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The Role of Driving Energy and Delocalized States for Charge Separation in Organic Semiconductors

2012· article· en· 1,176 citations· W2098527861 on OpenAlex· 10.1126/science.1217745

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Abstract

The electron-hole pair created via photon absorption in organic photoconversion systems must overcome the Coulomb attraction to achieve long-range charge separation. We show that this process is facilitated through the formation of excited, delocalized band states. In our experiments on organic photovoltaic cells, these states were accessed for a short time (<1 picosecond) via infrared (IR) optical excitation of electron-hole pairs bound at the heterojunction. Atomistic modeling showed that the IR photons promote bound charge pairs to delocalized band states, similar to those formed just after singlet exciton dissociation, which indicates that such states act as the gateway for charge separation. Our results suggest that charge separation in efficient organic photoconversion systems occurs through hot-state charge delocalization rather than energy-gradient-driven intermolecular hopping.

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The record

Venue
Science
Topic
Organic Electronics and Photovoltaics
Field
Engineering
Canadian institutions
Funders
Engineering and Physical Sciences Research CouncilFonds De La Recherche Scientifique - FNRSCorpus Christi College, University of CambridgeNatural Sciences and Engineering Research Council of CanadaAlexander von Humboldt-StiftungNederlandse Organisatie voor Wetenschappelijk OnderzoekStichting voor Fundamenteel Onderzoek der Materie
Keywords
Delocalized electronExcitonPhotoinduced charge separationPicosecondExcited stateChemical physicsIntermolecular forceAtomic physicsElectronOrganic semiconductorMolecular physicsCharge carrierDissociation (chemistry)ChemistryMaterials scienceOptoelectronicsCondensed matter physicsPhysicsPhotocatalysisMoleculeQuantum mechanics
Has abstract in OpenAlex
yes