Study on reconstruction and analytical method of seawater radioactive gamma spectrum.

Gamma detector detection technology based on NaI(Tl) scintillation crystal has become a popular research topic and has been applied in the field of marine radioactive environment automatic monitoring because of its advantages of low power consumption, low cost and strong environmental adaptability. However, insufficient energy resolution of the NaI(Tl) detector and great Compton scattering in the low-energy region caused by the abundance of natural radionuclides in seawater hinder the automatic analysis of radionuclides in seawater. This study adopts the combination of theoretical derivation, simulation experiment, water tank test and seawater field test, establishing an effective and feasible spectrum reconstruction method. The measured spectrum in seawater is regarded as the output signal formed by the convolution of the incident spectrum and the detector response function. The acceleration factor p is introduced to construct the Boosted-WNNLS deconvolution algorithm, which is used to iteratively reconstruct the spectrum. The analysis results of the simulation test, water tank test and field test meet the radionuclide analysis speed and accuracy requirements for the in-situ automatic monitoring of seawater radioactivity. The spectrum reconstruction method in this study converts the physical problem of insufficient detection accuracy of spectrometer in the practical application into a mathematical problem of deconvolution solution, restores the original radiation information in seawater, and improves the resolution of the seawater gamma spectrum.

2D inversion of in situ gamma-ray spectrometric measurements of 137Cs for site characterization.

Environmental contamination by radioactive materials can be characterized by in situ gamma surface measurements. During such measurements, the field of view of a gamma detector can be tens of meters wide, resulting in a count rate that integrates the signal over a large measurement support volume/area. The contribution of a specific point to the signal depends on various parameters, such as the height of the detector above the ground surface, the gamma energy and the detector properties, etc. To improve the spatial resolution of the activity concentration, contributions of a radionuclide from nearby areas to the count rate of a single measurement should be disentangled. The experiments described in this paper, deployed 2D inversion of in situ gamma spectrometric measurements using a non-negative least squares-based Tikhonov regularization method. Data were acquired using a portable LaBr3 gamma detector. The detector response as a function of the distance of the radioactive source, required for the inversion process, was simulated using the Monte Carlo N-Particle (MCNP) transport code. The uncertainty on activity concentration was calculated using the Monte Carlo error propagation method. The 2D inversion methodology was first satisfactorily assessed for 133Ba and 137Cs source activity distributions using reference pads. Secondly, this method was applied on a 137Cs contaminated site, making use of above-ground in-situ gamma spectrometry measurements, conducted on a regular grid. The inversion process results were compared with the results from in-situ borehole measurements and laboratory analyses of soil samples. The calculated 137Cs activity concentration levels were compared against the activity concentration value for exemption or clearance of materials which can be applied by default to any amount and any type of solid material. Using the 2D inversion and the Monte Carlo error propagation method, a high spatial resolution classification of the site, in terms of exceeding the exemption limit, could be made. The 137Cs activity concentrations obtained using the inversion process agreed well with the results from the in-situ borehole measurements and those from the soil samples, showing that the 2D inversion is a convenient approach to deconvolute the contribution of radioactive sources from nearby areas within a detector's field of view, and increases the resolution of spatial contamination mapping.

Unmanned stationary online monitoring system based on buoy for marine gamma radioactivity.

Research on unmanned online monitoring equipment for marine radioactivity surrounding nuclear power plants is of great significance. In this work, a small radioactivity monitoring system based on buoy was designed and manufactured for the emergency situation of nuclear accidents. The core of the radioactivity monitoring system is the underwater gamma spectrometer. The spectrometer can respond to gamma rays from 60 keV to 3 MeV, and can identify the nuclides whose characteristic rays belong to this energy range. The detection efficiency curve was calculated through Monte Carlo simulation and verified in a standard liquid source. A data acquisition processor was also designed to coordinate the detectors in the system and wirelessly transmit online monitoring data. Three experiments were carried out in the seawater around the Tianwan Nuclear Power Plant in Lianyungang, China using this online marine radioactivity monitoring system based on buoys. The stability and radioactivity monitoring capabilities of the system have been verified.

Background shielding by dense samples in low-level gamma spectrometry.

