RT info:eu-repo/semantics/article
T1 Adaptive Response to Solvation in Flexible Molecules: Oligo Hydrates of 4‐Hydroxy‐2‐butanone
A1 Li, Meng
A1 Li, Wenqin
A1 Pérez Cuadrado, Cristobal
A1 Lesarri Gómez, Alberto Eugenio
A1 Grabow, Jens‐Uwe
K1 Molecular spectroscopy
K1 Conformational behavior · Water clusters · Non-covalent interactions · Hydrogen bonding · Rotational spectroscopy
K1 2206.07 Espectroscopia Molecular
K1 2210.20 Espectroscopia Molecular
AB Structural changes induced by water play apivotal role in chemistry and biology but remainchallenging to predict, measure, and control at molecularlevel. Here we explore size-governed gas-phasewater aggregation in the flexible molecule 4-hydroxy-2-butanone, modeling the conformational adaptability offlexible substrates to host water scaffolds and thepreference for sequential droplet growth. The experimentwas conducted using broadband rotational spectroscopy,rationalized with quantum chemical calculations.Two different isomers were observed experimentallyfrom the di- to the pentahydrates (4-hydroxy-2-butanone-(H2O)n=2–5), including the 18O isotopologues forthe di- and trihydrates. Interestingly, to accommodatewater molecules effectively, the heavy atom skeleton of4-hydroxy-2-butanone reshapes in every observed isomerand does not correspond to the stable conformer ofthe free monomer. All solvates initiate from the alcoholgroup (proton donor) but retain the carbonyl group assecondary binding point. The water scaffolds closelyresemble those found in the pure water clusters,balancing between the capability of 4-hydroxy-2-butanonefor steering the orientation and position of thewater molecules and the ability of water to modulate themonomer’s conformation. The present work thus providesan accurate molecular description on how torsionallyflexible molecules dynamically adapt to water alongprogressing solvation.
PB Wiley
SN 1433-7851
YR 2024
FD 2024
LK https://uvadoc.uva.es/handle/10324/74548
UL https://uvadoc.uva.es/handle/10324/74548
LA eng
NO Angewandte Chemie International Edition, Julio 2024, e202404447
NO Producción Científica
DS UVaDOC
RD 03-abr-2025