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Optics Letters

Raman heterodyne detected electron-nuclear-double-resonance measurements of the nitrogen-vacancy center in diamond

Neil B. Manson, Xing-Fei He, Peter Fisk

Published Oct 1, 1990• 47 citations
Publisher

Abstract

We report two new applications of the Raman heterodyne detection technique. Raman heterodyne detected electron-nuclear double resonance and a double rf resonance technique are used to obtain the hyperfine structure of the nitrogen-vacancy center in diamond.
DOI
10.1364/ol.15.001094

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•Jul 2, 2018•1 citation
This thesis describes the Raman heterodyne detection of magnetic resonance in the ³A ground state of the nitrogen-vacancy C'-1· V) centre in diamond. The recently developed theory of Raman heterodyne spectroscopy was tested and compared with the spectra measured on the N-V centre. Among those results, the electron-nuclear double resonance (ENDOR), nuclear-nuclear double resonance (double NMR), Autler-Townes effect, coherence transfer and Zeeman quantum beat were observed for the first time using such techniques. Raman heterodyne techniques were also used to investigate the level anticrossing, hyperfine and nuclear quadrupole interactions, and spin relaxations of the N-V centre with high sensitivity and precision. This thesis is comprised of three parts. Part one includes Chapters 1 to 3, providing introductory accounts. Chapter l is an introduction to the N-V colour centre, which describes the defect configuration, the spin Hamiltonian and the calculations of energy levels and wave functions of the ³A ground state. Chapter 2 briefly describes the theory of Raman heterodyne spectroscopy - a coherent optical radio-frequency (RF) double resonance technique, in particular the Raman heterodyne signals at weak and intense RF fields. Chapter 3 deals with experimental details and techniques utilized in the studies. Part two consists of Chapters 4 and 5, where the Raman heterodyne theory is compared with experimental results. Chapter 4 presents the Raman heterodyne detected nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) lineshapes compared with theoretical results at various RF power levels, laser intensities and laser frequencies within the 6380A zero-phonon line. The double resonance spectra obtained by Raman heterodyne techniques are discussed in Chapter 5, where attention is paid to the analysis of their spectral profiles depending on the detection scheme. The application of Raman heterodyne techniques to the studies of magnetic resonance of the N-V centre is described in part three, consisting of Chapters 6 to 9. The EPR measurements are described in Chapter 6, which were used to study various interactions near the level anticrossing, in particular the spin alignment. The hyperfine and nuclear quadrupole interactions probed by the NMR, ENDOR and hole burning measurements are described in Chapter 7. From these measurements, the hyperfine and quadrupole parameters in the spin Hamiltonian were fully determined. Chapter 8 deals with the Autler-Townes effect in the NMR and EPR transitions. By measuring the Autler-Townes spittings, the magnitudes of matrix elements of the NMR transitions were examined and compared. Chapter 9 presents the coherent spin transient properties, including nutations, echoes, Zeeman beating and coherence transfer. The dephasing time and homogeneous linewidths of the NMR and EPR transitions were then determined from the echo measurements. Finally, the thesis is summarized in Chapter 10.
Spin defects in diamond serve as powerful building blocks for quantum technologies, especially for quantum sensing and networking. Electron-nuclear defects formed near optically active spins such as the nitrogen-vacancy center provide a resource for multi-qubit quantum registers. However, many remain uncharacterized, limiting their control and integration in quantum devices. Here, we identify the hyperfine components, including their relative sign, and nuclear spin species of two unknown dark spin defects using zero-field double electron-electron resonance spectroscopy and a protocol based on electron-nuclear double resonance. New ab initio calculations assign one defect to a known nitrogen interstitial, while the hydrogen-related defect matches no calculated or previously reported structure. We further use this protocol to demonstrate initialization, unitary control, and long-lived coherence of the hydrogen nuclear spin qubit, with a coherence time of 1.0(3) ms. These characterization and control tools establish a framework for harnessing unknown electron-nuclear defects for quantum registers.
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.
The Autler–Townes effect in nuclear magnetic resonance (NMR) and electron paramagnetic resonance has been observed using recently developed Raman heterodyne techniques. The measurements were carried out on the nitrogen-vacancy color center in diamond, where the 3A↔3E optical transition was driven by a single mode dye laser at 638 nm while the magnetic transitions in the 3A ground state were driven by two rf fields. The measured splittings in the NMR lines were found to be in good agreement with theoretical predictions. Using the Autler–Townes effect, the magnitude of the dipole moments of the mI=0↔±1 (mS=0) transitions in the ground state was determined, and found to be the same. Comparison of this latter result with the NMR spectra shows that Raman heterodyne signal intensities are determined by population factors.
Nitrogen-vacancy centers in diamond are sensitive probes of time-varying magnetic fields that can be used to identify unknown spin defects in their nearby environment. Performing spectral quantum measurements on such single quantum probes enables gaining information about the internal structure and dynamics of nearby spin defects that would otherwise be inaccessible through direct or indirect measurements with classical probes. Here, we identify a system composed of two electron-nuclear spin defects in a diamond crystal by performing a series of spectral identification measurements using a single nitrogen-vacancy center in diamond. Besides enabling the identification of new spin defects and studies of their formation mechanisms, these techniques will be useful for scaling up quantum systems by converting environmental spin defects into quantum resources.