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3. Highly-Efficient Charge Separation and Polaron Delocalization in Polymer-Fullerene Bulk-Heterojunctions: A Comparative Multi-Frequency EPR & DFT Study

Author

Niklas, Jens, Mardis, Kristy L., Banks, Brian P., Grooms, Gregory M., Sperlich, Andreas, Dyakonov, Vladimir, Beaupré, Serge, Leclerc, Mario, Xu, Tao, Yu, Luping, and Poluektov, Oleg G.

Subjects
Condensed Matter - Materials Science
Abstract

The ongoing depletion of fossil fuels has led to an intensive search for additional renewable energy sources. Solar-based technologies could provide sufficient energy to satisfy the global economic demands in the near future. Photovoltaic (PV) cells are the most promising man-made devices for direct solar energy utilization. Understanding the charge separation and charge transport in PV materials at a molecular level is crucial for improving the efficiency of the solar cells. Here, we use light-induced EPR spectroscopy combined with DFT calculations to study the electronic structure of charge separated states in blends of polymers (P3HT, PCDTBT, and PTB7) and fullerene derivatives (C60-PCBM and C70-PCBM). Solar cells made with the same composites as active layers show power conversion efficiencies of 3.3% (P3HT), 6.1% (PCDTBT), and 7.3% (PTB7), respectively. Under illumination of these composites, two paramagnetic species are formed due to photo-induced electron transfer between the conjugated polymer and the fullerene. They are the positive, P+, and negative, P-, polarons on the polymer backbone and fullerene cage, respectively, and correspond to radical cations and radical anions. Using the high spectral resolution of high-frequency EPR (130 GHz), the EPR spectra of these species were resolved and principal components of the g-tensors were assigned. Light-induced pulsed ENDOR spectroscopy allowed the determination of 1H hyperfine coupling constants of photogenerated positive and negative polarons. The experimental results obtained for the different polymer-fullerene composites have been compared with DFT calculations, revealing that in all three systems the positive polaron is distributed over distances of 40-60 A on the polymer chain. This corresponds to about 15 thiophene units for P3HT, approximately three units PCDTBT, and about three to four units for PTB7. No spin density...

Published
2013
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10. Fused benzothiadiazole : a building block for n-type organic acceptor to achieve high-performance organic solar cells

Author

Yuan, Jun, Mainville, Mathieu, Zhang, Yunqiang, Beaupré, Serge, Zhou, Liuyang, Johnson, Paul A., Zhang, Chujun, Leclerc, Mario, Lau, Tsz-Ki, Zhang, Guichuan, Yip, Hin-Lap, So, Shu Kong, Chen, Honggang, Li, Yongfang, Zou, Yingping, Yuan, Jun, Mainville, Mathieu, Zhang, Yunqiang, Beaupré, Serge, Zhou, Liuyang, Johnson, Paul A., Zhang, Chujun, Leclerc, Mario, Lau, Tsz-Ki, Zhang, Guichuan, Yip, Hin-Lap, So, Shu Kong, Chen, Honggang, Li, Yongfang, and Zou, Yingping

Abstract

Narrow bandgap n-type organic semiconductors (n-OS) have attracted great attention in recent years as acceptors in organic solar cells (OSCs), due to their easily tuned absorption and electronic energy levels in comparison with fullerene acceptors. Herein, a new n-OS acceptor, Y5, with an electron-deficient-core-based fused structure is designed and synthesized, which exhibits a strong absorption in the 600–900 nm region with an extinction coefficient of 1.24 × 105 cm−1, and an electron mobility of 2.11 × 10−4 cm2 V−1 s−1. By blending Y5 with three types of common medium-bandgap polymers (J61, PBDB-T, and TTFQx-T1) as donors, all devices exhibit high short-circuit current densities over 20 mA cm−2. As a result, the power conversion efficiency of the Y5-based OSCs with J61, TTFQx-T1, and PBDB-T reaches 11.0%, 13.1%, and 14.1%, respectively. This indicates that Y5 is a universal and highly efficient n-OS acceptor for applications in organic solar cells.

