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  1. Free, publicly-accessible full text available August 16, 2024
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    Metal–organic frameworks (MOFs) have emerged as promising porous optoelectronic compositions for energy conversion and sensing applications. The enormous structural possibilities, the large variety of photo- and redox-active building blocks along with several post-synthetic functionalization strategies make MOFs an ideal platform for photochemical and photoelectrochemical developments. Because MOFs assemble all the active building units in a dense fashion, the non-aggregated yet proximally positioned species ensure efficient photon absorption to drive photoinduced charge transfer (PCT) reactions for energy conversion and sensing. Hence, understanding the PCT processes within MOFs as a function of the topological and electronic structures of the donor–acceptor (D–A) moieties can provide transformative strategies to design new low-density compositions. 
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  5. Abstract

    High quantum yield triplets, populated by initially prepared excited singlets, are desired for various energy conversion schemes in solid working compositions like porous MOFs. However, a large disparity in the distribution of the excitonic center of mass, singlet‐triplet intersystem crossing (ISC) in such assemblies is inhibited, so much so that a carboxy‐coordinated zirconium heavy metal ion cannot effectively facilitate the ISC through spin‐orbit coupling. Circumventing this sluggish ISC, singlet fission (SF) is explored as a viable route to generating triplets in solution‐stable MOFs. Efficient SF is achieved through a high degree of interchromophoric coupling that facilitates electron super‐exchange to generate triplet pairs. Here we show that a predesigned chromophoric linker with extremely poor ISC efficiency (kISC) butform triplets in MOF in contrast to the frameworks that are built from linkers with sizablekISCbut. This work opens a new photophysical and photochemical avenue in MOF chemistry and utility in energy conversion schemes.

     
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