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arXiv:1705.10205 · Physical Review Letters

Neutral Silicon-Vacancy Center in Diamond: Spin Polarization and Lifetimes

Ben L. Green, Sinead Mottishaw, Ben G. Breeze, Andrew Mark Edmonds, Ulrika F. S. D’Haenens-Johansson, Marcus W. Doherty, S. D. Williams, Daniel J. Twitchen, Mark E. Newton

Published Aug 31, 2017• 79 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.119.096402

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cond-mat.mtrl-sciCross-listedarXiv:2603.07265•Mar 10, 2026
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.
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.
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 .
Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. In this work, we present the observation of previously unreported optical transitions in SiV0 that are capable of efficiently polarizing the ground state spin. We assign groups of transitions from 825 to 890 nm to higher-lying excited states of SiV0 through a combination of optical and spin measurements. We interpret these spectroscopic lines as transitions to bound exciton states of the defect. Optical spin polarization via these bound exciton states enables the observation of optically detected magnetic resonance of SiV0.
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 neutrally charged silicon-vacancy defect (SiV 0 ) is a colour centre in diamond with spin S = 1, a zero-phonon line (ZPL) at 946 nm and long spin coherence, which makes it a promising candidate for quantum network applications. For the proper performance of such colour centres, all of them must have identical optical characteristics. However, in practice, there are factors that influence each individual centre. One of these factors is non-uniform isotope composition for both carbon atoms in diamond lattice and silicon atoms of dopant. In this work, we studied the isotopic shifts of SiV 0 centres for CVD-grown epitaxial layers of isotopically enriched 12 C and 13 C diamonds, as well as for diamond with natural isotope composition but doped only with one isotope of Si ( 28 Si, 29 Si and 30 Si). The detected shift was 1.60 meV for 12 C/ 13 C couple and 0.33 meV for 28 Si/ 29 Si and 29 Si/ 30 Si couples, which are close to the previously obtained values of the isotopic shift for the negatively charged silicon vacancy (SiV − ), which indicates a similar model of interaction with the environment for these two charge states of the SiV colour centres. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.
Spin defects in diamond are promising platforms for quantum sensing. The longest electron spin relaxation times (T1T_1T1​) at room temperature for solid-state defects are observed in nitrogen vacancy centers in diamond, which can reach 6.67 ms, and substitutional nitrogen ("P1 centers") in diamond, which exhibit a T1T_1T1​ of 2 ms. No other solid-state defect has exhibited millisecond-scale spin relaxation times at room temperature thus far. Here, we characterize the spin properties of the WAR5 defect in diamond with pulsed electron spin resonance. The observed T1T_1T1​ is one of the longest for solid-state spin defects: 0.97(27) ms at room temperature and 14.38(19) min at 4 K. The observed coherence time (T2T_2T2​) is 246(7) μμμs, which can be extended to 6.49(34) ms at 4 K with dynamical decoupling. Furthermore, we demonstrate optical spin polarization with a range of wavelengths from 405 nm to 500 nm and propose potential zero-phonon line candidates.