Wang Yuanheng, Hait Diptarka, Johnson K Grace, Fajen O Jonathan, Zhang Juncheng Harry, Guerrero Rubén D, Martínez Todd J
Department of Chemistry and the PULSE Institute, Stanford University, Stanford, California 94305, USA.
SLAC National Accelerator Laboratory, Menlo Park, California 94024, USA.
J Chem Phys. 2024 Nov 7;161(17). doi: 10.1063/5.0233523.
The increasing availability of graphics processing units (GPUs) for scientific computing has prompted interest in accelerating quantum chemical calculations through their use. However, the complexity of integral kernels for high angular momentum basis functions often limits the utility of GPU implementations with large basis sets or for metal containing systems. In this work, we report the implementation of f function support in the GPU-accelerated TeraChem software package through the development of efficient kernels for the evaluation of Hamiltonian integrals. The high efficiency of the resulting code is demonstrated through density functional theory (DFT) calculations on increasingly large organic molecules and transition metal complexes, as well as coupled cluster singles and doubles calculations on water clusters. Preliminary investigations into Ni(I) catalysis with DFT and the photochemistry of MnH(CH3) with complete active space self-consistent field are also carried out. Overall, our GPU-accelerated software appears to be well-suited for fast simulation of large transition metal containing systems, as well as organic molecules.
用于科学计算的图形处理单元（GPU）日益普及，这引发了人们通过使用GPU来加速量子化学计算的兴趣。然而，高角动量基函数的积分内核的复杂性常常限制了在大基组或含金属体系中GPU实现的效用。在这项工作中，我们通过开发用于评估哈密顿积分的高效内核，报告了在GPU加速的TeraChem软件包中对f函数支持的实现。通过对越来越大的有机分子和过渡金属配合物进行密度泛函理论（DFT）计算，以及对水团簇进行耦合簇单双激发计算，证明了所得代码的高效率。还对Ni(I)催化的DFT和MnH(CH3)的完全活性空间自洽场光化学进行了初步研究。总体而言，我们的GPU加速软件似乎非常适合快速模拟大型含过渡金属体系以及有机分子。
