Far from equilibrium pulsed poled Mn-doped relaxor ferroelectrics: a positive aging relaxation process

IF 9.3 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Acta Materialia Pub Date : 2025-10-12 DOI:10.1016/j.actamat.2025.121627

Michael W. Mervosh , Clive A. Randall

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Abstract

The aging behavior of high temperature pulse poled (HTPP) Mn-doped relaxor ferroelectrics (RFE) was investigated. It was found that following HTPP, a far from equilibrium state can be realized. Within this state, the dielectric and piezoelectric properties increased with aging in both single crystal and textured ceramic materials. The degree of aging, as well as the time scales involved, surpassed previous aging studies. The single crystals experienced 40–60 % increases in d₃₃ and ε_r over the span of a month, and the textured ceramics experienced 15–20 % increases over multiple weeks. Changes in Rayleigh analysis, heat flow at phase transitions, and X-ray diffraction patterns pointed towards important intrinsic transformations in the systems induced by HTPP and positive aging. It is hypothesized that such a transformation can arise due to far from equilibrium conditions driven by the ultra-fast field switching of pulse poling. The resultant uncompensated depolarization field that forms from ineffective bulk screening depressed properties on day one. With time, the defect dipoles within the Mn-doped systems are assumed to align to generate an internal field counteracting the incomplete compensation of the depolarization field as evidenced by the asymmetric hysteresis loops. The pulse poled state and the associated positive aging properties were analyzed under a first order elastic Gibbs Landau-Devonshire Theory and other phenomenological descriptions of the physical properties. The HTPP induced internal electric field and electrostrictive coupling lead to the time dependent evolution of the first order ferroelectric character and piezoelectric property enhancement.

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远离平衡的脉冲极化掺锰弛豫铁电体：一个正老化弛豫过程

研究了高温脉冲极化掺锰弛豫铁电体（RFE）的老化行为。研究发现，在高温高压下，可以实现一个远离平衡的状态。在此状态下，单晶和织构陶瓷材料的介电和压电性能随老化而增加。衰老的程度，以及所涉及的时间尺度，超过了以往的衰老研究。单晶的d33和εr在一个月内增加了40-60%，而纹理陶瓷的d33和εr在数周内增加了15-20%。瑞利分析、相变热流和x射线衍射图的变化表明，HTPP和正时效诱导的体系发生了重要的内在转变。假设这种转变是由于脉冲极化的超快场开关驱动的远离平衡条件而产生的。由此产生的无补偿退极化场是由无效的大块筛分在第一天就降低了性能。随着时间的推移，假设mn掺杂体系内的缺陷偶极子排列在一起，产生一个内部场，抵消去极化场的不完全补偿，如不对称磁滞回线所证明的那样。在一阶弹性Gibbs Landau-Devonshire理论和其他物理性质的现象学描述下，分析了脉冲极化态和相关的正老化性质。HTPP诱导的内部电场和电致伸缩耦合导致了一阶铁电特性随时间的演化和压电性能的增强。

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来源期刊

Acta Materialia 工程技术-材料科学：综合

CiteScore

16.10

自引率

8.50%

发文量

801

审稿时长

53 days

期刊介绍： Acta Materialia serves as a platform for publishing full-length, original papers and commissioned overviews that contribute to a profound understanding of the correlation between the processing, structure, and properties of inorganic materials. The journal seeks papers with high impact potential or those that significantly propel the field forward. The scope includes the atomic and molecular arrangements, chemical and electronic structures, and microstructure of materials, focusing on their mechanical or functional behavior across all length scales, including nanostructures.