PKA Spectra Research Articles

Recommendation for computing neutron irradiation damage from evaluated nuclear data

Accurate evaluation of displacement damage is important for studying the nuclear materials after irradiation. The present work investigates neutron-induced displacement damage evaluation via damage cross sections. There are potential discrepancies between different evaluations on the damage cross sections induced by the (n,γ) reaction and potential discontinuity at 20 MeV incident neutron energy. These two issues are however not important for evaluating neutron irradiation damage in fission and fusion reactors. Due to some issues associated with the recoil distributions in evaluated nuclear data files, the corresponding damage cross sections are questionable, such as those of 52Cr in JEFF-3.3, 55Mn in JEFF-3.3 and ENDF/B-VIII.0, and 180,182,183,184,186W in ENDF/B-VIII.0. Therefore, the present work recommends using two-body kinematic considerations and the differential cross sections of light particles for evaluating neutron irradiation damage (via either displacement cross sections or PKA spectra), unless the recoil distributions have been pre-validated/verified. The recommended method reduces the 70% discrepancy between different nuclear data evaluations to 13% for evaluated displacement damage of tungsten in ITER tokamak.

Differential dpa calculations with SPECTRA-PKA

The processing code SPECTRA-PKA produces energy spectra of primary atomic recoil events (or primary knock-on atoms, PKAs) for any material composition exposed to an irradiation spectrum. Such evaluations are vital inputs for simulations aimed at understanding the evolution of damage in irradiated material, which is generated in cascade displacement events initiated by PKAs. These PKA spectra present the full complexity of the input (to SPECTRA-PKA) nuclear data-library evaluations of recoil events. However, the commonly used displacements per atom (dpa) measure, which is an integral measure over all possible recoil events of the displacement damage dose, is still widely used and has many useful applications – as both a comparative and correlative quantity. This paper describes the methodology employed that allows the SPECTRA-PKA code to evaluate dpa rates using the energy-dependent recoil (PKA) cross section data used for the PKA distributions. This avoids the need for integral displacement kerma cross sections and also provides new insight into the relative importance of different reaction channels (and associated different daughter residual and emitted particles) to the total integrated dpa damage dose. Results are presented for Fe, Ni, W, and SS316. Fusion dpa rates are compared to those in fission, highlighting the increased contribution to damage creation in the former from high-energy threshold reactions.

FISPACT-II: An Advanced Simulation System for Activation, Transmutation and Material Modelling

Fispact-II is a code system and library database for modelling activation-transmutation processes, depletion-burn-up, time dependent inventory and radiation damage source terms caused by nuclear reactions and decays.The Fispact-II code, written in object-style Fortran, follows the evolution of material irradiated by neutrons, alphas, gammas, protons, or deuterons, and provides a wide range of derived radiological output quantities to satisfy most needs for nuclear applications. It can be used with any ENDF-compliant group library data for nuclear reactions, particle-induced and spontaneous fission yields, and radioactive decay (including but not limited to TENDL-2015, ENDF/B-VII.1, JEFF-3.2, JENDL-4.0u, CENDL-3.1 processed into fine-group-structure files, GEFY-5.2 and UKDD-16), as well as resolved and unresolved resonance range probability tables for self-shielding corrections and updated radiological hazard indices. The code has many novel features including: extension of the energy range up to 1 GeV; additional neutron physics including self-shielding effects, temperature dependence, thin and thick target yields; pathway analysis; and sensitivity and uncertainty quantification and propagation using full covariance data.The latest ENDF libraries such as TENDL encompass thousands of target isotopes. Nuclear data libraries for Fispact-II are prepared from these using processing codes PREPRO, NJOY and CALENDF. These data include resonance parameters, cross sections with covariances, probability tables in the resonance ranges, PKA spectra, kerma, dpa, gas and radionuclide production and energy-dependent fission yields, supplemented with all 27 decay types. All such data for the five most important incident particles are provided in evaluated data tables.The Fispact-II simulation software is described in detail in this paper, together with the nuclear data libraries. The Fispact-II system also includes several utility programs for code-use optimisation, visualisation and production of secondary radiological quantities. Included in the paper are summaries of results from the suite of verification and validation reports available with the code.

