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Solid-state cooling using barocaloric materials is a promising avenue foreco-friendly, inexpensive and highly efficient cooling. To design barocaloriccompounds ready for deployment, it is essential to understand theirthermodynamic behaviour under working conditions. To this end, we have studiedthe rotational dynamics in the molecular-ionic crystal ammonium sulfate underpressure, providing detailed insight into the origin of its large barocaloriceffect. Using quasielastic neutron scattering experiments, we show thatrotation of the ammonium cations is facilitated by pressure in the low-entropyphase, with the rotational "hopping" motion increasing in frequency as thepressure-induced phase transition is approached. We explain this unusualbehaviour in terms of the competing hydrogen-bond networks represented by thetwo phases. This work includes the first results of a recently developedlow-background, high-pressure gas cell for neutron scattering, showcasing itspower in obtaining high-precision measurements of molecular dynamics underpressure.

Pressure dependence of atomic dynamics in barocaloric ammonium sulfate: I. Rotations