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Perovskite solar cells based on spiro-OMeTAD stabilized with an alkylthiol additive

Nature Photonics volume 17, pages 96–105 (2023)Cite this article

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Abstract

Spiro-OMeTAD, one of the most widely used hole-transport materials (HTMs) in optoelectronic devices, typically requires chemical doping with a lithium compound (LiTFSI) to attain sufficient conductivity and efficient hole extraction. However, the doping step requires an activation process that comprises exposure of the blend films to an ambient atmosphere. Additionally, the lithium dopant induces crystallization, and its hygroscopic nature negatively impacts device performance and lifetime. Here we report a facile approach based on the incorporation of a low-cost alkylthiol additive (1-dodecanethiol, DDT) in the spiro-OMeTAD HTM. We discover that DDT provides a more efficient and controllable doping process with significantly reduced doping duration, enabling the HTM to achieve comparable performance before air activation. The coordination between DDT and LiTFSI increases the concentration of dopants in the HTM bulk, reduces their accumulation at interfaces, and enhances the structural integrity of the HTM under wetting, heat and light stress. We fabricate perovskite solar cells using DDT-treated spiro-OMeTAD as the HTM. Our best devices exhibit a certified power conversion efficiency of 23.1%. Furthermore, the devices can retain 90% of peak performance under continuous illumination for 1,000 h. Our findings represent an important step forward in the production of doped spiro-OMeTAD, as well as its reliable application and future device commercialization.

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Fig. 1: The impact of DDT on p-doping.
Fig. 2: The impact of DDT on the lithium compound.
Fig. 3: The impact of DDT on device performance.
Fig. 4: The impact of DDT on wetting stability.
Fig. 5: The impact of DDT on thermal stability.
Fig. 6: The impact of DDT on illumination stability.

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The data that support the plots within this paper and other finding of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the Australian Government through the Australian Renewable Energy Agency (grant no. RND0751). X.H. acknowledges financial support by the Australian Research Council (ARC) Future Fellowship (FT190100756). X.L. acknowledges support from the Australian Centre of Advanced Photovoltaics (ACAP) for his Postdoc Fellowship (project ID RG193402-G). Responsibility for the views, information or advice expressed herein is not accepted by the Australian Government. We acknowledge the use of the facilities at the Solid State and Elemental Analysis Unit, and the Australian microscopy and microanalysis research facilities at the Electron Microscope Unit, University of New South Wales (UNSW). We acknowledge the assistance of B. Gong on the TOF-SIMS measurements and discussions. We acknowledge the assistance of Y. Yao on the AFM measurements and discussions. We acknowledge the assistance of M. Lee on the KPFM measurements. We acknowledge the assistance of Y. Wang on the preparation of NMR samples. We acknowledge the assistance of C. Qian on the fabrication of Sb2(S,Se)3 solar cells.

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Authors and Affiliations

  1. School of Photovoltaic and Renewable Energy Engineering, University of New South Wales, Sydney, New South Wales, Australia

    Xu Liu, Bolin Zheng, Lei Shi, Ziheng Liu, Jae Sung Yun, Eunyoung Choi, Meng Zhang, Jialiang Huang, Caixia Li, Kaiwen Sun, Mingrui He, Xiaojing Hao & Martin Green

  2. Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Foshan, Guangdong, China

    Lei Shi

  3. School of Chemical Engineering, University of New South Wales, Sydney, New South Wales, Australia

    Shujie Zhou & Jiangtao Xu

  4. School of Computer Science and Electronic Engineering, Advanced Technology Institute, University of Surrey, Guildford, Surrey, UK

    Jae Sung Yun

  5. School of New Energy and Materials, Southwest Petroleum University, Chengdu, China

    Meng Zhang

  6. National Centre for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming, China

    Yinhua Lv & Wen-Hua Zhang

  7. School of Materials Science and Engineering, University of New South Wales, Sydney, New South Wales, Australia

    Jan Seidel

  8. Institute of Functional Nano & Soft Materials and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, Jiangsu, China

    Jun Peng

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Contributions

X.L. conceived the idea of the project, designed the experiments, analysed the data and wrote the manuscript. X.L. performed the fabrication, optimization and characterization of the films and solar cells. X.L., Y.L. and W.-H.Z. contributed to the perovskite using a two-step method. X.L., B.Z., L.S. and M.Z. contributed to the characterization of the films and stability tests of the devices. X.L. and B.Z. contributed to UV–vis absorption spectra measurements. X.L., B.Z., J.X., S.Z. and X.H. contributed to NMR characterization of the films and the mechanism analysis of the devices. X.L., B.Z. and Z.L. performed the XRD and SEM characterizations. B.Z. and E.C. characterized the AFM process. J.S.Y., E.C. and J.S. carried out the KPFM measurements and analysed the data. X.L. performed the space-charge-limited current measurements and analysed the data. X.L., K.S. and M.Z. performed the PL measurements and analysed the data. X.L. and J.H. performed the EIS measurements and analysed the data. X.L. performed the FTIR measurements and analysed the data. X.L. analysed the TOF-SIMS data. C.L. contributed to the anti-reflection layer process. M.H. and J.P. assisted with the fabrication of large-area PSCs. All authors commented on the final version of the manuscript. X.H. and M.G. supervised the project, advised on its direction and helped prepare the manuscript.

