Charge Ordering Research Articles

Probing Phase Formation and Structural Transformations in Sodium Extraction and Insertion of NaFe1-yMnyPO4 through First-Principles Calculations.

Manganese (Mn) substitution is a widely explored strategy aimed at sustainably enhancing the energy density of iron (Fe)-based electrode materials by taking advantage of the higher redox potential of the former. However, excessive Mn content can lead to detrimental effects, offsetting the expected improvements. In experimental studies, triphylite NaFe0.8Mn0.2PO4 has been identified as an optimal composition with enhanced electrochemical performance compared to that of its parent phase NaFePO4. Higher Mn contents result in a loss of capacity and increased voltage hysteresis. In this study, density functional theory (DFT) calculations were employed to investigate the phase stability upon desodiation of Mn-poor and -rich NaxFe1-yMnyPO4 compositions. Our findings reveal distinct stability behaviors in antagonistic systems NaxFe0.75Mn0.25PO4 and NaxFe0.25Mn0.75PO4, where the presence of Na-vacancies and charge orderings appear to influence phase stability. In addition, the number of intermediate phases throughout the desodiation process is identified as a crucial factor in buffering the volume changes. This work sheds light on the superior electrochemical performance of lightly Mn-substituted phases and unveils a key parameter for designing future electrode materials with improved performance.

Depth-dependent study of time-reversal symmetry-breaking in the kagome superconductor AV3Sb5

The breaking of time-reversal symmetry (TRS) in the normal state of kagome superconductors AV3Sb5 stands out as a significant feature, but its tunability is unexplored. Using low-energy muon spin rotation and local field numerical analysis, we study TRS breaking as a function of depth in single crystals of RbV3Sb5 (with charge order) and Cs(V0.86Ta0.14)3Sb5 (without charge order). In the bulk of RbV3Sb5 (>33 nm from the surface), we observed an increase in the internal magnetic field width in the charge-ordered state. Near the surface (<33 nm), the muon spin relaxation rate is significantly enhanced and this effect commences at temperatures significantly higher than the onset of charge order. In contrast, no similar field width enhancement was detected in Cs(V0.86Ta0.14)3Sb5, either in the bulk or near the surface. These observations indicate a strong connection between charge order and TRS breaking and suggest that TRS breaking can occur prior to long-range charge order.

Microscopic probing of the superconducting and normal state properties of Ta2V3.1Si0.9 by muon spin rotation

The two-dimensional kagome lattice is an experimental playground for novel physical phenomena, from frustrated magnetism and topological matter to chiral charge order and unconventional superconductivity. A newly identified kagome superconductor, Ta2V3.1Si0.9 has recently gained attention for possessing a record high critical temperature, TC = 7.5 K for kagome metals at ambient pressure. In this study we conducted a series of muon spin rotation measurements to delve deeper into understanding the superconducting and normal state properties of Ta2V3.1Si0.9. We demonstrate that Ta2V3.1Si0.9 is a bulk superconductor with either a s+s-wave or anisotropic s-wave gap symmetry, and has an unusual paramagnetic shift in response to external magnetic fields in the superconducting state. Additionally, we observe an exceptionally low superfluid density − a distinctive characteristic of unconventional superconductivity − which remarkably is comparable to the superfluid density found in hole-doped cuprates. In its normal state, Ta2V3.1Si0.9 exhibits a significant increase in the zero-field muon spin depolarisation rate, starting at approximately 150 K, which has been observed in other kagome-lattice superconductors, and therefore hints at possible hidden magnetism. These findings characterise Ta2V3.1Si0.9 as an unconventional superconductor and a noteworthy new member of the vanadium-based kagome material family.

Light-Induced Polaronic Crystals in Single-Layer Transition Metal Dichalcogenides.

