Accelerating Linear-Response Time-Dependent Hybrid Density Functional Theory with Low-Rank Decomposition Techniques in the Plane-Wave Basis.

Abstract

We present an efficient low-rank implementation of linear-response time-dependent density functional theory for hybrid functionals (hybrid-LR-TDDFT) within the plane-wave pseudopotential framework. The adaptively compressed exchange (ACE) operator and the natural transition orbitals (NTOs) are introduced to build the low-rank representation of the nonlocal exchange operator in the hybrid-LR-TDDFT Hamiltonian. Numerical tests demonstrate that the ACE approximation significantly reduces the computational cost of applying the nonlocal exchange operator without loss of accuracy, and the NTO approximation can further accelerate the hybrid-LR-TDDFT calculations by introducing an NTO cutoff parameter. This new method enables us to effectively study the excitonic properties of two-dimensional MoS2 consisting of 216 atoms and ∼1900 electrons with range-separated hybrid functionals on a single graphics processing unit.