Coulomb Interaction Research Articles

Quantitative Equivalence and Performance Comparison of Particle and Field-Theoretic Simulations.

Particle and field-theoretic simulations are both commonly used methods to study the equilibrium properties of polymeric materials. Yet despite the formal equivalence of the two methods, no comprehensive comparisons of particle and field-theoretic simulations exist in the literature. In this work, we seek to fill this gap by performing a systematic and quantitative comparison of particle and field-theoretic simulations. In our comparison, we consider four representative polymeric systems: a homopolymer melt/solution, a diblock copolymer melt, a polyampholyte solution, and a polyelectrolyte gel. For each of these systems, we first demonstrate that particle and field-theoretic simulations are equivalent and yield exactly the same results for the pressure and the chemical potential. We next quantify the performance of each method across a range of different conditions including variations in chain length, system density, interaction strength, system size, and polymer volume fraction. The outcome of these calculations is a comprehensive look into the performance of each method and the systems and conditions when either particle or field-theoretic simulations are preferred. We find that field-theoretic simulations are equal to or faster than particle simulations for nearly all of the systems and conditions examined. In many situations, field-theoretic simulations are several orders of magnitude faster than particle simulations, especially if the polymer chains are long, the system density is high, and long-range Coulombic interactions are present. We also demonstrate that field-theoretic simulations are considerably faster at calculating the chemical potential and bypass the challenges associated with particle-based Widom insertion techniques. Taken together, our results provide quantitative evidence that field-theoretic simulations can reach and sample equilibrium considerably faster than particle simulations while simultaneously producing equivalent results.

Fate of surface gaps in magnetic topological insulators

Abstract In magnetic topological insulators, the surface states can exhibit a gap due to the breaking of time-reversal symmetry. Various experiments, while suggesting the existence of the surface gap, have raised questions about its underlying mechanism in the presence of different magnetic orderings. Here, we demonstrate that magnon-mediated electron-electron interactions, whose effects are not limited to the surfaces perpendicular to the magnetic ordering, can significantly influence surface states and their effective gaps. On the surfaces perpendicular to the spin quantization axis, many-body interactions can enhance the band gap to a degree that surpasses the non-interacting scenario. Then, on surfaces parallel to the magnetic ordering, we find that strong magnon-induced fermionic interactions can lead to features resembling a massless-like gap. These remarkable results largely stem from the fact that magnon-mediated interactions exhibit considerable long-range behavior compared to direct Coulomb interactions among electrons, thereby dominating the many-body properties at the surface of magnetic topological insulators.

Short-Range Coulomb Interaction Is a Key to Switch the Utilization of Higher Triplet Excitons in Multiresonance Thermally Activated Delayed Fluorescence Doped Film.

Multiresonance thermally activated delayed fluorescence (MR-TADF) materials have attracted widespread attention due to ultrahigh definition display standards. However, many MR-TADF materials lack TADF properties in both the solution and solid states. Interestingly, the TADF characteristics appear once these MR-TADF compounds are doped in a suitable host film, but the precise mechanism involved in the host-guest interaction remains uncertain. Herein, we systematically investigated the role of host-guest interactions employing doped films (DABNA-1@mCBP and DABNA-1@DPEPO) with opposite phenomena. The results indicate that mCBP with a V-shape and enhanced rigidity could facilitate the formation of an energy spacing layer by employing short-range Coulomb energy through the MR luminescent core, which could offset the sensitivity of the stacking distance, enhancing the coupling between T1 and T2, and thus switch the reverse internal conversion and the higher T2 reverse intersystem crossing process. This work is a further development of luminescence mechanisms and an update of the host-guest interaction criteria for the targeted design of doped films.

Formally Exact and Practically Useful Analytic Solution of Harmonium.

