In highly purified host, the coherence of quantum emitters is ultimately limited by hyperfine interactions between the emitter and lattice nuclei possessing non-zero nuclear magnetic moments. This limitation can only be mitigated through isotopic purification. In this work, we investigate CeO2 as a host composed entirely of nuclei with zero nuclear moment. High-quality CeO2 thin films were grown by PLD and doped with Tm and Er ions. Structural characterization using X-ray diffraction, atomic force microscopy, and ion channeling confirms single-crystalline, atomically smooth films with dopants substitutionally incorporated at Ce lattice sites. Photoluminescence lifetime measurements show significantly longer lifetimes for Er-doped CeO2 (2.9 - 5.3 ms) compared with Tm-doped films (14 - 68 μs). Moreover, the Er-doped PLD films exhibit longer lifetimes at ~1% dopant concentration than previously reported for MBE-grown films. Density functional theory calculations reveal a substantial overlap between unoccupied O 2p and Tm 4f states near the valence band maximum, whereas Er 4f states remain well isolated. This electronic interaction likely introduces non-radiative recombination pathways in Tm-doped CeO2, explaining the reduced lifetimes. These findings highlight the importance of selecting appropriate dopant-host combinations and optimized growth conditions to minimize non-radiative channels for quantum applications.
In highly purified host, the coherence of quantum emitters is ultimately limited by hyperfine interactions between the emitter and lattice nuclei possessing non-zero nuclear magnetic moments. This limitation can only be mitigated through isotopic purification. In this work, we investigate CeO2 as a host composed entirely of nuclei with zero nuclear moment. High-quality CeO2 thin films were grown by PLD and doped with Tm and Er ions. Structural characterization using X-ray diffraction, atomic force microscopy, and ion channeling confirms single-crystalline, atomically smooth films with dopants substitutionally incorporated at Ce lattice sites. Photoluminescence lifetime measurements show significantly longer lifetimes for Er-doped CeO2 (2.9 - 5.3 ms) compared with Tm-doped films (14 - 68 μs). Moreover, the Er-doped PLD films exhibit longer lifetimes at ~1% dopant concentration than previously reported for MBE-grown films. Density functional theory calculations reveal a substantial overlap between unoccupied O 2p and Tm 4f states near the valence band maximum, whereas Er 4f states remain well isolated. This electronic interaction likely introduces non-radiative recombination pathways in Tm-doped CeO2, explaining the reduced lifetimes. These findings highlight the importance of selecting appropriate dopant-host combinations and optimized growth conditions to minimize non-radiative channels for quantum applications.
ABSTRACT In a highly purified host, the coherence of quantum emitters is ultimately limited by hyperfine interactions between the emitter and lattice nuclei possessing non‐zero nuclear magnetic moments. This limitation can only be mitigated through isotopic purification. In this work, we investigate CeO 2 as a host composed entirely of nuclei with zero nuclear moment. High‐quality CeO 2 thin films were grown by PLD and doped with Tm and Er ions. Structural characterization using X‐ray diffraction, atomic force microscopy, and ion channeling confirms single‐crystalline, atomically smooth films with dopants substitutionally incorporated at Ce lattice sites. Photoluminescence lifetime measurements show significantly longer lifetimes for Er‐doped CeO 2 (2.9 – 5.3 ms) compared with Tm‐doped films (14 – 68 µs). Moreover, the Er‐doped PLD films exhibit longer lifetimes at ∼1% dopant concentration than previously reported for MBE‐grown films. Density functional theory calculations reveal a substantial overlap between unoccupied O 2p and Tm 4f states near the valence band maximum, whereas Er 4f states remain well isolated. This electronic interaction likely introduces non‐radiative recombination pathways in Tm‐doped CeO 2 , explaining the reduced lifetimes. These findings highlight the importance of selecting appropriate dopant‐host combinations and optimized growth conditions to minimize non‐radiative channels for quantum applications.
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%.
Epitaxial growth of erbium-doped cerium oxide (Er:CeO2) is achieved on Si (111) substrates by the cooperative integration of Si and oxide molecular beam epitaxy (MBE) technologies. Lattice matching between CeO2 and Si provides an attractive opportunity to build dilutely doped Er-based optical devices on a Si chip. The CeO2 host crystal is optically transparent for the telecom C-band wavelength and has quite a small magnetic moment, which serves as a disturbance-free environment for the two-level system formed in the doped Er. After the systematic optimization of the growth conditions for stoichiometric Er:CeO2; i.e., (Er + Ce)/O = 1/2, we varied the Er concentration in a range of 1 ~4%. The doped Er showed well-defined optical transitions at the wavelength of 1.533 μm irrespective of the Er concentration. With decreasing Er concentration, enhancement of the luminescence intensity, narrowing of the spectral width, and an increase in the radiative lifetime were observed. The results suggest that CeO2 on Si is promising as a platform for the doped-Er-based optical devices and their quantum optics applications.
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.
Rare-earth ions (REIs) have incomplete 4f shells and possess narrow optical intra-4f transitions due to shielding from electrons in the 5s and 5p orbitals, making them good candidates for solid-state optical quantum memory. The emission of Er3+ in the telecom C-band (1530 nm–1565 nm) makes it especially attractive for this application. In order to build practical, scalable devices, the REI needs to be embedded in a non-interacting host material, preferably one that can be integrated with silicon. In this paper, we show that Er3+ can be isovalently incorporated into epitaxial Y2O3 thin films on Si (111). We report on the synthesis of epitaxial, single-crystalline Er:Y2O3 on Si with a narrow inhomogeneous linewidth in the photoluminescence (PL) spectra, 5.1 GHz (<100 mK), and an optical excited state lifetime of 8.1 ms. The choice of Y2O3 was driven by its low nuclear spin and small lattice mismatch with Si. Using PL and electron paramagnetic resonance, we show that Er3+ substitutes for Y in the crystal lattice. The role of interfacial SiOx, diffusion of silicon into the film, and the effect of buffer layers on the inhomogeneous PL linewidth are examined. We also find that the linewidth decreased monotonically with film thickness but surprisingly exhibits no correlation with the film crystalline quality, as measured by the x-ray rocking curve scans, suggesting other factors at play that limit the inhomogeneous broadening in Y2O3 films.
Erbium (Er) is a rare-earth element that is expected to be a platform for manipulation of quantum information by utilizing telecommunication-wavelength photons.However, high-quality epitaxial growth of Er-doped host crystals is difficult, and the memory time of quantum information, which determines the performance of quantum manipulation, is much shorter than theoretically predicted.We investigated a good-compatibility rare-earth oxide as a host crystal for Er.The host oxide crystal, cerium oxide (CeO 2 ), had its nuclear spin removed (i.e., magnetically purified).The nuclear spin is the main factor that shortens the lifetime of quantum-information retention time.In this article, we describe high-quality epitaxial growth of CeO 2 and its optical properties as a thin film grown on a silicon substrate.