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Résumé
The theoretically disclosed, and experimentally confirmed, energy inversion of the lowest singlet (S1) and triplet (T1) excited states of organic molecules (i.e., Hund’s rule violation) is investigated herein with the aid of modern and nonempirically derived double-hybrid (DH) density functionals, in the search of the best trade-off between accuracy and computational cost of viable electronic structure methods. For that purpose, we have selected a family of parameter-free expressions differing in their specific formulation (DFT-0DH, DFT-QIDH, DFT0-2, SOS1-DFT-0DH, SOS1-DFT-QIDH, SOS1-DFT0-2, RSX-DFT-0DH, RSX-DFT-QIDH, SOS1-RSX-DFT-0DH, and SOS1-RSX-DFT-QIDH) as well as in the underlying exchange-correlation functional used (PBE vs r2SCAN). For the sake of evaluating which DH can correctly describe the singlet-triplet excited-state energy inversion, second-order approximate with singles and doubles method with a spin-component scaling (SCS-CC2) and equation-of-motion coupled cluster singles and doubles (EOM-CCSD) calculations are also carried out. The results highlight the importance of the delicate balance between all the energy terms composing DH density functionals, with the correlation part being particularly significant for achieving the most accurate results. We have also derived a new DH density functional (PBE-DH-INVEST) exploiting that relationship, providing low error metrics and expected to yield robust results in, e.g., high-throughput studies.
langue originale | Anglais |
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Pages (de - à) | 18313-18327 |
Nombre de pages | 15 |
journal | Journal of Physical Chemistry C |
Volume | 128 |
Numéro de publication | 43 |
Les DOIs | |
Etat de la publication | Publié - 31 oct. 2024 |
Empreinte digitale
Examiner les sujets de recherche de « Searching the Best Double-Hybrid Density Functional to Correctly Predict the Singlet-Triplet Excited-State Inversion in Organic Systems ». Ensemble, ils forment une empreinte digitale unique.Projets
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Renouvellement d’équipements pour le Consortium des Equipements de Calcul Intensif (CECI)
Bontempi, G. (Responsable du Projet), CHAMPAGNE, B. (CoPI), Geuzaine , C. (CoPI), RIGNANESE, G. M. (CoPI) & Lazzaroni, R. (CoPI)
1/01/22 → 31/12/23
Projet: Recherche
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IMAGINE: Influence des effets MAGgnétiques sur la conversion de spIN dans les matériaux organiques pi-conjugués émetteurs de lumière : Développement d’une approche de modélisation multiéchelle atomistique
Olivier, Y. (Responsable du Projet)
1/01/21 → 1/12/22
Projet: Recherche
Équipement
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Plateforme Technologique Calcul Intensif
Champagne, B. (!!Manager)
Plateforme technologique Calcul intensifEquipement/installations: Plateforme technolgique