Collimated scanning for large sample neutron activation analysis of inhomogeneous samples

A technique was developed for the identification of inhomogeneities in activity distribution and the correction of their effect on the interpretation of gamma spectrometry data in Large Sample Neutron Activation Analysis. The method was based on collimated gamma scanning using a germanium detector to obtain the activity pattern in the bulk sample and Monte Carlo simulations in order to correct the experimental data for the effect of the inhomogeneous activity distribution. The method was experimentally evaluated in the case of a large cylindrical reference sample of 2 L in volume containing quartz as matrix material and a known source of radioactivity and an excellent agreement was observed. The discussed technique improves the trueness of quantitative analysis of large samples with inhomogeneous activity distribution.     

{\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 Status of software for PGNAA bulk analysis by the Monte Carlo - Library Least-Squares (MCLLS) approach \par }

Summary {\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 The Center for Engineering Applications of Radioisotopes (CEAR) has been working for about ten years on the Monte Carlo - Library Least-Squares (MCLLS) approach for treating the nonlinear inverse analysis problem for PGNAA bulk analysis. This approach consists essentially of using Monte Carlo simulation to generate the libraries of all the elements to be analyzed plus any other required libraries. These libraries are then used in the linear Library Least-Squares (LLS) approach with unknown sample spectra to analyze for all elements in the sample. The other libraries include all sources of background which includes: (1) gamma-rays emitted by the neutron source, (2) prompt gamma-rays produced in the analyzer construction materials, (3) natural gamma-rays from K-40 and the uranium and thorium decay chains, and (4) prompt and decay gamma-rays produced in the NaI detector by neutron activation. A number of unforeseen problems have arisen in pursuing this approach including: (1) the neutron activation of the most common detector (NaI) used in bulk analysis PGNAA systems, (2) the nonlinearity of this detector, and (3) difficulties in obtaining detector response functions for this (and other) detectors. These problems have been addressed by CEAR recently and have either been solved or are almost solved at the present time. We have now finished the development of Monte Carlo simulation for all of the libraries except the prompt gamma-ray library from the activation of the NaI detector. We must first determine a treatment for the coincidence schemes for Na and particularly I to complete the Monte Carlo simulation of this last library. \par }     

Neutron self-shielding correction for prompt gamma neutron activation analysis of large samples

Summary Facilities and methods for INAA of large samples (up to 30 kg) have been developed and successfully tested at IRI, Delft. The methods encompass corrections for neutron self shielding in an isotropic neutron field and gamma self-absorption. The sample’s neutron absorption and scattering characteristics are determined by monitoring the neutron fluence rate around the sample and comparing the neutron densities measured with unperturbed fluence rates. We report on the possibility of developing similar methods for PGNAA. Relative self-shielding factors were measured as well as obtained from Monte Carlo computations. The agreement is good except for the most extreme case, with respect to absorption, attempted (CCl₄).     

Performance improvement of a PGNAA setup due to change in moderator design: A Monte Carlo study

Effect of neutron source-moderator geometry has been studied on the performance of a thermal neutron capture-based prompt gamma neutron activation analysis (PGNAA) setup. In the study prompt gamma-ray and thermal neutron yield was calculated for various positions of the neutron source inside 3–10 cm long high density polyethylene moderators. The study has been carried out for a Portland cement sample using Monte Carlo calculations. The maximum yields of the thermal neutrons and prompt gamma-rays have been observed for a neutron source at a distance of 1 cm from the sample. The maximum yield of the 1.94 and 6.42 MeV prompt gamma-ray from a Portland cement sample has been observed for moderators having length equal to or greater than 7 cm. The yield of both gamma rays is 2.57 times higher than the previously reported value for a PGNAA setup with the source placed outside a 5 cm thick moderator. The higher yield of gamma rays will result in higher sensitivity of the PGNAA setup.     

