ARTICLE IN PRESS

Radiation Physics and Chemistry 76 (2007) 15071510 www.elsevier.com/locate/radphyschem

Preliminary results from a polymer gel dosimeter for absorbed dose imaging in radiotherapy
M. Mariania, E. Vanossia,b, G. Gambarinib,c,, M. Carrarad, M. Valenteb,c
a

Dipartimento di Ingegneria Nucleare, Politecnico di Milano, Via Ponzio 34/3, 20133 Milano, Italy b INFN-Istituto Nazionale di Fisica Nucleare, Via Celoria 16, 20133 Milano, Italy c ` di Milano, Via Celoria 16, 20133 Milano, Italy Dipartimento di Fisica, Universita d ` di Fisica Sanitaria, Istituto Nazionale dei Tumori, Via Venezian 1, 20133 Milano, Italy Unita

Abstract The reliability for radiotherapy applications of a normoxic-polymer gel dosimeter, analysed by means of optical methods, was studied. The optical transmittance was measured with a spectrophotometer and imaged with a CCD camera. The characteristics of sensitivity, spatial resolution, image stability, linearity of the response and reproducibility were investigated and analysed. Radiation induces a radical polymerisation in the gel matrix and the resulting macromolecules remain xed in space making therefore possible the absorbed dose imaging. r 2007 Elsevier Ltd. All rights reserved.
Keywords: Gel dosimetry; Dose imaging; Polymer gel

1. Introduction The recent developments in radiotherapy techniques allow to obtain a local energy release in tumours saving the surrounding healthy tissue. Therefore there is the necessity of getting the images of in-phantom absorbed dose, especially when different radiation elds are adopted, achieving high precision and the most reliable resolution. In order to reach high accuracy and good reliability of these techniques, both dosimetric methods and computational tools are suitably developed and improved. Despite the fact that the treatment planning systems are supported by three-dimensional algorithms and that computerised models have achieved considerable level, it is more suitable also to perform experimental measurements in order to obtain physical validations. A technique for dose imaging still in progress and showing great development is the gel dosimetry, based on tissue-equivalent gels in which a chemical dosimeter is
Corresponding author. Dipartimento di Fisica, dellUniversita ` di Milano, Via Celoria 16, 20133 Milano, Italy. Tel.: +39 02 50317243; fax: +39 02 503177630. E-mail address: grazia.gambarini@mi.infn.it (G. Gambarini).

infused. Phantoms made up of such gels act as continuous dosimeters and consequently, the absorbed dose distribution can be imaged along proles, surfaces or phantoms volumes. The scientic community has proposed different kinds of gel dosimeters and several kinds of imaging techniques have also been developed (Maryanski et al., 1994). The two main investigated groups of gel dosimeters are represented by the Fricke-infused and the polymer gels. In the rst system, ionising radiation causes conversion of ferrous ions (Fe2+) to ferric ions (Fe3+) with the oxidation yield proportional to the absorbed dose. Owing to ferric ion diffusion in the aqueous matrix, it is necessary to perform dosimeter analysis at a short time after irradiation. In polymer gels, ionising radiation produces polymerisation, and no diffusive effects seem to take place. This work focuses the study on a polymer gel dosimeter system. As a growing amount of polymer is induced by irradiation at increasing doses, the polymer gel becomes increasingly opaque. This allows the absorbed dose distributions to be visualised and provides the opportunity for evaluation using optical methods. The monomer solution incorporated in the gelatine consists of acrylamide and N ; N 0 -methylene-bysacrylamide monomers, and these

0969-806X/$ - see front matter r 2007 Elsevier Ltd. All rights reserved. doi:10.1016/j.radphyschem.2007.02.080

ARTICLE IN PRESS
1508 M. Mariani et al. / Radiation Physics and Chemistry 76 (2007) 15071510

