Abstract
Two-terminal (2T) perovskite on organic tandem solar cells (PSC/OPV TSCs) are attracting attention due to their fast improvement in power conversion efficiency (PCE). Understanding both the optics and electronics is crucial in monolithic tandem devices. Here, we report an optoelectronic model developed for a 2T PSC/OPV TSC that helps determine the device’s most influential parameters and recombination mechanisms and elucidates the underlying physics. Our simulation results are validated with experiments, and a good agreement is obtained. The effects of surface coverage, bulk, and sheet resistances on charge carrier recombination in the interconnecting layer (ICL) are investigated with the model. When the ICL thickness is increased, we demonstrate that the mechanism in the ICL can change from charge carrier recombination to transport. Finally, a pathway toward the 30% practical PCE limit for PSC/OPV TSCs is identified, which requires the single-junction perovskite and organic sub-cells to reach PCEs of 22.3% and 20.4%, respectively. • An in-depth model for two-terminal perovskite/organic tandem cells is developed • Sensitivity and loss analyses are conducted to determine critical parameters • Layer functionality is interconnected with surface coverage and resistances • Guidelines toward 30% efficiency tandem cell with key parameters quantified Zhao et al. develop a comprehensive optoelectronic model to elucidate the underlying physics of two-terminal perovskite/organic tandem cells. To improve device efficiency, influential parameters and recombination losses are identified. Mechanisms in interconnecting layers concerning surface coverages and resistances are unveiled. This work demonstrates the potential for highly efficient tandem devices.
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