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Vol. 18 (2026)

Reproducible Fabrication of Perovskite Photovoltaics via Supramolecule Confinement Growth

https://doi.org/10.1007/s40820-025-01923-w
Xinyi Liu
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Jin Xie
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Ziren Zhou
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Huijun Lian
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Xinyuan Sui
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Qing Li
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Miaoyu Lin
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Da Liu
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Haiyang Yuan
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Feng Gao
Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden
Yongzhen Wu
Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Hua Gui Yang
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Shuang Yang
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Yu Hou
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China

Corresponding Author: Yu Hou

yhou@ecust.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 67

Abstract

The solution processibility of perovskites provides a cost-effective and high-throughput route for fabricating state-of-the-art solar cells. However, the fast kinetics of precursor-to-perovskite transformation is susceptible to processing conditions, resulting in an uncontrollable variance in device performance. Here, we demonstrate a supramolecule confined approach to reproducibly fabricate perovskite films with an ultrasmooth, electronically homogeneous surface. The assembly of a calixarene capping layer on precursor surface can induce host–guest interactions with solvent molecules to tailor the desolvation kinetics, and initiate the perovskite crystallization from the sharp molecule–precursor interface. These combined effects significantly reduced the spatial variance and extended the processing window of perovskite films. As a result, the standard efficiency deviations of device-to-device and batch-to-batch devices were reduced from 0.64–0.26% to 0.67–0.23%, respectively. In addition, the perovskite films with ultrasmooth top surfaces exhibited photoluminescence quantum yield > 10% and surface recombination velocities < 100 cm s−1 for both interfaces that yielded p-i-n structured solar cells with power conversion efficiency over 25%.


Highlights:
1 Demonstrating a new concept of “supermolecule confined growth” of perovskite thin films by constructing a compact, ultraflat 4-tert-butylthiacalix[4]arene capping layer atop perovskite precursor film to engineer the perovskite formation dynamics.
2 The supramolecule confined approach enabled the highly reproducible fabrication of perovskite films with a root mean square < 10 nm and electronic homogeneity, which significantly minimized the power conversion efficiency variations for both device-to-device and batch-to-batch solar cell devices.
3 The obtained perovskite films exhibited photoluminescence quantum yield > 10% and surface recombination velocities < 100 cm s−1 for both interfaces.

