The synthesis and characterization of acovalent allfullerene C 60 -Lu 3 N@I h -C 80 electron donor-acceptor conjugate has been realized by sequential 1,3-dipolar cycloaddition reactions of azomethine ylides on Lu 3 N@I h -C 80 and C 60 .T o the best of our knowledge,t his is the first time that two fullerenes behaving as both electron donor (Lu 3 N@I h -C 80 )and acceptor (C 60 )a re forming an electroactive dumbbell. DFT calculations reveal up to 16 diastereomeric pairs,that is,8with syn and 8w ith anti orientation, with the anti-RSSS isomer being the most stable.S pectroelectrochemical absorption and femtosecond transient absorption experiments support the notion that aC 60 ·À -Lu 3 N@I h -C 80 ·+ charge-separated state is formed. Spin conversion from the charge-separated singlet state C 60 ·À -Lu 3 N@I h -C 80 ·+ into the corresponding triplet state is facilitated by the heavy-atom effect stemming from the Lu 3 Ncluster,which, in turn, slows down the charge recombination by one order of magnitude.
Carbon dots (CDs) are strongly fluorescent advanced materials that are promising for applications in bio-imaging, sensors or luminescent displays. One of the most-widely used class of CDs is synthesized via...
Owing to the electron-donating and-accepting nature of corroles (Corr) and phthalocyanines (Pc), respectively,w ed esigned and developed two novel covalently linked Corr-Pc conjugates.T he synthetic route allows the preparation of the target conjugatesi ns atisfying yields. Comprehensives teady-state absorption, fluorescence, and electrochemical assayse nabled insights into energya nd electron-transfer processes upon photoexcitation. Coordinating ap yridine-appended subphthalocyanine (SubPc) to the Pc of the conjugate sets up the ways and means to realize the first example of an array composed by three different porphyrinoids,w hichd rives ac ascade of energy and charge-transfer processes. Importantly,t he SubPc assists in stabilizing the charge-separated state, that is, one-electron oxidized Corr and the one electron-reduced Pc,u pon photoexcitation by means of ar eductive charget ransfer to the SubPc. To the best of our knowledge, this is the first case of an intramolecular oxidation of aC orr within electron-donor-acceptorc onjugates by means of just photoexcitation. Moreover,t he combination of Corr,P c, and SubPc guarantees panchromatic absorption across the visible rangeo ft he solar spectrum, with the SubPc covering the "green gap" that usually affects porphyrinoids.
The synthesis and characterization of a library of unprecedented π-extended perylenes is reported. For this purpose, a successful step-by-step connection of three puzzle pieces, namely a perylene, an imidazole-quinoxaline bridge and an o-quinone was developed. Our synthetic route allows for facile access to linearly π-extended perylenes in a highly chemoselective manner. The absorption and fluorescence properties are solvent dependent and are bathochromically shifted relative to unbridged perylene references. Overall, the fluorescence quantum yields are high with values ranging from 46 % to 11 %. To complete the physico-chemical characterization, differential pulse and cyclic voltammograms were recorded showing two reductions and two oxidations for each of the linearly πextended perylenes.
Here, we present a novel butadiyne-linked HBC-ethynyl-porphyrin dimer, which exhibits in the ground state strong absorption cross sections throughout the UV and visible ranges of the solar spectrum.
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