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arXiv:1210.3201 · New Journal of Physics

Low-temperature investigations of single silicon vacancy colour centres in diamond

Elke Neu, Christian Hepp, Michael Zwicky Hauschild, S. Gsell, Martin Fischer, Hadwig Sternschulte, Doris Steinmüller‐Nethl, M. Schreck, Christoph Becher

Published Apr 4, 2013• 190 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1367-2630/15/4/043005

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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). ${g}^{(2)}$ 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.

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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.
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.
We introduce a process for the fabrication of high-quality, spatially isolated nano-diamonds on iridium via microwave-plasma-assisted chemical vapour deposition (CVD) growth. We perform spectroscopy of single silicon-vacancy (SiV) centres produced during the growth of the nano-diamonds. The colour centres exhibit extraordinary narrow zero-phonon-lines down to 0.7 nm at room temperature. Single photon count rates up to 4.8 Mcps at saturation make these SiV centres the brightest diamond-based single photon sources to date. We measure for the first time the fine structure of a single SiV centre, thus confirming the atomic composition of the investigated colour centres.
Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~10 3 ) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.
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.
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.
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.