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Dynamical structure factor of the three-dimensional quantum spin liquid candidate NaCaNi$_2$F$_7$

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 Added by Shu Zhang
 Publication date 2018
  fields Physics
and research's language is English




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We study the spin-1 pyrochlore material NaCaNi$_2$F$_7$ with a combination of molecular dynamics simulations, stochastic dynamical theory and linear spin wave theory. The dynamical structure factor from inelastic neutron scattering is well described with a near-ideal Heisenberg Hamiltonian incorporating small anisotropic terms {and weak second-neighbor interactions}. We find that all three approaches reproduce remarkably well the momentum dependence of the scattering intensity as well as its energy dependence with the exception of the lowest energies. These results are notable in that (i) the data show a complete lack of sharp quasiparticle excitations in momentum space over much, if not all, of the energy range; (ii) linear spin-wave theory appears to apply in a regime where it would be expected to fail for a number of reasons. We elucidate what underpins these surprises, and note that basic questions about the nature of quantum spin liquidity in such systems pose themselves as a result.



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A new pyrochlore compound, NaCaNi$_2$F$_7$, was recently synthesized and has a single magnetic site with spin-1 Ni$^{2+}$. We present zero field (ZF) and longitudinal field (LF) muon spin rotation ($mu$SR) measurements on this pyrochlore. Density functional theory (DFT) calculations show that the most likely muon site is located between two fluorine ions, but off-centre. A characteristic F-$mu$-F muon spin polarization function is observed at high temperatures where Ni spin fluctuations are sufficiently rapid. The Ni$^{2+}$ spins undergo spin freezing into a disordered ground state below 4~K, with a characteristic internal field strength of 140~G. Persistent Ni spin dynamics are present to our lowest temperatures (75~mK), a feature characteristic of many geometrically frustrated magnetic systems.
Two-dimensional triangular-lattice materials with spin-1/2 are perfect platforms for investigating quantum frustrated physics with spin fluctuations. Here we report the structure, magnetization, heat capacity and inelastic neutron scattering (INS) results on cesium ytterbium diselenide, CsYbSe$_2$. There is no long-range magnetic order down to 0.4 K at zero field. The temperature dependent magnetization, $M(T)$, reveals an easy-plane magnetic anisotropy. A maximum is found in $M(T)$ around emph{T}$sim$1.5 K when magnetic field $H$ is applied in the $ab$ plane, indicating the short-range interaction. The low-temperature isothermal magnetization $M(H)$ shows a one-third plateau of the estimated saturation moment, that is characteristic of a two-dimensional frustrated triangular lattice. Heat capacity shows field-induced long-range magnetic order for both $H||c$ and $H||ab$ directions. The broad peak in heat capacity and highly damped INS magnetic excitation at $T$=2 K suggests strong spin fluctuations. The dispersive in-plane INS, centered at the (1/3 1/3 0) point, and the absence of dispersion along $c$ direction suggests 120$^{circ}$ non-collinear 2D-like spin correlations. All these results indicate that the two-dimensional frustrated material CsYbSe$_2$ can be in proximity to the triangular-lattice quantum spin liquid. We propose an experimental low-temperature $H$-$T$ phase diagram for CsYbSe$_2$.
139 - H. Cao , A. Gukasov , I. Mirebeau 2008
We have studied the field induced magnetic structures in the spin liquid Tb$_2$Ti$_2$O$_7$, in a wide temperature (0.3$<$$T$$<$270 K) and field (0$<$$H$$<$7 T) range, by single crystal neutron diffraction with $bf{H}$ // [110] axis. We combined unpolarized neutron data with polarized ones, analyzed within the local susceptibility model. A ferromagnetic-like structure with $bf{k}$ = 0 propagation vector is induced, whose local order at low field and low temperature is akin to spin ice. The four Tb ions separate in $alpha$ and $beta$ chains having different values of the magnetic moments, which is quantitatively explained by taking the crystal field anisotropy into account. Above 2 T and below 2 K, an antiferromagnetic-like structure with $bf{k}$ = (0,0,1) is induced besides the $bf{k}$ = 0 structure. It shows a reentrant behavior and extends over a finite length scale. It occurs together with a broadening of the nuclear peaks, which suggests a field induced distortion and magnetostriction effect.
The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. In the pyrochlore Tb$_2$Hf$_2$O$_7$, we demonstrate that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly-fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.
Inelastic neutron scattering reveals a broad continuum of excitations in Pr$_2$Zr$_2$O$_7$, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields ($Delta$) acting on the non-Kramers Pr$^{3+}$ crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution $rho(Delta)propto (Delta^2+Gamma^2)^{-1}$ where $ Gamma=0.27(1)$ meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr$_2$Zr$_2$O$_7$ actually induces a quantum spin liquid.
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