No Arabic abstract
The frustrated magnet $alpha$-RuCl$_3$ constitutes a fascinating quantum material platform that harbors the intriguing Kitaev physics. However, a consensus on its intricate spin interactions and field-induced quantum phases has not been reached yet. Here we exploit multiple state-of-the-art many-body methods and determine the microscopic spin model that quantitatively explains major observations in $alpha$-RuCl$_3$, including the zigzag order, double-peak specific heat, magnetic anisotropy, and the characteristic M-star dynamical spin structure, etc. According to our model simulations, the in-plane field drives the system into the polarized phase at about 7 T and a thermal fractionalization occurs at finite temperature, reconciling observations in different experiments. Under out-of-plane fields, the zigzag order is suppressed at 35 T, above which, and below a polarization field of 100 T level, there emerges a field-induced quantum spin liquid. The fractional entropy and algebraic low-temperature specific heat unveil the nature of a gapless spin liquid, which can be explored in high-field measurements on $alpha$-RuCl$_3$.
An external magnetic field can induce a transition in $alpha$-RuCl$_3$ from an ordered zigzag state to a disordered state that is possibly related to the Kitaev quantum spin liquid. Here we present new field dependent inelastic neutron scattering and magnetocaloric effect measurements implying the existence of an additional transition out of the quantum spin liquid phase at an upper field limit $B_u$. The neutron scattering shows three distinct regimes of magnetic response. In the low field ordered state the response shows magnon peaks; the intermediate field regime shows only continuum scattering, and above $B_u$ the response shows sharp magnon peaks at the lower bound of a strong continuum. Measurable dispersion of magnon modes along the $(0,0,L)$ direction implies non-negligible inter-plane interactions. Combining the magnetocaloric effect measurements with other data a $T-B$ phase diagram is constructed. The results constrain the range where one might expect to observe quantum spin liquid behavior in $alpha$-RuCl$_3$.
We report a $^{35}$Cl nuclear magnetic resonance study in the honeycomb lattice, $alpha$-RuCl$_3$, a material that has been suggested to potentially realize a Kitaev quantum spin liquid (QSL) ground state. Our results provide direct evidence that $alpha$-RuCl$_3$ exhibits a magnetic field-induced QSL. For fields larger than $sim 10$ T a spin-gap opens up while resonance lines remain sharp, evidencing that spins are quantum disordered and locally fluctuating. The spin gap increases linearly with increasing magnetic field, reaching $sim50$ K at 15 T, and is nearly isotropic with respect to the field direction. The unusual rapid increase of the spin gap with increasing field and its isotropic nature are incompatible with conventional magnetic ordering and in particular exclude that the ground state is a fully polarized ferromagnet. The presence of such a field-induced, gapped QSL phase has indeed been predicted in the Kitaev model.
We study on transport and magnetic properties of hydrated and lithium-intercalated $alpha$-RuCl$_3$, Li$_x$RuCl$_3 cdot y$H$_2$O, for investigating the effect on mobile-carrier doping into candidate materials for a realization of a Kitaev model. From thermogravitometoric and one-dimensional electron map analyses, we find two crystal structures of this system, that is, mono-layer hydrated Li$_x$RuCl$_3 cdot y$H$_2$O~$(xapprox0.56, yapprox1.3)$ and bi-layer hydrated Li$_x$RuCl$_3 cdot y$H$_2$O~$(xapprox0.56, yapprox3.9)$. The temperature dependence of the electrical resistivity shows a temperature hysteresis at 200-270 K, which is considered to relate with a formation of a charge order. The antiferromagnetic order at 7-13 K in pristine $alpha$-RuCl$_3$~ is successfully suppressed down to 2 K in bi-layer hydrated Li$_x$RuCl$_3 cdot y$H$_2$O, which is sensitive to not only an electronic state of Ru but also an interlayer distance between Ru-Cl planes.
The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. Detection of these excitations remains challenging, because of their fractional quantum numbers and non-locality. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we uncover this effect in $alpha$-RuCl3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, JK~8 meV, that coincides with a giant acoustic phonon softening near the Z2 gauge flux energy scale. This fractional excitation induced phonon anomalies uncover the key ingredient of the quantum thermal Hall effect in $alpha$-RuCl3 and demonstrates a proof-of-principle method to detect fractional excitations in topological quantum materials.
We present comprehensive electron spin resonance (ESR) studies of in-plane oriented single crystals of $alpha$-RuCl$_3$, a quasi-two-dimensional material with honeycomb structure, focusing on its high-field spin dynamics. The measurements were performed in magnetic fields up to 16 T, applied along the [110] and [100] directions. Several ESR modes were detected. Combining our findings with recent inelastic neutron- and Raman-scattering data, we identify most of the observed excitations. Most importantly, we show that the low-temperature ESR response beyond the boundary of the magnetically ordered region is dominated by single- and two-particle processes with magnons as elementary excitations. The peculiarities of the excitation spectrum in the vicinity of the critical field are discussed.