Adaptive density-guided approach to double incremental potential energy surface construction

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We present a combination of the recently developed double incremental expansion of potential energy surfaces with the well-established adaptive density-guided approach to grid construction. This unique methodology is based on the use of an incremental expansion for potential energy surfaces, known as n-mode expansion; an incremental many-body representation of the electronic energy; and an efficient vibrational density-guided approach to automated determination of grid dimensions and granularity. The reliability of the method is validated calculating potential energy surfaces and obtaining fundamental excitation energies for three moderate-size chain-like molecular systems. The use of our methodology leads to considerable computational savings for potential energy surface construction compared to standard approaches while maintaining a high level of accuracy in the resulting potential energy surfaces. Additional investigations indicate that our method can be applied to covalently bound and strongly interacting molecular systems, even though these cases are known to be very unfavorable for fragmentation schemes. We therefore conclude that the presented methodology is a robust and flexible approach to potential energy surface construction, which introduces considerable computational savings without compromising the accuracy of vibrational spectra calculations.
Original languageEnglish
Article number194105
JournalJournal of Chemical Physics
Publication statusPublished - May 2020

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