Reaction Rate Measurements Research Articles

Electron Screening in Laboratory Nuclear Reactions

A thorough understanding of nuclear reaction rates at low energies is essential for improving our understanding of energy generation in stars and primordial and stellar nucleosynthesis. At low energies, fusion reactions between charged particles are strongly suppressed by the presence of the Coulomb barrier, which classically inhibits the penetration of one nucleus into another. The barrier penetration causes the cross section to have a steep energy dependence at low energies, making cross section measurements very challenging. Furthermore, little is known about the impact of surrounding electrons in stellar plasmas that are currently beyond the reach of experiments. As a result, measuring the bare cross sections as accurately as possible is essential. Reaction rate measurements at very low energies have been made possible in recent years by the development of high-current low-energy accelerators as well as enhanced target and detection methods. Nevertheless, the presence of atomic electrons, which alter the Coulomb barrier by screening the nuclear charge and increase the cross section at low energies compared to the case of bare nuclei, complicates these observations. A review of the experimental and corresponding theoretical work on laboratory electron screening performed so far will be presented.

Concurrent measurement of strain and chemical reaction rates in a calcite grain pack undergoing pressure solution: Evidence for surface-reaction controlled dissolution

Pressure solution is inferred to be a significant contributor to sediment compaction and lithification, especially in carbonate sediments. For a sediment deforming primarily by pressure solution, the compaction rate should be directly related to the rate of calcite dissolution, transport along grain contacts, and calcite reprecipitation. Previous experimental work has shown that there is evidence that deformation in wet calcite grain packs is consistent with control by pressure solution, but considerable ambiguity remains regarding the rate limiting mechanism. We present the results of laboratory compaction experiments designed to directly measure calcite dissolution and precipitation rates (recrystallization rates) concurrently with strain rate to test whether measured rates are consistent with predicted rates both in absolute magnitude and time evolution. Recrystallization rates are measured using trace element chemistry (Sr/Ca, Mg/Ca) and isotopes (87Sr/86Sr) of fluids flowing slowly through a compacting grain pack as it is being triaxially compressed. Imaging techniques are used to characterize the grain contacts and strain effects in the post-experiment grain pack. Our data show that calcite recrystallization rates calculated from all three geochemical parameters are in approximate agreement and that the rates closely track strain rate. The geochemically inferred rates are close to predicted rates in absolute magnitude. Uncertainty in grain contact dimensions makes distinguishing between surface reaction control and diffusion control difficult. Measured reaction rates decrease faster than predicted from standard pressure solution creep flow laws. This inconsistency may indicate that calcite dissolution rates at grain contacts are more complex, and more time-dependent, than suggested by geometric models designed to predict grain contact stresses.

An Electrochemical Perspective on Reaction Acceleration in Microdroplets.

Analytical techniques operating at the nanoscale introduce confinement as a tool at our disposal. This review delves into the phenomenon of accelerated reactivity within micro- and nanodroplets. A decade of accelerated reactivity observations was succeeded by several years of fundamental studies aimed at mechanistic enlightenment. Herein, we provide a brief historical context for rate enhancement in and around micro- and nanodroplets and summarize the mechanisms that have been proposed to contribute to such extraordinary reactivity. We highlight recent electrochemical reports that make use of restricted mass transfer to enhance electrochemical reactions and/or quantitatively measure reaction rates within droplet-confined electrochemical cells. A comprehensive approach to nanodroplet reactivity is paramount to understanding how nature takes advantage of these systems to provide life on Earth and, in turn, how to harness the full potential of such systems.

