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Issue 16, 2017
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Prediction of low-field nuclear singlet lifetimes with molecular dynamics and quantum-chemical property surface

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Abstract

Molecular dynamics and quantum chemistry methods are implemented to quantify nuclear spin-1/2 pair singlet-state relaxation rates for three molecular systems at low magnetic field and room temperature. Computational methodology is developed for weak interactions, particularly important for singlet states at low field. These include spin-rotation and spin-internal-motion effects, which describe the coupling of the spin-carrying nuclei to fluctuating local magnetic fields induced by the overall and internal molecular fluctuations, respectively. A high-dimensional tensor property surface using Kriging interpolation is developed to circumvent costly quantum-chemical calculations. Together with the intramolecular dipolar relaxation, all the simulated relaxation mechanisms are accounted for with a common theoretical framework. Comparison with experiment indicates that quantitative accuracy is obtained, sufficient to enable guidance in the molecular design of molecules with long-lived singlet order.

Graphical abstract: Prediction of low-field nuclear singlet lifetimes with molecular dynamics and quantum-chemical property surface

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Article information


Submitted
08 Dec 2016
Accepted
16 Jan 2017
First published
17 Jan 2017

Phys. Chem. Chem. Phys., 2017,19, 10237-10254
Article type
Paper

Prediction of low-field nuclear singlet lifetimes with molecular dynamics and quantum-chemical property surface

P. Håkansson, Phys. Chem. Chem. Phys., 2017, 19, 10237
DOI: 10.1039/C6CP08394C

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