Charge Gap Research Articles

Evidence for large thermodynamic signatures of in-gap fermionic quasiparticle states in a Kondo insulator

The mixed-valence compound YbB12 displays paradoxical quantum oscillations in electrical resistivity and magnetic torque in a regime with a well-developed insulating charge gap and in the absence of an electronic Fermi surface. However, signatures of such unusual fermionic quasiparticles in other bulk thermodynamic observables have been missing. Here we report the observation of a series of sharp double-peak features in the specific heat as a function of the magnetic field. The measured Hall resistivity evolves smoothly across the field values at which the characteristic anomalies appear in the thermodynamic response and rules out the possibility of conventional electrons as their origin. Our observations of thermodynamic anomalies in a bulk three-dimensional electrical insulator provide the evidence for the presence of emergent dispersing fermionic excitations within the insulating bulk, which sets the stage for further investigation of electron fractionalization in other correlated mixed-valence compounds.

Antiferromagnetic Chern insulator with large charge gap in heavy transition-metal compounds

Despite the discovery of multiple intrinsic magnetic topological insulators in recent years the observation of Chern insulators is still restricted to very low temperatures due to the negligible charge gaps. Here, we uncover the potential of heavy transition-metal compounds for realizing a collinear antiferromagnetic Chern insulator (AFCI) with a charge gap as large as 300 meV. Our analysis relies on the Kane-Mele-Kondo model with a ferromagnetic Hund coupling JH\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$J_{{\ extrm{H}}}$$\\end{document} between the spins of itinerant electrons and the localized spins of size S. We show that a spin-orbit coupling λSO≳0.03t\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\lambda _{{\ extrm{SO}}} \\gtrsim 0.03t$$\\end{document}, where t is the nearest-neighbor hopping element, is already large enough to stabilize an AFCI provided the alternating sublattice potential δ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\delta$$\\end{document} is in the range δ≈SJH\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\delta \\approx SJ_{{\ extrm{H}}}$$\\end{document}. We establish a remarkable increase in the charge gap upon increasing λSO\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\lambda _{{\ extrm{SO}}}$$\\end{document} in the AFCI phase. Using our results we explain the collinear AFCI recently found in monolayers of CrO and MoO with charge gaps of 1 and 50meV\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$50\\,\\hbox {meV}$$\\end{document}, respectively. In addition, we propose bilayers of heavy transition-metal oxides of perovskite structure as candidates to realize a room-temperature AFCI if grown along the [111] direction and subjected to a perpendicular electric field.

Interfacial Charge-Transfer Excitonic Insulator in a Two-Dimensional Organic-Inorganic Superlattice.

Excitonic insulators are long-sought-after quantum materials predicted to spontaneously open a gap by the Bose condensation of bound electron-hole pairs, namely, excitons, in their ground state. Since the theoretical conjecture, extensive efforts have been devoted to pursuing excitonic insulator platforms for exploring macroscopic quantum phenomena in real materials. Reliable evidence of excitonic character has been obtained in layered chalcogenides as promising candidates. However, owing to the interference of intrinsic lattice instabilities, it is still debatable whether those features, such as the charge density wave and gap opening, are primarily driven by the excitonic effect or by the lattice transition. Herein, we develop an intercalation chemistry strategy for obtaining a novel charge-transfer excitonic insulator in organic-inorganic superlattice interfaces that serves as an ideal platform to decouple the excitonic effect from the lattice effect. In this system, we observe a narrow excitonic gap, formation of a charge density wave without periodic lattice distortion, and metal-insulator transition, providing visualized evidence of exciton condensation occurring in thermal equilibrium. Our findings identify self-assembly intercalation chemistry as a new strategy for developing novel excitonic insulators.

Twisted graphene superlattices: resonating valence bond states and magnetic properties

Resonating valence bond (RVB) states are fundamental for understanding quantum spin liquids in two-dimensional (2D) systems. The RVB state is a collective phenomenon in which spins are uncoupled. 2D lattices such as triangular, honeycomb, and dice lattices were investigated using the Hubbard model and exact diagonalization method. We analyzed the total spin, spin–spin correlation functions, local magnetic moments, and spin and charge gaps as a function of on-site Coulomb repulsion, electron concentration, and electronic hopping parameters. Phase diagrams showed that RVB states can live in half-filled and hole-doped anisotropic triangular lattices. We found two types of RVB states: one in the honeycomb sublattice and the other in the centered hexagons in the triangular lattices. Owing to the novel discovery of exotic magnetic ordering in triangular moiré patterns in twisted bilayer graphene and transition metal dichalcogenide systems, our results provide physical insights into the onset of magnetism and possible spin liquid states in these layered materials.