Corresponding authors

Correspondence to Meng Zhang, Xiaojing Hao or Martin Green.

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UNSW has filed an international PCT patent (Application No. PCT/AU2021/050147) related to the subject matter of this manuscript. The authors declare no competing interests.

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Nature Photonics thanks Nazario Martin, Changduk Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Fig. 1, KPFM results of different HTMs. Supplementary Fig. 2, UPS results of different HTMs. Supplementary Fig. 3, NMR results of different HTMs. Supplementary Fig. 4, UV-vis absorption results of different HTMs. Supplementary UV-vis absorption results discussion. Supplementary Fig. 5, SEM results of different HTMs. Supplementary Fig. 6, Photographs of different HTMs exposed in air. Supplementary Fig. 7, FTIR results of different HTMs. Supplementary FTIR results discussion. Supplementary Fig. 8, Electrical characterization results of different HTMs. Supplementary Fig. 9, Impact of DDT and air activation on Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 devices via solvent engineering. Supplementary Fig. 10, EQE results of DDT-treated Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 devices via solvent engineering. Supplementary Fig. 11, J–V curves of the DDT-treated Cs0.05FAXMA1 − XPbI3 device (0.09 cm2) via sequential deposition. Supplementary Fig. 12, EQE results of DDT-treated Cs0.05FAXMA1 − XPbI3 devices via sequential deposition. Supplementary Fig. 13, J–V curves of the DDT-treated Cs0.05FAXMA1 − XPbI3 device (1.0 cm2) via sequential deposition. Supplementary Fig. 14, Impact of DDT and DDS on Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 devices via solvent engineering. Supplementary Fig. 15, Stability results of DDT-treat devices and DDS-treated devices in ambient air. Supplementary Fig. 16, AFM results of different HTMs. Supplementary Fig. 17, XRD results of different HTMs-based devices. Supplementary Fig. 18, AFM result of control HTM after wetting stress. Supplementary Fig. 19, TOF-SIMS results of control and DDT-treated devices after wetting stress. Supplementary Fig. 20, TOF-SIMS results of control and DDT-treated devices after thermal stress. Supplementary Fig. 21, J–V curve of thermal-aged device after re-depositing new HTM. Supplementary Fig. 22, Stability results of control and DDT-treated FA0.9Cs0.1PbI3 devices after thermal stress. Supplementary stability results discussion. Supplementary Fig. 23, TOF-SIMS results of control and DDT-treated devices after light stress. Supplementary Fig. 24, J–V curve of light-aged device after re-depositing new HTM. Supplementary Fig. 25, Impact of DDT on PTAA-based Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 devices via solvent engineering. Supplementary Fig. 26, EQE results of PTAA-based Cs0.05(FAPbI3)0.85(MAPbBr3)0.15 devices via solvent engineering. Supplementary Fig. 27, PL results of different PTAA-based HTMs. Supplementary Fig. 28, AFM results of different PTAA-based HTMs. Supplementary Table 1, Reported top efficiencies of PSCs since 2012. Supplementary Table 2, Reported top efficiencies of Sb2(S,Se)3 solar cells since 2020. Supplementary Table 3, Photovoltaic parameters of DDT-treated cells prepared by solvent engineering. Supplementary Table 4, Photovoltaic parameters of DDT-treated cells (0.09 cm2) prepared by sequential deposition. Supplementary Table 5, Photovoltaic parameters of DDT-treated cells (1.0 cm2) prepared by sequential deposition. Supplementary Table 6, Performance of DDS-treated cells and DDT-treated cells before and after ageing in ambient air. Supplementary Table 7, Performance of ODT-treated cells before and after ageing in ambient air. Supplementary Table 8, Performance of control and DDT-treated Cs0.05FAXMA1 − XPbI3 cells (0.09 cm2) before and after ageing in ambient air. Supplementary Table 9, Performance of DDT-treated Cs0.05FAXMA1 − XPbI3 cells (1.0 cm2) before and after ageing in ambient air. Supplementary Table 10, Performance of control and DDT-treated cells before and after wetting stress. Supplementary Table 11, Performance of control and DDT-treated cells before and after thermal stress. Supplementary Table 12, Performance of control and DDT-treated FA0.9Cs0.1PbI3 cells before and after thermal stress. Supplementary Table 13, Performance of control and DDT-treated cells before and after light stress. Supplementary Table 14, Photovoltaic parameters of control and DDT-treated Sb2(S,Se)3 cells. Certification reports.

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Liu, X., Zheng, B., Shi, L. et al. Perovskite solar cells based on spiro-OMeTAD stabilized with an alkylthiol additive. Nat. Photon. 17, 96–105 (2023). https://doi.org/10.1038/s41566-022-01111-x

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