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The layered honeycomb magnet $\alpha$-RuCl$_3$ has emerged as a promising candidate for realizing a Kitaev quantum spin liquid. Previous studies have reported oscillation-like anomalies in the longitudinal thermal conductivity and half-integer quantized thermal Hall conductivity above the antiferromagnetic critical field $H_c$, generating significant interest. However, the origins of these phenomena remain contentious due to strong sample dependence. Here we re-examine the magnetothermal transport properties using recently available ultra-pure $\alpha$-RuCl$_3$ single crystals to further elucidate potential signatures of the spin liquid state. Our findings reveal that while anomalies in thermal conductivity above $H_c$ persist even in ultraclean crystals, their magnitude is significantly attenuated, contrary to the quantum oscillations hypothesis. This suggests that the anomalies are likely attributable to localized stacking faults inadvertently introduced during magnetothermal transport measurements. The thermal Hall conductivity exhibits a half-quantized plateau, albeit with a narrower width than previously reported. This observation aligns with theoretical predictions emphasizing the importance of interactions between chiral edge currents and phonons. These results indicate that structural imperfections exert a substantial influence on both the oscillation-like anomalies and quantization effects observed in magnetothermal transport measurements of $\alpha$-RuCl$_3$., Comment: 6 pages, 4 figures

Quantum spin liquids (QSLs) represent an exotic quantum many-body state characterized by the suppression of long-range magnetic order due to strong quantum fluctuations. The kagome spin-1/2 antiferromagnet (AFM) is a prime candidate for realizing QSLs, but its ground state remains an unresolved conundrum. Here we investigate the recently discovered perfect kagome AFM YCu$_3$(OH)$_{6.5}$Br$_{2.5}$ to elucidate two central enigmas surrounding the kagome AFM. Ultra-sensitive torque magnetometry experiments reveal that the intrinsic magnetic susceptibility arising from the kagome layer remains nearly temperature-independent down to exceedingly low temperatures. This observation seemingly implies the emergence of gapless fermionic spin excitations akin to Pauli paramagnetism in metals. However, most strikingly, these results stand in stark contrast to the conspicuous absence of a temperature-linear contribution to the specific heat. These findings appear irreconcilable with the widely-discussed theoretical frameworks assuming fermionic quasiparticles (QPs), instead suggesting a transition of bosonic QPs into a superfluid state with a gapless Goldstone mode. Furthermore, magnetocaloric measurements evince an entropy anomaly, constituting thermodynamic evidence that magnetic fields instigate the opening of a spin gap, driving a quantum phase transition into a 1/9 magnetization plateau state. These results shed light on the nature of the low-energy excitations in zero and strong magnetic fields, providing crucial insights into the long-standing unresolved issues of the ground state of the kagome AFM., Comment: 23 pages, 9 figures

Single atomic defects are prominent windows to look into host quantum states because collective responses from the host states emerge as localized states around the defects. Friedel oscillations and Kondo clouds in Fermi liquids are quintessential examples. However, the situation is quite different for quantum spin liquid (QSL), an exotic state of matter with fractionalized quasiparticles and topological order arising from a profound impact of quantum entanglement. Elucidating the underlying local electronic property has been challenging due to the charge neutrality of fractionalized quasiparticles and the insulating nature of QSLs. Here, using spectroscopic-imaging scanning tunneling microscopy, we report atomically resolved images of monolayer $\alpha-RuCl_3$, the most promising Kitaev QSL candidate, on metallic substrates. We find quantum interference in the insulator manifesting as incommensurate and decaying spatial oscillations of the local density of states around defects with a characteristic bias dependence. The oscillation differs from any known spatial structures in its nature and does not exist in other Mott insulators, implying it is an exotic oscillation involved with excitations unique to $\alpha-RuCl_3$. Numerical simulations suggest that the observed oscillation can be reproduced by assuming that itinerant Majorana fermions of Kitaev QSL are scattered across the Majorana Fermi surface. The oscillation provides a new approach to exploring Kitaev QSLs through the local response against defects like Friedel oscillations in metals., Comment: v2 to appear in PRX

Fermionic superfluidity with a nontrivial Cooper-pairing, beyond the conventional Bardeen-Cooper-Schrieffer state, is a captivating field of study in quantum many-body systems. In particular, the search for superconducting states with finite-momentum pairs has long been a challenge, but establishing its existence has long suffered from the lack of an appropriate probe to reveal its momentum. Recently, it has been proposed that the nonreciprocal {\cred electron} transport is the most {\cred powerful} probe for the finite-momentum pairs, {\cred because it directly couples} to the supercurrents. Here we reveal such a pairing state by the non-reciprocal transport on tricolor superlattices with strong spin-orbit coupling combined with broken inversion-symmetry consisting of atomically thin $d$-wave superconductor CeCoIn$_5$. We find that while the second-harmonic resistance exhibits a distinct dip anomaly at the low-temperature ($T$)/high-magnetic field ($H$) corner in the $HT$-plane for ${\bm H}$ applied to the antinodal direction of the $d$-wave gap, such an anomaly is absent for ${\bm H}$ along the nodal direction. By meticulously isolating extrinsic effects due to vortex dynamics, we reveal the presence of a non-reciprocal response originating from intrinsic superconducting properties characterized by finite-momentum pairs. We attribute the high-field state to the helical superconducting state, wherein the phase of the order parameter is spontaneously spatially modulated.

