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Quantification of Through-Space Intervalence Charge Transfer in Cofacial Thiazolothiazole Metal-Organic Framework and Its Photochromic Behavior.
J Phys Chem Lett
January 2025
School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram, Thiruvananthapuram, Kerala 695551, India.
Electronic coupling between individual redox units in a molecular assembly dictates their charge transfer efficacy. Being a well-defined crystalline structure, the metal-organic framework (MOF) ensures proper positioning of redox-active moieties and provides a unique platform to unveil their charge transfer dynamics and quantification with structural relationships. Here, we demonstrate a novel redox-active MOF with near-infrared through-space intervalence charge transfer by introducing a mixed valence state inside redox-active thiazolothiazole-based ligands (DPTTZ) upon photo- or electrochemical reduction.
View Article and Find Full Text PDFThrough-Space Charge Transfer Dynamic Mechanism in V-Shaped Flexible Carbazole Aromatic Imides Dyads.
Chemistry
January 2025
Beijing University of Posts and Telecommunications, School of Science, Beijing, CHINA.
Cofacial electron donor-acceptor dyads exhibiting through-space charge-transfer (TSCT) characteristics are widely employed in the development of optoelectronic functional materials. The flexible molecular frameworks between the electron donor and acceptor components allow dynamic modulation of electronic coupling, influenced by excited-state structural relaxation or intermolecular interactions, thereby affecting the charge-transfer (CT) dynamics and the emission properties of TSCT states. In this work, we examine the TSCT dynamic processes of two electron donor-acceptor dyads, CzPhNI and CzPhPI formed by ortho-substitution of phenyl linkage with V-shaped flexible TSCT structures using carbazole as donor and naphthalimide or phthalimide as acceptor.
View Article and Find Full Text PDFTwo Blatter Radicals Face-to-Face: A Constrained Diradical Architecture.
J Am Chem Soc
January 2025
Faculty of Chemistry, University of Łódź, Tamka 12, 91403 Łódź, Poland.
Cofacial arrangement of two Blatter radicals enforced by the -naphthalene scaffold represents a new approach to stable diradicals with strong through-space interactions. Two stereoisomers of the naphthalene-diradicals, and , are investigated by XRD, VT-EPR, UV-vis, electrochemical, kinetic, and DFT methods. In solutions, both stereoisomers exist as open-shell singlets with Δ = -3.
View Article and Find Full Text PDFSynthesis of model heterojunction interfaces reveals molecular-configuration-dependent photoinduced charge transfer.
Nat Chem
September 2024
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
Control of the molecular configuration at the interface of an organic heterojunction is key to the development of efficient optoelectronic devices. Due to the difficulty in characterizing these buried and (probably) disordered heterointerfaces, the interfacial structure in most systems remains a mystery. Here we demonstrate a synthetic strategy to design and control model interfaces, enabling their detailed study in isolation from the bulk material.
View Article and Find Full Text PDFRare Guest-Induced Electrical Conductivity of Zn-Porphyrin Metallacage Inclusion Complexes Featuring π-Donor/Acceptor/Donor Stacks.
ACS Appl Mater Interfaces
January 2024
Department of Chemistry, Clemson University, 211 S. Palmetto Blvd., Clemson, South Carolina 29634, United States.
Charge-transfer (CT) interactions between co-facially aligned π-donor/acceptor (π-D/A) arrays engender unique optical and electronic properties that could benefit (supra)molecular electronics and energy technologies. Herein, we demonstrate that a tetragonal prismatic metal-organic cage (MOC1) having two parallel π-donor tetrakis(4-carboxyphenyl)-Zn-porphyrin (ZnTCPP) faces selectively intercalate planar π-acceptor guests, such as hexaazatriphenylene hexacarbonitrile (HATHCN), hexacyanotriphenylene (HCTP), and napthanelediimide (NDI) derivatives, forming 1:1 πA@MOC1 inclusion complexes featuring supramolecular π-D/A/D triads. The π-acidity of intercalated π-acceptors (HATHCN ≫ HCTP ≈ NDIs) dictated the nature and strength of their interactions with the ZnTCPP faces, which in turn influenced the binding affinities () and optical and electronic properties of corresponding πA@MOC1 inclusion complexes.
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