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King Saud University

**Arabian Journal of Chemistry
**

www.ksu.edu.sa

www.sciencedirect.com

ORIGINAL ARTICLE

**New numerical model for thermal quenching
**

mechanism in quartz based on two-stage thermal

stimulation of thermoluminescence model

a,b,* a

Ahmed Kadari , Dahane Kadri

a

Department of Physics, Electronic Microscopy and Materials Sciences Laboratory, Sciences and Technology University of

Oran, Algeria

b

Department of Sciences of the Matter, Faculty of Science and Technology and Science of the Matter, Ibn Khaldoun University,

Tiaret, Algeria

**Received 19 May 2012; accepted 30 May 2013
**

Available online 10 June 2013

**KEYWORDS Abstract The effect of thermal quenching plays an important role in the thermoluminescence (TL)
**

Thermoluminescence; of quartz on which many applications of TL are based. The studies of the stability and kinetics of

Thermal quenching; the 325 C thermoluminescence peak in quartz are described by Wintle (1975), which show the

Quartz; occurrence of thermal quenching, the decrease in luminescence efﬁciency with rise in temperature.

Model; The thermal quenching of thermoluminescence in quartz was studied experimentally by several

Luminescence efﬁciency authors. The simulations work presented in the literature is based on the single-stage thermal stim-

ulation model of thermoluminescence, in spite of that the mechanisms of this effect remain incom-

plete. This paper presents a new numerical model for thermal quenching in quartz, using the

previously published two-stage thermal stimulation of thermoluminescence model.

ª 2013 Production and hosting by Elsevier B.V. on behalf of King Saud University.

**1. Introduction It causes a signiﬁcant decrease of the luminescence signal
**

and disturbs the shape of the glow-peaks. Among the TL mate-

The thermal quenching of luminescence efﬁciency is an effect rials which exhibit thermal quenching, the most widely known

which is present in many thermoluminescent (TL) materials. and investigated are Al2O3:C (Akselrod et al., 1990, 1998; Kitis

et al., 1994) and Quartz (Wintle, 1975; McKeever et al., 1997;

Kitis et al., 2003; Petrov and Bailiff, 1996, 1997; Chitambo,

* Corresponding author at: Department of Sciences of the Matter,

2003). Heating rate is one of the most important experimental

Faculty of Science and Technology and Science of the Matter, Ibn variables, which changes the glow curve shape (Ogundare

Khaldoun University, Tiaret, Algeria. Tel.: +213 7 75 95 56 27.

et al., 2005). In TL dosimetry, the absorbed dose and TL inten-

E-mail address: kadariahmed_14@yahoo.fr (A. Kadari).

sity are affected by changes in the heating rate (Betts et al.,

Peer review under responsibility of King Saud University.

1993; Taylor and Lilley, 1982).

Many investigations have been carried out by scientists in

order to understand that how the TL glow curve changes un-

Production and hosting by Elsevier der different heating rates (Taylor and Lilley, 1982; Nakajima,

1878-5352 ª 2013 Production and hosting by Elsevier B.V. on behalf of King Saud University.

