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Quantum spin liquids (QSLs) represent exotic states of matter where quantum spins interact strongly yet evade long-range magnetic order down to absolute zero. Characterized by non-local quantum entanglement and resultant fractionalized excitations, QSLs have emerged as a frontier in condensed matter physics, bolstered by the recent identification of several candidate materials. This field holds profound implications for understanding strong correlations, topological order, and emergent phenomena in quantum materials. Among them, the spin-1/2 Kitaev honeycomb model, featuring bond-directional Ising interactions, provides a rare exactly solvable QSL example. Its ground state is a topological QSL, with spin degrees of freedom fractionalized into emergent Majorana fermions. Under an applied magnetic field, the Kitaev QSL transitions to a topologically non-trivial chiral spin liquid state with non-Abelian anyons, offering potential resources for topological quantum computation. The non-Abelian character of these anyons in the Kitaev QSL demonstrates a profound connection to certain topological superconductors and even-denominator fractional quantum Hall states. Since the theoretical prediction that the Kitaev model could manifest in spin-orbit-coupled materials such as honeycomb iridates and ruthenates, research has focused on identifying candidate compounds. In particular, experimental evidence suggests spin fractionalization and topological phenomena akin to the Kitaev model in the spin-orbit Mott insulator $\alpha$-RuCl$_3$. However, results and interpretations remain actively debated. This review presents a comprehensive survey of existing studies on Kitaev candidate materials, with a particular focus on $\alpha$-RuCl$_3$. Rather than offering conclusive remarks, our aim is to inspire future research by examining several key aspects of the current literature and perspectives., Comment: 65 pages, 33 figures. Review article submitted to Rev. Mod. Phys

Recently discovered high-T$_c$ superconductivity in pressurized bilayer nickelate La$_3$Ni$_2$O$_7$ (La-327) is believed to be driven by the non-phononic repulsive interaction. Depending on the strength of the interlayer repulsion, the symmetry of the superconducting order parameter is expected to be either $d$-wave or sign-changing bonding-antibonding $s_{\pm}$-wave. Unfortunately, due to the need of high pressure to reach superconducting phase, conventional spectroscopic probes to validate the symmetry of the order parameter are hard to use. Here, we study the effect of the point-like non-magnetic impurities on the superconducting state of La-327 and show that $s_{\pm}$-wave and $d$-wave symmetries show a very different behavior as a function of impurity concentration, which can be studied experimentally by irradiating the La-327 samples by electrons prior applying the pressure. While $d-$wave superconducting state will be conventionally suppressed, the $s_{\pm}$-wave state shows more subtle behavior, depending on the asymmetry between bonding and antibonding subspaces. For the electronic structure, predicted to realize in La-327, the $s_{\pm}-$wave state will be robust against complete suppression and the transition temperature, $T_c$ demonstrates a transition from convex to concave behavior, indicating a crossover from $s_{\pm}$-wave to $s_{++}$-wave symmetry as a function of impurity concentration. We further analyze the sensitivity of the obtained results with respect to the potential electronic structure modification., Comment: 9 pages, 2 figures + supplemental material (4 pages, 4 figures)

Kitaev quantum spin liquids (KSLs) in layered honeycomb magnets are known to host Majorana quasiparticles, whose excitations depend strongly on the direction of the applied magnetic field. In the high-field phase of $\alpha$-RuCl$_3$, specific heat measurements have revealed characteristic field-angle dependence of low-energy excitations consistent with the Kitaev model, providing bulk evidence for the KSL state. Here we present low-temperature measurements of specific heat $C(T)$ for another KSL candidate $\textrm{Na}_2\textrm{Co}_2\textrm{Te}\textrm{O}_6$ (NCTO) under field rotation within the honeycomb plane. Above the critical field of antiferromagnetic order, the field-angle dependence of $C/T$ exhibits minima along the bond directions, contrasting with the maxima observed in the KSL state of $\alpha$-RuCl$_3$. Our analysis indicates nodeless, fully-gapped excitations, which are inconsistent with the angle-dependent Majorana excitations with gapless nodes predicted by the Kitaev model. These findings suggest that low-energy excitations in NCTO are governed by gapped magnon excitations rather than Majorana quasiparticles, providing thermodynamic evidence against a KSL state., Comment: 6 pages, 4 figures

Kagome lattice $A$V$_3$Sb$_5$ ($A$ = K, Rb, and Cs) superconductors without magnetism from vanadium $d$-electrons are intriguing because they have a novel charge density wave (CDW) order around 90 K and display superconductivity at $\sim$3 K that competes with the CDW order. Recently, CsCr$_3$Sb$_5$, isostructural to $A$V$_3$Sb$_5$, was found to have concurrent structural and magnetic phase transition at $T^{\ast}\approx$ 55 K that can be suppressed by pressure to induce superconductivity [Liu \textit{et al.}, \href{https://doi.org/10.1038/s41586-024-07761-x}{Nature \textbf{632}, 1032 (2024)}]. Here, we use elastic and inelastic X-ray scattering to study the microscopic origin of the structural transition in CsCr$_3$Sb$_5$. Although our elastic measurements confirm the 4$\times$1$\times$1 superlattice order below $T^{\ast}$, its underlying correlation is rather short-ranged. Moreover, our inelastic measurements at the superlattice wavevectors around (3, 0, 0) find no evidence of a significant acoustic phonon anomaly below $T^{\ast}$, similar to the case of $A$V$_3$Sb$_5$. The absence of acoustic phonon anomaly indicates a weak electron-phonon coupling in CsCr$_3$Sb$_5$, suggesting that the structural transition is likely associated with an unconventional CDW order., Comment: Six pages, four figures

