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

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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
    New York University Grossman School of Medicine)

  • Emilia V. Silletta

    (Universidad Nacional de Córdoba, Facultad de Matemática, Astronomía, Física y Computación
    Instituto de Física Enrique Gaviola, CONICET)

  • Guillaume Madelin

    (New York University School of Medicine, Department of Radiology, Center for Biomedical Imaging
    New York University Grossman School of Medicine)

  • Alexej Jerschow

    (New York University, Department of Chemistry)

  • Benjamin Rotenberg

    (Sorbonne Université CNRS, Physico-Chimie des électrolytes et Nanosystèmes Interfaciaux)

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.

Suggested Citation

  • Iurii Chubak & Leeor Alon & Emilia V. Silletta & Guillaume Madelin & Alexej Jerschow & Benjamin Rotenberg, 2023. "Quadrupolar 23Na+ NMR relaxation as a probe of subpicosecond collective dynamics in aqueous electrolyte solutions," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-022-35695-3
    DOI: 10.1038/s41467-022-35695-3
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    References listed on IDEAS

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    1. Vasileios Balos & Sho Imoto & Roland R. Netz & Mischa Bonn & Douwe Jan Bonthuis & Yuki Nagata & Johannes Hunger, 2020. "Macroscopic conductivity of aqueous electrolyte solutions scales with ultrafast microscopic ion motions," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    2. Renato Torre & Paolo Bartolini & Roberto Righini, 2004. "Structural relaxation in supercooled water by time-resolved spectroscopy," Nature, Nature, vol. 428(6980), pages 296-299, March.
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