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arXiv:1407.7137

Isotopically varying spectral features of silicon vacancy in diamond

Andreas Dietrich, Kay D. Jahnke, Jan Binder, Tokuyuki Teraji, Junichi Isoya, Lachlan J. Rogers, Fedor Jelezko

Published Jan 1, 2014• 0 citations
arXivHTMLPDF

Abstract

Abstract The silicon-vacancy centre ( ) in diamond has exceptional spectral properties for single-emitter quantum information applications. Most of the fluorescence is concentrated in a strong zero phonon line (ZPL), with a weak phonon sideband extending for 100 nm that contains several clear features. We demonstrate that the ZPL position can be used to reliably identify the silicon isotope present in a single centre. This is of interest for quantum information applications since only the 29Si isotope has nuclear spin. In addition, we show that the sharp 64 meV phonon peak is due to a local vibrational mode of the silicon atom. The presence of a local mode suggests a plausible origin of the measured isotopic shift of the ZPL.

DOI
10.18725/oparu-46210

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ACS Photonics•Dec 10, 2018•36 citations
Abstract The silicon-vacancy centre ( ) in diamond has exceptional spectral properties for single-emitter quantum information applications. Most of the fluorescence is concentrated in a strong zero phonon line (ZPL), with a weak phonon sideband extending for 100 nm that contains several clear features. We demonstrate that the ZPL position can be used to reliably identify the silicon isotope present in a single centre. This is of interest for quantum information applications since only the 29Si isotope has nuclear spin. In addition, we show that the sharp 64 meV phonon peak is due to a local vibrational mode of the silicon atom. The presence of a local mode suggests a plausible origin of the measured isotopic shift of the ZPL.
The silicon-vacancy centre ( ) in diamond has exceptional spectral properties for single-emitter quantum information applications. Most of the fluorescence is concentrated in a strong zero phonon line (ZPL), with a weak phonon sideband extending for 100 nm that contains several clear features. We demonstrate that the ZPL position can be used to reliably identify the silicon isotope present in a single centre. This is of interest for quantum information applications since only the 29 Si isotope has nuclear spin. In addition, we show that the sharp 64 meV phonon peak is due to a local vibrational mode of the silicon atom. The presence of a local mode suggests a plausible origin of the measured isotopic shift of the ZPL.
The neutrally charged silicon-vacancy defect (SiV 0 ) is a colour centre in diamond with spin S = 1, a zero-phonon line (ZPL) at 946 nm and long spin coherence, which makes it a promising candidate for quantum network applications. For the proper performance of such colour centres, all of them must have identical optical characteristics. However, in practice, there are factors that influence each individual centre. One of these factors is non-uniform isotope composition for both carbon atoms in diamond lattice and silicon atoms of dopant. In this work, we studied the isotopic shifts of SiV 0 centres for CVD-grown epitaxial layers of isotopically enriched 12 C and 13 C diamonds, as well as for diamond with natural isotope composition but doped only with one isotope of Si ( 28 Si, 29 Si and 30 Si). The detected shift was 1.60 meV for 12 C/ 13 C couple and 0.33 meV for 28 Si/ 29 Si and 29 Si/ 30 Si couples, which are close to the previously obtained values of the isotopic shift for the negatively charged silicon vacancy (SiV − ), which indicates a similar model of interaction with the environment for these two charge states of the SiV colour centres. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.
Photoluminescence (PL) spectra of single silicon vacancy (SiV) centers in diamond frequently feature very narrow room temperature PL lines in the near-infrared (NIR) spectral region, mostly between 820 nm and 840 nm, in addition to the well known zero-phonon line (ZPL) at approximately 738 nm [E. Neu et al., Phys. Rev. B 84, 205211 (2011)]. We here exemplarily prove for a single SiV center that this NIR PL is due to an additional purely electronic transition (ZPL). For the NIR line at 822.7 nm, we find a room temperature linewidth of 1.4 nm (2.6 meV). The line saturates at similar excitation power as the ZPL. The ZPL and NIR line exhibit identical polarization properties. Cross-correlation measurements between the ZPL and the NIR line reveal anticorrelated emission and prove that the lines originate from a single SiV center, furthermore indicating a fast switching between the transitions (0.7 ns). g(2){g}^{(2)}g(2) autocorrelation measurements exclude that the NIR line is a vibronic sideband or that it arises due to a transition from/to a metastable (shelving) state.
The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that SiV centers in nanodiamonds exhibit a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range ≈730–742 nm and broad linewidths between 5 and 17 nm, whereas the second group comprises a very broad distribution of center wavelengths between 715 and 835 nm, but narrow linewidths from below 1 up to 4 nm. Supported by ab initio Kohn–Sham density functional theory calculations we show that the ZPL shifts of the first group are consistently explained by strain in the diamond lattice. Further, we suggest, that the second group showing the strongly inhomogeneous distribution of center wavelengths might be comprised of a new class of silicon-related defects. Whereas single photon emission is demonstrated for defect centers of both clusters, we show that emitters from different clusters show different spectroscopic features such as variations of the phonon sideband spectra and different blinking dynamics.
The properties of the negatively charged silicon-vacancy (SiV) centre in diamond were investigated in this thesis. Polarisation measurements revealed transition dipoles and the symmetry groups of the centre. In a diamond grown by chemical vapour deposition, a high spectral overlap of SiV centres with nearly transform limited optical line widths was found pointing to a low sensitivity of SiV centres to both strain and local electric fields. This low inhomogeneous distribution allowed for a quantum interference leading to a contrast of over 70 % in a Hong-Ou-Mandel experiment. Additionally, an isotopic shift at single site level could be confirmed and than used to identify the 64meV peak in the phonon sideband as a local vibrational mode. A low temperature investigation of optical line width and orbital relaxation time indicated a direct single-phonon process between the orbital states while at higher temperatures a two-phonon dephasing was found to be the main electron-phonon process. The results were consistently described by the microscopic model developed and additional strength was added by consistent studies of spin-orbit splitting and optical lifetime. By applying a magnetic field the spin degeneracy in the ground state was lifted allowing for spin initialisation with over 95 % fidelity with a spin relaxation time of over 2 milliseconds. Two resonant lasers were used to demonstrate coherent population trapping leading to a coherence time in the order of the orbital relaxation time. The coherence was concluded to be limited by orbital dephasing processes and we propose techniques to overcome them. One of them is to use nanodiamonds with a size smaller than half the phonon wavelength to suppress the dephasing process. Investigating the spectral properties at cryogenic temperatures, nearly lifetime limited line widths have been found, making these nanodiamonds good candidates for further spin applications with SiV centres.
Silicon-vacancy (SiV – ) color center in diamond is of high interest for applications in nanophotonics and quantum information technologies, as a single photon emitter with excellent spectral properties. To obtain spectrally identical SiV – emitters, we doped homoepitaxial diamond films in situ with 28 Si, 29 Si, and 30 Si isotopes using isotopically enriched (>99.9%) silane SiH 4 gas added in H 2 –CH 4 mixtures in the course of the microwave plasma-assisted chemical vapor deposition process. Zero-phonon line components as narrow as ∼4.8 GHz were measured in both absorption and luminescence spectra for the monoisotopic SiV – ensembles with a concentration of a few parts per billion. We determined with high accuracy the Si isotopic energy shift of SiV – zero-phonon line. The SiV – emission intensity is shown to be easily controlled by the doped epifilm thickness. Also, we identified and characterized the localized single photon SiV – sources. The developed doping process opens a way to produce the SiV – emitter ensembles with energy confined in an extremely narrow range.