Recent developments in laser-excited photoemission electron microscopy (laser-PEEM) advance the visualization of electronic nematicity and nematic domain structures in iron-based superconductors. In FeSe and BaFe$_2$(As$_{0.87}$P$_{0.13}$)$_2$ superconductors, it has been reported that the thickness of the electronic nematic domain walls is unexpectedly long, leading to the formation of mesoscopic nematicity wave [T. Shimojima $\textit{et al.}$, Science $\textbf{373}$ (2021) 1122]. This finding demonstrates that the nematic coherence length $\xi_{\rm nem}$ can be decoupled from the lattice domain wall. Here, we report that the electronic domain wall thickness shows a distinct variation in related materials: it is similarly long in FeSe$_{0.9}$S$_{0.1}$ whereas it is much shorter in undoped BaFe$_2$As$_2$. We find a correlation between the thick domain walls and the non-Fermi liquid properties of normal-state resistivity above the nematic transition temperature. This suggests that the nematic coherence length can be enhanced by underlying spin-orbital fluctuations responsible for the anomalous transport properties., Comment: 5 pages, 3 figures

We provide bulk transport evidence for twin-boundary pinning of vortices in FeSe. We measure interlayer resistance in FeSe in magnetic fields and find that, as the field is rotated in the $ab$ plane, the flux-flow resistivity is suppressed when the field direction is parallel to twinning planes. The width of the associated dip in the resistance vs in-plane field direction curve varies as $T^{1/2}B^{-3/4}$, consistent with the creation of kinked vortices near the parallel field geometry., Comment: 5 pages, 6 figures

The study of the iron-based superconductor, FeSe, has resulted in various topics, such as the interplay among superconductivity, nematicity, and magnetism, Bardeen-Cooper-Schrieffer Bose-Einstein-condensation (BCS-BEC) crossover, and Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) superconductivity. Recently, topologically protected nodal Fermi surfaces, referred to as Bogoliubov Fermi surfaces (BFSs), have garnered much attention. A theoretical model for the S-substituted FeSe system demonstrated that BFSs can manifest under the conditions of spin-orbit coupling, multi-band systems, and superconductivity with time-reversal symmetry breaking. Here we report the observation of spin fluctuations originating from BFSs in the superconducting (SC) state via $^{77}$Se-nuclear magnetic resonance measurements to 100 mK. In a heavily S-substituted FeSe, we found an anomalous enhancement of low-energy spin fluctuations deep in the SC state, which cannot be explained by an impurity effect. Such unusual behavior implies the presence of significant spin fluctuations of Bogoliubov quasiparticles, which are associated with possible nesting properties between BFSs.

Continued advances in quantum technologies rely on producing nanometer-scale wires. Although several state-of-the-art nanolithographic technologies and bottom-up synthesis processes have been used to engineer such wires, critical challenges remain in growing uniform atomic-scale crystalline wires and constructing their network structures. Here we discover a simple method to fabricate atomic-scale wires with various arrangements, including stripes, X-, Y-junctions, and nanorings. Single-crystalline atomic-scale wires of a Mott insulator, whose band gap is comparable to those of wide-gap semiconductors, are spontaneously grown on graphite substrates \DEL{and epitaxial monolayer graphene on SiC }by pulsed-laser deposition. These wires are one-unit-cell-thick and have an exact width of two- and four-unit-cells (1.4 and 2.8\,nm) and lengths up to a few $\mu m$. We show that the non-equilibrium reaction-diffusion processes may play an essential role in atomic pattern formation. Our findings offer a new perspective on the non-equilibrium self-organization phenomena on an atomic scale, paving a unique way for the quantum architecture of nano-network.

Recent studies in heavily hole-doped iron-based superconductor RbFe$_2$As$_2$ have suggested the emergence of novel electronic nematicity directed along the Fe-As direction, 45$^\circ$ rotated from the usual nematicity ubiquitously found in BaFe$_2$As$_2$ and related materials. This motivates us to study the physical properties of Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$, details of which remain largely unexplored. Here we report on the normal-state charge transport in Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$ superconductors by using high-quality single crystals in the range of Rb concentration $0.14\le x \le 1.00$. From the systematic measurements of the temperature dependence of electrical resistivity $\rho(T)$, we find a signature of a deviation from the Fermi liquid behavior around the optimal composition, which does not seem related to the antiferromagnetic quantum criticality but has a potential link to hidden nematic quantum criticality. In addition, electron correlations derived from the coefficient of $T^2$ resistivity show a marked increase with Rb content near the heavily hole-doped end, consistent with the putative Mott physics near the $3d^5$ electron configuration in iron-based superconductors., Comment: 6 pages, 4 figures

