There has been much recent interest in extending the technique of magnetic resonance imaging (MRI) down to the level of single spins with sub-optical wavelength resolution. However, the signal to noise ratio for images of individual spins is usually low and this necessitates long acquisition times and low temperatures to achieve high resolution. An exception to this is the nitrogen-vacancy (NV) color center in diamond whose spin state can be detected optically at room temperature. Here we apply MRI to magnetically equivalent NV spins in order to resolve them with resolution well below the optical wavelength of the readout light. In addition, using a microwave version of MRI we achieved a resolution that is 1/270 size of the coplanar striplines, which define the effective wavelength of the microwaves that were used to excite the transition. This technique can eventually be extended to imaging of large numbers of NVs in a confocal spot and possibly to image nearby dark spins via their mutual magnetic interaction with the NV spin.
Lasers have revolutionized optical science and technology, but their microwave counterpart, maser, has not realized its great potential due to its demanding work conditions (high-vacuum for gas maser and liquid-helium temperature for solid-state maser). Room-temperature solid-state maser is highly desirable, but under such conditions the lifetimes of emitters (usually electron spins) are usually too short (~ns) for population inversion. The only room-temperature solid-state maser is based on a pentacene-doped p-terphenyl crystal, which has long spin lifetime (~0.1 ms). This maser, however, ope…
We demonstrate a cavity-enhanced room-temperature magnetic field sensor based on nitrogen-vacancy centers in diamond. Magnetic resonance is detected using absorption of light resonant with the 1042 nm spin-singlet transition. The diamond is placed in an external optical cavity to enhance the absorption, and significant absorption is observed even at room temperature. We demonstrate a magnetic field sensitivity of 2.5 nT/sqrt(Hz), and project a photon shot-noise-limited sensitivity of 70 pT/sqrt(Hz) for a few mW of infrared light, and a quantum projection-noise-limited sensitivity of 250 fT/sqr…
We report the storage and retrieval of single photons, via a quantum memory, in the optical phonons of room-temperature bulk diamond. The THz-bandwidth heralded photons are generated by spontaneous parametric downconversion and mapped to phonons via a Raman transition, stored for a variable delay, and released on demand. The second-order correlation of the memory output is $g^{(2)}(0) = 0.65 \pm 0.07$, demonstrating preservation of non-classical photon statistics throughout storage and retrieval. The memory is low-noise, high-speed and broadly tunable; it therefore promises to be a versatile l…
A recent experiment [K. C. Lee et al., Science 334, 1253 (2011)] succeeded in detecting entanglement between two macroscopic specks of diamonds, separated by a macroscopic distance, at room temperature. This impressive results is a further confirmation of the validity of quantum theory in (at least parts of) the mesoscopic and macroscopic domain, and poses a challenge to collapse models, which predict a violation of the quantum superposition principle, which is the bigger the larger the system. We analyze the experiment in the light of such models. We will show that the bounds placed by experi…
Nitrogen-vacancy (NV) centres in diamond are appealing nano-scale quantum sensors for temperature, strain, electric fields and, most notably, for magnetic fields. However, the cryogenic temperatures required for low-noise single-shot readout that have enabled the most sensitive NV-magnetometry reported to date, are impractical for key applications, e.g. biological sensing. Overcoming the noisy readout at room-temperature has until now demanded repeated collection of fluorescent photons, which increases the time-cost of the procedure thus reducing its sensitivity. Here we show how machine learn…
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…
Diamond is a proven solid-state platform for spin-based quantum technology. The nitrogen-vacancy (NV) center in diamond has been used to realize small-scale quantum information processing (QIP) and quantum sensing under ambient conditions. A major barrier in the development of large-scale QIP in diamond is the connection of NV spin registers by a quantum bus at room temperature. Given that diamond is expected to be an ideal spin transport material, the coherent transport of spin directly between the spin registers offers a potential solution. Yet, there has been no demonstration of spin transp…
The sensitivity of a practical quantum magnetometer is challenged by both inhomogeneous coupling between sensors and environment and errors in quantum control. Based on the physical criteria of modern quantum sensing, we present a robust and effective composite-pulse for high fidelity operation against inhomogeneous broadening of sensor and control errors via optimized modulation of control field. Such a technique is verified on nitrogen-vacancy (NV) center in diamond to keep almost perfect operation up to a detuning as larger as $110\%$. The sensitivity of the magnetometer with NV center ense…
Entanglement is the central yet fleeting phenomena of quantum physics. Once being considered a peculiar counter-intuitive property of quantum theory it has developed into the most central element of quantum technology providing speed up to quantum computers, a path towards long distance quantum cryptography and increased sensitivity in quantum metrology. Consequently, there have been a number of experimental demonstration of entanglement between photons, atoms, ions as well as solid state systems like spins or quantum dots, superconducting circuits and macroscopic diamond. Here we experimental…
