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arXiv:1108.3743 · Physical Review B

Fluorescence and polarization spectroscopy of single silicon vacancy centers in heteroepitaxial nanodiamonds on iridium

Elke Neu, Martin Fischer, S. Gsell, M. Schreck, Christoph Becher

Published Nov 15, 2011• 91 citations
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Abstract

We introduce an advanced material system for the production and spectroscopy of single silicon vacancy (SiV) color centers in diamond. We use microwave plasma chemical vapor deposition to synthesize heteroepitaxial nanodiamonds of approximately 160 nm in lateral size with a thickness of approximately 75 nm. These oriented ``nanoislands'' combine the enhanced fluorescence extraction from subwavelength-sized nanodiamonds with defined crystal orientation. The investigated SiV centers display narrow zero-phonon lines down to 0.7 nm in the wavelength range 730--750 nm. We investigate in detail the phonon coupling and vibronic sidebands of single SiV centers, revealing significant inhomogeneous effects. Polarization measurements reveal polarized luminescence and preferential absorption of linearly polarized light.

DOI
10.1103/physrevb.84.205211

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We introduce an advanced material system for the production and spectroscopy of single silicon vacancy (SiV) color centers in diamond. We use microwave plasma chemical vapor deposition to synthesize heteroepitaxial nanodiamonds of approximately 160 nm in lateral size with a thickness of approximately 75 nm. These oriented ``nanoislands'' combine the enhanced fluorescence extraction from subwavelength-sized nanodiamonds with defined crystal orientation. The investigated SiV centers display narrow zero-phonon lines down to 0.7 nm in the wavelength range 730--750 nm. We investigate in detail the phonon coupling and vibronic sidebands of single SiV centers, revealing significant inhomogeneous effects. Polarization measurements reveal polarized luminescence and preferential absorption of linearly polarized light.
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 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.
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 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.
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.
We investigate native nitrogen (NV) and silicon vacancy (SiV) color centers in commercially available, heteroepitaxial, wafer-sized, mm thick, single-crystal diamond. We observe single, native NV centers with a density of roughly 1 NV per μm3μm^3μm3 and moderate coherence time (T2=5μsT_2 = 5 μsT2​=5μs) embedded in an ensemble of SiV centers. Low-temperature spectroscopy of the SiV zero phonon line fine structure witnesses high crystalline quality of the diamond especially close to the growth surface, consistent with a reduced dislocation density. Using ion implantation and plasma etching, we verify the possibility to fabricate nanostructures with shallow color centers rendering our diamond material promising for fabrication of nanoscale sensing devices. As this diamond is available in wafer-sizes up to 100mm100 mm100mm it offers the opportunity to up-scale diamond-based device fabrication.