The first four members of Bi-layered Srm−3Bi4TimO3m+3 homologous series with m=3, 4, 5, and 6, i.e., Bi4Ti3O12,SrBi4Ti4O15,Sr2Bi4Ti5O18, and Sr3Bi4Ti6O21, were grown on SrTiO3 (001) single-crystal substrates by pulsed-laser deposition. X-ray diffraction and high-resolution transmission electron microscopy (HRTEM) reveal that the films grew epitaxially with in-plane epitaxial alignment of [11̄0]Srm−3Bi4TimO3m+3‖[010]SrTiO3. HRTEM cross-sectional images show that the films with m=3, 4, and 5 are nearly free of intergrowth, whereas a number of growth defects were observed in the film with m=6. Using an evanescent microwave probe, the room-temperature dielectric constants of these epitaxial films are measured to be 221±13,205±15,261±29, and 249±17 for films with m=3, 4, 5, and 6, respectively.

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