Intersite Coulomb Interaction Research Articles

Antiferromagnitnyy eksitonnyy dielektrik

The effective the two-band Hamiltonian is obtained for iridium oxides with account for strong electron correlations (SEC) and the spin–orbit interaction. The intraatomic electron correlations in iridium ions induce the formation of Hubbard fermions (HF) filling the states in the valence band. Another consequence of SEC is associated with the emergence of the antiferromagnetic (AFM) exchange interaction between HF in accordance with the Anderson mechanism. As a result, a long-range antiferromagnetic order is established in the system, and in the conditions of band overlapping, the intersite Coulomb interaction induces a phase transition to the excitonic insulator (EI) state with a long-range AFM order. The system of integral self-consistent equations, the solution to which determines the excitonic order parameter components Δi, j(k), sublattice magnetization M, Hubbard fermion concentration nd, and chemical potential μ, is obtained using the atomic representation, the method of two-time temperature Green’s functions, and the Zwanzig–Mori projection technique. The symmetry classification of AFM EI phases is performed, and it is shown that in the nearest neighbor approximation, state Δi, j(k) with the s-type symmetry corresponds to the ground state, while the phases with the d- and p-symmetries are metastable.

Role of inter-site Coulomb interaction on the thermodynamic and ground state properties within the [formula omitted] model

In this work, we report the effect of nearest neighbor (NN) inter-site Coulomb interaction (V) with a certain finite value of on-site Coulomb repulsion (U) and NN antiferromagnetic exchange interaction (J) in the context of high-Tc cuprates. An exact diagonalization method has been applied in a 2D t−J−U model extended by NN inter-site Coulomb interaction in the tilted square cluster near optimal doping. The antiferromagnetic tendency is suppressed by the inter-site e−e repulsion. The inter-site Coulomb repulsion produces an effective on-site attraction between electrons, resulting in the creation of doublons against the on-site Coulomb repulsion. The computation of binding energy demonstrates the binding of holes for small U/t, resulting from the interplay between U and V. Superconductivity arises in a limited window of V depending on U. However, the effective dominance of either U or V results in the annihilation of these hole pairs. The presence of two peaks in specific heat is caused by two Coulomb interactions. The development of doublons as V increases leads to a more ordered state, lowering entropy. The thermodynamic properties also show that the t−J−U−V model acts as an attractive Hubbard model for U<V. However, a pure attractive t−J−U model cannot explain these phenomenologies.

Melting of electronic/excitonic crystals in 2D semiconductor moiré patterns: A perspective from the Lindemann criterion

Using the Lindemann criterion, we analyzed the quantum and thermal melting of electronic/excitonic crystals recently discovered in two-dimensional (2D) semiconductor moiré patterns. We show that the finite 2D screening of the atomically thin material can suppress (enhance) the inter-site Coulomb (dipolar) interaction strength, thus inhibits (facilitates) the formation of the electronic (excitonic) crystal. Meanwhile, a strong enough moiré confinement is found to be essential for realizing the crystal phase with a wavelength near 10 nm or shorter. From the calculated Lindemann ratio which quantifies the fluctuation of the site displacement, we estimate that the crystal will melt into a liquid above a critical temperature ranging from several tens Kelvin to above 100 K (depending on the system parameters).

Effects of Coulomb Blockade on the Charge Transport through the Topological States of Finite Armchair Graphene Nanoribbons and Heterostructures.

In this study, we investigate the charge transport properties of semiconducting armchair graphene nanoribbons (AGNRs) and heterostructures through their topological states (TSs), with a specific focus on the Coulomb blockade region. Our approach employs a two-site Hubbard model that takes into account both intra- and inter-site Coulomb interactions. Using this model, we calculate the electron thermoelectric coefficients and tunneling currents of serially coupled TSs (SCTSs). In the linear response regime, we analyze the electrical conductance (Ge), Seebeck coefficient (S), and electron thermal conductance (κe) of finite AGNRs. Our results reveal that at low temperatures, the Seebeck coefficient is more sensitive to many-body spectra than electrical conductance. Furthermore, we observe that the optimized S at high temperatures is less sensitive to electron Coulomb interactions than Ge and κe. In the nonlinear response regime, we observe a tunneling current with negative differential conductance through the SCTSs of finite AGNRs. This current is generated by electron inter-site Coulomb interactions rather than intra-site Coulomb interactions. Additionally, we observe current rectification behavior in asymmetrical junction systems of SCTSs of AGNRs. Notably, we also uncover the remarkable current rectification behavior of SCTSs of 9-7-9 AGNR heterostructure in the Pauli spin blockade configuration. Overall, our study provides valuable insights into the charge transport properties of TSs in finite AGNRs and heterostructures. We emphasize the importance of considering electron-electron interactions in understanding the behavior of these materials.

