Coulomb Repulsion Energy Research Articles

Mott interactions driven insulating behaviour in ruthenium based double perovskites: A2SmRuO6 (A = Ba & Sr)

Double perovskites (DP’s) are important for understanding the diverse physical properties arising from strongly correlated interactions. According to experimental observations, the DP’s A2SmRuO6 (A = Ba & Sr) are insulators; however, first-principles calculations using GGA approximations show that they are metallic. We observed a band gap (Eg) opening of 1.3 eV for Ba2SmRuO6 (BSRO) and 1.4 eV for Sr2SmRuO6 (SSRO) upon the insertion of Hubbard parameter (U) in the theoretical computations for accounting the electron-electron interactions. Further investigations using core-level spectroscopy reveal Eg of 1.05 eV for BSRO and 0.85 eV for SSRO. Furthermore, the calculations for Δ (charge transfer energy), U (coulomb repulsion energy), and W (bandwidth) from the combined spectra show U < Δ and U/W > 1.15, which confirms these compounds be classified as Mott-Hubbard insulators. These results expand our understanding of the strongly correlated compounds around the Fermi level, which might have applications in optoelectronics.

Incorporation of neodymium, holmium, erbium, and samarium (oxides) in zinc-borotellurite glass: Physical and optical comparative analysis

Investigating the effect of different types of rare-earth oxides on zinc borotellurite glass is important to determine the potential application in optical devices. The addition of rare-earth oxides in zinc borotellurite glass is well-known to enhance the optical properties due to the effects of 4f-4f transitions. In this work, we aim to compare the effect of different rare-earth oxides on zinc borotellurite glass denoted as ZBTNd, ZBTHo, ZBTEr and ZBTSm. The glass samples were successfully fabricated via the melt-quenched technique. The physical investigation of the glasses has been done by measuring the density and molar volume. It was found that ZBTNd glass has the lowest density than the other glasses due to the small atomic radius in neodymium oxide. High-density value for ZBTHo glass shows potential to be used as radiation shielding properties. The high value of molar volume for ZBTNd glass is advantageous for fiber optics as ZBTNd glass has good performance in elasticity. It was found that ZBTEr has a lower refractive index than the other glasses due to low dispersion characteristics. However, ZBTEr glass has good performance to be used in optical communication applications. It was found that the optical absorption shifts to a longer wavelength beginning from ZBTEr &gt; ZBTHo &gt; ZBTNd &gt; ZBTSm. The optical band gap energy for ZBTEr glass is higher than the other glasses due to the Coulomb repulsion energy for erbium which is greater than neodymium and samarium and slightly higher than holmium. The pattern of electronic polarizability for all glasses was found as follows ZBTSm&gt;ZBTNd&gt;ZBTEr&gt;ZBTHo. The optical basicity for ZBTEr was found highest which indicates a higher acidity, meanwhile, the ZBTNd glass has the lowest value which corresponds to a higher basicity.

4a,4b-Dihydrophenanthrene → cis-stilbene photoconversion: TD-DFT/DFT study.

DHP → CS photoconversion was analyzed in terms of electron density redistribution for the first time. The following explanation for the non-recovery of the C4a-C4b bond upon CS relaxation is proposed: during this process, the Coulomb repulsion energy between these pairs of atoms increases by almost one and a half times, and their bonding by an electron at LUMO is insufficient to recover the C4a-C4b bond. According to calculations, upon CS relaxation, the linker connecting the benzene rings undergoes significant structural changes. In this case, the distance between the C4a and C4b atoms increases from 3.00Å to 3.28Å. Calculations showed that the C4a-C4b vibration of the DHP bond has a very low intensity. Therefore, thermal motion does not contribute to the rupture of this bond. All calculations were performed using the Gaussian16 software package at the B3LYP/6-311 + + G(d,p)/IEFPCM theory level. B3LYP was the only hybrid functional supported by Gaussian16, which ensured the cleavage of the C4a-C4b bond of DHP while optimizing its S1 excited state. A quantitative description of the redistribution of electron density in the studied conformers was carried out using the analysis of the NPA of atomic charges. Cyclohexane was used as an implicitly specified non-polar solvent. Visualization of molecular orbitals, and electron densities, as well as plotting of calculated IR spectra, were performed using the Gaussview6 software package.

