Search

A programme to study photon- and neutron-induced reactions of medical interest, as well as accelerator-based methods of medical radionuclide production, has been instituted at JRC-Geel, making use of both existing and new infrastructure. A new electron beamline that can deliver quasi-monoenergetic beams has been commissioned at the GELINA electron linac and will be primarily dedicated to the study of photonuclear reactions and for medical radioisotope production studies via photon irradiation. The recently renewed MONNET 3.5 MV Tandem accelerator provides light ion beams for reactionbased quasi-mono-energetic neutron production and has been used for the study of 99Mo production via neutron irradiation of molybdenum nanoparticles. In this work we present an overview of the medical radionuclide activities at JRCGeel, with particular attention to aspects of the design, development and operational challenges of the new GELINA electron beamline. Some future perspectives of the programme are also discussed.

The design of new generation fast nuclear reactors requires highly accurate cross-section measurements in the MeV energy region. The 242Pu fission cross section is of particular interest for Pu incineration and nuclear waste production. There are discrepancies around 1 MeV incident neutron energy between libraries and among experimental data. Some data suggest the presence of a strong structure between 1 and 1.2 MeV whereas it is barely visible on some other data and its shape is very different among evaluations. The large majority of the 242Pu(n,f) measurements have been carried out with respect to the 235U(n,f) secondary-standard cross section. This introduces a strong correlation between measurements from different research teams. Moreover, this reference cross section exhibits structures, in particular a steep increase of +10% at 1 MeV. Therefore, we aim to re-measure the 242Pu(n,f) cross section relative to the primary-standard 1H(n,n)p cross section, by using a proton recoil detector. This standard has a very high accuracy (0.4%), is not used for other 242Pu measurements, and is structureless. An experiment has been carried out in October 2022 at the MONNET facility in JRC Geel, with incident neutron energies from 0.9 MeV to 2.0 MeV. The experimental setup will be presented, and the analysis procedure will be detailed.

The VElocity foR Direct particle Identification spectrometer (VERDI) is a 2E-2v fission spectrometer that allows the measurement of the total mass distribution of secondary fission fragments with a resolving power of 1-2 u. It consists of two time-of-flight (ToF) arms, with one Micro Channel Plate (MCP) detector and up to 32 Silicon PIPS (Passive Implanted Planar Silicon) detectors per arm. The MCPs provide the start timing signals and the PIPS detectors provide both the energy and the stopping ToF signals. In real conditions, the PIPS signals are affected by the formation of plasma from the interaction between the heavy ions and the detector material. The plasma contributes to a reduction in signal amplitude, resulting in a Pulse Height Defect (PHD), and introduces a signal delay, known as Plasma Delay Time (PDT). An experiment to characterize the PDT and PHD was performed at the LOHENGRIN recoil separator of the Institut Laue Langevin (ILL). Characteristic fission fragments from the 239Pu(n,f) reaction were separated based on their A/Q and E/Q ratios, allowing the measurement of a wide range of energies from 21 to 110 MeV and masses between 80 and 149 u. Six PIPS detectors were characterized to study their individual responses to the PDT and PHD effects. The signals were recorded in a digital acquisition system to completely exploit the offline analysis capabilities. Achieved combined timing and energy resolutions for fission fragments varied between 72(2) ps and 100(4) ps and 1.4% - 2% (FWHM), respectively. Preliminary PHD and PDT data are presented from the masses A=85, 95, 130 and 143. The PHD trends are strongly correlated with both the ion energy and mass. The PDT, on the other hand, shows a strong variation as a function of the ion kinetic energy but a smaller dependence on the ion mass.

