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
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- English
- Classification
- Chemistry
- License
- License undefined
- Identifiers
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- RERO DOC 258333
- DOI 10.1021/acs.inorgchem.5b00988
- Persistent URL
- https://folia.unifr.ch/unifr/documents/304758
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