent into a Mach-Zehnder interferometer with an output beamsplitter of adjustable reflection coefficient R. In addition, the choice of introducing or removing this beamsplitter is random and relativistically space-like separated from the entering of the photon inside the interferometer, as required for the Wheeler's delayed-choice regime. Each set value of R allows us to observe interference with visibility V and to obtain incomplete which-path information characterized by the distinguishability D. The measured values of V and D are found to obey the complementarity relation V^2 + D^2 =< 1.

Diamond nanocrystals containing highly photoluminescent color centers are attractive non-classical and near-field light sources. For near-field applications the size of the nanocrystal is crucial since it defines the optical resolution. NV (Nitrogen-Vacancy) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamond with size down to 25 nm can hold a single NV color center with bright and stable photoluminescence.

Wheeler has strikingly illustrated the wave-particle duality by the delayed-choice thought experiment, in which the configuration of a 2-path interferometer is chosen after a single-photon light-pulsed has entered it. We present a quantitative theoretical analysis of an experimental realization of Wheeler's proposal.

We report the realization of a solid-state triggered single-photon source with narrow emission in the near infrared at room temperature. It is based on the photoluminescence of a single nickel-nitrogen NE8 colour centre in a chemical vapour deposited diamond nanocrystal. Stable single-photon emission has been observed in the photoluminescence under both continuous-wave and pulsed excitations. The realization of this source represents a step forward in the application of diamond-based single-photon sources to Quantum Key Distribution (QKD) under practical operating conditions., Comment: 10 pages

We report an optical technique that yields an enhancement of single-molecule photostability, by greatly suppressing photobleaching pathways which involve photoexcitation from the triplet state. This is accomplished by dynamically switching off the excitation laser when a quantum-jump of the molecule to the triplet state is optically detected. This procedure leads to a lengthened single-molecule observation time and an increased total number of detected photons. The resulting improvement in photostability unambiguously confirms the importance of photoexcitation from the triplet state in photobleaching dynamics, and may allow the investigation of new phenomena at the single-molecule level.

The quantum "mystery which cannot go away" (in Feynman's words) of wave-particle duality is illustrated in a striking way by Wheeler's delayed-choice GedankenExperiment. In this experiment, the configuration of a two-path interferometer is chosen after a single-photon pulse has entered it : either the interferometer is \textit{closed} (\textit{i.e.} the two paths are recombined) and the interference is observed, or the interferometer remains \textit{open} and the path followed by the photon is measured. We report an almost ideal realization of that GedankenExperiment, where the light pulses are true single photons, allowing unambiguous which-way measurements, and the interferometer, which has two spatially separated paths, produces high visibility interference. The choice between measuring either the 'open' or 'closed' configuration is made by a quantum random number generator, and is space-like separated -- in the relativistic sense -- from the entering of the photon into the interferometer. Measurements in the closed configuration show interference with a visibility of 94%, while measurements in the open configuration allow us to determine the followed path with an error probability lower than 1%.

We demonstrate the association of two-photon nonlinear microscopy with balanced homodyne detection for investigating second harmonic radiation properties at nanoscale dimensions. Variation of the relative phase between second-harmonic and fundamental beams is retrieved, as a function of the absolute orientation of the nonlinear emitters. Sensitivity down to approximately 3.2 photon/s in the spatio-temporal mode of the local oscillator is obtained. This value is high enough to efficiently detect the coherent second-harmonic emission from a single KTiOPO4 crystal of sub-wavelength size., Comment: 9 pages to appear in Applied Physics Letters

We report on the observation of single colour centers in natural diamond samples emitting in the near infrared region when optically excited. Photoluminescence of these single emitters have several striking features, such as a narrow-band fully polarized emission (FWHM 2 nm) around 780 nm, a short excited-state lifetime of about 2 ns, and perfect photostability at room temperature under our excitation conditions. We present a detailed study of their photophysical properties. Development of a triggered single-photon source relying on this single colour centre is discussed in the prospect of its application to quantum key distribution., Comment: 9 pages

We present a full implementation of a quantum key distribution (QKD) system with a single photon source, operating at night in open air. The single photon source at the heart of the functional and reliable setup relies on the pulsed excitation of a single nitrogen-vacancy color center in diamond nanocrystal. We tested the effect of attenuation on the polarized encoded photons for inferring longer distance performance of our system. For strong attenuation, the use of pure single photon states gives measurable advantage over systems relying on weak attenuated laser pulses. The results are in good agreement with theoretical models developed to assess QKD security.

n a recent experiment, we reported the time-domain intensity noise measurement of a single photon source relying on single molecule fluorescence control. In this article we present data processing, starting from photocount timestamps. The theoretical analytical expression of the time-dependent Mandel parameter Q(T) of an intermittent single photon source is derived from ON<->OFF dynamics . Finally, source intensity noise analysis using the Mandel parameter is quantitatively compared to the usual approach relying on the time autocorrelation function, both methods yielding the same molecular dynamical parameters., Comment: 22 pages, 7 figures

We elucidate the crystalline nature and the three-dimensional orientation of isolated organic nanocrystals embedded in a sol-gel matrix, using a polarized nonlinear microscopy technique that combines two-photon fluorescence and second harmonic generation. This technique allows the distinction between mono-crystalline structures and nano-scale poly-crystalline aggregates responsible for incoherent second harmonic signals., Comment: Soumis le 01 sept. 2003

We present high resolution two-photon excitation microscopy studies combining two-photon fluorescence (TPF) and second harmonic generation (SHG) in order to probe orientational distributions of molecular ensembles at room temperature. A detailed polarization analysis of TPF and SHG signals is used in order to unravel the parameters of the molecular orientational statistical distribution, using a technique which can be extended and generalized to a broad variety of molecular arrangements. A polymer film containing molecules active for TPF and/or SHG emission is studied as a model system. Polarized TPF is shown to provide information on specific properties pertaining to incoherent emission in molecular media, such as excitation transfer. SHG, being highly sensitive to a slight departure from centrosymmetry such as induced by an external electric field in the medium, complements TPF. The response of each signal to a variable excitation polarization allows investigation of molecular behavior in complex environments which affect their orientations and interactions., Comment: submitted April 9th, 2003 to J. Phys. Chem. B