Keywords

Solar cells Reproducibility Perovskites Space-confined growth Supramolecules
Liu, Xinyi, Jin Xie, Ziren Zhou, Huijun Lian, Xinyuan Sui, Qing Li, Miaoyu Lin, Da Liu, Haiyang Yuan, Feng Gao, Yongzhen Wu, Hua Gui Yang, Shuang Yang, and Yu Hou. 2025. “Reproducible Fabrication of Perovskite Photovoltaics via Supramolecule Confinement Growth”. Nano-Micro Letters 18 (September):67. https://doi.org/10.1007/s40820-025-01923-w.
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References
  1. D.T. Moore, H. Sai, K.W. Tan, D.-M. Smilgies, W. Zhang et al., Crystallization kinetics of organic–inorganic trihalide perovskites and the role of the lead anion in crystal growth. J. Am. Chem. Soc. 137(6), 2350–2358 (2015). https://doi.org/10.1021/ja512117e
  2. C.M.M. Soe, G.P. Nagabhushana, R. Shivaramaiah, H. Tsai, W. Nie et al., Structural and thermodynamic limits of layer thickness in 2D halide perovskites. Proc. Natl. Acad. Sci. U.S.A. 116(1), 58–66 (2019). https://doi.org/10.1073/pnas.1811006115
  3. D. He, P. Chen, J.A. Steele, Z. Wang, H. Xu et al., Homogeneous 2D/3D heterostructured tin halide perovskite photovoltaics. Nat. Nanotechnol. 20(6), 779–786 (2025). https://doi.org/10.1038/s41565-025-01905-4
  4. Z. Wu, S. Sang, J. Zheng, Q. Gao, B. Huang et al., Crystallization kinetics of hybrid perovskite solar cells. Angew. Chem. Int. Ed. 63(17), e202319170 (2024). https://doi.org/10.1002/anie.202319170
  5. S. Li, Y. Xiao, R. Su, W. Xu, D. Luo et al., Coherent growth of high-Miller-index facets enhances perovskite solar cells. Nature 635, 874–881 (2024). https://doi.org/10.1038/s41586-024-08159-5
  6. N. Li, X. Niu, L. Li, H. Wang, Z. Huang et al., Liquid medium annealing for fabricating durable perovskite solar cells with improved reproducibility. Science 373(6554), 561–567 (2021). https://doi.org/10.1126/science.abh3884
  7. D. Liu, Y. Zheng, X.Y. Sui, X.F. Wu, C. Zou et al., Universal growth of perovskite thin monocrystals from high solute flux for sensitive self-driven X-ray detection. Nat. Commun. 15(1), 2390 (2024). https://doi.org/10.1038/s41467-024-46712-y
  8. Y. Huang, W. Zhang, Y. Xiong, Z. Yi, C. Huang et al., Recent advancements in ambient-air fabrication of perovskite solar cells. Exploration 5(3), 20240121 (2025). https://doi.org/10.1002/exp.20240121
  9. Q. Chang, P. He, H. Huang, Y. Peng, X. Han et al., Modified near-infrared annealing enabled rapid and homogeneous crystallization of perovskite films for efficient solar modules. Nano-Micro Lett. 17(1), 272 (2025). https://doi.org/10.1007/s40820-025-01792-3
  10. P. Wang, X. Zhang, Y. Zhou, Q. Jiang, Q. Ye et al., Solvent-controlled growth of inorganic perovskite films in dry environment for efficient and stable solar cells. Nat. Commun. 9(1), 2225 (2018). https://doi.org/10.1038/s41467-018-04636-4
  11. S. Wang, W. Tian, Z. Cheng, X. Shi, W. Fan et al., Fluorinated isopropanol for improved defect passivation and reproducibility in perovskite solar cells. Nat. Energy (2025). https://doi.org/10.1038/s41560-025-01791-z
  12. J. Xiu, B. Han, H. Gao, X. Chen, Z. Chen et al., A sustainable approach using nanocrystals functionalized green alkanes as efficient antisolvents to fabricate high-quality perovskite films. Adv. Energy Mater. 13(28), 2300566 (2023). https://doi.org/10.1002/aenm.202300566
  13. Q. Li, Y. Zheng, H. Wang, X. Liu, M. Lin et al., Graphene-polymer reinforcement of perovskite lattices for durable solar cells. Science 387(6738), 1069–1077 (2025). https://doi.org/10.1126/science.adu5563
  14. P. You, G. Li, G. Tang, J. Cao, F. Yan, Ultrafast laser-annealing of perovskite films for efficient perovskite solar cells. Energy Environ. Sci. 13(4), 1187–1196 (2020). https://doi.org/10.1039/c9ee02324k
  15. W. Feng, X. Liu, G. Liu, G. Yang, Y. Fang et al., Blade-coating (100)-oriented α-FAPbI(3) perovskite films via crystal surface energy regulation for efficient and stable inverted perovskite photovoltaics. Angew. Chem. Int. Ed. 63(39), e202403196 (2024). https://doi.org/10.1002/anie.202403196
  16. H. Liu, H. Wu, Z. Zhou, L. Ren, Y. Yang et al., Simultaneous mechanical and chemical synthesis of long-range-ordered perovskites. Nat. Synth. 4(2), 196–208 (2025). https://doi.org/10.1038/s44160-024-00687-2
  17. Z. Yi, X. Li, Y. Xiong, G. Shen, W. Zhang et al., Self-assembled monolayers (SAMs) in inverted perovskite solar cells and their tandem photovoltaics application. Interdiscip. Mater. 3, 203–244 (2024). https://doi.org/10.1002/idm2.12145
