“…Complex transition-metal oxides have attracted considerable attention of research due to their electrical, magnetic, and optical properties, which can be used for the development of various new concept devices, such as energy harvest, electrical, and chemical sensors, etc. − Perovskite cobaltates exhibit remarkable mixed conductivity and catalytic properties at high temperature as well as interesting magnetic and electrical transport properties at low temperature. − Among them, the oxygen-deficient double perovskite cobaltates LnBaCo 2 O 5.5+δ (Ln = Lanthanide) show particularly interesting phenomena of the order–disorder at the A-cation sites in the cobaltate system. − Especially, the very small difference in the A-site cations’ radii between La 3+ and Ba 2+ in the LaBaCo 2 O 5.5+δ (LBCO) can form complex A-site order, nanoarea order, and disorder layered perovskite structures and induce various exciting physical phenomena, such as various oxidation states (Co 2+ /Co 3+ /Co 4+ ) of cobalt, different spin state configurations, giant MR effect, metal insulator transition, etc. − In order to fully understand the magnetic and transport properties of such complex cobalt oxides, the single crystalline samples are critically desired. In our previous work, we have fabricated highly epitaxial single crystalline LBCO thin films on (001) LaAlO 3 , , (001) SrTiO 3 , , and (001) MgO and found that these films possess an extraordinary sensitivity to reducing/oxidizing environments and an exceedingly fast redox reaction at high temperature.…”