Metal halide perovskite solar cells have demonstrated a high power conversion efficiency (PCE), and further enhancement of the PCE requires a reduction of the bandgap-voltage offset (WOC) and the non-radiative recombination photovoltage loss (ΔVOC,nr). Here, we report an effective approach for reducing the photovoltage loss through the simultaneous passivation of internal bulk defects and dimensionally graded two-dimensional perovskite interface defects. Through this dimensionally graded perovskite formation approach, an open-circuit voltage (VOC) of 1.24 V was obtained with a champion PCE of 21.54% in a 1.63 eV perovskite system (maximum VOC = 1.25 V, WOC = 0.38 V and ΔVOC,nr = 0.10 V); we further decreased the WOC to 0.326 V in a 1.53 eV perovskite system with a VOC of 1.21 V and a PCE of 23.78% (certified 23.09%). This approach is equally effective in achieving a low WOC (ΔVOC,nr) in 1.56 eV and 1.73 eV perovskite solar cell systems, and further leads to the substantially improved operational stability of perovskite solar cells.
This is a preview of subscription content, access via your institution
Subscribe to Nature+
Get immediate online access to Nature and 55 other Nature journal
Subscribe to Journal
Get full journal access for 1 year
only $8.25 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Tax calculation will be finalised during checkout.
Get time limited or full article access on ReadCube.
All prices are NET prices.
The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.
Jeon, N. J. et al. A fluorene-terminated hole-transporting material for highly efficient and stable perovskite solar cells. Nat. Energy 3, 682–689 (2018).
Green, M. et al. Solar cell efficiency tables (version 57). Prog. Photovolt. Res. Appl. 29, 3–15 (2020).
Hardin, B. E., Snaith, H. J. & McGehee, M. D. The renaissance of dye-sensitized solar cells. Nat. Photonics 6, 162–169 (2012).
Tress, W. et al. Predicting the open-circuit voltage of CH3NH3PbI3 perovskite solar cells using electroluminescence and photovoltaic quantum efficiency spectra: the role of radiative and non-radiative recombination. Adv. Energy Mater. 5, 1400812 (2015).
Yin, W.-J., Yang, J.-H., Kang, J., Yan, Y. & Wei, S.-H. Halide perovskite materials for solar cells: a theoretical review. J. Mater. Chem. A 3, 8926–8942 (2015).
Yao, J. et al. Quantifying losses in open-circuit voltage in solution-processable solar cells. Phys. Rev. Appl. 4, 014020 (2015).
Luo, D. et al. Enhanced photovoltage for inverted planar heterojunction perovskite solar cells. Science 360, 1442–1446 (2018).
Zheng, D. et al. Simultaneous bottom-up interfacial and bulk defect passivation in highly efficient planar perovskite solar cells using nonconjugated small-molecule electrolytes. Adv. Mater. 31, 1903239 (2019).
Motti, S. G. et al. Defect activity in lead halide perovskites. Adv. Mater. 31, 1901183 (2019).
Yang, G. et al. Interface engineering in planar perovskite solar cells: energy level alignment, perovskite morphology control and high performance achievement. J. Mater. Chem. A 5, 1658–1666 (2017).
Kim, M. et al. Methylammonium chloride induces intermediate phase stabilization for efficient perovskite solar cells. Joule 3, 2179–2192 (2019).
Yin, W.-J., Shi, T. & Yan, Y. Unusual defect physics in CH3NH3PbI3 perovskite solar cell absorber. Appl. Phys. Lett. 104, 063903 (2014).
Stolterfoht, M. et al. The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells. Energy Environ. Sci. 12, 2778–2788 (2019).
Yang, G. et al. Effective carrier-concentration tuning of SnO2 quantum dot electron-selective layers for high-performance planar perovskite solar cells. Adv. Mater. 30, 1706023 (2018).
Saliba, M. et al. Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance. Science 354, 206–209 (2016).
Yadav, P. et al. The role of rubidium in multiple-cation-based high-efficiency perovskite solar cells. Adv. Mater. 29, 1701077 (2017).
Albadri, A. et al. Unraveling the impact of rubidium incorporation on the transport-recombination mechanisms in highly efficient perovskite solar cells by small-perturbation techniques. J. Phys. Chem. C 121, 24903–24908 (2017).
Shao, S. et al. Highly reproducible Sn-based hybrid perovskite solar cells with 9% efficiency. Adv. Energy Mater. 8, 1702019 (2018).
Cao, D. H., Stoumpos, C. C., Farha, O. K., Hupp, J. T. & Kanatzidis, M. G. 2D homologous perovskites as light-absorbing materials for solar cell applications. J. Am. Chem. Soc. 137, 7843–7850 (2015).
Lee, J.-W. et al. Formamidinium and cesium hybridization for photo- and moisture-stable perovskite solar cell. Adv. Energy Mater. 5, 1501310 (2015).
Zhang, T. et al. Crystallinity preservation and ion migration suppression through dual ion exchange strategy for stable mixed perovskite solar cells. Adv. Energy Mater. 7, 1700118 (2017).
Baldan, A. Review progress in Ostwald ripening theories and their applications to nickel-base superalloys. Part I: Ostwald ripening theories. J. Mater. Sci. 37, 2171–2202 (2002).
Yang, G., Qin, P., Fang, G. & Li, G. A Lewis base-assisted passivation strategy towards highly efficient and stable perovskite solar cells. Sol. RRL 2, 1800055 (2018).
