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基元构筑的功能材料皮米尺度结构

肖东东 谷林

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基元构筑的功能材料皮米尺度结构

肖东东, 谷林

Picoscale structure of functional materials constructed by functional units

Xiao Dong-Dong, Gu Lin
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  • 功能材料的结构设计与性能调控是材料科学与凝聚态物理领域的前沿热点问题, 功能基元的人工序构成为近年来提升材料功能特性、探索新奇物理现象的新范式. 准确理解功能基元构筑的新材料宏观物性的起源要求精确地表征功能基元的结构、形态和分布, 明晰功能基元之间耦合效应. 具有皮米测量精度的像差校正透射电子显微镜是解析低对称性材料和复杂化学体系材料原子结构、化学组成和电子组态的重要工具, 为实现高精度、多维度表征功能基元及其空间的构筑方式、建立构-效关系提供了新途径. 本文通过选取不同尺度下的代表性功能基元, 论述了皮米尺度下功能基元的本征特性与空间排布, 及其与宏观物性之间的关联, 突出了像差校正透射电子显微学的突破和发展, 为理解基元构筑的功能材料功能性起源提供了坚实的基础.
    Structure design and performance regulation of functional materials are the cutting-edge hot topic in the field of materials science and condensed mater physics. Constructing hierarchical structures with functional units recently has become a new paradigm to improve the functionality of functional materials and explore new physical phenomena. Understanding the origin of physical properties of functional materials constructed by functional units requires us to precisely characterize the structure, configuration and spatial patterns of functional units, and their couplings. Aberration-corrected transmission electron microscopy has proven to be powerful in revealing the atomic structure, chemistry and electronic configuration of the functional materials with low symmetry and complex compositions, which provides a new avenue to reveal the functional units and their spatial patterns with high precision from different aspects and finally establish the structure-propertys relationship. In this paper, we summarize the inherent characteristics of typical functional units with different sizes, and the hierarchical structures constructed by functional units at the picoscale, by which the relationship between structures and functionality is revealed. The breakthrough and development of aberration-corrected transmission electron microscopy lays a solid foundation for understanding the origin of functionality of new materials constructed by functional units.
      通信作者: 谷林, l.gu@iphy.ac.cn
      作者简介:
      肖东东, 中国科学院物理研究所副研究员. 2015年于中国科学院物理研究所获凝聚态物理专业博士学位. 2016—2019年期间先后在美国西北太平洋国家实验室、纽约州立大学宾汉姆顿分校从事博士后研究, 2019年2月加入中国科学院物理研究所先进材料与结构分析实验室. 主要研究方向是利用先进透射电子显微学方法研究锂/钠离子电池正极材料原子结构、电荷密度及动力学演化. 至今在Nature Communications, Journal of American Chemical Society, Advanced Materials等学术期刊发表论文80余篇
      谷林, 清华大学教授, 国家杰出青年科学基金获得者. 2002年清华大学本科毕业, 2005年在美国亚利桑那州立大学获博士学位. 2006—2010年期间先后在德国马普金属所和日本东北大学从事博士后研究工作. 2010年11 月至 2022年2月在中国科学院物理研究所先进材料与结构分析实验室任研究员, 2022年2月加入清华大学材料学院. 长期从事电子显微方法与功能材料功能性起源研究, 在功能材料原子结构、电子结构与物性的关联研究方面取得了系列成果, 发表论文900余篇, 他引71000余次, H因子>140. 获得国际电子显微学联合会青年科学家奖(2006); 国际锂电池会议青年科学家奖(2012); 中国科学院“卢嘉锡”青年人才奖(2013); 中国科学院杰出科技成就奖(主要完成人)(2013); 中国晶体学会青年科技奖(2018); 第十六届中国青年科技奖特别奖(2020); 入选科睿唯安材料科学领域(2018—2022)和化学领域(2019—2022)全球高被引科学家
    • 基金项目: 北京市自然科学基金(批准号: Z190010)资助的课题.
      Corresponding author: Gu Lin, l.gu@iphy.ac.cn
    • Funds: Project supported by the Natural Science Foundation of Beijing, China (Grant No. Z190010).
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  • 图 1  氧八面体功能基元旋转与原子尺度成像[49,57] (a), (b)分别为La2/3Sr1/3MnO3/NdGaO3和La2/3Sr1/3MnO3/SrTiO3 (9 uc)/NdGaO3界面的原子分辨环形明场像[49]; (c) CaTiO3 (111)薄膜沿[1$ \stackrel{-}{1} $0]带轴的环形明场像; (d) 利用深度神经网络分析图(c)所得到的CaTiO3薄膜中氧八面体旋转模式分布图; (e) CaTiO3薄膜中每个单胞的极化矢量分布[57]

    Fig. 1.  Oxygen octahedral rotation and atomic resolution imaging[49,57]: (a), (b) Atomic resolution annular bright-field scanning transmission electron microscopy (ABF-STEM) images of La2/3Sr1/3MnO3/NdGaO3 and La2/3Sr1/3MnO3/SrTiO3 (9 uc)/NdGaO3 heterostructures, respectively[49]; (c) atomic resolution ABF-STEM image of CaTiO3 (111) films along the [1$ \stackrel{-}{1} $0] zone axis; (d) oxygen octahedral rotation map obtained by deep neural network analysis of the sample regions in (c); (e) polarization vectors for each unit cell of CaTiO3 films [57].

