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Processes and preparation conditions for growing epitaxial thin films of Cu-based, layered oxychalcogenides LnCuOCh (Ln = La, Ce, Pr or Nd; Ch = S1-xSex or Se1-yTey) are reported. Epitaxial thin films on MgO (001) substrates were prepared by a reactive solid-phase epitaxy method. Four-axes high-resolution x-ray diffraction measurements revealed that the crystallographic orientation is (001) LnCuOCh || (001) MgO and the internal stress of the crystalline lattices in the films are relaxed during thermal-annealing process of the reactive solid-phase epitaxy. Furthermore, except for CeCuOS, systematic variations in the lattice constant by chalcogen or lanthanide ion substitutions were observed. These results demonstrated that the reactive solid-phase epitaxy is an efficient technique for fabricating LnCuOCh epitaxial films.
Several Cu(I)-containing layered oxysulfides were selected as candidates for wide-gap p-type semiconductors by extending a concept of a materials design for transparent p-type conducting oxides. The electrical and optical properties of the selected oxysulfides were investigated, and their electronic structures were analyzed by energy band calculations. LaCuOS, Sr2Cu2ZnO2S2 and Sr2CuGaO3S were found to be wide-gap p-type semiconductors, and LaCuOS showed the largest energy gap (Eg=3.1eV) among these layered oxysulfides. It was also found that LaCuOS shows band edge emission under uv excitation at room temperature, which is consistent with the results of the energy band calculations that LaCuOS has a direct-allowed-type energy gap at Γ point. In further materials research, analogous layered oxychalcogenides such as LaCuOSe and LnCuOS (Ln=Pr, Nd) were found to show similar optical and electrical properties to those of LaCuOS. Therefore, it is considered that the layered crystal structure and the electronic structure are responsible for the wide-gap p-type conductive properties in these materials.
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