We provide a novel exact analytic solution of harmonium with arbitrary Coulomb interaction strength, for ground as well as all the excited states, using our recently developed method for solving Schrödinger equations. By comparing three formally exact analytic representations of the wave function including the one that utilizes biconfluent Heun function, we find that the best and practically useful representation for the ground state is given by an exact factorized form involving a noninteger power pre-exponential factor, an exponentially decaying term and a modulator function. For excited states, additional factors are needed to account for the nodal information. We show that our method is far more efficient than basis-expansion-based methods in representing the wave function. With the exact wave functions, we have also analyzed the evolution trends of the electron density and natural occupation numbers with increasing interaction strength, which gives insight into the interesting physics in the strong correlation limit.

π+π− Coulomb interaction study and its use in data processing

In this work, the Coulomb effects (Coulomb correlations) in π+π− pairs produced in p+Ni collisions at 24 GeV/c, are studied using experimental π+π− pair distributions in Q, the relative momentum in the pair center-of-mass system (c.m.s.), and its projections QL (longitudinal component) and Qt (transverse component) relative to the pair direction in the laboratory system (LS). The major part of the pion pairs (“Coulomb pairs”) is produced in the decay of ρ, ω and Δ resonances and other short-lived sources. In these pairs, the significant Coulomb interaction occurs at small Q, dominating the π+π− interaction in the final state. The minor part of the pairs (“non-Coulomb pairs”) is produced if one or both pions arose from long-lived sources like η,η′ or from different interactions. In this case, the final state interaction is practically absent. The Q, QL, and Qt distributions of the Coulomb pairs in the c.m.s. have been simulated assuming they are described by the phase space modified by the known point-like Coulomb correlation function AC(Q), corrected for small effects due to the nonpointlike pair production and the strong two-pion interaction. The same distributions of non-Coulomb pairs have been simulated according to the phase space, but without AC(Q). In all Qt intervals, the experimental QL spectrum shows a peak around QL=0 caused by the Coulomb final state interaction. The full width at half maximum increases with Qt from 3 MeV/c for 0<Qt<0.25 MeV/c to 11 MeV/c for 4.0<Qt<5.0 MeV/c. The experimental QL distributions have been fitted with two free parameters: the fraction of Coulomb pairs and the normalization constant. The precision of the description of these distributions is better than 2% in Qt intervals 2–3, 3–4, and 4–5 MeV/c and better than 0.5% in the total Qt interval 0–5 MeV/c. It is shown that the number of Coulomb pairs in all Qt intervals, including the small Qt (small opening angles θ in the LS) is calculated with theoretical precision better than 2%. The comparison of the simulated and experimental numbers of Coulomb pairs at small Qt allows us to check and correct the detection efficiency for the pairs with small θ (0.06 mrad and smaller). It is shown that Coulomb pairs can be used as a new physical tool to check and correct the quality of the simulated events. The special property of the Coulomb pairs is the possibility of checking and correcting the detection efficiency, especially for the pairs with small opening angles. Published by the American Physical Society 2024

A DFT study on the role of excitons and electric field-induced symmetry breaking and topological properties of ZrBr

The control of band gap and topological properties is a crucial objective in the field of materials science, particularly for the application of 2D materials such as topological insulators. Zirconium monobromide (ZrBr), a topological insulator with band inversion, holds significant potential for various applications. In this study, we used Density Functional Theory (DFT) with different approximations namely, Generalized Gradient Approximation (GGA) with and without spin orbit coupling (SOC) as well as hybrid functional to investigate the electronic structure and the band gap of this compound. In addition, we introduced the excitonic effect by considering GW plus Bethe–Salpeter equation (GW-BSE) to compute the optical band gap and quasi-particle energy. We found that ZrBr present a low static dielectric function and weak exciton binding energy, generally lower than those of conventional semiconductors. This behavior is due to the reduced Coulomb interaction in the material. To further explore the material’s behavior, we apply an electric field in three directions to observe symmetry breaking and its impact on band gap tuning. This comprehensive analysis aims to explore the understanding and the potential applications of ZrBr as a topological insulator.

Interatomic Coulombic electron capture beyond the virtual photon approximation.

