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Register a new userMagnetic properties of the S=1/2 quasi square lattice antiferromagnet CuF2(H2O)2(pyz) (pyz=pyrazine) investigated by neutron scattering
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Andrew Christianson
Publication date
2012
fields
Physics
and research's language is
English
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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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The crystal structures of Ni$X_2$(pyz)$_2$ ($X$ = Cl (textbf{1}), Br (textbf{2}), I (textbf{3}) and NCS (textbf{4})) were determined at 298~K by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN$_4$$X_2$ units that are bridged by pyz ligands. The 2D layered motifs displayed by textbf{1}-textbf{4} are relevant to bifluoride-bridged [Ni(HF$_2$)(pyz)$_2$]$Z$F$_6$ ($Z$ = P, Sb) which also possess the same 2D layers. In contrast, terminal $X$ ligands occupy axial positions in textbf{1}-textbf{4} and cause a staggering of adjacent layers. Long-range antiferromagnetic order occurs below 1.5 (Cl), 1.9 (Br and NCS) and 2.5~K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and $g$ factor of textbf{2}, textbf{3} and textbf{4} are measured by electron spin resonance where no zero--field splitting was found. The magnetism of textbf{1}-textbf{4} crosses a spectrum from quasi-two-dimensional to three-dimensional antiferromagnetism. An excellent agreement was found between the pulsed-field magnetization, magnetic susceptibility and $T_textrm{N}$ of textbf{2} and textbf{4}. Magnetization curves for textbf{2} and textbf{4} calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. textbf{3} is characterized as a three-dimensional antiferromagnet with the interlayer interaction ($J_perp$) slightly stronger than the interaction within the two-dimensional [Ni(pyz)$_2$]$^{2+}$ square planes ($J_textrm{pyz}$).
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.
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.
Static and dynamic properties of the quasi-two-dimensional antiferromagnet K$_2$V$_3$O$_8$ have been investigated by $^{51}$V-NMR experiments on nonmagnetic V$^{5+}$ sites. Above the structural transition temperature $T_{rm{S}}$ = 115 K, NMR spectra are fully compatible with the $P4bm$ space group symmetry. The formation of superstructure below $T_{rm{S}}$ causes splitting of the NMR lines, which get broadened at lower temperatures so that individual peaks are not well resolved. Evolution of NMR spectra with magnetic field along $c$-axis below the magnetic transition temperature $T_{rm{N}} sim 4$ K is qualitatively consistent with a simple N{e}el order and a spin flop transition. However, broad feature of the spectra does not rule out possible incommensurate spin structure. The spin-lattice relaxation rate $1/T_1$ below $T_{rm{N}}$ shows huge enhancement for a certain range of magnetic field, which is independent of temperature and attributed to cross relaxation due to anomalously large nuclear spin-spin coupling between V$^{5+}$ and magnetic V$^{4+}$ sites. The results indicate strong gapless spin fluctuations, which could arise from incommesurate orders or complex spin textures.
Magnetic excitations of the quasi-1D S=1/2 Heisenberg antiferromagnet (HAF) Cs2CuCl4 have been measured as a function of magnetic field using neutron scattering. For T<0.62 K and B=0 T the weak inter-chain coupling produces 3D incommensurate ordering. Fields greater than Bc =1.66 T, but less than the field (~8 T) required to fully align the spins, are observed to decouple the chains, and the system enters a disordered intermediate-field phase (IFP). The IFP excitations are in agreement with the predictions of Muller et al. for the 1D S=1/2 HAF, and Talstra and Haldane for the related 1/r^2 chain (the Haldane-Shastry model). This behaviour is inconsistent with linear spin-wave theory.
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