A quantum-mechanics molecular-mechanics scheme for extended systems
We introduce and discuss a hybrid quantum-mechanics molecular-mechanics (QM-MM) approach for Car-Parrinello DFT simulations with pseudopotentials and planewaves basis, designed for the treatment of periodic systems. In this implementation the MM atoms are considered as additional QM ions having frac...
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todo:paper_09538984_v28_n33_p_Hunt2023-10-03T15:51:32Z A quantum-mechanics molecular-mechanics scheme for extended systems Hunt, D. Sanchez, V.M. Scherlis, D.A. DFT intefaces molecular dynamics QM-MM Condensed matter physics Dimers Machinery Mechanics Molecular dynamics Molecular mechanics Quantum theory Titanium dioxide Aqueous environment Condensed matter system intefaces Molecular dynamics simulations Periodic boundary conditions QM-MM Solid-liquid interfaces Vibrational dynamics Phase interfaces We introduce and discuss a hybrid quantum-mechanics molecular-mechanics (QM-MM) approach for Car-Parrinello DFT simulations with pseudopotentials and planewaves basis, designed for the treatment of periodic systems. In this implementation the MM atoms are considered as additional QM ions having fractional charges of either sign, which provides conceptual and computational simplicity by exploiting the machinery already existing in planewave codes to deal with electrostatics in periodic boundary conditions. With this strategy, both the QM and MM regions are contained in the same supercell, which determines the periodicity for the whole system. Thus, while this method is not meant to compete with non-periodic QM-MM schemes able to handle extremely large but finite MM regions, it is shown that for periodic systems of a few hundred atoms, our approach provides substantial savings in computational times by treating classically a fraction of the particles. The performance and accuracy of the method is assessed through the study of energetic, structural, and dynamical aspects of the water dimer and of the aqueous bulk phase. Finally, the QM-MM scheme is applied to the computation of the vibrational spectra of water layers adsorbed at the TiO2 anatase (1 0 1) solid-liquid interface. This investigation suggests that the inclusion of a second monolayer of H2O molecules is sufficient to induce on the first adsorbed layer, a vibrational dynamics similar to that taking place in the presence of an aqueous environment. The present QM-MM scheme appears as a very interesting tool to efficiently perform molecular dynamics simulations of complex condensed matter systems, from solutions to nanoconfined fluids to different kind of interfaces. © 2016 IOP Publishing Ltd. Fil:Hunt, D. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Sanchez, V.M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_09538984_v28_n33_p_Hunt |
| institution |
Universidad de Buenos Aires |
| institution_str |
I-28 |
| repository_str |
R-134 |
| collection |
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| topic |
DFT intefaces molecular dynamics QM-MM Condensed matter physics Dimers Machinery Mechanics Molecular dynamics Molecular mechanics Quantum theory Titanium dioxide Aqueous environment Condensed matter system intefaces Molecular dynamics simulations Periodic boundary conditions QM-MM Solid-liquid interfaces Vibrational dynamics Phase interfaces |
| spellingShingle |
DFT intefaces molecular dynamics QM-MM Condensed matter physics Dimers Machinery Mechanics Molecular dynamics Molecular mechanics Quantum theory Titanium dioxide Aqueous environment Condensed matter system intefaces Molecular dynamics simulations Periodic boundary conditions QM-MM Solid-liquid interfaces Vibrational dynamics Phase interfaces Hunt, D. Sanchez, V.M. Scherlis, D.A. A quantum-mechanics molecular-mechanics scheme for extended systems |
| topic_facet |
DFT intefaces molecular dynamics QM-MM Condensed matter physics Dimers Machinery Mechanics Molecular dynamics Molecular mechanics Quantum theory Titanium dioxide Aqueous environment Condensed matter system intefaces Molecular dynamics simulations Periodic boundary conditions QM-MM Solid-liquid interfaces Vibrational dynamics Phase interfaces |
| description |
We introduce and discuss a hybrid quantum-mechanics molecular-mechanics (QM-MM) approach for Car-Parrinello DFT simulations with pseudopotentials and planewaves basis, designed for the treatment of periodic systems. In this implementation the MM atoms are considered as additional QM ions having fractional charges of either sign, which provides conceptual and computational simplicity by exploiting the machinery already existing in planewave codes to deal with electrostatics in periodic boundary conditions. With this strategy, both the QM and MM regions are contained in the same supercell, which determines the periodicity for the whole system. Thus, while this method is not meant to compete with non-periodic QM-MM schemes able to handle extremely large but finite MM regions, it is shown that for periodic systems of a few hundred atoms, our approach provides substantial savings in computational times by treating classically a fraction of the particles. The performance and accuracy of the method is assessed through the study of energetic, structural, and dynamical aspects of the water dimer and of the aqueous bulk phase. Finally, the QM-MM scheme is applied to the computation of the vibrational spectra of water layers adsorbed at the TiO2 anatase (1 0 1) solid-liquid interface. This investigation suggests that the inclusion of a second monolayer of H2O molecules is sufficient to induce on the first adsorbed layer, a vibrational dynamics similar to that taking place in the presence of an aqueous environment. The present QM-MM scheme appears as a very interesting tool to efficiently perform molecular dynamics simulations of complex condensed matter systems, from solutions to nanoconfined fluids to different kind of interfaces. © 2016 IOP Publishing Ltd. |
| format |
JOUR |
| author |
Hunt, D. Sanchez, V.M. Scherlis, D.A. |
| author_facet |
Hunt, D. Sanchez, V.M. Scherlis, D.A. |
| author_sort |
Hunt, D. |
| title |
A quantum-mechanics molecular-mechanics scheme for extended systems |
| title_short |
A quantum-mechanics molecular-mechanics scheme for extended systems |
| title_full |
A quantum-mechanics molecular-mechanics scheme for extended systems |
| title_fullStr |
A quantum-mechanics molecular-mechanics scheme for extended systems |
| title_full_unstemmed |
A quantum-mechanics molecular-mechanics scheme for extended systems |
| title_sort |
quantum-mechanics molecular-mechanics scheme for extended systems |
| url |
http://hdl.handle.net/20.500.12110/paper_09538984_v28_n33_p_Hunt |
| work_keys_str_mv |
AT huntd aquantummechanicsmolecularmechanicsschemeforextendedsystems AT sanchezvm aquantummechanicsmolecularmechanicsschemeforextendedsystems AT scherlisda aquantummechanicsmolecularmechanicsschemeforextendedsystems AT huntd quantummechanicsmolecularmechanicsschemeforextendedsystems AT sanchezvm quantummechanicsmolecularmechanicsschemeforextendedsystems AT scherlisda quantummechanicsmolecularmechanicsschemeforextendedsystems |
| _version_ |
1807317422611365888 |