Electronic correlations in epitaxial CrN thin film

Chromium nitride (CrN) spurred enormous interest due to its coupled magnetostructural and unique metal-insulator transition. The underneath electronic structure of CrN remains elusive. Herein, the electronic structure of epitaxial CrN thin film has been explored by employing resonant photoemission spectroscopy (RPES) and X-ray absorption near edge spectroscopy study in combination with the first-principles calculations. The RPES study indicates the presence of a charge-transfer screened 3d ^n{underline{L}} (L: hole in the N-2p) and 3d ^{n-1} final-states in the valence band regime. The combined experimental electronic structure along with the orbital resolved electronic density of states from the first-principles calculations reveals the presence of Cr(3d)-N(2p) hybridized (3d ^n{underline{L}}) states between lower Hubbard (3d ^{n-1}) and upper Hubbard (3d ^{n+1}) bands with onsite Coulomb repulsion energy (U) and charge-transfer energy (Delta) estimated as approx 4.5 and 3.6 eV, respectively. It verifies the participation of ligand (N-2p) states in low energy charge fluctuations and provides concrete evidence for the charge-transfer (Delta<U) insulating nature of CrN thin film.

多体問題に対する微分形式による数値厳密解

The Many-body problem is very important issue in physics. Usually perturbation calculations based on the Green's function have been used to analyze such a problem, however, infinite orders of perturbation calculations are required to obtain exact solutions, thus resulting in the analytical and numerical difficulties. To overhaul such difficulties, we propose the new calculation method based on the differential forms, which are able to evaluate exact solutions if Hamiltonian is composed of Fermi particles. Since our proposed method is based on time evolution equations, comparisons with the calculations derived from Feynman Kernel is possible, with showing complete agreement. Furthermore we applied this method to the simplest Anderson Hamiltonian to investigate the appearance of magnetic moment. The calculation results show that magnetic moment easily disappears with small Coulomb repulsive energy, possibly implying the spin fluctuations.

Two electrons interacting at a mesoscopic beam splitter.

The nonlinear response of a beam splitter to the coincident arrival of interacting particles enables numerous applications in quantum engineering and metrology. Yet, it poses considerable challenges to control interactions on the individual particle level. Here, we probe the coincidence correlations at a mesoscopic constriction between individual ballistic electrons in a system with unscreened Coulomb interactions and introduce concepts to quantify the associated parametric nonlinearity. The full counting statistics of joint detection allows us to explore the interaction-mediated energy exchange. We observe an increase from 50% up to 70% in coincidence counts between statistically indistinguishable on-demand sources and a correlation signature consistent with the independent tomography of the electron emission. Analytical modelling and numerical simulations underpin the consistency of the experimental results with Coulomb interactions between two electrons counterpropagating in a quadratic saddle potential. Coulomb repulsion energy and beam splitter dispersion define a figure of merit, which in this experiment is demonstrated to be sufficiently large to enable future applications, such as single-shot in-flight detection and quantum logic gates.

Functional Properties of Tetrameric Molecular Cells for Quantum Cellular Automata: A Quantum-Mechanical Treatment Extended to the Range of Arbitrary Coulomb Repulsion

We discuss the problem of electron transfer (ET) in mixed valence (MV) molecules that is at the core of molecular Quantum Cellular Automata (QCA) functioning. Theoretical modelling of tetrameric bi-electronic MV molecular square (prototype of basic QCA cell) is reported. The model involves interelectronic Coulomb repulsion, vibronic coupling and ET between the neighboring redox sites. Unlike the majority of previous studies in which molecular QCA have been analyzed only for particular case when the Coulomb repulsion energy significantly exceeds the ET energy, here we do not imply assumptions on the relative strength of these two interactions. Moreover, in the present work we go beyond the adiabatic semiclassical approximation often used in theoretical analysis of such systems in spite of the fact that this approximation ignores such an important phenomenon as quantum tunneling. By analyzing the electronic density distributions in the cells and the ell-cell response functions obtained from a quantum-mechanical solution of a complex multimode vibronic problem we have concluded that such key features of QCA cell as bistability and switchability can be achieved even under failure of the condition of strong Coulomb repulsion provided that the vibronic coupling is strong enough. We also show that the semiclassical description of the cell-cell response functions loses its accuracy in the region of strong non-linearity, while the quantum-mechanical approach provides correct results for this critically important region.

