Anomalous magnetic and spin glass behavior in Nb substituted LaCo${}_{1-x}$Nb${}_x$O${}_3$

Abstract

We report the structural, magnetic, transport and electronic properties of Nb substituted LaCo${}_{1-x}$Nb${}_x$O${}_3$ ($x=$ 0--0.2). The Rietveld analysis of x-ray diffraction data demonstrate structural phase transitions from rhombohedral to orthorhombic and further to monoclinic with increasing the Nb concentration up to $x\ge$ 0.2. Interestingly, we observed dramatic changes in the magnetization (M) with increasing the Nb concentration, as the M sharply increases below 10~K even at 2.5\% substitution. Furthermore, ac susceptibility data show the spin-glass behavior in $x=$ 0.1 sample. We find that the density of states near the Fermi level decreases and the activation energy increases, which results in the decreasing conductivity with higher Nb concentration. A significant shift in the peak position of A${}_{2g}$ phonon mode has been observed using Raman spectroscopy, which indicates the change in the coupling due to the structural distortion with Nb substitution. The core-level photoemission study confirms that the Nb is present in 5+ valence state. Our study reveals that the nonmagnetic Nb${}^{5+}$ ($d^0$) substitution converts Co${}^{3+}$ ions to Co${}^{2+}$ and stabilize both in the high-spin state. Our results suggest that structural and spin-state transitions as well as the difference in the ionic radii between Nb${}^{5+}$ and Co${}^{3+}$ are playing an important role in tuning the physical properties.

arXiv commentto appear in PRB

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