Luke W. Campbell

Computer simulation of electron thermalization in CsI and CsI(Tl)

A Monte Carlo (MC) model was developed and implemented to simulate the thermalization of electrons in inorganic scintillator materials. The model incorporates electron scattering with both longitudinal optical and acoustic phonons. In this paper, the MC model was applied to simulate electron thermalization in CsI, both pure and doped with a range of thallium concentrations. The inclusion of internal electric fields was shown to increase the fraction of recombined electron-hole pairs and to broaden the thermalization distance and thermalization time distributions. The MC simulations indicate that electron thermalization, following γ-ray excitation, takes place within approximately 10 ps in CsI and that electrons can travel distances up to several hundreds of nanometers. Electron thermalization was studied for a range of incident γ-ray energies using electron-hole pair spatial distributions generated by the MC code NWEGRIM (NorthWest Electron and Gamma Ray Interaction in Matter). These simulations revealed ...

Monte Carlo simulations of electron thermalization in alkali iodide and alkaline-earth fluoride scintillators

A Monte Carlo model of electron thermalization in inorganic scintillators, which was developed and applied to CsI in a previous publication [Wang et al., J. Appl. Phys. 110, 064903 (2011)], is extended to another material of the alkali halide class, NaI, and to two materials from the alkaline-earth halide class, CaF2 and BaF2. This model includes electron scattering with both longitudinal optical (LO) and acoustic phonons as well as the effects of internal electric fields. For the four pure materials, a significant fraction of the electrons recombine with self-trapped holes and the thermalization distance distributions of the electrons that do not recombine peak between approximately 25 and 50 nm and extend up to a few hundreds of nanometers. The thermalization time distributions of CaF2, BaF2, NaI, and CsI extend to approximately 0.5, 1, 2, and 7 ps, respectively. The simulations show that the LO phonon energy is a key factor that affects the electron thermalization process. Indeed, the higher the LO pho...

Electron-Hole Pairs Created by Photons and Intrinsic Properties in Detector Materials

A Monte Carlo (MC) code has been developed to simulate the interaction of gamma-rays with semiconductors and scintillators, and the subsequent energy partitioning of fast electrons. The results provide insights on the processes involved in the electron-hole pair yield and intrinsic variance through simulations of full electron energy cascades. The MC code has been applied to simulate the production of electron-hole pairs and to evaluate intrinsic resolution in a number of semiconductors. In addition, the MC code is also able to consider the spatial distribution of electron-hole pairs induced by photons and electrons in detector materials, and has been employed to obtain details of the spatial distribution of electron-hole pairs in Ge, as a benchmark case. The preliminary results show that the distribution of electron-hole pairs exhibit some important features; (a) the density of electron-hole pairs along the main electron track is very high and (b) most electron-hole pairs produced by interband transitions are distributed at the periphery of the cascade volume. The spatial distribution and density of thermalized electron-hole pairs along the primary and secondary tracks are important for large scale simulations of electron-hole pair transport.

High-Energy Delayed Gamma Spectroscopy for Spent Nuclear Fuel Assay

High-accuracy, direct, nondestructive measurement of fissile and fissionable isotopes in spent fuel, particularly the Pu isotopes, is a well-documented, but still unmet challenge in international safeguards. As nuclear fuel cycles propagate around the globe, the need for improved materials accountancy techniques for irradiated light-water reactor fuel will increase. This modeling study investigates the use of delayed gamma rays from fission-product nuclei to directly measure the relative concentrations of 235U, 239Pu, and 241Pu in spent fuel assemblies. The method is based on the unique distribution of fission-product nuclei produced from fission in each of these fissile isotopes. Fission is stimulated in the assembly with a pulse-capable source of interrogating neutrons. The measured distributions of the short-lived fission products from the unknown sample are then fit with a linear combination of the known fission-product yield curves from pure 235U, 239Pu, and 241Pu to determine the original proportions of these fissile isotopes. Modeling approaches for the intense gamma-ray background promulgated by the long-lived fission-product inventory and for the high-energy gamma-ray signatures emitted by short-lived fission products from induced fission are described. Benchmarking measurements are presented and compare favorably with the results of these models. Results for the simulated assay of simplified individual fuel rods ranging from fresh to 60-GWd/MTU burnup demonstrate the utility of the modeling methods for viability studies, although additional work is needed to more realistically assess the potential of High-Energy Delayed Gamma Spectroscopy (HEDGS).

Monte Carlo simulation of gamma-ray response of BaF2 and CaF2

We have employed a Monte Carlo (MC) method to study intrinsic properties of two alkaline-earth halides, namely, BaF2 and CaF2, relevant to their use as radiation detector materials. The MC method follows the fate of individual electron-hole (e-h) pairs and thus allows for a detailed description of the microscopic structure of ionization tracks created by incident γ-ray radiation. The properties of interest include the mean energy required to create an e-h pair, W, Fano factor, F, the maximum theoretical light yield, and the spatial distribution of e-h pairs resulting from γ-ray excitation. Although W and F vary with incident photon energy at low energies, they tend to constant values at energies higher than 1 keV. W is determined to be 18.9 and 19.8 eV for BaF2 and CaF2, respectively, in agreement with published data. The e-h pair spatial distributions exhibit a linear distribution along the fast electron tracks with high e-h pair densities at the end of the tracks. Most e-h pairs are created by interband...