Mechanical properties and plasticity size effect of Fe-6%Cr irradiated by Fe ions and by neutrons

The mechanical behaviour of Fe6%Cr in the un-irradiated, self-ion irradiated and neutron irradiated conditions was measured and compared. Irradiations were performed to the same dose and at the same temperature but to very different damage rates for both methods. The materials were tested using nanoindentation and micromechanical testing, and compared with microstructural observations from Transmission Electron Microscopy (TEM) and Atom Probe Tomography (APT) reported elsewhere. Irradiated and un-irradiated micro-cantilevers with a wide range of dimensions were used to study the interrelationships between irradiation hardening and size effects in small-scale plasticity. TEM and APT results identified that the dislocation loop densities were ∼2.9 × 1022m−3 for the neutron irradiated material and only 1.4 × 1022m−3 for the ion irradiated material. Cr segregation to loops was only found for the neutron-irradiated material. The nanoindentation hardness increase due to neutron irradiation was 3 GPa and that due to ion irradiation 1 GPa. The differences between the effects of the two irradiation types are discussed, taking into account inconsistencies in damage calculations, and the differences in PKA spectra, dose rate and transmutation products for the two irradiation types.

PKA distributions: Contributions from transmutation products and from radioactive decay

The neutrons generated in fusion plasmas interact with materials via nuclear reactions. The resulting transmutations and atomic displacements have life-limiting consequences for fusion reactor components. A detailed understanding of the production, evolution and material consequences of the damage created by cascades of atomic displacements requires, as a vital primary input, a complete description of the energy-spectrum of initial (prompt) atomic displacement events (the primary knock on atoms or PKAs) produced by direct neutron nuclear interactions. There is also the possibility that the radionuclides produced under transmutation will create further PKAs as they decay, and so the rate of these must also be quantified. This paper presents the latest results from the analysis of PKA spectra under neutron irradiation, focussing particularly on the variation in PKA distributions due to changes in composition under transmutation, but also on the PKA contributions from radioactive decay of materials that become activated under irradiation.

Energy spectra of primary knock-on atoms under neutron irradiation

Materials subjected to neutron irradiation will suffer from a build-up of damage caused by the displacement cascades initiated by nuclear reactions. Previously, the main “measure” of this damage accumulation has been through the displacements per atom (dpa) index, which has known limitations. This paper describes a rigorous methodology to calculate the primary atomic recoil events (often called the primary knock-on atoms or PKAs) that lead to cascade damage events as a function of energy and recoiling species. A new processing code SPECTRA-PKA combines a neutron irradiation spectrum with nuclear recoil data obtained from the latest nuclear data libraries to produce PKA spectra for any material composition. Via examples of fusion relevant materials, it is shown that these PKA spectra can be complex, involving many different recoiling species, potentially differing in both proton and neutron number from the original target nuclei, including high energy recoils of light emitted particles such as α-particles and protons. The variations in PKA spectra as a function of time, neutron field, and material are explored. The application of PKA spectra to the quantification of radiation damage is exemplified using two approaches: the binary collision approximation and stochastic cluster dynamics, and the results from these different models are discussed and compared.

Neutronics analysis for FMITS at SNS

The fusion material community has a growing interest in irradiating materials under a spallation spectrum, in which the wide range of helium/dpa ratios provides a unique opportunity for verifying and adjusting simulation model studies of the radiation effects on structural fusion materials. One of such efforts is the recently proposed FMITS project to be carried out at SNS. The conceptual design of FMITS was completed and briefly presented here. In this design, two sample rods are placed 3cm and 5cm off the centreline, respectively, in front of the mercury target, where the back scattering neutron flux spectrum was found to be fairly close to the ITER fusion spectrum. The PKA spectra at the FMITS samples were also compared to those at ITER. The results show a good agreement between the two types of PKA spectra. At a nominal power of 1.4MW, the displacement production at samples of FMITS is 1.6–5.5dpa/yr for steel, and 1.8–3.4dpa/yr for SiC. The ratio of the gas production versus the displacement production is 13–75appmHe/dpa and 76–311appmH/dpa for steel, and 30–98appmHe/dpa and 28–145appmH/dpa for SiC. This study found no negative impact of FMITS on the SNS moderator performance based on the current conceptual design.

Absorption and Fluorescence Emission Attributes of a Fluorescent dye: 2,3,5,6-Tetracyano-p-Hydroquinone

Four cyano groups have been substituted on the aromatic ring of p-hydroquinone (2,3,5,6-tetracyanohydroquinone) in order to study the enhanced photoacidity of this molecule. The acid-base equilibria have been studied using absorption (for ground state pKa) and fluorescence (excited state pKa) spectra. Three distinct species (neutral, anionic and dianionic forms) were observed in the ground state and only two species (anionic and dianionic forms) were found in the excited state when studied at different pH/Ho in water. Absorption and emission characteristics were studied in various organic solvents, including protic and aprotic solvents. Deprotonation was also investigated using binary mixtures. It has been revealed that absorption and emission spectra are considerably changed with change in media. Proton transfer to the solvent has been observed in various solvents.

