Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Kim, Jieun; Takenaka, Hiroyuki; Qi, Yubo; Damodaran, Anoop R.; Fernandez, Abel; Gao, Ran; McCarter, Margaret R.; Saremi, Sahar; Chung, Linh; Rappe, Andrew M.; Martin, Lane W.

doi:10.1002/adma.201901060

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Journal Article · Wed Apr 10 00:00:00 EDT 2019 · Advanced Materials

DOI:https://doi.org/10.1002/adma.201901060· OSTI ID:1633233

^[1]; Takenaka, Hiroyuki ^[2]; Qi, Yubo ^[3]; Damodaran, Anoop R. ^[1]; Fernandez, Abel ^[1]; Gao, Ran ^[1]; McCarter, Margaret R. ^[1]; Saremi, Sahar ^[1]; Chung, Linh ^[1]; Rappe, Andrew M. ^[3]; Martin, Lane W. ^[4]

Univ. of California, Berkeley, CA (United States)
Univ. of Nebraska, Lincoln, NE (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Understanding and ultimately controlling the large electromechanical effects in relaxor ferroelectrics requires intimate knowledge of how the local-polar order evolves under applied stimuli. Here, the biaxial-strain-induced evolution of and correlations between polar structures and properties in epitaxial films of the prototypical relaxor ferroelectric 0.68PbMg_1/3Nb_2/3O₃–0.32PbTiO₃ are investigated. X-ray diffuse-scattering studies reveal an evolution from a butterfly- to disc-shaped pattern and an increase in the correlation-length from ≈8 to ≈25 nm with increasing compressive strain. Molecular-dynamics simulations reveal the origin of the changes in the diffuse-scattering patterns and that strain induces polarization rotation and the merging of the polar order. As the magnitude of the strain is increased, relaxor behavior is gradually suppressed but is not fully quenched. Analysis of the dynamic evolution of dipole alignment in the simulations reveals that, while, for most unit-cell chemistries and configurations, strain drives a tendency toward more ferroelectric-like order, there are certain unit cells that become more disordered under strain, resulting in stronger competition between ordered and disordered regions and enhanced overall susceptibilities. Ultimately, this implies that deterministic creation of specific local chemical configurations could be an effective way to enhance relaxor performance.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Gordon and Betty Moore Foundation (GBMF); National Science Foundation (NSF); US Army Research Office (ARO); US Department of the Navy, Office of Naval Research (ONR); USDOD; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; FG02-07ER46431; SC0012375

OSTI ID:: 1633233

Alternate ID(s):: OSTI ID: 1506136
OSTI ID: 1523531

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 21 Vol. 31; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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