Molecular layer epitaxy and the topmost surface structure in laser MBE of perovskite and other related oxides were investigated by in situ RHEED, in situ angle-resolved XPS (ARXPS) and ex situ co-axial ISS (CAICISS) analyses. Two-dimensional epitaxial growths of SrTiO3 (001) and BaCuO2(001) on SrTiO3(001) substrate were achieved by optimizing the growth conditions. Periodicities of RHEED oscillation corresponded well to the growth of a repeating unit cell (molecular layer). ARXPS and CAICISS spectra revealed that (Sr-0) atomic plane came at the top of SrTiO3(001) film growing on SrTiO3 (001) substrate with (Ti-O) atomic plane on the top. This indicates the structural conversion of the topmost atomic layer from TiO2 to SrO occurred during the SrTiO3 homoepitaxial growth.
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