Micro-Inclusion Engineering via Sc Incompatibility for Luminescence and Photoconversion Control in Ce3+-Doped Tb3Al5−xScxO12 Garnet

Author:

Bartosiewicz Karol1,Tomala Robert2,Szymański Damian2ORCID,Albini Benedetta3ORCID,Zeler Justyna4,Yoshino Masao5,Horiai Takahiko5ORCID,Socha Paweł6ORCID,Kurosawa Shunsuke578,Kamada Kei578ORCID,Galinetto Pietro3,Zych Eugeniusz3,Yoshikawa Akira5789

Affiliation:

1. Faculty of Physics, Kazimierz Wielki University, Powstańców Wielkopolskich Street 2, 85-090 Bydgoszcz, Poland

2. Institute of Low Temperature and Structure Research, Polish Academy of Sciences, 50-422 Wrocław, Poland

3. Department of Physics, University of Pavia, Via Bassi 6, 27100 Pavia, Italy

4. Faculty of Chemistry, University of Wrocław, Joliot-Curie Street 14 F, 50-383 Wrocław, Poland

5. New Industry Creation Hatchery Center, Tohoku University, Sendai 9808577, Japan

6. Łukasiewicz Research Network—Institute of Microelectronics and Photonics, Aleja Lotników 32/46, 02-668 Warsaw, Poland

7. Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Sendai 9808577, Japan

8. Institute of Laser Engineering, Osaka University, 2-6 Yamadaoka, Osaka 5650871, Japan

9. C&A Corporation, 1-16-23 Ichibancho, Sendai 9800811, Japan

Abstract

Aluminum garnets display exceptional adaptability in incorporating mismatching elements, thereby facilitating the synthesis of novel materials with tailored properties. This study explored Ce3+-doped Tb3Al5−xScxO12 crystals (where x ranges from 0.5 to 3.0), revealing a novel approach to control luminescence and photoconversion through atomic size mismatch engineering. Raman spectroscopy confirmed the coexistence of garnet and perovskite phases, with Sc substitution significantly influencing the garnet lattice and induced A1g mode softening up to Sc concentration x = 2.0. The Sc atoms controlled sub-eutectic inclusion formation, creating efficient light scattering centers and unveiling a compositional threshold for octahedral site saturation. This modulation enabled the control of energy transfer dynamics between Ce3+ and Tb3+ ions, enhancing luminescence and mitigating quenching. The Sc admixing process regulated luminous efficacy (LE), color rendering index (CRI), and correlated color temperature (CCT), with adjustments in CRI from 68 to 84 and CCT from 3545 K to 12,958 K. The Ce3+-doped Tb3Al5−xScxO12 crystal (where x = 2.0) achieved the highest LE of 114.6 lm/W and emitted light at a CCT of 4942 K, similar to daylight white. This approach enables the design and development of functional materials with tailored optical properties applicable to lighting technology, persistent phosphors, scintillators, and storage phosphors.

Funder

National Science Centre Poland

Publisher

MDPI AG

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