Highly Efficient, Linear-Scaling Seminumerical Exact-Exchange Method for Graphic Processing Units


Henryk Laqua, Travis H. Thompson, Jörg Kussmann, Christian Ochsenfeld

J. Chem. Theory Comput., 2020, 16, 3, 1456–1468


We present a highly efficient and asymptotically linear-scaling graphic processing unit accelerated seminumerical exact-exchange method (sn-LinK). We go beyond our previous central processing unit-based method (Laqua, H.; Kussmann, J.; Ochsenfeld, C. J. Chem. Theory Comput. 2018, 14, 3451−3458) by employing our recently developed integral bounds (Thompson, T. H.; Ochsenfeld, C. J. Chem. Phys. 2019, 150, 044101) and high-accuracy numerical integration grid (Laqua, H.; Kussmann, J.; Ochsenfeld, C. J. Chem. Phys. 2018, 149, 204111). The accuracy is assessed for several established test sets, providing errors significantly below 1mEh for the smallest grid. Moreover, a comprehensive performance analysis for large molecules between 62 and 1347 atoms is provided, revealing the outstanding performance of our method, in particular, for large basis sets such as the polarized quadruple-zeta level with diffuse functions.