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| 024 | 7 | _ | |a 10.1039/D5TC01411E |2 doi |
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| 100 | 1 | _ | |a Bartosiewicz, Karol |0 P:(DE-H253)PIP1099262 |b 0 |e Corresponding author |
| 245 | _ | _ | |a Shaping scintillation and UV-VIS-NIR luminescence properties through synergistic lattice disordered engineering and exciton-mediated energy transfer in Pr$^{3+}$ -doped Lu$_{1.5}$Y$_{1.5}$ Al$_{5− x}$Sc$_{x}$O$_{12}$ ( x = 0.0–2.0) garnets |
| 260 | _ | _ | |a London [u.a.] |c 2025 |b RSC |
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| 520 | _ | _ | |a This study investigated the crystallization behavior, luminescence and scintillation properties of Pr$^{3+}$-doped Lu$_{1.5}$Y$_{1.5}$Al$_{5−x}$Sc$_x$O$_{12}$ (0.0, 0.5, 1.0, 1.5, 2.0) garnets, grown using the micro-pulling-down method, to address challenges associated with the substitution of Sc$^{3+}$ for Al$^{3+}$ ions due to their mismatched ionic radii in the same octahedral crystallographic site. A specially engineered crucible with five independent crystallization capillaries was used, which revealed that Sc$^{3+}$ substitution caused localized melt heterogeneity, resulting in non-uniform melt ejection during crystallization. The threshold of Sc$^{3+}$ ions concentration (x = 1.5) was identified, beyond which further substitution led to the formation of a garnet/bixbyite-like distorted perovskite hypoeutectic structure. This discovered a novel method for crystallization of hypoeutectic crystal growth by exploiting ionic radii mismatches. Vibrational spectroscopy confirmed that Sc3+ ions incorporation disrupted lattice symmetry, increasing structural disorder around Pr3+ ions. This structural modification significantly enhanced luminescence, particularly in the visible and near-infrared (NIR) ranges, achieving a sixteenfold increase in NIR luminescence intensity. Synchrotron radiation excitation spectra revealed that the band gap energy progressively decreased with increasing Sc$^{3+}$ ions concentration. This finding provided crucial insights for designing materials based on band gap engineering strategies. A sixfold improvement in scintillation light yield, reaching 11 200 photons per MeV, was observed in the Lu$_{1.5}$Y$_{1.5}$Al$_{3.5}$Sc$_{1.5}$O$_{12}$ crystal (x = 1.5). The enhancement resulted from a Sc$^{3+}$-mediated energy transfer pathway $(Sc_{e^- \to h^-}$$^{3+}$$\to Pr^{3+})$, which optimized charge carrier dynamics by reducing deep trapping center density by an order of magnitude while preserving shallow traps. The EPR spectroscopy showed that Sc$^{3+}$ incorporation reduced concentration of trace impurities, enhancing scintillation light yield. It also confirmed that F$^{+}$–Pr$^{3+}$ interactions intensified Pr$^{3+}$ emission at 370 nm and identified the 410–420 nm band as originating from F$^+$–O$^−$ defect pairs. These findings demonstrate that controlled lattice modification through Sc$^{3+}$ incorporation allows for tuning structural and luminescent properties, offering a new approach for the design of advanced scintillators and luminescent materials with improved performance for targeted applications. |
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