Reaction Rate Ratios for Recent Fast Metal Experiments with Large Plutonium Masses

Reaction rate ratios are integral responses that are used within the criticality experiments field because they contain spectral information. While these types of measurements have been utilized for nuclear data validation with historic experiments, few experiments of this type have been utilized for recent experiments, as few exist. This work focuses on measured reaction rate ratios for two nearly bare plutonium critical assemblies with different geometries: one that is cube like (with a Pu mass of 40 kg) and one that is slab like (with a Pu mass of 109 kg). Irradiations were performed with both configurations in which foils were placed near the center of the assembly. Plutonium, highly enriched uranium, depleted uranium, and Au foils were included in the irradiation and counted via high-purity germanium detectors. From these measurements, reaction rate ratios were calculated. Measured and simulated values and uncertainties are presented for the reaction rate ratios. Ratios utilizing the following reactions are given in this work: 197Au(n, γ ), 197Au(n,2n), 235U(n,fission), 238U(n,fission), 238U(n,2n), 238U(n, γ ), and 239Pu(n,fission). Uncertainties for the measured reaction rate ratios ranged from 4% to 7%, and the contribution of various parameters to this uncertainty was investigated. The results are compared to historical experiments and should be used for nuclear data validation for future nuclear data library releases. These measurements are part of the EUCLID (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) project, which utilizes measurement responses in addition to keff (such as these reaction rate ratios) to help reduce uncertainties in 239Pu nuclear data.

Microscale Chaotic Mixing as a Driver for Chemical Reactions in Porous Media.

Mixing-induced reactions play a key role in a large range of biogeochemical and contaminant transport processes in the subsurface. Fluid flow through porous media was recently shown to exhibit chaotic mixing dynamics at the pore scale, enhancing microscale concentration gradients and controlling mixing rates. While this phenomenon is likely ubiquitous in environmental systems, it is not known how it affects chemical reactions. Here, we use refractive index matching and laser-induced fluorescence imaging of a bimolecular redox reaction to investigate the consequence of pore scale chaotic mixing on the reaction rates. The overestimation of measured reaction rates by the classical macrodispersion model highlights the persistence of incomplete mixing on the pore scale. We show that the reaction product formation is controlled by microscale chaotic mixing, which induces an exponential increase of the mixing interface and of the reaction rates. We derive a reactive transport model that captures experimental results and predicts that chaotic mixing has a first order control on reaction rates across a large range of time scales and Péclet and Damköhler numbers. These findings provide a new framework for understanding, assessing, and predicting mixing-induced reactions and their role on the fate and mobility of environmental compounds in natural porous media.

Scavenging of Superoxide Radical Anion by Fluorinated Organosilicon Additives

We have explored a set of structurally related fluorinated and non-fluorinated organosilicon additives and quantified their rates of reaction with the superoxide radical anion O2 •−. using rapid-scan cyclic voltammetry. Absolute reaction rate measurements in acetonitrile solvent show that O2 •− reacts with the fluorinated OS compounds with bimolecular rate constants k BM more than 1000x larger than k BM for the reaction between O2 •− and ethylene carbonate. We further identified the products of reaction of a model OS compound using multiple nuclear magnetic resonance (NMR) methods and with gas chromatography/mass spectroscopy. Chemical analysis measurements show that addition of potassium superoxide KO2 to a model fluorinated OS compound produces only one product. Our results indicate that that OS compounds improve battery performance by rapidly scavenging O2 •− in a way that produces a stable product and reduces or eliminates the competing chemical pathways associated with carbonate breakdown. These results provide new insights into how chemical structure impacts critical chemical reactions and may guide the design of new additives that further improve battery safety and stability.

A general method for studying reactive surface species, CT-SKAn: Charge-transfer spectrokinetic analysis

A spectrokinetic methodology was developed to determine reactive surface species by combining operando ultraviolet–visible spectroscopy and charge transfer kinetic models. The methodology consisted of three general steps: 1) concomitant measurement of reaction rates and charge transfer via ultraviolet–visible spectroscopy; 2) development of rate expressions from kinetic models involving the adsorbed species of interest. These rate expressions relate reaction rates, charge transfer, and partial pressures of gas phase species; and 3) evaluation of the goodness of fit of the rate expressions to the experimental data. The species whose rate expressions show the best fit are the more likely reactive surface species for the studied reaction. An example is presented for the determination of reactive oxygen species during ethanol oxidation over Au/TiO2. The charge transfer spectrokinetic analysis showed that surface hydroperoxyl, hydroxyl, and atomic oxygen species were reactive surface intermediates, whereas surface molecular oxygen was not.

