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Highly efficient near-UV-excitable Ca2YHf2Al3O12:Ce3+,Tb3+ green-emitting garnet phosphors with potential application in high color rendering warm-white LEDs
Journal of Materials Chemistry C ( IF 5.7 ) Pub Date : 2020/02/14 , DOI: 10.1039/d0tc00130a Shaoying Wang 1, 2, 3, 4 , Balaji Devakumar 5, 6, 7, 8 , Qi Sun 1, 2, 3, 4 , Jia Liang 1, 2, 3, 4 , Liangling Sun 1, 2, 3, 4 , Xiaoyong Huang 1, 2, 3, 4
Journal of Materials Chemistry C ( IF 5.7 ) Pub Date : 2020/02/14 , DOI: 10.1039/d0tc00130a Shaoying Wang 1, 2, 3, 4 , Balaji Devakumar 5, 6, 7, 8 , Qi Sun 1, 2, 3, 4 , Jia Liang 1, 2, 3, 4 , Liangling Sun 1, 2, 3, 4 , Xiaoyong Huang 1, 2, 3, 4
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Inorganic phosphors with broadband near-ultraviolet (near-UV) excitation and efficient visible emission are highly important for fabricating high-performance near-UV-pumped white light-emitting diodes (LEDs). Herein, we report on novel efficient near-UV-excitable Ce3+/Tb3+ ion co-activated Ca2YHf2Al3O12 (CYHA) green-emitting garnet phosphors, which were successfully prepared through a high-temperature solid-state reaction process. X-ray diffraction, field-emission scanning electron microscopy, energy-dispersive X-ray spectroscopy, elemental mapping, photoluminescence, CIE color coordinates, the internal and external quantum efficiency, and temperature-dependent emission spectra were used to characterize the samples. Interestingly, due to the efficient energy transfer from Ce3+ to Tb3+ ions in CYHA, the CYHA:Ce3+,Tb3+ samples presented a wide excitation band in the 370–470 nm region peaking around 408 nm owing to the 4f–5d transition of Ce3+ ions, and under 408 nm excitation they showed intense characteristic sharp green emission around 543 nm corresponding to the 5D4 → 7F0–6 transitions of Tb3+ ions. The energy transfer mechanism from Ce3+ to Tb3+ ions was ascribed to the quadruple–quadruple interaction, and the energy transfer efficiency reached as high as 93.2%. Notably, the composition-optimized CYHA:0.03Ce3+,0.6Tb3+ sample exhibited a high internal quantum efficiency (IQE) of 78.5% and external quantum efficiency (EQE) of 56%, which were much higher than those of the Tb3+ singly-activated CYHA:0.6Tb3+ sample (IQE = 8%, EQE = 2.2%). Finally, a prototype white LED device was made by combining a 400 nm near-UV-emitting LED chip with a phosphor blend of the as-prepared CYHA:0.03Ce3+,0.6Tb3+ green phosphors, commercial BaMgAl10O17:Eu2+ blue phosphors and commercial CaAlSiN3:Eu2+ red phosphors, which emitted bright warm-white light with good CIE chromaticity coordinates of (0.391, 0.356), a low correlated color temperature of 3528 K and a high color rendering index of 92.3 under 120 mA driving current. This work opens up new opportunities for the development of efficient color converters toward near-UV-pumped warm-white LEDs with high color rendering index.
