Polymorphous density-functional description of paramagnetic phases of quantum magnets

The kernel of the study of magnetic quantum materials focuses on the magnetic phase transitions, among which the most common phenomenon is the transition between low-temperature magnetic-ordered phase to high-temperature paramagnetic phase. A paramount question is if such paramagnetic phase of the correlated solids can be well described by single-particle band theory to facilitate the experimental observations. In this work, we investigate the properties of temperature-driven paramagnetic phase via two different approaches within the framework of density functional theory, monomorphous and polymorphous description. From a comprehensive comparison of total energies, symmetries and band structures, we demonstrate the necessity for a proper treatment of paramagnetic phases with several prototypical examples. For Pauli paramagnetism phase, the vanishing of spin moments permits us to apply a nonmagnetic monomorphous description, while for paramagnetism with disordered local moments, such description imposes unrealistic high symmetry, leading to a metallic state in certain cases, inconsistent with the experimental observation. In contrast, the polymorphous description based on a large-enough supercell with disordered local moments is able to count in the effects of distinct local environments, such as symmetry lowing, providing a more reliable paramagnetic electronic structure and total energy compared with experiments. Our work shed new insights on discovering the temperature-dependent magnetic phase transition in the field of magnetic quantum materials.