Charge Separation and Recombination at Polymer-Fullerene Heterojunctions: Delocalization and Hybridization Effects

The Journal of Physical Chemistry Letters
Gabriele D'AvinoDavid Beljonne

Abstract

We address charge separation and recombination in polymer/fullerene solar cells with a multiscale modeling built from accurate atomistic inputs and accounting for disorder, interface electrostatics and genuine quantum effects on equal footings. Our results show that bound localized charge transfer states at the interface coexist with a large majority of thermally accessible delocalized space-separated states that can be also reached by direct photoexcitation, thanks to their strong hybridization with singlet polymer excitons. These findings reconcile the recent experimental reports of ultrafast exciton separation ("hot" process) with the evidence that high quantum yields do not require excess electronic or vibrational energy ("cold" process), and show that delocalization, by shifting the density of charge transfer states toward larger effective electron-hole radii, may reduce energy losses through charge recombination.

References

Aug 6, 2009·Accounts of Chemical Research·Jean-Luc BrédasVeaceslav Coropceanu
Jan 13, 2010·Chemical Reviews·Tracey M Clarke, James R Durrant
Aug 10, 2010·Journal of the American Chemical Society·Jiye LeeTroy Van Voorhis
Aug 8, 2012·Proceedings of the National Academy of Sciences of the United States of America·Domenico Caruso, Alessandro Troisi
Dec 12, 2012·Nature Materials·G GranciniG Lanzani
Oct 22, 2013·Journal of the American Chemical Society·Hiroyuki Tamura, Irene Burghardt
Nov 19, 2013·Nature Materials·Koen VandewalAlberto Salleo
Jan 25, 2014·Journal of the American Chemical Society·Julien IdéClaudio Zannoni
Jan 28, 2014·Journal of the American Chemical Society·Brett M SavoieMark A Ratner
May 31, 2014·Science·Sarah Maria FalkeChristoph Lienau
Jul 22, 2014·Advanced Materials·Haibo Ma, Alessandro Troisi
Jul 23, 2014·Physical Chemistry Chemical Physics : PCCP·Frédéric CastetDavid Beljonne
Aug 8, 2014·Journal of the American Chemical Society·Alex J BarkerJustin M Hodgkiss
Sep 6, 2014·Journal of the American Chemical Society·Sean SweetnamMichael D McGehee
Apr 23, 2015·Journal of the American Chemical Society·Carl Poelking, Denis Andrienko
Jan 14, 2014·Journal of Chemical Theory and Computation·Guido RaosJulien Idé
Nov 20, 2015·Journal of Chemical Theory and Computation·Gabriele D'AvinoZoltán G Soos

❮ Previous
Next ❯

Citations

Aug 27, 2016·ACS Applied Materials & Interfaces·Riccardo VolpiMathieu Linares
Dec 28, 2016·Journal of the American Chemical Society·Patrick E HartnettMichael R Wasielewski
Mar 2, 2017·Journal of the American Chemical Society·Ti WangWai-Lun Chan
Apr 25, 2017·The Journal of Physical Chemistry Letters·Stavros AthanasopoulosAnna Köhler
May 10, 2017·ACS Applied Materials & Interfaces·Zilong ZhengJean-Luc Brédas
Sep 8, 2016·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Gabriele D'AvinoDavid Beljonne
Sep 29, 2018·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Tika R KafleWai-Lun Chan
Mar 21, 2017·Journal of Computational Chemistry·Riccardo Volpi, Mathieu Linares
Sep 23, 2019·The Journal of Chemical Physics·Takatoshi FujitaTakeo Hoshi
Mar 2, 2018·The Journal of Physical Chemistry Letters·Adam GluchowskiIvan Kassal
Sep 21, 2017·The Journal of Physical Chemistry Letters·Yun GengAlessandro Troisi
Dec 14, 2016·Chemical Reviews·Gordon J HedleyIfor D W Samuel
Mar 29, 2018·The Journal of Physical Chemistry. a·Takatoshi Fujita, Yuji Mochizuki
Oct 30, 2019·The Journal of Physical Chemistry Letters·Stavros AthanasopoulosAnna Köhler
Mar 19, 2019·Journal of the American Chemical Society·Flurin D EisnerJenny Nelson
Jan 9, 2019·Journal of the American Chemical Society·Elisa Collado-FregosoDieter Neher
Sep 14, 2021·The Journal of Physical Chemistry Letters·Shanika WanigasekaraWai-Lun Chan

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.