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ACS Photonics

Charge-State Tuning of Single SnV Centers in Diamond

Tobias Lühmann, Johannes Küpper, Stefan Dietel, Robert Staacke, Jan Meijer, Sébastien Pezzagna

Published Dec 3, 2020• 25 citations
Publisher

Abstract

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.

DOI
10.1021/acsphotonics.0c01123

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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.
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.
Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV 2– . These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.
Group-IV color centers in diamonds are promising not only as spin-photon interfaces for quantum networks but also as multicolor photoluminescence probes and all-optical temperature sensors for biological research. Therefore, generating group-IV color centers in detonation nanodiamonds (DNDs), the smallest class of diamond nanocrystals, has become a research focal point. This approach holds potential for the noninvasive introduction of diamond sensors into living cell organelles, enabling sensing of local structural and temperature changes with minimal disturbance. Following the successful generation of silicon- and germanium-vacancy centers in DNDs, the generation of tin-vacancy (SnV) centers was investigated. Similar to other group-IV color centers, the SnV centers exhibit strong photoluminescence. In addition, the SnV center offers a long spin coherence time compared with those of silicon- and germanium-vacancy centers. However, the strain induced by large Sn atoms poses substantial challenges for generating SnV centers in ultrasmall nanodiamonds. In this study, Sn-doped DNDs with a mean particle size of ~ 5 nm were subjected to a 3 days boiling acid treatment, which led to sharp zero-phonon lines of SnV centers at ~ 620 nm in the photoluminescence spectra. Photon autocorrelation measurements further revealed the presence of single SnV centers in these DNDs.
Charge-states modulation of nitrogen-vacancy (NV) centers incorporated into single crystal diamond films attracts increasing attention for solid-state qubits applications. Here, we discuss the electro- and photoluminescence emission properties of NV centers incorporated by gas phase nitrogen delta-doping of the intrinsic diamond layer of a positive-intrinsic-negative (PIN) junction diode. The experiments show that the charge state of NV centers can be intentionally controlled by applying well-defined external bias voltages. It can be switched from the negatively charged state NV− to the neutral charged state NV0 when a strong forward bias potential is applied. This can be switched back by application of reverse potentials. These results will be discussed assuming basic electronic properties of diamond PIN diodes, including the variation of spectral properties as well as the dynamics of charge state transitions.
The nitrogen-vacancy (NV) point defect center in diamond has recently received significant research interest, with over 850 papers published on the topic in the last 10 years.This interest is a result of optically-pumped spin polarization and optical readout of spin state with high fidelity: potential applications include high-spatial resolution magnetometry, quantum computing and quantum communications.Despite its favorable spin properties, the NV emission is highly broadband leading to low efficiencies for processes which require coherent light interactions e.g.photonic entanglement -a requirement for long distance quantum communication and distributed quantum computing.Further work in diamond has identified group-IV-vacancy pairs (SiV, GeV, SnV) with superlative optical properties (up to 70% coherent emission) but poor spin properties.Therefore, further work is required to identify a point defect which simultaneously possesses long spin lifetimes and narrow optical emission.We propose a route to the production of the previously-unidentified phosphorusvacancy (PV) via implantation of 31 Al (decays to 31 Si with 98.4% efficiency and t 1⁄ 2 = 644 ms), and its optical identification through monitoring the decay of 31 SiV to 31 PV with t 1⁄ 2 = 157 min, and the rise of PV by photoluminescence.PV will subsequently be studied using both ensemble and single-centercapable state-of-the-art characterization equipment to determine its optical and spin properties, which we expect to be extremely interesting in line with SiV, GeV, SnV and NV in diamond.Requested shifts: 6 shifts, (split into 2 runs over 1 years)