Nonequilibrium Thermodynamics of Charge Separation in Organic Solar Cells

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dc.citation.issue27
dc.citation.rankM21a
dc.citation.spage6389
dc.citation.volume12
dc.contributor.authorKaiser, Waldemar
dc.contributor.authorJanković, Veljko
dc.contributor.authorVukmirović, Nenad
dc.contributor.authorGagliardi, Alessio
dc.date.accessioned2024-06-13T13:51:37Z
dc.date.available2024-06-13T13:51:37Z
dc.date.issued2021-07-07
dc.description.abstractThis work presents a novel theoretical description of the nonequilibrium thermodynamics of charge separation in organic solar cells (OSCs). Using stochastic thermodynamics, we take realistic state populations derived from the phonon-assisted dynamics of electron-hole pairs within photoexcited organic bilayers to connect the kinetics with the free energy profile of charge separation. Hereby, we quantify for the first time the difference between nonequilibrium and equilibrium free energy profile. We analyze the impact of energetic disorder and delocalization on free energy, average energy, and entropy. For a high disorder, the free energy profile is well-described as equilibrated. We observe significant deviations from equilibrium for delocalized electron-hole pairs at a small disorder, implying that charge separation in efficient OSCs proceeds via a cold but nonequilibrated pathway. Both a large Gibbs entropy and large initial electron-hole distance provide an efficient charge separation, while a decrease in the free energy barrier does not necessarily enhance charge separation
dc.identifier.doi10.1021/acs.jpclett.1c01817.s001
dc.identifier.issn1948-7185
dc.identifier.scopus2-s2.0-85111225401
dc.identifier.urihttps://pub.ipb.ac.rs/handle/123456789/91
dc.identifier.wos000674852100020
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.ispartofThe Journal of Physical Chemistry Letters
dc.relation.ispartofabbrJ. Phys. Chem. Lett.
dc.rightsrestrictedAccess
dc.titleNonequilibrium Thermodynamics of Charge Separation in Organic Solar Cells
dc.typeArticle
dc.type.versionpublishedVersion
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