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Correlated translation-orientation tracking of single particles can provide important information for understanding the dynamics of live systems and their interaction with the probes. However, full six-dimensional (6D) motion tracking has yet to be achieved. Here, we developed synchronized 3D translation and 3D rotation tracking of single diamond particles based on nitrogen-vacancy center sensing. We first performed 6D tracking of diamond particles attached to a giant plasma membrane vesicle to demonstrate the method. Quantitative analysis of diamond particles' motion allowed elimination of the geometric effect and revealed the net rotation on the vesicle. 6D tracking was then applied to measure live cell dynamics. Motion characteristics of nanodiamonds on cell membranes under various controlled physiological conditions suggest that the nanodiamonds' rotation is associated with cell metabolic activities. Our technique extends the toolbox of single particle tracking and provides a unique solution to problems where correlated analysis of translation and rotation is critical.

Colour centres with long-lived spins are established platforms for quantum sensing and quantum information applications. Colour centres exist in different charge states, each of them with distinct optical and spin properties. Application to quantum technology requires the capability to access and stabilize charge states for each specific task. Here, we investigate charge state manipulation of individual silicon vacancies in silicon carbide, a system which has recently shown a unique combination of long spin coherence time and ultrastable spin-selective optical transitions. In particular, we demonstrate charge state switching through the bias applied to the colour centre in an integrated silicon carbide opto-electronic device. We show that the electronic environment defined by the doping profile and the distribution of other defects in the device plays a key role for charge state control. Our experimental results and numerical modeling evidence that control of these complex interactions can, under certain conditions, enhance the photon emission rate. These findings open the way for deterministic control over the charge state of spin-active colour centres for quantum technology and provide novel techniques for monitoring doping profiles and voltage sensing in microscopic devices.

In quantum sensing, precision is typically limited by the maximum time interval over which phase can be accumulated. Memories have been used to enhance this time interval beyond the coherence lifetime and thus gain precision. Here, we demonstrate that by using a quantum memory an increased sensitivity can also be achieved. To this end, we use entanglement in a hybrid spin system comprising a sensing and a memory qubit associated with a single nitrogen-vacancy centre in diamond. With the memory we retain the full quantum state even after coherence decay of the sensor, which enables coherent interaction with distinct weakly coupled nuclear spin qubits. We benchmark the performance of our hybrid quantum system against use of the sensing qubit alone by gradually increasing the entanglement of sensor and memory. We further apply this quantum sensor-memory pair for high-resolution NMR spectroscopy of single 13C nuclear spins., In quantum sensing, memories have been used to enhance measurement precision. Here, the authors demonstrate the use of a memory to increase sensitivity of single 13C nuclear spins spectroscopy by storing the full sensor state and entangling memory and sensor.

Quantum technology relies on proper hardware, enabling coherent quantum state control as well as efficient quantum state readout. In this regard, wide-bandgap semiconductors are an emerging material platform with scalable wafer fabrication methods, hosting several promising spin-active point defects. Conventional readout protocols for defect spins rely on fluorescence detection and are limited by a low photon collection efficiency. Here, we demonstrate a photo-electrical detection technique for electron spins of silicon vacancy ensembles in the 4H polytype of silicon carbide (SiC). Further, we show coherent spin state control, proving that this electrical readout technique enables detection of coherent spin motion. Our readout works at ambient conditions, while other electrical readout approaches are often limited to low temperatures or high magnetic fields. Considering the excellent maturity of SiC electronics with the outstanding coherence properties of SiC defects, the approach presented here holds promises for scalability of future SiC quantum devices., The efficiency of quantum state readout is one of the factors that determine the performance of point defects in semiconductors in practical applications. Here the authors demonstrate photo-electrical readout for silicon vacancies in silicon carbide, providing an alternative to optical detection.

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Single-photon emitting devices have been identified as an important building block for applications in quantum information and quantum communication. They allow us to transduce and collect quantum information over a long distance via photons as so-called flying qubits. In addition, substrates like silicon carbide provide an excellent material platform for electronic devices. In this work, we combine these two features and show that one can drive single photon emitters within a silicon carbide p-i-n-diode. To achieve this, we specifically designed a lateral oriented diode. We find a variety of new color centers emitting non-classical lights in the visible and near-infrared range. One type of emitter can be electrically excited, demonstrating that silicon carbide can act as an ideal platform for electrically controllable single photon sources.

