A comprehensive
study on the correlations of structural, magnetic,
and electronic properties of a new disordered Nd2CoFeO6 double perovskite has been conducted. The lack of strong
divergence of the magnetic susceptibility suggests competition between
magnetic interactions at the magnetic phase transition T
N = 246 K, which is confirmed by the absence of a heat
capacity peak. The magnetic susceptibility results indicate that the
Fe/Co spins form a classical noninteracting paramagnetic state above T ≈ 2.2T
N, while deviations
are found at intermediate temperatures indicating the presence of
strong short-range magnetic interactions. AC and DC electrical resistivity
results reveal a melting of insulating polaronic behavior to a metallic-like
conductivity, establishing an electronic crossover closely related
to both local magnetic moment and lattice-parameter evolution. We
show from density functional calculations that the magnetic configurations
have a strict relation to this crossover, being associated to a transition
from low to high spin states of Co3+ ions. This insulator–metal
transition has its origin driven by a local increase in the magnetic
moment of Co3+ ions. Our results point to a scenario in
which a continuous spin-state transition triggers a crossover between
distinct electronic states from the insulating polaronic behavior
to permanent metallic states.