Irradiation Of Solid Targets Research Articles

Behaviour, use and safety aspects of astatine-211 solvated in chloroform after dry distillation recovery

Targeted alpha therapy of disseminated cancer is an emerging technique where astatine-211 is one of the most promising candidate nuclides. Astatine-211 can be produced in medium energy cyclotrons by alpha particle bombardment of natural bismuth. The produced astatine is then commonly recovered from the irradiated solid target material through dry distillation. The dry distillation process often includes elution and solvation of condensed astatine with chloroform, forming Chloroform Eluate. In this work the handling and safe use of the high activity concentration Chloroform Eluate has been investigated. Correctly performed, evaporation of Chloroform Eluate results in a dry residue with complete recovery of the astatine. The dry residue can then serve as a versatile starting material, using appropriate oxidizing or reducing conditions, for subsequent downstream chemistry. However, it has been found that when evaporating the Chloroform Eluate, astatine can be volatilized if continuing the process beyond the point of dryness. This behavior is more pronounced when the Chloroform Eluate has received a higher absorbed dose. Upon water phase contact of the Chloroform Eluate, a major part of the astatine activity becomes water soluble, leaving the organic phase. A behavior which is also dependent on dose to the solvent.

High Separation Factor, High Molar Activity, and Inexpensive Purification Method for the Production of Pure 165Er.

Introduction: Auger electron-emitting radionuclides with low (0.001-1 keV) energy, short-range (2-500 nm), and high linear energy transfer (4-26 keV/μm) can play an important role in the targeted radionuclide therapy (TRT) of cancer. 165Er is a pure Auger electron-emitting radionuclide, making it a useful tool for the fundamental studies of the biological effects of Auger electrons. This work develops a simple, inexpensive, high separation factor, and high molar activity radiochemical isolation process for the production of 165Er (t1/2 10.36 h) suitable for TRT in vitro and in vivo studies using irradiated natHo solid targets. Methods: Small medical cyclotron proton-irradiation of natHo targets produced 165Er in GBq scale quantities. 165Er was isolated using cation exchange chromatographic resin (AG 50W-X8, 200-400 mesh, 20 mL, under atmospheric pressure) using α-hydroxyisobutyric acid (70 mM, pH 4.75) followed by extraction using TK212, TK211, and TK221 extraction chromatographic columns. Radio nuclidic and chemical purity of the final 165Er were confirmed using HPGe Gamma spectrometry and induction coupled plasma-mass spectrometry analysis, respectively. The purified 165Er was radiolabeled with two radiometal chelators (DOTA and Crown) and used to produce a new Auger electron-emitting radiopharmaceutical, [165Er]Er-Crown-TATE. Results: Irradiation of 200 mg natHo targets with 20-30 μA of 12.8 MeV protons produced 165Er at 25 ± 5 MBq·μA-1·h-1. The 4.5 ± 0.5 h radiochemical isolation yielded GBq scale of 165Er in 0.05 M HCl (2 mL) with a radiochemical yield of 78.0 ± 5.6% decay corrected to the end of bombardment (EoB) and a Ho/165Er separation factor of (1.14 ± 0.25) × 106. The product showed high radio nuclidic purity and chemical purity. Concentration-dependent radiolabeling experiments with Crown and DOTA were performed resulting in the successful labeling of 165Er with high (>90%) radiochemical yield. Radiolabeling experiments with Crown-TATE were performed 8 h after EoB and synthesized [165Er]Er-Crown-TATE at molar activities of 202.4 MBq·nmol-1 at the end of synthesis (EoS). Conclusions: A 3 h cyclotron irradiation and 4.5 h radiochemical separation produced GBq-scale 165Er suitable for producing radiopharmaceuticals at molar activities satisfactory for investigations of targeted radionuclide therapeutic effects of Auger electron emissions. This will enable future fundamental radiation biology experiments of pure Auger electron-emitting therapeutic radiopharmaceuticals, such as [165Er]Er-Crown-TATE, which will be used to understand the impact of Auger electrons in TRT.

