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Microscopic studies on thin film superconductors play an important role for probing non-equilibrium phase transitions and revealing dynamics at the nanoscale. However, magnetic sensors with nanometer scale spatial and picosecond temporal resolution are essential for exploring these. Here, we present an all-optical, microwave-free method, that utilizes the negatively charged nitrogen-vacancy (NV) center in diamond as a non-invasive quantum sensor and enables the spatial detection of the Meissner state in a superconducting thin film. We place an NV implanted diamond membrane on a superconducting LSCO thin film. The strong B-field dependence of the NV photoluminescence (PL) allows us to investigate the Meissner screening in LSCO under an externally applied magnetic field in a non-resonant manner.

The ability to perform nanoscale electric field imaging of elementary charges at ambient temperatures will have diverse interdisciplinary applications. While the nitrogen-vacancy (NV) center in diamond is capable of high-sensitivity electrometry, demonstrations have so far been limited to macroscopic field features or detection of single charges internal to diamond itself. In this work we greatly extend these capabilities by using a shallow NV center to image the electric field of a charged atomic force microscope tip with nanoscale resolution. This is achieved by measuring Stark shifts in the NV spin-resonance due to AC electric fields. To achieve this feat we employ for the first time, the integration of Qdyne with scanning quantum microscopy. We demonstrate near single charge sensitivity of $\eta_e = 5.3$ charges/$\sqrt{\text{Hz}}$, and sub-charge detection ($0.68e$). This proof-of-concept experiment provides the motivation for further sensing and imaging of electric fields using NV centers in diamond.

The nitrogen-vacancy (NV) center is a well utilized system for quantum technology, in particular quantum sensing and microscopy. Fully employing the NV center's capabilities for metrology requires a strong understanding of the behavior of the NV center with respect to changing temperature. Here, we probe the NV electronic spin density as the surrounding crystal temperature changes from 10 K to 700 K by examining its $^{13}$C hyperfine interactions. These results are corroborated with \textit{ab initio} calculations and demonstrate that the change in hyperfine interaction is small and dominated by a change in the hybridization of the orbitals constituting the spin density. Thus indicating that the defect and local crystal geometry is returning towards an undistorted structure at higher temperature.

Single photon emitters in silicon carbide (SiC) are attracting attention as quantum photonic systems. However, to achieve scalable devices it is essential to generate single photon emitters at desired locations on demand. Here we report the controlled creation of single silicon vacancy ($V_{Si}$) centres in 4H-SiC using laser writing without any post-annealing process. Due to the aberration correction in the writing apparatus and the non-annealing process, we generate single $V_{Si}$ centres with yields up to 30%, located within about 80 nm of the desired position in the transverse plane. We also investigated the photophysics of the laser writing $V_{Si}$ centres and conclude that there are about 16 photons involved in the laser writing $V_{Si}$ centres process. Our results represent a powerful tool in fabrication of single $V_{Si}$ centres in SiC for quantum technologies and provide further insights into laser writing defects in dielectric materials.

Quantum sensors have recently achieved to detect the magnetic moment of few or single nuclear spins and measure their magnetic resonance (NMR) signal. However, the spectral resolution, a key feature of NMR, has been limited by relaxation of the sensor to a few kHz at room temperature. The spectral resolution of NMR signals from single nuclear spins can be improved by, e.g., using quantum memories, however at the expense of sensitivity. Classical signals on the other hand can be measured with exceptional spectral resolution by using continuous measurement techniques, without compromising sensitivity. To apply these techniques to single-spin NMR, it is critical to overcome the impact of back action inherent of quantum measurements. Here we report sequential weak measurements on a single $^{13}$C nuclear spin. The back-action of repetitive weak measurements causes the spin to undergo a quantum dynamics phase transition from coherent trapping to coherent oscillation. Single-spin NMR at room-temperature with a spectral resolution of 3.8 Hz is achieved. These results enable the use of measurement-correlation schemes for the detection of very weakly coupled single spins., Comment: Article: 16 pages, 4 figures Supplementary: 23 pages, 9 figures

The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the transfer protocol suggest slower molecular diffusion near the diamond surface compared to that in bulk, an observation consistent with present models of the microscopic structure of a fluid close to a solid interface., Comment: 7 pages, 4 figures

We demonstrate super-resolution imaging of single rare-earth emitting centers, namely, trivalent cerium, in yttrium aluminum garnet (YAG) crystals by means of stimulated emission depletion (STED) microscopy. The achieved all-optical resolution is $\approx$ 80nm. Similar results were obtained on H3 color centers in diamond with resolution of $\approx$ 60nm. In both cases, STED resolution is improving slower than the inverse square-root of the depletion beam intensity. This is caused by excited state absorption (ESA) and interaction of the emitter with non-fluorescing crystal defects in its near surrounding.

