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Radiation Protection Dosimetry (2006), Vol. 119, No. 1–4, pp.

402–407
doi:10.1093/rpd/nci579 Advance Access published on April 27, 2006

THERMOLUMINESCENCE GLOW CURVES AND OPTICAL


STIMULATED LUMINESCENCE OF UNDOPED a-Al2O3
CRYSTALS
C. X. Zhang1,, Q. Tang1, L. B. Lin2 and D. L. Luo1
1
Department of physics, Zhongshan University, Guangzhou 510275, China
2
Radiation and Technology Laboratory, Sichuan University, Chengdu 610064, China

The characteristics of thermoluminescence (TL) and optical stimulated luminescence (OSL) in undoped a-Al2O3 single

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crystals were studied. The TL glow curves of the crystal samples irradiated at various dose levels were measured by RisØ
TL/OSL-DA-15B/C reader with U-340 or 7-59 filters at different heating rates. The glow peaks measured with U-340 at
210 C of the undoped a-Al2O3 can be well fitted by first-order kinetic equation whereas the glow peaks measured with 7-59
filters are a composite of two first-order glow peaks. It indicates that the TL glow curves are dependent upon the filter used in
the reader that is related to the emission spectra of luminescence materials. The OSL were also measured and fitted by two
exponential functions to get the luminescence intensities. The TL and OSL dose responses of the undoped a-Al2O3 crystal
were obtained in the dose range of 0.12–248 Gy and fitted by the composite action dose–response function to get nonlinear
characteristic parameters. The TL and OSL dose responses are linear–sublinear.

INTRODUCTION MATERIALS AND METHODS


The a-Al2O3 single crystals undoped or doped with The undoped a-Al2O3 single crystalline samples used
certain dopants, such as transition elements and in this experiment were grown with the flame fusion
carbon, have been studied for several decades and method in the Radiation and Technology Laborat-
used in radiation dosimetry. The TL phenomena of ory(7) at Sichuan University. The TL glow curves
a-Al2O3 single crystal irradiated with ultraviolet were measured by the RisØ TL/OSL-DA-15B/C
light, X rays and gamma rays were reviewed by reader using U-340 or 7-59 filters. The OSL were
Summers(1) 20 y ago. Akselrod et al.(2,3) reported always measured by the same equipment with a
the use of a-Al2O3:C highly sensitive TL and OSL U-340 filter with stimulation of blue lights (470 nm).
detectors in radiation dosimetry. Since then Kortov The TL emission spectra were also obtained with a
et al.(4) and Kitis et al.(5) have studied thermal spectrometer, which includes a linear heater and
quenching processes in a-Al2O3:C crystals and Ocean Optics optical spectrometer with a temperat-
reported that the peak shape and peak temperature ure control system(8). The TL wavelength range cov-
of the TL glow curves are related to the radiation ered in the experiments is from 200 to 800 nm and
dose irradiated on the crystals and to the heating the resolution of wavelength is 3 nm. The spectral
rate during the TL readout stage. They suggested intensity was corrected with the detector response
that the TL glow peaks of a-Al2O3:C are not first-
order kinetic peaks. Their experimental results also 3.0
show that after thermal quenching of a-Al2O3:C
crystals, the shape of TL glow peaks were distorted F
2.5
on the high temperature side, and the peak shifts
to higher temperature by increasing the heating
rates(6).
Optical Density

2.0
In this paper the characteristics of TL and OSL in
the undoped a-Al2O3 single crystals were studied. 1.5
The TL glow curves at various heating rates with
different filters in the TL reader were measured for 1.0
kinetic analysis. The dose responses of TL and OSL F+
in the undoped a-Al2O3 single crystals were also
0.5
analysed and reported.

0.0
200 250 300 350
Wavelength (nm)

Figure 1. Optical absorption spectrum of undoped



Corresponding author: [email protected] a-Al2O3 crystal.

Ó The Author 2006. Published by Oxford University Press. All rights reserved. For Permissions, please email: [email protected]
TL AND OSL OF UNDOPED a-Al2O3 CRYSTALS

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Figure 2. Isometric plot of TL emission spectra of undoped a-Al2O3 crystal irradiated with gamma rays at 100 Gy for a
heating rate of 5 C s1.

9000

1
7500

6000 2
TL intesity (a. u.)

