Low-rank approximations for accelerating plane-wave hybrid functional calculations in unrestricted and noncollinear...

The adaptively compressed exchange (ACE) operator combined with interpolative separable density fitting (ISDF) decomposition has been utilized to accelerate plane-wave hybrid functional calculations for restricted Kohn-Sham density functional theory (DFT), but the neglect of spin degree of freedom has limited its application in the exploration of systems where the spin property of the electron is critical. Herein, we derive the ACE-ISDF formulation for hybrid functional calculations in both unrestricted and noncollinear spin DFT with plane waves and periodic boundary conditions. We proposed an improved ISDF algorithm for the sum of Kohn-Sham orbital pairs to further reduce the computational cost for the spin-noncollinear case. Numerical results demonstrate that these improved ACE-ISDF low-rank approximations can not only significantly reduce the computational time by two orders of magnitude compared with conventional plane-wave hybrid functional calculations but also lead to a good convergence behavior when a moderate rank parameter is set, even for complex periodic magnetic systems. By using these ACE-ISDF approximations, we investigate the electronic and magnetic properties of two-dimensional periodic ferromagnetic semiconductors consisting of triangular zigzag graphene quantum dots and transition metal atoms. Our computational results showcase that hybrid functional calculations in spin DFT can provide not only accurate electronic structures but also accurate magnetic order temperature of ferromagnetic semiconductors compared to local or semilocal functional calculations.