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Register a new userJ$_{eff}$ description of the honeycomb Mott insulator ${alpha}$-RuCl$_3$
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Novel ground states might be realized in honeycomb lattices with strong spin-orbit coupling. Here we study the electronic structure of ${alpha}$-RuCl$_3$, in which the Ru ions are in a d5 configuration and form a honeycomb lattice, by angle-resolved photoemission, x-ray photoemission and electron energy loss spectroscopy supported by density functional theory and multiplet calculations. We find that ${alpha}$-RuCl$_3$ is a Mott insulator with significant spin-orbit coupling, whose low energy electronic structure is naturally mapped onto Jeff states. This makes ${alpha}$-RuCl$_3$ a promising candidate for the realization of Kitaev physics. Relevant electronic parameters such as the Hubbard energy U, the crystal field splitting 10Dq and the charge transfer energy are evaluated. Furthermore, we observe significant Cl photodesorption with time, which must be taken into account when interpreting photoemission and other surface sensitive experiments.
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We report on the unusual behavior of the in-plane thermal conductivity ($kappa$) and torque ($tau$) response in the Kitaev-Heisenberg material $alpha$-RuCl$_3$. $kappa$ shows a striking enhancement with linear growth beyond H = 7 T, where magnetic order disappears, while $tau$ for both of the in-plane symmetry directions shows an anomaly at the same field. The temperature- and field-dependence of $kappa$ are far more complex than conventional phonon and magnon contributions, and require us to invoke the presence of unconventional spin excitations whose properties are characteristic of a field-induced spin-liquid phase related to the enigmatic physics of the Kitaev model in an applied magnetic field
The pure Kitaev honeycomb model harbors a quantum spin liquid in zero magnetic fields, while applying finite magnetic fields induces a topological spin liquid with non-Abelian anyonic excitations. This latter phase has been much sought after in Kitaev candidate materials, such as $alpha$-RuCl$_3$. Currently, two competing scenarios exist for the intermediate field phase of this compound ($B=7-10$ T), based on experimental as well as theoretical results: (i) conventional multiparticle magnetic excitations of integer quantum number vs. (ii) Majorana fermionic excitations of possibly non-Abelian nature with a fractional quantum number. To discriminate between these scenarios a detailed investigation of excitations over a wide field-temperature phase diagram is essential. Here we present Raman spectroscopic data revealing low-energy quasiparticles emerging out of a continuum of fractionalized excitations at intermediate fields, which are contrasted by conventional spin-wave excitations. The temperature evolution of these quasiparticles suggests the formation of bound states out of fractionalized excitations.
We present high-field electron spin resonance (ESR) studies of the honeycomb-lattice material $alpha$-RuCl$_3$, a prime candidate to exhibit Kitaev physics. Two modes of antiferromagnetic resonance were detected in the zigzag ordered phase, with magnetic field applied in the $ab$ plane. A very rich excitation spectrum was observed in the field-induced quantum paramagnetic phase. The obtained data are compared with results of recent numerical calculations, strongly suggesting a very unconventional multiparticle character of the spin dynamics in $alpha$-RuCl$_3$. The frequency-field diagram of the lowest-energy ESR mode is found consistent with the behavior of the field-induced energy gap, revealed by thermodynamic measurements.
We perform Raman spectroscopy studies on $alpha$-RuCl$_3$ at room temperature to explore its phase transitions of magnetism and chemical bonding under pressures. The Raman measurements resolve two critical pressures, about $p_1=1.1$~GPa and $p_2=1.7$~GPa, involving very different intertwining behaviors between the structural and magnetic excitations. With increasing pressures, a stacking order phase transition of $alpha$-RuCl$_3$ layers develops at $p_1=1.1$~GPa, indicated by the new Raman phonon modes and the modest Raman magnetic susceptibility adjustment. The abnormal softening and splitting of the Ru in-plane Raman mode provide direct evidence of the in-plane dimerization of the Ru-Ru bonds at $p_2=1.7$~GPa. The Raman susceptibility is greatly enhanced with pressure increasing and sharply suppressed after the dimerization. We propose that the system undergoes Mott collapse at $p_2=1.7$~GPa and turns into a dimerized correlated band insulator. Our studies demonstrate competitions between Kitaev physics, magnetism, and chemical bondings in Kitaev compounds.
Thermodynamics of the Kitaev honeycomb magnet $alpha$-RuCl$_3$ is studied for different directions of in-plane magnetic field using measurements of the magnetic Gruneisen parameter $Gamma_B$ and specific heat $C$. We identify two critical fields $B_c^{rm AF1}$ and $B_c^{rm AF2}$ corresponding, respectively, to a transition between two magnetically ordered states and the loss of magnetic order toward a quantum paramagnetic state. The $B_c^{AF2}$ phase boundary reveals a narrow region of magnetic fields where inverse melting of the ordered phase may occur. No additional transitions are detected above $B_c^{rm AF2}$ for any direction of the in-plane field, although a shoulder anomaly in $Gamma_B$ is observed systematically at $8-10$ T. Large field-induced entropy effects imply additional low-energy excitations at low fields and/or strongly field-dependent phonon entropies. Our results establish universal features of $alpha$-RuCl$_3$ in high magnetic fields and challenge the presence of a field-induced Kitaev spin liquid in this material.
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