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Compact domain features have been observed in spin crossover [Fe{HB(pz)}(bipy)] molecular thin film systems via soft x-ray absorption spectroscopy and photoemission electron microscopy. The domains are in a mixed spin state that on average corresponds to roughly 2/3 the high spin occupation of the pure high spin state. Monte Carlo simulations support the presence of intermolecular interactions that can be described in terms of an Ising model in which interactions beyond nearest-neighbors cannot be neglected. This suggests the presence of short-range order to permit interactions between molecules beyond nearest neighbor that contribute to the formation of largely high spin state domains structure. The formation of a spin state domain structure appears to be the result of extensive cooperative effects.
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http://dx.doi.org/10.1088/1361-648X/ac6cbc | DOI Listing |
Acc Chem Res
September 2025
Department of Chemistry, FRQNT Centre for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street W, Montréal, Québec H3A 0B8, Canada.
ConspectusMolecular photochemistry, by harnessing the excited states of organic molecules, provides a platform fundamentally distinct from thermochemistry for generating reactive open-shell or spin-active species under mild conditions. Among its diverse applications, the resurgence of the Minisci-type reaction, a transformation historically reliant on thermally initiated radical conditions, has been fueled by modern photochemical strategies with improved efficiency and selectivity. Consequently, the photochemical Minisci-type reaction ranks among the most enabling methods for C()-H functionalizations of heteroarenes, which are of particular significance in medicinal chemistry for the rapid diversification of bioactive scaffolds.
View Article and Find Full Text PDFAdv Mater
September 2025
School of Materials Science and Engineering, Anhui University, Hefei, 230601, China.
Modulating the electronic structure of catalysts to maximize their power holds the key to address the challenges faced by zinc-iodine batteries (ZIBs), including the shuttle effect and slow redox kinetics at the iodine cathode. Herein, oxygen vacancies is innovatively introduced into CoO lattice to create high-spin-state Co active sites in nonstoichiometric CoO nanocrystals supported by carbon nanofibers (H-CoO/CNFs). This simple strategy intensifies crystal field splitting of Co 3d orbitals, optimizing the spin-orbital coupling between Co 3d orbitals and iodine species.
View Article and Find Full Text PDFMagn Reson Chem
September 2025
Institute of Scientific and Industrial Research, Osaka University, Osaka, Japan.
We reveal contrasting behaviors in molecular motion between the two materials, including the identification of resonance-enhanced dynamic features in elastomers. We present a depth-resolved analysis of molecular dynamics in semicrystalline polytetrafluoroethylene (PTFE) and fully amorphous fluorinated elastomer (SIFEL) films using static-gradient solid-state F NMR imaging. By measuring spin-lattice relaxation rates ( ) at multiple frequencies and evaluating the corresponding spectral density functions, we reveal distinct dynamic behaviors between the two materials.
View Article and Find Full Text PDFPhys Chem Chem Phys
September 2025
Masaryk University, Faculty of Science, Department of Chemistry, Kotlářská 2, Brno, 611 37, Czech Republic.
Structural and magnetic properties of ultra-small tetrahedron-shaped iron oxide nanoparticles were investigated using density functional theory. Tetrahedral and truncated tetrahedral models were considered in both non-functionalized form and with surfaces passivated by pseudo-hydrogen atoms. The focus on these two morphologies reflects their experimental relevance at this size scale and the feasibility of performing fully relaxed, atomistically resolved first-principles simulations.
View Article and Find Full Text PDFNanoscale
September 2025
St. Petersburg State University, 199034 St. Petersburg, Russia.
Using angle-resolved photoemission spectroscopy (ARPES) with spin resolution, scanning tunneling microscopy/spectroscopy (STM/STS) and density functional theory (DFT) methods, we study the electronic structure of graphene-covered and bare Au/Co(0001) systems and reveal intriguing features, arising from the ferrimagnetic order in graphene and the underlying gold monolayer. In particular, a spin-polarized Dirac-cone-like state, intrinsically related to the induced magnetization of Au, was discovered at point. We have obtained a good agreement between experiment and theory for bare and graphene-covered Au/Co(0001) and have proven that both Au ferrimagnetism and the Dirac-cone-like band are intimately linked to the triangular loop dislocations present at the Au/Co interface.
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