Effects of the Separation Distance between Two Triplet States Produced from Intramolecular Singlet Fission on the Two-Electron-Transfer Process.

To harvest two triplet excitons of singlet fission (SF) via a two-electron transfer efficiently, the revelation of the key factors that influence the two-electron-transfer process is necessary. Here, by using steady-state and transient absorption/fluorescence spectroscopy, we investigated the two-electron-transfer process from the two triplet excitons of intramolecular SF (iSF) in a series of tetracene oligomers (dimer, trimer, and tetramer) with 7,7,8,8-tetracyanoquinodimethane (TCNQ) as an electron acceptor in solution. Quantitative two-electron transfer could be conducted for the trimer and tetramer, and the rate for the tetramer is faster than that for the trimer. However, the maximum efficiency of the two-electron transfer in the dimer is relatively low (∼47%). The calculation result of the free energy change (ΔG) of the second-electron transfer for these three compounds (-0.024, -0.061, and -0.074 eV for the dimer, trimer, and tetramer, respectively) is consistent with the experimental observation. The much closer ΔG value to zero for the dimer should be responsible for its low efficiency of the two-electron transfer. Different ΔG values for these three oligomers are attributed to the different Coulomb repulsive energies between the two positive charges generated after the two-electron transfer that is caused by their various intertriplet distances. This result reveals for the first time the important effect of the Coulomb repulsive energy, which depends on the intertriplet distance, on the two-electron transfer process from the two triplet excitons of iSF.

Robust electronic and tunable magnetic states in Sm2 NiMnO6 ferromagnetic insulator

Ferromagnetic insulators (FM-Is) are the materials of interest for the new generation quantum electronic applications. Here, we have investigated the physical observables depicting FM-I ground states in epitaxial Sm2NiMnO6 (SNMO) double perovskite thin films fabricated under different conditions to realize the different level of Ni/Mn anti-site disorders (ASDs). The presence of ASDs immensely influence the characteristic magnetic and anisotropy behaviors in SNMO system by introducing short scale antiferromagnetic interactions in predominant long range FM ordered host matrix. Charge disproportion between cation sites, in the form of Ni2+ + Mn4+ → Ni3+ + Mn3+, causes mixed valency in both Ni and Mn species, which is found insensitive to ASD concentrations. Temperature dependent photo emission, photo absorption measurements duly combined with cluster model configuration interaction simulations, suggest that the eigenstates of Ni and Mn cations can be satisfactorily described as a linear combination of the unscreened d n and screened (: O 2p hole) states. The electronic structure across the Fermi level (E F) exhibits closely spaced Ni 3d, Mn 3d and O 2p states. From occupied and unoccupied bands, estimated values of the Coulomb repulsion energy (U) and ligand to metal charge transfer energy (Δ), indicate charge transfer insulating nature, where remarkable modification in Ni/Mn 3d—O 2p hybridization takes place across the FM transition temperature. Existence of ASD broadens the Ni, Mn 3d spectral features, whereas the spectral positions are found to be unaltered. Hereby, present work demonstrates SNMO thin film as a FM-I system, where the FM state can be tuned by manipulating ASD in the crystal structure, while the I state remains intact.

Difference in Coulomb Electrostatic Energy for Localized versus Delocalized Electrons and Electron Pairs—Exact Results Based on Cubic Charge Distributions

Wigner showed that a sufficiently thin electron gas will condense into a crystal of localized electrons. Here, we show, using a model based on cubic charge distributions that gives exact results, that the Coulomb repulsion energy of localized charge distributions is lower than that of delocalized distributions in spite of the fact that the total overall charge distribution is the same. Assuming a simple cubic geometry, we obtain an explicit result for the energy reduction. This reduction results from the exclusion of self-interactions of the electrons. The corresponding results for electron pairs are also discussed.