The negatively-charged nitrogen-vacancy (NV) center in diamond has been shown recently as an excellent sensor for external spins. Nevertheless, their optimum engineering in the near-surface region still requires quantitative knowledge in regard to their activation by vacancy capture during thermal annealing. To this aim, we report on the depth profiles of near-surface helium-induced NV centers (and related helium defects) by step-etching with nanometer resolution. This provides insights into the efficiency of vacancy diffusion and recombination paths concurrent to the formation of NV centers. It was found that the range of efficient formation of NV centers is limited only to approximately $10$ to $15\,$nm (radius) around the initial ion track of irradiating helium atoms. Using this information we demonstrate the fabrication of nanometric-thin ($\delta$) profiles of NV centers for sensing external spins at the diamond surface based on a three-step approach, which comprises (i) nitrogen-doped epitaxial CVD diamond overgrowth, (ii) activation of NV centers by low-energy helium irradiation and thermal annealing, and (iii) controlled layer thinning by low-damage plasma etching. Spin coherence times (Hahn echo) ranging up to $50\,$ $\mu$s are demonstrated at depths of less than $5\,$nm in material with $1.1\,\%$ of $^{13}$C (depth estimated by spin relaxation (T$_1$) measurements). At the end, the limits of the helium irradiation technique at high ion fluences are also experimentally investigated., Comment: 27 pages, 10 figures

Understanding the dynamics of molecules adsorbed to surfaces or confined to small volumes is a matter of increasing scientific and technological importance. Here, we demonstrate a pulse protocol using individual paramagnetic nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H spins from organic molecules located a few nanometers from the diamond surface. The protocol records temporal correlations among the interacting 1H spins, and thus is sensitive to the local system dynamics via its impact on the nuclear spin relaxation and interaction with the NV. We are able to gather information on the nanoscale rotational and translational diffusion dynamics by carefully analyzing the time dependence of the NMR signal. Applying this technique to various liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5 nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be adapted to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding.

Nitrogen impurities help to stabilize the negatively-charged-state of NV$^-$ in diamond, whereas magnetic fluctuations from nitrogen spins lead to decoherence of NV$^-$ qubits. It is not known what donor concentration optimizes these conflicting requirements. Here we used 10-MeV $^{15}$N$^{3+}$ ion implantation to create NV$^-$ in ultrapure diamond. Optically detected magnetic resonance of single centers revealed a high creation yield of $40\pm3$% from $^{15}$N$^{3+}$ ions and an additional yield of $56\pm3$% from $^{14}$N impurities. High-temperature anneal was used to reduce residual defects, and charge stable NV$^-$, even in a dilute $^{14}$N impurity concentration of 0.06 ppb were created with long coherence times.

Rare-earth-doped crystals are excellent hardware for quantum storage of optical information. Additional functionality of these materials is added by their waveguiding properties allowing for on-chip photonic networks. However, detection and coherent properties of rare-earth single-spin qubits have not been demonstrated so far. Here, we present experimental results on high-fidelity optical initialization, effcient coherent manipulation, and optical readout of a single electron spin of Ce$^{3+}$ ion in a YAG crystal. Under dynamic decoupling, spin coherence lifetime reaches $T_2$=2 ms and is almost limited by the measured spin-lattice relaxation time $T_1$=3.8 ms. Strong hyperfine coupling to aluminium nuclear spins suggests that cerium electron spins can be exploited as an interface between photons and long-lived nuclear spin memory. Combined with high brightness of Ce$^{3+}$ emission and a possibility of creating photonic circuits out of the host material, this makes cerium spins an interesting option for integrated quantum photonics., Comment: 10 pages, 4 figures