The layered honeycomb magnet $\alpha$-RuCl$_3$ is the most promising candidate for a Kitaev quantum spin liquid (KQSL) that can host charge-neutral Majorana fermions. Recent studies have shown significant sample dependence of thermal transport properties, which are a key probe of Majorana quasiparticles in the KQSL state, highlighting the importance of preparing high-quality single crystals of $\alpha$-RuCl$_3$. Here, we present a relatively simple and reliable method to grow high-quality single crystals of $\alpha$-RuCl$_3$. We use a two-step crystal growth method consisting of a purification process by chemical vapor transport (CVT) and a main crystal growth process by sublimation. The obtained crystals exhibit a distinct first-order structural phase transition from the monoclinic ($C2/m$) to the rhombohedral ($R\bar{3}$) structure at $\sim150$ K, which is confirmed by the nuclear quadrupole resonance spectra with much sharper widths than previously reported. The Raman spectra show the absence of defect-induced modes, supporting the good crystallinity of our samples. The jumps in the thermal expansion coefficient and specific heat at the antiferromagnetic (AFM) transition at 7.6-7.7 K are larger and sharper than those of previous samples grown by the CVT and Bridgman methods and do not show any additional AFM transitions at 10-14 K due to stacking faults. The longitudinal thermal conductivity in the AFM phase is significantly larger than previously reported, indicating a very long mean free path of heat carriers. All the results indicate that our single crystals are of superior quality with good crystallinity and few stacking faults, which provides a suitable platform for studying the Kitaev physics., Comment: 9 pages, 7 figures

The two-dimensional (2D) spin-1/2 kagome Heisenberg antiferromagnet is believed to host quantum spin liquid (QSL) states with no magnetic order, but its ground state remains largely elusive. An important outstanding question concerns the presence or absence of the 1/9 magnetization plateau, where exotic quantum states, including topological ones, are expected to emerge. Here we report the magnetization of a recently discovered kagome QSL candidate YCu$_3$(OH)$_{6.5}$Br$_{2.5}$ up to 57 T. Above 50 T, a clear magnetization plateau at 1/3 of the saturation moment of Cu$^{2+}$ ions is observed, supporting that this material provides an ideal platform for the kagome Heisenberg antiferromagnet. Remarkably, we found another magnetization plateau around 20 T, which is attributed to the 1/9 plateau. The temperature dependence of this plateau reveals the distinct spin gap, whose magnitude estimated by the plateau width is approximately 10% of the exchange interaction. The observation of 1/9 and 1/3 plateaus highlights the emergence of novel states in quantum spin systems., Comment: 5 pages, 4 figures

The quest for fascinating quantum states arising from the interplay between correlation, frustration, and topology is at the forefront of condensed-matter physics. Recently discovered nonmagnetic kagome metals $A$V${_3}$Sb${_5}$ ($A=$ K, Cs, Rb) with charge density wave (CDW) and superconducting instabilities may host such exotic states. Here we report that an odd electronic nematic state emerges above the CDW transition temperature ($T_{\rm CDW}=94$ K) in CsV${_3}$Sb${_5}$. High-resolution torque measurements reveal a distinct twofold in-plane magnetic anisotropy that breaks the crystal rotational symmetry below $T^*\approx130$ K. However, no relevant anomalies are detected in the elastoresistance data near $T^*$, which excludes the even-parity ferro-orbital nematicity often found in other superconductors. Moreover, in the temperature range between $T_{\rm CDW}$ and $T^*$, conical rotations of magnetic field yield a distinct first-order phase transition, indicative of time-reversal symmetry breaking. These results provide thermodynamic evidence for the emergence of an odd-parity nematic order, implying that an exotic loop-current state precedes the CDW in CsV$_3$Sb$_5$., Comment: A revised manuscript will appear in Nature Physics

Spin-triplet superconductors provide an ideal platform for realizing topological superconductivity with emergent Majorana quasiparticles. The promising candidate is the recently discovered superconductor UTe$ _2$, but the symmetry of the superconducting order parameter remains highly controversial. Here we determine the superconducting gap structure by the thermal conductivity of ultra-clean UTe$ _2$ single crystals. We find that the $a$ axis thermal conductivity divided by temperature $\kappa/T$ in zero-temperature limit is vanishingly small for both magnetic fields $\mathbf{H}||a$ and $\mathbf{H}||c$ axes up to $H/H_{c2}\sim 0.2$, demonstrating the absence of any types of nodes around $a$ axis contrary to the previous belief. The present results, combined with the reduction of the NMR Knight shift in the superconducting state, indicate that the superconducting order parameter belongs to the isotropic $A_u$ representation with a fully gapped pairing state, analogous to the B phase of superfluid $ ^3$He. These findings reveal that UTe$ _2$ is likely to be a long-sought three-dimensional (3D) strong topological superconductor characterized by a 3D winding number, hosting helical Majorana surface states on any crystal plane., Comment: 10pages, 4 figures

The field-induced quantum disordered state of layered honeycomb magnet $\alpha$-RuCl$_3$ is a prime candidate for Kitaev spin liquids hosting Majorana fermions and non-Abelian anyons. Recent observations of anomalous planar thermal Hall effect demonstrate a topological edge mode, but whether it originates from Majorana fermions or bosonic magnons remains controversial. Here we distinguish these origins from low-temperature measurements of high-resolution specific heat and thermal Hall conductivity with rotating in-plane fields. In the honeycomb bond direction, a distinct closure of the low-energy bulk gap is observed concomitantly with the sign reversal of the Hall effect. General discussions of topological bands show that this is the hallmark of an angle-rotation-induced topological transition of fermions, providing conclusive evidence for the Majorana-fermion origin of the thermal Hall effect in $\alpha$-RuCl$_3$., Comment: 21 pages, 7 figures

