Electronic and magnetic ground state of 4$d^3$ double perovskite ruthenates A$_2$LaRuO$_6$ (A $=$ Ca, Sr, Ba)

Abstract

4$d$ transition metal oxide (TMO) offers an intriguing puzzle for their electronic and magnetic ground state. They are in the cross-over regime of strong spin orbit interaction (SOI) and electron-electron correlation ($U$) with quenched orbital angular momentum. Our work unravels the electronic and magnetic ground state of the less investigated 4$d^{3}$ double perovskite ruthenates A$_{2}$LaRuO$_6$ (A = Ca, Ba). The negligible effect of SOI is evident from the bulk magnetic, specific heat measurements and density functional theory (DFT) calculations, indicating a classical spin-only magnetic ground state (${S}$ = 3/2) for the materials. Magnetization measurements show that both materials have long range antiferromagnetic order with high degree of magnetic frustration ($f$ $\approx$13 -15). Interestingly, a near $T^2$- behavior is observed in low-$T$ magnetic heat capacity measurement, indicating the presence of low-dimensional spin-wave exciation and magnetic frustration in both materials. The temperature dependent resistivity measurements and electronic band structure calculations confirm a conventional Mott insulating ground state in these two systems. Moreover, our experimental investigation and DFT calculations highlight the reason for the nonexistence of Sr$_2$LaRuO$_6$.