Realistic first-principles calculations of the magnetocaloric effect: applications to hcp Gd

We present an efficient computational approach to evaluate field-dependent entropy of magnetocaloric materials from ab-initio methods. The temperature dependence is reported for the entropy change, specific heat and magnetization for hcp Gd. To obtain optimal accuracy in the calculations, a mixed-scheme for magnetic Monte Carlo simulations is proposed and found to be superior to using pure quantum or classic statistics. It is demonstrated that lattice and magnetic contributions play a role in the entropy change and that the dominating contribution comes from the magnetic contribution. The total calculated entropy change agrees with measurements at room temperature. IMPACT STATEMENT Demonstration of the accuracy of ab-initio theory, coupled to statistical methods, for accurate calculations of the total entropy variation associated with the magnetic transition of Gd. Reproduction of experimental data of entropy change.

Automated summary

The study presents an efficient computational approach for evaluating the entropy change of magnetocaloric materials, with a focus on hcp Gd. It demonstrates the importance of the mixed-scheme for magnetic Monte Carlo simulations and highlights the dominant contribution of magnetism to the entropy change. The calculated total entropy change is in agreement with experimental measurements at room temperature.