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arXiv:1207.0645 · Optics Express

Photophysics of single silicon vacancy centers in diamond: implications for single photon emission

Elke Neu, Mario Agio, Christoph Becher

Published Aug 15, 2012• 191 citations
arXivHTMLPDF

Abstract

Single silicon vacancy (SiV) color centers in diamond have recently shown the ability for high brightness, narrow bandwidth, room temperature single photon emission. This work develops a model describing the three level population dynamics of single SiV centers in diamond nanocrystals on iridium surfaces including an intensity dependent de-shelving process. Furthermore, we investigate the brightness and photostability of single centers and find maximum single photon rates of 6.2 Mcps under continuous excitation. We investigate the collection efficiency of the fluorescence and estimate quantum efficiencies of the SiV centers.

DOI
10.1364/oe.20.019956

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Single silicon vacancy (SiV) color centers in diamond have recently shown the ability for high brightness, narrow bandwidth, room temperature single photon emission. This work develops a model describing the three level population dynamics of single SiV centers in diamond nanocrystals on iridium surfaces including an intensity dependent de-shelving process. Furthermore, we investigate the brightness and photostability of single centers and find maximum single photon rates of 6.2 Mcps under continuous excitation. We investigate the collection efficiency of the fluorescence and estimate quantum efficiencies of the SiV centers.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
The silicon vacancy (SiV) color centers in diamond have significant potential in the fields of quantum information, nanophotonics, bioimaging and sensing, due to its good structural stability at room temperature, strong photostability, short luminescence lifetime, narrow zero-phonon line bandwidth, and avoidance of biological autofluorescence. They have attracted extensive attention and in-depth research from researchers. The applications of SiV color centers in the above areas require addressing key issues such as control over the number and charge state of SiV color centers in diamond, as well as improving the luminous efficiency. Therefore, this review summarizes some recent relevant research progress, including common methods for preparing SiV color centers, control over their luminescence intensity, preparation of SiV single-photon sources, and research on the control of SiV color center charge states. Based on these, an outlook is provided for the preparation and application of SiV color centers in diamond.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size 50 nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.
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.
Optical sources that deliver single photons on demand play a key role in quantum cryptography and optical quantum computations. At present, color centers in wide-bandgap semiconductors, such as the nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers in diamond, are considered to be the most promising candidates for practical quantum information applications owing to their unique emission properties at room temperature. However, for practical reasons, single-photon sources should be pumped electrically, which is required for integrability, scalability, and energy efficiency. However, diamond and related wide-bandgap semiconductor materials are at the interface between insulators and semiconductors, which makes electrical excitation of color centers very challenging. Here, we report on our progress in the understanding of single-photon electroluminescence of color centers in diamond, discuss different factors affecting the brightness of these emitter under electrical excitation, and study how to improve the performance of electrically- pumped single-photon sources based on color centers in diamond.