QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water
We have investigated the reaction of peroxynitrite with carbon dioxide in aqueous solution by means of combined quantum-classical (QM-MM) molecular dynamics simulations. In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussian basis set, and the solvent was descr...
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| Acceso en línea: | http://hdl.handle.net/20.500.12110/paper_15499618_v3_n4_p1405_GonzalezLebrero |
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todo:paper_15499618_v3_n4_p1405_GonzalezLebrero2023-10-03T16:23:19Z QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water González Lebrero, M.C. Estrin, D.A. We have investigated the reaction of peroxynitrite with carbon dioxide in aqueous solution by means of combined quantum-classical (QM-MM) molecular dynamics simulations. In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussian basis set, and the solvent was described using the mean-field TIP4P force field. The free energy profile of this reaction has been computed using umbrella sampling and multiple steering molecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much more efficient than MSMD schemes, due to the possibility of employing a combination of classical and QM-MM thermalization schemes. We found the presence of a significant barrier in the free energy profile associated with the reaction in solution, which is not present in vacuum, that may be ascribed to the significant charge redistribution upon reaction and the concomitant solvation pattern changes. © 2007 American Chemical Society. Fil:González Lebrero, M.C. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Estrin, D.A. 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_15499618_v3_n4_p1405_GonzalezLebrero |
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Universidad de Buenos Aires |
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I-28 |
| repository_str |
R-134 |
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Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| description |
We have investigated the reaction of peroxynitrite with carbon dioxide in aqueous solution by means of combined quantum-classical (QM-MM) molecular dynamics simulations. In our QM-MM scheme, the reactant was modeled using density functional theory with a Gaussian basis set, and the solvent was described using the mean-field TIP4P force field. The free energy profile of this reaction has been computed using umbrella sampling and multiple steering molecular dynamics (MSMD) schemes. Umbrella sampling methods turned out to be much more efficient than MSMD schemes, due to the possibility of employing a combination of classical and QM-MM thermalization schemes. We found the presence of a significant barrier in the free energy profile associated with the reaction in solution, which is not present in vacuum, that may be ascribed to the significant charge redistribution upon reaction and the concomitant solvation pattern changes. © 2007 American Chemical Society. |
| format |
JOUR |
| author |
González Lebrero, M.C. Estrin, D.A. |
| spellingShingle |
González Lebrero, M.C. Estrin, D.A. QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| author_facet |
González Lebrero, M.C. Estrin, D.A. |
| author_sort |
González Lebrero, M.C. |
| title |
QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| title_short |
QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| title_full |
QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| title_fullStr |
QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| title_full_unstemmed |
QM-MM investigation of the reaction of peroxynitrite with carbon dioxide in water |
| title_sort |
qm-mm investigation of the reaction of peroxynitrite with carbon dioxide in water |
| url |
http://hdl.handle.net/20.500.12110/paper_15499618_v3_n4_p1405_GonzalezLebrero |
| work_keys_str_mv |
AT gonzalezlebreromc qmmminvestigationofthereactionofperoxynitritewithcarbondioxideinwater AT estrinda qmmminvestigationofthereactionofperoxynitritewithcarbondioxideinwater |
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1807319942575423488 |