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 Physics , 2014, DOI: 10.1103/PhysRevLett.113.030803 Abstract: We discuss multipulse magnetometry that exploits all three magnetic sublevels of the S=1 nitrogen-vacancy center in diamond to achieve enhanced magnetic field sensitivity. Based on dual frequency microwave pulsing, the scheme works in arbitrary magnetic bias fields and is twice as sensitive to ac magnetic fields as conventional two-level magnetometry. We derive the spin evolution operator for dual frequency microwave excitation and show its effectiveness for double-quantum state swaps. Using multipulse sequences of up to 128 pulses under optimized conditions, we show enhancement of the SNR by up to a factor of 2 in detecting NMR statistical signals, with a 4 times enhancement theoretically possible.
 Physics , 2011, DOI: 10.1103/PhysRevB.84.104301 Abstract: New schemes that exploit the unique properties of Nitrogen-Vacancy (NV) centers in diamond are presently being explored as a platform for high-resolution magnetic sensing. Here we focus on the ability of a NV center to monitor an adjacent mesoscopic nuclear spin bath. For this purpose, we conduct comparative experiments where the NV spin evolves under the influence of surrounding 13C nuclei or, alternatively, in the presence of asynchronous AC fields engineered to emulate bath fluctuations. Our study reveals substantial differences that underscore the limitations of the semi-classical picture when interpreting and predicting the outcome of experiments designed to probe small nuclear spin ensembles. In particular, our study elucidates the NV center response to bath fluctuations under common pulse sequences, and explores a detection protocol designed to probe time correlations of the nuclear spin bath dynamics. Further, we show that the presence of macroscopic nuclear spin order is key to the emergence of semi-classical spin magnetometry.
 Physics , 2013, DOI: 10.1088/0034-4885/77/5/056503 Abstract: The isolated electronic spin system of the Nitrogen-Vacancy (NV) centre in diamond offers unique possibilities to be employed as a nanoscale sensor for detection and imaging of weak magnetic fields. Magnetic imaging with nanometric resolution and field detection capabilities in the nanotesla range are enabled by the atomic-size and exceptionally long spin-coherence times of this naturally occurring defect. The exciting perspectives that ensue from these characteristics have triggered vivid experimental activities in the emerging field of "NV magnetometry". It is the purpose of this article to review the recent progress in high-sensitivity nanoscale NV magnetometry, generate an overview of the most pertinent results of the last years and highlight perspectives for future developments. We will present the physical principles that allow for magnetic field detection with NV centres and discuss first applications of NV magnetometers that have been demonstrated in the context of nano magnetism, mesoscopic physics and the life sciences.
 Physics , 2012, DOI: 10.1103/PhysRevLett.110.130802 Abstract: We demonstrate an absolute magnetometer immune to temperature fluctuation and strain inhomogeneity, based on quantum beats in the ground state of nitrogen-vacancy centers in diamond. We apply this technique to measure low-frequency magnetic field noise using a single nitrogen-vacancy center located within 500 nm of the surface of an isotopically-pure (99.99% C12) diamond. The photon-shot-noise limited sensitivity achieves 38 nT/Hz^1/2 for 4.45 s acquisition time, a factor of 2^1/2 better than the implementation which uses only two spin levels. For long acquisition times (>10 s), we realize up to a factor of 15 improvement in magnetic sensitivity, which demonstrates the robustness of our technique against thermal drifts. Applying our technique to nitrogen-vacancy center ensembles, we eliminate dephasing from longitudinal strain inhomogeneity, resulting in a factor of 2.3 improvement in sensitivity.
 Physics , 2013, DOI: 10.1063/1.4860997 Abstract: Experiments show that shallow nitrogen implantations (<10keV) result in a negatively charged nitrogen-vacancy center (NV-) yield of 0.01-0.1%. The most succesful technique for introducing NV- centers in the carbon matrix is ion implantation followed by annealing at 1100K. We investigated the influence of channeling effects during shallow implantation and statistical diffusion using molecular dynamics (MD) and Monte Carlo (MC) approaches. Energy barriers for the diffusion process were calculated using the density functional theory (DFT). Our simulations show a significant difference in the NV yield compared to the experiment. Statistically, 25% of the implanted nitrogens form a NV center after annealing.
