Te ions existed as Te 6+ in the Bi 6 Ti 5 TeO 22 ͑BTT͒ film grown at 300°C under a high oxygen pressure ͑OP͒ of 80.0 Pa and contributed to the formation of the crystalline BTT phase after subsequent annealing at 600°C. However, for the BTT film grown under a low OP of 53.3 Pa ͑or 9.33 Pa͒, Te 6+ ions, were converted to Te 4+ ions, which induced the phase transition of the BTT phase to the pseudo-Bi 4 Ti 3 O 12 and pseudo-Bi 2 Ti 2 O 7 phases after annealing at 600°C. The leakage current density decreased with increasing OP during the growth due to the decreased number of oxygen vacancies. The breakdown voltage also improved with increasing OP during the deposition. The Mn ions introduced in the BTT films by Mn doping existed as Mn 2+ or Mn 4+ and acted as the acceptors. This Mn doping to 10 mol % also reduced the leakage current density and increased the breakdown voltage by decreasing the number of intrinsic oxygen vacancies.Investigations on dielectric thin films with a high dielectric constant ͑k͒ which can be deposited at low temperatures ͑ഛ300°C͒ have multiplied for applications to the embedded decoupling capacitors for printed circuit board ͑PCB͒ and the gate insulators of ZnObased, thin-film transistors for organic light-emitting diodes ͑OLEDs͒ on plastic substrate. 1-3 The radio-frequency ͑rf͒ or analog/ mixed metal-insulator-metal ͑MIM͒ capacitors in semiconductor devices also require a dielectric thin film with low processing temperatures due to the limitation of the very large-scale integration back-end line integration temperature ͑Ͻ400°C͒. Previously, ͑Ba,Sr͒TiO 3 , Ta 2 O 5 , TaTiO, and BaSm 2 Ti 4 O 12 films grown at low temperatures were used as the gate insulators for OLEDs and rf MIM capacitors but suffered from a low-k value. 4-8 Ca-doped Pb͑Zr,Ti͒O 3 films were grown for use as the embedded capacitors for PCBs, but their growth temperature was too high for such application. 9 Recently, Bi-based, dielectric thin films such as Bi 6 Ti 5 TeO 22 ͑BTT͒, 10 Bi 5 Nb 3 O 15 , 11 and Bi 1.5 Zn 1.0 Nb 1.5 O 7 1,3,12 have been extensively studied because of their achievement of high-k value with low deposition temperatures. In particular, the high-k value of 69 with a low dissipation factor ͑Ͻ1.3%͒ 10 obtained by BTT films grown at 300°C using sputtering demonstrated their promise as a good candidate material for high-k dielectric films with low processing temperatures. However, their leakage current density was relatively high with a low breakdown voltage, 10 thereby necessitating the improvement of their electrical properties before the application of such BTT films. Furthermore, the structure of the BTT films was considerably influenced by the valence of the Te ions, which was determined by the oxygen pressure ͑OP͒ during the fabrication processes. 10 However, no detailed investigation on the variation of the crystal structure of the BTT film with OP has yet been conducted.In this work, BTT films were grown using pulsed laser deposition ͑PLD͒ and annealed under various OPs. The PLD method was selected...