Hybrid quantum systems seek to combine the strength of its constituents to master the fundamental conflicting requirements of quantum technology: fast and accurate systems control together with perfect shielding from the environment, including the measurements apparatus, to achieve long quantum coherence. Excellent examples for hybrid quantum systems are heterogeneous spin systems where electron spins are used for readout and control while nuclear spins are used as long-lived quantum bits. Here we show that joint initialization, projective readout and fast local and non-local gate operations are no longer conflicting requirements in those systems, even under ambient conditions. We demonstrate high-fidelity initialization of a whole spin register (99 %) and single-shot readout of multiple individual nuclear spins by using the ancillary electron spin of a nitrogen-vacancy defect in diamond. Implementation of a novel non-local gate generic to our hybrid electron-nuclear quantum register allows to prepare entangled states of three nuclear spins, with fidelities exceeding 85 %. An important tool for scalable quantum computation is quantum error correction. Combining, for the first time, optimal-control based error avoidance with error correction, we realize a three-qubit phase-flip error correction algorithm. Utilizing optimal control, all of the above algorithms achieve fidelities approaching fault tolerant quantum operation, thus paving the way to large scale integrations. Our techniques can be used to improve scaling of quantum networks relying on diamond spins, phosphorous in silicon or other spin systems like quantum dots, silicon carbide or rare earth ions in solids., Comment: V2: Added note to simultaneous related work arXiv:1309.5452

Spins of negatively charged nitrogen-vacancy (NV$^-$) defects in diamond are among the most promising candidates for solid-state qubits. The fabrication of quantum devices containing these spin-carrying defects requires position-controlled introduction of NV$^-$ defects having excellent properties such as spectral stability, long spin coherence time, and stable negative charge state. Nitrogen ion implantation and annealing enable the positioning of NV$^-$ spin qubits with high precision, but to date, the coherence times of qubits produced this way are short, presumably because of the presence of residual radiation damage. In the present work, we demonstrate that a high temperature annealing at 1000$^\circ$C allows 2 millisecond coherence times to be achieved at room temperature. These results were obtained for implantation-produced NV$^-$ defects in a high-purity, 99.99% $^{12}$C enriched single crystal chemical vapor deposited diamond. We discuss these remarkably long coherence times in the context of the thermal behavior of residual defect spins. [Published in Physical Review B {\bf{88}}, 075206 (2013)]

We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spin. We estimate a sensitivity down to $\approx 14$ electron spins detected within 10 s, using a single NV defect hosted in a 10-nm-size ND. These results pave the way towards $T_1$-based nanoscale imaging of the spin density in biological samples., Comment: Main text with 4 figures together with supplemental information

We demonstrate high resolution scanning fluorescence resonance energy transfer 10 microscopy between a single nitrogen-vacancy center as donor and graphene as acceptor. 11 Images with few nanometer resolution of single and multilayer graphene structures were 12 attained. An energy transfer efficiency of 30% at distances of 10nm between a single 13 defect and graphene was measured. Further the energy transfer distance dependence of 14 the nitrogen-vacancy center to graphene was measured to show the predicted d-4 15 dependence. Our studies pave the way towards a diamond defect center based versatile 16 single emitter scanning microscope., Comment: 12 pages, 3 figures

Magnetic resonance detection is one of the most important tools used in life-sciences today. However, as the technique detects the magnetization of large ensembles of spins it is fundamentally limited in spatial resolution to mesoscopic scales. Here we detect the natural fluctuations of nanoscale spin ensembles at ambient temperatures by measuring the decoherence rate of a single quantum spin in response to introduced extrinsic target spins. In our experiments 45 nm nanodiamonds with single nitrogen-vacancy (NV) spins were immersed in solution containing spin 5/2 Mn^2+ ions and the NV decoherence rate measured though optically detected magnetic resonance. The presence of both freely moving and accreted Mn spins in solution were detected via significant changes in measured NV decoherence rates. Analysis of the data using a quantum cluster expansion treatment of the NV-target system found the measurements to be consistent with the detection of ~2,500 motionally diffusing Mn spins over an effective volume of (16 nm)^3 in 4.2 s, representing a reduction in target ensemble size and acquisition time of several orders of magnitude over state-of-the-art electron spin resonance detection. These measurements provide the basis for the detection of nanoscale magnetic field fluctuations with unprecedented sensitivity and resolution in ambient conditions., Comment: 9 pages, 5 figures

