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arXiv:1804.09141 · Physical review. B./Physical review. B

Electronic structure of the neutral silicon-vacancy center in diamond

Ben L. Green, Marcus W. Doherty, Eishin Nako, Neil B. Manson, Ulrika F. S. D’Haenens-Johansson, S. D. Williams, Daniel J. Twitchen, Mark E. Newton

Published Apr 17, 2019• 49 citations
arXivHTMLPDF

Abstract

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 ${\mathrm{SiV}}^{0}$ is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of ${\mathrm{SiV}}^{0}$ under uniaxial stress, we find the previous excited electronic structure of a single $^{3}A_{1u}$ 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 ${\mathrm{SiV}}^{0}$ .

DOI
10.1103/physrevb.99.161112

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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 (T2\ensuremath≈1{T}_{2}\ensuremath{\approx}1T2​\ensuremath≈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 3Eu\ensuremath-3A2u^{3}E_{u}\text{\ensuremath{-}}^{3}A_{2u}3Eu​\ensuremath-3A2u​ 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 .
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.
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.
The neutral silicon--vacancy (SiV0^{0}0) center in diamond combines inversion symmetry with optical emission, making it a robust quantum emitter resilient to stray electric fields. Using first-principles density-functional theory, we quantify its response to isotropic strain spanning strong compression and tensile regimes (effective hydrostatic pressures of approximately −80-80−80 to 180180180~GPa). The coexistence of doubly degenerate ege_geg​ and eue_ueu​ levels produces a structural instability captured by a quadratic product Jahn--Teller model. Under isotropic compression, the zero-phonon line blue-shifts nearly linearly while the EgE_gEg​ phonon stiffens, suppressing vibronic instabilities and reducing Jahn--Teller quenching. Consequently, the Ham-reduced excited-state spin--orbit splitting increases substantially and the dark--bright vibronic gap widens. In contrast, isotropic tensile strain enhances vibronic effects and induces symmetry breaking beyond a critical strain, with tunneling-mediated dynamical averaging at the onset. Throughout the symmetry-preserving regime, parity remains well defined, so isotropic strain alone does not activate the dark transition. Charge-transition levels indicate photostability of the emission deep into the compressive regime, and near the highest photostable deformation (∼100\sim 100∼100~GPa), the radiative lifetime increases due to a reduced transition dipole moment despite the increasing optical energy. These trends yield compact calibration relations linking optical and spin observables to isotropic strain and establish SiV0^{0}0 as a symmetry-protected, strain-tunable quantum emitter operating into the multi-megabar-equivalent regime.
Neutral silicon vacancy (SiV^{0}) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV^{0} centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign these states as bound exciton states using group theory and density functional theory. These bound exciton states enable new control schemes for SiV^{0} as well as other emerging defect systems.
High Resolution Image Download MS PowerPoint Slide The negatively charged silicon vacancy center (SiV – ) in diamond is a promising, yet underexplored candidate for single-spin quantum sensing at sub-kelvin temperatures and tesla-range magnetic fields. A key ingredient for such applications is the ability to perform all-optical, coherent addressing of the electronic spin of near-surface SiV – centers. We present a robust and scalable approach for creating individual, ∼50 nm deep SiV – with lifetime-limited optical linewidths in diamond nanopillars through an easy-to-realize and persistent optical charge-stabilization scheme. The latter is based on single, prolonged 445 nm laser illumination that enables continuous photoluminescence excitation spectroscopy without the need for any further charge stabilization or repumping. Our results constitute a key step toward the use of near-surface, optically coherent SiV – for sensing under extreme conditions, and offer a powerful approach for stabilizing the charge-environment of diamond color centers for quantum technology applications.
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.