气候变化领域集成服务门户(CCPortal): Proton strings and rings in atypical nucleation of ferroelectricity in ice

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DOI	10.1073/pnas.2018837118
	Proton strings and rings in atypical nucleation of ferroelectricity in ice
	Lasave J.; Koval S.; Laio A.; Tosatti E.
发表日期	2021
ISSN	00278424
卷号	118 期号:1
英文摘要	Ordinary ice has a proton-disordered phase which is kinetically metastable, unable to reach, spontaneously, the ferroelectric (FE) ground state at low temperature where a residual Pauling entropy persists. Upon light doping with KOH at low temperature, the transition to FE ice takes place, but its microscopic mechanism still needs clarification. We introduce a lattice model based on dipolar interactions plus a competing, frustrating term that enforces the ice rule (IR). In the absence of IR-breaking defects, standard Monte Carlo (MC) simulation leaves this ice model stuck in a state of disordered proton ring configurations with the correct Pauling entropy. A replica exchange accelerated MC sampling strategy succeeds, without open path moves, interfaces, or off-lattice configurations, in equilibrating this defect-free ice, reaching its lowtemperature FE order through a well-defined first-order phase transition. When proton vacancies mimicking the KOH impurities are planted into the IR-conserving lattice, they enable standard MC simulation to work, revealing the kinetics of evolution of ice from proton disorder to partial FE order below the transition temperature. Replacing ordinary nucleation, each impurity opens up a proton ring generating a linear string, an actual FE hydrogen bond wire that expands with time. Reminiscent of those described for spin ice, these impurity-induced strings are proposed to exist in doped water ice too, where IRs are even stronger. The emerging mechanism yields a dependence of the long-time FE order fraction upon dopant concentration, and upon quenching temperature, that compares favorably with that known in real-life KOH doped ice. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Ferroelectricity; Ice; Nucleation; Proton strings and rings; Replica exchange Monte Carlo
语种	英语
scopus关键词	hydrogen; ice; iron; proton; proton ring; proton string; unclassified drug; Article; chemical interaction; chemical reaction; concentration (parameter); electricity; entropy; ferroelectricity; hydrogen bond; low temperature; Monte Carlo method; nucleation; phase transition; priority journal; transition temperature
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/181156
作者单位	Instituto de Física Rosario, Consejo Nacional de Investigaciones Científicas y Técnicas, Universidad Nacional de Rosario, Rosario, 2000, Argentina; International Center for Theoretical Physics, Trieste, I-34151, Italy; International School for Advanced Studies (SISSA), Trieste, I-34136, Italy; CNR-IOM Democritos, Trieste, I-34136, Italy
推荐引用方式 GB/T 7714	Lasave J.,Koval S.,Laio A.,et al. Proton strings and rings in atypical nucleation of ferroelectricity in ice[J],2021,118(1).
APA	Lasave J.,Koval S.,Laio A.,&Tosatti E..(2021).Proton strings and rings in atypical nucleation of ferroelectricity in ice.Proceedings of the National Academy of Sciences of the United States of America,118(1).
MLA	Lasave J.,et al."Proton strings and rings in atypical nucleation of ferroelectricity in ice".Proceedings of the National Academy of Sciences of the United States of America 118.1(2021).