EFFICIENCY CALIBRATION IN GAMMA SPECTROMETRY BY USING

232
Th SERIES RADIONUCLIDES*

L. DARABAN1, D. IANCU2, D. NITA3, LAURA DARABAN3

1
University Babeş-Bolyai, Faculty of Physics, Kogalniceanu Str. 1, 400084 Cluj-Napoca, Romania
2
C.N.C.A.N. Bucharest, Romania
3
University Babes-Bolyai, Faculty of Engineering and Environmental Science, Cluj-Napoca, Romania
Received November 15, 2012

In this paper a new method for preparation of any shape radioactive sources with a
desired activity is described, by using ThO2 in secular equilibrium for calibration in
efficiency of a HPGe detector. By knowing the absolute specific activity of ThO2 and
the disintegration probability of the γ- emitters from the 232Th series, the efficiency
curve of the spectrometer was well determined for different shape of samples. We also
used this method for preparation of calibration samples in Marinelli backers, by mixing
a determined quantity of ThO2 with artificial soil for environmental radioactivity
measurements in different types of soils from the forest and uranium mines zones, in
which radionuclides from the uranium family were identified and the total activity of
the samples was determined.
232
Key words: Th series, gamma spectrometry, calibration, efficiency curve, Marinelli
beaker, soil gamma activity.

1. INTRODUCTION

It is an often used practice, when determining the activity of gamma emitters

with HPGe detectors, to compare measurements of an unknown source with those
of a calibrated source of equivalent geometry and density. The total efficiency is
defined as the ratio of the number of pulses recoded in the spectrum and the
number of photons emitted by the source. When a standard source of 152Eu is
prepared, after the neutron activation also the impurity of 154Eu is obtained in the
sample. As shown in [1], the standardization of a 152Eu source is not an easy task, a
measurement in a coincidence system 4πβ−γ is required.

*
Paper presented at the First East European Radon Symposium – FERAS 2012, September 2–5,
2012, Cluj-Napoca, Romania.

Rom. Journ. Phys., Vol. 58, Supplement, P. S99–S107, Bucharest, 2013

S100 L. Daraban, D. Iancu, D. Nita, Laura Daraban 2

An efficiency calibration method was developed in our laboratory to measure

the radioactivity of volume samples with HPGe detectors. These semiconductor
detectors have a high resolution, determining the energies of the gamma radiation
emitted by the natural radioisotopes from the soil and building materials, especially
by uranium, radium and thorium. These elements give an average dose of
0,5 mGy/year. Also, the internal irradiation, a component of the natural irradiation,
is caused by the inhalation of air and ingestion of water and aliments (in the human
body).

2. EXPERIMENTAL

A gamma spectrometer with a HPGe semiconductor detector type 1519

Canberra was used for the measurements, operated under a high voltage of 3.5 kV,
with relative efficiency of 15%, equipped with a multichannel analyzer with 4096
channels working with the aquisition software Genie 2000. The detector is
surrounded by a Pb shield type NZ 138, designed to prevent gamma photons from
the environment to reach the detector, so that the radionuclides activity from the
soil at the natural level can be measured. This shielding system was manufactured
in our laboratory at the UBB Cluj-Napoca.

Fig. 1 – View of a Pb shield NZ 138 of the HPGe detector.

For natural samples with a very low activity it is difficult to separate the
recorded signal from the background radiation, especially in a laboratory
environment. In these conditions, measurements can be performed only using a Pb
shielding (Figure 1).
3 Efficiency calibration in gamma spectrometry by using 232Th series radionuclides S101

