A Theoretical Study on
the Structural and Energy Spectral
Properties of Ce<sup>3+</sup> Ions Doped in Various Fluoride Compounds
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Abstract
Geometry optimization and wave function-based complete-active-space
self-consistent field-embedded cluster calculations have been performed
for a series of Ce<sup>3+</sup>-doped fluoride compounds (CaF<sub>2</sub>, YF<sub>3</sub>, LaF<sub>3</sub>, KMgF<sub>3</sub>, LiYF<sub>4</sub>, K<sub>2</sub>YF<sub>5</sub>, and KY<sub>3</sub>F<sub>10</sub>) to investigate local coordination structures, crystal field parameters,
and 5d<sup>1</sup> energy-level structures of doping Ce<sup>3+</sup> ions. The crystal-field parameters of Ce<sup>3+</sup> are extracted
from the calculated energies and wave functions. The calculated crystal-field
parameters and 5d<sup>1</sup> energy-level structures show excellent
consistency with the experimental results. Our calculations show that
the onset of 4f → 5d absorption, which is important in phosphors
and scintillators, can be well-predicted. Apart from that, the distortion
of local structure due to doping, the wave functions, and the crystal-field
parameters of 4f<sup>1</sup> and 5d<sup>1</sup> states of Ce<sup>3+</sup> in the hosts can be obtained. Those can seldom be obtained by fitting
empirical crystal-field Hamiltonian to experimental data but are required
by some detailed theoretical analysis, such as the calculation of
transition intensities and hyperfine splittings. The obtained crystal-field
parameters of Ce<sup>3+</sup> may also be useful for other lanthanide
ions in the same hosts