Deconfined quantum criticality of nodal d -wave superconductivity, Néel order, and charge order on the square lattice at half-filling

We consider a SU(2) lattice gauge theory on the square lattice, with a single fundamental complex fermion and a single fundamental complex boson on each lattice site. Projective symmetries of the gauge-charged fermions are chosen so that they match with those of the spinons of the π-flux spin liquid. Global symmetries of all gauge-invariant observables are chosen to match with those of the particle-hole symmetric electronic Hubbard model at half-filling. Consequently, both the fundamental fermion and fundamental boson move in an average background π-flux, their gauge-invariant composite is the physical electron, and eliminating gauge fields in a strong gauge-coupling expansion yields an effective extended Hubbard model for the electrons. The SU(2) gauge theory displays several confining/Higgs phases: a nodal d-wave superconductor, and states with Néel, valence-bond solid, charge, or staggered current orders. There are also a number of quantum phase transitions between these phases that are very likely described by (2+1)-dimensional deconfined conformal gauge theories, and we present large flavor expansions for such theories. These include the phenomenologically attractive case of a transition between a conventional insulator with a charge gap and Néel order, and a conventional d-wave superconductor with gapless Bogoliubov quasiparticles at four nodal points in the Brillouin zone. We also apply our approach to the honeycomb lattice, where we find a bicritical point at the junction of Néel, valence bond solid (Kekulé), and Dirac semimetal phases. Published by the American Physical Society 2024

Microscopic Model for Fractional Quantum Hall Nematics.

Geometric fluctuations of the density mode in a fractional quantum Hall (FQH) state can give rise to a nematic FQH phase, a topological state with a spontaneously broken rotational symmetry. While experiments on FQH states in the second Landau level have reported signatures of putative FQH nematics in anisotropic transport, a realistic model for this state has been lacking. We show that the standard model of particles in the lowest Landau level interacting via the Coulomb potential realizes the FQH nematic transition, which is reached by a progressive reduction of the strength of the shortest-range Haldane pseudopotential. Using exact diagonalization and variational wave functions, we demonstrate that the FQH nematic transition occurs when the system's neutral gap closes in the long-wavelength limit while the charge gap remains open. We confirm the symmetry-breaking nature of the transition by demonstrating the existence of a "circular moat" potential in the manifold of states with broken rotational symmetry, while its geometric character is revealed through the strong fluctuations of the nematic susceptibility and Hall viscosity.

Strongly correlated electron system NiWO4: A new family of materials for triboelectrics using inherent Coulombic repulsion

The strongly correlated electron system (SCES) insulators promise a wide range of intriguing physical phenomena arising from the exotic charge gap depending on the strength of the Coulombic repulsion between d and f orbital cations. The SCES exhibits polaron hopping conduction, which requires a higher activation energy for carrier conduction between nearest cations, indicating a strong insulating character with relatively high permittivity. Here, we demonstrate that the NiWO4 SCES insulator, which is formed by Coulombic repulsion between the nearest d orbital of Ni, proposes a suitable triboelectric material unlisted system from conventional metal oxides. The higher degree of freedom in NiWO4 by the lower symmetry of monoclinic structure and an additional selection of composition exhibits high relative permittivity (∼13.8) in a wide range of temperatures (up to 180 ℃). The optimized simple mixture of NiWO4 and PDMS (polydimethylsiloxane) for the negatively charged material to triboelectric nanogenerator (TENG) presents 1.78 times higher output compared to the pristine PDMS film-based TENG. NiWO4, considering the physical properties of the SCES determined by Coulombic repulsion strength, paves the way for a new option of TENG materials following the high permittivity.

Charged spinning fermionic configurations and a mass gap

We consider a self-consistent axially symmetric system supported by a classical nonlinear spinor field minimally coupled to electric and magnetic Maxwell fields. The presence of the nonlinearity of the spinor field ensures the existence of a minimum positive energy of the system (a mass gap), of a minimum charge (a charge gap), and of a minimum magnetic moment. In turn, the presence of the electric charge results in qualitative changes in the behavior of physical characteristics of the systems under consideration as compared with the case of an electrically neutral spinor field. It is shown that, with a suitable choice of free system parameters, there exists a regular finite-energy particlelike solution describing a localized spinning object whose physical parameters correspond to the main characteristics of an electron/positron (including the spin equal to 1/2), but with the characteristic size comparable to the corresponding Compton wavelength. Also, we show that four local Dirac equations are equivalent to two nonlocal equations.

