We report the detection and polarization of nuclear spins in diamond at room temperature by using a single nitrogen-vacancy (NV) center. We use Hartmann-Hahn double resonance to coherently enhance the signal from a single nuclear spin while decoupling from the noisy spin bath, which otherwise limits the detection sensitivity. As a proof of principle, we (i) observe coherent oscillations between the NV center and a weakly coupled nuclear spin and (ii) demonstrate nuclear-bath cooling, which prolongs the coherence time of the NV sensor by more than a factor of 5. Our results provide a route to nanometer scale magnetic resonance imaging and novel quantum information processing protocols.

Bulk (13)C polarization can be strongly enhanced in diamond at room temperature based on the optical pumping of nitrogen-vacancy color centers. This effect was confirmed by irradiating single crystals at a ~50 mT field promoting anticrossings between electronic excited-state levels, followed by shuttling of the sample into an NMR setup and by subsequent (13)C detection. A nuclear polarization of ~0.5%--equivalent to the (13)C polarization achievable by thermal polarization at room temperature at fields of ~2000 T--was measured, and its bulk nature determined based on line shape and relaxation measurements. Positive and negative enhanced polarizations were obtained, with a generally complex but predictable dependence on the magnetic field during optical pumping. Owing to its simplicity, this (13)C room temperature polarizing strategy provides a promising new addition to existing nuclear hyperpolarization techniques.

We propose solid-state gyroscopes based on ensembles of negatively charged nitrogen-vacancy (${\rm NV^-}$) centers in diamond. In one scheme, rotation of the nitrogen-vacancy symmetry axis will induce Berry phase shifts in the ${\rm NV^{-}}$ electronic ground-state coherences proportional to the solid angle subtended by the symmetry axis. We estimate sensitivity in the range of $5\times10^{-3} {\rm rad/s/\sqrt{Hz}}$ in a 1 ${\rm mm^3}$ sensor volume using a simple Ramsey sequence. Incorporating dynamical decoupling to suppress dipolar relaxation may yield sensitivity at the level of $10^{-5} {\rm rad/s/\sqrt{Hz}}$. With a modified Ramsey scheme, Berry phase shifts in the ${\rm ^{14}N}$ hyperfine sublevels would be employed. The projected sensitivity is in the range of $10^{-5} {\rm rad/s/\sqrt{Hz}}$, however the smaller gyromagnetic ratio reduces sensitivity to magnetic-field noise by several orders of magnitude. Reaching $10^{-5} {\rm rad/s/\sqrt{Hz}}$ would represent an order of magnitude improvement over other compact, solid-state gyroscope technologies.Comment: 3 figures, 5 page

We report polarization of a dense nuclear-spin ensemble in diamond and its dependence on magnetic field and temperature. The polarization method is based on the transfer of electron spin polarization of negatively charged nitrogen vacancy color centers to the nuclear spins via the excited-state level anti-crossing of the center. We polarize 90% of the 14 N nuclear spins within the NV centers, and 70% of the proximal 13 C nuclear spins with hyperfine interaction strength of 13-14 MHz. Magnetic-field dependence of the polarization reveals sharp decrease in polarization at specific field values corresponding to cross-relaxation with substitutional nitrogen centers, while temperature dependence of the polarization reveals that high polarization persists down to 50 K. This work enables polarization of the 13 C in bulk diamond, which is of interest in applications of nuclear magnetic resonance, in quantum memories of hybrid quantum devices, and in sensing.

Negatively-charged nitrogen-vacancy (NV − ) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV − centers remain unresolved. Understanding these properties can validate theoretical models of NV − , improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the 1 A1 electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the 1 E → 1 A1 electronic transition in the NV − center. From this we calculated the 1 E → 1 A1 one-phonon absorption spectrum and found it to differ from that of the 3 E → 3 A2 transition, a result which is not anticipated by previous grouptheoretical models of the NV − electronic states. We identified a high-energy 169 meV localized phonon mode of the 1 A1 level.