JOURNAL OF RARE EARTHS, Vol. 35, No. 6, Jun. 2017, P.

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Optically stimulated luminescence (OSL) of LiMgPO4:Tm,Tb phosphor

GUO Jingyuan (郭竞渊), TANG Qiang (唐 强)*, ZHANG Chunxiang (张纯祥), LUO Daling (罗达玲),
LIU Xiaowei (刘小伟)
(School of Physics, Sun Yat-sen University, Guangzhou 510275, China)

Received 15 September 2016; revised 14 November 2016

Abstract: LiMgPO4:Tm,Tb phosphors were synthesized using a solid-state diffusion method. Their properties were investigated us-
ing X-ray diffraction (XRD), thermoluminescence (TL), scanning electron microscopy (SEM), and OSL dosimetric techniques. The
influence of light stimulation and thermal excitation on the TL and OSL, and the reusability of the phosphors for OSL regenaration
were also studied. The LiMgPO4:Tm,Tb phosphor exhibited high sensitivity to ionizing radiation, good signal reusability and a broad
linear dose response range (0.1–1000 Gy). Fading of the OSL signal was about 16% in eight days, after that the intensity kept stable.
The excellent luminescent and dosimetric properties of these LiMgPO4:Tm,Tb phosphors enable them to be promising candidates in
radiation dosimetry.

Keywords: optically stimulated luminescence; thermoluminescence; dosimetric properties; LiMgPO4:Tm,Tb; rare earths

Optically stimulated luminescence is currently a very
popular approach in radiation dosimetry. The advantages
and disadvantages of thermoluminescence and OSL in
the field of radiation dosimetry have been discussed by
McKeever and Moscovitch[1]. Much effort has been
dedicated to preparing artificial materials with OSL
properties, e.g., α-Al2O3:C crystals[2,3], SrSO4:Eu[4],
MgO:Tb[5], LiAlO2:Tb/Ce[6], MgAl2O4:Tb[7], and
Y3Al5O12:C[8]. In recent years, Zhang et al.[9] have stud-
ied the luminescence properties of LiMgPO4:Eu and the
effect of doping concentration on its crystal structure.
The LiMgPO4:Tb,B phosphor developed by Dhabekar et
al.[10] exhibited strong OSL, and its main TL peaks were
observed at approximately 230 ºC and 410 ºC. Menon et
al.[11] developed a LiMgPO4:Tb phosphor with the sensi-
tivity 2.5 times greater than that of CaSO4:Dy and the
upper limit of 1 kGy for the linear dose response. Gai et
al.[12] found that the OSL intensity of Sm3+ doped to
LiMgPO4:Tb,B could increase twice more than that of
LiMgPO4:Tb,B and reported that this material could be
used for real-time OSL dose measurements.
Recently, a new phosphor of LiMgPO4:Tm,Tb has
been successfully synthesized via high-temperature
solid-state reaction in our laboratory. This material ap-
pears to exhibit excellent OSL properties. In this study,
we synthesized LiMgPO4:Tm,Tb phosphors and studied
their OSL intensity, reusability, fading and TL glow
curves as well as their OSL dose response. These results
suggest promising applications of LiMgPO4:Tm,Tb
phosphors in radiation dosimetry. This work extends the
application of rare earth luminescent materials, particu-
larly in the radiometric techniques.
1 Experimental
The materials used in the preparation of LiMgPO4:
Tm,Tb were analytical-grade LiOH·H2O, NH4H2PO4 and
Mg(NO3)2·6H2O, and powder of rare earth Tm2O3
(99.9%) and Tb4O7 (99.9%) with Tm and Tb molarities
of 0.5 mol.%.
The samples were synthesized using high-temperature
solid-state reaction method. The appropriate relative
amounts of LiOH·H2O, NH4H2PO4, Mg(NO3)2·6H2O and
rare earth impurities were placed in an agate mortar, and
the mixture was fully ground into a smooth paste with a
moderate amount of deionized water. The mixture was
placed into a small alumina cup and evaporated to
dryness with an electric hot plate. Then, the mixture was
placed to a furnace and heated for 2 h at 1000 ºC. Finally,
the sample was quenched and cooled rapidly to room
temperature.
The structures of the LiMgPO4 samples were analysed
using a D-MAX 2200 VPC X-ray diffractometer (XRD)
with Cu radiation in a 2θ range of 10º–80º. The result
was compared with the standard card. The morphology
and structure of the as-prepared products were inspected
using scanning electron microscopy (SEM, FEI Quanta
400).
Irradiation and TL/OSL measurements were con-
ducted using an automatic Risø TL/OSL-15-B/C reader

Foundation item: Project supported by the National Natural Science Foundation of China (11375278)
* Corresponding author: TANG Qiang (E-mail: ststq@mail.sysu.edu.cn; Tel.: +86-20-84112748)
DOI: 10.1016/S1002-0721(17)60943-8
526 JOURNAL OF RARE EARTHS, Vol. 35, No. 6, Jun. 2017

system equipped with a 90Sr beta source and a U-340 de-

tection filter. The dose rate of the source was about 0.10
Gy/s. The OSL readouts were obtained using blue light-
emitting diodes (LEDs), with peak emission at 470 nm
and power of 90%. The heating rate of TL measurement
and preheat was 5 ºC/s.

