The electronic structures of URh (3), UPd (3), UPt (3), and UAu (3) are calculated with the self-interaction corrected local-spin-density approximation. We find that only in URh (3) the f electrons are fully delocalized. UPt (3) has one f electron localized at each U site, while a localized f(2) configuration of the U ion is found for UPd (3). It is predicted that, upon application of a pressure of 25 GPa, UPd (3) will acquire the f(1) configuration and possibly exhibit heavy-fermion behavior. We find that UAu (3) is characterized by the same mixed localized-delocalized f-electron manifold as UPd (3).
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http://dx.doi.org/10.1103/PhysRevLett.88.216403 | DOI Listing |
Chem Rev
November 2024
School of Materials and Chemical Technology, Institute of Science Tokyo, Ookayama 2-12-1, Meguro-ku, Tokyo 152-8552, Japan.
The electron density determines all properties of a system of nuclei and electrons. It is both computable and observable. Its topology allows gaining insight into the mechanisms of bonding and other phenomena in a way that is complementary to and beyond that available from the molecular orbital picture and the formal oxidation state (FOS) formalism.
View Article and Find Full Text PDFChemistry
January 2025
Universidad de Buenos Aires, Facultad de Ciencias Exactas y Naturales, Departamento de Química Inorgánica, Analítica y Química Física, Pabellón 2, Ciudad Universitaria, C1428EHA, Buenos Aires, Argentina.
Visible-light excitation of a family of bimetallic ruthenium polypyridines with the formula [Ru(tpy)(bpy)(-CN)Ru(py)L] (RuRuL), where L=Cl, NCS, DMAP and ACN, was used to prepare photoinduced mixed-valence (PI-MV) MLCT states as models of the photosynthetic reaction center. Ultrafast transient absorption spectroscopy allowed to monitor photoinduced IVCT bands between 6000 and 11000 cm. Mulliken spin densities resulting from DFT and (TD)DFT computations revealed the modulation of the charge density distribution depending on the ligand substitution pattern.
View Article and Find Full Text PDFPhys Chem Chem Phys
November 2023
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.
Two triplet excitons are generated through an ultrafast photophysical process, namely singlet fission (SF), providing a solution for efficient solar energy usage. In this work, we provide an effective guideline for designing SF materials by adjusting the planarity in cyclopentadithiophene (CPDT) derivatives. A practical strategy is proposed for tuning the quinoidal-biradical resonance structures by varying the electron push-pull groups of CPDTs for SF.
View Article and Find Full Text PDFAdv Mater
November 2023
School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia, 5005, Australia.
Photogenerated charge localization on material surfaces significantly affects photocatalytic performance, especially for multi-electron CO reduction. Dual single atom (DSA) catalysts with flexibly designed reactive sites have received significant research attention for CO photoreduction. However, the charge transfer mechanism in DSA catalysts remains poorly understood.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
July 2023
Department of Physics and Astronomy, Rice Center for Quantum Materials, Rice University, Houston, TX 77005.
Strange metals appear in a wide range of correlated materials. Electronic localization-delocalization and the expected loss of quasiparticles characterize beyond-Landau metallic quantum critical points and the associated strange metals. Typical settings involve local spins.
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