We report an {\it in-situ} scanning tunneling microscopy study of atomically thin films of CeCoIn$_5$, a $d$-wave heavy-fermion superconductor. Both hybridization and superconducting gaps are observed even in monolayer CeCoIn$_5$, providing direct evidence of superconductivity of heavy quasiparticles mediated by purely two-dimensional bosonic excitations. In these atomically thin films, $T_c$ is suppressed to nearly half of the bulk, but is similar to CeCoIn$_5$/YbCoIn$_5$ superlattices containing CeCoIn$_5$ layers with the same thickness as the thin films. Remarkably, the out-of-plane upper critical field $\mu_0H_{c2\perp}$ at zero temperature is largely enhanced from those of bulk and superlattices. The enhanced $H_{c2\perp}$ well exceeds the Pauli and bulk orbital limits, suggesting the possible emergence of unusual superconductivity with parity mixing caused by the inversion symmetry breaking.

The Kitaev quantum spin liquid (QSL) on the two-dimensional honeycomb lattice epitomizes an entangled topological state, where the spins fractionalize into Majorana fermions. This state has aroused tremendous interest because it harbors non-Abelian anyon excitations. The half-integer quantized thermal Hall (HIQTH) conductance observed in $\alpha$-RuCl$_3$ is a key signature of these excitations. However, the fate of this topologically nontrivial state at intense fields remains largely elusive. Here, we report the thermal conductivity $\kappa$ and specific heat $C$ of $\alpha$-RuCl$_3$ with in-plane magnetic fields $H$. For the field direction perpendicular to the Ru-Ru bond, where the HIQTH effect is observed, we find a discontinuous jump in $\kappa(H)$ and a peak anomaly in $C(H)$ at $\mu_0H^*\approx11$\,T, evidencing a weak first-order phase transition. Remarkably, the HIQTH effect vanishes close to $H^*$. Furthermore, we find that the spin-fractionalization feature is retained well above $H^\ast$. These imply the emergence of the phase transition that separates two QSL phases with distinct topological properties., Comment: 6 pages, 4 figures

Despite extensive investigations, a topological state that hosts Majorana edge modes in the magnetic field-induced quantum disordered state of the Kitaev candidate material $\alpha$-RuCl$_3$ has been hotly debated. To gain more insight into this issue, we measured the thermal Hall conductivity $\kappa_{xy}$ of various samples grown by the Bridgman method. The results show that the half-integer quantum thermal Hall effect is intimately related to the magnitude of longitudinal thermal conductivity and the N\'{e}el temperature at zero field, both of which are sample dependent. Samples exhibiting the half-integer quantum thermal Hall effect have larger zero-field thermal conductivity values than a threshold value, implying that a long mean free path of heat carriers is an important prerequisite. In addition, we find that samples with a higher N\'{e}el temperature exhibit a higher magnetic field at which quantization starts to occur. These results indicate that the quantization phenomenon is significantly affected by the impurity scatterings and the non-Kitaev interactions., Comment: 6 pages, 5 figures, final version

The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, characterized by Cooper pairs condensed at finite momentum, has been a long-sought state that remains unresolved in many classes of fermionic systems, including superconductors and ultracold atoms. A fascinating aspect of the FFLO state is the emergence of periodic nodal planes in real space, but its observation is still lacking. Here we investigate the superconducting order parameter at high magnetic fields $H$ applied perpendicular to the $ab$ plane in a high-purity single crystal of FeSe. The heat capacity and magnetic torque provide thermodynamic evidence for a distinct superconducting phase at the low-temperature/high-field corner of the phase diagram. Despite the bulk superconductivity, spectroscopic-imaging scanning tunneling microscopy performed on the same crystal demonstrates that the order parameter vanishes at the surface upon entering the high-field phase. These results provide the first demonstration of a pinned planar node perpendicular to $H$, which is consistent with a putative FFLO state., Comment: 11 pages, 9 figures, including Supplemental Material. Accepted for publication in Phys. Rev. Lett

In contrast to electron (fermion) systems, topological phases of charge neutral bosons have been poorly understood despite recent extensive research on insulating magnets. The most important unresolved issue is how the inevitable inter-bosonic interactions influence the topological properties. It has been proposed that the quantum magnet SrCu$_2$(BO$_3$)$_2$ with an exact ground state serves as an ideal platform for this investigation, as the system is expected to be a magnetic analogue of a Chern insulator with electrons replaced by bosonic magnetic excitations (triplons). Here, in order to examine topologically protected triplon chiral edge modes in SrCu$_2$(BO$_3$)$_2$, we measured and calculated the thermal Hall conductivity $\kappa_{xy}$. Our calculations show that the sign of $\kappa_{xy}$ is negative, which is opposite to the previous calculations, and its magnitude is 2$\pi$ times smaller. No discernible $\kappa_{xy}$ was observed, which is at most 20-30% of our calculations if present. This implies that even relatively weak inter-particle interactions seriously influence the topological transport properties at finite temperatures. These demonstrate that, in contrast to fermionic cases, the picture of non-interacting topological quasi-particles cannot be naively applied to bosonic systems, calling special attention to the interpretation of the topological bosonic excitations reported for various insulating magnets., Comment: 11 pages, 11 figures