Precise dd excitations and commensurate intersite Coulomb interactions in the dissimilar cuprates YBa2Cu3O7–y and La2–xSrxCuO4

Using high-resolution extreme ultraviolet resonant inelastic X-ray scattering (EUVRIXS) spectroscopy at Cu M-edge, we observed the doping dependent spectral shifts of inter-orbital (dd) excitations of YBa_2Cu_3O_(7-x) and La_(2-x)Sr_xCuO_4. With increasing hole doping level from undoped to optimally doped superconducting compositions, the leading edge of dd excitations is found to shift towards lower energy loss in a roughly linear trend that is irrespective to the cuprate species. The magnitude of energy shift can be explained by including a 0.15 eV Coulomb attraction between Cu 3d_(x^2-y^2) electrons and the doped holes on the surrounding oxygens in the atomic multiplet calculations. The consistent energy shift between distinct cuprate families suggests that this inter-site Coulomb interaction energy scale is relatively material-independent, and provides an important reference point for understanding charge density wave phenomena in the cuprate phase diagram.

Intersite Coulomb Interactions in Charge-Ordered Systems.

Using abinitio approaches for extended Hubbard interactions coupled to phonons, we reveal that the intersite Coulomb interaction plays important roles in determining various distinctive phases of the paradigmatic charge-ordered materials of Ba_{1-x}K_{x}AO_{3} (A=Bi and Sb). We demonstrated that all their salient doping dependent experiment features such as breathing instabilities, anomalous phonon dispersions, and transition between charge-density wave and superconducting states can be accounted for very well if self-consistently obtained nearest neighbor Hubbard interactions are included, thus establishing a minimal criterion for reliable descriptions of spontaneous charge orders in solids.

Spin and charge modulations of a half-filled extended Hubbard model

We introduce and analyze an extended Hubbard model, in which intersite Coulomb interaction as well as a staggered local potential (SLP) are considered, on the square lattice at half band filling, in the thermodynamic limit. Using both Hartree-Fock approximation and Kotliar and Ruckenstein slave boson formalism, we show that the model harbors charge order (CO) as well as joint spin and charge modulations (SCO) at finite values of the SLP, while the spin density wave (SDW) is stabilized for vanishing SLP, only. We determine their phase boundaries and the variations of the order parameters in dependence on the SLP, as well as on the on-site and nearest-neighbor interactions. Domains of coexistence of CO and SCO phases, suitable for resistive switching experiments, are unraveled. We show that the novel SCO systematically turns into the more conventional SDW phase when the zero-SLP limit is taken. We also discuss the nature of the different phase transitions, both at zero and finite temperature. In the former case, no continuous CO to SDW (or SCO) phase transition occurs. In contrast, a paramagnetic phase (PM), which is accompanied with continuous phase transitions towards both spin or charge ordered phases, sets in at finite temperature. A good quantitative agreement with numerical simulations is demonstrated, and a comparison between the two used approaches is performed.

Effect of strong intersite Coulomb interaction on the topological properties of a superconducting nanowire

For superconducting nanowire with the pairing of extended s-type symmetry, Rashba spin-orbit interaction in a magnetic field, the influence of strong intersite charge correlations on single-particle Majorana excitations is analyzed. This problem is investigated on the basis of the density matrix renormalization group numerical method. It is shown that with an increase in the repulsion intensity of electrons located at the neighboring sites, two subbands emerge in the lower Hubbard band of the open system. Based on calculations of the Majorana polarization and degeneracy of the entanglement spectrum, it was found that a topologically nontrivial phase with one edge state survives at the edge of each of the subbands where the concentration of electrons or holes is minimal. Keywords: superconducting nanowires, Majorana zero modes, strong electron correlations.

