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arXiv:2605.27841

Coherent Dark State Formation of a Lead-Vacancy Spin Qubit in Diamond

Yiyang Chen, Koyo Hirai, Tzyy Zheng Neo, Eiki Ota, Takashi Taniguchi, Masashi Miyakawa, Shinobu Onoda, Toshiharu Makino, Mutsuko Hatano, Takayuki Iwasaki

quant-phSubmitted May 27, 2026• Announced May 28, 2026• 0 citations• Revised Jun 16, 2026 (v2)
v1 · May 27, 2026v2 · Jun 16, 2026
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Abstract

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.

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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.
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.
Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.
We report the optical observation of lead-vacancy (PbV) centers in diamond fabricated by Pb ion implantation and subsequent high-temperature annealing (2100 °C) under high pressure (7.7 GPa). Their optical properties were characterized by photoluminescence at varying temperatures down to 5.7 K. We observed intense emission peaks at 550 and 554 nm, with a large splitting of approximately 3900 GHz. The two lines are thought to correspond to the zero phonon line (ZPL) of PbV centers with split ground and excited states. A cubic trend of the ZPL width was observed while varying the temperature. We performed polarization measurements of the two lines in a single PbV center, showing nearly orthogonal dipole polarizations. These optical measurements strongly indicate that the PbV center possesses D 3 d symmetry in the diamond lattice. The observed large ground state splitting significantly suppresses the phonon-mediated transition, which causes decoherence of the electron spin state of the group IV color centers in diamond, leading to the expectation of a long spin coherence time at a temperature ∼9 K.
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.
We report on quantum emission from Pb-related color centers in diamond following ion implantation and high-temperature vacuum annealing. First-principles calculations predict a negatively charged Pb-vacancy (PbV) center in a split-vacancy configuration, with a zero-phonon transition around 2.4 eV. Cryogenic photoluminescence measurements performed on emitters in nanofabricated pillars reveal several transitions, including a prominent doublet near 520 nm. The splitting of this doublet, 5.7 THz, exceeds that reported for other group-IV centers. These observations are consistent with the PbV center, which is expected to have a combination of narrow optical transitions and stable spin states, making it a promising system for quantum network nodes.
Abstract Quantum information processing (QIP) with solid state spin qubits strongly depends on the efficient initialisation of the qubit’s desired charge state. While the negatively charged tin-vacancy (SnV − ) centre in diamond has emerged as an excellent platform for realising QIP protocols due to long spin coherence times at liquid helium temperature and lifetime limited optical transitions, its usefulness is severely limited by termination of the fluorescence under resonant excitation. Here, we unveil the underlying charge cycle, potentially applicable to all group IV-vacancy (G4V) centres, and exploit it to demonstrate highly efficient and rapid initialisation of the desired negative charge state of single SnV centres while preserving long term stable optical resonances. In addition to investigating the optical coherence, we all-optically probe the coherence of the ground state spins by means of coherent population trapping and find a spin dephasing time of 5(1) μ s. Furthermore, we demonstrate proof-of-principle single shot spin state readout without the necessity of a magnetic field aligned to the symmetry axis of the defect.