dc.contributor.author | Choluj, Marta | |
dc.contributor.author | Alam, Mehboob | |
dc.contributor.author | Beerepoot, Maarten T. P. | |
dc.contributor.author | Sitkiewicz, Sebastian P. | |
dc.contributor.author | Matito Gras, Eduard | |
dc.contributor.author | Ruud, Kenneth | |
dc.contributor.author | Zaleśny, Robert | |
dc.date.accessioned | 2022-02-10T11:13:15Z | |
dc.date.available | 2022-02-10T11:13:15Z | |
dc.date.issued | 2022-02-08 | |
dc.identifier.citation | Journal of chemical theory and computation 18(2) : 1046-1060 (2022) | es_ES |
dc.identifier.issn | 1549-9626 | |
dc.identifier.uri | http://hdl.handle.net/10810/55415 | |
dc.description.abstract | We present a benchmark study of density functional approximation (DFA) performances in predicting the two-photon-absorption strengths in pi-conjugated molecules containing electron-donating/-accepting moieties. A set of 48 organic molecules is chosen for this purpose, for which the two-photon-absorption (2PA) parameters are evaluated using different DFAs, including BLYP, PBE, B3LYP, PBE0, CAM-B3LYP, LC-BLYP, and optimally tuned LC-BLYP. Minnesota functionals and omegaB97X-D are also used, applying the two-state approximation, for a subset of molecules. The efficient resolution-of-identity implementation of the coupled-cluster CC2 model (RI-CC2) is used as a reference for the assessment of the DFAs. Two-state models within the framework of both DFAs and RI-CC2 are used to gain a deeper insight into the performance of different DFAs. Our results give a clear picture of the performance of the density functionals in describing the two-photon activity in dipolar pi-conjugated systems. The results show that global hybrids are best suited to reproduce the absolute values of 2PA strengths of donor-acceptor molecules. The range-separated functionals CAM-B3LYP and optimally tuned LC-BLYP, however, show the highest linear correlations with the reference RI-CC2 results. Hence, we recommend the latter DFAs for structure-property studies across large series of dipolar compounds. | es_ES |
dc.description.sponsorship | M.C. and R.Z. gratefully acknowledge support from the National
Science Centre, Poland (Grant 2018/30/E/ST4/00457).
M.M.A. acknowledges support from the Indian Institute of
Technology Bhilai, India, through a Research Initiation Grant
(IITBhilai/D/2258). M.T.P.B. and K.R. acknowledge support
from the Research Council of Norway through a Centre of
Excellence Grant (Grant 262695), and E.M. and S.P.S.
acknowledge funding from the Spanish Ministry of Science
(Grants MCIN/AEI/10.13039/501100011033, PGC2018-
098212-B-C21,EUR2019-103825 and "FEDER Una manera
de hacer Europa") and the Basque Government/Eusko
Jaurlaritza (GV/EJ) (Grants IT1254-19, PIBA19-0004, and 2019-CIEN-000092-01 and PRE_2020_2_0015). The authors
thank Lizaveta Petrusevich for the preparation of the table of
contents graphic. Computational resources generously provided
by the Wrocław Center for Networking and Supercomputing are
also acknowledged. | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | American Chemical Society | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICINN/PGC2018- 098212-B-C21 | es_ES |
dc.rights | info:eu-repo/semantics/openAccess | es_ES |
dc.rights.uri | http://creativecommons.org/licenses/by/3.0/es/ | * |
dc.title | Choosing Bad versus Worse: Predictions of Two-Photon-Absorption Strengths Based on Popular Density Functional Approximations | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.rights.holder | 2022 The Authors. Published by American Chemical Society. Attribution 4.0 International (CC BY 4.0) | es_ES |
dc.rights.holder | Atribución 3.0 España | * |
dc.relation.publisherversion | https://pubs.acs.org/doi/10.1021/acs.jctc.1c01056 | es_ES |
dc.identifier.doi | 10.1021/acs.jctc.1c01056 | |
dc.departamentoes | Polímeros y Materiales Avanzados: Física, Química y Tecnología | es_ES |
dc.departamentoeu | Polimero eta Material Aurreratuak: Fisika, Kimika eta Teknologia | es_ES |