Open AccessNanoscale Multireference Quantum Chemistry: Full Configuration Interaction on Graphical Processing Units
Author(s) -
B. Scott Fales,
Benjamin G. Levine
Publication year - 2015
Publication title -
journal of chemical theory and computation
Language(s) - Uncategorized
Resource type - Journals
SCImago Journal Rank - 2.001
H-Index - 185
eISSN - 1549-9626
pISSN - 1549-9618
DOI - 10.1021/acs.jctc.5b00634
Subject(s) - atomic orbital , basis set , excited state , hamiltonian (control theory) , computational science , chemical space , configuration interaction , chemistry , electron , nanotechnology , computer science , molecule , physics , atomic physics , quantum mechanics , materials science , drug discovery , mathematical optimization , biochemistry , mathematics
Methods based on a full configuration interaction (FCI) expansion in an active space of orbitals are widely used for modeling chemical phenomena such as bond breaking, multiply excited states, and conical intersections in small-to-medium-sized molecules, but these phenomena occur in systems of all sizes. To scale such calculations up to the nanoscale, we have developed an implementation of FCI in which electron repulsion integral transformation and several of the more expensive steps in σ vector formation are performed on graphical processing unit (GPU) hardware. When applied to a 1.7 × 1.4 × 1.4 nm silicon nanoparticle (Si72H64) described with the polarized, all-electron 6-31G** basis set, our implementation can solve for the ground state of the 16-active-electron/16-active-orbital CASCI Hamiltonian (more than 100,000,000 configurations) in 39 min on a single NVidia K40 GPU.