Abstract
In this paper, we propose an improved excitation generation algorithm for the full configuration interaction quantum Monte Carlo method, which is particularly effective in systems described by localized orbitals. The method is an extension of the precomputed heat-bath strategy of Holmes et al., with more effective sampling of double excitations and a novel approach for nonuniform sampling of single excitations. We demonstrate the effectiveness of the algorithm for a chain of 30 hydrogen atoms with atom-localized orbitals, a stack of benzene molecules, and an Fe(II)-porphyrin model complex, whereby we show an overall efficiency gain by a factor of two to four, as measured by variance reduction per wall-clock time.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
