Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains

Weakly coupled ferroelectric/dielectric superlattice thin-film heterostructures exhibit complex nanoscale polarization configurations that arise from a balance of competing electrostatic, elastic, and domain-wall contributions to the free energy. A key feature of these configurations is that the pol...

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Autores principales: Hyeon Jun Lee, Youngjun Ahn, Samuel D. Marks, Eric C. Landahl, Shihao Zhuang, M. Humed Yusuf, Matthew Dawber, Jun Young Lee, Tae Yeon Kim, Sanjith Unithrattil, Sae Hwan Chun, Sunam Kim, Intae Eom, Sang-Yeon Park, Kyung Sook Kim, Sooheyong Lee, Ji Young Jo, Jiamian Hu, Paul G. Evans
Formato: article
Lenguaje:EN
Publicado: American Physical Society 2021
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Acceso en línea:https://doaj.org/article/e576f4a1cf0a4697aca92bac2741c769
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Sumario:Weakly coupled ferroelectric/dielectric superlattice thin-film heterostructures exhibit complex nanoscale polarization configurations that arise from a balance of competing electrostatic, elastic, and domain-wall contributions to the free energy. A key feature of these configurations is that the polarization can locally have a significant component that is along the thin-film surface normal direction with an overall configuration maintaining zero net in-plane polarization. PbTiO_{3}/SrTiO_{3} thin-film superlattice heterostructures on a conducting SrRuO_{3} bottom electrode on SrTiO_{3} have a room-temperature stripe nanodomain pattern with a nanometer-scale lateral period. Ultrafast time-resolved x-ray free electron laser diffraction and scattering experiments reveal that above-bandgap optical pulses induce propagating acoustic pulses and a perturbation of the domain diffuse scattering intensity arising from the nanoscale stripe domain configuration. With 400-nm optical excitation, two separate acoustic pulses are observed: a high-amplitude pulse resulting from strong optical absorption in the bottom electrode and a weaker pulse arising from the depolarization-field-screening effect due to absorption directly within the superlattice. The picosecond scale variation of the nanodomain diffuse scattering intensity is consistent with a larger polarization change than would be expected due to the polarization-tetragonality coupling of uniformly polarized ferroelectrics. The polarization change is consistent, instead, with polarization rotation facilitated by the reorientation of the in-plane component of the polarization at the domain boundaries of the striped polarization structure. The complex steady-state configuration within these ferroelectric heterostructures leads to ultrafast polarization rotation phenomena that have previously been available only through the selection of bulk crystal composition.