  18. L.E. Lehner, S. Demchyshyn, K. Frank, A. Minenkov, D.J. Kubicki et al., Elucidating the origins of high preferential crystal orientation in quasi-2D perovskite solar cells. Adv. Mater. 35(5), e2208061 (2023). https://doi.org/10.1002/adma.202208061
  19. D. Cui, X. Liu, T. Wu, X. Lin, X. Luo et al., Making room for growing oriented FASnI3 with large grains via cold precursor solution. Adv. Funct. Mater. 31(25), 2100931 (2021). https://doi.org/10.1002/adfm.202100931
  20. J. Wang, J. Huang, M. Abdel-Shakour, T. Liu, X. Wang et al., Colloidal zeta potential modulation as a handle to control the crystallization kinetics of tin halide perovskites for photovoltaic applications. Angew. Chem. Int. Ed. 63(17), e202317794 (2024). https://doi.org/10.1002/anie.202317794
  21. Z. Fang, B. Deng, Y. Jin, L. Yang, L. Chen et al., Surface reconstruction of wide-bandgap perovskites enables efficient perovskite/silicon tandem solar cells. Nat. Commun. 15(1), 10554 (2024). https://doi.org/10.1038/s41467-024-54925-4
  22. Y. Xiong, Z. Yi, W. Zhang, Y. Huang, Z. Zhang et al., Recent advances in perovskite/Cu(In,Ga)Se2 tandem solar cells. Mater. Today Electron. 7, 100086 (2024). https://doi.org/10.1016/j.mtelec.2023.100086
  23. B. Ge, H.W. Qiao, Z.Q. Lin, Z.R. Zhou, A.P. Chen et al., Deepening the valance band edges of NiOx contacts by alkaline earth metal doping for efficient perovskite photovoltaics with high open-circuit voltage. Sol. RRL 3(8), 1900192 (2019). https://doi.org/10.1002/solr.201900192
  24. D. Koo, Y. Cho, U. Kim, G. Jeong, J. Lee et al., High-performance inverted perovskite solar cells with operational stability via n-type small molecule additive-assisted defect passivation. Adv. Energy Mater. 10(46), 2001920 (2020). https://doi.org/10.1002/aenm.202001920
  25. G. Kresse, J. Hafner, Ab initiomolecular dynamics for liquid metals. Phys. Rev. B 47(1), 558–561 (1993). https://doi.org/10.1103/physrevb.47.558
  26. G. Kresse, J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54(16), 11169–11186 (1996). https://doi.org/10.1103/physrevb.54.11169
  27. G. Kresse, J. Furthmüller, Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6(1), 15–50 (1996). https://doi.org/10.1016/0927-0256(96)00008-0
  28. G. Kresse, D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59(3), 1758–1775 (1999). https://doi.org/10.1103/physrevb.59.1758
  29. S. Grimme, Semiempirical GGA-type density functional constructed with a long-range dispersion correction. J. Comput. Chem. 27(15), 1787–1799 (2006). https://doi.org/10.1002/jcc.20495
  30. P.C. Rusu, G. Giovannetti, G. Brocks, Dipole formation at interfaces of alkanethiolate self-assembled monolayers and Ag(111). J. Phys. Chem. C 111(39), 14448–14456 (2007). https://doi.org/10.1021/jp073420k
  31. M.J. Frisch et al., Gaussian 09, Revision B. 01. Gaussian, Inc., Wallingford (2010).
  32. C. Lee, W. Yang, R. Parr, Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density. Phys. Rev. B 37(2), 785–789 (1988). https://doi.org/10.1103/physrevb.37.785
  33. R. Ditchfield, W.J. Hehre, J.A. Pople, Self-consistent molecular-orbital methods. IX. An extended Gaussian-type basis for molecular-orbital studies of organic molecules. J. Chem. Phys. 54(2), 724–728 (1971). https://doi.org/10.1063/1.1674902
  34. B. Xu, T.M. Swager, Rigid bowlic liquid crystals based on tungsten-oxo Calix [4] arenes: host-guest effects and head-to-tail organization. J. Am. Chem. Soc. 115(3), 1159–1160 (1993). https://doi.org/10.1021/ja00056a056
  35. J. Rebek Jr., Host–guest chemistry of calixarene capsules. Chem. Commun. 8, 637–643 (2000). https://doi.org/10.1039/a910339m
  36. M.O. Vysotsky, V. Böhmer, I. Thondorf, Hydrogen bonded calixarene capsules kinetically stable in DMSO. Chem. Commun. 18, 1890–1891 (2001). https://doi.org/10.1039/b105613c
  37. N. Mozhzhukhina, L.P. Méndez De Leo, E.J. Calvo, Infrared spectroscopy studies on stability of dimethyl sulfoxide for application in a Li–air battery. J. Phys. Chem. C 117(36), 18375–18380 (2013). https://doi.org/10.1021/jp407221c
  38. J. Xu, A. Buin, A.H. Ip, W. Li, O. Voznyy et al., Perovskite-fullerene hybrid materials suppress hysteresis in planar diodes. Nat. Commun. 6, 7081 (2015). https://doi.org/10.1038/ncomms8081
  39. C.-H. Chiang, C.-G. Wu, Bulk heterojunction perovskite–PCBM solar cells with high fill factor. Nat. Photonics 10(3), 196–200 (2016). https://doi.org/10.1038/nphoton.2016.3