Advancing 2D reaction rate measurements in BNCT: Validation of the indirect neutron radiography method

The precise characterization of neutron beams is a cornerstone of Boron Neutron Capture Therapy (BNCT). While Instrumental Neutron Activation Analysis (INAA) is the standard technique for neutron flux measurement, it is limited in its ability to capture two-dimensional (2D) reaction rate distributions. This study aims to validate the Indirect Neutron Radiography (INR) method for 2D reaction rate quantification, addressing critical variables such as temperature sensitivity and signal fading. We designed and constructed an optimized INR platform comprising an Imaging Plate (IP), readout device, activation detectors (copper foils), and real-time temperature monitoring. Comprehensive experiments were conducted to investigate the impact of ambient temperature and fading time on IP signal reliability. A robust calibration curve was formulated, linking IP signals to dose deposition metrics, thereby enabling precise reaction rate assessments. The study found that IP signals are minimally sensitive to temperature variations (less than 0.1% change per 1 °C), but are subjected to linear fading over time, necessitating stringent temperature control and time-dependent signal corrections. A mathematical relationship between IP signals and dose deposition was established, represented by Y = 20,500 × x0.01803-21103. Application of the INR method revealed that the depth-dependent reaction rates in copper strips closely aligned with those acquired through INAA, exhibiting a relative deviation of less than 5% within a 4cm depth range inside the phantom. Our findings demonstrate that the INR method offers a robust alternative to traditional INAA for capturing 2D reaction rates, effectively addressing complexities like temperature sensitivity and signal fading. While challenges persist, particularly in the realm of measurement errors, this study lays the groundwork for further methodological refinements and broadens the scope for future research in BNCT neutron beam characterization.

Single Droplet Tweezer Revealing the Reaction Mechanism of Mn(II)-Catalyzed SO2 Oxidation.

Sulfate aerosol is one of the major components of secondary fine particulate matter in urban haze that has crucial impacts on the social economy and public health. Among the atmospheric sulfate sources, Mn(II)-catalyzed SO2 oxidation on aerosol surfaces has been regarded as a dominating one. In this work, we measured the reaction kinetics of Mn(II)-catalyzed SO2 oxidation in single droplets using an aerosol optical tweezer. We show that the SO2 oxidation occurs at the Mn(II)-active sites on the aerosol surface, per a piecewise kinetic formulation, one that is characterized by a threshold surface Mn(II) concentration and gaseous SO2 concentration. When the surface Mn(II) concentration is lower than the threshold value, the reaction rate is first order with respect to both Mn(II) and SO2, agreeing with our traditional knowledge. But when surface Mn(II) concentration is above the threshold, the reaction rate becomes independent of Mn(II) concentration, and the reaction order with respect to SO2 becomes greater than unity. The measured reaction rate can serve as a tool to estimate sulfate formation based on field observation, and our established parametrization corrects these calculations. This framework for reaction kinetics and parametrization holds promising potential for generalization to various heterogeneous reaction pathways.

Unveiling the Essential Parameters Driving Mineral Reactions during CO2 Storage in Carbonate Aquifers through Proxy Models

