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Quantum Mechanics/Extremely Localized Molecular Orbital Method: A Fully Quantum Mechanical Embedding Approach for Macromolecules

Cite this: J. Phys. Chem. A 2019, 123, 43, 9420–9428
Publication Date (Web):September 20, 2019
https://doi.org/10.1021/acs.jpca.9b08882
Copyright © 2019 American Chemical Society

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    Abstract

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    The development of methods for the quantum mechanical study of macromolecules has always been an important challenge in theoretical chemistry. Nowadays, the techniques proposed in this context can be used to investigate very large systems and can be subdivided into two main categories: fragmentation and embedding strategies. In this paper, by modifying and improving the local self-consistent field approach originally proposed for quantum mechanics/molecular mechanics techniques, we introduce the new multiscale embedding quantum mechanics/extremely localized molecular orbital (QM/ELMO) method. The new strategy enables treatment of chemically relevant regions of large biological molecules through usual methods of quantum chemistry while describing the remaining parts of the systems by means of frozen extremely localized molecular orbitals transferred from properly constructed libraries. Test calculations have shown the correct functioning and the high reliability of the new approach, thus anticipating its possible applications to different fields of physical chemistry, such as rational drug design and structural refinements of proteins.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpca.9b08882.

    • Details about all the performed computations, details about extremely localized molecular orbitals and their libraries (with Figure S1 showing plots of ELMOs), details about all the similarity indexes used to compare the obtained molecular electron densities and electrostatic potentials, Table S1 reporting the Hartree–Fock and QM/ELMO energy values resulting from the test calculations performed on Trp45 in the α-helix and β-sheet conformations, Tables S2 and S3 showing the Hartree–Fock and QM/ELMO energy differences between the conformations of the Ser100 and Trp45 homopeptides, Table S4 reporting the computational cost of the Hartree–Fock and QM/ELMO calculations carried out on Trp45, and Table S5 providing the list of all the residues included in the quantum mechanical (high-level) regions (QM1 and QM2) for the QM/ELMO (ONIOM) calculations performed on the protein:ligand complex (PDF)

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