Abstract

In this paper, the first investigation of stimulated Raman scattering (SRS) effects in the tetragonal crystal LiLuF4 is presented. It is known as a promising host-material for trivalent lasant lanthanides (Ln3+). We discovered its three “original” and one “combined” SRS-promoting modes at room temperature under picosecond laser excitation in the visible and near-IR spectral range. Apart from multi-phonon Stokes and anti-Stokes generation, we observed cross-cascaded χ(3) ↔ χ(3) processes involving different pairs of SRS-active phonons. Furthermore, a comparative estimation of the stead-state Raman gain coefficient for first Stokes generation in LiLuF4 related to the most active SRS-phonon mode with ωSRS1 ≈ 323 cm−1 has been carried out for both the visible and near-IR. A brief review of the pioneering publications on laser action in Ln3+-ions of all known fluoride SRS-active single crystals is given in tabular form as well.

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