Beyond Isotropic Tumbling Models: Nuclear Spin Relaxation in Liquids from First Principles

Abstract

Relaxed rolling: First-principles MD simulations are used to compute the longitudinal quadrupolar relaxation of the 17O and 2H nuclei of liquid water at ambient conditions. The limits of the commonly assumed simple exponential decay of the EFG autocorrelation functions is elucidated (see graph) and their relation to the physics of the system is demonstrated.