Research Progress on Vacuum Solid-State Reaction Preparation and Lattice Substitution of TAG Magneto-Optic Ceramics

Abstract

Abstract: As a typical garnet transparent ceramic used in high-energy solid-state laser systems, terbium aluminum garnet (Tb₃Al₅O₁₂, TAG) magneto-optic ceramics have become a focal point of research due to their excellent magneto-optic properties and high-power performance. This paper focuses on TAG magneto-optic ceramics prepared by vacuum solid-state reaction, with particular emphasis on the optimization of sintering aids and lattice doping modifications. By comparison, the most suitable additives for TAG ceramics were identified. The study highlights the longstanding challenge in improving the quality of TAG ceramics, which arises from the reliance on large doses of sintering aids and the resulting compositional inhomogeneity caused by sintering aid residues. To address these issues, we present our latest research, which involves co-doping the lattice with Mg²⁺ and Si⁴⁺. This approach enables the preparation of higher optical quality TAG ceramics via a one-step vacuum solid-state sintering process, without reducing the absolute amount of MgO and TEOS. The best sample achieve a transmittance of 82.48% at 1 064 nm, which, to our knowledge, is the highest value reported using a similar sintering method based on domestic powders. This lattice doping strategy, rather than the traditional mass-ratio addition of sintering aids, offers a promising new approach for further improving the quality of garnet transparent ceramics used in high-energy laser systems.

Key words: TAG, magneto-optic transparent ceramics, sintering aid, compositional inhomogeneity, lattice co-doping, Mg²⁺-Si⁴⁺

CLC Number:

O734

CHEN Jie, SHEN Shiji, TIAN Yanna, ZHOU Shengming. Research Progress on Vacuum Solid-State Reaction Preparation and Lattice Substitution of TAG Magneto-Optic Ceramics[J]. Journal of Synthetic Crystals, 2024, 53(11): 1927-1935.

