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Nutation Spectroscopy of a Weakly Interacting Heterobimetallic Spin System.
Chemistry
January 2025
Institut de Chimie, UMR 7177 (CNRS-Université de Strasbourg), 4 rue Blaise Pascal, 67000, Strasbourg, France.
The use of V and Cu spins to design weakly coupled and dissymmetric spin systems has been examined. Such systems were synthesized using porphyrin-based complexes, with external coordination sites allowing for the formation of dimers via a Pd linker ion. Continuous-wave (CW) Electron Paramagnetic Resonance (EPR) spectroscopy allowed the unequivocal magnetic characterization of the mononuclear precursors VO and Cu.
View Article and Find Full Text PDFAn engineered POSS drug delivery system for copper(II) anticancer metallodrugs in a selective application toward melanoma cells.
Dalton Trans
July 2024
Departamento de Química Fundamental, Instituto de Química, Universidade de São Paulo, Av. Prof. Lineu Prestes 748, 05508-000 São Paulo, SP, Brazil.
In this work, a polyhedral silsesquioxane (POSS) was used as an engineered drug delivery system for two oxindolimine-copper(II) anticancer complexes, [Cu(isaepy)] and [Cu(isapn)]. The interest in hybrid POSS comes from the necessity of developing materials that can act as adjuvants to improve the cytotoxicity of non-soluble metallodrugs. Functionalization of POSS with a triazole ligand (POSS-atzac) permitted the anchorage of such copper complexes, producing hybrid materials with efficient cytotoxic effects.
View Article and Find Full Text PDFA Stable Aluminum Tris(dithiolene) Triradical.
J Am Chem Soc
June 2024
Department of Chemistry and the Center for Computational Chemistry, The University of Georgia, Athens, Georgia 30602-2556, United States.
A stable aluminum tris(dithiolene) triradical () was experimentally realized through a low-temperature reaction of the sterically demanding lithium dithiolene radical () with aluminum iodide. Compound was characterized by single-crystal X-ray diffraction, UV-vis and EPR spectroscopy, SQUID magnetometry, and theoretical computations. The quartet ground state of triradical has been unambiguously confirmed by variable-temperature continuous wave EPR experiments and SQUID magnetometry.
View Article and Find Full Text PDFAnalysis of early intermediate states of the nitrogenase reaction by regularization of EPR spectra.
Nat Commun
May 2024
Institut für Physikalische Chemie, Albert-Ludwigs-Universität Freiburg, Freiburg, Germany.
Due to the complexity of the catalytic FeMo cofactor site in nitrogenases that mediates the reduction of molecular nitrogen to ammonium, mechanistic details of this reaction remain under debate. In this study, selenium- and sulfur-incorporated FeMo cofactors of the catalytic MoFe protein component from Azotobacter vinelandii are prepared under turnover conditions and investigated by using different EPR methods. Complex signal patterns are observed in the continuous wave EPR spectra of selenium-incorporated samples, which are analyzed by Tikhonov regularization, a method that has not yet been applied to high spin systems of transition metal cofactors, and by an already established grid-of-error approach.
View Article and Find Full Text PDFProbing structural and dynamic properties of MAPbCl hybrid perovskite using Mn EPR.
Dalton Trans
April 2024
Faculty of Physics, Vilnius University, Sauletekio 3, 10257 Vilnius, Lithuania.
Hybrid methylammonium (MA) lead halide perovskites have emerged as materials exhibiting excellent photovoltaic performance related to their rich structural and dynamic properties. Here, we use multifrequency (X-, Q-, and W-band) electron paramagnetic resonance (EPR) spectroscopy of Mn impurities in MAPbCl to probe the structural and dynamic properties of both the organic and inorganic sublattices of this compound. The temperature dependent continuous-wave (CW) EPR experiments reveal a sudden change of the Mn spin Hamiltonian parameters at the phase transition to the ordered orthorhombic phase indicating its first-order character and significant slowing down of the MA cation reorientation.
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