http://dx.doi.org/10.1016/j.arabjc.2013.05.027

p N. spondingly in the excited state of the recombination center. ne(cm3) is the instantaneous occupancy of the excited of a TL glow peak shifts to higher temperatures. tron is in the excited state. the maximum pancy. The di- C = 2.64 eV indicating that the quenching rect radiative transition from the excited level into the ground properties are independent of the wavelength of the observed electronic state of recombination center is given by the prob- luminescence. An(cm3 s1) is the retrapping probability coefﬁcient of 1 þ C: expð kT Þ electrons from conduction band into the excited state. The decrease of cence mechanism (Chen et al. m Ground electronic state of recombination center nv Figure 1 Schematic diagram of the thermal quenching model for quartz. 1975). where C and W are ‘quenching parameters’. ing excitation and heating stages. Larsen. n1 N. At a higher state. Chen et al. with increasing heating rate. tive process into the ground state. Once the elec- that the whole area under TL peak decreases. coefﬁcients (s1). sents the activation energy for this process and ANR a mal quenching. The proposed model dn1 Fig. T is the sample Am(cm3 s1) is the recombination probability of electrons with temperature and k is the Boltzmann constant (Akselrod and holes in the recombination centers. The activation energy and the frequency factor for this temperature. g(T). In the model described below. In this study the thermal ability Am. ne An2 Excited electronic state of recombination center ANR W=0. it can either retrap with a probabil- The thermal quenching efﬁciency versus temperature. ity of p(s1) or be thermally excited into the conduction band. this recombination is assumed to produce the TL quenching parameter values of (Wintle. tigate a new numerical model which described a thermal M(cm3) and m(cm3) are. measured the thermal quenching parameters the excited state of recombination center (located below the of annealed natural quartz using radioluminescence as conduction band) is denoted by the probability An2.New numerical model for thermal quenching mechanism 799 1976. n2 Am Non radiative recombination TL M. nc(cm3) are the 1 instantaneous concentration of electrons in the conduction gðTÞ ¼ W . a decrease the competing thermally assisted process is given by a Boltz- in TL intensity was observed with an increase in the heating mann factor of the form ANR. The effect of thermal quenching may be observed while per. The aim of the present paper is to inves. N(cm3) is the concentration forming a series of TL measurements with different heating of the trapping state. The activation energy and the frequency factor for this transi- 1997): tion are E2(eV) and s2(s1). 1963). 2002). The various transitions shown and the parameters used in the model are described in the text. using the two-stage thermal stimulation of the thermoluminescence model. 1 are: 2. 1996.8 · 107 and W = 0. based on the previously suggested two. As a result of many studies. the luminescence is quenched more intensely so transition are E1(eV) and s1(s1). . Typically.exp(W/kBT) where W repre- rate. photons with an instantaneous intensity I. The probability for ered as reference values. constant representing the non-radiative transition probability creases (Spooner and Franklin. respectively. (2012). The model consists of luminescence efﬁciency with temperature increase due to the many trapping states and one kind of recombination center. ð1Þ band. The simultaneous differential equations governing the pro- cess during the heating stage.. traps and holes in the ground electronic state of recombina- stage thermal stimulation of thermoluminescence model by tion center. except at 495 nm. The electronic transition from the conduction band into (Wintle. respectively. shown in Fig. respectively the concentration of quenching in quartz. (2010). s1. 1978. whose efﬁciency increases as temperature in. N2(cm3) and n2(cm3) resolved optically stimulated luminescence has been studied by are the concentrations of electron traps and ﬁlled traps corre- Pagonis et al. 1998). n1(cm3) is their instantaneous occu- rates. 2002). 1975) will be consid. The dashed arrow denotes the non. Spooner and Franklin. 1 shows the energy level diagram of the proposed model ¼ s1 n1 expðE1 =kTÞ þ pne .64 eV E1. ð2Þ dt based on the two-stage thermal stimulation of thermolumines- nc An1 E2. is given by the following equation (Petrov and Bailiff.radia- The thermal quenching mechanism in quartz based on time. s2 N. This phenomenon has been explained to be due to ther. Jain. increased probability of non-radiative transitions is known as with the corresponding electronic transitions taking place dur- thermal quenching (Curie. 2012).

1975).64 eV. the numerical solution was performed 3 7 cm . The parameters used were E1 = 1. Am = 2. E2 = 0. ð9Þ sented model is that it reproduces the thermoluminescence where n0 is the total number of trapped electrons at time t = 0. 1975). The peak has a characteristic be found from Eq. . for appro- priately chosen sets of trapping parameters. K = 2. The phenomenon is called phosphorescence. The basic assumptions they made were that once an electron escapes from a trap there is no signiﬁcant TðtÞ ¼ T0 þ bt ð10Þ probability for it to get retrapped and that the luminescence with b the constant heating rate and T0 the temperature at time intensity at any temperature is directly proportional to rate t = 0. This gives for the intensity as function of temperature at which the detrapping occurs. W = 0. if n is the con- 1 dn centration of ﬁlled traps at any time t (temperature = T) then IðtÞ ¼ b dt the intensity of TL is given by: s dn E ¼ n0 IðtÞ ¼ ¼ sn exp : ð7Þ b dt kT Z E s T E exp : exp exp dT0 . p = s1 = 1011 s1. (11) is the well-known Randall–Wilkins ﬁrst-order constant. 2. It is a goal point that the physical model does ¼ n0 s not need to resort to the quasi-equilibrium approximation. An2 = 108 cm3 s1. Method of analysis becomes depleted).8 · 10 . Figure 2 Simulated results of a TL peak. But if the ferent heating rate values (from 5 to 20 K/s). N2 = 1. function of time according to: out any overlapping. Usually TL is observed as the temperature is raised as a linear matical representation for the luminescence glow peaks with. ð11Þ This differential equation describes the charge transport in kT b T0 kT0 the lattice as a ﬁrst-order process. N = 1.6 eV. Speciﬁcally when TL glow curves are measured using dif. ANR = 107 cm3 s1. A second important point of the pre.0 eV. The result As the temperature increases. At a constant tem- in the thermoluminescence (TL) signal due to thermal quench. If the temperature is kept Eq. (TL) glow peak at 598 K of quartz (Wintle. takes place which initiates luminescence).1 · 1010 cm3. the heating rate was b = 1 using the MATLAB ode15s program. An important re- sult of the model is that it reproduces the well-known decrease where I0 is the initial intensity at time t = 0.1 · 1010 In the present study. the intensity initially increases of simulating the TL glow curves using the set of trapping (detrapping of the trapped charge carriers and recombination parameters given in the caption is shown in Fig.800 A. enhancement of the non radiative recombination in the forbid. kTðtÞ 0 kTðt0Þ den band of this material.64 eV (Wintle. The Z t thermal quenching phenomena can be also explained by the E E exp : exp s exp dt0 . to solve numerically the relevant sets of Eqs. This program was used Ks1. (7) becomes: and the TL intensity reduces. ð4Þ dt 10 dnc dm dn1 dne dn2 8 ¼ : ð5Þ dt dt dt dt dt 6 The emitted light is taken to be proportional to the rate of 4 recombination so that: 2 dm I¼ ¼ Am n2 gðTÞ. s2 = 1012 s1. W = Temperature (K) 0. 1945a. Kadari. The intensity has thus the shape of a peak and (if derived from Eq. ð6Þ dt 0 where g is the luminescence efﬁciency. then reaches a max- imum and ﬁnally decreases (as the number of charges carriers 4.8 · 107 and W is an activation energy. 3. Results and discussions An1 = 1012 cm3 s1. which may be due to the well dn known phenomena of thermal quenching of TL due to increase IðtÞ ¼ dt in heating rates.38 · 104 s1. K is a dimensionless 400 450 500 550 600 650 700 750 constant 2. time. p = s exp(E/kT) is constant and the intensity can expression of a single glow peak. During heating. with increasing temperature varies in time p is no longer a constant and the heating rate the glow peaks shift toward higher temperature solution of the differential Eq. Kadri dne ¼ An1 ðN n1 ne Þnc þ s1 n1 expðE1 =kTÞ s2 ne 16 dt Tmax = 598K expðE2 =kTÞ pne .b) provided the simplest mathe. perature the decay is thus a simple exponential function of ing. (7)) is called a ﬁrst-order glow peak. (7) by integration: asymmetric shape being wider on the low temperature side IðtÞ ¼ I0 expðtpÞ. ð8Þ than on the high temperature side. (Randall and Wilkins. (2)–(6). D. ð3Þ 14 TL intensity (arb. units) 12 dn2 ¼ An2 nc ðN2 n2 Þ Am n2 n2 ANR expðW=kTÞ.

