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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

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

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

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