Size-driven transition of an 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...Size-driven transition of an 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 PbZrO_(3).Here,we use first-principles density functional theory to predict the stability of polar phases in Pt/PbZrO_(3)/Pt nanocapacitors.In a few atomic layer thick slabs of PbZrO_(3) sandwiched between Pt electrodes,we find that the polar phase originating from the well established R3c phase of bulk PbZrO_(3) is energetically favorable over the antipolar phase originating from the Pbam phase of bulk PbZrO_(3).The famous triple-well potential of antiferroelectric PbZrO_(3) 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 PbZrO_(3).展开更多
Publisher Correction:Ferroelectricity at the extreme thickness limit in the archetypal antiferroelectric PbZrO_(3)Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4...Publisher Correction:Ferroelectricity at the extreme thickness limit in the archetypal antiferroelectric PbZrO_(3)Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License,which permits any non-commercial use,sharing,distribution and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the CreativeCommonslicence,and indicate if you modified the licensed material.You do not have permission under this licence to share adapted material derived from this article or parts of it.The images or other third party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.To view a copy of this licence,visit http://creativecommons.org/licenses/by-nc-nd/4.0/.展开更多
基金support by the U.S.National Science Foundation under grant No.DMR-2219476I.P.acknowledges financial support by the U.S.Department of Energy,Office of Basic Energy Sciences,Division of Materials Sciences and Engineering under grant DE-SC0005245+3 种基金Computational support was provided by the National Energy Research Scientific Computing Center(NERSC)a U.S.Department of Energy,Office of Science User Facility located at Lawrence Berkeley National Laboratory,operated under Contract No.DE-AC02-05CH11231 using NERSC award BES-ERCAP-0025236L.J.acknowledges support from SFI grant SFI/21/US/3785A.K.gratefully acknowledges support from Department of Education and Learning NI through grant USI-211.
文摘Size-driven transition of an 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 PbZrO_(3).Here,we use first-principles density functional theory to predict the stability of polar phases in Pt/PbZrO_(3)/Pt nanocapacitors.In a few atomic layer thick slabs of PbZrO_(3) sandwiched between Pt electrodes,we find that the polar phase originating from the well established R3c phase of bulk PbZrO_(3) is energetically favorable over the antipolar phase originating from the Pbam phase of bulk PbZrO_(3).The famous triple-well potential of antiferroelectric PbZrO_(3) 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 PbZrO_(3).
文摘Publisher Correction:Ferroelectricity at the extreme thickness limit in the archetypal antiferroelectric PbZrO_(3)Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License,which permits any non-commercial use,sharing,distribution and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the CreativeCommonslicence,and indicate if you modified the licensed material.You do not have permission under this licence to share adapted material derived from this article or parts of it.The images or other third party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.To view a copy of this licence,visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