2 Results and discussion

2.1 X-ray diffraction

Fig. 1(a) shows XRD patterns of the standard card of
LiMgPO4, which belongs to the orthorhombic space
group. As shown in Fig. 1(b), the four major peaks ob-
served in the XRD patterns obtained herein agree very
well with those in the standard XRD pattern. In addition,
the Tm3+ and Tb3+ dopants had very few effects on the
structure of the LiMgPO4 phase. The XRD patterns of
the LiMgPO4:Tm,Tb powder are in good agreement with
the standard XRD pattern.

2.2 Scanning electron microscopy (SEM)

The morphology of the material was determined using
a high-resolution scanning electron microscope (SEM).
The main features on the surface of the crystalline LiM-
gPO4:Tm,Tb are depicted in the SEM micrograph in Fig.
2, indicating an uneven morphology with a well defined Fig. 2 Scanning electron microscope (SEM) images of LiMgPO4:
structure including cracks, flakes and well distributed Tm,Tb
fine particles.

2.3 TL
The TL glow curve of LiMgPO4:Tm,Tb powdered
samples irradiated with 90Sr beta radiation doses of 1 Gy
is shown in Fig. 3. The heating rate was 5 ºC/s. The TL
glow curve of LiMgPO4:Tm,Tb phosphor has three main
TL glow peaks, which are located at about 90, 200 and
300 ºC in the range of 0–500 ºC. The peak of LiM-
gPO4:Tm,Tb occurred at about 90 ºC is too low to be
used for practical TLDs. On the other hand, the main peak

Fig. 3 TL glow curve of LiMgPO4:Tm,Tb

occurred at 300 ºC has a good stability for routine TL do-

simetric applications.