Kondo insulators have recently aroused great interest because they are promising materials that host a topological insulator state caused by the strong electron interactions. Moreover, recent observations of the quantum oscillations in the insulating state of Kondo insulators have come as a great surprise. Here, to investigate the surface electronic state of a prototype Kondo insulator YbB$_{12}$, we measured transport properties of single crystals and microstructures. In all samples, the temperature dependence of the electrical resistivity is insulating at high temperatures and the resistivity exhibits a plateau at low temperatures. The magnitude of the plateau value decreases with reducing sample thickness, which is quantitatively consistent with the surface electronic conduction in the bulk insulating YbB$_{12}$. Moreover, the magnetoresistance of the microstructures exhibits a weak-antilocalization effect at low field. These results are consistent with the presence of topologically protected surface state, suggesting that YbB$_{12}$ is a candidate material of the topological Kondo insulator. The high field resistivity measurements up to $\mu_0H$ = 50 T of the microstructures provide supporting evidence that the quantum oscillations of the resistivity in YbB$_{12}$ occurs in the insulating bulk., Comment: This is the version of the article before peer review or editing, as submitted by an author to Journal of Physics D: Applied Physics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at 10.1088/1361-6463/ac10d9

Despite tremendous investigations, a quantum spin liquid state realized in spin-1/2 kagome Heisenberg antiferromagnet remains largely elusive. In herbertsmithite ZnCu$_3$(OH)$_6$Cl$_2$, a quantum spin liquid candidate on the perfect kagome lattice, precisely characterizing the intrinsic physics of the kagome layers is extremely challenging due to the presence of interlayer Cu/Zn antisite disorder within its crystal structure. Here we measured the specific heat and thermal conductivity of single crystal herbertsmithite in magnetic fields with high resolution. Our results are highlighted by the excellent scaling collapse of the intrinsic magnetic specific heat contribution arising from the kagome layers as a function of $T/H$ (temperature/magnetic field). In addition, no residual linear term in the thermal conductivity $\kappa/T(T\rightarrow 0)$ is observed in zero and applied magnetic fields, indicating the absence of itinerant gapless excitations. These results suggest a new picture for a quantum spin liquid state of the kagome layers of herbertsmithite, wherein localized orphan spins arise and interact with random exchanges in conjunction with a non-itinerant quantum spin liquid.

Materials where localized magnetic moments are coupled to itinerant electrons, the so-called Kondo lattice materials, provide a very rich backdrop for strong electron correlations. They are known to realize many exotic phenomena, including unconventional superconductivity, strange metals, and correlated topological phases of matter. Here, we report what appears to be electron fractionalization in insulating Kondo lattice material YbIr$_3$Si$_7$, with emergent neutral excitations that carry heat but not electric current and contribute to metal-like specific heat. We show that these neutral particles change their properties as the material undergoes a transformation between two antiferromagnetic phases in an applied magnetic field. In the low-field AF-I phase, we find that the low temperature linear specific heat coefficient $\gamma$ and the residual linear term in the thermal conductivity $\kappa/T(T\rightarrow 0)$ are finite, demonstrating itinerant gapless excitations. These results, along with a spectacular violation of the Wiedemann-Franz law, directly indicate that YbIr$_3$Si$_7$ is a charge insulator but a thermal metal. Nuclear magnetic resonance spectrum reveals a spin-flop transition to a high field AF-II phase. Near the transition field, $\gamma$ is significantly enhanced. Most surprisingly, inside the AF-II phase, $\kappa/T$ exhibits a sharp drop below $\sim300$ mK, indicating either opening of a tiny gap or a linearly vanishing density of states. This finding demonstrates a transition from a thermal metal into an insulator/semimetal driven by the spin-flop magnetic transition. These results suggest that spin degrees of freedom directly couple to the neutral fermions, whose emergent Fermi surface undergoes a field-driven instability at low temperatures., Comment: 10 pages, 8 figures

An anapole state that breaks inversion and time reversal symmetries with preserving translation symmetry of underlying lattice has aroused great interest as a new quantum state, but only a few candidate materials have been reported. Recently, in a spin-orbit coupled Mott insulator \SIR, the emergence of a possible hidden order phase with broken inversion symmetry has been suggested at $T_{\Omega}$ above the N\'{e}el temperature by optical second harmonic generation measurements. Moreover, polarized neutron diffraction measurements revealed the broken time reversal symmetry below $T_{\Omega}$, which was supported by subsequent muon spin relaxation experiments. However, the nature of this mysterious phase remains largely elusive. Here, we investigate the hidden order phase through the combined measurements of the in-plane magnetic anisotropy with exceptionally high-precision magnetic torque and the nematic susceptibility with elastoresistance. A distinct two-fold in-plane magnetic anisotropy along the [110] Ir-O-Ir bond direction sets in below $\sim T_{\Omega}$, providing thermodynamic evidence for a nematic phase transition with broken $C_4$ rotational symmetry. However, in contrast to the even-parity nematic transition reported in other correlated electron systems, the nematic susceptibility exhibits no divergent behavior towards $T_{\Omega}$. These results provide bulk evidence for an odd-parity order parameter with broken rotational symmetry in the hidden order state. We discuss the hidden order in terms of an anapole state, in which polar toroidal moment is induced by two current loops in each IrO$_6$ octahedron of opposite chirality. Contrary to the simplest loop-current pattern previously suggested, the present results are consistent with a pattern in which the intra-unit cell loop-current flows along only one of the diagonal directions in the IrO$_4$ square., Comment: 11 pages, 10 figures