molecules can be chemically polymerised and cross-linked by irradiation to give a so-called polyacrylamide gel (PAG) (Baldock et al., 1998). The monomer solution contains also an antioxidant playing the role of oxygen scavenger and useful to enable the synthesis and the manufacturing of polymer gel dosimeters under normal atmospheric conditions. These kinds of gels will be referred to as normoxic gel (Fong et al., 2001). The possibility of performing in-phantom dose proling and imaging is of great importance for validating the BNCT (boron neutron capture therapy) treatment planning (Farajollahi et al., 2000). The method, based on gel dosimeters in form of layers for spatial determination of absorbed doses in thermal or epithermal neutron elds, has revealed to be very reliable. In fact, gel dosimeters in form of layer give the possibility not only of obtaining spatial dose distributions, but also, of achieving measurements of each distinctive dose contribution in neutron elds, by means of a properly optimised procedure. The layergeometry gives the advantage of avoiding sensible alteration of neutron transport, even if the elemental gel composition is changed by adding particular isotopes (for example 10B), as necessary to perform the separation of dose contributions (Gambarini et al., 2004). 2. Materials and methods The normoxic gel dosimeter studied in this work is named PAG (polymer acrylamide gelatine) gel and it has the following composition: powder gelatine (type A, 300 bloom, Sigma-Aldrich) in the amount of 4% or 5% or 6% of the nal weight; acrylamide [3% w/w, CH2 CHCONH2 ]; N ; N 0 methylene-bisacrylamide [3% w/w, H2 C CHCONH2 CH2 ]; tetrakis (hydroxymethyl) phosphonium chloride (THP) [2 mM, CH2 OH4 PCl]. Highly puried and deionised water [90% or 89% or 88% w/w, H2O] was utilised for all preparations. Acrylamide and bysacrylamide are the monomers that react giving the polymer; THP is the antioxidant and the gelatine acts as a matrix that xes the molecules. The preparation of the gel starts by pouring into a glass beaker 50% of the total weight of water, then a suitable amount of gelatine is added to the stirred solvent. After the gelatine has swelled from soaking, the mixture is heated at $50 1C to ensure the gelatine is completely dissolved. To another beaker with the remaining amount of stirred water, acrylamide and the N ; N 0 methylene-bisacrylamide are added and the solution heated at $50 1C to ensure the monomers are completely dissolved. At this point the monomer solution is mixed to the gelatine one and the antioxidant is added. The uid, till warm, is used to ll two kinds of containers that are then stored in a refrigerator overnight. The day after the samples are irradiated and the response is studied vs. the absorbed dose. The polymer gel can be analysed in the two different containers: spectrophotometer vials of 1 cm in optical length, and layers of 3 mm in

optical length. The layers are made by two transparent sheets of polystyrene hold to a frame with two small holes to ll, by means of a syringe, the dosimeter solution before its gelling. The optical analyses were performed by an UVVIS spectrophotometer (Lambda EZ210) and a CCD camera (Starlight Xpress SXL8-P), which is a low-noise camera with Peltier thermoelectric cooling, able to capture and digitise high-resolution, 12-bits, images. Dosimeter-gel samples are optically analysed by measuring the visible-light transmittance through gel samples uniformly illuminated. From the grey level (GL) images of the transmitted light, acquired before and after radiation exposure by means of the CCD, the difference in optical density, which is proportional to absorbed dose (Maryanski et al., 1996), was deduced. Polymer gel dosimeters of different shapes were exposed to photon elds of various energies and the light transmittance measured. Reproducibility and linearity studies regarding the normoxic polymer gel were carried out. The polymer gel response was investigated by varying the time between gel preparation and radiation exposure and, also, the time between irradiation and analysis. In-phantom 3D images are realised. The dose proles in the central axis of the phantom were extracted and compared with ionisation chamber measurement. The reliability of dose images and depthdose proles obtained with the gel dosimeters has been investigated by Monte Carlo calculations by means of the program PENELOPE, simulating experimental geometries. The polymer gel was also studied in order to be used for application in BNCT. The gel was analysed with the addition of 10B. As a preliminary test the response of gel dosimeters having both the standard composition and containing a suitable concentration of 10B, was investigated. Gel layers were irradiated in different phantoms exposed to the thermal column of the nuclear reactor TRIGA MARK II (Training Research Isotope Production General Atomic) of the Laboratory of Applied Nuclear Energy (LENA) at the University of Pavia, thus obtaining the images of the various dose components. The results were analysed in order to verify the possibility of utilising normoxic gels for BNCT. 3. Results Normoxic polymer gel was investigated as regards properties of dose-sensitivity, dose-range of utilisation, reproducibility, changing of the response with time after irradiation and stability in time of the spatial distribution of the measured dose effect. The samples irradiated modify their opacity as it can be seen in Fig. 1. The response of the irradiated dosimeters at different concentrations of the gelling agent is studied vs. the adsorbed doses. In particular, they are studied in the gelatine amount of 6%, 5% and 4% of the nal weight. The viscosity of the

ARTICLE IN PRESS
M. Mariani et al. / Radiation Physics and Chemistry 76 (2007) 15071510 1509

dosimeter-gel obtained with 6% of gelatine is too high also before gelling, so it is not suitable for lling the dosimeter layers, that are obtained by syringing the hot gel through holes of 1 mm diameter. For this reason the dosimeters with 6% of gelatine, prepared in vials, were analysed with the spectrophotometer and not with the CCD camera. The variation in light transmittance induced by radiation, measured with the spectrophotometer (variation of extinction coefcient a I t I 0 eab ) is reported vs. dose (Fig. 2).

Fig. 1. Irradiated samples of polymer gel dosimeter at increasing doses.

1.8 1.6 1.4 1.2 [cm-1] 1.0 0.8 0.6 0.4 0.2 0.0 0 5 10 15 20 25 30 35 40 45 50 55 Absorbed Dose [Gy] Polymer gel with 4% of gelatine Polymer gel with 5% of gelatine Polymer gel with 6% of gelatine

Fig. 2. Variation of the extinction coefcient (a) reported vs. the absorbed dose.

