Water–biomolecule clusters studied by photoemission spectroscopy and multilevel atomistic simulations: hydration or solvation?. Issue 28 (6th July 2021)

• Record Type: Journal Article
• Authors: Mattioli, Giuseppe; Avaldi, Lorenzo; Bolognesi, Paola; Bozek, John D.; Castrovilli, Mattea C.; Chiarinelli, Jacopo; Domaracka, Alicja; Indrajith, Suvasthika; Maclot, Sylvain; Milosavljević, Aleksandar R.; Nicolafrancesco, Chiara; Rousseau, Patrick
• Is Part Of: Physical chemistry chemical physics. Volume 23:Issue 28(2021)
• Page Start: 15049
• Page End: 15058
• Publication Date: 2021-07-06
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d1cp02031e
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : The self-organization patterns unravelled for the water-uracil clusters may disclose new routes for controlling the delivery of precise amount of molecular blends via the insertion in a controlled environment, preserving their size and composition. Abstract : The properties of mixed water–uracil nanoaggregates have been probed by core electron–photoemission measurements to investigate supramolecular assembly in the gas phase driven by weak interactions. The interpretation of the measurements has been assisted by multilevel atomistic simulations, based on semi-empirical tight-binding and DFT-based methods. Our protocol established a positive-feedback loop between experimental and computational techniques, which has enabled a sound and detailed atomistic description of such complex heterogeneous molecular aggregates. Among biomolecules, uracil offers interesting and generalized skeletal features; its structure encompasses an alternation of hydrophilic H-bond donor and acceptor sites and hydrophobic moieties, typical in biomolecular systems, that induces a supramolecular core–shell-like organization of the mixed clusters with a water core and an uracil shell. This structure is far from typical models of both solid-state hydration, with water molecules in defined positions, or liquid solvation, where disconnected uracil molecules are completely surrounded by water.