Optically Induced Picosecond Lattice Compression in the Dielectric Component of a Strongly Coupled Ferroelectric/Dielectric Superlattice

Deepankar Sri Gyan, Hyeon Jun Lee, Youngjun Ahn, River B. Carson, Jerome Carnis, Tae Yeon Kim, Sanjith Unithrattil, Jun Young Lee, Sae Hwan Chun, Sunam Kim, Intae Eom, Minseok Kim, Sang Youn Park, Kyung Sook Kim, Ho Nyung Lee, Ji Young Jo, Paul G. Evans

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Abstract

Above-bandgap femtosecond optical excitation of a ferroelectric/dielectric BaTiO3/CaTiO3 superlattice leads to structural responses that are a consequence of the screening of the strong electrostatic coupling between the component layers. Time-resolved X-ray free-electron laser diffraction shows that the structural response to optical excitation includes a net lattice expansion of the superlattice consistent with depolarization-field screening driven by the photoexcited charge carriers. The depolarization-field-screening-driven expansion is separate from a photoacoustic pulse launched from the bottom electrode on which the superlattice is epitaxially grown. The distribution of diffracted intensity of superlattice X-ray reflections indicates that the depolarization-field-screening-induced strain includes a photoinduced expansion in the ferroelectric BaTiO3 and a contraction in CaTiO3. The magnitude of expansion in BaTiO3 layers is larger than the contraction in CaTiO3. The difference in the magnitude of depolarization-field-screening-driven strain in the BaTiO3 and CaTiO3 components can arise from the contribution of the oxygen octahedral rotation patterns at the BaTiO3/CaTiO3 interfaces to the polarization of CaTiO3. The depolarization-field-screening-driven polarization reduction in the CaTiO3 layers points to a new direction for the manipulation of polarization in the component layers of a strongly coupled ferroelectric/dielectric superlattice.

Original languageEnglish
Article number2101051
JournalAdvanced Electronic Materials
Volume8
Issue number6
DOIs
StatePublished - Jun 2022

Funding

The authors acknowledge support from the U.S. DOE, Basic Energy Sciences, Materials Sciences and Engineering Division, under contract no. DE-FG02-04ER46147. H.J.L. acknowledges support by the National Research Foundation of Korea under grant 2017R1A6A3A11030959. Y.J.A. acknowledges support from the National Science Foundation through grant number DMR-1609545. J.C. acknowledges support from the CNRS project GOtoXFEL. The authors acknowledge the use of characterization facilities supported by the National Science Foundation through the University of Wisconsin Materials Research Science and Engineering Center (DMR-1720415). The experiment was performed at the XSS beamline of PAL-XFEL (proposal no. 2018-2nd-XSS-016) funded by the Ministry of Science and ICT of Korea. The synthesis work at ORNL was supported by U.S. DOE, Basic Energy Sciences, Materials Sciences and Engineering Division. The authors acknowledge support from the U.S. DOE, Basic Energy Sciences, Materials Sciences and Engineering Division, under contract no. DE‐FG02‐04ER46147. H.J.L. acknowledges support by the National Research Foundation of Korea under grant 2017R1A6A3A11030959. Y.J.A. acknowledges support from the National Science Foundation through grant number DMR‐1609545. J.C. acknowledges support from the CNRS project GOtoXFEL. The authors acknowledge the use of characterization facilities supported by the National Science Foundation through the University of Wisconsin Materials Research Science and Engineering Center (DMR‐1720415). The experiment was performed at the XSS beamline of PAL‐XFEL (proposal no. 2018‐2nd‐XSS‐016) funded by the Ministry of Science and ICT of Korea. The synthesis work at ORNL was supported by U.S. DOE, Basic Energy Sciences, Materials Sciences and Engineering Division.

FundersFunder number
University of Wisconsin Materials Research Science and Engineering Center2018‐2nd‐XSS‐016, DMR‐1720415
National Science FoundationDMR‐1609545
U.S. Department of Energy
Basic Energy Sciences
College of Natural Resources and Sciences, Humboldt State University
Division of Materials Sciences and EngineeringDE‐FG02‐04ER46147
Ministry of Science, ICT and Future Planning
National Research Foundation of Korea2017R1A6A3A11030959
Centre National de la Recherche Scientifique

    Keywords

    • X-ray free-electron laser diffraction
    • depolarization-field screening
    • ferroelectric/dielectric superlattice
    • ultrafast structural phenomena

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