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arXiv:2508.18991 · Nano Letters

Optical Charge State Manipulation of Lead-Vacancy Centers in Diamond

Yiyang Chen, Yoshiyuki Miyamoto, Eiki Ota, Ryotaro Abe, Takashi Taniguchi, Shinobu Onoda, Mutsuko Hatano, Takayuki Iwasaki

Published Nov 13, 2025• 2 citations
arXivHTMLPDF

Abstract

Group-IV vacancy centers in diamond exhibit excellent optical and spin coherence properties, making them highly promising and scalable spin qubit candidates. Since only specific charge states are magneto-optically active, control over the charge state is fundamental for quantum applications. Here, we realize the charge state control of lead-vacancy centers (PbV) through multicolor laser irradiation. We achieve tunable population manipulation of the negatively charged state from 0 to 89%, paving the way for spin control of the negatively charged PbV center. Furthermore, through analysis of charge state dynamics, we propose a charge cycle between the neutral and negatively charged states, indicating a possible pathway to the neutral PbV center with a spin-1 system.

DOI
10.1021/acs.nanolett.5c04448

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Group-IV vacancy centers in diamond exhibit excellent optical and spin coherence properties, making them highly promising and scalable spin qubit candidates. Since only specific charge states are magneto-optically active, control over the charge state is fundamental for quantum applications. Here, we realize the charge state control of lead-vacancy centers (PbV) through multicolor laser irradiation. We achieve tunable population manipulation of the negatively charged state from 0 to 89%, paving the way for spin control of the negatively charged PbV center. Furthermore, through analysis of charge state dynamics, we propose a charge cycle between the neutral and negatively charged states, indicating a possible pathway to the neutral PbV center with a spin-1 system.
A lead-vacancy (PbV) center in diamond exhibits coherent emission above the liquid helium temperature, making it highly attractive for quantum network applications. Here, we report the magneto-optical and spin properties of PbV centers in diamond. We record a spin lifetime of 12 ms at 7.5 K under large off-axis magnetic field. Furthermore, we observe formation of the coherent dark state by coherent population trapping and estimate a spin dephasing time of 177 ns at 6.5 K. This work demonstrates the outstanding thermal robustness of the PbV spin compared to other group-IV centers above 4 K.
Tin-vacancy (SnV) and other group-IV vacancy centers in diamond (SiV, GeV, and PbV) are intensively studied as promising alternatives to the nitrogen-vacancy (NV) center for quantum-based applications. The knowledge and the control of their charge state are therefore major issues. Here, using p-i-p planar junctions, we explore the charge states of implanted single SnV centers. We find two classes of centers, emitting either at 620 nm (SnV – ) or at 646.8 nm but not both. We demonstrate the active and reversible tuning of individual SnV – centers. However, unlike the NV centers, which we tune reversibly and continuously between NV – (638 nm), NV 0 (575 nm), and NV + (dark) states, the two kinds of SnV centers do not tune from one to the other. These findings indicate that the 646.8 nm line is likely owing to another Sn-related defect rather than to the neutral charge state of the split vacancy SnV defect along the ⟨111⟩ axis. Furthermore, p-i-p structures can be used efficiently to induce a tunable band bending, stabilize SnV – and NV – states, and explore the charge-state transition energies of many defect centers.
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.
Group-IV color centers in diamond are a promising light-matter interface for quantum networking devices.The negatively charged tin-vacancy center (SnV) is particularly interesting, as its large spin-orbit coupling offers strong protection against phonon dephasing and robust cyclicity of its optical transitions toward spin-photon-entanglement schemes.Here, we demonstrate multiaxis coherent control of the SnV spin qubit via an all-optical stimulated Raman drive between the ground and excited states.We use coherent population trapping and optically driven electronic spin resonance to confirm coherent access to the qubit at 1.7 K and obtain spin Rabi oscillations at a rate of Ω=2π ¼ 19.0ð1Þ MHz.All-optical Ramsey interferometry reveals a spin dephasing time of T Ã 2 ¼ 1.3ð3Þ μs, and four-pulse dynamical decoupling already extends the spin-coherence time to T 2 ¼ 0.30ð8Þ ms.Combined with transform-limited photons and integration into photonic nanostructures, our results make the SnV a competitive spin-photon building block for quantum networks.
Group IV vacancy color centers in diamond are promising spin-photon interfaces with strong potential for applications in photonic quantum technologies. Reliable methods for controlling and stabilizing their charge state are urgently needed for scaling to multiqubit devices. Here, we manipulate the charge state of silicon vacancy (SiV) ensembles by combining luminescence and photocurrent spectroscopy. We controllably convert the charge state between the optically active SiV − and dark SiV 2− with megahertz rates and >90% contrast by judiciously choosing the local potential applied to in-plane surface electrodes and the laser excitation wavelength. We observe intense SiV − photoluminescence under hole capture, measure the intrinsic conversion time from the dark SiV 2− to the bright SiV − to be 36.4(67) ms, and demonstrate how it can be enhanced by a factor of 10 5 via optical pumping. Moreover, we obtain previously unknown information on the defects that contribute to photoconductivity, indicating the presence of substitutional nitrogen and divacancies.
In this paper, we provide a comprehensive overview of the microwave-induced manipulation of electronic spin states in negatively charged group-IV color centers in diamond with a particular emphasis on the influence of strain. Central to our investigation is the consideration of the full vectorial attributes of the magnetic fields involved, which are a dc field for lifting the degeneracy of the spin levels and an ac field for microwave control between two spin levels. We observe an intricate interdependence between their spatial orientations, the externally applied strain, and the resultant efficacy in spin-state control. In most studies to date the ac and dc magnetic field orientations have been insufficiently addressed, which has led to the conclusion that strain is indispensable for the effective microwave control of heavier group-IV vacancies, such as tin- and lead-vacancy color centers. In contrast, we find that the alignment of the dc magnetic field orthogonal to the symmetry axis and the ac field parallel to it can make the application of strain obsolete for effective spin manipulation. Furthermore, we explore the implications of this field configuration on the spin's optical initialization, readout, and gate fidelities. Published by the American Physical Society 2024