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Charge Generation via Relaxed Charge-Transfer States in Organic Photovoltaics by an Energy-Disorder-Driven Entropy Gain
Linköpings universitet, Institutionen för fysik, kemi och biologi, Ytors Fysik och Kemi. Linköpings universitet, Tekniska fakulteten.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.
Linköpings universitet, Institutionen för fysik, kemi och biologi. Linköpings universitet, Tekniska fakulteten.
Linköpings universitet, Institutionen för fysik, kemi och biologi, Biomolekylär och Organisk Elektronik. Linköpings universitet, Tekniska fakulteten.ORCID-id: 0000-0002-2582-1740
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2018 (engelsk)Inngår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, nr 24, s. 12640-12646Artikkel i tidsskrift (Fagfellevurdert) Published
Abstract [en]

In organic photovoltaics, efficient charge generation relies on our ability to convert excitons into free charges. Efficient charge separation from "energetic excitons" has been understood to be governed by delocalization effects promoted by molecular aggregation. A remaining puzzle is, however, the mechanism underlying charge generation via relaxed interfacial charge-transfer (CT) excitons that also exhibit an internal quantum efficiency close to unity. Here, we provide evidence for efficient charge generation via CT state absorption over a temperature range of 50-300 K, despite an intrinsically strong Coulomb binding energy of about 400 meV that cannot be modified by fullerene aggregation. We explain our observation by entropy-driven charge separation, with a key contribution from energy disorder. The energy disorder reduces the charge generation barrier by substantially gaining the entropy as electron hole distance increases, resulting in efficient CT exciton dissociation. Our results underline an emerging consideration of energy disorder in thermodynamic stability of charge pairs and highlight the energy disorder as a dominant factor for generating charges via the CT state. A discussion for a trade-off in harvesting charges from relaxed CT excitons is also provided.

sted, utgiver, år, opplag, sider
AMER CHEMICAL SOC , 2018. Vol. 122, nr 24, s. 12640-12646
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URN: urn:nbn:se:liu:diva-149714DOI: 10.1021/acs.jpcc.8b03432ISI: 000436381600008OAI: oai:DiVA.org:liu-149714DiVA, id: diva2:1234397
Merknad

Funding Agencies|Swedish Research Council [VR-2015-00436]; Wallenberg Scholar grant; Knut and Alice Wallenberg Foundation [KAW 2014.0041]

Tilgjengelig fra: 2018-07-24 Laget: 2018-07-24 Sist oppdatert: 2018-07-24

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