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Solid-state methods for cooling and heating promise a more sustainablealternative to current compression cycles of greenhouse gases and inefficientfuel-burning heaters. Barocaloric effects (BCE) driven by hydrostatic pressure($p$) are especially encouraging in terms of large adiabatic temperaturechanges ($|\Delta T| \sim 10$ K) and colossal isothermal entropy changes($|\Delta S| \sim 100$ JK$^{-1}$kg$^{-1}$). However, BCE typically requirelarge pressure shifts due to irreversibility issues, and sizeable $|\Delta T|$and $|\Delta S|$ seldom are realized in a same material. Here, we demonstratethe existence of colossal and reversible BCE in LiCB$_{11}$H$_{12}$, awell-known solid electrolyte, near its order-disorder phase transition at$\approx 380$ K. Specifically, for $\Delta p \approx 0.23$ $(0.10)$ GPa wemeasured $|\Delta S_{\rm rev}| = 280$ $(200)$ JK$^{-1}$kg$^{-1}$ and $|\DeltaT_{\rm rev}| = 32$ $(10)$ K, which individually rival with state-of-the-artbarocaloric shifts obtained under similar pressure conditions. Furthermore,over a wide temperature range, pressure shifts of the order of $0.1$ GPa yieldhuge reversible barocaloric strengths of $\approx 2$JK$^{-1}$kg$^{-1}$MPa$^{-1}$. Molecular dynamics simulations were carried outto quantify the role of lattice vibrations, molecular reorientations and iondiffusion on the disclosed colossal BCE. Interestingly, lattice vibrations werefound to contribute the most to $|\Delta S|$ while the diffusion of lithiumions, despite adding up only slightly to the accompanying entropy change, wascrucial in enabling the molecular order-disorder phase transition. Our workexpands the knowledge on plastic crystals and should motivate the investigationof BCE in a variety of solid electrolytes displaying ion diffusion andconcomitant molecular orientational disorder.

Colossal reversible barocaloric effects in a plastic crystal mediated by lattice vibrations and ion diffusion