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Radiation Protection Dosimetry Vol. 106, No. 1, pp.

33–43 (2003)
Published by Nuclear Technology Publishing
 2003 Crown coypright

THE RESPONSE OF LiF THERMOLUMINESCENCE


DOSEMETERS TO PHOTON BEAMS IN THE ENERGY RANGE
FROM 30 kV X RAYS TO 60Co GAMMA RAYS
S. D. Davis(1,2), C. K. Ross(1), P. N. Mobit(3), L. Van der Zwan(1), W. J. Chase(4) and K. R. Shortt(5)
(1)
Ionizing Radiation Standards, Institute for National Measurement Standards
National Research Council, Ottawa, ON K1A 0R6, Canada
(2)
Medical Physics Unit, McGill University Health Centre, Montreal General Hospital
1650 Cedar Ave, Montreal, QC H3G 1A4, Canada
(3)
Department of Oncology, University of Calgary and Department of Medical Physics
Tom Baker Cancer Centre, 1131-29 Street NW, Calgary, AB, T2N 4N2, Canada
(4)
Ontario Power Generation, 1549 Victoria Street East, Whitby, ON L1N 9E3, Canada
(5)
Dosimetry and Medical Radiation Physics Section, International Atomic Energy Agency

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P. O. Box 200, Wagramer Strasse 5, A-1400 Vienna, Austria

Received March 28 2003, amended May 27 2003, accepted June 6 2003

Abstract — The energy response of standard (TLD-100) and high-sensitivity (TLD-100H) LiF thermoluminescence dosemeters
(TLDs) has been studied for photon beams with mean energies from about 25 keV to 1100 keV. Canadian primary standards for
air kerma were used to establish the air kerma rates for each of the photon beams. TLDs were mounted in a PMMA holder and
the air kerma response was measured as a function of energy. The EGSnrc Monte Carlo code was used to model the TLD holder
and calculate the absorbed dose to the TLD chip per unit air kerma for each beam. The measured and calculated results were
combined to obtain the intrinsic dose response of the TLD chip. Broadly, our results are consistent with existing data, which
show a marked difference in the energy dependence of the two materials. However, the precision of our measurements (standard
uncertainty of about 0.6%) has permitted the identification of features that have not been noted before. In particular, the energy
dependence of the two materials is quite different in the important energy region delimited by 137Cs and 60Co gamma rays.

INTRODUCTION filters (5), either to provide build-up, or to provide spec-


tral information. Any attempt to use calculational tech-
Because of their small size, high sensitivity and ease
niques such as Monte Carlo codes to model the response
of use, thermoluminescence dosemeters (TLDs) are
of these composite structures requires knowledge of the
widely used for radiation dosimetry (1–3). The most com-
energy response of the TLD element.
monly used TLD material is based on crystalline LiF,
Bilski et al (6) suggest that the properties of LiF:
which has been doped with small quantities of Mg and
Mg,Cu,P produced by different manufacturers may not
Ti, and is denoted by LiF:Mg,Ti. More recently, a high
be the same. The energy response of the formulation of
sensitivity form of LiF has become available, and is
LiF:Mg,Cu,P denoted by MCP-N has been studied (6–8)
denoted by LiF:Mg,Cu,P, because the dopants are now
extensively by a group at the Institute of Nuclear Phys-
Mg, Cu and P.
ics (INP) in Kraków, Poland. MCP-N was developed at
The characteristics of both LiF:Mg,Ti and
INP so that the manufacturing process could be care-
LiF:Mg,Cu,P are summarised by McKeever et al (3) and
fully controlled. Olko et al (7) report measurements of
they provide extensive references to the original litera-
the energy response of MCP-N for photon energies from
ture describing these materials. The present work is con-
about 12 to 1200 keV, and provide a microdosimetric
cerned with the energy dependence of the response of
interpretation of the observed variation.
these materials to ionising radiation. Accurate knowl-
In addition to MCP-N, LiF:Mg,Cu,P is available as
edge of the energy response is important for fundamen-
GR-200 from Beijing Radiation Detector Works in
tal reasons, because any detailed model of thermolumi-
China and as TLD-100H from Thermo Electron RM&P
nescence must be able to explain the observed energy
(formerly Harshaw TLD) in the USA. Sáez-Vergara
dependence. The energy response is also of practical
et al (9) have studied the energy dependence of the vari-
importance (4) because TLDs are often used in radiation
ous formulations of LiF:Mg,Ti and LiF:Mg,Cu,P. Their
fields that have a broad spectrum of energies. In the
TLD chips were mounted in either PMMA or PVC hol-
areas of radiation protection and environmental moni-
ders, and the results of their measurements are summar-
toring, TLD chips are often mounted behind various
ised in Figures 1 and 2. These figures show that the
holder has a major effect on the air kerma response.
They also indicate that the response does not depend
Contact author E-mail: carl.ross@nrc.ca strongly on the details of the manufacturing process.

