Resolving the dynamic correlated disorder in KTa1−xNbxO3

Xing He; Mayanak K. Gupta; Douglas L. Abernathy; Garrett E. Granroth; Feng Ye; Barry L. Winn; Lynn Boatner; Olivier Delaire

doi:10.1073/pnas.2419159122

Resolving the dynamic correlated disorder in KTa_1−xNb_xO₃

Xing He
, Mayanak K. Gupta
, Douglas L. Abernathy
, Garrett E. Granroth
, Feng Ye
, Barry L. Winn
, Lynn Boatner
, Olivier Delaire

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, we provide insights into the longstanding controversy regarding the off-centering of transition metal (TM) ions in the archetypal ferroelectric alloy KTa_1−xNb_xO₃ (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically correlated TM off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds light into an exemplary ferroelectric system and shows the importance of mapping the full S(Q, E) to reveal critical spatiotemporal correlations of atomic disorder from which functional properties emerge.

Original language	English
Article number	e2419159122
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	122
Issue number	7
DOIs	https://doi.org/10.1073/pnas.2419159122
State	Published - Feb 19 2025

Funding

ACKNOWLEDGMENTS. X.H. and O.D. were supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Award No. DE-SC0019978. The KTa1-xNbxO3 single-crystal was synthesized by L.B., and KTaO3 single-crystal was purchased through MSE Supplies. The use of Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE. Theoretical calculations were performed using resources of the National Energy Research Scientific Computing Center, a U.S. X.H. and O.D. were supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Award No. DE-SC0019978. The KTa1-xNbxO3 single-crystal was synthesized by L.B., and KTaO3 single-crystal was purchased through MSE Supplies. The use of Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE. Theoretical calculations were performed using resources of the National Energy Research Scientific Computing Center, a U.S. DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231.

Keywords

atomistic simulations
disordered alloys
ferroelectrics
neutron scattering
phase transitions

Access to Document

10.1073/pnas.2419159122

Cite this

@article{1868e493262d485da411f9549bdb435e,

title = "Resolving the dynamic correlated disorder in KTa1−xNbxO3",

abstract = "Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, we provide insights into the longstanding controversy regarding the off-centering of transition metal (TM) ions in the archetypal ferroelectric alloy KTa1−xNbxO3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically correlated TM off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds light into an exemplary ferroelectric system and shows the importance of mapping the full S(Q, E) to reveal critical spatiotemporal correlations of atomic disorder from which functional properties emerge.",

keywords = "atomistic simulations, disordered alloys, ferroelectrics, neutron scattering, phase transitions",

author = "Xing He and Gupta, \{Mayanak K.\} and Abernathy, \{Douglas L.\} and Granroth, \{Garrett E.\} and Feng Ye and Winn, \{Barry L.\} and Lynn Boatner and Olivier Delaire",

note = "Publisher Copyright: Copyright {\textcopyright} 2025 the Author(s).",

year = "2025",

month = feb,

day = "19",

doi = "10.1073/pnas.2419159122",

language = "English",

volume = "122",

journal = "Proceedings of the National Academy of Sciences of the United States of America",

issn = "0027-8424",

publisher = "National Academy of Sciences",

number = "7",

}

TY - JOUR

T1 - Resolving the dynamic correlated disorder in KTa1−xNbxO3

AU - He, Xing

AU - Gupta, Mayanak K.

AU - Abernathy, Douglas L.

AU - Granroth, Garrett E.

AU - Ye, Feng

AU - Winn, Barry L.

AU - Boatner, Lynn

AU - Delaire, Olivier

PY - 2025/2/19

Y1 - 2025/2/19

N2 - Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, we provide insights into the longstanding controversy regarding the off-centering of transition metal (TM) ions in the archetypal ferroelectric alloy KTa1−xNbxO3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically correlated TM off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds light into an exemplary ferroelectric system and shows the importance of mapping the full S(Q, E) to reveal critical spatiotemporal correlations of atomic disorder from which functional properties emerge.

AB - Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, we provide insights into the longstanding controversy regarding the off-centering of transition metal (TM) ions in the archetypal ferroelectric alloy KTa1−xNbxO3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically correlated TM off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds light into an exemplary ferroelectric system and shows the importance of mapping the full S(Q, E) to reveal critical spatiotemporal correlations of atomic disorder from which functional properties emerge.

KW - atomistic simulations

KW - disordered alloys

KW - ferroelectrics

KW - neutron scattering

KW - phase transitions

UR - https://www.scopus.com/pages/publications/85218435094

U2 - 10.1073/pnas.2419159122

DO - 10.1073/pnas.2419159122

M3 - Article

C2 - 39928874

AN - SCOPUS:85218435094

SN - 0027-8424

VL - 122

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

IS - 7

M1 - e2419159122

ER -