Diamond nanopillars with diameters of 1 μm down to 50 nm have been fabricated from two types of diamond thin films, namely nanocrystalline diamond (NCD) and ultrananocrystalline diamond (UNCD) using electron beam lithography (EBL) and reactive ion etching (RIE) in an inductively coupled oxygen plasma (ICP). Aim of the study was to investigate the suitability of these pillars to incorporate nitrogen-vacancy (NV) color centers for applications in quantum information technology (QIT). The first part of the investigation is devoted to a characterization of the pillars, their shape, size, and properties. The second part of this investigation concerns the optical properties of NCD and UNCD nanopillars and the incorporation of NV centers within them. Among others, fluorescence mapping and photoluminescence measurements have been employed for this purpose. It turned out that NCD pillars are quite promising for the applications in QIT envisioned. At the present time, the opposite is the case for UNCD pillars. The reasons for these differences will be discussed on the basis of the differences of the two materials NCD and UNCD.

Silicon carbide is a promising platform for single photon sources, quantum bits (qubits) and nanoscale sensors based on individual color centers. Towards this goal, we develop a scalable array of nanopillars incorporating single silicon vacancy centers in 4H-SiC, readily available for efficient interfacing with free-space objective and lensed-fibers. A commercially obtained substrate is irradiated with 2 MeV electron beams to create vacancies. Subsequent lithographic process forms 800 nm tall nanopillars with 400-1,400 nm diameters. We obtain high collection efficiency, up to 22 kcounts/s optical saturation rates from a single silicon vacancy center, while preserving the single photon emission and the optically induced electron-spin polarization properties. Our study demonstrates silicon carbide as a readily available platform for scalable quantum photonics architecture relying on single photon sources and qubits., Comment: 18 pages, 8 figures

Newly discovered van der Waals materials like MoS$_2$, WSe$_2$, hexagonal boron nitride (h-BN), and recently $\mathrm{C}_2\mathrm{N}$ have sparked intensive research to unveil the quantum behavior associated with their 2D structure. Of great interest are 2D materials that host single quantum emitters. h-BN, with a band gap of 5.95 eV, has been shown to host single quantum emitters which are stable at room temperature in the UV and visible spectral range. In this paper we investigate correlations between h-BN structural features and emitter location from bulk down to the monolayer at room temperature. We demonstrate that chemical etching and ion irradiation can generate emitters in h-BN. We analyze the emitters' spectral features and show that they are dominated by the interaction of their electronic transition with a single Raman active mode of h-BN. Photodynamics analysis reveals diverse rates between the electronic states of the emitter. The emitters show excellent photo stability even under ambient conditions and in monolayers. Comparing the excitation polarization between different emitters unveils a connection between defect orientation and the h-BN hexagonal structure. The sharp spectral features, color diversity, room-temperature stability, long-lived metastable states, ease of fabrication, proximity of the emitters to the environment, outstanding chemical stability, and biocompatibility of h-BN provide a completely new class of systems that can be used for sensing and quantum photonics applications., In Nano Letters, ACS, 2016. Title change. Revision according to peer-review report. SI can be downloaded from http://pubs.acs.org/doi/suppl/10.1021/acs.nanolett.6b03268/suppl_file/nl6b03268_si_001.pdf

Nitrogen-vacancy (NV) centers were incorporated during hot filament chemical vapor deposition of diamond nanocrystallites and nanocrystalline diamond (NCD) films. From the latter nanopillars with different diameters were prepared applying electron beam lithography and inductively coupled plasma reactive ion etching. The deposition of either single crystallites or closed films was controlled by the nucleation density on the silicon substrates and the process duration. Optical investigations revealed the presence of ensembles of color centers in both nanostructures. An enhancement of the fluorescence emission by an order of magnitude was observed after the structuring of the NCD films.

Spins in solids are cornerstone elements of quantum spintronics. Leading contenders such as defects in diamond or individual phosphorus dopants in silicon have shown spectacular progress, but either lack established nanotechnology or an efficient spin/photon interface. Silicon carbide (SiC) combines the strength of both systems: it has a large bandgap with deep defects and benefits from mature fabrication techniques. Here, we report the characterization of photoluminescence and optical spin polarization from single silicon vacancies in SiC, and demonstrate that single spins can be addressed at room temperature. We show coherent control of a single defect spin and find long spin coherence times under ambient conditions. Our study provides evidence that SiC is a promising system for atomic-scale spintronics and quantum technology.