Electronic structure of superconducting nickelates probed by resonant photoemission spectroscopy

The discovery of infinite-layer nickelate superconductors has spurred enormous interest. While the Ni$^{1+}$ cations possess nominally the same 3$d^9$ configuration as Cu$^{2+}$ in cuprates, the electronic structure variances remain elusive. Here, we present a soft x-ray photoemission spectroscopy study on parent and doped infinite-layer Pr-nickelate thin films with a doped perovskite reference. By identifying the Ni character with resonant photoemission and comparison to density functional theory + U (on-site Coulomb repulsion energy) calculations, we estimate U ~5 eV, smaller than the charge transfer energy $\Delta$ ~8 eV, confirming the Mott-Hubbard electronic structure in contrast to charge-transfer cuprates. Near the Fermi level ($E_F$), we observe a signature of occupied rare-earth states in the parent compound, which is consistent with a self-doping picture. Our results demonstrate a correlation between the superconducting transition temperature and the oxygen 2$p$ hybridization near $E_F$ when comparing hole-doped nickelates and cuprates.

Rational Design of 3d Transition-Metal Compounds for Thermoelectric Properties by Using Periodic Trends in Electron-Correlation Modulation.

The electronic structures in solid-state transition-metal compounds can be represented by two parameters: the charge-transfer energy (Δ), which is the energy difference between the p-band of an anion and an upper Hubbard band contributed by transition-metal d-orbitals, and the onsite Coulomb repulsion energy (U), which represents the energy difference between lower and upper Hubbard bands composed of split d-orbitals in transition metals. These parameters can facilitate the classification of various types of electronic structures. In this study, the dependences of anion species (N3-, P3-, As3-, O2-, S2-, Se2-, Te2-, F-, Cl-, Br-, and I-) on Δ and U of 566 different binary and ternary 3d transition-metal compounds were investigated using ionic-model calculations. We were able to identify the systematic chemical trends in the variations in Δ and U values with the anion species of 11 different families of 3d transition-metal compounds in a comprehensive manner. The effective use of Δ-U diagrams given here, to facilitate the discovery and development of functional compounds, was demonstrated on thermoelectric compounds by classifying the thermoelectric properties of 3d transition-metal compounds and by predicting unrealized high-performance thermoelectric compounds.

Conjugation length effect on the conducting behavior of single-crystalline oligo(3,4-ethylenedioxythiophene) (nEDOT) radical cation salts.

The conjugation length is a unique structural factor for oligomer-based π-conjugated conductors as it modulates their electronic structures. Herein, we demonstrated the conjugation length effects on conductivity by comparing a dimer and trimer of single-crystalline oligo(3,4-ethylenedioxythiophene) radical cation salts. The dimer showed a uniform-stacked columnar structure, while the trimer showed stacked columns of the π-dimerized donor and weaker intracolumnar interactions. Nevertheless, the trimer exhibited higher conductivity, suggesting a considerable decrease in the on-site Coulomb repulsion energy of the conjugation-expanded system.

Nearly Room-Temperature Ferromagnetism in a Pressure-Induced Correlated Metallic State of the van der Waals Insulator CrGeTe_{3}.

A complex interplay of different energy scales involving Coulomb repulsion, spin-orbit coupling, and Hund's coupling energy in 2D van der Waals (vdW) material produces a novel emerging physical state. For instance, ferromagnetism in vdW charge transfer insulator CrGeTe_{3} provides a promising platform to simultaneously manipulate the magnetic and electrical properties for potential device implementation using few nanometers thick materials. Here, we show a continuous tuning of magnetic and electrical properties of a CrGeTe_{3} single crystal using pressure. With application of pressure, CrGeTe_{3} transforms from a ferromagnetic insulator with Curie temperature T_{C}∼66 K at ambient condition to a correlated 2D Fermi metal with T_{C} exceeding ∼250 K. Notably, absence of an accompanying structural distortion across the insulator-metal transition (IMT) suggests that the pressure induced modification of electronic ground states is driven by electronic correlation furnishing a rare example of bandwidth-controlled IMT in a vdW material.