Light-induced ordered states can emerge in materials after irradiation with ultrafast laser pulses. However, their prediction is challenging because the inverted band occupation confounds our chemical intuition. Hence, we use a recently developed constrained density functional perturbation theory approach to systematically screen single-layer transition metal dichalcogenides (TMDs) for light-induced ordered states. We demonstrate that all examined single-layer TMDs reveal similar light-induced charge orderings. The corresponding reconstructions are periodic arrangements of polarons (polaronic crystals), characterized by triangular metal clusters and having no equivalent at equilibrium conditions. The polarons are accompanied by localized midgap states in the electronic band structure, detectable by experimental methods. We assess the selenides as the most promising candidates for potential photoexcitation experiments because they transition at low critical fluences, have low transition barriers, and maintain an open band gap under photoexcitation. Our work paves the way for innovative material design approaches targeting light-induced phases.

Charge order near the antiferromagnetic quantum critical point in the trilayer high Tc cuprate HgBa2Ca2Cu3O8+δ

We study the transport properties of underdoped trilayer cuprate HgBa2Ca2Cu3O8+δ with doping level p = 0.10–0.12 in magnetic field up to 88 T. We report for the first time in a cuprate superconductor a dramatic change of the quantum oscillation spectrum versus temperature, which is accompanied by a sign change of the Hall effect below T ≈10 K. Based on numerical simulations, we infer a Fermi surface reconstruction in the inner plane from an antiferromagnetic state (hole pockets) to a biaxial charge density wave state (electron pockets). We show that both orders compete and share the same hotspots of the Fermi surface, and we discuss our result in the context of spin-fermion models.

Latent Electronic (Anti-)Ferroelectricity in BiNiO_{3}.

BiNiO_{3} exhibits an unusual metal-insulator transition from Pnma to P1[over ¯] that is related to charge ordering at the Bi sites, which is intriguingly distinct from the charge ordering at Ni sites usually observed in related rare-earth nickelates. Here, using first principles calculations, we first rationalize the phase transition from Pnma to P1[over ¯], revealing an overlooked intermediate P2_{1}/m bridging phase and a complex interplay between distinct degrees of freedom. Going further, we point out that the charge ordering at Bi sites in the P1[over ¯] phase is not unique. We highlight an alternative polar ordering giving rise to a ferroelectric Pmn2_{1} phase nearly degenerated in energy with P1[over ¯] and showing an in-plane electric polarization of 53 μC/cm^{2} directly resulting from the charge ordering. The close energy of Pmn2_{1} and P1[over ¯] phases, together with low energy barrier between them, make BiNiO_{3} a potential electronic antiferroelectric in which the field-induced transition from nonpolar to polar would relate to nonadiabatic intersite electron transfer. We also demonstrate the possibility to stabilize an electronic ferroelectric ground state from strain engineering in thin films, using an appropriate substrate.

Two Distinct Charge Orders in Infinite-Layer PrNiO2+δ Revealed by Resonant X-Ray Diffraction

Abstract Research of infinite-layer nickelates has unveiled a broken translation symmetry, which has sparked significant interest in its root, its relationship to superconductivity, and its comparison to charge order in cuprates. In this study, resonant x-ray scattering measurements were performed on thin films of infinite-layer PrNiO2+δ . The results show significant differences in the superlattice reflection at the Ni L 3 absorption edge compared to that at the Pr M 5 resonance in their dependence on energy, temperature, and local symmetry. These differences point to two distinct charge orders, although they share the same in-plane wavevectors. It is suggested that these dissimilarities could be linked to the excess oxygen dopants, given that the resonant reflections were observed in an incompletely reduced PrNiO2+δ film. Furthermore, azimuthal analysis indicates that the oxygen ligands likely play a crucial role in the charge modulation revealed at the Ni L 3 resonance.

Dielectric relaxation and electrical conduction mechanism via hopping of polarons in (Pb0.3Bi0.7)(Zn0.1Nb0.2Fe0.7)O3 perovskite compound: A study based on CBH model

This work analyses the dielectric and conducting properties of the PZN-modified BF solid solution (0.3PZN-0.7BF) synthesized at 850 °C by solid-state reaction. The Rietveld refinement of 0.3PZN-0.7BF solid solution displays three phases: tetragonal Pb(Fe0.5Nb0.5)O3 (76.68 %), α-BZN (21 %), and Bi2Fe4O9 (2.32 %). Dielectric parameter frequency dispersion implies normal ferroelectricity. Thermal relaxation shifts dielectric loss, imaginary impedance (Z''), and loss modulus (M'') peaks to higher frequencies. Electrical investigation indicates electrode polarization, dipole orientation, charge ordering, oxygen vacancies, and defects. Investigations suggest p-type polarons dominate conductivity. At room temperature and 1 MHz, the compound has 117 dielectric constant and 0.009 tangent loss. Conductivity and impedance testing show semi-conductivity. UV–Vis spectrum investigation shows a 1.97 eV energy band gap, supporting its semiconductor properties. Photovoltaic and optoelectronic device applications benefit from 0.3PZN-0.7BF solid solution optical and electrical property studies.