Abdi-Jalebi, M. et al. Maximizing and stabilizing luminescence from halide perovskites with potassium passivation. Nature 555, 497–501 (2018).
Wang, Z. et al. Efficient ambient-air-stable solar cells with 2D–3D heterostructured butylammonium-caesium-formamidinium lead halide perovskites. Nat. Energy 2, 17135 (2017).
Eperon, G. E. et al. Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells. Energy Environ. Sci. 7, 982–988 (2014).
Rau, U. Reciprocity relation between photovoltaic quantum efficiency and electroluminescent emission of solar cells. Phys. Rev. B 76, 085303 (2007).
Tress, W. et al. Interpretation and evolution of open-circuit voltage, recombination, ideality factor and subgap defect states during reversible light-soaking and irreversible degradation of perovskite solar cells. Energy Environ. Sci. 11, 151–165 (2018).
Green, M. A. Radiative efficiency of state‐of‐the‐art photovoltaic cells. Prog. Photovolt. Res. Appl. 20, 472–476 (2012).
Bi, D. et al. Efficient luminescent solar cells based on tailored mixed-cation perovskites. Sci. Adv. 2, e1501170 (2016).
Liu, J., Leng, J., Wu, K., Zhang, J. & Jin, S. Observation of internal photoinduced electron and hole separation in hybrid two-dimentional perovskite films. J. Am. Chem. Soc. 139, 1432–1435 (2017).
Nelson J. The Physics of Solar Cells (World Scientific, 2003).
Turren-Cruz, S.-H. et al. Enhanced charge carrier mobility and lifetime suppress hysteresis and improve efficiency in planar perovskite solar cells. Energy Environ. Sci. 11, 78–86 (2018).
Lin, Y. et al. Unveiling the operation mechanism of layered perovskite solar cells. Nat. Commun. 10, 1008 (2019).
Sarritzu, V. et al. Optical determination of Shockley-Read-Hall and interface recombination currents in hybrid perovskites. Sci. Rep. 7, 44629 (2017).
Jackson, W. B., Amer, N. M., Boccara, A. & Fournier, D. Photothermal deflection spectroscopy and detection. Appl. Opt. 20, 1333–1344 (1981).
Stranks, S. D. et al. Recombination kinetics in organic-inorganic perovskites: excitons, free charge, and subgap states. Phys. Rev. Appl. 2, 034007 (2014).
Stranks, S. D. Nonradiative losses in metal halide perovskites. ACS Energy Lett. 2, 1515–1525 (2017).
Shao, Y., Yuan, Y. & Huang, J. Correlation of energy disorder and open-circuit voltage in hybrid perovskite solar cells. Nat. Energy 1, 15001 (2016).
Chen, B., Rudd, P. N., Yang, S., Yuan, Y. & Huang, J. Imperfections and their passivation in halide perovskite solar cells. Chem. Soc. Rev. 48, 3842–3867 (2019).
McMeekin, D. P. et al. A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells. Science 351, 151–155 (2016).
Zhao, D. et al. Four-terminal all-perovskite tandem solar cells achieving power conversion efficiencies exceeding 23%. ACS Energy Lett. 3, 305–306 (2018).
Yu, Y. et al. Synergistic effects of lead thiocyanate additive and solvent annealing on the performance of wide-bandgap perovskite solar cells. ACS Energy Lett. 2, 1177–1182 (2017).
Zhou, Y. et al. Benzylamine-treated wide-bandgap perovskite with high thermal-photostability and photovoltaic performance. Adv. Energy Mater. 7, 1701048 (2017).
Domanski, K., Alharbi, E. A., Hagfeldt, A., Grätzel, M. & Tress, W. Systematic investigation of the impact of operation conditions on the degradation behaviour of perovskite solar cells. Nat. Energy 3, 61–67 (2018).
Kong, J. et al. Long-term stable polymer solar cells with significantly reduced burn-in loss. Nat. Commun. 5, 5688 (2014).
Chen, B. et al. Synergistic effect of elevated device temperature and excess charge carriers on the rapid light-induced degradation of perovskite solar cells. Adv. Mater. 31, e1902413 (2019).
Lin, Y. et al. Excess charge-carrier induced instability of hybrid perovskites. Nat. Commun. 9, 4981 (2018).
G.L. would like to thank support from the Research Grants Council of Hong Kong (Grant No. C5037-18G, 15246816 and 15218517), the Shenzhen Science and Technology Innovation Commission (Project No. JCYJ20170413154602102, JCYJ20200109105003940) and the funding provided by the Hong Kong Polytechnic University (Project Code: 1-ZE29, 1-BBAS and the Sir Sze-yuen Chung Endowed Professorship Fund (8-8480)). G.F. acknowledges support of the National High Technology Research and Development Program (No. 2015AA050601), the National Natural Science Foundation of China (No. 11674252 and 62074117) and the Natural Science Foundation of Hubei Province (No. 2019AAA020). X.L. and M.Q. acknowledge financial support from the Research Grant Council of Hong Kong (General Research Fund No. 14314216).
The authors declare no competing interests.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Yang, G., Ren, Z., Liu, K. et al. Stable and low-photovoltage-loss perovskite solar cells by multifunctional passivation. Nat. Photon. 15, 681–689 (2021). https://doi.org/10.1038/s41566-021-00829-4
This article is cited by
Science China Chemistry (2023)
Nature Photonics (2022)
Bulletin of Materials Science (2022)
Science China Chemistry (2022)