Abstract
All-perovskite tandem solar cells promise higher power-conversion efficiency (PCE) than single-junction perovskite solar cells (PSCs) while maintaining a low fabrication cost1,2,3. However, their performance is still largely constrained by the subpar performance of mixed lead–tin (Pb–Sn) narrow-bandgap (NBG) perovskite subcells, mainly because of a high trap density on the perovskite film surface4,5,6. Although heterojunctions with intermixed 2D/3D perovskites could reduce surface recombination, this common strategy induces transport losses and thereby limits device fill factors (FFs)7,8,9. Here we develop an immiscible 3D/3D bilayer perovskite heterojunction (PHJ) with type II band structure at the Pb–Sn perovskite–electron-transport layer (ETL) interface to suppress the interfacial non-radiative recombination and facilitate charge extraction. The bilayer PHJ is formed by depositing a layer of lead-halide wide-bandgap (WBG) perovskite on top of the mixed Pb–Sn NBG perovskite through a hybrid evaporation–solution-processing method. This heterostructure allows us to increase the PCE of Pb–Sn PSCs having a 1.2-µm-thick absorber to 23.8%, together with a high open-circuit voltage (Voc) of 0.873 V and a high FF of 82.6%. We thereby demonstrate a record-high PCE of 28.5% (certified 28.0%) in all-perovskite tandem solar cells. The encapsulated tandem devices retain more than 90% of their initial performance after 600 h of continuous operation under simulated one-sun illumination.
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All data are available in the main text or the supplementary materials. Further data are available from the corresponding author on reasonable request.
References
Jošt, M., Kegelmann, L., Korte, L. & Albrecht, S. Monolithic perovskite tandem solar cells: a review of the present status and advanced characterization methods toward 30% efficiency. Adv. Energy Mater. 10, 1904102 (2020).
Li, Z. et al. Cost analysis of perovskite tandem photovoltaics. Joule 2, 1559–1572 (2018).
Albrecht, S. & Rech, B. Perovskite solar cells: on top of commercial photovoltaics. Nat. Energy 2, 16196 (2017).
Savill, K. J., Ulatowski, A. M. & Herz, L. M. Optoelectronic properties of tin–lead halide perovskites. ACS Energy Lett. 6, 2413–2426 (2021).
Yang, Y. et al. Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films. Nat. Energy 2, 16207 (2017).
Ricciarelli, D., Meggiolaro, D., Ambrosio, F. & De Angelis, F. Instability of tin iodide perovskites: bulk p-doping versus surface tin oxidation. ACS Energy Lett. 5, 2787–2795 (2020).
Park, S. M., Abtahi, A., Boehm, A. M. & Graham, K. R. Surface ligands for methylammonium lead iodide films: surface coverage, energetics, and photovoltaic performance. ACS Energy Lett. 5, 799–806 (2020).
La-Placa, M. G. et al. Vacuum-deposited 2D/3D perovskite heterojunctions. ACS Energy Lett. 4, 2893–2901 (2019).
Chen, C. et al. Arylammonium-assisted reduction of the open-circuit voltage deficit in wide-bandgap perovskite solar cells: the role of suppressed ion migration. ACS Energy Lett. 5, 2560–2568 (2020).
Lin, R. et al. Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(II) oxidation in precursor ink. Nat. Energy 4, 864–873 (2019).
Xiao, K. et al. All-perovskite tandem solar cells with 24.2% certified efficiency and area over 1 cm2 using surface-anchoring zwitterionic antioxidant. Nat. Energy 5, 870–880 (2020).
Xiao, K. et al. Scalable processing for realizing 21.7%-efficient all-perovskite tandem solar modules. Science 376, 762–767 (2022).
Gao, H. et al. Thermally stable all-perovskite tandem solar cells fully using metal oxide charge transport layers and tunnel junction. Sol. RRL 5, 2100814 (2021).
Lin, R. et al. All-perovskite tandem solar cells with improved grain surface passivation. Nature 603, 73–78 (2022).
Park, K., Lee, J. H. & Lee, J. W. Surface defect engineering of metal halide perovskites for photovoltaic applications. ACS Energy Lett. 7, 1230–1239 (2022).
Liu, J. et al. Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx. Science 377, 302–306 (2022).
Azmi, R. et al. Damp heat-stable perovskite solar cells with tailored-dimensionality 2D/3D heterojunctions. Science 376, 73–77 (2022).
Wei, M. et al. Combining efficiency and stability in mixed tin–lead perovskite solar cells by capping grains with an ultrathin 2D layer. Adv. Mater. 32, 1907058 (2020).
Chen, H. et al. Quantum-size-tuned heterostructures enable efficient and stable inverted perovskite solar cells. Nat. Photonics 16, 352–358 (2022).
Azpiroz, J. M., Mosconi, E., Bisquert, J. & De Angelis, F. Defect migration in methylammonium lead iodide and its role in perovskite solar cell operation. Energy Environ. Sci. 8, 2118–2127 (2015).
Mosconi, E. & De Angelis, F. Mobile ions in organohalide perovskites: interplay of electronic structure and dynamics. ACS Energy Lett. 1, 182–188 (2016).
Haruyama, J., Sodeyama, K., Han, L. & Tateyama, Y. First-principles study of ion diffusion in perovskite solar cell sensitizers. J. Am. Chem. Soc. 137, 10048–10051 (2015).