Gigahertz electromagnetic pulse emission from femtosecond relativistic laser-irradiated solid targets.

The interactions between high-intensity laser and matter produce particle flux and electromagnetic radiation over a wide energy range. The generation of extremely intense transient fields in the radio frequency-microwave regime has been observed in femtosecond-to-nanosecond laser pulses with 1011-1020-W/cm2 intensity on both conductive and dielectric targets. These fields typically cause saturation and damage to electronic equipment inside and near an experimental chamber; nevertheless, they can also be effectively used as diagnostic tools. Accordingly, the characterization of electromagnetic pulses (EMPs) is extremely important and currently a popular topic for present and future laser facilities intended for laser-matter interaction. The picosecond and sub-picosecond laser pulses are considerably shorter than the characteristic electron discharge time (∼0.1 ns) and can be efficient in generating GHz EMPs. The EMP characterization study of femtosecond laser-driven solid targets is currently mainly in the order of 100 mJ laser energy, in this study, the EMP generated by intense (Joule class) femtosecond laser irradiation of solid targets has been measured as a function of laser energy, laser pulse duration, focal spot size, and target materials. And a maximum electric field of the EMP reaching up to 105 V/m was measured. Analyses of experimental results confirm a direct correlation between measured EMP energy and laser parameters in the ultrashort pulse duration regime. The EMP signals generated by femtosecond laser irradiation of solid targets mainly originate from the return current inside the target after hot electron excitation. Numerical simulations of EMP are performed according to the target charging model, which agree well with the experimental results.

Radiation of extreme ultraviolet source and out-of-band from laser-irradiated low-density SnO<sub>2</sub> target

The extreme ultraviolet (EUV) lithography technology required for high-end chip manufacturing is the first of 35 “bottleneck” key technologies that China is facing currently. The high conversion efficiency EUV source and low out-of-band radiation play a significant role in the application of the EUV lithography system. In this work, the EUV source and out-of-band radiation are studied by using laser irradiated solid Sn target and low-density SnO<sub>2</sub> target. The result shows that a strong EUV radiation at a wavelength of 13.5 nm is generated when the laser irradiates the two forms of Sn targets. Owing to the self-absorption effect of the solid Sn target plasma, the maximum intensity of the wavelength is not located at the position of 13.5 nm, which is working wavelength of EUV lithography system. However, the peak radiation spectrum is located at the position of 13.5 nm with low-density SnO<sub>2</sub> target due to its weaker plasma self-absorption effect. In addition, the satellite lines are weaker in low-density SnO<sub>2</sub> target than in the solid Sn target, so that the spectrum efficiency of the EUV at 13.5 nm (2% bandwidth) is increased by about 20%. On the other hand, the experimental study of the out-of-band radiation is carried out. The out-of-band radiation spectral results show that the out-of-band radiation is mainly dominated by the continuum spectrum. Compared with the solid Sn target, the low-density SnO<sub>2</sub> target contains a part of the low <i>Z</i> element O (<i>Z</i> = 8), resulting in a low-intensity continuum spectrum. In addition, the collision probability of ion-ion and electron-ion both become low when the laser irradiates the low-density SnO<sub>2</sub> target, resulting in a short out-of-band radiation duration time. Therefore, the out-of-band radiation generated by the laser irradiated on the low-density SnO<sub>2</sub> target is weak based on the above reasons. The angular distribution of out-of-band radiation measurement results shows that the intensity of out-of-band radiation decreases with the angle increasing. A cosine function <inline-formula><tex-math id="M2">\begin{document}$A \cos ^\alpha \theta$\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20222385_M2.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="6-20222385_M2.png"/></alternatives></inline-formula> can fit the angular distribution of the total radiation.

