Ambiguity in B-Site cation ordering: A Case study of the double perovskite Ca${}_2$CoNbO${}_6$

Abstract

The ordering of cations in the B sublattice remains a challenging issue in double perovskites. In this work, a combined experimental and theoretical approach was employed to investigate the Co/Nb distribution in Ca${}_2$CoNbO${}_6$ and its influence on magnetic and transport properties. The density functional theory, supported by magnetic susceptibility measurements, indicates that Co adopts a high-spin Co${}^{3+}$ state. No long-range magnetic ordering was observed down to low temperatures; however, the presence of short-range correlations points to the partial disorder in the Co/Nb sublattice. This interpretation is further supported by electron paramagnetic resonance, which also reveals slight oxygen nonstoichiometry. Electrical transport follows a small-polaron hopping mechanism with an activation energy of 0.25 eV. The Seebeck coefficient reaches 0.4 mV/K at 600 K.

18 pages, 12 figures