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NSNI 2010

Investigations on 3He Filled Proportional Counters Aimed at Various Neutron Applications


S. S. Desai and A.M. Shaikh Solid State Physics Division, Bhabha Atomic Research Division, Trombay, Mumbai 400085. Email : ssdesai@barc.gov.in

Abstract
Solid State Physics Division is involved in development of gas filled neutron detectors for more than two decades, for various applications such as neutron beam research and area-beam monitoring. These detectors show excellent characteristics and long life and are continuously under modification to suit the specific applications. Developments are aimed at improving the operational stability of detectors in hostile environments like high gamma field and extreme operating temperatures and enhancing life of the detector. Position sensitive detectors (PSD) mounted at neutron scattering instruments around Dhruva and CIRUS have demands of high efficiency, larger dimensions with finer position resolutions and the geometry that intercepts maximum scattered beam. We present the basic characterization of 3He filled detectors supporting the development of wide spectrum of detectors. Performance of He3 filled neutron detectors depends on the additive gases and their concentration. Gas gain and Diethorn gas constants are measured and results are used to design the operating parameters of large area and high pressure detectors. Detector fill gas is optimized for proportional region and low gamma sensitivity. Investigations are carried out on 3He filled neutron detectors with additive gases with low photon absorption cross section CF4 and CO2. Detector with CO2 as additive gas shows good gamma discrimination up to flux of 8 R/hr. These investigations are also used to design high efficiency and high resolution PSDs. Newly assembled 15 PSDs in a stack of 3 layers show the gain in efficiency of 600 % and improvement in resolution by 2 mm.

Introduction
He filled proportional counters for high efficiency thermal neutron detection have numerous applications in neutron scattering, monitoring and study of fissile materials. Our group at SSPD is involved in development of gas filled neutron detectors for more than two decades, for various applications as neutron beam research and area-beam monitoring. These detectors show excellent characteristics and life of detectors over 20 years. Detector development technology is continuously under modification, in order to suit the specific applications. Developments are aimed at improving the operational stability of detectors operated in hostile environments like high gamma field and extreme operating temperatures and enhancing life of the detector. Position sensitive detectors (PSD) mounted at neutron scattering instruments around Dhruva and CIRUS reactors make these instruments self sufficient through the in-house development. The demands on PSDs are for high efficiency, larger dimensions with finer position resolutions and the geometry that intercepts maximum scattered beam. It enables to use very precious neutron judicially and reduce the experimental beam time. We present the basic characterization of 3He filled detectors supporting the development of detectors for various applications.
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Gamma sensitivity arising from the additive gases limits its application in high gamma environment [1]. BF3 detectors are comparatively better, but show lower efficiency. In such conditions, proper gas combination and concentration can be optimized for 3He detectors, to minimize gamma sensitivity, maintaining the proportional region.

Gas amplification factor


Proportional region of the detector is well defined on the basis of gas gain characteristics and Diethorn curve [2]. The electron multiplication is a complex process, which depends on many factors such as electric field gradient, anode and cathode radius, detector capacitance, gas pressure, gas composition, gas purity, electronegative gases and non-ionizing processes involved during the collisions. For X-ray detectors applications are towards the energy spectroscopy. Linear calibration graph of pulse height with incident energy should show a good dynamic range over the X-ray photon energy under investigation. Whereas, neutron detectors based on neutron capture reaction of 3He and BF3 are widely used for counting application and not for spectroscopic applications. In spite of integrated counting applications, it is important to operate these detectors in proportional region. The choice of fill gas and gas pressure is needed to maintain considerable range of proportional region. The detector meant for counting application needs to show good
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He is available in pure gas form and detector with perfect geometry shows good pulse height resolution.
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NSNI 2010

energy resolutions at the 764 keV and 2.31 MeV as the Q energies of the neutron capture reactions and maximum number of full energy events with minimum wall effects. For a given amplification settings, plateau characteristics gives the information of counting changes between the pulse height ranging from lower level discrimination to upper level discrimination. These measurements may not be strictly in the proportional region. Whereas the plateau measurements within the proportional region show better length and slope. Hence it is important to choose the operating voltage of a detector on the basis of gas gain curve. Operation of detectors for counting applications at lower gas gain increases the life of the detector

