Nanographene-Based Decoration as a Panchromatic Antenna for Metalloporphyrin Conjugates.
metalloporphyrins
nanographenes
organic solar cells
panchromatic
photocatalysis
redox
solar fuels
Journal
Small (Weinheim an der Bergstrasse, Germany)
ISSN: 1613-6829
Titre abrégé: Small
Pays: Germany
ID NLM: 101235338
Informations de publication
Date de publication:
Oct 2023
Oct 2023
Historique:
revised:
16
05
2023
received:
21
03
2023
medline:
17
6
2023
pubmed:
17
6
2023
entrez:
17
6
2023
Statut:
ppublish
Résumé
Porphyrins, a type of heterocyclic aromatic compounds consisting of tetrapyrroles connected by four substituted methine groups, are appealing building blocks for solar energy applications. However, their photosensitization capability is limited by their large optical energy gap, which results in a mismatch in absorption toward efficient harvesting of the solar spectrum. Porphyrin π-extension by edge-fusing with nanographenes can be employed for narrowing their optical energy gap from 2.35 to 1.08 eV, enabling the development of porphyrin-based panchromatic dyes with an optimized energy onset for solar energy conversion in dye-sensitized solar fuel and solar cell configurations. By combining time-dependent density functional theory with fs transient absorption spectroscopy, it is found that the primary singlets, which are delocalized across the entire aromatic part, are transferred into metal centred triplets in only 1.2 ps; and subsequently, relax toward ligand-delocalized triplets. This observation implies that the decoration of the porphyrin moiety with nanographenes, while having a large impact on the absorption onset of the novel dye, promotes the formation of a ligand-centred lowest triplet state of large spatial extension, potentially interesting for boosting interactions with electron scavengers. These results reveal a design strategy for broadening the applicability of porphyrin-based dyes in optoelectronics.
Identifiants
pubmed: 37329205
doi: 10.1002/smll.202301596
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
e2301596Subventions
Organisme : European Research Council
Pays : International
Informations de copyright
© 2023 Wiley-VCH GmbH.
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