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Magnetic properties of quasi-two-dimensional $S$ = 1/2 Heisenberg antiferromagnet with distorted square lattice

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 Added by Hironori Yamaguchi
 Publication date 2017
  fields Physics
and research's language is English




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We successfully synthesize single crystals of the verdazyl radical $alpha$-2,3,5-Cl$_3$-V. $Ab$ $initio$ molecular orbital calculations indicate that the two dominant antiferromagnetic interactions, $J_{rm{1}}$ and $J_{rm{2}}$ ($alpha =J_{rm{2}}/J_{rm{1}}simeq 0.56$), form an $S$ = 1/2 distorted square lattice. We explain the magnetic properties based on the $S$ = 1/2 square lattice Heisenberg antiferromagnet using the quantum Monte Carlo method, and examine the effects of the lattice distortion and the interplane interaction contribution. In the low-temperature regions below 6.4 K, we observe anisotropic magnetic behavior accompanied by a phase transition to a magnetically ordered state. The electron spin resonance signals exhibit anisotropic behavior in the temperature dependence of the resonance field and the linewidth. We explain the frequency dependence of the resonance fields in the ordered phase using a mean-field approximation with out-of-plane easy-axis anisotropy, which causes a spin-flop phase transition at approximately 0.4 T for the field perpendicular to the plane. Furthermore, the anisotropic dipole field provides supporting information regarding the presence of the easy-axis anisotropy. These results demonstrate that the lattice distortion, anisotropy, and interplane interaction of this model are sufficiently small that they do not affect the intrinsic behavior of the $S$ = 1 / 2 square lattice Heisenberg antiferromagnet.



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We have explored the magnetic excitation spectrum of the S=1/2 square lattice Heisenberg antiferromagnet, K2V3O8 using both triple-axis and time-of-flight inelastic neutron scattering. The long-wavelength spin waves are consistent with the previously determined Hamiltonian for this material. A small energy gap of 72+/-9 micro-eV is observed at the antiferromagnetic zone center and the near-neighbor exchange constant is determined to be 1.08+/-0.03 meV. A finite ferromagnetic interplanar coupling is observed along the crystallographic c-axis with a magnitude of Jc=-0.0036+/-0.006 meV. However, upon approaching the zone boundary, the observed excitation spectrum deviates significantly from the expectation of linear spin wave theory resulting in split modes at the (pi/2,pi/2) zone boundary point. The effects of magnon-phonon interaction, orbital degrees of freedom, multimagnon scattering, and dilution/site randomness are considered in the context of the mode splitting. Unfortunately, no fully satisfactory explanation of this phenomenon is found and further theoretical and experimental work is needed.
We have performed elastic and inelastic neutron experiments on single crystal samples of the coordination polymer compound CuF2(H2O)2(pyz) (pyz=pyrazine) to study the magnetic structure and excitations. The elastic neutron diffraction measurements indicate a collinear antiferromagnetic structure with moments oriented along the [0.7 0 1] real-space direction and an ordered moment of 0.60 +/- 0.03 muB/Cu. This value is significantly smaller than the single ion magnetic moment, reflecting the presence of strong quantum fluctuations. The spin wave dispersion from magnetic zone center to the zone boundary points (0.5 1.5 0) and (0.5 0 1.5) can be described by a two dimensional Heisenberg model with a nearest neighbor magnetic exchange constant J2d = 0.934 +/-0.0025 meV. The inter-layer interaction Jperp in this compound is less than 1.5% of J2d. The spin excitation energy at the (0.5 0.5 0.5) zone boundary point is reduced when compared to the (0.5 1 0.5) zone boundary point by ~10.3 +/- 1.4 %. This zone boundary dispersion is consistent with quantum Monte Carlo and series expansion calculations which include corrections for quantum fluctuations to linear spin wave theory.
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