Actinide and lanthanide thin layers with specific requirements regarding thickness, homogeneity, chemical purity, mechanical stability, and backing properties are applied in a multitude of physics and chemistry experiments. A novel target preparation method, the so-called “Drop-on-Demand” (DoD) technique, based on a commercial nanoliter (nL) dispenser is applied since a few years in the Nuclear Chemistry unit at Johannes Gutenberg University Mainz. The wetting behaviour of the nL droplets on the substrate’s surface is a key parameter determining the spatial distribution of the deposited material after evaporation. By switching from aqueous to organic solvents as well as by substrate surface modifications, the wetting behaviour can be influenced. Recent investigations on this influence and applications of the DoD method are presented. The produced actinide deposits were characterized by optical and scanning electron microscopy, by α spectroscopy as well as by radiographic imaging.

In this paper we present results from two recent studies, both related to the emission of prompt fission γ rays. Firstly, we have analyzed data from the reaction 235U(n, f) induced by fast neutrons of average energy E̅n E̅n = 1.7 MeV. The deduced spectral characteristics are an average multiplicity M̅γ M̅γ = 7.11 ± 0.44 γ rays per fission and an average total γ-ray energy release in fission E̅γ,tot E̅γ,tot = 5.51 ± 0.46 MeV, corresponding to an average γ-ray energy ɛ̅γ ɛ̅γ = 0.77 ± 0.08 MeV. Secondly, we have addressed – and answered – the question how those characteristics in general depend on the width of the chosen prompt time window and the timing resolution, determined by the employed detectors and electronics. The conclusion is that once this is known, it is possible to compare results from different experiments in a more meaningful way.

A position-sensitive twin Frisch-grid ionization chamber has been constructed for future photofission experiments using nearly monochromatic, linearly polarized gamma-ray beams. By exchanging the anode plates in the standard ionization chamber on both sides by an array of grid- and strip-anodes, which are rotated by 90° relative to each other and read out by means of resistive charge division, a position sensitivity is achieved that allows the azimuthal fragment emission angle and hence the fission axis orientation to be determined. The performance of this gaseous detector has been studied using the well-known 252Cf spontaneous fission process. The fission axis orientation could be determined relative to an arbitrary axis in space with a resolution better than 7° FWHM. Measured pre-neutron mass and total kinetic energy distributions are consistent with literature, which ensures that the mass and energy resolution for fission fragments is not affected by the position-sensitive structure.

Neutron-induced reaction measurements, e.g. cross-sections and particle emission yields, require samples, called "targets", with specific properties depending on the reaction being studied and the quantities being measured. The target characteristics influence the results of these measurements and can have a strong impact on the total uncertainty of neutron-induced reaction data, which are important for industry and in research. This paper gives an overview of the main techniques applied in the target preparation laboratory at JRC-Geel for production and characterization of targets for neutron-induced reaction data measurements. The use of different targets is demonstrated with a few examples of total and reaction cross-section as well as nuclear fission experiments. In addition, on-going investigations and technical developments are presented.

There exists experimental evidence for strong fluctuations of the average neutron multiplicity from resonance to resonance in 239Pu(n,f). These fluctuations have been shown to impact nuclear reactor benchmarks by reducing the criticality. The fluctuating neutron multiplicity can be explained as a consequence of the competition between direct fission and the (n,γf) process. However, there is also evidence for fluctuations of the fission fragment mass yields from resonance to resonance. The mass yield fluctuations may also contribute to fluctuations of the neutron multiplicity averaged over all fission fragment masses. In order to model the contribution to the neutron multiplicity fluctuations by the fission fragment mass yield fluctuations new data on the correlations between fission fragment properties and neutron multiplicities are in need. We present experiments carried out to determine prompt neutron multiplicity correlations with fission fragment masses and total kinetic energies in the reaction 239Pu(n,f). The experiment has been performed at the GELINA facility at JRC-Geel. A twin position-sensitive Frisch-grid ionization chamber is used for fission fragment identification via the double kinetic energy technique. An array of scintillation detectors is employed for neutron counting. Correlations between average neutron multiplicities and fission fragment properties have been measured with improved resolution in both mass and TKE, compared to data from the literature.