Doping of carbon nanoparticles with impurity atoms is central to their application. However, doping has proven elusive for very small carbon nanoparticles because of their limited availability and a lack of fundamental understanding of impurity stability in such nanostructures. Here, we show that isolated diamond nanoparticles as small as 1.6 nm, comprising only ∼400 carbon atoms, are capable of housing stable photoluminescent colour centres, namely the silicon vacancy (SiV). Surprisingly, fluorescence from SiVs is stable over time, and few or only single colour centres are found per nanocrystal. We also observe size-dependent SiV emission supported by quantum-chemical simulation of SiV energy levels in small nanodiamonds. Our work opens the way to investigating the physics and chemistry of molecular-sized cubic carbon clusters and promises the application of ultrasmall non-perturbative fluorescent nanoparticles as markers in microscopy and sensing.

Electron and nuclear spins associated with point defects in insulators are promising systems for solid state quantum technology. While the electron spin usually is used for readout and addressing, nuclear spins are exquisite quantum bits and memory systems. With these systems single-shot readout of nearby nuclear spins as well as entanglement aided by the electron spin has been shown. While the electron spin in this example is essential for readout it usually limits nuclear spin coherence. This has set of the quest for defects with spin-free ground states. Here, we isolate a hitherto unidentified defect in diamond and use it at room temperature to demonstrate optical spin polarization and readout with exceptionally high contrast (up to 45%), coherent manipulation of an individual excited triplet state spin, and coherent nuclear spin manipulation using the triplet electron spin as a meta-stable ancilla. By this we demonstrate nuclear magnetic resonance and Rabi oscillations of the uncoupled nuclear spin in the spin-free electronic ground state. Our study demonstrates that nuclei coupled to single metastable electron spins are useful quantum systems with long memory times despite electronic relaxation processes., 4 pages, 5 figures

FoF1-ATP synthases in Escherichia coli (E. coli) bacteria are membrane-bound enzymes which use an internal proton-driven rotary double motor to catalyze the synthesis of adenosine triphosphate (ATP). According to the 'chemiosmotic hypothesis', a series of proton pumps generate the necessary pH difference plus an electric potential across the bacterial plasma membrane. These proton pumps are redox-coupled membrane enzymes which are possibly organized in supercomplexes, as shown for the related enzymes in the mitochondrial inner membrane. We report diffusion measurements of single fluorescent FoF1-ATP synthases in living E. coli by localization microscopy and single enzyme tracking to distinguish a monomeric enzyme from a supercomplex-associated form in the bacterial membrane. For quantitative mean square displacement (MSD) analysis, the limited size of the observation area in the membrane with a significant membrane curvature had to be considered. The E. coli cells had a diameter of about 500 nm and a length of about 2 to 3 \mum. Because the surface coordinate system yielded different localization precision, we applied a sliding observation window approach to obtain the diffusion coefficient D = 0.072 \mum2/s of FoF1-ATP synthase in living E. coli cells., Comment: 12 pages, 6 figures

FoF1-ATP synthase is the essential membrane enzyme maintaining the cellular level of adenosine triphosphate (ATP) and comprises two rotary motors. We measure subunit rotation in FoF1-ATP synthase by intramolecular Foerster resonance energy transfer (FRET) between two fluorophores at the rotor and at the stator of the enzyme. Confocal FRET measurements of freely diffusing single enzymes in lipid vesicles are limited to hundreds of milliseconds by the transit times through the laser focus. We evaluate two different methods to trap the enzyme inside the confocal volume in order to extend the observation times. Monte Carlo simulations show that optical tweezers with low laser power are not suitable for lipid vesicles with a diameter of 130 nm. A. E. Cohen (Harvard) and W. E. Moerner (Stanford) have recently developed an Anti-Brownian electrokinetic trap (ABELtrap) which is capable to apparently immobilize single molecules, proteins, viruses or vesicles in solution. Trapping of fluorescent particles is achieved by applying a real time, position-dependent feedback to four electrodes in a microfluidic device. The standard deviation from a given target position in the ABELtrap is smaller than 200 nm. We develop a combination of the ABELtrap with confocal FRET measurements to monitor single membrane enzyme dynamics by FRET for more than 10 seconds in solution., Comment: 12 pages, 10 figures

The detection of single molecules has facilitated many advances in life- and material-sciences. Commonly, it founds on the fluorescence detection of single molecules, which are for example attached to the structures under study. For fluorescence microscopy and sensing the crucial parameters are the collection and detection efficiency, such that photons can be discriminated with low background from a labeled sample. Here we show a scheme for filtering the excitation light in the optical detection of single stranded labeled DNA molecules. We use the narrow-band filtering properties of a hot atomic vapor to filter the excitation light from the emitted fluorescence of a single emitter. The choice of atomic sodium allows for the use of fluorescent dyes, which are common in life-science. This scheme enables efficient photon detection, and a statistical analysis proves an enhancement of the optical signal of more than 15% in a confocal and in a wide-field configuration., Comment: 9 pages, 5 figures