  40. Y. Wu, X. Yang, W. Chen, Y. Yue, M. Cai et al., Perovskite solar cells with 18.21% efficiency and area over 1 cm2 fabricated by heterojunction engineering. Nat. Energy 1(11), 16148 (2016). https://doi.org/10.1038/nenergy.2016.148
  41. A. Amat, E. Mosconi, E. Ronca, C. Quarti, P. Umari et al., Cation-induced band-gap tuning in organohalide perovskites: interplay of spin–orbit coupling and octahedra tilting. Nano Lett. 14(6), 3608–3616 (2014). https://doi.org/10.1021/nl5012992
  42. S. Liu, J. Li, W. Xiao, R. Chen, Z. Sun et al., Buried interface molecular hybrid for inverted perovskite solar cells. Nature 632(8025), 536–542 (2024). https://doi.org/10.1038/s41586-024-07723-3
  43. P. Ferdowsi, U. Steiner, J.V. Milić, Host-guest complexation in hybrid perovskite optoelectronics. J. Phys. Mater. 4(4), 042011 (2021). https://doi.org/10.1088/2515-7639/ac299f
  44. H. Zhang, F.T. Eickemeyer, Z. Zhou, M. Mladenović, F. Jahanbakhshi et al., Multimodal host-guest complexation for efficient and stable perovskite photovoltaics. Nat. Commun. 12(1), 3383 (2021). https://doi.org/10.1038/s41467-021-23566-2
  45. Y. Zhu, X. Liu, X. Sui, G. Chen, Q. Li et al., Intermediate-phase homogenization through intermolecular interactions toward reproducible fabrication of perovskite solar cells. Adv. Energy Mater. 15(29), 2500536 (2025). https://doi.org/10.1002/aenm.202500536
  46. J. Zhang, R. Dai, J. Yang, Y. Liu, J. Yu et al., Regulation of crystallization by introducing a multistage growth template affords efficient and stable inverted perovskite solar cells. Energy Environ. Sci. 18(7), 3235–3247 (2025). https://doi.org/10.1039/D4EE06199C
  47. S. Chen, X. Xiao, B. Chen, L.L. Kelly, J. Zhao et al., Crystallization in one-step solution deposition of perovskite films: upward or downward? Sci. Adv. 7(4), eabb2412 (2021). https://doi.org/10.1126/sciadv.abb2412
  48. X. Zheng, Y. Hou, C. Bao, J. Yin, F. Yuan et al., Managing grains and interfaces via ligand anchoring enables 22.3%-efficiency inverted perovskite solar cells. Nat. Energy 5(2), 131–140 (2020). https://doi.org/10.1038/s41560-019-0538-4
  49. J. Wang, L. Bi, X. Huang, Q. Feng, M. Liu et al., Bilayer interface engineering through 2D/3D perovskite and surface dipole for inverted perovskite solar modules. eScience 4(6), 100308 (2024). https://doi.org/10.1016/j.esci.2024.100308
  50. Y. Wang, B. Li, H. Wang, Z. Zhang, Z. Dang et al., A soft nonpolar-soluble two-dimensional perovskite for general construction of mixed-dimensional heterojunctions. Adv. Mater. 37(14), e2419750 (2025). https://doi.org/10.1002/adma.202419750
  51. J. Wang, W. Fu, S. Jariwala, I. Sinha, A.K.Y. Jen et al., Reducing surface recombination velocities at the electrical contacts will improve perovskite photovoltaics. ACS Energy Lett. 4(1), 222–227 (2019). https://doi.org/10.1021/acsenergylett.8b02058
  52. B. Chen, H. Chen, Y. Hou, J. Xu, S. Teale et al., Passivation of the buried interface via preferential crystallization of 2D perovskite on metal oxide transport layers. Adv. Mater. 33(41), e2103394 (2021). https://doi.org/10.1002/adma.202103394
  53. Y. Yang, M. Yang, D.T. Moore, Y. Yan, E.M. Miller et al., Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films. Nat. Energy 2(2), 16207 (2017). https://doi.org/10.1038/nenergy.2016.207
  54. J. Wu, R. Zhu, G. Li, Z. Zhang, J. Pascual et al., Inhibiting interfacial nonradiative recombination in inverted perovskite solar cells with a multifunctional molecule. Adv. Mater. 36(35), e2407433 (2024). https://doi.org/10.1002/adma.202407433
  55. X. Zhang, F. Liu, Y. Guan, Y. Zou, C. Wu et al., Reducing the Voc loss of hole transport layer-free carbon-based perovskite solar cells via dual interfacial passivation. Nano-Micro Lett. 17(1), 258 (2025). https://doi.org/10.1007/s40820-025-01775-4
  56. H. Kanda, N. Shibayama, A.J. Huckaba, Y. Lee, S. Paek et al., Band-bending induced passivation: high performance and stable perovskite solar cells using a perhydropoly(silazane) precursor. Energy Environ. Sci. 13(4), 1222–1230 (2020). https://doi.org/10.1039/C9EE02028D
  57. M. Stolterfoht, P. Caprioglio, C.M. Wolff, J.A. Márquez, J. Nordmann 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(9), 2778–2788 (2019). https://doi.org/10.1039/C9EE02020A
  58. F. Ye, S. Zhang, J. Warby, J. Wu, E. Gutierrez-Partida et al., Overcoming C(60)-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane. Nat. Commun. 13(1), 7454 (2022). https://doi.org/10.1038/s41467-022-34203-x
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