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Physical Review Letters

Randomly Hopping Majorana Fermions in the Diluted Kitaev System α - Ru0.8Ir0.2Cl3

Seung-Hwan Do, Chanhyeon Lee, Takumi Kihara, Y. S. Choi, Sungwon Yoon, Kangwon Kim, Hyeonsik Cheong, Wei‐Tin Chen, F. C. Chou, Hiroyuki Nojiri, Kwang‐Yong Choi

Published Jan 31, 2020• 52 citations
Publisher

Abstract

dc and ac magnetic susceptibility, magnetization, specific heat, and Raman scattering measurements are combined to probe low-lying spin excitations in α-Ru_{1-x}Ir_{x}Cl_{3} (x≈0.2), which realizes a disordered spin liquid. At intermediate energies (ℏω>3 meV), Raman spectroscopy evidences linearly ω-dependent Majorana-like excitations, obeying Fermi statistics. This points to robustness of a Kitaev paramagnetic state under spin vacancies. At low energies below 3 meV, we observe power-law dependences and quantum-critical-like scalings of the thermodynamic quantities, implying the presence of a weakly divergent low-energy density of states. This scaling phenomenology is interpreted in terms of the random hoppings of Majorana fermions. Our results demonstrate an emergent hierarchy of spin excitations in a diluted Kitaev honeycomb system subject to spin vacancies and bond randomness.