    图 2  不同铁电极化畴组态的原子结构[7,9,77,79] (a) BiFeO3-BaTiO3-SrTiO3薄膜[010]带轴的原子分辨高角环形暗场像, 黄色虚线勾画了纳米尺度铁电畴, 区域I、II、III分别为菱方相、四方相和两相界面[9]; (b) (K, Na)NbO3 (KNN)沿[110]方向衬度反转的环形明场像, O、R、T分别代表正交晶系、菱方晶系和四方晶系, 虚线区域标示了从R相到O相再到T相的极化旋转[7]; (c) PbTiO3/SrTiO3铁电多层薄膜中通量全闭合畴原子结构, 绿色和蓝色虚线表示90°畴壁, 红色虚线表示180°畴壁[77]; (d) PbTiO3/SrTiO3超晶格中长程有序排列的涡旋畴[79]. 图中所有箭头表示极化位移矢量

    Fig. 2.  Atomic structure of different domain configurations[7,9,77,79]: (a) Atomic resolution high angle annular dark field (HAADF)-STEM image of BiFeO3-BaTiO3-SrTiO3 film along the [010] direction, wherein the yellow dashed lines delineate the nanodomains, Region I, II, III are rhombohedral, tetragonal domain and interface between them, respectively[9]; (b) contrast-reversed ABF-STEM image of (K, Na)NbO3 (KNN) along [110] zone axis, O, R, and T indicate orthorhombic, rhombohedral and tetragonal phase, respectively. dashed lines regions highlighted by dash line show polarization rotation from R to O to T[7]; (c) atomic structure of flux-closure domain in the PbTiO3/SrTiO3 superlattice, the green and blue dashed lines indicate the 90° domain walls, the red dashed lines indicate the 180° domain walls[77]; (d) long-range ordered vortex-antivortex arrays in the PbTiO3/SrTiO3 superlattice[79]. All of arrows indicate the polar displacement vector.

    图 3  典型晶相功能基元构筑的功能氧化物材料原子结构[15, 90, 95] (a) LuFe2O4(左上)和LuFeO3(右上)的晶体结构、原子分辨高角环形暗场像以及由两者构筑的(LuFeO3)m/(LuFe2O4)1 (6 ≤ m ≤ 10)超晶格[15]; (b) (SrRuO3)1/(BaTiO3)10超晶格原子结构以及极化矢量分布(左图), 其中箭头表示钙钛矿B位原子相对于氧八面体中心的位移, 右图为垂直于超晶格界面方向钙钛矿A位和B位原子的衬度曲线[90]; (c) Li1.2Mn0.567Ni0.166Co0.067O2正极材料同一区域沿[$1\bar10 $]rh带轴的高角环形暗场像(左图)和环形明场像(右图), 其中P, R分别表示单斜的类Li2MnO3结构平行四边形和矩形对称性, 右图中的结构模型表示交互生长的两相和异质界面的原子排列[95]

    Fig. 3.  Atomic structure of functional oxide materials constructed by typical crystal phases[15, 90, 95]: (a) Crystal structure and atomic resolution HAADF-STEM images of LuFe2O4 (top left) and LuFeO3 (top right), (LuFeO3)m/(LuFe2O4)1 superlattice series for 6 ≤ m ≤ 10[15]; (b) superlattice atomic structure of (SrRuO3)1/(BaTiO3)10 with an overlay of the polar vectors (left), yellow arrows represent the displacement of the B-site from the mass center of oxygen octahedron in perovskite, and STEM intensity profiles of A-site and B-site atoms in perovskite across superlattice interface of BaTiO3/SrRuO3 (right)[90]. (c) HAADF (left) and ABF-STEM (right) images of the intergrowth two-phase and hetero-interface in the same region along the [$1 \bar1 0 $]rh zone axis, wherein P and R indicate parallelogram and rectangular symmetry of the monoclinic Li2MnO3-like structure and inserted image in the right image shows the intergrowth two-phase and hetero-interface atomic arrangements[95].

    表 1  皮米尺度像差校正透射电子显微学成像技术比较

    Table 1.  Comparison of aberration-corrected transmission electron microscopy imaging techniques at the picoscale.

    成像技术空间分辨率/pm测量精度/pm样品厚度/nm所需条件特点
    出射波重构80[30]3 <σ<10[31]< 10重构软件同时获取振幅和相位信息
    负球差成像57[32]σ <1[33]< 5负球差系数对轻元素敏感
    高角环形暗场成像40.5[34]σ<1[27]< 50环形探测器对重元素敏感
    环形明场成像44.4[35]1.5 <σ <3.8[36]< 50环形探测器对轻元素敏感
    积分差分相位衬度成像63[37]0.97 <σ <2.3[33]< 50四象限探测器对轻元素敏感、低剂量
    电子叠层衍射成像23[38]σ < 1[38, 39]< 50高速探测器、特定算法深亚埃分辨、低剂量
    下载: 导出CSV
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出版历程
  • 收稿日期:  2023-01-10
  • 修回日期:  2023-03-07
  • 上网日期:  2023-04-13
  • 刊出日期:  2023-06-05

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