  In many transition metal oxides (TMOs), oxygen stoichiometry is one of the
most 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 the
right oxygen stoichiometry, especially in a high vacuum environment, has been
viewed as a challenge. In this work, we show that through proper control of the
plume kinetic energy, stoichiometric crystalline films can be synthesized
without generating oxygen defects, even in high vacuum. We use a model
homoepitaxial system of SrTiO3 (STO) thin films on single crystal STO
substrates. Physical property measurements indicate that oxygen vacancy
generation in high vacuum is strongly influenced by the energetics of the laser
plume, and it can be controlled by proper laser beam delivery. Therefore, our
finding not only provides essential insight into oxygen stoichiometry control
in high vacuum for understanding the fundamental properties of STO-based thin
films and heterostructures, but expands the utility of pulsed laser epitaxy of
other materials as well.
