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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Suppression of phonon sidebands in the spectrum of nitrogen vacancy centers in diamond nano-crystals

Hong-Quan Zhao, Masazumi Fujiwara, Shigeki Takeuchi

Published Feb 9, 2012• 1 citation
Publisher

Abstract

We report the substrate effects on the zero-phonon transitions and suppression of phonon side bands in the NV center spectrum. Fluorescence spectra of NV centers in cryogenic temperatures were measured by depositing diamond nanocrystals on different substrates including glass slides, undoped Si, and silica (1~2μm) on undoped Si (SiO2/Si). We found that SiO2/Si substrate was an effective substrate to suppress the phonon side band from spectra of NV- centers. Temperature dependence of NV- zero-phonon line Debye-Waller factor on Si and SiO2/Si were measured, from 2.5K to 230K, Debye-Waller factor decreased linearly on both of the two substrates.

DOI
10.1117/12.906638

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We report the substrate effects on the zero-phonon transitions and suppression of phonon side bands in the NV center spectrum. Fluorescence spectra of NV centers in cryogenic temperatures were measured by depositing diamond nanocrystals on different substrates including glass slides, undoped Si, and silica (1~2μm) on undoped Si (SiO2/Si). We found that SiO2/Si substrate was an effective substrate to suppress the phonon side band from spectra of NV- centers. Temperature dependence of NV- zero-phonon line Debye-Waller factor on Si and SiO2/Si were measured, from 2.5K to 230K, Debye-Waller factor decreased linearly on both of the two substrates.
Substrates effect is observed on the suppression of the phonon sideband from nitrogen vacancy (NV) centers in 50nm diamond nanocrystals at cryogenic temperatures. As a quantitative parameter of the population of phonon sidebands, the Debye-Waller factor is estimated from fluorescence spectra on glass, silicon, and silica-on-silicon substrates. Fluorescence spectra of negatively charged NV centers in nanodiamonds on silica-on-silicon substrates have average and maximum Debye-Waller factors of 12.7% (which is about six times greater than that of samples on glass substrates) and 19.3%, respectively. This effect is expected to be very important for future applications of NV centers in quantum information science and nanosensing.
Recently, the nitrogen vacancy (NV) center has emerged as a deterministic single-photon source at room temperature. However, the presence of phonon sideband emission limits the use of NV centers in various quantum optical applications. Here we report a novel way to suppress the phonon sideband emission of NV centers aided with the enhancement of zero phonon line intensity using photonic crystals at room temperature. We study the photonic stop gap mediated charge state conversion in NV centers. The enhancement of phonon sideband emission from the same structures by implementing a different measurement geometry is also discussed. The studies open new avenues in studying the NV center-based quantum nanophotonics and biophotonics.
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.
Photoluminescence (PL) spectra of single nitrogen vacancy (NV) centers in 50-nm diamond nanocrystals at the zero-phonon line (ZPL) were directly observed using a Fabry-Perot interferometer at cryogenic temperatures. The narrowest linewidth of ZPL was 1.2 GHz (1.9 ± 0.7 GHz on average), comparable to ZPL linewidths in PL spectra reported for NV centers in pure bulk diamond. This observation is important to the application of NV centers for use in quantum communication and computation devices, and in nano-sensing.
We discuss charge state ratio-dependent spectral and temporal emission properties of nitrogen-vacancy (NV) centers in bulk diamonds. An understanding of the charge state ratio in artificially grown diamonds is important to design them for NV-based magnetometry. We show that the NV charge state ratio strongly correlates with the intensity of the zero-phonon line (ZPL) of NV−, which is supported by an emission dip at 2.87 GHz in spin-selective optical transitions. The Debye–Waller factor of NV centers depends on the charge state ratio, and it increases for NV− with an increase in the charge state ratio. We observe that the energy separation between the second phonon sideband (PSB) and ZPL does not scale multiplicatively with that of the energy separation between first PSB and ZPL. This deviation becomes more pronounced with an increase in charge state ratio, suggesting anharmonicity of vibrational energy levels, rather than the usually reported harmonicity. Further, we discuss the inherent relation between decay rates and charge states as a function of emission wavelengths. The excited state lifetime of NV0 remains constant, whereas the NV− lifetime decreases with an increase in the charge state ratio, with an overall decrease of 37%. Our results show an emission spectra-based approach to estimate the charge state ratio in diamond crystals, which is helpful for quantum-enhanced sensing and magnetometry.
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.