33
S. D. DAVIS, C. K. ROSS, P. N. MOBIT, L. VAN DER ZWAN, W. J. CHASE and K. R. SHORTT
In previous work Shortt et al (10) measured the air et al (11). The results of Sáez-Vergara et al (9) (Figures 1
kerma response of TLD-100 to 137Cs and 60Co gamma and 2) are also consistent with the results of Shortt et al
rays. They showed that the holder could have a signifi- for LiF:Mg,Ti. However, Sáez-Vergara et al point out
cant effect on the response, but also noted that the that the change in response of LiF:Mg,Cu,P from 137Cs
intrinsic response was about 2.5% greater for 137Cs than to 60Co is different from that of LiF:Mg,Ti.
for 60Co. Although the radiation absorption character- In this paper only the LiF formulations commercially
istics of LiF would not predict such a difference, it was available from Thermo Electron RM&P are considered.
consistent with a more extensive study of the energy They are denoted by TLD-100 and TLD-100H for
dependence of LiF:Mg,Ti carried out by Tochilin LiF:Mg,Ti and LiF:Mg,Cu,P, respectively. The results
of measurements on the energy dependence of the air
1.6 kerma response of TLD-100 and TLD-100H for photons
in the energy range from 25 keV to 1100 keV are
reported. Monte Carlo calculations have been used to
model the TLD holder and to determine the dose to the
1.4 TLD chip per unit air kerma. Thus, it was possible to
Relative air kerma response

LiF:Mg,Ti
extract the energy dependence of the dose response of

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the bare TLD chip. The observed structure is correlated
1.2 with the calculated electron spectrum and our results are
compared with earlier data, including the results
obtained with MCP-N.
1.0
MATERIALS AND METHODS
The TLD-100 and TLD-100H chips have slightly dif-
0.8 LiF:Mg,Cu,P
ferent formats. Both are 0.38 mm thick, but the TLD-
100 chips have a square cross section, 3.2 mm on a side,
10 100 1000 whereas the TLD-100H chips have a circular cross sec-
Mean photon energy (keV)
tion, 3.6 mm in diameter. TLD-100 has a density of
2.64 g cm⫺3 and the dopants Mg and Ti are present at
Figure 1. Graphical summary of the measured data tabulated concentrations of 200 and 10 ppm by weight, respect-
by Sáez-Vergara et al (9) for various formulations of LiF:Mg,Ti ively. The density of TLD-100H is 2.48 g cm⫺3 and the
and LiF:Mg,Cu,P. The data were obtained by a Spanish sec- dopant concentrations are 3000, 2000 and 40 ppm by
ondary calibration laboratory, INTE-UPC, and by the Spanish
weight for P, Mg and Cu, respectively*. Both TLD-100
national laboratory for ionising radiation, CIEMAT. In this
case the TLD chips were mounted in a PMMA holder. The
and TLD-100H contain the naturally occurring isotopic
standard uncertainty on each datum point ranges from 0.05% ratio of 6Li to 7Li. Our protocol for using TLD-100 is
to 2%, although it is generally about 1%. described in detail by Janovský and Ross (12). Briefly,
the chips are first annealed at 400ºC for 1 h, followed
by a second anneal at 100ºC for 2 h. Each time the chips
1.4
are removed from the oven, they are rapidly cooled on
a large brass block. After irradiation, but before readout,
the TLDs are annealed for 12 min at 100ºC, to clear the
1.2 LiF:Mg,Ti low energy traps. The TLD light output is read using a
Relative air kerma response

Victoreen 2800M reader. The response of the photomul-


tiplier used in the reader has its maximum in the blue–
1.0 green region of the spectrum, and a blue glass filter is
installed between the planchet and the entrance window
of the photomultiplier. The readout cycle consists of a
LiF:Mg,Cu,P preheat to 100ºC which takes about 2 s, followed by
0.8
heating at 5ºC s⫺1 to 240ºC. The temperature is held at
240ºC for 15 s, giving a total read time of 45 s. Nitrogen
gas, at a flow rate of 16 cm3 s⫺1 is used to remove oxy-
0.6 gen from the sample compartment. The planchet is

10 100 1000
Mean photon energy (keV)
* The composition and density data for TLD-100 and TLD-
Figure 2. Same as Figure 1 except that the TLD chips were 100H were kindly provided by K. J. Velbeck of Thermo Elec-
mounted in a PVC holder. tron RM&P.

34
ENERGY RESPONSE OF LiF TLDs
allowed to cool to 40ºC before the chip is removed from chips that are placed symmetrically about the central
the reader. axis. In addition to supporting the chips, the holder is
The TLD-100H chips are annealed for 15 min at also designed to provide charged particle equilibrium at
240ºC, followed by rapid cooling. After irradiation but the position of the TLD. For the 60Co and 137Cs
before readout, they are annealed for 12 min at 130ºC. irradiations, the thickness of the PMMA overlying the
For these short anneal times, there is some question as TLDs was 6.2 mm, while for the X ray irradiations the
to exactly how long the chips were at the specified tem- thickness was reduced to 1.6 mm.
perature. The approach to equilibrium was measured The 60Co and 137Cs irradiation facilities at the
after the ovens had been opened long enough to insert National Research Council (NRC) have been described
the TLD holders. It is estimated that, in both cases, the in some detail by Shortt et al (10). The 60Co air kerma
chips were at the specified temperature for about 10 has been established using a graphite cavity chamber as
min. The readout cycle is the same as that used for the a primary standard (13). The 137Cs air kerma was obtained
TLD-100 chips. using commercial ionisation chambers calibrated against
The calibration procedure is the same for both the the 60Co primary standard. The estimated change in the
TLD-100 and TLD-100H chips (12). The chips are response of the chambers between 60Co and 137Cs was
irradiated in groups of 25 using 60Co gamma rays in a obtained using Monte Carlo calculations (14). The stan-
dard uncertainty on either the 60Co or 137Cs air kerma

