Radiation Protection Dosimetry Advance Access published May 4, Radiation Protection Dosimetry (2015), pp. 1 5

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Radiat Protect osimetry Advance Access published May 4, 2015 Radiat Protect osimetry (2015), pp. 1 5 doi:10.1093/rpd/ncv293 EQUIVALENCE OF PURE PROPANE AN PROPANE TE GASES FOR MICROOSIMETRIC MEASUREMENTS S. Chiriotti 1,2,3, *,. Moro 3, P. Colautti 3, V. Conte 3 and B. Grosswendt 4 1 Belgian Nuclear Research Centre, SCK CEN, Mol, Belgium 2 Center of Molecular Imaging, Radiotherapy and Oncology, Institut de Recherche Expérimentale et Clinique, Université catholique de Louvain (UCL), Brussels, Belgium 3 Laboratori Nazali di Legnaro, INFN-LNL, Legnaro, Italy 4 Guest at LNL-INFN, Legnaro, Italy *Corresponding author: scalvare@sckcen.be A tissue-equivalent proportal counter (TEPC) simulates micrometric volumes of tissue if the energy deposited in the counter cavity is the same as that in the tissue volume. Nevertheless, a TEPC measures only the isats created in the gas, which are later converted into imparted energy. Therefore, the equivalence of the simulated diameter (r) in two gases should be based on the equality of the mean number of s pairs in the gas rather than on the imparted energy. Propane-based tissue-equivalent gas is the most commonly used gas mixture at present, but it has the drawback that its composit may change with time. From this point of view, the use of pure propane offers practical advantages: higher gas gain and longer stability. In this work, microdosimetric measurements performed with pure propane, at site sizes 0.05 mg cm 22 r 0.3 mg cm 22, demonstrate that the response of a propane-filled detector in gamma and in neutron fields is almost the same if an appropriate gas density is used. INTROUCTION In microdosimetry, tissue-equivalent proportal counters (TEPCs) are commonly assumed to measure the distribut of energy imparted in micrometric volumes of tissue when irradiated by ising radiat. To achieve this aim, at least the elemental composit of the walls and the filling gas of a TEPC should be as close as possible to that of tissue. In this respect, propane-based tissue-equivalent (C 3 H 8 TE) gas (1) is generally accepted as a good approximat for the elemental composit of tissue and represents at present the most frequently used filling gas of TEPCs. Particularly in sealed TEPCs, the drawback of using gas mixtures is due to the fact that the composit of the filling gas may change with time due to a different absorpt of the gas mixture components with the detector walls. From this point of view, the use of pure propane as the filling gas of a sealed TEPC offers practical advantages: (1) the composit of the filling gas is more stable on long-time operat, and (2) higher gas gains can be reached when compared with the C 3 H 8 2TE gas mixture. The disadvantage of using pure C 3 H 8 gas instead of the C 3 H 8 2TE gas is related to the different atomic composit of C 3 H 8 (mass fracts: 18.3 % H, 81.7 % C) when compared with that of the commonly accepted C 3 H 8 2TE gas mixture (mass fracts: 10.3 % H, 56.9 % C, 3.5 % N, 29.3 % O). Sometimes, in particular for measurements in space environment, the use of pure C 3 H 8 is preferred. It is often considered to have nearly the same response as C 3 H 8 2TE. Therefore, it was the aim of the present article to develop an experimental procedure that can be applied in measurements with C 3 H 8 -filled TEPCs to get a detector response very similar to that of TEPCs filled with the C 3 H 8 2TE gas mixture. ue to the fact that proportal counters measure the charge distribut caused by ising radiat instead of the distribut of energy imparted, the attent of this work was focussed more on the isat cross sects in the two gases rather than on the corresponding stopping powers. MATERIAL EQUIVALENCE In radiat dosimetry, two sites of different materials are considered equivalent if the absorbed dose or the mean imparted energy 1 to each site are equal. Applying this principle to the sensitive volume of a TEPC filled either with the C 3 H 8 2TE gas mixture or with pure C 3 H 8 requires that the mean energy imparted, which is caused by a charged particle (e.g. an electron or a proton) when penetrating through the detector volume on one of its diameters, is independent of the filling gas. If the secondary electrons are completely absorbed inside the detect volume, the material equivalence can be expressed by the following equat: ðs=rþ C3H8 ðrþ C3H8 ¼ðS=rÞ C3H8 TE ðrþ C3H8 TE ð1þ Here, ðs=rþ C3H8 TE and ðs=rþ C3H8 are the mass collis stopping powers of the primary particle in the C 3 H 8 2TE and in pure C 3 H 8 gases, respectively; ðrþ C 3 H 8 TE and ðrþ C 3 H 8 are the masses per area of # The Author 2015. Published by Oxford University Press. All rights reserved. For Permisss, please email: journals.permisss@oup.com