Fig 1. Gas gain curves for various neutron detectors

Gas gain curves for various gases


Gas gain M [3] is measured using the equation (1) Where X is the full energy of 10B (n, ) or 3He (n, p) reaction as per the fill gas used; the values are 2.31 MeV and 0.764 MeV respectively, v is the preamplifier output, Cf is the feed back capacitance of the preamplifier, e is the electron charge: and W, the average energy required to form an ion pair. Measurements are taken on number of detectors with similar geometry to check reproducibility of the results. The various gases used in the measurements are high purity gases: BF3 with 90% 10B-enrichment, 3He 99.95% with tritium 1 x 1011 %, Ar, Kr, CF4 iC4H10 and CO2 with purity ranging from 99.998 to 99.9%. The gas mixture in 3He detectors is in 2:1 proportion. Thermal neutrons from a Pu-Be source are used for all the neutron detector measurements. Diethorn derived following expression (eqn. 1) for M for gas filled proportional counters. (2)

Fig 2 Diethorn plot of the data shown in Fig 1 for various neutron proportional counter gases

Table 1 Diethorn constants for detector fill gases


Gas/ Gas W (V/ion Intercept Slope K x 104 V (eV) mixture pair) (Volts)-1 (Volts)-1 V/cmbar
3 3

He+Kr

30.67 30.81 32.90 35.50

0.177(6) 0.0201(6) 34.5(9) 0.675(35) 0.157(9) 0.0182(4) 38.7(16) 0.560(19 0.173(8) 0.0178(8) 39.0(17) 1.720(19) 0.168(9) 0.0153(7) 45.6(39) 5.593(71)

He+Ar+ CO2 He+CF4 BF3

The gas gain as a function of applied anode voltage V, for different gas mixtures, electrode dimensions and pressures are shown in Figure 1. It can be seen from the graph that the gas gain (M) is an exponential function of the applied voltage in the whole range of 10 < M < 103. It is not desirable to have gain measurements below 10, as fluctuations in avalanche affect the signal to noise ratio significantly. The upper limit in M depends on electrostatic capacitance of the detector, input capacitance of the preamplifier and size of the primary charge cloud.

approximate errors obtained from uncertainties in the slopes and intercepts by error analysis. Among the 3He filled counters for a given size, the one filled with Ar+CO2 operates at lower anode voltage compared to that with Kr or CF4 gas. The operating voltage in CF4 added 3He counters is highest CF4 being a polyatomic molecule has number of low lying excitation, vibrational and rotational levels, and its addition to noble gases increases the field required, hence the operating voltage to reach similar gains. The values of Diethorn gas constants can be used for design of detector with any dimensions and geometry and the corresponding operating parameters are estimated and values are found within 5 % of the anode bias value.
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Fig 2 shows the Diethorn plot for the same detectors as in Fig 1 and carries the same symbols. The values of V and K are listed in table 2 along with the

NSNI 2010

Gamma sensitivity and choice of additive gases


The type of gas and optimum concentration is determined for high gamma field operation on the basis

Fig 4 Gas gain characteristics for various concentrations of CO2

Table 2 Diethorn constants for various CO2 %


Fig 3. Photon absorption cross-sections for additive gases as a function of incident photon energies. Gas combination CO2 % in 4 bar
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of gamma sensitivity. Fig 3 shows the photon absorption cross section calculated for various additive gases [4]. Polyatomic additive gases such as CO2, CF4 and iC4H10 show lower gamma sensitivity as compared to noble gases Ar and Kr. As compared to CO2, iC4H10 shows lower gamma sensitivity, higher stopping power and anode bias. The larger molecular size results in excessive nonionizing events and higher electric field needed is to attain particular gain. However the detectors used for monitoring purpose have portable modules and are not convenient to operate at high anode bias. Thus CO2, which gives a longer proportional region at smaller concentrations, is chosen for investigations in high gamma field. Whereas iC4H10 with high stopping power are used for PSD operated in high gamma field [5]. Neutron detectors with 12 length and 1 (12C-type) brass cathode and 25 m of anode filled with 3He + CO2 at 4 bar fill pressure with variable CO2 concentration of 3%, 5% and 11% are fabricated and tested for their performance using thermal neutrons from Pu-Be source. Gas gain measurements (Fig 4) are carried out using Gaussian fit and pulser gain normalization. Pulse height spectra from all three CO2 concentrations are compared for wall effects and full energy events as mentioned in table 2. Linear proportional region in gas gain plots (Fig. 4) of 300 V, 350 V and 400 V are observed for 3%, 5% and 11% of admix concentrations respectively. Gain values beyond these limit show under-exponential behavior and are excluded from gas constants calculation. V values for all detectors are
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Full energy events % 36.8 42.5 59.7 46.3

