Excited-State Electronic Structure with Configuration Interaction Singles and Tamm–Dancoff Time-Dependent Density Functional Theory on Graphical Processing Units
Autor: | Christine M. Isborn, Todd J. Martínez, Nathan Luehr, Ivan S. Ufimtsev |
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Rok vydání: | 2011 |
Předmět: |
Chemistry
Ab initio Electronic structure Time-dependent density functional theory Chromophore Configuration interaction Molecular physics Article Computer Science Applications Computational chemistry Excited state Density functional theory Physics::Chemical Physics Physical and Theoretical Chemistry Excitation |
Zdroj: | Journal of Chemical Theory and Computation |
ISSN: | 1549-9626 1549-9618 |
Popis: | Excited-state calculations are implemented in a development version of the GPU-based TeraChem software package using the configuration interaction singles (CIS) and adiabatic linear response Tamm-Dancoff time-dependent density functional theory (TDA-TDDFT) methods. The speedup of the CIS and TDDFT methods using GPU-based electron repulsion integrals and density functional quadrature integration allows full ab initio excited-state calculations on molecules of unprecedented size. CIS/6-31G and TD-BLYP/6-31G benchmark timings are presented for a range of systems, including four generations of oligothiophene dendrimers, photoactive yellow protein (PYP), and the PYP chromophore solvated with 900 quantum mechanical water molecules. The effects of double and single precision integration are discussed, and mixed precision GPU integration is shown to give extremely good numerical accuracy for both CIS and TDDFT excitation energies (excitation energies within 0.0005 eV of extended double precision CPU results). |
Databáze: | OpenAIRE |
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