A finite residual linear term in the thermal conductivity at zero temperature in insulating magnets indicates the presence of gapless excitations of itinerant quasiparticles, which has been observed in some candidate materials of quantum spin liquids (QSLs). In the organic triangular insulator beta'-EtMe3Sb[Pd(dmit)2]2, a QSL candidate material, the low-temperature thermal conductivity depends on the cooling process and the finite residual term is observed only in samples with large thermal conductivity. Moreover, the cooling rate dependence is largely sample dependent. Here we find that, while the low-temperature thermal conductivity significantly depends on the cooling rate, the high-temperature resistivity is almost perfectly independent of the cooling rate. These results indicate that in the samples with the finite residual term, the mean free path of the quasiparticles that carry the heat at low temperatures is governed by disorders, whose characteristic length scale of the distribution is much longer than the electron mean free path that determines the high-temperature resistivity. This explains why recent X-ray diffraction and nuclear magnetic resonance measurements show no cooling rate dependence. Naturally, these measurements are unsuitable for detecting disorders of the length scale relevant for the thermal conductivity, just as they cannot determine the residual resistivity of metals. Present results indicate that very careful experiments are needed when discussing itinerant spin excitations in beta'-EtMe3Sb[Pd(dmit)2]2., Comment: 14 pages, 4 figures, to appear in Scientific Reports

Electronic nematicity in correlated metals often occurs alongside another instability such as magnetism. As a result, the question remains whether nematicity alone can drive unconventional superconductivity or anomalous (quantum critical) transport in such systems. In FeSe, nematicity emerges in isolation, providing a unique opportunity to address this question. Studies to date, however, have proved inconclusive; while signatures of nematic criticality are observed upon sulfur substitution, they appear to be quenched under the application of pressure due to the emergent magnetism. Here, we study the temperature and pressure dependence of the low-temperature resistivity of FeSe$_{1-x}$S$_{x}$ crystals at $x$ values just beyond the nematic quantum critical point. Two distinct components to the resistivity are revealed; one whose magnitude falls with increasing pressure and one which grows upon approaching the magnetic state at higher pressures. These findings indicate that nematic and magnetic critical fluctuations in FeSe$_{1-x}$S$_{x}$ are completely decoupled, in marked contrast to other Fe-based superconductors, and that nematic fluctuations alone may be responsible for the transport signatures of quantum criticality found in FeSe$_{1-x}$S$_{x}$ at ambient pressure.

The mechanism behind the nematicity of FeSe is not known. Through elastoresitivity measurements it has been shown to be an electronic instability. However, so far measurements have extended only to small strains, where the response is linear. Here, we apply large elastic strains to FeSe, and perform two types of measurements. (1) Using applied strain to control twinning, the nematic resistive anisotropy at temperatures below the nematic transition temperature Ts is determined. (2) Resistive anisotropy is measured as nematicity is induced through applied strain at fixed temperature above Ts. In both cases, as nematicity strengthens the resistive anisotropy peaks about about 7%, then decreases. Below ~40 K, the nematic resistive anisotropy changes sign. We discuss possible implications of this behaviour for theories of nematicity. We report in addition: (1) Under experimentally accessible conditions with bulk crystals, stress, rather than strain, is the conjugate field to the nematicity of FeSe. (2) At low temperatures the twin boundary resistance is ~10% of the sample resistance, and must be properly subtracted to extract intrinsic resistivities. (3) Biaxial inplane compression increases both in-plane resistivity and the superconducting critical temperature Tc, consistent with a strong role of the yz orbital in the electronic correlations., Comment: 18 pages, 13 figures. To be published in Phys. Rev. X

Nematic orders emerge nearly universally in iron-based superconductors, but elucidating their origins is challenging because of intimate couplings between orbital and magnetic fluctuations. The iron-based ladder material BaFe2S3, which superconducts under pressure, exhibits antiferromagnetic order below TN ~ 117K and a weak resistivity anomaly at T* ~ 180K, whose nature remains elusive. Here we report angle-resolved magnetoresistance (MR) and elastoresistance (ER) measurements in BaFe2S3, which reveal distinct changes at T*. We find that MR anisotropy and ER nematic response are both suppressed near T*, implying that an orbital order promoting isotropic electronic states is stabilized at T*. Such an isotropic state below T* competes with the antiferromagnetic order, which is evidenced by the nonmonotonic temperature dependence of nematic fluctuations. In contrast to the cooperative nematic orders in spin and orbital channels in iron pnictides, the present competing orders can provide a new platform to identify the separate roles of orbital and magnetic fluctuations., Comment: 7 pages 5 figures, to be published in Phys. Rev. Res

To fully capitalize on the potential and versatility of resonant inelastic x-ray scattering (RIXS), it is essential to develop the capability to interpret different RIXS contributions through calculations, including the dependence on momentum transfer, from first-principles for correlated materials. Toward that objective, we present new methodology for calculating the full RIXS response of a correlated metal in an unbiased fashion. Through comparison of measurements and calculations that tune the incident photon energy over a wide portion of the Fe L$_3$ absorption resonance of the example material BaFe$_2$As$_2$, we show that the RIXS response in BaFe$_2$As$_2$ is dominated by the direct channel contribution, including the Raman-like response below threshold, which we explain as a consequence of the finite core-hole lifetime broadening. Calculations are initially performed within the first-principles Bethe-Salpeter framework, which we then significantly improve by convolution with an effective spectral function for the intermediate-state excitation. We construct this spectral function, also from first-principles, by employing the cumulant expansion of the Green's function and performing a real-time time dependent density functional theory calculation of the response of the electronic system to the perturbation of the intermediate-state excitation. Importantly, this allows us to evaluate the indirect RIXS response from first-principles, accounting for the full periodicity of the crystal structure and with dependence on the momentum transfer., Comment: 18 pages, submitted

