Liu Jie, Hu Wei, Yang Jinlong
Hefei National Laboratory, University of Science and Technology of China, Hefei230088, China.
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui230026, China.
J Chem Theory Comput. 2022 Nov 8;18(11):6713-6721. doi: 10.1021/acs.jctc.2c00763. Epub 2022 Oct 15.
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 MoS consisting of 216 atoms and ∼1900 electrons with range-separated hybrid functionals on a single graphics processing unit.
我们提出了一种在平面波赝势框架内用于杂化泛函（hybrid-LR-TDDFT）的线性响应含时密度泛函理论的高效低秩实现方法。引入自适应压缩交换（ACE）算符和自然跃迁轨道（NTOs）来构建hybrid-LR-TDDFT哈密顿量中非局部交换算符的低秩表示。数值测试表明，ACE近似在不损失精度的情况下显著降低了应用非局部交换算符的计算成本，并且NTO近似通过引入一个NTO截止参数可以进一步加速hybrid-LR-TDDFT计算。这种新方法使我们能够在单个图形处理单元上有效地研究由216个原子和约1900个电子组成的二维MoS的激子性质，采用范围分离杂化泛函。
