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J Radioanal Nucl Chem

DOI 10.1007/s10967-013-2474-2

Assessments on energy and efficiency calibration of an alpha


spectrometry system using standard sources
M. R. Calin M. A. Saizu I. Radulescu

Received: 12 September 2012


Akademiai Kiado, Budapest, Hungary 2013

Abstract Studies and evaluations of the main parameters


of a high resolution multi-chamber alpha spectrometer and
its full calibration using standard sources of 241Am, 233U
and 244Cm are presented for the validation of the complex
method of characterization of an alpha spectrometer dedicated for alpha radioactive concentration measurements of
various environmental samples. The resolution and efficiency were determined at all possible source-detector
distances for all eight solid state ORTEC ULTRA-AS
detectors. In addition, the solid angles associated to different measurement geometries and the repeatability of the
results were assessed. A detailed inter-comparison of the
results was performed drawing important conclusions
regarding the quality of the alpha detector response to the
alpha radiation of the standard sources used in
measurements.
Keywords Alpha-ray spectrometry 
Energy and efficiency calibration  FWHM 
Multi-chamber  Alpha-spectroscopy workstation

Introduction
Alpha-particle spectrometry of high resolution is a measurement method widely used in many applications like
nuclear decay data measurements, geological studies and

M. R. Calin  M. A. Saizu  I. Radulescu (&)


Department of Life and Environmental Physics,
Horia Hulubei National Institute for Physics and Nuclear
EngineeringIFIN HH, 30 Reactorului Street,
P.O. Box MG-6, 077125 Magurele, Romania
e-mail: rileana@ifin.nipne.ro

isotopic composition determination of alpha-particle


emitting radionuclides [1]. Among applications, of significance is the accurate measurement of low level activity of
environmental samples. The reason for this is that the
detector exhibits such low background and high efficiency
that renders enhancement of the lower detection limits up
to 23 orders of magnitude compared to gamma spectrometry/high purity germanium detector [2].
The design of the ion-implanted-silicon charged-particle
detectors assures that the alpha particles are not stopped in
their very thin entrance window. Their energy is totally
absorbed in the alpha detector to produce ion pairs that are
generating an electrical signal with the amplitude directly
proportional to the energy absorbed [3]. Moreover, during
measurement, the detector surface and the sample are
maintained under high vacuum. This fact eliminates the
loss of alpha particle energy due to interactions between
the alpha particles and air atoms. The individual energies
of the alpha radionuclides can be identified by spectrometric methods after energy calibration of the corresponding spectrometer, i.e., determining a relation between
the energy absorbed by the alpha detector and the amplitude of the corresponding electrical signal.
SALMROM laboratory designed for a, b, c spectrometry and radon measurements from the Department of Life
and Environmental Sciences of Horia Hulubei National
Institute for Physics and Nuclear Engineering, Bucharest
(IFIN-HH), Romania, uses a state-of-the-art multi-chamber
alpha spectrometer, type Octete Plus from ORTEC company [4] for activity measurements of alpha emitting
radionuclides in environmental samples.
The aim of this paper is to characterize the aforementioned spectrometer applying appropriate methods for the
energy and efficiency calibration. Calibration measurements were conducted for the evaluation of the main

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J Radioanal Nucl Chem

parameters using standard radioactive sources. Repeatability of the results was tested for method validation
purposes. To our knowledge, this paper constitutes a first
attempt to evaluate the performance of a multi-chamber
alpha spectrometer by complete individual measurements
of its ion-implanted-silicon alpha detectors and to present
the results in a comparative manner.

Materials and methods


The experimental equipment is a multi-chamber/multichannel analyzer alpha spectroscopy workstation, type
ORTEC Octete Plus that has fully integrated control for its
internal alpha spectrometers. It incoporates eight independent high-quality modular vacuum chambers equipped
with a high-performance ion-implanted-silicon chargedparticle detector, its associated electronics, a multichannel
pulse-height analyzer and a test pulser [4]. The detectors,
ULTRA-AS type and BU-019-300-AS model with
300 mm2 active area are operated in the 0 7 10 MeV
energy range. The bias voltage applied to each detector was
50 V. Inside each chamber there is a Sample Holder that
allows the measurement of the sources of 1 7 25 mm
active diameter at different sample-detector distances
between 4 7 40 in 4 mm increments decided by the
chamber wall slots [4]. Each chamber is individually
controlled by specialized ORTEC MCA Emulation
and Analysis software for alpha detector spectra as
MAESTRO-32 [5] and Alpha Vision-32 [6]. Alpha standard electro-deposited disc sources of radionuclides from
the actinide series such as 241Am, 233U and 244Cm were
used in all the measurements. The uncertainty of the source
activities was 3 % at the 95 % confidence level.
The sources were placed at all available source-detector
distances of the chambers for the determination of the

