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There exists experimental evidence for strong fluctuations of the average neutron multiplicity from resonance to resonance in Pu-239(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,gamma f) 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 Pu-239(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., QC 20210503

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, 7(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. Cf-252(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 17(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 Cf-252(sf) and another one of thermal-neutron induced fission in U-235(n,f). Results from Cf-252(sf) are reported here.

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.

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.

For nuclear modelling and improved evaluation of nuclear data, knowledge of fluctuations of the prompt neutron multiplicity as a function of incident neutron energy is requested for the major actinides 235U and 239Pu. Experimental investigations of the prompt fission neutron emission in resonance-neutron induced fission on 235U are taking place at the GELINA facility of the IRMM. The experiment employs an array of scintillation detectors (SCINTIA) in conjunction with a newly designed 3D position-sensitive twin Frisch-grid ionization chamber. In addition, the mass-dependent prompt neutron multiplicity, (A), has attracted particular attention. Recent, sophisticated nuclear fission models predict that the additional excitation energy, brought into the fission system at higher incident neutron energies, leads to an increased neutron multiplicity only for heavy fragments, as observed in the 237Np(n,f) reaction. A first feasibility study has been performed at the JRC-IRMM VdG accelerator to measure nu(A) for 235U(n,f).

Pu-240 has recently been pointed out by a sensitivity study of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) to be one of the isotopes whose fission cross section lacks accuracy to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). In the High Priority Request List (HPRL) of the OECD, it is suggested that the knowledge of the Pu-240(n, f) cross section should be improved to an accuracy within 1-3 %, compared to the present 5%. A measurement of the Pu-240 cross section has been performed at the Van de Graaff accelerator of the Joint Research Center (JRC) Institute for Reference Materials and Measurements (IRMM) using quasi-monoenergetic neutrons in the energy range from 0.5 MeV to 3 MeV. A twin Frisch-grid ionization chamber (TFGIC) has been used in a back-to-back configuration as fission fragment detector. The Pu-240(n, f) cross section has been normalized to three different isotopes: Np-237(n, f), U-235(n, f), and U-238(n, f). Additionally, the secondary standard reactions were benchmarked through measurements against the primary standard reaction U-235(n, f) in the same geometry. A comprehensive study of the corrections applied to the data and the associated uncertainties is given. The results obtained are in agreement with previous experimental data at the threshold region. For neutron energies higher than 1 MeV, the results of this experiment are slightly lower than the ENDF/B-VII.1 evaluation, but in agreement with the experiments of Laptev et al. (2004) as well as Staples and Morley (1998)., Postprint (published version)

A sensitivity analysis for the new generation of fast reactors [Salvatores (2008)] has shown the importance of improved cross section data for several actinides. Among them, the240,242Pu(n,f) cross sections require an accuracy improvement to 1-3% and 3-5%, respectively, from the current level of 6% and 20%. At the Van de Graaff facility of the Institute for Reference Materials and Measurements (JRC-IRMM) the fission cross section of the two isotopes was measured relative to two secondary standard reactions,237Np(n,f) and238U(n,f), using a twin Frisch-grid ionization chamber. The secondary standard reactions were benchmarked through measurements against the primary standard reaction235U(n,f) in the same geometry. Sample masses were determined by means of low-geometry alpha counting or/and a 2p Frisch-grid ionization chamber, with an uncertainty lower than 2%. The neutron flux and the impact of scattering from material between source and target was examined, the largest effect having been found in cross section ratio measurements between a fissile and a fertile isotope. Our240,242Pu(n,f) cross sections are in agreement with previous experimental results and slightly lower than present evaluations. In case of the242Pu(n,f) reaction no evidence for a resonance at En=1.1 MeV was found., Postprint (published version)

