Frequency non-degenerate sequential excitation of the impurity trapped exciton in strontium fluoride crystals doped with ytterbium

Abstract

We model the dynamic behaviour observed for impurity-trapped excitons in SrF2:Yb2+ using transient photoluminescence enhancement induced via a two-frequency, sequential excitation process employing an UV optical parametric amplifier synchronized to an IR free electron laser (FEL). We observe sharp transitions interpreted as a change of state of the localized hole and broad bands interpreted as a change of state of the delocalized electron. Our modeling indicates that the 4f crystal-field interaction is 25% smaller than in CaF2. The photoluminescence enhancement transients are analyzed across a range of excitation frequencies using a system of rate equations. The temporal behavior is explained in terms of intra-excitonic relaxation, local lattice heating by the FEL, and liberation of electrons from trap states.