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 demonstrate an all-optical thermometer based on an ensemble of silicon-vacancy centers (SiVs) in diamond by utilizing a temperature dependent shift of the SiV optical zero-phonon line transition frequency, $Δλ/ΔT= 6.8\,\mathrm{GHz/K}$. Using SiVs in bulk diamond, we achieve $70\,\mathrm{mK}$ precision at room temperature with a sensitivity of $360\,\mathrm{mK/\sqrt{Hz}}$. Finally, we use SiVs in $200\,\mathrm{nm}$ nanodiamonds as local temperature probes with $521\,\mathrm{ mK/\sqrt{Hz}}$ sensitivity. These results open up new possibilities for nanoscale thermometry in biology, chemistry, a…
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'…
Diamond quantum thermometry exploits the optical and electrical spin properties of colour defect centres in diamonds and, acts as a quantum sensing method exhibiting ultrahigh precision and robustness. Compared to the existing luminescent nanothermometry techniques, a diamond quantum thermometer can be operated over a wide temperature range and a sensor spatial scale ranging from nanometres to micrometres. Further, diamond quantum thermometry is employed in several application, including electronics and biology, to explore these fields with nanoscale temperature measurements. This review cover…
Versatile nanoscale sensors that are susceptible to changes in a variety of physical quantities often exhibit limited selectivity. This paper reports a novel scheme based on microwave-dressed spin states for optically probed nanoscale temperature detection using diamond quantum sensors, which provides selective sensitivity to temperature changes. By combining this scheme with a continuous pump-probe scheme using ensemble nitrogen-vacancy centers in nanodiamonds, a sub-microsecond temporal resolution with thermal sensitivity of 3.7 K$\cdot$Hz$^{-1/2}$ that is insensitive to variations in extern…
We present measurements of the Electronic Spin Resonance (ESR) of Nitrogen Vacancy (NV) centers in diamonds that are levitating in a ring Paul trap under vacuum. We observe ESR spectra of NV centers embedded in micron-sized diamonds at vacuum pressures down to $2\times 10^{-1}$ mbar, limited by the green laser heating of the diamond. We also observe the NV photoluminescence at vacuum pressures down to $10^{-2}$ mbar and discuss the steps required to control the NV spin under ultra-high vacuum.
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…
Sensitive probing of temperature variations on nanometer scales represents an outstanding challenge in many areas of modern science and technology. In particular, a thermometer capable of sub-degree temperature resolution as well as integration within a living system could provide a powerful new tool for many areas of biological research, including temperature-induced control of gene expression and cell-selective treatment of disease. Here, we demonstrate a new approach to nanoscale thermometry that utilizes coherent manipulation of the electronic spin associated with nitrogen-vacancy (NV) col…
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…
In this study, we analyze the operational process of nanodiamond (ND) quantum thermometry based on wide-field detection of optically detected magnetic resonance (ODMR) of nitrogen vacancy centers, and compare its performance with that of confocal ODMR detection. We found that (1) the thermometry results are significantly affected by the shape and size of the camera region of interest (ROI) surrounding the target NDs and that (2) by properly managing the ROI and acquisition parameters of the camera, a temperature precision comparable to confocal detection in living cells can be obtained by wide…
The nitrogen vacancy (NV) center in diamond has emerged as a leading solid-state quantum sensor for applications including magnetometry, electrometry, thermometry, and chemical sensing. However, an outstanding challenge for practical applications is that existing NV-based sensing techniques require bulky and discrete instruments for spin control and detection. Here, we address this challenge by integrating NV based quantum sensing with complementary metal-oxide-semiconductor (CMOS) technology. Through tailored CMOS-integrated microwave generation and photodetection, this work dramatically redu…
Quantum sensors with solid state electron spins have attracted considerable interest due to their nanoscale spatial resolution.A critical requirement is to suppress the environment noise of the solid state spin sensor.Here we demonstrate a nanoscale thermometer based on silicon carbide (SiC) electron spins.We experimentally demonstrate that the performance of the spin sensor is robust against dephasing due to a self protected machenism. The SiC thermometry may provide a promising platform for sensing in a noisy environment ,e.g. biological system sensing.
