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Hydration of biologically relevant tetramethylammonium cation by neutron scattering and molecular dynamics.
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SYSNO ASEP 0581785 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Hydration of biologically relevant tetramethylammonium cation by neutron scattering and molecular dynamics. Author(s) Mason, Philip E. (UOCHB-X) RID, ORCID
Martinek, Tomáš (UOCHB-X) ORCID
Fábián, Balázs (UOCHB-X) ORCID
Vazdar, M. (CZ)
Jungwirth, Pavel (UOCHB-X) RID, ORCID
Ticháček, Ondřej (UOCHB-X) ORCID, RID
Duboué-Dijon, E. (FR)
Martinez-Seara, Hector (UOCHB-X) RID, ORCIDSource Title Physical Chemistry Chemical Physics. - : Royal Society of Chemistry - ISSN 1463-9076
Roč. 26, č. 4 (2024), s. 3208-3218Number of pages 11 s. Language eng - English Country GB - United Kingdom Keywords X-ray-scattering ; aqueous-solutions ; water-structure R&D Projects GA19-19561S GA ČR - Czech Science Foundation (CSF) Research Infrastructure e-INFRA CZ II - 90254 - CESNET, zájmové sdružení právnických osob Method of publishing Open access Institutional support UOCHB-X - RVO:61388963 UT WOS 001138421100001 EID SCOPUS 85182174499 DOI 10.1039/d3cp05449g Annotation Neutron scattering and molecular dynamics studies were performed on a concentrated aqueous tetramethylammonium (TMA) chloride solution to gain insight into the hydration shell structure of TMA, which is relevant for understanding its behavior in biological contexts of, e.g., properties of phospholipid membrane headgroups or interactions between DNA and histones. Specifically, neutron diffraction with isotopic substitution experiments were performed on TMA and water hydrogens to extract the specific correlation between hydrogens in TMA (HTMA) and hydrogens in water (HW). Classical molecular dynamics simulations were performed to help interpret the experimental neutron scattering data. Comparison of the hydration structure and simulated neutron signals obtained with various force field flavors (e.g. overall charge, charge distribution, polarity of the CH bonds and geometry) allowed us to gain insight into how sensitive the TMA hydration structure is to such changes and how much the neutron signal can capture them. We show that certain aspects of the hydration, such as the correlation of the hydrogen on TMA to hydrogen on water, showed little dependence on the force field. In contrast, other correlations, such as the ion-ion interactions, showed more marked changes. Strikingly, the neutron scattering signal cannot discriminate between different hydration patterns. Finally, ab initio molecular dynamics was used to examine the three-dimensional hydration structure and thus to benchmark force field simulations. Overall, while neutron scattering has been previously successfully used to improve force fields, in the particular case of TMA we show that it has only limited value to fully determine the hydration structure, with other techniques such as ab initio MD being of a significant help. Workplace Institute of Organic Chemistry and Biochemistry Contact asep@uochb.cas.cz ; Kateřina Šperková, Tel.: 232 002 584 ; Jana Procházková, Tel.: 220 183 418 Year of Publishing 2025 Electronic address https://doi.org/10.1039/D3CP05449G
Number of the records: 1