Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics

Abstract Efficient delocalization of photo-generated excitons is a key to improving the charge-separation efficiencies in state-of-the-art organic photovoltaic (OPV) absorber. While the delocalization in non-fullerene acceptors has been widely studied, we expand the scope by studying the properties...

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Main Authors: Kui Jiang, Robert J. E. Westbrook, Tian Xia, Cheng Zhong, Jianxun Lu, Azzaya Khasbaatar, Kaikai Liu, Francis R. Lin, Sei-Hum Jang, Jie Zhang, Yuqing Li, Ying Diao, Zhanhua Wei, Hin-Lap Yip, David S. Ginger, Alex K.-Y. Jen
Format: Article
Language:English
Published: Nature Portfolio 2025-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-58352-x
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author Kui Jiang
Robert J. E. Westbrook
Tian Xia
Cheng Zhong
Jianxun Lu
Azzaya Khasbaatar
Kaikai Liu
Francis R. Lin
Sei-Hum Jang
Jie Zhang
Yuqing Li
Ying Diao
Zhanhua Wei
Hin-Lap Yip
David S. Ginger
Alex K.-Y. Jen
author_facet Kui Jiang
Robert J. E. Westbrook
Tian Xia
Cheng Zhong
Jianxun Lu
Azzaya Khasbaatar
Kaikai Liu
Francis R. Lin
Sei-Hum Jang
Jie Zhang
Yuqing Li
Ying Diao
Zhanhua Wei
Hin-Lap Yip
David S. Ginger
Alex K.-Y. Jen
author_sort Kui Jiang
collection DOAJ
description Abstract Efficient delocalization of photo-generated excitons is a key to improving the charge-separation efficiencies in state-of-the-art organic photovoltaic (OPV) absorber. While the delocalization in non-fullerene acceptors has been widely studied, we expand the scope by studying the properties of the conjugated polymer donor D18 on both the material and device levels. Combining optical spectroscopy, X-ray diffraction, and simulation, we show that D18 exhibits stronger π–π interactions and interchain packing compared to classic donor polymers, as well as higher external photoluminescence quantum efficiency (~26%). Using picosecond transient absorption spectroscopy and streak camera photoluminescence measurements, we show that the initial D18 excitons form delocalized intermediates, which decay radiatively with high efficiency in neat films. In single-component OPV cells based on D18, these intermediate excitations can be harvested with an internal quantum efficiency >30%, while in blends with acceptor Y6 they provide a pathway to free charge generation that partially bypasses performance-limiting charge-transfer states at the D18:Y6 interface. Our study demonstrates that donor polymers can be further optimized using similar design strategies that have been successful for non-fullerene acceptors, opening the door to even higher OPV efficiencies.
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spelling doaj-art-89c680ebd6dc4eafa06bb4cb2d2f1b192025-08-20T01:54:25ZengNature PortfolioNature Communications2041-17232025-04-0116111110.1038/s41467-025-58352-xPhotoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaicsKui Jiang0Robert J. E. Westbrook1Tian Xia2Cheng Zhong3Jianxun Lu4Azzaya Khasbaatar5Kaikai Liu6Francis R. Lin7Sei-Hum Jang8Jie Zhang9Yuqing Li10Ying Diao11Zhanhua Wei12Hin-Lap Yip13David S. Ginger14Alex K.-Y. Jen15Department of Chemistry, City University of Hong KongDepartment of Chemistry, University of WashingtonDepartment of Materials Science and Engineering, City University of Hong KongDepartment of Chemistry, Wuhan UniversityXiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Institute of Luminescent Materials and Information Displays, College of Materials Science and Engineering, Huaqiao UniversityDepartment of Chemical & Biomolecular Engineering, University of Illinois Urbana-ChampaignDepartment of Materials Science and Engineering, City University of Hong KongDepartment of Chemistry, City University of Hong KongDepartment of Materials Science and Engineering, University of WashingtonCenter for Photonics Information and Energy Materials, Shenzhen Institutes of Advanced Technology, Chinese Academy of SciencesXiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Institute of Luminescent Materials and Information Displays, College of Materials Science and Engineering, Huaqiao UniversityDepartment of Chemical & Biomolecular Engineering, University of Illinois Urbana-ChampaignXiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Institute of Luminescent Materials and Information Displays, College of Materials Science and Engineering, Huaqiao UniversityDepartment of Materials Science and Engineering, City University of Hong KongDepartment of Chemistry, University of WashingtonDepartment of Chemistry, City University of Hong KongAbstract Efficient delocalization of photo-generated excitons is a key to improving the charge-separation efficiencies in state-of-the-art organic photovoltaic (OPV) absorber. While the delocalization in non-fullerene acceptors has been widely studied, we expand the scope by studying the properties of the conjugated polymer donor D18 on both the material and device levels. Combining optical spectroscopy, X-ray diffraction, and simulation, we show that D18 exhibits stronger π–π interactions and interchain packing compared to classic donor polymers, as well as higher external photoluminescence quantum efficiency (~26%). Using picosecond transient absorption spectroscopy and streak camera photoluminescence measurements, we show that the initial D18 excitons form delocalized intermediates, which decay radiatively with high efficiency in neat films. In single-component OPV cells based on D18, these intermediate excitations can be harvested with an internal quantum efficiency >30%, while in blends with acceptor Y6 they provide a pathway to free charge generation that partially bypasses performance-limiting charge-transfer states at the D18:Y6 interface. Our study demonstrates that donor polymers can be further optimized using similar design strategies that have been successful for non-fullerene acceptors, opening the door to even higher OPV efficiencies.https://doi.org/10.1038/s41467-025-58352-x
spellingShingle Kui Jiang
Robert J. E. Westbrook
Tian Xia
Cheng Zhong
Jianxun Lu
Azzaya Khasbaatar
Kaikai Liu
Francis R. Lin
Sei-Hum Jang
Jie Zhang
Yuqing Li
Ying Diao
Zhanhua Wei
Hin-Lap Yip
David S. Ginger
Alex K.-Y. Jen
Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
Nature Communications
title Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
title_full Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
title_fullStr Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
title_full_unstemmed Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
title_short Photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high-performance organic photovoltaics
title_sort photoluminescent delocalized excitons in donor polymers facilitate efficient charge generation for high performance organic photovoltaics
url https://doi.org/10.1038/s41467-025-58352-x
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