Study of the radionuclide deposition in the radioactive ion line of the Selective Production of Exotic Species (SPES) facility.

SPES (Selective Production of Exotic Species) is a second generation facility for the production of radioactive ion beams that is going to be commissioned at the Laboratori Nazionali di Legnaro of INFN at Legnaro, Padua, Italy. Radioactive neutron-rich isotopes are expected to be produced by nuclear fission induced by a 40 MeV, 200 µA primary proton beam impinging on a 238UCx target. The expected reaction rate is about 1013 fission/s. Radioactive ion beams are produced using the isotope separation on-line technique. The production of such an amount of radioactive species raises radiological issues throughout the life cycle of the facility. A study of the radioactive contamination of the components of the radioactive ion beam line is performed with the FLUKA Monte Carlo simulation code, under realistic hypotheses for the produced isobaric beams. The present results complete previous studies focused on the radiological impact of the production target irradiation, the residual activation of the primary proton beam line and the radioactive contamination of the ion source complex. The overall ambient dose equivalent rate due to the different radiation sources is calculated at several positions inside the production bunker and at different times after a typical one-year operating period of the facility with the 238UCx target at full power. The obtained results and the developed methodology provide the guidelines and the needed tools to plan ordinary and extraordinary interventions as well as final decommissioning of the SPES facility.

Production and characterization of 111Ag radioisotope for medical use in a TRIGA Mark II nuclear research reactor.

Radio Pharmaceutical Therapy (RPT) comes forth as a promising technique to treat a wide range of tumors while ensuring low collateral damage to nearby healthy tissues. This kind of cancer therapy exploits the radiation following the decay of a specific radionuclide to deliver a lethal dose to tumor tissues. In the framework of the ISOLPHARM project of INFN, 111Ag was recently proposed as a promising core of a therapeutic radiopharmaceutical. In this paper, the production of 111Ag via neutron activation of 110Pd-enriched samples inside a TRIGA Mark II nuclear research reactor is studied. The radioisotope production is modeled using two different Monte Carlo codes (MCNPX and PHITS) and a stand-alone inventory calculation code FISPACT-II, with different cross section data libraries. The whole process is simulated starting from an MCNP6-based reactor model producing the neutron spectrum and flux in the selected irradiation facility. Moreover, a cost-effective, robust and easy-to-use spectroscopic system, based on a Lanthanum Bromo-Chloride (LBC) inorganic scintillator, is designed and characterized, with the aim of using it, in the future, for the quality control of the ISOLPHARM irradiated targets at the SPES facility of the Legnaro National Laboratories of INFN. natPd and 110Pd-enriched samples are irradiated in the reactor main irradiation facility and spectroscopically characterized using the LBC-based setup and a multiple-fit analysis procedure. Experimental results are compared with theoretical predictions of the developed models, showing that inaccuracies in the available cross section libraries prevent an accurate reproduction of the generated radioisotope activities. Nevertheless, models are normalized to our experimental data allowing for a reliable planning of the 111Ag production in a TRIGA Mark II reactor.

New solid state laser system for SPES: Selective Production of Exotic Species project at Laboratori Nazionali di Legnaro.

The Selective Production of Exotic Species project is under construction at Laboratori Nazionali di Legnaro-INFN. The aim of the collaboration is to produce highly pure Radioactive Ion Beams (RIBs) from fission fragments of a uranium carbide (UCx) target activated by a cyclotron proton beam. In order to select a specific atomic species, the main tool to be applied is the resonant laser ionization technique. We have just completed the installation of a dedicated all solid state laser system whose elements are tunable to transitions of all the elements/isotopes of interest for the project. The new laser system is based on three Titanium:sapphire laser sources, independently pumped by three Nd:YLF pump lasers, and it can be coupled to two high harmonic generation (second harmonic generation, third harmonic generation, and fourth harmonic generation) setups. The power, wavelength, and position of the laser beams are continuously monitored and stabilized by using automated active systems to improve the beam production stability of RIBs. This paper presents the main features of the laser system and examples of application of a laser ion source, including a first demonstration of photoionization of stable silver, one of the most requested elements for RIB application.

Study of the radioactive contamination of the ion source complex in the Selective Production of Exotic Species (SPES) facility.