S. CHIRIOTTI ETAL. the site diameter in the two different gases and r is the To give an impress of the differences in generating corresponding gas density. Equat (1) is valid only primary isats in pure C 3 H 8 and in the for particles that have ranges markedly larger than the C 3 H 82 TE gas mixture, Figure 1 shows the mean free target size. If the mass stopping powers are the same isat path lengths ðlrþ C3H8 and ðlrþ C3H8 TE for in the two gases for all primary particle types and energies, electrons and protons as a funct of the particle the site sizes of the two filling gases expressed in mass per area would be the same. In view of the different atomic composits of the two filling gases, however, the mass stopping power energy E. For a detailed descript of the calculat of isat path lengths for electrons and protons in C 3 H 8 and the C 3 H 8 2TE gases, see Refs. (2,3). At first glance, it can be seen in Figure 1 that for ratio ðs=rþ C 3 H 8 TE =ðs=rþ C 3 H 8 = 1 and depends on particle type and energy. Therefore, the ratio ðlrþ C3H8 TE electrons and protons ðlrþ C3H8 is always smaller than independently of the particle energy. This ðrþ C 3 H 8 =ðrþ C 3 H 8 TE varies in the same way. means that, exposed to the same irradiat field, the In addit to these principle problems in the definit of material equivalence, one should also bear in mind that, instead of the distribut of energy imparted, a TEPC measures the distribut of isats amount of primary isats formed in the detect volume of a TEPC is always greater if pure C 3 H 8 instead of the TE gas mixture is used. Hence, also a higher gas gain can be reached when using C 3 H 8. created in the radiat-sensitive volume of the To be able to estimate the site size ðrþ C3H8 of a counter, which are converted later to a distribut of TEPC filled with pure C 3 H 8, which leads to the same energy imparted using an appropriate calibrat response funct as the TEPC filled with the factor. In view of this fact, the material equivalence of C 3 H 8 2TE gas mixture according to Equat (2), different filling gases of a TEPC should be based more the convers factor ðlrþ C3H8 =ðlrþ C3H8 TE is plotted on the equality of isat distributs rather than in Figure 2 for electrons and protons as a funct of on the equality of the distributs of imparted energy. particle energy E. To define material equivalence based on isats, assume that single primary particles are pene- ratio ðlrþ C3H8 =ðlrþ C3H8 TE as a funct of energy is As it is obvious from a first glance at Figure 2, the trating through the detect volume of a TEPC on smaller and less dependent on energy than the corresponding ratio of (S/r), in particular for the protons. one of its diameters. If the range of the primary particles is markedly longer than the diameter of the gas cavity, the mean number of primary isats caused by a particle inside the detect volume is given by the ratio ðrþ=ðlrþ, where (r) is the mass per area of the particle s track length within the target and ðlrþ is the mass per area of the mean free path length with respect to primary isat. ðlrþ is proportal to the reciprocal of the isat cross sect of the target material and depends on the type and energy of ising particles. TEPCs filled with pure C 3 H 8 havethesameresponse funct as TEPCs filled with the C 3 H 8 2TE if the measured isat spectra are the same for the same radiat field. This means that, at least, the number of primary isats must be the same: ðrþ C3H8 ðlrþ C3H8 ¼ ðrþc3h8 TE ðlrþ C3H8 TE ð2þ Here, ðlrþ C3H8 and ðlrþ C3H8 TE are the masses per area of the mean free isat path lengths for C 3 H 8 and the C 3 H 8 2TE gas mixture. Equat (2) shows the same structure as Equat (1) with (S/r) exchanged by the reciprocal of ðlrþ,andthediscuss of Equat (1) is also valid for Equat (2). Therefore, the mass per area ðrþ C 3 H 8, which is equivalent to ðrþ C 3 H 8 TE, varies as a funct of energy and particle type like ðlrþ C3H8 =ðlrþ C3H8 TE. Page 2 of 5 Figure 1. Primary isat mean free path of electrons (top) and protons (bottom) in C 3 H 8 and C 3 H 8 2TE gases.

