Letter | Published:

A solvent- and vacuum-free route to large-area perovskite films for efficient solar modules

Nature volume 550, pages 9295 (05 October 2017) | Download Citation



Recent advances in the use of organic–inorganic hybrid perovskites for optoelectronics have been rapid, with reported power conversion efficiencies of up to 22 per cent for perovskite solar cells1,2,3,4,5,6,7,8,9. Improvements in stability have also enabled testing over a timescale of thousands of hours10,11,12,13,14. However, large-scale deployment of such cells will also require the ability to produce large-area, uniformly high-quality perovskite films. A key challenge is to overcome the substantial reduction in power conversion efficiency when a small device is scaled up: a reduction from over 20 per cent to about 10 per cent is found15,16,17,18,19,20,21 when a common aperture area of about 0.1 square centimetres is increased to more than 25 square centimetres. Here we report a new deposition route for methyl ammonium lead halide perovskite films that does not rely on use of a common solvent1,2,4,5,6,7,8,9,10,11,12,13,14,15 or vacuum3: rather, it relies on the rapid conversion of amine complex precursors to perovskite films, followed by a pressure application step. The deposited perovskite films were free of pin-holes and highly uniform. Importantly, the new deposition approach can be performed in air at low temperatures, facilitating fabrication of large-area perovskite devices. We reached a certified power conversion efficiency of 12.1 per cent with an aperture area of 36.1 square centimetres for a mesoporous TiO2-based perovskite solar module architecture.

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  1. 1.

    , , & Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. J. Am. Chem. Soc. 131, 6050–6051 (2009)

  2. 2.

    et al. Sequential deposition as a route to high-performance perovskite-sensitized solar cells. Nature 499, 316–319 (2013)

  3. 3.

    , & Efficient planar heterojunction perovskite solar cells by vapour deposition. Nature 501, 395–398 (2013)

  4. 4.

    et al. Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells. Nat. Mater. 13, 897–903 (2014)

  5. 5.

    et al. A vacuum flash-assisted solution process for high-efficiency large-area perovskite solar cells. Science 353, 58–62 (2016)

  6. 6.

    et al. Interface engineering of highly efficient perovskite solar cells. Science 345, 542–546 (2014)

  7. 7.

    et al. Compositional engineering of perovskite materials for high-performance solar cells. Nature 517, 476–480 (2015)

  8. 8.

    et al. High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science 348, 1234–1237 (2015)

  9. 9.

    et al. Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat. Energy 1, 16142 (2016)

  10. 10.

    et al. A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability. Science 345, 295–298 (2014)

  11. 11.

    et al. Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance. Science 354, 206–209 (2016)

  12. 12.

    et al. Improved performance and stability of perovskite solar cells by crystal crosslinking with alkylphosphonic acid omega-ammonium chlorides. Nat. Chem. 7, 703–711 (2015)

  13. 13.

    et al. Improving efficiency and stability of perovskite solar cells with photocurable fluoropolymers. Science 354, 203–206 (2016)

  14. 14.

    et al. Diffusion engineering of ions and charge carriers for stable efficient perovskite solar cells. Nat. Commun. 8, 15330 (2017)

  15. 15.

    et al. Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers. Science 350, 944–948 (2015)

  16. 16.

    et al. Solid-state solar modules based on mesoscopic organometal halide perovskite: a route towards the up-scaling process. Phys. Chem. Chem. Phys. 16, 3918–3923 (2014)

  17. 17.

    et al. Nonhazardous solvent systems for processing perovskite photovoltaics. Adv. Energy Mater. 6, 1600386 (2016)

  18. 18.

    et al. Pinhole-free perovskite films for efficient solar modules. Energy Environ. Sci. 9, 484–489 (2016)

  19. 19.

    et al. High efficiency photovoltaic module based on mesoscopic organometal halide perovskite. Prog. Photovolt. Res. Appl. 24, 436–445 (2016)

  20. 20.

    et al. Perovskite solar cells and large area modules (100 cm2) based on an air flow-assisted PbI2 blade coating deposition process. J. Power Sources 277, 286–291 (2015)

  21. 21.

    et al. Stable large-area (10 × 10 cm2) printable mesoscopic perovskite module exceeding 10% efficiency. Sol. RRL 1, 1600019 (2017)

  22. 22.

    , , , & Formation dynamics of CH3NH3PbI3 perovskite following two-step layer deposition. J. Phys. Chem. Lett. 7, 96–102 (2016)

  23. 23.

    , , & FTIR study of adsorption and reactions of methylamine on powdered TiO2. J. Phys. Chem. B 105, 5928–5934 (2001)

  24. 24.

    , & Infrared studies of sub-monolayer methylamine and trimethylamine adsorption on Ni(111). Surf. Sci. 427–428, 282–287 (1999)

  25. 25.

    et al. Persistent dopants and phase segregation in organolead mixed-halide perovskites. Chem. Mater. 28, 6848–6859 (2016)

  26. 26.

    et al. Long-range balanced electron- and hole-transport lengths in organic-inorganic CH3NH3PbI3. Science 342, 344–347 (2013)

  27. 27.

    et al. Methylamine-gas-induced defect-healing behavior of CH3NH3PbI3 thin films for perovskite solar cells. Angew. Chem. Int. Ed. 54, 9705–9709 (2015)

  28. 28.

    et al. Soft-cover deposition of scaling-up uniform perovskite thin films for high cost-performance solar cells. Energy Environ. Sci. 9, 2295–2301 (2016)

  29. 29.

    et al. Solvent annealing of perovskite-induced crystal growth for photovoltaic-device efficiency enhancement. Adv. Mater. 26, 6503–6509 (2014)

  30. 30.

    et al. Solar cell efficiency tables (version 49). Prog. Photovolt. Res. Appl. 25, 3–13 (2017)

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This work was supported by the National Natural Science Foundation of China (grant nos 11574199 and 11674219), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Natural Science Foundation of Shanghai (17ZR1414800). We thank B. Dai from Instrumental Analysis Center of SJTU and G. Lu from Shanghai Institute of Organic Chemistry for NMR measurements, and Y. Wu for discussions. M.G. thanks the European Research Council (ERC) for support of this work under a Proof of Concept project associated with his Mesolight Advanced Research Grant (ARF).

Author information

Author notes

    • Han Chen
    • , Fei Ye
    •  & Wentao Tang

    These authors contributed equally to this work.


  1. State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, 800 Dong Chuan Road, Minhang District, Shanghai 200240, China

    • Han Chen
    • , Fei Ye
    • , Wentao Tang
    • , Jinjin He
    • , Maoshu Yin
    • , Yanbo Wang
    • , Xudong Yang
    •  & Liyuan Han
  2. Research Network and Facility Services Division, National Institute for Materials Science, Tsukuba, Ibaraki 305-0047, Japan

    • Fengxian Xie
    •  & Liyuan Han
  3. Suzhou Liyuan New Energy Technology Co., M1, 2 Peiyuan Road, Hi-tech Industrial Development Zone, Suzhou, China

    • Enbing Bi
  4. Laboratory of Photonics and Interfaces, Institute of Chemical and Engineering Science, Swiss Federal Institute of Technology, Station 6, CH-1015 Lausanne, Switzerland

    • Michael Grätzel


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L.H. and X.Y. designed and directed the study. H.C., F.Y. and W.T. conceived and performed the main experimental work. J.H., M.Y., Y.W., F.X. and E.B. contributed to the characterization. X.Y., H.C., F.Y. and W.T. analysed the data. X.Y., M.G. and L.H. wrote the manuscript. All authors reviewed the paper.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to Xudong Yang or Liyuan Han.

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