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DOE OSTI · 3377985

Scan‐Path‐ and Initial‐State‐Dependent Superdomain Switching in (111)‐Oriented PZT

Vasudevan, Rama K. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000346928579)·Ahmad, Laveeza [Univ. of Texas, Arlington, TX (United States)]·Pant, Bharat [Univ. of Texas, Arlington, TX (United States)]·Bulanadi, Ralph [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000267794031)·Haque, Asraful [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)]·Kaur, Puneet [National Cheng Kung Univ., Tainan City (Taiwan)]·Neumayer, Sabine [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000281671230)·Yang, Jan‐Chi [National Cheng Kung Univ., Tainan City (Taiwan)]·Liu, Yongtao [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000301521783)·Cao, Ye [Univ. of Texas, Arlington, TX (United States)] (ORCID:0000000273657447)·Jesse, Stephen [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000211688483)·Checa, Marti [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000326076866)
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Abstract

Polarization switching in ferroelectric materials arises from the collective evolution of complex domain hierarchies, yet deterministic control over these processes remains challenging. Here, we investigate scan-path- and initial-state-dependent switching in epitaxial (111)-oriented PbZr 0.2 Ti 0.8 O 3 thin films using automated AFM-based writing combined with quantitative 3D piezoresponse force microscopy. We show that the scan trajectory acts as an experimentally accessible control parameter for superdomain formation. Box-in-box raster scans reproducibly stabilize ordered stripe superdomains with a reduced subset of symmetry-allowed variants, whereas spiral trajectories generate frustrated mixed-variant states with a broader distribution of final microstructures. Automated pulsing experiments further show that the local superdomain configuration at the nucleation site strongly influences the final written morphology. Phase-field modeling qualitatively reproduces the contrast between representative initial-state geometries and supports the role of compatibility constraints among competing ferroelastic pathways. These findings establish scan-path and initial-state engineering as practical handles to program ferroic order in hierarchical ferroelectric domain structures.

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Vasudevan, Rama K. [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000346928579), Ahmad, Laveeza [Univ. of Texas, Arlington, TX (United States)], Pant, Bharat [Univ. of Texas, Arlington, TX (United States)], Bulanadi, Ralph [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000267794031), Haque, Asraful [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)], Kaur, Puneet [National Cheng Kung Univ., Tainan City (Taiwan)], Neumayer, Sabine [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000281671230), Yang, Jan‐Chi [National Cheng Kung Univ., Tainan City (Taiwan)], Liu, Yongtao [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000301521783), Cao, Ye [Univ. of Texas, Arlington, TX (United States)] (ORCID:0000000273657447), Jesse, Stephen [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000211688483), Checa, Marti [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:0000000326076866). 2026-07-06. Scan‐Path‐ and Initial‐State‐Dependent Superdomain Switching in (111)‐Oriented PZT. https://doi.org/10.1002/aelm.70472

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