  Realistic, first-principles-based interatomic potentials have been used in
molecular dynamics simulations to study the effect of cation composition on the
ionic conductivity in the Zr2Y2O7-Y3NbO7 system and to link the dynamical
properties to the degree of lattice disorder. Across the composition range,
this system retains a disordered fluorite crystal structure and the vacancy
concentration is constant. The observed trends of decreasing conductivity and
increasing disorder with increasing Nb5+ content were reproduced in simulations
with the cations randomly assigned to positions on the cation sublattice. The
trends were traced to the influences of the cation charges and relative sizes
and their effect on vacancy ordering by carrying out additional calculations in
which, for example, the charges of the cations were equalised. The simulations
did not, however, reproduce all the observed properties, particularly for
Y3NbO7. Its conductivity was significantly overestimated and prominent diffuse
scattering features observed in small area electron diffraction studies were
not always reproduced. Consideration of these deficiencies led to a preliminary
attempt to characterise the consequence of partially ordering the cations on
their lattice, which significantly affects the propensity for vacancy ordering.
The extent and consequences of cation ordering seem to be much less pronounced
on the Zr2Y2O7 side of the composition range.