Generalizing the Liquid Drop Model (LDM) to Assess (Q_β^+-value) for Nuclei in the Range of 10≤Z≤98.

In this research, a new formula of positive beta decay energy (Q_β^+-value) was obtained for light, medium and heavy nuclei (even – even, even – odd, odd – even and odd – odd) for the range of nuclei (10≤Z≤98). Instead of mass differences values, this formula is expressed in the form of nuclear binding energies. After multiple mathematical derivations, the decay energy is defined using the liquid drop model (LDM) to arrive at a final equation for the positive beta decay energy. The (Q_β^+-value) was calculated using four terms: the first term represents the symmetry energy with the opposite sign as in the liquid drop model, the second term represents the Coulomb repulsion energy, and the other two terms represent the pairing and constant (C) terms, where (C) is provided by the mass difference between the neutron and proton. In the investigation of our novel formula of (Q_β^+-value).The findings showed a good match between experimental and theoretical values, especially for heavy and medium nuclei, but a less match for light nuclei due to the presence of a magic numbers. In the investigation of our novel Q_β^+-value formula, the standard deviation (σ) was used to calculate the dependency of (LDM).

Lattice reconstruction induced multiple ultra-flat bands in twisted bilayer WSe2

Moiré superlattices in van der Waals heterostructures provide a tunable platform to study emergent properties that are absent in the natural crystal form. Twisted bilayer transition metal dichalcogenides (TB-TMDs) can host moiré flat bands over a wide range of twist angles. For twist angle close to 60°, it was predicted that TB-TMDs undergo a lattice reconstruction which causes the formation of ultra-flat bands. Here, by using scanning tunneling microscopy and spectroscopy, we show the emergence of multiple ultra-flat bands in twisted bilayer WSe2 when the twist angle is within 3° of 60°. The ultra-flat bands are manifested as narrow tunneling conductance peaks with estimated bandwidth less than 10 meV, which is only a fraction of the estimated on-site Coulomb repulsion energy. The number of these ultra-flat bands and spatial distribution of the wavefunctions match well with the theoretical predictions, strongly evidencing that the observed ultra-flat bands are induced by lattice reconstruction. Our work provides a foundation for further study of the exotic correlated phases in TB-TMDs.

Pure spin-current diode based on interacting quantum dot tunneling junction* *Project supported by the National Natural Science Foundation of China (Grant No. 11404322) and the Natural Science Foundation of Huai’an (Grant No. HAB202150).

A magnetic field-controlled spin-current diode is theoretically proposed, which consists of a junction with an interacting quantum dot sandwiched between a pair of nonmagnetic electrodes. By applying a spin bias V S across the junction, a pure spin current can be obtained in a certain gate voltage regime,regardless of whether the Coulomb repulsion energy exists. More interestingly, if we applied an external magnetic field on the quantum dot, we observed a clear asymmetry in the spectrum of spin current I S as a function of spin bias, while the charge current always decays to zero in the Coulomb blockade regime. Such asymmetry in the current profile suggests a spin diode-like behavior with respect to the spin bias, while the net charge through the device is almost zero. Different from the traditional charge current diode, this design can change the polarity direction and rectifying ability by adjusting the external magnetic field, which is very convenient. This device scheme can be compatible with current technologies and has potential applications in spintronics or quantum processing.

