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arXiv:2503.09147 · ACS Photonics

Coherence Properties of Rare-Earth Spins in Micrometer-Thin Films

Zihua Chai, Zhaocong Wang, Xinghang Chen, Quanshen Shen, Zeyu Gao, Junyu Guan, Hanyu Zhang, Ya Wang, Yang Tan, Feng Chen, Kangwei Xia

Published Feb 27, 2025• 5 citations
arXivHTMLPDF

Abstract

Rare-earth ions in bulk crystals are excellent solid-state quantum systems in quantum information science owing to their exceptional optical and spin coherence properties. However, the weak fluorescence of single rare-earth ions presents a significant challenge for scalability, necessitating the integration into microcavities. Thin films serve as a promising material platform for the integration, yet fabrication without compromising the properties of the materials and rare-earth ions remains challenging. In this work, we fabricate micrometer-thin yttrium aluminum garnet (YAG) films from bulk crystals using ion implantation techniques. The resulting films preserve the single-crystalline structure of the original bulk crystal. Notably, the embedded rare-earth ions are photostable and exhibit bulk-like spin coherence properties. Our results demonstrate the compatibility of bulk-like spin properties with the thin-film fabrication technique, facilitating the efficient integration of rare-earth ions into on-chip photonic devices and advancing the applications of rare-earth ions in quantum technologies.

