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Advanced Optical Materials

Rare Earth‐Diamond Hybrid Structures for Optical Quantum Technologies

Ionuț Gabriel Balașa, María Arranz-Martinez, Pauline Perrin, Midrel Wilfried Ngandeu Ngambou, Alexandre Hebbrecht, Diana Serrano, Jocelyn Achard, Alexandre Tallaire, Philippe Goldner

Published Aug 23, 2024• 13 citations
Publisher

Abstract

Abstract Diamond containing nitrogen‐vacancy centers (NV−) is one of the most investigated materials for quantum technologies, because of this system's exceptional spin properties. Although the NV− optical transition is very bright, it suffers from spectral diffusion and weak zero‐phonon line, and is in the visible range. This limits integration into quantum photonic structures and interfacing with optical fiber networks. In contrast, rare earth (RE) ions exhibit extremely narrow and stable optical transitions, including erbium's 1.5 µm telecom wavelength. Combining RE with NV− properties through short‐range interactions is however challenging as RE do not readily enter the diamond lattice. In this work, a thin‐film‐based architecture in which RE and NV− centers can interact while preserving their unique properties is introduced. Thin films of Er3+:Y2O3 are grown by chemical vapor deposition on diamond substrates with well‐crystallized and highly textured structures. An extensive spectroscopic study of Er3+ transitions at room and low temperatures further reveals that photoluminescence spectra and decays are close to bulk materials. It is also shown that Y2O3 thin film deposition has no detrimental effects on NV− optical and spin properties. RE thin films deposited on diamond can thus be suitable for building hybrid materials for new functionalities in quantum sensing, communication, and processing.

