TeraChem: Accelerating electronic structure and ab initio molecular dynamics with graphical processing units

Abstract

Developed over the past decade, TeraChem is an electronic structure and ab initio molecular dynamics software package designed from the ground up to leverage graphics processing units (GPUs) to perform large-scale ground and excited state quantum chemistry calculations in the gas and the condensed phase. TeraChem’s speed stems from the reformulation of conventional electronic structure theories in terms of a set of individually optimized high-performance electronic structure operations (e.g., Coulomb and exchange matrix builds, one- and two-particle density matrix builds) and rank-reduction techniques (e.g., tensor hypercontraction). Recent efforts have encapsulated these core operations and provided language-agnostic interfaces. This greatly increases the accessibility and flexibility of TeraChem as a platform to develop new electronic structure methods on GPUs and provides clear optimization targets for emerging parallel computing architectures.

Resolving the ultrafast dynamics of the anionic green fluorescent protein chromophore in water

“…79 Electronic structure calculations were performed with TeraChem. [80][81][82][83][84] Solvated initial conditions. A Boltzmann sampling procedure provided initial conditions (ICs) for the solvated chromophore.…”

Extended tight‐binding quantum chemistry methods

“…In this respect, in 2017 GFN1‐xTB filled a gap in the market of off‐the‐shelf atomistic models as it is fast, robust, reasonably accurate, and works for many metallic systems. It was quickly adapted by the community and implemented in various QC programs like AMS, 18 CP2K, 19 Cuby4, 20 DFTB+, 21 entos, 22 ORCA, 23,24 and TeraChem 25,26 …”

PyUNIxMD: A Python‐based excited state molecular dynamics package

“…QM_calculator class provides interfaces to various external (or internal, for simple model calculations) QM programs. PyUNIxMD supports complete active space self-consistent field (CASSCF) in Columbus 69 and Molpro, 33 multireference configuration interaction (MRCI) in Columbus, timedependent density-functional theory (TDDFT) in Gaussian 09 70 and Q-Chem, 32 state-interaction state-averaged spin-restricted ensemble Kohn-Sham (SSR) in TeraChem, 71 Depending on the availability of NACVs calculations, PyUNIxMD supports Ehrenfest and CTMQC dynamics. For example, NACVs can be calculated with CASSCF or SSR method.…”