Ligand field density functional theory calculation of the 4f2 → 4f15d1 transitions in the quantum cutter Cs2KYF6:Pr3+
Literature Information
Harry Ramanantoanina, Fanica Cimpoesu, Claude Daul
Herein we present a Ligand Field Density Functional Theory (LFDFT) based methodology for the analysis of the 4fn → 4fn−15d1 transitions in rare earth compounds and apply it for the characterization of the 4f2 → 4f15d1 transitions in the quantum cutter Cs2KYF6:Pr3+ with the elpasolite structure type. The methodological advances are relevant for the analysis and prospection of materials acting as phosphors in light-emitting diodes. The positions of the zero-phonon energy corresponding to the states of the electron configurations 4f2 and 4f15d1 are calculated, where the praseodymium ion may occupy either the Cs+-, K+- or the Y3+-site, and are compared with available experimental data. The theoretical results show that the occupation of the three undistorted sites allows a quantum-cutting process. However size effects due to the difference between the ionic radii of Pr3+ and K+ as well as Cs+ lead to the distortion of the K+- and the Cs+-site, which finally exclude these sites for quantum-cutting. A detailed discussion about the origin of this distortion is also described.
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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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