DOI
10.1002/adom.202401487

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Abstract Diamond containing nitrogen‐vacancy centers (NV−) is one of the most investigated materials for quantum technologies, because of this system's exceptional spin properties. Although the NV− optical transition is very bright, it suffers from spectral diffusion and weak zero‐phonon line, and is in the visible range. This limits integration into quantum photonic structures and interfacing with optical fiber networks. In contrast, rare earth (RE) ions exhibit extremely narrow and stable optical transitions, including erbium's 1.5 µm telecom wavelength. Combining RE with NV− properties through short‐range interactions is however challenging as RE do not readily enter the diamond lattice. In this work, a thin‐film‐based architecture in which RE and NV− centers can interact while preserving their unique properties is introduced. Thin films of Er3+:Y2O3 are grown by chemical vapor deposition on diamond substrates with well‐crystallized and highly textured structures. An extensive spectroscopic study of Er3+ transitions at room and low temperatures further reveals that photoluminescence spectra and decays are close to bulk materials. It is also shown that Y2O3 thin film deposition has no detrimental effects on NV− optical and spin properties. RE thin films deposited on diamond can thus be suitable for building hybrid materials for new functionalities in quantum sensing, communication, and processing.
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.
The obtention of quantum-grade rare-earth-doped oxide thin films that can be integrated with optical cavities and microwave resonators is of great interest for the development of scalable quantum devices. Among the different growth methods, chemical vapor deposition (CVD) offers high flexibility and has demonstrated the ability to produce oxide films hosting rare-earth ions with narrow linewidths. However, growing epitaxial films directly on silicon is challenging by CVD due to a native amorphous oxide layer formation at the interface. In this manuscript, we investigate the CVD growth of erbium-doped yttrium oxide (Er:Y2O3) thin films on different substrates, including silicon, sapphire, quartz, or yttria stabilized zirconia (YSZ). Alternatively, growth was also attempted on an epitaxial Y2O3 template layer on Si (111) prepared by molecular beam epitaxy (MBE) in order to circumvent the issue of the amorphous interlayer. We found that the substrate impacts the film morphology and the crystalline orientations, with different textures observed for the CVD film on the MBE-oxide/Si template (111) and epitaxial growth on YSZ (001). In terms of optical properties, Er3+ ions exhibit visible and IR emission features that are comparable for all samples, indicating a high-quality local crystalline environment regardless of the substrate. Our approach opens interesting prospects to integrate such films into scalable devices for optical quantum technologies.
The obtention of quantum-grade rare-earth doped oxide thin films that can be integrated with optical cavities and microwave resonators is of great interest for the development of scalable quantum devices. Among the different growth methods, Chemical Vapour Deposition (CVD) offers high flexibility and has demonstrated the ability to produce oxide films hosting rare-earth ions with narrow linewidths. However, growing epitaxial films directly on silicon is challenging by CVD due to a native amorphous oxide layer formation at the interface. In this manuscript, we investigate the CVD growth of erbium-doped yttrium oxide (Er:Y2O3) thin films on different substrates, including silicon, sapphire, quartz or yttria stabilized zirconia (YSZ). Alternatively, growth was also attempted on an epitaxial Y2O3 template layer on Si (111) prepared by molecular beam epitaxy (MBE) in order to circumvent the issue of the amorphous interlayer. We found that the substrate impacts the film morphology and the crystalline orientations, with different textures observed for the CVD film on the MBE-oxide/Si template (111) and epitaxial growth on YSZ (001). In terms of optical properties, Er3+ ions exhibit visible and IR emission features that are comparable for all samples, indicating a high-quality local crystalline environment regardless of the substrate. Our approach opens interesting prospects to integrate such films into scalable devices for optical quantum technologies.
The electronic spin associated with the nitrogen vacancy (NV) color center in diamond is an excellent candidate for a solid-state qubit functioning as a quantum register or sensor. However, the lack of thin film technologies for crystalline diamond with low impurity levels hampers the development of photonic interfaces to such diamond-based qubits. We present a method for manufacturing slabs of diamond of 200 nm thickness and several microns in extent from high-purity single crystal chemical vapor deposition diamond. We measure spin coherence times approaching 100 μ s and observe increased photoluminescence collection from shallow implant NV centers in these slabs. We anticipate these slabs to be appealing as quantum memory nodes in hybrid diamond nanophotonic systems.
Since quantum information technologies are expected to offer communication security and high computational capacities, research in the field is currently attracting a lot of attention. Among the materials studied so far, rare earth doped inorganic insulators are one of the most promising. With the different available trivalent rare earth ions, the visible and the IR range including the telecom wavelength at 1.5 μm can be covered. Transitions are usually narrow, and at low temperatures, long optical and spin coherence times can often be observed. Investigations using bulk single crystals have already led to many promising results. Recently, spectroscopic studies have been extended to other forms of inorganic materials, such as transparent ceramics, thin films, and nanoparticles for single rare‐earth qubits. Progress in these areas is expected to offer many new possibilities for the design of quantum light‐matter interfaces and scalable quantum memories and processors.
Abstract Nitrogen‐vacancy (NV) centers in diamond are optically addressable spin defects with great potential for nanoscale quantum sensing. A key application of NV centers is the detection of external spins at the diamond surface. Among metals, platinum thin films – widely used in spintronics, catalysis, and electrochemistry – provide a particularly interesting system for such studies. However, the interaction between NV centers and metals is known to affect their quantum sensing capabilities. In this work, five platinum‐covered diamond samples containing shallow NVs created via nitrogen implantation with different energies (2.5–60 keV) are used to investigate the optical and quantum properties of NV ensembles beneath metal films. A substantial reduction of the photoluminescence lifetime and a pronounced decrease of the NV − population are found for NV ensembles located near the diamond‐platinum interface. As a result, optically detected magnetic resonance experiments could only be efficiently performed on diamonds implanted with at least 20 keV, where a strong increase in the T 2 coherence time beneath the platinum thin films is observed. The study describes the various processes affecting NV centers near diamond‐platinum interfaces and provides guidance for the integration of thin metal films with near‐surface NV centers.