Using oxygen-17 as a nuclear probe, spin relaxometry was applied to study the high-density and low-density states of amorphous ice, covering temperatures below and somewhat above their glass transitions. These findings are put in perspective with results from deuteron nuclear magnetic resonance and with calculations based on dielectrically detected correlation times. This comparison reveals the presence of a wide distribution of correlation times. Furthermore, oxygen-17 central-transition echo spectra were recorded for wide ranges of temperature and pulse spacing. The spectra cannot be described by a single set of quadrupolar parameters, suggesting a distribution of H–O–H opening angles that is broader for high-density than for low-density amorphous ice. Simulations of the pulse separation dependent spin-echo spectra for various scenarios demonstrate that a small-step frequency diffusion process, assigned to the presence of homonuclear oxygen–oxygen interactions, determines the shape evolution of the pulse-separation-dependent spectra.
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