In a recent measurement of prompt γ rays from the spontaneous fission of 252Cf an experimental setup was chosen that allowed the study of angular correlations between γ rays and the nuclei from which they were emitted. The observed angular distribution of prompt fission γ rays was then analyzed to estimate the relative contributions from radiation of different multipolarity. Preliminary results are presented and compared to previous angular correlationmeasurements from different fission processes and recent results from calculations with the Monte Carlo Hauser-Feshbach code FIFRELIN.

New standard (n,f) cross sections other than 235U are important to study the relevant cross sections for Generation-IV power plants. A specific need for such standards is for performing new experiments with quasimonoenergetic neutron beams, such as those produced by Van de Graaf accelerators. Neutrons down-scattered to low energies in the experimental environment, so called room-return, become relevant for this type of measurements. Hence, a standard (n,f) cross section with a fission threshold is of great interest, in order to suppress the contribution from room-return background. For this reason we have performed two experiments at the VDG of the National Physical Laboratory to measure absolutely the (n,f) cross sections of 235U, 238U and 237Np in the fast neutron energy region. Our preliminary results are in agreement with the most up-to-date evaluations.

A recent set-up of a multi-cathode Frisch-grid ionization chamber and experimental results of a proof-of-principle experiment are presented. Preliminary data on the obtained polar angular and mass distributions as well as total kinetic energy of fission fragments produced in neutron-induced fission of 232Th and 238U are discussed that show that the chamber has been operated successfully. For the additional measurement of the azimuthal angular distribution, a design of segmented anodes has been tested. Preliminary data do not allow a suffcient reconstruction of the azimuthal angle.

In a recent measurement of prompt γ rays from the spontaneous fission of 252Cf an experimental setup was chosen that allowed the study of angular correlations between γ rays and the nuclei from which they were emitted. The observed angular distribution of prompt fission γ rays was then analyzed to estimate the relative contributions from radiation of different multipolarity. First preliminary results are presented and compared to previous angular correlation measurements from different fission processes and recent results from calculations with the Monte Carlo Hauser-Feshbach code FIFRELIN.

Nowadays, there is an increased interest in a complete study of the neutron-induced fission of 237Np. This is due to the need of accurate and reliable nuclear data for nuclear science and technology. 237Np is generated (and accumulated) in the nuclear reactor core during reactor operation. As one of the most abundant long-lived isotopes in spent fuel (“waste”), the incineration of 237Np becomes an important issue. One scenario for burning of 237Np and other radio-toxic minor actinides suggests they are to be mixed into the fuel of future fast-neutron reactors, employing the so-called transmutation and partitioning technology. For testing present fission models, which are at the basis of new generation nuclear reactor developments, highly accurate and detailed neutron-induced nuclear reaction data is needed. However, the EXFOR nuclear database for 237Np on neutron-induced capture cross-section, σγ, and fission cross-section, σf, as well as on the characteristics of capture and fission resonance parameters (Γγ, Γf, σoΓf, fragments mass-energy yield distributions, multiplicities of neutrons vn and γ-rays vγ), has not been updated for decades.

Recent years have seen an increased interest in prompt fission γ-ray (PFG) measurements motivated by a high priority request of the OECD/NEA for high precision data, mainly for the nuclear fuel isotopes 235U and 239Pu. Our group has conducted a PFG measurement campaign using state-of-the-art lanthanum halide detectors for all the main actinides to a precision better than 3%. The experiments were performed in a coincidence setup between a fission trigger and γ-ray detectors. The time-of-flight technique was used to discriminate photons, traveling at the speed of light, and prompt fission neutrons. For a full rejection of all neutrons below 20 MeV, the PFG time window should not be wider than a few nanoseconds. This window includes most PFG, provided that no isomeric states were populated during the de-excitation process. When isomeric states are populated, PFGs can still be emitted up to 1 yus after the instant of fission or later. To study these γ-rays, the detector response to neutrons had to be determined and a correction had to be applied to the γ-ray spectra. The latest results for PFG characteristics from the reaction 239Pu(nth,f) will be presented, together with an analysis of PFGs emitted up to 200 ns after fission in the spontaneous fission of 252Cf as well as for thermal-neutron induced fission on 235U and 239Pu. The results are compared with calculations in the framework of the Hauser-Feshbach Monte Carlo code CGMF and FIFRELIN.

