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Verfasst von:Han, Jie [VerfasserIn]   i
 Rehn, Dirk R. [VerfasserIn]   i
 Buckup, Tiago [VerfasserIn]   i
 Dreuw, Andreas [VerfasserIn]   i
Titel:Evaluation of single-reference DFT-based approaches for the calculation of spectroscopic signatures of excited states involved in singlet fission
Verf.angabe:Jie Han, Dirk Robert Rehn, Tiago Buckup, and Andreas Dreuw
E-Jahr:2020
Jahr:September 21, 2020
Umfang:15 S.
Fussnoten:Gesehen am 17.11.2020
Titel Quelle:Enthalten in: The journal of physical chemistry <Washington, DC> / A
Ort Quelle:Washington, DC : Soc., 1997
Jahr Quelle:2020
Band/Heft Quelle:124(2020), 41, Seite 8446-8460
ISSN Quelle:1520-5215
Abstract:Singlet fission (SF) has the potential to dramatically increase solar cell efficiency by converting one singlet exciton to two free triplet excitons via a correlated triplet pair intermediate. Identification and characterization of excited states involved in SF are of great importance for understanding the fundamentals of SF. Despite their importance, it is still nontrivial to distinguish various species in transient absorption spectra due to their spectral overlaps and ultrashort lifetimes. Theoretical modeling of SF and its electronically excited state absorption (ESA) is generally challenging due to the multiexciton nature of the correlated triplet pair, which usually requires description by expensive high-level ab initio methods. In this work, taking the bis((triisopropylsilyl)ethynyl) (TIPS)-pentacene monomer and its covalently linked dimer as representative examples, we demonstrate the use of single-reference DFT-based approaches to simulate the ESA spectra during SF. In particular, the singlet and triplet ESA are evaluated by TDDFT, QR-TDDFT, SLR-TDDFT, SF-TDDFT, and UTDDFT, in combination with ten different exchange-correlation functionals. The correlated triplet pair and its ESA are characterized by broken-symmetry DFT and TDDFT, and the role of orbital relaxation is highlighted. With a rational choice of exchange-correlation functionals, we found the resulting spectra to show good agreement with transient absorption experiments and certain improvements over high-order CI methods.
DOI:doi:10.1021/acs.jpca.0c07236
URL:Bitte beachten Sie: Dies ist ein Bibliographieeintrag. Ein Volltextzugriff für Mitglieder der Universität besteht hier nur, falls für die entsprechende Zeitschrift/den entsprechenden Sammelband ein Abonnement besteht oder es sich um einen OpenAccess-Titel handelt.

Volltext ; Verlag ; Resolving-System: https://doi.org/10.1021/acs.jpca.0c07236
 Volltext: https://pubs.acs.org/doi/10.1021/acs.jpca.0c07236
 DOI: https://doi.org/10.1021/acs.jpca.0c07236
Datenträger:Online-Ressource
Sprache:eng
K10plus-PPN:173889598X
Verknüpfungen:→ Zeitung

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