Innovative detection methods for radiation hardness

The thesis deals with new methods for the characterization of ion beams and detection of radiation used in radiation hardness applications, namely charged particles, X- and gamma-radiation and neutrons. As far as the detection of charged particles, X- and gamma- rays the radiochromic films, dosimeters intensively employed in medical physics, were found suitable for these purposes. The calibration of radiochromic films was carried out with the law that describe the physical phenomenon of the film darkening. On this line the independence of the response of a kind of film to incident radiation type, energy and dose rate was demonstrated. These results were crucial for the full dosimetry characterization of a 90-Sr/90-Y beta source, recently proposed as irradiation source for Total Ionizing Dose tests as alternative to the well-established 60-Co source. Furthermore, since standard methods of reading of radiochromic films do not allow real-time dosimetry, the design, development and related tests of a new opto-electronic-based real-time radiochromic film reader is presented in this thesis. Owing to the wide employment of radiochromic films in the applications and to the potential diffusion on the market, a National Patent was filed in January 2018 through the INFN Tech-Transfer. The problem of neutron detection and production has been addressed at two charged particle accelerators. In particular, for the first time a neutron beam line was implemented at the IBA 18/18 medical cyclotron of University of Bern and the test of a new prototype of polysiloxane-based scintillator was carried out at the tandem accelerator of Laboratori Nazionali del Sud (LNS) in Catania. All these topics are discussed in this thesis and in dedicated publications on international scientific journals

Radiation Damage in Polyethylene Naphthalate Thin-Film Scintillators.

This paper describes the scintillation features and the radiation damage in polyethylene naphthalate 100 µm-thick scintillators irradiated with an 11 MeV proton beam and with a 1 MeV electron beam at doses up to 15 and 85 Mrad, respectively. The scintillator emission spectrum, optical transmission, light yield loss, and scintillation pulse decay times were investigated before and after the irradiation. A deep blue emission spectrum peaked at 422 nm, and fast and slow scintillation decay time constants of the order of 1-2 ns and 25-30 nm, respectively, were measured. After irradiation, transmittance showed a loss of transparency for wavelengths between 380 and 420 nm, and a light yield reduction of ~40% was measured at the maximum dose of 85 Mrad

A novel experimental approach to characterize neutron fields at high- and low-energy particle accelerators.

The characterization of particle accelerator induced neutron fields is challenging but fundamental for research and industrial activities, including radiation protection, neutron metrology, developments of neutron detectors for nuclear and high-energy physics, decommissioning of nuclear facilities, and studies of neutron damage on materials and electronic components. This work reports on the study of a novel approach to the experimental characterization of neutron spectra at two complex accelerator environments, namely the CERF, a high-energy mixed reference field at CERN in Geneva, and the Bern medical cyclotron laboratory, a facility used for multi-disciplinary research activities, and for commercial radioisotope production for nuclear medicine. Measurements were performed through an innovative active neutron spectrometer called DIAMON, a device developed to provide in real time neutron energy spectra without the need of guess distributions. The intercomparison of DIAMON measurements with reference data, Monte Carlo simulations, and with the well-established neutron monitor Berthold LB 6411, has been found to be highly satisfactory in all conditions. It was demonstrated that DIAMON is an almost unique device able to characterize neutron fields induced by hadrons at 120 GeV/c as well as by protons at 18 MeV colliding with different materials. The accurate measurement of neutron spectra at medical cyclotrons during routine radionuclide production for nuclear medicine applications is of paramount importance for the facility decommissioning. The findings of this work are the basis for establishing a methodology for producing controlled proton-induced neutron beams with medical cyclotrons

Methodology for measuring photonuclear reaction cross sections with an electron accelerator based on Bayesian analysis

Accurate measurements of photonuclear reaction cross sections are crucial for a number of applications, including radiation shielding design, absorbed dose calculations, reactor physics and engineering, nuclear safeguard and inspection, astrophysics, and nuclear medicine. Primarily motivated by the study of the production of selected radionuclides with high-energy photon beams (mainly 225Ac, 47Sc, and 67Cu), we have established a methodology for the measurement of photonuclear reaction cross sections with the microtron accelerator available at the Swiss Federal Institute of Metrology (METAS). The proposed methodology is based on the measurement of the produced activity with a High Purity Germanium (HPGe) spectrometer and on the knowledge of the photon fluence spectrum through Monte Carlo simulations. The data analysis is performed by applying a Bayesian fitting procedure to the experimental data and by assuming a functional trend of the cross section, in our case a Breit-Wigner function. We validated the entire methodology by measuring a well-established photonuclear cross section, namely the 197Au({\gamma},n)196Au reaction. The results are consistent with those reported in the literature

Half-life measurement of 44Sc and 44mSc.

The half-lives of 44Sc and 44mSc were measured by following their decay rate using several measurement systems: two ionization chambers and three γ-spectrometry detectors with digital and/or analogue electronics. For 44Sc, the result was the combination of seven half-life values giving a result of 4.042(7) h, which agrees with the last reported value of 4.042(3) h and confirms the near to 2% deviation from the recommended half-life of 3.97(4) h. Scandium-44 is present as an impurity in the production of 44Sc by cyclotron proton irradiation. Its half-life was determined by measurements performed a few days after End of Bomardment (EoB), so that the 44Sc decayed down to a negligible level. Seven measurements were combined to obtain an average of 58.7(3) h, which is in agreement with the recommended value of 58.6(1) h

Radiochromic Films for the Two-Dimensional Dose Distribution Assessment

Radiochromic films are mainly used for two-dimensional dose verification in photon, electron, and proton therapy treatments. Moreover, the radiochromic film types available today allow their use in a wide dose range, corresponding to applications from low-medical diagnostics to high-dose beam profile measurements in charged particle medical accelerators. An in-depth knowledge of the characteristics of radiochromic films, of their operating principles, and of the dose reading techniques is of paramount importance to exploit all the features of this interesting and versatile radiation detection system. This short review focuses on these main aspects by considering the most recent works on the subject

Alternative routes for 64Cu production using an 18 MeV medical cyclotron in view of theranostic applications.

