Quadrupolar 23Na+ NMR relaxation as a probe of subpicosecond collective dynamics in aqueous electrolyte solutions

Iurii Chubak, Leeor Alon, Emilia V. Silletta, Guillaume Madelin, Alexej Jerschow () and Benjamin Rotenberg ()
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Iurii Chubak: Sorbonne Université CNRS, Physico-Chimie des électrolytes et Nanosystèmes Interfaciaux
Leeor Alon: New York University School of Medicine, Department of Radiology, Center for Biomedical Imaging
Emilia V. Silletta: Universidad Nacional de Córdoba, Facultad de Matemática, Astronomía, Física y Computación
Guillaume Madelin: New York University School of Medicine, Department of Radiology, Center for Biomedical Imaging
Alexej Jerschow: New York University, Department of Chemistry
Benjamin Rotenberg: Sorbonne Université CNRS, Physico-Chimie des électrolytes et Nanosystèmes Interfaciaux

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Nuclear magnetic resonance relaxometry represents a powerful tool for extracting dynamic information. Yet, obtaining links to molecular motion is challenging for many ions that relax through the quadrupolar mechanism, which is mediated by electric field gradient fluctuations and lacks a detailed microscopic description. For sodium ions in aqueous electrolytes, we combine ab initio calculations to account for electron cloud effects with classical molecular dynamics to sample long-time fluctuations, and obtain relaxation rates in good agreement with experiments over broad concentration and temperature ranges. We demonstrate that quadrupolar nuclear relaxation is sensitive to subpicosecond dynamics not captured by previous models based on water reorientation or cluster rotation. While ions affect the overall water retardation, experimental trends are mainly explained by dynamics in the first two solvation shells of sodium, which contain mostly water. This work thus paves the way to the quantitative understanding of quadrupolar relaxation in electrolyte and bioelectrolyte systems.

Date: 2023
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DOI: 10.1038/s41467-022-35695-3

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