Accelerating High-Pressure Simulations: Open-Source Implementation of the GOSTSHYP Model on GPUs

The Gaussians On Surface Tesserae Simulate HYdrostatic Pressure (GOSTSHYP) approach is a reliable method for calculating pressure-induced changes in molecular geometries, energies, electronic and spectroscopic properties, and reactivity. We present an open-source implementation of GOSTSHYP on Graphics Processing Units (GPUs) in the PySCF/GPU4PySCF program package, featuring energies and analytical nuclear gradients. With a rigorous spatial screening of the integrals and GPU kernels optimized in an agent-driven workflow, the GOSTSHYP terms take less than 1% of the self-consistent field time for systems with more than a few hundred atoms. Accordingly, high-pressure calculations come at essentially the cost of the corresponding calculations without pressure, as demonstrated for amylose chains with more than a thousand atoms and for the pressure-induced oligomerization of fullerene C 60 .