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field where the air kerma rate is accurately known. After
readout, the individual calibration factor, defined as the is approximately 0.5%.
ratio of the delivered air kerma to the TLD reading, is The 60Co irradiations to establish the individual chip
determined for each of the 25 chips. The TLDs are sensitivities and the 60Co reference irradiations were
annealed again, and divided into groups of five. One carried out using an irradiator manufactured by Atomic
group is irradiated in a 60Co reference field to determine Energy of Canada Ltd and identified as the Theratron
if there has been any overall change in sensitivity. If so, Junior. The irradiations were done at a point 3 m from
this change is applied to the readings of the remaining the source where the field had a square cross section,
four groups, which are irradiated in unknown fields. The 80 cm on a side and the air kerma rate was approxi-
work of Janovský and Ross (12) and of Shortt et al (10) mately 2.4 ⫻ 10⫺2 mGy s⫺1.
indicated that this procedure led to results where the The X ray air kerma is established with a standard
standard uncertainty on the mean of a set of five read- uncertainty of approximately 0.5% using free-air cham-
ings was typically about 0.5%. bers. One chamber is used to cover the energy range up
The holder used to irradiate the TLDs is shown in to 60 kV, while the second can be used up to 300 kV (15).
Figure 3. It is constructed from PMMA, and holds five Filter assemblies are available to generate the ISO series
of narrow spectrum beams (16). Table 1 lists the X ray
TLD cavity
beams that were used and gives their measured half-
value layer (HVL). The TLDs were irradiated at 1 m
from the X ray source, where the field has a circular
cross section, 15 cm in diameter.

Table 1. Characteristics of the X ray beams used for


measurements and calculations. Each beam is intended to
satisfy the requirements of the ISO narrow spectrum
series (16). The second column is the measured HVL of the
NRC beam, while the third column is the HVL reported
for the GSF beams (22). The final column is the mean photon
energy calculated using the GSF spectra.

Identifier HVL Mean energy


(keV)
NRC beams GSF beams
5 cm
N-30 1.20 Al 1.12 Al 24.2
Figure 3. Basic design of the PMMA holder used for the N-40 0.083 Cu 0.081 Cu 32.5
irradiations. The holder is 32 mm in diameter and has five cyl- N-60 0.23 Cu 0.23 Cu 47.3
indrical cavities, each large enough to accommodate one TLD N-80 0.58 Cu 0.57 Cu 64.5
chip. The TLD cavities are placed symmetrically with respect N-100 1.10 Cu 1.09 Cu 82.6
to the flat faces of the holder, but different wall thicknesses N-150 2.37 Cu 2.29 Cu 117
were used, depending on the beam energy. For the X ray N-200 4.00 Cu 3.91 Cu 164
irradiations, the wall thickness was 1.6 mm, while for the 137Cs N-250 5.19 Cu 5.11 Cu 207
and 60Co irradiations the thickness was 6.2 mm.

35
S. D. DAVIS, C. K. ROSS, P. N. MOBIT, L. VAN DER ZWAN, W. J. CHASE and K. R. SHORTT
The Monte Carlo calculations were carried out using Seelentag et al (22) from the Gesellschaft für Strahlen-
the EGSnrc code (17). The user code DOSRZnrc was und Umweltforschung (GSF) have reported extensive
used to calculate the absorbed dose to the TLD chip per measurements of X ray spectra. Tabulated data from
unit fluence, while the electron spectrum in the chip was Seelentag et al for the photon spectra of the ISO series
obtained using FLURZnrc. These codes require the of narrow-spectrum X ray beams have been used here
geometry to have cylindrical symmetry so a simplifi- as source inputs for the simulations. Table 1 gives the
cation of the actual holder geometry was necessary. HVL and mean photon energy for the GSF beams. The
137
Most of the simulations were carried out using a single Cs and 60Co spectra were taken from the EGSnrc
chip located at the centre of a cylindrical PMMA phan- distribution (23).
tom. However, some tests were also done with a ring Most of the calculations were carried out on a
of TLD material at the same position as the individual 733 MHz computer. The air kerma calculations required
chips in the actual holder. about 30 min to achieve an uncertainty of 0.01% using
The material data sets for EGSnrc are prepared by a 1 ⫻ 108 histories. The calculation of the dose to the chip
pre-processor called PEGS4. The default photon cross required from 5 ⫻ 108 to 2.2 ⫻ 109 histories, depending
sections available to PEGS4 are those of Storm and on the photon energy and phantom thickness, to achieve
Israel (18). Revised photoelectric cross sections have been an uncertainty of less than 0.1%. The computing time
compiled by Berger et al (19), and they provide a pro-

