A footprint of zero-point entropy in higher-temperature magnetic thermodynamics

Abstract

Identifying extensively degenerate zero-temperature states is key in characterizing spin-liquid-candidate materials and spin ices. In experiments, finding zero-point entropy (ZPE) is often attempted by measuring the entropy released by a material when cooled down from very high to very low temperatures. Such investigations are often unreliable and lead to controversial results because accessible temperatures may be insufficient to accurately capture essential low- and high-temperature features of magnetic materials. The purpose of this paper is to point out a simple, easily accessible signature of nonzero ZPE: the Maxwell's relation $\left(\partial S/\partial H\right)_T = \left(\partial M/\partial T\right)_H$ can appear violated if a vanishing ZPE is assumed incorrectly. This relation can further be used for estimating the ZPE. In many materials below characteristic temperatures, the criterion of non-vanishing ZPE has a particularly simple form: $\left(\frac{\partial C}{\partial H}\right)_T\left(\frac{\partial M}{\partial T}\right)_H<0$. We discuss these effects and the ZPE signature in the benchmark test case of the well-studied spin ice $Dy_2Ti_2O_7$.