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Register a new userPressure-Induced Restoration of the Reversed Crystal-Field Splitting in $alpha$-Sr$_2$CrO$_4$
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Motivated by an experimental finding that the successive phase transitions in $alpha$-Sr$_2$CrO$_4$ observed at ambient pressure ceases to exist under high pressures, we carry out the density-functional-theory-based electronic structure calculations and demonstrate that the reversal of the crystal-field splitting reported previously is restored under high pressures, so that the orbital degrees of freedom disappears, resulting in the single phase transition that divides the system into high-temperature Mott insulating and low-temperature antiferromagnetic insulating phases.
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The origin of successive phase transitions observed in the layered perovskite $alpha$-Sr$_2$CrO$_4$ is studied by the density-functional-theory-based electronic structure calculation and mean-field analysis of the proposed low-energy effective model. We find that, despite the fact that the CrO$_6$ octahedron is elongated along the $c$-axis of the crystal structure, the crystal-field level of nondegenerate $3d_{xy}$ orbitals of the Cr ion is lower in energy than that of doubly degenerate $3d_{yz}$ and $3d_{xz}$ orbitals, giving rise to the orbital degrees of freedom in the system with a $3d^2$ electron configuration. We show that the higher (lower) temperature phase transition is caused by the ordering of the orbital (spin) degrees of freedom.
The rich phenomenology engendered by the coupling between the spin and orbital degrees of freedom has become appreciated as a key feature of many strongly-correlated electron systems. The resulting emergent physics is particularly prominent in a number of materials, from Fe-based unconventional superconductors to transition metal oxides, including manganites and vanadates. Here, we investigate the electronic ground states of $alpha$-Sr$_2$CrO$_4$, a compound that is a rare embodiment of the spin-1 Kugel-Khomskii model on the square lattice -- a paradigmatic platform to capture the physics of coupled magnetic and orbital electronic orders. We have used resonant X-ray diffraction at the Cr-$K$ edge to reveal N{e}el magnetic order at the in-plane wavevector $mathbf{Q}_N = (1/2, 1/2)$ below $T_N = 112$ K, as well as an additional electronic order at the stripe wavevector $mathbf{Q}_s = (1/2, 0)$ below T$_s$ $ sim 50$ K. These findings are examined within the framework of the Kugel-Khomskii model by a combination of mean-field and Monte-Carlo approaches, which supports the stability of the spin N{e}el phase with subsequent lower-temperature stripe orbital ordering, revealing a candidate mechanism for the experimentally observed peak at $mathbf{Q}_s$. On the basis of these findings, we propose that $alpha$-Sr$_2$CrO$_4$ serves as a new platform in which to investigate multi-orbital physics and its role in the low-temperature phases of Mott insulators.
Motivated by recent experimental progress in transition metal oxides with the K$_2$NiF$_4$ structure, we investigate the magnetic and orbital ordering in $alpha$-Sr$_2$CrO$_4$. Using first principles calculations, first we derive a three-orbital Hubbard model, which reproduces the {it ab initio} band structure near the Fermi level. The unique reverse splitting of $t_{2g}$ orbitals in $alpha$-Sr$_2$CrO$_4$, with the $3d^2$ electronic configuration for the Cr$^{4+}$ oxidation state, opens up the possibility of orbital ordering in this material. Using real-space Hartree-Fock for multi-orbital systems, we constructed the ground-state phase diagram for the two-dimensional compound $alpha$-Sr$_2$CrO$_4$. We found stable ferromagnetic, antiferromagnetic, antiferro-orbital, and staggered orbital stripe ordering in robust regions of the phase diagram. Furthermore, using the density matrix renormalization group method for two-leg ladders with the realistic hopping parameters of $alpha$-Sr$_2$CrO$_4$, we explore magnetic and orbital ordering for experimentally relevant interaction parameters. Again, we find a clear signature of antiferromagnetic spin ordering along with antiferro-orbital ordering at moderate to large Hubbard interaction strength. We also explore the orbital-resolved density of states with Lanczos, predicting insulating behavior for the compound $alpha$-Sr$_2$CrO$_4$, in agreement with experiments. Finally, an intuitive understanding of the results is provided based on a hierarchy between orbitals, with $d_{xy}$ driving the spin order, while electronic repulsion and the effective one dimensionality of the movement within the $d_{xz}$ and $d_{yz}$ orbitals driving the orbital order.
SrTm$_2$O$_4$ has been investigated using heat capacity, magnetic susceptibility, magnetization in pulsed fields, and inelastic neutron scattering measurements. These results show that the system is highly anisotropic, has gapped low-energy dispersing magnetic excitations, and remains in a paramagnetic state down to 2K. Two theoretical crystal field models were used to describe the single-ion properties of SrTm$_2$O$_4$without any optimization procedures; a standard point-charge model and a Density Functional Theory (DFT) based model that uses Wannier functions. The DFT model was found to better describe the system at low energy by predicting a singlet ground state for one Tm site and a doublet for the second Tm site and anisotropy of second site Tm dominating the anisotropy of the system. Additionally, muon spin rotation/relaxation ($mu^+$psr) spectra reveal oscillations, typically a sign of long-range magnetic order. We attribute these observations to lattice distortion induced by muon implantation, causing renormalization of the gap size.
We demonstrate that the onset of complex spin orders in ACr$_2$O$_4$ spinels with magnetic A$=$Co, Fe and Cu ions lowers the lattice symmetry. This is clearly indicated by the emergence of anisotropic lattice dynamics -- as evidenced by the pronounced phonon splittings -- even when experiments probing static distortions fail. We show that the crystal symmetry in the magnetic phase is reduced from tetragonal to orthorhombic for FeCr$_2$O$_4$ and CuCr$_2$O$_4$ with Jahn-Teller active A-site ions. The conical spin structure in FeCr$_2$O$_4$ is also manifested in the phonon frequencies. In contrast, the multiferroic CoCr$_2$O$_4$ with no orbital degrees of freedom remains nearly cubic in its ground state.
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