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; Cimpoesu, Fanica; Göttel, Christian; Sahnoun, Mohammed; Herden, Benjamin; Suta, Markus; Wickleder, Claudia; Urland, Werner; Daul, Claude

doi:10.1021/acs.inorgchem.5b00988

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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

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