First-principles calculations of photoluminescence and defect states of Ce³⁺-doped (Ca/Sr)₂B₅O₉Cl

Jiajia CAI, Weiguo JING, Jun CHENG, Yongfan ZHANG, Yonghu CHEN, Min YIN, Yau Yuen YEUNG, Chang-Kui DUAN

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Abstract

Reliable predictions of electronic levels, excited-state geometric relaxation, and the relative energies of ground and excited levels to host band edges are of paramount importance for Ce³⁺-doped luminescent materials. By combining the constrained occupancy approach and the hybrid density functional calculation in the framework of a generalized Kohn-Sham formalism, we derived a calculation scheme for the band gap of the host material, the equilibrium configurations of ground-state Ce³⁺ and excited-state (Ce³⁺)*, and their relative energies with respect to host band edges in terms of hole capture or electron ionization for Ce³⁺ in M₂B₅O₉Cl (M=Ca, Sr) charge compensated by Na⁺. The results of first-principles calculations for 4f→5d excitations, Stokes shifts, and the relative position of 5d levels to conduction-band edge agree well with experiments. The moderate computational cost of the present scheme, which can be applied in efficient prediction of the optical properties of many different Ce-doped materials, is of important value in screening potential lanthanide-doped scintillators and phosphors from minimal information about the host crystal structure. Copyright © 2019 American Physical Society.
Original languageEnglish
Article number125107
JournalPhysical Review B
Volume99
Issue number12
DOIs
Publication statusPublished - Mar 2019

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Photoluminescence
photoluminescence
Excited states
Phosphors
Defects
defects
excitation
ionization
Lanthanoid Series Elements
electronic levels
predictions
Conduction bands
Rare earth elements
Ground state
scintillation counters
phosphors
Ionization
Density functional theory
Screening
conduction bands

Citation

Cai, J., Jing, W., Cheng, J., Zhang, Y., Chen, Y., Yin, M., . . . Duan, C.-K. (2019). First-principles calculations of photoluminescence and defect states of Ce³⁺-doped (Ca/Sr)₂B₅O₉Cl. Physical Review B, 99(12). Retrieved from Retrieved from https://doi.org/10.1103/PhysRevB.99.125107