2.1. METHODOLOGY OF THE CALIBRATION IN ENERGY

AND EFFICIENCY OF THE EQUIPMENT

The efficiency calibration of the analyzer channels using standard sources is a

procedure periodically performed for the HPGe detector, as in [2] establishing the
connection between the energy of the gamma radiation and the number of the
channel. After the identification of the energy using standard sources, the
efficiency value is calculated taking into account the probability of disintegration
for each energy. This data is necessary for the calibration of the detector in
efficiency, as in the formula:
ε=N/(εg·t·Λ·p) (1)
where: ε = is the detector efficiency
N = is the peak area in number of counts at that energy
Λ = is the absolute activity of the standard [Bq]
t = is the measurement time
p = is the probability of disintegration of the radionuclide
εg = is the geometric efficiency.
By applying the formula (1), the peak areas N for each peak energy can be
deduced and by taking into account the scheme factor (p), the detector efficiency
can be calculated [3-5].
In the beginning we used a standard point-source of known activity of
3.33 kBq of 226Ra, which emits many energy lines, as in the spectrum presented in
Figure 3, where 226Ra is in secular equilibrium with its descendents [6]. The
efficiency is calculated again with the same formula and the obtained results are
presented in Table 1 and Figure 2.

Table 1
Detector efficiency calculation using a source of 226Ra
Energy Peak Scheme factor
(keV) area (p) Detector efficiency (%)
243.7 171868 0.074 19.5
296.8 364903 0.19 16.2
353.4 589516 0.37 13.4
609.8 363348 0.46 6.6
769 21707 0.049 3.7
934.7 12566 0.03 3.5
1120.9 62058 0.15 3.5
1239.6 17966 0.057 2.6
1378.4 14570 0.04 3.1
S102 L. Daraban, D. Iancu, D. Nita, Laura Daraban 4

Figure 2 - Characteristic spectrum of 226Ra and its descendants with 60Co.

Fig. 3 – Detector efficiency curve using a source of 226Ra.

5 Efficiency calibration in gamma spectrometry by using 232Th series radionuclides S103

In Figure 3 it can be noticed that the shape of the efficiency curve is similar
with those from the literature for this type of detector.

2.2. EFFICIENCY CALIBRATION OF VOLUM SAMPLES WITH ThO2

IN SECULAR EQUILIBRIUM

In order to measure the radioactivity of the soil (and other samples with low
activity) it is important to use samples in high volumes. In our laboratory we
conceived and manufactured some Marinelli beakers adapted to the shape of the
shielding in the laboratory. In order to measure the radioactivity of the soil (and
other samples with low activity), it is important to use samples in high volumes. In
our laboratory we conceived and executed some Marinelli beakers adapted to the
shape of the shielding in the laboratory. Further, a sample containing oxide of Th
older than 30 years [7-10] was used as thorium progeny implantation for alpha
spectrometry and also as a calibration source in efficiency as in [11-14], where the
absolute activity per gram of ThO2 was of 3565 ± 15 Bq/g. In this procedure the
geometrical factor was included in equation by using a beaker with the same
geometry as the sample. The main gamma lines of 232Th at secular equilibrium with
its daughter radionuclides are presented in Table 2, it can be seen that 212Bi decays
by both emitting an alpha particle (36 %) and beta particle (64 %).

Table 2
232
The Th series parameters
Energy (keV) Radionuclide Intensity (%)
228
209.4 Ac 4.55
228
270.3 Ac 3.77
228
328 Ac 3.36
228
338.4 Ac 12.01
228
463.0 Ac 4.64
228
911.1 Ac 29.0
228
968.9 Ac 17.46
228
1459.2 Ac 0.92
228
1587.9 Ac 3.71
208
510.7 Tl 22.5
208
583.1 Tl 86.0
208
860.5 Tl 12.0
208
2614.5 Tl 100
212
727.17 Bi 11.8
212
238.6 Pb 43.1

In order to measure the radioactivity of the soil (and other samples with low
activity), it is important to use samples in high volume. In our laboratory we
manufactured some Marinelli beakers adapted to the shape of the shielding in the
laboratory.
S104 L. Daraban, D. Iancu, D. Nita, Laura Daraban 6

