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Register a new userQuantum Tunneling of the Magnetization in the Ising Chain Compound Ca3Co2O6
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The magnetic behavior of the Ca3Co2O6 spin chain compound is characterized by a large Ising-like character of its ferromagnetic chains, set on triangular lattice, that are antiferromagnetically coupled. At low temperature, T < 7K, the 3D antiferromagnetic state evolves towards a spin frozen state. In this temperature range, magnetic field driven magnetization of single crystals (H//chains) exhibits stepped variations. The occurrence of these steps at regular intervals of the applied magnetic field, Hstep=1.2T, is reminiscent of the quantum tunneling of the magnetization (QTM) of molecular based magnets. Magnetization relaxation experiments also strongly support the occurrence of this quantum phenomenon. This first observation of QTM in a magnetic oxide belonging to the large family of the A3BBO6 compounds opens new opportunities to study a quantum effect in a very different class of materials from molecular magnets.
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We report that the major features in the temperature dependence of dc and ac magnetization of a well-known spin-chain compound, Ca3Co2O6, which has been known to exhibit two complex magnetic transitions due to geometrical frustration (one near 24 K and the other near 10 K), are found to be qualitatively unaffected in its nano form synthesized by high-energy ball-milling. However, the multiple steps in isothermal magnetization - a topic of current interest in low-dimensional systems - known for the bulk form well below 10 K is absent in the nano particles. We believe that this finding will be useful to the understanding of the step magnetization behavior of such spin-chain systems.
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.
The one-dimensional cobaltate Ca3Co2O6 is an intriguing material having an unconventional magnetic structure, displaying quantum tunneling phenomena in its magnetization. Using a newly developed experimental method, s-core-level non-resonant inelastic x-ray scattering (s-NIXS), we were able to image the atomic Co 3d orbital that is responsible for the Ising magnetism in this system. We show that we can directly observe that it is the complex d2 orbital occupied by the sixth electron at the high-spin Co-trig{3+} (d6) sites that generates this behavior. This is extremely rare in the research field of transition metal compounds, and is only made possible by the delicately balanced prismatic trigonal coordination. The ability to directly relate the orbital occupation with the local crystal structure is essential to model the magnetic properties of this system.
Using inelastic neutron scattering, we have observed a quasi-one-dimensional dispersive magnetic excitation in the frustrated triangular-lattice spin-2 chain oxide Ca3Co2O6. At the lowest temperature (T = 1.5 K), this magnon is characterized by a large zone-center spin gap of ~27 meV, which we attribute to the large single-ion anisotropy, and disperses along the chain direction with a bandwidth of ~3.5 meV. In the directions orthogonal to the chains, no measurable dispersion was found. With increasing temperature, the magnon dispersion shifts towards lower energies, yet persists up to at least 150 K, indicating that the ferromagnetic intrachain correlations survive up to 6 times higher temperatures than the long-range interchain antiferromagnetic order. The magnon dispersion can be well described within the predictions of linear spin-wave theory for a system of weakly coupled ferromagnetic chains with large single-ion anisotropy, enabling the direct quantitative determination of the magnetic exchange and anisotropy parameters.
We report a single-crystal study on the magnetism of the rare-earth compound PrTiNbO$_6$ that experimentally realizes the zigzag pseudospin-$frac{1}{2}$ quantum antiferromagnetic chain model. Random crystal electric field caused by the site mixing between non-magnetic Ti$^{4+}$ and Nb$^{5+}$, results in the non-Kramers ground state quasi-doublet of Pr$^{3+}$ with the effective pseudospin-$frac{1}{2}$ Ising moment. Despite the antiferromagnetic intersite coupling of about 4 K, no magnetic freezing is detected down to 0.1 K, whilst the system approaches its ground state with almost zero residual spin entropy. At low temperatures, a sizable gap of about 1 K is observed in zero field. We ascribe this gap to off-diagonal anisotropy terms in the pseudospin Hamiltonian, and argue that rare-earth oxides open an interesting venue for studying magnetism of quantum spin chains.
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