EtMe$_3$Sb[Pd(dmit)$_2$]$_2$, an organic Mott insulator with nearly isotropic triangular lattice, is a candidate material for a quantum spin liquid, in which the zero-point fluctuations do not allow the spins to order. The itinerant gapless excitations inferred from the thermal transport measurements in this system have been a hotly debated issue recently. While the presence of a finite linear residual thermal conductivity, $\kappa_0/T \equiv \kappa/T (T \rightarrow 0)$, has been shown [M. Yamashita {\it et al.} Science {\bf 328}, 1246 (2010)], recent experiments [P. Bourgeois-Hope {\it et al.}, Phys. Rev. X {\bf 9}, 041051 (2019); J. M. Ni {\it et al.}, Phys. Rev. Lett. {\bf 123}, 247204 (2019)] have reported the absence of $\kappa_0/T$. Here we show that the low-temperature thermal conductivity strongly depends on the cooling process of the sample. When cooling down very slowly, a sizable $\kappa_0/T$ is observed. In contrast, when cooling down rapidly, $\kappa_0/T$ vanishes and, in addition, the phonon thermal conductivity is strongly suppressed. These results suggest that possible random scatterers introduced during the cooling process are responsible for the apparent discrepancy of the thermal conductivity data in this organic system. The present results provide evidence that the true ground state of EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ is likely to be a quantum spin liquid with itinerant gapless excitations., Comment: 4 pages, 2 figures; (v2) minor revisions, accepted to PRB Rapid Communication

Heat transport mediated by Majorana edge modes in a magnetic insulator leads to a half-integer thermal quantum Hall conductance, which has recently been reported for the two-dimensional honeycomb material $\alpha$-RuCl$_3$. While the conventional electronic Hall effect requires a perpendicular magnetic field, we find that this is not the case in $\alpha$-RuCl$_3$. Strikingly, the thermal Hall plateau appears even for a magnetic field with no out-of-plane components. The field-angular variation of the quantized thermal Hall conductance has the same sign structure of the topological Chern number, which is either $\pm$1, as the Majorana band structure of the pure Kitaev spin liquid. This observation of a half-integer anomalous thermal Hall effect firmly establishes that the Kitaev interaction is primarily responsible and that the non-Abelian topological order associated with fractionalization of the local magnetic moments persists even in the presence of non-Kitaev interactions in $\alpha$-RuCl$_3$., Comment: 14 pages, 4 figures

A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A long-standing open problem, which is a key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T-TaS$_2$ is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted and electron irradiated crystals of 1T-TaS$_2$. In pure 1T-TaS$_2$, the linear temperature term of the heat capacity $\gamma T$ and the finite residual linear term of the thermal conductivity in the zero-temperature limit $\kappa_{0}/T\equiv\kappa/T(T\rightarrow0)$ are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances $\kappa_0/T$, it strongly suppresses $\gamma$. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T-Ta(S$_{1-x}$Se$_x$)$_2$ leads to vanishing of $\kappa_0/T$, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. Electron irradiation in pure 1T-TaS$_2$ largely enhances $\gamma$ and changes the scaling function dramatically, suggesting a possible new state of spin liquid., Comment: 10 pages, 9 figures. arXiv admin note: text overlap with arXiv:1803.06100

Quantum oscillations (QOs) in transport and thermodynamic parameters at high magnetic fields are an unambiguous signature of the Fermi surface, the defining characteristic of a metal. Therefore, recent observations of QOs in insulating SmB$_6$ and YbB$_{12}$, in particular the QOs of the resistivity $\rho_{xx}$ in YbB$_{12}$, have been a big surprise, pointing to the formation of a novel state of quantum matter. Despite the large charge gap inferred from the insulating behaviour of $\rho_{xx}$, these compounds seemingly host a Fermi surface at high magnetic fields. However, the nature of the ground state in zero field has been little explored. Here we report the use of low-temperature heat-transport measurements to discover gapless, itinerant, charge-neutral excitations in the ground state of YbB$_{12}$. At zero field, despite $\rho_{xx}$ being far larger than that of conventional metals, a sizable linear temperature dependent term in the thermal conductivity is clearly resolved in the zero-temperature limit ($\kappa_{xx}/T(T\rightarrow0)=\kappa_{xx}^0/T\neq0$). Such a residual $\kappa_{xx}^0/T$ term at zero field, which is absent in SmB$_6$, leads to a spectacular violation of the Wiedemann-Franz law: the Lorenz ratio $L=\kappa_{xx}\rho_{xx}/T$ is $10^{4}$-$10^{5}$ times larger than that expected in conventional metals. These data indicate that YbB$_{12}$ is a charge insulator but a thermal metal, suggesting the presence of itinerant neutral fermions. Remarkably, more insulating crystals with larger activation energies exhibit a larger amplitude of the resistive QOs as well as a larger $\kappa_{xx}^0/T$, in stark contrast to conventional metals. Moreover, we find that these fermions couple to magnetic field, despite their charge neutrality. Our findings expose novel gapless and highly itinerant, charge-neutral quasiparticles in this unconventional quantum state., Comment: 7 pages, 4 figures. This is the original submitted version. Final version is accepted for publication in Nature Physics

In metals, orbital motions of conduction electrons on the Fermi surface are quantized in magnetic fields, which is manifested by quantum oscillations in electrical resistivity. This Landau quantization is generally absent in insulators. Here we report a notable exception in an insulator, ytterbium dodecaboride (YbB12). Despite much larger than that of metals, the resistivity of YbB12 exhibits profound quantum oscillations. This unconventional oscillation is shown to arise from the insulating bulk, yet the temperature dependence of their amplitude follows the conventional Fermi liquid theory of metals. The large effective masses indicate the presence of Fermi surface consisting of strongly correlated electrons. Our result reveals a mysterious bipartite ground state of YbB12: it is both a charge insulator and a strongly correlated metal., Comment: This is the original submitted version

