Papers › Structure, Organization and Heterogeneity of Water-Containing Deep Eutectic Solvents

Structure, Organization and Heterogeneity of Water-Containing Deep Eutectic Solvents

18 Jul 2022arXiv:2207.08529links table onlyarchive 2025-07-28

Kai Töpfer, Andrea Pasti, Anuradha Das, Seyedeh Maryam Salehi, Luis Itza Vazquez-Salazar, David Rohrbach, Thomas Feurer, Peter Hamm, Markus Meuwly

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The spectroscopy and structural dynamics of a deep eutectic mixture (KSCN/acetamide) with varying water content is investigated from 2D IR (with the C-N stretch vibration of the SCN^- anions as the reporter) and THz spectroscopy. Molecular dynamics simulations correctly describe the non-trivial dependence of both spectroscopic signatures depending on water content. For the 2D IR spectra, the MD simulations relate the steep increase in the cross relaxation rate at high water content to parallel alignment of packed SCN^- anions. Conversely, the non-linear increase of the THz absorption with increasing water content is mainly attributed to the formation of larger water clusters. The results demonstrate that a combination of structure sensitive spectroscopies and molecular dynamics simulations provides molecular-level insights into emergence of heterogeneity of such mixtures by modulating their composition.

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