Measurements of the magnetic Grüneisen parameter ($Γ_B$) and specific heat on the Kitaev material candidate $α$-RuCl$_3$ are used to access in-plane field- and temperature-dependence of the entropy up to 12 T and down to 1 K. No signatures corresponding to phase transitions are detected beyond the boundary of the magnetically ordered region, but only a shoulder-like anomaly in $Γ_B$, involving an entropy increment as small as $10^{-5} R\log 2$. These observations put into question the presence of a thermodynamic phase transition between the purported quantum spin liquid and the field-polarized state of $α$-RuCl$_3$. We show theoretically that at low temperatures $Γ_B$ is sensitive to crossings in the lowest excitations within gapped phases, and identify the measured shoulder-like anomaly as being of such origin. Exact diagonalization calculations demonstrate that the shoulder-like anomaly can be reproduced in extended Kitaev models that gain proximity to an additional phase at finite field without entering it. We discuss manifestations of this proximity in other measurements.
Thermodynamics of the Kitaev honeycomb magnet $α$-RuCl$_3$ is studied for different directions of in-plane magnetic field using measurements of the magnetic Grüneisen parameter $Γ_B$ 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 …
Emergent low-energy thermodynamics and universal $B/T$ scaling in $α$-RuCl$_3$
Institute of Science and Technology Austria（奥地利科学技术研究院）；Department of Physics, Stockholm University（斯德哥尔摩大学物理系）；Laboratory of Atomic and Solid State Physics, Cornell University（康奈尔大学原子与固态物理实验室）；Canadian Institute for Advanced Research（加拿大高级研究院）；National High Magnetic Field Laboratory, Florida State University（佛罗里达州立大学国家高磁场实验室）；Department of Physics, University of Toronto（多伦多大学物理系）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Institute for Theoretical Physics, Julius-Maximilians-Universität Würzburg（维尔茨堡大学理论物理研究所）；Würzburg-Dresden Cluster of Excellence ctd.qmat, Julius-Maximilians-Universität Würzburg（维尔茨堡大学维尔茨堡-德累斯顿卓越集群ctd.qmat）
Fractionalized excitations are of considerable interest in recent condensed-matter physics. Fractionalization of the spin degrees of freedom into localized and itinerant Majorana fermions are predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. As function of temperature, theory predicts a characteristic two-peak structure of the heat capacity as fingerprint of these excitations. Here we report on detailed heat-capacity experiments as function of temperature and magnetic field in high-quality single crystals of…
The pursuit of quantum spin liquid (QSL) in the Kitaev honeycomb magnets has drawn intensive attention recently. In particular, $α$-RuCl$_3$ has been widely recognized as a promising candidate for the Kitaev QSL. Although the compound exhibits an antiferromagnetic order under zero field, it is believed to be endowed with fractionalized excitations, and can be driven to the QSL phase by magnetic fields. Here, based on a realistic $K$-$J$-$Γ$-$Γ'$ model for $α$-RuCl$_3$ [1], we exploit the exponential tensor renormalization group approach to explore the phase diagram of the compound under magnet…
We present high-field electron spin resonance (ESR) studies of the honeycomb-lattice material $α$-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 $α$-RuCl$_3$. The frequency-field diagram of the lowes…
The exactly-solvable Kitaev model of two-dimensional honeycomb magnet leads to a quantum spin liquid (QSL) characterized by Majorana fermions, relevant for fault-tolerant topological quantum computations. In the high-field paramagnetic state of $α$-RuCl3, half-integer quantization of thermal Hall conductivity has been reported as a signature of edge current, but the bulk nature of this state remains elusive. Here, from high-resolution heat capacity measurements under in-plane field rotation, we find strongly angle-dependent low-energy excitations in bulk $α$-RuCl3. The excitation gap has a sex…
Material realization of the non-Abelian Kitaev spin liquid phase - an example of Ising topological order (ITO) - has been the subject of intense research in recent years. The $4d$ honeycomb Mott insulator $α$-RuCl$_3$ has emerged as a leading candidate, as it enters a field-induced magnetically disordered state where a half-integer quantized thermal Hall conductivity $κ_{xy}$ was reported. Further, a recent report of a sign change in the quantized $κ_{xy}$ across a certain crystallographic direction is strong evidence for a topological phase transition between two ITOs with opposite Chern numb…
What is the correct low-energy spin Hamiltonian description of $α$-RuCl$_3$? The material is a promising Kitaev spin liquid candidate, but is also known to order magnetically, the description of which necessitates additional interaction terms. The nature of these interactions, their magnitudes and even signs, remain an open question. In this work we systematically investigate dynamical and thermodynamic magnetic properties of proposed effective Hamiltonians. We calculate zero-temperature inelastic neutron scattering (INS) intensities using exact diagonalization, and magnetic specific heat usin…