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ranged from 3 to 70 h. The FLURZnrc calculations used
gram called XCOM to extract the cross section data. 1 ⫻ 107 histories and required from 0.5 to 7 h of com-
The XCOM cross sections differ by up to 5% from those puting time.
of Storm and Israel for photoelectric interactions below
200 keV. Hobeila and Seuntjens (20) have implemented
RESULTS
the XCOM photoelectric cross sections in EGSnrc and
they provided us with the data file to be used with The air kerma response is defined here as the ratio of
PEGS4. We have carried out calculations with both data the measured TLD reading to the value of the air kerma
sets to determine the sensitivity of our results to the for the field in which the chip was irradiated. Similarly,
photoelectric cross sections. The PEGS4 data sets were the dose response is defined as the ratio of the measured
generated for photon and electron kinetic energies in the TLD reading to the absorbed dose delivered to the chip.
range from 1 to 2000 keV. The absorbed dose to the chip is denoted by DTLD and
The simulations using DOSRZnrc report the absorbed is approximately equivalent to the absorbed dose to pure
dose per unit fluence at the front face of the holder, so LiF, although the Monte Carlo model includes the
a separate set of simulations was needed to relate the dopants.
fluence to the air kerma. The air kerma per unit fluence Figure 4 shows typical glow curves for TLD-100 and
was calculated using the technique described by Borg TLD-100H. The TLD-100 chip was irradiated in an air
et al (21). The absorbed dose to a 2 ␮m thick air slab with
a 10 cm radius was calculated using DOSRZnrc for each
of the incident photon beams. The cut-off energy for 700
electron transport was set very high (2000 keV) so that
electrons deposited their energy locally. With no elec- 600
TLD-100H
tron transport, the absorbed dose is equivalent to the
kerma. This approach to determining the air kerma has 500
Reader output (nA)

the advantage that a consistent set of photon cross sec-


tions are used for both the kerma and dose calculations. 400
For the air kerma calculations, the photon cut-off was
300
set to 1 keV. For the calculations of the absorbed dose
to the TLD chip, the photon and electron energy cut- 200 TLD-100
offs were 1 keV and 10 keV, respectively. This meant TLD-100H
that, for any interaction that resulted in a photon below 100
1 keV or an electron with kinetic energy below 10 keV,
its energy was deposited locally. All of the improved 0
electron transport options in EGSnrc were turned on for
10 100 200 300 400 500
the simulations, as well as all the low energy photon
and electron options. The same transport options were Time (ds)
used with FLURZnrc to calculate the electron spectrum
Figure 4. Typical glow curves obtained for TLD-100 and TLD-
except that the electron cut-off was lowered from 100H. The air kerma values were 20 mGy and 1.5 mGy for
10 keV to 1 keV. The energy width of the scoring bins TLD-100 and TLD-100H, respectively. The TLD-100 glow
for the electron spectra was modified depending on the curve has been scaled using a factor of 2.57 to have the same
incident photon energy, and the number of bins varied area as the TLD-100H curve. The TLD-100H material is
from 30 to 80. approximately 34 times more sensitive than TLD-100.

36
ENERGY RESPONSE OF LiF TLDs
kerma field approximately 13 times greater than that would give the same reader output for both the test
used for the TLD-100H chip. In addition, the TLD-100 beam and the 60Co reference beam were compared. To
glow curve was multiplied by a factor of about 2.6 so do so, each data set for the test beam was fitted to a
that the areas under the curves in Figure 4 are the same. straight line, as illustrated in Figure 5. The result is an
Thus, for our TLD protocol, we find that TLD-100H is equation of the form
approximately 34 times more sensitive than TLD-100.
R = (sKa + i)Ka, (1)
The TLD reading for each chip was obtained by inte-
grating between channels 42 and 430, where one chan- where R is the reader output, Ka is the air kerma and s
nel corresponds to 0.1 s. and i are the slope and intercept, respectively. Equation
The background signal was obtained by comparing 1 was used to find the value of Ka for the test beam that
the reading of the empty planchet with that of a chip would give the same reader output, R, obtained using
that had recently been annealed. It was found that the the 60Co reference beam. The relative air kerma
background with a chip present was typically about 10% response was then obtained as the ratio of the air kerma
greater than the empty planchet reading. Thus, a back- delivered by the Co irradiation to that for the test beam.
ground reading of 1.1 times the empty planchet value The maximum effect of ignoring the non-linearity is
was subtracted from each TLD reading and amounted about 0.6% and occurs for the N-150 beam.