Via the interatomic Coulombic electron capture (ICEC) process, an electron can be captured by an atom or a molecule, while the binding and excess energy is transferred, via a long-range Coulomb interaction, to a neighboring atom or molecule. The transferred energy can be used to ionize or electronically excite the neighboring species. When the two species are asymptotically far apart, an analytical formula for the ICEC cross sections can be derived. The latter can then be estimated using only the energies and the photoionization cross sections of each species. In this work, we develop an analytical model that allows us to predict the ICEC cross sections when the size of the involved species is comparable to the distance between the two entities. Using abinitio R-matrix results for various systems, we show that the new model reduces the error of the asymptotic formula by two orders of magnitude on average while only using parameters that can be taken from the properties of each species.

Effective Model Reduction Scheme for the Electronic Structure of Highly Doped Semiconducting Polymers.

Highly doped organic polymers have emerged as prominent candidates within novel technological disciplines, yet the fundamental correlation between structure and charge transport characteristics still remains missing. Toward this objective, an efficient model reduction scheme for highly doped polymer chains is developed considering the paradigmatic case of poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT-PSS). The reduced model accounts for the chemical and structural details of the conducting polymer chain in addition to the long-range Coulombic interactions between charge carriers (holes) and dopant ions and the Coulombic repulsion between holes residing on the PEDOT chain. The model is shown to reproduce the intrachain hole-density profile of bulk polymer chains within a mean-field description. Furthermore, and critically, the model is adept at determining the energy distribution of doped PEDOT samples that in effect, influences the hole distribution among polymer chains. The hole distribution so obtained broadly upholds the approximation of a homogeneous charge-carrier distribution in doped polymers commonly found in the literature. In addition, it is observed that the spin configuration of the charge carriers dictates the energetics of the doped chains while it is a critical function of the chain length, carrier density, and disorder parameters.

Quantum field theory of electrons and nuclei

Abstract We develop a non-relativistic quantum field theory of electrons and nuclei with Coulomb interactions. We derive the exact equations of motion and write these equations in the form of Hedin’s equations for all species of identical particles involved. Theory derived allows the computation of exact observables and provides a rigorous starting point to derive approximations in a systematic way.

Coordination, hydration, and diffusion of vanadyl cations in negatively charged polymer membranes

Charged polymer membranes that selectively transport ions are crucial for advancing electrochemical technologies for water purification, resource recovery, and energy generation/storage. Recent studies suggest that the ion selectivity trends of such membranes are due to ion dehydration at the membrane/solution interface, where ions that require less energy to shed their hydration can partition more favorably into the membrane. However, direct evidence of ion dehydration in polymer membranes at relevant conditions is scarce, with claims based primarily on correlations between ion hydration energies and membrane transport properties. The objective of this study was to investigate the electronic environment, local coordination, and hydration of vanadyl counter-ion in negatively charged membranes with broadly varying water content via x-ray absorption spectroscopy. The results highlight that vanadyl counter-ions maintain similar oxidation state, electronic state, and coordination number in the membranes as in aqueous solutions of vanadyl sulfate and that vanadyl dehydration is unlikely in these membranes. However, as the membrane water content decreases, the vanadyl diffusion coefficient decreases and the activation energy of diffusion increases. We attribute these significant changes in membrane transport properties to increased Coulombic interactions between vanadyl and the fixed charge groups, resulting from a decreased dielectric constant of the membrane, rather than to ion dehydration at the membrane/solution interface. This study represents significant progress in understanding the mechanisms that govern ion transport in charged polymer membranes over a broad range of water content, highlighting the critical role of Coulombic interactions between the fixed charges and mobile ions.

