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arXiv:2412.07087 · ACS Photonics

Charge State Transition of Spectrally Stabilized Tin-Vacancy Centers in Diamond

Keita Ikeda, Yiyang Chen, Peng Wang, Yoshiyuki Miyamoto, Takashi Taniguchi, Shinobu Onoda, Mutsuko Hatano, Takayuki Iwasaki

Published Mar 4, 2025• 4 citations
arXivHTMLPDF

Abstract

High Resolution Image Download MS PowerPoint Slide Solid-state quantum emitters are important platforms for quantum information processing. The fabrication of the emitters with stable photon frequency and narrow line width is a fundamental issue, and it is essential to understand optical conditions under which the emitter keeps a bright charge state or transitions to a dark state. For these purposes, in this study, we investigate the spectral stability and charge state transition of tin-vacancy (SnV) centers in diamond. The photoluminescence excitation spectra of multiple SnV centers are basically stable over time with nearly transform-limited line widths under resonant excitation, while simultaneous irradiation of resonant and nonresonant lasers makes spectra from the SnV centers unstable. We find that the instability occurs due to the charge state transition to a dark state. The charge state transition rates are quantitatively investigated depending on the laser powers. Lastly, with first-principles calculations, we model the charge state transition of the SnV center under laser irradiation.

DOI
10.1021/acsphotonics.4c02490

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High Resolution Image Download MS PowerPoint Slide Solid-state quantum emitters are important platforms for quantum information processing. The fabrication of the emitters with stable photon frequency and narrow line width is a fundamental issue, and it is essential to understand optical conditions under which the emitter keeps a bright charge state or transitions to a dark state. For these purposes, in this study, we investigate the spectral stability and charge state transition of tin-vacancy (SnV) centers in diamond. The photoluminescence excitation spectra of multiple SnV centers are basically stable over time with nearly transform-limited line widths under resonant excitation, while simultaneous irradiation of resonant and nonresonant lasers makes spectra from the SnV centers unstable. We find that the instability occurs due to the charge state transition to a dark state. The charge state transition rates are quantitatively investigated depending on the laser powers. Lastly, with first-principles calculations, we model the charge state transition of the SnV center under laser irradiation.
Abstract The recently discovered negatively charged tin-vacancy centre in diamond is a promising candidate for applications in quantum information processing (QIP). We here present a detailed spectroscopic study encompassing single photon emission and polarisation properties, the temperature dependence of emission spectra as well as a detailed analysis of the phonon sideband and Debye–Waller factor. Using photoluminescence excitation spectroscopy we probe an energetically higher lying excited state and prove fully lifetime limited linewidths of single emitters at cryogenic temperatures. For these emitters we also investigate the stability of the charge state under resonant excitation. These results provide a detailed insight into the spectroscopic properties of the SnV− centre and lay the foundation for further studies regarding its suitability in QIP.
Quantum emitters in diamond are a promising candidate for quantum network applications. Here, we show basic properties of tin-vacancy (SnV) centers in diamond, which we recently discovered. The SnV center shows a sharp zero phonon line and a high fluorescence intensity. The SnV center has a possibility to have a long spin coherence time in the Kelvin temperature range, in contrast to other group-IV color centers, i.e. silicon-vacancy and germanium-vacancy centers. We discuss important experiments regarding spin and optical properties of the SnV quantum emitter for further development towards quantum network.
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.
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.
Diamond tin-vacancy centers have emerged as a promising platform for quantum information science and technology. A key challenge for their use in more-complex quantum experiments and scalable applications is the ability to prepare the center in the desired charge state with the optical transition at a predefined frequency. Here we report on heralding such successful preparation using a combination of laser excitation, photon detection, and real-time logic. We first show that fluorescence photon counts collected during an optimized resonant probe pulse strongly correlate with the subsequent charge state and optical-transition frequency, enabling real-time heralding of the desired state through threshold photon counting. We then implement and apply this heralding technique to photoluminescence-excitation measurements, coherent optical driving, and an optical Ramsey experiment, finding strongly increased optical coherence with increasing threshold. Finally, we demonstrate that the prepared optical frequency follows the probe laser across the inhomogeneous linewidth, enabling tuning of the transition frequency over multiple homogeneous linewidths. Published by the American Physical Society 2024
Integrating solid-state quantum emitters with photonic circuits is essential for realizing large-scale quantum photonic processors. Negatively charged tin-vacancy (SnV – ) centers in diamond have emerged as promising candidates for quantum emitters because of their excellent optical and spin properties, including narrow-linewidth emission and long spin coherence times. SnV – centers need to be incorporated in optical waveguides for efficient on-chip routing of the photons they generate. However, such integration has yet to be realized. In this Letter, we demonstrate the coupling of SnV – centers to a nanophotonic waveguide. We realize this device by leveraging our recently developed shallow ion implantation and growth method for the generation of high-quality SnV – centers and the advanced quasi-isotropic diamond fabrication technique. We confirm the compatibility and robustness of these techniques through successful coupling of narrow-linewidth SnV – centers (as narrow as 36 ± 2 MHz) to the diamond waveguide. Furthermore, we investigate the stability of waveguide-coupled SnV – centers under resonant excitation. Our results are an important step toward SnV – -based on-chip spin-photon interfaces, single-photon nonlinearity, and photon-mediated spin interactions.