Measuring spins is the corner stone of a variety of analytical techniques including modern magnetic resonance imaging (MRI). The full potential of spin imaging and sensing across length scales is hindered by the achievable signal-to-noise in inductive detection schemes. Here we show that a proximal Nitrogen-Vacancy (NV) ensemble serves as a precision sensing array. Monitoring its quantum relaxation enables sensing of freely diffusing and unperturbed magnetic ions in a microfluidic device. Multiplexed CCD acquisition and an optimized detection scheme enable direct spin noise imaging under ambient conditions with experimental sensitivities down to 1000 statistically polarized spins, of which only 35 ions contribute to a net magnetization, and 20 s acquisition time. We also demonstrate imaging of spin labeled cellular structures with spatial resolutions below 500 nm. Our study marks a major step towards sub-{\mu}m imaging magnetometry and applications in microanalytics, material and life sciences., Comment: 11 pages, 4 figures

The nitrogen-vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV-) or neutral (NV0), with photo induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination in dependence of the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. Results of this work are the steady state NV- population, which was found to be always < 75% for 450 to 610 nm excitation wavelength, the relative absorption cross-section of NV- for 540 to 610 nm, and the energy of the NV- ground state of 2.6 eV below the conduction band. These results will help to further understand the photo-physics of the NV centre., Comment: 9 pages, 7 figures

In this paper, we study the photoinduced switching of the nitrogen-vacancy (NV) center between two different charge states - negative (NV-) and neutral (NV0) at liquid helium temperature. The conversion of NV- to NV0 on a single defect is experimentally proven and its rate scales quadratically with power under resonant excitation. In addition, we found that resonant excitation of the neutral NV changes the charge state, recovering its negative configuration. This type of conversion significantly improves spectral stability of NV- defect and allows high fidelity initialization of the spin qubit. A possible mechanism for ionization and recovery of the NV- defect is discussed. This study provides better understanding of the charge dynamics of the NV center, which is relevant for quantum information processing based on NV defect in diamond., Comment: 5 pages, 4 figures

The ground state spin of the negatively charged nitrogen-vacancy center in diamond has many exciting applications in quantum metrology and solid state quantum information processing, including magnetometry, electrometry, quantum memory and quantum optical networks. Each of these applications involve the interaction of the spin with some configuration of electric, magnetic and strain fields, however, to date there does not exist a detailed model of the spin's interactions with such fields, nor an understanding of how the fields influence the time-evolution of the spin and its relaxation and inhomogeneous dephasing. In this work, a general solution is obtained for the spin in any given electric-magnetic-strain field configuration for the first time, and the influence of the fields on the evolution of the spin is examined. Thus, this work provides the essential theoretical tools for the precise control and modeling of this remarkable spin in its current and future applications., Comment: 14 pages, 8 figures

Quantum non-locality has been experimentally investigated by testing different forms of Bell's inequality, yet a loophole-free realization has not been achieved up to now. Much less explored are temporal Bell inequalities, which are not subject to the locality assumption, but impose a constrain on the system's time-correlations. In this paper, we report on the experimental violation of a temporal Bell's inequality using a nitrogen vacancy defect (NV) in diamond and provide a novel quantitative test of quantum coherence. We therefore present a new technique to initialize the electronic state of the NV with high fidelity, a necessary requirement for reliable quantum information processing and/or the implementation of protocols for quantum metrology., Comment: 4 pages, 3 figures

We demonstrate electrical control of the single photon emission spectrum from chromium-based colour centres implanted in monolithic diamond. Under an external electric field the tunability range is typically three orders of magnitude larger than the radiative linewidth and at least one order of magnitude larger than the observed linewidth. The electric and magnetic field dependence of luminescence gives indications on the inherent symmetry and we propose Cr-X or X-Cr-Y type noncentrosymmetric atomic configurations as most probable candidates for these centres.