Quantum memories provide intermediate storage of quantum information until it is needed for the next step of a quantum algorithm or a quantum communication process. Relevant figures of merit are therefore the fidelity with which the information can be written and retrieved, the storage time, and also the speed of the read-write process. Here, we present experimental data on a quantum memory consisting of a single $^{13}$C nuclear spin that is strongly coupled to the electron spin of a nitrogen-vacancy (NV) center in diamond. The strong hyperfine interaction of the nearest-neighbor carbon resul…
We demonstrate electrical detection of the $^{14}$N nuclear spin coherence of NV centers at room temperature. Nuclear spins are candidates for quantum memories in quantum-information devices and quantum sensors, and hence the electrical detection of nuclear spin coherence is essential to develop and integrate such quantum devices. In the present study, we used a pulsed electrically detected electron-nuclear double resonance technique to measure the Rabi oscillations and coherence time ($T_2$) of $^{14}$N nuclear spins in NV centers at room temperature. We observed $T_2 \approx$ 0.9 ms at room …
A defect in diamond with millisecond-scale spin relaxation time at room temperature
Princeton University（普林斯顿大学）；University of California, Santa Barbara（加州大学圣塔芭芭拉分校）；US Naval Research Laboratory（美国海军研究实验室）；University of North Carolina at Chapel Hill（北卡罗来纳大学教堂山分校）；University of Iowa（爱荷华大学）
Cavity quantum electrodynamics (C-QED) effects, such as Rabi splitting, Rabi oscillations and superradiance, have been demonstrated with nitrogen vacancy center spins in diamond in microwave resonators at cryogenic temperature. In this article we explore the possibility to realize strong collective coupling and the resulting C-QED effects with ensembles of spins at room temperature. Thermal excitation of the individual spins by the hot environment leads to population of collective Dicke states with low symmetry and a reduced collective spin-microwave field coupling. However, we show with simul…
Nuclear spins support long lived quantum coherence due to weak coupling to the environment, but are difficult to rapidly control using nuclear magnetic resonance (NMR) as a result of the small nuclear magnetic moment. We demonstrate a fast ~ 500 ns nuclear spin phase gate on a 14N nuclear spin qubit intrinsic to a nitrogen-vacancy (NV) center in diamond. The phase gate is enabled by the hyperfine interaction and off-resonance driving of electron spin transitions. Repeated applications of the phase gate bang-bang decouple the nuclear spin from the environment, locking the spin state for up to ~…
We report the observation of room-temperature superradiance from single, highly luminescent diamond nanocrystals with spatial dimensions much smaller than the wavelength of light, and each containing a large number (~10^3) of embedded nitrogen-vacancy (NV) centres. After excitation of the nanodiamonds with an off-resonant, green laser pulse, we observe i) ultrafast radiative lifetimes down to ~ 1 ns, and ii) super-Poissonian photon bunching in the autocorrelation function of the light emitted from the fastest nanodiamonds. We explain our findings with a detailed theoretical model based on coll…
Strongly-correlated quantum many-body systems exhibits a variety of exotic phases with long-range quantum correlations, such as spin liquids and supersolids. Despite the rapid increase in computational power of modern computers, the numerical simulation of these complex systems becomes intractable even for a few dozens of particles. Feynman's idea of quantum simulators offers an innovative way to bypass this computational barrier. However, the proposed realizations of such devices either require very low temperatures (ultracold gases in optical lattices, trapped ions, superconducting devices) …
Phosphorus-doped diamond is relevant for applications in sensing, optoelectronics and quantum photonics, since the unique optical properties of color centers in diamond can be combined with the n-type conductivity attained by the inclusion of phosphorus. Here, we investigate the photoluminescence signal of the nitrogen-vacancy and silicon-vacancy color centers in phosphorus-doped diamond as a function of temperature starting from ambient conditions up to about 100$^\circ$ Celsius, focusing on the zero-phonon line (ZPL). We find that the wavelength and width of the ZPL of the two color centers …
The maser, older sibling of the laser, has been confined to relative obscurity due to its reliance on cryogenic refrigeration and high-vacuum systems. Despite this it has found application in deep-space communications and radio astronomy due to its unparalleled performance as a low-noise amplifier and oscillator. The recent demonstration of a room-temperature solid- state maser exploiting photo-excited triplet states in organic pentacene molecules paves the way for a new class of maser that could find applications in medicine, security and sensing, taking advantage of its sensitivity and low n…
We report bulk, room-temperature hyperpolarization of 13C nuclear spins observed via high-field nuclear magnetic resonance (NMR). The hyperpolarization is achieved by optical pumping (OP) of nitrogen vacancy defect centers in diamond accompanied by dynamic nuclear polarization (DNP). The technique harnesses the large optically-induced spin polarization of NV- centers at room temperature, which is many orders of magnitude greater than thermal equilibrium polarization and typically achievable only at sub-Kelvin temperatures. Transfer of the spin polarization to the 13C nuclear spins is accomplis…
The diamond nitrogen-vacancy (NV) center is a leading platform for quantum information science due to its optical addressability and room-temperature spin coherence. However, measurements of the NV center's spin state typically require averaging over many cycles to overcome noise. Here, we review several approaches to improve the readout performance and highlight future avenues of research that could enable single-shot electron-spin readout at room temperature.
