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arXiv:2001.00109 · Physical Review Research

Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond

A. Jarmola, I. Fescenko, V. M. Acosta, M. W. Doherty, F. K. Fatemi, T. Ivanov, D. Budker, V. S. Malinovsky

Published Apr 28, 2020• 26 citations
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Abstract

This paper elucidates the optical nuclear-spin-readout and the non-linear temperature and magnetic-field dependence of the nuclear spin transitions in Nitrogen vacancy ensembles, and how these systems can be used for quantum sensing
DOI
10.1103/physrevresearch.2.023094

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Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperature T yielding d|Q|/dT=-35.0(2) Hz/K at T=297 K. The temperature and magnetic field dependencies reported here are important for quantum sensing applications such as rotation sensing and potentially for applications in quantum information processing.
Isolated nuclear spins provide a promising building block for quantum information science, motivating development of techniques to characterize, control, and detect them in suitable systems. Working with the nitrogen-vacancy center in diamond, we demonstrate robust initialization, manipulation, and readout of individual 13C^{13}\text{C}13C, 15N^{15}\text{N}15N, and 14N^{14}\text{N}14N nuclear spins and identify a mechanism to extend our results to arbitrary magnetic field environments. These techniques enable precise characterization of nuclear-spin hyperfine parameters and coherence properties and may pave the way for nuclear-spin-based quantum information architectures in diamond.
Abstract Solid state spins have demonstrated significant potential in quantum sensing with applications including fundamental science, medical diagnostics and navigation. The quantum sensing schemes showing best performance under ambient conditions all utilize microwave or radio-frequency driving, which poses a significant limitation for miniaturization, energy efficiency, and non-invasiveness of quantum sensors. We overcome this limitation by demonstrating a purely optical approach to coherent quantum sensing. Our scheme involves the 15N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond as a sensing resource, and exploits NV spin dynamics in oblique magnetic fields near the NV’s excited state level anti-crossing to optically pump the nuclear spin into a quantum superposition state. We demonstrate all-optical free-induction decay measurements—the key protocol for low-frequency quantum sensing—both on single spins and spin ensembles. Our results pave the way for highly compact quantum sensors to be employed for magnetometry or gyroscopy applications in challenging environments.
Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR), and exhibit linewidths narrowed by factors as high as ~130 at room temperature over typical electron-type transitions observed from this spin system. We anticipate the use of these decoherence-protected transitions, in combination with dynamical decoupling methods, for storage of quantum information.
For quantum sensing, it is vital to develop an efficient technique for determining the quantum state of the sensor. We optimize the weighting of the photoluminescence intensity for readout of the spin state of the nitrogen-vacancy (NV) center in diamond. We find that adopting a physical model that considers the optical transitions and relaxations of the NV center allows for an efficient readout. Our method improves the signal-to-noise ratio of the readout by 5.4% in a short time of 3 s, while the existing methods typically require 1 min of integration time. We also show that our technique enhances the readout of the nuclear spin memory. The demonstrated way is helpful for a wide range of measurements, from a few minutes to several days.
Precision measurements based on optically detected nuclear magnetic resonance offer exquisite sensitivity to absolute shifts in spin transition frequencies, with potential applications in fundamental physics experiments and inertial sensing. We investigate 13C nuclear spins in diamond as a candidate system for solid-state implementations, which hold the promise for high-fidelity readout of large numbers of coherent nuclear spins in millitesla or lower magnetic fields. We demonstrate a technique that allows for both optical polarization and readout of large ensembles of ~10^{16} polarized nuclear spins. Our method takes advantage of state-selective Landau-Zener transitions under microwave frequency sweeping, which bidirectionally transfer spin polarization between Nitrogen-Vacancy (NV) electron spins and remote 13C nuclear spins. Using natural isotopic abundance diamonds with nitrogen densities of ~0.5-10 ppm, we perform optically-detected 13C Ramsey spectroscopy and realize a nuclear-spin-dependent fluorescence contrast exceeding 0.5% peak-to-peak. We observe nuclear spin dephasing times T2*~2 ms that only modestly improve with homonuclear dipolar decoupling, indicating that they are limited by the longitudinal spin relaxation of nearby NV electron spins. We study the magnetic field dependence of the optical readout and find comparable contrast and dephasing times for magnetic fields in the range 8-20 mT. Our method can be interpreted as a type of repetitive readout, where each NV center optically reads out the spin state of ~10^2 nuclei before nuclear spins depolarize.