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Journal of the Optical Society of America B

Origin of persistent hole burning of N–V centers in diamond

David A. Redman, Steven W. Brown, Stephen Colby Rand

Published May 1, 1992• 58 citations
Publisher

Abstract

New satellite features and antiholes in the persistent hole-burning spectrum of N–V centers in diamond, as well as their dependences on applied electric fields and frequency within the inhomogeneous absorption line, are reported. These results, together with reassignments of spin states of this center, permit an understanding of the origin of the satellite holes as well as of possible mechanisms for the persistent hole-burning phenomenon itself. In addition we report narrow optical interference fringes in heterodyne-detected spectra of persistent spectral holes in the N–V defect center in diamond and discuss a recent suggestion for high-resolution Ramsey-fringe hole-burning spectroscopy of solids based on phase-separated fields.

DOI
10.1364/josab.9.000768

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Electronic structure of the nitrogen-vacancy color center in diamond.

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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.

•Jan 1, 1991•0 citations
New satellite features and antiholes in the persistent hole-burning spectrum of N–V centers in diamond, as well as their dependences on applied electric fields and frequency within the inhomogeneous absorption line, are reported. These results, together with reassignments of spin states of this center, permit an understanding of the origin of the satellite holes as well as of possible mechanisms for the persistent hole-burning phenomenon itself. In addition we report narrow optical interference fringes in heterodyne-detected spectra of persistent spectral holes in the N–V defect center in diamond and discuss a recent suggestion for high-resolution Ramsey-fringe hole-burning spectroscopy of solids based on phase-separated fields.
In this presentation we report on several spectral features associated with Si impurity in diamond related to spectral hole-burning. Diamond, with its hardness and high temperature stability, is a potentially useful material for high temperature hole-burning storage. The first hole-burning in bulk diamonds [1] was observed from color centers in the spectra of N3 at 415 nm, H4 at 496 nm, N-V at 637 nm, and GR1 at 741 nm. Recently, hole-burning was observed for color centers N-V at 637 nm and 574 nm of electron irradiated chemical-vapor deposited (CVD) diamonds [2].
The persistent spectral hole burning effect has been observed for the nitrogen vacancy (NV) center and the 2.16 eV center in chemical-vapor deposited (CVD) diamond. This sideband is the first observation of spectral hole burning in CVD diamond. Holes are burned in the inhomogeneously broadened zero-phonon lines of both the centers by dye lasers. The holes were observed by photoluminescence excitation spectroscopy, with monitoring of the phonon-sideband emission, at temperatures up to 130 K for the NV center and up to 100 K for the 2.16 eV center.
Persistent spectral hole-burning (PHB) of inhomogeneously broadened absorption lines in solids occurs when a homogeneous class of absorbing centers in resonance with a narrowband laser beam undergoes a photolnduced change in optical absorption that persists for times longer than any excited state lifetime. Persistent spectral holes for impurity centers in solids can provide important information about guest–light and guest–host interactions, such as dephasing, Zeeman and Stark splittings, and photochemical reaction mechanisms.
Silicon-vacancy (SiV) centers in diamond are promising systems for quantum information applications due to their bright single-photon emission and optically accessible spin states. Furthermore, SiV centers in low-strain diamond are insensitive to perturbations of the dielectric environment; i.e., they show very weak spectral diffusion. This property renders ensembles of SiV centers interesting for sensing applications. We here report on photoluminescence excitation (PLE) spectroscopy on an SiV ensemble in a low strain, chemical vapor deposition-grown high-quality diamond layer, where we measure the fine structure with high resolution and obtain the line widths and splittings of the SiV centers. We investigate the temperature dependence of the width and position of the fine structure peaks. Our measurements reveal line widths of about 10 GHz as compared to a lifetime limited width on the order of 0.1 GHz. This difference arises from the inhomogeneous broadening of the transitions caused by residual strain. To overcome inhomogeneous broadening we use spectral hole burning spectroscopy, which enables us to measure a nearly lifetime limited homogeneous line width of 279 MHz. Furthermore, we demonstrate evidence of coherent interaction in the system by driving a $\mathrm{\ensuremath{\Lambda}}$ scheme. Additional measurements on single emitters created by ion implantation confirm the homogeneous line widths seen in the spectral hole burning experiments and relate the ground-state splitting to the decoherence rate.
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.