Fig. 1 Average efficiency for


241
Am, 233U and 244Cm sources

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detectors efficiency and resolution. The values of the


efficiency were calculated dividing the resultant net count
rate (cps) by the alpha emission rate of the source (alpha/s)
as declared in the alpha source calibration certificate [7].
For all efficiency calculations, the region of interest (ROI)
was between channel 600 and 1,935 of the pulse height
spectra acquired for 1,800 s with a multi-channel analyser
of 2,048 channels. The net activity data were derived after
considering the background and integral area in the above
ROI. From the differential pulse height distributions representing the response of the alpha ULTRA-AS detectors to
the energy lines of the sources, the energy calibration of the
alpha spectrometer was performed and the energy resolution of the detectors were determined, by calculating the
full width at half maximum (FWHM), that emphasize their
capability to separate close energy lines. The sourcedetector distances with the best resolution were considered
optimum and on these, repeated measurements were conducted to estimate the bias of the results. Considering the
geometrical characteristics of the sources and those of the
detectors, it was determined the variation of the solid angle
with the source-detector distance. For the validation of the
method used to calibrate the alpha chambers it was measured another certified alpha source of 241Am (manufacturer CEA BNM LMRI).

Results and discussion


Detector efficiency and resolution
Figure 1 presents the average of the experimental values of
the efficiency versus source-detector distance.
The best fit of them was obtained considering power law
functions of the form y = ax-b. The parameters of the
fitting curves, a and b, and the residual sum of squares

J Radioanal Nucl Chem


Fig. 2 Average efficiency
values for the cell no. 5 of the
alpha spectrometry system

(RSS) are 3.6, 1.26 and 0.03 for 241Am, 5.5, 1.38 and 0.05
for 233U and 5.3, 1.37 and 0.04 for 244Cm. Due to the
straggling effects, the efficiency of the alpha detector has a
rapid decrease for source-detector distances less than
1.529 (detector diameter), reaching then a stable level for
higher distances. At small source-detector distance, the
values of 241Am efficiency respecting to those of 233U and
244
Cm are systematically lower due to geometrical differences of the source active areas. Moreover, because of the
characteristics of the alpha particle interaction with the ionimplanted-silicon charged-particle detectors, the efficiency
of the alpha detectors is constant regardless of the incident
alpha energy [8] and that it depends on the measurement
geometry, as it is represented in Fig. 2.
The values of the FWHM at the main energy lines of the
241
Am, 233U and 244Cm sources, are represented, in Fig. 3,
for seven chambers, as a function of the source-detector
distance.
It can be seen, for all three alpha sources, that the variation of the resolution with the source-detector distance
has two distinct parts: a fast decreasing of the FWHM for
distances corresponding to the 420 mm and a smooth
decrease of the FWHM for source-detector distances in the
range from 24 to 40 mm [9]. The straggling effect is
responsible for the high variation of the resolution on the
first five source-detector distances of each chamber making
difficult the identification and quantification of the 241Am,
233
U and 244Cm alpha energy lines. The data of the
chamber no. 7 are not presented in Fig. 3 because of a high
leakage current ranging from 120 to 180 nA, developed by
the detector due to a scratch on its front surface. The other
ion-implanted detectors have standard leakage currents in
the tenths of nanoamperes, from 30 to 60 nA. In Table 1
the optimum values of the energy resolution of the