Disclosing the magnetic ground state of PrBaMn2O6

In this work, we report a neutron diffraction study on a single crystal of the layered PrBaMn2O6 perovskite. This compound undergoes two consecutive magnetic transitions with decreasing temperature. At TC ≈ 309 K, a long-range ferromagnetic ordering is established with the Mn magnetic moments oriented along the c axis. Below TN ≈ 240 K, a spin reorientation gives rise to a sudden decrease of the magnetization and the formation of an antiferromagnetic order. This magnetic transition is also accompanied by an electronic localization caused by a structural phase transition from a high-temperature tetragonal phase (P4/mmm) into a low-temperature orthorhombic one (P21am). Our neutron diffraction study at 12 K has unambiguously identified that the ground magnetic structure for this compound is a layered antiferromagnetic structure along the c axis with the Mn moments oriented in the ab plane along one diagonal of the primitive tetragonal cell. No sign of magnetic scattering associated to a CE-type magnetic structure was found in our study, discarding its occurrence in this compound. This result excludes the occurrence of a charge order transition to account for the electronic localization and it is fully consistent with previous structural studies showing a unique crystallographic site for Mn atom in the low-temperature phase. A symmetry analysis was carried out to identify the magnetic space group of the ferromagnetic order above TN and the two possible groups for the antiferromagnetic ordering below TN.

Interplay between charge ordering and superconducting correlations in the extended Hubbard model

We examine effects of charge ordering on superconducting correlations in the extended Hubbard model with Falicov-Kimball coupling in two dimensions. Charge orderings are generated by f-electron distributions on the localized f orbitals, which act as an internal potential for itinerant d electrons moving in the Hubbard d band. For the small finite cluster of L=4×4\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$L=4 \ imes 4$$\\end{document} sites the model is studied exactly over the complete set of f-electron distributions, while for larger clusters the projector Quantum-Monte-Carlo method and the reduced set of f-electron distributions (the periodic, phase separated and phase segregated configurations) is used. It is found that the enhancement of superconducting correlations in the d-wave channel depends strongly on the type of f-electron ordering and changes significantly with f and d electron concentration (nf\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_f$$\\end{document},nd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_d$$\\end{document}) as well as with interband Coulomb interaction Ufd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$U_{fd}$$\\end{document}. In particular, it is found that for small values of Ufd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$U_{fd}$$\\end{document} and nd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_d$$\\end{document} the superconducting correlations are the most significantly enhanced for segregated configurations (all f-electrons clump together), for all f-electron concentrations, while for higher d-band fillings axial stripes (bands) with f-electron concentrations nf∼0.5\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_f \\sim 0.5$$\\end{document} yield the largest enhancement of superconducting correlations. The region of axial striped phases is systematically reduced with increasing Ufd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$U_{fd}$$\\end{document} and for sufficiently large Ufd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$U_{fd}$$\\end{document} (Ufd∼2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$U_{fd}\\sim 2$$\\end{document}) it persists only in the region of small nf\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_f$$\\end{document} and nd\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$n_d$$\\end{document} values.