High-temperature superconductivity and a wide variety of exotic superconducting states discovered in FeSe-based materials have been at the frontier of research on condensed matter physics over the past decade. Unique properties originating from the multiband electronic structure, strongly orbital-dependent phenomena, extremely small Fermi energy, electronic nematicity, and topological aspects give rise to many distinct and fascinating superconducting states. Here, we provide an overview of our current understanding of the superconductivity of {\it bulk} FeSe-based materials, focusing on FeSe and the isovalent substituted FeSe$_{1-x}$S$_{x}$ and FeSe$_{1-x}$Te$_{x}$. We discuss the highly nontrivial superconducting properties in FeSe, including extremely anisotropic pairing states, crossover phenomena from Bardeen--Cooper--Schrieffer (BCS) to Bose--Einstein condensation (BEC) states, a novel field-induced superconducting phase, and broken time-reversal symmetry. We also discuss the evolution of the superconducting gap function with sulfur and tellurium doping, paying particular attention to the impact of quantum critical nematic fluctuations and the topological superconductivity. FeSe-based materials provide an excellent playground to study various exotic superconducting states., Comment: 33 pages, 32 figures, invited review article

Quantum spin liquids realize massive entanglement and fractional quasiparticles from localized spins, proposed as an avenue for quantum science and technology. In particular, topological quantum computations are suggested in the non-abelian phase of Kitaev quantum spin liquid with Majorana fermions, and detection of Majorana fermions is one of the most outstanding problems in modern condensed matter physics. Here, we propose a concrete way to identify the non-abelian Kitaev quantum spin liquid by magnetic field angle dependence. Topologically protected critical lines exist on a plane of magnetic field angles, and their shapes are determined by microscopic spin interactions. A chirality operator plays a key role in demonstrating microscopic dependences of the critical lines. We also show that the chirality operator can be used to evaluate topological properties of the non-abelian Kitaev quantum spin liquid without relying on Majorana fermion descriptions. Experimental criteria for the non-abelian spin liquid state are provided for future experiments., Comment: 11 pages, 7 figures, 1 table, and supplementary information

Response to uniaxial stress has become a major probe of electronic materials. Tuneable uniaxial stress may be applied using piezoelectric actuators, and so far two methods have been developed to couple samples to actuators. In one, actuators apply force along the length of a free, beam-like sample, allowing very large strains to be achieved. In the other, samples are affixed directly to piezoelectric actuators, allowing study of mechanically delicate materials. Here, we describe an approach that merges the two: thin samples are affixed to a substrate, that is then pressurized uniaxially using piezoelectric actuators. Using this approach, we demonstrate application of large elastic strains to mechanically delicate samples: the van der Waals-bonded material FeSe, and a sample of CeAuSb$_2$ that was shaped with a focused ion beam., Comment: 11 pages, 9 figures

Unconventional superconductivity arises at the border between the strong coupling regime with local magnetic moments and the weak coupling regime with itinerant electrons, and stems from the physics of criticality that dissects the two. Unveiling the nature of the quasiparticles close to quantum criticality is fundamental to understand the phase diagram of quantum materials. Here, using resonant inelastic x-ray scattering (RIXS) and Fe-K$_\beta$ emission spectroscopy (XES), we visualize the coexistence and evolution of local magnetic moments and collective spin excitations across the superconducting dome in isovalently-doped BaFe$_2$(As$_{1-x}$P$_x$)$_2$ (0.00$\leq$x$\leq0.$52). Collective magnetic excitations resolved by RIXS are gradually hardened, whereas XES reveals a strong suppression of the local magnetic moment upon doping. This relationship is captured by an intermediate coupling theory, explicitly accounting for the partially localized and itinerant nature of the electrons in Fe pnictides. Finally, our work identifies a local-itinerant spin fluctuations channel through which the local moments transfer spin excitations to the particle-hole (paramagnons) continuum across the superconducting dome., Comment: Accepted in Communications Physics

To identify the key parameter for optimal superconductivity in iron pnictides, we measured the $^{31}$P-NMR relaxation rate on BaFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ ($x = 0.22$ and 0.28) under pressure and compared the effects of chemical substitution and physical pressure. For $x = 0.22$, structural and antiferromagnetic (AFM) transition temperatures both show minimal changes with pressure up to 2.4~GPa, whereas the superconducting transition temperature $T_{\rm c}$ increases to twice its former value. In contrast, for $x=0.28$ near the AFM quantum critical point (QCP), the structural phase transition is quickly suppressed by pressure and $T_{\rm c}$ reaches a maximum. The analysis of the temperature-dependent nuclear relaxation rate indicates that these contrasting behaviors can be quantitatively explained by a single curve of the $T_{\rm c}$ dome as a function of Weiss temperature $\theta$, which measures the distance to the QCP. Moreover, the $T_{\rm c}$-$\theta$ curve under pressure precisely coincides with that with chemical substitution, which is indicative of the existence of a universal relationship between low-energy AFM fluctuations and superconductivity on BaFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$., Comment: 5 pages, 6 figures

