ArXiv · 2026
Rare-earth-ion based molecular crystals are emerging as a promising platform for quantum information applications, combining long optical coherence times with the chemical tunability of coordination chemistry. Here we present a comprehensive optical characterisation of twelve Eu³⁺-based molecular complexes, with a focus on the coherent ⁵D₀ ⟶ ⁷F₀ transition at ∼580 nm. Judd-Ofelt analyses are performed across all complexes, providing insights into ligand-field environments, local point-group symmetries, and the resulting branching ratios of the coherent transition. We find that lower point-group symmetry (C₁, C₂) yields higher branching ratios of the ⁵D₀ ⟶ ⁷F₀ transition, exceeding 1% in several complexes. Optical inhomogeneous linewidths measured at 4.2 K reveal narrow linewidths for some complexes of below ten GHz, indicative of a highly ordered crystalline environment. Optical coherence measurements of one of the complexes, 5-Eu, yields an optical coherence time of T₂ᵒᵖᵗ = 2.3 μs at 4.2 K, comparable to the best-performing molecular systems reported to date. Systematic characterisation and quantitative comparison will be key to find structure-property relations guiding rational design of optimised complexes for quantum information applications.
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