A Monte Carlo code to get response spectrum of ions for Neutron Depth Profiling

This paper presents a Monte Carlo code to get response spectrum of ions for the Neutron Depth Profiling (NDP) technique called Monte Carlo NDP (MC-NDP) that simulates the behavior of ions transmitted through a sample matrix and generates the energy spectrum for a specified detector. The MC-NDP model is based on the Ziegler–Biersack–Littmark Model, but incorporates the advantages of TRIM and CORTEO. The Impulse Approximation method is used to determine the flight length with the indexical interpolation method rather than the Magic algorithm for the scattering angle between ions and nucleus. This makes MC-NDP more efficient and convenient to simulate entire ion histories by a Monte Carlo approach. MC-NDP’s results agree well with both TRIM results and the experimental data.     

Coincidence and anti-coincidence measurements in prompt gamma neutron activation analysis with pulsed cold neutron beams

A novel approach is implemented to alleviate some persistent problems in neutron capture prompt gamma activation analysis (PGAA). Detection sensitivities of PGAA are often restricted by the following factors: poor signal to noise ratios, interferences from background signals, and, in some cases, overlapping energy lines from different origins, namely ultra short-lived decay lines interfering with prompt decay. Timing the gamma-ray acquisition with the actual capture events using a pulsed beam of cold neutrons allows discrimination between prompt and delayed emissions from a sample source as well as against background events. Coincidence gating selects the prompt gamma-ray emissions. Contributions of background capture gamma-rays are suppressed because of different flight times of neutrons to the sources of background radiation, providing a reduction in direct gamma-ray interferences. Anti-coincidence gating allows measurement of only decay radiation that originates from short-lived activated states of the nuclides after capture. Spectra of decaying nuclides are free of interfering prompt activities, as well as have lower continuum background from Compton scattering of high-energy prompt gamma-rays in the detector. The measurements provide the opportunity to use ultra-short half-life nuclides for analytical purposes, no sample transfer times are lost, and repetitive activation and counting cycles are achieved with the use of pulsed neutron beams.     

Validation of true coincidence summing correction in Genie 2000 V3.2

A new cascade summing correction method with the algorithm extended to include true coincidence summing effects from low-energy gamma-rays, KX-rays from Electron Capture and Internal Conversion, and to include the 511 keV positron annihilation photons has been developed and implemented in Genie 2000 V3.2 released in 2009. To validate the accuracy and precision of the extended correction method, measurements of calibrated sources containing cascading nuclides from various types of ISOCS/LabSOCS characterized High Purity Germanium detectors have been analyzed. Validation of the true coincidence summing correction factors for the extended correction method has been made by comparison to the results from the Monte Carlo code MCNP-CP. In addition, comparison between the measured and the known activities of the cascading nuclides was performed, which shows that the method is effective and accurate.     

Estimation of background interference in prompt-gamma neutron activation using MCNP

Prompt-gamma neutron activation (PGNA) is used to measure total-bodynitrogen and hydrogen in humans. Background interference in the gamma spectraarises from both subject and shielding. A Monte Carlo simulation program (MCNP4B2)was used to examine the neutron and gamma signals in the PGNA system ( ²⁴¹AmBe source). N and H peak regions were assessed in the presenceand absence of calibration phantoms. The simulations suggested extracorporealH peak contributions of up to 30%, depending on subject body habitus. MostN background could be attributed to detector pileup events. The MCNP resultsallowed us to improve shielding design and develop background correction algorithmsto improve measurement precision.     

Detecting polarized gamma-rays by pair production

Recently, a GEANT Monte Carlo code was used to design an outline of the geometry and to simulate the performance of a high energy (10 MeV–10 GeV) gamma-ray detector (Depaola, 1997. Monte Carlo simulation of the ARGO. Nuclear Instruments and Methods A 342, 302–307). It was shown that the incident direction and energy of the incoming photons can be determined from the tracks of the produced electrons–positron pairs. A natural follow-up problem is to study whether this system can be used to detect linearly polarized gamma-rays. In principle, this can be done by measuring the azimuthal distribution of the produced pairs since the cross-section has a dependence with the vector polarization direction. In this work we first determine the azimuthal angular distribution from the differential cross-section for pair production. We then show that the azimuthal distribution of the produced pairs has a very simple angular dependence and can be approximated very accurately by cross-section for coplanar events. Finally, we use the simplified cross-section to simulate the performance of the detector.     