In a recent measurement of prompt γ rays from the spontaneous fission of 252Cf an experimental setup was chosen that allowed the study of angular correlations between γ rays and the nuclei from which they were emitted. The observed angular distribution of the prompt fission γ rays was then analyzed to estimate the relative contributions from radiation of different multipolarity. From that we hope to obtain more detailed information about the early stage of the de-excitation process of fission fragments, right after prompt neutron emission. First preliminary results are presented below.

The determination of nuclear level densities and radiative strength functions is one of the most important tasks in low-energy nuclear physics. Accurate experimental values of these parameters are critical for the study of the fundamental properties of nuclear structure. The step-like structure in the dependence of the level densities p on the excitation energy of nuclei Eex is observed in the two-step gamma cascade measurements for nuclei in the 28 ≤ A ≤ 200 mass region. This characteristic structure can be explained only if a co-existence of quasi-particles and phonons, as well as their interaction in a nucleus, are taken into account in the process of gamma-decay. Here we present a new improvement to the Dubna practical model for the determination of nuclear level densities and radiative strength functions. The new practical model guarantees a good description of the available intensities of the two step gamma cascades, comparable to the experimental data accuracy.

Experimental activities at JRC-Geel on prompt fission neutron (PFN) emission in response to OECD/NEA nuclear data requests are presented in this contribution. Specifically, on-going investigations of PFN emission from the reaction 235U(n,f) in the region of the resolved resonances, taking place at the GELINA facility, are presented. The focus of this contribution lies on studies of PFN correlations with fission fragment properties. The experiment employs a scintillation detector array for neutron detection, while fission fragment properties are determined via the double kinetic energy technique using a position sensitive twin ionization chamber. This setup allows us to study several correlations between properties of neutron and fission fragments simultaneously. Results on PFN correlations with fission fragment properties from the present study differ significantly from earlier studies on this reaction, induced by thermal neutrons.

This work aims at measuring prompt-fission neutrons at different excitation energies of the nucleus. Two independent techniques, the 2E-2v and the 2E techniques, are used to map the characteristics of the mass-dependent prompt fission neutron multiplicity, v(A), when the excitation energy is increased. The VERDI 2E-2v spectrometer is being developed at JRC-GEEL. The Fission Fragment (FF) energies are measured using two arrays of 16 silicon (Si) detectors each. The FFs velocities are obtained by time-of-flight, measured between micro-channel plates (MCP) and Si detectors. With MCPs placed on both sides of the fission source, VERDI allows for independent timing measurements for both fragments. 252Cf(sf) was measured and the present results revealed particular features of the 2E-2v technique. Dedicated simulations were also performed using the GEF code to study important aspects of the 2E-2v technique. Our simulations show that prompt neutron emission has a non-negligible impact on the deduced fragment data and affects also the shape of v(A). Geometrical constraints lead to a total-kinetic energy-dependent detection efficiency. The 2E technique utilizes an ionization chamber together with two liquid scintillator detectors. Two measurements have been performed, one of 252Cf(sf) and another one of thermal-neutron induced fission in 235U(n,f). Results from 252Cf(sf) are reported here.