EQUIVALENCE OF PURE PROPANE AN PROPANE TE GASES Figure 2. Ratio ðlrþ C3H8 In addit, it is almost the same for electrons in the energy range between 1 and 10 3 kev and for protons at energies between 10 and 10 5 kev. A similar response of the TEPC is therefore expected if propane is set to a lower gas density with respect to the TE gas, according to the ðlrþ ratio, which is between 0.75 and 0.8. Ideally, the number of measured isats should be the same for the whole energy spectrum of incoming particles, in particular in the proton-edge reg, which is often used for calibrat. The number of isats produced by protons at the p-edge can be expressed as N gas ðrgas Þ¼y gas ðrgas Þ l=w gas Here, y gas is the corresponding lineal energy calculated from the energy range tables published by Internatal Commiss on Radiat Units (ICRU) (4), W is the mean energy required to form an pair by protons (6) in a given gas and l is the mean chord length of the cavity. In Figure 3 (top), the number of isats for the two gases, N C3H8 N C3H8 TE =ðlrþ C3H8 TE for electrons (top) and protons (bottom). (S/r) for protons are taken from Ref. (4) and (S/r) for electrons from Ref. (5). and, is plotted as a funct of the site size r. ue to the shorter isat mean free path length in propane, N C3H8. NC3H8 TE. In order to have N C3H8 ¼ NC3H8 TE, the density of propane must be reduced. If the N C3H8 data are shifted to larger values of r by a factor of (0.75) 21, they perfectly agree with the N C3H8 TE data. For instance, in pure propane at ðrþ C3H8 ¼ 0:075 mg cm 2, N C3H8 ¼ 3373 is obtained, which is almost the same as N C3H8 TE ¼ 3375 at ðrþ C3H8 TE ¼ 0:1mgcm 2. Figure 3. N p-edge in C 3 H 8 2TE (line) and C 3 H 8 (symbols) as a funct of mass per area r (top) and as a funct of equivalent site size d at density r ¼ 1gcm 23 (bottom). In order to have the same number of isats N p-edge in both gases, the gas density of pure C 3 H 8 must be reduced by a factor of 0.75 when compared with the gas density of C 3 H 8 2TE. Consequently, to get the same equivalent site size d, the following equats are used: d ¼ ðrþc3h8 TE ð1gcm 3 Þ ; d ¼ ðrþ C3H8 0:75 ð1gcm 3 Þ ð3þ If plotted as a funct of d, the number of isats in the two gases is almost the same (bottom Figure 3). MATERIALS AN METHOS The measurements were performed at INFN-LNL using a spherical TEPC with an internal diameter of 5 cm, an anode diameter of 100 mm and 3-mm-thick walls made of tissue-equivalent plastic (A-150). The TEPC was filled either with pure C 3 H 8 gas or with the C 3 H 8 2TE gas mixture. The mass per area of the cavity diameter r was varied between 0.05 and 0.3 mg cm 22 by changing the gas density. To study the detector response for low linear energy transfer (LET) fields, the TEPC was exposed to a 137 Cs g-source, whereas for high-let fields, it was exposed to fast neutrons, 0.58 MeV in mean energy, produced from the 8 Be(p,n) react by bombarding a thick beryllium target with 3 MeV protons at the CN Van de Graaff accelerator of LNL. For both filling gases, the microdosimetric spectra for the 137 Cs and the neutron fields were collected at 10 different gas densities, giving a total of 40 spectra. At each density, the neutron and photon spectra were measured in the same working condits of the TEPC. Page 3 of 5

S. CHIRIOTTI ETAL. Figure 4. 137 Cs (left) and neutron microdosimetric spectra measured at d ¼ 2 mm: C 3 H 8 2TE (line) and C 3 H 8 (circles). The neutron spectra for both gases were calibrated using the proton edge, by applying the technique discussed in detail by Conte et al. (7). The most precise marker point (h TC ) is given by the intercept of the tangent through the inflect point of the fitted Fermi funct with the abscissa. The lineal energy values at the p-edge, y ðdþ, were calculated using the energy range tables published by ICRU (4) for the TE gas mixture. Afterwards, they were assigned to the marker h TC. For each density, the same calibrat factor was applied to the 137 Cs spectrum. To give an