Structural, transport, and magnetic properties of narrow bandwidth Nd1 -xCaxCoO3 and comparisons to Pr1 -xCaxCoO3

D. Phelan, Y. Suzuki, S. Wang, A. Huq, C. Leighton

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Low bandwidth Pr-based cobalt perovskites, such as Pr1-xCa xCoO3, have received significant recent attention as they undergo first-order spin-state transitions with a strong influence on magnetic and transport properties. The unique nature of the Pr-O bond has been implicated as the impetus for these transitions, as it is thought that temperature-dependent charge transfer can occur between Pr and Co ions, i.e., a partial Pr3+→Pr4+ and Co4+→Co3 + valence shift. In the present work, we have studied the related compound Nd1-xCaxCoO3. The Nd3 + ions have very similar ionic radius to Pr3+ but do not induce a temperature-dependent valence shift (at least in the composition range studied here), enabling deconvolution of the intrinsic low bandwidth physics from the unique effects of Pr-O bonding in Pr1-xCa xCoO3. To this end, we have characterized the structural, magnetic, and electronic transport characteristics of Nd1 -xCaxCoO3 bulk polycrystals, using neutron diffraction, small-angle neutron scattering, dc and ac magnetometry, and magnetotransport, and have established the Nd1-xCa xCoO3 magnetic phase diagram. This phase diagram contains regimes of short-range ferromagnetism and long-range ferromagnetism, in addition to ferrimagnetism. We argue that, with the exception of the valence transition that occurs at high x (e.g., x = 0.5) in Pr1-xCa xCoO3 and the low-temperature ordering of Nd3 +moments that results in the ferrimagnetism in Nd1 -xCaxCoO3, the two systems are nearly isostructural and have similar magnetic and transport properties. The low bandwidth physics intrinsic to both systems is summarized as encompassing long-range ferromagnetism with a relatively low Curie temperature due to Co-O-Co bond buckling (<60 K for Nd1-xCaxCoO3 ), short-range ferromagnetism that emerges at much higher temperatures (∼270 K for Nd1-xCaxCoO3 ), and likely stems from oxygen deficiency, exchange-spring behavior related to magnetoelectronic phase separation, and a doping-driven insulator-metal transition. In addition to elucidating the essential physics of narrow bandwidth perovskite cobaltites, the results thus further confirm the importance of the unique features of the Pr-O bond in driving the abrupt spin-state transition in Pr1-xCaxCoO3.

Original languageEnglish (US)
Article number075119
JournalPhysical Review B - Condensed Matter and Materials Physics
Issue number7
StatePublished - Aug 9 2013


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