Cyclotron production of 64Cu by proton irradiation of enriched 64Ni target: Validation of Geant4 simulation parameters through experimental data

The use of radioisotopes in nuclear medicine applications became essential for the diagnosis and follow-up imaging of many oncological, cardiovascular, and neurodegenerative diseases, in a safe and non-invasive way. Their use in the personalized treatment of tumors is on the verge to change the oncological patient management. Optimization of the radioisotopes production aims to maximize the production efficiency while minimizing side reactions and costs. A practical approach to balance these non-converging ways is to employ the simulation tools in the process design phase and experimental setup. In this way, the production yield can be estimated and the radionuclide impurities content that appears during the bombardment of the target of interest can be optimally set below acceptable limits. Copper-64 is an emerging radionuclide in nuclear medicine theragnostic applications due to three decay modes, namely electron capture, electron (β−) and positron (β+) emissions, and a 12.7 h half-life, favorable for visualization of fast biological processes. Optimization of 64Cu production by irradiation of enriched 64Ni targets with protons in a particular geometry on a TR-19 cyclotron is discussed in this work. The simulated activity produced on different levels of enrichment of the 64Ni targets was calculated using the Monte Carlo simulation in the Geant4 platform, where a customized solid target irradiation system set-up was replicated; the obtained parameters were implemented in the experiments and the results were compared, aiming to validate the simulation parameters through experimental data.As the simulated and experimental results regarding the production of 64Cu via64Ni(p,n)64Cu reaction are in good compliance, the tool can be further applied for the optimization of the production of other radionuclides on the same set-up.

Monitoring of the heavy-ion beam distribution using poly- and monochromatic x-ray fluorescence imaging.

In this work, the first proof of the principal of an in situ diagnostics of the heavy-ion beam intensity distribution in irradiation of solid targets is proposed. In this scheme, x-ray fluorescence that occurs in the interaction of heavy-ions with target atoms is used for imaging purposes. The x-ray conversion to optical radiation and a transport-system was developed, and its first test was performed in experiments at the Universal Linear Accelerator in Darmstadt, Germany. The Au-beam intensity distribution on thin foils and Cu-mesh targets was imaged using multiple x-ray pinholes (polychromatic imaging) and 2D monochromatic imaging of Cu Kα radiation by using a toroidally bent silicon crystal. The presented results are of importance for application in experiments on the investigation of the equation of states of high energy density matter using high intensity GeV/u heavy-ion beams of ≥1010 particles/100ns.

Compact high-flux X-ray source based on irradiation of solid targets by gigahertz and megahertz bursts of femtosecond laser pulses

In this study, we demonstrate the significant increase in the hard X-ray yield (more than 1011 photons/s in 4π solid angle in 6 - 40 keV range) that can be achieved in an ambient air environment when solid targets are irradiated by sequences of high average power (90 W) bursts of femtosecond laser pulses, generated in GHz burst laser amplifier operated at high repetition rate (100 kHz). The combination of the prepulse and ∼ 10 times greater driving pulse not only enhances X-ray generation efficiency (∼ 10−6) by more than two orders of magnitude compared to the single pulse regime but also protects a target allowing continuous operation for 3 hours with only 30% predictable and gradual drop of X-ray yield. In addition, we show that X-ray yield enhancement becomes around 6 times more pronounced at higher repetition rates (100 kHz compared to < 5 kHz). The simplicity and relative cost-effectiveness of the presented X-ray source makes it an attractive solution for future applications in ultrafast X-ray imaging and spectroscopy.

Terahertz Emission Enhanced by a Laser Irradiating on a T-Type Target

The generation of high field terahertz emission based on the interaction between an ultra-intense laser and solid targets has been widely studied in recent years because of its wide potential applications in biological imaging and material science. Here, a novel scheme is proposed to enhance the terahertz emission, in which a linearly polarized laser pulse irradiates a T-type target including a longitudinal target followed by a transverse target. By using two-dimensional particle-in-cell simulations, we find that the electron beam, modulated by the direct laser acceleration via the interaction of the laser with the longitudinal solid target, plays a crucial role in enhancing the intensity of terahertz emission and controlling its spatial distribution. Compared with the single-layer target, the maximum radiated electromagnetic field’s intensity passing through the spatial probe point is enhanced by about one order of magnitude, corresponding to the terahertz emission power increasing by two orders of magnitude or so. In addition, the proposed scheme is robust with respect to the thickness and length of the target. Such a scheme may provide important theoretical and data support for the enhancement of terahertz emission efficiency based on the ultra-intense laser irradiation of solid targets.