Unveiling the charge density wave mechanism in vanadium-based Bi-layered kagome metals

The charge density wave (CDW), as a hallmark of vanadium-based kagome superconductor AV3Sb5 (A = K, Rb, Cs), has attracted intensive attention. However, the fundamental controversy regarding the underlying mechanism of CDW therein persists. Recently, the vanadium-based bi-layered kagome metal ScV6Sn6, reported to exhibit a long-range charge order below 94 K, has emerged as a promising candidate to further clarify this core issue. Here, employing micro-focusing angle-resolved photoemission spectroscopy (μ-ARPES) and first-principles calculations, we systematically studied the unique CDW order in vanadium-based bi-layered kagome metals by comparing ScV6Sn6 with its isostructural counterpart YV6Sn6, which lacks a CDW ground state. Combining ARPES data and the corresponding joint density of states (DOS), we suggest that the VHS nesting mechanism might be invalid in these materials. Besides, in ScV6Sn6, we identified multiple hybridization energy gaps resulting from CDW-induced band folding, along with an anomalous band dispersion, implying a potential electron-phonon coupling-driven mechanism underlying the formation of the CDW order. Our finding not only comprehensively maps the electronic structure of V-based bi-layer kagome metals but also provides constructive experimental evidence for the unique origin of CDW in this system.

Observation of flat bands and Dirac cones in a pyrochlore lattice superconductor

Emergent phases often appear when the electronic kinetic energy is comparable to the Coulomb interactions. One approach to seek material systems as hosts of such emergent phases is to realize localization of electronic wavefunctions due to the geometric frustration inherent in the crystal structure, resulting in flat electronic bands. Recently, such efforts have found a wide range of exotic phases in the two-dimensional kagome lattice, including magnetic order, time-reversal symmetry breaking charge order, nematicity, and superconductivity. However, the interlayer coupling of the kagome layers disrupts the destructive interference needed to completely quench the kinetic energy. Here we demonstrate that an interwoven kagome network—a pyrochlore lattice—can host a three dimensional (3D) localization of electron wavefunctions. Meanwhile, the nonsymmorphic symmetry of the pyrochlore lattice guarantees all band crossings at the Brillouin zone X point to be 3D gapless Dirac points, which was predicted theoretically but never yet observed experimentally. Through a combination of angle-resolved photoemission spectroscopy, fundamental lattice model and density functional theory calculations, we investigate the novel electronic structure of a Laves phase superconductor with a pyrochlore sublattice, CeRu2. We observe evidence of flat bands originating from the Ce 4f orbitals as well as flat bands from the 3D destructive interference of the Ru 4d orbitals. We further observe the nonsymmorphic symmetry-protected 3D gapless Dirac cone at the X point. Our work establishes the pyrochlore structure as a promising lattice platform to realize and tune novel emergent phases intertwining topology and many-body interactions.

Orbital selective commensurate modulations of the local density of states in ScV6Sn6 probed by nuclear spins

The kagome network is a unique platform that harbors a diversity of special electronic states due to its inherent band structure features comprising Dirac cones, van Hove singularities, and flat bands. Some kagome-based metals have recently been found to exhibit favorable properties, including superconductivity, charge order, and signatures of an anomalous Hall effect. The kagome system ScV6Sn6 is a promising candidate for studying the emergence of an unconventional charge order and accompanying effects. We use 51V nuclear magnetic resonance to explore the local properties of the charge ordered phase in single crystalline ScV6Sn6, aided by density functional theory. We show the local charge symmetry of V to reflect a commensurate modulation with q=13,13,13\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\\bf{q}}}=\\left(\\frac{1}{3},\\frac{1}{3},\\frac{1}{3}\\right)$$\\end{document}, the density of states to drop by about a factor of 2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\sqrt{2}$$\\end{document} during the phase transition, and an unusual orientation dependent change in the shift splitting symmetry to reveal orbital selective modulations of the local density of states.

Information-theoretic quantities as effective descriptors of electrophilicity and nucleophilicity in density functional theory.

