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Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells

Nature Nanotechnology volume 9, pages 927–932 (2014)Cite this article

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Abstract

Perovskite solar cells with submicrometre-thick CH3NH3PbI3 or CH3NH3PbI3–xClx active layers show a power conversion efficiency as high as 15%. However, compared to the best-performing device, the average efficiency was as low as 12%, with a large standard deviation (s.d.). Here, we report perovskite solar cells with an average efficiency exceeding 16% and best efficiency of 17%. This was enabled by the growth of CH3NH3PbI3 cuboids with a controlled size via a two-step spin-coating procedure. Spin-coating of a solution of CH3NH3I with different concentrations follows the spin-coating of PbI2, and the cuboid size of CH3NH3PbI3 is found to strongly depend on the concentration of CH3NH3I. Light-harvesting efficiency and charge-carrier extraction are significantly affected by the cuboid size. Under simulated one-sun illumination, average efficiencies of 16.4% (s.d. ± 0.35), 16.3% (s.d. ± 0.44) and 13.5% (s.d. ± 0.34) are obtained from solutions of CH3NH3I with concentrations of 0.038 M, 0.050 M and 0.063 M, respectively. By controlling the size of the cuboids of CH3NH3PbI3 during their growth, we achieved the best efficiency of 17.01% with a photocurrent density of 21.64 mA cm–2, open-circuit photovoltage of 1.056 V and fill factor of 0.741.

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Figure 1: Two-step spin-coating procedure for CH3NH3PbI3 cuboids.
Figure 2: Surface cross-sectional scanning electron microscopy images and dependence of MAPbI3 cuboid size on CH3NH3I concentration.
Figure 3: MAPbI3 nucleation, crystal growth and cell configuration.
Figure 4: Effects of MAPbI3 cuboid size on photovoltaic parameters, light-harvesting efficiency and photo-CELIV transients.
Figure 5: Current density–voltage curve and incident photon-to-electron conversion efficiency values for the best-performing device.

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Acknowledgements

This work was supported by National Research Foundation of Korea (NRF) grants, funded by the Ministry of Science, ICT & Future Planning (MSIP) of Korea under contracts nos. NRF-2010-0014992, NRF-2012M1A2A2671721, NRF-2012M3A7B4049986 (Nano Material Technology Development Program) and NRF-2012M3A6A7054861 (Global Frontier R&D Program on Center for Multiscale Energy System). M.G. acknowledges an Advanced Research Grant (ARG 247404) from the European Research Council (ERC), funded under the ‘Mesolight’ project.

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Authors and Affiliations

  1. School of Chemical Engineering and Department of Energy Science, Sungkyunkwan University, Suwon, 440-746, Korea

    Jeong-Hyeok Im, In-Hyuk Jang & Nam-Gyu Park

  2. Laboratory for Photonics and Interfaces, Institute of Chemical Sciences and Engineering, School of Basic Sciences, Ecole Polytechnique Fédérale de Lausanne, Lausanne, CH-1015, Switzerland

    Norman Pellet & Michael Grätzel

  3. Max-Planck-Institute for Solid-State Research, Heisenbergstrasse 1, Stuttgart, 70569, Germany

    Norman Pellet

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Contributions

N.G.P. conceived the experiments, performed data analysis and prepared the manuscript. J.H.I. and I.H.J. prepared materials, fabricated devices and characterized device structure and performance. M.G. analysed optical and IPCE data and edited the manuscript. N.P. measured light-harvesting efficiency and photo-CELIV. All authors discussed the results and commented on the manuscript.

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Correspondence to Michael Grätzel or Nam-Gyu Park.

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Im, JH., Jang, IH., Pellet, N. et al. Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells. Nature Nanotech 9, 927–932 (2014). https://doi.org/10.1038/nnano.2014.181

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