Investigations of prompt fission neutron (PFN) emission are of importance in understanding the fission process in general and the sharing of excitation energy among the fission fragments in particular. Experimental activities at JRC-Geel on PFN emission in response to OECD/NEA nuclear data requests is presented in this contribution. The focus lies on on-going investigations of PFN emission from the reaction 235U(n,f) in the region of the resolved resonances taking place at the GELINA facility. For this reaction strong fluctuations of fission fragment mass distributions and mean total kinetic energy have been observed as a function of incident neutron energy in the resonance region. In addition, fluctuations of prompt neutron multiplicities have also been observed. The goal of the present study is to verify the current knowledge of PFN multiplicity fluctuations and to study correlations with fission fragment properties. The experiment employs a scintillation detector array for neutron detection, while fission fragment properties are determined via the double kinetic energy technique using a position sensitive twin ionization chamber. Results on PFN multiplicity correlations with fission fragment properties from the present study show significant differences compared to earlier studies on this reaction, induced by thermal neutrons. Specifically, the total kinetic energy dependence of the neutron multiplicity per fission shows an inverse slope FX1TKE/FX2ν approximately 35% weaker than observed in earlier studies of thermal neutron induced fission on 235U. The inverse slope is related to the energy carried away per emitted neutron and is, thereby, closely connected to the energy balance of the fission reaction. The present result should have strong impact on the modeling of both prompt neutron and prompt γ-ray emission in fission of the 236U compound nucleus.

The nuclear de-excitation process of fission fragments (FF) provides fundamental information for the understanding of nuclear fission and nuclear structure in neutron-rich isotopes. The variation of the prompt-neutron multiplicity, ν(A), as a function of the incident neutron energy (En) is one of many open questions. It leads to significantly different treatments in various fission models and implies that experimental data are analyzed based on contradicting assumptions. One critical question is whether the additional excitation energy (Eexc) is manifested through an increase of ν(A) for all fragments or for the heavy ones only. A systematic investigation of ν(A) as a function of En has been initiated. Correlations between prompt-fission neutrons and fission fragments are obtained by using liquid scintillators in conjunction with a Frisch-grid ionization chamber. The proof-of-principle has been achieved on the reaction 235U(nth,f) at the Van De Graff (VdG) accelerator of the JRC-Geel using a fully digital data acquisition system. Neutrons from 252Cf(sf) were measured separately to quantify the neutron-scattering component due to surrounding shielding material and to determine the intrinsic detector efficiency. Prelimenary results on ν(A) and spectrum in correlation with FF properties are presented.

As a consequence of recent experimental results, previously established systematics for prompt fission γ-ray spectra (PFGS) characteristics as function of both atomic and mass number of the compound system have been revised. Although based on purely empirical dependences, it allows estimating average gamma-ray multiplicity, mean and total photon energy in cases, where the target nuclei are either not available or not accessible experimentally. Based on this systematics, we show in this paper that PFGS characteristics may also be predicted for fission induced by fast neutrons. Our calculations were performed for the target nuclei 238U, 235U and 239Pu in the neutron energy range from 0 to 20 MeV, and the results are compared to existing experimental and theoretical values.

Benchmark reactor calculations have revealed an underestimation of γ-heat following fission of up to 28%. To improve the modelling of new nuclear reactors, the OECD/NEA initiated a nuclear data High Priority Request List (HPRL) entry for the major isotopes (235U, 239Pu). In response to that HPRL entry, we executed a dedicated measurement program on prompt fission γ-rays employing state-of-the-art lanthanum bromide (LaBr3) detectors with superior timing and good energy resolution. Our new results from 252Cf(sf), 235U(nth,f) and 241Pu(nth,f) provide prompt fission γ-ray spectra characteristics : average number of photons per fission, average total energy per fission and mean photon energy; all within 2% of uncertainty. We present preliminary results on 239Pu(nth,f), recently measured at the Budapest Neutron Centre and supported by the CHANDA Trans-national Access Activity, as well as discussing our different published results in comparison to the historical data and what it says about the discrepancy observed in the benchmark calculations.