Effect of strong intersite Coulomb interaction on the topological properties of a superconducting nanowire

For superconducting nanowire with the pairing of extended s-type symmetry, Rashba spin-orbit interaction in a magnetic field, the influence of strong intersite charge correlations on single-particle Majorana excitations is analyzed. This problem is investigated on the basis of the density matrix renormalization group numerical method. It is shown that with an increase in the repulsion intensity of electrons located at the neighboring sites, two subbands emerge in the lower Hubbard band of the open system. Based on calculations of the Majorana polarization and degeneracy of the entanglement spectrum, it was found that a topologically nontrivial phase with one edge state survives at the edge of each of the subbands where the concentration of electrons or holes is minimal. Keywords: superconducting nanowires, Majorana zero modes, strong electron correlations.

Quantum spin liquid and cluster Mott insulator phases in the Mo3O8 magnets

We unveil the microscopic origin of largely debated magnetism in the Mo3O8 quantum systems. Upon considering an extended Hubbard model at 1/6 filling on the anisotropic kagomé lattice formed by the Mo atoms, we argue that its ground state is determined by the competition between kinetic energy and intersite Coulomb interactions, which is controlled by the trimerisation of the kagomé lattice into the Mo3O13 clusters, and the sign of hopping parameters, specifying the electron localisation at such clusters. Based on first-principles calculations, we show that the strong interaction limit reveals a plaquette charge order with unpaired spins at the resonating hexagons that can be realised in LiZn2Mo3O8, and whose origin is solely related to the opposite signs of intracluster and intercluster hoppings, in contrast to all previous scenarios. On the other hand, both Li2InMo3O8 and Li2ScMo3O8 are demonstrated to fall into the weak interaction limit where the electrons are well localised at the Mo3O13 clusters. While the former is found to exhibit long-range antiferromagnetic order, the latter is more likely to reveal short-range order with quantum spin liquid-like excitations. Our results not only reproduce most of the experimentally observed features of the Mo3O8 systems, but will also help to describe various properties in other quantum cluster magnets.

Ultrabosonic behavior in photoexcited one-dimensional Mott insulators in the region of weak intersite Coulomb interaction

This paper reports a unique behavior expected for the optical excitations in one-dimensional Mott insulators. When the intersite Coulombic attraction does not work between two elementary charge excitations, i.e., a doublon and a holon, the lowest optical excitations are described as an unbound pair of them, still having finite mutual correlation due to the forbidden double occupancy on the same site. We find that, in such a situation, the pairs obey a particle statistics that exceeds that of ordinary bosons. This feature appears most directly in the enhancement factor of the matrix element for the pair photocreation. We discuss the possible mechanism for this ultrabosonic behavior and also demonstrate that this behavior is maintained even if we include a small amount of interiste Coulomibic interaction. Lastly, this enhancement factor almost coincides with that for ordinary bosons when the degree of the intersite interaction exceeds a certain value that switches on the formation of a bound doublon-holon pair.

Extended Falicov-Kimball model at weak onsite and intersite Coulomb interactions

We analyze in detail a behavior of the order parameter in the half-filled extended Falicov-Kimball model for small Coulomb interactions (both onsite U and intersite V). The parameter is defined as the difference of localized electron concentrations in both sublattices of the Bethe lattice (in the limit of large coordination number). Using two methods, namely, the dynamic mean field theory and the Hartree-Fock approximation, we found the ranges of U and V for which the anomalous temperature dependence of the order parameter, characterized by the sharp reduction near T ≈ TC /2, occurs (TC is the temperature of the continuous order-disorder transition). In order to quantitatively describe this anomaly, we defined a function that measures the departure of the order parameter dependence from the standard mean-field S=1/2 Ising-like curve. We determined the U-dependent critical value VTC of V above which the anomaly disappears. Indicators of the anomalous behavior of the parameter dependence can be also observed in the temperature dependence of the specific heat.

