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Multiphoton-Excited Fluorescence of Silicon-Vacancy Color Centers in Diamond

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 Added by James Higbie
 Publication date 2017
  fields Physics
and research's language is English




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Silicon-vacancy color centers in nanodiamonds are promising as fluorescent labels for biological applications, with a narrow, non-bleaching emission line at 738,nm. Two-photon excitation of this fluorescence offers the possibility of low-background detection at significant tissue depth with high three-dimensional spatial resolution. We have measured the two-photon fluorescence cross section of a negatively-charged silicon vacancy (SiV$^-$) in ion-implanted bulk diamond to be $0.74(19) times 10^{-50}{rm cm^4;s/photon}$ at an excitation wavelength of 1040,nm. In comparison to the diamond nitrogen vacancy (NV) center, the expected detection threshold of a two-photon excited SiV center is more than an order of magnitude lower, largely due to its much narrower linewidth. We also present measurements of two- and three-photon excitation spectra, finding an increase in the two-photon cross section with decreasing wavelength, and discuss the physical interpretation of the spectra in the context of existing models of the SiV energy-level structure.



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Single crystal diamond membranes that host optically active emitters are highly attractive components for integrated quantum nanophotonics. In this work we demonstrate bottom-up synthesis of single crystal diamond membranes containing the germanium vacancy (GeV) color centers. We employ a lift-off technique to generate the membranes and perform chemical vapour deposition in a presence of germanium oxide to realize the insitu doping. Finally, we show that these membranes are suitable for engineering of photonic resonators such as microring cavities with quality factors of 1500. The robust and scalable approach to engineer single crystal diamond membranes containing emerging color centers is a promising pathway for realization of diamond integrated quantum nanophotonic circuits on a chip.
The spatial resolution and fluorescence signal amplitude in stimulated emission depletion (STED) microscopy is limited by the photostability of available fluorophores. Here, we show that negatively-charged silicon vacancy (SiV) centers in diamond are promising fluorophores for STED microscopy, owing to their photostable, near-infrared emission and favorable photophysical properties. A home-built pulsed STED microscope was used to image shallow implanted SiV centers in bulk diamond at room temperature. The SiV stimulated emission cross section for 765-800 nm light is found to be (4.0 +/- 0.3) x 10^(-17) cm^2, which is approximately 2-4 times larger than that of the negatively-charged diamond nitrogen vacancy center and approaches that of commonly-used organic dye molecules. We performed STED microscopy on isolated SiV centers and observed a lateral full-width-at-half-maximum spot size of 89 +/- 2 nm, limited by the low available STED laser pulse energy (0.4 nJ). For a pulse energy of 5 nJ, the resolution is expected to be ~20 nm. We show that the present microscope can resolve SiV centers separated by <150 nm that cannot be resolved by confocal microscopy.
We characterize a high-density sample of negatively charged silicon-vacancy (SiV$^-$) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of ce{SiV^-} centers that is not typically observed in photoluminescence, and which exhibits significant spectral inhomogeneity and extended electronic $T_2$ times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.
We demonstrate a new approach for engineering group IV semiconductor-based quantum photonic structures containing negatively charged silicon-vacancy (SiV$^-$) color centers in diamond as quantum emitters. Hybrid SiC/diamond structures are realized by combining the growth of nanoand micro-diamonds on silicon carbide (3C or 4H polytype) substrates, with the subsequent use of these diamond crystals as a hard mask for pattern transfer. SiV$^-$ color centers are incorporated in diamond during its synthesis from molecular diamond seeds (diamondoids), with no need for ionimplantation or annealing. We show that the same growth technique can be used to grow a diamond layer controllably doped with SiV$^-$ on top of a high purity bulk diamond, in which we subsequently fabricate nanopillar arrays containing high quality SiV$^-$ centers. Scanning confocal photoluminescence measurements reveal optically active SiV$^-$ lines both at room temperature and low temperature (5 K) from all fabricated structures, and, in particular, very narrow linewidths and small inhomogeneous broadening of SiV$^-$ lines from all-diamond nano-pillar arrays, which is a critical requirement for quantum computation. At low temperatures (5 K) we observe in these structures the signature typical of SiV$^-$ centers in bulk diamond, consistent with a double lambda. These results indicate that high quality color centers can be incorporated into nanophotonic structures synthetically with properties equivalent to those in bulk diamond, thereby opening opportunities for applications in classical and quantum information processing.
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