Electrophilicity and nucleophilicity are two vastly important chemical concepts gauging the capability of atoms in molecules to accept and donate the maximal number of electrons. In our earlier studies, we proposed to simultaneously quantify them using the Kullback-Leibler divergence from the information-theoretic approach in density functional theory. However, several issues with this scheme remain to be clarified such as its general validity, predictability, and relationship with other information-theoretic quantities. In this work, we revisit the matter with bigger datasets and deeper theoretical insights. Five information-theoretic quantities including Kullback-Leibler divergence, Hirshfeld charge, Ghost-Berkowitz-Parr entropy, and second and third orders of relative Onicescu information energy are found to be reliable and robust descriptors of electrophilicity and nucleophilicity propensities. Employing these five descriptors, we design a list of new compounds and predict their electrophilicity and nucleophilicity scales. This work should markedly improve our confidence and capability in applying information-theoretic quantities to evaluate electrophilicity and nucleophilicity propensities and henceforth pave the route for more applications of these quantities from information-theoretic approach in density functional theory in the future. All structures were fully optimized at the M06-2X/6-311 + G(d) level of DFT functional using the Gaussian 16 package (version C01) with integration grids and tight self-consistent-field convergence. The solvent effect was taken into account by using the implicit solvent model (CPCM) in the CH2Cl2 solvent, and all 3D contour surfaces of Fukui function, local temperature, and ITA (information-theoretic approach) quantities were generated by GaussView. The Multiwfn 3.8 program was used to calculate the ITA indexes and atomic charges.

Avoided metallicity in a hole-doped Mott insulator on a triangular lattice

Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO2 layer of the delafossite PdCrO2, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.

From Fractional Quantum Anomalous Hall Smectics to Polar Smectic Metals: Nontrivial Interplay Between Electronic Liquid Crystal Order and Topological Order in Correlated Topological Flat Bands.

Symmetry-breaking orders can not only compete with each other, but also be interwined, and the interwined topological and symmetry-breaking orders make the situation more intriguing. This work examines the archetypal correlated flat band model on a checkerboard lattice at filling ν = 2/3 and we find the unique interplay between smectic charge order and topological order gives rise to two novel quantum states. As the interaction strength increases, the system first transitions from a Fermi liquid into FQAH smectic (FQAHS) state, where FQAH topological order coexists cooperatively with smectic charge order with enlarged ground-state degeneracy and interestingly, the Hall conductivity is σxy = ν = 2/3, different from the band-folding or doping scenarios. Further increasing the interaction strength, the system undergoes another quantum phase transition and evolves into a polar smectic metal (PSM) state. This emergent PSM is an anisotropic non-Fermi liquid, whose interstripe tunneling is irrelevant while it is metallic inside each stripe. Different from the FQAHS and conventional smectic orders, this PSM spontaneously breaks the two-fold rotational symmetry, resulting in a nonzero electric dipole moment and ferroelectric order. In addition to the exotic ground states, large-scale numerical simulations are also used to study low-energy excitations and thermodynamic characteristics. We find the onset temperature of the incompressible FQAHS state, which also coincides with the onset of non-polar smectic order, is dictated by the magneto-roton modes. Above this onset temperature, the PSM state exists at intermediate-temperature regime. Although the T = 0 quantum phase transition between PSM and FQAHS is first order, the thermal FQAHS-PSM transition could be continuous. We expect the features of the exotic states and thermal phase transitions could be accessed in future experiments.

Evolution from a charge-ordered insulator to a high-temperature superconductor in Bi2Sr2(Ca,Dy)Cu2O8+δ

How Cooper pairs form and condense has been the main challenge in the physics of copper-oxide high-temperature superconductors. Great efforts have been made in the ‘underdoped’ region of the phase diagram, through doping a Mott insulator or cooling a strange metal. However, there is still no consensus on how superconductivity emerges when electron-electron correlations dominate and the Fermi surface is missing. To address this issue, here we carry out high-resolution resonant inelastic X-ray scattering and scanning tunneling microscopy studies on prototype cuprates Bi2Sr2Ca0.6Dy0.4Cu2O8+δ near the onset of superconductivity, combining bulk and surface, momentum- and real-space information. We show that an incipient charge order exists in the antiferromagnetic regime down to 0.04 holes per CuO2 unit, entangled with a particle-hole asymmetric pseudogap. The charge order induces an intensity anomaly in the bond-buckling phonon branch, which exhibits an abrupt increase once the system enters the superconducting dome. Our results suggest that the Cooper pairs grow out of a charge-ordered insulating state, and then condense accompanied by an enhanced interplay between charge excitations and electron-phonon coupling.

