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Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences

SiV 0 centres in diamond: effect of isotopic substitution in carbon and silicon

Kirill N. Boldyrev, Eduard S. Sektarov, A. P. Bolshakov, Victor Ralchenko, Vadim Sedov

Published Dec 3, 2023• 3 citations
Publisher

Abstract

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'.

DOI
10.1098/rsta.2023.0170

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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'.
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.
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 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.
This thesis reports research conducted on point defects in single crystal diamond utilising the complementary techniques of electron paramagnetic resonance (EPR), optical absorption and photoluminescence (PL) spectroscopy. Intentional silicon-doping of chemical vapour deposition (CVD) diamond allowed the production of samples grown on differently oriented substrates and containing distinct silicon isotopic abundances. The EPR spectrum of the neutral charge state of the silicon split-vacancy centre in diamond, (Si-V)0, has been characterised in the literature. Evidence for the assignment of the 1.31 eV zero phonon line (ZPL) seen in absorption and PL to the 3A2g -> 3A1u transition arising at (Si-V)0 is presented. Reversible charge transfer between the negatively charged centre, (Si-V)− (ZPL at 1.68 eV), and (Si-V)0 enabled the determination of calibration factors relating defect concentrations to their respective ZPL intensities. Preferential alignment of trigonal centres, such as (Si-V), in CVD material grown on {110}-substrates has been observed. The formation of (Si-V) centres during CVD synthesis and via irradiation and annealing of silicon-doped diamond was studied. Variable temperature EPR spectroscopy under illumination was used to investigate the optical spin polarisation (SP) of the (Si-V)0 3A2g ground state. Two different mechanisms for the SP are considered; selective intersystem crossing of (Si-V)0, and photoionisation of (Si-V)−. The properties of (Si-V)0 are compared to those of the extensively studied negatively charged nitrogen vacancy centre, (N-V)−. The effective spin-lattice relaxation and spin polarisation rates for both centres during continuous illumination are explored using pulsed EPR methods. A new defect, labelledWAR3, with spin S = 1 2 was observed in silicon-doped diamond and characterised using multifrequency EPR. Analysis of the data revealed that WAR3 is the neutral charge state of a silicon divacancy complex decorated by a hydrogen atom, (Si-V2:H)0. The experimentally derived 29Si and 1H hyperfine parameters are in good agreement with the values calculated using the spindensity- functional technique, confirming this model and ruling out a non-planar structure.
We demonstrate optical spin polarization of the neutrally charged silicon-vacancy defect in diamond (SiV^{0}), an S=1 defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but nonzero at below-resonant energies. We measure an ensemble spin coherence time T_{2}>100 μs at low-temperature, and a spin relaxation limit of T_{1}>25 s. Optical spin-state initialization around 946 nm allows independent initialization of SiV^{0} and NV^{-} within the same optically addressed volume, and SiV^{0} emits within the telecoms down-conversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that SiV^{0} is a promising candidate for a long-range quantum communication technology.
We study single silicon vacancy (SiV) centres in chemical vapour deposition (CVD) nanodiamonds on iridium as well as an ensemble of SiV centres in a high-quality, low-stress CVD diamond film by using temperature-dependent luminescence spectroscopy in the temperature range 5–295 K. We investigate in detail the temperature-dependent fine structure of the zero-phonon line (ZPL) of the SiV centres. The ZPL transition is affected by inhomogeneous as well as temperature-dependent homogeneous broadening and blue shifts by about 20 cm −1 upon cooling from room temperature to 5 K. We employ excitation power-dependent g (2) measurements to explore the temperature-dependent internal population dynamics of single SiV centres and infer mostly temperature-independent dynamics.