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arXiv:1310.3131 · Physical Review B

Electronic structure of the negatively charged silicon-vacancy center in diamond

Lachlan J. Rogers, Kay D. Jahnke, Marcus W. Doherty, Andreas Dietrich, Liam Paul McGuinness, Christoph Müller, Tokuyuki Teraji, Hitoshi Sumiya, Junichi Isoya, Neil B. Manson, Fedor Jelezko

Published Jun 2, 2014• 227 citations
arXivHTMLPDF

Abstract

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 ${\mathrm{D}}_{3\mathrm{d}}$ 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.

DOI
10.1103/physrevb.89.235101

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The negatively charged silicon-vacancy (SiV\ensuremath−{}^{\ensuremath{-}}\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⟨111\ensuremath⟩\ensuremath{\langle}111\ensuremath{\rangle}\ensuremath⟨111\ensuremath⟩ 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.
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.
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 negatively charged silicon-vacancy center (SiV) in diamond is a potential high-quality source of single-indistinguishable photons for quantum information processing and quantum electrodynamics applications[1]. Protected by inversion symmetry, the SiV possesses bright narrow-band and spectrally stable optical transition. However, when embedded in bulk diamond, this emitter suffers from relatively low extraction efficiency attributed to total internal reflection as well as nondeterministic location. On the other hand, its implementation in nanodiamonds or nanostructures prepared by a top-down approach can mitigate the issue of total internal reflection, but impeded by optical dephasing owing to their degraded surface quality.
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.
The negatively charged silicon-vacancy center (SiV) in diamond is a potential high-quality single-photon source for quantum information processing and quantum electrodynamics applications[1]. The dipole moment of the SiV is aligned predominantly along its symmetry axis which connects the interstitial silicon atom and the two adjacent vacancies with 4 possible-orientations. Since the SiV addressing is done optically the demand for efficient excitation and optical out-coupling is essential for realizing high-quality single-photon sources. In addition to relatively low extraction efficiency when embedded in bulk diamond, attributed to total internal reflection, in a-oriented diamond, which is commonly used, each SiV possesses a dominant dipole component aligned normal to the diamond-air interface. Thus, resulting in a poor optical out-coupling since a dipole radiates primarily into the plane orthogonal to its axis.
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 .