Published
2020

11. Fused benzothiadiazole : a building block for n-type organic acceptor to achieve high-performance organic solar cells

Author

Yuan, Jun, Zhang, Yunqiang, Zhou, Liuyang, Zhang, Chujun, Lau, Tsz-Ki, Zhang, Guichuan, Yip, Hin-Lap, So, Shu Kong, Beaupré, Serge, Mainville, Mathieu, Johnson, Paul Andrew, Leclerc, Mario, Chen, Honggang, Li, Yongfang, Zou, Yingping, Yuan, Jun, Zhang, Yunqiang, Zhou, Liuyang, Zhang, Chujun, Lau, Tsz-Ki, Zhang, Guichuan, Yip, Hin-Lap, So, Shu Kong, Beaupré, Serge, Mainville, Mathieu, Johnson, Paul Andrew, Leclerc, Mario, Chen, Honggang, Li, Yongfang, and Zou, Yingping

Abstract

Narrow bandgap n-type organic semiconductors (n-OS) have attracted great attention in recent years as acceptors in organic solar cells (OSCs), due to their easily tuned absorption and electronic energy levels in comparison with fullerene acceptors. Herein, a new n-OS acceptor, Y5, with an electron-deficient-core-based fused structure is designed and synthesized, which exhibits a strong absorption in the 600–900 nm region with an extinction coefficient of 1.24 × 105 cm−1, and an electron mobility of 2.11 × 10−4 cm2 V−1 s−1. By blending Y5 with three types of common medium-bandgap polymers (J61, PBDB-T, and TTFQx-T1) as donors, all devices exhibit high short-circuit current densities over 20 mA cm−2. As a result, the power conversion efficiency of the Y5-based OSCs with J61, TTFQx-T1, and PBDB-T reaches 11.0%, 13.1%, and 14.1%, respectively. This indicates that Y5 is a universal and highly efficient n-OS acceptor for applications in organic solar cells.

Published
2019

13. Fused Benzothiadiazole: A Building Block for n‐Type Organic Acceptor to Achieve High‐Performance Organic Solar Cells

Author

Yuan, Jun, primary, Zhang, Yunqiang, additional, Zhou, Liuyang, additional, Zhang, Chujun, additional, Lau, Tsz‐Ki, additional, Zhang, Guichuan, additional, Lu, Xinhui, additional, Yip, Hin‐Lap, additional, So, Shu Kong, additional, Beaupré, Serge, additional, Mainville, Mathieu, additional, Johnson, Paul A., additional, Leclerc, Mario, additional, Chen, Honggang, additional, Peng, Hongjian, additional, Li, Yongfang, additional, and Zou, Yingping, additional

Published
2019
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25. New Fluorinated Dithienyldiketopyrrolopyrrole Monomers and Polymers for Organic Electronics

Author

Bura, Thomas, Beaupré, Serge, Ibraikulov, Olzhas A., Légaré, Marc-André, Quinn, Jesse, Lévêque, Patrick, Heiser, Thomas, Li, Yuning, Leclerc, Nicolas, and Leclerc, Mario

Abstract

Diketopyrrolopyrrole (DPP) derivatives are among the most efficient materials studied for both polymer solar cells (PSCs) and organic field-effect transistors (OFETs) applications. We report here the synthesis of new fluorinated dithienyldiketopyrrolopyrrole (fDT-DPP) monomers suitable for direct heteroarylation polymerization. fDT-DPP copolymers were then prepared to probe the effect of the fluorination. It was found that they feature deeper HOMO energy levels and smaller bandgaps than their non-fluorinated analogues. Moreover, some fDT-DPP copolymers show ambipolar behavior when tested in OFETs. For example, P2shows hole mobility up to 0.8 cm2V–1s–1and electron mobility up to 0.5 cm2V–1s–1. Inverted PSCs with power conversion efficiency (PCE) up to 7.5% were also obtained for P5. These results reported here (OFETs and PSCs) confirm that the fluorination of dithienyl-DPP moieties improves the performance of organic electronics devices. This study is also evidencing the strength of the direct heteroarylation polymerization and fDT-DPP as a new class of conjugated polymers.

Published
2024
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28. Elucidating the Impact of Molecular Packing and Device Architecture on the Performance of Nanostructured Perylene Diimide Solar Cells

Author

Aluicio-Sarduy, Eduardo, primary, Singh, Ranbir, additional, Kan, Zhipeng, additional, Ye, Tengling, additional, Baidak, Aliaksandr, additional, Calloni, Alberto, additional, Berti, Giulia, additional, Duò, Lamberto, additional, Iosifidis, Agathaggelos, additional, Beaupré, Serge, additional, Leclerc, Mario, additional, Butt, Hans-Jürgen, additional, Floudas, George, additional, and Keivanidis, Panagiotis E., additional

Published
2015
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29. Is there a photostable conjugated polymer for efficient solar cells?

