Optical spectra and emission characteristics of terbium-doped potassium–lead double chloride crystals (KPb2Cl5:Tb3+)

Abstract

Optical transitions in KPb2Cl5:Tb3+ crystals are studied experimentally and theoretically. The absorption cross-section spectra are plotted and the oscillator strengths of transitions from the ground terbium state to excited multiplets are determined. Intensity parameters Ωt for KPC:Tb3+ are determined by the Judd–Ofelt method to be Ω2 = 2.70 × 10–20 cm2, Ω4 = 7.0 × 10–20 cm2, and Ω6 = 0.72 × 10–20 cm2. These values were used to calculate such characteristics of spontaneous radiative transitions as oscillator strengths, probabilities of radiative transitions, and radiative lifetimes. The emission spectra of KPb2Cl5:Tb3+ crystals upon UV excitation and the decay kinetics of luminescence from the excited 5 D 3 and 5 D 4 levels are studied experimentally, the lifetimes of these levels are determined, and the dependences of the rates of nonradiative relaxation from the excited 7 F j (j = 0–5), 5 D 4, and 5 D 3 levels to lower-lying terbium levels are calculated. It is shown that the population of the 5 D 4 level in KPC:Tb3+ crystals occurs according to a cascade scheme, which leads to quenching of the 5 D 3 level. The calculated data agree well with the known experimental rates of multiphonon nonradiative transitions for Dy:KPC, Nd:KPC, Er:KPC, Tb:KPB, and Nd:KPB crystals. It is shown that transitions in the near-IR (3–6 μm) region in double halide crystals (MPb2Hal5) are almost unquenched and the rates of nonradiative relaxation of excited levels spaced by energy gaps ΔE ji > 1000 cm–1 are W ji NR < 103s–1. This circumstance suggests that it is possible to obtain stimulated emission in KPb2Cl5:RE3+ crystals in the IR spectral region up to 6 μm.