Highly Efficient Photocatalytic Remediation of Carcinogenic Anthracene and Phenanthrene by green Synthesized N‐doped Prussian blue Analogues

AbstractPolycyclic aromatic hydrocarbons (PAHs) are classified as priority pollutants because of their persistent nature, carcinogenicity, and mutagenicity; therefore, they must be eliminated. Herein, synthesis of nitrogen‐doped metal hexacyanoferrate nanoparticles (N−MHCF; M=Cu, Zn) was achieved using the green protocol in co‐precipitation techniques for the oxidative removal of PAH pollutants, namely, anthracene (ANT) and phenanthrene (PHE). PXRD and XPS analysis confirmed the doping of Nitrogen in MHCF nanocomposite. The optimum conditions, concentration of PAHs (10 mg L−1), and catalyst dose (20 mg) at neutral pH under sunlight to eliminate PAHs were reported. The degradation followed the Langmuir model and Ist‐order kinetics. The highest photodegraFdation was found for N−CuHCF (ANT: 95 %; PHE: 93 %), as compared to N−ZnHCF (ANT: 90 %; PHE: 87 %), which might be due to a high negative zeta charge (−30.3 mV), surface area, and lower band gap energy (1.7 eV). The GC‐MS technique showed that photocatalysts (N−MHCF) break down PAH contaminants into minor metabolites in exposure to solar irradiation. Up to eight consecutive cycles of use were possible with nanocomposites without any appreciable decrease in activity. Largely because of favorable surface characteristics, N−MHCF nanostructure fabricated via the green method is of great importance with a bright future in industries.

The undecidable charge gap and the oil drop experiment

The undecidable charge gap and the oil drop experiment

Thermodynamics of resonating-valence-bond states toward the understanding of quantum spin liquid phenomena.

A quantum spin liquid (QSL) is a state of matter in which spins do not exhibit magnetic order. In contrast to paramagnets, the spins in a QSL interact strongly, similar to conventional ordered magnets; however the thermodynamic stability of QSLs is rarely studied. Here, the thermodynamic properties of centered hexagon nanoclusters were investigated using the Hubbard model, which was solved using exact numerical diagonalization. The total spin, spin-spin correlation functions, local magnetic moments, charge and spin gaps, and magnetocaloric effect were analyzed for a half-filled band as a function of the ratio between the on-site Coulomb repulsion and electronic hopping (U/t). The centered hexagon nanocluster exhibited an antiferromagnetic (AFM) behavior with exotic magnetic ordering. Resonating-valence-bond (RVB) states were observed for intermediate values of U/t, in which short-range spin-spin correlation functions were suppressed to minimize spin frustration. The AFM order was examined in terms of the Néel-like temperature derived from the temperature dependence of the magnetic susceptibility. An interesting result is that the systems under external magnetic fields exhibited an inverse magnetocaloric effect, which was remarkable for intermediate values of U/t, where the RVB state was observed. Owing to the novel discovery of exotic magnetic ordering in triangular moiré patterns in twisted bilayer graphene (TBLG) systems, these results provide insights into the onset of magnetism and the possible spin liquid states in these graphene moiré materials.

Vanadium in strongly correlated electron system Ni1-xVxWO4: Paradoxically boosted deNOx reaction under SOx environment via modulating electron correlation

The persistent challenge of NOx selective catalytic reduction degradation in the presence of SOx has remained unresolved for decades. In this study, we report a paradoxical boosted denitration performance more than 20% under the SOx environment through controlling the charge state of V utilizing strongly correlated electron systems (SCES) in Ni1−xVxWO4. Substitutional doped V at the Ni site, and the computed charge gap from DFT confirms the SCES. Through the manipulation of the strong correlation between V and Ni, V preserves the between + 2–3 charge state in the presence of SOx. Furthermore, we achieved a stable oxidation/reduction cycle and higher denitration efficiency by altering the oxidation point of (NH4)HSO4-contaminated Ni1−xVxWO4. This results from deliberate decrease in Coulombic repulsion between Ni and V, improving electron transfer for catalytic performance. This revelation offers a resolution of exceptional denitration performance within SOx in industrial exhaust systems, exploiting the foundational principles of SCES.