Embedded Many‐Body Green's Function Methods for Electronic Excitations in Complex Molecular Systems

ABSTRACTMany‐body Green's function theory in the GW approximation with the Bethe–Salpeter equation (BSE) provides a powerful framework for the first‐principles calculations of single‐particle and electron–hole excitations in perfect crystals and molecules alike. Application to complex molecular systems, for example, solvated dyes, molecular aggregates, thin films, interfaces, or macromolecules, is particularly challenging as they contain a prohibitively large number of atoms. Exploiting the often localized nature of excitation in such disordered systems, several methods have recently been developed in which GW‐BSE is applied to a smaller, tractable region of interest that is embedded into an environment described with a lower‐level method. Here, we review the various strategies proposed for such embedded many‐body Green's functions approaches, including quantum–quantum and quantum–classical embeddings, and focus in particular on how they include environment screening effects either intrinsically in the screened Coulomb interaction in the GW and BSE steps or via extrinsic electrostatic couplings.

Analytical treatment of the Yukawa screened Coulomb interaction in a plane-wave basis

The calculation of the many-electron (screened) Coulomb and exchange integrals is a very common task to perform in modern electronic structure theory. While an analytical treatment of the complete integrals is too complicated to be attempted directly, essential insight can be gained by focusing on the most significant contributions, as determined by a physical criterion. The monopole term of the screened Coulomb interaction is particularly important, since it defines the Hubbard interaction U among a set of localized electrons, which is an essential parameter for effective models of strongly correlated systems. Here, we derive an analytical solution for the matrix elements of the screened Coulomb interaction on a plane-wave basis, which is routinely used in the most common methods for electronic structure calculations. Screening is treated using a Yukawa potential, which is suitable to describe the valence electrons in the Fermi level region. For the solution of the integrals, the plane waves and the Yukawa potential are first expanded in Bessel functions of first and second kind. Then, by means of the lower and upper incomplete gamma functions, we are able to obtain closed-form integrals of a series that remains convergent for realistic parameters. Our exact solution for the radial integrals of the monopole term can find usage in plane-wave codes for electronic structure calculations, both as an output tool as well as within the computational cycle, as e.g., for many-body extensions of density-functional theory. Considering the importance of Bessel functions in solid state physics and electronic structure theory, it is also easy to foresee that our solution to the various integrals across this work may become useful to several other problems in the field.

Softening of the optical phonon by reduced interatomic bonding strength without depolarization.

Softening of the transverse optical (TO) phonon, which could trigger ferroelectric phase transition, can usually be achieved by enhancing the long-range Coulomb interaction over the short-range bonding force1, for example, by increasing the Born effective charges2. However, it suffers from depolarization effects3,4 as the induced ferroelectricity is suppressed on size reduction of the host materials towards high-density nanoscale electronics. Here, we present an alternative route to drive the TO phonon softening by showing that the abnormal soft TO phonon in rocksalt-structured ultrawide-bandgap BeO (ref. 5) is mainly induced by a substantial reduction in the short-range bonding interaction due to the Be-O bond stretching caused by an electron cloud-overlap-induced Coulomb repulsion between two adjacent oxygen ions that are arranged octahedrally around an extremely small Be ion. We further demonstrate the emergence of robust ferroelectricity in strain-induced perovskite BaZrO3 and ultrathin HfO2 and ZrO2 films6,7 grown epitaxially on lattice-mismatched SiO2/Si substrate arising from the softening of the TO phonon driven by a reduction in the short-range bonding strength of biaxial strain-induced stretching bonds. These findings shed light on developing a unified theory for ferroelectricity enhancement in ultrathin films free from depolarization fields by tailoring chemical bonds using ionic radius differences, strains, doping and lattice distortions.

Solvent Effect on Cation⊗3π Interactions: A First-Principles Study.