To study the mutual interaction between unconventional superconductivity and magnetic order through an interface, we fabricate Kondo superlattices consisting of alternating layers of heavy-fermion superconductor CeCoIn$_5$ and antiferromagnetic (AFM) heavy-fermion metal CeIn$_3$. The strength of the AFM fluctuations is tuned by applying hydrostatic pressure to CeCoIn$_5(m)$/CeIn$_3(n)$ superlattices with $m$ and $n$ unit-cell-thick layers of CeCoIn$_5$ and CeIn$_3$, respectively. Superconductivity in CeCoIn$_5$ and AFM order in CeIn$_3$ coexist in spatially separated layers. At ambient pressure, N\'{e}el temperature $T_N$ of the CeIn$_3$ block layers (BLs) of CeCoIn$_5$(7)/CeIn$_3(n)$ shows little dependence on $n$, in contrast to CeIn$_3(n)$/LaIn$_3$(4) superlattices where $T_N$ is strongly suppressed with decreasing $n$. This suggests that each CeIn$_3$ BL is magnetically coupled by the RKKY interaction through the adjacent CeCoIn$_5$ BL and a 3D magnetic state is formed. With applying pressure to CeCoIn$_5$(7)/CeIn$_3$(13), $T_N$ of the CeIn$_3$ BLs is suppressed up to 2.4 GPa, showing a similar pressure dependence as CeIn$_3$ single crystals. An analysis of upper critical field reveals that the superconductivity in the CeCoIn$_5$ BLs is barely influenced by the AFM fluctuations in the CeIn$_3$ BLs, even when the CeIn$_3$ BLs are in the vicinity of the AFM quantum critical point. This is in stark contrast to CeCoIn$_5$/CeRhIn$_5$ superlattice where the superconductivity in the CeCoIn$_5$ BLs is profoundly affected by AFM fluctuations in the CeRhIn$_5$ BLs. The present results show that although AFM fluctuations are injected into the CeCoIn$_5$ BLs from the CeIn$_3$ BLs through the interface, they barely affect the force which binds superconducting electron pairs. These results demonstrate that 2D AFM fluctuations are essentially important for the pairing interactions in CeCoIn$_5$., Comment: 8 pages, 9 figures

The quantum Hall effect (QHE) in two-dimensional (2D) electron gases, which is one of the most striking phenomena in condensed matter physics, involves the topologically protected dissipationless charge current flow along the edges of the sample. Integer or fractional electrical conductance are measured in units of $e^2/2\pi\hbar$, which is associated with edge currents of electrons or quasiparticles with fractional charges, respectively. Here we discover a novel type of quantization of the Hall effect in an insulating 2D quantum magnet. In $\alpha$-RuCl$_3$ with dominant Kitaev interaction on 2D honeycomb lattice, the application of a parallel magnetic field destroys the long-range magnetic order, leading to a field-induced quantum spin liquid (QSL) ground state with massive entanglement of local spins. In the low-temperature regime of the QSL state, we report that the 2D thermal Hall conductance $\kappa_{xy}^{2D}$ reaches a quantum plateau as a function of applied magnetic field. $\kappa_{xy}^{2D}/T$ attains a quantization value of $(\pi/12)(k_B^2/\hbar)$, which is exactly half of $\kappa_{xy}^{2D}/T$ in the integer QHE. This half-integer thermal Hall conductance observed in a bulk material is a direct signature of topologically protected chiral edge currents of charge neutral Majorana fermions, particles that are their own antiparticles, which possess half degrees of freedom of conventional fermions. These signatures demonstrate the fractionalization of spins into itinerant Majorana fermions and $Z_2$ fluxes predicted in a Kitaev QSL. Above a critical magnetic field, the quantization disappears and $\kappa_{xy}^{2D}/T$ goes to zero rapidly, indicating a topological quantum phase transition between the states with and without chiral Majorana edge modes. Emergent Majorana fermions in a quantum magnet are expected to have a major impact on strongly correlated topological quantum matter., Comment: 7 pages, 8 figures. Submitted version

The pseudogap phenomenon in cuprates is the most mysterious puzzle in the research of high-temperature superconductivity. In particular, whether the pseudogap is associated with a crossover or phase transition has been a long-standing controversial issue. The tetragonal cuprate HgBa$_2$CuO$_{4+\delta}$, with only one CuO$_2$ layer per primitive cell, is an ideal system to tackle this puzzle. Here, we measure the anisotropy of magnetic susceptibility within the CuO$_2$ plane with exceptionally high-precision magnetic torque experiments. Our key finding is that a distinct two-fold in-plane anisotropy sets in below the pseudogap temperature $T^*$, which provides thermodynamic evidence for a nematic phase transition with broken four-fold symmetry. Most surprisingly, the nematic director orients along the diagonal direction of the CuO$_2$ square lattice, in sharp contrast to the bond nematicity reported in various iron-based superconductors and double-layer YBa$_2$Cu$_3$O$_{6+\delta}$, where the anisotropy axis is along the Fe-Fe and Cu-O-Cu directions, respectively. Another remarkable feature is that the enhancement of the diagonal nematicity with decreasing temperature is suppressed around the temperature at which short-range charge-density-wave (CDW) formation occurs. This is in stark contrast to YBa$_2$Cu$_3$O$_{6+\delta}$, where the bond nematicity is not influenced by the CDW. Our result suggests a competing relationship between diagonal nematic and CDW order in HgBa$_2$CuO$_{4+\delta}$., Comment: 7 pages, 8 figures

