Bridging experiment and theory of relaxor ferroelectrics at the atomic scale with multislice electron ptychography. Zhu, M., Xu, M., Qi, Y., Gilgenbach, C., Kim, J., Zhang, J., Denzer, B. R, Martin, L. W, Rappe, A. M, & LeBeau, J. M arXiv [cond-mat.mtrl-sci], 21 August, 2024. doi abstract bibtex Introducing structural and/or chemical heterogeneity into otherwise ordered crystals can dramatically alter material properties. Lead-based relaxor ferroelectrics are a prototypical example, with decades of investigation having connected chemical and structural heterogeneity to their unique properties. While theory has pointed to the formation of an ensemble of ``slush''-like polar domains, the lack of direct, spatially resolved volumetric data comparable to simulations presents a significant challenge in measuring the spatial distribution and correlation of local chemistry and structure with the physics underlying relaxor behavior. Here, we address this challenge through three-dimensional volumetric characterization of the prototypical relaxor ferroelectric ȩ0.68Pb(Mg$_{1/3}$Nb$_{2/3}$)O3-0.32PbTiO$_3$ using multislice electron ptychography. Direct comparison with molecular dynamics simulations reveals the intimate relationship between the polar structure and unit-cell level charge imbalance induced by chemical disorder. Further, polar nanodomains are maintained through local correlations arising from residual short-range chemical order. Acting in concert with the chemical heterogeneities, it is also shown that compressive strain enhances out-of-plane correlations and ferroelectric-like order without affecting the in-plane relaxor-like structure. Broadly, these findings provide a pathway to enable detailed atomic scale understanding for hierarchical control of polar domains in relaxor ferroelectric materials and devices, and also present significant opportunities to tackle other heterogeneous systems using complementary theoretical and experimental studies.
@ARTICLE{Zhu2024-vw,
title = "Bridging experiment and theory of relaxor ferroelectrics at
the atomic scale with multislice electron ptychography",
author = "Zhu, Menglin and Xu, Michael and Qi, Yubo and Gilgenbach,
Colin and Kim, Jieun and Zhang, Jiahao and Denzer, Bridget R
and Martin, Lane W and Rappe, Andrew M and LeBeau, James M",
journal = "arXiv [cond-mat.mtrl-sci]",
abstract = "Introducing structural and/or chemical heterogeneity into
otherwise ordered crystals can dramatically alter material
properties. Lead-based relaxor ferroelectrics are a
prototypical example, with decades of investigation having
connected chemical and structural heterogeneity to their
unique properties. While theory has pointed to the formation
of an ensemble of ``slush''-like polar domains, the lack of
direct, spatially resolved volumetric data comparable to
simulations presents a significant challenge in measuring the
spatial distribution and correlation of local chemistry and
structure with the physics underlying relaxor behavior. Here,
we address this challenge through three-dimensional
volumetric characterization of the prototypical relaxor
ferroelectric
\ce{0.68Pb(Mg$_{1/3}$Nb$_{2/3}$)O3-0.32PbTiO$_3$} using
multislice electron ptychography. Direct comparison with
molecular dynamics simulations reveals the intimate
relationship between the polar structure and unit-cell level
charge imbalance induced by chemical disorder. Further, polar
nanodomains are maintained through local correlations arising
from residual short-range chemical order. Acting in concert
with the chemical heterogeneities, it is also shown that
compressive strain enhances out-of-plane correlations and
ferroelectric-like order without affecting the in-plane
relaxor-like structure. Broadly, these findings provide a
pathway to enable detailed atomic scale understanding for
hierarchical control of polar domains in relaxor
ferroelectric materials and devices, and also present
significant opportunities to tackle other heterogeneous
systems using complementary theoretical and experimental
studies.",
month = "21~" # aug,
year = 2024,
archivePrefix = "arXiv",
primaryClass = "cond-mat.mtrl-sci",
eprint = "2408.11685",
keywords = "LeBeau Group",
doi = "10.48550/arXiv.2408.11685"
}
