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Register a new userTetravalent doping of CeO$_2$: The impact of valence electron character on group IV dopant influence
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Added by
Danny E. P. Vanpoucke Dr.
Publication date
2013
fields
Physics
and research's language is
English
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Fluorite CeO$_2$ doped with group IV elements is studied within the DFT and DFT+U framework. Concentration dependent formation energies are calculated for Ce$_{1-x}$Z$_x$O$_2$ (Z= C, Si, Ge, Sn, Pb, Ti, Zr, Hf) with $0leq x leq 0.25$ and a roughly decreasing trend with ionic radius is observed. The influence of the valence and near valence electronic configuration is discussed, indicating the importance of filled $d$ and $f$ shells near the Fermi level for all properties investigated. A clearly different behavior of group IVa and IVb dopants is observed: the former are more suitable for surface modifications, the latter are more suitable for bulk modifications. indent For the entire set of group IV dopants, there exists an inverse relation between the change, due to doping, of the bulk modulus and the thermal expansion coefficients. Hirshfeld-I atomic charges show that charge transfer effects due to doping are limited to the nearest neighbor oxygen atoms.
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The modification of the properties of CeO$_2$ through aliovalent doping are investigated within the emph{ab-initio} density functional theory framework. Lattice parameters, dopant atomic radii, bulk moduli and thermal expansion coefficients of fluorite type Ce$_{1-x}$M$_{x}$O$_{2-y}$ (with M$ = $ Mg, V, Co, Cu, Zn, Nb, Ba, La, Sm, Gd, Yb, and Bi)are presented for dopant concentrations in the range $0.00 leq x leq 0.25$. The stability of the dopants is compared and discussed, and the influence of oxygen vacancies is investigated. It is shown that oxygen vacancies tend to increase the lattice parameter, and strongly decrease the bulk modulus. Defect formation energies are correlated with calculated crystal radii and covalent radii of the dopants, but are shown to present no simple trend. The previously observed inverse relation between the thermal expansion coefficient and the bulk modulus is shown to persist independent of the inclusion of charge compensating vacancies.
The appearance of microcracks in CeO$_2$ buffer layers, as used in buffer layer architectures for coated superconductors, indicates the presence of stress between this buffer layer and the substrate. This stress can originate from the differences in thermal expansion or differences in lattice parameters between the CeO$_2$ buffer layer and the substrate. In this article, we study, by means of textit{ab initio} density functional theory calculations, the influence of group IV doping elements on the lattice parameter and bulk modulus of CeO$_2$. Vegards law behavior is found for the lattice parameter in systems without oxygen vacancies, and the Shannon crystal radii for the doping elements are retrieved from the lattice expansions. We show that the lattice parameter of the doped CeO$_2$ can be matched to that of the La$_2$Zr$_2$O$_7$ coated NiW substrate substrate for dopant concentrations of about $5%$, and that bulk modulus matching is either not possible or would require extreme doping concentrations.
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We present Hall-effect measurements of two-leg ladder compounds Sr_{14-x}Ca_xCu_24O_41 (0 <= x <= 11.5) with the aim to determine the number of carriers participating in dc transport. Distribution of holes between the ladder and chain subsystems is one of the crucial questions important for understanding the physics of these compounds. Our Hall effect and resistivity measurements show typical semiconducting behavior for x < 11.5. However, for x=11.5, the results are completely different, and the Hall coefficient and resistivity behavior is qualitatively similar to that of high temperature copper-oxide superconductors. We have determined the effective number of carriers at room temperature and compared it to the number of holes in the ladders obtained by other experimental techniques. We propose that going from x=0 to x=11.5 less than 1 hole per formula unit is added to the ladders and is responsible for a pronounced change in resistivity with Ca doping.
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