Show simple item record

dc.contributor.authorZheng, Zilong
dc.contributor.authorTummala, Naga Rajesh
dc.contributor.authorFu, Yao-Tsung
dc.contributor.authorCoropceanu, Veaceslav
dc.contributor.authorBredas, Jean-Luc
dc.date.accessioned2017-05-23T09:30:36Z
dc.date.available2017-05-23T09:30:36Z
dc.date.issued2017-05-17
dc.identifier.citationZheng Z, Tummala NR, Fu Y-T, Coropceanu V, Brédas J-L (2017) Charge-Transfer States in Organic Solar Cells: Understanding the Impact of Polarization, Delocalization, and Disorder. ACS Applied Materials & Interfaces. Available: http://dx.doi.org/10.1021/acsami.7b02193.
dc.identifier.issn1944-8244
dc.identifier.issn1944-8252
dc.identifier.pmid28481497
dc.identifier.doi10.1021/acsami.7b02193
dc.identifier.urihttp://hdl.handle.net/10754/623702
dc.description.abstractWe investigate the impact of electronic polarization, charge delocalization, and energetic disorder on the charge-transfer (CT) states formed at a planar C60/pentacene interface. The ability to examine large complexes containing up to seven pentacene molecules and three C60 molecules allows us to take explicitly into account the electronic polarization effects. These complexes are extracted from a bilayer architecture modeled by molecular dynamics simulations and evaluated by means of electronic-structure calculations based on long-range-separated functionals (ωB97XD and BNL) with optimized range-separation parameters. The energies of the lowest charge-transfer states derived for the large complexes are in very good agreement with the experimentally reported values. The average singlet-triplet energy splittings of the lowest CT states are calculated not to exceed 10 meV. The rates of geminate recombination as well as of dissociation of the triplet excitons are also evaluated. In line with experiment, our results indicate that the pentacene triplet excitons generated through singlet fission can dissociate into separated charges on a picosecond time scale, despite the fact that their energy in C60/pentacene heterojunctions is slightly lower than the energies of the lowest CT triplet states.
dc.description.sponsorshipWe acknowledge the financial support of this work at the Georgia Institute of Technology by the Department of the Navy, Office of Naval Research, under the MURI “Center for Advanced Organic Photovoltaics” (Award Nos. N00014-14-1-0580 and N00014-16-1-2520) and by King Abdullah University of Science and Technology (V.C.). A KAUST competitive research funding and the Office of Naval Research – Global (Award No. N62909-15-1-2003) supported the work at King Abdullah University of Science and Technology.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttp://pubs.acs.org/doi/full/10.1021/acsami.7b02193
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/full/10.1021/acsami.7b02193.
dc.subjectOrganic Photovoltaics
dc.subjectCharge-transfer States
dc.subjectElectronic Couplings
dc.subjectPentacene-fullerene Blends
dc.subjectSinglet−triplet Energy Splitting
dc.subjectRange-separated Hybrid Functionals
dc.titleCharge-Transfer States in Organic Solar Cells: Understanding the Impact of Polarization, Delocalization, and Disorder
dc.typeArticle
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentLaboratory for Computational and Theoretical Chemistry of Advanced Materials
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Applied Materials & Interfaces
dc.eprint.versionPost-print
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology , Atlanta, Georgia 30332-0400, United States.
kaust.personBredas, Jean-Luc
refterms.dateFOA2018-05-08T00:00:00Z
dc.date.published-online2017-05-17
dc.date.published-print2017-05-31


Files in this item

Thumbnail
Name:
ACS-AMI-Ms-Clean-050417.pdf
Size:
1.326Mb
Format:
PDF
Description:
Accepted Manuscript
Thumbnail
Name:
ACS-AMI-SI-Revs2-050417.docx
Size:
6.334Mb
Format:
Microsoft Word 2007
Description:
Supporting Information

This item appears in the following Collection(s)

Show simple item record