References

[1] 李晋闽. 高功率全固态激光器研究及应用[J]. 红外与激光工程, 2007, 36(增刊): 1-3.
LI J M. Research and application of high power all-solid-state laser[J]. Infrared and Laser Engineering, 2007, 36(supplement): 1-3 (in Chinese).
[2] YASUHARA R, TOKITA S, KAWANAKA J, et al. Cryogenic temperature characteristics of Verdet constant on terbium gallium garnet ceramics[J]. Optics Express, 2007, 15(18): 11255-11261.
[3] LIN H, ZHOU S M, TENG H. Synthesis of Tb₃Al₅O₁₂ (TAG) transparent ceramics for potential magneto-optical applications[J]. Optical Materials, 2011, 33(11): 1833-1836.
[4] CHEN C, YI X Z, ZHANG S, et al. Vacuum sintering of Tb₃Al₅O₁₂ transparent ceramics with combined TEOS+MgO sintering aids[J]. Ceramics International, 2015, 41(10): 12823-12827.
[5] STAROBOR A, YASYHARA R, SNETKOV I, et al. TSAG-based cryogenic Faraday isolator[J]. Optical Materials, 2015, 47: 112-117.
[6] IKESUE A, AUNG Y L, MAKIKAWA S, et al. Polycrystalline (Tb_xY_1-x)₂O₃ Faraday rotator[J]. Optics Letters, 2017, 42(21): 4399-4401.
[7] YANAGITANI T, NOZAWA H, YAGI H. Transparent rare earth aluminum garnet ceramics: US11053166[P]. 2021-07-06.
[8] IKARI M. Paramagnetic garnet-type transparent ceramic, magneto-optical material and magneto-optical device: US20190353939[P]. 2019-11-21.
[9] DAI J W, SNETKOV I L, PALASHOV O V, et al. Fabrication, microstructure and magneto-optical properties of Tb₃Al₅O₁₂ transparent ceramics[J]. Optical Materials, 2016, 62: 205-210.
[10] DUAN P P, LIU P, XU X D, et al. Fabrication of transparent Tb₃Al₅O₁₂ ceramics by hot isostatic pressing sintering[J]. Journal of the American Ceramic Society, 2017, 100(7): 2893-2900.
[11] ZHANG S Y, LIU P, XU X D, et al. Effect of the MgO on microstructure and optical properties of TAG (Tb₃Al₅O₁₂) transparent ceramics using hot isostatic pressing[J]. Optical Materials, 2018, 80: 7-11.
[12] IKESUE A, AUNG Y L, LUPEI V. Ceramic lasers[M]. Cambridge, UK: Cambridge University Press, 2013.
[13] DAI J W, PAN Y B, XIE T F, et al. Highly transparent Tb₃Al₅O₁₂ magneto-optical ceramics sintered from co-precipitated powders with sintering aids[J]. Optical Materials, 2018, 78: 370-374.
[14] HAO D M, SHAO X C, TANG Y R, et al. Effect of Si⁴⁺ doping on the microstructure and magneto-optical properties of TAG transparent ceramics[J]. Optical Materials, 2018, 77: 253-257.
[15] KLUG F J, PROCHAZKA S, DOREMUS R H. Alumina-silica phase diagram in the mollite region[J]. Journal of the American Ceramic Society, 1987, 70(10): 750-759.
[16] BOYD F R, ENGLAND J L, DAVIS B T C. Effects of pressure on the melting and polymorphism of enstatite, MgSiO₃[J]. Journal of Geophysical Research, 1964, 69(10): 2101-2109.
[17] LI Y K, ZHOU S M, LIN H, et al. Fabrication of Nd∶YAG transparent ceramics with TEOS, MgO and compound additives as sintering aids[J]. Journal of Alloys and Compounds, 2010, 502(1): 225-230.
[18] HAO D M, CHEN J, AO G, et al. Effect of Tb₄O₇ excess on the microstructure and magneto-optical properties of TAG transparent ceramic[J]. Optical Materials, 2019, 94: 47-52.
[19] CHEN J, LIN H, HAO D M, et al. Exaggerated grain growth caused by ZrO₂-doping and its effect on the optical properties of Tb₃Al₅O₁₂ ceramics[J]. Scripta Materialia, 2019, 162: 82-85.
[20] AUNG Y L, IKESUE A. Development of optical grade (Tb_xY_1-x)₃Al₅O₁₂ ceramics as Faraday rotator material[J]. Journal of the American Ceramic Society, 2017, 100(9): 4081-4087.
[21] ZHANG L X, STAROBOR A V, HU D J, et al. Highly transparent Tb₃Al₅O₁₂ ceramics for kilowatt-level Faraday isolator[J]. Journal of the American Ceramic Society, 2024, 107(6): 3653-3658.
[22] HAMAMOTO K, NISHIO M, TOKITA S, et al. Properties of TAG ceramics at room and cryogenic temperatures and performance estimations as a Faraday isolator[J]. Optical Materials Express, 2021, 11(2): 434.
[23] CHEN C, ZHOU S M, LIN H, et al. Fabrication and performance optimization of the magneto-optical (Tb_1-xR_x)₃Al₅O₁₂ (R=Y, Ce) transparent ceramics[J]. 2012, 101(13): 131908.
[24] HAO D M, CHEN J, AO G, et al. Fabrication and performance investigation of Thulium-doped TAG transparent ceramics with high magneto-optical properties[J]. Optical Materials, 2019, 94: 311-315.
[25] YAKOVLEV A I, SNETKOV I L, PALASHOV O V, et al. Magneto-optical and thermo-optical properties of Ce, Pr, and Ho doped TAG ceramics[J]. IEEE Journal of Quantum Electronics, 2019, 55(5): 7000108.
[26] CHEN J, ZHOU S M. TAG magneto-optic ceramics and its application in high power optical isolators[C]//Sixteenth National Conference on Laser Technology and Optoelectronics. June 3-6, 2021. Shanghai, China. SPIE, 2021.
[27] ZHANG L X, HU D J, LI X, et al. Effect of Y substitution on the microstructure, magneto-optical, and thermal properties of (Tb_1-xY_x)₃Al₅O₁₂ transparent ceramics[J]. Journal of Advanced Ceramics, 2024, 13(4): 529-538.
[28] FURUSE H, YASUHARA R, HIRAGA K, et al. High Verdet constant of Ti-doped terbium aluminum garnet (TAG) ceramics[J]. Optical Materials Express, 2015, 6(1): 191.
[29] STAROBOR A, PALASHOV O, ZHOU S M. Thermo-optical properties of terbium-aluminum garnet ceramics doped with silicon and titanium[J]. Optics Letters, 2016, 41(7): 1510-1513.
[30] LI X Y, ZHANG L X, HU D J, et al. Fabrication and characterizations of Tb₃Al₅O₁₂-based magneto-optical ceramics[J]. International Journal of Applied Ceramic Technology, 2023, 20(1): 493-499.
[31] IKESUE A, YOSHIDA K, YAMAMOTO T, et al. Optical scattering centers in polycrystalline Nd∶YAG laser[J]. Journal of the American Ceramic Society, 1997, 80(6): 1517-1522.
[32] CHEN C, NI Y, ZHOU S M, et al. Preparation of (Tb_0.8Y_0.2)₃Al₅O₁₂ transparent ceramic as novel magneto-optical isolator material[J]. Chinese Optics Letters, 2013, 11(2): 21601-21603.
[33] CHEN C, LI X L, FENG Y, et al. Optimization of CeO₂ as sintering aid for Tb₃Al₅O₁₂ Faraday magneto-optical transparent ceramics[J]. Journal of Materials Science, 2015, 50(6): 2517-2521.
[34] SHEN S J, CHEN J, JIANG R J, et al. Fabrication of high optical quality TAG ceramics by vacuum sintering and non-stoichiometric Mg²⁺-Si⁴⁺ co-doping[J]. Journal of the European Ceramic Society, 2025, 45(2): 116893.