Influence of Lipopolysaccharide on the Surface Proton-Binding Behavior of Shewanella spp.

This study investigates the potentiometric properties of several strains of Shewanella spp. and determines whether these properties can be correlated with lipopolysaccharide (LPS) type. The LPS of eight Shewanella strains was characterized using silver-stained sodium dodecyl sulfate-polyacrylamide gel electrophoresis (SDS-PAGE) and their potentiometric properties determined using high-resolution acid-base titrations. Titrations showed that total ligand concentrations (L(T)) ranged from 0.903 +/- 0.007 micromol/mg (S. baltica 63) to 1.387 +/- 0.007 micromol/mg (S. amazonensis SB2B). Smooth strains (possessing O-side chains) exhibited higher mean L(T) values than rough strains (no O-side chain). A Tukey's honestly significantly different (HSD) test revealed, smooth strains exhibited significantly higher L(T) values than rough strains in 69% of comparisons. Comparison of individual pK(a) concentrations revealed that smooth LPS strains of Shewanella were relatively enriched in reactive groups at pK(a) 5, suggesting their LPS O-side chains contained detectable carboxyl groups. Combined pKa spectra from all eight Shewanella strains produced a common trend indicating that the way in which the surface proton-buffering capacity changes with pH is similar for the species studied here.

Proton binding by hydrous ferric oxide and aluminum oxide surfaces interpreted using fully optimized continuous pKa spectra.

A modified regularized least squares pKa spectrum approach is proposed to determine proton stability constants and concentrations for binding sites on hydrous ferric oxide (HFO) and aluminum oxide surfaces. Acid-base titration data are fit to a continuous binding site model for the system represented as a pKa spectrum. The modified parameter fitting method optimizes simultaneously for both smoothness of the pKa spectrum and goodness-of-fit, whereas other methods optimize for goodness-of-fit given a fixed smoothness factor. The modified method is tested with aluminum oxide and recovers values consistent with theoretical values. The regularized pKa spectrum method optimized for smoothness is applied to prepared samples of two types of HFO. The prepared HFO samples differ only in the total iron concentration of the parent solution. The resultant pKa distributions are compared to proton binding constants from MUSIC model results for crystalline iron oxides. The types of binding sites in the HFO sample are consistent with theoretical binding site stability constants for crystalline iron oxides. Overall, the prepared HFO samples have binding constants most consistent with values for lepidocrocite and goethite.

Cell surface electrochemical heterogeneity of the Fe(III)-reducing bacteria Shewanella putrefaciens.

Acid-base titration experiments and electrostatic force microscopy (EFM) were used to investigate the cell surface electrochemical heterogeneity of the Fe(III)-reducing bacteria, Shewanella putrefaciens. The acid-base titrations extended from pH 4 to 10, and the titration data were fit using a linear programming pKa spectrum approach. Overall, a five-site model accounted for the observed titration behavior with the most acidic sites corresponding to carboxylic groups and phosphodiester groups, intermediate sites phosphoryl groups, and two basic sites equivalent to amine or hydroxyl groups. The pH for the point of zero charge on the bacteria was 5.4. In EFM images of cells rinsed in solutions at pH 4.0, 7.0, and 8.0, a pronounced increase in small (< or = 100 nm diameter) high contrast patches was observed on the cells with increasing pH. The pH dependence of EFM image contrast paralleled the pattern of cell surface charge development inferred from the titration experiments; however, quantitative analysis of high contrast regions in the EFM images yielded lower surface charge values than those anticipated from the titration data. For example at pH 7, the calculated surface charge of high contrast regions in EFM images of the bacterial cells was -0.23 microC/cm2 versus -20.0 microC/cm2 based on the titration curve. The differences in surface charge estimates between the EFM images and titration data are consistent not only with charge development throughout the entire volume of the bacterial cell wall (i.e., in association with functional groups that are not directly exposed at the cell surface) but also with the presence of a thin structural layer of water containing charge-compensating counterions. In combination, the pKa spectra and EFM data demonstrate that a particularly high degree of electrochemical heterogeneity exists within the cell wall and at the cell surface of S. putrefaciens.

