Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/5.0007615· OSTI ID:1647459
 [1];  [1];  [1];  [1];  [2];  [3];  [4];  [5];  [6];  [7];  [1]
  1. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. IBM, Yorktown Heights, NY (United States)
  3. NVIDIA, Santa Clara, CA (United States)
  4. Adobe, San Jose, CA (United States)
  5. Univ. of California, Berkeley, (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Intel Corporation, Santa Clara, CA (United States)
  7. Stanford Univ. School of Medicine, Stanford, CA (United States)

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. Finally, 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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); National Science Foundation (NSF)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1647459
Alternate ID(s):
OSTI ID: 1633117
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 22 Vol. 152; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (90)

On the Calculation of Polycenter Integrals journal January 1969
Two-electron integral evaluation on the graphics processor unit journal January 2007
Acceleration of the GAMESS-UK electronic structure package on graphical processing units journal May 2011
Improvements on the direct SCF method: Improved Direct SCF Method journal January 1989
Exploiting graphical processing units to enable quantum chemistry calculation of large solvated molecules with conductor-like polarizable continuum models journal October 2018
Simplifications in the generation and transformation of two-electron integrals in molecular calculations journal October 1977
On the applicability of LCAO-Xα methods to molecules containing transition metal atoms: The nickel atom and nickel hydride journal January 1977
Electron correlation theories and their application to the study of simple reaction potential surfaces journal November 1978
Many-body perturbation theory, coupled-pair many-electron theory, and the importance of quadruple excitations for the correlation problem journal November 1978
Spin-restricted ensemble-referenced Kohn-Sham method: basic principles and application to strongly correlated ground and excited states of molecules journal November 2014
Psi4: an open-source ab initio electronic structure program : Psi4: an electronic structure program
  • Turney, Justin M.; Simmonett, Andrew C.; Parrish, Robert M.
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 4 https://doi.org/10.1002/wcms.93
journal October 2011
A new method for large-scale Cl calculations journal August 1972
On the Beebe-Linderberg two-electron integral approximation journal December 1986
Use of approximate integrals in ab initio theory. An application in MP2 energy calculations journal June 1993
Integral approximations for LCAO-SCF calculations journal October 1993
Libxc: A library of exchange and correlation functionals for density functional theory journal October 2012
FPGA acceleration of a quantum Monte Carlo application journal May 2008
Compressed sensing and Cholesky decomposition on FPGAs and GPUs journal August 2012
Molecular integrals Over Gaussian Basis Functions book January 1994
Ab Initio Nonadiabatic Quantum Molecular Dynamics journal February 2018
TeraChem Cloud: A High-Performance Computing Service for Scalable Distributed GPU-Accelerated Electronic Structure Calculations journal April 2020
Tensor Hypercontraction Second-Order Møller–Plesset Perturbation Theory: Grid Optimization and Reaction Energies journal June 2015
Quantum Chemistry for Solvated Molecules on Graphical Processing Units Using Polarizable Continuum Models journal June 2015
Ab Initio Interactive Molecular Dynamics on Graphical Processing Units (GPUs) journal September 2015
Nanoscale Multireference Quantum Chemistry: Full Configuration Interaction on Graphical Processing Units journal September 2015
Automated Code Engine for Graphical Processing Units: Application to the Effective Core Potential Integrals and Gradients journal December 2015
Automated Discovery and Refinement of Reactive Molecular Dynamics Pathways journal January 2016
“Balancing” the Block Davidson–Liu Algorithm journal June 2016
Hybrid CPU/GPU Integral Engine for Strong-Scaling Ab Initio Methods journal June 2017
Arbitrary Angular Momentum Electron Repulsion Integrals with Graphical Processing Units: Application to the Resolution of Identity Hartree–Fock Method journal June 2017
A Robust and Accurate Tight-Binding Quantum Chemical Method for Structures, Vibrational Frequencies, and Noncovalent Interactions of Large Molecular Systems Parametrized for All spd-Block Elements ( Z = 1–86) journal April 2017
An Ab Initio Exciton Model Including Charge-Transfer Excited States journal July 2017
Robust and Efficient Spin Purification for Determinantal Configuration Interaction journal August 2017
Nonadiabatic Ab Initio Molecular Dynamics with the Floating Occupation Molecular Orbital-Complete Active Space Configuration Interaction Method journal December 2017
P si 4N um P y : An Interactive Quantum Chemistry Programming Environment for Reference Implementations and Rapid Development journal May 2018
Simulating Electron Dynamics of Complex Molecules with Time-Dependent Complete Active Space Configuration Interaction journal June 2018
Large-Scale Electron Correlation Calculations: Rank-Reduced Full Configuration Interaction journal June 2018
GFN2-xTB—An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions journal January 2019
Efficient Treatment of Large Active Spaces through Multi-GPU Parallel Implementation of Direct Configuration Interaction journal January 2020
Ab Initio Multiple Spawning Photochemical Dynamics of DMABN Using GPUs journal December 2016
GPU-Accelerated State-Averaged Complete Active Space Self-Consistent Field Interfaced with Ab Initio Multiple Spawning Unravels the Photodynamics of Provitamin D 3 journal June 2016
Nonadiabatic Photodynamics of Retinal Protonated Schiff Base in Channelrhodopsin 2 journal May 2019
Ab Initio Nonadiabatic Dynamics of Multichromophore Complexes: A Scalable Graphical-Processing-Unit-Accelerated Exciton Framework journal July 2014