Charge and spin gaps in the ionic Hubbard model with density-dependent hopping

Charge and spin gaps in the ionic Hubbard model with density-dependent hopping

A New Charge-Ordered Molecular Conductor: κ-(BEDT-TTF)2K+(18-crown-6)[CoII(NCS)4]∙(H2O)

A new molecular conductor, i.e., κ-(BEDT-TTF)2K+(18-crown-6)[CoII(NCS)4]∙(H2O), is semiconductive with substantial charge gap values (ΔE) of 0.57 eV (measured) and 0.37 eV (calculated). There is a full band separation despite formal average charge on BEDT-TTF of +0.5 and κ(kappa)-type packing of BEDT-TTF dimers that favors high conductivity. X-ray crystal structure analysis reveals complete charge ordering with full Coulomb charge on unique BEDT-TTF radical cations A (QA = +1), while unique molecules B are uncharged (QB = 0). Geometries of A (flat) and B (bent) differ considerably and are in accordance with the ascribing charges. Charge segregation is enhanced by forming tight face-to-face BEDT-TTF dimers AA (QAA = +2) and BB (QBB = 0). Strongly interacting double-charged dimers AA form “superstripes” running along a that are interleaved along b with chains of neutral dimers BB. Peculiar extremely thick (13.7 Å) four-decker insulating anion layers cast strong Coulomb potential onto the conductive layers predetermining charge localization in the latter.

Calcium oxide nanoparticles: Biosynthesis, characterization and photocatalytic activity for application in yellow tartrazine dye removal

Dyes are substances that have a high polluting potential, due to their low biodegradability and chemical stability, causing serious environmental damage when disposed of incorrectly. Yellow tartrazine (YT) dye as an environmental liability requires attention, since it causes toxic effects in fish (Danio rerio) with a potential allergic effect in humans. In this context, the present study aims to synthesize and characterize calcium oxide nanoparticles (CaO-NPs) to evaluate the photocatalytic activity for the YT photodegradation under visible irradiation. CaO-NPs were synthesized by the biosynthesis method from golden linseed (Linum usitatissimum L.) extract. Central Composite Rotational Design (CCRD 23) was used to determine the ideal condition for the photocatalytic tests. X-ray diffraction (XRD), zeta potential (ZP), physical adsorption of N2, zero charge point (pHzcp), Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy (ATR-FTIR), Scanning Electron Microscopy by Energy Dispersive Spectroscopy (SEM-EDS), Diffuse Reflectance Spectroscopy (DRS) and Field Emission Gun – Scanning Electron Microscope (FEG-SEM) were used to the CaO-NPs characterization. Thus, CaO-NPs presented SBET = 14±0.02 m2g−1, Dp = 20.9±0.02 nm and Vp = 0.054±0.004 cm3g−1, characteristic of a mesoporous material. ATR-FTIR spectrum showed characteristic stretches of specific functional groups (–CH, –CO, C = C, Ca-O, –OH) from plant extract and metallic precursor. CaO-NPs showed pHZCP equal to 7.74, positive surface charge (+12.7 mV) and bang gap energy of 2.61 eV. FEG-SEM micrographs showed that has a small agglomeration with defined morphology, but with irregular particle size (around 48 nm), and SEM-EDS micrographs showed an elemental composition (in weight) of the 50.24% oxygen, 3.32% magnesium, 2.29% iron, 10.44% calcium, 14.07% silicon, 3.33% aluminum and 0.63% potassium. Regarding CCRD 23, the ideal condition was the pH = 7.0, [CaO-NPs] = 1.2 g/L and [YT] = 20 mg/L, with 76.2% of photodegradation and a pseudo first-order reaction specific reaction rate k = 0.089 min−1. After V cycles of CaO-NPs recycling, there was a decrease of around 22.83%, indicating a saturation of the active sites available in the nanocatalyst Therefore, CaO-NPs showed potential application for TY photodegradation to be used in wastewater treatment being an alternative nanocatalyst, meeting nanotechnology and sustainable development.

Unconventional room-temperature carriers in the triangular-lattice Mott insulator TbInO3

The strong correlations between electrons in Mott insulator materials may produce highly entangled many-body states with unconventional emergent excitations. The signatures of such excitations, if any, are commonly believed to be observable only at low temperatures. Here, we challenge this common belief and show using terahertz time-domain spectroscopy that exotic carriers exist even at room temperature in TbInO3, a candidate material for realizing a low-temperature quantum spin-liquid phase. In particular, over the entire temperature range of 1.5–300 K, we observe a quadratic frequency dependence in the real part of the in-plane optical conductivity as well as Fano asymmetry of an optical phonon mode strongly interacting with the excitation continuum. These features are robust even under external magnetic fields of up to 7 T. Our data confirm the presence of emergent charge carriers within the Mott charge gap of TbInO3, suggesting that it is possible to probe and manipulate highly entangled quantum many-body states at room temperature.