Fast spectrum neutron-induced fission cross-section data for transuranic isotopes are of special demand from the nuclear data community. In particular highly accurate data are needed for the new generation IV nuclear applications. The aim is to obtain precise neutron-induced fission cross sections for 240Pu and 242Pu. To do so, accurate data on spontaneous fission half-lives must be available. Also, minimizing uncertainties in the detector efficiency is a key point. We studied both isotopes by means of a twin Frisch-grid ionization chamber with the goal of improving the present data on the neutron-induced fission cross section. For the two plutonium isotopes the high a-particle decay rates pose a particular problem to experiments due to piling-up events in the counting gas. Argon methane and methane were employed as counting gases, the latter showed considerable improvement in signal generation due to its higher drift velocity. The detection efficiency for both samples was determined, and improved spontaneous fission half-lives were obtained with very low statistical uncertainty (0.13% for 240Pu and 0.04% for 242Pu): for 240Pu, T 1/2,SF=1.165×1011 yr (1.1%), and for 242Pu, T 1/2,SF=6.74×1010 yr (1.3%). Systematic uncertainties are due to sample mass (0.4% for 240Pu and 0.9% for 242Pu) and efficiency (1%). © 2013 American Physical Society., Postprint (published version)

Ionization chambers with Frisch grids have been very successfully applied to neutron-induced fission-fragment studies during the past 20 years. They are radiation resistant and can be easily adapted to the experimental conditions. The use of Frisch grids has the advantage to remove the angular dependency from the charge induced on the anode plate. However, due to the Grid Inefficiency (GI) in shielding the charges, the anode signal remains slightly angular dependent. The correction for the GI is, however, essential to determine the correct energy of the ionizing particles. GI corrections can amount to a few percent of the anode signal. Presently, two contradicting correction methods are considered in literature. The first method adding the angular-dependent part of the signal to the signal pulse height; the second method subtracting the former from the latter. Both additive and subtractive approaches were investigated in an experiment where a Twin Frisch-Grid Ionization Chamber (TFGIC) was employed to detect the spontaneous fission fragments (FF) emitted by a 252Cf source. Two parallel-wire grids with different wire spacing (1 and 2 mm, respectively), were used individually, in the same chamber side. All the other experimental conditions were unchanged. The 2 mm grid featured more than double the GI of the 1 mm grid. The induced charge on the anode in both measurements was compared, before and after GI correction. Before GI correction, the 2 mm grid resulted in a lower pulse-height distribution than the 1 mm grid. After applying both GI corrections to both measurements only the additive approach led to consistent grid independent pulse-height distributions. The application of the subtractive correction on the contrary led to inconsistent, grid-dependent results. It is also shown that the impact of either of the correction methods is small on the FF mass distributions of 235U(nth, f).

A recent theoretical approach concerning the grid-inefficiency (GI) problem in Twin Frisch–Grid Ionization Chambers was validated experimentally. The experimental verification focused on the induced signal on the anode plate. In this work the investigation was extended by studying the grid signal. The aim was to verify the grid-signal dependency on the grid inefficiency σ. The measurements were made with fission fragments from 252Cf(sf), using two different grids, with 1 and 2 mm wire distances, leading to the GI values: σ=0.031 and σ=0.083, respectively. The theoretical grid signal was confirmed because the detected grid pulse-height distribution was smaller for the larger σ. By applying the additive GI correction approach, the two grid pulse heights were consistent. In the second part of the work, the corrected grid signal was used to deduce emission angles of the fission fragments. It is inconvenient to treat the grid signal by means of conventional analogue electronics, because of its bipolarity. Therefore, the anode and grid signals were summed to create a unipolar, angle-dependent pulse height. Until now the so-called summing method has been the well-established approach to deduce the angle from the grid signal. However, this operation relies strongly on an accurate and stable calibration between the two summed signals. By application of digital-signal processing, the grid signal's bipolarity is no longer an issue. Hence one can bypass the intermediate summation step of the two different pre-amplifier signals, which leads to higher stability. In this work the grid approach was compared to the summing method in three cases: 252Cf(sf), 235U(n,f) and 234U(n,f). By using the grid directly, the angular resolution was found equally good in the first case but gave 7% and 20% improvements, respectively, in the latter cases.

The neutron-induced fission of 234U has been studied for neutron energies ranging from 200 keV to 5 MeV. Special focus was put around the prominent vibrational resonance in the sub-barrier region around 800 keV incident neutron energy. The aim was to investigate the fission fragment (FF) characteristics and search for fluctuations in energy and mass distributions. The strong angular anisotropy in the case of 234U(n,f) was verified and correlations with changes in energy and mass distributions were found. The TKE around the resonance increases contrary to earlier literature data. Furthermore, the TKE and mass distribution were found to be dependent on emission angle. At the resonance, the TKE was smallest near the 0° emission of the FF. This effect was consistent and coherent with a change in the mass distribution around the resonance. The mass distribution was observed to be less asymmetric near 0° emission. From a fitting analysis based on the Multi-Modal Random Neck-Rupture (MMRNR) model, we found the yield of the standard-1 mode increasing around the resonance. Because the TKE is increasing at larger angles and the mass distribution becomes more symmetric also at larger angles, we conclude that this behavior is due to an increase of the standard-1 mode at these larger angles. Based on the formalism of MMRNR, such difference in angular distribution may be an indication of a different outer barrier height for the standard-1 and standard-2 modes.

