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Register a new userOn the surface paramagnetism of diamond
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We present measurements of spin relaxation times (T_1, T_1,rho, T_2) on very shallow (<5 nm) nitrogen-vacancy (NV) centers in high-purity diamond single crystals. We find a reduction of spin relaxation times up to 30x compared to bulk values, indicating the presence of ubiquitous magnetic impurities associated with the surface. Our measurements yield a density of 0.01-0.1 Bohr magnetons per nm^2 and a characteristic correlation time of 0.28(3) ns of surface states, with little variation between samples (implanted, N-doped) and surface terminations (H, F and O). A low temperature measurement further confirms that fluctuations are thermally activated. The data support the atomistic picture where impurities are associated with the top carbon layers, and not with terminating surface atoms or adsorbate molecules. The low spin density implies that the presence of a single surface impurity is sufficient to cause spin relaxation of a shallow NV center.
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Undoped diamond, a remarkable bulk electrical insulator, exhibits a high surface conductivity in air when the surface is hydrogen-terminated. Although theoretical models have claimed that a two-dimensional hole gas is established as a result of surface energy band bending, no definitive experimental demonstration has been reported so far. Here, we prove the two-dimensional character of the surface conductivity by low temperature characterization of diamond in-plane gated field-effect transistors that enable the lateral confinement of the transistors drain-source channel to nanometer dimensions. In these devices, we observe Coulomb blockade effects of multiple quantum islands varying in size with the gate voltage. The charging energy and thus the size of these zero-dimensional islands exhibits a gate voltage dependence which is the direct result of the two-dimensional character of the conductive channel formed at hydrogen-terminated diamond surfaces.
Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by $^{15}$N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths ($<$ 60 MHz) are observed for the majority of the normal-implant (7$^circ$, $approx$ 100 nm deep) $^{15}$NV centers. Long-term stability of the NV$^-$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85$^circ$, $approx$ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.
We present an enhancement of spin properties of the shallow (<5nm) NV centers by using ALD to deposit titanium oxide layer on the diamond surface. With the oxide layer of an appropriate thickness, increases about 2 up to 3.5 times of both relaxation time and evolution time were achieved and the shallow NV center charge states stabilized as well. Moreover, the coherence time kept almost unchanged. This surface coating technique could produce a protective coating layer of controllable thickness without any damages to the solid quantum system surface, making it possible to prolong T1 time and T2* time, which would be a possible approach to the further packaging technique for the applicating solid quantum devices.
We present a promising method for creating high-density ensembles of nitrogen-vacancy centers with narrow spin-resonances for high-sensitivity magnetic imaging. Practically, narrow spin-resonance linewidths substantially reduce the optical and RF power requirements for ensemble-based sensing. The method combines isotope purified diamond growth, in situ nitrogen doping, and helium ion implantation to realize a 100 nm-thick sensing surface. The obtained 10^(17) cm^(-3) nitrogen-vacancy density is only a factor of 10 less than the highest densities reported to date, with an observed spin resonance linewidth over 10 times more narrow. The 200 kHz linewidth is most likely limited by dipolar broadening indicating even further reduction of the linewidth is desirable and possible.
The negatively-charged nitrogen-vacancy (NV) center in diamond has been shown recently as an excellent sensor for external spins. Nevertheless, their optimum engineering in the near-surface region still requires quantitative knowledge in regard to their activation by vacancy capture during thermal annealing. To this aim, we report on the depth profiles of near-surface helium-induced NV centers (and related helium defects) by step-etching with nanometer resolution. This provides insights into the efficiency of vacancy diffusion and recombination paths concurrent to the formation of NV centers. It was found that the range of efficient formation of NV centers is limited only to approximately $10$ to $15,$nm (radius) around the initial ion track of irradiating helium atoms. Using this information we demonstrate the fabrication of nanometric-thin ($delta$) profiles of NV centers for sensing external spins at the diamond surface based on a three-step approach, which comprises (i) nitrogen-doped epitaxial CVD diamond overgrowth, (ii) activation of NV centers by low-energy helium irradiation and thermal annealing, and (iii) controlled layer thinning by low-damage plasma etching. Spin coherence times (Hahn echo) ranging up to $50,$ $mu$s are demonstrated at depths of less than $5,$nm in material with $1.1,%$ of $^{13}$C (depth estimated by spin relaxation (T$_1$) measurements). At the end, the limits of the helium irradiation technique at high ion fluences are also experimentally investigated.
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