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Probing microhydration-induced effects on carbonyl compounds.

Olivier Aroule1, Mahmoud Jarraya2, Emilie-Laure Zins1

  • 1MONARIS UMR 8233 CNRS, Sorbonne Université, 4 place Jussieu, 75252 Paris Cedex 5, France. emilie-laure.zins@sorbonne-universite.fr.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Spectroscopy

Background:

  • Microhydration of organic molecules is vital for atmospheric, biological, and industrial processes.
  • Accurate experimental and theoretical descriptions of microhydration remain challenging.
  • The HyDRA challenge focused on understanding water-solute interactions.

Purpose of the Study:

  • To study monohydrate isomers and properties of four organic solutes with a C=O bond: cyclooctanone (CON), 1,3-dimethyl-2-imidazolidinone (DMI), methyl lactate (MLA), and 2,2,2-trifluoroacetophenone (TPH).
  • To evaluate the utility of O-H and C=O elongation shifts and UV-Vis spectroscopy in characterizing microhydration.
  • To analyze non-covalent interactions in monohydrated complexes using quantum chemistry tools and propose a classification.

Main Methods:

  • Detailed study of monohydrate isomers for CON, DMI, MLA, and TPH.
  • Analysis of O-H and C=O bond elongation shifts.
  • UV-Vis spectroscopy and quantum chemistry methods (electron density topology, electron pairing function, core-valence bifurcation index).

Main Results:

  • O-H elongation shift is confirmed as a useful indicator of complexation.
  • C=O elongation shift and UV-Vis spectroscopy are also effective for characterizing microhydration.
  • A close linear dependency was found between the core-valence bifurcation index and electron density (ρ).

Conclusions:

  • C=O elongation shifts and UV-Vis spectroscopy provide valuable insights into microhydration.
  • Quantum chemistry analyses, including CVBI and ρ, offer a detailed understanding of non-covalent interactions.
  • A novel classification of intermolecular water-solute interactions has been proposed based on the findings.