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to a correction of from 0.1% to 2.3%, depending on the The measured air kerma response is tabulated for
dose level and TLD type. each beam quality in Table 2 and shown graphically as
Figure 5 shows typical results obtained using a set of a function of beam energy in Figure 6. The response
25 TLDs. One group of five chips was irradiated in a for each energy has been normalised to the measured
60
Co reference beam to establish the overall set sensi- response for 60Co gamma rays. In order to determine
tivity. The remaining chips were divided into groups of the TLD dose response as a function of energy it is
five, and irradiated in a test beam at a point in space necessary to relate the air kerma to the absorbed dose
where the air kerma was known. Each group was delivered to the chip. We first consider a simple model
irradiated for a different time so that a range of air in which a LiF chip is embedded in a uniform phantom
kerma values was covered. Figure 5 suggests that the of LiF, thick enough to provide charged particle equilib-
response versus air kerma is slightly non-linear, and we rium at the position of the chip. The incident photon
have observed a similar trend with all the other data beam is taken to be parallel and monoenergetic and we
sets. We suspect that this non-linearity is an artifact of assume that photon attenuation and scatter can be neg-
the reader, but have not demonstrated it conclusively. lected. Then the absorbed dose to the TLD, DTLD, is
In order that the non-linearity, regardless of its ori- given by

冉 冊
gins, does not bias our results the air kerma values that
␮en
DTLD = ⌿ , (2)
1.02 ␳ LiF

where ⌿ is the photon energy fluence and (␮en/␳)LiF is


1.00
Relative air kerma response

Table 2. Measured air kerma response for TLD-100 and


TLD-100H for several beam qualities. The response is
0.98 reported relative to the measured response to 60Co gamma
rays. The Type A standard uncertainty in the last digit is
given in parentheses.
0.96
Identifier Relative air kerma response

TLD-100 TLD-100H
0.94

N-30 1.445(7) 0.930(7)


0.5 1.0 1.5 2.0
N-40 1.464(8) 1.004(6)
Air kerma (mGy)
N-60 1.387(6) 0.971(6)
Figure 5. Typical results obtained using a set of 25 high-sensi- N-80 1.272(6) 0.846(5)
tivity TLDs. Five chips (crosses) out of the set of 25 were N-100 1.211(7) 0.778(4)
irradiated with 60Co ␥-rays to establish the overall sensitivity N-150 1.163(6) 0.775(5)
of the set. The remaining four groups (circles) were irradiated N-200 – 0.825(6)
using N-60 X rays. The irradiation time for each group was N-250 1.110(6) –
137
adjusted so that the air kerma varied from about 0.5 to 2 mGy. Cs 1.023(5) 0.972(6)
60
The results are normalised to the mean 60Co response. The Co 1.000 1.000
dashed line is a linear fit to the N-60 data.

37
S. D. DAVIS, C. K. ROSS, P. N. MOBIT, L. VAN DER ZWAN, W. J. CHASE and K. R. SHORTT
the mass energy absorption coefficient for LiF. For the Because g is never bigger than 0.003 in this energy
same energy fluence, ⌿, the air kerma, Ka, is given by range, it was ignored in the calculations.

冉 冊
Detailed Monte Carlo simulations to estimate the
␮en 1
Ka = ⌿ , (3) absorbed dose per unit air kerma have also been carried
␳ air (1 ⫺ g) out. Because the Monte Carlo user code requires cylin-
where (␮en/␳)air is the mass energy absorption coef- drical symmetry, the holder geometry was approximated
ficient for air and g is the fraction of the incident energy as a single TLD at the centre of a cylindrical PMMA
that is lost to radiative processes. Data for the mass phantom. In order to test the sensitivity of the model to
energy absorption coefficients were obtained from Hub- the phantom radius, DTLD/Ka as a function of the radius
bell and Seltzer (24), and DTLD/Ka is plotted in Figure 7. was calculated and the results are shown in Figure 8.
Because of scattered photons, the response increases as
the holder radius increases. The effect becomes larger
TLD-100 as the photon energy decreases, reaching a maximum at
1.4 TLD-100H about 60 kV. These results provide no clear-cut choice
Relative air kerma response

for a holder radius to approximate the true geometry.


However, the radius cannot be greater than 16 mm,

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1.2
which is the radius of the holder used for the measure-
ments, and it should not be less than 8 mm, which is
the minimum distance from a TLD chip to the edge of
the holder. The maximum change in response for radii
1.0 from 8 to 16 mm is about 1.7%.
As a second approximation, a holder with the same
radius as the actual holder (16 mm) but with a ring of
0.8 TLD material at 9 mm from the centre was considered.
This model maintains the cylindrical symmetry required
10 100 1000
by the EGSnrc user codes and the holder radius is cor-
Mean photon energy (keV)
rect. However, the individual TLDs are distorted into a
uniform ring of TLD material. For all the photon beams,
Figure 6. Measured air kerma response of TLD-100 and TLD- the results from the ring model corresponded well with
100H as a function of photon energy. Each datum point is those for the chip-centred model with a holder radius of
based on at least one set of measurements similar to that shown 13 mm (Figure 8). All subsequent calculations are based
in Figure 5. The Type A standard uncertainty on each point is on the chip-centred model with a radius of 13 mm.
typically 0.6%.
1.30 1.025

Ring geometry
1.25 Simple model 1.020
MC, TLD-100
1.20 MC, TLD-100H
Relative response

