Ramanantoanina, Harry Cimpoesu, Fanica Göttel, Christian Sahnoun, Mohammed Herden, Benjamin Suta, Markus Wickleder, Claudia Urland, Werner Daul, Claude 2015-09-08 The most efficient way to provide domestic lighting nowadays is by light-emitting diodes (LEDs) technology combined with phosphors shifting the blue and UV emission toward a desirable sunlight spectrum. A route in the quest for warm-white light goes toward the discovery and tuning of the lanthanide-based phosphors, a difficult task, in experimental and technical respects. A proper theoretical approach, which is also complicated at the conceptual level and in computing efforts, is however a profitable complement, offering valuable structure–property rationale as a guideline in the search of the best materials. The Eu²⁺-based systems are the prototypes for ideal phosphors, exhibiting a wide range of visible light emission. Using the ligand field concepts in conjunction with density functional theory (DFT), conducted in nonroutine manner, we develop a nonempirical procedure to investigate the 4f⁷–4f⁶5d¹ luminescence of Eu²⁺ in the environment of arbitrary ligands, applied here on the CsMgBr₃:Eu²⁺-doped material. Providing a salient methodology for the extraction of the relevant ligand field and related parameters from DFT calculations and encompassing the bottleneck of handling large matrices in a model Hamiltonian based on the whole set of 33 462 states, we obtained an excellent match with the experimental spectrum, from first-principles, without any fit or adjustment. This proves that the ligand field density functional theory methodology can be used in the assessment of new materials and rational property design. application/pdf https://folia.unifr.ch/global/documents/304758 https://folia.unifr.ch/documents/304758/files/dau_pla.pdf eng info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.inorgchem.5b00988 info:eu-repo/semantics/openAccess License undefined Inorganic Chemistry. - 2015, vol. 54, no. 17, p. 8319–8326 info:eu-repo/classification/udc/54 Prospecting lighting applications with ligand field tools and density functional theory: a first-principles account of the 4f⁷–4f⁶5d¹ Luminescence of CsMgBr₃:Eu²⁺ http://purl.org/coar/resource_type/c_6501