The present invention has been achieved by perceiving thefact to the effect that a semiconductor production process-likemanner such as CVD method or the like by which materials and filmthickness can be controlled in an atomic scale may be utilizedin case of preparing thin-film crystal, and employing suchsemi-conductor production process-like manner being quite differentfrom conventional technique. The invention relates to preparationof crystalline thin-films for solid-state lasers wherein asubstrate contained in a vessel under a high vacuum condition isheated, materials for forming the laser material are suppliedonto the surface of the aforesaid substrate in the form of gas,ion, single metal or metal compound to grow crystal on thesurface of the aforesaid substrate, and a material of active ionicspecies is supplied onto the surface of the aforesaid substratesimultaneously with supply of the aforesaid materials for formingthe laser host crystal, thereby controlling valence number of thematerial of active ionic species so as to be identical with thevalence number of the metal ion constituting the crystal of theaforesaid laser host crystal.
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