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Register a new userThree-dimensional localization spectroscopy of individual nuclear spins with sub-Angstrom resolution
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We report on precise localization spectroscopy experiments of individual 13C nuclear spins near a central electronic sensor spin in a diamond chip. By detecting the nuclear free precession signals in rapidly switchable external magnetic fields, we retrieve the three-dimensional spatial coordinates of the nuclear spins with sub-Angstrom resolution and for distances beyond 10 Angstroms. We further show that the Fermi contact contribution can be constrained by measuring the nuclear g-factor enhancement. The presented method will be useful for mapping the atomic-scale structure of single molecules, an ambitious yet important goal of nanoscale nuclear magnetic resonance spectroscopy.
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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.
Magnetic resonance imaging (MRI) has revolutionized biomedical science by providing non-invasive, three-dimensional biological imaging. However, spatial resolution in conventional MRI systems is limited to tens of microns, which is insufficient for imaging on molecular and atomic scales. Here we demonstrate an MRI technique that provides sub-nanometer spatial resolution in three dimensions, with single electron-spin sensitivity. Our imaging method works under ambient conditions and can measure ubiquitous dark spins, which constitute nearly all spin targets of interest and cannot otherwise be individually detected. In this technique, the magnetic quantum-projection noise of dark spins is measured using a single nitrogen-vacancy (NV) magnetometer located near the surface of a diamond chip. The spatial distribution of spins surrounding the NV magnetometer is imaged with a scanning magnetic-field gradient. To evaluate the performance of the NV-MRI technique, we image the three-dimensional landscape of dark electronic spins at and just below the diamond surface and achieve an unprecedented combination of resolution (0.8 nm laterally and 1.5 nm vertically) and single-spin sensitivity. Our measurements uncover previously unidentified electronic spins on the diamond surface, which can potentially be used as resources for improved magnetic imaging of samples proximal to the NV-diamond sensor. This three-dimensional NV-MRI technique is immediately applicable to diverse systems including imaging spin chains, readout of individual spin-based quantum bits, and determining the precise location of spin labels in biological systems.
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it has recently been extended into the visible and UV spectral range. However, resolving MHz energy splittings with ultrashort laser pulses has still remained a challenge. Here, we analyze two-dimensional Fourier spectra for resonant optical excitation of resident electrons to localized trions or donor-bound excitons in semiconductor nanostructures subject to a transverse magnetic field. Particular attention is devoted to Raman coherence spectra which allow one to accurately evaluate tiny splittings of the electron ground state and to determine the relaxation times in the electron spin ensemble. A stimulated step-like Raman process induced by a sequence of two laser pulses creates a coherent superposition of the ground state doublet which can be retrieved only optically due to selective excitation of the same sub-ensemble with a third pulse. This provides the unique opportunity to distinguish between different complexes that are closely spaced in energy in an ensemble. The related experimental demonstration is based on photon echo measurements in an n-type CdTe/(Cd,Mg)Te quantum well structure detected by a heterodyne technique. The difference in the sub-$mu$eV range between the Zeeman splittings of donor-bound electrons and electrons localized at potential fluctuations can be resolved even though the homogeneous linewidth of the optical transitions is larger by two orders of magnitude.
Nuclear magnetic resonance (NMR) spectroscopy has approached the limit of single molecule sensitivity, however the spectral resolution is currently insufficient to obtain detailed information on chemical structure and molecular interactions. Here we demonstrate more than two orders of magnitude improvement in spectral resolution by performing correlation spectroscopy with shallow nitrogen-vacancy (NV) magnetic sensors in diamond. In principle, the resolution is sufficient to observe chemical shifts in $sim$1 T magnetic fields, and is currently limited by molecular diffusion at the surface. We measure oil diffusion rates of $D = 0.15 - 0.2$,nm$^2/mathrm{mu}$s within (5 nm)$^3$ volumes at the diamond surface.
We experimentally demonstrate high degree of polarization of 13C nuclear spins weakly interacting with nitrogen-vacancy (NV) centers in diamond. We combine coherent microwave excitation pulses with optical illumination to provide controlled relaxation and achieve a polarity-tunable, fast nuclear polarization of degree higher than 85% at room temperature for remote 13C nuclear spins exhibiting hyperfine interaction strength with NV centers of the order of 600 kHz. We show with the aid of numerical simulation that the anisotropic hyperfine tensor components naturally provide a route to control spin mixing parameter so that highly efficient nuclear polarization is enabled through careful tuning of nuclear quantization axis by external magnetic field. We further discuss spin dynamics and wide applicability of this method to various target 13C nuclear spins around the NV center electron spin. The proposed control method demonstrates an efficient and versatile route to realize, for example, high-fidelity spin register initialization and quantum metrology using nuclear spin resources in solids.
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