Photo-excitation is a very powerful way to instantaneously drive a material into a novel quantum state without any fabrication, and variable ultrafast techniques have been developed to observe how electron-, lattice-, and spin-degrees of freedom change. One of the most spectacular phenomena is photo-induced superconductivity, and it has been suggested in cuprates that the transition temperature Tc can be enhanced from original Tc with significant lattice modulations. Here we show another photo-induced high-Tc superconducting state in the iron-based superconductor FeSe with semi-metallic hole and electron bands. The transient electronic state in the entire Brillouin zone is directly observed by the time- and angle-resolved photoemission spectroscopy using extreme ultraviolet pulses obtained from high harmonic generation. Our results of dynamical behaviors on timescales from 50 fs to 800 ps consistently support the favorable superconducting state after photo-excitation well above Tc. This finding demonstrates that multiband iron-based superconductors emerge as an alternative candidate for photo-induced superconductors.

The 12%-S doped FeSe system has a high Tc of 30 K at a pressure of 3.0 GPa. We have successfully investigated its microscopic properties for the first time via $^{77}$Se-NMR measurements under pressure. The antiferromagnetic (AFM) fluctuations at the optimal pressure (~3 GPa) exhibited unexpected suppression compared with the AFM fluctuations at ambient pressure, even though the optimal pressure is close to the phase boundary of the AFM phase induced at the high-pressure region. In addition, we revealed that the SC phase at an applied field of 6.02 T exhibited a remarkable double-dome structure in the pressure-temperature phase diagram, unlike the SC phase at zero field., Comment: arXiv admin note: substantial text overlap with arXiv:1807.07118

It is a long-standing important issue in heavy fermion physics whether $f$-electrons are itinerant or localized when the magnetic order occurs. Here we report the {\it in situ} scanning tunneling microscopy observation of the electronic structure in epitaxial thin films of CeRhIn$_5$, a prototypical heavy fermion compound with antiferromagnetic ground state. The conductance spectra above the N\'eel temperature $T_N$ clearly resolve the energy gap due to the hybridization between local 4$f$ electrons and conduction bands as well as the crystal electric field excitations. These structures persist even below $T_N$. Moreover, an additional dip in the conductance spectra develops due to the antiferromagnetic order. These results provide direct evidence for the presence of itinerant heavy $f$-electrons participating in the Fermi surface even in the magnetically ordered state of CeRhIn$_5$.

Recent progress in the fabrication techniques of superlattices (SLs) has made it possible to sandwich several-layer-thick block layers (BLs) of heavy-fermion superconductor CeCoIn5 between conventional-metal YbCoIn5 BLs or spin-density-wave-metal CeRhIn5 BLs of a similar thickness. However, the magnetic state in each BL, particularly at the interface, is not yet understood, as experimental techniques applicable to the SL system are limited. Here, we report measurements of 59Co nuclear magnetic resonance, which is a microscopic probe of the magnetic properties inside the target BLs. In the CeCoIn5/YbCoIn5 SL, the low-temperature magnetic fluctuations of the CeCoIn5 BL are weakened as expected from the Rashba spin-orbit effect. However, in the CeCoIn5/CeRhIn5 SL, the fluctuations show an anomalous enhancement below 6 K, highlighting the importance of the magnetic proximity effect occurring near a magnetic-ordering temperature TN ~ 3 K of the CeRhIn5 BL. We suggest that the magnetic properties of the BLs can be altered by the interfacial interaction, which is an alternative route to modify the magnetic properties., Comment: 5 pages, 4 figures

Local electronic effects in the vicinity of an impurity provide pivotal insight into the origin of unconventional superconductivity, especially when the materials are located on the edge of magnetic instability. In high-temperature cuprate superconductors, a strong suppression of superconductivity and appearance of low-energy bound states are clearly observed near nonmagnetic impurities. However, whether these features are common to other strongly correlated superconductors has not been established experimentally. Here, we report the {$in$} {$situ$} scanning tunneling microscopy observation of electronic structure around a nonmagnetic Zn impurity in heavy-fermion CeCo(In$_{1-x}$Zn$_x$)$_5$ films, which are epitaxially grown by the state-of-the-art molecular beam epitaxy technique. The films have very wide atomically flat terraces and Zn atoms residing on two different In sites are clearly resolved. Remarkably, no discernible change is observed for the superconducting gap at and around the Zn atoms. Moreover, the local density of states around Zn atoms shows little change inside the $c$-$f$ hybridization gap, which is consistent with calculations for a periodic Anderson model without local magnetic order. These results indicate that no nonsuperconducting region is induced around a Zn impurity and do not support the scenario of antiferromagnetic droplet formation suggested by indirect measurements in Cd-doped CeCoIn$_5$. These results also highlight a significant difference of the impurity effect between cuprates and CeCoIn$_5$, in both of which $d$-wave superconductivity arises from the non-Fermi liquid normal state near antiferromagnetic instabilities.