In low activity gamma spectrometric measurements of large, dense samples, the bulk sample material shields the HPGe crystal from external background sources. If not accounted for in studies that utilise background-subtraction methods, this effect may result in systematic errors in the sample activity and detection limit estimation. We introduce a Monte Carlo based method to minimise the impact of this effect on sample gamma spectra. It is validated using simulated detector backgrounds and applied to a measurement of low-activity [Formula: see text] . One main prerequisite for the correct application of this method is to know in advance the nuclides which contribute to the detector background spectrum and their spatial distribution. With a thorough understanding of the detector backgrounds, the method improves the accuracy of sensitive low-background measurements of low-activity samples. Even without knowing the background sources and their distribution, conservative results may still be presented that account for the potential systematic errors introduced by this background shielding effect.

Study of radionuclides and heavy metal migration through soil profiles (0-60 cm) at points near the targets of NATO strikes in 1995: environmental monitoring and assessment.

The activity concentrations of natural and artificial radionuclides (40K, 232Th, 226Ra, 238U, 137Cs) and concentrations of six heavy metals of interest (Cd, Cr, Cu, Ni, Pb and Zn) were investigated in 18 soil samples through soil depths (0-10, 10-20, 20-30, 30-40.40-50, 50-60 cm) at the three selected sites in the Hadzici. Since at this area ammunition with depleted uranium had been used during the NATO strikes in 1995, this study was conducted with the aim to assess the radiological and environmental health hazards. Radioactivity was determined by gamma spectrometry using HPGe and LEGE detectors and content of heavy metals by using a flame atomic absorption spectrometry. The correlation with distribution of the radionuclides and their activity concentrations through depths was found only at the site 1 for 40K, 232Th and 226Ra, where minimum/maximum activity concentrations for 40K were 814.42 Bq/kg/1039.48 Bq/kg, for 232Th 53.98 Bq/kg/74.12 Bq/kg and for 226Ra 50.32 Bq/kg/65.73 Bq/kg. Vertical distribution of 137Cs along 3 site profiles was used for distinction of cultivated and uncultivated soil. Using the activity ratio of 238U/226Ra and 235U/238U, the presence of depleted uranium (DU) was established at the site 3. Obtained Igeo values for determined heavy metals showed that all of three sites were unpolluted to moderately polluted. Pb content in all three sites showed correlation with concentration decreasing with increasing soil depth.

Natural radioactivity assessment and geophysical interpretation of parts of Igarra area, Southern Nigeria.

To evaluate the concentration of natural radionuclides and to carry out geophysical interpretation of part of Igarra area, Southern Nigeria, an integrated geophysical approach was adopted involving radiometric, gravity, and magnetic methods. The RS-230 Super-Spec spectrometer, G-512 Lacoste and Romberg gravimeter, and the GSM-19v7.0 Overhauser instrument were used for the radiometric, gravity, and magnetic data acquisitions, respectively, along a specified traverse within the area. The datasets were processed using Oasis Montaj, Grav-Master, and Ms-Excel software. Gravity results show that the mean free air and Bouguer anomalies in the area are - 67.42 and - 84.22 mGal, while magnetic survey indicates that the mean corrected magnetic field intensity in this area is 32218.49 nT. Radiometric survey results show that the mean radioactivity concentrations of thorium ([Formula: see text], uranium ([Formula: see text]), and potassium ([Formula: see text]) are 31.81 Bq/kg, 26.48 Bq/kg, and 167.33 Bq/kg, respectively. Further analysis also revealed that the mean radioactivity equivalent of the area is 84.86 Bq/kg; absorbed dose rate is 72.74nGy/h, while the mean external hazard index is 0.30. A novel model equation for estimating absorbed dose rate from radioactivity equivalent was also obtained and validated. The gravity and magnetic survey results indicate the presence of low-density and high magnetic basement rocks underlying this area, while radiometric results reveal that radiations in this area did not exceed acceptable standards of 370 Bq/kg for radioactivity equivalent, 84 nGy/h for absorbed dose rate, and unity which corresponds to 370 Bq/kg for external hazard index as recommended by the United Nations Scientific Committee on the Effects of Atomic Radiation and the International Atomic Energy Agency.

