First-principles study of Ce${}^{3+}$ doped lanthanum silicate nitride phosphors: Neutral excitation, Stokes shift, and luminescent center identification

Abstract

We study from first principles two lanthanum silicate nitride compounds, LaSi${}_3$N${}_5$ and La${}_3$Si${}_6$N${}_{11}$, pristine as well as doped with Ce${}^{3+}$ ion, in view of explaining their different emission color, and characterising the luminescent center. The electronic structures of the two undoped hosts are similar, and do not give a hint to quantitatively describe such difference. The $4f\to 5d$ neutral excitation of the Ce${}^{3+}$ ions is simulated through a constrained density-functional theory method coupled with a $\Delta$SCF analysis of total energies, yielding absorption energies. Afterwards, atomic positions in the excited state are relaxed, yielding the emission energies and Stokes shifts. Based on these results, the luminescent centers in LaSi${}_3$N${}_5$:Ce and La${}_3$Si${}_6$N${}_{11}$:Ce are identified. The agreement with the experimental data for the computed quantities is quite reasonable and explains the different color of the emitted light. Also, the Stokes shifts are obtained within 20\% difference relative to experimental data.

arXiv comment12 pages, 10 figures

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• Ab initio Study of Luminescence in Ce-doped Lu${}_2$SiO${}_5$: The Role of Oxygen Vacancies on Emission Color and Thermal Quenching Behavior
• A First-Principles Explanation of the Luminescent Line Shape of SrLiAl${}_3$N${}_4$:Eu${}^{2+}$ Phosphor for Light-Emitting Diode Applications
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• Beyond the one-dimensional configuration coordinate model of photoluminescence
• Investigation of photon emitters in Ce-implanted hexagonal boron nitride