1.015
1.15
DTLD /Ka

1.10 1.010

1.05
1.005
1.00 60
Co
0.95 1.000 N-150
N-60
0.90
0.995
10 100 1000 6 8 10 12 14 16 18 20
Energy (keV) Holder radius (mm)

Figure 7. Calculated air kerma response as a function of photon Figure 8. Effect of the holder radius on the calculated value of
energy. The pluses were obtained by considering a LiF TLD DTLD/Ka, for a single TLD chip mounted at the centre of the
to be embedded in a uniform phantom of LiF. The effects of holder. The results are given relative to the value for a phantom
photon attenuation and scattering within the phantom were neg- with a radius of 8 mm. The results obtained for a ring approxi-
lected. The results of the EGSnrc Monte Carlo calculations are mation to the distribution of TLD material are also shown. The
shown by the circles and crosses for TLD-100 and TLD-100H, ring results are plotted to show that a single chip at the centre
respectively. The statistical uncertainty on each point calcu- of a holder with a radius of 13 mm gives similar results for all
lated using the Monte Carlo technique is about 0.1%. beam qualities.

38
ENERGY RESPONSE OF LiF TLDs
The calculations of DTLD/Ka were repeated for both the chip will not affect the measured energy depen-
sets of photoelectric cross sections. Although differ- dence. However, the dose due to low energy X rays will
ences of up to 3% were observed in the values of DTLD show more variation over the thickness of the chip than
60
and Ka per unit incident fluence, the maximum effect Co gamma rays. In order to estimate the effect of light
on the ratio, DTLD/Ka, was 0.6%. As expected, the ratio absorption on our measured response we used the mass
is rather insensitive to the details of the photoelectric energy absorption coefficients for LiF to estimate the
cross section. The Monte Carlo calculations also depend dose distribution within the chip for N-30 X rays and
60
on knowledge of the X ray spectra. Because spectral Co gamma rays. By combining the light attenuation
measurements for the NRC beams were not available and dose distribution data, it is estimated that the correc-
the spectra measured at the GSF (22) were used. Spectral tion to be applied to the N-30 response relative to that
differences will be most important for the low energy for 60Co is only about 0.2% and will be even smaller
beams because the photon cross sections are a strong for higher energy X ray beams. Because of the small
function of energy below about 80 keV. In order to test size of the correction, and in the absence of data specific
the sensitivity of DTLD/Ka to the X ray spectrum, the N- to TLD-100 and TLD-100H, our results have not been
30 result was re-calculated using the spectrum measured corrected for light attenuation within the chip. Olko
at the Physikalish-Technische Bundesanstalt (PTB) (25). et al (27) have carried out a similar calculation for MCP-

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The GSF and PTB spectra give values of 1.12 and 1.16 N and show the results graphically for a wide range of
for the HVL (mm of Al), respectively. The difference photon energies.
in DTLD/Ka for the two spectra is 0.4%, suggesting that The EGSnrc results for DTLD/Ka are tabulated in
our results are not unduly sensitive to knowledge of the Table 3 and shown graphically in Figure 7. By combin-
X ray spectra. ing the measured air kerma response from Figure 6 with
The measured TLD signal arises from light that the Monte Carlo results for DTLD/Ka from Figure 7, the
escapes from within the chip. Because the TLD material TLD dose response as a function of energy can be
is not perfectly transparent, the portion of the TLD clos- obtained. The results are tabulated in Table 3 and shown
est to the photomultiplier will contribute more to the graphically in Figure 9 for both TLD-100 and TLD-
signal than portions at greater depth. Ipe et al (26) have 100H. These data represent the TLD reading per unit
measured the light attenuation in the Polish formulations absorbed dose to the chip, normalised to the value for
60
of LiF:Mg,Ti and LiF:Mg,Cu,P which are denoted by Co gamma rays.
MTS-N and MCP-N, respectively. They find that the
light attenuation is similar in the two materials and we
DISCUSSION
assume that the same would apply for TLD-100 and
TLD-100H. As long as the dose distribution within the Both TLD-100 and TLD-100H are thermoluminesc-
chip does not depend on energy, light absorption within ent materials based on LiF. However, Figure 9 shows

Table 3. The results calculated using EGSnrc for the dose


to the chip per unit air kerma are given in columns 2 and 1.1
3 for TLD-100 and TLD-100H, respectively. The values of
DTLD/Ka have a statistical uncertainty of about 0.1%. The
measured values of the air kerma response from Table 2 1.0
Relative dose response

were combined with the calculated values of DTLD/Ka to


obtain the dose response of the TLD chip and the results
are given in columns 4 and 5. The Type A standard uncer- 0.9
tainty in the last digit is given in parentheses.

