19.31% binary organic solar cell and low non-radiative recombination enabled by non-monotonic intermediate state transition

Jiehao Fu^{1

2}, Patrick W K Fong^{1

2}, Heng Liu³, Chieh-Szu Huang⁴, Xinhui Lu³, Shirong Lu⁵, Maged Abdelsamie^{6

7}, Tim Kodalle⁸, Carolin M Sutter-Fella⁸, Yang Yang⁹, Gang Li^{10

11}

Affiliations

¹ Department of Electronic and Information Engineering, Research Institute for Smart Energy (RISE), Photonic Research Institute (PRI), Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, China.
² The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, 518057, China.
³ Department of Physics, The Chinese University of Hong Kong, Shatin, Hong Kong, 999077, China.
⁴ Department of Materials Science and Engineering, University of California Los Angeles (UCLA), Los Angeles, CA, 90095, USA.
⁵ School of Materials Science and Engineering, Taizhou University, Taizhou, 318000, China.
⁶ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁷ Materials Science and Engineering Department, King Fahd University of Petroleum and Minerals, Dhahran, Saudi Arabia.
⁸ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁹ Department of Materials Science and Engineering, University of California Los Angeles (UCLA), Los Angeles, CA, 90095, USA. yangy@ucla.edu.
¹⁰ Department of Electronic and Information Engineering, Research Institute for Smart Energy (RISE), Photonic Research Institute (PRI), Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, China. gang.w.li@polyu.edu.hk.
¹¹ The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, 518057, China. gang.w.li@polyu.edu.hk.

PMID: 36997533
PMCID: PMC10063688
DOI: 10.1038/s41467-023-37526-5

19.31% binary organic solar cell and low non-radiative recombination enabled by non-monotonic intermediate state transition

Jiehao Fu et al. Nat Commun. 2023.

. 2023 Mar 30;14(1):1760.

doi: 10.1038/s41467-023-37526-5.

Authors

Affiliations

¹ Department of Electronic and Information Engineering, Research Institute for Smart Energy (RISE), Photonic Research Institute (PRI), Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, China.
² The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, 518057, China.
³ Department of Physics, The Chinese University of Hong Kong, Shatin, Hong Kong, 999077, China.
⁴ Department of Materials Science and Engineering, University of California Los Angeles (UCLA), Los Angeles, CA, 90095, USA.
⁵ School of Materials Science and Engineering, Taizhou University, Taizhou, 318000, China.
⁶ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁷ Materials Science and Engineering Department, King Fahd University of Petroleum and Minerals, Dhahran, Saudi Arabia.
⁸ Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
⁹ Department of Materials Science and Engineering, University of California Los Angeles (UCLA), Los Angeles, CA, 90095, USA. yangy@ucla.edu.
¹⁰ Department of Electronic and Information Engineering, Research Institute for Smart Energy (RISE), Photonic Research Institute (PRI), Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, China. gang.w.li@polyu.edu.hk.
¹¹ The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, 518057, China. gang.w.li@polyu.edu.hk.

PMID: 36997533
PMCID: PMC10063688
DOI: 10.1038/s41467-023-37526-5

Abstract

Non-fullerene acceptors based organic solar cells represent the frontier of the field, owing to both the materials and morphology manipulation innovations. Non-radiative recombination loss suppression and performance boosting are in the center of organic solar cell research. Here, we developed a non-monotonic intermediate state manipulation strategy for state-of-the-art organic solar cells by employing 1,3,5-trichlorobenzene as crystallization regulator, which optimizes the film crystallization process, regulates the self-organization of bulk-heterojunction in a non-monotonic manner, i.e., first enhancing and then relaxing the molecular aggregation. As a result, the excessive aggregation of non-fullerene acceptors is avoided and we have achieved efficient organic solar cells with reduced non-radiative recombination loss. In PM6:BTP-eC9 organic solar cell, our strategy successfully offers a record binary organic solar cell efficiency of 19.31% (18.93% certified) with very low non-radiative recombination loss of 0.190 eV. And lower non-radiative recombination loss of 0.168 eV is further achieved in PM1:BTP-eC9 organic solar cell (19.10% efficiency), giving great promise to future organic solar cell research.

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Conflict of interest statement

The authors declare no competing interests.

Figures

**Fig. 1. Chemical structures and thermal behaviors between TCB and active materials.**
Chemical structures of PM6 (a), TCB (b), and Y6 (c). d DSC thermograms (cooling process) of PM6, PM6:TCB, and TCB. e DSC thermograms (cooling process) of Y6, Y6:TCB, and TCB. f DSC thermograms (cooling process) of PM6:Y6, PM6:Y6:TCB, and TCB. Here exo. is the abbreviation of exothermic.

**Fig. 2. Device performance of OSCs with DIO and TCB processing.**
a Device structure used in this work. b J–V curves for PM6: Y6-based OSCs with benchmark solvent additive DIO and with TCB. c EQE spectra for PM6:Y6-based OSCs with DIO and with TCB. d PCE histograms of PM6:Y6-based OSCs with DIO and with TCB. e EQE_EL of PM6:Y6 devices with different treatments at various injected current densities. f Detailed energy loss in the DIO processed and TCB processed PM6:Y6 devices. Source data are provided as a Source Data file.

**Fig. 3. Morphology—Surface topography and molecular stacking.**
AFM height images of Y6 films (a, e) and PM6:Y6 films (b, f) with DIO and TCB treatment. 2D GIWAXS diffraction patterns (c, g) and 1D GIWAXS diffraction patterns (d) of PM6:Y6 blend films with DIO and TCB treatment. h The areas of π-π and lamellar diffraction peak for PM6:Y6 blend films with DIO and TCB treatment. Source data are provided as a Source Data file.

**Fig. 4. In situ UV-vis characterization.**
The color mapping of in situ UV-vis reflectance spectra as a function of spin-coating time for PM6:Y6 blends with DIO (a) and with TCB (b). Normalized in situ absorption intensity at the wavelength of 600 nm (c) and 750 nm (f) as a function of spin-coating time for PM6:Y6 blends with DIO and with TCB. Normalized absorption spectra (here we defined the absorption of sample as the difference between the reflectance of background and the reflectance of sample) at representative time points for PM6:Y6 blends with DIO (d) and with TCB (e). Source data are provided as a Source Data file.

**Fig. 5. A schematic diagram illustrating working mechanisms induced by different treatments.**
a DIO treatment. b TCB treatment.

**Fig. 6. The generality of TCB and the analysis of V_OC loss as well as light stability.**
a J–V curves for the DIO processed and TCB processed OSCs based on PM1:BTP-eC9. b J–V curves for the DIO processed and TCB processed OSCs based on PM6:BTP-eC9. c EQE_EL of OSCs at various injected current densities. d Detailed energy loss in the DIO-processed and TCB-processed OSCs based on PM1:BTP-eC9. e Detailed V_OC loss in the DIO processed and TCB processed OSCs based on PM6:BTP-eC9. f Comparison of PCE versus ∆E₃ in reported OSCs with over 18% efficiency. g Light stability tests for PM6:BTP-eC9 based OSCs with different treatments, all OSCs were encapsulated and stored under continuous illumination equivalent to 1 sun in air. Source data are provided as a Source Data file.

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19.31% binary organic solar cell and low non-radiative recombination enabled by non-monotonic intermediate state transition

Affiliations

19.31% binary organic solar cell and low non-radiative recombination enabled by non-monotonic intermediate state transition

Authors

Affiliations

Abstract

Conflict of interest statement

Figures

References

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