Narrow Optical Line Widths in Erbium Implanted in TiO 2
Christopher M. Phenicie, Paul Stevenson, Sacha Welinski, Brendon C. Rose, Abraham T. Asfaw, R. J. Cava, S. A. Lyon, Nathalie P. de Leon, Jeff D. Thompson
Atomic and atomlike defects in the solid state are widely explored for quantum computers, networks, and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er 3+ ions can be introduced via ion implantation into TiO 2, a host crystal that has not been studied extensively for rare earth ions and has a low natural abundance of nuclear spins. We observe efficient incorporation of the implanted Er 3+ into the Ti 4+ site (>50% yield) and measure narrow inhomogeneous spin and optical line widths (20 and 460 MHz, respectively) that are comparable to bulk-doped crystalline hosts for Er 3+ . This work demonstrates that ion implantation is a viable path to studying rare earth ions in new hosts and is a significant step toward realizing individually addressed rare earth ions with long spin coherence times for quantum technologies.
Atomic and atomlike defects in the solid state are widely explored for quantum computers, networks, and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er 3+ ions can be introduced via ion implantation into TiO 2, a host crystal that has not been studied extensively for rare earth ions and has a low natural abundance of nuclear spins. We observe efficient incorporation of the implanted Er 3+ into the Ti 4+ site (>50% yield) and measure narrow inhomogeneous spin and optical line widths (20 and 460 MHz, respectively) that are comparable to bulk-doped crystalline hosts for Er 3+ . This work demonstrates that ion implantation is a viable path to studying rare earth ions in new hosts and is a significant step toward realizing individually addressed rare earth ions with long spin coherence times for quantum technologies.
Erbium-doped materials can serve as spin-photon interfaces with optical transitions in the telecom C band, making them an exciting class of materials for long-distance quantum communication. However, the spin and optical coherence times of Er3+ ions are limited by currently available host materials, motivating the development of new Er3+-containing materials. Here we demonstrate the use of ion implantation to efficiently screen prospective host candidates, and show that disorder introduced by ion implantation can be mitigated through post-implantation thermal processing to achieve inhomogeneous linewidths comparable to bulk linewidths in as-grown samples. We present optical spectroscopy data for each host material, which allows us to determine the level structure of each site, allowing us to compare the environments of Er3+ introduced via implantation and via doping during growth. We demonstrate that implantation can generate a range of local environments for Er3+, including those observed in bulk-doped materials, and that the populations of these sites can be controlled with thermal processing.
Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.
Rare-earth ions (REIs) doped into solid-state crystal hosts offer an attractive platform for realizing quantum interconnects that can function as quantum memories and quantum repeaters. The 4f valence electrons of REIs are shielded by 5s and 5p electrons and undergo highly coherent transitions even when embedded in host crystals. In particular, Er3+ has an optical transition in the telecom band that is suitable for low-loss communication. Recently, REIs in thin film systems have gained interest due to potential advantages in providing a flexible host crystal environment, enabling scalable on-chip integration with other quantum devices. Here, we investigate the structural and optical properties of Er-doped anatase TiO2 thin films on LaAlO3 (001) substrates. By choosing a system with minimal lattice mismatch and adjusting Er-dopant concentration, we achieve optical inhomogeneous linewidths of 5 GHz at 4.5 K. We show that 9 nm-thick buffer and capping layers can reduce the linewidth by more than 40%, suggesting a pathway to further narrowing linewidths in this system. We also identify that Er3+ ions mainly incorporate into substitutional Ti4+ sites with non-polar D2d symmetry, which makes Er dopants insensitive to the first order to local electric fields from impurities and is desirable for coherence properties of Er3+ spins.
Development of a Scalable Quantum Memory Platform -- Materials Science of Erbium-Doped TiO2 Thin Films on Silicon
Rare-earth ions (REI) have emerged as an attractive candidate for solid-state qubits, particularly as a quantum memory. Their 4f-4f transitions are shielded by filled 5s and 5p orbitals, offering a degree of protection from external electric fields. Embedded within a thin film oxide host, REIs could enable a qubit platform with significant memory capabilities. Furthermore, a silicon-compatible thin film form factor would enable the use of standard semiconductor fabrication processes to achieve chip-based integrability and scalability for functional quantum networks. Towards this goal, we have carried out optical and microstructural studies of erbium-doped polycrystalline and epitaxial TiO2 thin films on Si (100), r-sapphire, and SrTiO3 (100). We observe that the inhomogeneous optical linewidth of the Er photoluminescence is comparable or better for polycrystalline Er:TiO2(grown on Si) in comparison to single crystal epitaxial films on sapphire or SrTiO3, implying a relative insensitivity to extended defects. We investigated the effect of the film/substrate and film/air interface and found that the inhomogeneous linewidth and spectral diffusion can be significantly improved via bottom buffer and top capping layers of undoped TiO2. Using such approaches, we obtain inhomogeneous linewidths of 5.2 GHz and spectral diffusion of 180 MHz in Er:TiO2 /Si(100) films and have demonstrated the engineerability of quantum-relevant properties in these thin films.
Isotopically enriched epitaxial CaWO4 thin films for Er3+ spin-photon quantum interfaces
Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability1−3. Among them, Er3+ doped CaWO4 is promising because it possesses narrow optical linewidth transitions and a long spin coherence time4−6. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% 183W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er3+ doped CaWO4 thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO4 thin films using an isotopically purified 186WO3 source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. 183W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO4 thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.