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Quantum spin fluctuations in the spin liquid state of Tb2Ti2O7

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 Added by Hiroaki Kadowaki
 Publication date 2011
  fields Physics
and research's language is English




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Neutron scattering experiments on a polycrystalline sample of the frustrated pyrochlore magnet Tb2Ti2O7, which does not show any magnetic order down to 50 mK, have revealed that it shows condensation behavior below 0.4 K from a thermally fluctuating paramagnetic state to a spin-liquid ground-state with quantum spin fluctuations. Energy spectra change from quasielastic scattering to a continuum with a double-peak structure at energies of 0 and 0.8 K in the spin-liquid state. Specific heat shows an anomaly at the crossover temperature.



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The pyrochlore antiferromagnet Tb2Ti2O7 has proven to be an enigma to experimentalists and theorists working on frustrated magnetic systems. The experimentally determined energy level structure suggests a local <111> Ising antiferromagnet at low temperatures, T < 10 K. An appropriate model then predicts a long-range ordered Q = 0 state below approximately 2 K. However, muon spin resonance experiments reveal a paramagnetic structure down to tens of milli-Kelvin. The importance of fluctuations out of the ground state effective Ising doublet has been recently understood, for the measured paramagnetic correlations can not be described without including the higher crystal field states. However, these fluctuations treated within the random phase approximation (RPA) fail to account for the lack of ordering in this system below 2 K. In this work, we briefly review the experimental evidence for the collective paramagnetic state of Tb2Ti2O7. The basic theoretical picture for this system is discussed, where results from classical spin models are used to motivate the investigation of quantum effects to lowest order via the RPA. Avenues for future experimental and theoretical work on Tb2Ti2O7 are presented.
We have studied the spin correlations with $bf{k}$= ($frac12$, $frac12$, $frac12$) propagation vector which appear below 0.4, K in tbti spin liquid by combining powder neutron diffraction and specific heat on Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ samples with $x$=0, 0.01, -0.01. The $bf{k}$= ($frac12$, $frac12$, $frac12$) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1),K. Refining the subtracted patterns at 0.07,K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 mub ordered on a length scale of about 20 AA. In addition, long range order involving a small spin component of 0.1 to 0.2 mub is detected for the $x$= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ($frac12$, $frac12$, $frac12$) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.
Neutron scattering, a.c. magnetic susceptibility and specific heat studies have been carried out on polycrystalline Dy2Zr2O7. Unlike the pyrochlore spin ice Dy2Ti2O7, Dy2Zr2O7 crystallizes into the fluorite structure and the magnetic Dy3+ moments randomly reside on the corner-sharing tetrahedral sublattice with non-magnetic Zr ions. Antiferromagnetic spin correlations develop below 10 K but remain dynamic down to 40 mK. These correlations extend over the length of two tetrahedra edges and grow to 6 nearest neighbors with the application of a 20 kOe magnetic field. No Paulings residual entropy was observed and by 8 K the full entropy expected for a two level system is released. We propose that the disorder melts the spin ice state seen in the chemically ordered Dy2Ti2O7 compound, but the spins remain dynamic in a disordered, liquid-like state and do not freeze into a glass-like state that one might intuitively expect.
Spin freezing in the $A$-site spinel FeAl$_2$O$_4$ which is a spin liquid candidate is studied using remnant magnetization and nonlinear magnetic susceptibility and isofield cooling and heating protocols. The remnant magnetization behavior of FeAl$_2$O$_4$ differs significantly from that of a canonical spin glass which is also supported by analysis of the nonlinear magnetic susceptibility term $chi_3 (T)$. Through the power-law analysis of $chi_3 (T)$, a spin-freezing temperature, $T_g$ = 11.4$pm$0.9~K and critical exponent, $gamma$ = 1.48$pm$0.59 are obtained. Cole-Cole analysis of magnetic susceptibility shows the presence of broad spin relaxation times in FeAl$_2$O$_4$, however, the irreversible dc susceptibility plot discourages an interpretation based on conventional spin glass features. The magnetization measured using the cooling-and-heating-in-unequal-fields protocol brings more insight to the magnetic nature of this frustrated magnet and reveals unconventional glassy behaviour. Combining our results, we arrive at the conclusion that the present sample of FeAl$_2$O$_4$ consists of a majority spin liquid phase with glassy regions embedded.
The Kitaev model on a honeycomb lattice predicts a paradigmatic quantum spin liquid (QSL) exhibiting Majorana Fermion excitations. The insight that Kitaev physics might be realized in practice has stimulated investigations of candidate materials, recently including alpha-RuCl3. In all the systems studied to date, non-Kitaev interactions induce magnetic order at low temperature. However, in-plane magnetic fields of roughly 8 Tesla suppress the long-range magnetic order in alpha-RuCl3 raising the intriguing possibility of a field-induced QSL exhibiting non-Abelian quasiparticle excitations. Here we present inelastic neutron scattering in alpha-RuCl3 in an applied magnetic field. At a field of 8 Tesla, the spin waves characteristic of the ordered state vanish throughout the Brillouin zone. The remaining single dominant feature of the response is a broad continuum centered at the Gamma point, previously identified as a signature of fractionalized excitations. This provides compelling evidence that a field-induced QSL state has been achieved.
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