Shaping scintillation and UV-VIS-NIR luminescence properties through synergistic lattice disordered engineering and exciton-mediated energy transfer in Pr3+-doped Lu1.5Y1.5Al5−xScxO12 (x = 0.0–2.0) garnets

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61389005%3A_____%2F25%3A00636320" target="_blank" >RIV/61389005:_____/25:00636320 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/68378271:_____/25:00638638 RIV/61389021:_____/25:00648059 RIV/68407700:21340/25:00385588

Výsledek na webu

<a href="https://pubs.rsc.org/en/content/articlelanding/2025/tc/d5tc01411e" target="_blank" >https://pubs.rsc.org/en/content/articlelanding/2025/tc/d5tc01411e</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1039/d5tc01411e" target="_blank" >10.1039/d5tc01411e</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Shaping scintillation and UV-VIS-NIR luminescence properties through synergistic lattice disordered engineering and exciton-mediated energy transfer in Pr3+-doped Lu1.5Y1.5Al5−xScxO12 (x = 0.0–2.0) garnets

Popis výsledku v původním jazyce

This study investigated the crystallization behavior, luminescence and scintillation properties of Pr3+-doped Lu1.5Y1.5Al5-xScxO12 (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 Sc3+ for Al3+ 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 Sc3+ substitution caused localized melt heterogeneity, resulting in non-uniform melt ejection during crystallization. The threshold of Sc3+ 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 Sc3+ 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 Lu1.5Y1.5Al3.5Sc1.5O12 crystal (x = 1.5). The enhancement resulted from a Sc3+-mediated energy transfer pathway , 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 Sc3+ incorporation reduced concentration of trace impurities, enhancing scintillation light yield. It also confirmed that F+-Pr3+ interactions intensified Pr3+ 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 Sc3+ 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.

Název v anglickém jazyce

Shaping scintillation and UV-VIS-NIR luminescence properties through synergistic lattice disordered engineering and exciton-mediated energy transfer in Pr3+-doped Lu1.5Y1.5Al5−xScxO12 (x = 0.0–2.0) garnets

Popis výsledku anglicky

This study investigated the crystallization behavior, luminescence and scintillation properties of Pr3+-doped Lu1.5Y1.5Al5-xScxO12 (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 Sc3+ for Al3+ 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 Sc3+ substitution caused localized melt heterogeneity, resulting in non-uniform melt ejection during crystallization. The threshold of Sc3+ 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 Sc3+ 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 Lu1.5Y1.5Al3.5Sc1.5O12 crystal (x = 1.5). The enhancement resulted from a Sc3+-mediated energy transfer pathway , 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 Sc3+ incorporation reduced concentration of trace impurities, enhancing scintillation light yield. It also confirmed that F+-Pr3+ interactions intensified Pr3+ 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 Sc3+ 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.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

<a href="/cs/project/GF24-14580L" target="_blank" >GF24-14580L: Pokročilé monokrystalické tenkovrstvé scintilátory na bázi komplexních oxidových sloučenin: inženýrství přenosu energie pro optimalizaci výkonu</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Materials Chemistry C

ISSN

2050-7526

e-ISSN

2050-7534

Svazek periodika

13

Číslo periodika v rámci svazku

27

Stát vydavatele periodika

GB - Spojené království Velké Británie a Severního Irska

Počet stran výsledku

22

Strana od-do

13691-13712

Kód UT WoS článku

001503155100001

EID výsledku v databázi Scopus

2-s2.0-105007801254