J Radioanal Nucl Chem
DOI 10.1007/s10967-017-5451-3
Design and performance of a miniature TDCR counting system
K. Mitev1 • P. Cassette2 • V. Jordanov3 • H. R. Liu4 • Ch. Dutsov1
Received: 31 May 2017
Akadémiai Kiadó, Budapest, Hungary 2017
Abstract A portable liquid scintillation counting system Introduction
based on the triple-to-double coincidence ratio (TDCR)
method was developed at Sofia University ‘‘St. Kliment The triple-to-double coincidence ratio (TDCR) method was
Ohridski’’. The system consists of a miniature TDCR developed for the direct determination of the absolute
counter with cylindrical optical chamber and a specialized activities of beta- and electron-capture decaying radionu-
TDCR counting module named nanoTDCR. The clides in liquid scintillator cocktail ([1], and the references
nanoTDCR module is produced by the labZY company and therein). This method is largely used by the National
provides several important new TDCR counting function- Metrology Institutes (NMIs) for primary standardization
alities like: individual extending-type dead-time in each [2]. Recently, portable TDCR counters were developed at
channel; simultaneous counting with two different ENEA (Italy), LNHB (France), NPL (UK) and PTB
extendable dead-times and two different coincidence win- (Germany) in the framework of the European Metrofission
dows and simultaneous TDCR counting and spectrum project [3]. These TDCR counting systems differ in their
acquisition. The performance of the new system was tested design and in their electronics. However, the portable sys-
in benchmark comparisons with the LNHB’s primary tems show comparable performance and activity mea-
TDCR counting system of activity measurements of surement results which are typical of the TDCR metrology
241
Am, 3H, 14C and 63Ni. Good agreement between the two instruments used in the NMIs [3]. The developments in the
systems was observed. framework of the Metrofission project indicate that it is
important to develop portable TDCR counting systems.
Keywords TDCR counter Miniature TDCR system Portable TDCRs are also found useful for in situ activity
NanoTDCR Extending dead time Absolute activity measurements and calibrations in nuclear medicine
measurement departments in hospitals [4]. This work addresses the
challenges of developing a portable TDCR counting sys-
tem and it is the first application of the TDCR counting
Electronic supplementary material The online version of this
article (doi:10.1007/s10967-017-5451-3) contains supplementary method in Bulgaria. In addition, the development of a
material, which is available to authorized users. primary TDCR standardization method in Bulgaria is
necessary, because of the wide usage of the liquid scintil-
& K. Mitev
[email protected] lation counting (LSC) technique in various fields and to
address the needs of the radionuclide metrology.
1
Faculty of Physics, Sofia University ‘‘St. Kliment Ohridski’’, The objective of this work is to present the design and
5 James Bourchier Blvd, 1164 Sofia, Bulgaria validation tests of a miniature TDCR counting system
2
CEA, LIST, Laboratoire National Henri Becquerel, LNE- developed at the Sofia University ‘‘St. Kliment Ohridski’’,
LNHB, 91191 Gif-sur-Yvette, France Bulgaria. The system (hereafter referred to as TDCR-SU)
3
LABZY, LLC, Santa Fe, NM, USA was developed for absolute activity measurements of beta-
4
Division of Ionizing Radiation, National Institute of or alpha- emitters in liquid scintillation (LS) cocktails. It
Metrology, Beijing 100029, People’s Republic of China consists of a miniature TDCR counter equipped with
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Fig. 1 The TDCR-SU system
dedicated, innovative front-end electronics module (here- relatively low supply voltage (?850 V) [5]. The three
after referred to as the nanoTDCR module). In this work, PMTs, which are denoted as ‘‘A’’, ‘‘B’’ and ‘‘C’’, have a
we present the construction of the TDCR counter, the grounded cathode in order to ensure low dark noise [5].
functionality of the novel nanoTDCR electronic counting Differently from the ENEA system, which has a triangular
module and results from validation comparisons with the optical chamber, the TDCR-SU counter has a cylindrical
French primary TDCR counting system at the Laboratoire optical chamber in which the PMTs are fixed at 120 C, but
National Henri Becquerel (LNHB). at a certain distance from the LS vial aiming to achieve a
full solid angle view of the vial (Fig. 2). The optical
chamber is made of Polytetrafluoroethylene (Teflon) and
Experimental the housing is made of Polyoxymethylene (POM). The
assembly of the TDCR-SU system is illustrated in Fig. 3.
