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The invention provides a means for preparing rare-earth-doped α-(Al1-xGax)2O3 films by molecular beam epitaxy (MBE), The invention provides a composition of matter, rare-earth-doped α-(Al1-xGax)2O3 films, and methods to provide thin films of this material. The invention also provides a means to prepare thin film rare-earth-doped α-(Al1-xGax)2O3, including Nd : α-(Al1-xGax)2O3, for use in solid state lasers. Rare-earth-doped α-Ga2O3 and rare-earth-doped alloys of α-a2O3 and α-Αl2O3 with the same single-crystal structure independent of Ga/Al ratio are disclosed herein.