Ultra-thin layers of liquids on a surface behave differently from bulk liquids due to liquid-surface interactions. Some examples are significant changes in diffusion properties and the temperature at which the liquid-solid phase transition takes place. Indeed, molecular dynamics simulations suggest that thin layers of water on a diamond surface may remain solid even well above room temperature. However, because of the small volumes that are involved, it is exceedingly difficult to examine these phenomena experimentally with current technologies. In this context, shallow NV centers promise a hi…
Dynamic nuclear polarization via contact with electronic spins has emerged as an attractive route to enhance the sensitivity of nuclear magnetic resonance (NMR) beyond the traditional limits imposed by magnetic field strength and temperature. Among the various alternative implementations, the use of nitrogen vacancy (NV) centers in diamond - a paramagnetic point defect whose spin can be optically polarized at room temperature - has attracted widespread attention, but applications have been hampered by the need to align the NV axis with the external magnetic field. Here we overcome this hurdle …
Hyperpolarisation at room temperature is one of the most important research fields in order to improve liquid, gas or nanoparticle tracer for Magnetic Resonance Imaging (MRI) in medical applications. In this paper we utilize nuclear magnetic resonance (NMR) to investigate the hyperpolarisation effect of negatively charged nitrogen vacancy (NV) centres on carbon-13 nuclei and their spin diffusion in a diamond single crystal close to the excited state level anti crossing (ESLAC) around 50 mT. Whereas the electron spins of the NV centre can be easily polarized in its m = 0 ground state at room te…
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…
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…
Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR)…
The development of a robust light source that emits one photon at a time is an outstanding challenge in quantum science and technology. Here, at the transition from many to single photon optical communication systems, fully quantum mechanical effects may be utilized to achieve new capabilities, most notably perfectly secure communication via quantum cryptography. Practical implementations place stringent requirements on the device properties, including stable photon generation, room temperature operation, and efficient extraction of many photons. Single photon light emitting devices based on f…
We present the experimental reconstruction of the Wigner function of an individual electronic spin qubit associated with a nitrogen-vacancy (NV) center in diamond at room temperature. This spherical Wigner function contains the same information as the density matrix for arbitrary spin systems. As an example, we exactly characterize the quantum state of a single qubit undergoing a nearly pure dephasing process by Wigner function. The fidelities and purities during this process are extracted from the experimental reconstructed Wigner functions, whose dynamics agree with the theoretical predictio…
Realization of devices based on quantum laws might lead to building processors that outperform their classical analogues and establishing unconditionally secure communication protocols. Solids do usually present a serious challenge to quantum coherence. However, owing to their spin-free lattice and low spin orbit coupling, carbon materials and particularly diamond are suitable for hosting robust solid state quantum registers. We show that scalable quantum logic elements can be realized by exploring long range magnetic dipolar coupling between individually addressable single electron spins asso…
A simple, room-temperature, cavity- and vacuum-free interface for a photon-matter interaction is implemented. In the experiment, a heralded single photon generated by the process of spontaneous parametric down-conversion is absorbed by an ensemble of nitrogen-vacancy color centers. The broad absorption spectrum associated with the phonon sideband solves the mismatch problem of a narrow absorption bandwidth in a typical atomic medium and broadband spectrum of quantum light. The heralded single photon source is tunable in the spectral range 452-575 nm, which overlaps well with the absorption spe…
We present an experimental and theoretical study of electronic spin decoherence in ensembles of nitrogen-vacancy (NV) color centers in bulk high-purity diamond at room temperature. Under appropriate conditions, we find ensemble NV spin coherence times (T_2) comparable to that of single NVs, with T_2 > 600 microseconds for a sample with natural abundance of 13C and paramagnetic impurity density ~10^15 cm^(-3). We also observe a sharp decrease of the coherence time with misalignment of the static magnetic field relative to the NV electronic spin axis, consistent with theoretical modeling of NV c…
Nuclear spins in solids exhibit long coherence times due to the small nuclear gyromagnetic ratio. This weak environmental coupling comes at the expense of slow quantum gate operations, which should be as fast as possible for many applications in quantum information processing and sensing. In this work, we use nitrogen-vacancy (NV) centers in diamond to probe the nuclear spins within dark paramagnetic nitrogen defects (P1 centers) in the diamond lattice. The gyromagnetic ratio of the P1 nuclear spin is augmented by hyperfine coupling to the electron spin, resulting in greatly enhanced coupling …
Color centers in diamond are very promising candidates among the possible realizations for practical single-photon sources because of their long-time stable emission at room temperature. The popular nitrogen-vacancy center shows single-photon emission, but within a large, phonon-broadened spectrum (~100nm), which strongly limits its applicability for quantum communication. By contrast, Ni-related centers exhibit narrow emission lines at room temperature. We present investigations on single color centers consisting of Ni and Si created by ion implantation into single crystalline IIa diamond. We…
We experimentally demonstrate room-temperature storage of quantum entanglement using two nuclear spins weakly coupled to the electronic spin carried by a single nitrogen-vacancy center in diamond. We realize universal quantum gate control over the three-qubit spin system and produce entangled states encoded within the decoherence-free subspace of the two nuclear spins. By injecting arbitrary collective noise, we demonstrate that the decoherence-free entangled state has coherence time longer than that of other entangled states by an order of magnitude in our experiment.
