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arXiv:2409.07421

Laser Activation of Single Group-IV Colour Centres in Diamond

Xingrui Cheng, Andreas Thurn, Guangzhao Chen, Gareth J. F. Jones, Maddison Coke, Mason Adshead, Cathryn P. Michaels, Osman Balcı, Ferrari, Andrea C., Mete Atatüre, Richard J. Curry, Jason M. Smith, Patrick S. Salter, Dorian A. Gangloff

Published Sep 11, 2024• 0 citations
arXivHTMLPDF

Abstract

Spin-photon interfaces based on group-IV colour centres in diamond offer a promising platform for quantum networks. A key challenge in the field is realizing precise single-defect positioning and activation, which is crucial for scalable device fabrication. Here we address this problem by demonstrating a two-step fabrication method for tin vacancy (SnV-) centres that uses site-controlled ion implantation followed by local femtosecond laser annealing with in-situ spectral monitoring. The ion implantation is performed with sub-50 nm resolution and a dosage that is controlled from hundreds of ions down to single ions per site, limited by Poissonian statistics. Using this approach, we successfully demonstrate site-selective creation and modification of single SnV- centres. The technique opens a window onto materials tuning at the single defect level, and provides new insight into defect structures and dynamics during the annealing process. While demonstrated for SnV- centres, this versatile approach can be readily generalised to other implanted colour centres in diamond and wide-bandgap materials.

DOI
10.48550/arxiv.2409.07421

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Spin-photon interfaces based on group-IV colour centres in diamond offer a promising platform for quantum networks. A key challenge in the field is realizing precise single-defect positioning and activation, which is crucial for scalable device fabrication. Here we address this problem by demonstrating a two-step fabrication method for tin vacancy (SnV-) centres that uses site-controlled ion implantation followed by local femtosecond laser annealing with in-situ spectral monitoring. The ion implantation is performed with sub-50 nm resolution and a dosage that is controlled from hundreds of ions down to single ions per site, limited by Poissonian statistics. Using this approach, we successfully demonstrate site-selective creation and modification of single SnV- centres. The technique opens a window onto materials tuning at the single defect level, and provides new insight into defect structures and dynamics during the annealing process. While demonstrated for SnV- centres, this versatile approach can be readily generalised to other implanted colour centres in diamond and wide-bandgap materials.
Abstract Spin-photon interfaces based on group-IV colour centres in diamond offer a promising platform for quantum networks. A key challenge in the field is realising precise single-defect positioning and activation, which is crucial for scalable device fabrication. Here we address this problem by demonstrating a two-step fabrication method for tin vacancy (SnV−) centres that uses site-controlled ion implantation followed by local femtosecond laser annealing with in-situ spectral monitoring. The ion implantation is performed with sub-50 nm resolution and a dosage that is controlled from hundreds of ions down to single ions per site, limited by Poissonian statistics. Using this approach, we successfully demonstrate site-selective creation and modification of single SnV− centres. Our in-situ spectral monitoring opens a window onto materials tuning at the single defect level, and provides new insight into defect structures and dynamics during the annealing process. While demonstrated for SnV− centres, this versatile approach can be readily generalised to other implanted colour centres in diamond and wide-bandgap materials.
Group IV color centers in diamond have garnered great interest for their potential as optically active solid-state spin qubits. The future utilization of such emitters requires the development of precise site-controlled emitter generation techniques that are compatible with high-quality nanophotonic devices. This task is more challenging for color centers with large group IV impurity atoms, which are otherwise promising because of their predicted long spin coherence times without a dilution refrigerator. For example, when applied to the negatively charged tin-vacancy (SnV – ) center, conventional site-controlled color center generation methods either damage the diamond surface or yield bulk spectra with unexplained features. Here we demonstrate a novel method to generate site-controlled SnV – centers with clean bulk spectra. We shallowly implant Sn ions through a thin implantation mask and subsequently grow a layer of diamond via chemical vapor deposition. This method can be extended to other color centers and integrated with quantum nanophotonic device fabrication.
Abstract We present a high throughput and systematic method for the screening of colour centres in diamond with the aim of searching for and reproducibly creating new optical centres down to the single defect level, potentially of interest for a wide range of diamond-based quantum applications. The screening method presented here should, moreover, help to identify some already indexed defects among hundreds in diamond (Zaitsev 2001 Optical Properties of Diamond (Berlin: Springer)) but also some promising defects of a still unknown nature, such as the recently discovered ST1 centre (Lee et al 2013 Nat. Nanotechnol . 8 487; John et al 2017 New J. Phys . 19 053008). We use ion implantation in a systematic manner to implant several chemical elements. Ion implantation has the advantage of addressing single atoms inside the bulk with defined depth and high lateral resolution, but the disadvantage of producing intrinsic defects. The implanted samples are annealed in vacuum at different temperatures (between 600 °C and 1600 °C with 200 °C steps) and fully characterised at each step in order to follow the evolution of the defects: formation, dissociation, diffusion, re-formation and charge state, at the ensemble level and, if possible, at the single centre level. We review the unavoidable ion implantation defects (such as the GR1 and 3H centres), discuss ion channeling and thermal annealing and estimate the diffusion of the vacancies, nitrogen and hydrogen. We use different characterisation methods best suited for our study (from widefield fluorescence down to sub-diffraction optical imaging of single centres) and discuss reproducibility issues due to diamond and defect inhomogeneities. Nitrogen is also implanted for reference, taking advantage of the considerable knowledge on NV centres as a versatile sensor in order to retrieve or deduce the conditions and local environment in which the different implanted chemical elements are embedded. We show here the preliminary promising results of a long-term study and focus on the elements O, Mg, Ca, F and P from which fluorescent centres were found.
Split-vacancy color centers in diamonds are promising solid-state platforms for the implementation of photonic quantum technologies. These luminescent defects are commonly fabricated upon low-energy ion implantation and subsequent thermal annealing. Their technological uptake will require the availability of reliable methods for the controlled, large-scale production of localized individual photon emitters. This task is partially achieved by controlled ion implantation to introduce selected impurities in the host material and requires the development of challenging beam focusing or collimation procedures coupled with single-ion detection techniques. We report on the protocol for the direct optical activation of split-vacancy color centers in diamond via localized processing with a continuous-wave laser at mW optical powers. We demonstrate the activation of photoluminescent Mg- and Sn-related centers at both the ensemble and single-photon emitter levels in ion-implanted, high-purity diamond crystals without further thermal processing. The proposed lithographic method enables the activation of individual color centers at specific positions of a large-area sample by means of a relatively inexpensive equipment offering real-time, in situ monitoring of the process.
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.
Nanodiamonds containing single tin-vacancy (SnV) centers have the potential for integration into nanophotonic devices employed in quantum technologies such as quantum sensing, quantum information processing and quantum communication. The present study assessed single SnV centers in nanodiamonds less than 10 nm in size. Such centers were generated by implanting Sn ions into size-selected small nanodiamonds followed by high-temperature annealing. A sharp emission peak with a line width of 2.6 nm was observed at 618.7 nm, corresponding to the zero phonon line of SnV centers in bulk diamond. The Debye–Waller factor for this peak at room temperature was estimated to be 0.38 and so was slightly greater than the value for bulk diamond. A second-order correlation function yielded a g 2 (0) value of 0.04 ± 0.11, indicating single-photon emission. The successful creation of single SnV centers in nanodiamonds is a critical step toward integrating nanophotonic devices for photonic quantum technologies.