Ferroelectricity at the extreme thickness limit in the archetypal antiferroelectric PbZrO3

IF 9.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Nikhilesh Maity, Milan Haddad, Nazanin Bassiri-Gharb, Amit Kumar, Lewys Jones, Sergey Lisenkov, Inna Ponomareva
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引用次数: 0

Abstract

Size-driven transition of aNote, that the phasesn antiferroelectric into a polar ferroelectric or ferrielectric state is a strongly debated issue from both experimental and theoretical perspectives. While critical thickness limits for such transitions have been explored, a bottom-up approach in the ultrathin limit considering few atomic layers could provide insight into the mechanism of stabilization of the polar phases over the antipolar phase seen in bulk PbZrO3. Here, we use first-principles density functional theory to predict the stability of polar phases in Pt/PbZrO3/Pt nanocapacitors. In a few atomic layer thick slabs of PbZrO3 sandwiched between Pt electrodes, we find that the polar phase originating from the well established R3c phase of bulk PbZrO3 is energetically favorable over the antipolar phase originating from the Pbam phase of bulk PbZrO3. The famous triple-well potential of antiferroelectric PbZrO3 is modified in the nanocapacitor limit in such a way as to swap the positions of the global and local minima, stabilizing the polar phase relative to the antipolar one. The size effect is decomposed into the contributions from dimensionality reduction, surface charge screening, and interfacial relaxation, which reveals that it is the creation of well-compensated interfaces that stabilizes the polar phases over the antipolar ones in nanoscale PbZrO3.

Abstract Image

原型反铁电PbZrO3中厚度极限处的铁电性
aNote的尺寸驱动转变,即相反铁电态转变为极性铁电态或铁电态,从实验和理论角度都是一个备受争议的问题。虽然已经探索了这种转变的临界厚度限制,但在考虑少量原子层的超薄极限下,自下而上的方法可以深入了解在体PbZrO3中看到的极性相相对于反极性相的稳定机制。本文采用第一性原理密度泛函理论预测了Pt/PbZrO3/Pt纳米电容器中极性相的稳定性。在Pt电极之间夹几层厚的PbZrO3原子层板中,我们发现来自体PbZrO3的R3c相的极性相在能量上优于来自PbZrO3的Pbam相的反极性相。著名的反铁电PbZrO3的三阱电位在纳米电容器的限制下被修改,这样可以交换全局和局部最小值的位置,相对于反极性相稳定极性相。将尺寸效应分解为维数降低、表面电荷筛选和界面弛豫的贡献,表明在纳米尺度PbZrO3中,良好补偿的界面的产生使极性相相对于反极性相稳定。
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来源期刊
npj Computational Materials
npj Computational Materials Mathematics-Modeling and Simulation
CiteScore
15.30
自引率
5.20%
发文量
229
审稿时长
6 weeks
期刊介绍: npj Computational Materials is a high-quality open access journal from Nature Research that publishes research papers applying computational approaches for the design of new materials and enhancing our understanding of existing ones. The journal also welcomes papers on new computational techniques and the refinement of current approaches that support these aims, as well as experimental papers that complement computational findings. Some key features of npj Computational Materials include a 2-year impact factor of 12.241 (2021), article downloads of 1,138,590 (2021), and a fast turnaround time of 11 days from submission to the first editorial decision. The journal is indexed in various databases and services, including Chemical Abstracts Service (ACS), Astrophysics Data System (ADS), Current Contents/Physical, Chemical and Earth Sciences, Journal Citation Reports/Science Edition, SCOPUS, EI Compendex, INSPEC, Google Scholar, SCImago, DOAJ, CNKI, and Science Citation Index Expanded (SCIE), among others.
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