Minimum detectable activity concentration of radio-cesium by a LaBr3(Ce) detector for in situ measurements on the ground-surface and in boreholes.

A 3.81 × 3.81 cm LaBr3(Ce) detector based portable measurement setup has been developed for in situ gamma spectrometric survey of a contaminated site. This system is suitable for above- and below ground surface gamma spectrometric measurements of 137Cs. However, the minimum detectable activity concentration (MDAC), an important parameter of a measurement system, should be estimated for planning purposes of the gamma spectrometric survey. In this study, the MDAC of 137Cs for the measurement setup was investigated. The efficiency of the measurement setups was calculated from Monte Carlo simulations using MCNP code. The numerical model of the different studied set-ups, used in MCNP, performed well for the known cases. The results show that the MDAC varies with the position of the detector with respect to ground surface. A 5-20 min acquisition time, depending on the detector position, can be sufficient to get a MDAC of about 10% of the exemption limit of 137Cs (100 Bq/kg).

Radioactive risk assessment of beach sand along the coastline of Mediterranean Sea at El-Arish area, North Sinai, Egypt.

Beach sand includes various levels of natural radioactivity, which can cause health effects. The natural radioactivity was measured in the beach sand along the coastline of the Mediterranean Sea at the east of the El-Arish area, Egypt. Using the HPGe spectrometer, the contribution of radionuclides 226Ra, 232Th and 40K in the gamma emitted radiation illustrated that the 226Ra, 232Th and 40K activity concentrations are 8.8 ± 3.9, 30.8 ± 12.2 and 106.9 ± 46.8 Bq kg-1, respectively, which is lower than the reported worldwide limit 33, 45 and 412 Bq kg-1. The radioactive hazards associated with the beach sand along the coastline of the Mediterranean Sea at the east of the El-Arish area were investigated. The obtained results among the radiological hazard parameters, the radium equivalent content (Raeq), the absorbed dose rate (Dair), annual effective dose (AED), external (Hex) and internal (Hin) hazard indices were estimated. Moreover, the excess lifetime cancer risk (ELCR) and the annual gonadal dose equivalent (AGDE) were also computed and illustrated their values less than the recommended levels. Multivariate statistical approaches like Pearson correlation, the principal component analysis (PCA) and the hierarchical cluster analysis (HCA) were applied to investigate the correlation between the radionuclides and the corresponding radiological hazard variables. Based on the statistical analysis, the 226Ra and 232Th mainly contribute to the radioactive risk of beach sand. Finally, no significant risk of the public associated with utilizing beach sand in building materials.

Design and Characterization of an Extremely-Sensitive, Large-Volume Gamma-Ray Spectrometer for Environmental Samples.

A large volume gamma spectrometer was designed and constructed to analyze foodstuffs and environmental samples having low radionuclide concentrations. This system uses eight 11-cm × 42.5-cm × 5.5-cm NaI(Tl) detectors, chosen due to their relatively high sensitivity and availability and arranged in an octagonal configuration. The sensitive volume of the system is ~28 cm in diameter and ~42 cm deep. Shielding consists of an 86-cm × 86-cm square, 64-cm-tall lead brick enclosure with 18-cm-thick lead walls lined by 0.3-cm-thick copper plates. An aluminum top was machined to suspend the detectors within this shield. The shielding reduces background counts by 72% at 100 keV and 42% at 1,000 keV. The positional variability in sensitivity of the well was determined by both simulation and experiment. A 2.1-L volume of nearly uniform sensitivity, varying less than 10%, exists in the well's center. Energy resolutions of 14.6% and 7.8% were measured for Am and Cs, respectively. Energy resolution shows a 0.2% variation for both Am and Cs as a function of position within all regions of the well's central sensitive volume. Dead time was also determined to be less than 35% for all sources measured in the system, the largest of which had an activity of 1,760 kBq. Simulated results for various source geometries show higher counts for smaller samples, especially at lower energies due to less attenuation of low energy photons. Minimum detectable activities were determined for all source energies used, less than 5.1 Bq kg for reasonable background and sample counting times.

Prompt gamma spectroscopy for absolute range verification of 12C ions at synchrotron-based facilities.