3
4
4500 5
6
8
10
3000 15 20

1500

0
50 100 150 200 250 300 350
Temperature (oC)

Figure 3. Experimental glow curves of undoped a-Al2O3 crystal for the heating rates from 1 to 20 C s1 with
U-340 filter.

function. A heating rate of 5 C s1 was used in the spectrometer is shown in Figure 1. The intensive
3-D spectral measurements. Before the emission 205 nm band owing to F-centre and the 230 nm
spectral measurements the samples were annealed bands owing to Fþ centre reported by
at 600 C for 15 min and then irradiated with 60Co investigators(1,2) are shown in Figure 1. The isomet-
gamma rays at 100 Gy. ric plot of TL emission spectrum of the undoped
a-Al2O3 crystal irradiated by gamma rays at 100 Gy
is shown in Figure 2. It is assumed that the emission
RESULTS AND DISCUSSIONS peak at 210 C with 416 nm is due to the relaxation
of an electron from the excited 3P state to the 1S
Absorption and emission spectra
ground state in the F-centre and a sharp line with
The optical absorption spectrum of the undoped 695 nm owing to internal transitions of Cr3þ ions
a-Al2O3 measured with a UV-Lambda 900 (R lines)(6). However, the emission band at 320 nm
403
C. X. ZHANG ET AL.
þ
owing to radiative decay of F centre has not been It can be seen that the values of peak height as well
observed in the experiment. as peak area reduce with increase in heating rate
whereas the values of activation energy as well as
Heating rate dependence of TL characteristics frequency factor increase with increases in heating
rate. It is also shown in Table 1 that the values of
The TL glow curves of the undoped a-Al2O3 single geometrical factor(9) mg ¼ d/v remain unchanged in
crystals measured with a U-340 filter after irradi- the range of 1–20 C s1 heating rates (d ¼ T2  Tm,
ation of 0.12 Gy 90Sr beta rays in the range of o ¼ T2  T1, Tm, T1 and T2 being peak temperature,
1–20 C s1 heating rates shown in Figures 3 and 4 the temperature at the half intensity on the rising and
indicate that the glow curve measured with the falling sides of the peak, respectively).
U-340 filter (solid squares) at 5 C s1 heating The glow curves for different heating rates meas-
rate is well fitted by the first-order kinetic equation ured using the 7-59 filter instead of the U-340 filter in
(solid line) using PEAKFIT program. The kinetic the RisØ TL/OSL-DA-15B/C reader are shown in

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parameters and peak parameters of glow peaks Figure 5. It is seen that there are two glow peaks
at different heating rates are presented in Table 1. series: (1) the first series consists of peak temperat-
ures from 50 to 130 C called low temperature glow
peak series; (2) the second series consists of glow

Table 1. Parameters were obtained through fitting glow


curves by first-order TL kinetics equation.

Rates E (eV) s (s1) Peak Peak mg


( C s1) height area
(counts) (counts)

1 1.231 2.77  1012 7537.07 281,372 0.42


2 1.225 2.21  1012 5644.58 221,417 0.42
3 1.234 2.45  1012 5205.49 209,302 0.42
4 1.245 2.65  1012 4325.06 177,671 0.41
5 1.260 3.34  1012 3971.36 164,857 0.42
6 1.274 4.11  1012 3873.78 162,275 0.41
8 1.303 5.63  1012 3488.96 149,006 0.42
Figure 4. Glow curves measured with U-340 filter (solid 10 1.351 1.41  1012 3240.67 137,276 0.41
squares) at 5 C s1 heating rate. The solid line stands for 15 1.417 2.24  1012 2642.37 116,629 0.42
fitting curve of the first-order kinetic equation. 20 1.499 6.17  1012 2425.81 108,222 0.42

120000
1

100000
TL intesity (a. u.)

80000 2

3
60000
4
5
6
40000 8
10
15
20000 20

0
50 100 150 200 250 300 350
Temperature (oC)

Figure 5. Experimental glow curves of undoped a-Al2O3 crystal for the heating rates from 1 to 20 C s1 measured with
7-59 filter.

