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We have investigated the growth of BaTiO3 thin films deposited on pure and 1%Nb-doped SrTiO3(001) single crystals using atomic oxygen assisted molecularbeam epitaxy (AO-MBE) and dedicated Ba and Ti Knudsen cells. Thicknesses up to30 nm were investigated for various layer compositions. We demonstrate 2Dgrowth and epitaxial single crystalline BaTiO3 layers up to 10 nm beforeadditional 3D features appear; lattice parameter relaxation occurs during thefirst few nanometers and is completed at {\guillemotright}10 nm. The presenceof a Ba oxide rich top layer that probably favors 2D growth is evidenced forwell crystallized layers. We show that the Ba oxide rich top layer can beremoved by chemical etching. The present work stresses the importance ofstoichiometry and surface composition of BaTiO3 layers, especially in view oftheir integration in devices.

Surface composition of BaTiO3/SrTiO3(001) films grown by atomic oxygen plasma assisted molecular beam epitaxy