Numerical simulation is a commonly employed technique for studying carbon dioxide (CO2) storage processes in porous media, particularly saline aquifers. It enables the representation of diverse trapping mechanisms and the assessment of CO2 retention capacity within the subsurface. The intricate physicochemical phenomena involved necessitate the incorporation of multiphase flow, accurate depiction of fluid and rock properties, and their interactions. Among these factors, geochemical reaction rates and mechanisms are pivotal for successful CO2 trapping in carbonate reactive rocks. However, research on kinetic parameters and the influence of lithology on CO2 storage remains limited. This limitation is partly due to the challenges faced in laboratory experiments, where the time scale of the reactions and the lack of in situ conditions hinder accurate measurement of mineral reaction rates. This study employs proxy models constructed using response surfaces calibrated with simulation results to address uncertainties associated with geochemical reactions. Monte Carlo simulation is utilized to explore a broader range of parameters and identify influential factors affecting CO2 mineralization. The findings indicate that an open database containing kinetic parameters can support uncertainty assessment. Additionally, the proxy models effectively represent objective functions related to CO2 injectivity and mineralization, with calcite dissolution playing a predominant role. pH, calcite concentration, and CO2 injection rate significantly impact dolomite precipitation, while quartz content remains unaffected.

Identification of reaction intermediates in the decomposition of formic acid on Pd.

Uncovering the role of reaction intermediates is crucial to developing an understanding of heterogeneous catalysis because catalytic reactions often involve complex networks of elementary steps. Identifying the reaction intermediates is often difficult because their short lifetimes and low concentrations make it difficult to observe them with surface sensitive spectroscopic techniques. In this paper we report a different approach to identify intermediates for the formic acid decomposition reaction on Pd(111) and Pd(332) based on accurate measurements of isotopologue specific thermal reaction rates. At low surface temperatures (∼400 K) CO2 formation is the major reaction pathway. The CO2 kinetic data show this occurs via two temporally resolved reaction processes. Thus, there must be two parallel pathways which we attribute to the participation of two intermediate species in the reaction. Isotopic substitution reveals large and isotopologue specific kinetic isotope effects that allow us to identify the two key intermediates as bidentate formate and carboxyl. The decomposition of the bidentate formate is substantially slower than that of carboxyl. On Pd(332), at high surface temperatures (643 K to 693 K) we observe both CO and CO2 production. The observation of CO formation reinforces the conclusion of calculations that suggest the carboxyl intermediate plays a major role in the water-gas shift reaction, where carboxyl exhibits temperature dependent branching between CO2 and CO.

Analysis of Reaction Rate and Product Selectivity of Ethanol Electrolytic Oxidation Reaction in the Flow Reactor

