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Design of Lead-Free Antiferroelectric (1 − x)NaNbO3−xSrSnO3 Compositions Guided by First-Principles Calculations

Zhang, Mao-Hua and Hadaeghi, Niloofar and Egert, Sonja and Ding, Hui and Zhang, Hongbin and Groszewicz, Pedro B. and Buntkowsky, Gerd and Klein, Andreas and Koruza, Jurij (2021):
Design of Lead-Free Antiferroelectric (1 − x)NaNbO3−xSrSnO3 Compositions Guided by First-Principles Calculations.
In: Chemistry of Materials, 33 (1), pp. 266-274. ACS Publications, ISSN 0897-4756,
DOI: 10.1021/acs.chemmater.0c03685,
[Article]

Abstract

Antiferroelectric materials exhibit a unique electricfield- induced phase transition, which enables their use in energy storage, electrocaloric cooling, and nonvolatile memory applications. However, in many prototype antiferroelectrics this transition is irreversible, which prevents their implementation. In this work, we demonstrate a general approach to promote the reversibility of this phase transition by targeted modification of the material’s local structure. A new NaNbO3-based composition, namely (1− x)NaNbO3−xSrSnO3, was designed with a combination of firstprinciples calculations and experimental characterization. Our theoretical study predicts stabilization of the antiferroelectric state over the ferroelectric state with an energy difference of 1.4 meV/f.u. when 6.25 mol % of SrSnO3 is incorporated into NaNbO3. A series of samples was prepared using solid-state reactions, and the structural changes upon SrSnO3 incorporation were investigated using X-ray diffraction and 23Na solid-state nuclear magnetic resonance spectroscopy. The results revealed an increase in the unit cell volume and a more disordered, yet less distorted local Na environment, which were related to the stabilization of the antiferroelectric order. The SrSnO3-modified compositions exhibited well-defined double polarization loops and an eight times higher energy storage density as compared to unmodified NaNbO3. Our results indicate that this first-principles calculations based approach is of great potential for the design of new antiferroelectric compositions.

Item Type: Article
Erschienen: 2021
Creators: Zhang, Mao-Hua and Hadaeghi, Niloofar and Egert, Sonja and Ding, Hui and Zhang, Hongbin and Groszewicz, Pedro B. and Buntkowsky, Gerd and Klein, Andreas and Koruza, Jurij
Title: Design of Lead-Free Antiferroelectric (1 − x)NaNbO3−xSrSnO3 Compositions Guided by First-Principles Calculations
Language: English
Abstract:

Antiferroelectric materials exhibit a unique electricfield- induced phase transition, which enables their use in energy storage, electrocaloric cooling, and nonvolatile memory applications. However, in many prototype antiferroelectrics this transition is irreversible, which prevents their implementation. In this work, we demonstrate a general approach to promote the reversibility of this phase transition by targeted modification of the material’s local structure. A new NaNbO3-based composition, namely (1− x)NaNbO3−xSrSnO3, was designed with a combination of firstprinciples calculations and experimental characterization. Our theoretical study predicts stabilization of the antiferroelectric state over the ferroelectric state with an energy difference of 1.4 meV/f.u. when 6.25 mol % of SrSnO3 is incorporated into NaNbO3. A series of samples was prepared using solid-state reactions, and the structural changes upon SrSnO3 incorporation were investigated using X-ray diffraction and 23Na solid-state nuclear magnetic resonance spectroscopy. The results revealed an increase in the unit cell volume and a more disordered, yet less distorted local Na environment, which were related to the stabilization of the antiferroelectric order. The SrSnO3-modified compositions exhibited well-defined double polarization loops and an eight times higher energy storage density as compared to unmodified NaNbO3. Our results indicate that this first-principles calculations based approach is of great potential for the design of new antiferroelectric compositions.

Journal or Publication Title: Chemistry of Materials
Journal volume: 33
Number: 1
Publisher: ACS Publications
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Nonmetallic-Inorganic Materials
LOEWE
LOEWE > LOEWE-Schwerpunkte
LOEWE > LOEWE-Schwerpunkte > FLAME - Fermi Level Engineering Antiferroelektrischer Materialien für Energiespeicher und Isolatoren
Date Deposited: 13 Jan 2021 07:14
DOI: 10.1021/acs.chemmater.0c03685
Official URL: https://pubs.acs.org/doi/10.1021/acs.chemmater.0c03685
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