Arbitrary-Order Density Functional Response Theory from Automatic Differentiation journal May 2010
Coupled Cluster Theory on Graphics Processing Units I. The Coupled Cluster Doubles Method journal April 2011
Dynamic Precision for Electron Repulsion Integral Evaluation on Graphical Processing Units (GPUs) journal March 2011
Excited-State Electronic Structure with Configuration Interaction Singles and Tamm–Dancoff Time-Dependent Density Functional Theory on Graphical Processing Units journal May 2011
Semiempirical Quantum Chemical Calculations Accelerated on a Hybrid Multicore CPU–GPU Computing Platform journal June 2012
Generating Efficient Quantum Chemistry Codes for Novel Architectures journal November 2012
Acceleration of Electron Repulsion Integral Evaluation on Graphics Processing Units via Use of Recurrence Relations journal December 2012
Parametrization and Benchmark of DFTB3 for Organic Molecules journal November 2012
Acceleration of High Angular Momentum Electron Repulsion Integrals and Integral Derivatives on Graphics Processing Units journal March 2015
Quantum Chemistry on Graphical Processing Units. 1. Strategies for Two-Electron Integral Evaluation journal January 2008
Accelerating Density Functional Calculations with Graphics Processing Unit journal July 2008
Quantum Chemistry on Graphical Processing Units. 2. Direct Self-Consistent-Field Implementation journal March 2009
Quantum Chemistry on Graphical Processing Units. 3. Analytical Energy Gradients, Geometry Optimization, and First Principles Molecular Dynamics journal August 2009
Uncontracted Rys Quadrature Implementation of up to G Functions on Graphical Processing Units journal February 2010
Toward a systematic molecular orbital theory for excited states journal January 1992
First-Principles Characterization of the Elusive I Fluorescent State and the Structural Evolution of Retinal Protonated Schiff Base in Bacteriorhodopsin journal October 2019
Optimizing Conical Intersections without Derivative Coupling Vectors:  Application to Multistate Multireference Second-Order Perturbation Theory (MS-CASPT2) journal January 2008
Ab Initio Quantum Chemistry for Protein Structures journal October 2012
Tensor Hypercontraction Equation-of-Motion Second-Order Approximate Coupled Cluster: Electronic Excitation Energies in O(N4) Time journal July 2013
Charge Transfer and Polarization in Solvated Proteins from Ab Initio Molecular Dynamics journal June 2011
Discovering chemistry with an ab initio nanoreactor journal November 2014
The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction journal April 2019
Atomistic non-adiabatic dynamics of the LH2 complex with a GPU-accelerated ab initio exciton model journal January 2017
Coulombic potential energy integrals and approximations journal May 1973
On some approximations in applications of X α theory journal October 1979
A full coupled‐cluster singles and doubles model: The inclusion of disconnected triples journal February 1982
Fully optimized contracted Gaussian basis sets of triple zeta valence quality for atoms Li to Kr journal April 1994
The integral‐direct coupled cluster singles and doubles model journal March 1996
Tensor hypercontraction density fitting. I. Quartic scaling second- and third-order Møller-Plesset perturbation theory journal July 2012
Tensor hypercontraction. II. Least-squares renormalization journal December 2012
Communication: Tensor hypercontraction. III. Least-squares tensor hypercontraction for the determination of correlated wavefunctions journal December 2012
Quartic scaling second-order approximate coupled cluster singles and doubles via tensor hypercontraction: THC-CC2 journal March 2013
Communication: Acceleration of coupled cluster singles and doubles via orbital-weighted least-squares tensor hypercontraction journal May 2014
An atomic orbital-based formulation of the complete active space self-consistent field method on graphical processing units journal June 2015
Efficient implementation of effective core potential integrals and gradients on graphical processing units journal July 2015
Atomic orbital-based SOS-MP2 with tensor hypercontraction. I. GPU-based tensor construction and exploiting sparsity journal May 2016
Atomic orbital-based SOS-MP2 with tensor hypercontraction. II. Local tensor hypercontraction journal January 2017
A direct-compatible formulation of the coupled perturbed complete active space self-consistent field equations on graphical processing units journal May 2017
Analytical derivatives of the individual state energies in ensemble density functional theory method. I. General formalism journal July 2017
Analytical gradients for tensor hyper-contracted MP2 and SOS-MP2 on graphical processing units journal October 2017
Reduced scaling CASPT2 using supporting subspaces and tensor hyper-contraction journal July 2018
Density-fitted singles and doubles coupled cluster on graphics processing units journal January 2014
The atomic simulation environment—a Python library for working with atoms journal June 2017
Electronic wave functions - I. A general method of calculation for the stationary states of any molecular system journal February 1950
Diffractive imaging of dissociation and ground-state dynamics in a complex molecule journal August 2019
Self-consistent-charge density-functional tight-binding method for simulations of complex materials properties journal September 1998
Graphical Processing Units for Quantum Chemistry journal November 2008

Similar Records

TeraChem: A graphical processing unit-accelerated electronic structure package for large-scale ab initio molecular dynamics
Journal Article · Sun Jul 26 00:00:00 EDT 2020 · Wiley Interdisciplinary Reviews: Computational Molecular Science · OSTI ID:1656582

SQMBox: Interfacing a semiempirical integral library to modular ab initio electronic structure enables new semiempirical methods
Journal Article · Mon Feb 20 23:00:00 EST 2023 · Journal of Chemical Physics · OSTI ID:1989354

Tensor-decomposition techniques for ab initio nuclear structure calculations: From chiral nuclear potentials to ground-state energies
Journal Article · Mon Mar 18 00:00:00 EDT 2019 · Physical Review. C · OSTI ID:1566691