Perovskite solar cells are remarkably efficient; however, they are prone to degradation in water, oxygen and ultraviolet light. Cation engineering in 3D perovskite absorbers has led to reduced degradation. Alternatively, 2D Ruddlesden–Popper layered perovskites exhibit improved stability, but have not delivered efficient solar cells so far. Here, we introduce n-butylammonium cations into a mixed-cation lead mixed-halide FA0.83Cs0.17Pb(IyBr1−y)3 3D perovskite. We observe the formation of 2D perovskite platelets, interspersed between highly orientated 3D perovskite grains, which suppress non-radiative charge recombination. We investigate the relationship between thin-film composition, crystal alignment and device performance. Solar cells with an optimal butylammonium content exhibit average stabilized power conversion efficiency of 17.5 ± 1.3% with a 1.61-eV-bandgap perovskite and 15.8 ± 0.8% with a 1.72-eV-bandgap perovskite. The stability under simulated sunlight is also enhanced. Cells sustain 80% of their ‘post burn-in’ efficiency after 1,000 h in air, and close to 4,000 h when encapsulated.
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Ogomi, Y. et al. CH3NH3Snx Pb(1−x)I3 perovskite solar cells covering up to 1060 nm. J. Phys. Chem. Lett. 5, 1004–1011 (2014).
Noh, J. H., Im, S. H., Heo, J. H., Mandal, T. N. & Seok, S. Il. Chemical management for colorful, efficient, and stable inorganic-organic hybrid nanostructured solar cells. Nano Lett. 13, 1764–1769 (2013).
Stranks, S. D. et al. Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber. Science 342, 341–344 (2013).
Oga, H., Saeki, A., Ogomi, Y., Hayase, S. & Seki, S. Improved understanding of the electronic and energetic landscapes of perovskite solar cells: high local charge carrier mobility, reduced recombination, and extremely shallow traps. J. Am. Chem. Soc. 136, 13818–13825 (2014).
Jeon, N. J. et al. Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells. Nat. Mater. 13, 897–903 (2014).
Snaith, H. J. Perovskites: the emergence of a new era for low-cost, high-efficiency solar cells. J. Phys. Chem. Lett. 4, 3623–3630 (2013).
Yang, W. S., Park, B., Jung, E. H. & Jeon, N. J. Iodide management in formamidinium-lead-halide-based perovskite layers for efficient solar cells. Science 356, 1376–1379 (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).
Pearson, A. J. et al. Oxygen degradation in mesoporous Al2O3/CH3NH3PbI3−xClx perovskite solar cells: kinetics and mechanisms. Adv. Energy Mater. 6, 1600014 (2016).
Wang, Z. et al. Efficient and air-stable mixed-cation lead mixed-halide perovskite solar cells with n-doped organic electron extraction layers. Adv. Mater. 29, 1604186 (2016).
Aristidou, N. et al. The role of oxygen in the degradation of methylammonium lead trihalide perovskite photoactive layers. Angew. Chem. Int. Edn 54, 8208–8212 (2015).
Leguy, A. M. A. et al. Reversible hydration of CH3NH3PbI3 in films, single crystals, and solar cells. Chem. Mater. 27, 3397–3407 (2015).
Conings, B. et al. Intrinsic thermal instability of methylammonium lead trihalide perovskite. Adv. Energy Mater. 5, 1500477 (2015).
Misra, R. K. et al. Temperature- and component-dependent degradation of perovskite photovoltaic materials under concentrated sunlight. J. Phys. Chem. Lett. 6, 326–330 (2015).
McMeekin, D. P. et al. A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells. Science 351, 151–155 (2016).
Yi, C. et al. Entropic stabilization of mixed A-cation ABX 3 metal halide perovskites for high performance perovskite solar cells. Energy Environ. Sci. 9, 656–662 (2016).
Lee, J. W. et al. Formamidinium and cesium hybridization for photo- and moisture-stable perovskite solar cell. Adv. Energy Mater. 5, 1501310 (2015).
Muljarov, E. A., Tikhodeev, S. G., Gippius, N. A. & Ishihara, T. Excitons in self-organized semiconductor/insulator superlattices: PbI-based perovskite compounds. Phys. Rev. B 51, 14370–14378 (1995).
Stoumpos, C. C. et al. Ruddlesden–Popper hybrid lead iodide perovskite 2D homologous semiconductors. Chem. Mater. 28, 2852–2867 (2016).
Smith, I. C., Hoke, E. T., Solis-Ibarra, D., McGehee, M. D. & Karunadasa, H. I. A layered hybrid perovskite solar-cell absorber with enhanced moisture stability. Angew. Chem. Int. Edn 53, 11232–11235 (2014).
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).
Yao, K., Wang, X., Xu, Y. X., Li, F. & Zhou, L. Multilayered perovskite materials based on polymeric-ammonium cations for stable large-area solar cell. Chem. Mater. 28, 3131–3138 (2016).
Tsai, H. et al. High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells. Nature 536, 312–316 (2016).
