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Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells

Abstract

The performance of perovskite solar cells is predominantly limited by non-radiative recombination, either through trap-assisted recombination in the absorber layer or via minority carrier recombination at the perovskite/transport layer interfaces. Here, we use transient and absolute photoluminescence imaging to visualize all non-radiative recombination pathways in planar pin-type perovskite solar cells with undoped organic charge transport layers. We find significant quasi-Fermi-level splitting losses (135 meV) in the perovskite bulk, whereas interfacial recombination results in an additional free energy loss of 80 meV at each individual interface, which limits the open-circuit voltage (VOC) of the complete cell to ~1.12 V. Inserting ultrathin interlayers between the perovskite and transport layers leads to a substantial reduction of these interfacial losses at both the p and n contacts. Using this knowledge and approach, we demonstrate reproducible dopant-free 1 cm2 perovskite solar cells surpassing 20% efficiency (19.83% certified) with stabilized power output, a high VOC (1.17 V) and record fill factor (>81%).

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Fig. 1: Schematic device architecture and energetics.
Fig. 2: Optimization of electrode design.
Fig. 3: Impact of transport layers on kinetics of charge recombination.
Fig. 4: Visualization of non-radiative interfacial recombination through absolute photoluminescence imaging.
Fig. 5: Suppression of interfacial recombination through interlayers.
Fig. 6: 20% efficient pin-type perovskite cells with 1 cm2 active area.

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Acknowledgements

We thank P. Caprioglio for SEM measurements, L. Fiedler for laboratory assistance and F. Jaiser, F. Dornack and A. Pucher for providing measurement and laboratory equipment. P.M. is a Sêr Cymru Research Chair funded by the Welsh European Funding Office (Sêr Cymru II Program) and is formerly an Australian Research Council Discovery Outstanding Researcher Award Fellow. P.L.B is an Australian Research Council Laureate Fellow (FL160100067). S.Z is partly funded by a Chinese Scholarship Council studentship and the Australian Government through the Australian Renewable Energy Agency (ARENA) Australian Centre for Advanced Photovoltaics. Responsibility for the views, information or advice expressed herein is not accepted by the Australian Government. We thank M. Harvey and Brisbane Materials Technology Pty Ltd for the provision of their proprietary anti-reflection coating formulation. J.A.M. acknowledges A. Redinger for fruitful discussions. S.A. acknowledges funding from the German Federal Ministry of Education and Research (BMBF), within the project ‘Materialforschung für die Energiewende’ (grant no. 03SF0540), and the German Federal Ministry for Economic Affairs and Energy (BMWi) through the ‘PersiST’ project (grant no. 0324037C). Support by the joint University Potsdam–HZB graduate school ‘hypercells’ is acknowledged.

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M.S. planned the project together with C.M.W. and D.N., drafted the manuscript and reviewer response, fabricated most cells and films with help of S.Z. and D.R., performed electrical measurements, measured TRPL with C.J.H. and absolute PL on FAPI cells. C.M.W. provided main conceptual ideas regarding the identification of the recombination losses, contributed to device fabrication and TRPL measurements, and performed coupled optical and Shockley–Queisser modelling. J.A.M. performed all hyperspectral PL measurements and performed corresponding data analysis and interpretation. S.Z. helped with device optimization and fabrication. C.J.H. performed fluence- and wavelength-dependent TRPL measurements and analysed data. T.U. performed numerical drift diffusion simulations with SCAPS1D and analysed and interpreted the optical measurements. D.R. fabricated certified 1 cm2 cells with M.S., as well as MAPI/FAPI cells and films. D.N. supervised the study, analysed and interpreted all electrical and optical measurements, and contributed to manuscript drafting. All co-authors contributed to data analysis, interpretation, proof reading and addressing reviewer comments.

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Correspondence to Martin Stolterfoht or Thomas Unold or Dieter Neher.

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Supplementary Figures 1–18, Supplementary Tables 1–2, Supplementary Note 1, Supplementary References

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Stolterfoht, M., Wolff, C.M., Márquez, J.A. et al. Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells. Nat Energy 3, 847–854 (2018). https://doi.org/10.1038/s41560-018-0219-8

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