Orbital degree of freedom in high entropy oxides

The spin, charge, and lattice degrees of freedom and their interplay in high entropy oxides were intensively investigated in recent years. However, how the orbital degree of freedom is affected by the extreme disorder in high entropy oxides has not been studied. In this work, using perovskite structured RVO3 as a materials playground, we report how the disorder arising from mixing different rare earth ions at the rare earth site affects the orbital ordering of V3+ t2g electrons. Since each member of RVO3 (R = rare earth and Y) crystallizes into the same orthorhombic Pbnm structure, the configurational entropy should not be critical for the stability of (R1, ...,Rn)VO3. The spin and orbital ordering was studied by measuring magnetic properties and specific heat of single crystals. Rather than the number and type of rare earth ions, the average and variance of ionic radius are the key factors determining the spin and orbital order in (R1, ...,Rn)VO3. When the size variance is small, the average ionic radius takes precedence in dictating spin and orbital order. Increasing size variance suppresses the G-type orbital order (G-OO) and C-type antiferromagnetic order (C-AF) but favors the C-OO/G-AF state and spin-orbital entanglement. These findings suggest that the extreme disorder introduced by mixing multiple rare earth ions in high entropy perovskites might be employed to preserve the orbital degree of freedom to near the magnetic order, which is necessary for the electronic driven orbital ordering in a Kugel-Khomskii compound.