The TDCR-SU system consists of an optical chamber, an The LS vial is inserted manually in the counter from the lid
FPGA-based counting module, a high voltage power sup- on the top.
ply, and a portable computer (Fig. 1). The system is highly
compact and transportable. The major parts of the system, The nanoTDCR electronic counting module
namely the TDCR counter and the nanoTDCR module are
described hereafter. The nanoTDCR electronic counting module is a standalone
FPGA-based device dedicated to TDCR measurements (see
The TDCR-SU counter Fig. 1). It is a scientific development of the labZY com-
pany [6] and is currently a commercial product of this
The design of the TDCR-SU counter was inspired by the company. It has fast input amplifiers (50 X adapted) and
ENEA portable TDCR system [5]. Similarly to that system, can be connected directly to the PMT’s anodes. It has fast
the TDCR-SU counter is equipped with three Hamamatsu discriminators, software-adjustable thresholds, stable refer-
R7600U-200 square photomultiplier tubes (PMTs), which ence voltage and MCA spectra for threshold adjustment
have small dimensions (30 9 30 mm2), wide spectral and radionuclide verification. The nanoTDCR module has
response (300–600 nm), high quantum efficiency and an external output of the master FPGA clock to allow
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Fig. 2 Cross-sectional front a and top b views of the TDCR-SU counter
Fig. 3 Assembly of the TDCR-SU counter: a the optical chamber, b the housing, c mounting of the optical chamber in the housing, d the
assembled TDCR-SU counter
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traceability to the International System of units (SI) of the coincidence windows and to acquire a spectrum, a TDCR
measured counting rates. The nanoTDCR weighs 135 g counter equipped with one nanoTDCR module is able to
and is housed in a very compact enclosure measuring carry out measurements in an equivalent mode of four
92 9 38 9 25 mm3. MAC3 measurements and also additional measurement for
By design, the nanoTDCR module has similar func- spectrum acquisition. Moreover, the nanoTDCR module
tionality as the MAC3 TDCR counting module [7], but it can perform consecutive/repetitive runs of fixed real or live
also has some distinctive features and additional capabili- time with fixed 30 ls gap between each run. The module is
ties such as: controlled by a software developed by labZY. The software
is capable of obtaining UTC from NTP servers with stan-
• Individual extended-type dead-time in each channel
dard metrology grade NTP accuracy in the range from 30
instead of one common dead time, as in the MAC3
to 50 ms. Thus, each nanoTDCR measurement has an
module;
accurate timestamp indicating the start of the measurement.
• Simultaneous counting with two different dead time
The functionality of the software and its graphical user
extensions (software selectable from 80 ns to 500 ls);
interface (GUI) are shown in Fig. 4. A detailed description
• Simultaneous counting with two different coincidence
of the algorithms and the principle of operation of the
windows (software selectable from 8 to 190 ns);
nanoTDCR module are beyond the scope of this work and
• Live-time clocks in each channel (single and coinci-
will be given elsewhere. The Supplementary information to
dent) for each coincidence window and each dead-time
this paper contains more detailed description of:
extension;
• Counters (pulses and associated live-time clocks) for A, • the functionality of the GUI of the nanoTDCR
B, C, AB, BC, AC, D and T for each coincidence software;
window and each dead-time extension; • the structure of the TDCR data file generated by the
• Online checksum calculation: nanoTDCR software. In this file the settings and the
AB ? BC ? AC = 2T ? D; TDCR measurements are recorded;
• Capability of simultaneous TDCR counting and spec- • the web-accessible database, which was developed for
trum acquisition from a PMT. storage, filtering and exporting data from the TDCR
files. The database is intended to facilitate the TDCR
Thanks to its capability to perform counting simulta-
analysis and activity calculations for a large number of
neously by setting two dead-time extensions, two
TDCR measurements.
