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Register a new userNearest-neighbor Kitaev exchange blocked by charge order in electron doped $alpha$-RuCl$_{3}$
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A quantum spin-liquid might be realized in $alpha$-RuCl$_{3}$, a honeycomb-lattice magnetic material with substantial spin-orbit coupling. Moreover, $alpha$-RuCl$_{3}$ is a Mott insulator, which implies the possibility that novel exotic phases occur upon doping. Here, we study the electronic structure of this material when intercalated with potassium by photoemission spectroscopy, electron energy loss spectroscopy, and density functional theory calculations. We obtain a stable stoichiometry at K$_{0.5}$RuCl$_3$. This gives rise to a peculiar charge disproportionation into formally Ru$^{2+}$ (4$d^6$) and Ru$^{3+}$ (4$d^5$). Every Ru 4$d^5$ site with one hole in the $t_{2g}$ shell is surrounded by nearest neighbors of 4$d^6$ character, where the $t_{2g}$ level is full and magnetically inert. Thus, each type of Ru sites forms a triangular lattice and nearest-neighbor interactions of the original honeycomb are blocked.
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$alpha$-RuCl$_{3}$ is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of $alpha$-RuCl$_{3}$ by a resonant inelastic x-ray scattering study at the Ru $L_{3}$ absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilized by competing ferromagnetic correlations. The classical ground state of the experimentally determined Hamiltonian is actually ferromagnetic. The zigzag state is stabilized via a quantum order by disorder mechanism, leaving ferromagnetism -- along with the Kitaev spin liquid -- as energetically proximate metastable states. The three closely competing states and their collective excitations hold the key to the theoretical understanding of the unusual properties of $alpha$-RuCl$_{3}$ in magnetic fields.
The honeycomb Kitaev-Heisenberg model is a source of a quantum spin liquid with Majorana fermions and gauge flux excitations as fractional quasiparticles. In the quest of finding a pertinent material, $alpha$-RuCl$_{3}$ recently emerged as a prime candidate. Here we unveil highly unusual low-temperature heat conductivity $kappa$ of $alpha$-RuCl$_{3}$: beyond a magnetic field of $B_capprox$ 7.5 T, $kappa$ increases by about one order of magnitude, resulting in a large magnetic field dependent peak at about 7 K, both for in-plane as well as out-of-plane transport. This clarifies the unusual magnetic field dependence unambiguously to be the result of severe scattering of phonons off putative Kitaev-Heisenberg excitations in combination with a drastic field-induced change of the magnetic excitation spectrum. In particular, an unexpectedly large energy gap arises, which increases approximately linearly with the magnetic field and reaches a remarkably large $hbaromega_0/k_Bapprox $ 50 K at 18 T.
We calculate the magnetic interactions between two nearest neighbor substitutional magnetic ions (Co or Mn) in ZnO by means of density functional theory and compare it with the available experimental data. Using the local spin density approximation we find a coexistence of ferro- and antiferromagnetic couplings for ZnO:Co, in contrast to experiment. For ZnO:Mn both couplings are antiferromagnetic but deviate quantitatively from measurement. That points to the necessity to account better for the strong electron correlation at the transition ion site which we have done by applying the LSDA+U method. We show that we have to distinguish two different nearest neighbor exchange integrals for the two systems in question which are all antiferromagnetic with values between -1.0 and -2.0 meV in reasonable agreement with experiment.
Raman scattering has been employed to investigate lattice and magnetic excitations of the honeycomb Kitaev material $alpha$-RuCl$_3$ and its Heisenberg counterpart CrCl$_3$. Our phonon Raman spectra give evidence for a first-order structural transition from a monoclinic to a rhombohedral structure for both compounds. Significantly, only $alpha$-RuCl$_3$ features a large thermal hysteresis, consistent with the formation of a wide phase of coexistence. In the related temperature interval of $70-170$ K, we observe a hysteretic behavior of magnetic excitations as well. The stronger magnetic response in the rhombohedral compared to the monoclinic phase evidences a coupling between the crystallographic structure and low-energy magnetic response. Our results demonstrate that the Kitaev magnetism concomitant with fractionalized excitations is susceptible to small variations of bonding geometry.
We have investigated the longitudinal thermal conductivity of $alpha$-RuCl$_{3}$, the magnetic state of which is considered to be proximate to a Kitaev honeycomb model, along with the spin susceptibility and magnetic specific heat. We found that the temperature dependence of the thermal conductivity exhibits an additional peak around 100 K, which is well above the phonon peak temperature ($sim$ 50 K). The higher-temperature peak position is comparable to the temperature scale of the Kitaev couplings rather than the Neel temperatures below 15 K. The additional heat conduction was observed for all five samples used in this study, and was found to be rather immune to a structural phase transition of $alpha$-RuCl$_{3}$, which suggests its different origin from phonons. Combined with experimental results of the magnetic specific heat, our transport measurement suggests strongly that the higher-temperature peak in the thermal conductivity is attributed to itinerant spin excitations associated with the Kitaev couplings of $alpha$-RuCl$_{3}$. A kinetic approximation of the magnetic thermal conductivity yields a mean free path of $sim$ 20 nm at 100 K, which is well longer than the nearest Ru-Ru distance ($sim$ 3 AA), suggesting the long-distance coherent propagation of magnetic excitations driven by the Kitaev couplings.
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