No Arabic abstract
The magnetism in Mn$_3$Si$_2$Te$_6$ has been investigated using thermodynamic measurements, first principles calculations, neutron diffraction and diffuse neutron scattering on single crystals. These data confirm that Mn$_3$Si$_2$Te$_6$ is a ferrimagnet below a Curie temperature of $T_C$ approximately 78K. The magnetism is anisotropic, with magnetization and neutron diffraction demonstrating that the moments lie within the basal plane of the trigonal structure. The saturation magnetization of approximately 1.6$mu_B$/Mn at 5K originates from the different multiplicities of the two antiferromagnetically-aligned Mn sites. First principles calculations reveal antiferromagnetic exchange for the three nearest Mn-Mn pairs, which leads to a competition between the ferrimagnetic ground state and three other magnetic configurations. The ferrimagnetic state results from the energy associated with the third-nearest neighbor interaction, and thus long-range interactions are essential for the observed behavior. Diffuse magnetic scattering is observed around the 002 Bragg reflection at 120K, which indicates the presence of strong spin correlations well above $T_C$. These are promoted by the competing ground states that result in a relative suppression of $T_C$, and may be associated with a small ferromagnetic component that produces anisotropic magnetism below $approx$330K.
We demonstrate that the onset of complex spin orders in ACr$_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.
Colossal magnetoresistance is of great fundamental and technological significance and exists mostly in the manganites and a few other materials. Here we report colossal magnetoresistance that is starkly different from that in all other materials. The stoichiometric Mn3Si2Te6 is an insulator featuring a ferrimagnetic transition at 78 K. The resistivity drops by 7 orders of magnitude with an applied magnetic field above 9 Tesla, leading to an insulator-metal transition at up to 130 K. However, the colossal magnetoresistance occurs only when the magnetic field is applied along the magnetic hard axis and is surprisingly absent when the magnetic field is applied along the magnetic easy axis where magnetization is fully saturated. The anisotropy field separating the easy and hard axes is 13 Tesla, unexpected for the Mn ions with nominally negligible orbital momentum and spin-orbit interactions. Double exchange and Jahn-Teller distortions that drive the hole-doped manganites do not exist in Mn3Si2Te6. The phenomena fit no existing models, suggesting a unique, intriguing type of electrical transport.
Compounds with two-dimensional (2D) layers of magnetic ions weakly connected by van der Waals bonding offer routes to enhance quantum behavior, stimulating both fundamental and applied interest. CrPS4 is one such magnetic van der Waals material, however, it has undergone only limited investigation. Here we present a comprehensive series of neutron scattering measurements to determine the magnetic structure and exchange interactions. The observed magnetic excitations allow a high degree of constraint on the model parameters not normally associated with measurements on a powder sample. The results demonstrate the 2D nature of the magnetic interactions, while also revealing the importance of interactions along 1D chains within the layers. The subtle role of competing interactions is observed, which manifest in a non-trivial magnetic transition and a tunable magnetic structure in a small applied magnetic field through a spin-flop transition. Our results on the bulk compound provide insights that can be applied to an understanding of the behavior of reduced layer CrPS4.
Using powder neutron diffraction we have discovered an unusual magnetic order-order transition in the Ising spin chain compound Ca3Co2O6. On lowering the temperature an antiferromagnetic phase with propagation vector k=(0.5,-0.5,1) emerges from a higher temperature spin density wave structure with k=(0, 0, 1.01). This transition occurs over an unprecedented time-scale of several hours and is never complete.
A pressure and temperature dependent Raman study of the vibrational and spin dynamics in CuGeO3 is presented. A new low temperature, high pressure phase has been identified, and a pressure-temperature phase-diagram is proposed for CuGeO3. The pressure dependence of the effective exchange interaction, of the spin-Peierls gap, and of the spin-Peierls temperature strongly supports a model in which next nearest neighbor interactions stabilise the SP ground state. The Raman data allow for a quantitative estimate of the pressure dependence of the next nearest neighbor interactions.