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ACS Photonics

Monoisotopic Ensembles of Silicon-Vacancy Color Centers with Narrow-Line Luminescence in Homoepitaxial Diamond Layers Grown in H2–CH4–[x]SiH4 Gas Mixtures (x = 28, 29, 30)

Victor Ralchenko, Vadim Sedov, Мартьянов Артём Константинович, A. P. Bolshakov, Kirill N. Boldyrev, Vladimir S. Krivobok, С. Н. Николаев, Stepan V. Bolshedvorskii, Olga R. Rubinas, Alexey V. Akimov, А.А. Khomich, E.V. Bushuev, R. A. Khmelnitsky, В. И. Конов

Published Dec 10, 2018• 36 citations
Publisher

Abstract

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.

DOI
10.1021/acsphotonics.8b01464

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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 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) 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.
Abstract Silicon-vacancy (SiV) centers in diamond are promising for quantum photonics due to their narrow zero-phonon line and excellent photonic properties. Here, we demonstrate controlled growth of delta-doped SiV layers in nanocrystalline diamond films by a single-step microwave plasma chemical vapor deposition growth process. By manipulating nitrogen flow during growth, we achieved a uniform layer of SiVs in diamond while maintaining consistent microstructural properties throughout the film. While a correlation between microstructural change and doping density is observed, optical emission spectroscopy analysis reveals that the mechanism between the two processes is different. Atom probe tomography confirms the uniform distribution of silicon atoms in the diamond matrix, even at concentrations as high as 3.6 × 1021 cm−3. The approach shows promise for the precise tuning of the layer thickness and doping concentration, and offers a scalable approach for creating high-quality SiV layers in diamond, advancing their integration into nanophotonic cavities for quantum technologies.
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.
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.
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.