Parameter-free prediction of phase transition in PbTiO3 through combination of quantum mechanics and statistical mechanics

Liu, Zi-Kui; Shang, Shun-Li; Du, Jinglian; Wang, Yi

doi:10.1016/j.scriptamat.2023.115480

Parameter-free prediction of phase transition in PbTiO₃ through combination of quantum mechanics and statistical mechanics

Journal Article · Thu Apr 20 00:00:00 EDT 2023 · Scripta Materialia

DOI:https://doi.org/10.1016/j.scriptamat.2023.115480· OSTI ID:2422207

^[1]; ^[1]; Du, Jinglian ^[2]; Wang, Yi ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Pennsylvania State Univ., University Park, PA (United States); Northwestern Polytechnical Univ., Xi'an, Shaanxi (China)

Thermodynamics of ferroelectric materials and their ferroelectric to paraelectric (FE-PE) transitions is commonly described by the phenomenological Landau theory and more recently by effective Hamiltonian and various potentials, all with model parameters fitted to experimental or theoretical data. Here, in this work, we show that the zentropy theory, which considers the total entropy of a system as a weighted sum of entropies of configurations that the system may experience and the statistical entropy among the configurations, can predict the FE-PE transition without fitting parameters. For PbTiO₃, the configurations are identified as the FE configurations with 90- or 180° domain walls in addition to the ground state FE configuration without domain wall. With the domain wall energies predicted from first-principles based on density functional theory in the literature as the only inputs, the FE-PE transition for PbTiO₃ is predicted showing remarkable agreement with experiments, unveiling the microscopic fundamentals of the transition.

View Accepted Manuscript (DOE)

Research Organization:: Pennsylvania State Univ., University Park, PA (United States); Pennsylvania State University, University Park, PA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0023185

OSTI ID:: 2422207

Alternate ID(s):: OSTI ID: 1971418
OSTI ID: 3022578

Journal Information:: Scripta Materialia, Journal Name: Scripta Materialia Vol. 232; ISSN 1359-6462

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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97 MATHEMATICS AND COMPUTING
Ferroelectric to paraelectric (FE-PE) transitions
First-principles calculations
PbTiO3
Statistical mechanics
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Parameter-free prediction of phase transition in PbTiO3 through combination of quantum mechanics and statistical mechanics

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Parameter-free prediction of phase transition in PbTiO₃ through combination of quantum mechanics and statistical mechanics