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M"],"bibdata":{"bibtype":"article","type":"article","title":"Bridging experiment and theory of relaxor ferroelectrics at the atomic scale with multislice electron ptychography","author":[{"propositions":[],"lastnames":["Zhu"],"firstnames":["Menglin"],"suffixes":[]},{"propositions":[],"lastnames":["Xu"],"firstnames":["Michael"],"suffixes":[]},{"propositions":[],"lastnames":["Qi"],"firstnames":["Yubo"],"suffixes":[]},{"propositions":[],"lastnames":["Gilgenbach"],"firstnames":["Colin"],"suffixes":[]},{"propositions":[],"lastnames":["Kim"],"firstnames":["Jieun"],"suffixes":[]},{"propositions":[],"lastnames":["Zhang"],"firstnames":["Jiahao"],"suffixes":[]},{"propositions":[],"lastnames":["Denzer"],"firstnames":["Bridget","R"],"suffixes":[]},{"propositions":[],"lastnames":["Martin"],"firstnames":["Lane","W"],"suffixes":[]},{"propositions":[],"lastnames":["Rappe"],"firstnames":["Andrew","M"],"suffixes":[]},{"propositions":[],"lastnames":["LeBeau"],"firstnames":["James","M"],"suffixes":[]}],"journal":"arXiv [cond-mat.mtrl-sci]","abstract":"Introducing structural and/or chemical heterogeneity into otherwise ordered crystals can dramatically alter material properties. Lead-based relaxor ferroelectrics are a prototypical example, with decades of investigation having connected chemical and structural heterogeneity to their unique properties. While theory has pointed to the formation of an ensemble of ``slush''-like polar domains, the lack of direct, spatially resolved volumetric data comparable to simulations presents a significant challenge in measuring the spatial distribution and correlation of local chemistry and structure with the physics underlying relaxor behavior. Here, we address this challenge through three-dimensional volumetric characterization of the prototypical relaxor ferroelectric ȩ0.68Pb(Mg$_{1/3}$Nb$_{2/3}$)O3-0.32PbTiO$_3$ using multislice electron ptychography. Direct comparison with molecular dynamics simulations reveals the intimate relationship between the polar structure and unit-cell level charge imbalance induced by chemical disorder. Further, polar nanodomains are maintained through local correlations arising from residual short-range chemical order. Acting in concert with the chemical heterogeneities, it is also shown that compressive strain enhances out-of-plane correlations and ferroelectric-like order without affecting the in-plane relaxor-like structure. Broadly, these findings provide a pathway to enable detailed atomic scale understanding for hierarchical control of polar domains in relaxor ferroelectric materials and devices, and also present significant opportunities to tackle other heterogeneous systems using complementary theoretical and experimental studies.","month":"21 August","year":"2024","archiveprefix":"arXiv","primaryclass":"cond-mat.mtrl-sci","eprint":"2408.11685","keywords":"LeBeau Group","doi":"10.48550/arXiv.2408.11685","bibtex":"@ARTICLE{Zhu2024-vw,\n title = \"Bridging experiment and theory of relaxor ferroelectrics at\n the atomic scale with multislice electron ptychography\",\n author = \"Zhu, Menglin and Xu, Michael and Qi, Yubo and Gilgenbach,\n Colin and Kim, Jieun and Zhang, Jiahao and Denzer, Bridget R\n and Martin, Lane W and Rappe, Andrew M and LeBeau, James M\",\n journal = \"arXiv [cond-mat.mtrl-sci]\",\n abstract = \"Introducing structural and/or chemical heterogeneity into\n otherwise ordered crystals can dramatically alter material\n properties. Lead-based relaxor ferroelectrics are a\n prototypical example, with decades of investigation having\n connected chemical and structural heterogeneity to their\n unique properties. While theory has pointed to the formation\n of an ensemble of ``slush''-like polar domains, the lack of\n direct, spatially resolved volumetric data comparable to\n simulations presents a significant challenge in measuring the\n spatial distribution and correlation of local chemistry and\n structure with the physics underlying relaxor behavior. Here,\n we address this challenge through three-dimensional\n volumetric characterization of the prototypical relaxor\n ferroelectric\n \\ce{0.68Pb(Mg$_{1/3}$Nb$_{2/3}$)O3-0.32PbTiO$_3$} using\n multislice electron ptychography. Direct comparison with\n molecular dynamics simulations reveals the intimate\n relationship between the polar structure and unit-cell level\n charge imbalance induced by chemical disorder. Further, polar\n nanodomains are maintained through local correlations arising\n from residual short-range chemical order. Acting in concert\n with the chemical heterogeneities, it is also shown that\n compressive strain enhances out-of-plane correlations and\n ferroelectric-like order without affecting the in-plane\n relaxor-like structure. Broadly, these findings provide a\n pathway to enable detailed atomic scale understanding for\n hierarchical control of polar domains in relaxor\n ferroelectric materials and devices, and also present\n significant opportunities to tackle other heterogeneous\n systems using complementary theoretical and experimental\n studies.\",\n month = \"21~\" # aug,\n year = 2024,\n archivePrefix = \"arXiv\",\n primaryClass = \"cond-mat.mtrl-sci\",\n eprint = \"2408.11685\",\n keywords = \"LeBeau Group\",\n doi = \"10.48550/arXiv.2408.11685\"\n}\n\n","author_short":["Zhu, M.","Xu, M.","Qi, Y.","Gilgenbach, C.","Kim, J.","Zhang, J.","Denzer, B. R","Martin, L. 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