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arXiv:1310.3106 · Physical Review Letters

Electronic Structure of the Silicon Vacancy Color Center in Diamond

Christian Hepp, Tina Müller, Victor Waselowski, Jonas N. Becker, Benjamin Pingault, Hadwig Sternschulte, Doris Steinmüller‐Nethl, Ádám Gali, Jeronimo R. Maze, Mete Atatüre, Christoph Becher

Published Jan 24, 2014• 435 citations
arXivHTMLPDF

Abstract

The negatively charged silicon vacancy (SiV) color center in diamond has recently proven its suitability for bright and stable single photon emission. However, its electronic structure so far has remained elusive. We here explore the electronic structure by exposing single SiV defects to a magnetic field where the Zeeman effect lifts the degeneracy of magnetic sublevels. The similar responses of single centers and a SiV ensemble in a low strain reference sample prove our ability to fabricate almost perfect single SiVs, revealing the true nature of the defect's electronic properties. We model the electronic states using a group-theoretical approach yielding a good agreement with the experimental observations. Furthermore, the model correctly predicts polarization measurements on single SiV centers and explains recently discovered spin selective excitation of SiV defects.

DOI
10.1103/physrevlett.112.036405

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The negatively charged silicon vacancy (SiV) color center in diamond has recently proven its suitability for bright and stable single photon emission. However, its electronic structure so far has remained elusive. We here explore the electronic structure by exposing single SiV defects to a magnetic field where the Zeeman effect lifts the degeneracy of magnetic sublevels. The similar responses of single centers and a SiV ensemble in a low strain reference sample prove our ability to fabricate almost perfect single SiVs, revealing the true nature of the defect's electronic properties. We model the electronic states using a group-theoretical approach yielding a good agreement with the experimental observations. Furthermore, the model correctly predicts polarization measurements on single SiV centers and explains recently discovered spin selective excitation of SiV defects.
Color centers in diamond are point defects within the diamond host lattice that absorb and emit light at optical frequencies. Besides contributing to the striking visual characteristics of "fancy colored" diamonds as gemstones, the centers--particularly the negatively charged nitrogen-vacancy (NV) center and silicon-vacancy (SiV-) center--offer a number of possibilities for quantum computation and quantum information processing. In this talk, I will summarize recent progress made in characterizing negatively charged silicon-vacancy centers in diamond using the technique of optical multidimensional coherent spectroscopy (MDCS). By comparing photoluminescence-based and heterodyne-detection based signal collection schemes in a high-density SiV- center sample, we have selectively identified a population of long-lived and nonradiative silicon-vacancy centers in diamond with more than 40 times as much inhomogeneous spectral broadening as the radiative silicon-vacancy center states that are more commonly observed using photoluminescence. Estimates of the degree of inhomogeneity and overall sample characteristics indicate that strain is likely to play a large role in the formation of these nonradiative states. The findings open possibilities for being able to actively tune the degree of radiative coupling in silicon-vacancy center systems, opening possibilities for new types of quantum-optical devices.
The silicon-vacancy (SiV) and nitrogen-vacancy (NV) centers in diamond are commonly regarded as prototypical defects for solid-state quantum information processing. Here, we show that when silicon and nitrogen are simultaneously introduced into the diamond lattice, these defects can strongly interact and form larger complexes. Nitrogen atoms strongly bind to Si and SiV centers, and complex formation can occur. Using a combination of hybrid density functional theory and group theory, we analyze the electronic structure and provide various useful physical properties, such as hyperfine structure, quasilocal vibrational modes, and a zero-phonon line, to enable experimental identification of these complexes. We demonstrate that the presence of substitutional silicon adjacent to nitrogen significantly shifts the donor level toward the conduction band, resulting in an activation energy for the SiN center that is comparable to phosphorus. We also find that the neutral SiNV center is of particular interest due to its photon emission at $\ensuremath{\sim}1530\phantom{\rule{0.28em}{0ex}}\mathrm{nm}$, which falls within the CCC band of telecom wavelengths and its paramagnetic nature. In addition, the optical transition associated with the SiNV0{\mathrm{SiNV}}^{0}SiNV0 color center exhibits very small electron-phonon coupling (Huang-Rhys factor = 0.78) resulting in high quantum efficiency (Debye-Waller factor = 46%) for single-photon emission. These features render this new center very attractive for a potential application in scalable quantum telecommunication networks.
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 negatively charged silicon-vacancy (SiV${}^{\ensuremath{-}}$) center in diamond is a promising single-photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\ensuremath{\langle}111\ensuremath{\rangle}$ aligned split-vacancy structure with D3d{\mathrm{D}}_{3\mathrm{d}}D3d​ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738-nm optical resonance.
Electrically driven emission from negatively charged silicon-vacancy (SiV)− centers in single crystal diamond is demonstrated. The SiV centers were generated using ion implantation into an i region of a p-i-n single crystal diamond diode. Both electroluminescence and the photoluminescence signals exhibit the typical emission that is attributed to the (SiV)− centers. Under forward and reversed biased PL measurements, no signal from the neutral (SiV)0 defect could be observed. The realization of electrically driven (SiV)− emission is promising for scalable nanophotonics devices employing color centers in single crystal diamond.
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.