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Synthesizing molecules with significant topological features, such as catenanes, tailored with specific groups to confer desired functionality, is essential for investigating various properties arising from the entanglement due to mechanical bonds. This investigation can pave the way for uncovering novel functional materials employing mechanically interlocked molecules (MIMs). In this direction, we have synthesized a π‐donor (D) and π‐acceptor (A) functionalized [2]catenane using a non‐labile Co(III) metal ion as a template with pyridine‐diamide templating center and utilizing click reaction for ring‐closing. The donor group is a fluorene derivative, and the acceptor is a benzophenazine derivative, commonly employed in synthesizing conjugated polymers for various optoelectronic devices. Synthetically, the acceptor group was introduced into a macrocycle with a pyridine diamide unit. It was then threaded with a ligand having alkyne terminals to obtain the desired [2]pseudorotaxane utilizing cobalt ion as a template. Ring‐closing was then performed with a di‐azide functionalized molecule with the donor chromophore. The desired D−A functionalized [2]catenane was obtained after demetalation. All the starting materials, macrocycle, and entangled structures have been characterized by 1H‐NMR, 13C‐NMR, and mass spectroscopy. Some of these materials were also characterized by single‐crystal X‐ray analysis. The photophysical properties are studied by UV‐visible and fluorescence spectroscopy. [ABSTRACT FROM AUTHOR]

Asymmetric wide‐band gap fullerene‐free acceptors (FFAs) play a crucial role in organic solar cells (OSCs). Here, we designed and synthesized a simple asymmetric coumarin‐anthracene conjugate named CA‐CN with optical band gap of 2.1 eV in a single‐step condensation reaction. Single crystal X‐ray structure analysis confirms various multiple intermolecular non‐covalent interactions. The molecular orbital energy levels of CA‐CN estimated from cyclic voltammetry were found to be suitable for its use as an acceptor for OSCs. Binary OSCs fabricated using CA‐CN as acceptor and PTB7‐Th as the donor achieve a power conversion efficiency (PCE) of 11.13 %. We further demonstrate that the insertion of 20 wt % of CA‐CN as a third component in ternary OSCs with PTB7‐Th : DICTF as the host material achieved an impressive PCE of 14.91 %, an improvement of ~43 % compared to the PTB7‐Th : DICTF binary device (10.38 %). Importantly, the ternary blend enhances the absorption coverage from 400 to 800 nm and improves the morphology of the active layer. The findings highlight the efficacy of an asymmetric design approach for FFAs, which paves the way for developing high‐efficiency OSCs at low cost. [ABSTRACT FROM AUTHOR]

Two N‐heterocyclic olefin‐phosphines (NHOP), and the corresponding ruthenium complexes were synthesized and structurally characterized. One of the cationic complexes [(BzIM)(NHOP)Ru(p‐cymene)Cl2]I was employed as a catalyst in N‐benzylbenzamides/alkyne coupling reactions. With this catalytic protocol a variety of substituted isoquinolones were synthesized through ortho‐selective double C−H bond functionalization involving oxidative annulation followed by olefination reactions. All these products were achieved in one‐pot manner without the use of additives. [ABSTRACT FROM AUTHOR]

Cryptophanes show different conformations in solution and solid state depending upon various factors, such as the length of connecting linkers, medium, and nature of the incoming guest molecule(s). A cyclotriguaiacylenes (CTG) based cryptophane molecule was synthesized using click chemistry containing three triazole linkers and studied as well. This molecule shows two conformations, out‐out crown‐crown (CC), and out‐in CC, in the presence or absence of guest molecule(s), as studied both in solution and solid state. The out‐in CC, in which both CTG fragments are in crown conformation with one crown sitting above the other, could be obtained by slow escape of the trapped acetone molecules from out‐out CC in solid state. This transformation could be obtained through a single‐crystal‐to‐single‐crystal (SCSC) transformation from a large volume out‐out CC to a smaller volume out‐in CC conformation which is also supported by density functional theory calculations. [ABSTRACT FROM AUTHOR]

This study investigates the anion‐directed assembly of discrete copper (II) complexes. The ligands of choice are two N7‐alkyl‐purine‐based neutral ligands. These ligands facilitate the exclusive coordination through the N3 and N9 positions, preventing polymeric chain formation. Perchlorate ions promoted the formation of discrete paddlewheel‐like complexes with the general formula [Cu2(μ‐Pur)4(CH3CN)2]4+, while chloride ions yielded chloride‐bridged dimers of the form [Cu2(Pur)2(μ‐Cl)2Cl2]. Copper‐copper bond distances within these complexes ranged from 2.92 to 2.98 Å. Magnetic susceptibility measurement of chloride‐bridged complexes exhibited antiferromagnetic coupling, whereas paddlewheel complexes displayed more complex alternating ferromagnetic and antiferromagnetic interactions. Chloride‐bridged compounds exhibited strong near‐infrared absorption. [ABSTRACT FROM AUTHOR]

Synthesizing molecules with significant topological features, such as catenanes, tailored with specific groups to confer desired functionality, is essential for investigating various properties arising from the entanglement due to mechanical bonds. This investigation can pave the way for uncovering novel functional materials employing mechanically interlocked molecules (MIMs). In this direction, we have synthesized a π-donor (D) and π-acceptor (A) functionalized [2]catenane using a non-labile Co(III) metal ion as a template with pyridine-diamide templating center and utilizing click reaction for ring-closing. The donor group is a fluorene derivative, and the acceptor is a benzophenazine derivative, commonly employed in synthesizing conjugated polymers for various optoelectronic devices. Synthetically, the acceptor group was introduced into a macrocycle with a pyridine diamide unit. It was then threaded with a ligand having alkyne terminals to obtain the desired [2]pseudorotaxane utilizing cobalt ion as a template. Ring-closing was then performed with a di-azide functionalized molecule with the donor chromophore. The desired D-A functionalized [2]catenane was obtained after demetalation. All the starting materials, macrocycle, and entangled structures have been characterized by 1 H-NMR, 13 C-NMR, and mass spectroscopy. Some of these materials were also characterized by single-crystal X-ray analysis. The photophysical properties are studied by UV-visible and fluorescence spectroscopy., (© 2024 The Authors. Chemistry - An Asian Journal published by Wiley-VCH GmbH.)

Cryptophanes show different conformations in solution and solid state depending upon various factors, such as the length of connecting linkers, medium, and nature of the incoming guest molecule(s). A cyclotriguaiacylenes (CTG) based cryptophane molecule was synthesized using click chemistry containing three triazole linkers and studied as well. This molecule shows two conformations, out-out crown-crown (CC), and out-in CC, in the presence or absence of guest molecule(s), as studied both in solution and solid state. The out-in CC, in which both CTG fragments are in crown conformation with one crown sitting above the other, could be obtained by slow escape of the trapped acetone molecules from out-out CC in solid state. This transformation could be obtained through a single-crystal-to-single-crystal (SCSC) transformation from a large volume out-out CC to a smaller volume out-in CC conformation which is also supported by density functional theory calculations., (© 2023 Wiley-VCH GmbH.)