Atomic-Scale Time-Resolved Imaging of Krypton Dimers, Chains and Transition to a One-Dimensional Gas.
Atomic-Scale Time-Resolved Imaging of Krypton Dimers, Chains and Transition to a One-Dimensional Gas.
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氪二聚体、链和一维气体跃迁的原子尺度时间分辨成像。
DOI：
10.1021/acsnano.3c07853
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发表时间：
2024-01-30
期刊：
影响因子：
17.1
通讯作者：
Khlobystov, Andrei N.
中科院分区：
文献类型：
--
作者：
Cardillo-Zallo, Ian;Biskupek, Johannes;Bloodworth, Sally;Marsden, Elizabeth S.;Fay, Michael W.;Ramasse, Quentin M.;Rance, Graham A.;Stoppiello, Craig T.;Cull, William J.;Weare, Benjamin L.;Whitby, Richard J.;Kaiser, Ute;Brown, Paul D.;Khlobystov, Andrei N.
关键词：
使用时间分辨透射电子显微镜（TEM）研究了稀有气体元素的单原子动力学，直接观察提供了对纳米级物质的化学键合，反应性和状态的更深入理解。我们报告了一个纳米级的系统，包括内嵌富勒烯封装在单壁碳纳米管（（Kr@C60）@SWCNT），能够交付和释放氪原子的需求，通过合并的主机富勒烯笼的作用下的电子束（原位）或热（非原位）。利用X射线能量色散谱（EDS）、电子能量损失谱（EELS）和X射线光电子能谱（XPS）研究了Kr原子的状态和动力学。使用像差校正高分辨率TEM（AC-HRTEM），像差校正扫描TEM（AC-STEM）和单原子光谱成像（STEM-EELS）精确测量Kr原子位置。电子束驱动形成2Kr@C120胶囊，其中确定了货车范德华Kr 2和瞬时共价[Kr 2]+键合状态。热聚结导致形成更长的聚结嵌套纳米管含有更松散的结合Krn链（n = 3-6）。在某些情况下，Kr原子位置的离域被STEM分析确认为向一维（1D）气体的转变，因为Kr原子在长的、退火良好的嵌套纳米管内仅被限制在一个平移自由度。通过拉曼光谱研究了这种嵌套纳米管结构。这种材料代表了在环境条件下稳定的高度压缩和尺寸约束的1D气体。直接原子尺度成像揭示了这种稀有气体元素的难以捉摸的成键状态和以前看不见的一维气态物质，表明TEM是在单原子水平上发现化学的有力工具。
Single-atom dynamics of noble-gas elements have been investigated using time-resolved transmission electron microscopy (TEM), with direct observation providing for a deeper understanding of chemical bonding, reactivity, and states of matter at the nanoscale. We report on a nanoscale system consisting of endohedral fullerenes encapsulated within single-walled carbon nanotubes ((Kr@C60)@SWCNT), capable of the delivery and release of krypton atoms on-demand, via coalescence of host fullerene cages under the action of the electron beam (in situ) or heat (ex situ). The state and dynamics of Kr atoms were investigated by energy dispersive X-ray spectroscopy (EDS), electron energy loss spectroscopy (EELS), and X-ray photoelectron spectroscopy (XPS). Kr atom positions were measured precisely using aberration-corrected high-resolution TEM (AC-HRTEM), aberration-corrected scanning TEM (AC-STEM), and single-atom spectroscopic imaging (STEM-EELS). The electron beam drove the formation of 2Kr@C120 capsules, in which van der Waals Kr2 and transient covalent [Kr2]+ bonding states were identified. Thermal coalescence led to the formation of longer coalesced nested nanotubes containing more loosely bound Krn chains (n = 3–6). In some instances, delocalization of Kr atomic positions was confirmed by STEM analysis as the transition to a one-dimensional (1D) gas, as Kr atoms were constrained to only one degree of translational freedom within long, well-annealed, nested nanotubes. Such nested nanotube structures were investigated by Raman spectroscopy. This material represents a highly compressed and dimensionally constrained 1D gas stable under ambient conditions. Direct atomic-scale imaging has revealed elusive bonding states and a previously unseen 1D gaseous state of matter of this noble gas element, demonstrating TEM to be a powerful tool in the discovery of chemistry at the single-atom level.
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