Combining low-cost electronic structure theory and low-cost parallel computing architecture.

ABSTRACT

The computational efficiency of low-cost electronic structure methods can be further improved by leveraging heterogenous computing architectures. The software package TeraChem has been developed since 2008 to make use of graphical processing units (GPUs), particularly their strong single-precision performance, for the acceleration of quantum chemical calculations. Here, we present the implementation of three low-cost methods, namely HF-3c, PBEh-3c, and the recently introduced ωB97X-3c. We show that these can benefit in terms of performance when combined with "consumer grade" GPUs by leveraging the mixed precision integral handling in TeraChem. The current limitation of the latter's GPU integral library is that Gaussian integrals only for functions with angular momentum l < 3 can be computed, which generally restricts the achievable accuracy in terms of the one-particle basis set. Particularly, the implementation of the ωB97X-3c method now enables higher accuracy with this setting which, in turn, provides the most efficient implementation accessible with consumer-grade hardware. We furthermore show that the implemented 3c methods can be combined with the hh-TDA formalism. This gives new and efficient low-cost multi-configurational excited states methods, which are benchmarked for the description of lowest vertical excitation energies in this work. All in all, the combination of these efficient electronic structure theory methods with affordable highly parallelized computing hardware provides an optimal computational and monetary cost to accuracy ratio.