Identifier DTLD/Ka Relative dose response 0.8

TLD-100 TLD-100H TLD-100 TLD-100H


0.7 TLD-100
TLD-100H
N-30 1.208 1.242 1.100(5) 0.689(5)
N-40 1.253 1.285 1.075(6) 0.718(5) 0.6
N-60 1.211 1.238 1.053(5) 0.722(5) 10 100 1000
N-80 1.117 1.133 1.047(5) 0.687(4)
Mean photon energy (keV)
N-100 1.042 1.051 1.069(6) 0.681(4)
N-150 0.983 0.986 1.089(6) 0.723(5) Figure 9. Results from the present work for the dose response
N-200 0.958 0.959 – 0.790(6) as a function of energy for TLD-100 and TLD-100H. Each
N-250 0.951 0.952 1.073(6) – datum point was obtained by dividing the measured air kerma
137
Cs 0.924 0.924 1.018(6) 0.968(6) response from Figure 6 with the value of DTLD/Ka calculated
60
Co 0.920 0.919 1.000 1.000 using the EGSnrc Monte Carlo code. The Type A standard
uncertainty on each point is typically 0.6%.

39
S. D. DAVIS, C. K. ROSS, P. N. MOBIT, L. VAN DER ZWAN, W. J. CHASE and K. R. SHORTT
that the dose response as a function of energy of the Figure 10. There is fair agreement between our results
two materials is very different. The dose response of for TLD-100H and those for MCP-N, indicating that
TLD-100H decreases dramatically as the photon energy these two formulations of high sensitivity LiF have
decreases while that of TLD-100 shows a slight increase similar characteristics.
in the same energy region. Both response curves exhibit Olko et al (7) have developed a microdosimetric model
additional structure as the photon energy decreases to help explain the dose response curve of LiF:Mg,Cu,P.
below about 100 keV. In earlier work (10) we had shown They point out that the structure below 100 keV arises
that the dose response of TLD-100 was greater for 137Cs from the change in the electron spectrum because the
than for 60Co. The opposite effect for TLD-100H is photoelectric effect becomes more dominant as the pho-
found, that is, the dose response is less for 137Cs than ton energy decreases. In order to demonstrate this point,
for 60Co. Sáez-Vergara et al (9) already noted that the EGSnrc was used to calculate the mean electron energy
change in response between 137Cs and 60Co was differ- for all electrons set in motion with energy greater than
ent for LiF:Mg,Ti and LiF:Mg,Cu,P. However, their 1 keV. The mean electron energy as a function of the
data does not clearly show the 3.3 (⫾0.5)% change that photon energy is shown in Figure 11. Starting from
60
we measure for TLD-100H. Co, the mean electron energy decreases as the photon
Several measurements of the energy response of energy decreases. However, near 100 keV, the mean

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LiF:Mg,Ti have been reported in the literature. Budd energy no longer continues to decrease, and it increases
et al (28) reported measurements in the energy range from slightly until about 60 keV. Below 60 keV the mean
30 to 148 keV and compared their results to earlier electron energy again begins to decrease as the photon
work. Although there is considerable scatter within the energy decreases. This suggests that the structure in the
data, the general trend is consistent. That is, the meas- dose response curves for both TLD-100 and TLD-100H
ured response to low energy X rays relative to 60Co is roughly correlated with the change in the mean elec-
gamma rays is greater than expected based on the tron energy with photon energy.
energy deposited in the material. One of the most exten- Olko et al (7) have calculated the mean lineal energy,
sive sets of measurements were carried out by Tochilin yF, for a target diameter of 40 nm for each of the photon
et al (11) and the smooth curve they drew through their beams. They show, in Figure 4 of their paper, that the
data is reproduced in Figure 10. The typical uncertainty measured dose response of LiF:Mg,Cu,P is well corre-
on each of their datum points was about 5% so they lated with yF. EGSnrc does not permit the calculation
were not able to detect the structure we observe between of microdosimetric quantities, but it can be used to cal-
20 and 100 keV. culate the restricted electron stopping power, (L/␳)TLD,
Olko et al (7) have measured the dose response as a which is also an indicator of local energy deposition.
function of energy for the formulation of LiF:Mg,Cu,P The electron stopping power for each of the photon
identified as MCP-N and their results are shown in

1.2
Olko et al.(29) (prediction) 15

Stopping power (MeV cm2 g–1)


Mean electron energy (keV)

1.1
Relative dose response

NRC
1.0 100 10
Tochilin et al.(11)
0.9
Olko et al.(7)

5
0.8
NRC
0.7
10 0
10 100 1000
0.6
10 100 1000 Mean photon energy (keV)
Mean photon energy (keV)
Figure 11. Results obtained using EGSnrc for the mean elec-
Figure 10. Comparison of the dose response as a function of tron energy (diamonds) and the mean restricted collisional stop-
energy for TLD-100 and TLD-100H with the results obtained ping power (circles) as a function of the mean photon energy.
by Tochilin et al (11) for LiF:Mg,Ti and the results of Olko The energy cut-off used for calculating the restricted stopping
et al (7) for the formulation of LiF:Mg,Cu,P identified as MCP- power was 1 keV. The results are the mean values for TLD-
N. The dotted curve near the top of the figure is a model predic- 100 and TLD-100H, although the differences between the two
tion developed by Olko et al (29) for LiF:Mg,Ti. materials are generally less than 1%.

