From angstroms to microns: a nuclear fuel microstructure evolution model whose parameters are calculated at the atomic scale
Controlling the behavior of fission gases in nuclear fuel (uranium oxide) is an important industrial issue, as fission gas release or precipitation limit the use of fuels at extended burn-ups. The gas behavior is strongly influenced by the material’s microstructure evolution due to the aggregation of irradiation-induced defects (gas bubbles, dislocation loops and lines). Cluster dynamics (CD) (a kind of rate theory model) is relevant for modelling the nucleation/growth of the defect clusters, there gas content and the gas release. The current model has been parameterized following a multiscale approach, based on atomistic calculations (ab initio or empirical potentials). This model has been successfully applied to annealing experiments of UO2 samples implanted with rare gas atoms and has emphasized the impact of the irradiation damage on gas release. The aim of this PhD thesis is now to improve the model, particularly the damage parameterization, and to extend its validation domain through in depth comparison of simulation with a large set of recently obtained experimental results, such as gas release measurement by annealing of sample implanted in ion beam accelerator, bubble and loop observation by transmission electrons microscopy of implanted or in-pile irradiated samples. This global analysis will finally yield an improved parameterization of the CD model.
The research subject combines a “theoretical” dimension (improving the model) with an “experimental” one (interpreting existing experiments or designing some new ones). The variety of techniques will introduce you into the experimental world and thus broaden your scientific skills. You will be welcomed at the Fuel Behavior Modeling Laboratory (part of the Institute for Research on Nuclear Systems for Low-Carbon Energy Production, IRESNE, CEA Cadarache), where you will benefit from an open environment rich in academic collaborations. You also have to manage collaborations for the experiments analysis, for the model development and for the specification of additional atomistic calculations. You will be at the interface of atomistic techniques, large-scale simulation and various experimental techniques. Therefore, You will develop a broad view of irradiation effects in materials and of multi-scale modelling in solids in general.
This project is an opportunity to contribute to the overall development of numerical physics applied to multi-scale modeling of materials, occupying a pivotal position and adopting a global viewpoint. This will allow experiencing yourself the way computed fundamental microscopic data finally helps solving complex practical issues.
Further readings:
Skorek et al. (2012). Modelling Fission Gas Bubble Distribution in UO2. Defect and Diffusion Forum, 323–325, 209.
Bertolus et al. (2015). Linking atomic and mesoscopic scales for the modelling of the transport properties of uranium dioxide under irradiation. Journal of Nuclear Materials, 462, 475–495.
Atomistic investigation of the thermophysical properties of metallic nuclear fuel UMo
Uranium – molybdenum alloys UMo present excellent thermal properties and a good uranium density. For those reasons, they are considered as nuclear fuel candidates for research reactors. It is therefore crucial for the CEA to deploy new computational methodologies in order to investigate the evolution of their thermo-physical properties under irradiation conditions.
This project is centered on the application of atomistic methods in order to investigate the stability and diffusion of intra-granular xenon clusters within the metallic nuclear fuel UMo.
The first step of your work will involve continuing the development of atomic-scale computational models for UMo, as initiated within the host laboratory. These models use machine learning methods to develop interatomic potentials and will be validated by comparison with existing experimental data for this material. They will then be used to assess the temperature-dependent evolution and the impact of defect accumulation (both point and extended defects) on several thermophysical properties critical to fuel modeling, such as elastic properties, density, thermal expansion, as well as thermal properties like specific heat and thermal conductivity. In collaboration with other researchers in the department, you will format these results for integration into the Scientific Computing Tools used to simulate the behavior of nuclear fuels.
In a second phase, you will be responsible for extending the validity of your models to account for the formation of fission gases such as xenon within UMo single crystals. This will enable you to simulate the stability of xenon clusters in UMo crystals. These calculations, performed using classical molecular dynamics methods, will be systematically compared with experimental observations obtained via transmission electron microscopy.
The results obtained during the various stages of this project will be completely innovative and will be the subject of scientific publications as well as presentations at international scientific conferences. Besides, this work will enable you to complement your training by acquiring skills applicable to many areas of materials science, including ab initio calculations, machine learning-based interatomic potential fitting, classical molecular dynamics, use of CEA supercomputers, and key concepts in statistical physics and condensed matter physics—fields in which the supervising team members are recognized experts.