Large sample neutron activation analysis of a reference inhomogeneous sample

A benchmark experiment was performed for Neutron Activation Analysis (NAA) of a large inhomogeneous sample. The reference sample was developed in-house and consisted of SiO₂ matrix and an Al–Zn alloy “inhomogeneity” body. Monte Carlo simulations were employed to derive appropriate correction factors for neutron self-shielding during irradiation as well as self-attenuation of gamma rays and sample geometry during counting. The large sample neutron activation analysis (LSNAA) results were compared against reference values and the trueness of the technique was evaluated. An agreement within ±10% was observed between LSNAA and reference elemental mass values, for all matrix and inhomogeneity elements except Samarium, provided that the inhomogeneity body was fully simulated. However, in cases that the inhomogeneity was treated as not known, the results showed a reasonable agreement for most matrix elements, while large discrepancies were observed for the inhomogeneity elements. This study provided a quantification of the uncertainties associated with inhomogeneity in large sample analysis and contributed to the identification of the needs for future development of LSNAA facilities for analysis of inhomogeneous samples.     

Use of monte carlo modeling to aid interpretation and quantification of the low energy-loss electron yield at low primary energies

Experimental low-loss electron (LLE) yields were measured as a function of loss energy for a range of elemental standards using a high-vacuum scanning electron microscope operating at 5 keV primary beam energy with losses from 0 to 1 keV. The resulting LLE yield curves were compared with Monte Carlo simulations of the LLE yield in the particular beam/sample/detector geometry employed in the experiment to investigate the possibility of modeling the LLE yield for a series of elements. Monte Carlo simulations were performed using both the Joy and Luo [Joy, D.C. & Luo, S., Scanning 11(4), 176988 (2005)] to assess the influence of the more recent stopping power data on the simulation results. Further simulations have been conducted to explore the influence of sample/detector geometry on the LLE signal in the case of layered samples consisting of a thin C overlayer on an elemental substrate. Experimental LLE data were collected from a range of elemental samples coated with a thin C overlayer, and comparisons with Monte Carlo simulations were used to establish the overlayer thickness.     

Full energy peak efficiency calibration of HPGe detector for point and extended sources using Monte Carlo code

Monte Carlo simulation is important to get efficiencies for cases where the experimental efficiencies are difficult to get such as for samples with nonstandard geometries and for large samples. In this paper, efficiency of the HPGe detector, routinely used in our lab for a variety of samples, has been computed for point source geometry and its parameters has been optimized to match MCNP and experimental efficiencies within 5% at different sample to detector distances. This optimized geometry was then validated by efficiency transfer to other geometries.     

Investigation of mass attenuation coefficients of water, concrete and bakelite at different energies using the FLUKA Monte Carlo code

The mass attenuation coefficients of water, bakelite and concrete sample defined in the simulation package were obtained using the FLUKA Monte Carlo code at 59.5, 80.9, 140.5, 356.5, 661.6, 1173.2 and 1332.5 keV photon energies. The results for the mass attenuation coefficients obtained by simulation have been compared with experimental and the theoretical ones and good agreement has been observed. The results indicate that this process can be followed to determine the data on the attenuation of gamma-rays with the several energies in other materials. Also, the deposited energy by 661.6 keV photons at several thicknesses of each media was determined as being an important data for radiation shielding studies.     

Single crystal HPGe (80%) versus BGO shielded CLOVER detector for high precision decay rate measurements: a comparative study

In this study, various detector configurations have been investigated in order to explore the optimal condition for decay rate measurements of radioactive samples using gamma spectroscopy technique. A limitation of detecting low energy gamma rays from decaying radioactive nuclei, is the Compton background which can be significantly reduced by rejecting Compton scattered events through active Bismuth germanate (BGO) shielding. On the other hand, for a CLOVER detector without BGO shielding, one can place the radioactive samples very close to the detector for enhancing geometrical efficiency. A single crystal High Purity Germanium (HPGe) detector can also be used for decay rate measurements. In order to measure the decay rate of nuclei decaying via gamma emission with reasonable intensity, optimal close geometry options have been investigated for various HPGe detector configurations.

