Magnetic and conduction properties in 1D organic radical materials: an ab initio inspection for a challenging quest
文献情報
Martin Vérot, Jean-Baptiste Rota, Boris Le Guennic
The chemical control of magnetic and conduction properties for organic radicals is mainly based on t, the resonance integral, and U, the on-site repulsion, used in the Hubbard model. A qualitative analysis based on the competition between the kinetic and the Coulomb contribution, and the expression of the magnetic exchange coupling suggests that U should be roughly 800 cm−1 while the resonance integral |t| should be 200 cm−1 to reach bifunctionality. Ab initio wavefunction-based calculations allowed us to quantitatively measure those quantities for several organic materials considered as 1D systems starting from their reported crystal structures. The extraction of t and U parameters from the exchange coupling constants between neighbouring radicals allowed us to anticipate a possible metallic behaviour. Finally, the impact of chemical changes in the constitutive units is measured to rationalize the macroscopic behaviour modifications. It is shown that the intriguing regime characterized by simultaneous itinerant and localized electrons might be achieved by molecular engineering.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.












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