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High-field spin-flop state in green dioptase

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 Added by Giacomo Marmorini
 Publication date 2021
  fields Physics
and research's language is English




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The high-field magnetic properties and magnetic order of the gem mineral green dioptase Cu$_6[$Si$_6$O$_{18}]cdot 6$H$_2$O have been studied by means of single-crystal neutron diffraction in magnetic fields up to $21~$T and magnetization measurements up to $30~$T. In zero field, the Cu$^{2+}$-moments in the antiferromagnetic chains are oriented along the $c$-axis with a small off-axis tilt. For a field applied parallel to the $c$-axis, the magnetization shows a spin-flop-like transition at $B^*=12.2~$T at $1.5~$K. Neutron diffraction experiments show a smooth behavior in the intensities of the magnetic reflections without any change in the periodicity of the magnetic structure. Bulk and microscopic observations are well described by a model of ferromagnetically coupled antiferromagnetic $XXZ$ spin-$frac{1}{2}$ chains, taking into account a change of the local easy-axis direction. We demonstrate that the magnetic structure evolves smoothly from a deformed Neel state at low fields to a deformed spin-flop state in a high field via a strong crossover around $B^*$. The results are generalized for different values of interchain coupling and spin anisotropy.



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The gem-stone dioptase Cu6Si6O18.6H2O has a chiral crystal structure of equilateral triangular helices consisting of Cu-3d spins. It shows an antiferromagnetic order with an easy axis along c at TN = 15.5 K under zero field, and a magnetization jump at HC = 13.5 T when the field is applied along c-axis. By 29Si-NMR measurements, we have revealed that the high-field state is essentially the two sub-lattice structure, and that the component within ab-plane is collinear. The result indicates no apparent match with the geometrical pattern of helical spin chain.
Spin-orbit coupled honeycomb magnets with the Kitaev interaction have received a lot of attention due to their potential of hosting exotic quantum states including quantum spin liquids. Thus far, the most studied Kitaev systems are 4d/5d-based honeycomb magnets. Recent theoretical studies predicted that 3d-based honeycomb magnets, including Na2Co2TeO6 (NCTO), could also be a potential Kitaev system. Here, we have used a combination of heat capacity, magnetization, electron spin resonance measurements alongside inelastic neutron scattering (INS) to study NCTOs quantum magnetism, and we have found a field-induced spin disordered state in an applied magnetic field range of 7.5 T < B (vertical to b-axis) < 10.5 T. The INS spectra were also simulated to tentatively extract the exchange interactions. As a 3d-magnet with a field-induced disordered state on an effective spin-1/2 honeycomb lattice, NCTO expands the Kitaev model to 3d compounds, promoting further interests on the spin-orbital effect in quantum magnets.
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Neutron diffraction measurements under high magnetic fields have been performed for the multiferroic compound HoMn$_{2}$O$_{5}$. At zero field, high-temperature incommensurate magnetic (HT-ICM) -- commensurate magnetic (CM) -- low-temperature incommensurate magnetic (LT-ICM) orders occur with decreasing temperature, where ferroelectric polarization arises only in the CM phase. Upon applying a magnetic field, the LT-ICM phase completely disappears and the CM phase is induced at the lowest temperature. This field-induced CM state is completely associated with the field-induced electric polarization in this material [Higashiyama {it et al}., Phys. Rev. B {bf 72}, 064421 (2005).], strongly indicating that the commensurate spin state is essential to the ferroelectricity in the multiferroic $R$Mn$_{2}$O$_{5}$ system.
We report here a comprehensive study of the AFM structures of the Eu and Mn magnetic sublattices as well as the interplay between Eu and Mn magnetism in this compound by using both polarized and non-polarized single-crystal neutron diffraction. Magnetic susceptibility, specific heat capacity measurements and the temperature dependence of magnetic diffractions suggest that the AFM ordering temperature of the Eu and Mn moments is at 22 and 337 K, respectively. The magnetic moments of both Eu and Mn ions are oriented along the crystallographic $c$ axis, and the respective magnetic propagation vector is $textbf{k}_{Eu} = (0,0,1)$ and $textbf{k}_{Mn}=(0,0,0)$. With proper neutron absorption correction, the ordered moments are refined at 3 K as 7.7(1) $mu_B$ and 4.1(1) $mu_B$ for the Eu and Mn ions, respectively. In addition, a spin-flop (SF) phase transition of the Eu moments in an applied magnetic field along the $c$ axis was confirmed to take place at a critical field of B$_c$ $sim$ 5.3 T. The evolution of the Eu magnetic moment direction as a function of the applied magnetic field in the SF phase was also determined. Clear kinks in both field and temperature dependence of the magnetic reflections ($pm1$, 0, 1) of Mn were observed at the onset of the SF phase transition and the AFM order of the Eu moments, respectively. This unambiguously indicates the existence of a strong coupling between Eu and Mn magnetism. The interplay between two magnetic sublattices could bring new possibilities to tune Dirac fermions via changing magnetic structures by applied fields in this class of magnetic topological semimetals.
Spin-flop transition (SFT) consists in a jump-like reversal of antiferromagnetic magnetic moments into a non-collinear state when the magnetic field increases above the critical value. Potentially the SFT can be utilized in many applications of a rapidly developing antiferromagnetic spintronics. However, the difficulty of using them in conventional antiferromagnets lies in (a) too large switching magnetic fields (b) the need for presence of a magnetic anisotropy, and (c) requirement to apply magnetic field along the correspondent anisotropy axis. In this work we propose to use artificial ferrimagnets in which the spin-flop transition occurs without anisotropy and the transition field can be lowered by adjusting exchange coupling in the structure. This is proved by experiment on artificial Fe-Gd ferrimagnets where usage of Pd spacers allowed us to suppress the transition field by two orders of magnitude.
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