Multi-site proton interactions with natural organic matter

Water samples from various locations in Norway were used to isolate natural organic matter (NOM). The NOM was isolated using both reverse osmosis and low-pressure low-temperature evaporation for each sample site. These samples were titrated from −log[H +] 3 to 11 at 0.1 unit intervals. The data were analyzed using the Discrete Site Analysis (DISI) technique for pK a intervals of 0.2. The acidity constants are grouped into four classes: strong (pK a < 5), intermediate strong (5.1 < pK a < 7.5), intermediate weak (7.6 < pK a < 9.2), and weak (pK a > 9.3). All samples, regardless of isolation method, were found to contain strong and weak ligands, along with some intermediate ligands. For the same sample site, the concentration of these ligands were found to be dependent on isolation method and titration direction (acid then base vs. base then acid). In addition, the concentration and classes of ligands present were found to vary between sample sites. Suwannee River fulvic acid was analyzed as a reference sample, and was qualitatively similar to the NOM samples but quantitatively different. Overall, the differences in pKa spectra due to isolation method and/or titration direction are almost as significant as differences between sample location, but there are no consistent trends in effects of isolation method or titration direction on characterization of NOM.

A Comparison of the microstructure and tensile behaviour of irradiated fcc and bcc metals

AbstractAs part of an on-going research program, findings are presented from a comparison of the microstructures and associated tensile properties of fcc and bcc materials after high energy proton irradiation, to fluences between 10−4 and 1 dpa, at 300-320 K. Results for this comparison between Cu, Pd, 304 and 316 stainless steel on one side and Fe and the F82H ferritic-martensitic low activation steel on the other are discussed, showing a strong difference in defect accumulation behaviour between the differing crystal structures. The overall deformation behaviour is similar, with an initial localised deformation taking place in all cases, even though the actual deformation mode itself might be different. Furthermore, a comparison is made with some of the materials that have also been irradiated with fission neutrons, showing no influence of the PKA spectra for these irradiation conditions.

Comparison of pka energy spectra, gas-atom production and damage energy deposition in neutron irradiation at various facilities

By dividing neutron-energy spectrum into four energy groups, (I) <10 eV, (II) 10 eV to 0.1 MeV, (III) 0.1 MeV to 10 MeV and (IV) > 10 MeV, contributions to damage parameters (PKA spectrum, damage energy and gas-atom production) from each of the energy group were calculated for neutron irradiations at various facilities with the SPECTER code developed by Greenwood and Smither [1]. The normalized PKA spectra and the gas-atom productions were compared to examine differences in damage parameters. Such comparisons were carried out among (1) irradiations at various positions in different fission reactors (i.e. KUR, JOYO and FFTF-MOTA), and among (2) those at various fission reactors. Damage parameters were also calculated at STARFIRE fusion reactor and RTNS-II. A possible method to correlate damages at different fission reactors is discussed. It is suggested that damages in fusion reactor can be simulated by the superposition of irradiations with fission and D-T neutrons.

Simplified Method of Calculation of PKA Spectra, DPA Cross Sections and Kerma Factors for Medium and Heavy Weight Nuclides

Simplified Method of Calculation of PKA Spectra, DPA Cross Sections and Kerma Factors for Medium and Heavy Weight Nuclides

Simplified method of calculation of PKA spectra, DPA cross sections and kerma factors for medium and heavy weight nuclides.

KEYWORDS: PKA spectrumDPA cross sectionkerma factorkinetic energycomputer calculationssimplified methodmedium weight nucleiheavy weight nucleiironevaluated data AleMeV range 0–50charge particle

Hardening of molybdenum irradiated by neutrons and alpha-particles

Abstract Radiation hardening caused in molybdenum by reactor neutron irradiation and 28-MeV alpha-particle bombardment is studied. 28-MeV alpha-particles are used as a model irradiation simulating CTR radiation effects. It is shown that at earlier stages of irradiation neutrons are more effective in the sense of hardening influence, but as the damage level increases, alpha-particles become the stronger hardening irradiation. It is concluded that radiation hardening of molybdenum is determined by defect structure in whose creation both low and high energy processes of radiation damage take place. PKA spectra are of great importance in the production of hardening defects.

The primary recoil spectrum in the simulation of fast-reactor radiation damage by charged-particle bombardment

The energy spectrum of primary knock-on atoms in iron subject to a typical fast-reactor neutron spectrum is calculated and compared to the PKA.spectrum calculated in nickel under bombardment by 46.5 MeV nickel ions (as on the Harwell VEC), 5 MeV nickel ions, 22 MeV carbon ions, 5 MeV protons and 1 MeV electrons. The damage produced by each PKA spectrum is calculated, and the proportion of the damage produced by high-energy recoils estimated. Comparison of the PKA spectra indicates that the nickel-ion bombardments are the closest simulation of fast-reactor damage.