ATOMIC AND NUCLEAR PHYSICS

RESULTS OBTAINED BY THE RADIONUCLIDE METROLOGY

LABORATORY OF IFIN-HH, IN THE INTERNATIONAL COMPARISONS
OF STANDARD SOLUTIONS, DURING 20022004*

MARIA SAHAGIA, ANAMARIA CRISTINA RAZDOLESCU, E.L. GRIGORESCU,

A. LUCA, C. IVAN
National Institute of R&D for Physics and Nuclear Engineering Horia Hulubei,
IFIN-HH, POB MG6, Bucharest, Romania
(Received December 21, 2004)

Our laboratory has participated in international comparisons of standard

sources and solutions, organized by the International Committee of Weights and
Measures (CIPM), the EUROMET system, the former COMECOM, and bilateral
comparisons, since 1962. The last comparisons, organized by the CIPM, regarded the
radionuclides: 32P, 54Mn, 65Zn, 192Ir, 204Tl and 241Am.
We participated at the comparisons organized for all the cited radionuclides, by
using the following methods of standardization: the liquid scintillation, triple to
double coincidence ratio was used for 204Tl , 32P, 241Am; the 4C, coincidence
method, in the variant of the efficiency extrapolation was used for the radionuclides:
241
Am, 192Ir, 65Zn, 54Mn, with the detection of the alpha and beta rays, Auger
electrons, X rays in the proportional counter.
The paper presents a summary of the methods used for standardization and the
obtained results.

1. INTRODUCTION

Our laboratory has a long tradition of participation in international

comparisons of standard sources and solutions and of the standardization methods,
organized by the International Committee of Weights and Measures (CIPM), the
EUROMET system, former COMECOM, and bilateral comparisons, starting with
the year 1962.On the other side, starting with 1976, at the Bureau International de
Poids et Mesures (BIPM) the International Reference System (SIR) was put in
operation; it allowed the check of the activity of radioactive standards prepared and
certified by National Metrology Institutes, specially for gamma-ray emitters. Both
actions were preparative steps in accepting the concept of the degree of

*
Paper presented at the 5th International Balkan Workshop on Applied Physics, 57 July 2004,
Constana, Romania.

Rom. Journ. Phys., Vol. 51, Nos. 12, P. 2126, Bucharest, 2006
22 Maria Sahagia et al. 2

equivalence for the national standards, at the international level, for the ionizing
radiations, in preparing an international system of recognition of the standards,
certificates and measurements [1, 2].
In 1999, a great number of national metrology institutes signed the
International Committee of Weights and Measures Mutual Recognition
Arrangement (CIPM- MRA), as a technical base for mutual recognition of
standards and certificates. In the field of radionuclide metrology, an amplified
number of international comparisons were organized by the BIPM and the
evaluation of the former comparisons, as well as of the measurements made in the
frame of the SIR, were carried out. An impressing rich Data Base, known as
BIPM- Key Comparison Data Base (KCDB), Appendix B, of the CIPM-MRA was
constructed. It is accessible on the address: www.bipm.org. KCDB, and it reflects
the degree of equivalence for the worldwide metrology laboratories. In the field of
the activity unit, Becquerel, our Institute is registered with 19 results.
The radionuclides for the most recent comparisons, were chosen such as to cover
several areas of interest, as follows:
- to respond the necessities of practical use of radionuclides: 32P, 192Ir,
radionuclides used in medicine, life sciences, industry
- to assure the most precise standards for radionuclides used in the
calibration of the gamma spectrometers, for scientific purposes, as well as
for environmental radioactivity survey and other analyses: 241Am, 54Mn,
65
Zn, or for the calibration of beta contaminometers: 204Tl
- to check various types of standardization methods, and various types of
radionuclides: 241Am is an alphagamma emitter; 32P and 204Tl are pure
beta emitters; 192Ir has a very complex decay scheme, including beta and
electron capture decays, followed by emission of gamma rays; 54Mn is an
electron capture-gamma emitter, while 65Zn is an electron capture beta
plus-gamma emitter.
We participated at all these comparisons, by using various methods of
standardization.

2. STANDARDIZATION METHODS

2.1. THE LIQUID SCINTILLATION, TRIPLE TO DOUBLE COINCIDENCE RATIO

(LSC-TDCR)

The method was first developed at the R.C., Poland and at the LNHB, France
[3, 4]. Nowadays, it is fully applied at the international scale, including our
laboratory. Our equipment consists in a detection unit, provided with three photo-
multipliers, acted by the light emitted in the vial containing the radioactive solution
dissolved in a liquid scintillator, and the electronic unit; the principle of the method
was described in detail in the paper [5].
3 International comparisons of standard solutions 23

The equipment and the method had been verified previously in the 89Sr,
CIPM and in the bilateral, IFIN-HH, Romania LNHB, France, 3H comparisons
[6,7].
The method was used for 204Tl and 32P, two beta emitters. 32P is a high energy
beta emitter, Ebeta maxim= 1710.4 keV, while 204Tl has a 97.5% beta decay branch,
with Ebeta maxim= 763.4 keV and a 2.5% decay branch by electron capture.
Leaving from the general theory of the TDCR principle, it is necessary to
determine the detection efficiency. The following process is used:
The counting rates on the triple and on the double coincidence channels, T
and D, are registered; the theoretical detection efficiencies on the same channels, t
and d, are calculated, by taking into account the decay scheme parameters and the
scintillator photomultipliers system characteristics; the counting rate ratios and
the calculated efficiencies ratios are compared; when these ratios are equal, means:
T/D = t/d (1)
the theoretical models of efficiency calculations, with their parameters, are good,
and the activity to be measured is calculated as:
No=D/ d or No=T/ t (2)
No is the activity of the source
The method was also used for standardization of 241Am. In this special case, due to
the high detection efficiency of the alpha particles in the scintillator, the values
t = d =1, and
No=D (2)