The calibration of Marinelli beakers can be made locally in each laboratory

by using mixtures of soil-radionuclides for the calibration using old Th (in
equilibrium with its daughter nuclei), in the shape of ThO2 or Th(NO3)4 [3], as in
Table 3, in a mixture with a matrix of soil of CaCO3, SiO2, Al2O3 or other
compounds with the density similar to that of the samples that are about to be
analized, following the calibration procedures described in [10, 11].
In order to calibrate the Marinelli beaker with ThO2 it is necessary to prepare
a standard mixture (artificial soil) in a beaker containing SiO2 with 2 % Al2O3, with
a total mass of 260 g, to which we added a quantity of 218 g CaSO4· 2H2O
(gypsum). The half-life of ThO2 of an order to tenth of years was enough in order
to establish a secular equilibrium. The Marinelli beaker was filled with a mixture of
a total mass of 541 g, from which 0.32 g of ThO2 (Carlo Erba, Italy) and added it to
the matrix of 1239.04 Bq activity was homogeneously dispersed in the entire
volume of the sample. In order to obtain an uniform dispersion of ThO2 in the
artificial soil is necessary to mix them using a special procedure described in [11].
The measurement time was about 1 hour and the result is presented in Figure 4.

Fig. 4 – Characteristic gamma spectrum for the artificial ( SiO2 · Al2O3 ·CaSO4) soil,
impurified with 0.32 g of ThO2 with an absolute activity of Λ =1239 Bq.
7 Efficiency calibration in gamma spectrometry by using 232Th series radionuclides S105

Table 3
Data from the calibration spectrum using ThO2 in Marinelli beaker
Statistic error εi
Ni pi (Scheme
Energy for peak area (detector Radionuclide
(peak area) factor)
calculation efficiency)
keV Counts/hour (%) (%) (%) -
237.4 47718 0.6 43.1 89 Pb-212
336.5 7388 2 12 50 Ac-228
581.8 12407 1 86 20 Tl-208
725 2732 5 11 19 Bi-212
910 8420 2 29 23 Ac-228
966.4 6057 2 17.5 28 Ac-228

The slope of efficiency with Marinelli beacker is done in Figure 5.

Efficiency with Marinelli beacker

100
90
Detector effciency (%)

80
70
60
50
40
30
20
10
0
0 200 400 600 800 1000 1200
Energy (keV)

Fig. 5 – The detector efficiency for large sample in Marinelli beacker determined with ThO2.

3. APPLICATIONS FOR THE MEASUREMENT OF SOIL SAMPLES

A sample of soil is characterized by defining its structure, the agricultural

state and the vegetative bed [12-14]. After the calibraton of detector was measured
the gamma spectrum of a sample of mosses (Sphagnum sp.) with soil from Baita
river, an area with uranium ore. From the Figure 6 spectra results the presence of
S106 L. Daraban, D. Iancu, D. Nita, Laura Daraban 8

226 214 214

the following nuclides from uranium family: Ra, Pb and Bi in a
contaminated sample.

Fig. 6 – Characteristic gamma spectrum of a sample of mosses (Sphagnum sp.) with soil from Baita
river, with a total activity of 544 Bq (without the contribution of 40K and the presence of 137Cs),
measured for 1 hour.

If the annual average of the γ-global activity for the samples of uncultivated
soil was about 311.5 Bq/kg and the maxium value was of 390.9 Bq/kg recorded on,
the values are situated in the range of variation of the natural background in the
area [13-14]. The activities of the radionuclides from natural samples show values
in this range.

4. CONCLUSIONS

In these experiments a shielding made of low level background Pb was used

and the measurements were performed with a HPGe gamma spectrometer in order
to aquire the gamma spectra for the measured samples.
In the beginning an energy calibration of the spectrometer was made and then
a calibration in efficiency using standard samples with 226Ra small samples and
other type Marinelli beakers containing ThO2 in secular equilibrium was also
studied. The characteristic gamma spectrum of the pure ThO2 was then obtained,
9 Efficiency calibration in gamma spectrometry by using 232Th series radionuclides S107

by knowing the scheme factors and the descendent radionuclides. The calibration
in efficiency was also made for samples of artificial soil containg ThO2.
This method was then applied to a sample of soil from the area of mines with
uranium, obtaining a spectrum in which it was possible to identify radionuclides
from the uranium series. The total gamma activity of a contaminated sample of
390.9 Bq/kg was determined, measured for natural radionuclides. The obtained
results were placed under the level of warning, fiting into the limits of variation of
the natural background in the area, measured also on natural soil samples from the
Faget forest.

Acknowledgements. This paper was realised with the support of POSDRU/89/1.5/5/60/89

project funded by the European Social Found and Romanian Government.

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