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
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Publicado: American Physical Society 2021
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spelling oai:doaj.org-article:e576f4a1cf0a4697aca92bac2741c7692021-12-02T17:58:15ZStructural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains10.1103/PhysRevX.11.0310312160-3308https://doaj.org/article/e576f4a1cf0a4697aca92bac2741c7692021-08-01T00:00:00Zhttp://doi.org/10.1103/PhysRevX.11.031031http://doi.org/10.1103/PhysRevX.11.031031https://doaj.org/toc/2160-3308Weakly 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.Hyeon Jun LeeYoungjun AhnSamuel D. MarksEric C. LandahlShihao ZhuangM. Humed YusufMatthew DawberJun Young LeeTae Yeon KimSanjith UnithrattilSae Hwan ChunSunam KimIntae EomSang-Yeon ParkKyung Sook KimSooheyong LeeJi Young JoJiamian HuPaul G. EvansAmerican Physical SocietyarticlePhysicsQC1-999ENPhysical Review X, Vol 11, Iss 3, p 031031 (2021)
institution DOAJ
collection DOAJ
language EN
topic Physics
QC1-999
spellingShingle Physics
QC1-999
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
Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
description 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.
format article
author 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
author_facet 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
author_sort Hyeon Jun Lee
title Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
title_short Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
title_full Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
title_fullStr Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
title_full_unstemmed Structural Evidence for Ultrafast Polarization Rotation in Ferroelectric/Dielectric Superlattice Nanodomains
title_sort structural evidence for ultrafast polarization rotation in ferroelectric/dielectric superlattice nanodomains
publisher American Physical Society
publishDate 2021
url https://doaj.org/article/e576f4a1cf0a4697aca92bac2741c769
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