Woo Jeheon, Kim Woo Youn, Choi Sunghwan
Department of Chemistry, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.
National Institute of Supercomputing and Networking, Korea Institute of Science and Technology Information, Daejeon 34141, Republic of Korea.
J Chem Theory Comput. 2022 May 10;18(5):2875-2884. doi: 10.1021/acs.jctc.1c01263. Epub 2022 Apr 18.
For fast density functional calculations, a suitable basis that can accurately represent the orbitals within a reasonable number of dimensions is essential. Here, we propose a new type of basis constructed from Tucker decomposition of a finite-difference (FD) Hamiltonian matrix, which is intended to reflect the system information implied in the Hamiltonian matrix and satisfies orthonormality and separability conditions. By introducing the system-specific separable basis, the computation time for FD density functional calculations for seven two- and three-dimensional periodic systems was reduced by a factor of 2-71 times, while the errors in both the atomization energy per atom and the band gap were limited to less than 0.1 eV. The accuracy and speed of the density functional calculations with the proposed basis can be systematically controlled by adjusting the rank size of Tucker decomposition.
对于快速密度泛函计算，一个能够在合理维度数量内准确表示轨道的合适基组至关重要。在此，我们提出一种由有限差分（FD）哈密顿矩阵的塔克分解构建的新型基组，其旨在反映哈密顿矩阵中隐含的系统信息，并满足正交归一性和可分离性条件。通过引入特定于系统的可分离基组，七个二维和三维周期系统的FD密度泛函计算的计算时间减少了2至71倍，而每个原子的原子化能和带隙的误差均限制在小于0.1 eV以内。使用所提出基组的密度泛函计算的准确性和速度可以通过调整塔克分解的秩大小来系统地控制。
