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Correlation of the orbach relaxation coefficient with optical linewidths - laf sub 3-er super 3 super plus.

P. L. Scott, W. C. Scott, William M. Yen

Published Feb 15, 1965• 0 citations
OpenAlex

Abstract

Excited state lifetime equivalence to Orbach relaxation coefficient correlated with optical linewidths of trivalent erbium doped lanthanum fluoride

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CORRELATION OF THE ORBACH RELAXATION COEFFICIENT WITH OPTICAL LINEWIDTHS: LaFsub3sub 3sub3:Ersup3sup 3sup3sup+sup +sup+
We have employed a purely optical method to measure spin-lattice relaxation in the lower excited (4)S(3/2) state of Er(3+) in LaF(3) at helium temperatures. Above 3 K the relaxation is dominated by an Orbach process through the upper (4)S(3/2) state. Below 3 K the relaxation is caused by some residual mechanism that obscures the Kramers-Van Vleck direct process. By relating the Orbach relaxation measurements to the homogeneous broadening of the upper (4)S(3/2) level, we determine values of the transition rates between the upper and lower (4)S(3/2) states.
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%.
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.