40
ENERGY RESPONSE OF LiF TLDs
beams has been calculated, using an electron energy cut- CONCLUSIONS
off of 1 keV. Because the values for TLD-100 and TLD-
A high precision comparison of the dose response
100H do not differ by more than 1%, the two have been
versus energy of TLD-100 and TLD-100H has been
averaged. The results are tabulated in Table 4 and
carried out. Both these LiF-based dosemeters are widely
shown graphically in Figure 11. It can be seen that the
used and are available from the same supplier. By carry-
restricted stopping power shows a structure below
ing out Monte Carlo calculations of the absorbed dose
100 keV that is reminiscent of the structure of the dose
to the chip per unit incident fluence, it was possible to
response curves. In order to test the correlation between
eliminate the effects of the holder on the measured
the dose response and the restricted stopping power, the
response. Our results are in general agreement with
dose response versus the stopping power has been plot-
other work, indicating that the specific formulation of
ted in Figure 12. Although the stopping power is a
the TLD material does not play a major role in affecting
rough predictor of the dose response, it does not perform
its energy response.
as well as yF.
The dose response of TLD-100H shows a large vari-
In a later paper, Olko et al (29) studied the energy
ation with energy and must be accounted for if the TLDs
response of LiF:Mg,Ti. The formulation they used is
are to be calibrated at one beam quality but used at
identified as MTS-N and was produced at their institute
another. Even between 60Co and 137Cs we see a change

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(INP). Their experimental results show considerable
of 3.3%. This is similar in size, but in the opposite direc-
scatter but are consistent with our data. They also
tion, to the effect reported earlier by Shortt et al (10) for
developed a microdosimetric model to help explain their
TLD-100. For TLD-100, the change in response with
results. Their model depends on a target diameter which
energy is considerably smaller than for TLD-100H.
they take as a free parameter and varies from 8 to
In addition to their importance for radiation protec-
40 nm. Their model results for a target diameter of
tion dosimetry both TLD-100 and TLD-100H dosemet-
40 nm have been reproduced in Figure 10. Their model
ers are used for brachytherapy dosimetry. For this appli-
shows a structure similar to that measured here,
cation, high precision is required but there remains some
although the fit is not perfect. Furthermore, the model
uncertainty regarding the energy dependence of the
indicates that the response continues to increase as the
dosemeters (30–32). The mean photon energies of the most
photon energy decreases. This prediction is consistent
commonly used brachytherapy seeds (33) range from
with our measurements but in disagreement with the
22 keV to 380 keV. Our measurements show that the
work of Tochilin et al. However, for target diameters
variation of the dose response with energy will lead to
smaller than 20 nm, the calculated response tends to
corrections of up to 10% for TLD-100 and up to 47%
decrease below about 25 keV. Additional measurements
for TLD-100H in this energy range, assuming the dose-
below N-30 are needed to determine how the response
meters have been calibrated using 60Co gamma rays.
changes in this low energy region.

ACKNOWLEDGEMENTS
Table 4. Quantities calculated using the EGSnrc Monte One of the authors (S. D. Davis) is grateful for the fin-
Carlo code. The meaning of each symbol is as follows: E␥, ancial support provided by Ontario Power Generation.
mean photon energy of the incident beam; Ee, mean elec-
tron energy; (L/␳)TLD, mean restricted collisional stopping
power. Ee includes all electrons with an energy greater than 1.1
the cut-off of 1 keV and is the mean of the values for TLD-
100 and TLD-100H. The stopping power was calculated
with a cut-off of 1 keV and is the mean of the values for 1.0
Relative dose response

TLD-100 and TLD-100H.

0.9
Identifier E␥ (keV) Ee (keV) (L/␳)TLD
(MeV cm2 g⫺1)
0.8
N-30 24.2 14.4 16.3
N-40 32.5 19.3 13.4
N-60 47.3 26.9 11.7 0.7 TLD-100
N-80 64.5 33.0 12.1 TLD-100H
N-100 82.6 33.7 13.3
N-150 117 31.1 12.5 0.6
N-200 164 36.2 9.23 0 5 10 15
N-250 207 47.9 7.09 2 –1
137 Stopping power (MeV cm g )
Cs 613 206 2.55
60
Co 1055 421 1.78 Figure 12. The dose response of TLD-100 and TLD-100H as
a function of the mean restricted collisional stopping power.

41
S. D. DAVIS, C. K. ROSS, P. N. MOBIT, L. VAN DER ZWAN, W. J. CHASE and K. R. SHORTT
Another (P. N. Mobit) would like to acknowledge the sup- chington in constructing TLD holders. Stewart Walker,
port provided by the Alberta Heritage Foundation for Feridoun Faravash and Hong Shen helped with electronic
Medical Research. The support of the technical staff of the issues, computer systems and X ray irradiations, respect-
Ionizing Radiation Standards Group was critical in leading ively. They are grateful to Dr Jan Seuntjens and Fadi Hob-
to the timely completion of this work. The authors would eila of McGill University for providing them with revised
like to acknowledge, in particular, the work of David Mar- cross section data for low energy X rays.

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