Abstract
We report a thorough study of single crystals by measuring magnetic properties, specific heat, thermal conductivity, Raman scattering, x-ray and neutron diffraction with the motivation of revealing the lattice response to the spin-orbital entanglement in . Upon cooling from room temperature, the orbitally disordered paramagnetic state changes around K to a spin-orbital entangled state which is then followed by a transition at K to -type orbital-ordered (OO) and -type antiferromagnetic ordered (AF) ground state. In the temperature interval , the octahedra have two comparable in-plane V-O bonds which are longer than the out-of-plane V-O1 bond. This octahedral site distortion supports the spin-orbital entanglement of partially filled and degenerate yz/zx orbitals. However, this distortion is incompatible with the steric octahedral site distortion intrinsic to orthorhombic perovskites. Their competition induces a second-order transition from the spin-orbital entangled state to a -OO/-AF ground state where the long-range OO suppresses the spin-orbital entanglement. Our analysis suggests that the spin-orbital entangled state and -OO are comparable in energy and compete with each other. Rare-earth site disorder favors the spin-orbital entanglement rather than a cooperative Jahn-Teller distortion. The results also indicate for a -OO/-AF state in and an orbital flipping transition at .
3 More- Received 29 August 2018
- Revised 4 June 2019
DOI:https://doi.org/10.1103/PhysRevB.100.184423
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