Publication date: 17th February 2025
Perovskite solar cells (PSCs) have emerged as a leading photovoltaic technology due to their remarkable efficiency and improved stability. However, the intricate interplay of electronic and ionic processes that dictate their performance remains poorly understood. Impedance spectroscopy (IS) provides a robust characterization approach to probe these processes across multiple time scales. Despite its potential, the coupling of recombination, charge transport, and extraction phenomena within IS responses complicates the accurate identification of dominant resistive mechanisms.
This study introduces a novel method for evaluating recombination resistance using current-voltage (j–V) curve reconstruction as a diagnostic tool. Our analysis includes four PSC configurations with varying charge extraction and recombination characteristics. By correlating fitted parameters from IS spectra with experimental j–V data, we demonstrate that recombination resistance can reliably be distinguished in systems with optimized charge extraction. Conversely, hindered charge extraction introduces significant coupling effects, masking recombination resistance within the IS-derived resistive parameters.
We validated our approach across devices employing different transport layers and selective contacts, including PEDOT:PSS and MeO-2PACz. The reconstructed j–V curves align with experimental measurements in configurations where recombination dominates, highlighting the efficacy of the method in decoupling resistive contributions. For devices with hindered charge extraction, such as those incorporating ICBA as the electron transport material, discrepancies between reconstructed and experimental j–V curves underscore the influence of transport resistance.
These findings emphasize the necessity of precise identification and decoupling of physical processes within IS spectra for advancing PSC diagnostics. The study contributes to a deeper understanding of the operational dynamics in perovskite photovoltaics, paving the way for enhanced device design and optimization.
This research represents a significant step toward the commercialization of PSCs, offering tools for improved characterization and performance evaluation critical to their long-term viability.
P. F. B. acknowledges his grant CIACIF/2022/183 funded by MCIN/AEI/10.13039/501100011033 and, as appropriate, by “ESF Investing in your future”. O. E. S. acknowledges her predoctoral contract with reference GRISOLIAP/2021/112. T. S. R. and P. P. B. acknowledge the financial support of Generalitat Valenciana through the CIDEGENT contracts (CIDEGENT/2021/044 and CIDEXG/2022/34). This study forms part of the Advanced Materials programme and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and by the Generalitat Valenciana (code MFA/2022/040). This publication is part of the grant CNS2023-144270 funded by MICIU/AEI/10.13039/501100011033 and by European Union NextGenerationEU/PRTR.
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