Green, M. A. et al. Solar cell efficiency tables (Version 60). Prog. Photovolt. Res. Appl. 30, 687–701 (2022).
Hu, S. et al. Optimized carrier extraction at interfaces for 23.6% efficient tin–lead perovskite solar cells. Energy Environ. Sci. 15, 2096–2107 (2022).
Burgelman, M., Nollet, P. & Degrave, S. Modelling polycrystalline semiconductor solar cells. Thin Solid Films 361, 527–532 (2000).
Kapil, G. et al. Tin-lead perovskite fabricated via ethylenediamine interlayer guides to the solar cell efficiency of 21.74%. Adv. Energy Mater. 11, 2101069 (2021).
Jang, Y. W. et al. Intact 2D/3D halide junction perovskite solar cells via solid-phase in-plane growth. Nat. Energy 6, 63–71 (2021).
Menzel, D. et al. Field effect passivation in perovskite solar cells by a LiF interlayer. Adv. Energy Mater. 12, 2201109 (2022).
Rau, U. Reciprocity relation between photovoltaic quantum efficiency and electroluminescent emission of solar cells. Phys. Rev. B 76, 085303 (2007).
Wu, Y. et al. Perovskite solar cells with 18.21% efficiency and area over 1 cm2 fabricated by heterojunction engineering. Nat. Energy 1, 16148 (2016).
Tong, J. et al. Carrier lifetimes of >1 μs in Sn-Pb perovskites enable efficient all-perovskite tandem solar cells. Science 364, 475–479 (2019).
Krogmeier, B., Staub, F., Grabowski, D., Rau, U. & Kirchartz, T. Quantitative analysis of the transient photoluminescence of CH3NH3PbI3/PC61BM heterojunctions by numerical simulations. Sustain. Energy Fuels 2, 1027–1034 (2018).
Caprioglio, P. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).
Santbergen, R. et al. GenPro4 optical model for solar cell simulation and its application to multijunction solar cells. IEEE J. Photovolt. 7, 919–926 (2017).
Li, L. et al. Flexible all-perovskite tandem solar cells approaching 25% efficiency with molecule-bridged hole-selective contact. Nat. Energy 7, 708–717 (2022).
Rühle, S. Tabulated values of the Shockley–Queisser limit for single junction solar cells. Sol. Energy 130, 139–147 (2016).
Thiesbrummel, J. et al. Understanding and minimizing Voc losses in all-perovskite tandem photovoltaics. Adv. Energy Mater. 13, 2202674 (2022).
Stolterfoht, M. et al. Approaching the fill factor Shockley–Queisser limit in stable, dopant-free triple cation perovskite solar cells. Energy Environ. Sci. 10, 1530–1539 (2017).
Wen, J. et al. Steric engineering enables efficient and photostable wide-bandgap perovskites for all-perovskite tandem solar cells. Adv. Mater. 34, 2110356 (2022).
Wu, P. et al. Efficient and thermally stable all-perovskite tandem solar cells using all-FA narrow-bandgap perovskite and metal-oxide-based tunnel junction. Adv. Energy Mater. 12, 220948 (2022).
Han, Q. et al. Low-temperature processed inorganic hole transport layer for efficient and stable mixed Pb-Sn low-bandgap perovskite solar cells. Sci. Bull. 64, 1399–1401 (2019).
Han, Y. et al. Degradation observations of encapsulated planar CH3NH3PbI3 perovskite solar cells at high temperatures and humidity. J. Mater. Chem. A 3, 8139–8147 (2015).
Acknowledgements
This work was financially supported by the National Key R&D Program of China (2022YFB4200304), National Natural Science Foundation of China (U21A2076, 61974063), Natural Science Foundation of Jiangsu Province (BE2022021, BE2022026, BK20202008, BK20190315), Fundamental Research Funds for the Central Universities (0213/14380219, 0213/14380218, 0213/14380216, 0205/14380252), Frontiers Science Center for Critical Earth Material Cycling Fund (DLTD2109) and Program for Innovative Talents and Entrepreneur in Jiangsu. We would also like to thank the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences (no. A2107).
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H.T. conceived the idea and directed the overall project. R.L., Y.W. and Q.L. fabricated all the devices and conducted the characterization. B.T. and F.F. performed the TA measurements. J.L. and Y.D. performed the HR-STEM and EDX measurements. C.D. and C.M. performed ToF-SIMS characterization. Y.G. performed the optical and electrical simulation of single and tandem solar cells with GenPro4. R.L. and J.L. carried out the SCAPS-1D simulation. H.G., P.W., C.L., S.Z., J.W., K.X., Z.L. and L.L. carried out device fabrication and materials characterization. R.L. and H.T. wrote the manuscript. All authors discussed the results and commented on the paper.
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Hairen Tan is the founder, chief scientific officer and chairman of Renshine Solar Co., Ltd., a company that is commercializing perovskite photovoltaics. The other authors declare no competing interests.
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Supplementary Figs. 1–49, Supplementary Notes 1–7 and Supplementary Tables 1–16 – see contents page for details.
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Lin, R., Wang, Y., Lu, Q. et al. All-perovskite tandem solar cells with 3D/3D bilayer perovskite heterojunction. Nature 620, 994–1000 (2023). https://doi.org/10.1038/s41586-023-06278-z
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DOI: https://doi.org/10.1038/s41586-023-06278-z
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