Ultrafast Symmetry-Breaking Charge Separation in Covalent Boron-Dipyrromethene Dimers Modulated by Coulombic and Charge Transfer Coupling
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Le résumé fourni par la source
To mimic the light capture and charge generation in natural light-harvesting systems, photoinduced symmetry-breaking charge separation (SBCS) in various multichromophoric systems has been widely investigated. Yet, the thermodynamic and kinetic constraints of SBCS hinder its further development and application. Therefore, a comprehensive understanding of the SBCS mechanism is still needed. Herein, photoinduced dynamics in a series of boron dipyrromethene (BODIPY) dimers were investigated by femtosecond time-resolved transient absorption spectroscopy and quantum chemical calculations. Two key criteria pertinent for ultrafast SBCS are unveiled: limited excitonic coupling and effective charge transfer (CT) coupling in excited-state geometry. The former establishes the thermodynamic foundation for SBCS, making the process thermodynamically feasible. Once this feasibility is established, enhancing CT coupling becomes critical as it enables the effective coupling between the environmental fluctuations (such as intramolecular nuclear motion and solvation) and CS reaction, which drives SBCS on a picosecond time scale. Our work highlights the ultrafast SBCS mechanism in multichromophoric systems, suggests the factors responsible for the ultrafast and complete CS, and thereby establishes a potential strategy for the design of optoelectronic materials.
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Le contrôle bibliographique ouvert
DOI retrouvé dans Crossref DOI retrouvé ; titre concordant.
- Titre Crossref
- Ultrafast Symmetry-Breaking Charge Separation in Covalent Boron-Dipyrromethene Dimers Modulated by Coulombic and Charge Transfer Coupling
- Date Crossref
- 29/12/2025
- Éditeur
- American Chemical Society (ACS)
- Type
- journal-article
Ce recoupement confirme des métadonnées liées au DOI. Il ne confirme ni la méthode ni les conclusions de l’étude, et il ne compte pas comme une seconde source scientifique indépendante.
Où se fait cette recherche
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Beijing University of Posts and Telecommunications pays non établi dans la noticeUniversité ou école supérieure
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State Key Laboratory of Information Photonics and Optical Communications pays non établi dans la noticeStructure de recherche
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Southern University of Science and Technology pays non établi dans la noticeUniversité ou école supérieure
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and School of Science State Key Laboratory of Information Photonic and Optical Communications pays non établi dans la noticeUniversité ou école supérieure
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Department of Materials Science and Engineering pays non établi dans la noticeInstitution
Beijing University of Posts and Telecommunications, State Key Laboratory of Information Photonics and Optical Communications et Southern University of Science and Technology, avec 2 autres affiliations.
Une affiliation ne permet pas de déduire la nationalité d’un auteur.