VERDI (VElocity foR Direct particle Identification) is a fission-fragment spectrometer recently put into operation at JRC-Geel. It allows measuring the kinetic energy and velocity of both fission fragments simultaneously. The velocity provides information about the pre-neutron mass of each fission fragment when isotropic prompt-neutron emission from the fragments is assumed. The kinetic energy, in combination with the velocity, provides the post-neutron mass. From the difference between pre- and post-neutron masses, the number of neutrons emitted by each fragment can be determined. Multiplicity as a function of fragment mass and total kinetic energy is one important ingredient, essential for understanding the sharing of excitation energy between fission fragments at scission, and may be used to benchmark nuclear de-excitation models. The VERDI spectrometer design is a compromise between geometrical efficiency and mass resolution. The spectrometer consists of an electron detector located close to the target and two arrays of silicon detectors, each located 50 cm away from the target. In the present configuration pre-neutron and post-neutron mass distributions are in good agreement with reference data were obtained. Our latest measurements performed with spontaneously fissioning 252Cf is presented along with the developed calibration procedure to obtain pulse height defect and plasma delay time corrections.

The investigation of prompt γ-ray emission in nuclear fission has a great relevance for the assessment of prompt heat generation in a reactor core and for the better understanding of the de-excitation mechanism of fission fragments. Some years ago experimental data was scarce and available only from a few fission reactions, 233,235U(nth, f), 239Pu(nth, f), and 252Cf(sf). Initiated by a high priority data request published by the OECD/NEA a dedicated prompt fission γ-ray measurement program is being conducted at the Joint Research Centre Geel. In recent years we obtained new and accurate prompt fission γ-ray spectrum (PFGS) characteristics (average number of photons per fission, average total energy per fission and mean photon energy) from 252Cf(sf), 235U(nth, f) and 239,241Pu(nth, f) within 2% of uncertainty. In order to understand the dependence of prompt fission γ-ray emission on the compound nuclear mass and excitation energy, we started a first measurement campaign on spontaneously fissioning plutonium and curium isotopes. Results on PFGS characteristics from 240,242Pu(sf) show a dependence on the fragment mass distribution rather than on the average prompt neutron multiplicity, pointing to a more complex competition between prompt fission γ-ray and neutron emission.

For investigation of the basic characteristics of 14.1 MeV neutron induced nuclear reactions on a number of important isotopes for nuclear science and engineering, a new experimental setup TANGRA has been constructed at the Frank Laboratory of Neutron Physics of the Joint Institute for Nuclear Research in Dubna. For testing its performance, the angular distribution of γ-rays (and neutrons) from the inelastic scattering of 14.1 MeV neutrons on high-purity carbon was measured and the angular anisotropy of γ-rays from the reaction 12C(n, n′γ)12C was determined. This reaction is important from fundamental (differential cross-sections) and practical (non-destructive elemental analysis of materials containing carbon) point of view. The preliminary results for the anisotropy of the γ-ray emission from the inelastic scattering of 14.1- MeV neutrons on carbon are compared with already published literature data. A detailed data analysis for determining the correlations between inelastic scattered neutron and γ-ray emission will be published elsewhere.

Investigations of prompt emission in fission is of importance in understanding the fission process in general and the sharing of excitation energy among the fission fragments in particular. Experimental activities at IRMM on prompt neutron emission from fission in response to OECD/NEA nuclear data requests is presented in this contribution. Main focus lies on currently on-going investigations of prompt neutron emission from the reaction 235U(n,f) in the region of the resolved resonances. For this reaction strong fluctuations of fission fragment mass distributions and mean total kinetic energy have been observed [Nucl. Phys. A 491, 56 (1989)] as a function of incident neutron energy in the resonance region. In addition fluctuations of prompt neutron multiplicities were also observed [Phys. Rev. C 13, 195 (1976)]. The goal of the present study is to verify the current knowledge of prompt neutron multiplicity fluctuations and to study correlations with fission fragment properties.