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Ce3+掺杂石榴石基荧光材料凭借其良好的物化特性、高荧光转换效率、较短的荧光寿命、激发光谱与紫外/蓝光发光二极管发射谱的高效匹配等特点，被广泛用于照明、显示、医学成像等领域。得益于石榴石结构丰富的阳离子格位，通过多种类基质化学组分取代可实现Ce3+发射波长从460～610 nm范围内的连续可调，不仅大大拓宽了其潜在应用场景，也为Ce3+发光理论的建立和完善提供了广泛的素材。然而随着近年来相关实验探索的大幅增加，种类较为庞杂的Ce3+掺杂石榴石基荧光材料特性与发射波长调控理论常常出现无法解释甚至矛盾之处，成为阻碍Ce3+掺杂石榴石基荧光材料发展的重要瓶颈之一。针对这一问题，本文简要介绍了基质化学组分取代调控Ce3+发射波长的几种主要理论，综述了近年来Ce3+掺杂石榴石基荧光材料的研究进展，并结合理论与实验，主要从[CeO8]畸变因子角度出发，讨论了离子取代对Ce3+发光性能的影响。
Abstract：For the favorable physicochemical properties,high fluorescence conversion efficiencies,a relatively short fluorescence lifetime,and an efficient spectral congruence between excitation and ultraviolet/blue LED emission spectra,Ce～(3+)-doped garnet-based fluorescent materials can be used in encompassing lighting,displays,medical imaging,etc..For leveraging the diverse cation sites within a garnet structure,the emission wavelength of Ce～(3+)can be continuously adjusted from 460 nm to 610 nm via the incorporation of varied matrix chemical constituents.This versatile tunability broadens the horizons of their potential applications and augments the repertoire of materials available for advancing Ce～(3+)luminescence theory.However,recent work on Ce～(3+)-doped garnet-based fluorescent materials has unveiled certain anomalies and even contradictions within the characteristics and the emission wavelength modulation theory,becoming one of the prominent bottlenecks hindering the development of this material.To address this issue,this review represented the relative theories of substrate chemical component substitution and the modulation of Ce～(3+)emission wavelengths.The review also summarized recent advancements in Ce～(3+)-doped garnet-based fluorescent materials,and the influence of ion substitution on Ce～(3+)luminescence performance with the distortion factor of[CeO＿8].This review discussed the Ce～(3+)-doped yttrium aluminum garnet structure as a prototype and comprehensively analyzed the impacts of commonly used doping ions that occupy the[AO＿8],[BO＿6],and[CO＿4]sites on the emission wavelength,thermal quenching resistance,and the[CeO＿8]distortion factor of Ce～(3+).The ion substitution of a single lattice generally necessitates that the substituting ion and the substituted ion have the same valence state and exhibit a minimal disparity in atomic radius.In the case of[AO＿8]lattice substitution,Y～(3+)can be replaced with rare-earth ions,i.e.,Lu～(3+),Tb～(3+),Gd～(3+),and La～(3+).When the radius of the doped rare-earth ions is greater that that of Y～(3+),the emission wavelength of Ce～(3+)shifts towards the red end of the spectrum.Conversely,when the radius is smaller,the shift occurs in the opposite direction.The ion substitution of octahedral lattice sites mainly involves the replacement of Al～(3+)by Ga～(3+),Sc～(3+),and In～(3+).With an escalation in the concentration of doped ions like Ga～(3+),Sc～(3+),and In～(3+),the peak wavelength of the Ce～(3+)emission spectrum has a blue shift.In addition,the incorporation of Sc～(3+)effectively enhances the thermal quenching resistance of Ce～(3+),while the inclusion of Ga～(3+)diminishes the thermal quenching resistance of Ce～(3+).The main substitutions of dodecahedral-octahedral lattice ion pairs include Ca～(2+)–Hf～(4+)and Ca～(2+)–Zr～(4+)replacing Y～(3+)–Al～(3+).The emission and excitation peak wavelengths of Ce～(3+)gradually blueshifts as Ca～(2+)–Hf～(4+)and Ca～(2+)–Zr～(4+)doping contents increase.The substitution of dodecahedral–tetrahedral lattice