Introduction In recent years, the development of the electrolysis hydrogen production process has been vigorously promoted due to the widespread use of hydrogen energy. However, oxygen, a byproduct of the anode reaction, has not been utilized. On the other hand, chemical products are produced industrially by electro-organic synthesis, and if the anode reaction could be used directly as a chemical synthesis reaction, the overall benefit would be further enhanced. At the same time, the high selectivity and controllability of the electrochemical process make it possible to produce highly selective chemical products by anodic reactions. The objective of this study is to develop a process for simultaneous electrolytic hydrogen production at the cathode and highly selective acetaldehyde production at the anode. Experimental A schematic diagram of the experimental setup is shown in Figs. 1 and 2. Platinum electrodes were placed on silicone gaskets with flow channels, and the gaskets were sandwiched between silicone gaskets, PTFE plates, and stainless-steel endplates. A cation exchange membrane NR-212 was placed in the center to separate the reactions at the two electrodes. A 0 to 0.5 mol/L sulfuric acid solution containing 0.01 to 1.0 mol/L ethanol or a 0 to 0.5 mol/L sulfuric acid solution containing 0.01 to 1.0 mol/L acetaldehyde was supplied to the anode, and a 0 to 0.5 mol/L sulfuric acid solution was supplied to the cathode. Results and Discussion The experimental results are analyzed based on the premise of surface reaction rate limitation and steady-state conditions. As shown in Fig. 3, the ethanol conversion increased with rise in A/v (ratio of electrode area to flow rate), reaching its maximum value at A/v of 88.4 min/cm. This can be attributed to the difficulty in discharging bubbles generated from the electro-oxidation reaction as the A/v was raised. To ensure that the reactions occurred under reaction rate-limiting conditions, acetaldehyde electro-oxidation experiments were conducted with feed concentrations of 0 to 0.5 M sulfuric acid solutions containing 1.0 M acetaldehyde at the anode, and 0 to 0.5 M sulfuric acid solutions at the cathode, an A/v of 88.4 min/cm, and a potential difference of 1.0 V. The reaction rate was also affected by the reduction in the hydroxide ion concentration due to the increased sulfuric acid concentration, leading to the lower measured reaction rates. In the result of Fig. 4, it can be inferred that when the concentration of sulfuric acid was below 0.1 M, the reaction rate was governed by diffusion. Subsequently, acetaldehyde electro-oxidation experiments were performed under acetaldehyde concentrations ranging from 0.01 to 1 M, a sulfuric acid concentration of 0.1 M, the fixed A/v, and potential differences between 0.8 and 1.2 V to elucidate the impact of reactant concentration on the reaction rate. The results in Fig. 5 demonstrate that while the reaction rates increased with raising the acetaldehyde concentration, it eventually approached a plateau, attributable to the saturation of active sites with acetaldehyde on the Pt electrode.The results of ethanol electro-oxidation experiments were shown in Figs. 6 and 7, decrease in acetaldehyde selectivity was observed with a feed concentration of a 0.1 M sulfuric acid solution, attributable to the formation of acetic acid and carbon dioxide as byproducts. Subsequently, in comparison to sulfuric acid concentrations below 0.2 M, under the conditions of 0.5 M sulfuric acid concentration and low conversion, the acetaldehyde selectivity exhibited a gradual decline as the conversion increased. This indicates that the influence of sulfuric acid concentration on the oxidation reaction of acetaldehyde to acetic acid was more significant than that on the oxidation reaction of ethanol to acetaldehyde. A plausible explanation for this phenomenon is that the oxidation of acetaldehyde is considerably inhibited by the adsorption of sulfate ions to the active sites, as it is associated with a second-order reaction of adsorbed species concentration. Consequently, altering the sulfuric acid concentration results in changes in the ethanol electro-oxidation reaction selectivity. Conclusions The selectivity of ethanol electro-oxidation reaction was significantly influenced by potential difference and electrolyte concentration. Notably, acetic acid was not produced at potential differences below 0.8 V. Sulfuric acid concentration affected reaction selectivity, with a greater impact on acetaldehyde-to-acetic-acid oxidation. Despite the higher selectivity observed at 0.6 V, the reaction rate was low. Employing an appropriate potential difference and electrolyte concentration can facilitate achievement both of higher selectivity and an enhanced reaction rate. Optimal conversion was achieved at an A/v of 88.4 min/cm, while the maximum acetaldehyde selectivity of approximately 95 % was observed at an applied voltage of 1.2 V and 0.5 M sulfuric acid concentration. Figure 1

Development of HELIOS/BIPR/PARCS/MCNP6 Computation Route for WWER RPV Neutron Fluence Analysis and Validation Against Ex-Vessel Detector Measurement Data

A computational route was developed for precise calculation of fast neutron fluence on a WWER-type reactor pressure vessel (RPV). The method is based on the transfer of neutronics data from HELIOS-2 lattice calculations and nodal diffusion neutronics data (power, density, and temperature) from BIPR7.1 and PARCS 3.36/PATHS core calculations into a three-dimensional (pinwise axially distributed) fixed neutron source for modeling of transport of fast neutrons from the reactor core to the outer surface of the RPV using MCNP6.2. Validation of the proposed computational method was carried out based on comparative analysis of MCNP6.2-predicted and neutron dosimetry–measured reaction rates [54Fe(n,p)54Мn, 93Nb(n,nʹ)93mNb, and 58Ni(n,р)58Со] on the outer surface of the Armenian Nuclear Power Plant (ANPP) Unit 2 RPV. Validation revealed that the MCNP6.2-predicted fast neutron fluence results are very sensitive to the ENDF-B neutron data. Particularly, MCNP6.2 with ENDF/B-VIII.0 significantly underpredicts (20% to 30%) fast neutron fluence while using ENDF/B-VII.1 data overpredicts it. Adding revised beta-released evaluations of 54Fe, 56Fe, 57Fe, and 16O from the International Nuclear Data Evaluation Network (INDEN) to ENDF/B-VIII.0 allows one to obtain reasonable agreement with measurement results for all types of measured reaction rates.

