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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.
Spins of negatively charged nitrogen-vacancy (NV$^-$) defects in diamond are among the most promising candidates for solid-state qubits. The fabrication of quantum devices containing these spin-carrying defects requires position-controlled introducti on of NV$^-$ defects having excellent properties such as spectral stability, long spin coherence time, and stable negative charge state. Nitrogen ion implantation and annealing enable the positioning of NV$^-$ spin qubits with high precision, but to date, the coherence times of qubits produced this way are short, presumably because of the presence of residual radiation damage. In the present work, we demonstrate that a high temperature annealing at 1000$^circ$C allows 2 millisecond coherence times to be achieved at room temperature. These results were obtained for implantation-produced NV$^-$ defects in a high-purity, 99.99% $^{12}$C enriched single crystal chemical vapor deposited diamond. We discuss these remarkably long coherence times in the context of the thermal behavior of residual defect spins. [Published in Physical Review B {bf{88}}, 075206 (2013)]
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