Deithorn constants VVolts 19.37 23.03 26.65 23.78 KV/cm/atm 7141.8 8790.3 11025.6 14999.6

He + CO2 (3%) He + CO2 (5%)

3 3 3

He + CO2 (11%)

He + CO2 (LND)

comparable but K value increases with additive and is highest for LND detector. Pulse rise time of all detectors is 0.7 to 1 sec and is faster than Kr filled detectors. Thus count rates up to 105 can be measured without any gamma pile up. Values of gas constants K and V are useful to design detectors of any dimensions.

Gamma tolerance of neutron detectors


Detectors were filled with 3He and stopping gases Kr, CF4 and CO2. Detector with 5 % of CO2 concentration with total fill gas of 4 bar is optimized. Gamma tolerance is performed with variable gamma fields at Multi-source Gamma Exposure Facility, RSSD. In case of CF4, gamma and neutron pulses merged at gamma exposure of 1 R/hr (Fig 5). Kr filled detector show merging of neutron and gamma pulses at the flux of 0.5 R/hr It is observed that detectors filled with 3He + CO2 showed excellent performance till gamma exposure of 8 R/hr (Fig. 6). After long term operations CO2 is expected to degrade to CO and oxygen radical during quenching. The detectors are coated with activated carbon on the inner wall of the cathode. The coating absorbs the oxygen radical and other gas impurities and improves

NSNI 2010 efficiency, but it puts some constraint on casing tolerance and increase in rise time of the pulse. Rise in ballistic deficit deteriorates the position resolution [6]. In this case Kr is used as stopping gas as scanning area is away from direct beam. Thus on optimizing the maximum pressure to 10 bar 3He and 2 bar Kr, detector bank show overall gain of 600% and reduction in data collection time by equivalent factor. The differential position resolution is ~1 mm and integral position resolution is 3-4 mm. In case of PSD to operate in high gamma flux, iC4H10 is chosen as per Fig 3. The detectors filled with 3He + iC4H10 at total pressure 3 bar and various isobutane concentrations are studied for performance. 20 % isobutane is optimized as per the gas gain curve linear region and pulse spread. Charge centroid spread (Rp+Rt) equal to 1.6 mm [7] Operating voltage for 1-D PSD to attain the gas gain of 500 is estimated from values of Diethorn gas constants as 2360 V and the measured value is 2410 V, which is within 3% error of the calculated value. Gamma discrimination for the 20% of gas mixture is better than that obtained for equivalent Kr gas mixture.

Fig 5 Pulse height spectra of detector (3He + CF4) with neutron and variable gamma exposure

Acknowledgement
Authors like to express gratitude to Head RSSD and the staff members for making available Multi source gamma exposure facility.
Fig 6. Pulse height spectra of detector (3He + CO2) at 4 bar pressure with neutron and variable gamma exposure

References
1. 2. 3. 4. 5. 6. 7. T. E. Valentine, N. W. Hill, J. A. Williams, V. C. Miller, Report ORNL/TM-1999/239-Sept 1999. W. Diethorn, NYO-6628 (1956) as in Radiation Detection and Measurement, G.F. Knoll 1989), p 170. S. S. Desai and A. M. Shaikh, Journal of Neutron Research, Vol. no. 14 June 2006, 121-129. http://physics.nist.gov/xcom. [2005] S. S. Desai, A. M. Shaikh Nucl. Instru. Meth.A 557 (2006) 607 S. S. Desai, A. M. Shaikh, Rev. Sci. Instrum.78, (2007) 023304. L.C Northcliffe and R. F. Schilling Nucl. Data Tables, A7 (1970) 233

the gamma tolerance. It can act as getter and increase the life of detector even after the continuous operation in high field.

Optimization of fill gas for PSD


The powder Diffractometer and Hi-Q Diffractometer at Dhruva reactor scan scattering angles in the range 3 to 140 and make use of five identical (PSDs). In order to improve the overall throughput of these spectrometers, up gradation to bank of 15 high efficiency and high-resolution PSD is carried out. Rise in 3He pressure improves the

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