Neutron source strength verification via reaction rate measurement and Monte Carlo simulation

Determining the neutron source strength is essential to ensure optimal use of the source and to implement adequate radiation protection measures. In this study, the source strength of two (α,n) neutron sources – a newly acquired 185 GBq 241AmBe and a legacy source 74 GBq 239PuBe – were verified. Source strength verification was performed by measuring the induced activities in irradiated 115In foils and comparing the results to MCNP calculated reaction rates. The results for 241AmBe agree well with a maximum and average deviations of 8.1% and 4.1%, respectively. While for 239PuBe the maximum deviation is 11.7% and the average deviation is 6.3%. Results of this study provide a reliable reference for the application of the sources, in particular, for the 241AmBe which is used as the external neutron source of the PRR1-Subcritical Assembly for Training, Education, and Research (PRR1-SATER), and for the design of a neutron irradiator that will repurpose the 239PuBe.

Kinetics of the Temperature-Dependent eaq - and ⋅OH Radical Reactions with Cr(III) Ions in Aqueous Solutions.

The reactivity of chromium(III) species with the major oxidizing and reducing radiolysis products of water was investigated in aqueous solutions at temperatures up to 150 °C. The reaction between the hydrated electron (eaq - ) and Cr(III) species showed a positive temperature dependence over this temperature range. The reaction was also studied in pH 2.5 and 3.5 solutions for the first time. This work also studied the reaction between acidic Cr(III) species and the hydroxyl radical (⋅OH). It was found that Cr3+ did not react significantly with the ⋅OH radical, but the first hydrolysis species, Cr(OH)2+ , did with a rate coefficient of k= (7.2±0.3)×108 M-1 s-1 at 25 °C. The oxidation of Cr(OH)2+ by the ⋅OH radical formed an absorbing product species that ultimately oxidized to give Cr(VI). These newly measured reaction rates allow for the development of improved models of aqueous chromium speciation for the effective remediation of liquid high-level nuclear waste via vitrification processes.

Enhanced Mixing and Reaction in Converging Flows: Theory and Pore‐Scale Imaging

AbstractMixing fronts at the interface of opposing flows are compressed at a constant rate. The resulting exponential stretching of fluid elements leads to enhanced chemical gradients and biogeochemical processes. This process is similar as what occurs in the pore space of 3D chaotic flows. However, it is so far not known how such fluid compression controls the amplitude of mixing and reaction rates in porous media. Here we derive analytical predictions for the mixing width, the maximum reaction rate and the reaction intensity in compressed mixing fronts as a function of the Péclet and Damköhler numbers. We developed an experimental setup providing pore scale measurements of mixing and reaction rates in mixing fronts at the interface of converging flows. The theory accurately predicts the scaling of mixing and reaction with the Péclet number both in porous micromodels and simple Hele‐Shaw cells. Additionally, we found that the presence of pore scale heterogeneities in the porous micromodels enhances reaction rates by a factor of 4 compared to the Hele‐Shaw cells. Using numerical simulations of pore scale velocity fields, we attributed this phenomenon to the enhancement of pore‐scale compression due to the presence of grains in accelerating flows. These findings provide new insights into the dynamics of mixing‐induced reactions in porous media.

