Atomistic and experimental study on thermal conductivity of bulk and porous cerium dioxide.

Cerium dioxide (CeO ₂ ) is a surrogate material for traditional nuclear fuels and an essential material for a wide variety of industrial applications both in its bulk and nanometer length scale. Despite this fact, the underlying physics of thermal conductivity (k _L ), a crucial design parameter in industrial applications, has not received enough attention. In this article, a systematic investigation of the phonon transport properties was performed using ab initio calculations unified with the Boltzmann transport equation. An extensive examination of the phonon mode contribution, available three-phonon scattering phase space, mode Grüneisen parameter and mean free path (MFP) distributions were also conducted. To further augment theoretical predictions of the k _L , measurements were made on specimens prepared by spark plasma sintering using the laser flash technique. Since the sample porosity plays a vital role in the value of measured k _L , the effect of porosity on k _L by molecular dynamics (MD) simulations were investigated. Finally, we also determined the nanostructuring effect on the thermal properties of CeO ₂ . Since CeO ₂ films find application in various industries, the dependence of thickness on the in-plane and cross-plane k _L for an infinite CeO ₂ thin film was also reported.