First-principles study of two-dimensional ferroelectrics using self-consistent Hubbard parameters

The discovery of two-dimensional (2D) materials possessing switchable spontaneous polarization with atomic thickness opens up exciting opportunities to realize ultrathin, high-density electronic devices with potential applications ranging from memories and sensors to photocatalysis and solar cells. First-principles methods based on density functional theory (DFT) have facilitated the discovery and design of 2D ferroelectrics (FEs). However, DFT calculations employing local and semilocal exchange-correlation functionals failed to predict accurately the band gaps for this family of low-dimensional materials. Here, we present a DFT+$U$+$V$ study on 2D FEs represented by single-layer $\alpha$-In$_2$Se$_3$ and its homologous III$_2$-VI$_3$ compounds with both out-of-plane and in-plane polarization, using Hubbard parameters computed from first-principles. We find that ACBN0, a pseudo-hybrid density functional that allows self-consistent determination of $U$ parameters, improves the prediction of band gaps for all investigated 2D FEs with a computational cost much lower than the hybrid density functional. The inter-site Coulomb interaction $V$ becomes critical for accurate descriptions of the electronic structures of van der Waals heterostructures such as bilayer In$_2$Se$_3$ and In$_2$Se$_3$/InTe. Pertinent to the study of FE-based catalysis, we find that the application of self-consistent $U$ corrections can strongly affect the adsorption energies of open-shell molecules on the polar surfaces of 2D FEs.

Nonlocal Coulomb interaction and spin-freezing crossover as a route to valence-skipping charge order

Multiorbital systems away from global half-filling host intriguing physical properties promoted by Hund’s coupling. Despite increasing awareness of this regime dubbed Hund’s metal, effect of nonlocal interaction is still elusive. Here we study a three-orbital model with 1/3 filling (two electrons per site) including the intersite Coulomb interaction (V). Using the GW plus extended dynamical mean-field theory, the valence-skipping charge order transition is shown to be driven by V. Most interestingly, the instability to this transition is significantly enhanced in the spin-freezing crossover regime, thereby lowering the critical V to the formation of charge order. This behavior is found to be closely related to the population profile of the atomic multiplet states in the spin-freezing regime. In this regime, maximum spin states are dominant in each total charge subspace with substantial amount of one- and three-electron occupations, which leads to almost equal population of one- and the maximum spin three-electron state. Our finding unveils another feature of the Hund’s metal and has potential implications for the broad range of multiorbital systems as well as the recently discovered charge order in iron pnictides.

ZQ Berry phase for higher-order symmetry-protected topological phases

We propose the $\mathbb{Z}_Q$ Berry phase as a topological invariant for higher-order symmetry-protected topological (HOSPT) phases for two- and three-dimensional systems. It is topologically stable for electron-electron interactions assuming the gap remains open. As a concrete example, we show that the Berry phase is quantized in $\mathbb{Z}_4$ and characterizes the HOSPT phase of the extended Benalcazar-Bernevig-Hughes (BBH) model, which contains the next-nearest neighbor hopping and the intersite Coulomb interactions. In addition, we introduce the $\mathbb{Z}_4$ Berry phase for the spin-model-analog of the BBH model, whose topological invariant has not been found so far. Furthermore, we demonstrate the Berry phase is quantized in $\mathbb{Z}_4$ for the three-dimensional version of the BBH model. We also confirm the bulk-corner correspondence between the $\mathbb{Z}_4$ Berry phase and the corner states in the HOSPT phases.

Bandwidth renormalization due to the intersite Coulomb interaction

The theory of correlated electrons is currently moving beyond the paradigmatic Hubbard U, towards the investigation of intersite Coulomb interactions. Recent investigations have revealed that these interactions are relevant for the quantitative description of realistic materials. Physically, intersite interactions are responsible for two rather different effects: screening and bandwidth renormalization. We use a variational principle to disentangle the roles of these two processes and study how appropriate the recently proposed Fock treatment of intersite interactions is in correlated systems. The magnitude of this effect in graphene is calculated based on cRPA values of the intersite interaction. We also apply the variational principle to benzene and find effective parameters comparable to those obtained by ab initio density matrix downfolding.