2.2 THE 4C, COINCIDENCE METHOD, IN THE VARIANT

OF THE EFFICIENCY EXTRAPOLATION

This method was used for the radionuclides: 192Ir, 65Zn, 54Mn, with the
detection of the beta rays, Auger electrons, X rays, in the proportional counter
(PC).The method was described in detail in literature [8].
192
Ir, has a very complex decay scheme, decaying by beta minus/plus and
electron capture, both of decays being followed by the emission of a high number
of gamma rays, with energies within the interval 205.79 keV612.45 keV. For
obtaining a linear graph of extrapolation, linearity conditions had to be
accomplished; they were applied such were found in our laboratory [9], by
choosing a proper energetic measurement window on the gamma channel. 65Zn
decays by electron capture, with a decay probability of 98.5%, and by positron
emission, with a probability of 1.5%. Its emissions on the beta channel consist from
positrons, X-rays and Auger electrons. The emitted gamma rays are: annihilation,
511 keV and 1115.6 keV. An original method of assurance of the linearity
24 Maria Sahagia et al. 4

conditions was found in our laboratory [9] and further developed [10]; it consisted
in the combination of the selection of measurement window with the use of lead
absorbers. 54Mn decays by electron capture, followed by the emission of 834.84
keV gamma quanta. Its decay scheme is simple, but the special difficulty is due to
the very low energy of X-rays and Auger electrons emitted after decay, resulting in
a low detection efficiency; when the extrapolation method is applied, a long
extrapolation interval must be used, and supplementary type B uncertainties can
occur. In order to reduce them, the extrapolation procedure was applied for every
measured source.

2.3 THE 2PC() , 4PC() COINCIDENCE METHOD

The method was applied for the standardization of 241Am, an alpha-gamma

emitter. The method is simpler, due to the high detection efficiency of the alpha
radiations in the proportional counter, on one side, and due to the elimination of the
decay scheme corrections, allowing the use of the classical coincidence formulae;
both detection geometries, 2sr and 4sr were used, in order to check of occurrence
of parasite impulses, which could be detected.

3. RESULTS

3.1 RADIONUCLIDES 32P AND 204Tl

In both cases, BIPM published the results as comparison reports; an official

document, regarding the degree of equivalence will be issued for 204Tl. In the case
of this radionuclide, our result was A = 102.2 kBq g-1, with uc = 1.6 kBq g-1(1.6%)
(k =1), where A, uc , k, are respectively the massic activity of the solution, the
combined uncertainty, and the coverage factor, according to the Standard [11]; it is
very near the LNHB-France, IRMM- JRC, EC and is only 0.30% higher than the
mean value, evaluated at the BIPM.
In the case of 32P, although it was considered as a simple comparison, due to
the high beta energy, a significant amount of radionuclide impurities were detected
by all the participants, not declared before the comparison. Their content amounted
at: 33P (7.3 2.5%), 35S (2.0 0.2%).The total amount of impurities was 9.3%; they
were different from 32P. The evaluation of impurities, both pure beta emitters, was
possible only by following the decay curve of the mixture. The value determined in
our Lab was A = 27.2 kBq g-1, with uc = 0.92 kBq g-1 (3.4%), (k =1); the high
uncertainty value is mainly due to impurities evaluation. The spread of all results
from participants was high, and the decision which was taken by the Consultative
Committee CCRI(II) of CIPM is the repetition of the comparison..
5 International comparisons of standard solutions 25

3.2. RADIONUCLIDES 192Ir, 65Zn, 54Mn

The BIPM report of comparison was first issued for the radionuclide 192Ir.
Afterwards, the Draft B Report Ir-192 2004/06/14, entitled BIPM comparison
BIPM.RI(II)-K1.Ir-192 of the activity measurements of the radionuclide 192Ir and
links for the international comparison CCRI(II)-K2.Ir-192 was introduced in the
CIPM- MRA, Appendix B, KCDB.
Our result was A = 204.81 kBqg-1, with uc = 0.33 kBq g-1 (k =1), very near
the results of NPL-UK and PTB-Germany. It is 0.52% higher than the mean value.
A worldwide mean of the reference value, Key Comparison Reference Value
(KCRV), was established. It was declared that our result is included in the KCRV
calculation.
In the case of 65Zn, our result is A = 54.78 kBq g-1, with uc = 0.27 kBq g-1
(k= 1) on the reference date.
For the radionuclide 54Mn, our result was: A = 312.69 kBqg-1, with uc = 0.84
kBq g-1, (k =1).

3.3 RADIONUCLIDE 241Am

For this radionuclide, two different results, corresponding to the two methods
of standardization were transmitted to the BIPM. They were: A = 296.9 kBqg-1,
with uc = 1.1 kBq g-1 (k=1), corresponding to the coincidence method, and
A = 294.5 kBqg-1, with uc = 1.4 kBq g-1 (k=1), corresponding to the LSC-TDCR
method. The two independent results agree within the limit of 0.81%, with a
calculated coverage value k =1.33.

4. CONCLUSIONS

Our laboratory participated at six international comparisons, for the

radionuclides: 32P, 54Mn, 65Zn, 192Ir, 204Tl and 241Am, involving various
measurement methods, in a very short period;
The obtained results are very satisfactory, our laboratory being well
situated at the international level;
The large scale comparisons, together with the SIR measurements, assure
the linkage and consistence of measurements, as the technical base for the practical
application of the CIPM-MRA document.

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313 (2000).
26 Maria Sahagia et al. 6

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