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Quantum Oscillations of the Metallic Triangular-lattice Antiferromagnet PdCrO2

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 Added by Jun Sung Kim
 Publication date 2013
  fields Physics
and research's language is English




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We report the de Haas-van Alphen (dHvA) oscillations and first-principle calculations for triangular antiferromagnet PdCrO2 showing unconventional anomalous Hall effect (AHE). The dHvA oscillations in PdCrO2 reveal presence of several 2 dimensional Fermi surfaces of smaller size than found in nonmagnetic PdCoO2. This evidences Fermi surface reconstruction due to the non-collinear 120 antiferromagnetic ordering of the localized Cr, consistent with the first principle calculations. The temperature dependence of dHvA oscillations shows no signature of additional modification of Cr spin structure below TN. Considering that the 120 helical ordering of Cr spins has a zero scalar spin chirality, our results suggest that PdCrO2 is a rare example of the metallic triangular antiferromagnets whose unconventional AHE can not be understood in terms of the spin chirality mechanism.



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We performed neutron single crystal and synchrotron X-ray powder diffraction experiments in order to investigate the magnetic and crystal structures of the conductive layered triangular-lattice antiferromagnet PdCrO2 with a putative spin chirality, which contributes to an unconventional anomalous Hall effect. We revealed that the ground-state magnetic structure is a commensurate and nearly-coplanar 120-degrees spin structure. The 120-degrees plane in different Cr layers seem to tilt with one another, leading to a small noncoplanarity. Such a small but finite non-coplanar stacking of the 120-degrees planes gives rise to a finite scalar spin chirality, which may be responsible for the unconventional nature of the Hall effect of PdCrO2.
Quantum triangular-lattice antiferromagnets are important prototype systems to investigate phenomena of the geometrical frustration in condensed matter. Apart from highly unusual magnetic properties, they possess a rich phase diagram (ranging from an unfrustrated square lattice to a quantum spin liquid), yet to be confirmed experimentally. One major obstacle in this area of research is the lack of materials with appropriate (ideally tuned) magnetic parameters. Using Cs$_2$CuCl$_4$ as a model system, we demonstrate an alternative approach, where, instead of the chemical composition, the spin Hamiltonian is altered by hydrostatic pressure. The approach combines high-pressure electron spin resonance and magnetization measurements, allowing us not only to quasi-continuously tune the exchange parameters, but also to accurately monitor them. Our experiments indicate a substantial increase of the exchange coupling ratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergent field-induced phases.
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This work examines the critical anisotropy required for the local stability of the collinear ground states of a geometrically-frustrated triangular-lattice antiferromagnet (TLA). Using a Holstein-Primakoff expansion, we calculate the spin-wave frequencies for the 1, 2, 3, 4, and 8-sublattice (SL) ground states of a TLA with up to third neighbor interactions. Local stability requires that all spin-wave frequencies are real and positive. The 2, 4, and 8-SL phases break up into several regions where the critical anisotropy is a different function of the exchange parameters. We find that the critical anisotropy is a continuous function everywhere except across the 2-SL/3-SL and 3-SL/4-SL phase boundaries, where the 3-SL phase has the higher critical anisotropy.
Yb- and Ce-based delafossites were recently identified as effective spin-1/2 antiferromagnets on the triangular lattice. Several Yb-based systems, such as NaYbO2, NaYbS2, and NaYbSe2, exhibit no long-range order down to the lowest measured temperatures and therefore serve as putative candidates for the realization of a quantum spin liquid. However, their isostructural Ce-based counterpart KCeS2 exhibits magnetic order below TN = 400 mK, which was so far identified only in thermodynamic measurements. Here we reveal the magnetic structure of this long-range ordered phase using magnetic neutron diffraction. We show that it represents the so-called stripe-yz type of antiferromagnetic order with spins lying approximately in the triangular-lattice planes orthogonal to the nearest-neighbor Ce-Ce bonds. No structural lattice distortions are revealed below TN, indicating that the triangular lattice of Ce3+ ions remains geometrically perfect down to the lowest temperatures. We propose an effective Hamiltonian for KCeS2, based on a fit to the results of ab initio calculations, and demonstrate that its magnetic ground state matches the experimental spin structure.
The spin wave excitations of the geometrically frustrated triangular lattice antiferromagnet (TLA) $rm CuFeO_2$ have been measured using high resolution inelastic neutron scattering. Antiferromagnetic interactions up to third nearest neighbors in the ab plane (J_1, J_2, J_3, with $J_2/J_1 approx 0.44$ and $J_3/J_1 approx 0.57$), as well as out-of-plane coupling (J_z, with $J_z/J_1 approx 0.29$) are required to describe the spin wave dispersion relations, indicating a three dimensional character of the magnetic interactions. Two energy dips in the spin wave dispersion occur at the incommensurate wavevectors associated with multiferroic phase, and can be interpreted as dynamic precursors to the magnetoelectric behavior in this system.
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