Exceptional Magnetocaloric Responses in a Gadolinium Silicate with Strongly Correlated Spin Disorder for Sub-Kelvin Magnetic Cooling

The development of magnetocaloric materials with a significantly enhanced volumetric cooling capability is highly desirable for the application of adiabatic demagnetization refrigerators in confined spatial environments. Here, the thermodynamic characteristics of a magnetically frustrated spin-7/2 Gd9.33[SiO4]6O2 is presented, which exhibits strongly correlated spin disorder below approximate to 1.5 K. A quantitative model is proposed to describe the magnetization results by incorporating nearest-neighbor Heisenberg antiferromagnetic and dipolar interactions. Remarkably, the recorded magnetocaloric responses are unprecedentedly large and applicable below 1.0 K. It is proposed that the S = 7/2 spin liquids serve as versatile platforms for investigating high-performance magnetocaloric materials in the sub-kelvin regime, particularly those exhibiting a superior cooling power per unit volume. It is hereby presented that the thermodynamic properties of a magnetically frustrated spin-7/2 silicate exhibiting strongly correlated spin disorder, which provides promising platforms for investigating magnetocaloric materials with an enhanced volumetric cooling capacity, particularly those suitable for sub-kelvin temperature applications. image