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Unusual Magnetic Response of an $S = 1$ Antiferromagetic Linear-Chain Material

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 Added by Mark W. Meisel
 Publication date 2014
  fields Physics
and research's language is English




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An $S=1$ antiferromagnetic polymeric chain, [Ni(HF$_2$)(3-Clpy)$_4$]BF$_4$ (py = pyridine), has previously been identified to have intrachain, nearest-neighbor antiferromagnetic interaction strength $J/k_{mathrm{B}} = 4.86$ K and single-ion anisotropy (zero-field splitting) $D/k_{mathrm{B}} = 4.3$ K, so the ratio $D/J = 0.88$ places this system close to the $D/J approx 1$ gapless critical point between the topologically distinct Haldane and Large-$D$ phases. The magnetization was studied over a range of temperatures, 50 mK $leq T leq 1$ K, and magnetic fields, $B leq 10$ T, in an attempt to identify a critical field, $B_{mathrm{c}}$, associated with the closing of the Haldane gap, and the present work places an upper bound of $B_{mathrm{c}} leq (35 pm 10)$ mT. At higher fields, the observed magnetic response is qualitatively similar to the excess signal observed by other workers at 0.5 K and below 3 T. The high-field (up to 14.5 T), multi-frequency (nomially 200 GHz to 425 GHz) ESR spectra at 3 K reveal several broad features considered to be associated with the linear-chain sample.



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We have measured the specific heat of an S=1/2 antiferromagnetic alternating Heisenberg chain pentafulorophenyl nitronyl nitroxide under magnetic fields up to H>H_C2. This compound has the field-induced magnetic ordered (FIMO) phase between H_C1 and H_C2. Characteristic behaviors are observed depending on the magnetic field up to above H_C2 outside of the H-T boundary for the FIMO. Temperature and field dependence of the specific heat are qualitatively in good agreement with the theoretical calculation on an S=1/2 two-leg ladder. [Wang et al. Phys. Rev. Lett 84 5399 (2000)] This agreement suggests that the observed behaviors are related with the low-energy excitation in the Tomonaga-Luttinger liquid.
Magnetoelectric properties were investigated for an S=1/2 chain antiferromagnet CuCl2, which turns out to be the first example of non-chalcogen based spiral-spin induced multiferroics. Upon the onset of helimagnetic order propagating along the b-axis under zero magnetic field (H), we found emergence of ferroelectric polarization along the c-axis. Application of H along the b-axis leads to spin-flop transition coupled with drastic suppression of ferroelectricity, and rotation of H around the b-axis induces the rotation of spin-spiral plane and associated polarization direction. These behaviors are explained well within the framework of the inverse Dzyaloshinskii-Moriya model, suggesting the robustness of this magnetoelectric coupling mechanism even under the strong quantum fluctuation.
We present the results of the magnetization and dielectric constant measurements on untwinned single crystal samples of the frustrated S=1/2 chain cuprate LiCu_2O_2. Novel magnetic phase transitions were observed. A spin flop transition of the spiral spin plane was observed for the field orientations H||a,b. The second magnetic transition was observed at H~15 T for all three principal field directions. This high field magnetic phase is discussed as a collinear spin-modulated phase which is expected for an S=1/2 nearest-neighbor ferromagnetic and next-nearest-neighbor antiferromagnetic chain system.
The low energy magnetic excitation spectrum of the Heisenberg antiferromagnetic $S = 1/2$ chain system Sr$_2$CuO$_3$ with Ni- and Ca-impurities is studied by neutron spectroscopy. In all cases, a defect-induced spectral pseudogap is observed and shown to scale proportionately to the number of scattering centers in the spin chains.
Magnetic response of uranium dioxide (UO2) has been investigated through temperature and magnetic field dependent dc magnetization measurements. UO2 is a paramagnet at room temperature. The magnetic susceptibility, however, deviates from Curie-Weiss (CW) like paramagnetic behavior below T = 280 K. Further down the temperature UO2 undergoes phase transition to an antiferromagnetic state below TN = 30.6 K. The zero field cooled (ZFC) and field cooled (FC) magnetizations exhibit some distinct thermomagnetic irreversibility below TN. The temperature dependence of the FC magnetization is more like a ferromagnet, whereas ZFC magnetization exhibits distinct structures not usually observed in the antiferromagnets. In low applied magnetic field this thermomagnetic irreversibility in magnetization exists in a subtle way even in the paramagnetic regime above TN up to a fairly high temperature, but vanishes in high applied magnetic fields. Deviation from CW law and irreversibility between ZFC and FC magnetization indicate that the paramagnetic state above TN is not a trivial one. Magnetic response below TN changes significantly with the increase in the applied magnetic field. Thermomagnetic irreversibility in magnetization initially increases with the increase in the strength of applied magnetic field, but then gets reduced in the high applied fields. A subtle signature of a magnetic field induced phase transition is also observed in the isothermal magnetic field vartaion of magnetization. All these experimetal results highlight the non-trivial nature of the antiferromagnetic state in UO2
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