Optical and microstructural characterization of Er3+ doped epitaxial cerium oxide on silicon
Gregory D. Grant, Jiefei Zhang, Ignas Masiulionis, Swarnabha Chattaraj, Kathryn E. Sautter, Sean E. Sullivan, Rishi Chebrolu, Yuzi Liu, Jessica B. Martins, Jens Niklas, Alan Dibos, Sumit Kewalramani, J. W. Freeland, Jianguo Wen, Oleg G. Poluektov, F. Joseph Heremans, D. D. Awschalom, Supratik Guha
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 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%.
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.
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.
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.
This work explores erbium-doped calcium molybdate (Er:CaMoO4) thin films grown on silicon and yttria stabilized zirconia (YSZ) substrates, as a potential solid state system for C-band (utilizing the ∼1.5 μm Er3+ 4f–4f transition) quantum emitters for quantum network applications. Through molecular beam epitaxial growth experiments and electron microscopy, X-ray diffraction, and reflection electron diffraction studies, we identify an incorporation limited deposition regime that enables a 1:1 Ca:Mo ratio in the growing film leading to single phase CaMoO4 formation that can be in situ doped with Er (typically 2–100 ppm). We further show that growth on silicon substrates is single phase but polycrystalline in morphology, while growth on YSZ substrates leads to high-quality epitaxial single crystalline CaMoO4 films. We perform preliminary optical and microwave characterization on the suspected Y1–Z1 transition of 2 ppm, 200 nm epitaxial Er:CaMoO4 annealed thin films and extract an optical inhomogeneous linewidth of 9.1(1) GHz, an optical excited state lifetime of 6.7(2) ms, a spectral diffusion-limited homogeneous linewidth of 6.7(4) MHz, and an EPR linewidth of 1.10(2) GHz.
This work explores erbium-doped calcium molybdate (Er:CaMoO4) thin films grown on silicon and yttria stabilized zirconia (YSZ) substrates, as a potential solid state system for C-band (utilizing the ∼1.5 μm Er3+ 4f–4f transition) quantum emitters for quantum network applications. Through molecular beam epitaxial growth experiments and electron microscopy, X-ray diffraction, and reflection electron diffraction studies, we identify an incorporation limited deposition regime that enables a 1:1 Ca:Mo ratio in the growing film leading to single phase CaMoO4 formation that can be in situ doped with Er (typically 2–100 ppm). We further show that growth on silicon substrates is single phase but polycrystalline in morphology, while growth on YSZ substrates leads to high-quality epitaxial single crystalline CaMoO4 films. We perform preliminary optical and microwave characterization on the suspected Y1–Z1 transition of 2 ppm, 200 nm epitaxial Er:CaMoO4 annealed thin films and extract an optical inhomogeneous linewidth of 9.1(1) GHz, an optical excited state lifetime of 6.7(2) ms, a spectral diffusion-limited homogeneous linewidth of 6.7(4) MHz, and an EPR linewidth of 1.10(2) GHz.
Microstructural and preliminary optical and microwave characterization of erbium doped CaMoO4 thin films
This work explores erbium-doped calcium molybdate (CaMoO4) thin films grown on silicon and yttria stabilized zirconia (YSZ) substrates, as a potential solid state system for C-band (utilizing the $\sim$1.5 μm Er3+ 4f-4f transition) quantum emitters for quantum network applications. Through molecular beam epitaxial growth experiments and electron microscopy, X-ray diffraction and reflection electron diffraction studies, we identify an incorporation limited deposition regime that enables a 1:1 Ca:Mo ratio in the growing film leading to single phase CaMoO4 formation that can be in-situ doped with Er (typically 2-100 ppm). We further show that growth on silicon substrates is single phase but polycrystalline in morphology; while growth on YSZ substrates leads to high-quality epitaxial single crystalline CaMoO4 films. We perform preliminary optical and microwave characterization on the suspected Y1−Z1 transition of 2 ppm, 200 nm epitaxial CaMoO4 annealed thin films and extract an optical inhomogeneous linewidth of 9.1(1) GHz, an optical excited state lifetime of 6.7(2) ms, a spectral diffusion-limited homogeneous linewidth of 6.7(4) MHz, and an EPR linewidth of 1.10(2) GHz.