Abstract
We have investigated unusual phase transitions that were triggered by chemical doping in $\mathrm{C}{\mathrm{a}}_{3}\mathrm{R}{\mathrm{u}}_{2}{\mathrm{O}}_{7}$. Our experiments showed that doping with a few percent of Mn ($g4%$) can change the quasi-two-dimensional metallic state of $\mathrm{C}{\mathrm{a}}_{3}\mathrm{R}{\mathrm{u}}_{2}{\mathrm{O}}_{7}$ into a Mott insulating state with a G-type antiferromagnetic order, but this Mott state cannot be induced by Fe doping. By combining these results with first-principles calculations, we show that lattice-orbital coupling (LOC) plays an important role in the Mott transition. Interestingly, the transition temperature ${T}_{\mathrm{MIT}}$ is found to be predetermined by a structural parameter denoted by $c/\sqrt{ab}$ at temperatures far above N\'eel temperature ${T}_{\mathrm{N}}$. This LOC-assisted Mott transition clearly contrasts with the band-filling picture. It is addressed that this type of Mott transition originates in the strong scattering centers formed by specific $3d$ dopants. The dopant-scattering picture is then applied to explain the puzzling doping effects that occur in other ruthenates and $3d$ oxides. Our findings will advance the general understanding of how the unusual properties of $4d$ correlated systems are governed by the complex interplay that occurs among the charge, spin, lattice, and orbital degrees of freedom.
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