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Competing Antiferromagnetic-Ferromagnetic States in $it{d^7}$ Kitaev Honeycomb Magnet

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 Added by Hector Vivanco
 Publication date 2020
  fields Physics
and research's language is English




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The Kitaev model is a rare example of an analytically solvable and physically instantiable Hamiltonian yielding a topological quantum spin liquid ground state. Here we report signatures of Kitaev spin liquid physics in the honeycomb magnet $Li_3Co_2SbO_6$, built of high-spin $it{d^7}$ ($Co^{2+}$) ions, in contrast to the more typical low-spin $it{d^5}$ electron configurations in the presence of large spin-orbit coupling. Neutron powder diffraction measurements, heat capacity, and magnetization studies support the development of a long-range antiferromagnetic order space group of $it{C_C}2/it{m}$, below $it{T_N}$ = 11 K at $it{mu_0H}$ = 0 T. The magnetic entropy recovered between $it{T}$ = 2 K and 50 K is estimated to be 0.6Rln2, in good agreement with the value expected for systems close to a Kitaev quantum spin liquid state. The temperature-dependent magnetic order parameter demonstrates a $beta$ value of 0.19(3), consistent with XY anisotropy and in-plane ordering, with Ising-like interactions between layers. Further, we observe a spin-flop driven crossover to ferromagnetic order with space group of $it{C}2/it{m}$ under an applied magnetic field of $it{mu_0H}$ $approx$ 0.7 T at $it{T}$ = 2 K. Magnetic structure analysis demonstrates these magnetic states are competing at finite applied magnetic fields even below the spin-flop transition. Both the $it{d^7}$ compass model, a quantitative comparison of the specific heat of $Li_3Co_2SbO_6$, and related honeycomb cobaltates to the anisotropic Kitaev model further support proximity to a Kitaev spin liquid state. This material demonstrates the rich playground of high-spin $it{d^7}$ systems for spin liquid candidates, and complements known $it{d^5}$ Ir- and Ru-based materials.



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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.
Quantum spin liquid is a disordered magnetic state with fractional spin excitations. Its clearest example is found in an exactly solved Kitaev honeycomb model where a spin flip fractionalizes into two types of anyons, quasiparticles that are neither fermions nor bosons: a pair of gauge fluxes and a Majorana fermion. Here we demonstrate this kind of fractionalization in the Kitaev paramagnetic state of the honeycomb magnet $alpha$-RuCl$_3$. The spin-excitation gap measured by nuclear magnetic resonance consists of the predicted Majorana fermion contribution following the cube of the applied magnetic field, and a finite zero-field contribution matching the predicted size of the gauge-flux gap. The observed fractionalization into gapped anyons survives in a broad range of temperatures and magnetic fields despite inevitable non-Kitaev interactions between the spins, which are predicted to drive the system towards a gapless ground state. The gapped character of both anyons is crucial for their potential application in topological quantum computing.
We study the Kitaev-Heisenberg-$Gamma$ model with antiferromagnetic Kitaev exchanges in the strong anisotropic (toric code) limit to understand the phases and the intervening phase transitions between the gapped $Z_2$ quantum spin liquid and the spin-ordered (in the Heisenberg limit) as well as paramagnetic phases (in the pseudo-dipolar, $Gamma$, limit). We find that the paramagnetic phase obtained in the large $Gamma$ limit has no topological entanglement entropy and is proximate to a gapless critical point of a system described by an equal superposition of differently oriented stacked one-dimensional $Z_2times Z_2$ symmetry protected topological phases. Using a combination of exact diagonalization calculations and field-theoretic analysis we map out the phases and phase transitions to reveal the complete phase diagram as a function of the Heisenberg, the Kitaev, and the pseudo-dipolar interactions. Our work shows a rich plethora of unconventional phases and phase transitions and provides a comprehensive understanding of the physics of anisotropic Kitaev-Heisenberg-$Gamma$ systems along with our recent paper [Phys. Rev. B 102, 235124 (2020)] where the ferromagnetic Kitaev exchange was studied.
We show that the topological Kitaev spin liquid on the honeycomb lattice is extremely fragile against the second-neighbor Kitaev coupling $K_2$, which has recently been shown to be the dominant perturbation away from the nearest-neighbor model in iridate Na$_2$IrO$_3$, and may also play a role in $alpha$-RuCl$_3$ and Li$_2$IrO$_3$. This coupling naturally explains the zigzag ordering (without introducing unrealistically large longer-range Heisenberg exchange terms) and the special entanglement between real and spin space observed recently in Na$_2$IrO$_3$. Moreover, the minimal $K_1$-$K_2$ model that we present here holds the unique property that the classical and quantum phase diagrams and their respective order-by-disorder mechanisms are qualitatively different due to the fundamentally different symmetries of the classical and quantum counterparts.
195 - Y. Nagai , T. Jinno , Y. Yoshitake 2018
Quantum spin liquid involves fractionalized quasipariticles such as spinons and visons. They are expressed as itinerant Majorana fermions and $Z_2$ fluxes in the Kitaev model with bond-dependent exchange interactions on a honeycomb spin lattice. The observation has recently attracted attention for a candidate material $alpha$-RuCl$_3$, showing spin liquid behaviour induced by a magnetic field. Since the observable spin excitation is inherently composed of the two quasiparticles, which further admix each other by setting in the magnetic field as well as non-Kitaev interactions, their individual identification remains challenging. Here we report an emergent low-lying spin excitation through nuclear magnetic and quadrupole resonance measurements down to $sim 0.4$ K corresponding to $1/500$ of the exchange energy under the finely tuned magnetic field across the quantum critical point. We determined the critical behaviour of low-lying excitations and found evolution of two kinds of the spin gap at high fields. The two excitations exhibit repulsive magnetic field dependence, suggesting anti-crossing due to the hybridization between fractionalized quasiparticles.
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