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arXiv:2309.13490

Nanocavity-Mediated Purcell Enhancement of Er in TiO2 Thin Films Grown via Atomic Layer Deposition

Ji, Cheng, Michael T. Solomon, Gregory D. Grant, Kōichi Tanaka, Muchuan Hua, Jianguo Wen, Sagar Kumar Seth, Connor P. Horn, Ignas Masiulionis, Manish Kumar Singh, Sean E. Sullivan, F. Joseph Heremans, D. D. Awschalom, Supratik Guha, Alan Dibos

Published Sep 23, 2023• 1 citation
arXivHTMLPDF

Abstract

The use of trivalent erbium (Er$^{3+}$), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunications devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface makes it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO$_2$) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping control over the Er concentration. Even though the as-grown films are amorphous, after oxygen annealing they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO$_2$. Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (300) of their optical lifetime. Our findings demonstrate a low-temperature, non-destructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories.

DOI
10.48550/arxiv.2309.13490

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High Resolution Image Download MS PowerPoint Slide The use of trivalent erbium (Er 3+ ), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunication devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface make it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO 2 ) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping controls over the Er concentration. Even though the as-grown films are amorphous after oxygen annealing, they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO 2 . Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (≈300) of their optical lifetime. Our findings demonstrate a low-temperature, nondestructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories.

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The use of trivalent erbium (Er3+^{3+}3+), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunications devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface makes it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO2_22​) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping control over the Er concentration. Even though the as-grown films are amorphous, after oxygen annealing they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO2_22​. Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (300) of their optical lifetime. Our findings demonstrate a low-temperature, non-destructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories.
High Resolution Image Download MS PowerPoint Slide The use of trivalent erbium (Er 3+ ), typically embedded as an atomic defect in the solid-state, has widespread adoption as a dopant in telecommunication devices and shows promise as a spin-based quantum memory for quantum communication. In particular, its natural telecom C-band optical transition and spin-photon interface make it an ideal candidate for integration into existing optical fiber networks without the need for quantum frequency conversion. However, successful scaling requires a host material with few intrinsic nuclear spins, compatibility with semiconductor foundry processes, and straightforward integration with silicon photonics. Here, we present Er-doped titanium dioxide (TiO 2 ) thin film growth on silicon substrates using a foundry-scalable atomic layer deposition process with a wide range of doping controls over the Er concentration. Even though the as-grown films are amorphous after oxygen annealing, they exhibit relatively large crystalline grains, and the embedded Er ions exhibit the characteristic optical emission spectrum from anatase TiO 2 . Critically, this growth and annealing process maintains the low surface roughness required for nanophotonic integration. Finally, we interface Er ensembles with high quality factor Si nanophotonic cavities via evanescent coupling and demonstrate a large Purcell enhancement (≈300) of their optical lifetime. Our findings demonstrate a low-temperature, nondestructive, and substrate-independent process for integrating Er-doped materials with silicon photonics. At high doping densities this platform can enable integrated photonic components such as on-chip amplifiers and lasers, while dilute concentrations can realize single ion quantum memories.
High Resolution Image Download MS PowerPoint Slide Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects, such as erbium, suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Moreover, many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here, we present a scalable approach toward CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of 5 × 10 4 and corresponding Purcell-enhanced optical emission rates of the erbium ensembles in excess of 200. This easily fabricated materials platform represents an important step toward realizing telecom quantum memories in a scalable qubit architecture compatible with mature silicon technologies.
The use of rare earth ions (REIs)—typically embedded as atomic defects in solids—has emerged as a promising strategy for practical quantum memories. In particular, the Er ion has garnered significant attention due to its telecom C-band optical transition, which makes it a suitable candidate for integration into existing optical fiber networks without the need for photon wavelength conversion. However, successful scalability of such a quantum memory platform would benefit greatly from employing a host material that is fully compatible with silicon and modern CMOS fabrication processes. In this study, we present the synthesis of Er-doped TiO2 thin films directly on standard silicon or silicon-on-insulator (SOI) substrates using atomic layer deposition (ALD). Our thin film exhibits favorable emitter properties at cryogenic temperatures (T = 3.5 K), including a narrow inhomogeneous linewidth and optical lifetime approaching that of bulk values. Additionally, the ALD process provides ample opportunities for device fabrication and integration with other components, further enhancing its potential for practical applications. Overall, our findings suggest that Er-doped TiO2 thin films synthesized via ALD represent a promising approach for developing practical quantum memories that can be seamlessly integrated with silicon photonics. This work lays a foundation for the development of quantum technologies with potential applications in communication, computing, and cryptography.
Defects and dopant atoms in solid state materials are a promising platform for realizing single photon sources and quantum memories, which are the basic building blocks of quantum repeaters needed for long distance quantum networks. In particular, trivalent erbium (Er3+) is of interest because it couples C-band telecom optical transitions with a spin-based memory platform. In order to produce quantum repeaters at the scale required for quantum networks it is imperative to integrate these necessary building blocks with mature and scalable semiconductor processes. In this work, we demonstrate the optical isolation of single Er3+ ions in CMOS-compatible titanium dioxide (TiO2) thin films monolithically integrated on a silicon-on-insulator photonics platform. Our results demonstrate an initial step toward the realization of a monolithically integrated and scalable quantum photonics package based on Er3+ doped thin films.
Solid-state spin-based quantum systems have emerged as popular platforms for quantum networking applications due to their optical interfaces, their long-lived quantum memories, and their natural compatibility with semiconductor manufacturing. Photonic crystal cavities are often used to enhance radiative emission; however, fabrication of the necessary subwavelength cavities is typically limited to small batch electron beam lithography. In this work, we demonstrate high quality factor, small mode volume nanobeam cavities fabricated on a scalable silicon photonic foundry platform. The foundry fabricated cavities are then interfaced with single erbium ions through backend deposition of TiO 2 thin films lightly doped with erbium. Single ion lifetime measurements indicate Purcell enhancement up to about 500, thereby demonstrating a route toward manufacturable deterministic single photon sources in the telecom C-band.
Controlled growth of rare-earth-doped TiO2_{2}2​ thin films on III-V semiconductors for hybrid quantum photonic interfaces
Quantum photonic networks require two distinct functionalities: bright single-photon sources and long-lived quantum memories. III-V semiconductor quantum dots excel as deterministic and coherent photon emitters, while rare-earth ions such as erbium (Er3+^{3+}3+) in crystalline oxides offer exceptional spin and optical coherence at telecom wavelengths. Combining these systems and their functionalities via direct epitaxy is challenging due to lattice mismatch and incompatible growth conditions. Here we demonstrate low-temperature pulsed laser deposition of Er3+^{3+}3+-doped TiO2_{2}2​ thin films directly on GaAs and GaSb substrates. Controlled surface preparation with an arsenic cap and an oxygen-deficient buffer layer enables the growth of epitaxial anatase TiO2_{2}2​ (001) at 390o^{o}oC with sub-300 pm surface roughness, while avoiding interface degradation. In contrast, high-temperature oxide desorption or growth temperatures drive the transition to rough, polycrystalline rutile film, as confirmed by transmission electron microscopy. Minimal coincident interface area (MCIA) modeling explains the orientation-selective growth on GaAs and GaSb. Raman and cryogenic photoluminescence excitation spectroscopy verify the crystal phase and optical activation of Er3+^{3+}3+ ions. This multi-parameter growth strategy helps preserve III-V quantum dot functionality and yields smooth surfaces suitable for low-loss nanophotonic structures. Our results establish a materials platform for monolithically integrating rare-earth quantum memories with semiconductor photon sources, paving the way toward scalable hybrid quantum photonic chips.