Since the progress in the fabrication techniques of thin-films of exotic materials such as strongly correlated heavy-fermion compounds, microscopic studies of the magnetic and electronic properties inside the films have been needed. Herein, we report the first observation of 115In nuclear quadrupole resonance (NQR) in an epitaxial film of the heavy-fermion superconductor CeCoIn5, for which the microscopic field gradient within the unit cell as well as magnetic and superconducting properties at zero field are evaluated. We find that the nuclear spin-lattice relaxation rate in the film is in excellent agreement with that of bulk crystals, whereas the NQR spectra show noticeable shifts and significant broadening indicating a change in the electric-field distribution inside the film. The analysis implies a displacement of In layers in the film, which however does not affect the magnetic fluctuations and superconducting pairing. This implies that inhomogeneity of the electronic field gradient in the film sample causes no pair breaking effect., Comment: 12 pages, 6 figures

In many classes of unconventional superconductors, the question of whether the superconductivity is enhanced by the quantum-critical fluctuations on the verge of an ordered phase remains elusive. One of the most direct ways of addressing this issue is to investigate how the superconducting dome traces a shift of the ordered phase. Here, we study how the phase diagram of the iron-based superconductor BaFe$_2$(As$_{1-x}$P$_x$)$_2$ changes with disorder via electron irradiation, which keeps the carrier concentrations intact. With increasing disorder, we find that the magneto-structural transition is suppressed, indicating that the critical concentration is shifted to the lower side. Although the superconducting transition temperature $T_c$ is depressed at high concentrations ($x\gtrsim$0.28), it shows an initial increase at lower $x$. This implies that the superconducting dome tracks the shift of the antiferromagnetic phase, supporting the view of the crucial role played by quantum-critical fluctuations in enhancing superconductivity in this iron-based high-$T_c$ family., Comment: 5 pages, 4 figures

When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly-correlated spins keep to fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here we utilize thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report on the observation of anomalous excitations that may unveil the unique features of the SL state. Our principal finding is a negative thermal Hall conductivity (k_xy) which the charge-neutral spin excitations in a gapless SL state of the two-dimensional kagome insulator volborthite Cu_3V_2O_7(OH)_2 \cdot 2H_2O exhibit, in much the same way in which charged electrons give rise to the conventional electric Hall effect. We find that k_xy is absent in the high-temperature paramagnetic state and develops upon entering the SL state in accordance with the growth of the short-range spin correlations, demonstrating that k_xy is a key signature of the elementary excitation formed in the SL state. These results suggest the emergence of nontrivial elementary excitations in the gapless SL state which feel the presence of fictitious magnetic flux, whose effective Lorentz force is found to be less than 1/100 of that experienced by free electrons., Comment: 9 pages, 4 figures, Proc. Natl. Acad. Sci. USA (2016)

There is growing evidence that the superconducting semimetal FeSe ($T_c\sim8$ K) is in the crossover regime between weak-coupling Bardeen-Cooper-Schrieffer (BCS) and strong-coupling Bose-Einstein-condensate (BEC) limits. We report on longitudinal and transverse thermal conductivities, $\kappa_{xx}$ and $\kappa_{xy}$, respectively, in magnetic fields up to 20 T. The field dependences of $\kappa_{xx}$ and $\kappa_{xy}$ imply that a highly anisotropic small superconducting gap forms at the electron Fermi-surface pocket whereas a more isotropic and larger gap forms at the hole pocket. Below $\sim1.0$ K, both $\kappa_{xx}$ and $\kappa_{xy}$ exhibit distinct anomalies (kinks) at the upper critical field $H_{c2}$ and at a field $H^*$ slightly below $H_{c2}$. The analysis of the thermal Hall angle ($\kappa_{xy}/\kappa_{xx}$) indicates a change of the quasiparticle scattering rate at $H^*$. These results provide strong support to the previous suggestion that above $H^*$ a distinct field-induced superconducting phase emerges with an unprecedented large spin imbalance., Comment: 7 pages, 3 figures, to be published in JPSJ

The resistivity $\rho$ and Hall resistivity $\rho_H$ are measured on FeSe at pressures up to $P$ = 28.3 kbar in magnetic fields up to $B$ = 14.5 T. The $\rho(B)$ and $\rho_H(B)$ curves are analyzed with multicarrier models to estimate the carrier density and mobility as a function of $P$ and temperature ($ T\leqslant$ 110 K). It is shown that the pressure-induced antiferromagnetic transition is accompanied by an abrupt reduction of the carrier density and scattering. This indicates that the electronic structure is reconstructed significantly by the antiferromagnetic order., Comment: 6 pages, 5 figures + SM ( 2 pages, 2 figures)

