The double exchange model describing interactions of itinerant electrons with localized spins is usually used to explain ferromagnetism in metals. We show that for a variety of crystal lattices of different dimensionalities and for a wide range of model parameters the ferromagnetic state is unstable against a non-collinear spiral magnetic order. We revisit the phase diagram of the double exchange model on a triangular lattice and show in a large part of the diagram the incommensurate spiral state has a lower energy than the previously discussed commensurate states. These results indicate that double exchange systems are inherently frustrated and can host unconventional spin orders.
Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as the quantum spin liquids (QSLs) in real materials. In this work, we address exchange interactions in Sr2CuTe$_{1-x}$W$_{x}$O, a series of double perovskites that realize the spin-1/2 square lattice and were suggested to harbor a QSL ground state arising from random distribution of non-magnetic ions. Our {it ab initio} multi-reference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor explained by the crucial role of unoccupied states of non-magnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the end compounds, as well as explain the magnetic excitations in Sr2CuTe$_{0.5}$W$_{0.5}$O as emerging from the bond-disordered exchange couplings. Our results provide crucial understanding of the role of non-magnetic cations in exchange interactions paving the way to further exploration of QSL phases in bond-disordered materials.
A 20% substitution of Bi with La in the perovskite Bi1-xLaxFe0.5Sc0.5O3 system obtained under high-pressure and high-temperature conditions has been found to induce an incommensurately modulated structural phase. The room temperature X-ray and neutron powder diffraction patterns of this phase were successfully refined using the Imma(0,0,g)s00 superspace group (g=0.534(3)) with the modulation applied to Bi/La- and oxygen displacements. The modulated structure is closely related to the prototype antiferroelectric structure of PbZrO3 which can be considered as the lock-in variant of the latter with g =0.5. Below T_N = 220 K, the neutron diffraction data provide evidence for a long-range G-type antiferromagnetic ordering commensurate with the average Imma structure. Based on a general symmetry consideration, we show that the direction of the spins is controlled by the antisymmetric exchange imposed by the two primary structural distortions, namely oxygen octahedral tilting and incommensurate atomic displacements. The tilting is responsible for the onset of a weak ferromagnetism, observed in magnetization measurements, whereas the incommensurate displacive mode is dictated by the symmetry to couple a spin-density wave. The obtained results demonstrate that antisymmetric exchange is the dominant anisotropic interaction in Fe3+ based distorted perovskites with a nearly quenched orbital degree of freedom.
We report a neutron diffraction study of the magnetic phase transitions in the charge-density-wave (CDW) TbTe$_3$ compound. We discover that in the paramagnetic phase there are strong 2D-like magnetic correlations, consistent with the pronounced anisotropy of the chemical structure. A long-range incommensurate magnetic order emerges in TbTe$_3$ at $T_{mag1}$ = 5.78 K as a result of continuous phase transitions. We observe that near the temperature $T_{mag1}$ the magnetic Bragg peaks appear around the position (0,0,0.24) (or its rational multiples), that is fairly close to the propagation vector $(0,0,0.29)$ associated with the CDW phase transition in TbTe$_3$. This suggests that correlations leading to the long-range magnetic order in TbTe$_3$ are linked to the modulations that occur in the CDW state.
Materials that realize Kitaev spin models with bond-dependent anisotropic interactions have long been searched for, as the resulting frustration effects are predicted to stabilize novel forms of magnetic order or quantum spin liquids. Here we explore the magnetism of $gamma$-Li$_2$IrO$_3$, which has the topology of a 3D Kitaev lattice of inter-connected Ir honeycombs. Using resonant magnetic x-ray diffraction we find a complex, yet highly-symmetric incommensurate magnetic structure with non-coplanar and counter-rotating Ir moments. We propose a minimal Kitaev-Heisenberg Hamiltonian that naturally accounts for all key features of the observed magnetic structure. Our results provide strong evidence that $gamma$-Li$_2$IrO$_3$ realizes a spin Hamiltonian with dominant Kitaev interactions.
The ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems.