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The low-temperature optical properties of a SrTiO3 crystal doped with 0.7% wt. Nb and a pure SrTiO3 reference crystal were studied using spectroscopic ellipsometry. The optical constants and dielectric functions were obtained in the spectral range of 0.8–8.8 eV at temperatures from 10 to 300 K, and the optical conductivity was obtained in the spectral range of 0.03–1 eV at 300 K. Analysis of the optical conductivity spectra in the infrared spectral range confirmed the presence of free electrons and additional absorption hump between 0.1 and 0.4 eV (806 and 3226 cm−1) in doped SrTiO3 and optical phonons in both doped and undoped SrTiO3. The performed analysis of optical absorption spectra in the range 0.8–8.8 eV revealed frustration of the indirect bandgap and an increase in the direct bandgap energy by ∼0.03 eV in Nb-doped SrTiO3, compared to undoped SrTiO3 over the whole temperature range. The energies of the peaks' maxima of the dielectric function spectra did not significantly differ for doped and pure SrTiO3. For both Nb-doped and pure SrTiO3, temperature dependence of the direct bandgap energy and that of the index of refraction showed inflection between 100 and 150 K, which may be considered evidence of an antiferrodistortive phase transition from a cubic to a tetragonal structure. [ABSTRACT FROM AUTHOR]

Technologically important high-permittivity dielectrics are often achieved using cationic engineering of ABO3-type perovskite para(ferro)electrics. Here, we experimentally and theoretically explore the potential of less conventional anionic engineering in ABO3 dielectrics. We demonstrate that in an archetypal representative SrTiO3, nitrogen substitution can occur on two distinct oxygen atomic sites, reduce crystal symmetry, and lead to significant changes in the patterns and frequencies of lattice vibrations. These phonon transformations diminish permittivity, whereas contribution from nitrogen-induced nanoregions can raise it. The effects of nitrogen are found to be especially strong in epitaxial films. We anticipate that the revealed phenomena may be relevant for a broad class of high-permittivity perovskite oxides. [ABSTRACT FROM AUTHOR]

In ABO3 perovskite oxide ferroelectrics, electrical conductivity ranges from insulator- to superconductor-type and is virtually critical for all applications of these materials. Compared to bulk ceramics and crystals, ferroelectric thin films can enable advanced control of the conductivity. Here, small-polaron hopping conductivity was evidenced and examined in various pulsed-laser-deposited films of ferroelectric BaTiO3 and reference films of SrTiO3. For this, AC conductivity was studied in a broad range of temperatures and frequencies for films sandwiched between the bottom and top electrodes. In the BaTiO3 films, with increasing temperature, a significant increase in activation energy for small-polaron hopping was found and ascribed to strong electron–phonon coupling and complex lattice oscillations therein. Plain relations of the activation energy to microstructure, composition, or phase transitions were lacking, which corroborated the critical role of phonons. Additionally, a phonon-less transport was detected. It was anticipated that owing to strong electron–phonon coupling, rich phonon ensembles, and coexistence of phonon-stimulated and phonon-less processes, the small-polaron conductivity can heavily vary in ferroelectric films that necessitates further studies. [ABSTRACT FROM AUTHOR]

The electronic properties, including bandgap and conductivity, are critical for nearly all applications of multifunctional perovskite oxide ferroelectrics. Here we analysed possibility to induce semiconductor behaviour in these materials, which are basically insulators, by replacement of several percent of oxygen atoms with nitrogen, hydrogen, or vacancies. We explored this approach for one of the best studied members of the large family of ABO3 perovskite ferroelectrics — strontium titanate (SrTiO3). The atomic and electronic structure of defects were theoretically investigated using the large-scale first-principles calculations for both bulk crystal and thin films. The results of calculations were experimentally verified by studies of the optical properties at photon energies from 25 meV to 8.8 eV for in-situ prepared thin films. It was demonstrated that substitutions and vacancies prefer locations at surfaces or phase boundaries over those inside crystallites. At the same time, local states in the bandgap can be produced by vacancies located both inside the crystals and at the surface, but by nitrogen substitution only inside crystals. Wide-bandgap insulator phases were evidenced for all defects. Compared to pure SrTiO3 films, bandgap widening due to defects was theoretically predicted and experimentally detected. [ABSTRACT FROM AUTHOR]

Cutting-edge acousto-optic devices require optically transparent thin films, which possess a high index of refraction and large elasto-optic coefficients. For the wide near-infrared to ultraviolet spectral region, the mainstream technology employs lithium niobate crystals, which interferes with the vital demands of global sustainability. Here, we demonstrate unprecedented elasto-optic properties in thin films of sustainable and environmentally friendly strontium titanate [SrTiO3 (STO)]. Compared to cubic STO, a nearly twofold increase in elasto-optic coefficients is achieved in epitaxial tetragonal STO films, which concurrently exhibit excellent transparency and a high index of refraction at wavelengths from 400 to 1700 nm. The room-temperature non-polar state is evidenced by the thermo-optical behavior of the films. The obtained enhancement is related to the tetragonal antiferrodistortive phase of STO. It is suggested that such films can form a platform for future sustainable acousto-optic materials. [ABSTRACT FROM AUTHOR]