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arXiv:2006.11878 · Physical review. B./Physical review. B

Electronic structure and magneto-optical properties of silicon-nitrogen-vacancy complexes in diamond

Marcin Roland Zemła, Kamil Czelej, Paulina Kamińska, Chris G. Van de Walle, Jacek A. Majewski

Published Sep 1, 2020• 26 citations
arXivHTMLPDF

Abstract

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 $C$ band of telecom wavelengths and its paramagnetic nature. In addition, the optical transition associated with the ${\mathrm{SiNV}}^{0}$ 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.

DOI
10.1103/physrevb.102.115102

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arXiv:1804.09141•Physical review. B./Physical review. B•Apr 17, 2019•49 citations
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∼1530nm\ensuremath{\sim}1530\phantom{\rule{0.28em}{0ex}}\mathrm{nm}\ensuremath∼1530nm, 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.
Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.
We demonstrate optical spin polarization of the neutrally charged silicon-vacancy defect in diamond (SiV^{0}), an S=1 defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but nonzero at below-resonant energies. We measure an ensemble spin coherence time T_{2}>100 μs at low-temperature, and a spin relaxation limit of T_{1}>25 s. Optical spin-state initialization around 946 nm allows independent initialization of SiV^{0} and NV^{-} within the same optically addressed volume, and SiV^{0} emits within the telecoms down-conversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that SiV^{0} is a promising candidate for a long-range quantum communication technology.
Color centers in diamond have emerged as leading solid-state ``artificial atoms'' for a range of quantum technologies, from quantum sensing to quantum networks. Concerted research activities are now underway to identify new color centers that combine stable spin and optical properties of the nitrogen vacancy (${\mathrm{NV}}^{\ensuremath{-}}$) with the spectral stability of the silicon vacancy (${\mathrm{SiV}}^{\ensuremath{-}}$) centers in diamond, with recent research identifying other group-IV color centers with superior properties. In this paper, we investigate a class of diamond quantum emitters from first principles, the group-III color centers, which we show to be thermodynamically stable in a spin-1, electric-field-insensitive structure. From ab initio electronic structure methods, we characterize the product Jahn-Teller (pJT) effect present in the excited-state manifold of these group-III color centers, where we capture symmetry-breaking distortions associated with strong electron-phonon coupling. These predictions can guide experimental identification of group-III vacancy centers and their use in applications in quantum information science and technology.
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 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.
The neutrally charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency optical spin initialization with long spin lifetimes (${T}_{2}\ensuremath{\approx}1$ ms at 4 K) and up to 90% of optical emission into its 946-nm zero-phonon line. However, the electronic structure of SiV0{\mathrm{SiV}}^{0}SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0{\mathrm{SiV}}^{0}SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u^{3}A_{1u}3A1u​ state is incorrect, and identify instead a coupled $^{3}E_{u}\text{\ensuremath{-}}^{3}A_{2u}$ system, the lower state of which has forbidden optical emission at zero stress and efficiently decreases the total emission of the defect. We propose a solution employing finite strain to define a spin-photon interface scheme using SiV0{\mathrm{SiV}}^{0}SiV0 .