Abstract
AbstractCarbohydrates are ubiquitous biomolecules in nature. The vast majority of their biomolecular activity takes place in aqueous environments. Molecular reactivity and functionality are, therefore, often strongly influenced by not only interactions with equivalent counterparts, but also with the surrounding water molecules. Glycoaldehyde (Gly) represents a prototypical system to identify the relevant interactions and the balance that governs them. Here we present a broadband rotational‐spectroscopy study on the stepwise hydration of the Gly dimer with up to three water molecules. We reveal the preferred hydrogen‐bond networks formed when water molecules sequentially bond to the sugar dimer. We observe that the dimer structure and the hydrogen‐bond networks at play remarkably change upon the addition of just a single water molecule to the dimer. Further addition of water molecules does not significantly alter the observed hydrogen‐bond topologies.
Highlights
A well-established approach to learn about these interactions is to generate and characterize small molecular self-aggregates and/or their complexes with a few water molecules in the gas phase using supersonic jets.[3]
Zinn et al.[11] studied the self-aggregation of Gly using rotational spectroscopy and provided accurate structural information of two qualitatively different Gly dimers in the gas phase. In this Communication, we present the structure and hydrogen bonds (HB) networks at play for the mixed (Gly)2-(H2O)1–3 complexes using the high resolution and sensitivity of chirped-pulse Fourier-transform microwave (CP-FTMW) spectroscopy.[12,13]
We observe that the Gly-dimer structure drastically changes with respect to that previously reported[11] upon the addition of only one water molecule
Summary
A well-established approach to learn about these interactions is to generate and characterize small molecular self-aggregates and/or their complexes with a few water molecules in the gas phase using supersonic jets.[3] Under these isolated conditions, several monomer units or water molecules can be added to the structure of the cluster in a stepwise, controlled manner. Gly has been shown to be a key intermediate in the formation of larger sugars through the formose reaction,[5] and it has even been discovered in the interstellar medium.[6] Using rotational spectroscopy, the structure and HB networks of the monomer[7] and the complex with one molecule of water[8] were investigated.
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