You will join the Fuel Behavior Modeling Laboratory at the Research Institute for Nuclear Systems for Low-Carbon Energy Production (IRESNE, CEA Cadarache), a dynamic research team where you will have regular opportunities to interact with fellow PhD students and researchers. This environment also provides extensive opportunities for national and international collaboration, including with:
• Developers and users of the MAIA fuel performance code (dedicated to research reactor fuel studies),
• Experimental researchers from the Nuclear Fuel Studies Department,
• Teams from other CEA centers (Saclay, CEA/DAM),
• International partners.
This rich and multidisciplinary context will enable you to fully engage with the scientific community focused on nuclear materials science.
[1] Dubois, E. T., Tranchida, J., Bouchet, J., & Maillet, J. B. (2024). Atomistic simulations of nuclear fuel UO2 with machine learning interatomic potentials. Physical Review Materials, 8(2), 025402.
[2] Chaney, D., Castellano, A., Bosak, A., Bouchet, J., Bottin, F., Dorado, B., ... & Lander, G. H. (2021). Tuneable correlated disorder in alloys. Physical Review Materials, 5(3), 035004.
Modeling of Critical Heat Flux Using Lattice Boltzmann Methods: Application to the Experimental Devices of the RJH
LBM (Lattice Boltzmann Methods) are numerical techniques used to simulate transport phenomena in complex systems. They allow modeling fluid behavior in terms of particles moving on a discrete grid (a "lattice"). Unlike classical methods, which solve the differential equations of fluids directly, LBM simulate the evolution of the fluid particle distribution functions in a discrete space using propagation and collision rules.
The choice of lattice in LBM is a crucial step, as it directly affects the accuracy, efficiency, and stability of the simulations. The lattice determines how fluid particles interact and move through space, as well as how the discretization of space and time is performed.
LBM methods exhibit a natural parallelism because the computations at each grid point are relatively independent. Compared to classical CFD methods, LBM can better capture certain complex phenomena (such as multiphase, turbulent, or porous media flows) because they rely on a mesoscopic modeling of the fluid, directly derived from particle kinetics, rather than on a macroscopic resolution of the Navier–Stokes equations. This approach allows for a finer representation of interfaces, nonlinear effects, and local interactions, which are often difficult to model accurately using classical CFD methods. LBM therefore enables the capture of complex phenomena at a lower computational cost. Recent studies have notably shown that LBM can reproduce the Nukiyama boiling curve (pool boiling) and, consequently, accurately calculate the critical heat flux. This flux corresponds to a bulk boiling, known as a boiling crisis, which results in a sudden degradation of heat transfer.
The critical heat flux is a crucial issue for the experimental devices (DEX) of the Jules Horowitz Reactor, as they are cooled by water either via natural convection (fuel capsule-type devices) or forced convection (loop-type devices). Thus, to ensure the proper cooling of the DEX and reactor safety, it is essential to verify that the critical heat flux is not reached within the studied parameter range. It must therefore be determined with precision. Previous studies conducted on a fuel-capsule-type DEX using the NEPTUNE-CFD code (classical CFD methods) have shown that modeling is limited to regions far from the critical heat flux. In general, flows with high void fractions (greater than 10%) cannot be easily resolved using classical CFD approaches.
The student will first define a lattice to apply LBM to a RJH device under natural convection. They will consolidate the results obtained for the critical heat flux on this configuration by comparing them with available data. Finally, exploratory calculations under forced convection (laminar to turbulent regime) will be conducted.
The student will be hosted at the IRESNE institute.
Impact of the porosity on the MOX (U,Pu)O2 fuel
The nuclear fuel performances depend on their thermomecanical behaviors and, therefore, their thermal conductivity. This property varies significantly with high porsity levels especially in mixed oxided (composed of uranium and plutonium) used in fast ractors.
The aim of this thesis is to assess the impact of the pore qualities and shapes on the thermal conductivity on fissile materials and to propose a thermal conductivity law depending of the quantity, the length, the shape and the interconnectivity of its porosity. To reach this goal, recent measures on thermal properties are in progress by laser heating, allowing a better understanding of the fuel behavior in temperature ranges mostly unexplored like very high temperatures (until 2500°C), are in progress in the european research center (JRC) in Karlsruhe. These measures are performed on materials with different microstructures. These measures will be interpreted from thermograms and compared to simulation results (image analysis, converting 2D image in a 3D problem, TM-FFT)[1].
This thesis will take place in the French Institute for Research on Nuclear Systems for Low-Carbon Energy production (IRESNE) in the Expertise and Validation on multi-fuel Applications Laboratory (LEVA). LEVA is part of the Fuel Study and Simulation Department and its missions consist of :
- Answer to industrial demands by providing studies ;
- Validation of the Scientific Calculation Tools (OCS) of the PLEIADES plateform ;
- Enhance the fuel behavior understanding ;
- Manage the Fuel databases.
