Optimization and Parallelization of DFT and TDDFT in GAMESS on DoD HPC Machines

The quantum chemistry package General Atomic and Molecular Electronic Structure System (GAMESS) is employed in the first-principles modeling of complex molecular systems by using the density functional theory (DFT) as well as a number of other post-Hartree-Fock (HF) methods. Both DFT and time-dependent DFT (TDDFT) are of particular interest to the Department of Defense (DoD) Computational Biology, Chemistry, and Materials Science (CCM). Millions of CPU hours per year are expended by GAMESS calculations on DoD high performance computing (HPC) systems. Therefore, any reduction in wall-clock time for these calculations will represent a significant saving in CPU hours. As part of this work, three areas for improvement were identified: 1) replacement of the exchange-correlation (XC) integration grid, 2) TDDFT parallelization, and 3) profiling and optimization of the DFT and TDDFT. We summarize the work performed in these task areas and present the resulting speed-up. Our software enhancements are available to the general public in the 11APR2008R1 version of GAMESS.

[1]  V. I. Lebedev,et al.  Spherical quadrature formulas exact to orders 25–29 , 1977 .

[2]  G. Scuseria,et al.  An efficient implementation of time-dependent density-functional theory for the calculation of excitation energies of large molecules , 1998 .

[3]  C. W. Murray,et al.  Quadrature schemes for integrals of density functional theory , 1993 .

[4]  E. Gross,et al.  Density-Functional Theory for Time-Dependent Systems , 1984 .

[5]  P. Hohenberg,et al.  Inhomogeneous Electron Gas , 1964 .

[6]  V. Barone,et al.  Recent advances in density functional methods , 1995 .

[7]  M. E. Casida.  Time-Dependent Density Functional Response Theory for Molecules , 1995 .

[8]  Benny G. Johnson,et al.  A standard grid for density functional calculations , 1993 .

[9]  Kimihiko Hirao,et al.  Excited state geometry optimizations by analytical energy gradient of long-range corrected time-dependent density functional theory. , 2006, The Journal of chemical physics.

[10]  V. Lebedev,et al.  A QUADRATURE FORMULA FOR THE SPHERE OF THE 131ST ALGEBRAIC ORDER OF ACCURACY , 1999 .

[11]  Michael F. Herman,et al.  Nonadiabatic surface hopping Herman-Kluk semiclassical initial value representation method revisited: applications to Tully's three model systems. , 2005, The Journal of chemical physics.

[12]  Filipp Furche,et al.  Adiabatic time-dependent density functional methods for excited state properties , 2002 .

[13]  A. Becke.  A multicenter numerical integration scheme for polyatomic molecules , 1988 .

[14]  Mark S. Gordon,et al.  General atomic and molecular electronic structure system , 1993, J. Comput. Chem..

[15]  Kimihiko Hirao,et al.  An efficient state-specific scheme of time-dependent density functional theory , 2006 .

[16]  V. I. Lebedev,et al.  Quadratures on a sphere , 1976 .

[17]  Michel Dupuis,et al.  Implementation of solvent reaction fields for electronic structure , 2002 .