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Applied Physics Letters

Persistent hole burning of the nitrogen vacancy center and the 2.16 eV center of chemical-vapor deposited diamond

Yoshihiro Yokota, Jing Sheng, Toshimichi Ito, Akio Hiraki, Atusi Kurita, Takashi Kushida, Hiroshi Kawarada

Published Nov 2, 1992• 9 citations
Publisher

Abstract

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.

DOI
10.1063/1.108299

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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.
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].
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.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.
Photoluminescence excitation spectroscopy of nitrogen vacancy (NV) centers in type Ib diamond nanocrystals shows that in spite of spectral diffusion and spin-nonconserving transitions, zero-phonon linewidth as small as 16MHz16\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}16MHz, which is nearly lifetime limited, can be observed at low temperature. Relatively small effects of spectral diffusion have also been observed in a small fraction of NV centers.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.
Abstract Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi-localized vibrational modes as well as ultrafast spectral diffusion on the picosecond timescale. The intrinsic, ensemble-averaged homogeneous linewidth is found to be in the tens of GHz range by extrapolating to zero temperature. We also observe a temperature-dependent Stark splitting of the excited state manifold, relevant to NV sensing protocols.