Abstract
Metal halide perovskite solar cells (PSCs) represent a promising low-cost thin-film photovoltaic technology, with unprecedented power conversion efficiencies obtained for both single-junction and tandem applications1,2,3,4,5,6,7,8. To push PSCs towards commercialization, it is critical, albeit challenging, to understand device reliability under real-world outdoor conditions where multiple stress factors (for example, light, heat and humidity) coexist, generating complicated degradation behaviours9,10,11,12,13. To quickly guide PSC development, it is necessary to identify accelerated indoor testing protocols that can correlate specific stressors with observed degradation modes in fielded devices. Here we use a state-of-the-art positive-intrinsic-negative (p–i–n) PSC stack (with power conversion efficiencies of up to approximately 25.5%) to show that indoor accelerated stability tests can predict our six-month outdoor ageing tests. Device degradation rates under illumination and at elevated temperatures are most instructive for understanding outdoor device reliability. We also find that the indium tin oxide/self-assembled monolayer-based hole transport layer/perovskite interface most strongly affects our device operation stability. Improving the ion-blocking properties of the self-assembled monolayer hole transport layer increases averaged device operational stability at 50 °C–85 °C by a factor of about 2.8, reaching over 1,000 h at 85 °C and to near 8,200 h at 50 °C, with a projected 20% degradation, which is among the best to date for high-efficiency p–i–n PSCs14,15,16,17.
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The data that support the findings of this study are available from the corresponding authors on reasonable request.
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Acknowledgements
The work was authored in part by the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the US Department of Energy (DOE) under contract no. DE-AC36-08GO28308. We acknowledge the support on examining stability protocols from DE-FOA-0002064 and award no. DE-EE0008790, and the support on general device fabrication, characterization and testing from the Advanced Perovskite Cells and Modules programme of the National Center for Photovoltaics, funded by the US Department of Energy Office of Energy Efficiency and Renewable Energy, Solar Energy Technologies Office. We also acknowledge the support on first-principle calculations from the Center for Hybrid Organic–Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the DOE. The DFT calculations were performed using computational resources sponsored by the DOE’s Office of Energy Efficiency and Renewable Energy and located at the National Renewable Energy Laboratory, and the DOS calculations used resources of the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under contract no. DE-AC02-05CH11231 using NERSC award BES-ERCAP0017591. We would like to thank C. Velez and A. F. Palmstrom for support on atomic layer depositions, and B. W. Stevens for support on e-beam evaporation of metal feed through for packaging devices. The views expressed in the article do not necessarily represent the views of the DOE or the US Government. The US Government retains, and the publisher, by accepting the article for publication, acknowledges that the US Government retains, a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for US Government purposes.
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Q.J. and K.Z. conceived the idea. Q.J. fabricated perovskite solar cells and conducted device efficiency measurements. R.T. conducted device operational stability measurements at different temperatures under the supervision of J.J.B. Q.J. packaged the devices for outdoor operation, damp heat, and thermal cycling studies, with guidance and help from E.A.G. R.A.K. conducted electrochemical measurements and analysis. J.M.N. conducted the thermal cycling study and UV stress study. Y.X. and X.W. conducted the DFT calculation and analysis under the supervision of Y.Y. Q.J. and K.Z. wrote the first draft of the manuscript. All authors discussed the results and contributed to the revisions of the manuscript.
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Extended data figures and tables
Extended Data Fig. 1 Statistical analysis of stability testing protocols.
a, Analysis of different protocols used in recent publications as summarized in Supplementary Table 1. Of the various ISOS stability testing protocols, the published literature clearly focuses on the operational protocol. b, The temperatures used for operational stability vary across a wide range, with most such tests conducted at room temperature.
Extended Data Fig. 2 Device performance certification.
The certification results of a representative device measured by an accredited independent photovoltaic (PV) calibration and measurement laboratory (Japan Electrical Safety and Environment Technology Laboratories, JET). The device shows a stabilized power conversion efficiency (PCE) of 24.3%.
Extended Data Fig. 3 Photograph of a representative packaged device.
A calcium flake (indicated by the red circle) deposited onto PET flexible substrate was placed inside the package as a sensor to monitor moisture ingress.
Extended Data Fig. 4 Typical operational stability of PSCs at different temperatures.
a–e, Operational stability tests with the temperature controlled at 25 °C (a), 33 °C (b), 50 °C (c), 65 °C (d), and 85 °C (e), respectively. Both reverse and forward J–V scan results are used as indicated.
Extended Data Fig. 5 Effect of light intensity and temperature on PSC performance.
a–d, Effect of changing AM1.5 G illumination intensity (0.25 to 1.0 suns) on the J–V curves (a), output power (b), short-circuit current density Jsc (c), and open-circuit voltage (Voc) (d) for a typical PSC. e, Effect of varying operational temperature on the PCE of PSCs. The temperature coefficient is k = −0.077%/K.
Extended Data Fig. 6 Simulated diurnal cycle study.
a, b, Two typical examples are shown in (a) and (b), respectively. The diurnal cycle was simulated by using repeated 12-hour light on and 12-hour light off cycles. The temperature was controlled at approximately 35 °C.
Extended Data Fig. 7 UV stress study.
a, UV exposure using the lamp UVA-340, with 1 W/m2/nm at 340 nm. The error bars represent the standard deviations from 6 individual cells. b, UV exposure using a 4-W UV lamp, 365 nm wavelength. The error bars represent the standard deviations from 12 individual cells.
Extended Data Fig. 8 SAM comparison.
a, Configuration of H2O molecule binding with MeO-2PACz and Me-4PACz molecules. b, Configuration of MeO-2PACz and Me-4PACz molecules on perovskite (100) surface. c, Potentiostatic current density–time (J-t) plots for the indicated ITO/HTL held at −1.05 V versus Ag|AgCl in a 0.2-M methylammonium chloride (MACl) aqueous electrolyte, just above the threshold to induce MA-mediated In3+ → In0 reduction. d, e, Photographs comparing perovskite deposition on top of Me-4PACz and mixed MeO-2PACz and Me-4PACz on patterned (d) and nonpatterned (e) ITO substrates.
Extended Data Fig. 9 J–V measurement and maximum power point tracking (MPPT) of a typical packaged PSC.
The measurements were conducted prior to outdoor test and after 16 weeks of outdoor aging.
Extended Data Fig. 10 Typical spectrum of white LED-based solar simulator.
This lamp was used for indoor, temperature-dependent stability tests.
Supplementary information
Supplementary Information
Supplementary Table 1.
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Jiang, Q., Tirawat, R., Kerner, R.A. et al. Towards linking lab and field lifetimes of perovskite solar cells. Nature 623, 313–318 (2023). https://doi.org/10.1038/s41586-023-06610-7
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DOI: https://doi.org/10.1038/s41586-023-06610-7
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