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Spin Density Wave in Insulating Ferromagnetic Frustrated Chain LiCuVO$_4$

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 Added by Takatsugu Masuda
 Publication date 2011
  fields Physics
and research's language is English




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We study field induced quantum phase in weakly-coupled ferromagnetic frustrated chain LiCuVO$_4$ by neutron diffraction technique. A new incommensurate magnetic peak is observed at $H ge 8.5$ T. The field dependent propagation vector is identified with the spin density wave correlation in the theoretically predicted magnetic quadrupole order. Quantum fluctuation, geometrical frustration, and interchain interaction induce the exotic spin density wave long-range order in the insulating magnet.

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We report on a heat capacity study of high quality single crystal samples of lcvo -- a frustrated spin $S=1/2$ chain system -- in magnetic field amounting to 3/4 of the saturation field. At low fields up to about 7~T, a linear temperature dependence of the specific heat, $C_ppropto T$, resulting from 1D magnetic correlations in the spin chains is followed upon cooling by a sharp lambda anomaly of the transition into a 3D helical phase with $C_ppropto T^3$ behavior at low temperature. The transition from a spin liquid into a spin-modulated (SM) phase at higher fields occurs via a hump-like anomaly which, as the temperature decreases further turns into a $C_ppropto T^2$ law distinctive for a quasi-2D system. We suggest an explanation for how nonmagnetic defects in the Cu$^{2+}$ chains can suppress 3D long-range ordering in the SM phase and leave it undisturbed in a helical phase.
We investigated the magnetoelastic properties of the quasi-one-dimensional spin-1/2 frustrated magnet LiCuVO$_4$. Longitudinal-magnetostriction experiments were performed at 1.5 K in high magnetic fields of up to 60 T applied along the $b$ axis, i.e., the spin-chain direction. The magnetostriction data qualitatively resemble the magnetization results, and saturate at $H_{text{sat}} approx 54$ T, with a relative change in sample length of $Delta L/L approx 1.8times10^{-4}$. Remarkably, both the magnetostriction and the magnetization evolve gradually between $H_{text{c3}} approx 48$ T and $H_{text{sat}}$, indicating that the two quantities consistently detect the spin-nematic phase just below the saturation. Numerical analyses for a weakly coupled spin-chain model reveal that the observed magnetostriction can overall be understood within an exchange-striction mechanism. Small deviations found may indicate nontrivial changes in local correlations associated with the field-induced phase transitions.
Chirality or the handedness of objects is of prime importance in life science, biology, chemistry and physics. It is also a major symmetry ingredient in frustrated magnets revealing spin-spiral ground states. Vector chiral phases, with the twist (either clock- or counter clock-wise) between neighbouring spins being ordered, but with disorder with respect to the angles between adjacent spins, have been predicted almost five decades ago. Experimental proofs, however, are rare and controversial. Here, we provide experimental evidence for such a phase in LiCuVO$_4$, a one-dimensional quantum magnet with competing ferromagnetic and antiferromagnetic interactions. The vector chiral state is identified via a finite ferroelectric polarization arising at temperatures well above the multiferroic phase exhibiting long-range three-dimensional spin-spiral and polar order. On increasing temperatures, spin order becomes suppressed at TN, while chiral long-range order still exist, leaving a temperature window with chirality-driven ferroelectricity in the presence of an external magnetic field.
In this joint experimental and theoretical work magnetic properties of the Cu$^{2+}$ mineral szenicsite Cu$_3$(MoO$_4$)(OH)$_4$ are investigated. This compound features isolated triple chains in its crystal structure, where the central chain involves an edge-sharing geometry of the CuO$_4$ plaquettes, while the two side chains feature a corner-sharing zig-zag geometry. The magnetism of the side chains can be described in terms of antiferromagnetic dimers with a coupling larger than 200 K. The central chain was found to be a realization of the frustrated antiferromagnetic $J_1$-$J_2$ chain model with $J_1simeq 68$ K and a sizable second-neighbor coupling $J_2$. The central and side chains are nearly decoupled owing to interchain frustration. Therefore, the low-temperature behavior of szenicsite should be entirely determined by the physics of the central frustrated $J_1$-$J_2$ chain. Our heat-capacity measurements reveal an accumulation of entropy at low temperatures and suggest a proximity of the system to the Majumdar-Ghosh point of the antiferromagnetic $J_1$-$J_2$ spin chain, $J_2/J_1=0.5$.
The frustrated one-dimensional (1D) quantum magnet LiCuSbO$_4$ is one rare realization of the $J_1-J_2$ spin chain model with an easily accessible saturation field, formerly estimated to 12~T. Exotic multipolar nematic phases were theoretically predicted in such compounds just below the saturation field, but without unambiguous experimental observation so far. In this paper we present extensive experimental research of the compound in the wide temperature (30mK$-$300K) and field (0$-$13.3T) range by muon spin rotation ($mu$SR), $^7$Li nuclear magnetic resonance (NMR) and magnetic susceptibility (SQUID). $mu$SR experiments in zero magnetic field demonstrate the absence of long range 3D ordering down to 30mK. Together with former heat capacity data [S.E. Dutton emph{et al}, Phys. Rev. Lett. 108, 187206 (2012)], magnetic susceptibility measurements suggest short range correlated vector chiral phase in the field range $0-4$T. In the intermediate field values (5$-$12T), the system enters in a 3D ordered spin density wave phase with 0.75$mu_B$ per copper site at lowest temperatures (125mK), estimated by NMR. At still higher field, the magnetization is found to be saturated above 13T where the spin lattice $T_1^{-1}$ relaxation reveals a spin gap estimated to 3.2(2)K. We narrow down the possibility of observing a multipolar nematic phase to the range 12.5$-$13T.
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