Solid-state refrigeration technology based on caloric effects are promising to replace the currently used vapor compression cycles. However, their application is restricted due to limited performances of caloric materials. Here, we have identified colossal barocaloric effects (CBCEs) in a class of disordered solids called plastic crystals. The obtained entropy changes are about 380 J kg -1 K -1 in the representative neopentylglycol around room temperature. Inelastic neutron scattering reveals that the CBCEs in plastic crystals are attributed to the combination of the vast molecular orientational disorder, giant compressibility and high anharmonic lattice dynamics. Our study establishes the microscopic scenario for CBCEs in plastic crystals and paves a new route to the next-generation solid-state refrigeration technology.

A thermoelectric material consisting of Cu 2 Se incorporated with up to 0.45 wt% of graphene nanoplates is reported. The carbon-reinforced Cu 2 Se exhibits an ultra-high thermoelectric figure-of-merit of zT = 2.44 ± 0.25 at 870 K. Microstructural characterization reveals dense, nanostructured grains of Cu 2 Se with multilayer-graphene and graphite agglomerations located at grain boundaries. High temperature X-ray diffraction shows that the graphene incorporated Cu 2 Se matrix retains a cubic structure and the composite microstructure is chemically stable. Based on the experimental structure, density functional theory was used to calculate the formation energy of carbon point defects and the associated phonon density of states. The isolated carbon inclusion is shown to have a high formation energy in Cu 2 Se whereas graphene and graphite phases are enthalpically stable relative to the solid solution. Neutron 2 spectroscopy proves that there is a frequency mismatch in the phonon density of states between the carbon honeycomb phases and cubic Cu 2 Se. This provides a mechanism for the strong scattering of phonons at the composite interfaces, which significantly impedes the conduction of heat and enhances thermoelectric performance.

We use neutron scattering to show that ferromagnetic (FM) phase transition in the two-dimensional (2D) honeycomb lattice CrI 3 is a weakly first order transition and controlled by spin-orbit coupling (SOC) induced magnetic anisotropy, instead of magnetic exchange coupling as in a conventional ferromagnet. With increasing temperature, the magnitude of magnetic anisotropy, seen as a spin gap at the Brillouin zone center, decreases in a power law fashion and vanishes at T C , while the in-plane and c-axis spin-wave stiffnesses associated with magnetic exchange couplings remain robust at T C. We also compare parameter regimes where spin waves in CrI 3 can be described by a Heisenberg Hamiltonian with Dzyaloshinskii-Moriya interaction or a Heisenberg-Kitaev Hamiltonian. These results suggest that the SOC induced magnetic anisotropy plays a dominant role in stabilizing the FM order in single layer 2D van der Waals ferromagnets.

Inelastic neutron scattering (INS) has been used to investigate the crystal field (CF) magnetic excitations of the analogs of the most representative lanthanoid-polyoxometalate single-molecule magnet family: Na[Ln(WO)] (Ln = Nd, Tb, Ho, Er). Ab initio complete active space self-consistent field/restricted active space state interaction calculations, extended also to the Dy analog, show good agreement with the experimentally determined low-lying CF levels, with accuracy better in most cases than that reported for approaches based only on simultaneous fitting to CF models of magnetic or spectroscopic data for isostructural Ln families. In this work we demonstrate the power of a combined spectroscopic and computational approach. Inelastic neutron scattering has provided direct access to CF levels, which together with the magnetometry data, were employed to benchmark the ab initio results. The ab initio determined wave functions corresponding to the CF levels were in turn employed to assign the INS transitions allowed by selection rules and interpret the observed relative intensities of the INS peaks. Ultimately, we have been able to establish the relationship between the wave function composition of the CF split Ln ground multiplets and the experimentally measured magnetic and spectroscopic properties for the various analogs of the Na[Ln(WO)] family.

No abstract