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To simulate the luminescence emission spectra of Ce3+-activated phosphors, we propose a method based on scalar-relativistic density functional theory with corrections for on-site Coulomb interaction and first-principles molecular dynamics (FPMD) calculations, considering atomic thermal motion that is not limited to harmonic oscillations. The FPMD calculations at finite temperature were performed with the excited-state (ES) electron configuration corresponding to the Ce 4f05d1 state. Subsequently, the transition energies and probabilities of multiple 4f05d1→4f15d0 transitions in each FPMD snapshot were calculated using the N−1 electron configuration in which the highest occupied level in the ground-state (GS) configuration is vacated. According to Janak's theorem, the energy of each Kohn-Sham orbital obtained using this configuration corresponds to the total energy of ES produced by one-electron excitation from GS or GS. The time-averaged spectrum was calculated by accumulating emission lines located at the transition energy with amplitudes proportional to the probabilities. The spectra calculated for Ce3+-activated yttrium aluminum garnet exhibit shapes and positions that resemble those measured at temperatures above 300 K. The peak energies and full widths at half maximum at 300 K for the series of Ce3+-activated phosphors correlate with the experimental values, demonstrating the potential for predicting emission spectra of novel phosphors.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: Ce3+-activated phosphor, first-principles molecular dynamics, photoluminescence

Date published: 2026-05-27

Publisher: Wiley

Journal:

• Advanced Theory and Simulations (ISSN: 25130390) vol. 9 issue. 6 e02287

Funding:

• Japan Science and Technology Agency JPMJCR19J2

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1002/adts.202502287

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Updated at: 2026-06-01 16:26:03 +0900

Published on MDR: 2026-06-01 18:34:09 +0900