1. Structural evidence for ultrafast polarization rotation in ferroelectric/dielectric superlattice nanodomains
- Author
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Lee, Hyeon Jun, Ahn, Youngjun, Marks, Samuel D., Landahl, Eric C., Zhuang, Shihao, Yusuf, M. Humed, Dawber, Matthew, Lee, Jun Young, Kim, Tae Yeon, Unithrattil, Sanjith, Chun, Sae Hwan, Kim, Sunam, Eom, Intae, Park, Sang-Yeon, Kim, Kyung Sook, Lee, Sooheyong, Jo, Ji Young, Hu, Jiamian, and Evans, Paul G.
- Subjects
Condensed Matter - Materials Science - Abstract
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 not along the thin-film surface normal direction, while maintaining zero net in-plane polarization. PbTiO3/SrTiO3 thin-film superlattice heterostructures on a conducting SrRuO3 bottom electrode on SrTiO3 have a room-temperature stripe nanodomain pattern with nanometer-scale lateral period. Ultrafast time-resolved x-ray free electron laser diffraction and scattering experiments reveal that above-bandgap optical pulses induce rapidly 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 polarization rotation phenomena that have been previously available only through the selection of bulk crystal composition.
- Published
- 2021