Assessment of First-Principles and Semiempirical Methodologies for Absorption and Emission Energies of Ce${}^{3+}$-Doped Luminescent Materials

Abstract

In search of a reliable methodology for the prediction of light absorption and emission of Ce${}^{3+}$-doped luminescent materials, 13 representative materials are studied with first-principles and semiempirical approaches. In the first-principles approach, that combines constrained density-functional theory and $\Delta$SCF, the atomic positions are obtained for both ground and excited states of the Ce${}^{3+}$ ion. The structural information is fed into Dorenbos' semiempirical model. Absorption and emission energies are calculated with both methods and compared with experiment. The first-principles approach matches experiment within 0.3 eV, with two exceptions at 0.5 eV. In contrast, the semiempirical approach does not perform as well (usually more than 0.5 eV error). The general applicability of the present first-principles scheme, with an encouraging predictive power, opens a novel avenue for crystal site engineering and high-throughput search for new phosphors and scintillators.

arXiv comment12 pages, 3 figures

References in corpus (2)

• First-Principles Studies of Luminescence in Ce doped Inorganic Scintillators
• First-principles study of Ce${}^{3+}$ doped lanthanum silicate nitride phosphors: Neutral excitation, Stokes shift, and luminescent center identification

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• Beyond the one-dimensional configuration coordinate model of photoluminescence
• First-principles study on luminescence properties of Eu-doped defect pyrochlore oxide KNbWO${}_6\cdot$H${}_2$O:Eu${}^{3+}$