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In many transition metal oxides (TMOs), oxygen stoichiometry is one of themost critical parameters that plays a key role in determining the structural,physical, optical, and electrochemical properties of the material. However,controlling the growth to obtain high quality single crystal films having theright oxygen stoichiometry, especially in a high vacuum environment, has beenviewed as a challenge. In this work, we show that through proper control of theplume kinetic energy, stoichiometric crystalline films can be synthesizedwithout generating oxygen defects, even in high vacuum. We use a modelhomoepitaxial system of SrTiO3 (STO) thin films on single crystal STOsubstrates. Physical property measurements indicate that oxygen vacancygeneration in high vacuum is strongly influenced by the energetics of the laserplume, and it can be controlled by proper laser beam delivery. Therefore, ourfinding not only provides essential insight into oxygen stoichiometry controlin high vacuum for understanding the fundamental properties of STO-based thinfilms and heterostructures, but expands the utility of pulsed laser epitaxy ofother materials as well.

Growth control of oxygen stoichiometry in homoepitaxial SrTiO3 films by pulsed laser epitaxy in high vacuum