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We systematically study cross-relaxation (CR) and ion clustering in Tm3+:CaF2 crystals using a spectroscopic approach. For this, the luminescence from the 3H4 and 3F4 states was monitored for a broad range of Tm3+ doping concentrations, from 0.01 at.% to 7 at.%. The decay curves were fitted using a model of two ions classes, namely isolated ions showing no energy-transfer processes and ions with neighbors exhibiting both CR and energy-transfer upconversion (ETU), and accounting for energy-migration. The fraction of ions with neighbors and the microscopic concentration-independent CR and ETU parameters are deduced. The critical Tm3+ doping level for which at least half of the active ions are clustered is only 0.7 at.%. The obtained results are relevant for achieving efficient laser operation of Tm3+:CaF2 crystals at the 3F4 → 3H6 (at ~1.9 μm) and the 3H4 → 3H5 (at ~2.3 μm) transitions.

Cross-relaxation and ion clustering in Tm3+:CaF2 crystals