中文翻译：
高效近紫外激发的Ca2YHf2Al3O12：Ce3 +，Tb3 +发射绿色的石榴石磷光体，可能在高显色暖白光LED中应用
具有宽带近紫外（近UV）激发和有效可见光发射的无机磷光体对于制造高性能近紫外泵浦的白色发光二极管（LED）至关重要。在此，我们报道了新型有效的近紫外可激发Ce 3+ / Tb 3+离子共激活的Ca 2 YHf 2 Al 3 O 12。（CYHA）发射绿色石榴石的荧光粉，它是通过高温固态反应过程成功制备的。X射线衍射，场发射扫描电子显微镜，能量色散X射线光谱，元素映射，光致发光，CIE色坐标，内部和外部量子效率以及与温度有关的发射光谱被用来表征样品。有趣的是，由于CYHA中从Ce 3+到Tb 3+离子的有效能量转移，CYHA：Ce 3+，Tb 3+样品在370-470 nm区域出现了一个宽激发带，由于在408 nm附近达到峰值。 Ce 3+的4f-5d转变离子，在408 nm激发下，它们在543 nm附近显示出强烈的特征性鲜明绿色发射，对应于Tb 3+离子的5 D 4 → 7 F 0-6跃迁。从Ce 3+到Tb 3+离子的能量转移机理归因于四重四重相互作用，能量转移效率高达93.2％。值得注意的是，经成分优化的CYHA：0.03Ce 3+，0.6Tb 3+样品具有78.5％的高内部量子效率（IQE）和56％的外部量子效率（EQE），远高于Tb 3+单激活CYHA：0.6Tb3个以上的样本（IQE = 8％，EQE = 2.2％）。最后，通过将400 nm近紫外光发射LED芯片与所制备的CYHA：0.03Ce 3+，0.6Tb 3+绿色荧光粉，商用BaMgAl 10 O 17的荧光粉混合物结合在一起，制成了原型白光LED器件： Eu 2+蓝色荧光粉和商用CaAlSiN 3：Eu 2+红色磷光体发出明亮的暖白光，在120 mA驱动电流下具有良好的CIE色度坐标为（0.391，0.356），较低的相关色温为3528 K和较高的显色指数为92.3。这项工作为高效彩色转换器向具有高显色指数的近紫外泵浦的暖白LED的开发提供了新的机会。
更新日期：2020-04-03
中文翻译：
高效近紫外激发的Ca2YHf2Al3O12：Ce3 +，Tb3 +发射绿色的石榴石磷光体，可能在高显色暖白光LED中应用
具有宽带近紫外（近UV）激发和有效可见光发射的无机磷光体对于制造高性能近紫外泵浦的白色发光二极管（LED）至关重要。在此，我们报道了新型有效的近紫外可激发Ce 3+ / Tb 3+离子共激活的Ca 2 YHf 2 Al 3 O 12。（CYHA）发射绿色石榴石的荧光粉，它是通过高温固态反应过程成功制备的。X射线衍射，场发射扫描电子显微镜，能量色散X射线光谱，元素映射，光致发光，CIE色坐标，内部和外部量子效率以及与温度有关的发射光谱被用来表征样品。有趣的是，由于CYHA中从Ce 3+到Tb 3+离子的有效能量转移，CYHA：Ce 3+，Tb 3+样品在370-470 nm区域出现了一个宽激发带，由于在408 nm附近达到峰值。 Ce 3+的4f-5d转变离子，在408 nm激发下，它们在543 nm附近显示出强烈的特征性鲜明绿色发射，对应于Tb 3+离子的5 D 4 → 7 F 0-6跃迁。从Ce 3+到Tb 3+离子的能量转移机理归因于四重四重相互作用，能量转移效率高达93.2％。值得注意的是，经成分优化的CYHA：0.03Ce 3+，0.6Tb 3+样品具有78.5％的高内部量子效率（IQE）和56％的外部量子效率（EQE），远高于Tb 3+单激活CYHA：0.6Tb3个以上的样本（IQE = 8％，EQE = 2.2％）。最后，通过将400 nm近紫外光发射LED芯片与所制备的CYHA：0.03Ce 3+，0.6Tb 3+绿色荧光粉，商用BaMgAl 10 O 17的荧光粉混合物结合在一起，制成了原型白光LED器件： Eu 2+蓝色荧光粉和商用CaAlSiN 3：Eu 2+红色磷光体发出明亮的暖白光，在120 mA驱动电流下具有良好的CIE色度坐标为（0.391，0.356），较低的相关色温为3528 K和较高的显色指数为92.3。这项工作为高效彩色转换器向具有高显色指数的近紫外泵浦的暖白LED的开发提供了新的机会。
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