Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd <sub>1/4</sub> Y <sub>1/4</sub> Tb <sub>1/4</sub> Lu <sub>1/4</sub> ) <sub>3</sub> Al <sub>5</sub> O <sub>12</sub> :Ce

Compositionally complex oxides have garnered increasing interest for their enhanced phase stability and tunable functional properties, yet their development as bulk single crystal scintillators remains limited. Herein, we report the Czochralski growth and characterization of (Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce (GYTLAG), a compositionally complex garnet incorporating four dodecahedrally coordinated principal rare earth elements. The garnet phase was confirmed by powder and single crystal X-ray diffraction, and macroscopic defects are described. X-ray absorption near-edge structure measurements confirm the 3+ oxidation state of all rare earths and support their occupation of the same crystallographic site; white line intensity variations correlate with the anticipated segregation behavior. Elemental segregation is quantified by SEM/EDS and ICP-OES, and a linear trend was established between the segregation coefficient and the difference between each rare earth’s ionic radius (r) and the average ionic radius (AIR) of the dodecahedral site. This trend offers a predictive framework for compositional control in future REAG crystals grown by the Czochralski method. Photoluminescence and radioluminescence measurements reveal both Ce3+ and Tb3+ emission. Scintillation pulses exhibit four-component decay with dominant ∼230 μs and ∼1.2 ms components, and the light yield is estimated to be up to 43,000 ph/MeV under 137Cs γ-ray excitation. GYTLAG also demonstrates a strong radioluminescence efficiency and 50% lower afterglow at 20 ms compared to a LuAG:Ce reference, underscoring its promise for scintillator applications.

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Publication Details

Journal
Crystal Growth & Design
Published
2025-11-06
DOI
https://doi.org/10.1021/acs.cgd.5c01030
Citations
1
Primary Topic
Radiation Detection and Scintillator Technologies
Type
article
Field-Weighted Citation Impact
1.88
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Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce

Haidong Zhou, Arjen van Veelen, Luis Stand, Michael Köehler et al.
1 citations
Crystal Growth & Design
Radiation Detection and Scintillator Technologies
1.88
article

Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce

Haidong Zhou, Arjen van Veelen, Luis Stand, Michael Köehler, Charles L. Melcher, Mariya Zhuravleva, Rebecca A. Lalk, Yauhen Tratsiak, Nicholas Anastasi, Aya Rutherford
article en
1 citations

Abstract

Compositionally complex oxides have garnered increasing interest for their enhanced phase stability and tunable functional properties, yet their development as bulk single crystal scintillators remains limited. Herein, we report the Czochralski growth and characterization of (Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce (GYTLAG), a compositionally complex garnet incorporating four dodecahedrally coordinated principal rare earth elements. The garnet phase was confirmed by powder and single crystal X-ray diffraction, and macroscopic defects are described. X-ray absorption near-edge structure measurements confirm the 3+ oxidation state of all rare earths and support their occupation of the same crystallographic site; white line intensity variations correlate with the anticipated segregation behavior. Elemental segregation is quantified by SEM/EDS and ICP-OES, and a linear trend was established between the segregation coefficient and the difference between each rare earth’s ionic radius (r) and the average ionic radius (AIR) of the dodecahedral site. This trend offers a predictive framework for compositional control in future REAG crystals grown by the Czochralski method. Photoluminescence and radioluminescence measurements reveal both Ce3+ and Tb3+ emission. Scintillation pulses exhibit four-component decay with dominant ∼230 μs and ∼1.2 ms components, and the light yield is estimated to be up to 43,000 ph/MeV under 137Cs γ-ray excitation. GYTLAG also demonstrates a strong radioluminescence efficiency and 50% lower afterglow at 20 ms compared to a LuAG:Ce reference, underscoring its promise for scintillator applications.

Crystal Growth & DesignVol. 25(22)
Los Alamos National Laboratory (US), Radiation Monitoring Devices (United States) (US), International Centre for Diffraction Data (US), Materials Research Center (IN), University of Tennessee at Knoxville (US)
Openalex Percentile: Top 12%
Radiation Detection and Scintillator Technologies
1.88
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