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arXiv:1303.0421 · Physical Review A

Nuclear-spin-dependent coherent population trapping of single nitrogen-vacancy centers in diamond

D. Andrew Golter, Khodadad N. Dinyari, Hailin Wang

Published Mar 1, 2013• 20 citations
arXivHTMLPDF

Abstract

Coherent population trapping (CPT) provides a highly sensitive means for probing the energy-level structure of an atomic system. For a nitrogen-vacancy center in diamond, the CPT offers an alternative to the standard optically detected magnetic resonance method for measuring the hyperfine structure of the electronic ground states. We show that the nuclear-spin-dependent CPT measures directly the hyperfine splitting of these states due to the ${}^{14}$N nuclear spin. The CPT spectral response obtained in the presence of a strong microwave field, resonant or nearly resonant with a ground-state spin transition, maps out the dynamic Stark splitting induced by the coherent spin excitation.

DOI
10.1103/physreva.87.035801

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Coherent population trapping (CPT) provides a highly sensitive means for probing the energy-level structure of an atomic system. For a nitrogen-vacancy center in diamond, the CPT offers an alternative to the standard optically detected magnetic resonance method for measuring the hyperfine structure of the electronic ground states. We show that the nuclear-spin-dependent CPT measures directly the hyperfine splitting of these states due to the 14{}^{14}14N nuclear spin. The CPT spectral response obtained in the presence of a strong microwave field, resonant or nearly resonant with a ground-state spin transition, maps out the dynamic Stark splitting induced by the coherent spin excitation.
Abstract We employ the electronic spin of a single nitrogen-vacancy (NV) defect in diamond to detect and control the quantum state of remote nuclear spins coupled by hyperfine interaction. More precisely, our work focuses on individual 13C^{13}\text {C}13C 13 C nuclei featuring a moderate hyperfine coupling strength ( ∼1\sim 1∼1 ∼ 1 MHz) with the NV’s electron spin. Two different methods providing an efficient room-temperature polarization of these peculiar 13C^{13}\text {C}13C 13 C nuclear spins are described. The first one is based on a polarization transfer from the NV electron spin to the 13C^{13}\text {C}13C 13 C nucleus, which is mediated by the anisotropic component of the hyperfine interaction. The second one relies on coherent population trapping (CPT) within a Λ\Lambda Λ Λ -type energy-level configuration in the microwave domain, which enables to initialize the 13C^{13}\text {C}13C 13 C nuclear spin in any quantum state superposition on the Bloch sphere. This CPT protocol is performed in an unusual regime for which relaxation from the excited level of the Λ\Lambda Λ Λ -scheme is externally triggered by optical pumping and separated in time from coherent microwave excitations. For these two polarization techniques, we investigate the impact of optical illumination on the nuclear spin polarization efficiency. This work adds new methods to the quantum toolbox used for coherent control of individual nuclear spins in diamond, which might find applications in quantum metrology. Graphical Abstract
Coherent population trapping at zero magnetic field was observed for nitrogen-vacancy centers in diamond under optical excitation. This was measured as a reduction in photoluminescence when the detuning between two excitation lasers matched the 2.88 GHz crystal-field splitting of the color center ground states. This behavior is highly sensitive to strain, which modifies the excited states, and was unexpected following recent experiments demonstrating optical readout of single nitrogen-vacancy electron spins based on cycling transitions. These results demonstrate for the first time that three-level Lambda configurations suitable for proposed quantum information applications can be realized simultaneously for all four orientations of nitrogen-vacancy centers at zero magnetic field.
We demonstrate coherent population trapping of a single nuclear spin in a room-temperature solid. To this end, we exploit a three-level system with a Λ configuration in the microwave domain, which consists of nuclear spin states addressed through their hyperfine coupling to the electron spin of a single nitrogen-vacancy defect in diamond. Moreover, the Λ-scheme relaxation is externally controlled through incoherent optical pumping and separated in time from consecutive coherent microwave excitations. Such a scheme allows us (i) to monitor the sequential accumulation of population into the dark state and (ii) to reach a novel regime of coherent population trapping dynamics for which periodic arrays of dark resonances can be observed, owing to multiple constructive interferences. This Letter offers new prospects for quantum state preparation, information storage in hybrid quantum systems, and metrology.
Coherent population trapping is demonstrated in single nitrogen-vacancy centers in diamond under optical excitation. For sufficient excitation power, the fluorescence intensity drops almost to the background level when the laser modulation frequency matches the 2.88 GHz splitting of the ground states. The results are well described theoretically by a four-level model, allowing the relative transition strengths to be determined for individual centers. The results show that all-optical control of single spins is possible in diamond.
We study coherent population trapping and AC Stark effect using microwave transitions between the sublevels of the ground state of the NV-center. Sublevels with different projections of the nuclear spin of the nitrogen atom are used to implement the -scheme. Dependence of the characteristics of the coherent population trapping dip on the control field frequency and intensity is studied. Various schemes for observing the AC Stark effect are considered. Keywords: NV-center, coherent population trapping, AC Stark.
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.