Finally, the collaboration with JRC Karlsuhe will be a chance to work within an international framework which also is a strenght of LEVA.
This work will be valorized through conferences participations and publications in peer-reviewed journals. Furthermore, the PhD student will have the possibility to acquire or strengthen some technical skills (experimental data interpretation, modelling) applicable in various fields of material science and engineering.
[1] This work forms a natural extension of the PHD thesis "The Thermal conductivity of mixed oxide fuel (MOX) : effect of temperature, elementary chemical composition, microstructure and burn-up in reactor" - TEL - Thèses en ligne.
Experimental study of the behavior of fission gases in Fast Neutron Reactor fuels irradiated at low power.
With the emergence of new start-ups in the nuclear field, it is essential to extend the validation basis for Fast Neutron Reactor (FNR) fuel performance codes to lower linear power operating regimes, an area that has yet to be fully explored.
Given the lower temperatures reached in the fuel, the microstructure induced by irradiation is completely different from what is typically observed at higher linear power (formation of a central hole, columnar grains, etc.). These lower operating temperatures also lead to a decrease in fission gas release (FGR), which can cause significant gas swelling of the fuel. At the same time, low operating temperatures can also lead to an increase in the density of defects (dislocations) induced during irradiation (lower defect annealing efficiency), resulting in an indirect increase in fuel swelling.
It is therefore important to determine the density of dislocations in the fuel, as their ambivalent role shows that they can slow down the release of gases by trapping them and promoting their storage in intragranular bubbles, while also facilitating their migration if they form a connected network.
In order to improve our understanding of the phenomena involved and the models of fuel swelling under irradiation, it is essential to have experimental results such as the densities and sizes of Fission Gas (FG) bubbles and the densities of dislocations in these operating regimes.
The Laboratory for Fuel Characterization and Property Studies (LCPC) within the Research Institute for Nuclear Systems for Low-Carbon Energy Production (IRESNE), to which the PhD student will be affiliated, is equipped with state-of-the-art instruments recently acquired (TEM, SEM-FIB, SIMS, EPMA, XRD) for the study of irradiated materials allowing him to develop advanced experimental skills within the specific context of a Basic Nuclear Installation. This work will be carried out in close collaboration with the teams responsible for developing the multiphysics scientific computing tools of the PLEIADES software platform. It is clear that the skills acquired during the thesis will be valuable in a future career in both academia and industry. The doctoral student will also be able to promote their work to the international academic community and the industrial world through oral presentations and peer-reviewed articles.
TRANSIENT LIQUID PHASE SINTERING OF UOX AND MOX FUEL PELLETS
The subject is related to the manufacture of UOX and MOX fuels. The main objective is to identify dopant pairs that allow the formation of a transient liquid phase during the fuel sintering step. For this, phase diagram calculations using the CALPHAD method will have to be carried out, also taking into account the requirements related to the irradiation phase once the fuel is loaded into the reactor. The most promising pairs will then be evaluated in the context of the manufacture of a UOX fuel and a MOX fuel. The experiments to be carried out will essentially be: the preparation of a powdery material, the shaping by pressing of this material in the form of cylinders representative of fuel pellets and the study of the high-temperature sintering of these UOX and MOX formulation cylinders. After sintering, a very important step will be the characterization at the macroscopic and microscopic scales of these pellets. The first year of the thesis will take place at the CEA center in Cadarache. The next two will take place at the CEA site in Marcoule. The first year of the PhD will take place at the CEA Cadarache center within the ICPE Uranium Fuel Laboratory. The following two years will be spent at the INB Atalante facility on the CEA Marcoule site. The candidate will work in two facilities unique in Europe and will be able to develop experience working in a nuclear environment with a highly innovative approach that will lead to the publication of original scientific results.
Study of new concepts for miniaturizable and parallelizable liquid-liquid extractors
In the process of developing procedures, their miniaturization represents a major challenge for upstream research and development (R&D). Indeed, the miniaturization of procedures offers numerous advantages in terms of reducing the volume of raw materials, waste management, screening possibilities, automation, and safety for personnel.
To date, the counter-current liquid-liquid extraction process does not have a convincing miniaturization solution, although the applications are numerous: in pharmacy, chemical synthesis, nuclear, or nuclear medicine.
