Ising Supercriticality and Universal Magnetocalorics in Spiral Antiferromagnet Nd$_3$BWO$_9$

Abstract

The celebrated analogy between the pressure-temperature phase diagram of a liquid-gas system and the field-temperature phase diagram of a ferromagnet has long been a cornerstone for understanding universality of phase transitions and critical phenomena. Here we extend this analogy to a highly frustrated antiferromagnet, the spiral Ising compound Nd$_3$BWO$_9$ with kagome layers. In its phase diagram, we identify a metamagnetic transition line with a critical endpoint (CEP) located at $μ_0H_{\mathrm{c}} \simeq 1.04$ T and $T_{\mathrm{c}} \simeq 0.3$ K. Above the CEP, an Ising supercritical regime emerges with crossover lines that follow a universal scaling law, as evidenced by the specific heat, magnetic susceptibility, and magnetocaloric measurements. Remarkably, we observe highly sensitive magnetic cooling near the emergent CEP, characterized by a divergent magnetic Grüneisen ratio $Γ_H \propto 1/t^{β+γ-1}$, with $β+ γ\simeq 1.563$ the sum of critical exponents of the 3D Ising universality class and $t \equiv (T-T_{\rm c})/T_{\rm c}$ the reduced temperature. Adiabatic demagnetization from 2 K and 4 T reaches a minimum temperature of 195 mK, via a self-cascading process that combines supercritical and topological cooling. Our findings open a new avenue for studying supercritical phenomena and magnetic refrigeration with the frustrated rare-earth compounds RE$_3$BWO$_9$ and, more broadly, in Ising-anisotropic antiferromagnets such as spin ices.