TY - JOUR
T1 - Strain-Driven Mixed-Phase Domain Architectures and Topological Transitions in Pb1−xSrxTiO3 Thin Films
AU - Kavle, Pravin
AU - Zorn, Jacob A.
AU - Dasgupta, Arvind
AU - Wang, Bo
AU - Ramesh, Maya
AU - Chen, Long Qing
AU - Martin, Lane W.
N1 - Funding Information:
P.K. and J.A.Z. contributed equally to this work. P.K. acknowledges support from the Army Research Office via Grant W911NF‐21‐1‐0118. J.A.Z. acknowledges the support of 3M Incorporated for their support via a fellowship. A.D. acknowledges support from the Army Research Office via Grant W911NF‐21‐1‐0126. J.A.Z., B.W., L.‐Q.C., and L.W.M. acknowledge support from the Army Research Office under the ETHOS MURI via cooperative agreement W911NF‐21‐2‐0162. M.R. acknowledges support from the Intel Corp. under the COFEEE program. Computations for this research were performed on the Pennsylvania State University's Institute for Cyber and Data Science Advanced CyberInfrastructure (ICDS‐ACI). This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI‐1548562. Specifically, it used the Bridges system, which is supported by NSF award number ACI‐1445606, at the Pittsburgh Supercomputing Center (PSC). The authors acknowledge the Texas Advanced Computing Center (TACC) at The University of Texas at Austin for providing HPC resources that have contributed to the research results reported within this paper.
Funding Information:
P.K. and J.A.Z. contributed equally to this work. P.K. acknowledges support from the Army Research Office via Grant W911NF-21-1-0118. J.A.Z. acknowledges the support of 3M Incorporated for their support via a fellowship. A.D. acknowledges support from the Army Research Office via Grant W911NF-21-1-0126. J.A.Z., B.W., L.-Q.C., and L.W.M. acknowledge support from the Army Research Office under the ETHOS MURI via cooperative agreement W911NF-21-2-0162. M.R. acknowledges support from the Intel Corp. under the COFEEE program. Computations for this research were performed on the Pennsylvania State University's Institute for Cyber and Data Science Advanced CyberInfrastructure (ICDS-ACI). This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1548562. Specifically, it used the Bridges system, which is supported by NSF award number ACI-1445606, at the Pittsburgh Supercomputing Center (PSC). The authors acknowledge the Texas Advanced Computing Center (TACC) at The University of Texas at Austin for providing HPC resources that have contributed to the research results reported within this paper.
Publisher Copyright:
© 2022 Wiley-VCH GmbH.
PY - 2022/9/15
Y1 - 2022/9/15
N2 - The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice-mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain-driven control of hierarchical domain structures in Pb1−xSrxTiO3 solid-solution thin films wherein two types, c/a and a1/a2, of nanodomains can coexist. Combining phase-field simulations, epitaxial thin-film growth, detailed structural, domain, and physical-property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet-like a1/a2 domains in a c/a domain matrix, to a connected-labyrinth geometry of c/a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet-like c/a domains in an a1/a2 domain matrix. A relationship between the different mixed-phase modulation patterns and its topological nature is established. Annealing the connected-labyrinth structure leads to domain coarsening forming distinctive regions of parallel c/a and a1/a2 domain stripes, offering additional design flexibility. Finally, it is found that the connected-labyrinth domain patterns exhibit the highest dielectric permittivity.
AB - The potential for creating hierarchical domain structures, or mixtures of energetically degenerate phases with distinct patterns that can be modified continually, in ferroelectric thin films offers a pathway to control their mesoscale structure beyond lattice-mismatch strain with a substrate. Here, it is demonstrated that varying the strontium content provides deterministic strain-driven control of hierarchical domain structures in Pb1−xSrxTiO3 solid-solution thin films wherein two types, c/a and a1/a2, of nanodomains can coexist. Combining phase-field simulations, epitaxial thin-film growth, detailed structural, domain, and physical-property characterization, it is observed that the system undergoes a gradual transformation (with increasing strontium content) from droplet-like a1/a2 domains in a c/a domain matrix, to a connected-labyrinth geometry of c/a domains, to a disconnected labyrinth structure of the same, and, finally, to droplet-like c/a domains in an a1/a2 domain matrix. A relationship between the different mixed-phase modulation patterns and its topological nature is established. Annealing the connected-labyrinth structure leads to domain coarsening forming distinctive regions of parallel c/a and a1/a2 domain stripes, offering additional design flexibility. Finally, it is found that the connected-labyrinth domain patterns exhibit the highest dielectric permittivity.
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U2 - 10.1002/adma.202203469
DO - 10.1002/adma.202203469
M3 - Article
C2 - 35917499
AN - SCOPUS:85135793668
SN - 0935-9648
VL - 34
JO - Advanced Materials
JF - Advanced Materials
IS - 37
M1 - 2203469
ER -