The nitrogen-vacancy (NV) center in diamond is supposed to be a building block for quantum computing and nanometer scale metrology at ambient conditions. Therefore, precise knowledge of its quantum states is crucial. Here, we experimentally show that under usual operating conditions the NV exists in an equilibrium of two charge states (70% in the expected negative (NV-) and 30% in the neutral one (NV0)). Projective quantum non-demolition measurement of the nitrogen nuclear spin enables the detection even of the additional, optically inactive state. The nuclear spin can be coherently driven also in NV0 (T1 ~ 90 ms and T2 ~ 6 micro-s)., Comment: 4 pages, 3 figures

We investigate the effect of surface termination on the charge state of nitrogen vacancy centers, which have been ion-implanted few nanometers below the surface of diamond. We find that, when changing the surface termination from oxygen to hydrogen, previously stable NV- centers convert into NV0 and, subsequently, into an unknown non-fluorescent state. This effect is found to depend strongly on the implantation dose. Simulations of the electronic band structure confirm the dissappearance of NV- in the vicinity of the hydrogen-terminated surface. The band bending, which induces a p-type surface conductive layer leads to a depletion of electrons in the nitrogen vacancies close to the surface. Therefore, hydrogen surface termination provides a chemical way for the control of the charge state of nitrogen-vacancy centers in diamond. Furthermore, it opens the way to an electrostatic control of the charge state with the use of an external gate electrode., Comment: 12 pages, 4 figures

Optical detection of single defect centers in the solid state is a key element of novel quantum technologies. This includes the generation of single photons and quantum information processing. Unfortunately the brightness of such atomic emitters is limited. Therefore we experimentally demonstrate a novel and simple approach that uses off-the-shelf optical elements. The key component is a solid immersion lens made of diamond, the host material for single color centers. We improve the excitation and detection of single emitters by one order of magnitude, as predicted by theory., Comment: 10 pages, 3 figures

Two proof-of-principle experiments towards T1-limited magnetic resonance imaging with NV centers in diamond are demonstrated. First, a large number of Rabi oscillations is measured and it is demonstrated that the hyperfine interaction due to the NV's 14N can be extracted from the beating oscillations. Second, the Rabi beats under V-type microwave excitation of the three hyperfine manifolds is studied experimentally and described theoretically., Comment: 6 pages, 8 figures

We report the realization of a quantum circuit in which an ensemble of electronic spins is coupled to a frequency tunable superconducting resonator. The spins are Nitrogen-Vacancy centers in a diamond crystal. The achievement of strong coupling is manifested by the appearance of a vacuum Rabi splitting in the transmission spectrum of the resonator when its frequency is tuned through the NV center electron spin resonance., Comment: 4 pages, 3 figures

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 associated with separate color centers in diamond. Strong distance dependence of coupling was used to characterize the separation of single qubits 98 A with unprecedented accuracy (3 A) close to a crystal lattice spacing. Our demonstration of coherent control over both electron spins, conditional dynamics, selective readout as well as switchable interaction, opens the way towards a room temperature solid state scalable quantum register. Since both electron spins are optically addressable, this solid state quantum device operating at ambient conditions provides a degree of control that is currently available only for atomic systems., Comment: original submitted version of the manuscript

We perform a review of various approaches to the implementation of quantum memories, with an emphasis on activities within the quantum memory sub-project of the EU Integrated Project "Qubit Applications". We begin with a brief overview over different applications for quantum memories and different types of quantum memories. We discuss the most important criteria for assessing quantum memory performance and the most important physical requirements. Then we review the different approaches represented in "Qubit Applications" in some detail. They include solid-state atomic ensembles, NV centers, quantum dots, single atoms, atomic gases and optical phonons in diamond. We compare the different approaches using the discussed criteria., Comment: 22 pages, 12 figures

In drug discovery research there is a clear and urgent need for non-invasive detection of cell membrane ion channel operation with wide-field capability. Existing techniques are generally invasive, require specialized nano structures, or are only applicable to certain ion channel species. We show that quantum nanotechnology has enormous potential to provide a novel solution to this problem. The nitrogen-vacancy (NV) centre in nano-diamond is currently of great interest as a novel single atom quantum probe for nanoscale processes. However, until now, beyond the use of diamond nanocrystals as fluorescence markers, nothing was known about the quantum behaviour of a NV probe in the complex room temperature extra-cellular environment. For the first time we explore in detail the quantum dynamics of a NV probe in proximity to the ion channel, lipid bilayer and surrounding aqueous environment. Our theoretical results indicate that real-time detection of ion channel operation at millisecond resolution is possible by directly monitoring the quantum decoherence of the NV probe. With the potential to scan and scale-up to an array-based system this conclusion may have wide ranging implications for nanoscale biology and drug discovery., Comment: 7 pages, 6 figures