Analysis of electromagnetic pulses generated from ultrashort laser irradiation of solid targets at CLAPA

Electromagnetic pulses (EMPs) produced by the interaction of a TW femtosecond laser with solid targets at the Compact Laser Plasma Accelerator (CLAPA) are measured and interpreted. The statistical results confirm that the intensities of the EMPs are closely related to both target material and thickness. The signal of the titanium target is more abundant than that of the copper target with the same thickness, and the intensity of EMP is positively correlated with the target thickness for aluminium foil. With the boosted EMP radiations, the energy of accelerated protons is also simultaneously enhanced. In addition, EMPs emitted from the front of the target exceed those from the rear, which are also pertinent to the specific target position. The resonant waveforms in the target chamber are analyzed using the fast Fourier transform, and the local resonance and the attenuation lead to changes of the frequency spectra of EMPs with variation of detecting positions, which is well supported by the modeling results. The findings are beneficial to gaining insight into the mechanism of EMP propagation in a typical target chamber and providing more information for EMP shielding design.

New advances in the computational simulation of Aqueous Homogeneous Reactor for medical isotopes production

Aqueous Homogeneous Reactors (AHRs) or simply solution reactors present nowadays a promising alternative to produce medical isotopes, especially 99Mo. The AHR medical production concept has been proposed to produce medical isotopes directly in the fuel solution, resulting in a potentially competitive alternative in comparison with the solid target irradiation method in heterogeneous reactors. Furthermore, the utilization of AHRs for medical isotopes production has been strengthened because of the successful operation of the ARGUS reactor since 1981 and its conversion to low-enriched uranium (LEU) fuel during 2012-2014. Those successes positively influenced in the decisions to construct a Proof-Of-Concept production site based on the ARGUS operational experience in Sarov (500 km from Moscow) and to restore the Argus-FTI at the Umarov Physical and Technical Institute in Dushanbe, Tajikistan. However, demonstrating the viability of the AHRs for medical isotopes requires solving several significant challenges related with the safe operation of these reactors. Consequently, not only for the design, licensing and safe operation of the AHRs, but also for the prediction of accident scenarios it is very important to be able to simulate and predict the behavior of the fuel solutions through a group of relevant physical parameters. Accordingly, this paper aims to show the advances made to improve the predictive capabilities during the multi-physics computational modeling of AHRs.

Simulation of hard x-rays source produced by a picosecond laser irradiated solid target for Compton radiography

A bremsstrahlung radiation hard x-ray source, produced by a picosecond intense laser irradiated solid target, was used to diagnose an implosion capsule at stagnation phase via Compton radiography in experiments. By performing Monte Carlo and particle-in-cell simulation, we investigated the influence of target materials and laser intensity on the >70 keV bremsstrahlung hard x-ray emission. We found that the brightness of the hard x-rays is proportional to the atomic number multiplied by area density (ZρL), which indicates that the higher Z and higher density gold or uranium material will produce the brightest hard x-rays source at the same thickness. In relativistic laser solid interactions, hot electron recirculation plays an important role in hard x-ray emission. Without recirculation, hard x-ray conversion efficiency decays when increasing the laser intensity. While the hard x-ray emission comes to the maximal saturated conversion efficiency at relativistic laser intensity if considering the electron recirculation. These results provide valuable insights into the experimental design of Compton radiography.