Quan, L. N. et al. Ligand-stabilized reduced-dimensionality perovskites. J. Am. Chem. Soc. 138, 2649–2655 (2016).
Milot, R. L. et al. Charge-carrier dynamics in 2D hybrid metal-halide perovskites. Nano Lett. 16, 7001–7007 (2016).
Liao, Y. et al. Highly oriented low-dimensional tin halide perovskites with enhanced stability and photovoltaic performance. J. Am. Chem. Soc. 139, 6693–6699 (2017).
Quan, L. N. et al. Tailoring the energy landscape in quasi-2D halide perovskites enables efficient green light emission. Nano Lett. 17, 3701–3709 (2017).
Li, N. et al. Mixed cation FAxPEA1−xPbI3 with enhanced phase and ambient stability toward high-performance perovskite solar cells. Adv. Energy Mater. 7, 1601307 (2017).
He, B. B., Preckwinkel, U. & Smith, K. L. Comparison between conventional and two-dimensional XRD. Adv. X-Ray Anal. 46, 37–42 (2003).
Tan, K. W. et al. Thermally induced structural evolution and performance of mesoporous block copolymer-directed alumina perovskite solar cells. ACS Nano 8, 4730–4739 (2014).
Yuan, M. et al. Perovskite energy funnels for efficient light-emitting diodes. Nat. Nanotech. 11, 872–877 (2016).
Ong, H. C., Zhu, A. X. E. & Du, G. T. Dependence of the excitonic transition energies and mosaicity on residual strain in ZnO thin films. Appl. Phys. Lett. 80, 941–943 (2002).
Ko, H. J. et al. Improvement of the quality of ZnO substrates by annealing. J. Cryst. Growth 269, 493–498 (2004).
Nagao, K. & Kagami, E. X-ray thin film measurement techniques: VII. Pole figure measurement. Rigaku J. 27, 6–14 (2011).
Kieslich, G. et al. Solid-state principles applied to organic-inorganic perovskites: new tricks for an old dog. Chem. Sci. 5, 4712–4715 (2014).
Filip, M. R., Eperon, G. E., Snaith, H. J. & Giustino, F. Steric engineering of metal-halide perovskites with tunable optical band gaps. Nat. Commun. 5, 5757 (2014).
Safdari, M. et al. Layered 2D alkyldiammonium lead iodide perovskites: synthesis, characterization, and use in solar cells. J. Mater. Chem. A 4, 15638–15646 (2016).
Morozov, S. V. et al. Type II-type I conversion of GaAs/GaAsSb heterostructure energy spectrum under optical pumping. J. Appl. Phys. 113, 163107 (2013).
Van Reenen, S., Kemerink, M. & Snaith, H. J. Modeling anomalous hysteresis in perovskite solar cells. J. Phys. Chem. Lett. 6, 3808–3814 (2015).
Belisle, R. A. et al. Interpretation of inverted photocurrent transients in organic lead halide perovskite solar cells: proof of the field screening by mobile ions and determination of the space charge layer widths. Energy Environ. Sci. 10, 192–204 (2017).
Snaith, H. J. et al. Anomalous hysteresis in perovskite solar cells. J. Phys. Chem. Lett. 5, 1511–1515 (2014).
Li, W. et al. Enhanced UV-light stability of planar heterojunction perovskite solar cells with caesium bromide interface modification. Energy Environ. Sci. 9, 490–498 (2016).
Shao, Y., Xiao, Z., Bi, C., Yuan, Y. & Huang, J. Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells. Nat. Commun. 5, 5784 (2014).
Peters, C. H. et al. High efficiency polymer solar cells with long operating lifetimes. Adv. Energy Mater. 1, 491–494 (2011).
Bush, K. A. et al. 23.6%-efficient monolithic perovskite/silicon tandem solar cells with improved stability. Nat. Energy 2, 17009 (2017).
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).
Wang, Q. et al. Scaling behavior of moisture-induced grain degradation in polycrystalline hybrid perovskite thin films. Energy Environ. Sci. 10, 516–522 (2017).
Zhang, Y. et al. Two-step grain-growth kinetics of sub-7 nm SnO2 nanocrystal under hydrothermal condition. J. Phys. Chem. C 119, 19505–19512 (2015).
This work was part-funded by EPSRC, UK, the European Union Seventh Framework Program under grant agreement number 604032 of the MESO project and AFOSR through project FA9550-15-1-0115. We thank A. A. Haghighirad for discussions concerning XRD analysis, and D. P. McMeekin for discussion concerning device fabrication and film composition analysis. We would also like to thank M. T. Klug and R. Xiang for helping with illustrations.
The authors declare no competing financial interests.
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Wang, Z., Lin, Q., Chmiel, F. et al. Efficient ambient-air-stable solar cells with 2D–3D heterostructured butylammonium-caesium-formamidinium lead halide perovskites. Nat Energy 2, 17135 (2017). https://doi.org/10.1038/nenergy.2017.135
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