Giant Magnetocaloric Effect in a Honeycomb Spiral Spin-Liquid Candidate

Abstract

Unlike conventional magnetic states, which lack degeneracy, the spiral spin liquid (SSL) fluctuates among degenerate spiral configurations, with ground-state wave vectors forming a continuous contour or surface in reciprocal space. At low temperatures, the field-induced crossover from the polarized ferromagnetic state to the SSL results in a large entropy increase and decalescence, indicating its potential for magnetic cooling. However, magnetic cooling using a SSL has yet to be reported. Here, we investigate the magnetocaloric effect and cooling performance of single-crystal GdZnPO, a spin-7/2 honeycomb-lattice SSL candidate, under a magnetic field $H$ $<$ $H_\mathrm{c}$ ($\mu_0H_\mathrm{c}$ $\sim$ 12 T) applied perpendicular to the honeycomb plane and below the crossover temperature ($\sim$2 K). For $H$ $\geq$ $H_\mathrm{c}$, GdZnPO enters a polarized non-degenerate ferromagnetic state. Our results demonstrate that GdZnPO exhibits a giant low-temperature magnetocaloric effect near $H_\mathrm{c}$, surpassing other magnetocaloric materials. This giant magnetocaloric effect is well-explained by the frustrated honeycomb spin model of GdZnPO, suggesting the stability of the SSL below $H_\mathrm{c}$ down to very low temperatures. Additionally, its magnetic cooling performance remains robust up to at least 4.5 K, making GdZnPO a promising candidate for magnetic refrigeration down to $\sim$36 mK through cycling the applied magnetic field within a narrow range.