Repulsive Coulomb Interaction Research Articles

Interplay between the charge density wave phase and a pseudogap under antiferromagnetic correlations

In this study, we explore the impact of short-range antiferromagnetic correlations on the charge density wave (CDW) phase in strongly correlated electron systems exhibiting the pseudogap phenomenon. Our investigation employs an n-pole approximation to consider the repulsive Coulomb interaction (U) and antiferromagnetic correlations. Considering an one-band Hubbard model to account for the Coulomb interaction and a BCS-like model for the CDW order parameter, we observed that an increase in U enhances antiferromagnetic fluctuations, resulting in a flattened re-normalized band around the antinodal point (π,0). The pseudogap manifests itself in the band structure and density of states, prompting exploration of various U and occupation number values. Our findings indicate that antiferromagnetic correlations significantly influence the CDW state, as the Fermi surface is reconstructed within the ordered phase. Furthermore, we found a Lifshitz transition inside both the CDW phase and the normal state, with the latter preceding the onset of the pseudogap.

Evidence for correlated electron pairs and triplets in quantum Hall interferometers

The pairing of electrons is ubiquitous in electronic systems featuring attractive inter–electron interactions, as exemplified in superconductors. Counterintuitively, it can also be mediated in certain circumstances by the repulsive Coulomb interaction alone. Quantum Hall (QH) Fabry–Pérot interferometers (FPIs) tailored in a two–dimensional electron gas under a perpendicular magnetic field have been argued to exhibit such an unusual electron pairing, seemingly without attractive interactions. Here, we show evidence in graphene QH FPIs, revealing not only a similar electron pairing at bulk filling factor νB = 2, but also an unforeseen emergence of electron tripling characterized by a fractional Aharonov–Bohm flux period of h/3e (h is the Planck constant and e the electron charge) at νB = 3. Leveraging plunger–gate spectroscopy, we demonstrate that electron pairing (tripling) involves correlated charge transport on two (three) entangled QH edge channels. This spectroscopy indicates a quantum interference flux periodicity determined by the sum of the phases acquired by the distinct QH edge channels having slightly different interfering areas. Phase jumps observed in the pajama maps can be accounted for by the frequency beating between pairing/tripling modes and the outer interfering edge.

Electrostatically Interacting Wannier Qubits in Curved Space

A derivation of a tight-binding model from Schrödinger formalism for various topologies of position-based semiconductor qubits is presented in the case of static and time-dependent electric fields. The simplistic tight-binding model enables the description of single-electron devices at a large integration scale. The case of two electrostatically Wannier qubits (also known as position-based qubits) in a Schrödinger model is presented with omission of spin degrees of freedom. The concept of programmable quantum matter can be implemented in the chain of coupled semiconductor quantum dots. Highly integrated and developed cryogenic CMOS nanostructures can be mapped to coupled quantum dots, the connectivity of which can be controlled by a voltage applied across the transistor gates as well as using an external magnetic field. Using the anti-correlation principle arising from the Coulomb repulsion interaction between electrons, one can implement classical and quantum inverters (Classical/Quantum Swap Gate) and many other logical gates. The anti-correlation will be weakened due to the fact that the quantumness of the physical process brings about the coexistence of correlation and anti-correlation at the same time. One of the central results presented in this work relies on the appearance of dissipation-like processes and effective potential renormalization building effective barriers in both semiconductors and in superconductors between not bended nanowire regions both in classical and in quantum regimes. The presence of non-straight wire regions is also expressed by the geometrical dissipative quantum Aharonov–Bohm effect in superconductors/semiconductors when one obtains a complex value vector potential-like field. The existence of a Coulomb interaction provides a base for the physical description of an electrostatic Q-Swap gate with any topology using open-loop nanowires, with programmable functionality. We observe strong localization of the wavepacket due to nanowire bending. Therefore, it is not always necessary to build a barrier between two nanowires to obtain two quantum dot systems. On the other hand, the results can be mapped to the problem of an electron in curved space, so they can be expressed with a programmable position-dependent metric embedded in Schrödinger’s equation. The semiconductor quantum dot system is capable of mimicking curved space, providing a bridge between fundamental and applied science in the implementation of single-electron devices.

Counterion Loss from Charged Surface-Bound Complexes Drives the Formation of Loosely Packed Monolayers.