The Isotope Separation On-Line (ISOL) technique is today established as one of the primary methods to produce high-intensity and high-quality radioactive beams. This technique produces, for a given amount of the desired isotope, many orders of magnitude of other radioactive species. Due to the activation generated by interactions of the primary beam, intense neutron fields, and deposition of the produced radioactive ions inside beam line elements, an ISOL facility in operation becomes an intense radioactive source. Therefore, the biological hazard imposes severe radiological safety challenges to the design, operation, maintenance, and final decommissioning of such facilities. A challenging component is the ion source complex, where the ion extraction electrode provides the extraction of radioactive ions from the ion source and the first acceleration to the extracted beam. The radioactive contamination of this sub-component is studied, by means of the FLUKA code, in the case of the Selective Production of Exotic Species facility, which is in the advanced construction phase at Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Legnaro, Padua, Italy. The developed model includes isotope production by the interactions of a 40 MeV energy proton beam on a 238UCx target, selection of radioactive isotopes that are able to stick on the electrode tip, time evolution of the deposited isotopes during the operation and cooling periods before maintenance interventions, and evaluation of the ambient dose equivalent rate generated by the contamination of the electrode tip. Based on these results, the possibility of manual interventions for maintenance and emergency vs the use of remote handling systems is discussed.

Development of implantation substrates for the collection of radionuclides of medical interest produced via ISOL technique at INFN-LNL.

Accelerator-based techniques with electromagnetic mass separation are considered among the most innovative and promising strategies to produce non-conventional radionuclides for nuclear medicine. Such approach was successfully used at CERN, where the dedicated MEDICIS facility was built, and at TRIUMF, where the ISAC radioactive beam facility was used to produce unconventional α-emitters. In such framework, the Legnaro National Laboratories of the Italian Institute of Nuclear Physics (INFN-LNL) proposed the ISOLPHARM project (ISOL technique for radioPHARMaceuticals), which will exploit radionuclides producible with the SPES (Selective Production of Exotic Species) ISOL (Isotope Separation On-Line) facility to develop novel radiopharmaceuticals. The ISOL technique utilizes the irradiation with a primary beam of particles/nuclei of a production target where radionuclides are produced. A radioactive ion beam is subsequently extracted from the production target unit, and transported up to an analyzing magnet, where non-isobaric contaminants are filtered out. The so-obtained purified radioactive beam is dumped onto an implantation substrate, referred as collection target. Then, the desired nuclides can be chemically harvested from the collected isobars, and the isotopically pure atom collection can be employed to radiolabel high specific activity radiopharmaceuticals. Metallic deposition targets in the form of coated metal foils were mostly used at TRIUMF and CERN. At ISOLPHARM, a different approach is under investigation which foresees the use of soluble cold-pressed collection targets, possibly facilitating the chemical purification process of the collected radionuclides. In this study, the production and characterization of some of the ISOLPHARM collection targets is presented, in particular, soluble salts (NaCl and NaNO3) and organic materials widely used for pharmaceutical tablets production are considered. All such materials proved to be potentially suitable as collection targets, since solid samples were easily produced and resulted compatible with the vacuum conditions required for the ion implantation process. Furthermore, some of the selected substrates were used for proof-of-concept deposition tests with stable silver, to prove their suitability as ISOLPHARM deposition substrates for silver-111, a promising candidate for radiotherapy. Such tests highlighted possible scenarios useful for the development of new alternative materials, as the use of insoluble organic targets.

Effect of graphite and graphene oxide on thorium carbide microstructural and thermal properties.

Thorium carbide to be tested as target material for the production of 225Ac with the ISOL method, was produced via carbothermal reduction of ThO2 nanoparticles by graphite and graphene oxide, respectively. The use of graphene oxide (GO) as carbon source resulted in a reduced reactivity compared to graphite, confirmed by the presence of unreacted ThO2 mainly in the core of the samples. The reacted ThO2 or ThC2-GO showed a faster reactivity in air, mainly observed as ThC2 amorphization. The specific surface area of the ThC2-GO samples was almost doubled compared to ThC2-graphite samples. The effect of these microstructural features was analysed in terms of thermal diffusivity and calculated thermal conductivity that were both reduced in ThC2-GO samples, however the difference with ThC2-graphite samples decreased at increasing temperature. The present study shows that the use of unreduced GO inhibits the solid-state reaction between ThO2 and C; on the other hand, the high reactivity of the ThC2 so produced is expected to be beneficial for the 225Ac production with the ISOL method, affording a high release efficiency. It is expected that the use of reduced GO could represent a good solution for highly efficient ThC2 targets.

Morphological and functional effects of graphene on the synthesis of uranium carbide for isotopes production targets.

The development of tailored targets for the production of radioactive isotopes represents an active field in nuclear research. Radioactive beams find applications in nuclear medicine, in astrophysics, matter physics and materials science. In this work, we study the use of graphene both as carbon source for UO2 carbothermal reduction to produce UCx targets, and also as functional properties booster. At fixed composition, the UCx target grain size, porosity and thermal conductivity represent the three main points that affect the target production efficiency. UCx was synthesized using both graphite and graphene as the source of carbon and the target properties in terms of composition, grain size, porosity, thermal diffusivity and thermal conductivity were studied. The main output of this work is related to the remarkable enhancement achieved in thermal conductivity, which can profitably improve thermal dissipation during operational stages of UCx targets.