 Physics , 2014, DOI: 10.1063/1.4892544 Abstract: The nitrogen vacancy (NV) center in diamond is a sensitive probe of magnetic field and a promising qubit candidate for quantum information processing. The performance of many NV-based devices improves by aligning the NV(s) parallel to a single crystallographic direction. Using ab initio theoretical techniques, we show that NV orientation can be controlled by high-temperature annealing in the presence of strain under currently accessible experimental conditions. We find that $(89\pm7)\%$ of NVs align along the [111] crystallographic direction under 2\% compressive biaxial strain (perpendicular to [111]) and an annealing temperature of 970$^\circ$C.
 Physics , 2009, DOI: 10.1103/PhysRevB.80.115202 Abstract: Nitrogen-vacancy (NV) centers in millimeter-scale diamond samples were produced by irradiation and subsequent annealing under varied conditions. The optical and spin relaxation properties of these samples were characterized using confocal microscopy, visible and infrared absorption, and optically detected magnetic resonance. The sample with the highest NV- concentration, approximately 16 ppm = 2.8 x 10^{18} cm^{-3}, was prepared with no observable traces of neutrally-charged vacancy defects. The effective transverse spin relaxation time for this sample was T2* = 118(48) ns, predominately limited by residual paramagnetic nitrogen which was determined to have a concentration of 52(7) ppm. Under ideal conditions, the shot-noise limited sensitivity is projected to be ~150 fT/\sqrt{Hz} for a 100 micron-scale magnetometer based on this sample. Other samples with NV- concentrations from .007 to 12 ppm and effective relaxation times ranging from 27 to 291 ns were prepared and characterized.
 Physics , 2012, DOI: 10.1088/1367-2630/15/1/013041 Abstract: The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen-vacancy centre in diamond - a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen-vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of nitrogen-vacancy magnetometry are developed for a randomly diffusing diamond nanocrystal. We find that the accumulation of geometric phases, due to the rotation of the nanodiamond plays a crucial role in the application of a diffusing nanodiamond as a bio-label and magnetometer. Specifically, we show that a freely diffusing nanodiamond can offer real-time information about local magnetic fields and its own rotational behaviour, beyond continuous optically detected magnetic resonance monitoring, in parallel with operation as a fluorescent biomarker.
 Physics , 2014, Abstract: Coherent control of the nitrogen-vacancy (NV) center in diamond's triplet spin state has traditionally been accomplished with resonant ac magnetic fields under the constraint of the magnetic dipole selection rule, which forbids direct control of the $|-1>\leftrightarrow |+1>$ spin transition. We show that high-frequency stress resonant with the spin state splitting can coherently control NV center spins within this subspace. Using a bulk-mode mechanical microresonator fabricated from single-crystal diamond, we apply intense ac stress to the diamond substrate and observe mechanically driven Rabi oscillations between the $|-1>$ and $|+1>$ states of an NV center spin ensemble. Additionally, we measure the inhomogeneous spin dephasing time ($T_{2}^{*}$) of the spin ensemble using a mechanical Ramsey sequence and compare it to the dephasing times measured with a magnetic Ramsey sequence for each of the three spin qubit combinations available within the NV center ground state. These results demonstrate coherent spin driving with a mechanical resonator and could enable the creation of a phase-sensitive $\Delta$-system within the NV center ground state.
 Physics , 2010, DOI: 10.1063/1.3507884 Abstract: We demonstrate magnetometry by detection of the spin state of high-density nitrogen-vacancy ensembles in diamond using optical absorption at 1042 nm. With this technique, measurement contrast, and collection efficiency can approach unity, leading to an increase in magnetic sensitivity compared to the more common method of collecting red fluorescence. Working at 75 K with a sensor with effective volume $50 \times 50 \times 300$ microns^3, we project photon shot-noise limited sensitivity of 5 pT in one second of acquisition and bandwidth from dc to a few megahertz. Operation in a gradiometer configuration yields a noise floor of 7 nTrms at ~110 Hz in one second of acquisition.
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