Performance of the AMOEBA Water Model in the Vicinity of QM Solutes: A Diagnosis Using Energy Decomposition Analysis - Publikacja - MOST Wiedzy

Wyszukiwarka

Performance of the AMOEBA Water Model in the Vicinity of QM Solutes: A Diagnosis Using Energy Decomposition Analysis

Abstrakt

The importance of incorporating solvent polarization effects into the modeling of solvation processes has been well-recognized, and therefore a new generation of hybrid quantum mechanics/molecular mechanics (QM/MM) approaches that accounts for this effect is desirable. We present a fully self-consistent, mutually polarizable QM/MM scheme using the AMOEBA force field, in which the total energy of the system is variationally minimized with respect to both the QM electronic density and the MM induced dipoles. This QM/AMOEBA model is implemented through the Q-Chem/LibEFP code interface and then applied to the evaluation of solute-solvent interaction energies for various systems ranging from the smallest water dimer to neutral and ionic solutes (NH3-, NH4+, CN-) surrounded by increasing numbers (up to 100) of water molecules. In order to analyze the obtained interaction energies, we also utilize an energy decomposition analysis (EDA) scheme which identifies contributions from permanent electrostatics, polarization and van der Waals (vdW) interaction for the interaction between the QM solute and the solvent molecules described by AMOEBA. This facilitates a component-wise comparison against the full QM references where the corresponding energy components are obtained via a modified version of the absolutely localized molecular orbitals (ALMO)-EDA. The results show that the present QM/AMOEBA model can yield reasonable solute-solvent interaction energies for neutral and cationic species, which, however, highly relies on the delicate balance between insufficiently favorable permanent electrostatics and softened vdW interaction. For anionic solutes where the charge penetration effect becomes more pronounced, the QM/MM interface turns out to be unbalanced. These results are consistent with and further elucidate our findings in a previous study using a slightly different QM/AMOEBA model (J. Chem. Phys. 145, 124106 (2016)), and the implications on future improvement of this model are also discussed.

Cytowania

  • 2 3

    CrossRef

  • 2 1

    Web of Science

  • 2 1

    Scopus

Autorzy (6)

Cytuj jako

Pełna treść

pełna treść publikacji nie jest dostępna w portalu

Słowa kluczowe

Informacje szczegółowe

Kategoria:
Publikacja w czasopiśmie
Typ:
artykuł w czasopiśmie wyróżnionym w JCR
Opublikowano w:
Journal of Chemical Theory and Computation nr 13, strony 1963 - 1979,
ISSN: 1549-9618
Język:
angielski
Rok wydania:
2017
Opis bibliograficzny:
Mao Y., Shao Y., Dziedzic J., Skylaris C., Head-Gordon T., Head-Gordon M.: Performance of the AMOEBA Water Model in the Vicinity of QM Solutes: A Diagnosis Using Energy Decomposition Analysis// Journal of Chemical Theory and Computation. -Vol. 13, nr. 5 (2017), s.1963-1979
DOI:
Cyfrowy identyfikator dokumentu elektronicznego (otwiera się w nowej karcie) 10.1021/acs.jctc.7b00089
Weryfikacja:
Politechnika Gdańska

wyświetlono 17 razy

Publikacje, które mogą cię zainteresować

Meta Tagi