Incommensurate charge super-modulation and hidden dipole order in layered kitaev material α-RuCl3

The magnetism of Kitaev materials has been widely studied, but their charge properties and the coupling to other degrees of freedom are less known. Here we investigate the charge states of α-RuCl3, a promising Kitaev quantum spin liquid candidate, in proximity to graphite. We discover that few-layered α-RuCl3 experiences a clear modulation of charge states, where a Mott-insulator to weak charge-transfer-insulator transition in the 2D limit occurs by means of heterointerfacial polarization. More notably, distinct signals of incommensurate charge and lattice super-modulations, regarded as an unconventional charge order, accompanied in the insulator. Our theoretical calculations have reproduced the incommensurate charge order by taking into account the antiferroelectricity of α-RuCl3 that is driven by dipole order in the internal electric fields. The findings imply that there is strong coupling between the charge, spin, and lattice degrees of freedom in layered α-RuCl3 in the heterostructure, which offers an opportunity to electrically access and tune its magnetic interactions inside the Kitaev compounds.

Impeding conduction by breaking the charge carrier hopping in charge-ordered perovskite BaBiO3 ([formula omitted]): Experimental and theoretical electronic structural correlations

BaBiO3 (BBO), a charge-ordered perovskite with mixed-valent states of Bi (Bi3+ and Bi5+), is known for its charge density wave (CDW) semiconducting and topological insulating properties. BBO has been extensively investigated for its superconducting, electrical, and photocatalytic properties. The present study aims to understand the alterations in the CDW and electronic properties of BaBi0.53+Bi0.55+O3 by valence-selective substitution of Bi3+ and Bi5+ with La3+ and Nb5+, respectively, in the solid solutions BaBi0.5−x3+LaxBi0.55+O3 and BaBi0.53+Bi0.5−y5+NbyO3 (x = y = 0.0, 0.1, 0.3, and 0.5). The samples synthesized via high-temperature solid-state reaction method were characterized by powder X-ray diffraction and various spectroscopic techniques (FT-IR, Laser Raman, EPR, XPS, and UPS). Impedance analysis revealed an upsurge in total impedance with the substitution of Bi3+/Bi5+ by La3+/Nb5+ indicating the blocking of electron/hole hopping by disruption of the charge ordering of redox pair Bi3+ and Bi5+. The valence-selective substitution of Bi3+/Bi5+ in BaBiO3 resulted in an alteration of the electronic structure and changes in the bandwidth of BaBi0.5−x3+LaxBi0.55+O3 and BaBi0.53+Bi0.5−y5+NbyO3 (x = y = 0.0, 0.1, 0.3, and 0.5) solid solutions, which were confirmed by both theoretical density of states (DOS) calculations and experimental ultraviolet photoelectron spectroscopic (UPS) studies.

Effects of electronic correlation on topological properties of Kagome semimetal Ni3In2S2.

Kagome metals gain attention as they manifest a spectrum of quantum phenomena such as superconductivity, charge order, frustrated magnetism, and allied correlated states of condensed matter. With regard to electronic band structure, several of them exhibit non-trivial topological characteristics. Here, we present a thorough investigation on the growth and the physical properties of single crystals of Ni3In2S2 which is established to be a Dirac nodal line Kagome semimetal. Extensive characterization is attained through temperature and field-dependent resistivity, angle-dependent magnetoresistance and specific heat measurements. The central question we seek to address is the effect of electronic correlations in suppressing the manifestation of topological characteristics. In most metals, the Fermi liquid behaviour is restricted to a narrow range of temperatures. Here we show that Ni3In2S2 follows the Fermi-liquid behaviour up to 86K. This phenomenon is further supported by a high Kadowaki-Woods ratio obtained through specific heat analysis. Different interpretations of the magneto-transport study reveal that magnetoresistance exhibits linear behavior, suggesting the presence of Dirac semi-metallic signatures at lower temperatures. The angle-dependent magneto-transport study obeys the Voigt-Thomson formula. This, on the contrary, implies the classical origin of magnetoresistance. Thus, the effect of strong electron correlation in Ni3In2S2 manifests itself in the anisotropic magneto-transport. Furthermore, the magnetization measurement shows the presence of de-Haas van Alphen oscillations. Calculations of Berry phase provide insights into the topological features in the Kagome semimetal Ni3In2S2.&#xD.