404
TL AND OSL OF UNDOPED a-Al2O3 CRYSTALS

peaks from 170 to 280 C called high temperature undoped a-Al2O3 crystal irradiated by 90Sr beta rays
glow peak series. The peak heights of the low tem- at 1.2 Gy dose level measured and fitted by an OSL
perature glow peak series increase with increase in model with two optical active traps(10), in which the
heating rate, whereas the peak heights of the high OSL intensity is expressed as follows:
temperature glow peak series reduce with increase in    
heating rate. It is indicated that the TL glow curves t t
IOSL ¼ I01 exp þ I02 exp , ð1Þ
are dependent upon the filter used in the readout t1 t2
equipment that is related to the emission spectra of
where I01 and I02 are the initial CW-OSL intensity
luminescence material. In addition, it is noticed that
at time t ¼ 0 for the first and second component,
the high temperature glow peak cannot be well fitted
respectively, whereas t1 and t2 are the decay
by one first-order kinetic glow peak but by two first-
constants. These parameters were obtained by fitting
order kinetic glow peaks shown in Figure 6. It is
experimental decay curves measured at various dose
presumed that the glow curves measured with a

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levels in the dose range of 0.12–248 Gy. The average
U-340 filter are mainly due to the TL emission at
decay constant t1 ¼ 2.64  0.07 s, which indicates
416 nm wavelength, whereas the glow curves meas-
that values of decay constant t1 are not related to the
ured with a 7-59 filter are from the emissions at
absorbed dose.
416 nm and the sharp line at 695 nm owing to the
transitions of Cr3þ ions.
Dose responses of TL and OSL
Dose dependence of TL characteristics
The TL and OSL dose responses of the undoped
The TL glow curves of the undoped a-Al2O3 samples a-Al2O3 crystal irradiated to 90Sr beta rays in the
irradiated with 90Sr beta rays at various dose levels dose range of 0.12–248 Gy were obtained and fitted
in the range of 0.12–248 Gy were measured with a by the composite action dose–response function
U-340 filter in the TL/OSL reader. The glow peak detailed in previous papers(11). The relative response
series were well fitted by the first-order kinetic F(D) is given by
equation. It can be seen that the activation energy      
and geometrical factor mg do not depend upon the D D D
F ðDÞ ¼ 1  exp  ð1  R Þ exp ,
absorbed dose shown in Figure 7, and the peak D0 D0 D0
temperature is almost unrelated to the absorbed ð2Þ
dose shown in Figure 8. In addition, the geometrical
factor average equals 0.415  0.001 for the dose where R is the proportion of one-hit events and is
range of 0.12–248 Gy, and it might be one of the called the one-hit factor that characterises the
criteria for first-order kinetic peak. nonlinear behaviour of the TL dose responses;
linear–sublinear behaviour for 1/2  R  1 and
linear–supralinear–sublinear behaviour for 0 < R < 1.
OSL characteristics
D0 is the characteristic dose. The TL dose responses
Figure 9 illustrates the decay curve of the CW-OSL of the undoped a-Al2O3 for the 210 C glow peak
signal with the stimulation of 470 nm lights for the were shown in Figure 10 and fitted by Equation 2

1.4 1.4
1
1.2 1.2
Activation Energy (eV)

1.0 1.0

0.8 0.8

0.6 0.6
2
0.4 0.4

0.2 0.2

0.0 0.0
10-1 100 101 102
Dose (Gy)

Figure 6. Glow curves measured with 7-59 filter (solid Figure 7. Dose dependence of activation energy (Curve 1)
squares) at 5 C s1 heating rate. The solid lines stand for and geometrical factor (Curve 2) for undoped a-Al2O3
fitting curves of the first-order kinetic equation. crystal measured with 5 C s1 heating rate.

405
C. X. ZHANG ET AL.
230 10 7

TL & OSL intensity (arb. units)


220
10 6
Peak temperature (oC)

OSL

210
10 5

200
10 4
TL
190

10 3

180

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10-1 100 101 102
Dose (Gy) 10 2

Figure 8. Relationship between peak temperatures and


absorbed doses for undoped a-Al2O3 crystal measured with 10 -1 10 0 10 1 10 2
5 C s1 heating rate. Dose (Gy)

Figure 10. Dose responses of the TL (closed circles) and


2 the OSL (open squares).

10 5 Table 2. Nonlinear characteristic parameters of TL and


8
OSL dose responses.
OSL intensity (arb.units)

7
6
Dose responses R D0 (Gy) Smax (a. u.)
5

4
1 TL 0.72 69.9 6.35  104
3 OSL 1.0 60.0 5.61  106

2
2

10 4
0 10 20 30 40 50 REFERENCES
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