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Journal of Luminescence
journal homepage: www.elsevier.com/locate/jlumin
School of Textile and Material Engineering, Dalian Polytechnic University, Dalian 116034, China
Department of Electronic Engineering and State Key Laboratory of Millimeter Waves, City University of Hong Kong, Tat Chee Avenue, Kowloon,
Hong Kong, China
art ic l e i nf o
a b s t r a c t
Article history:
Received 28 January 2016
Received in revised form
20 May 2016
Accepted 27 May 2016
Available online 2 June 2016
Sm3 doped multicomponent antimony phosphate (MSP) luminescent glasses were prepared and tunable white uorescence has been investigated. Broad visible emission depending on excitation wavelength is validated to be dominated by discrepant Sb3 emitting centers. Group of narrow emissions
from Sm3 is benecial to adding yellow and red components in Sm3 doped MSP glasses, which is
strengthened by effective energy transfer from Sb3 to Sm3 . Excitation wavelength selection and Sm3
concentration adjustment are two feasible routes to optimize luminescence color in Sm3 doped MSP
glasses and the color tunability of uorescence indicates that amorphous Sm3 doped MSP glass
phosphors possess potential for ideal white light devices.
& 2016 Elsevier B.V. All rights reserved.
Keywords:
Color tunability
Sm3
Antimony phosphate glasses
Glass phosphors
1. Introduction
Inorganic luminescent materials have been intensively investigated for their application in solar energy harvesting, reversed
oxygen sensing, optical information storaging, microbeam radiation curing, vivo bio-imaging and indoor lighting, etc [110]. In the
eld of indoor lighting, Sb3 has received a lot of attention due to
its broad emission covering near ultraviolet to red in spectral
region under deep-UV excitation and Sb3 -containing polycrystalline materials have been successfully used in commercial
white uorescent lamp [11,12]. Compared with polycrystalline
powder, amorphous glasses as lighting matrix have arisen great
interest because of their good thermal stability, long working
lifespan, high mechanical operability and ne emission homogeneity [1336]. Particularly, phosphate glasses with advantages
such as low production cost, high rare earth (RE) ions solubility
and large emission cross sections have been attracted much
interest in recent years [3748].
Fluorescence in Sb3 -containing phosphate glasses exhibits
insufciency of yellow and red components for pure white light,
although broad visible emission is captured and uorescent color
is near white to naked eyes [49,50]. RE ions are often being taken
into consideration to improve light performance due to their
n
Corresponding author.
E-mail addresses: zhangjj@dlpu.edu.cn (J.J. Zhang),
lhai8686@yahoo.com (H. Lin).
http://dx.doi.org/10.1016/j.jlumin.2016.05.052
0022-2313/& 2016 Elsevier B.V. All rights reserved.
2. Experimental details
MSP host glasses were prepared from Na2CO3, BaCO3, Al(OH)3, ZnO,
Sb2O3, and NH4H2PO4 powders according to the molar composition
15.11Na2O0.85BaO9.82Al2O313.84ZnO5.02Sb2O355.36P2O5. Additional 0.1 wt%, 0.5 wt%, 1.0 wt% and 2.0 wt% Sm2O3 was introduced into
MSP glass composition based on host weight to prepare Sm3 doped
MSP glasses, respectively. Firstly, the well-mixed powders were
148
Fig. 1. Normalized emission and excitation spectra of MSP host glasses. Inserted
photo shows uorescence from MSP host glasses under 254 nm UV lamp radiation.
Fig. 2. XRD pattern of 0.5 wt% Sm2O3 doped MSP glass powder. Inset shows DTA
curve of 0.5 wt% Sm2O3 doped MSP glasses.
149
Fig. 6. Emission spectra of Sm3 doped MSP glasses under excitation of 254 nm.
Inserted photos show uorescences from relevant Sm3 doped MSP glasses under
254 nm UV lamp radiation.
Fig. 5. Peak-normalized relative spectral distributions (left) and color coordinates in CIE-1931 chromaticity diagrams (right) for MSP host glasses. Points 1 to 4 correspond to
host glass under the excitation of 240, 260, 280 and 300 nm, respectively.
150
Fig. 7. Peak-normalized relative spectral distributions (left) and color coordinates in CIE-1931 chromaticity diagrams (right) for Sm3 doped MSP glasses under 254 nm
excitation. Points 14 correspond to undoped, 0.5 wt%, 1.0 wt% and 2.0 wt% Sm2O3 doped MSP glasses under the excitation of 254 nm, respectively.
Fig. 10. Absorption spectrum of 2.0 wt% Sm2O3 doped MSP glasses.
Ref.
