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Register a new userStructural dimerization in the commensurate magnetic phases of NaFe(WO$_4$)$_2$ and MnWO$_4$
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Added by
Sebastian Biesenkamp
Publication date
2020
fields
Physics
and research's language is
English
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The structural distortion and magnetoelastic coupling induced through commensurate magnetism has been investigated by neutron diffraction in structurally related MnWO$_4$ and NaFe(WO$_4$)$_2$. Both systems exhibit a competition of incommensurate spiral and commensurate spin up-up-down-down ordering along the magnetic chains. In the latter commensurate phases, the alternatingly parallel and antiparallel arrangement of Fe$^{3+}$ respectively Mn$^{2+}$ moments leads to sizeable bond-angle modulation and thus to magnetic dimerization. For NaFe(WO$_4$)$_2$ this structural distortion has been determined to be strongest for the low-field up-up-down-down arrangement, and the structural refinement yields a bond-angle modulation of $pm 1.15(16)$ degrees. In the commensurate phase of MnWO$_4$, superstructure reflections signal a comparable structural dimerization and thus strong magneto-elastic coupling different to that driving the multiferroic order. Pronounced anharmonic second- and third-order reflections in the incommensurate and multiferroic phase of MnWO$_4$ result from tiny commensurate fractions that can depin multiferroic domains.
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The crystal structure of the double tungstate NaFe(WO$_4$)$_2$ arises from that of the spin-driven multiferroic MnWO$_4$ by inserting non-magnetic Na layers. NaFe(WO$_4$)$_2$ exhibits a three-dimensional incommensurate spin-spiral structure at low temperature and zero magnetic field, which, however, competes with commensurate order induced by magnetic field. The incommensurate zero-field phase corresponds to the condensation of a single irreducible representation but it does not imply ferroelectric polarization because spirals with opposite chirality coexist. Sizable anharmonic modulations emerge in this incommensurate structure, which are accompanied by large magneto-elastic anomalies, while the onset of the harmonic order is invisible in the thermal expansion coefficient. In magnetic fields applied along the monoclinic axis, we observe a first-order transition to a commensurate structure that again is accompanied by large magneto-elastic effects. The large magnetoelastic coupling, a reduction of the $b$ lattice parameter, is thus associated only with the commensurate order. Upon releasing the field at low temperature, the magnetic order transforms to another commensurate structure that considerably differs from the incommensurate low-temperature phase emerging upon zero-field cooling. The latter phase, which exhibits a reduced ordered moment, seems to be metastable.
The crystal and magnetic structure of multiferroic LiFe(WO$_4$)$_2$ were investigated by temperature and magnetic-field dependent specific heat, susceptibility and neutron diffraction experiments on single crystals. Considering only the two nearest-neighbour magnetic interactions, the system forms a $J_1$, $J_2$ magnetic chain but more extended interactions are sizeable. Two different magnetic phases exhibiting long-range incommensurate order evolve at $T_{text{N}1}approx 22.2 text{ K}$ and $T_{text{N}2}approx 19 text{ K}$. First, a spin-density wave develops with moments lying in the $ac$ plane. In its multiferroic phase below $T_{text{N}2}$, LiFe(WO$_4$)$_2$ exhibits a spiral arrangement with an additional spin-component along $b$. Therefore, the inverse Dzyaloshinskii-Moriya mechanism fully explains the multiferroic behavior in this material. A partially unbalanced multiferroic domain distribution was observed even in the absence of an applied electric field. For both phases only a slight temperature dependence of the incommensurability was observed and there is no commensurate phase emerging at low temperature or at finite magnetic fields up to $6text{ T}$. LiFe(WO$_4$)$_2$ thus exhibits a simple phase diagram with the typical sequence of transitions for a type-II multiferroic material.
Sr$_2$RuO$_4$, an unconventional superconductor, is known to possess an incommensurate spin density wave instability driven by Fermi surface nesting. Here we report a static spin density wave ordering with a commensurate propagation vector $q_c$ = (0.25 0.25 0) in Fe-doped Sr$_2$RuO$_4$, despite the magnetic fluctuations persisting at the incommensurate wave vectors $q_{ic}$ = (0.3 0.3 L) as in the parent compound. The latter feature is corroborated by the first principles calculations, which show that Fe substitution barely changes the nesting vector of the Fermi surface. These results suggest that in addition to the known incommensurate magnetic instability, Sr$_2$RuO$_4$ is also in proximity to a commensurate magnetic tendency that can be stabilized via Fe doping.
The relationship between magnetic order and ferroelectric properties has been investigated for MnWO$_4$ with long-wavelength magnetic structure. Spontaneous electric polarization is observed in an elliptical spiral spin phase. The magnetic-field dependence of electric polarization indicates that the noncollinear spin configuration plays a key role for the appearance of ferroelectric phase. An electric polarization flop from the b direction to the a direction has been observed when a magnetic field above 10T is applied along the b axis. This result demonstrates that an electric polarization flop can be induced by a magnetic field in a simple system without rare-earth f-moments.
We report on the electronic ground state of a layered perovskite vanadium oxide Sr$_2$VO$_4$ studied by the combined use of synchrotron radiation x-ray diffraction (SR-XRD) and muon spin rotation/relaxation ($mu$SR) techniques, where $mu$SR measurements were extended down to 30 mK. We found an intermediate orthorhombic phase between $T_{rm c2} sim$~130 K and $T_{rm c1} sim$~100 K, whereas a tetragonal phase appears for $T > T_{rm c2}$ and $T < T_{rm c1}$. The absence of long-range magnetic order was confirmed by $mu$SR at the reentrant tetragonal phase below $T_{rm c1}$, where the relative enhancement in the $c$-axis length versus that of the $a$-axis length was observed. However, no clear indication of the lowering of the tetragonal lattice symmetry with superlattice modulation, which is expected in the orbital order state with superstructure of $d_{yz}$ and $d_{zx}$ orbitals, was observed by SR-XRD below $T_{rm c1}$. Instead, it was inferred from $mu$SR that a magnetic state developed below $T_{rm c0} sim$~10 K, which was characterized by the highly inhomogeneous and fluctuating local magnetic fields down to 30 mK. We argue that the anomalous magnetic ground state below $T_{rm c0}$ originates from the coexistence of ferromagnetic and antiferromagnetic correlations.
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