2.4 OSL decay curves

Fig. 1 XRD patterns of standard XRD pattern (JCPDS file No.
32-0574) (a) and a powder sample of LiMgPO4:Tm,Tb (b)
The phosphors of LiMgPO4:Tm,Tb and Al2O3:C
(commercial dosimeter) have equal mass exposed to the
same dose (1Gy) by 90Sr beta source. The OSL meas-
urements were conducted at room temperature. The time
per data point was 0.4 s. Continuous wave OSL (CW-
OSL) decay curves of LiMgPO4:Tm,Tb were compared
with that of Al2O3:C under the same measurement condi-
tion shown in Fig. 4. The OSL integral intensities of the
GUO Jingyuan et al., Optically stimulated luminescence (OSL) of LiMgPO4:Tm,Tb phosphor
two samples were compared. The OSL intensity of
LiMgPO4:Tm,Tb phosphor is close to that of Al2O3:C.
The OSL curves of the LiMgPO4:Tm,Tb phosphors
exposed to the same dose (1 Gy) with different preheat
temperatures (40–240 ºC) are shown in Fig. 5. The pre-
heating which lasted 10 s was conducted to empty shal-
low electron traps in the material. The time per data point
was 2 s. In the case of 40 ºC preheating, the OSL inten-
sity of LiMgPO4:Tm,Tb decayed to 58% of maximum
value after 10s of stimulation. The results show that the
OSL intensity gradually declined with increasing preheat
temperature.
The OSL of the samples was measured at a given tem-
perature (read temperature) after direct heating to this
temperature. Similar to the above experiments, we first
preheated the sample to 260 ºC, and then recorded the
OSL signals in various read temperatures from 40 ºC to
240 ºC. The time of the preheating last 10 s and the time
per data point was 2 s. The results are shown in Fig. 6.
Due to the combined action of the light and thermal ex-
citation, a higher luminescence intensity was obtained.
The curve with the highest sensitivity corresponded to a
read temperature of 240 ºC. Preheating the samples to
260 ºC cleared the electrons in the trap corresponding to
the main TL peak at 90 and 200 ºC, but not those in the
trap corresponding to the prominent TL peak at 300 ºC.
Fig. 4 OSL curves of LiMgPO4:Tm,Tb and Al2O3:C phosphors
stimulated with blue LEDs
Fig. 5 OSL signals after different preheating temperatures
527
However, due to thermal assistance, the electrons have
greater excitation probability. Under the effect of light
excitation, the trapped electrons had a higher photoioni-
zation cross-section, leading to a stronger OSL glow.
Therefore, the OSL signals gradually increased with read
temperature, as shown in Fig. 6.
To study the relationship between TL and OSL in the
sample, especially related to the traps at the 300 ºC TL
peak, the following experiment was conducted. First, we
preheated the sample to 240 ºC after irradiation at 1 Gy,
and measured the TL of the samples and then computed
the TL integral intensity (ITL0). Next, we preheated the
sample to 240 ºC after irradiation at 1 Gy again and then
recorded the OSL signal of the sample (read tempera-
tures ranged from 60 to 220 ºC) and computed the OSL
integral intensity (IOSL). Then, we measured the TL of the
samples and computed the TL integral intensity (ITL1).
The results are shown in Fig. 7. The ΔITL would be cal-
culated as ΔITL=ITL0–ITL1. The value of ΔITL indicates the
degree to which the TL signal faded during the OSL
measurement at different read temperatures (60–220 ºC).
The results show that OSL signal is much weaker than
TL fading. It is illustrated that OSL traps are only a sub-
group of the trap centre.
Fig. 6 OSL signals at different read temperatures
Fig. 7 Relationship between TL and OSL (ΔITL indicates the
degree to which the TL signal was fading during the
OSL measurement, IOSL indicates OSL integral intensity
during the OSL measurement. The abscissa indicates
read temperatures during the OSL measurement)
528
2.5 OSL dose response
To study their dose responses, the LiMgPO4:Tm,Tb
phosphors were exposed to a 90Sr beta source at doses
from 0.1 Gy to 1000 Gy. The OSL signals were inte-
grated from 0 s to 7.2 s, and the average OSL signal for
the last 10 s was used for background subtraction, as
shown in Fig. 8. The result indicates that the OSL
dose-response of LiMgPO4:Tm,Tb to beta rays was lin-
ear in the dose range of 0.1–1000 Gy.
2.6 Reusability of LiMgPO4:Tm,Tb
To study the reusability of the phosphors, the samples
were completely bleached at 500 ºC with 120 s and ex-
posed to 1 Gy of 90Sr beta rays. The OSL decay curves
were repeatedly measured 25 times. The intensities of the
ten highest points in the OSL glow curve were summed
to obtain the reported value, as shown in Fig. 9. It can be
seen that the sensitivity of LiMgPO4:Tm,Tb has few
changes in the conditions on bleaching. The results of
this experiment show that the relative standard deviation
for 25 measurements was 0.16%, indicating that the
LiMgPO4:Tm,Tb phosphor samples exhibit good reus-
ability.
2.7 Fading of LiMgPO4:Tm,Tb
Fading study was carried out by exposing the sample
to 1 Gy of 90Sr beta rays, and the exposed samples were
Fig. 8 Dose response curve for LiMgPO4:Tm,Tb
Fig. 9 Reusability of LiMgPO4:Tm,Tb
JOURNAL OF RARE EARTHS, Vol. 35, No. 6, Jun. 2017
kept in lead pot with dark environment before measure-
ment. The samples were measured on the different days
and the result is shown in Fig. 10. It can be seen that
there is a loss of about 16% of the OSL signal within 8
days after which the intensity gets stabilized.
Fig. 10 Fading of OSL signal with time at room temperature
3 Conclusions
A new OSL material LiMgPO4:Tm,Tb phosphor was
prepared via high-temperature solid-state reaction after
heating at 1000 ºC for 2 h. The phosphor exhibited main
TL peak at 300 ºC and its OSL sensitivity was close to
that of Al2O3:C. The LiMgPO4:Tm,Tb phosphor was
polycrystalline powder, and have the advantages of sim-
ple preparation and low cost. In addition, the OSL signals
of LiMgPO4:Tm,Tb phosphors exhibited good linearity
over dose range of 0.1–1000 Gy and good reusability as
well. The disadvantages of the phosphor are that the
components of slow decay are relatively large and the
time of bleaching is relatively long, but the temperature
corresponding to the trap is relatively high, which may
be applied in high temperature environment. Furthermore,
fading study showed that a loss of about 16% of the OSL
signal within 8 days after that the intensity obtained sta-
bilized. The OSL signals after different preheat tempera-
tures revealed that the OSL intensity gradually declined
with increasing preheat temperature. And the OSL sig-
nals gradually increased with read temperature, due to
thermal assistance. The relationship between TL and
OSL illustrated that OSL traps are only a subgroup of the
trap centre. These results suggest that LiMgPO4:Tm,Tb
phosphors have potential to be used in OSL dosimetry.
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