Monte Carlo estimation of radiation fields and radio activations in the 64Ni solid target irradiation for 64Cu production and its validation with experimental findings

64Cu is an emerging theranostic radioisotope which is generating interest in the field of PET imaging and planning of therapy. A prototype solid target is being designed for producing 64Cu at RMC, BARC. This study evaluates radiation safety aspects involved in the use of the new solid target using FLUKA Monte Carlo code. The radiological hazards are quantified during the production of 64Cu and further handling of the target assembly for post irradiation processing. Analysis of ambient dose equivalent rates from the target assembly shows that during the sufficient quantity of 64Cu production, radiation fields outside the cyclotron vault at RMC BARC are below the allowed limit. The studies also confirm that the 4 h decay after the end of bombardment is suitable for post irradiation handling of the target.

Increasing analyzable steel thickness for thin layer activation experiments

The thin layer activation technique (TLA) is very effective in wear analysis for tribological systems where disassembly is costly or impractical. Since its development in the 1970s, TLA has been applied through direct irradiation of solid targets using ionizing particle beams to obtain an activation with a specific profile. This profile is then used to measure wear in a variety of experiments. These experiments rely heavily on how deep the normalized activation occurs. Depths of $$30\,\upmu {\text{m}}$$ to $$50\,\upmu {\text{m}}$$ are obtained for constant activation by the standard method, which for many experiments is sufficient. However, many others would benefit greatly from a $$300\,\upmu {\text{m}}$$ constant activation layer, such as high-performance engines, softer alloys (brakes), and oil transport systems. Achieving this aim was the goal of this paper. First, we needed to find an adequate irradiation line for the TLA technique. Then, another technique/system was developed (the Attenuation Wheel), which would bring the depth of constant activation from $$50\,\upmu {\text{m}}$$ to $$300\,\upmu {\text{m}}$$.

Accounting for the Edge Effects of Electric and Magnetic Fields in the Spectroscopy of Ion Flows from Relativistic Laser Plasma

Analytical formulas are obtained that describe stationary fields in magnetic and electric separators of charged particles of ion spectrometers of two types taking edge effects into account: a time-of-flight spectrometer with magnetic separation and a Thomson mass spectrometer. Based on a numerical solution of the equation of ion motion in magnetic and electric fields taking the edge effects into account, it is shown that calculation using the effective constant-field method without taking the edge effects into account leads to errors not only in determining the ion energy, but also in the estimation of the mass and charge compositions of the ion flow, which is formed under irradiation of solid targets with femtosecond laser pulses of relativistic intensity. On the basis of the developed approaches, experimental data that were obtained using spectrometers of both types at a laser radiation intensity of above 1018 W/cm2 on targets are interpreted and it is shown that the developed algorithms provide their fast and efficient analysis.

Highly-collimated, high-charge and broadband MeV electron beams produced by magnetizing solids irradiated by high-intensity lasers

Laser irradiation of solid targets can drive short and high-charge relativistic electron bunches over micron-scale acceleration gradients. However, for a long time, this technique was not considered a viable means of electron acceleration due to the large intrinsic divergence (∼50° half-angle) of the electrons. Recently, a reduction in this divergence to 10°–20° half-angle has been obtained, using plasma-based magnetic fields or very high contrast laser pulses to extract the electrons into the vacuum. Here we show that we can further improve the electron beam collimation, down to ∼1.5° half-angle, of a high-charge (6 nC) beam, and in a highly reproducible manner, while using standard stand-alone 100 TW-class laser pulses. This is obtained by embedding the laser-target interaction in an external, large-scale (cm), homogeneous, extremely stable, and high-strength (20 T) magnetic field that is independent of the laser. With upcoming multi-PW, high repetition-rate lasers, this technique opens the door to achieving even higher charges (>100 nC).