Fig. 4 The GUI of the labZY nanoTDCR software
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Results and discussion with the nanoTDCR with low, optimal and high thresholds.
Based on the results from the performed studies, the
The evaluation of the performance of the TDCR-SU sys- determined optimal thresholds are 3.6, 4.0 and 4.0 mV for
tem is done by comparison to the primary TDCR counter the PMTs A, B and C, respectively.
(RCTD1) at LNHB. The correct operation of the
nanoTDCR module is first verified by comparison with the
MAC3 TDCR module. The thresholds of the PMTs of the
TDCR-SU counter are then set in the valley between the
single photon peak and the noise peak using the
nanoTDCR MCA functionality. The entire TDCR-SU
system is then benchmarked against the LNHB’s RCTD1
system by TDCR counting and analysis of 241Am, 3H, 14C
and 63Ni sources.
Evaluation of the performance of the nanoTDCR
counting module
As a preliminary test, the nanoTDCR counting module was
first compared to the MAC3 counting module, using the
RCTD1 counter. The logical outputs of the constant frac-
tion discriminators of the RCTD1 system were connected
to the nanoTDCR inputs and simultaneous counting with
the MAC3 and nanoTDCR units was performed. Four
241
Am samples with Ultima GoldTM with activities in the
480–4600 Bq interval were used. A comparison of the
obtained results is given in Table 1, showing a good
agreement between the MAC3 and nanoTDCR counting
results. The differences are smaller than 0.3% and can be
attributed to the different live times of the two systems.
Adjustment of the thresholds of the TDCR-SU
system
The proper operation of a TDCR counting system requires
the precise adjustment of the thresholds in the valley
between the noise peak and the single electron peak (SEP)
observed in each channel. In this work the adjustment was
performed using the MCA functionality of the nanoTDCR
module. The PMTs were operated at ?850 V anode volt-
age and the SEP spectra were acquired without any source Fig. 5 Single photon spectra of PMT B of the TDCR-SU counter
in the counter. Figure 5 depicts the SEP spectra acquired acquired with low (a), optimal (b) and high (c) thresholds
Table 1 Comparison between the MAC3 and nanoTDCR coincidence counting rates
RCTD1 with Coincidences AB, s-1 Coincidences BC, s-1 Coincidences AC, s-1 Coincidences ABC, s-1
source
MAC3 NanoTDCR D (%) MAC3 NanoTDCR D (%) MAC3 NanoTDCR D (%) MAC3 NanoTDCR D (%)
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Am-No1 490 490.5 -0.11 490 490.2 -0.04 490 490.2 -0.03 490 490.0 0.00
241
Am-No 2 1517 1519.7 -0.18 1516 1519.4 -0.22 1516 1519.3 -0.22 1516 1519.1 -0.21
241
Am-No 3 2557 2563.0 -0.23 2557 2562.6 -0.22 2557 2562.6 -0.22 2557 2562.3 -0.21
241
Am-No 4 4604 4599.7 0.09 4604 4599.4 0.10 4604 4598.8 0.11 4604 4599.1 0.11
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Comparison between the RCDT1 and TDCR-SU performance of the TDCR-SU system in the case of 63Ni
systems will be studied in the future with measurements with very
low counting uncertainties in order to reduce random
The second part of the comparison was performed with the fluctuations and to study the influence of the 63Ni beta-
four 241Am sources mentioned earlier. The sources were spectrum.