Realizing new classes of ground states in strongly correlated electron systems continues to be at the forefront of condensed matter physics. Heavy-fermion materials, whose electronic structure is essentially three-dimensional, are one of the most suitable systems for obtaining novel electronic states because they demonstrate many fascinating properties. Recently, a state-of-the-art MBE technique has been developed to reduce the dimensionality of the heavy electrons by fabricating heavy fermion superlattices, which can produce new electronic states present in two-dimensional (2D) heavy fermion system. In superlattices of antiferromagnetic heavy fermion CeIn3 and conventional metal LaIn3, the magnetic order is suppressed by reducing the thickness of the CeIn3 layers. The 2D confinement of heavy fermion also leads to the enhancement of the effective mass and the deviation from the Fermi liquid properties, which are associated with the dimensional tuning of quantum criticality. In superconducting superlattices of heavy fermion superconductor CeCoIn5 and nonmagnetic metal YbCoIn5, superconductivity is realized even at one-unit-cell-thick layer of CeCoIn5. The thickness reduction of the CeCoIn5 layers drastically changes the temperature and angular dependencies of the upper critical field. This result would be attributed to a suppression of the Pauli pair-breaking effect through the local inversion symmetry breaking (ISB) at the interfaces of CeCoIn5 block layers. The importance of the ISB in this system has also been supported by site-selective nuclear magnetic resonance spectroscopy. In addition, recent experiment of CeCoIn5/YbCoIn5 superlattices have shown that the degree of the ISB are controllable, which offers the prospect of achieving even more fascinating superconducting states. These Kondo superlattices, thus, pave the way for exploring unusual metallic and superconducting states., Comment: An invited review article for Reports on Progress in Physics, 23 pages, 13 figures, and 1 table

We discuss the charge carrier dynamics of the heavy-fermion compound CeCoIn$_5$ in the metallic regime measured by means of quasi-optical THz spectroscopy. The transmittance of electromagnetic radiation through a CeCoIn$_5$ thin film on a dielectric substrate is analyzed in the single-particle Drude framework. We discuss the temperature dependence of the electronic properties, such as the scattering time and dc-conductivity and compare with transport measurements of the sheet resistance. Towards low temperatures, we find an increasing mismatch between the results from transport and Drude-analyzed optical measurements and a growing incapability of the simple single-particle picture describing the charge dynamics, likely caused by the evolving heavy-fermion nature of the correlated electron system.

In this report, we comprehensively study the effect of H$^+$ irradiation on the critical current density, $J_c$, and vortex pinning in FeSe single crystal. It is found that the value of $J_c$ for FeSe is enhanced more than twice after 3-MeV H$^+$ irradiation. The scaling analyses of the vortex pinning force based on the Dew-Hughes model reveal that the H$^+$ irradiation successfully introduce point pinning centers into the crystal. We also find that the vortex creep rates are strongly suppressed after irradiation. Detailed analyses of the critical current dependent pinning energy based on the collective creep theory and extend Maley's method show that the H$^+$ irradiation enhances the value of $J_c$ before the flux creep, and also reduces the size of flux bundle, which will further reduce the field dependence of $J_c$ due to vortex motion., Comment: 4 pages, 4figures

We have studied the superlattices with alternating block layers (BLs) of heavy-fermion superconductor CeCoIn5 and conventional-metal YbCoIn5 by site-selective nuclear magnetic resonance(NMR) spectroscopy, which uniquely offers spatially-resolved dynamical magnetic information. We find that the presence of antiferromagnetic fluctuations is confined to the Ce-BLs, indicating that magnetic degrees of freedom of f-electrons are quenched inside the Yb-BLs. Contrary to simple expectations that the two-dimensionalization enhances fluctuations, we observe that antiferromagnetic fluctuations are rapidly suppressed with decreasing Ce-BL thickness. Moreover, the suppression is more prominent near the interfaces between the BLs. These results imply significant effects of local inversion-symmetry breaking at the interfaces., Comment: 5 pages, 4 figures, accepted for publication as a Rapid Communication in Physical Review B

We present a comprehensive study of the vortex pinning and dynamics in a high-quality FeSe single crystal, which is free from doping introduced inhomogeneities and charged quasi-particle-scattering because of its innate superconductivity. Critical current density, $J_c$, is found to be almost isotropic, and reaches a value $\sim$ 3 $\times$ 10$^4$ A/cm$^2$ at 2 K (self-field) for both $H$ $\|$ $c$ and $ab$. The normalized magnetic relaxation rate $S$ (= $\mid$dln$M$/dln$t$$\mid$) shows a temperature insensitive plateau behavior in the intermediate temperature range with a relatively high creep rate ($S$ $\sim$ 0.02 under zero field), which is interpreted in the framework of the collective creep theory. A crossover from the elastic to plastic creep is observed, while the fish-tail effect is absent for both $H$ $\|$ $c$ and $ab$. Based on this observation, the origin of the fish-tail effect is also discussed. Combining the results of $J_c$ and $S$, vortex motion in FeSe single crystal is found to be dominated by sparse strong point-like pinning from nm-sized defects or imperfections. The weak collective pinning is also observed and proved in the form of large bundles. Besides, the vortex phase diagram of FeSe is also constructed and discussed., Comment: 7 pages, 5 figures

To elucidate the origin of nematic order in Fe-based superconductors, we report a Raman scattering study of lattice dynamics, which quantify the extent of $C_4$-symmetry breaking, in BaFe$_2$As$_2$ and FeSe. FeSe possesses a nematic ordering temperature $T_\mathrm{s}$ and orbital-related band-energy split below $T_\mathrm{s}$ that are similar to those in BaFe$_2$As$_2$, but unlike BaFe$_2$As$_2$ it has no long-range magnetic order. We find that the $E_g$ phonon-energy split in FeSe sets in only well below $T_\mathrm{s}$, and its saturated value is substantially smaller than that in BaFe$_2$As$_2$. Together with reported results for the Ba(Fe$_{1-x}$Co$_{x}$)$_2$As$_2$ family, the data suggest that magnetism exerts a major influence on the lattice., Comment: 4 pages, 4 figures