To reveal the nature of elementary excitations in a quantum spin liquid (QSL), we measured low temperature thermal conductivity and specific heat of 1T-TaS$_2$, a QSL candidate material with frustrated triangular lattice of spin-1/2. The nonzero temperature linear specific heat coefficient $\gamma$ and the finite residual linear term of the thermal conductivity in the zero temperature limit $\kappa_0/T=\kappa/T(T\rightarrow 0)$ are clearly resolved. This demonstrates the presence of highly mobile gapless excitations, which is consistent with fractionalized spinon excitations that form a Fermi surface. Remarkably, an external magnetic field strongly suppresses $\gamma$, whereas it enhances $\kappa_0/T$. This unusual contrasting behavior in the field dependence of specific heat and thermal conductivity can be accounted for by the presence of two types of gapless excitations with itinerant and localized characters, as recently predicted theoretically (I. Kimchi et al., arXiv:1803.00013 (2018)). This unique feature of 1T-TaS$_2$ provides new insights into the influence of quenched disorder on the QSL., Comment: 6 pages, 4 figures

Quantum spin liquid (QSL) is an exotic quantum phase of matter whose ground state is quantum-mechanically entangled without any magnetic ordering. A central issue concerns emergent excitations that characterize QSLs, which are hypothetically associated with quasiparticle fractionalization and topological order. Here we report highly unusual heat conduction generated by the spin degrees of freedom in a QSL state of the pyrochlore magnet Pr$_2$Zr$_2$O$_7$, which hosts spin-ice correlations with strong quantum fluctuations. The thermal conductivity in high temperature regime exhibits a two-gap behavior, which is consistent with the gapped excitations of magnetic ($M$-) and electric monopoles ($E$-particles). At very low temperatures below 200\,mK, the thermal conductivity unexpectedly shows a dramatic enhancement, which well exceeds purely phononic conductivity, demonstrating the presence of highly mobile spin excitations. This new type of excitations can be attributed to emergent photons ($\nu$-particle), coherent gapless spin excitations in a spin-ice manifold., Comment: 5 pages, 6 figures

Unconventional superconductivity and magnetism are intertwined on a microscopic level in a wide class of materials. A new approach to this most fundamental and hotly debated issue focuses on the role of interactions between superconducting electrons and bosonic fluctuations at the interface between adjacent layers in heterostructures. Here we fabricate hybrid superlattices consisting of alternating atomic layers of heavy-fermion superconductor CeCoIn$_5$ and antiferromagnetic (AFM) metal CeRhIn$_5$, in which the AFM order can be suppressed by applying pressure. We find that the superconducting and AFM states coexist in spatially separated layers, but their mutual coupling via the interface significantly modifies the superconducting properties. An analysis of upper critical fields reveals that near the critical pressure where AFM order vanishes, the force binding superconducting electron-pairs acquires an extremely strong-coupling nature. This demonstrates that superconducting pairing can be tuned non-trivially by magnetic fluctuations (paramagnons) injected through the interface, leading to maximization of the pairing interaction., Comment: 8 pages, 9 figures

In the quest for exotic superconducting pairing states, the Rashba effect, which lifts the electron-spin degeneracy as a consequence of strong spin-orbit interaction (SOI) under broken inversion symmetry, has attracted considerable interest. Here, to introduce the Rashba effect into two-dimensional (2D) strongly correlated electron systems, we fabricate non-centrosymmetric (tricolor) superlattices composed of three kinds of $f$-electron compounds with atomic thickness; $d$-wave heavy fermion superconductor CeCoIn$_5$ sandwiched by two different nonmagnetic metals, YbCoIn$_5$ and YbRhIn$_5$. We find that the Rashba SOI induced global inversion symmetry breaking in these tricolor Kondo superlattices leads to profound changes in the superconducting properties of CeCoIn$_5$, which are revealed by unusual temperature and angular dependences of upper critical fields that are in marked contrast with the bulk CeCoIn$_5$ single crystals. We demonstrate that the Rashba effect incorporated into 2D CeCoIn$_5$ block layers is largely tunable by changing the layer thickness. Moreover, the temperature dependence of in-plane upper critical field exhibits an anomalous upturn at low temperatures, which is attributed to a possible emergence of a helical or stripe superconducting phase. Our results demonstrate that the tricolor Kondo superlattices provide a new playground for exploring exotic superconducting states in the strongly correlated 2D electron systems with the Rashba effect., Comment: 11 pages, 6 figures

The Kitaev quantum spin liquid displays the fractionalization of quantum spins into Majorana fermions. The emergent Majorana edge current is predicted to manifest itself in the form of a finite thermal Hall effect, a feature commonly discussed in topological superconductors. Here we report on thermal Hall conductivity $\kappa_{xy}$ measurements in $\alpha$-RuCl$_3$, a candidate Kitaev magnet with the two-dimensional honeycomb lattice. In a spin-liquid (Kitaev paramagnetic) state below the temperature characterized by the Kitaev interaction $J_K/k_B \sim 80$ K, positive $\kappa_{xy}$ develops gradually upon cooling, demonstrating the presence of highly unusual itinerant excitations. Although the zero-temperature property is masked by the magnetic ordering at $T_N=7$ K, the sign, magnitude, and $T$-dependence of $\kappa_{xy}/T$ at intermediate temperatures follows the predicted trend of the itinerant Majorana excitations., Comment: 6 pages, 4 figures

