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Abstract
Condensation processes are of key importance in nature and play a fundamental role in chemistry and physics. Owing to size effects at the nanoscale, it is conceptually desired to experimentally probe the dependence of condensate structure on the number of constituents one by one. Here we present an approach to study a condensation process atom-by-atom with the scanning tunnelling microscope, which provides a direct real-space access with atomic precision to the aggregates formed in atomically defined ‘quantum boxes’. Our analysis reveals the subtle interplay of competing directional and nondirectional interactions in the emergence of structure and provides unprecedented input for the structural comparison with quantum mechanical models. This approach focuses on—but is not limited to—the model case of xenon condensation and goes significantly beyond the well-established statistical size analysis of clusters in atomic or molecular beams by mass spectrometry.
Highlights
Condensation processes are of key importance in nature and play a fundamental role in chemistry and physics
As a model condensate we choose Xe atoms, which provide an ideal probe of the weak interactions because of their closed-shell electronic configuration
For the classification of the structural arrangements of the occ-n inside the pores, we initially focus on two aspects: first, whether a certain n-mer exhibits a subset of the adsorption sites observed for the occ-12, meaning that the (O3 Â O3)R30° structure, exhibited by each tetramer of occ-12, is preserved, and second, whether the considered occ-n can be described either as occ-(n-1) with one additional Xe atom, or as superposition of condensate structures observed for lower occupancies
Summary
Condensation processes are of key importance in nature and play a fundamental role in chemistry and physics. Our analysis reveals the subtle interplay of competing directional and nondirectional interactions in the emergence of structure and provides unprecedented input for the structural comparison with quantum mechanical models. This approach focuses on—but is not limited to—the model case of xenon condensation and goes significantly beyond the well-established statistical size analysis of clusters in atomic or molecular beams by mass spectrometry. We demonstrate how the atom-by-atom condensation of noble gas atoms proceeds under the influence of competing interactions This is conveniently probed within the atomically defined cavities of a supramolecular network, generated on the metal substrate. This approach is based on the ability of such on-surface networks to trap different adsorbates and to create host–guest systems[14,15,16,17,18,19,20]
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