Superconductors close to quantum phase transitions often exhibit a simultaneous increase of electronic correlations and superconducting transition temperatures. Typical examples are given by the recently discovered iron-based superconductors. We investigated the band-specific quasiparticle masses of AFe2As2 single crystals with A = K, Rb, and Cs and determined their pressure dependence. The evolution of electronic correlations could be tracked as a function of volume and hole doping. The results indicate that with increasing alkali-metal ion radius a quantum critical point is approached. The critical fluctuations responsible for the enhancement of the quasiparticle masses appear to suppress the superconductivity., Comment: main text: 5 pages, 4 figures; supplemental material: 6 pages, 6 figures, 3 tables

We report Shubnikov-de Haas (SdH) oscillation measurements on FeSe under high pressure up to $P$ = 16.1 kbar. We find a sudden change in SdH oscillations at the onset of the pressure-induced antiferromagnetism at $P$ $\sim$ 8 kbar. We argue that this change can be attributed to a reconstruction of the Fermi surface by the antiferromagnetic order. The negative d$T_c$/d$P$ observed in a range between $P$ $\sim$ 8 and 12 kbar may be explained by the reduction in the density of states due to the reconstruction. The ratio of the transition temperature to the effective Fermi energy remains high under high pressure: $k_BT_c/E_F$ $\sim$ 0.1 even at $P$ = 16.1 kbar., Comment: 12 pages , 10 figures

We report on $^{75}$As-NMR measurements in single crystalline BaFe$_{2}$(As$_{0.96}$P$_{0.04}$)$_{2}$ for magnetic fields parallel to the orthorhombic $[110]_{\rm o}$ and $[100]_{\rm o}$ directions above the structural transition temperature $T_{\rm S}\simeq121$ K. A large difference in the linewidth between the two field directions reveals in-plane anisotropy of the electric field gradient, even in the tetragonal phase. This provides microscopic evidence of population imbalance between As-$4p_{x}$ and $4p_{y}$ orbitals, which reaches $|n_x-n_y|/|n_x+n_y| \sim 15$\% at $T\rightarrow T_{\rm S}$ and is a natural consequence of the orbital ordering of Fe-3$d_{xz}$ and $d_{yz}$ electrons. Surprisingly, this orbital polarization is found to be already static near room temperature, suggesting that it arises from the pinning of anisotropic orbital fluctuations by disorder. The effect is found to be stronger below $\sim 160$ K, which coincides with the appearance of nematicity in previous torque and photoemission measurements. These results impose strong constraints on microscopic models of the nematic state., Comment: 6 pages, 6 figures. Supplemental Materials are included. To appear in J. Phys. Soc. Jpn. (Vol.84 No. 4)

We report measurements of resistance and ac magnetic susceptibility on FeSe single crystals under high pressure up to 27.2 kbar. The structural phase transition is quickly suppressed with pressure, and the associated anomaly is not seen above $\sim$18 kbar. The superconducting transition temperature evolves nonmonotonically with pressure, showing a minimum at $\sim12$ kbar. We find another anomaly at 21.2 K at 11.6 kbar. This anomaly most likely corresponds to the antiferromagnetic phase transition found in $\mu$SR measurements [M. Bendele \textit{et al.}, Phys. Rev. Lett. \textbf{104}, 087003 (2010)]. The antiferromagnetic and superconducting transition temperatures both increase with pressure up to $\sim25$ kbar and then level off. The width of the superconducting transition anomalously broadens in the pressure range where the antiferromagnetism coexists., Comment: 3 figures

We use magnetic force microscopy (MFM) to characterize superconductivity across the superconducting dome in ${\rm {BaFe}_2 \left(As_{1-x}P_x\right)_2}$, a pnictide with a peak in the penetration depth ($\lambda_{ab}$) at optimal doping ($\rm x_{opt}$), as shown in sample-wide measurements. Our local measurements show a peak at $\rm x_{opt}$ and a $T_C$ vs. $\lambda_{ab}^{-2}$ dependence similar on both sides of $\rm x_{opt}$. Near the underdoped edge of the dome $\lambda_{ab}$ increases sharply suggesting that superconductivity competes with another phase. Indeed MFM vortex imaging shows correlated defects parallel to twin boundaries only in underdoped samples and not for $\rm x\ge x_{opt}$., Comment: 23 pages (11 main text, 12 support material)

We have observed Shubnikov-de Haas oscillations in FeSe. The Fermi surface deviates significantly from predictions of band-structure calculations and most likely consists of one electron and one hole thin cylinder. The carrier density is in the order of 0.01 carriers/ Fe, an order-of-magnitude smaller than predicted. Effective Fermi energies as small as 3.6 meV are estimated. These findings call for elaborate theoretical investigations incorporating both electronic correlations and orbital ordering., Comment: 6 pages, 6 figures, 1 table, published in Phys. Rev. B