Radiation response of inorganic scintillators: Insights from Monte Carlo simulations

The spatial and temporal scales of hot particle thermalization in inorganic scintillators are critical factors determining the extent of second- and third-order nonlinear quenching in regions with high densities of electron-hole pairs, which, in turn, leads to the light yield nonproportionality observed, to some degree, for all inorganic scintillators. Therefore, kinetic Monte Carlo simulations were performed to calculate the distances traveled by hot electrons and holes as well as the time required for the particles to reach thermal energy following γ-ray irradiation. CsI, a common scintillator from the alkali halide class of materials, was used as a model system. Two models of quasi-particle dispersion were evaluated, namely, the effective mass approximation model and a model that relied on the group velocities of electrons and holes determined from band structure calculations. Both models predicted rapid electron-hole pair recombination over short distances (a few nanometers) as well as a significant extent of charge separation between electrons and holes that did not recombine and reached thermal energy. However, the effective mass approximation model predicted much longer electron thermalization distances and times than the group velocity model. Comparison with limited experimental data suggested that the group velocity model provided more accurate predictions. Nonetheless, both models indicated that hole thermalization is faster than electron thermalization and thus is likely to be an important factor determining the extent of third-order nonlinear quenching in high-density regions. The merits of different models of quasi-particle dispersion are also discussed.

Measurement and analysis of gamma-rays emitted from spent nuclear fuel above 3 MeV.

The gamma-ray spectrum of spent nuclear fuel in the 3-6 MeV energy range is important for active interrogation since gamma rays emitted from nuclear decay are not expected to interfere with measurements in this energy region. There is, unfortunately, a dearth of empirical measurements from spent nuclear fuel in this region. This work is an initial attempt to partially fill this gap by presenting an analysis of gamma-ray spectra collected from a set of spent nuclear fuel sources using a high-purity germanium detector array. This multi-crystal array possesses a large collection volume, providing high energy resolution up to 16 MeV. The results of these measurements establish the continuum count-rate in the energy region between 3 and 6 MeV. Also assessed is the potential for peaks from passive emissions to interfere with peak measurements resulting from active interrogation delayed emissions. As one of the first documented empirical measurements of passive emissions from spent fuel for energies above 3 MeV, this work provides a foundation for active interrogation model validation and detector development.

Monte Carlo simulation of electron thermalization in scintillator materials: Implications for scintillator nonproportionality

The lack of reliable quantitative estimates of the length and time scales associated with hot electron thermalization after a gamma-ray induced energy cascade obscures the interplay of various microscopic processes controlling scintillator performance and hampers the search for improved detector materials. We apply a detailed microscopic kinetic Monte Carlo model of the creation and subsequent thermalization of hot electrons produced by gamma irradiation of six important scintillating crystals to determine the spatial extent of the cloud of excitations produced by gamma rays and the time required for the cloud to thermalize with the host lattice. The main ingredients of the model are ensembles of microscopic track structures produced upon gamma excitation (including the energy distribution of the excited carriers), numerical estimates of electron-phonon scattering rates, and a calculated particle dispersion to relate the speed and energy of excited carriers. All these ingredients are based on first-princi...

Applications of Monte Carlo Methods to Simulate Gamma Ray Interactions in Si and Ge

A Monte Carlo code is employed to simulate the electron cascade subsequent to a gamma ray interaction in two common semiconductors, silicon and germanium, over the energy range of 50 eV to 2 MeV. The partitioning of the gamma ray energy into the various loss mechanisms determines the performance of the detector, generally parameterized by the average energy to create a charge carrier pair, W, and the intrinsic variance or Fano factor, F. In this work, W and F are found as a function of energy, exhibiting saw-toothed variation at the shell edges and a well defined high energy value well above the K edge. Our calculated results are in agreement with experiment Valence to conduction interband transitions and plasmon excitations are the dominant source of electron-hole pairs.

Streamlined Monte Carlo simulation of environmental gamma-ray backgrounds for radiation detector sensitivity comparisons

In recent research to compare detection sensitivities of gamma spectrometers applied to in situ and field laboratory scenarios, the authors lacked background data for comparable detection sensitivity calculations. To overcome this, experimental measurements and Monte Carlo modeling of terrestrial gamma radiation were undertaken. Inspired by Vojtyla’s research to reduce the computing burden of modeling bremsstrahlung from lead surfaces, this related approach defines a gamma-ray surface source representing emission of background gamma-rays from the earth. This work presents a surface source based on the 40K, 137Cs, uranium, and thorium content of Hanford soil, and compares modeled backgrounds to experimental in situ gamma measurements.