Nuclear spins nearby nitrogen-vacancy (NV) centers in diamond are excellent quantum memory for quantum computing and quantum sensing, but are difficult to be initialized due to their weak interactions with the environment. Here we propose and demonstrate a magnetic-field-independent, deterministic and highly efficient polarization scheme by introducing chopped laser pulses into the double-resonance initialization method. With this method, we demonstrate initialization of single-nuclear-spin approaching $98.1\%$ and a $^{14}N$-$^{13}C$ double-nuclear-spin system approaching $96.8\%$ at room tem…
Single-crystal diamond cavity optomechanical devices are a promising example of a hybrid quantum system: by coupling mechanical resonances to both light and electron spins, they can enable new ways for photons to control solid state qubits. However, realizing cavity optomechanical devices from high quality diamond chips has been an outstanding challenge. Here we demonstrate single-crystal diamond cavity optomechanical devices that can enable photon-phonon-spin coupling. Cavity optomechanical coupling to $2\,\text{GHz}$ frequency ($f_\text{m}$) mechanical resonances is observed. In room tempera…
Color centers in diamond as single photon emitters, are leading candidates for future quantum devices due to their room temperature operation and photostability. The recently discovered chromium related centers are particularly attractive since they possess narrow bandwidth emission and a very short lifetime. In this paper we investigate the fabrication methodologies to engineer these centers in monolithic diamond. We show that the emitters can be successfully fabricated by ion implantation of chromium in conjunction with oxygen or sulfur. Furthermore, our results indicate that the background …
A fundamental result of quantum mechanics is that the fluctuations of a bosonic field are given by its temperature $T$. An electromagnetic mode with frequency $ω$ in the microwave band has a significant thermal photon occupation at room temperature according to the Bose-Einstein distribution $\bar{n} = k_BT / \hbarω$. The room temperature thermal state of a 3 GHz mode, for example, is characterized by a mean photon number $\bar{n} \sim 2000$ and variance $Δn^2 \approx \bar{n}^2$. This thermal variance sets the measurement noise floor in applications ranging from wireless communications to posi…
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 …
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…
Nitrogen-Vacancy (NV) color centers in diamond have emerged as promising quantum solid-state systems, with applications ranging from quantum information processing to magnetic sensing. One of the most useful properties of NVs is the ability to read their ground-state spin projection optically at room temperature. This work provides a theoretical analysis of Purcell enhanced NV optical coupling, through which we find optimal parameters for maximal Signal to Noise Ratio (SNR) of the optical spin-state readout. We conclude that a combined increase in spontaneous emission (through Purcell enhancem…
Deterministic coupling of single solid-state emitters to nanocavities is the key for integrated quantum information devices. We here fabricate a photonic crystal cavity around a preselected single silicon-vacancy color center in diamond and demonstrate modification of the emitters internal population dynamics and radiative quantum efficiency. The controlled, room-temperature cavity coupling gives rise to a resonant Purcell enhancement of the zero-phonon transition by a factor of 19, coming along with a 2.5-fold reduction of the emitter's lifetime.
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 introduce an alternate route to dynamically polarize the nuclear spin host of nitrogen-vacancy (NV) centers in diamond. Our approach articulates optical, microwave and radio-frequency pulses to recursively transfer spin polarization from the NV electronic spin. Using two complementary variants of the same underlying principle, we demonstrate nitrogen nuclear spin initialization approaching 80% at room temperature both in ensemble and single NV centers. Unlike existing schemes, our approach does not rely on level anti-crossings and is thus applicable at arbitrary magnetic fields. This versat…