A central issue in the quest to understand the superconductivity in cuprates is the nature and origin of the pseudogap state, which harbours anomalous electronic states such as Fermi arc, charge density wave (CDW), and $d$-wave superconductivity. A fundamentally important, but long-standing controversial problem has been whether the pseudogap state is a distinct thermodynamic phase characterized by broken symmetries below the onset temperature $T^*$. Electronic nematicity, a fourfold ($C_4$) rotational symmetry breaking, has emerged as a key feature inside the pseudogap regime, but the presence or absence of a nematic phase transition and its relationship to the pseudogap remain unresolved. Here we report thermodynamic measurements of magnetic torque in the underdoped regime of orthorhombic YBa$_2$Cu$_3$O$_y$ with a field rotating in the CuO$_2$ plane, which allow us to quantify magnetic anisotropy with exceptionally high precision. Upon entering the pseudogap regime, the in-plane anisotropy of magnetic susceptibility increases after exhibiting a distinct kink at $T^*$. Our doping dependence analysis reveals that this anisotropy is preserved below $T^*$ even in the limit where the effect of orthorhombicity is eliminated. In addition, the excess in-plane anisotropy data show a remarkable scaling behaviour with respect to $T/T^*$ in a wide doping range. These results provide thermodynamic evidence that the pseudogap onset is associated with a second-order nematic phase transition, which is distinct from the CDW transition that accompanies translational symmetry breaking. This suggests that nematic fluctuations near the pseudogap phase boundary have a potential link to the strange metallic behaviour in the normal state, out of which high-$T_c$ superconductivity emerges., Comment: 6 pages, 4 figures. An updated manuscript with SI will appear in Nature Physics

FeSe has a unique ground state in which superconductivity coexists with a nematic order without long-range magnetic ordering at ambient pressure. Here, to study how the pairing interaction evolves with nematicity, we measured the thermal conductivity and specific heat of FeSe$_{1-x}$S$_x$, where the nematicity is suppressed by isoelectronic sulfur substitution. We find that in the whole nematic ($0\leq x \leq 0.17$) and tetragonal ($x=0.20$) regimes, the application of small magnetic field causes a steep increase of both quantities. This indicates the existence of deep minima or line nodes in the superconducting gap function, implying that the pairing interaction is significantly anisotropic in both the nematic and the tetragonal regimes. Moreover, the present results indicate that the position of gap minima/nodes in the tetragonal regime appears to be essentially different from that in the nematic regime. These results place an important constraint on current theories., Comment: 6 pages, 4 figures

A key aspect of unconventional pairing by the antiferromagnetic spin-fluctuation mechanism is that the superconducting energy gap must have opposite sign on different parts of the Fermi surface. Recent observations of non-nodal gap structure in the heavy-fermion superconductor CeCu$_2$Si$_2$ were then very surprising, given that this material has long been considered a prototypical example of a superconductor where the Cooper pairing is magnetically mediated. Here we present a study of the effect of controlled point defects, introduced by electron irradiation, on the temperature-dependent magnetic penetration depth $\lambda(T)$ in CeCu$_2$Si$_2$. We find that the fully-gapped state is robust against disorder, demonstrating that low-energy bound states, expected for sign-changing gap structures, are not induced by nonmagnetic impurities. This provides bulk evidence for $s_{++}$-wave superconductivity without sign reversal., Comment: 5 pages, 4 figures + Supplemental Material (1 page, 1 figure). Will appear in Phys. Rev. Lett

In exotic superconductors including high-$T_c$ copper-oxides, the interactions mediating electron Cooper-pairing are widely considered to have a magnetic rather than the conventional electron-phonon origin. Interest in such exotic pairing was initiated by the 1979 discovery of heavy-fermion superconductivity in CeCu$_2$Si$_2$, which exhibits strong antiferromagnetic fluctuations. A hallmark of unconventional pairing by anisotropic repulsive interactions is that the superconducting energy gap changes sign as a function of the electron momentum, often leading to nodes where the gap goes to zero. Here, we report low-temperature specific heat, thermal conductivity and magnetic penetration depth measurements in CeCu$_2$Si$_2$, demonstrating the absence of gap nodes at any point on the Fermi surface. Moreover, electron-irradiation experiments reveal that the superconductivity survives even when the electron mean free path becomes substantially shorter than the superconducting coherence length. This indicates that superconductivity is robust against impurities, implying that there is no sign change in the gap function. These results show that, contrary to long-standing belief, heavy electrons with extremely strong Coulomb repulsions can condense into a fully-gapped s-wave superconducting state, which has an on-site attractive pairing interaction., Comment: 8 pages, 5 figures + Supplement (3 pages, 5 figures)

The effects of reduced dimensions and the interfaces on antiferromagnetic quantum criticality are studied in epitaxial Kondo superlattices, with alternating $n$ layers of heavy-fermion antiferromagnet CeRhIn$_5$ and 7 layers of normal metal YbRhIn$_5$. As $n$ is reduced, the Kondo coherence temperature is suppressed due to the reduction of effective Kondo screening. The N\'{e}el temperature is gradually suppressed as $n$ decreases and the quasiparticle mass is strongly enhanced, implying dimensional control toward quantum criticality. Magnetotransport measurements reveal that a quantum critical point is reached for $n=3$ superlattice by applying small magnetic fields. Remarkably, the anisotropy of the quantum critical field is opposite to the expectations from the magnetic susceptibility in bulk CeRhIn$_5$, suggesting that the Rashba spin-orbit interaction arising from the inversion symmetry breaking at the interface plays a key role for tuning the quantum criticality in the two-dimensional Kondo lattice., Comment: Main text: 5 pages, 4 figures; Supplemental material:6 pages, 3 figures. Accepted for publication in Physical Review Letters