Cation⊗3π interactions play a special role in the behaviors of biological molecules and carbon-based materials in aqueous solutions, yet the effects of solvation on these interactions remain poorly understood. This study examines the sequential attachment of water molecules to cation⊗3π systems (cation = Li⁺, Na⁺, K⁺), revealing that solvation influences interaction strengths in opposing ways: solvation of the metal cation decreases the strengths of cation⊗3π interactions, while the solvation of the benzene molecule increases the strengths of cation⊗3π interactions, compared with the strengths of cation⊗3π interactions in the gas phase. The mechanism analyses revealed that in the presence of surrounding water molecules, the stability of cation⊗3π systems is generally enhanced by cation-π, π-π, water-π, and water-ion interactions, while water-water interactions typically have a destabilizing effect. In addition, the primary effect of water molecules at different adsorption sites is to modulate the Coulombic multipole-multipole interactions and the overlap between monomeric charge distributions, thereby influencing the changes in strengths of cation⊗3π interactions. Moreover, AIMD simulations further underscore the practical significance of cation⊗3π interactions. These findings provide valuable insights into the structures and the strengths of cation⊗3π interactions with the effect of solvation.

Bound States and Scattering of Magnons on a Superconducting Vortex in Ferromagnet-superconductor Heterostructures

We study the magnon spectrum in a thin ferromagnetic-superconductor heterostructure in the presence of a single superconducting vortex. We employ the Bogolubov–de Gennes Hamiltonian which describes the magnons in the presence of the stray magnetic field and the non-uniform magnetic texture induced by the vortex. We find that the vortex localizes magnon states approximately in the same way as a charge center produces electron bound states due to screened Coulomb interaction in the two-dimensional electron gas. The number of these localized states is substantially determined by the material parameters of the ferromagnetic film only. We solve the scattering problem for an incident plane spin wave and compute the total and transport cross sections. We demonstrate that the vortex-induced non-uniform magnetic texture in chiral ferromagnetic film produces a skew scattering of magnons. We explore the peculiarities of the quantum scattering problem that correspond to orbiting in the classical limit.

Exceptionally Short Tetracoordinated Carbon-Halogen Bonds in Hexafluorodihalocubanes.

Molecules that contain bonds whose length significantly deviates from the average are of interest in the context of understanding the nature and limits of the chemical bonds. However, it is difficult to disentangle the individual contributions of the multiple factors that give rise to such bond-length deviations as reports on such molecules remain scarce. In the present study, we have succeeded in synthesizing hexafluorodihalocubanes of the type C8F6X2 (2) (X = Cl (2Cl), Br (2Br), I (2I)), which represent a new series of molecules with unusual C(sp3)-halogen bonds. The C(sp3)-halogen bonds of 2Cl, 2Br, and 2I, determined via single-crystal X-ray diffraction analysis, are approximately 0.07-0.09 Å shorter than typical C(sp3)-halogen bonds. In particular, the carbon-iodine bonds of 2I are the shortest C(sp3)-I bonds reported to date. The solution-state structures and electronic states of the C(sp3)-halogen bonds in these hexafluorodihalocubanes were analyzed by X-ray absorption spectroscopy, which revealed detailed information on the length of these C(sp3)-halogen bonds in solution and the solid state as well as on the electron-deficient nature of 2. Detailed theoretical calculations and a comparison with halotrinitromethanes (1), which represent another series of molecules with shortened C(sp3)-halogen bonds, revealed that the factors responsible for the shortening of the C(sp3)-halogen bond vary among the different C(sp3)-halogen bonds, i.e., for C(sp3)-Cl and C(sp3)-Br, the s-character and hyperconjugation effects predominate, whereas for C(sp3)-I, the interatomic Coulombic interaction effect prevails.

Analytic continuation of differential cross-sections as a way to determine asymptotic normalization coefficients. Application to the 16O(d,p)17O reaction

Asymptotic normalization coefficients (ANC) are important nuclear characteristics. This paper discusses a method for determining ANC values from experimental data on differential cross-sections of nuclear transfer reactions. The method is based on the use of the analytic continuation of these cross-sections to the pole point of the reaction amplitude with respect to the variable [Formula: see text], where [Formula: see text] is the center-of-mass scattering angle. The method under consideration is used to determine the ANC for the channel [Formula: see text]O(1/2[Formula: see text]; 0.871[Formula: see text]MeV) [Formula: see text]O(0[Formula: see text]; 0[Formula: see text]MeV) [Formula: see text] from the data on the [Formula: see text]O(0[Formula: see text]; 0[Formula: see text]MeV)[Formula: see text]O (1/2[Formula: see text]; 0.871[Formula: see text]MeV) reaction. When determining the ANC, the corrections caused by the Coulomb interaction in the initial, final and intermediate states of the reaction were taken into account. It is shown that these corrections have a great impact on the extracted ANC value.

