Nuclear Instruments and Methods 174 (1980) 593-597

North-Holland Publishing Company

A NEW TECHNIQUE FOR CALIBRATING A NaI(TI) SCINTILLOMETER USED TO MEASURE GAMMA

DOSE-RATES IN ARCHAEOLOGICAL SITES

Y. LIRITZIS and R.B. GALLOWAY

Physics Department, University of Edinburgh, Scotland

Received 12 November 1979 and in revised form 21 April 1980

A new calibration technique is described for relating the counting rate recorded by a portable 2" 2" NaI(T1) scintlllometer
to the dose-rate absorbed by quartz grains. The quartz grams were used as a thermoluminescence dosimeter employing the 110C
peak. To avoid fading the thermolumlnescence was built up while the quartz grains were maintained at liquid nitrogen tempera-
ture. Four different spectral media were used for the calibration, namely potassium doped sand, uranium doped sand, thormm
doped sand and uranium doped peat. In each case the dose-rates were also determined with LiF and CaSO4 " Dy phosphors. The
responses of the &fferent phosphors are compared and the dependence of thetr sensitivity on gamma-ray energy is discussed The
emphasis is on the significance of the calibration procedure for a scintillometer employed on archaeological sites for dose-rate
determination in connection with thermoluminescence dating.

1. Introduction doped concrete blocks and CaF 2 and CaSO4 : D y

In the determination o f the age of p o t t e r y by ther-
moluminescence it is necessary to know the radiation
dose-rate that the p o t t e r y fragment has recewed
during its centuries of burial. A substantial contribu-
tion to this dosage is due to gamma-rays from radio
elements in the surrounding soil and in the "inclu-
sion-dating" technique [1] this soil dose is typically
30% and can approach 50% of the effective total.
Although there are some well established techniques
for estimation of the dose-rate from this gamma-
radiation from the soil, the present newly employed
technique is to determine the gamma-dose experi-
enced by quartz grains rather than by other dostmet-
r~c phosphors. Otherwise it is necessary to match the
effective atomic number of any dosimeter system as
closely as possible to the atomic number of the irra-
diated material of interest if the dose absorbed in the
dosimeter is to be related meaningfully to the dose
absorbed in the material. Consequently, the ideal
dosimeter would be quartz which is commonly used
to provide the total archaeological thermolumines-
cent absorbed dose in dating.
Murray and Aitken [2] and Huxtable et al. [3]
have reported on the use of a NaI(T1) gamma-ray
scintillometer in the context of archaeological ther-
moluminescence dating with dose-rate calibration
based on the use o f uranium, thorium and potassium
thermoluminescent dosimeters. The more general use
of NaI(T1) detectors in the study of terrestrial
gamma-rays has been discussed b y Adams and
Lowder [4] and by Lovborg and Kirkegaard [5].
A technique commonly employed to measure the
environmental gamma-ray dose-rate at an archaeologi-
cal excavation site is to bury phosphors for a period
and then deduce the dose-rate from the induced ther-
moluminescence. Natural calcium fluoride has been
used in this way by Aitken [6,7]; CaSO4 : Dy by
Yamashita et al. [8], Mejdahl [9,10]; CaF~, CaSO4 :
Dy, obsidian and A1203 by Murray and Aitken [2].
The main difficulty so far as thermotuminescence
dating is concerned is that in general the phosphors
have a different response with respect to gamma-ray
energy from quartz. Attempts to shield the phos-
phors with other materials in order to equalise the
phosphor and quartz energy dependent responses
may still leave some error.
Another method [ 1 1 - 1 3 ] used to determine the
gamma-ray dose-rate from the soil is by alpha-particle
counting of a representative sample using a ZnS(Ag)
scintillator screen to estimate the contribution from
uranium and thorium (on the assumption of a 'nor-
mal' ratio of Th : U content of 3.16) along with
determination of the potassium content, eg. by flame
p h o t o m e t r y or by X-ray fluorescence analysis. In this
there may be some doubt as to whether the small

593
 594 K Liritzts, R.B Galloway I Calibrating a NaI{TI) scmtillometer

samples actually analysed are truely representative t/rl> i l h t r \ .~iLiq N 2 Inlet

of the soil surrounding the buried artefact over the
range from which significant gamma-dose IS contrib- f)( "*,ar t l a , k
uted. Liq N2~ ~ - - %and

In the present approach it is assumed that the irra- fablt It i l l l l .