measured on the RCTD1 system and then on the TDCR-SU The LNHB’s primary TDCR system RCTD1 is equip-
system for 10 min counting time. The results are shown in ped with BURLE 8850 PMTs which are cylindrical with a
Table 2. Taking into account the statistical uncertainties of 51 mm diameter photocathode. The TDCR-SU system is
the measurement, there is an excellent agreement between equipped with Hamamatsu R7600U-200 PMTs, which are
RCTD1 and TDCR-SU for sources No 1 and 2, good 30 9 30 mm square PMTs. The two systems have different
agreement for source No 3 and a satisfactory agreement for optical chambers. It is therefore particularly interesting to
source No 4. The differences between the two counting compare the two systems in terms of the counting effi-
systems are smaller than 0.3% and do not show a sys- ciency for the logical sum of the double coincidences (D).
tematic trend, which indicates a linear response of the The comparison was performed with three sources: 3H in
TDCR-SU system for counting rates in the interval toluene- based LSC, 14C in toluene-based LSC and 63Ni in
480–4600 s-1. Ultima Gold AB. The results of the comparison are shown
In the third test the performance of the TDCR-SU in Table 4 and they indicate lower efficiency of the TDCR-
counter was compared to the performance of the LNHB’s SU system with respect to the LNHB TDCR one. The
RCTD1 counter by primary TDCR measurements of 3H, differences increase with the decrease of the maximum
14
C and 63Ni sources (Table 3). The activities of the 3H, energy of the beta- spectrum of the nuclides (Eb,max). The
14
C and 63Ni sources were determined from the measured lower efficiency of the TDCR-SU system compared to the
T/AB, T/AC, T/BC coincidence ratios using the TDCR07c RCDT1 system may be due to: lower light collection of the
program [8]. Same cocktail data and kB values were used TDCR-SU system because of the smaller photocathode or
in the calculations for the RCTD1 and TDCR-SU systems. light loses due to the larger distance of the TDCR-SU
Excellent agreement between the two systems was PMTs from the vial. Nevertheless, based on the estimated
observed for the 3H and 14C sources within the estimated counting efficiency of the TDCR-SU for the logical sum of
uncertainties. The agreement for the 63Ni source is not as double coincidences (eD), the TDCR-SU system demon-
good as for the two previous radionuclides, due to the low strates excellent performance as an ultra-compact and
counting statistics, but the results are still compatible if portable TDCR counting system.
expanded uncertainties (k = 2) are considered. The
Table 2 Comparison between the RCTD1 and TDCR-SU counting systems
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Am Logical sum of the net double coincidences (D), s-1 Net triple coincidences (T), s-1 Ratio T/D
RCTD1 TDCR-SU D (%) RCTD1 TDCR-SU D (%) RCTD1 TDCR-SU D (%)
No 1 487.0 (9) 486.4 (9) 0.12 487.0 (9) 486.1 (9) 0.18 1.0000 0.9994 0.06
No 2 1513.0 (16) 1515.2 (16) -0.15 1513.0 (16) 1514.1 (16) -0.07 1.0000 0.9993 0.07
No 3 2553.0 (21) 2559.5 (21) -0.25 2554.0 (21) 2557.6 (21) -0.14 1.0004 0.9992 0.11
No 4 4600.0 (28) 4591.2 (28) 0.19 4601.0 (28) 4588.0 (28) 0.28 1.0002 0.9993 0.09
The estimated statistical uncertainties of D and T are given for k = 1
Table 3 Comparison between the RCTD1 and TDCR-SU TDCR activity measurements for 3H, 14
C and 63
Ni sources
ASU
Source Activity measured by RCTD1, LNHB, Bq Activity measured by TDCR-SU, Bq D ¼ ARCTD1
A RCTD1
3
H in toluene-based LS cocktail 1010.7 (2.1) [0.21%] 1010.9 (5.1) [0.50%] -0.02%
14