Li2OZnOSrOP2O5B2O3
NaFAlF3ZnONa2HPO4P2O5
PbOGeO2TeO2
PbF2WO3TeO2
KFK2OBaOAl2O3P2O5
Li2OZnF2PbOP2O5B2O3
Li2OAlF3TeO2B2O3
CaF2CaOBaOAl2O3B2O3
PbOBaOZnOLiFB2O3
K2OCaOZnOTeO2
Na2OB2O3SiO2
K2OBaF2La2O3SiO2
Na2OBaOAl2O3ZnOSb2O3P2O5
0.44
0.63
0.73
1.30
1.50
1.53
1.61
1.92
2.44
2.48
2.74
2.81
3.08
2.91
5.84
4.56
3.08
3.75
2.94
3.53
6.35
8.54
2.99
2.10
3.05
3.36
2.29
4.56
2.05
1.54
1.89
2.71
1.79
3.44
6.40
1.82
5.86
1.52
1.81
[81]
[82]
[83]
[84]
[85]
[86]
[87]
[88]
[89]
[90]
[91]
[64]
This work
Table 2
Spontaneous transition probabilities Arad, uorescence branching ratios ij, and
radiative lifetime rad of Sm3 in MSP glasses.
Transition
from 4G5/2 to
Energy
(cm 1)
7407
8788
9947
10793
11283
11416
11527
12882
14300
15634
16844
17878
0.20
1.90
2.43
14.31
2.19
0.22
1.93
3.45
26.16
96.57
90.80
7.09
F11/2
F9/2
6
F7/2
6
F5/2
6
F3/2
6
H15/2
6
F1/2
6
H13/2
6
H11/2
6
H9/2
6
H7/2
6
H5/2
6
0
0
1.19
3.79
5.53
0
0
0
0
0
12.95
15.36
0.20
1.90
3.62
18.10
7.72
0.22
1.93
3.45
26.16
96.57
103.75
22.45
0.07
0.66
1.27
6.33
2.70
0.08
0.67
1.21
9.14
33.75
36.27
7.85
3.50
151
Fig. 11. Fluorescence decay (ex 400 nm, em 600 nm) curves for the 6H7/2 level of Sm3 in 0.1 wt%, 0.5 wt%, 1.0 wt% and 2.0 wt% Sm2O3 doped MSP glasses.
152
exp-avg
(ms)
0.1
0.5
1.0
2.0
3.25
3.14
2.76
2.33
92.9
89.6
78.8
66.6
22.0
22.0
22.0
22.0
10.8
54.6
121.5
Fig. 12. Emission spectra of 0.5 wt% Sm2O3 doped MSP glasses under different excitations. Inset: Photos in (d) and (e) present uorescences of 0.5 wt% Sm2O3 doped MSP
glasses under 308 nm LED excitation and 365 nm UV lamp radiation, respectively.
153
Fig. 13. Relative spectral distributions (left) and color coordinates in CIE-1931 chromaticity diagrams (right) for 0.5 wt% Sm2O3 doped MSP glasses under different excitations. Points 15 correspond to 0.5 wt% Sm2O3 doped MSP glasses under the excitation of 240, 260, 280, 315 and 360 nm, respectively.
Fig. 14. Emission spectra of 2.0 wt% Sm2O3 doped MSP glasses under different excitation wavelength. Inset: Photos in (d) and (e) show uorescences of 2.0 wt% Sm2O3 doped
MSP glasses under 308 nm LED excitation and 365 nm UV lamp radiation, respectively.
observed in 0.5 wt% Sm2O3 doped MSP glasses under 308 nm LED
excitation, as inserted photo in Fig. 12(d). At excitation of 360 nm,
emission component mainly comes from Sm3 and the CIE chromaticity point is located in yellow region, as shown in Fig. 13. The
orange emission could be validated by photo of uorescence color,
as inset in Fig. 12(e). Emission spectra indicate that excitation
wavelength selection is still a feasible way to tune luminescence
color of Sm3 doped MSP glasses.
For investigating uorescence behavior of MSP glasses with
high Sm3 concentration, emission spectra of 2.0 wt% Sm2O3
doped MSP glasses under various excitation wavelengths are
presented in Fig. 14. Warm white and bright orange uorescences
are observed in 2.0 wt% Sm2O3 doped MSP glass under 308 nm
LED excitation and 365 nm UV lamp radiation, as exhibited in
photos in Fig. 14(d) and (e), respectively. With concentration
increase of Sm3 , obvious intensity decrease of Sb3 and clear
intensity increase of Sm3 occurs, reecting on color coordinates
4. Conclusions
Sm3 doped multicomponent antimony phosphate luminescent (MSP) glasses were prepared and tunable white uorescence
has been investigated. Bluishwhite uorescence dominated by at
least two discrepant Sb3 emitting centers in MSP host glasses is
observed under UV excitation. Radiative transition parameters of
154
Fig. 15. Relative spectral distributions (left) and color coordinates in CIE-1931 chromaticity diagrams (right) for 2.0 wt% Sm2O3 doped MSP glasses under different excitations. Points 1 to 5 correspond to 2.0 wt% Sm2O3 doped MSP glasses under the excitation of 240, 260, 280, 315 and 360 nm, respectively.
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
Acknowledgments
This work was supported by the Scientic Research Foundation
for Universities from Education Bureau of Liaoning Province
(L2014226) and the Science and Technology Foundation of Liaoning Province, China (2015020187).
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