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Van der Waals interactions and the limits of isolated atom models at interfaces

机译:范德华相互作用和界面处孤立原子模型的局限性

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摘要

Van der Waals forces are among the weakest, yet most decisive interactions governing condensation and aggregation processes and the phase behaviour of atomic and molecular matter. Understanding the resulting structural motifs and patterns has become increasingly important in studies of the nanoscale regime. Here we measure the paradigmatic van der Waals interactions represented by the noble gas atom pairs Ar–Xe, Kr–Xe and Xe–Xe with a Xe-functionalized tip of an atomic force microscope at low temperature. Individual rare gas atoms were fixed at node sites of a surface-confined two-dimensional metal–organic framework. We found that the magnitude of the measured force increased with the atomic radius, yet detailed simulation by density functional theory revealed that the adsorption induced charge redistribution strengthened the van der Waals forces by a factor of up to two, thus demonstrating the limits of a purely atomic description of the interaction in these representative systems.
机译:范德华力是支配缩合和聚集过程以及原子和分子物质的相行为的最弱但最决定性的相互作用之一。在纳米尺度研究中,了解由此产生的结构图案和图案变得越来越重要。在这里,我们用低温力原子力显微镜的Xe功能化尖端,测量由稀有气体原子对Ar–Xe,Kr–Xe和Xe–Xe表示的范德华相互作用。单个稀有气体原子固定在表面受限的二维金属有机框架的节点位置。我们发现测得的力的大小随原子半径的增加而增加,但是通过密度泛函理论进行的详细模拟显示,吸附诱导的电荷再分布将范德华力提高了两倍,从而证明了纯粹的极限。这些代表性系统中相互作用的原子描述。

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