Radiation resistance of elastomeric O-rings in mixed neutron and gamma fields: Testing methodology and experimental results.

Materials and components employed in the presence of intense neutron and gamma fields are expected to absorb high dose levels that may induce deep modifications of their physical and mechanical properties, possibly causing loss of their function. A protocol for irradiating elastomeric materials in reactor mixed neutron and gamma fields and for testing the evolution of their main mechanical and physical properties with absorbed dose has been developed. Four elastomeric compounds used for vacuum O-rings, one fluoroelastomer polymer (FPM) based and three ethylene propylene diene monomer rubber (EPDM) based, presently available on the market have been selected for the test. One EPDM is rated as radiation resistant in gamma fields, while the other elastomers are general purpose products. Particular care has been devoted to dosimetry calculations, since absorbed dose in neutron fields, unlike pure gamma fields, is strongly dependent on the material composition and, in particular, on the hydrogen content. The products have been tested up to about 2 MGy absorbed dose. The FPM based elastomer, in spite of its lower dose absorption in fast neutron fields, features the largest variations of properties, with a dramatic increase in stiffness and brittleness. Out of the three EPDM based compounds, one shows large and rapid changes in the main mechanical properties, whereas the other two feature more stable behaviors. The performance of the EPDM rated as radiation resistant in pure gamma fields does not appear significantly better than that of the standard product. The predictive capability of the accelerated irradiation tests performed as well as the applicable concepts of threshold of radiation damage is discussed in view of the use of the examined products in the selective production of exotic species facility, now under construction at the Legnaro National Laboratories of the Italian Istituto Nazionale di Fisica Nucleare. It results that a careful account of dose rate effects and oxygen penetration in the material, both during test irradiations and in operating conditions, is needed to obtain reliable predictions.

The SPES surface ionization source.

Ion sources and target systems play a crucial role in isotope separation on line facilities, determining the main characteristics of the radioactive ion beams available for experiments. In the context of the selective production of exotic species (SPES) facility, a 40 MeV, 200 µA proton beam directly impinges a uranium carbide target, generating approximately 1013 fissions per second. The radioactive isotopes produced by the 238U fissions are delivered to the 1+ ion source by means of a tubular transfer line. Here they can be ionized and subsequently accelerated toward the experimental areas. In this work, the characterization of the surface ionization source currently adopted for the SPES facility is presented, taking as a reference ionization efficiency and transversal emittance measurements. The effects of long term operation at high temperature are also illustrated and discussed.

A preliminary study for the production of high specific activity radionuclides for nuclear medicine obtained with the isotope separation on line technique.

Radiopharmaceuticals represent a fundamental tool for nuclear medicine procedures, both for diagnostic and therapeutic purposes. The present work aims to explore the Isotope Separation On-Line (ISOL) technique for the production of carrier-free radionuclides for nuclear medicine at SPES, a nuclear physics facility under construction at INFN-LNL. Stable ion beams of strontium, yttrium and iodine were produced using the SPES test bench (Front-End) to simulate the production of 89Sr, 90Y, 125I and 131I and collected with good efficiency on suitable targets.

Electrical-thermal-structural finite element simulation and experimental study of a plasma ion source for the production of radioactive ion beams.

The production target and the ion source constitute the core of the selective production of exotic species (SPES) facility. In this complex experimental apparatus for the production of radioactive ion beams, a 40 MeV, 200 µA proton beam directly impinges a uranium carbide target, generating approximately 10(13) fissions per second. The transfer line enables the unstable isotopes generated by the (238)U fissions in the target to reach the ion source, where they can be ionized and finally accelerated to the subsequent areas of the facility. In this work, the plasma ion source currently adopted for the SPES facility is analyzed in detail by means of electrical, thermal, and structural numerical models. Next, theoretical results are compared with the electric potential difference, temperature, and displacement measurements. Experimental tests with stable ion beams are also presented and discussed.

Thermal-electric coupled-field finite element modeling and experimental testing of high-temperature ion sources for the production of radioactive ion beams.

In isotope separation on line facilities the target system and the related ion source are two of the most critical components. In the context of the selective production of exotic species (SPES) project, a 40 MeV 200 µA proton beam directly impinges a uranium carbide target, generating approximately 10(13) fissions per second. The radioactive isotopes produced in this way are then directed to the ion source, where they can be ionized and finally accelerated to the subsequent areas of the facility. In this work both the surface ion source and the plasma ion source adopted for the SPES facility are presented and studied by means of numerical thermal-electric models. Then, numerical results are compared with temperature and electric potential difference measurements, and finally the main advantages of the proposed simulation approach are discussed.

