Supramolecular Secondary Ion Mass Spectrometry - Revealing Molecular Surroundings and Inter-Molecular Interactions in Organic Matter
2020
While supramolecular chemistry is a firmly established research field in laboratory conditions,
the experimental study of non-covalent interactions, such as hydrogen bonding and piinteractions, between different molecules in chemically rich, non-crystalline matter remains
highly challenging. We demonstrate that soft ion bombardment can trigger the joint desorption of
weakly interacting adjacent molecules, and that this in turn allows molecular interaction probabilities, surroundings, and arrangement in organic matter to be probed. Assemblies of
organic molecules linked by hydrogen bonds or dipole- interactions are extracted here with
preservation of chemistry and structure as single-charged supramolecular secondary ions.
Among the examples shown is the desorption of stable 12-molecular clusters of the amino acid
L-proline, which suggest an icosahedral on-surface self-assembly, and the desorption of supramolecular linear oligomers of 2,5-piperazinedione. The second half of the study lays down
the statistical framework for the reconstruction of a molecular interactome based on the relative
abundances of supramolecular dimers of different compositions within a mass spectrum acquired
on organic matter containing more than one type of molecule.
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