Enhanced deep-freezing magneto- and elasto-caloric effects by modifying lattice anharmonicity and electronic structures

Designing the high performance magneto or elastocaloric effect in NiMnIn alloys with spin-lattice coupling in a deep freezing temperature range of 200 K to 255 K is challenging due to the limited lattice entropy change and large negative contribution of magnetic entropy change during phase transitions. In this work, we systematically study the first order magneto-structural transition in NiMnIn based alloys by in-situ microstructural characterizations, physical property measurements, and first principles calculations. A multi element alloying strategy involving Cu and Ga co doping is proposed to manipulate the phase transition. The co doping reduces the lattice anharmonicity and thermal expansion coefficient of the martensitic phase, leading to an increase in the unit cell volume change and lattice entropy change. It also modifies the electronic density of states, causing a decrease in the magnetization change .The relief of the lattice mismatch reduces hysteresis losses in the refrigeration cycle. These synergetic effects yield excellent magneto and elastocaloric effects,with the effective magnetocaloric refrigeration capacity reaching up to 182 J/kg under the magnetic field of 5 T or an adiabatic temperature change of -4 K under a low field of 1.5 T and the elastocaloric coefficient of performance to 30 or an adiabatic temperature change of -7 K with the strain of 5% at 230 K, offering a potential solution for solid-state deep-freezing refrigeration.