The first five members of the Srn+1TinO3n+1 Ruddlesden–Popper homologous series, i.e., Sr2TiO4,Sr3Ti2O7,Sr4Ti3O10,Sr5Ti4O13, and Sr6Ti5O16, have been grown by reactive molecular beam epitaxy. A combination of atomic absorption spectroscopy and reflection high-energy electron diffraction intensity oscillations were used for the strict composition control necessary for the synthesis of these phases. X-ray diffraction and high-resolution transmission electron microscope images confirm that these films are epitaxially oriented and nearly free of intergrowths. Dielectric measurements indicate that the dielectric constant tensor coefficient ε33 increases from a minimum of 44±4 in the n=1(Sr2TiO4) film to a maximum of 263±2 in the n=∞(SrTiO3) film.

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