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Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry

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Water Triggers Hydrogen-Bond-Network Reshaping in the Glycoaldehyde Dimer.

Cristóbal Pérez^1,2, Amanda L Steber^1,2, Berhane Temelso³

¹Deutsches Elektronen-Synchrotron DESY, Notkestraße 85, 22607, Hamburg, Germany.

Angewandte Chemie (International Ed. in English)

|February 26, 2020

Summary

The hydration of glycoaldehyde dimers by water molecules significantly alters their structure and hydrogen-bonding networks. Even a single water molecule causes substantial changes, with further additions having minimal impact.

Keywords:

Chirality Hydration Hydrogen bonding Rotational Spectroscopy Self-aggregation

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Area of Science:

Carbohydrate chemistry
Physical chemistry
Supramolecular chemistry

Background:

Carbohydrates are vital biomolecules, with their functions heavily influenced by aqueous environments.
Understanding molecular interactions in water is crucial for carbohydrate chemistry.
Glycoaldehyde (Gly) serves as a model system for studying these hydration effects.

Purpose of the Study:

To investigate the stepwise hydration of the glycoaldehyde dimer.
To identify the preferred hydrogen-bond networks formed with water molecules.
To understand how water influences carbohydrate structure and interactions.

Main Methods:

Broadband rotational spectroscopy was employed.
The study focused on the glycoaldehyde dimer with up to three water molecules.
Analysis of spectral data revealed hydrogen-bond network formation.

Main Results:

The addition of even a single water molecule drastically alters the glycoaldehyde dimer's structure.
Preferred hydrogen-bond networks were identified as water molecules sequentially hydrated the dimer.
Further hydration beyond one water molecule did not significantly change the observed hydrogen-bond topologies.

Conclusions:

Water molecules play a critical role in shaping carbohydrate structure and interactions.
The initial hydration event is the most impactful for glycoaldehyde dimers.
Rotational spectroscopy is a powerful tool for elucidating hydration structures in biomolecules.