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Optics Letters

Ultraviolet four-wave mixing and phase conjugation with metastable color-center states in diamond

Stephen Colby Rand

Published Feb 1, 1988• 5 citations
Publisher

Abstract

We report the observation of cw four-wave mixing and phase conjugation in the UV on the N3 color-center resonance in diamond. Using a jitter-free technique, the nearly degenerate four-wave mixing spectrum has been measured and the ultranarrow, 250-Hz-wide resonance analyzed to understand the metastable-state decay process responsible for the low quantum efficiency and large nonlinear susceptibility of this aggregated nitrogen structure. The results establish the existence and lifetime of a new excited state of the defect.

DOI
10.1364/ol.13.000140

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Raman-excited spin coherences were experimentally observed in nitrogen-vacancy (N-V) diamond color centers by means of nondegenerate four-wave mixing and electromagnetically induced transparency. The maximal absorption suppression was found to be 17%, which corresponds to 70% of what is possible given the random geometric orientation of the N-V center in diamond. In the context of quantum computing in solids, this level of transparency represents efficient preparation of quantum bits, as well as the ability to perform arbitrary single-quantum-bit rotations.

Optics Letters•Mar 15, 2001•109 citations
We report the observation of cw four-wave mixing and phase conjugation in the UV on the N3 color-center resonance in diamond. Using a jitter-free technique, the nearly degenerate four-wave mixing spectrum has been measured and the ultranarrow, 250-Hz-wide resonance analyzed to understand the metastable-state decay process responsible for the low quantum efficiency and large nonlinear susceptibility of this aggregated nitrogen structure. The results establish the existence and lifetime of a new excited state of the defect.
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 nitrogen-vacancy center in diamond exhibits a zero-phonon transition art 637 nm that has been assigned as an A→E transition at a site with trigonal symmetry.1 Paramagnetic resonance studies revealed a triplet feature that was originally assigned to an excited state.2 More recently, it was argued that the triplet signal actually arose from the ground state,3,4We employ a new method of ultra-high-resolution nearly degenerate four-wave-mixing (NDFWM) spectroscopy, as well as persistent hole burning and electron paramagnetic resonance, to measure the metastable spin singlet excited-state lifetime and the g round-state spin-lattice relaxation time and also to prove that the ground state is indeed a triplet.
A new phase-modulation technique for nonlinear laser spectroscopy is applied with a relative resolving power in the sub-Hz range to measure fundamental relaxation processes of the N-V center in diamond. Complementary EPR experiments versus temperature establish the spin character of the ground state in the absence of optical illumination and show that spin-lattice decay occurs via two-phonon processes involving the dominant vibrational mode. The combined results permit deduction of reliable fine-structure assignments for three states of the center and accurate values for zero-field intersystem crossing and spin-lattice relaxation rates from linewidths of individual resonances in the four-wave-mixing spectrum.
Raman-excited spin coherences were experimentally observed in nitrogen-vacancy (N-V) diamond color centers by means of nondegenerate four-wave mixing and electromagnetically induced transparency. The maximal absorption suppression was found to be 17%, which corresponds to 70% of what is possible given the random geometric orientation of the N-V center in diamond. In the context of quantum computing in solids, this level of transparency represents efficient preparation of quantum bits, as well as the ability to perform arbitrary single-quantum-bit rotations.