     

Monte Carlo simulation of PGNAA system for determining element content in the rock sample

The element content in rock sample can be determined by prompt gamma ray activation analysis technology. The neutron distributions under the conditions with different moderating materials, moderator size and distance from neutron source to lead-out hole were simulated using Monte Carlo method, and then the optimal structure parameters to get the highest thermal neutron flux was obtained. The PGNAA system with optimal parameters based on ²⁵²Cf neutron source was founded. In addition, the rock and element standard samples were irradiated by thermal neutron in this system. Moreover, the element content was calculated by processing gamma ray spectroscopy recorded, and it is in agreement with result of XRF method.     

Assessment of the suitability of Monte Carlo simulation for activity measurements of extended sources

Monte Carlo simulations can be a powerful tool in calibrating high-resolution gamma-ray spectrometry based on high pure germanium (HPGe) detectors. The purpose of this work is to examine the applicability of Monte Carlo simulations for the computation of the efficiency transfer in various measurement geometries on the basis of the detected efficiency for point source geometry. For this, GEANT4 code was applied for the computation of the detection efficiency for incident gamma energy of radionuclide placed at different distances from HPGe detector from 50 to 2,000 keV in addition for volume sources of different compositions and densities. The experimental efficiency curves were compared with the prediction of the GEANT4 code. Efficiency is computed at discrete values of point and volume sources in different distances to derive new efficiencies values for other distances.     

Multiple prompt gamma-ray analysis and construction of its beam line

By combining neutron activation analysis with multiple gamma-ray detection (gamma-gamma coincidence), we have proved better sensitivity and resolution for the trace element analysis than the ordinary single gamma-ray detection method. We now try to apply the multiple gamma-ray detection method to the prompt gamma ray analysis (PGA). We have established a new cold neutron beam line for PGA in Japan Research Reactor, JRR-3M, at Tokai establishment of Japan Atomic Energy Research Institute (JAERI). It consists of a beam shutter, a beam attenuator, a gamma-ray detector array, a sample changer, and a beam stopper. We construct a high-efficiency gamma-ray detector array specially designed for this purpose. Its performance has been evaluated with the Monte Carlo simulation code, GEANT 4.5.0.     

An atlas of selected beta-ray spectra and depth-dose distributions in lithium fluoride and soft tissue generated by a fast Monte Carlo-based sampling method

A method to generate depth-dose distributions due to beta radiation in LiF and soft tissue is proposed. In this method, the EGS4 Monte Carlo radiation transport code is initially used to generate a library of monoenergetic electron depth-dose distributions in the material for electron energies in the range of 10 keV to 5 MeV in 10 keV increments. A polynomial least-squares fit is applied to each distribution. In addition, a theoretical model is developed to generate beta-ray energy spectra of selected radionuclides. A standard Monte Carlo random sampling technique is then employed to sample the spectra and generate the depth-dose distributions in LiF and soft tissue. The proposed method has an advantage over more traditional methods in that the actual radiation transport in the media is performed only once for a set of monoenergetic cases and the beta depth-dose distributions are easily generated by sampling this previously-acquired database in a matter of minutes. This method therefore reduces the demand on computer resources and time. The method can be used to calculate depth-dose distribution due to any beta-emitting nuclide or combination of nuclides with up to ten beta components.     

Comparison between HPGe and CdZnTe detector for the correlation between calculated radioactivity and measured dose using an activated concrete sample

An activated concrete sample was counted at different source to detector distances with CdZnTe and HPGe detectors. The experimental count rates for different radionuclides were converted to dose rate using Monte Carlo code and compared with the Measured dose rates obtained using digital survey meter. The results agreed well for both the detectors. This indicates that CdZnTe detector having a better portability but poorer resolution than HPGe detector can be effectively used for online monitoring of radioactivity as well as dose rate calculations.