detectors at the 241Am line of 5.4856 MeV are given for


each chamber in the same set-up conditions.
Considering the optimum source-detector distance as
that corresponding to the best detectors energy resolution,
there were performed ten measurements of 1,800 s, using
the 241Am source, for studying the efficiency and energy
resolution repeatability The average values of the detector
efficiency and resolution together with their relative standard experimental error values as a measure of their dispersion S(n-1) [%] and the relative standard experimental
error of the mean values S(aver) [%] are presented in
Table 2. The standard errors of these values relative to the
resolution of 19 keV warranted by the producer were in the
range 0.75.3 %.
Evaluation of the solid angles
The optimum values of ULTRA-AS detectors resolution of
the tested alpha spectrometer were obtained for sourcedetector distances with low solid angles that allow the
detection of alpha particle emitted perpendicularly by the
source in conditions of minimum scattering effects and
energy loss of alpha particles in the source layer and
detector window. The geometry design of every chamber
assures a precise definition of the source-detector distances.
It creates the ideal conditions for a high reproducibility of
the measurements and accuracy of the results, due to the
constant detection efficiency.
In the range (440) mm, in a co-axial geometry, there
were determined the solid angles subtended by the
ULTRA-AS detectors of diameter 19.6 mm and a circular
disc source with an active area of 7 mm diameter, using the
formula from the references [1013]. The values obtained
were represented in Fig. 4.

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J Radioanal Nucl Chem


Fig. 3 Detector FWHM at:
a 5.4856 MeV for 241Am,
b 4.824 MeV for 233U and
c at 5.805 MeV for 244Cm

Background consideration
The background of the ULTRA-AS detector is nearly
negligible. Since the surface area of the detector is small

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and the contact electrodes are extremely thin, there is only


a small amount of material that is available to contribute to
the detector background [8]. The measurement background
for all chambers is ranging from 17 to 42 counts per day,

J Radioanal Nucl Chem


Table 1 Optimum resolution for each chamber
Chamber/distance source-detector
(mm)

Resolution calculated
(keV)

1/32

18.44

2/24

18.88

3/32

19.14

4/32

18.95

5/28

19.09

6/24

18.55

8/24

19.74

for the energy window of 39.7 MeV. As a result, for


energies above 3 MeV, the background is \9.2 counts per
day per cm2 of active detector area, or \27.5 counts per
day for a 300 mm2 surface area detector.

Calibration method validation


According to the quality assurance requirements for laboratories [1418], in order to validate the calibration method
to obtain measurement results with high accuracy, it was
considered important to measure another certified standard
alpha disk source of 241Am of unknown activity at the
moment of the measurement. The source was located at
32 cm source-detector distance of the chamber 5, considered as the optimum position from the alpha spectrometer
resolution point of view. The obtained result of
4,472 90 Bq indicates a comparable activity value with
that of 4,424 88 Bq declared in the calibration certificate, with a very low relative error of 1 %.

Table 2 Efficiency and FWHM repeatability for


Chamber

Fig. 4 Normalized solid angle variation on the source-detector


distance

Conclusions
A comprehensive characterization of the multi-chamber/
multi-channel analyzer alpha spectrometer ORTEC Octete
Plus was performed. Many measurements were done to
assess the main spectrometric parameters of all eight
ULTRA-AS detectors. In addition, the determination of the
solid angle for quantifying the fraction of the total emitted
radiation detected was achieved. The tests of efficiency and
resolution repeatability evaluation and of measuring
another alpha source demonstrate the fact that the alpha
spectrometer was correctly calibrated in energy and in
efficiency and that the measurement methods used are
robust and can be validated. The spectrometer was
designed to assure a very good reproducibility of the
measurement geometry with direct impact on data accuracy. More comprehensive data analysis and spectra
modelling are considered for the future.

241

Am at optimum source-detector distance

241

Am

Efficiency (cps/alpha/s)

FWHM (keV)

Efficiency average

S (n-1) (%)

S (aver) (%)

FWHM average

S (n-1) (%)

S (aver) (%)

0.042456

0.1033

0.0311

18.872

1.959

0.591

0.067763

0.3004

0.0906

19.213

2.974

0.897

3
4

0.042446
0.042331

0.2704
1.4060

0.0815
0.4239

18.828
19.042

1.731
1.072

0.522
0.323

0.054065

0.2271

0.0685

19.593

4.122

1.243

0.070239

0.3739

0.1127

19.009

3.271

0.986

0.068514

0.5126

0.1546

20.008

3.667

1.106

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J Radioanal Nucl Chem


Acknowledgments This study was supported by the PNCDI II
Program, Project No. PN 09 37 03 01/2012 of Romanian Ministry for
Education and Research.

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