example, the neutron spectra measured in the two gases, at ðrþ C3H8 ¼ 0:075 mg cm 2 in propane and at ðrþ C3H8 TE ¼ 0:1mgcm 2 in the TE gas, were calibrated, according to Equat (3), using y ð1 mmþ for the TE gas mixture. RESULTS AN ISCUSSION To give an impress of the results, Figure 4 shows the microdosimetric spectra for 137 Cs on the left and for 0.58 MeV neutrons on the right at equivalent site size d ¼ 2 mm. A good correspondence in the shape of the spectra is observed with only minor differences in the gamma spectra. A similar good agreement was observed also for the other gas densities. To get an overview of the results in the whole range of site sizes, the dose-mean lineal energy for the gamma component was calculated. As the lower threshold of the spectral distributs was set at the noise level y ¼ 0.4 kev mm 21, this dose-mean lineal energy was indicated as y þ. Figure 5 shows y þ in pure propane (spheres) and in the TE gas mixture (squares) as a funct of the equivalent site size d: the agreement between the y þ for propane and for the TE gas as a funct of the equivalent site size d is almost perfect within the estimated type A standard uncertainties of 1.5 %. Within these uncertainties, the experimental data can be described by a power funct of d (the straight lines in Figure 5. ose-mean lineal energy y þ for 137 Cs as a funct of the equivalent site size d for C 3 H 8 (circles) and C 3 H 8 2TE (squares). For details, see the text. the figure). The y þ in propane obtained without taking into account the 0.75 factor in Equat (3) is also shown (open circles). In this case, an underestimat between 5 and 10 % clearly demonstrates the improvement by using the 0.75 factor. CONCLUSIONS The aim of this work was to investigate how different is the response of a TEPC filled with pure C 3 H 8 instead of the common C 3 H 8 2TE gas, in gamma and neutron fields. The comparison of the microdosimetric spectra for 137 Cs and neutron fields, in the equivalent diameter range investigated in this study, confirms that the C 3 H 8 -filled TEPC has almost the same response funct as the C 3 H 8 2TE-filled detector if the mass per area in pure C 3 H 8 is reduced by a factor of 0.75 when compared with C 3 H 8 2TE. By applying this factor, pure propane gas can be used as a substitute of the TE gas mixture. The microdosimetric spectra are almost the same, and the derived dose-mean lineal energies do not differ significantly, within the estimated uncertainty of 1.5 %. The applicability of Equat (3) in mixed fields and higher neutron energies is under investigat. FUNING This work is supported by the Fifth Scientific Commiss of the Istituto Nazale di Fisica Nucleare (INFN) of Italy. REFERENCES 1. Internatal Commiss on Radiat Units and Measurements. Microdosimetry. ICRU Report 36 (1983). 2. e Nardo, L., Colautti, P., Conte, V., Baek, W. Y., Grosswendt, B. and Tornielli, G. Ionizat-cluster distributs of a-particles in nanometric volumes of propane: Page 4 of 5

EQUIVALENCE OF PURE PROPANE AN PROPANE TE GASES measurement and calculat. Radiat. Environ. Biophys. 41, 235 256 (2002). 3. Grosswendt, B. Format of izat clusters in nanometric structures of propane-based tissue-equivalent gas or liquid water by electrons and a-particles. Radiat. Environ. Biophys. 41, 103 112 (2002). 4. Internatal Commiss on Radiat Units and Measurements. Stopping Powers and Ranges for Protons and Alpha Particles. ICRU Report 49 (1993). 5. Salvat, F., Fernández-Varea, J. and Sempau, J. PENELOPE 2011: A Code System for Monte Carlo Simulat of Electron and Photon Transport. OEC Nuclear Energy Agency (2011). 6.Baek,W.,Grosswendt,B.andWillems,G.W Values of protons in alkane-based TE gases and dimethylether in the energy range 1 to 100 kev: measurements and additivity models. Radiat. Prot. osim. 110, 61 68 (2004). 7. Conte, V., Moro,., Grosswendt, B. and Colautti, P. Lineal Energy Calibrat of Mini Tissue Equivalent Gas- Proportal Counters (TEPC). AIP Conf. Proc. 1530, 171 178 (2013). Page 5 of 5