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Title: Role of Ce 4 + in the scintillation mechanism of codoped Gd 3 Ga 3 Al 2 O 12 : Ce

Abstract

To control the time-response performance of widely used cerium-activated scintillators in cutting-edge medical-imaging devices, such as time-of-flight positron-emission tomography, a comprehensive understanding of the role of Ce valence states, especially stable Ce 4+, in the scintillation mechanism is essential. However, despite some progress made recently, an understanding of the physical processes involving Ce 4+ is still lacking. The aim of this work is to clarify the role of Ce 4+ in scintillators by studying Ca 2+ codoped Gd 3Ga 3Al 2O1 2∶Ce (GGAG∶Ce). By using a combination of optical absorption spectra and x-ray absorption near-edge spectroscopies, the correlation between Ca 2+codoping content and the Ce 4+ fraction is seen. The energy-level diagrams of Ce 3+ and Ce 4+ in the Gd 3Ga 3Al 2O 12 host are established by using theoretical and experimental methods, which indicate a higher position of the 5d 1 state of Ce 4+ in the forbidden gap in comparison to that of Ce 3+. Underlying reasons for the decay-time acceleration resulting from Ca 2+ codoping are revealed, and the physical processes of the Ce 4+-emission model are proposed and further demonstrated by temperature-dependent radioluminescence spectra under x-ray excitation.

Authors:
 [1];  [2];  [3];  [2];  [2]
  1. Univ. of Tennessee, Knoxville, TN (United States); Chinese Academy of Science, Shanghai (China)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Wake Forest Univ., Winston-Salem, NC (United States)
Publication Date:
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1180297
Grant/Contract Number:  
AC02-05CH1123
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physical Review Applied
Additional Journal Information:
Journal Name: Physical Review Applied Journal Volume: 2 Journal Issue: 4; Journal ID: ISSN 2331-7019
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English

Citation Formats

Wu, Yuntao, Meng, Fang, Li, Qi, Koschan, Merry, and Melcher, Charles L. Role of Ce4+ in the scintillation mechanism of codoped Gd3Ga3Al2O12:Ce. United States: N. p., 2014. Web. doi:10.1103/PhysRevApplied.2.044009.
Wu, Yuntao, Meng, Fang, Li, Qi, Koschan, Merry, & Melcher, Charles L. Role of Ce4+ in the scintillation mechanism of codoped Gd3Ga3Al2O12:Ce. United States. doi:10.1103/PhysRevApplied.2.044009.
Wu, Yuntao, Meng, Fang, Li, Qi, Koschan, Merry, and Melcher, Charles L. Fri . "Role of Ce4+ in the scintillation mechanism of codoped Gd3Ga3Al2O12:Ce". United States. doi:10.1103/PhysRevApplied.2.044009.
@article{osti_1180297,
title = {Role of Ce4+ in the scintillation mechanism of codoped Gd3Ga3Al2O12:Ce},
author = {Wu, Yuntao and Meng, Fang and Li, Qi and Koschan, Merry and Melcher, Charles L.},
abstractNote = {To control the time-response performance of widely used cerium-activated scintillators in cutting-edge medical-imaging devices, such as time-of-flight positron-emission tomography, a comprehensive understanding of the role of Ce valence states, especially stable Ce4+, in the scintillation mechanism is essential. However, despite some progress made recently, an understanding of the physical processes involving Ce4+ is still lacking. The aim of this work is to clarify the role of Ce4+ in scintillators by studying Ca2+ codoped Gd3Ga3Al2O12∶Ce (GGAG∶Ce). By using a combination of optical absorption spectra and x-ray absorption near-edge spectroscopies, the correlation between Ca2+codoping content and the Ce4+ fraction is seen. The energy-level diagrams of Ce3+ and Ce4+ in the Gd3Ga3Al2O12 host are established by using theoretical and experimental methods, which indicate a higher position of the 5d1 state of Ce4+ in the forbidden gap in comparison to that of Ce3+. Underlying reasons for the decay-time acceleration resulting from Ca2+ codoping are revealed, and the physical processes of the Ce4+-emission model are proposed and further demonstrated by temperature-dependent radioluminescence spectra under x-ray excitation.},
doi = {10.1103/PhysRevApplied.2.044009},
journal = {Physical Review Applied},
number = 4,
volume = 2,
place = {United States},
year = {Fri Oct 17 00:00:00 EDT 2014},
month = {Fri Oct 17 00:00:00 EDT 2014}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1103/PhysRevApplied.2.044009

Citation Metrics:
Cited by: 46 works
Citation information provided by
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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA + U method
journal, January 1997

  • Anisimov, Vladimir I.; Aryasetiawan, F.; Lichtenstein, A. I.
  • Journal of Physics: Condensed Matter, Vol. 9, Issue 4, p. 767-808
  • DOI: 10.1088/0953-8984/9/4/002

Ab initiomolecular dynamics for liquid metals
journal, January 1993


2 inch diameter single crystal growth and scintillation properties of Ce:Gd3Al2Ga3O12
journal, August 2012


Special quasirandom structures
journal, July 1990


Rationale for mixing exact exchange with density functional approximations
journal, December 1996

  • Perdew, John P.; Ernzerhof, Matthias; Burke, Kieron
  • The Journal of Chemical Physics, Vol. 105, Issue 22, p. 9982-9985
  • DOI: 10.1063/1.472933