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ACS Photonics

Effect of Negative Thermal Expansion on the Zero-Phonon Line of Implanted Silicon Vacancy Color Centers in Diamond

Stephen Revesz, Adolfo Misiara, John Abraham, Edward S. Bielejec, Hebin Li, Michael Titze

Published May 15, 2024• 8 citations
Publisher

Abstract

The charged silicon vacancy (SiV – ) color center in diamond can be created by focused ion beam (FIB) implantation, allowing deterministic creation of single photon emitters. Here, we create FIB-implanted SiV – color centers in a diamond substrate spanning 8 orders of magnitude of the ion beam fluence. We show that the SiV – zero-phonon line (ZPL) brightness at 4 K is constant with increasing ion beam fluence, while exhibiting slight inhomogeneous broadening. The temperature-dependent ZPL line shift revealed a blue-shift below 70 K that we attribute to the negative thermal expansion of diamond, showing the SiV – ability as a sensitive probe of its host crystal environment. We demonstrate a versatile line shift model constructed on the basis of the Grüneisen parameter description of the thermal expansion coefficient and the electron–phonon interaction.

DOI
10.1021/acsphotonics.3c01846

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The charged silicon vacancy (SiV – ) color center in diamond can be created by focused ion beam (FIB) implantation, allowing deterministic creation of single photon emitters. Here, we create FIB-implanted SiV – color centers in a diamond substrate spanning 8 orders of magnitude of the ion beam fluence. We show that the SiV – zero-phonon line (ZPL) brightness at 4 K is constant with increasing ion beam fluence, while exhibiting slight inhomogeneous broadening. The temperature-dependent ZPL line shift revealed a blue-shift below 70 K that we attribute to the negative thermal expansion of diamond, showing the SiV – ability as a sensitive probe of its host crystal environment. We demonstrate a versatile line shift model constructed on the basis of the Grüneisen parameter description of the thermal expansion coefficient and the electron–phonon interaction.
Among promising color centers for single-photon sources in diamond, the negatively charged silicon-vacancy (SiV − ) has 70% of its emission to the zero-phonon line (ZPL), in contrast to the negatively charged nitrogen vacancy (NV − ), which has a broad spectrum. Fabricating single centers of useful defect complexes with high yield and excellent grown-in defect properties by ion implantation has proven to be challenging. We have fabricated bright single SiV − centers by 60-keV focused ion beam implantation and subsequent annealing at 1000 °C with high positioning accuracy and a high yield of 15%.
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.
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.
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.
Abstract Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV − ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)‐based SiV − centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV − centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV − centers featuring stable high‐purity single‐photon emission through Si implantation into NDs with an average size of ∼20 nm. We observe room temperature emission, with zero‐phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group‐IV diamond color centers with applications in quantum photonics, sensing, and biomedicine.
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.