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Single Molecules

Spectroscopy of Single N-V Centers in Diamond

Fedor Jelezko, C. Tietz, A. Gruber, I. Popa, Alexander P. Nizovtsev, S. Ya. Kilin, Jörg Wrachtrup

Published Dec 1, 2001• 105 citations
Publisher

Abstract

Over the past few years, the detection of single N-V centers in diamond has attracted much interest, since it is expected to lead to innovative applications in various domains of quantum information. The N-V center in diamond is a defectconsisting of a substitutional nitrogen atom adjacent to a carbon-atom vacancy. The optical transition between the 3A ground state and the 3E excited state has a very high quantum efficiency allowing single defect spectroscopy. Because of the paramagnetic nature of the ground electronic state, single N-V defects are believed to be promising candidates for solid state quantum computation. To date, however, the photophysics of the defect is not entirely understood. The existence of a singlet metastable state 1A was challenged in a series of papers reporting hole-burning, optically detected magnetic resonance and single molecule experiments. We present here an overview of recent low and room temperature data, indicating the important role of a metastable state of the defect in single center experiments.

DOI
10.1002/1438-5171(200112)2:4<255::aid-simo255>3.0.co;2-d

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Over the past few years, the detection of single N-V centers in diamond has attracted much interest, since it is expected to lead to innovative applications in various domains of quantum information. The N-V center in diamond is a defectconsisting of a substitutional nitrogen atom adjacent to a carbon-atom vacancy. The optical transition between the 3A ground state and the 3E excited state has a very high quantum efficiency allowing single defect spectroscopy. Because of the paramagnetic nature of the ground electronic state, single N-V defects are believed to be promising candidates for solid state quantum computation. To date, however, the photophysics of the defect is not entirely understood. The existence of a singlet metastable state 1A was challenged in a series of papers reporting hole-burning, optically detected magnetic resonance and single molecule experiments. We present here an overview of recent low and room temperature data, indicating the important role of a metastable state of the defect in single center experiments.
The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 ±\pm± 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 ±\pm± 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 ±\pm± 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
Summary form only given. Fluorescence excitation method of single molecule spectroscopy has been applied recently to study individual nitrogen-vacancy (N-V) defect centers in diamond. These objects are of great interest owing to the proposal to build quantum computer at /sup 13/C nuclear spins neighboring the N-V center. Based on new spectroscopic information we have developed simple models of the N-V center and used them to describe a wide range of experiments dealing both with single centers and with their ensembles. The first model emphasizes possible tunneling of N atom into vacancy and describes that in terms of double well potentials. The second model takes into account the spin-triplet character of the ground electronic state of the center and allows to describe a variety of fluorescence detected magnetic resonance phenomena.
Nitrogen-vacancy (NV) defect centers in diamond have generated much interest for their uses in quantum information and sensing. Despite the ongoing improvements in sensitivity and the range of new applications, much about the NV basic physics remains unresolved, which is important to understand in order to fully exploit potential uses. In this work I describe a series of experiments on NV basic properties, applications, and projects in between. First, I describe an NV singlet absorption spectroscopy experiment, which searched for additional NV electronic states and studied the 1A1 phonon modes. Next, I discuss an NV microwave saturation spectroscopy experiment, which is useful for NV thermometry, removes inhomogeneous broadening, and can yield information about diamond magnetic spin bath dynamics. I then describe an NV relaxation experiment that senses GHz-frequency magnetic noise, which we demonstrated using paramagnetic substitutional nitrogen (P1) centers. Finally, I describe open questions on the NV singlet states, saturation spectroscopy, and relaxation (and how to address them), and report on my ongoing work on using NVs for nuclear polarization and rotation sensing.
In an effort to realize a two-bit processor for a quantum computer on the basis of single nitrogen-vacancy defect centers (NV centers) in diamond, the optically detected nutations of the electron spin of a single NV center in the ground state and of the nuclear spin of a 13 C atom located at a diamond lattice site nearest to the NV center are studied. The photodynamics of NV and NV + 13 C centers under different temperatures and optical excitation conditions is discussed. A seven-level model of a center excited by radiation from an Ar + laser at room temperature is proposed. On the basis of this model, the experimental spectra of optically detected electron paramagnetic and electron-nuclear double resonances of single NV and NV + 13 C centers in diamond nanocrystals, as well as experimental data on the optically detected nutations of the electron and nuclear spins of these centers caused by the actions of pulsed microwave and radiofrequency fields, respectively, are interpreted.