Radiometals play a fundamental role in the development of personalized nuclear medicine. In particular, copper radioisotopes are attracting increasing interest since they offer a varying range of decay modes and half-lives and can be used for imaging (60Cu, 61Cu, 62Cu and 64Cu) and targeted radionuclide therapy (64Cu and 67Cu), providing two of the most promising true theranostic pairs, namely 61Cu/67Cu and 64Cu/67Cu. Currently, the most widely used in clinical applications is 64Cu, which has a unique decay scheme featuring β+-, β--decay and electron capture. These characteristics allow its exploitation in both diagnostic and therapeutic fields. However, although 64Cu has extensively been investigated in academic research and preclinical settings, it is still scarcely used in routine clinical practice due to its insufficient availability at an affordable price. In fact, the most commonly used production method involves proton irradiation of enriched 64Ni, which has a very low isotopic abundance and is therefore extremely expensive. In this paper, we report on the study of two alternative production routes, namely the 65Cu(p,pn)64Cu and 67Zn(p, α)64Cu reactions, which enable low and high 64Cu specific activities, respectively. To optimize the 64Cu production, while minimizing the mass of copper used as a target in the first case, or the co-production of other copper radioisotopes in the second case, an accurate knowledge of the production cross sections is of paramount importance. For this reason, the involved nuclear reaction cross sections were measured at the Bern medical cyclotron laboratory by irradiating enriched 65CuO and enriched 67ZnO targets. On the basis of the obtained results, the production yield and purity were calculated to assess the optimal irradiation conditions. Several production tests were performed to confirm these findings

Novel solid target and irradiation methods for theranostic radioisotope production at the Bern medical cyclotron

The production of medical radioisotopes for theranostics is essential for the development of personalized nuclear medicine. Among them, radiometals can be used to label proteins and peptides and their supply in quantity and quality suitable for clinical applications represents a scientific challenge. A research program is ongoing at the Bern medical cyclotron, where an IBA Cyclone 18/18 HC is in operation. The cyclotron provides 18 MeV proton beams up to 150 μA and is equipped with a Solid Target Station (STS) and a 6 m Beam Transport Line (BTL), ending in a separate bunker with independent access. A novel magnetic target coin was realized to bombard isotope-enriched materials in the form of compressed powders, together with a compact focalization system to enhance the irradiation procedure. For an optimized production yield with the required radionuclidic purity, novel methods were developed to precisely measure the extracted beam energy and the involved reaction cross sections. In particular, a target station was realized to measure nuclear cross sections using materials in the form of powder deposited on an aluminium disc by sedimentation, bombarded by a monitored flat beam

Optimized production of 67Cu based on cross section measurements of 67Cu and 64Cu using an 18 MeV medical cyclotron.

RadioNuclide Therapy (RNT) in nuclear medicine is a cancer treatment based on the administration of radioactive substances that specifically target cancer cells in the patient. These radiopharmaceuticals consist of tumor-targeting vectors labeled with β-, α, or Auger electron-emitting radionuclides. In this framework, 67Cu is receiving increasing interest as it provides β--particles accompanied by low-energy γ radiation. The latter allows to perform Single Photon Emission Tomography (SPECT) imaging for detecting the radiotracer distribution for an optimized treatment plan and follow-up. Furthermore, 67Cu could be used as therapeutic partner of the β+-emitters 61Cu and 64Cu, both currently under study for Positron Emission Tomography (PET) imaging, paving the way to the concept of theranostics. The major barrier to a wider use of 67Cu-based radiopharmaceutical is its lack of availability in quantities and qualities suitable for clinical applications. A possible but challenging solution is the proton irradiation of enriched 70Zn targets, using medical cyclotrons equipped with a solid target station. This route was investigated at the Bern medical cyclotron, where an 18 MeV cyclotron is in operation together with a solid target station and a 6-m-long beam transfer line. The cross section of the involved nuclear reactions were accurately measured to optimize the production yield and the radionuclidic purity. Several production tests were performed to confirm the obtained results

Experimental assessment of nuclear cross sections for the production of Tb radioisotopes with a medical cyclotron.

155Tb is one of the most interesting radionuclides for theranostic applications. It is suitable for SPECT imaging and it can be used as a true diagnostic partner of the therapeutic 149Tb and 161Tb. Its production by proton irradiation using enriched 155Gd and 156Gd oxide targets is currently being investigated and represents a promising solution. To achieve the level of radionuclidic purity required in the clinical setting, the co-production of Tb impurities has to be minimized. For this purpose, an accurate knowledge of the cross sections of the nuclear reactions involved is of paramount importance. In this paper, we report on the assessment of cross sections of the reactions 154Gd(p,xn)153,154,154m1,154m2Tb, 155Gd(p,xn)154,154m1,154m2,155Tb, 156Gd(p,xn)155,156Tb and 157Gd(p,2n)156Tb derived with a specific data analysis procedure developed by our group. This method allows to disentangle the nuclear contributions from the production cross section by inverting linear systems of equations and it requires the measurement of the cross sections from as many materials as the reactions involved in the production of the radionuclide under study. For this purpose, the experimental data previously measured by our group at the Bern medical cyclotron by irradiating natural Gd2O3, enriched 155Gd2O3 and enriched 156Gd2O3 targets were used. For some of these nuclear reactions, cross sections were assessed for the first time. On the basis of our findings, production yield and purity can be calculated for any kind of isotopic composition of the enriched material