units) Tm Ex ¼ kTm 2:52 2 : ð12Þ 15 x The frequency factor is deﬁned by: 10 bE s¼ expðE=kTm Þ: ð13Þ kT2m 5 From the simulated result presented in Fig. 3. (1) is shown in Fig. glow peaks become wider and shift toward higher tempera- The schematic presentation of thermal quenching efﬁciency tures. Heating rate effect Thermal quenching causes a shift of the temperature of maxi- mum intensity Tm of a TL glow-peak toward lower tempera- tures (Akselrod et al. (which are almost temperature-independent) and non-radiative transitions – de-excitation of material by thermal agitation – which increases with temperature.6 20 η (T) 0. 2.8 0.41. 6. whereas at high the activation temperature. the TL efﬁciency conditions dictated by thermal quenching. The peak-shape method β=1K/s (Chen. using typical kinetic thermal activation energies.. ing rate increases and this reduction in TL sensitivity is well described using a Mott–Seitz theory (Akselrod et al. this energy is given by the following expression: β=20K/s TL intensity (arb. The luminescence efﬁciency Temperature (K) The luminescence efﬁciency is generally a temperature sensitive Figure 4 Effect of the heating rate b on the shape and the factor. 25 with a geometrical factor of l = 0. units) 350K 1.2 eV and s = 1. this will mean that the higher parameters for the 598 K TL peak of quartz (activation energy temperature peaks are observed under decreased luminescence and frequency factor). while their intensity decreases signiﬁcantly. Berkane- ture. As the heating rate increases. reaching a maximum at 350 K and reducing signiﬁcantly Krachi et al. The shift of the temperature maximum of due to thermal quenching.. The result of simulating the TL glow curves using dif- phosphor having one kind of luminescence centre and several ferent heating rates is shown in Fig. from this simulated result we can heating rates the peak temperature may be such that thermal see that the sensitivity increases with the activation tempera. quenching is strong (Nanjundaswamy et al. 1998). 1969) has been used for evaluating the activation en. Speciﬁcally when TL glow curves the thermoluminescence glow curves is represented in Fig. This position of the 598 K glow peak. Thus at low heating rates the TL peak may appear in a gives the dependence of the thermal quenching efﬁciency on range where thermal quenching is minimal. efﬁciency decreasing with increase of temperature. 4 as a function of heating rate. In the case of a TL creases. β=5K/s 20 β=10K/s ergy. given by Eq. glow-peak represented in Fig. 0 500 550 600 650 700 750 5. . we get Ex = 1.0 21 0. the curve in this ﬁgure.New numerical model for thermal quenching mechanism 801 The peak 598 K shown looks like a simple ﬁrst-order peak. (2002) studied the heating rate effect on TL re- at 550 K. So the Tm of the quenched Another important result of the model is that it reproduces the glow-peak is shifted to higher temperatures as a function of well-known decrease in the thermoluminescence (TL) signal the heating rate. the TL intensity is found to decrease as the heating rate in- 22 Maximum TL intensity (arb.. The TL intensity is plotted as a is so because of a competition between radiative transitions function of temperature.06 · 1010 s1. are measured using a variable heating rate from 1 to 20 K/s.2 550K 18 0. 2002). 5. 4. 2. Parameter values are the same as Fig. This behavior can be described by the thermal sponse and showed that the TL response decreases when heat- quenching effect.4 19 0. of Figure 3 The thermal quenching efﬁciency of quartz.0 0 5 10 15 20 300 350 400 450 500 550 600 650 700 Heating rate (K/s) Temperature (K) Figure 5 The behavior of the peak maximum intensity Im. 1998).

