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arXiv:1705.10486 · New Journal of Physics

Photoluminescence excitation spectroscopy of SiV−and GeV−color center in diamond

Stefan Häußler, Gergő Thiering, Andreas Dietrich, Niklas Waasem, Tokuyuki Teraji, Junichi Isoya, Takayuki Iwasaki, Mutsuko Hatano, Fedor Jelezko, Ádám Gali, Alexander Kubanek

Published May 18, 2017• 106 citations

Abstract

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.

DOI: 10.1088/1367-2630/aa73e5

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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 $\mathrm{\ensuremath{\Lambda}}$ 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.

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.

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.

Silicon-vacancy (SiV) centers in diamond are gaining an increased interest for application, such as in quantum technologies and sensing. Due to the strong luminescence concentrated in its sharp zero-phonon line at room temperature, SiV centers are being investigated as single-photon sources for quantum communication, and also as temperature probes for sensing. Here, we discussed strategies for the fabrication of SiV centers in diamond based on Si-ion implantation followed by thermal activation. SiV color centers in high-quality single crystals have the best optical properties, but polycrystalline micro and nanostructures are interesting for applications in nano-optics. Moreover, we discuss the photoluminescence properties of SiV centers in phosphorous-doped diamond, which are relevant for the creation of electroluminescent devices, and nanophotonics strategies to improve the emission characteristics of the SiV centers. Finally, the optical properties of such centers at room and high temperatures show the robustness of the center and give perspectives for temperature-sensing applications.

Diamonds with impurity color centers are a novel class of functional materials with potential for various photonics applications such as quantum optics, metrology, sensorics, and life sciences. When introducing defect centers, a broad range of questions arises about the nature of the photophysical processes in the new materials, in particular regarding the relationship between spectral and morphological properties. Here we present results of comprehensive spectroscopic studies on diamond films with germanium-vacancy (GeV – ) centers, synthesized by chemical vapor deposition from gaseous germane (GeH 4 ). The combination of different techniques (emission and fluorescence excitation spectroscopy, epi-microscopy, and nanoscopy up to the single-emitter level) at room and cryogenic temperatures has shed light onto the spatial distribution of the spectral properties of the GeV – centers in different microregions of the diamond crystal and its relation to local strain/stress. We demonstrate a clear correlation between inhomogeneous broadening and morphological heterogeneities of the sample. Ultranarrow (tens of MHz) stable zero-phonon lines have been observed, which are a prerequisite for various applications.

Atomic-sized fluorescent defects in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. In this study, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.