The physical range uncertainty limits the exploitation of the full potential of charged particle therapy. In this work, we face this issue aiming to measure the absolute Bragg peak position in the target. We investigate p, 4He, 12C and 16O beams accelerated at the Heidelberg Ion-Beam Therapy Center. The residual range of the primary 12C ions is correlated to the energy spectrum of the prompt gamma radiation. The prompt gamma spectroscopy method was demonstrated for proton beams accelerated by cyclotrons and is developed here for the first time for heavier ions accelerated by a synchrotron. We develop a detector system that includes (i) a spectroscopic unit based on cerium(III) bromide and bismuth germanium oxide scintillating crystals, (ii) a beam trigger based on an array of scintillating fibers and (iii) a data acquisition system based on a FlashADC. We test the system in two different scenarios. In the first series of experiments, we detect and identify 19 independent spectral lines over a wide gamma energy spectrum in the presence of the four ion species for different targets, including a water target with a titanium insert. In the second series of experiments, we introduce a collimator aiming to relate the spectral information to the range of the primary particles. We perform extensive measurements for a 12C beam and demonstrate submillimetric precision for the measurement of its Bragg peak position in the experimental setup. The features of the energy and time spectra for gamma radiation induced by p, 4He and 16O are investigated upstream and downstream from the Bragg peak position. We conclude the analysis by extrapolating the required future developments, which would be needed to achieve range verification with a 2 mm accuracy during a single fraction delivery of [Formula: see text] physical dose.

Development of the Environmental Radiation Survey Program and Its Application to In Situ Gamma-Ray Spectrometry.

An environmental radiation survey using a gamma-ray spectrometer is used to rapidly detect radioactive contamination over a wide area of ground that was released from nuclear events. For the successful application of a gamma-ray spectrometer to the calculation of the radioactivity concentration in the ground and the dose rate at 1 m above the ground, it is necessary to build a calibration procedure to obtain the counting efficiency at the in situ measurement, which means in situ calibration factor to report the calculation results from the measured net count rate according to the diverse detection geometries. This study is focused on the development of a program to calculate the in situ calibration factor and report the survey results in the environmental radiation surveys using three kinds of gamma-ray spectrometers, which have been widely used in the field of in situ measurements: a coaxial HPGe detector, cylindrical NaI(Tl), and rectangular NaI(Tl). The program is based on the results of diverse theoretical calculations of the unscattered photon fluence at the detector height, detector responses of three detectors, and their angular corrections. The developed program was successfully applied to the estimation of the radioactivity concentration of nuclides in the ground and the dose rate at 1 m height above the ground induced from them.

A full-scale clinical prototype for proton range verification using prompt gamma-ray spectroscopy.

We present a full-scale clinical prototype system for in vivo range verification of proton pencil-beams using the prompt gamma-ray spectroscopy method. The detection system consists of eight LaBr3 scintillators and a tungsten collimator, mounted on a rotating frame. Custom electronics and calibration algorithms have been developed for the measurement of energy- and time-resolved gamma-ray spectra during proton irradiation at a clinical dose rate. Using experimentally determined nuclear reaction cross sections and a GPU-accelerated Monte Carlo simulation, a detailed model of the expected gamma-ray emissions is created for each individual pencil-beam. The absolute range of the proton pencil-beams is determined by minimizing the discrepancy between the measurement and this model, leaving the absolute range of the beam and the elemental concentrations of the irradiated matter as free parameters. The system was characterized in a clinical-like situation by irradiating different phantoms with a scanning pencil-beam. A dose of 0.9 Gy was delivered to a [Formula: see text] cm3 target with a beam current of 2 nA incident on the phantom. Different range shifters and materials were used to test the robustness of the verification method and to calculate the accuracy of the detected range. The absolute proton range was determined for each spot of the distal energy layer with a mean statistical precision of 1.1 mm at a 95% confidence level and a mean systematic deviation of 0.5 mm, when aggregating pencil-beam spots within a cylindrical region of 10 mm radius and 10 mm depth. Small range errors that we introduced were successfully detected and even large differences in the elemental composition do not affect the range verification accuracy. These results show that our system is suitable for range verification during patient treatments in our upcoming clinical study.

Investigating the potentialities of Monte Carlo simulation for assessing soil water content via proximal gamma-ray spectroscopy.

