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An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings

Author(s)
Pavanello, Michele; Van Voorhis, Troy; Visscher, Lucas; Neugebauer, Johannes
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Abstract
Quantum–mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlap matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Ångstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.
Date issued
2013-02
URI
http://hdl.handle.net/1721.1/82590
Department
Massachusetts Institute of Technology. Department of Chemistry
Journal
The Journal of Chemical Physics
Publisher
American Institute of Physics (AIP)
Citation
Pavanello, Michele, Troy Van Voorhis, Lucas Visscher, and Johannes Neugebauer. “An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings.” The Journal of Chemical Physics 138, no. 5 (2013): 054101. © 2013 American Institute of Physics
Version: Final published version
ISSN
00219606
1089-7690

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