Author

Tournebize, Aurélien, primary, Gardette, Jean-Luc, additional, Taviot-Guého, Christine, additional, Bégué, Didier, additional, Arnaud, Marc Alexandre, additional, Dagron-Lartigau, Christine, additional, Medlej, Hussein, additional, Hiorns, Roger C., additional, Beaupré, Serge, additional, Leclerc, Mario, additional, and Rivaton, Agnès, additional

Published
2015
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31. Random D–A1–D–A2 terpolymers based on benzodithiophene, thiadiazole[3,4-e]isoindole-5,7-dione and thieno[3,4-c]pyrrole-4,6-dione for efficient polymer solar cells.

Author

Beaupré, Serge, Shaker-Sepasgozar, Sepideh, Najari, Ahmed, and Leclerc, Mario

Abstract

Recent developments on regio-regular and random terpolymers based on a donor/acceptor architecture (D1–A–D2–A or D–A1–D–A2) have shown promising results for their use as donor materials in bulk heterojunction (BHJ) polymer solar cells. New random terpolymers including benzo[1,2-b:4,5-b′]-dithiophene (BDT) as the electron-donor moiety and thiadiazolo[3,4-e]isoindole-5,7-dione (TID) and thieno[3,4-c]pyrrole-4,6-dione (TPD) as electron-accepting moieties were synthesized by Stille cross-coupling polymerization. Incremental addition of TPD (from 0 to 90%) led to the following random terpolymers: P[(BDT-TID)x-(BDT-TPD)y]n. Their electro-optical and photovoltaic properties were investigated. These high molecular weight and highly processable random terpolymers exhibited broad and strong absorption (300–800 nm), moderate bandgaps (1.52 eV to 1.64 eV) and deep-lying HOMO/LUMO energy levels (−5.6 eV and −3.9 eV, respectively). First, the optimized inverted device ITO/ZnO/P1:PC71BM/MoO3/Ag (where P1 is a typical D/A copolymer; TID 100%; TPD 0%) showed a power conversion efficiency up to 6.36% which is higher than the PCE reported in the literature for an analog of P1 (3.42%). Then, devices based on random terpolymers (P2–P10) showed power conversion efficiencies ranging from 5.06% (for P7; 40% TID/60% TPD) up to 6.70% (for P2; 90% TID/10% TPD) when PC61PM is used as the electron acceptor. A PCE as high as 7.30%, a Voc of 0.81 V, a Jsc of 13.86 mA cm−2 and a FF of 65% were achieved for P2 when PC71PM was used. This PCE is among the highest PCE values reported for random terpolymer-based polymer solar cells. [ABSTRACT FROM AUTHOR]

Published
2017
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33. Charge Transfer: Electronic Structure of Fullerene Heterodimer in Bulk-Heterojunction Blends (Adv. Energy Mater. 7/2014)

Author

Poluektov, Oleg G., primary, Niklas, Jens, additional, Mardis, Kristy L., additional, Beaupré, Serge, additional, Leclerc, Mario, additional, Villegas, Carmen, additional, Erten-Ela, Sule, additional, Delgado, Juan L., additional, Martín, Nazario, additional, Sperlich, Andreas, additional, and Dyakonov, Vladimir, additional

Published
2014
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38. Highly-efficient charge separation and polaron delocalization in polymer–fullerene bulk-heterojunctions: a comparative multi-frequency EPR and DFT study

Author

Niklas, Jens, primary, Mardis, Kristy L., additional, Banks, Brian P., additional, Grooms, Gregory M., additional, Sperlich, Andreas, additional, Dyakonov, Vladimir, additional, Beaupré, Serge, additional, Leclerc, Mario, additional, Xu, Tao, additional, Yu, Luping, additional, and Poluektov, Oleg G., additional

Published
2013
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46. Donor–acceptor alternating copolymers containing thienopyrroledione electron accepting units: preparation, redox behaviour, and application to photovoltaic cells

Author

Ottone, Chiara, primary, Berrouard, Philippe, additional, Louarn, Guy, additional, Beaupré, Serge, additional, Gendron, David, additional, Zagorska, Malgorzata, additional, Rannou, Patrice, additional, Najari, Ahmed, additional, Sadki, Said, additional, Leclerc, Mario, additional, and Pron, Adam, additional

Published
2012
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49. Effect of mixed solvents on PCDTBT:PC70BM based solar cells

Author

Alem, Salima, primary, Chu, Ta-Ya, additional, Tse, Shing C., additional, Wakim, Salem, additional, Lu, Jianping, additional, Movileanu, Raluca, additional, Tao, Ye, additional, Bélanger, Francis, additional, Désilets, Denis, additional, Beaupré, Serge, additional, Leclerc, Mario, additional, Rodman, Sheila, additional, Waller, David, additional, and Gaudiana, Russell, additional

Published
2011
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