baI I
diation of the NaI(T1) crystal in a hole in the ground
is not drastically different from the irradiation of the
buried sherd of interest. For a 3" 3" NaI(T1) crystal
situated above the radioactive matrices Lovborg and
garkegaard [5] showed that the integrated counting
rate above a Fixed energy threshold of 0.37 MeV is
proportional to the dose-rate. A similar proportional-
ity can be expected for the 47r geometry obtained by
placing a 2" 2" NaI(Tt) detector in a narrow hole
drilled into the ground. Although the gamma-radia-
tion from rocks and soils originates from the
naturally occurring radionuclides 4K, :a2Th, 2SSu,
2SSU and their decay products, much of the gamma- I ~,~444a /RT7 ~ T ' H .......... "."'
ray flux in the soil (more than 60%) is composed of
low energy photons as a result of energy degredation
Fig. 1. (a) Cross-section of one of the boxes. (b) Detailed
by scattering of the primary photons [14,15]. This setting of the quartz grains and the dosimeters reside the
low energy weighting of the gamma-ray energy spec- hquid nitrogen dewar.
trum is significant in deciding on a proper relevant
doslmetric technique.
could accommodate up to 550 mg. Each assembly of
phosphors, including three capsules of quartz grains,
2. Calibration of the NaI(TI) scintillometer was arranged in a dewar which was placed in the
centre of each of the boxes (fig. 1). These dewars
For measuring gamma-ray dose-rates the 2 " 2" were kept filled with liquid nitrogen using an auto-
NaI(T1) scintillometer (model PSR6 supplied by matic filler for a period of 20 days for the quartz
Nuclear Enterprises Ltd., Sighthill, Edinburgh) was 110C peak to develop. The other dosimeters, which
calibrated relative to the thermoluminescent response did not require liquid nitrogen cooling to prevent
of quartz grains using the 110C peak of quartz. The fading of the thermohiminescence signal, were left in
calibration was done with four different gamma-ray position for two months. The experiment was con-
emitting media, namely, potassium carbonate ducted indoors so that there were no weathering
(20.5 kg) mixed with sand (150 kg), thorium (120 g
monazite sand) doped sand (150 kg), uranium (11 g
pitchblende ore) doped sand (150 kg) and uranium
1~!
(5.7 g pitchblende ore) doped peat (67.5 kg). Each
mixture was contained in a box measuring 58 cm
40 cm X50 cm. Because of the small amounts of
radioactive materials used per unit weight of sand and
peat, uniform distribution of the dopants cannot be lOO

assumed. The gamma-ray dose-rate within each of

these matrices was measured by thermoluminescence 5o
dosimetry. The dosimeters used were quartz, LiF/
teflon disc in polythene, CaSO4 : Dy in a brass tube
, i

and CaSO4:Dy in a polythene tube. The quartz o mo 200 300 400 500 600

grains were 75-106 /~m In size and were specially m rad,,/y r

annealled and etched to avoid any pre-dose effect. F i g . 2. C a h b r a t i o n curves obtained for the NaI(T1) scintfl-
The prepared grains were placed in capsules which lometer using different dosimeters.
 Y Lirttzis, R B. Galloway / Calibrating a NaI(TI] scintillometer 595

Table 1
Gamma-ray dose-rates (mRad/y) for the phosphors and quartz

Sand and Sand and Peat and Sand and

potassmm thorium u~anium uranium

CaSO4 Dy (m brass) 336 11 468 -+ 12 410 24 487 27

CaSO4 Dy (m polythene) 336 4 536 3 518 24 585 9
L1F 238 8 325 3 261 13 366 3
$102 (quartz) capsule 1 255 18 396 19 338 19 410 22
2 233 15 380 27
3 254 16 372 26 318 10 384 +_24
Scmtillometer C/S (7.0%) 81 7 124 5 107.3 131 2

effects on the boxes of sod. Readings were taken with the different capsules of quartz, table 1, and so the
the scintillometer probe inserted into the dewars average was used in the calibration. Read-out of the
both before and after the period o f exposure o f the therlnoluminescence and dose calibration of the phos-
dosimeters. The scintdlometer discrimination level phors and quartz with a standard beta-source
was set at 0.37 MeV before and checked after each followed estabhshed procedures [10,16]. The result-
measurement using a 137Cs gamma-ray test source. ing calibration curves for the scintdlometer are shown
The average scintillometer readings are compared in fig. 2
with the dose-rates measured with the phosphors
and the capsules of quartz grains in table 1. Three
capsules of quartz grains were used to see whether 3. Discussion
any significant attenuation of gamma-dose occurred
towards the centre o f the sand filled table-tenms Fig. 3 shows the calculated energy dependence of
ball which simulated the sherd. There is no statisti- the mass energy-absorption coefficient relative to air
cally significant difference between the dose-rates for for different materials relevant to gamma-ray

\x

bOll+100~l~20 ~ _ ~ C aSO4
( ONC R E T F T ~ /

\\\\ ,.,,
SOl 1 \\\
ANI)gd4%KzCO 3 / ~
atr
'qANI)~

L,F ~~/SOI I ~50gH~)

PEAT
O.OlO
J i I I t t l L I l a I l : l l a ~ J J i i i i iij l J J i I I I Ill
0 1 I 0 10.0

