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An integration of perovskite and cadmium telluride (CdTe) solar cells in a tandem configuration has the potential to yield efficient thin-film tandem solar cells. Owing to the promise of higher efficiency at low cost, the presented study aims to explore the potential for combining this commercially established CdTe photovoltaics (PV) with next-generation perovskite PV. Here, we developed four-terminal (4-T) CdTe/perovskite tandem solar cells, starting with 18.3% efficient near-infrared-transparent perovskite solar cells (NIR-TPSCs) with an average transmission (Tavg) of 24.76% in the 300−900 nm wavelength range. These were then integrated with 19.56% efficient opaque CdTe solar cells, achieving 23.42% efficiency in a 4-T tandem configuration. Additionally, using a refractive index matching liquid increases the overall power conversion efficiency (PCE)to 24.2%. This pioneering achievement marks the first instance of a 4-T CdTe/perovskite thin-film tandem solar cell exceeding a PCE of 24.2%, a significant 123.72% increase in overall PCE. 

Abstract Silver cluster‐based solids have garnered considerable attention owing to their tunable luminescence behavior. While surface modification has enabled the construction of stable silver clusters, controlling interactions among clusters at the molecular level has been challenging due to their tendency to aggregate. Judicious choice of stabilizing ligands becomes pivotal in crafting a desired assembly. However, detailed photophysical behavior as a function of their cluster packing remained unexplored. Here, we modulate the packing pattern of Ag₁₂clusters by varying the nitrogen‐based ligand. CAM‐1 formed through coordination of the tritopic linker molecule and NC‐1 with monodentate pyridine ligand; established via non‐covalent interactions. Both the assemblies show ligand‐to‐metal‐metal charge transfer (LMMCT) based cluster‐centered emission band(s). Temperature‐dependent photoluminescence spectra exhibit blue shifts at higher temperatures, which is attributed to the extent of the thermal reverse population of the S₁state from the closely spaced T₁state. The difference in the energy gap (ΔE_ST) dictated by their assemblies played a pivotal role in the way that Ag₁₂cluster assembly in CAM‐1 manifests a wider ΔE_STand thus requires higher temperatures for reverse intersystem crossing (RISC) than assembly of NC‐1. Such assembly‐defined photoluminescence properties underscore the potential toolkit to design new cluster‐ assemblies with tailored optoelectronic properties.