In this paper, we study the optical properties of single defects emitting in the near infrared in nanodiamonds at liquid helium temperature. The nanodiamonds are synthesized using a microwave chemical vapor deposition method followed by nickel implantation and annealing. We show that single defects exhibit several striking features at cryogenic temperature: the photoluminescence is strongly concentrated into a sharp zero-phonon line in the near infrared, the radiative lifetime is in the nanosecond range and the emission is perfectly linearly polarized. The spectral stability of the defects is then investigated. An optical resonance linewidth of 4 GHz is measured using resonant excitation on the zero-phonon line. Although Fourier-transform limited emission is not achieved, our results show that it might be possible to use consecutive photons emitted in the near infrared by single defects in diamond nanocrystals to perform two photon interference experiments, which are at the heart of linear quantum computing protocols., Comment: 12pages, 5 figures

Precise readout of spin states is crucial for any approach towards physical realization of a spin-based quantum computer and for magnetometry with single spins. Here, we report a new method to strongly improve the optical readout fidelity of electron spin states associated with single nitrogen-vacancy (NV) centers in diamond. The signal-to-noise ratio is enhanced significantly by performing conditional flip-flop processes between the electron spin and the nuclear spin of the NV center's nitrogen atom. The enhanced readout procedure is triggered by a short preparatory pulse sequence. As the nitrogen nuclear spin is intrinsically present in the system, this method is universally applicable to any nitrogen-vacancy center., Comment: 4 pages with 4 figures, 2 pages of additional material, references added, paragraph added in additional material

In this report, the polarization properties of the photoluminescence emitted by single nitrogen-vacancy (NV) color centers in diamond are investigated using resonant excitation at cryogenic temperature. We first underline that the two excited-state orbital branches are associated with two orthogonal transition dipoles. Using selective excitation of one dipole, we then show that the photoluminescence is partially unpolarized owing to fast relaxation between the two orbitals induced by the thermal bath. This result might be important in the context of the realization of indistinguishable single photons using NV defect in diamond., Comment: 4 pages, 4 figures

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 diamond-based quantum information processing., Comment: 4 pages, 4 figures

The conformational kinetics of enzymes can be reliably revealed when they are governed by Markovian dynamics. Hidden Markov Models (HMMs) are appropriate especially in the case of conformational states that are hardly distinguishable. However, the evolution of the conformational states of proteins mostly shows non-Markovian behavior, recognizable by non-monoexponential state dwell time histograms. The application of a Hidden Markov Model technique to a cyclic system demonstrating semi-Markovian dynamics is presented in this paper and the required extension of the model design is discussed. As standard ranking criteria of models cannot deal with these systems properly, a new approach is proposed considering the shape of the dwell time histograms. We observed the rotational kinetics of a single F1-ATPase alpha3beta3gamma sub-complex over six orders of magnitude of different ATP to ADP and Pi concentration ratios, and established a general model describing the kinetics for the entire range of concentrations. The HMM extension described here is applicable in general to the accurate analysis of protein dynamics., Comment: 23 pages, 11 figures

Color centers in diamond nanocrystals are a new class of fluorescence markers that attract significant interest due to matchless brightness, photostability and biochemical inertness. Fluorescing diamond nanocrystals containing defects can be used as markers replacing conventional organic dye molecules, quantum dots or autofluorescent proteins. They can be applied for tracking and ultrahigh-resolution localization of the single markers. In addition the spin properties of diamond defects can be utilized for novel magneto-optical imaging (MOI) with nanometer resolution. We develop this technique to unravel the details of the rotary motions and the elastic energy storage mechanism of a single biological nanomotor FoF1-ATP synthase. FoF1-ATP synthase is the enzyme that provides the 'chemical energy currency' adenosine triphosphate, ATP, for living cells. The formation of ATP is accomplished by a stepwise internal rotation of subunits within the enzyme. Previously subunit rotation has been monitored by single-molecule fluorescence resonance energy transfer (FRET) and was limited by the photostability of the fluorophores. Fluorescent nanodiamonds advance these FRET measurements to long time scales., Comment: 10 pages, 4 figures