This study on 234U(n,f) focused on the vibrational resonance at the incident neutron energy En=770 keV. Due to the strong angular anisotropy, Fluctuations of the fission fragment (FF) properties were predicted. The bipolar angular anisotropy was verified in this work and a possible new correlation to anisotropic FF emission has been observed. The mass distribution was found to have the biggest difference in asymmetry, at the vibrational resonance and was less asymmetric in emission along the axis of the beam direction. A corresponding anisotropy in the total kinetic energy was also observed. The observed effect was consistent with the change in the mass distribution. At last, the experimental data were fitted based on the Multi-Modal Random Neck Rupture (MM-RNR) model. The yield of the standard-1 mode was found to increase at the resonance.

In this paper we demonstrate the employment of LaCl3 : Ce scintillation detectors for the identification of prompt fission gamma-rays from gamma-radiation in contrast to other reactions. We present the properties of cylindrical 1.5 in. x 1.5 in. detectors in terms of intrinsic activity, energy resolution, intrinsic full peak efficiency and intrinsic timing resolution. In addition, we show results from the measurement of gamma-rays emitted in coincidence with the spontaneous fission of Cf-252, which lead us to the conclusion that the properties of the detectors used in this work, in particular the good timing resolution and a reasonably good energy resolution, are more than just sufficient for the assessment of prompt gamma-heat in future nuclear reactors as requested by the OECD. Hence, in our opinion, LaCl3 : Ce detectors, compared to those made out of LaBr3 : Ce crystals, represent an appropriate and quasi low-cost choice for the above mentioned applications.

In the present investigation the performance of digital data acquisition (DA) and analogue data acquisition (AA) systems are compared in neutron-induced fission experiments. The DA results are practically identical to the AA results in terms of angular-, energy- and mass-resolution, and both compare very well with literature data. However, major advantages were found with the digital techniques. DA allows for a very efficient αparticle pile-up correction. This is important when considering the accurate measurement of fission-fragment characteristics of highly αactive actinide isotopes relevant for the safe operation of Generation IV reactors and the successful reduction of long-lived radioactive nuclear waste. In case of a strong αemitter, when applying the αparticle pile-up correction, the peak-to-valley ratio of the energy distribution was significantly improved. In addition, DA offers a very flexible expanded off-line analysis and reduces the number of electronic modules drastically, leading to an increased stability against electronic drifts when long measurement times are required.

Recent fission cross-section calculations for the reaction 238U(n, f ), based on an extended statistical model, predict a significant change of fission fragment properties, such as the mean mass by A = 1.5 and a notable increase in total kinetic energy in the region of the vibrational resonance at an incident neutron energy En = 0.9 MeV. This model includes individual fission cross-sections by the asymmetric standard 1 (S1) and standard 2 (S2) as well as the symmetric super-long (SL) mode. In order to verify the model predictions, a dedicated experiment on 238U has been carried out to measure fission-fragment mass yield distributions for incident neutron energies from En = 2.0 MeV down to 0.9 MeV, where the fission characteristics at the vibrational resonance at En = 0.9 MeV were investigated for the first time. The previously reported distinct structure in the angular anisotropy around En = 1.2 and 1.6 MeV wasobserved at En = 0.9 MeV as well. The predicted large changes in fission fragment mass yield and total kinetic energy could not be confirmed. In the resonance the mean total kinetic energy is only about 0.5 MeV higher than at En = 1.8 MeV. At the same time, a slight decrease of the mean heavy fragment mass was observed, probably indicating a slightly increased contribution of the S1 fission mode.

