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arXiv:2209.08710 · Physical Review Applied

Neutral Silicon-Vacancy Centers in Diamond via Photoactivated Itinerant Carriers

Zi-Huai Zhang, Andrew Mark Edmonds, Nicola Palmer, Matthew Markham, Nathalie P. de Leon

Published Mar 7, 2023• 14 citations
arXivHTMLPDF

Abstract

Neutral silicon-vacancy ($\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}$) centers in diamond are promising candidates for quantum network applications because of their exceptional optical properties and spin coherence. However, the stabilization of $\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}$ centers requires careful Fermi-level engineering of the diamond host material, making further technological development challenging. Here, we show that $\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}$ centers can be efficiently stabilized by photoactivated itinerant carriers. Even in this nonequilibrium configuration, the resulting $\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}$ centers are stable enough to allow for resonant optical excitation and optically detected magnetic resonance. Our results pave the way for on-demand generation of $\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}$ centers as well as other emerging quantum defects in diamond.

DOI
10.1103/physrevapplied.19.034022

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Neutral silicon-vacancy (Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0) centers in diamond are promising candidates for quantum network applications because of their exceptional optical properties and spin coherence. However, the stabilization of Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers requires careful Fermi-level engineering of the diamond host material, making further technological development challenging. Here, we show that Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers can be efficiently stabilized by photoactivated itinerant carriers. Even in this nonequilibrium configuration, the resulting Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers are stable enough to allow for resonant optical excitation and optically detected magnetic resonance. Our results pave the way for on-demand generation of Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers as well as other emerging quantum defects in diamond.
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.
Neutral silicon vacancy centers (SiV^{0}) in diamond are promising candidates for quantum applications; however, stabilizing SiV^{0} requires high-purity, boron-doped diamond, which is not a readily available material. Here, we demonstrate an alternative approach via chemical control of the diamond surface. We use low-damage chemical processing and annealing in a hydrogen environment to realize reversible and highly stable charge state tuning in undoped diamond. The resulting SiV^{0} centers display optically detected magnetic resonance and bulklike optical properties. Controlling the charge state tuning via surface termination offers a route for scalable technologies based on SiV^{0} centers, as well as charge state engineering of other defects.
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.
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 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'.
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.