The dynamics of single electron and nuclear spins in a diamond lattice with different 13C nuclear spin concentration is investigated. It is shown that coherent control of up to three individual nuclei in a dense nuclear spin cluster is feasible. The free induction decays of nuclear spin Bell states and single nuclear coherences among 13C nuclear spins are compared and analyzed. Reduction of a free induction decay time T2* and a coherence time T2 upon increase of nuclear spin concentration has been found. For diamond material with depleted concentration of nuclear spin, T2* as long as 30 microseconds and T2 of up to 1.8 ms for the electron spin has been observed. The 13C concentration dependence of T2* is explained by Fermi contact and dipolar interactions with nuclei in the lattice. It has been found that T2 decreases approximately as 1/n, where n is 13C concentration, as expected for an electron spin interacting with a nuclear spin bath., Comment: 4 pages, 4 figures, 1 movie (avi), 1 supplementary material (pdf)

The exciton dynamics on flat (001) rubrene crystal surfaces have been compared with those under confined pyramidal geometry by time-resolved photoluminescence with micrometer spatial resolution. The luminescence spectra can be interpreted in terms of generation of a free and a self-trapped exciton. Their ratio depends significantly on the structural size which we explain by the optical absorption profile of the pyramids in combination with the exciton diffusion constant. For the latter a lower limit of 0.2 cm2/s at 4 K has been estimated. Temperature-dependent decay times reveal activation barriers between free and self-trapped exciton of 3 meV and 14 meV., Comment: 4 pages, 4 figures

We report a versatile method to efficiently polarize single nuclear spins in diamond, which is based on optical pumping of a single NV color center and mediated by a level-anti crossing in its excited state. A nuclear spin polarization higher than 98% is achieved at room temperature for the 15N nuclear spin associated to the NV center, corresponding to $\mu$K effective nuclear spin temperature. We then show simultaneous deterministic initialization of two nuclear spins (13C and 15N) in close vicinity to a NV defect. Such robust control of nuclear spin states is a key ingredient for further scaling up of nuclear-spin based quantum registers in diamond., Comment: 4 pages, 4 figures

Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single Nitrogen-Vacancy color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3E excited state, which is invaluable for the development of diamond-based quantum information processing., Comment: 10 pages, 4 figures

Photon interference among distant quantum emitters is a promising method to generate large scale quantum networks. Interference is best achieved when photons show long coherence times. For the nitrogen-vacancy defect center in diamond we measure the coherence times of photons via optically induced Rabi oscillations. Experiments reveal a close to Fourier transform (i.e. lifetime) limited width of photons emitted even when averaged over minutes. The projected contrast of two-photon interference (0.8) is high enough to envisage the applications in quantum information processing. We report 12 and 7.8 ns excited state lifetime depending on the spin state of the defect., Comment: 9 pages, 4 figures

Confocal time resolved single-molecule spectroscopy using pulsed laser excitation and synchronized multi channel time correlated single photon counting (TCSPC) provides detailed information about the conformational changes of a biological motor in real time. We studied the formation of adenosine triphosphate, ATP, from ADP and phosphate by FoF1-ATP synthase. The reaction is performed by a stepwise internal rotation of subunits of the lipid membrane-embedded enzyme. Using fluorescence resonance energy transfer, FRET, we detected rotation of this biological motor by sequential changes of intramolecular distances within a single FoF1-ATP synthase. Prolonged observation times of single enzymes were achieved by functional immobilization to the glass surface. The stepwise rotary subunit movements were identified by Hidden Markov Models (HMM) which were trained with single-molecule FRET trajectories. To improve the accuracy of the HMM analysis we included the single-molecule fluorescence lifetime of the FRET donor and used alternating laser excitation to co-localize the FRET acceptor independently within a photon burst. The HMM analysis yielded the orientations and dwell times of rotary subunits during stepwise rotation. In addition, the action mode of bactericidal drugs, i.e. inhibitors of FoF1-ATP synthase like aurovertin, could be investigated by the time resolved single-molecule FRET approach., Comment: 12 pages, 9 figures