ions is mainly achieved by M～(2+)–Si～(4+)(M=Mg,Ca,Sr,Ba) replacing Y～(3+)–Al～(3+),with alkaline earth metals occupying the dodecahedral lattice and Si～(4+)occupying the tetrahedral lattice.In the garnet system,when M～(2+)–Si～(4+)replaces Y～(3+)–Al～(3+),the emission wavelength of Ce～(3+)undergoes a blue shift with the increase of M～(2+)ion radius,resulting in improving the thermal stability.The substitution of octahedral–tetrahedral lattice ions mainly involves Mg～(2+)–Si～(4+)/Ge～(4+)replacing Al～(3+)–Al～(3+),where Mg～(2+)occupies the octahedral lattice and Si～(4+)/Ge～(4+)occupies the tetrahedral lattice.Among them,Mg～(2+)–Si～(4+)replacing Al～(3+)–Al～(3+)is an effective method to achieve a large redshift of Ce～(3+)emission wavelength.The introduction of Mg～(2+)–Ge～(4+)also leads to the redshift of Ce～(3+)emission wavelength,but the extent of this redshift is considerably less than that achieved by Mg～(2+)–Si～(4+).The chemical components in dodecahedral-octahedral-tetrahedral lattice co-substitutions are more intricate,with Ca～(2+)and Mg～(2+)occupying the dodecahedral lattice,Mg～(2+),Sc～(3+),and Hf～(4+)occupying the octahedral lattice,and Si～(4+)and Ge～(4+)in the tetrahedral lattice.Different lattice ions on the co–substitution affect the luminescence performance of Ce～(3+).Summary and prospects The effect of ion substitution on the luminescence performance of Ce～(3+)is analyzed via utilizing Ce～(3+)-doped yttrium aluminum garnet fluorescent material as a prototype.The comparative study reveals that the most effective redshift of Ce～(3+)emission wavelength appears when Mg～(2+)–Si～(4+)occupies the octahedral-tetrahedral lattice configuration.This results in a possibility of red shifting the emission wavelength of Ce～(3+)at 610 nm,thereby significantly enhancing the color rendering capabilities of white LED/LD lighting systems.Conversely,an effective blue shift in Ce～(3+)emission wavelength appears in Ca～(2+)–Zr～(4+)located in the dodecahedral-octahedral lattice,with a potential shifting at 460 nm.Furthermore,the inclusion of Sc～(3+)in the octahedral lattice and Ba～(2+)–Si～(4+)in the dodecahedral-tetrahedral lattice markedly improves the thermal quenching resistance of Ce～(3+).Hence,this combination exhibits substantial advantages for high-power LED and LD lighting applications.In contrast,the introduction of Ca～(2+)–Mg～(2+)–Si～(4+)/Ge～(4+)into the dodecahedral-octahedral-tetrahedral lattice configuration leads to a poor thermal quenching resistance for Ce～(3+),indicating a unsuitability for white light LED/LD illumination.Furthermore,the d＿(88)/d＿(81) ratio is related to the Ce～(3+)emission wavelength and thermal stability,based on the degree of[CeO＿8]distortion.It is indicated that at an equivalent Ce～(3+)doping concentration,an increase in the d＿(88)/d＿(81) ratio corresponds to a redshift in emission wavelength and a decrease in thermal stability.Among the research results available,little work on the impact of d＿(88)/d＿(81)value on the luminescence performance has been done yet.A future research on the in-depth physical models and subsequent experimental validation for Ce～(3+)-doped garnet-based fluorescent materials is needed.
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基本信息:
DOI：10.14062/j.issn.0454-5648.20230668
中图分类号:O482.31
引用信息:
[1]田燕娜,范金太,姜本学,等.Ce~(3+)掺杂石榴石基荧光材料的光谱调控研究进展[J].硅酸盐学报,2024,52(03):1128-1148.DOI:10.14062/j.issn.0454-5648.20230668.
基金信息:
上海市自然科学基金面上项目(22ZR1470800)
2024-02-20
2024-02-20
2024-02-20