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

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.

SUBMITTER: Chubak I

PROVIDER: S-EPMC9816157 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Quadrupolar <sup>23</sup>Na<sup>+</sup> NMR relaxation as a probe of subpicosecond collective dynamics in aqueous electrolyte solutions.

Chubak Iurii I Alon Leeor L Silletta Emilia V EV Madelin Guillaume G Jerschow Alexej A Rotenberg Benjamin B

Nature communications 20230105 1

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 fluctuation ...[more]

PMID: 36604414

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Project description:PurposeTo capture the multiquantum coherence (MQC) 23 Na signal. Different phase-cycling options and sequences are compared in a unified theoretical layout, and a novel sequence is developed.MethodsAn open source simulation overview is provided with graphical explanations to facilitate MQC understanding and access to techniques. Biases such as B0 inhomogeneity and stimulated echo signal were simulated for 4 different phase-cycling options previously described. Considerations for efficiency and accuracy lead to the implementation of a 2D Cartesian single and triple quantum imaging of sodium (CRISTINA) sequence employing two 6-step cycles in combination with a multi-echo readout. CRISTINA was compared to simultaneous single-quantum and triple-quantum-filtered MRI of sodium (SISTINA) under strong static magnetic gradient. CRISTINA capabilities were assessed on 8 × 60 mL, 0% to 5% agarose phantom with 50 to 154 mM 23 Na concentration at 7 T. CRISTINA was demonstrated subsequently in vivo in the brain.ResultsSimulation of B0 inhomogeneity showed severe signal dropout, which can lead to erroneous MQC measurement. Stimulated echo signal was highest at the time of triple-quantum coherences signal maximum. However, stimulated echo signal is separated by Fourier Transform as an offset and did not interfere with MQC signals. The multi-echo readout enabled capturing both single-quantum coherences and triple-quantum coherences signal evolution at once. Signal combination of 2 phase-cycles with a corresponding B0 map was found to recover the signal optimally. Experimental results confirm and complement the simulations.ConclusionConsiderations for efficient MQC measurements, most importantly avoiding B0 signal loss, led to the design of CRISTINA. CRISTINA captures triple-quantum coherences and single-quantum coherences signal evolution to provide complete sodium signal characterization including T2∗ fast, T2∗ slow, MQC amplitudes, and sodium concentration.

Dataset Information

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

Publications

Quadrupolar <sup>23</sup>Na<sup>+</sup> NMR relaxation as a probe of subpicosecond collective dynamics in aqueous electrolyte solutions.

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Dataset Information

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

Publications

Quadrupolar <sup>23</sup>Na<sup>+</sup> NMR relaxation as a probe of subpicosecond collective dynamics in aqueous electrolyte solutions.

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OmicsDI is part of the ELIXIR infrastructure

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