Fast protein folding is governed by memory-dependent friction

When described by a low-dimensional reaction coordinate, the folding rates of most proteins are determined by a subtle interplay between free-energy barriers, which separate folded and unfolded states, and friction. While it is commonplace to extract free-energy profiles from molecular trajectories, a direct evaluation of friction is far more elusive and typically relies on fits of measured reaction rates to memoryless reaction-rate theories. Here, using memory-kernel extraction methods founded on a generalized Langevin equation (GLE) formalism, we directly calculate the time-dependent friction acting on the fraction of native contacts reaction coordinate Q, evaluated for eight fast-folding proteins, taken from a published set of large-scale molecular dynamics protein simulations. Our results reveal that, across the diverse range of proteins represented in this dataset, friction is more influential than free-energy barriers in determining protein folding rates. We also show that proteins fold in a regime where the finite decay time of friction significantly reduces the folding times, in some instances by as much as a factor of 10, compared to predictions based on memoryless friction.

Investigations on the effect of alkalis on C-S-H growth rates and their impact on early C3S hydration rates

In this work, we investigated the influence of alkalis on C-S-H precipitation and growth rates in solutions supersaturated with respect to C-S-H. Therefore, we used an experimental setup that leads to C-S-H precipitation and growth in solutions with a known KOH concentration. The results show that the KOH concentration in solution generally leads to an increase of the C-S-H growth rates at lower supersaturation levels. Based on these findings, we calculated theoretical reaction rates of C3S hydration using the precipitation rates of C-S-H. The comparison between these calculated rates and measured reaction rates from hydration experiments shows good agreement, allowing us to present a quantitative model for the effect of alkalis in combination with aluminum. Furthermore, we provide a quantitative analysis of how alkalis and aluminum modify reaction rates during the acceleration period of C3S hydration, which can be explained by different behaviors in the nucleation and growth of C-S-H.

Experimental Analyses of Capture Reaction Rates for Epithermal and Resonance Neutrons in Source-Driven Subcritical Cores

Neutron irradiation experiments are carried out in source-driven subcritical cores with high-energy neutrons generated by spallation reactions between a 100-MeV proton beam and a lead-bismuth target at the Kyoto University Critical Assembly. The main objective of the experiments is to investigate the effect of epithermal and resonance neutrons on the accuracy of capture reaction rates with respect to a subcriticality variation. Activation foils of copper, indium, tantalum, and tungsten are employed to obtain capture reaction rates for epithermal and resonance neutrons by applying the cadmium difference method. Also, the applicability of the foils for the measurement of the reaction rates for epithermal and resonance neutrons is substantiated in the critical irradiation experiments performed prior to the subcritical experiments. The subcritical experiments are conducted with three different subcriticalities by changing the control rod insertion pattern. The measured reaction rates are compared with the calculated values obtained by the Monte Carlo code MVP with JENDL-4.0, and the ratio of the calculation and experiment values of the reaction rates shows equivalent values within the 1σ errors regardless of a difference in the subcriticality. The compared results indicate that the numerical analyses have a consistent accuracy of reaction rates in epithermal and resonance energy regions for a subcriticality variation in source-driven subcritical cores.

Measurement of 6Li burn-up reaction rate using a single crystal CVD diamond detector under fast neutron irradiation environment

The study aimed to develop a technique for measuring the 6Li burn-up rate using a single crystal diamond (SCD) detector (SDD) made by chemical vapor deposition (CVD) with a thin lithium fluoride foil. The method relied on pulse shape discrimination (PSD) to separate pulses by nuclear reaction products of 6Li from pulses due to fast neutrons and gamma-rays.By applying the PSD method, the rectangular shape pulses induced by events occurred at the specific depth positions of the SCD, i.e., the incident surface, the ballistic center region (BCR), and the rear surface, were extracted. Thereafter, pulses occurred each specific depth position of the SCD were discriminated according to the pulse width.Due to a short range of nuclear reaction products in the SCD, pulses at the incident surface should be induced by both fast neutrons and nuclear reaction products, although pulses at the BCR are caused by fast neutron only. The study demonstrated that quantitative measurements of nuclear reaction products in the 6Li burn-up reaction under fast neutron irradiation can be achieved using only one SDD by analyzing event rates at the incident surface and in the BCR region.