110 100 90 OD normalised [%] 80 70 60 50 40 30 20 10 0 0 2 4 6 8 10 12 Depth [cm] 14 16 18 20

Treatment Planning System Polymer gel profile- calculated Polymer gel profile - measured Fricke gel profile - measured

These results show an initial linearity until 20 Gy and then a signal saturation; similar behaviour is also observed in dosimeter-gels containing 4% or 5% of gelatine. The gelling concentration of 4% allows a simple preparation of gel layers and consequently, a better uniformity between samples, therefore this concentration was selected as nal choice for the best synthesis of the gel dosimeters. The polymer gel response investigated at different waiting-times before the radiation exposure showed that just only two days after the preparation of the gel, the polymerisation did not take-place in the irradiated samples, therefore sample exposures were always performed one day after gel-dosimeter preparation. In order to study post-irradiation stability properties, the polymer gel response was followed by measuring the time prole of the absorbance after irradiation. The results show a negligible variation of the response vs. dose. In fact, gel samples imaged up to 50 days after irradiation maintained their own image unchanged. A set of gel layers, close one to the other, were exposed to high energy (18 MeV) photons of a radiotherapy unit, in order to check the reliability of dose imaging. The dose prole measured with the gel dosimeter is reported vs. depth in Fig. 3. In the same gure, the prole obtained with PENELOPE software and the prole measured with the Fricke and the polymeric dosimeters are reported. A signicative difference between measured and calculated values of the polymer dosimeter is evident in the nal part of the prole (Fig. 3). In order to check the application of polymer gel dosimeters in BNCT, two gel layers, close one to the other, were exposed to the thermal column of the nuclear reactor. One layer contained polymer gel standard, the other one contained also 10B. The dose measured with the gel is reported vs. depth in Fig. 4 with the different contributions to the dose from the gamma rays and the charged particles, Fig. 4a, and from the 10B neutron reactions, Fig. 4b.

4. Conclusion Normoxic polymer gel layers have presented a good interval of linearity (up to about 20 Gy) when exposed to uniform radiation elds and also a good reproducibility. The dose and dose proles (or distribution) remained unchanged with time after irradiation, at least for 50 days. Irradiation of gel layers with a beam parallel to the layer plane, brought to dose proles which were not so good. It is important to perform more studies regarding normoxic polymer gel, in order to understand if the obtained dose proles are a consequence of a specic peculiarity of such dosimeters and if the reliability of the system can be improved by optimising the modalities of preparing gel matrix and samples. More specic studies concerning irradiation with neutron have to be carried out, in order

Fig. 3. Dose proles inter-comparison: (i) measured with polymer- and Fricke-gel dosimeters; (ii) obtained by PENELOPE software; (iii) calculated with the treatment planning system.

ARTICLE IN PRESS
1510 M. Mariani et al. / Radiation Physics and Chemistry 76 (2007) 15071510

Fig. 4. Separation of the different contributions of the absorbed dose: (a) total dose due to gamma rays and fast neutrons; (b) dose due to 10B reactions.

to understand the possibility for real application of the polymer gel dosimeter to the BNCT. Acknowledgements The work was partially supported by INFN (Italy) and partially by MIUR. The authors are grateful to Royalite Plastics s.r.l., Div. Caleppio, for having supplied polystyrene plates for making phantoms and gel-samples transparent windows. References
Baldock, C., Burford, R.P., Billingham, N., Wagner, G.S., Patval, S., Badawi, R.D., Keevil, S.F., 1998. Experimental procedure for the manufacture and calibration of polyacrylamide gel (PAG) for magnetic resonance imaging (MRI) radiation dosimetry. Phys. Med. Biol. 43, 695702.

Farajollahi, A.R., Bonnett, D.E., Tattam, D., Green, S., 2000. The potential use of polymer gel dosimetry in boron neutron capture therapy. Phys. Med. Biol. 45, N9N14. Fong, P.M., Keil, D.C., Does, M.D., Gore, J.C., 2001. Polymer gels for magnetic resonance imaging of radiation dose distributions at normal room atmosphere. Phys. Med. Biol. 46, 31053113. Gambarini, G., Birattari, C., Mariani, M., Marchesini, R., Pirola, L., Prestini, P., Sella, M., Tomatis, S., 2004. Study of light transmittance from layers of Fricke-xylenol-orange-gel dosimeters. Nucl. Instrum. Methods B. 213, 321324. Maryanski, M.J., Schultz, R.J., Ibbott, G.S., Gatenby, J.C., Xie, J., Horton, D., Gore, J.C., 1994. Magnetic resonance imaging of radiation dose distributions using a polymer-gel dosimeter. Phys. Med. Biol. 39, 14371455. Maryanski, M.J., Zastavker, Y.Z., Gore, J.C., 1996. Radiation dose distributions in three dimensions from tomographic optical density scanning of polymer gels: II. Optical properties of the BANG polymer gel. Phys. Med. Biol. 41, 27052717.