Producing nano-structures with embedded bright ensembles of lifetime-limited emitters is a challenge with potential high impact in a broad range of physical sciences. In this work, we demonstrate controlled charge transfer to and from dark states exhibiting very long lifetimes in high density ensembles of SiV centers hosted in a CVD-grown diamond nano-pyramid. Further, using a combination of resonant photoluminescence excitation and a frequency-selective persistent hole burning technique that exploits such charge state transfer, we could demonstrate close to lifetime-limited linewidths from th…
Nitrogen-vacancy centres (NVs) in diamond are attractive for research straddling quantum information science and nanoscale magnetometry and thermometry. While ultrapure bulk diamond NVs sustain the longest spin coherence times among optically accessible spins, nanodiamond NVs display persistently poor spin coherence. Here we introduce high-purity nanodiamonds accommodating record-long NV coherence times, >60 us, observed via universal dynamical decoupling. We show that the main contribution to decoherence comes from nearby nitrogen impurities rather than surface states. We protect the NV spin …
We propose and theoretically analyze an experiment where displacement sensing of an optically levitated nanoparticle in front of a surface can be used to measure the induced dipole-dipole interaction between the nanoparticle and its thermal image. This is achieved by using a surface that is transparent to the trapping light but reflective to infrared radiation, with a reflectivity that can be time modulated. This dipole-dipole interaction relies on the thermal radiation emitted by a silica nanoparticle having sufficient temporal coherence to correlate the reflected radiation with the thermal f…
We present measurements of silica optomechanical resonators, known as bottle resonators, passively cooled in a cryogenic environment. These devices possess a suite of properties that make them advantageous for preparation and measurement in the mechanical ground state, including high mechanical frequency, high optical and mechanical quality factors, and optomechanical sideband resolution. Performing thermometry of the mechanical motion, we find that the optical and mechanical modes demonstrate quantitatively similar laser-induced heating, limiting the lowest average phonon occupation observed …
We present a new approach combining top down fabrication and bottom up overgrowth to create diamond photonic nanostructures in form of single-crystalline diamond nanopyramids. Our approach relies on diamond nanopillars, that are overgrown with single-crystalline diamond to form pyramidal structures oriented along crystal facets. To characterize the photonic properties of the pyramids, color centers are created in a controlled way using ion implantation and annealing. We find very high collection efficiency from color centers close to the pyramid apex. We further show excellent smoothness and s…
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely…
Resonantly enhanced emission from the zero phonon line of a diamond nitrogen-vacancy (NV) center in single crystal diamond is demonstrated experimentally using a hybrid whispering gallery mode nanocavity. A 900 nm diameter ring nanocavity formed from gallium phosphide, whose sidewalls extend into a diamond substrate, is tuned onto resonance at low-temperature with the zero phonon line of a negatively charged NV center implanted near the diamond surface. When the nanocavity is on resonance, the zero phonon line intensity is enhanced by approximately an order of magnitude, and the spontaneous em…
We propose and analyze a novel mechanism for long-range spin-spin interactions in diamond nanostructures. The interactions between electronic spins, associated with nitrogen-vacancy centers in diamond, are mediated by their coupling via strain to the vibrational mode of a diamond mechanical nanoresonator. This coupling results in phonon-mediated effective spin-spin interactions that can be used to generate squeezed states of a spin ensemble. We show that spin dephasing and relaxation can be largely suppressed, allowing for substantial spin squeezing under realistic experimental conditions. Our…
We show that nitrogen-vacancy (NV) centers in diamond interfaced with a suspended carbon nanotube carrying a dc current can facilitate a spin-nanomechanical hybrid device. We demonstrate that strong magnetomechanical interactions between a single NV spin and the vibrational mode of the suspended nanotube can be engineered and dynamically tuned by external control over the system parameters. This spin-nanomechanical setup with strong, \emph{intrinsic} and \emph{tunable} magnetomechanical couplings allows for the construction of hybrid quantum devices with NV centers and carbon-based nanostructu…
