Giant magnetocaloric effect at low fields in triangular-lattice NdMgAl$_{11}$O$_{19}$

Abstract

Magnetic refrigeration in the sub-Kelvin regime requires refrigerant materials to retain a large magnetic entropy at low temperatures by suppressing magnetic ordering. Quantum spin liquids (QSLs), which evade long-range magnetic ordering while retaining strong quantum fluctuations to the lowest temperatures, therefore provide a promising platform for realizing high-performance magnetic refrigerants. Here, we investigate the magnetic ground state and the magnetocaloric effect of the hexaaluminate, NdMgAl$_{11}$O$_{19}$, in which the Nd$^{3+}$ ions form a network of triangular lattices. Magnetic susceptibility and specific heat measurements indicate a magnetically dynamic state down to 50~mK, consistent with a QSL state. Specific heat measurements further reveal substantial magnetic entropy retained below 50~mK. Quasi-adiabatic demagnetization measurements demonstrate a superior cooling performance of NdMgAl$_{11}$O$_{19}$, which can be cooled to 113~mK from 1.9~K by only a small magnetic field change of 2~T. The outstanding refrigeration performance is attributed to the persistent spin fluctuations associated with the QSL-like ground state, together with a large effective \textit{g} factor and the smallness of the exchange interactions along the easy-axis direction. This study demonstrates that frustration, combined with strong spin-orbit coupling and crystal-electric-field effect in the rare earth magnets provides a promising design principle for next-generation cryogenic magnetic refrigerants.