Magnetic field control of current through model graphene nanosheets

We study magnetic field control of current through model graphene nanosheet junctions within the framework of the tight-binding approximation. Geometrical asymmetry in the coupling of graphene nanosheets to the contact leads emerges as one of the most important determining factors for the magnetic field control of current. The asymmetric connection split the otherwise degenerate energy levels of the structures leading to energy-resolved transmission peaks which the applied field modulates for a transmission maximum by narrowing the energy gap between the split energy levels. Also, the contact coupling strength plays a decisive role in controlling current in small structures, while its role is significantly less in large structures that have more closely-spaced energy levels. Model calculations on a graphene nanosheet junction with inter-site Coulomb interaction is found to sustain sensitivity to the applied magnetic field. Although several factors bear direct effect on the electron transport through molecular junctions, suitably constructed graphene nanosheet junctions would greatly enhance the prospects of current control under applied magnetic fields.

Charge dynamics in strongly-correlated electronic systems

We consider the dynamic charge susceptibility and the charge density waves in strongly-correlated electronic systems within the two-dimensional t-J-V model. Using the equation of motion method for the relaxation functions in terms of the Hubbard operators, we calculate the static susceptibility and the spectrum of charge fluctuations as functions of doped hole concentrations and temperature. Charge density waves emerge for a sufficiently strong intersite Coulomb interaction. Calculation of the dynamic charge susceptibility reveals a strong damping of charge density waves for a small hole doping and propagating high-energy charge excitations at large doping.

Atomization of correlated molecular-hydrogen chain: A fully microscopic variational Monte Carlo solution

We discuss electronic properties and their evolution for the linear chain of $H_2$ molecules in the presence of a uniform external force $f$ acting along the chain. The system is described by an extended Hubbard model within a fully microscopic approach. Explicitly, the microscopic parameters describing the intra- and inter-site Coulomb interactions are determined together with the hopping integrals by optimizing the system ground state energy and the single-particle wave functions in the correlated state. The many-body wave function is taken in the Jastrow form and the Variational Monte-Carlo (VMC) method is used in combination with an ab initio approach to determine the energy. Both the effective Bohr radii of the renormalized single-particle wave functions and the many-body wave function parameters are determined for each $f$. Hence, the evolution of the system can be analyzed in detail as a function of the equilibrium intermolecular distance, which in turn is determined for each $f$ value. The transition to the atomic state, including the Peierls distortion stability, can thus be studied in a systematic manner, particularly near the threshold of the dissociation of the molecular into atomic chain. The computational reliability of VMC approach is also estimated.

Exciton-phonon cooperative mechanism of the triple- q charge-density-wave and antiferroelectric electron polarization in TiSe2

We investigate the microscopic mechanisms of the charge-density-wave (CDW) formation in a monolayer TiSe$_2$ using a realistic multiorbital $d$-$p$ model with electron-phonon coupling and intersite Coulomb (excitonic) interactions. First, we estimate the tight-binding bands of Ti $3d$ and Se $4p$ orbitals in the monolayer TiSe$_2$ on the basis of the first-principles band structure calculations. We thereby show orbital textures of the undistorted band structure near the Fermi level. Next, we derive the electron-phonon coupling using the tight-binding approximation and show that the softening occurs in the transverse phonon mode at the M point of the Brillouin zone. The stability of the triple-$q$ CDW state is thus examined to show that the transverse phonon modes at the M$_1$, M$_2$, and M$_3$ points are frozen simultaneously. Then, we introduce the intersite Coulomb interactions between the nearest-neighbor Ti and Se atoms that lead to the excitonic instability between the valence Se $4p$ and conduction Ti $3d$ bands. Treating the intersite Coulomb interactions in the mean-field approximation, we show that the electron-phonon and excitonic interactions cooperatively stabilize the triple-$q$ CDW state in TiSe$_2$. We also calculate a single-particle spectrum in the CDW state and reproduce the band folding spectra observed in photoemission spectroscopies. Finally, to clarify the nature of the CDW state, we examine the electronic charge density distribution and show that the CDW state in TiSe$_2$ is of a bond-type and induces a vortex-like antiferroelectric polarization in the kagome network of Ti atoms.