Understanding heat transport is relevant to develop efficient strategies for thermal management in microelectronics for instance, as well as for fundamental science purposes. However, measuring temperatures in nanostructured environments and in cryogenic conditions remains a challenging task, that requires both high sentitivity and a non-invasive approach. Here we present a portable nanothermometer based on a molecular two-level quantum system that operates in the 3 - 30 K temperature range, with excellent temperature and spatial resolutions on the order of mK and $μ$m, respectively. We valida…
We propose experimentally feasible means for non-destructive thermometry of homogeneous Bose Einstein condensates in different spatial dimensions ($d\in\{1,2,3\}$). Our impurity based protocol suggests that the fundamental error bound on thermometry at the sub nano Kelvin domain depends highly on the dimension, in that the higher the dimension the better the precision. Furthermore, sub-optimal thermometry of the condensates by using measurements that are experimentally feasible is explored. We specifically focus on measuring position and momentum of the impurity that belong to the family of Ga…
Optomechanical devices sensitively transduce and actuate motion of nanomechanical structures using light. Single--crystal diamond promises to improve the performance of optomechanical devices, while also providing opportunities to interface nanomechanics with diamond color center spins and related quantum technologies. Here we demonstrate dissipative waveguide--optomechanical coupling exceeding 35 GHz/nm to diamond nanobeams supporting both optical waveguide modes and mechanical resonances, and use this optomechanical coupling to measure nanobeam displacement with a sensitivity of $9.5$ fm/$\s…
For atoms or molecules in optical lattices, conventional thermometry methods are often unsuitable due to low particle numbers or a lack of cycling transitions. However, a differential spectroscopic light shift can map temperature onto the line shape with a low sensitivity to trap anharmonicity. We study narrow molecular transitions to demonstrate precise frequency-based lattice thermometry, as well as carrier cooling. This approach should be applicable down to nanokelvin temperatures. We also discuss how the thermal light shift can affect the accuracy of optical lattice clocks.
We demonstrate the fabrication of single-crystalline diamond nanopillars on a (111)-oriented chemical vapor deposited diamond substrate. This crystal orientation offers optimal coupling of nitrogen-vacancy (NV) center emission to the nanopillar mode and is thus advantageous over previous approaches. We characterize single native NV centers in these nanopillars and find one of the highest reported saturated fluorescence count rates in single crystalline diamond in excess of 10${}^6$ counts per second. We show that our nano-fabrication procedure conserves the preferential alignment as well as th…
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…
Nitrogen-vacancy (NV) centers in diamond are promising quantum sensors for their long spin coherence time under ambient conditions. However, their spin resonances are relatively insensitive to non-magnetic parameters such as temperature. A magnetic-nanoparticle-nanodiamond hybrid thermometer, where the temperature change is converted to the magnetic field variation near the Curie temperature, was demonstrated to have enhanced temperature sensitivity (11 mK Hz^{-1/2}) [Phys. Rev. X 8, 011042 (2018)], but the sensitivity was limited by the large spectral broadening of ensemble spins in nanodiamo…
Capturing the rotational motion of single nanoparticles has been hindered owing to the difficulty of acquiring directional information under the optical diffraction limit. Here, we demonstrate that electron spins of single nitrogen vacancy (NV) centers can sense the rotational Brownian motion of their host nanodiamonds. When nanodiamonds are gradually detached from the substrates that they were fixed to, their optically detected spin resonance peaks are broadened by 1.8 MHz, which corresponds to the rotational diffusion constant of nanoparticles with a diameter of 11.4 nm from the Einstein-Smo…
The past decade has seen great advances in developing color centers in diamond for sensing, quantum information processing, and tests of quantum foundations. Increasingly, the success of these applications as well as fundamental investigations of light-matter interaction depend on improved control of optical interactions with color centers -- from better fluorescence collection to efficient and precise coupling with confined single optical modes. Wide ranging research efforts have been undertaken to address these demands through advanced nanofabrication of diamond. This review will cover recen…
Precise control over the position of a single quantum object is important for many experiments in quantum science and nanotechnology. We report on a technique for high-accuracy positioning of individual diamond nanocrystals. The positioning is done with a home-built nanomanipulator under real-time scanning electron imaging, yielding an accuracy of a few nanometers. This technique is applied to pick up, move and position a single NV defect center contained in a diamond nanocrystal. We verify that the unique optical and spin properties of the NV center are conserved by the positioning process.
