In search of the ground state crystal structure of Ta${}_2$O${}_5$ from ab-initio and Monte Carlo simulations

Abstract

Tantalum oxides (Ta${}_2$O${}_5$) are characterised by attractive physical and chemical properties, such as high dielectric constants and anti-reflection behaviour. Recently, Ta${}_2$O${}_5$ nanoparticles have also been proposed as possible enhancers of the relative biological effectiveness in hadrontherapy for cancer treatment. In principle, their electronic properties can be accurately investigated from first-principles simulations. However, the existence of several stable polymorphs of these oxides represents a major difficulty in order to calculate and disentangle their respective spectral features. To assess this problem, we use linear-response time-dependent density functional to investigate the energy loss function $\mbox{Im} (-1/\barε)$, which is a unique fingerprint of the material, in the optical limit for various polymorphs. We show that the experimental reflection energy loss signals can be rationalized and interpreted by assuming that the $\gamma$-phase of Ta${}_2$O${}_5$ represents the underlying structural model. We notice that both the inclusion of local field effects and spin-orbit coupling are crucial to compute the energy loss functions of this material. Finally, to further validate the $\gamma$-Ta${}_2$O${}_5$ polymorph as a model for experimental tantalum oxide, we compute the reflection energy loss spectra using a Monte Carlo approach, finding an excellent agreement with the experimental data.

13 pages, 6 figures