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低温扫描透射电子显微镜观察锰氧化物中不调和电荷有序的本质和演化。

Nature and evolution of incommensurate charge order in manganites visualized with cryogenic scanning transmission electron microscopy.

机构信息

Department of Physics, Cornell University, Ithaca, NY 14853.

Rutgers Center for Emergent Materials, Rutgers University, Piscataway, NJ 08854.

出版信息

Proc Natl Acad Sci U S A. 2018 Feb 13;115(7):1445-1450. doi: 10.1073/pnas.1714901115. Epub 2018 Jan 30.

Abstract

Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map, at atomic resolution, the nature of incommensurate charge-lattice order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ([Formula: see text]93 K). In diffraction, the ordering wave vector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the ordered state forms lattice-locked regions over a few wavelengths interspersed with phase defects and changing periodicity. The cations undergo picometer-scale ([Formula: see text]6 pm to 11 pm) transverse displacements, suggesting that charge-lattice coupling is strong. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93 K. Such local phase variations govern the long-range correlations of the charge-ordered state and locally change the periodicity of the modulations, resulting in wave vector shifts in reciprocal space. These atomically resolved observations underscore the importance of lattice coupling and phase inhomogeneity, and provide a microscopic explanation for putative "incommensurate" order in hole-doped oxides.

摘要

在掺杂空穴的氧化物中,不和谐的电荷有序与巨磁电阻、高温超导和电子向列性等奇异现象交织在一起。在这里,我们使用室温和低温([Formula: see text]93 K)下的扫描透射电子显微镜,以原子分辨率绘制了一种锰氧化物中不和谐电荷-晶格有序的性质。在衍射中,有序波矢随冷却而变化,这种行为通常与不和谐的顺序有关。然而,通过实空间测量,我们发现有序态在几个波长范围内形成与相位缺陷和周期性变化交错的晶格锁定区域。阳离子经历皮米级([Formula: see text]6 pm 到 11 pm)的横向位移,表明电荷-晶格耦合很强。我们进一步揭示了室温下周期性晶格位移中的相位非均匀性以及 93 K 时的相干性。这种局部相变化控制了电荷有序态的长程相关性,并局部改变了调制的周期性,导致倒易空间中波矢的移动。这些原子分辨率的观察结果强调了晶格耦合和相位非均匀性的重要性,并为掺杂空穴的氧化物中所谓的“不和谐”有序提供了微观解释。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/246d/5816166/aa8496069077/pnas.1714901115fig01.jpg

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