Color centers in diamond are versatile solid state atomic-like systems suitable for quantum technological applications. In particular, the negatively charged silicon vacancy center (SiV) can exhibit a narrow photoluminescence (PL) line and lifetime-limited linewidth in bulk diamonds at cryogenic temperature. We present a low-temperature study of chemical vapour deposition (CVD)-grown diamond nano-pyramids containing SiV centers. The PL spectra feature a bulk-like zero-phonon line with ensembles of SiV centers, with a linewidth below 10 GHz which demonstrates very low crystal strain for such a …
Observation of Shear Strain in Ion-Implanted Diamond Substrate and Diamond Nanophotonic Structures
Indian Institute of Technology Bombay（印度理工学院孟买分校）；Center for Research in Nano Technology and Science, Indian Institute of Technology Bombay（印度理工学院纳米科技与科学研究中心）；Solid State Physics Laboratory（固体物理实验室）；School of Physical Sciences, UM-DAE Centre for Excellence in Basic Sciences, University of Mumbai（孟买大学基础科学卓越中心物理学院）
Nitrogen-Vacancy (NV) spin in diamond is a versatile quantum sensor, being able to measure physical quantities such as magnetic field, electric field, temperature, and pressure. In the present work, we demonstrate a multiplexed sensing of magnetic field and temperature. The dual frequency driving technique we employ here is based on frequency-division multiplexing, which enables sensing both measurables in real time. The pair of NV resonance frequencies for dual frequency driving must be selected to avoid coherent population trapping of NV spin states. With an enhanced optical collection effic…
Powered by the mutual developments in instrumentation, materials andtheoretical descriptions, sensing and imaging capabilities of quantum emitters insolids have significantly increased in the past two decades. Quantum emitters insolids, whose properties resemble those of atoms and ions, provide alternative waysto probing natural and artificial nanoscopic systems with minimum disturbance andultimate spatial resolution. Among those emerging quantum emitters, the nitrogen-vacancy (NV) color center in diamond is an outstanding example due to its intrinsicproperties at room temperature (highly-lumi…
The quantum properties of the fluorescence light emitted by diamond nanocrystals containing a single nitrogen-vacancy (NV) colored center is investigated. We have observed photon antibunching with very low background light. This system is therefore a very good candidate for the production of single photon on demand. In addition, we have measured larger NV center lifetime in nanocrystals than in the bulk, in good agreement with a simple quantum electrodynamical model.
The development of materials processing techniques for optical diamond nanostructures containing a single color center is an important problem in quantum science and technology. In this work, we present the combination of ion implantation and top-down diamond nanofabrication in two scenarios: diamond nanopillars and diamond nanowires. The first device consists of a 'shallow' implant (~20nm) to generate Nitrogen-vacancy (NV) color centers near the top surface of the diamond crystal. Individual NV centers are then isolated mechanically by dry etching a regular array of nanopillars in the diamond…
We demonstrate the controlled preparation of heteroepitaxial diamond nano- and microstructures on silicon wafer based iridium films as hosts for single color centers. Our approach uses electron beam lithography followed by reactive ion etching to pattern the carbon layer formed by bias enhanced nucleation on the iridium surface. In the subsequent chemical vapor deposition process, the patterned areas evolve into regular arrays of (001) oriented diamond nano-islands with diameters of <500nm and a height of approx. 60 nm. In the islands, we identify single SiV color centers with narrow zero phon…
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.