DOI
10.1021/acsphotonics.4c02520

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Rare-earth ions in bulk crystals are excellent solid-state quantum systems in quantum information science owing to their exceptional optical and spin coherence properties. However, the weak fluorescence of single rare-earth ions presents a significant challenge for scalability, necessitating the integration into microcavities. Thin films serve as a promising material platform for the integration, yet fabrication without compromising the properties of the materials and rare-earth ions remains challenging. In this work, we fabricate micrometer-thin yttrium aluminum garnet (YAG) films from bulk crystals using ion implantation techniques. The resulting films preserve the single-crystalline structure of the original bulk crystal. Notably, the embedded rare-earth ions are photostable and exhibit bulk-like spin coherence properties. Our results demonstrate the compatibility of bulk-like spin properties with the thin-film fabrication technique, facilitating the efficient integration of rare-earth ions into on-chip photonic devices and advancing the applications of rare-earth ions in quantum technologies.
Rare-earth ion ensembles doped in single crystals are a promising materials system with widespread applications in optical signal processing, lasing, and quantum information processing. Incorporating rare-earth ions into integrated photonic devices could enable compact lasers and modulators, as well as on-chip optical quantum memories for classical and quantum optical applications. To this end, a thin film single crystalline wafer structure that is compatible with planar fabrication of integrated photonic devices would be highly desirable. However, incorporating rare-earth ions into a thin film form-factor while preserving their optical properties has proven challenging. We demonstrate an integrated photonic platform for rare-earth ions doped in a single crystalline thin film lithium niobate on insulator. The thin film is composed of lithium niobate doped with Tm 3+ . The ions in the thin film exhibit optical lifetimes identical to those measured in bulk crystals. We show narrow spectral holes in a thin film waveguide that require up to 2 orders of magnitude lower power to generate than previously reported bulk waveguides. Our results pave the way for scalable on-chip lasers, optical signal processing devices, and integrated optical quantum memories.
Coherent quantum devices play a central role in quantum science and engineering. Rare-earth ions such as erbium in solids feature numerous 4f- intra-shell transitions that are effectively shielded from their crystalline surroundings by closed outer shells, allowing for long spin coherence times and narrow optical transitions. Recent ensemble experiments have established the rare-earth doped crystals as the leading materials for optical quantum memories. However, the development of large-scale quantum devices based on rare-earth doped materials has remained a challenge. Here we describe a scalable quantum photonic platform based on epitaxially grown oxide thin films doped with trivalent ions on silicon substrates. The platform builds upon the recent developments of high quality epitaxial rare-earth doped oxides on silicon, and highlights the integration of quantum coherent materials with existing silicon technologies for ultimate device scalability. The proposed device platform builds upon our capability to epitaxially grow high quality, near-lattice-matched Y2O3 thin films on silicon. The epitaxial thin film is of high structural quality and offers several distinct advantages: (1) significantly less optical loss and better quantum emitter coherence; (2) atomic precision placement of rare-earth emitters (via delta doping) with respect to the photonic mode for controllable ion-photon coupling; (3) scalable top-down device fabrication using standard lithography and etching techniques; (4) heterogeneous integration with silicon takes full advantage of existing silicon photonics technologies for routing, tuning, and modulation of the quantum emission from rare-earth ions.
Abstract Rare earth doped crystals show, at low temperatures, extremely narrow optical homogeneous linewidths, as well as long spin coherence lifetimes, a unique combination in the solid state. This makes these materials attractive for optical quantum technologies like quantum communication and processing. Most of the results in this field have so far used bulk crystals because of their exceptional spectroscopic properties. Crystalline thin films can combine these properties with the possibilities offered by integration in photonic circuits in terms of compactness, stability, energy efficiency, and scalability. In this review, recent results on different platforms containing rare earth ions and targeting quantum technologies, including lithium niobate and silicon films, and oxide films deposited on Si, are summarized. Current approaches for obtaining thin films and devices are described, together with RE spectroscopic properties and applications to quantum technologies. The opportunities and challenges offered or faced by the different platforms are also discussed.
Rare-earth ion doped crystals possess stable solid state physicochemical properties and long optical coherence time and spin coherence time, thus showing important development prospect in quantum information science and technology area. Investigations on macroscopic bulk rare-earth single crystals have obtained many promising results, especially in the field of optical quantum memory. With the rapid development of quantum information science, a variety of new functions or multifunctional integrations are found in rare earth crystal systems, such as on chip quantum storage, microwave to optical frequency conversion, scalable quantum single photon sources, and quantum logic gates. As a result, beyond the macroscopic bulk rare-earth single crystals, micro/nano-scale rare-earth crystals have received much attention in recent years and they are regarded as promising candidates in highly integrated hybrid quantum systems and miniaturized quantum devices. Moreover, wet chemical method synthesized micro/nano-scale rare-earth crystals have lower growth difficulty and more flexible manipulation in volume, shape and composition. Therefore, exploring high-performance micro/nano-scale rare-earth crystals and precisely manipulating their quantum states have become one of the important directions in today’s quantum information science and technology research. In this review, we first briefly introduce the basic concepts and high resolution spectroscopic techniques that are commonly used in rare earth ion doped crystals for quantum information science and technologies, such as hole burning technique and photon echo technique. Then we summarize comprehensively recent research status and development trends of rare earth ion doped polycrystalline nanoparticles, thin films, single crystal based micro systems, and some other micro/nano-scale rare earth platforms in terms of material fabrication, quantum coherence property, dephasing mechanisms, and also quantum device explorations. The latest research advances in quantum information applications such as quantum storage, quantum frequency conversion, quantum single photon sources and quantum logic gates are given. Finally, we discuss the possible optimization directions and strategies to improve the component design, material synthesis and quantum performance of micro/nano-scale rare earth crystals and their related quantum devices. This review highlights that the micro/nano-scale rare earth crystals may offer many new possibilities for designing quantum light-matter interfaces, thus are promising quantum systems to develop scalable and integrated quantum devices in the future.
As an active material with favorable linear and nonlinear optical properties, thin-film lithium niobate has demonstrated its potential in integrated photonics. Integration with rare-earth ions, which are promising candidates for quantum memories and transducers, will enrich the system with new applications in quantum information processing. Here, we investigate the optical properties at 1.5 μm wavelengths of rare-earth ions (Er3+) implanted in thin-film lithium niobate waveguides and micro-ring resonators. Optical quality factors near a million after post-annealing show that ion implantation damage can be repaired. The transition linewidth and fluorescence lifetime of erbium ions are characterized. The ion-cavity coupling is observed through a Purcell enhanced fluorescence from which a Purcell factor of 3.8 ± 0.5, compared with waveguide lifetime, is extracted. This platform is compatible with top-down lithography processes and leads to a scalable path for controlling spin-photon interfaces in photonic circuits.