Cs diffusion in cubic silicon carbide

Undesired release of Cs through a silicon carbide coating of nuclear fuel is a significant concern for the design of the Very High Temperature Reactor (VHTR). However, mechanisms of Cs transport are currently unclear. To better understand the possible mechanisms of Cs release here we use density functional theory to study diffusion of Cs in crystalline bulk SiC. Cs point defects and Cs - vacancy clusters have been investigated for stability and structure. The most stable state for the Cs impurity in SiC, under n-type doping conditions, is found to be a negatively charged Cs atom substituting for a C atom and bound to two Si vacancies (CsC-2VSi3-). Bulk diffusion coefficients are estimated for several Cs impurity states. The CsC-2VSi3- defect structure is found to have the lowest overall activation energy for diffusion with a value of approximately 5.14 eV. This activation energy agrees well with diffusion activation energies estimated for Cs in SiC based on high temperature integral release experiments.