A new spectrometer has been built at the EC-JRC IRMM to investigate isomer decay in the millisecond range and activation cross sections of isotopes, where isomeric states exist and are populated. The spectrometer is equipped with high-resolution gamma-ray detectors and an ionisation chamber for the measurement of charged particles, e.g., fission fragments. NEPTUNE provides pulsed quasi mono-energetic neutrons at pulse repetition frequencies up to 5 kHz and tuneable neutron pulse widths ranging from 10 µs into the ms-region. For this purpose a beam chopper based on a parallel-plate capacitor has been integrated into the accelerator beam line in order to deflect the charged-particle beam onto a tantalum beam dump. First research has been performed with the NEPTUNE spectrometer dedicated to the shape isomer search in the odd-A uranium isotopes 235U, 237U and 239U. In further experiments the population of long-lived spin isomers was investigated.

Although the recoil mass-separator LOHENGRIN at Institute Laue-Langevin was originally designed for the spectrometry of binary fission fragments, it was also used in the past for measuring light-charged particles from ternary fission. However, due to limited electric field settings the energy distribution of the lightest particles was not completely accessible. In this contribution we report on an energy degrader technique that allows the measurement of the entire energy spectra of ternary particles with LOHENGRIN. We demonstrate how the measured particle spectra are distorted by the energy degrader and present results from a Monte Carlo simulation that shows how the original energy distributions are reconstructed. Finally, we apply this procedure to experimental data of ternary particles from the reaction 235U(nth, f).

Quantitative predictions of fission product yields are relevant for the reliable operation of different modern nuclear applications. This concerns the realistic characterizations of the radio-toxicity of the fuel elements after the envisaged extended irradiation, as well as sub-critical assemblies, where the number of delayed neutrons from minor actinides is determined by the characteristic emission yields of the corresponding so-called pre-cursor isotopes. However, to be able to make more reliable quantitative predictions of fission characteristics requires the better understanding of the fission process itself. For this purpose a better knowledge about the distinct structure of the nuclear energy landscape around the fission barrier is indispensable. In particular, the question should be answered, whether the fission barrier is either double- or triple-humped or even multi-humped as been proposed within the multi-modal neck rupture model. Despite quite some effort based on different experimental techniques and theoretical approaches, this question remains still unanswered. There is still no consistent picture of the fission barrier available and hence, different sets of barrier parameters are in use, unable to describe the different observed phenomena in a coherent way. With the systematic investigation of shape isomer population, its decay modes as well as the branching ratio, precise information can be obtained to resolve the puzzling situation. The experimental approach will be discussed and results from first experiments presented.

The shape isomer in 235U has been searched for in a neutron-induced fission experiment on 234U, which was performed at the isomer spectrometer NEPTUNE of the EC-JRC IRMM. A neutron source, with a tunable pulse frequency in the Hz to kHz range and its individually adjustable neutron pulse width in connection with an appropriate detector system turned out to be the ideal instrument to perform an isomer search, when decay half-lives above 100 us are expected. From the delayed fission events observed for two different NEPTUNE settings and at mean incident neutron energies En = 0.95 and 1.27 MeV the isomeric fission half-life could be determined to be T_1/2 = (3.6 ± 1.8) ms. The corresponding cross section was determined to sigma_if = (10 ± 8) ub. With these results an experimental confirmation for the existence of a superdeformed shape isomer in odd-uranium isotopes is given for the first time., Artikelnummer: 042502

For mass numbers A = 80 to 124 the recoil mass spectrometer LOHENGRIN of the Institute Laue-Langevin in Grenoble was used to measure with high resolution the light fission-fragment mass yields and kinetic energy distributions from thermal-neutron induced fission of 252Cf* for the first time, using 251Cf as target material. The obtained mean light fragment mass AL = (107 ± 2) and the corresponding mean kinetic energy Ek,L = (103±2) MeV are within the expected trend. Emission yields around A = 115 are enhanced and the corresponding mean kinetic energy is higher compared to spontaneous fission of 252Cf. This could be explained by the existence of an additional super-deformed fission mode.

The recoil mass-separator LOHENGRIN at Institute Laue-Langevin was originally designed for the spectrometry of binary fission fragments. Nevertheless, it was also used in the past for measuring light-charged particles from ternary fission. However, due to the electric field settings the energy distribution of the lightest particles was not completely accessible, which made the determination of mean kinetic energies, widths and, hence, emission yields difficult. In this paper we present an energy degrader technique that allows for the measurement of the entire energy spectrum of even the lightest ternary particles with LOHENGRIN.