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Magnetic Field Dependence of CDW Phases in Per2M(mnt)2 (M=Pt, Au)

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 Added by James S. Brooks
 Publication date 2005
  fields Physics
and research's language is English




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Recently the authors discovered that the suppression of the charge density wave (CDW) ground states by high magnetic fields in the organic conductor series Per2M(mnt)2 is followed by additional high field, CDW-like phases. The purpose of this presentation is to review these compounds, to consider the relevant parameters of the materials that describe the manner in which the CDW ground state may undergo new field induced changes above the Pauli limit.



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The Per2M(mnt)2 class of organic conductors exhibit a charge density wave (CDW) ground state below about 12 K, which may be suppressed in magnetic fields of order 20 to 30 T. However, for both cases of counter ion M(mnt)2 species studied (M = Au (zero spin) and M = Pt (spin 1/2)), new high field ground states evolve for further increases in magnetic field. We report recent investigations where thermopower, Hall effect, high pressure and additional transport measurements have been carried out to explore these new high field phases.
A finite transfer integral $t_a$ orthogonal to the conducting chains of a highly one-dimensional metal gives rise to empty and filled bands that simulate an indirect-gap semiconductor upon formation of a commensurate charge-density-wave (CDW). In contrast to semiconductors such as Ge and Si with bandgaps $sim 1$ eV, the CDW system possesses an indirect gap with a greatly reduced energy scale, enabling moderate laboratory magnetic fields to have a major effect. The consequent variation of the thermodynamic gap with magnetic field due to Zeeman splitting and Landau quantization enables the electronic bandstructure parameters (transfer integrals, Fermi velocity) to be determined accurately. These parameters reveal the orbital quantization limit to be reached at $sim 20$ T in (Per)$_2M$(mnt)$_2$ salts, making them highly unlikely candidates for a recently-proposed cascade of field-induced charge-density wave states.
Analysis of neutron diffraction, dc magnetization, ac magnetic susceptibility, heat capacity, and electrical resistivity for DyRuAsO in an applied magnetic field are presented at temperatures near and below those at which the structural distortion (T_S = 25 K) and subsequent magnetic ordering (T_N = 10.5 K) take place. Powder neutron diffraction is used to determine the antiferromagnetic order of Dy moments of magnitude 7.6(1) mu_B in the absence of a magnetic field, and demonstrate the reorientation of the moments into a ferromagnetic configuration upon application of a magnetic field. Dy magnetism is identified as the driving force for the structural distortion. The magnetic structure of analogous TbRuAsO is also reported. Competition between the two magnetically ordered states in DyRuAsO is found to produce unusual physical properties in applied magnetic fields at low temperature. An additional phase transition near T* = 3 K is observed in heat capacity and other properties in fields greater than about 3 T. Magnetic fields of this magnitude also induce spin-glass-like behavior including thermal and magnetic hysteresis, divergence of zero-field-cooled and field-cooled magnetization, frequency dependent anomalies in ac magnetic susceptibility, and slow relaxation of the magnetization. This is remarkable since DyRuAsO is a stoichiometric material with no disorder detected by neutron diffraction, and suggests analogies with spin-ice compounds and related materials with strong geometric frustration.
We present powder and single-crystal neutron diffraction and bulk measurements of the Kagome-staircase compound Ni3V2O8 (NVO) in fields up to 8.5T applied along the c-direction. (The Kagome plane is the a-c plane.) This system contains two types of Ni ions, which we call spine and cross-tie. Our neutron measurements can be described with the paramagnetic space group Cmca for T < 15K and each observed magnetically ordered phase is characterized by the appropriate irreducible representation(s). Our zero-field measurements show that at T_PH=9.1K NVO undergoes a transition to an incommensurate order which is dominated by a longitudinally-modulated structure with the spine spins mainly parallel to the a-axis. Upon further cooling, a transition is induced at T_HL=6.3K to an elliptically polarized incommensurate structure with both spine and cross-tie moments in the a-b plane. At T_LC=4K the system undergoes a first-order phase transition, below which the magnetic structure is a commensurate antiferromagnet with the staggered magnetization primarily along the a-axis and a weak ferromagnetic moment along the c-axis. A specific heat peak at T_CC=2.3K indicates an additional transition, which we were however not able to relate to a change of the magnetic structure. Neutron, specific heat, and magnetization measurements produce a comprehensive temperature-field phase diagram. The symmetries of the two incommensurate magnetic phases are consistent with the observation that only one phase has a spontaneous ferroelectric polarization. All the observed magnetic structures are explained theoretically using a simplified model Hamiltonian, involving competing nearest- and next-nearest-neighbor exchange interactions, spin anisotropy, Dzyaloshinskii-Moriya and pseudo-dipolar interactions.
We report the nonlocal spin Seebeck effect (nlSSE) in a lateral configuration of Pt/Y$_3$Fe$_5$O$_{12}$(YIG)/Pt systems as a function of the magnetic field $B$ (up to 10 T) at various temperatures $T$ (3 K < $T$ < 300 K). The nlSSE voltage decreases with increasing $B$ in a linear regime with respect to the input power (the applied charge-current squared $I^2$). The reduction of the nlSSE becomes substantial when the Zeeman energy exceeds thermal energy at low temperatures, which can be interpreted as freeze-out of magnons relevant for the nlSSE. Furthermore, we found the non-linear power dependence of the nlSSE with increasing $I$ at low temperatures ($T$ < 20 K), at which the $B$-induced signal reduction becomes less visible. Our experimental results suggest that in the non-linear regime high-energy magnons are over populated than those expected from the thermal energy. We also estimate the magnon spin diffusion length as functions of $B$ and $T$.
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