Proximal gamma-ray spectroscopy recently emerged as a promising technique for non-stop monitoring of soil water content with possible applications in the field of precision farming. The potentialities of the method are investigated by means of Monte Carlo simulations applied to the reconstruction of gamma-ray spectra collected by a NaI scintillation detector permanently installed at an agricultural experimental site. A two steps simulation strategy based on a geometrical translational invariance is developed. The strengths of this approach are the reduction of computational time with respect to a direct source-detector simulation, the reconstruction of 40K, 232Th and 238U fundamental spectra, the customization in relation to different experimental scenarios and the investigation of effects due to individual variables for sensitivity studies. The reliability of the simulation is effectively validated against an experimental measurement with known soil water content and radionuclides abundances. The relation between soil water content and gamma signal is theoretically derived and applied to a Monte Carlo synthetic calibration performed with the specific soil composition of the experimental site. Ready to use general formulae and simulated coefficients for the estimation of soil water content are also provided adopting standard soil compositions. Linear regressions between input and output soil water contents, inferred from simulated 40K and 208Tl gamma signals, provide excellent results demonstrating the capability of the proposed method in estimating soil water content with an average uncertainty <1%.

In situ measurement of radioactive contamination of bottom sediments.

A gamma spectrometric method is presented for in situ radiation monitoring of bottom sediments with contaminated layer of unknown thickness to be determined. The method, based on the processing of experimental spectra using the results of their simulation by the Monte Carlo method, is proposed and tested in practice. A model for the transport of gamma radiation from deposited radionuclides 137Cs and 134Cs to a scintillation detection unit located on the upper surface of the contaminated layer of sediments is considered. The relationship between the effective radius of the contaminated site and the thickness of the layer has been studied. The thickness of the contaminated layer is determined by special analysis of experimental and thickness-dependent simulated spectra. The technique and algorithm developed are verified as a result of full-scale studies performed with the submersible gamma-spectrometer.

Monte Carlo method for gamma spectrometry based on GEANT4 toolkit: Efficiency calibration of BE6530 detector.

The combination of gamma-ray spectrometry, the development of related Monte Carlo method and the GEANT4 (GEometry ANd Tracking) toolkit have been developed for gamma spectrometry simulation. The main objective was to validate simulation models of broad energy germanium (BEGe) detector geometry built in our laboratory (BE6530 model). Monte Carlo simulation of the geometry of BE6530 detector for efficiency calibration was carried out with GEANT4 toolkit. The simulated efficiencies curves using MC were compared with experimental results. Measurement uncertainties for both simulation and experimental estimations of the efficiency were assessed in order to see whether the consequences of the realistic measurement fall inside adequate cut-off points. The validation of the simulation was carried out by experimentally estimating the activity concentration in a reference sample and the comparison showed good correlation between experimental and simulation. Therefore, from the outcomes of this study, it can be concluded that Monte-Carlo simulation is a helpful, reasonable option that additionally gives more prominent adaptability, greater flexibility, precision and accuracy, and gained time when determining the detector response and efficiency in routine of environmental radioactivity monitoring.

Environmental risk assessment of radioactivity and heavy metals in soil of Toplica region, South Serbia.

Activity levels of natural and artificial radionuclides and content of ten heavy metals (As, Cd, Co, Cr, Cu, Mn, Ni, Pb, Zn and Hg) were investigated in 41 soil samples collected from Toplica region located in the south part of Serbia. Radioactivity was determined by gamma spectrometry using HPGe detector. The obtained mean activity concentrations ± standard deviations of radionuclides 226Ra, 232Th, 40K and 137Cs were 29.9 ± 9.4, 36.6 ± 11.5, 492 ± 181 and 13.4 ± 18.7 Bq kg-1, respectively. According to Shapiro-Wilk normality test, activity concentrations of 226Ra and 232Th were consistent with normal distribution. External exposure from radioactivity was estimated through dose and radiation risk assessments. Concentrations of heavy metals were measured by using ICP-OES, and their health risks were then determined. Enrichment by heavy metals and pollution level in soils were evaluated using the enrichment factor, the geoaccumulation index (Igeo), pollution index and pollution load index. Based on GIS approach, the spatial distribution maps of radionuclides and heavy metal contents were made. Spearman correlation coefficient was used for correlation analysis between radionuclide activity concentrations and heavy metal contents.

