Photoluminescence Properties of SrCaLuScAl2Si2O12:Ce3＋ Broadband Green-Emitting Garnet Phosphor and Its Application in White Light-Emitting Diodes

doi:10.6023/A26030065

Abstract

White light-emitting diodes (WLEDs) fabricated by combining blue chips with red and green phosphors enable high-color-quality full-spectrum lighting. However, the development of phosphors featuring broadband green emission is critical for achieving such high-quality full-spectrum illumination. In this study, a garnet-structured broadband green phosphor SrCaLu_1－_xScAl₂Si₂O₁₂:xCe^3＋ (0.01≤x≤0.06, hereafter denoted as SCL:xCe^3＋) was successfully synthesized via a high-temperature solid-state reaction. The optimal doping concentration for SCL:xCe^3＋ was determined to be x=0.04, beyond which concentration quenching occurs due to non-radiative energy transfer between adjacent Ce^3＋ ions. The phosphor exhibits a broad excitation spectrum consisting of two distinct bands centered at approximately 350 and 450 nm, originating from the 4f→5d transitions of Ce^3＋ ions occupying the dodecahedral A sites (Sr^2＋/Ca^2＋/Lu^3＋ positions) in the garnet lattice. The main excitation peak at 450 nm is well matched with the emission of commercial blue LED chips. Upon 450 nm excitation, SCL:0.04Ce^3＋ emits broadband green light covering the spectral range of 470~700 nm with a dominant peak at 530 nm. The emission spectrum can be well deconvoluted into two Gaussian components centered at 526 and 581 nm, corresponding to 5d→²F_5/2 and 5d→²F_7/2 transitions of Ce^3＋, respectively. Notably, compared with the commercial (Ba,Sr)₂SiO₄: Eu^2＋ green phosphor (full width at half maximum, FWHM=71 nm), SCL:0.04Ce^3＋ exhibits a broader emission bandwidth (FWHM=105 nm). The weak electron-phonon coupling in SCL:0.04Ce^3＋ contributes to its high internal/external quantum efficiency (62.4%/23.0%), excellent thermal stability (retaining 69% of its room-temperature luminescence intensity at 423 K), and superior color stability (ΔC=2.1×10^－3 at 423 K). A WLED device fabricated by coating SCL:0.04Ce^3＋ green phosphor together with commercial CaAlSiN₃:Eu^2＋ red phosphor onto a 450 nm blue LED chip achieves a color rendering index (Ra) as high as 93, a correlated color temperature (CCT) of 4685 K, and a luminous efficacy of 124 lm/W under a driving current of 20 mA. As the driving current increases from 20 to 300 mA, the device delivers stable warm white light with high color quality, exhibiting a small CCT variation and negligible color coordinate shift. These results demonstrate that the SCL:0.04Ce^3＋ broadband green phosphor reported herein holds promising potential for high-quality full-spectrum lighting applications.

Key words: SrCaLuScAl₂Si₂O₁₂:Ce^3＋, garnet, broadband green phosphor, white light-emitting diode, high color rendering index

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Hanyue Zhang, Risheng Wang, Hao Yang, Lingling Zhang, Fang Song, Zhihua Leng. Photoluminescence Properties of SrCaLuScAl₂Si₂O₁₂:Ce^3＋ Broadband Green-Emitting Garnet Phosphor and Its Application in White Light-Emitting Diodes[J]. Acta Chimica Sinica, 2026, 84(7): 1087-1095.

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Fig. & Tab. 8

Figure 1. (a) Integrated emission intensity of the SCL:0.01Ce3＋,y%H3BO3 samples, (b) XRD patterns of the SCL:xCe3＋ (0.01≤x≤0.06) samples, (c) XRD refinement result of SCL:0.04Ce3＋ sample, and (d) crystal structure diagram of the SCL host

Figure 2. (a, b) SEM images, (c) particle size distribution and (d~k) EDS elemental mapping of the SCL:0.04Ce3＋ sample

Figure 3. (a) DFT-calculated band structure, (b) PDOS, (c) DOS and (d) UV-Vis diffuse reflectance spectrum of the SCL host (inset: [F(R)hν]2 versus hν curve)

Figure 4. (a) PLE spectra, (b) PL spectra and (c) relative intensity variation, (d) normalized emission spectra, (e) peak position and FWHM, and (f) CIE coordinates of the SCL:xCe3＋ samples (insets show digital photographs taken under daylight and UV light respectively)

Figure 5. (a) Gaussian fitting of the emission spectrum for SCL:0.04Ce3＋, (b) schematic diagram of energy level transitions, normalized (c) excitation and emission spectra and (d) integrated intensities at different excitation wavelengths for SCL:0.04Ce3＋ and commercial (Ba,Sr)₂SiO₄:Eu2＋ phosphors, and (e) internal/external quantum efficiencies at different excitation wavelengths and (f) fluorescence decay curves of the SCL:0.04Ce3＋ sample

Figure 6. (a) Temperature-dependent emission spectra, (b) fitting plot of ln(I0/I－1) versus 1/kT, (c) variations of peak position and FWHM with temperature, (d) temperature-dependent fitting curve of FWHM, (e) temperature-dependent CIE coordinates (inset: digital photograph of the corresponding sample) and (f) chromaticity shift as a function of temperature for the SCL:0.04Ce3＋ sample

荧光粉	λ_em/nm	λ_ex/nm	FWHM/nm	IQE/%	I_{423 K}	Ref
CaY₂ZrScAl₃O₁₂:Ce^3＋	514	421	113	63.1	55	[17]
Ca₂LaHf₂Al₃O₁₂:Ce^3＋	515	408	116	46.5	24	[36]
Ca₂LaZr₂Ga₃O₁₂:Ce^3＋	515	430	102	35.2	30	[37]
Lu₃Mg₂GaSi₂O₁₂:Ce^3＋	530	460	93.98	32.6	81.94	[38]
BaY₂Sc₂Al₂SiO₁₂:Ce^3＋	532	439	125	80.1	73.9	[39]
LuMgAl₅SiO₁₂:Ce^3＋	528	436	102	53.7	51	[40]
Y₂BaScAl₃SiO₁₂:Ce^3＋	541	452	121	72.3	62	[41]
SrLu₂Al₃ScSiO₁₂:Ce^3＋	525	439	111	93	44	[42]
Lu_1.5Ca_1.5Al_3.5Si_1.5O₁₂:Ce^3＋	533	451	108	92.2	76	[43]
SCL:0.04Ce^3＋	530	450	105	62	69	This work

Table 1. Performance parameters of the SCL:0.04Ce3＋ phosphor in comparison with previously reported garnet-type green phosphors

Figure 7. (a) EL spectra (inset is the corresponding digital photograph) and (b) CRI values of the WLED device, (c) photographs of pencils illuminated by the commercial fluorescent lamp and fabricated WLED device, and (d) EL spectra, (e) CIE chromaticity diagram and (f) CIE 1931 chromaticity coordinates of the fabricated WLED device at different driving currents

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SrCaLuScAl₂Si₂O₁₂:Ce^3＋宽带绿色荧光粉的发光性能及其在白光发光二极管上的应用

Photoluminescence Properties of SrCaLuScAl₂Si₂O₁₂:Ce^3＋ Broadband Green-Emitting Garnet Phosphor and Its Application in White Light-Emitting Diodes

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SrCaLuScAl2Si2O12:Ce3＋宽带绿色荧光粉的发光性能及其在白光发光二极管上的应用