Dissecting Mott and charge-density wave dynamics in the photoinduced phase of 1T−TaS2

The two-dimensional transition-metal dichalcogenide 1T−TaS2 is a complex material standing out for its puzzling low temperature phase marked by signatures amenable to both Mott-insulating and charge-density wave states. Electronic Mott states, coupled to a lattice, respond to coherent optical excitations via a modulation of the lower (valence) Hubbard band. Such dynamics is driven by strong electron-phonon coupling and typically lasts for tens of picoseconds, mimicking coherent structural distortions. Instead, the response occurring at the much faster timescale, mainly dominated by electronic many-body effects, is still a matter of intense research. By performing time- and angle-resolved photoemission spectroscopy, we investigated the photoinduced phase of 1T−TaS2 and found out that its lower Hubbard band promptly reacts to coherent optical excitations by shifting its binding energy towards a slightly larger value. This process lasts for a time comparable to the optical pump pulse length, mirroring a transient change of the onsite Coulomb repulsion energy (U). Such an observation suggests that the correction to the bare value of U, ascribed to the phonon-mediated screening which slightly opposes the Hubbard repulsion, is lost within an interval of a few tens of femtoseconds and can be understood as a fingerprint of electronic states largely decoupled from the lattice. Additionally, these results enforce the hypothesis, envisaged in the current literature, that the transient photoinduced states belong to a sort of crossover phase instead of an equilibrium metallic one.

Multiplet structure for perovskite-type Ba0.9Ca0.1Ti0.9Zr0.1O3 by core–hole spectroscopies

Core–hole spectroscopies such as x-ray photoelectron spectroscopy (XPS) and high-resolution electron energy loss spectroscopy (HR-EELS) in combination with multiplet calculation are important tools to elucidate the electronic structure of transition metal compounds. This work presents a comparison between the electronic structure obtained by XPS and HR-EELS for polycrystalline perovskite-type Ba0.9Ca0.1Ti0.9Zr0.1O3. Raman analysis suggests that Ca2+ cations could partly occupy the Ti4+ cations in the B-site of a perovskite structure with the tetragonal phase. A multiplet structure was determined by XPS for Ti 2p and by HR-EELS for Ca L2,3 and Ti L2,3 edges. Octahedral (Oh) symmetry in the crystal field (CF) effects reproduces the local distortion of TiO6 octahedra. The charge transfer (CT) effects were also considered to reproduce L3-edge EELS shoulders and the satellite in the Ti 2p XPS region. CF and CT parameters, 10 Dq, (charge transfer energy) Δ, and (Coulomb repulsion energy) Udd, are reported for future reference. The broadening of the Ti L2-edge suggests the presence of the Coster–Kronig electron decay process. Multiplet calculation in Oh symmetry for the Ca L2,3-edge could support the Raman interpretation.

Gross-Pitaevskii-Poisson model for an ultracold plasma: Density waves and solitons

We introduce 1D and 2D models of a degenerate bosonic gas composed of ions with positive and negative charges (cations and anions). The system may exist in the mean-field condensate state, enabling the competition of the Coulomb coupling, contact repulsion, and kinetic energy of the particles, provided that their effective mass is reduced by means of a lattice potential. The model combines the Gross-Pitaevskii (GP) equations for the two-component wave function of the cations and anions, coupled to the Poisson equation for the electrostatic potential mediating the Coulomb coupling. The contact interaction in the GP system can be derived, in the Thomas-Fermi approximation, from a system of three GP equations, which includes the wave function of heavy neutral atoms. In the system with fully repulsive contact interactions, we construct stable spatially periodic patterns (density waves, DWs). The transition to DWs is identified by analysis of the modulational instability of a uniformly mixed neutral state. The DW pattern, which represents the system's ground state (GS), is predicted by a variational approximation. In 2D, a stable pattern is produced too, with a quasi-1D shape. The 1D system with contact self-attraction in each component produces bright solitons of three types: neutral ones, with fully mixed components; dipoles, with the components separated by the inter-species contact repulsion; and quadrupoles, with a layer of one component sandwiched between side lobes formed by the other. The transition from the neutral solitons to dipoles is accurately modeled analytically. A chart of the GSs of the different types (neutral solitons, dipoles, or quadrupoles) is produced. Different soliton species do not coexist as stable states. Collisions between traveling solitons are elastic for dipole-dipole pairs, while dipole-antidipole ones merge into stable quadrupoles via multiple collisions.