Electric-field-induced enhancement of exciton binding energy in one-dimensional phosphorene atomic chain

An electric field normally increases the separation between the electron and hole in an exciton without intrinsic polarization and suppresses their Coulombic interaction, resulting in the reduction of its binding energy. Our study of one-dimensional (1D) excitons in phosphorene atomic chains, by using the exact diagonalization method, however, reveals that an electric field applied along the chain axis actually increases the exciton binding energies. Further analysis shows that the electric field tends to enhance the long-range interaction between the electron and hole while suppressing their short-range interaction by inducing an alternating charge distribution along the atomic chain. The zigzag symmetry is believed to account for this unique excitonic phenomenon in the 1D system.

Particle-Hole Asymmetric Ferromagnetism and Spin Textures in the Triangular Hubbard-Hofstadter Model

In a lattice model subject to a perpendicular magnetic field, when the lattice constant is comparable to the magnetic length, one enters the “Hofstadter regime,” where continuum Landau levels become fractal magnetic Bloch bands. Strong mixing between bands alters the nature of the resulting quantum phases compared to the continuum limit; lattice potential, magnetic field, and Coulomb interaction must be treated on equal footing. Using determinant quantum Monte Carlo and density matrix renormalization group techniques, we study this regime numerically in the context of the Hubbard-Hofstadter model on a triangular lattice. In the field-filling phase diagram, we find a broad wedge-shaped region of ferromagnetic ground states for filling factor ν≤1, bounded below by filling factor ν=1 and bounded above by half filling the lowest Hofstadter subband. We observe signatures of SU(2) quantum Hall ferromagnetism at filling factors ν=1 and ν=3. The phases near ν=1 are particle-hole asymmetric, and we observe a rapid decrease in ground-state spin polarization consistent with the formation of skyrmions only on the electron doped side. At large fields, above the ferromagnetic wedge, we observe a low-spin metallic region with spin correlations peaked at small momenta. We argue that the phenomenology of this region likely results from exchange interaction mixing fractal Hofstadter subbands. The phase diagram derived beyond the continuum limit points to a rich landscape to explore interaction effects in magnetic Bloch bands. Published by the American Physical Society 2024

Stimulated Raman scattering and enhancement mechanisms in alkali metal hydroxide aqueous solutions under laser-induced dynamic pressure.

Stimulated Raman scattering (SRS) in lithium hydroxide-water/heavy water (LiOH-H2O/D2O) solutions with varying concentrations was investigated under laser-induced high-pressure conditions using an Nd: YAG laser. The spectra revealed a significant enhancement in SRS signals, characterized by the emergence of low-wavenumber Raman peaks and a shift of the main SRS peak of liquid water to lower frequencies, evolving from a single peak to two or three peaks, which suggested the formation of an ice-like structure. Additionally, the normalized SRS intensity was higher than that of pure water. The enhancement of SRS signals during LiOH dissolution was attributed to the cooperative modulation between hydrogen bonding (HB, O-H:O) by OH- and Coulombic electronic interactions generated by monovalent Li+, which strengthened HB interactions, increased the Raman gain coefficient, and induced structural modifications akin to pressure effects. Besides, the increased density amplified the dynamic high-pressure effects during the laser-induced breakdown (LIB) process, further boosting the SRS signals. This work provides valuable insights into the interaction mechanisms between alkali metal hydroxides and H2O/D2O under laser-induced pressure conditions, offering a comprehensive approach to understanding and enhancing the SRS effect in aqueous solutions.