High-resolution thermal expansion and magnetostriction measurements were performed on single crystals of $α$-RuCl$_3$ in magnetic fields applied parallel to the Ru-Ru bonds. The length changes were measured in the direction perpendicular to the honeycomb planes. Our data show clear thermodynamic characteristics for the field-induced phase transition at the critical field $μ_0H_{c1} = 7.8(2)$ T where the antiferromagnetic zigzag order is suppressed. At higher fields, a kink in the magnetostriction coefficient signals an additional phase transition around $μ_0H_{c2} \approx 11$ T. The extracted …
$α$-RuCl3 is a magnetic insulator exhibiting quantum spin liquid phases possibly found in the Kitaev honeycomb model. Much of the effort towards determining Hamiltonian parameters has focused on low magnetic field ordered phases. We study this problem in the high magnetic field limit where mean-field theory is better justified. We do so by machine-learning model parameters from over 200,000 low dimensional data points by combining available magnetization, torque, and torsion data sets. Our machine, an artificial neural network-mean-field theory (ANN-MFT) encoder, maps thermodynamic conditions …
We report magnetic, thermodynamic, thermal expansion, and on detailed optical experiments on the layered compound $α$-RuCl$_3$ focusing on the THz and sub-gap optical response across the structural phase transition from the monoclinic high-temperature to the rhombohedral low-temperature structure, where the stacking sequence of the molecular layers is changed. This type of phase transition is characteristic for a variety of tri-halides crystallizing in a layered honeycomb-type structure and so far is unique, as the low-temperature phase exhibits the higher symmetry. One motivation is to unrave…
We consider the exchange couplings present in an effective Hamiltonian of $α$-RuCl$_3$, known as the K-$Γ$ model. This material has a honeycomb lattice, and is expected to be a representative of the Kitaev materials (which can realize the 2d Kitaev model). However, the behaviour of RuCl$_3$ shows that the exchange interactions of the material are not purely Kitaev-like, especially because it has an antiferromagnetic ordering at low temperatures and under low strengths of an externally applied magnetic field. Fitting the data obtained from the measurements of the magnetotropic coefficient (the …
Recent theoretical studies have suggested that Kitaev physics and such effects as formation of a mysterious spin-liquid state can be expected not only in RuCl3 and iridates, but also in conventional $3d$ transition metal compounds. Using DC and AC magnetometry, thermodynamic and $^{23}$Na nuclear magnetic resonance measurements (NMR) we studied such a candidate material Na3Co2SbO6. A full phase diagram of Na3Co2SbO6 in a wide range of magnetic fields and temperatures is presented. The results demonstrate transformation of the antiferromagnetic structure under the external magnetic field, gradu…
A decade ago, Alexei Kitaev proposed an exactly solvable $S$ = 1/2 model on a two-dimensional honeycomb lattice, where the spins fractionalize into Majorana fermions and form a topological quantum spin liquid (QSL) in the ground state. It was soon recognized that a family of complex iridium oxides, as well as ruthenium chloride, with honeycomb structure are magnetic insulators and accommodate essential ingredients of the Kitaev model, due to the interplay of electron correlation and spin-orbit coupling. This initiated a race to materialize the Kitaev QSL and to capture the signature of Majoran…
In the Kitaev honeycomb model, the quantum spin fractionalizes into itinerant Majorana and gauge flux spontaneously upon cooling, leading to rich experimental ramifications at finite temperature and an upsurge of research interest. In this work, we employ the exponential tensor renormalization group approach to explore the Kitaev model under various perturbations, including the external fields, Heisenberg, and the off-diagonal couplings that are common in the Kitaev materials. Through large-scale manybody calculations, we find a Kitaev fractional liquid at intermediate temperature that is robu…
We investigate the thermodynamics and transient dynamics of the (unbiased) Ohmic two-state system by exploiting the equivalence of this model to the interacting resonant level model. For the thermodynamics, we show, by using the numerical renormalization group (NRG) method, how the universal specific heat and susceptibility curves evolve with increasing dissipation strength, $α$, from those of an isolated two-level system at vanishingly small dissipation strength, with the characteristic activated-like behavior in this limit, to those of the isotropic Kondo model in the limit $α\to 1^{-}$. For…
Recently, a surprising low-temperature behavior has been revealed in a two-leg ladder Ising model with trimer rungs (Weiguo Yin, arXiv:2006.08921). Motivated by these findings, we study this model from another perspective and demonstrate that the reported observations are related to a critical phenomenon in the standard Ising chain. We also discuss a related curiosity, namely, the emergence of a power-law behavior characterized by quasicritical exponents.
