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

Journal Article · · Physical Review. X

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-04ER46147; AC02-06CH11357
OSTI ID:
1812421
Alternate ID(s):
OSTI ID: 1814749
Journal Information:
Physical Review. X, Journal Name: Physical Review. X Vol. 11 Journal Issue: 3; ISSN 2160-3308
Publisher:
American Physical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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