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arXiv:1603.04295 · Physical review. B./Physical review. B

Photoluminescence excitation and spectral hole burning spectroscopy of silicon vacancy centers in diamond

Carsten Arend, Jonas N. Becker, Hadwig Sternschulte, Doris Steinmüller‐Nethl, Christoph Becher

Published Jul 5, 2016• 43 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevb.94.045203

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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 \ensuremathΛ\mathrm{\ensuremath{\Lambda}}\ensuremathΛ 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.
Color centers in diamond are important quantum emitters for a broad range of applications ranging from quantum sensing to quantum optics. Understanding the internal energy level structure is of fundamental importance for future applications. We experimentally investigate the level structure of an ensemble of few negatively charged silicon-vacancy (SiV − ) and germanium-vacancy (GeV − ) centers in bulk diamond at room temperature by photoluminescence (PL) and excitation (PLE) spectroscopy over a broad wavelength range from 460 to and perform power-dependent saturation measurements. For SiV − our experimental results confirm the presence of a higher energy transition at . By comparison with detailed theoretical simulations of the imaginary dielectric function we interpret the transition as a dipole-allowed transition from -state to -state where the corresponding a 2 u -level lies deeply inside the diamond valence band. Therefore, the transition is broadened by the diamond band. At higher excitation power of we indicate signs of a parity-conserving transition at supported by saturation measurements. For GeV − we demonstrate that the PLE spectrum is in good agreement with the mirror image of the PL spectrum of the zero-phonon line. Experimentally we do not observe a higher lying energy level up to a transition wavelength of . The observed PL spectra are identical, independent of excitation wavelength, suggesting a rapid decay to excited state and followed by optical transition to ground state. Our investigations convey important insights for future quantum optics and quantum sensing experiments based on SiV − -center and GeV − -center in diamond.
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.
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.
The persistent spectral hole burning effect has been observed for the nitrogen vacancy (NV) center and the 2.16 eV center in chemical-vapor deposited (CVD) diamond. This sideband is the first observation of spectral hole burning in CVD diamond. Holes are burned in the inhomogeneously broadened zero-phonon lines of both the centers by dye lasers. The holes were observed by photoluminescence excitation spectroscopy, with monitoring of the phonon-sideband emission, at temperatures up to 130 K for the NV center and up to 100 K for the 2.16 eV center.
Color centers in diamond are versatile solid state atomic-like systems suitable for quantum technological applications. In particular, the negatively charged silicon vacancy center (SiV) exhibits a narrow photoluminescence (PL) line and lifetime-limited linewidth in a bulk at cryogenic temperature. We present a low-temperature study of chemical vapour deposition (CVD)-grown diamond nano-pyramids containing SiV centers. The PL spectra feature a bulk-like zero-phonon line with ensembles of SiV centers, with a linewidth below 10 GHz which demonstrates very low crystal strain for such a nano-object.