G. Matmon, S. A. Lynch, T. F. Rosenbaum, A. J. Fisher, and G. Aeppli
Because of its role as a model system with tunable quantum fluctuations and quenched disorder, and the desire for optical control and readout of its states, we have used high-resolution optical absorption spectroscopy to measure the crystal-field excitations for Ho3+ ions in LiHoxY1−xF4 from the terahertz to visible regimes. We show that many of the excitations yield very narrow lines visibly split even by the nuclear hyperfine interaction, making Ho3+ in LiHoxY1−xF4 a candidate host for optically addressable electronuclear qubits with quality factors as high as Q=4.7×105 , where the higher-lying levels are electronic singlets. Optical transitions in the easily accessible near- and mid-infrared are narrow enough to allow readout of the ground-state electronuclear qubits responsible for the interesting magnetism of LiHoxY1−xF4 . While many of the higher-lying states have been observed previously, we also report here detailed spectra of terahertz excitations. The strengths of the electric and magnetic dipole crystal-field transition lines of five of the lowest excited spin-orbit manifolds of dilute LiYF4 :Ho3+ were calculated and compared with measurement. The magnitude of the nuclear hyperfine coupling was used to assign the correct upper and lower states to transition lines.
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