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dc.contributor.author
Provasi, Patricio Federico
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dc.contributor.author
Modesto Costa, Lucas
dc.contributor.author
Sampaio, Felipe
dc.contributor.author
Silva, Tércio
dc.contributor.author
da Cunha, Antônio R.
dc.contributor.author
Andrade Filho, Tarciso
dc.contributor.author
Gester, Rodrigo
dc.date.available
2023-11-30T13:41:35Z
dc.date.issued
2023-01
dc.identifier.citation
Provasi, Patricio Federico; Modesto Costa, Lucas; Sampaio, Felipe; Silva, Tércio; da Cunha, Antônio R.; et al.; The Importance of the Density Functional Theory Exchange-Correlation Hartree-Fock Term in Magnetic Resonance: Application to an Aqueous Environment; American Chemical Society; Journal of Physical Chemistry A; 127; 3; 1-2023; 619-626
dc.identifier.issn
1089-5639
dc.identifier.uri
http://hdl.handle.net/11336/218891
dc.description.abstract
Within the framework of Density Functional Theory (DFT), the relevance of the term Hartree-Fock exchange (HFE) for a variety of molecular properties is a critical point. For this reason, we spend efforts to understand these relationships in nuclear magnetic resonance (NMR) parameters in a water solvent. This work takes advantage of the appropriate aug-cc-pVTZ-J basis set and the Minnesota family of DFT methods, which consider different portions of HFE contributions. With regard to solvent participation, the results are based on a sequential Monte Carlo/Quantum Mechanics procedure, which builds the structures of the liquid under realistic thermodynamic conditions. Compared to the accurate results of second-order polarization propagator approximation (SOPPA) and experimental data, all NMR parameters show a huge dependence on the size of the HFE contribution. For instance, the inclusion of this term in 1JOH and 2JHH indirect spin-spin couplings does vary with 49.661 and 25.459 Hz, respectively. The M06-HF method accounts for 100% of HFE and better matches the σO and σH shielding constants. On the other hand, 1JOH and 2JHH demand a medium contribution (54% of HFE), the best description being associated with the M06-2X method. Thus, the dependence varies regarding the phenomenology of the property in focus and the order for independent treatments. For elements that participate in hydrogen bonds simultaneously as donor and acceptor actors, the results indicate that explicit solvent molecules must be considered in the quantum mechanical calculations for better modeling of paramagnetic shielding constants.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
American Chemical Society
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dc.rights
info:eu-repo/semantics/restrictedAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
RMN
dc.subject
Solvent effect
dc.subject
Hartree–Fock exchange term
dc.subject
Explicit solvent molecules
dc.subject.classification
Física Atómica, Molecular y Química
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dc.subject.classification
Ciencias Físicas
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dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
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dc.title
The Importance of the Density Functional Theory Exchange-Correlation Hartree-Fock Term in Magnetic Resonance: Application to an Aqueous Environment
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2023-11-29T13:23:22Z
dc.journal.volume
127
dc.journal.number
3
dc.journal.pagination
619-626
dc.journal.pais
Estados Unidos
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dc.journal.ciudad
Washington
dc.description.fil
Fil: Provasi, Patricio Federico. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Modelado e Innovación Tecnológica. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Modelado e Innovación Tecnológica; Argentina
dc.description.fil
Fil: Modesto Costa, Lucas. Universidade Federal Rural do Rio de Janeiro; Brasil. Instituto Militar de Engenharia; Brasil. Universidade Federal do Sul e Sudeste do Pará; Brasil
dc.description.fil
Fil: Sampaio, Felipe. Universidade Federal do Sul e Sudeste do Pará; Brasil
dc.description.fil
Fil: Silva, Tércio. Universidade do Estado do Pará; Brasil
dc.description.fil
Fil: da Cunha, Antônio R.. Universidade Federal Do Maranhão; Brasil
dc.description.fil
Fil: Andrade Filho, Tarciso. Universidade Federal do Sul e Sudeste do Pará; Brasil
dc.description.fil
Fil: Gester, Rodrigo. Universidade Federal do Sul e Sudeste do Pará; Brasil
dc.journal.title
Journal of Physical Chemistry A
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dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpca.2c05623
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/acs.jpca.2c05623
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