C in toluene-based LS cocktail 1728.2 (2.4) [0.14%] 1731.3 (4.7) [0.27%] -0.18%
63
Ni in Ultima Gold AB LS cocktail 1325.9 (4.1) [0.31%] 1313.9 (4.9) [0.37%] 0.91%
The values in the brackets indicate the estimated standard uncertainty (k = 1) and those in the square brackets the estimated relative uncertainty
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Table 4 Comparison between the RCTD1 and TDCR-SU counting efficiencies for the logical sum of double coincidences
eD;RCTD1 eSU
Nuclide Eb,max, keV Counting efficiency for logical sum of double coincidences (eD) D¼ eD;RCTD1
RCTD1, LNHB TDCR-SU
3
H 18.564 (3) 0.6982 0.5671 18.8%
63
Ni 66.980 (15) 0.7965 0.7058 11.4%
14
C 156.476 (4) 0.9634 0.9510 1.29%
Conclusions References
A novel, miniature TDCR counting system was developed 1. Malonda G, Carles G, L’Annunziata M (2012) Handbook of
radioactivity analysis, vol 3. Academic Press, Amsterdam
at the Faculty of Physics of Sofia University (Bulgaria) and 2. Broda R, Cassette P, Kossert K (2007) Radionuclide metrology
validated thanks to a comparison with the TDCR LNHB using liquid scintillation counting. Metrologia 44:S36–S52
counter. A new acquisition module and acquisition soft- 3. Cassette P, Capogni M, Johansson L, Kossert K, Nähle O, Sephton
ware for TDCR counting were developed. The nanoTDCR J, De Felice P (2013) Development of portable liquid scintillation
counters for on-site primary measurement of radionuclides using
module offers variety of useful new features and allows the triple-to-double coincidence ratio method. In: Proceedings of
performing TDCR measurements with traceability to time the 3rd International Conference on Advancements in Nuclear
and frequency units. Instrumentation, Measurement Methods and their Applications
The performance of the TDCR-SU counting system was (ANIMMA), Marseille, 2013, doi 10.1109/ANIMMA.2013.
6727876
benchmarked against the LNHB’s primary TDCR system 4. Donatiello S, Capogni M, De Felice P, Cannatà V, D’Arienzo M,
for activity measurements of 241Am, 3H, 14C and 63Ni Strigari L, Tapner M (2016) Absolute measurement in situ of the
90
sources. Good agreement was observed between the results Y activity in liquid solution by TDCR method and calibration of
of the two measurement systems. an ionization chamber. Phys Med 32:e104
5. Capogni M, De Felice P (2014) A prototype of a portable TDCR
All in all, the new TDCR-SU counting system exhibits a system at ENEA. Appl Radiat Isot 93:45–51
good performance in particular due to its low weight and 6. Triple-to-double coincidence ratio liquid scintillation counting
compactness and its extended possibilities for detector system (TDCR) and MCA, http://www.labzy.com/index.html#na
adjustments and data acquisition. It could be used as noTDCR. Accessed 24 May 2017
7. Bouchard J, Cassette P (2000) MAC3: an electronic module for the
portable instrument for on-site measurements, e.g. for very processing of pulses delivered by a three photomultiplier liquid
short-lived radionuclides used in nuclear medicine. scintillation counting system. Appl Radiat Isot 52:669–672
8. Detection efficiency calculation for pure-beta radionuclides,
Acknowledgements This work is supported by the Bulgarian LNHB program with short tutorial, 2012 version, TDCR07c.zip:
National Science Fund under Contract DFNI T02/13’’POLYRAD’’. http://www.nucleide.org/ICRM_LSCWG/icrmsoftware.htm.
The authors are indebted to Mr. Nikolay Markov and Mr. Todor Accessed 24 May 2017
Todorov for the mechanical work on the TDCR counter, which was
manufactured and assembled in Bulgaria.
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