Unveiling the Potential of Two‐Terminal Perovskite/Organic Tandem Solar Cells: Mechanisms, Status, and Challenges

Abstract Perovskite/organic tandem solar cells (PO‐TSCs) demonstrate exceptional suitability for emerging applications such as building‐integrated photovoltaics, wearable devices, and greenhouse farming. By leveraging the distinctive attributes of perovskite and organic materials, which encompass expanded solar spectrum utilization, chemically benign solubility, and soft nature, PO‐TSCs position themselves as ideal candidates for high‐performance semi‐transparent photovoltaics (ST‐PVs). Despite these advantages, their development significantly lags behind other perovskite‐based counterparts, such as perovskite/perovskite, perovskite/silicon, and perovskite/Cu(In, Ga)Se₂. To address existing challenges and unlock the full potential of PO‐TSCs, an exploration of the fundamental mechanisms governing tandem photovoltaic devices is embarked. Delving into critical aspects such as charge generation/separation, energy level alignment, and material choices becomes pivotal for optimizing PO‐TSC performance. The investigation of monolithic two‐terminal PO‐TSCs offers insights into achievements and barriers, recognizing the competitive landscape with other TSC counterparts. Further scrutiny of perovskite absorbers and organic absorbers in TSCs reveals strategies aimed at enhancing stability and efficiency. The discussion extends to interconnection layers, elucidating their role in optimizing light transmission and balancing carrier recombination. In conclusion, a compelling outlook on the dynamic landscape of PO‐TSCs is presented, highlighting the remarkable efficiency progression and signaling their potential to revolutionize solar energy harvesting technologies.