Journal ArticleMultimodular Wide-Band Capturing Nanohybrids: Role of Carbon Nanotubes in Slowing Charge Recombination in Supramolecular C ₆₀ -BisstyrylBODIPY-(Zinc Porphyrin) ₂ Donor–Acceptor Molecular CleftKazemi, Shahrzad [Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, Texas 76203-5017, United States]; Alsaleh, Ajyal Z [Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, Texas 76203-5017, United States]; Karr, Paul A [Department of Physical Sciences and Mathematics, Wayne State College, 1111 Main Street, Wayne, Nebraska 68787, United States]; D’Souza, Francis [Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, Texas 76203-5017, United States] (ORCID:0000000338158949)CarrieraThe importance of diameter-sorted single-wall carbon nanotubes (SWCNTs) non-covalently bound to a donor-acceptor molecular cleft, 1, in prolonging the lifetime of charge-separated states is successfully demonstrated. For this, using a multi-step synthetic procedure, a wide-band capturing, multi-modular, C60-bisstyrylBODIPY-(zinc porphyrin)2, molecular cleft 1, was newly synthesized and shown to bind diameter sorted SWCNTs. The molecular cleft and its supramolecular assemblies were characterized by a suite of physico-chemical techniques. Free-energy calculations suggested that both the (6,5) and (7,6) SWCNTs bound to 1 act as hole acceptors during the photo-induced sequential electron transfer events. Consequently, selective excitation of 1 in 1:SWCNT hybrids revealed a two-step electron transfer leading to the formation of charge-separated states. Due to the distal separation of the cation and anion radical species within the supramolecules, improved lifetimes of the charge-separated states could be achieved. The present supramolecular strategy of improving charge separation involving SWCNTs and donor-acceptor molecular cleft highlights the potential application of these hybrid materials for various light energy harvesting and optoelectronic applications.ACS2024-05-1510673201Journal of the American Chemical Society1461913509 to 135180002-7863https://doi.org/10.1021/jacs.4c029722345836National Science Foundation