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Thin films of orthorhombic La0.9Sr0.1MnO3, have been grown by computer-controlled laser molecular-beam epitaxy on SrTiO3(001) substrate and vicinal SrTiO3(001) substrates. Electron diffractions and high-resolution imaging reveal that the as-received thin films with thickness of 300 nm are epitaxially grown on the substrates. The microstructures in the film grown on SrTiO3(001) substrate are clarified in terms of the oriented microdomains, while the films on vicinal SrTiO3(001) substrates are predominated by a single [101]-oriented growth, which provides a useful routine for a design of preferred physical properties. Based on the minimization of surface energy, the mechanism of such a single domain formation is proposed. [ABSTRACT FROM AUTHOR]