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Bulk-heterojunction organic solar cells (OSCs) have received considerable attention with significant progress recently and offer a promising outlook for portable energy resources and building-integrated photovoltaics in the future. Now, it is urgent to promote the research of OSCs toward their commercialization. For the commercial application of OSCs, it is of great importance to develop high performance, high stability, and low cost photovoltaic materials. In this review, a comprehensive overview of the fundamental requirements of photoactive layer materials and interface layer materials toward commercialization is provided, mainly focusing on high performance, green manufacturing, simplifying device fabrication processes, stability, and cost issues. Furthermore, the perspectives and opportunities for this emerging field of materials science and engineering are also discussed.

The construction of monolithic two‐terminal tandem solar cells (2T TSCs) offers the possibility of pursuing high power conversion efficiency (PCE) by overcoming the single‐junction Shockley–Queisser limit in photovoltaics. However, little attention is paid to simultaneously improve the stability by utilizing the complementary properties of various photoactive layers. Here, beyond the stacked photoactive layers featuring complementary absorption, all‐inorganic perovskite (CsPbI1.8Br1.2) is chosen as the photoactive layer of the front wide‐bandgap subcell for its intrinsic high thermal stability and ultraviolet (UV)‐filtering function to address the burn‐in and UV degradation of organic rear subcells. To realize their monolithic integration, the charge recombination efficiency in the interconnecting layer (ICL) between the two types of subcells is tentatively improved by surface reconstruction of all‐inorganic perovskite using trimethylammonium chloride. The repaired CsPbI1.8Br1.2 surface enables effective suppression of nonradiative recombination and facilitates hole transport, providing efficient charge recombination in the ICL in the 2T TSC. As a result, the all‐inorganic perovskite/organic 2T TSC delivers a promising PCE of 21.04%, accompanied by an ultrahigh open‐circuit voltage (Voc) of 2.05 V, which is nearly equal to the superposition of the respective Voc values of the subcells. More importantly, the 2T TSC simultaneously shows outstanding operational and UV stabilities.

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