Optical and microstructural studies of erbium-doped TiO2 thin films on silicon, SrTiO3, and sapphire
Manish Kumar Singh, Gregory D. Grant, Gary Wolfowicz, Jianguo Wen, Sean E. Sullivan, Abhinav Prakash, Alan Dibos, F. Joseph Heremans, D. D. Awschalom, Supratik Guha
Rare-earth ion doped oxide thin films integrated on silicon substrates provide a route toward scalable, chip-scale platforms for quantum coherent devices. Erbium-doped TiO2 is an attractive candidate: the Er3+ optical transition is compatible with C-band optical fiber communications, while TiO2 is an insulating dielectric compatible with silicon process technology. Through structural and optical studies of Er-doped TiO2 thin films grown via molecular beam deposition on silicon, SrTiO3, and sapphire substrates, we have explored the impact of polycrystallinity and microstructure on the optical properties of the Er emission. Comparing polycrystalline TiO2(rutile)/Si with single-crystalline TiO2(rutile)/r-sapphire and polycrystalline TiO2(anatase)/Si with single-crystalline TiO2(anatase)/SrTiO3, we observe that the inhomogeneous linewidth (Γinh) of the most prominent peak in the Er spectrum (the Y1–Z1 transition, 1520 and 1533 nm in rutile and anatase TiO2) is significantly narrower in the polycrystalline case. This implies a relative insensitivity to extended structural defects and grain boundaries in such films (as opposed to, e.g., point defects). We show that the growth of an undoped, underlying TiO2 buffer on Si can reduce Γinh by a factor of 4–5. Expectedly, Γinh also reduces with decreasing Er concentrations: we observe a ∼2 order of magnitude reduction from ∼1000 ppm Er to ∼10 ppm Er. Γinh then gets limited to a residual value of ∼5 GHz that is insensitive to further reduction in the Er concentration. Based upon the above results, we argue that the optical properties in these thin films are limited by the presence of high “grown-in” point defect concentrations.
Rare-earth ion doped oxide thin films integrated on silicon substrates provide a route toward scalable, chip-scale platforms for quantum coherent devices. Erbium-doped TiO2 is an attractive candidate: the Er3+ optical transition is compatible with C-band optical fiber communications, while TiO2 is an insulating dielectric compatible with silicon process technology. Through structural and optical studies of Er-doped TiO2 thin films grown via molecular beam deposition on silicon, SrTiO3, and sapphire substrates, we have explored the impact of polycrystallinity and microstructure on the optical properties of the Er emission. Comparing polycrystalline TiO2(rutile)/Si with single-crystalline TiO2(rutile)/r-sapphire and polycrystalline TiO2(anatase)/Si with single-crystalline TiO2(anatase)/SrTiO3, we observe that the inhomogeneous linewidth (Γinh) of the most prominent peak in the Er spectrum (the Y1–Z1 transition, 1520 and 1533 nm in rutile and anatase TiO2) is significantly narrower in the polycrystalline case. This implies a relative insensitivity to extended structural defects and grain boundaries in such films (as opposed to, e.g., point defects). We show that the growth of an undoped, underlying TiO2 buffer on Si can reduce Γinh by a factor of 4–5. Expectedly, Γinh also reduces with decreasing Er concentrations: we observe a ∼2 order of magnitude reduction from ∼1000 ppm Er to ∼10 ppm Er. Γinh then gets limited to a residual value of ∼5 GHz that is insensitive to further reduction in the Er concentration. Based upon the above results, we argue that the optical properties in these thin films are limited by the presence of high “grown-in” point defect concentrations.
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) 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.
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%.
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 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.
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.