I- % [ R (,Y \leV
Fig. 3. Energy dependence of gamma-ray mass energy-absorption coefficients relative to air for materials relevant to thermolum]-
nescence dating, calculated from the data tabulated by Storm and Israel [17].
596 Y Liritzis, R B. Galloway / Calibrating a NaI(Tl) scintillometer

doslmetry for thermoluminescence dating. The differ- Table 3

ences are most marked for p h o t o n energies below Uniformity of dopant in boxes by alpha counting
200 keV. For the phosphors the curves indicate the
Sample Estimated (PPM) a Calculated
energy dependence of the thermoluminescent sensi-
by alpha counting from mass of
tivity. The curves therefore emphasise, in view of the dopant
large low energy component of the soil gamma-ray
energy spectrum, the importance for quartz inclusion Th extract 5 2.4
thermoluminescence dating o f determining the Sand Th top, box 76.5 66.8 +_ 7% 78.7
gamma-ray dose-rate with a phosphor with a response Th middle, box 71 6
equivalent to that of quartz or with an instrument U top 134 0
calibrated with respect to the response of quartz itself U middle, box 43.0
Sand Ubottom, edge 10.0 49.0 51% 43.7
as here described. Similarly the curves o f fig. 3 U extract 9.8
explain, albeit qualitatively, why different calibra-
U top 5.3
tions are found for the NaI(T1) scintillometer in rela- U middle, box 100.0
tion to different phosphors (fig. 2). Peat U mlddle, edge 68.7 63.0_+ 35% 48.6
The fig. 2 calibration curve for quartz has been U extract 78.4
used to convert NaI(TI) scmtiUometer readings taken
a With allowance for the U and Th of the sand and peat
in situ to dose-rate values in a thermoluminescence themselves subtracted.
dating programme [18]. This curve for quartz is o f
the form,
dose-rate = 3.08 (count-rate) -+ 14 m R a d / y .
mixing throughly the small amounts of radioactive
Finally, it is of interest to compare the measured ores with the sand and peat. While 20.5 kg o f potas-
absorbed dose-rates in quartz with the values calcu- sium carbonate was used and 120 g o f m o n a z i t e sand
lated from the radioactive content of each box, for thorium doping only 11 g and 5.7 g o f pitch-
taking account of the known weight of active mate- blende were mixed with the sand and peat respec-
rial added and o f the uranium, thorium and potas- tively to provide uranium doping. The inhomogeneity
sium contents of the sand and peat. The latter were was investigated by alpha-particle counting o f samples
determined b y alpha-particle counting and by X-ray from different locations in the boxes (table 3) and
fluorescence analysis. The density of the peat was the thorium doped sand was indeed more uniformly
0.4 g/cm 3 while that of the beach-sand was surpris- mixed than the uranmm doped materials. This diffi-
ingly 1.3 g/cm 3, lower than quartz because o f dftu- culty was anticipated, but the principal idea was to
tion by shells. F o r the purpose of calculation the keep the activity levels as near as possible to those of
boxes were considered of infinite size. The compari- actual softs while having sufficient activity to carry
son, table 2 shows acceptable agreement for potas- out the calibration with adequate accuracy. It should
sium and thorium, but not for uranium in peat or be emphasised that homogeneity of mxxing is not
sand. The principal reason for these discrepancies essential to the calibration of the scintillometer by
seems to be irthomogeneity due to the difficulty of the technique employed.

Table 2
Comparison of calculated and measured gamma-ray dose-rates (mRad/y) for quartz

Box Calculated from Calculated from Total Mean

dopant sand/peat calculated measured value

sand and uranium 554 26.3 580 397 16

sand and thormm 384 26 3 410 383 14
peat and uramum 616 27 4 643 328 -+ 11
sand and potassium 207 26.3 233 247 +_09
 Y. Liritzts, R.B Galloway / Calibrating a NaI(77) scinttllometer
4. Conclusion
The above new calibration technique for relating
the countmg-rate determined with a portable NaI(T1)
scintillometer to the dose-rate absorbed by quartz
grams using different sod media provides a convenient
means of measuring the environmental gamma-ray
dose-rate in an archaeological site, which is an impor-
tant parameter in the age equation of the thermo-
luminescence dating method. The experimental
arrangement simulated the actual situations in sltu
and so is clearly relevant to the use of the technique
m the field. As a result of such a cahbration a
portable scintillometer can be used to measure with
high confidence gamma-ray dose-rates for thermo-
luminescence dating m an extremely short period of
time.
The authors thank Dr. H. McKerrell for sthnulat-
ing discussions and Dr. V. Mejdahl for his valuable
comments. We acknowledge with thanks the loan of
the thermoluminescence measuring equipment by the
Trustees of the National Museum of AntNuities of
Scotland. Y.L. is particularly grateful to the National
Hellenic Research Foundation, the Royal Society
(London) and the University of Edinburgh for finan-
cial assistance.
597
References
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