The CEA-ISEC in Marcoule has developed new microfluidic tools to perform these operations in a simple and operational manner, based on a fine understanding of the instabilities of two-phase flows in capillaries.
This 3-year study topic proposes:
- To experiment, understand, and finely model the flows and mass transfers;
- To optimize and then transpose the phenomena to industrially significant volumes;
- To publish and participate in international conferences.
The doctoral student will benefit from learning about the world of research in a team that values quality in the supervision and future of its doctoral students, in a multidisciplinary team ranging from process engineering to instrumentation, with projects ranging from research to industry.
General competencies in chemical engineering and mass transfer are required. Competencies in collaborating with our academic partners will be essential to the success of the study project.
Development of 4D-STEM with variable tilts
The development of 4D-STEM (Scanning Transmission Electron Microscopy) has profoundly transformed transmission electron microscopy (TEM) by enabling the simultaneous recording of spatial (2D) and diffraction (2D) information at each probe position. These so-called “4D” datasets make it possible to extract a wide variety of virtual contrasts (bright-field imaging, annular dark-field imaging, ptychography, strain and orientation mapping) with nanometer-scale spatial resolution.
In this context, 4D-STEM with variable beam tilts (4D-STEMiv) is an emerging approach that involves sequentially acquiring electron diffraction patterns for different incident beam tilts. Conceptually similar to precession electron diffraction (PED), this method offers greater flexibility and opens new possibilities: improved signal-to-noise ratio, faster two-dimensional imaging at higher spatial resolution, access to three-dimensional information (orientation, strain, phase), and optimized coupling with spectroscopic analyses (EELS, EDX).
The development of 4D-STEMiv thus represents a major methodological challenge for the structural and chemical characterization of advanced materials, particularly in the fields of nanostructures, two-dimensional materials, and ferroelectric systems.
Monitoring and modeling the evolution of microstructural properties during the fabrication of MOX fuel
The nuclear fuel MOX (Mixed OXide), a ceramic obtained from a mixture of uranium and plutonium oxides, represents a strategic alternative for the valorization of plutonium resulting from the reprocessing of spent fuel. MOX pellets are produced industrially using a powder metallurgy process combined with material densification through high-temperature sintering. The rejected products are reintroduced into the process in the form of "chamotte" powder. Yet, the influence of the content and nature of this chamotte on the microstructural stability of the material remains poorly understood, particularly during the pressing and sintering stages. This aspect is critical for both the mechanical integrity and the in-reactor behavior of MOX fuels. A better understanding of these phenomena, combined with refined modeling, would make it possible to optimize industrial processes and ultimately improve the reliability of these fuels.
The objective of this PhD project is to study and model the evolution of the microstructural properties of MOX fuel as a function of the proportion and nature of the chamotte added during fabrication. The thesis strategy will rely on an integrated approach combining experimental studies with numerical simulations. It will be based on multi-scale characterization of the microstructure, coupling imaging and spectroscopy techniques, as well as on the three-dimensional reconstruction of the microstructure from experimental 2D images. The ultimate goal is to establish a link between the elastic properties of the material and its microstructure. This work will build on a combined experimental and modeling approach, bringing together the expertise of the supervisory team for experiments on plutonium-bearing materials, and for numerical modeling (micromechanical modeling, FFT-based calculations).
At the end of this PhD, the graduate student, with initial training in the physical chemistry of materials, will master a wide range of experimental techniques as well as advanced numerical modeling methods applied to ceramic materials. These skills will open up many job opportunities in academic research or industrial R&D, both within and outside the nuclear sector.
Metallurgy under extreme conditions
The microstructure-properties relationship is a core concept of metallurgy, and of materials engineering in general. For instance, the hardness of quenched steels emerges from their martensitic microstructure, induced by a phase change in iron. Here we are concerned about metallurgy under extreme conditions in which metallic samples undergo pressurizations in the 100 GPa (=1 million atmospheres) range, making it possible to synthesise new crystalline phases with potentially interesting properties (hardness, magnetism, etc.).
Studied systems will include tin, then indium and cobalt. The three of them exhibit a rich polymorphism under high pressure and temperature. We will seek to elucidate the role of defects such as twinning and plasticity on the mechanism and kinetics of these transitions. This will be done by comparing experimental observations with microstructure predictions obtained through mesoscopic simulation. High pressure/ high temperature will be mainly generated by laser-heated diamond anvil cells, and characterisation tools will include in situ X-ray imaging by diffraction and tomography, as well as electron microscopy. The X-ray sources used will be synchrotron sources and the European free-electron X-ray laser.