Journal article

Prospecting lighting applications with ligand field tools and density functional theory: a first-principles account of the 4f⁷–4f⁶5d¹ Luminescence of CsMgBr₃:Eu²⁺

  • Ramanantoanina, Harry Department of Chemistry, University of Fribourg, Switzerland
  • Cimpoesu, Fanica Institute of Physical Chemistry, Bucharest, Romania
  • Göttel, Christian Department of Chemistry, University of Fribourg, Switzerland
  • Sahnoun, Mohammed Laboratoire de physique de la matière et modélisation mathématique, Université de Mascara, Algerie
  • Herden, Benjamin Department of Chemistry, University of Fribourg, Switzerland
  • Suta, Markus Faculty of Science and Technology, University of Siegen, Germany
  • Wickleder, Claudia Faculty of Science and Technology, University of Siegen, Germany
  • Urland, Werner Department of Chemistry, University of Fribourg, Switzerland
  • Daul, Claude Department of Chemistry, University of Fribourg, Switzerland
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    08.09.2015
Published in:
  • Inorganic Chemistry. - 2015, vol. 54, no. 17, p. 8319–8326
English 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.
Faculty
Faculté des sciences et de médecine
Department
Département de Chimie
Language
  • English
Classification
Chemistry
License
License undefined
Identifiers
Persistent URL
https://folia.unifr.ch/unifr/documents/304758
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