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arXiv:1804.05583 · AIP Advances

Diamond nano-pyramids with narrow linewidth SiV centers for quantum technologies

L. Nicolas, Tom Delord, Paul H. Huillery, Elke Neu, Gabriel Hetet

Published Jun 1, 2018• 15 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1063/1.5035484

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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.
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.
Producing nano-structures with embedded bright ensembles of lifetime-limited emitters is a challenge with potential high impact in a broad range of physical sciences. In this work, we demonstrate controlled charge transfer to and from dark states exhibiting very long lifetimes in high density ensembles of SiV centers hosted in a CVD-grown diamond nano-pyramid. Further, using a combination of resonant photoluminescence excitation and a frequency-selective persistent hole burning technique that exploits such charge state transfer, we could demonstrate close to lifetime-limited linewidths from the SiV centers. Such a nanostructure with thousands of bright narrow linewidth emitters in a volume much below λ3λ^3λ3 will be useful for coherent light-matter coupling, for biological sensing, and nanoscale thermometry.
The negatively charged silicon-vacancy center (SiV) in diamond is a potential high-quality source of single-indistinguishable photons for quantum information processing and quantum electrodynamics applications[1]. Protected by inversion symmetry, the SiV possesses bright narrow-band and spectrally stable optical transition. However, when embedded in bulk diamond, this emitter suffers from relatively low extraction efficiency attributed to total internal reflection as well as nondeterministic location. On the other hand, its implementation in nanodiamonds or nanostructures prepared by a top-down approach can mitigate the issue of total internal reflection, but impeded by optical dephasing owing to their degraded surface quality.
Abstract Silicon vacancy (SiV) centers in diamonds have attracted much attention because of their stability and narrow emission linewidth, and are promising for applications in quantum information technology. SiV-center-encapsulated nanodiamonds have also attracted much attention because of their potential to be coupled to various photonic devices. One efficient way to fabricate nanodiamonds that contain SiV centers is Si ion implantation into nanodiamonds. However, the evaluation of a single SiV center in a nanodiamond produced by this method at low temperatures has not been performed. In this study, we report on the optical properties of a single SiV center in a nanodiamond produced by ion implantation at cryogenic temperatures. The emission spectrum from a single SiV center ( g 2 ( 0 ) = 0.19 ) was observed with four distinct fine splittings of the zero-phonon line (ZPL) at 4 K. At an excitation power of 50 μ W, the full width at half maximum of the ZPL reached the spectrometer resolution limit (0.09 nm). The temperature dependence of the emission peak is consistent with that of the emission coming from an SiV center under high strain. The results obtained in this work suggest that nanodiamonds containing single SiV centers formed using this method will be an important building block for the realization of quantum information applications.
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.