Application of a Monte Carlo method to the uncertainty assessment in in situ gamma-ray spectrometry.

In situ gamma-ray spectrometry has since the introduction of portable germanium detectors been a widely used method for the assessment of radionuclide ground deposition activity levels. It is, however, a method that is most often associated with fairly large and, more important, poorly known combined measurement uncertainties. In this work an uncertainty analysis of in situ gamma ray spectrometry in accordance with the Guide to the Expression of Uncertainty in Measurements is presented. The uncertainty analysis takes into account uncertainty contributions from the calibration of the detector system, the assumed activity distribution in soil, soil density, detector height and air density. As a result, measurement results from in situ gamma spectrometry will serve as a better basis for decision-making in e.g. radiological emergencies.

Improvement of in-situ gamma spectrometry methods by Monte-Carlo simulations.

Performing in-situ measurements of gamma radiation originating from soil requires adequate detection efficiency curves, which can be obtained by Monte-Carlo simulations. In simulations, soil density of 1.046 g/cm3 was used, with the following elemental composition of soil in which gamma radiation was generated: O - 47%, Si -35%, Al - 8%, Fe - 3.9%, C - 2.1%, Ca - 1.4%, K - 1.3%, N - 0.6%, Mg - 0.6%, N - 0.1%. Soil matrix was represented by cylindrical volume of 1.5 m diameter and 0.5m thickness, while germanium detector was placed at 1 m height above the soil. The simulated gamma spectrum, originated from K-40, as well as from members of Th-232 chain, and daughters of Ra-226, was obtained. Homogeneous distribution of various radionuclides (Ra-226, Th-232, K-40) in soil matrix is considered in this work. Gamma spectra obtained in simulations were analyzed, and together with simulated detection efficiency data they provide comparison with real experimental measurements and practical application of results derived by Monte-Carlo simulations. As a result of this work, the corresponding detection efficiency curve for HPGe detector was obtained, which can be applied for in-situ measurements of radionuclide concentration in soil, assuming uniform radionuclide distribution. In order to validate our simulation results regarding detection efficiency, we performed in-situ measurements of soil radioactivity and compared the obtained activity concentrations with laboratory measurements. We found a good agreement, within activity concentration uncertainty, between in-situ measurement results and average values of activity concentrations obtained by laboratory measurements.

Assessment of the calibration of gamma spectrometry systems in forest environments.

A Monte Carlo simulation was used to develop a model of the response of a portable gamma spectrometry system in forest environments. This model was used to evaluate any corrections needed to measurements of 137Cs activity per unit area calibrated assuming an open field geometry. These were shown to be less than 20% for most forest environments. The model was also used to assess the impact of activity in the canopy on ground level measurements. For similar activity per unit area in the lower parts of the canopy as on the ground, 10-25% of the ground based measurement would be due to activity in the canopy, depending on the depth profile in the soil. The model verifies that an optional collimator cap can assess activity in the canopy by repeat survey.

A New Approach for the Determination of Dose Rate and Radioactivity for Detected Gamma Nuclides Using an Environmental Radiation Monitor Based on an NaI(Tl) Detector.

To expand the application of dose rate spectroscopy to the environment, the method using an environmental radiation monitor (ERM) based on a 3' × 3' NaI(Tl) detector was used to perform real-time monitoring of the dose rate and radioactivity for detected gamma nuclides in the ground around an ERM. Full-energy absorption peaks in the energy spectrum for dose rate were first identified to calculate the individual dose rates of Bi, Ac, Tl, and K distributed in the ground through interference correction because of the finite energy resolution of the NaI(Tl) detector used in an ERM. The radioactivity of the four natural radionuclides was then calculated from the in situ calibration factor-that is, the dose rate per unit curie-of the used ERM for the geometry of the ground in infinite half-space, which was theoretically estimated by Monte Carlo simulation. By an intercomparison using a portable HPGe and samples taken from the ground around an ERM, this method to calculate the dose rate and radioactivity of four nuclides using an ERM was experimentally verified and finally applied to remotely monitor them in real-time in the area in which the ERM had been installed.