The photoluminescence of nitrogen-vacancy (NV) centers in diamond nanoparticles exhibits specific properties as compared to NV centers in bulk diamond. For instance large fluctuations of lifetime and brightness from particle to particle have been reported. It has also been observed that for nanocrystals much smaller than the mean luminescence wavelength, the particle size sets a lower threshold for resolution in Stimulated Emission Depletion (STED) microscopy. We show that all these features can be quantitatively understood by realizing that the absorption-emission of light by the NV center is…
Color centers in diamond are promising spin qubits for quantum computing and quantum networking. In photon-mediated entanglement distribution schemes, the efficiency of the optical interface ultimately determines the scalability of such systems. Nano-scale optical cavities coupled to emitters constitute a robust spin-photon interface that can increase spontaneous emission rates and photon extraction efficiencies. In this work, we introduce the fabrication of 2D photonic crystal slab nanocavities with high quality factors and cubic wavelength mode volumes -- directly in bulk diamond. This plana…
Long-term observations of photoluminescence at the single-molecule level were until recently very diffcult, due to the photobleaching of organic ?uorophore molecules. Although inorganic semiconductor nanocrystals can overcome this diffculty showing very low photobleaching yield, they suffer from photoblinking. A new marker has been recently introduced, relying on diamond nanoparticles containing photoluminescent color centers. In this work we compare the photoluminescence of single quantum dots (QDs) to the one of nanodiamonds containing a single-color center. Contrary to other markers, photol…
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.
Integrating solid-state quantum emitters with nanophotonic resonators is essential for efficient spin-photon interfacing and optical networking applications. While diamond color centers have proven to be excellent candidates for emerging quantum technologies, their integration with optical resonators remains challenging. Conventional approaches based on etching resonators into diamond often negatively impact color center performance and offer low device yield. Here, we developed an integrated photonics platform based on templated atomic layer deposition of TiO2 on diamond membranes. Our fabric…
We introduce a process for the fabrication of high quality, spatially isolated nano-diamonds on iridium via microwave plasma assisted CVD-growth. We perform spectroscopy of single silicon-vacancy (SiV)-centres produced during the growth of the nano-diamonds. The colour centres exhibit extraordinary narrow zero-phonon-lines down to 0.7 nm at room temperature. Single photon count rates up to 4.8 Mcps at saturation make these SiV-centres the brightest diamond based single photon sources to date. We measure for the first time the fine structure of a single SiV-centre thus confirming the atomic com…
We demonstrate a new approach for engineering group IV semiconductor-based quantum photonic structures containing negatively charged silicon-vacancy (SiV$^-$) color centers in diamond as quantum emitters. Hybrid SiC/diamond structures are realized by combining the growth of nanoand micro-diamonds on silicon carbide (3C or 4H polytype) substrates, with the subsequent use of these diamond crystals as a hard mask for pattern transfer. SiV$^-$ color centers are incorporated in diamond during its synthesis from molecular diamond seeds (diamondoids), with no need for ionimplantation or annealing. We…
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…
We investigate native nitrogen (NV) and silicon vacancy (SiV) color centers in commercially available, heteroepitaxial, wafer-sized, mm thick, single-crystal diamond. We observe single, native NV centers with a density of roughly 1 NV per $μm^3$ and moderate coherence time ($T_2 = 5 μs$) embedded in an ensemble of SiV centers. Low-temperature spectroscopy of the SiV zero phonon line fine structure witnesses high crystalline quality of the diamond especially close to the growth surface, consistent with a reduced dislocation density. Using ion implantation and plasma etching, we verify the possi…
We demonstrate the fabrication of photonic crystal nanobeam cavities with rectangular cross section into bulk diamond. In simulation, these cavities have an unloaded quality factor (Q) of over 1 million. Measured cavity resonances show fundamental modes with spectrometer-limited quality factors larger than 14,000 within 1nm of the NV center's zero phonon line at 637nm. We find high cavity yield across the full diamond chip with deterministic resonance trends across the fabricated parameter sweeps.