Nanodiamond crystals containing single color centers have been grown by chemical vapor deposition (CVD). The fluorescence from individual crystallites was directly correlated with crystallite size using a combined atomic force and scanning confocal fluorescence microscope. Under the conditions employed, the optimal size for single optically active nitrogen-vacancy (NV) center incorporation was measured to be 60 to 70 nm. The findings highlight a strong dependence of NV incorporation on crystal size, particularly with crystals less than 50 nm in size., Comment: 16 pages, 4 figures, In Print Nano Letters (2007)

FoF1-ATP synthase is the enzyme that provides the 'chemical energy currency' adenosine triphosphate, ATP, for living cells. The formation of ATP is accomplished by a stepwise internal rotation of subunits within the enzyme. We monitor subunit rotation by a single-molecule fluorescence resonance energy transfer (FRET) approach using two fluorophores specifically attached to the enzyme. To identify the stepsize of rotary movements by the motors of ATP synthase we simulated the confocal single-molecule FRET data of freely diffusing enzymes and developed a step finder algorithm based on 'Hidden Markov Models' (HMM). The HMM is able to find the proximity factors, P, for a three-level system and for a five-level system, and to unravel the dwell times of the simulated rotary movements. To identify the number of hidden states in the system, a likelihood parameter is calculated for the series of one-state to eight-state HMMs applied to each set of simulated data. Thereby, the basic prerequisites for the experimental single-molecule FRET data are defined that allow for discrimination between a 120 degree stepping mode or a 36 degree substep rotation mode for the proton-driven Fo motor of ATP synthase., Comment: 12 pages, 5 figures

Optical and microwave double resonance techniques are used to obtain the excited state structure of single nitrogen-vacancy centers in diamond. The excited state is an orbital doublet and it is shown that it can be split and associated transition strengths varied by external electric fields and by strain. A group theoretical model is developed. It gives a good account of the observations and contributes to an improved understanding of the electronic structure of the center. The findings are important for quantum information processing and other applications of the center., Comment: 4 pages, 4 figures

Lifetime limited optical excitation lines of single nitrogen vacancy (NV) defect centers in diamond have been observed at liquid helium temperature. They display unprecedented spectral stability over many seconds and excitation cycles. Spectral tuning of the spin selective optical resonances was performed via the application of an external electric field (i.e. the Stark shift). A rich variety of Stark shifts were observed including linear as well as quadratic components. The ability to tune the excitation lines of single NV centers has potential applications in quantum information processing., Comment: 13 pages, 4 figures

Using fluorescence spectroscopy we directly measure entropy production of a single two-level system realized experimentally as an optically driven defect center in diamond. We exploit a recent suggestion to define entropy on the level of a single stochastic trajectory (Seifert, Phys. Rev. Lett. {\bf 95}, 040602 (2005)). Entropy production can then be split into one of the system itself and one of the surrounding medium. We demonstrate that the total entropy production obeys various exact relations for finite time trajectories., Comment: Phys. Rev. Lett., in press

Coherent coupling between single quantum objects is at the heart of modern quantum physics. When coupling is strong enough to prevail over decoherence, it can be used for the engineering of correlated quantum states. Especially for solid-state systems, control of quantum correlations has attracted widespread attention because of applications in quantum computing. Such coherent coupling has been demonstrated in a variety of systems at low temperature1, 2. Of all quantum systems, spins are potentially the most important, because they offer very long phase memories, sometimes even at room temperature. Although precise control of spins is well established in conventional magnetic resonance3, 4, existing techniques usually do not allow the readout of single spins because of limited sensitivity. In this paper, we explore dipolar magnetic coupling between two single defects in diamond (nitrogen-vacancy and nitrogen) using optical readout of the single nitrogen-vacancy spin states. Long phase memory combined with a defect separation of a few lattice spacings allow us to explore the strong magnetic coupling regime. As the two-defect system was well-isolated from other defects, the long phase memory times of the single spins was not diminished, despite the fact that dipolar interactions are usually seen as undesirable sources of decoherence. A coherent superposition of spin pair quantum states was achieved. The dipolar coupling was used to transfer spin polarisation from a nitrogen-vacancy centre spin to a nitrogen spin, with optical pumping of a nitrogen-vacancy centre leading to efficient initialisation. At the level anticrossing efficient nuclear spin polarisation was achieved. Our results demonstrate an important step towards controlled spin coupling and multi-particle entanglement in the solid state.