Extending GPU-Accelerated Gaussian Integrals in the TeraChem Software Package to f Type Orbitals: Implementation and Applications

TL;DR

This paper extends GPU-accelerated quantum chemistry calculations in TeraChem to include f-type orbitals, enabling faster simulations of large organic and transition metal systems with demonstrated efficiency in DFT, CCSD, and CASSCF methods.

Contribution

The implementation of f orbital support in TeraChem's GPU kernels is a novel enhancement that improves computational speed for complex quantum chemical calculations.

Findings

Efficient GPU kernels for f orbital integrals were developed.

Demonstrated speedup in DFT and CCSD calculations on large molecules.

Application to transition metal systems and catalysis studies.

Abstract

The increasing availability of GPUs for scientific computing has prompted interest in accelerating quantum chemical calculations through their use. The complexity of integral kernels for high angular momentum basis functions however often limits the utility of GPU implementations with large basis sets or for metal containing systems. In this work, we report 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 (CCSD) calculations on water clusters. Preliminary investigations into Ni(I) catalysis with DFT and the photochemistry of MnH(CH$_3$) with complete active space self-consistent field (CASSCF) 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.