A High Working Temperature Multiferroic Induced by Inverse Temperature Symmetry Breaking

化学 多铁性 反向 相变 对称性破坏 凝聚态物理 对称(几何) 居里温度 铁弹性 铁学 相(物质) 纳米技术 材料科学 量子力学 铁磁性 光电子学 量子相变 有机化学 物理 量子临界点 铁电性 电介质 数学 几何学
作者
Lei-Yu Zhan,Yu Zhou,Na Li,Linjie Zhang,Xiao‐Juan Xi,Zhao‐Quan Yao,Jiong‐Peng Zhao,Xian‐He Bu
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (8): 5414-5422 被引量:10
标识
DOI:10.1021/jacs.3c12842
摘要

Molecular-based multiferroic materials that possess ferroelectric and ferroelastic orders simultaneously have attracted tremendous attention for their potential applications in multiple-state memory devices, molecular switches, and information storage systems. However, it is still a great challenge to effectively construct novel molecular-based multiferroic materials with multifunctionalities. Generally, the structure of these materials possess high symmetry at high temperatures, while processing an obvious order–disorder or displacement-type ferroelastic or ferroelectric phase transition triggered by symmetry breaking during the cooling processes. Therefore, these materials can only function below the Curie temperature (Tc), the low of which is a severe impediment to their practical application. Despite great efforts to elevate Tc, designing single-phase crystalline materials that exhibit multiferroic orders above room temperature remains a challenge. Here, an inverse temperature symmetry-breaking phenomenon was achieved in [FPM][Fe3(μ3-O)(μ-O2CH)8] (FPM stands for 3-(3-formylamino-propyl)-3,4,5,6-tetrahydropyrimidin-1-ium, which acts as the counterions and the rotor component in the network), enabling a ferroelastoelectric phase at a temperature higher than Tc (365 K). Upon heating from room temperature, two-step distinct symmetry breaking with the mm2Fm species leads to the coexistence of ferroelasticity and ferroelectricity in the temperature interval of 365–426 K. In the first step, the FPM cations undergo a conformational flip-induced inverse temperature symmetry breaking; in the second step, a typical ordered–disordered motion-induced symmetry breaking phase transition can be observed, and the abnormal inverse temperature symmetry breaking is unprecedented. Except for the multistep ferroelectric and ferroelastic switching, this complex also exhibits fascinating nonlinear optical switching properties. These discoveries not only signify an important step in designing novel molecular-based multiferroic materials with high working temperatures, but also inspire their multifunctional applications such as multistep switches.
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