近年来,透射电子显微镜经历了一场革命,可以对生物材料和(生物)化学系统进行常规低温成像,也可以通过专用反应池或石墨烯吸附对液体进行成像。然而,这些方法通常需要对大量样本进行成像并重建平均表示,并且通常缺乏分析能力。在这里,使用原子探针断层扫描,我们提供原子的冷冻液体和分析亚纳米三维重建的原子分析。被分析的冰与纳米多孔金(NPG)接触并嵌入其中。我们首次报道了由高纯度重水和高纯度重水中的50 mM NaCl溶液形成的2-3微米厚冰层的数据。我们提出了一个标本制备策略,使用NPG膜,此外,我们报告的纳米多孔金和冷冻盐水溶液之间的界面的分析,在整个界面的Na和Cl浓度的明显趋势。我们探索了一系列的实验参数,以表明散装水样品的原子探针分析来与自己的特殊挑战,并讨论可能产生所观察到的现象的物理过程。我们的研究表明,使用冷冻水作为载体的近原子尺度的分析对象在解决方案中的原子探针层析成像的可行性。
英文摘要:
Transmission electron microscopy has undergone a revolution in recent years with the possibility to perform routine cryo-imaging of biological materials and (bio)chemical systems, as well as the possibility to image liquids via dedicated reaction cells or graphene-sandwiching. These approaches however typically require imaging a large number of specimens and reconstructing an average representation and often lack analytical capabilities. Here, using atom probe tomography we provide atom-by-atom analyses of frozen liquids and analytical sub-nanometre three dimensional reconstructions. The analyzed ice is in contact with, and embedded within, nanoporous gold (NPG). We report the first such data on 2-3 microns thick layers of ice formed from both high purity deuterated water and a solution of 50mM NaCl in high purity deuterated water. We present a specimen preparation strategy that uses a NPG film and, additionally, we report on an analysis of the interface between nanoporous gold and frozen salt water solution with an apparent trend in the Na and Cl concentrations across the interface. We explore a range of experimental parameters to show that the atom probe analyses of bulk aqueous specimens come with their own special challenges and discuss physical processes that may produce the observed phenomena. Our study demonstrates the viability of using frozen water as a carrier for near-atomic scale analysis of objects in solution by atom probe tomography.
Near-surface Defects Break Symmetry in Water Adsorption on CeO$_{2-x}$(111)
National Institute for Materials Science (NIMS)(物质材料研究机构);Departamento de Física Teórica de la Materia Condensada, Universidad Autónoma de Madrid(马德里自治大学凝聚态理论物理系);Instituto de Catálisis y Petroleoquímica (CSIC)(催化与石油化工研究所(西班牙国家研究委员会));Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid(马德里自治大学凝聚态物理中心);Graduate School of Engineering Science, Osaka University(大阪大学工学研究科)