Photo-ionization of aluminum in a hot cavity for the selective production of exotic species project.

SPES (Selective Production of Exotic Species) is an Isotope Separation On-Line (ISOL) based accelerator facility that will be built in the Legnaro-Istituto Nazionale di Fisica Nucleare (INFN) Laboratory (Italy), intended to provide intense neutron-rich radioactive ion beams obtained by proton-induced fission of a uranium carbide (UCx) target. Besides this main target material, silicon carbide (SiC) will be the first to be used to deliver p-rich beams. This target will also validate the functionality of the SPES facility with aluminum beam as result of impinging SiC target with proton beam. In the past, off line studies on laser photoionization of aluminum have been performed in Pavia Spectroscopy Laboratory and in Laboratori Nazionali di Legnaro; a XeCl excimer laser was installed in order to test the laser ionization in the SPES hot cavity. With the new Wien filter installed a better characterization of the ionization process in terms of efficiency was performed and results are discussed.

Ongoing characterization of the forced electron beam induced arc discharge ion source for the selective production of exotic species facility.

An intense research and development activity to finalize the design of the target ion source system for the selective production of exotic species (SPES) facility (operating according to the isotope separation on line technique) is at present ongoing at Legnaro National Laboratories. In particular, the characterization of ion sources in terms of ionization efficiency and transversal emittance is currently in progress, and a preliminary set of data is already available. In this work, the off-line ionization efficiency and emittance measurements for the SPES forced electron beam induced arc discharge ion source in the case of a stable Ar beam are presented in detail.

A steady-state high-temperature method for measuring thermal conductivity of refractory materials.

A new methodology and an instrumental setup for the thermal conductivity estimation of isotropic bulk graphite and different carbides at high temperatures are presented. The method proposed in this work is based on the direct measurement of temperature and emissivity on the top surface of a sample disc of known dimensions. Temperatures measured under steady-state thermal equilibrium are then used to estimate the thermal conductivity of the sample by making use of the inverse parameter estimation technique. Thermal conductivity values obtained in this way are then compared to the material data sheets and values found in literature. The reported work has been developed within the Research and Development framework of the SPES (Selective Production of Exotic Species) project at INFN-LNL (Istituto Nazionale di Fisica Nucleare - Laboratori Nazionali di Legnaro).

Off-line ionization tests using the surface and the plasma ion sources of the SPES project.

The development of new target ion source systems for the selective production of exotic species (SPES) facility is currently in progress at Legnaro National Laboratories. In this context, the study of ion sources and their performance in terms of ionization efficiency and transversal emittance is a crucial point in order to maximize the available yields, particularly for short-lived isotopes. In this work, preliminary off-line ionization efficiency and emittance measurements for the SPES surface and plasma ion sources are presented. The plasma source emittance measurements are supported by dedicated numerical calculations.

Studies for aluminum photoionization in hot cavity for the selective production of exotic species project.

Selective production of exotic species (SPES) is an ISOL-based accelerator facility that will be built in the Legnaro INFN Laboratory (Italy), intended to provide an intense neutron-rich radioactive ion beams obtained by proton induced fission of an uranium carbide target. Beside this main target, a silicon carbide (SiC) target will the first to be used to deliver some p-rich beams. This target will validate also the functionality of the SPES facility with aluminum beam as result of hitting SiC target with protons. In the past off-line studies on laser photoionization of aluminum have performed in Pavia Spectroscopy Laboratory and in Laboratori Nazionali di Legnaro where, recently, a XeCl excimer laser was installed in order to test the laser ionization in the SPES hot cavity. Results are promising to justify further studies with this technique, aiming a better characterization of the SPES ion extraction capability under laser photoionization.

Therapeutic approach to patients complaining of high blood pressure in a cardiological emergency room.

OBJECTIVE: To evaluate the management of patients complaining of high blood pressure (BP) in a cardiological emergency room. METHODS: Patients referred to the cardiological emergency room with the main complaint of high blood pressure were consecutively selected. The prescriptions and the choice of antihypertensive drugs were assessed. The classification of these patients as hypertensive emergencies or pseudoemergencies, according to the physician who provided initial care, was recorded. RESULTS: From a total of 858 patients presenting to the emergency room, 80 (9.3%) complained of high BP, and 61 (76.3%) received antihypertensive drugs. Sublingual nifedipine was the most commonly used drug (59%). One patient received intravenous medication, one patient was hospitalized and 6 patients (7.5%) were classified as hypertensive emergencies or pseudoemergencies. CONCLUSION: High BP could seldom be classified as a hypertensive emergency or pseudoemergency, even though it was a frequent complaint (9.3% of visits). Currently, the therapeutic approach is not recommended, even in specialized clinics.