Charge gap in SU(3) Yang–Mills-plus-nonlinear-spinor-field theory

Particlelike solutions in SU(3) gauge Yang–Mills theory with color magnetic and electric fields sourced by a nonlinear spinor field are obtained. The asymptotic behavior of these fields is studied. It is shown that the electric field exhibits the Coulomb asymptotic behavior, and one of the color components of the magnetic field behaves asymptotically as the field of a magnetic dipole. This allows one to determine the corresponding charge and magnetic moment. It is shown that profiles of the color charge and magnetic moment have global minima, which may be called charge and magnetic moment gaps. The relationship between the total energy of the system and the color charge is obtained. The physical reason for the appearance of the mass, charge, and magnetic moment gaps in the theory under consideration is discussed.

Itinerant spin polaron and metallic ferromagnetism in semiconductor moiré superlattices

Itinerant spin polaron and metallic ferromagnetism are theoretically predicted in the Mott insulator in semiconductor moir\'e superlattices doped below and above half filling of the narrow moir\'e band, respectively. The existence of a spin polaron can be directly identified from the kink in the dependence of the charge gap on the magnetic field.

In Vitro Safety Assessment of In-House Synthesized Titanium Dioxide Nanoparticles: Impact of Washing and Temperature Conditions.

Titanium dioxide nanoparticles (TiO2 NPs) have been widely used in food, cosmetics, and biomedical research. However, human safety following exposure to TiO2 NPs remains to be fully understood. The aim of this study was to evaluate the in vitro safety and toxicity of TiO2 NPs synthesized via the Stöber method under different washing and temperature conditions. TiO2 NPs were characterized by their size, shape, surface charge, surface area, crystalline pattern, and band gap. Biological studies were conducted on phagocytic (RAW 264.7) and non-phagocytic (HEK-239) cells. Results showed that washing amorphous as-prepared TiO2 NPs (T1) with ethanol while applying heat at 550 °C (T2) resulted in a reduction in the surface area and charge compared to washing with water (T3) or a higher temperature (800 °C) (T4) and influenced the formation of crystalline structures with the anatase phase in T2 and T3 and rutile/anatase mixture in T4. Biological and toxicological responses varied among TiO2 NPs. T1 was associated with significant cellular internalization and toxicity in both cell types compared to other TiO2 NPs. Furthermore, the formation of the crystalline structure induced toxicity independent of other physicochemical properties. Compared with anatase, the rutile phase (T4) reduced cellular internalization and toxicity. However, comparable levels of reactive oxygen species were generated following exposure to the different types of TiO2, indicating that toxicity is partially driven via non-oxidative pathways. TiO2 NPs were able to trigger an inflammatory response, with varying trends among the two tested cell types. Together, the findings emphasize the importance of standardizing engineered nanomaterial synthesis conditions and evaluating the associated biological and toxicological consequences arising from changes in synthesis conditions.

Effects of the intramolecular structural change on the superconducting phase of the TMTTF systems

The tetramethyltetrathiafulvalene (TMTTF) system is one of the key materials to reveal mechanisms for unconventional superconductivity which is driven by electronic correlation. Recent experimental studies show that only the SbF6 salt, which exhibit the strongest charge order among the PF6 and AsF6 and SbF6 salts have anomalously high superconducting phase transition pressure for the insulating-superconducting phase and superconducting-metallic phase transitions. To investigate the relationship between the superconductivity and the strength of the charge order of these salts, we constructed an extended Hubbard model with the periodic boundary condition that takes into account the site-deformation potential driven by the intramolecular structural change which causes the nonuniform charge order. The superconductivity was examined by the Drude weight and the charge gap obtained by exact diagonalization. It was found that site-deformation potentials driven by the intramolecular conformational change, even small changes, move the insulator-superconductor transition point to higher pressure, i.e. too large transfer integrals. Without the site-deformation potentials, the transfer integral at the transition point is too small as compared with those values deduced from the first-principles calculations at the structures under atmospheric pressure and it is difficult to reproduce the transition.