Radiat. M. Luff.. 184..J. Drupieski.. I.S. Our model can be applied to several Kitis. G.. 2002. Geophys. P.. in many thermoluminescent materials. Gorelova. J. Petrov. J. P.. Prot. Phys... 1997.K. 107.. McKeever. 2012). 1998. Agersnap Larsen. Randall. Pagonis. ing rate increases as expected in theory. Randall. M. J. S.. J. T. 2002. S. S. 184. F.S... N... 2002. C. J. J.. 1975. Greilich. Charalambous. 27.C. the present model.. M.. Prot. A. we can explain the thermal quenching effect 40.S. 3364. M.. 570–585. Two-stage thermal which may explain the thermal quenching effect for the 325 C stimulation of thermoluminescence. Chen. A Akselrod. 65. Papadopoulos. Status Solidi A 198. we propose a simple energy-band model Chen. D Appl. 2003. L. C... Radiat. 843. R. Lumin.A. Agersnap. B. 41. 1945b. 183.A. Lepper. 1996. L. Lawless. Vinceller. S.H.W. 1993. Meas. G.F. Proc. Tuyn. London. Dosim. Luminescence in Crystals. L. Townsend.. Kadari. London. Agersnap Larsen. In the present paper. Dosim. N..G. 26. 35. R.D.. I. V. J. An important result of the model is that it repro- McKeever... 1978.802 A. description of the thermal quenching kinetics in the case of TL 312. Wiley. 2003. Jain.. 1982. E.. Lumin. Radiat. J.. Kitis. Appl.A. 15 (6). Ankjærgaard. Phys. Pagonis. Phys.O.. 15.T. Radiat.. Appl.L.K. 1963.. Meas. Bindi.. A.S. A Akselrod. Dosim. D. 84. 1179. Phys. Berkane-Krachi... Soc. R.. Proc. 305. . Khayrat. 2053. Appl. 55. 2010. glow peak of thermoluminescence of quartz studied previously Chitambo. V.S... Murray. Meas. D. Kadri 7. V. Franklin. Bailiff. 1994. 366–389.A. Kortov. duces the thermoluminescence (TL) peak of quartz (325 C G. D... Bailiff. S. D Appl. K. Soc. V. Wintle.G. 1997. Meas. Wilkins.A. M. model (Chen et al. References Petrov. Iacconi. and the maximum TL intensity of peaks decreases as the heat. 1998. 161. Spooner. 1945a.W. V. 1–5. Phys. Duller. Radiat. Pagonis. Ser. 167. J.A.W. 390–407. 130. E. S. 1990. 37.A. S. Phys. M. J. Phys. New York. F. 3364–3373. V. Lilley. Astr. S.. R. 17. 2012. The investigation present here is based on Curie. R. Radiat. the peak temperatures of all peaks shift to high temperatures Nanjundaswamy. A. Phys. 1969.S. Radiat. Couturier. Another important result of this study showed that Nakajima. by Wintle (1975). Larsen. the two-stage thermal stimulation of thermoluminescence Jain. 40. 33. McKeever. R. Meas. 185. G. S. A. Akselrod. Balogun. 84... 902–909. N. J. 59.. Conclusion Betts. 1976. D Appl. Appl. Meas.. 949. 100. 2005. J. In the future and using Ogundare. J.... Whitley.S. Phys. Prot. McKeever.W.. Phys.. J.L. Chen. experiments. J. types of luminescence experiments and provides a satisfactory Radiat. Hussain.W.S. R. J.N.. Jpn. 159. Phys.H...... Soc.. 35. Appl. 60.T. M. Bøtter-Jensen...H.K.F. Taylor. peak). Lawless. N.S.. 6. 27. 1895. J. Phys. Ser..... R. Wilkins.. Radiat. 289. A..D.

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