Analysis of nascent silicon phase-change gratings induced by femtosecond laser irradiation in vacuum

The formation of periodic surface structures is a general effect of femtosecond laser irradiation of solid targets showing promising interest in material science and technology. However, the experiments are typically carried out in air, a condition in which the target surface becomes densely decorated with nanoparticles that can influence the formation of the surface structures in the early stage of the irradiation process. Here we report an investigation of structures generation on a silicon surface irradiated in vacuum (10−5 mbar) with a low number of laser pulses (N ≤ 10) that exploits several microscopy techniques (optical, atomic force, electron and Raman). Our analyses allow identifying the creation of silicon phase-change gratings consisting of alternating amorphous and crystalline periodic lines, with almost no material removal, located at the periphery of a shallow ablation crater. These gratings originate from two different kinds of defects: (i) the first is characterized by a peculiar lobed shape that is produced by the first few laser pulses; (ii) the second is provided by the one-dimensional, linear singularity defined by the ablation edge of the nascent crater. Both kind of defects lead to grating structures extending outwards the amorphous central area of the crater along the direction of the laser polarization. Comparative analysis with the surface formed in air, in the same experimental conditions, evidences the important role played by nanoparticles densely decorating the target in air and the striking variation occurring in vacuum.

Graphite oxide based targets applied in laser matter interaction

In the present work, we propose the production of a hybrid graphene based material suitable to be laser irradiated with the aim to produce quasi-monoenergetic proton beams using a femtosecond laser system. The unique lattice structure of the irradiated solid thin target can affect the inside electron propagation, their outgoing from the rear side of a thin foil, and subsequently the plasma ion acceleration. The produced targets, have been characterized in composition, roughness and structure and for completeness irradiated. The yield and energy of the ions emitted from the laser-generated plasma have been monitored and the emission of proton stream profile exhibited an acceleration of the order of several MeVs/charge state.

A solvent-extraction module for cyclotron production of high-purity technetium-99m

The design and fabrication of a fully-automated, remotely controlled module for the extraction and purification of technetium-99m (Tc-99m), produced by proton bombardment of enriched Mo-100 molybdenum metallic targets in a low-energy medical cyclotron, is here described. After dissolution of the irradiated solid target in hydrogen peroxide, Tc-99m was obtained under the chemical form of 99mTcO4-, in high radionuclidic and radiochemical purity, by solvent extraction with methyl ethyl ketone (MEK). The extraction process was accomplished inside a glass column-shaped vial especially designed to allow for an easy automation of the whole procedure. Recovery yields were always >90% of the loaded activity. The final pertechnetate saline solution Na99mTcO4, purified using the automated module here described, is within the Pharmacopoeia quality control parameters and is therefore a valid alternative to generator-produced 99mTc. The resulting automated module is cost-effective and easily replicable for in-house production of high-purity Tc-99m by cyclotrons

A method to achieve rapid localised deep heating in a laser irradiated solid density target

Rapid heating of small buried regions by laser generated fast electrons may be useful for applications such as extreme ultraviolet (XUV) radiation sources or as drivers for shock experiments. In non-structured targets, the heating profile possesses a global maximum near the front surface. This paper presents a new target design that uses resistive guiding to concentrate the fast electron current density at a finite depth inside the target. The choice of geometry uses principles of non-imaging optics. A global temperature maximum at depths up to 50 μm into the target is achieved. Although theoretical calculations suggest that small source sizes should perform better than large ones, simulations show that a large angular spread at high intensities results in significant losses of the fast electrons to the sides. A systematic parameter scan suggests an optimal laser intensity. A ratio of 1.6 is demonstrated between the maximum ion temperature and the ion temperature at the front surface.

Mono-energetic ions emission by nanosecond laser solid target irradiation

An experimental campaign aiming to investigate the acceleration mechanisms through laser–matter interaction in nanosecond domain has been carried out at the LENS (Laser Energy for Nuclear Science) laboratory of INFN-LNS, Catania. Pure Al targets were irradiated by 6ns laser pulses at different pumping energies, up to 2J. Advanced diagnostics tools were used to characterize the plasma plume and ion production. We show the preliminary results of this experimental campaign, and especially the ones showing the production of multicharged ions having very narrow energy spreads.