An Expressway towards Heaven: High-Throughput Hybrid Density Functional Theory for Complex Condensed-Phase Systems Containing Thousands of Atoms using SeA

By climbing the five rungs of Jacob's ladder, the Density Functional Theory (DFT) hierarchy approaches the "heaven" of chemical accuracy needed for accurate and reliable modeling of complex materials. In particular, fourth-rung hybrid functionals can provide semi-quantitative accuracy, and have therefore been used to gain a fundamental understanding of important gas-phase systems and reactive processes. However, such hybrid DFT based applications remain rare for large-scale condensed-phase systems due to the prohibitive computational cost associated with evaluating the exact-exchange (EXX) interaction in periodic systems. In this work, we provide an accurate, efficient, and robust algorithmic framework for performing high-throughput hybrid DFT calculations for large-scale finite-gap condensed-phase systems containing thousands of atoms. The resulting SeA approach (SeA = SCDM+exx+ACE) seamlessly integrates three recent theoretical developments, including orbital localization via the non-iterative selected columns of the density matrix (SCDM) method, a black-box linear-scaling EXX solver (exx), and the adaptively compressed exchange (ACE) operator. By harnessing three levels of computational savings, SeA performs hybrid DFT based calculations at an overall time-to-solution comparable to second-rung GGA functionals (i.e., the computational workhorse for condensed-phase systems). We showcase the capabilities of SeA to treat a wide range of condensed-phase systems—without the need for system-dependent parameters—including molecular crystals, aqueous solutions, interfaces, and highly porous materials.