DOI
10.1103/physrevlett.124.047204

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dc and ac magnetic susceptibility, magnetization, specific heat, and Raman scattering measurements are combined to probe low-lying spin excitations in α-Ru_{1-x}Ir_{x}Cl_{3} (x≈0.2), which realizes a disordered spin liquid. At intermediate energies (ℏω>3 meV), Raman spectroscopy evidences linearly ω-dependent Majorana-like excitations, obeying Fermi statistics. This points to robustness of a Kitaev paramagnetic state under spin vacancies. At low energies below 3 meV, we observe power-law dependences and quantum-critical-like scalings of the thermodynamic quantities, implying the presence of a weakly divergent low-energy density of states. This scaling phenomenology is interpreted in terms of the random hoppings of Majorana fermions. Our results demonstrate an emergent hierarchy of spin excitations in a diluted Kitaev honeycomb system subject to spin vacancies and bond randomness.
The 5d-electron honeycomb compound H_{3}LiIr_{2}O_{6} [K. Kitagawa et al., Nature (London) 554, 341 (2018)NATUAS0028-083610.1038/nature25482] exhibits an apparent quantum spin liquid state. In this intercalated spin-orbital compound, a remarkable pileup of low-energy states was experimentally observed in specific heat and spin relaxation. We show that a bond-disordered Kitaev model can naturally account for this phenomenon, suggesting that disorder plays an essential role in its theoretical description. In the exactly soluble Kitaev model, we obtain, via spin fractionalization, a random bipartite hopping problem of Majorana fermions in a random flux background. This has a divergent low-energy density of states of the required power-law form N(E)∝E^{-ν} with a drifting exponent which takes on the value ν≈1/2 for relatively strong bond disorder. Breaking time-reversal symmetry removes the divergence of the density of states, as does applying a magnetic field in experiment. We discuss the implication of our scenario, both for future experiments and from a broader perspective.
We investigate the properties of the Kitaev honeycomb model with both site dilution and exchange randomness. Embarking on this work, we review disorder in some strongly correlated electron systems, including spin-½ and spin-1 Heisenberg antiferromagnetic chains, two dimensional Heisenberg antiferromagnets, the cuprates and graphene. We outline some aspects of resonating valence bond phases, valence bond solids, spin liquids and quantum computation that are pertinent to an understanding of the Kitaev model. The properties of the Kitaev model without disorder are discussed and it is found to be a critical spin liquid, with algebraic correlations in two spin operators sigma^{alpha}_{i}sigma^{alpha}_{j}, where i and j,/em> are either end of a link of type alpha = x, y or z on the honeycomb lattice. The Kitaev model is exactly solvable and we show that this remains so in the presence of site dilution and exchange randomness. We find that vacancies bind a flux. In the gapped phase, a vacancy forms an effective paramagnetic moment. With two or more vacancies we describe the interaction of their effective moments and show that a finite density of vacancies leads to a divergent macroscopic susceptibility at small fields. In the gapless phase the effective moment has a susceptibility that is, to leading order at small fields, chi(h)~log(1/h). Interaction between the moments from two vacancies on opposite sublattices cuts off this divergence in susceptibility at a large but finite constant. Two vacancies on the same sublattice behave quite differently and we find the combined susceptibility is parametrically larger than that of an isolated vacancy, chi(h)sim [h(log(1/h))^{3/2}]^{-1}. We also investigate the effects of slowly varying, quenched disorder in exchange coupling. We demonstrate that this does not qualitatively affect the susceptibility but show that the heat capacity C ~ T^{2/z}, where z is a measure of the disorder and increases from one with increasing disorder strength.
Long-range entanglement in quantum spin liquids (QSLs) leads to novel low-energy excitations with fractionalized quantum numbers and (in two dimensions) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalization is their coupling to phonons. Here, we present Raman scattering results for the S=1/2S=1/2S=1/2 honeycomb iridate Cu2IrO3{\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}Cu2​IrO3​, a candidate Kitaev QSL with fractionalized Majorana fermions and Ising flux excitations. We observe anomalous low-temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum, both of which, as we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at $\ensuremath{\sim}120$ K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide evidence of spin fractionalization in Cu2IrO3{\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}Cu2​IrO3​.
A Kitaev quantum spin liquid involves fractionalized quasiparticles called itinerant Majorana fermions and localized gauge fluxes. The topological character with chiral excitations under a magnetic field is currently in an active debate. For a candidate spin liquid $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, we report low-energy spin excitations through nuclear magnetic and quadrupole resonance measurements down to temperatures three orders of magnitude lower than the exchange energy. In a field-driven disordered state, we found the evolution of two kinds of gapped spin excitations with distinct field dependences. The result is indicative of a field-induced hybridization between fractionalized quasiparticles, as inferred by the perturbation theory for the Kitaev model. The detailed field dependence of spin dynamics across the quantum critical region shows the emergence of a gapless intermediate phase between the gapped zigzag order phase and spin-disordered phases.
We investigate the properties of the Kitaev honeycomb model with both site dilution and exchange randomness. Embarking on this work, we review disorder in some strongly correlated electron systems, including spin-½ and spin-1 Heisenberg antiferromagnetic chains, two dimensional Heisenberg antiferromagnets, the cuprates and graphene. We outline some aspects of resonating valence bond phases, valence bond solids, spin liquids and quantum computation that are pertinent to an understanding of the Kitaev model. The properties of the Kitaev model without disorder are discussed and it is found to be a critical spin liquid, with algebraic correlations in two spin operators sigma^{alpha}_{i}sigma^{alpha}_{j}, where i and j are either end of a link of type alpha = x, y or z on the honeycomb lattice. The Kitaev model is exactly solvable and we show that this remains so in the presence of site dilution and exchange randomness. We find that vacancies bind a flux. In the gapped phase, a vacancy forms an effective paramagnetic moment. With two or more vacancies we describe the interaction of their effective moments and show that a finite density of vacancies leads to a divergent macroscopic susceptibility at small fields. In the gapless phase the effective moment has a susceptibility that is, to leading order at small fields, chi(h)~log(1/h). Interaction between the moments from two vacancies on opposite sublattices cuts off this divergence in susceptibility at a large but finite constant. Two vacancies on the same sublattice behave quite differently and we find the combined susceptibility is parametrically larger than that of an isolated vacancy, chi(h)sim [h(log(1/h))^{3/2}]^{-1}. We also investigate the effects of slowly varying, quenched disorder in exchange coupling. We demonstrate that this does not qualitatively affect the susceptibility but show that the heat capacity C ~ T^{2/z}, where z is a measure of the disorder and increases from one with increasing disorder strength.
We study the effects of the flux configurations on the emergent Majorana fermions in the S=12S=\frac{1}{2}S=21​ Kitaev model on a honeycomb lattice, where quantum spins are fractionalized into itinerant Majorana fermions and localized fluxes. A quantum spin liquid appears as the ground state of the Kitaev model in the flux-free sector, which has intensively been investigated so far. In this flux sector, the Majorana fermion system has linear dispersions and shows power-law behavior in the Majorana correlations. On the other hand, periodically arranged flux configurations yield low-energy excitations in the Majorana fermion system, which are distinctly different from those in the flux-free state. We find that one of the periodically arranged flux states results in the gapped Majorana dispersion and the exponential decay in the Majorana correlations. The Kitaev system with another flux configuration exhibits a semi-Dirac-type dispersion, leading to the power-law decay with a smaller power than that in the flux-free sector along symmetry axes. We also examine the effect of the randomness in the flux configurations and clarify that the Majorana density of states is filled by increasing the flux density, and power-law decay in the Majorana correlations remains. The present results could be important to control the motion of Majorana fermions, which carries the spin excitations, in the Kitaev candidate materials.