The functionality of multicomponent self-assembled monolayers (SAMs) can be severely diminished by the segregation of like components into nanoscale domains, a process that maximizes favorable short-range intermolecular interactions. Here, we explore the use of a modular family of sulfur-functionalized metal bis(terpyridine) complexes ([M(tpy-R)2]2+(PF6-)2) to prepare mixed SAMs, considering that the comparable structure, dimensions, and ionic composition of these species should render them interchangeable within the adsorbed surface layer. While surface voltammetry experiments show that these SAMs do exhibit compositions representative of their assembly solutions, they also suggest, in line with previous reports, that adjacent complexes in the monolayer are separated by a gap of ∼ 1 nm. Remarkably, X-ray photoelectron spectroscopy studies reveal no F 1s peak features that would confirm the proliferation of PF6- counterions on the surface. We propose that the loosely packed structure of these SAMs results from the loss or exchange of PF6- counterions, which introduces significant repulsive Coulomb interactions between the adsorbed 2+ charged complexes. The hypothesis is supported by an electrostatic model which indicates that these complexes should form close-packed SAMs if mobile counterions are present. First-principles calculations demonstrate that complex-counterion binding interactions are weakened by charge transfer to the gold substrate, suggesting that this may play an important role in the formation of such low-coverage SAMs. Together, this study raises important questions regarding the assembly, organization, and composition of charged SAMs and highlights new opportunities in the design of multicomponent monolayer assemblies with free volume, for example, to facilitate surface-based reactions or support molecular switches.

Demethylation C–C coupling reaction facilitated by the repulsive Coulomb force between two cations

Carbon chain elongation (CCE) is normally carried out using either chemical catalysts or bioenzymes. Herein we demonstrate a catalyst-free approach to promote demethylation C–C coupling reactions for advanced CCE constructed with functional groups under ambient conditions. Accelerated by the electric field, two organic cations containing a methyl group (e.g., ketones, acids, and aldehydes) approach each other with such proximity that the energy of the repulsive Coulomb interaction between these two cations exceeds the bond energy of the methyl group. This results in the elimination of a methyl cation and the coupling of the residual carbonyl carbon groups. As confirmed by high-resolution mass spectrometry and isotope-labeling experiments, the C–C coupling reactions (yields up to 76.5%) were commonly observed in the gas phase or liquid phase, for which the mechanism was further studied using molecular dynamics simulations and stationary-point calculations, revealing deep insights and perspectives of chemistry.

Spectroscopic Evidence for Doubly Hydrogen-Bonded Cationic Dimers in the Solid, Liquid, and Gaseous Phases of Carboxyl-Functionalized Ionic Liquids.

Intermolecular interactions determine whether matter sticks together, gases condense into liquids, or liquids freeze into solids. The most prominent example is hydrogen bonding in water, responsible for the anomalous properties in the liquid phase and polymorphism in ice. The physical properties are also exceptional for ionic liquids (ILs), wherein a delicate balance of Coulomb interactions, hydrogen bonds, and dispersion interactions results in a broad liquid range and the vaporization of ILs as ion pairs. In this study, we show that strong, local, and directional hydrogen bonds govern the structures and arrangements in the solid, liquid, and gaseous phases of carboxyl-functionalized ILs. For that purpose, we explored the H-bonded motifs by X-ray diffraction and attenuated total reflection (ATR) infrared (IR) spectroscopy in the solid state, by ATR and transmission IR spectroscopy in the liquid phase, and by cryogenic ion vibrational predissociation spectroscopy (CIVPS) in the gaseous phase at low temperature. The analysis of the CO stretching bands reveals doubly hydrogen-bonded cationic dimers (c═c), resembling the archetype H-bond motif known for carboxylic acids. The like-charge doubly hydrogen-bonded ion pairs are present in the crystal structure of the IL, survive phase transition into the liquid state, and are still present in the gaseous phase even in (2,1) complexes wherein one counterion is removed and repulsive Coulomb interaction increased. The interpretation of the vibrational spectra is supported by quantum chemical methods. These observations have implications for the fundamental nature of the hydrogen bond between ions of like charge.

The local electronic interaction and strain effects on transverse dynamical spin susceptibility of [formula omitted]-graphyne

We present the behaviors of dynamical transverse spin susceptibilities of undoped β-graphyne monolayer using the Green’s function approach in the context of Hubbard model Hamiltonian. Such dynamical spin susceptibility is proportional to inelastic cross section of neutron beam from the layer. Specially, the effects of magnetic field, on-site coulomb repulsion strength and strain parameter on the spin excitation modes of β-graphyne monolayer are investigated via calculating correlation function of transverse components of spin density operators. Our results show the increase of absolute value of compressive strain parameter leads to move the magnetic excitation modes to higher energies. Also the intensity of peaks in inelastic cross section reduces with absolute value of compressive strain parameter. We also show that applying biaxial tensile strain causes to decrease the intensity of peaks in dynamical transverse spin susceptibility. Finally the effects of magnetic field and on-site coulomb repulsion interaction strength on frequency dependence of dynamical spin structure factor of β-graphyne layer are studied. Moreover the frequency positions of spin excitation mode of β-graphyne monolayer have been investigated due to the effects of biaxial strains, applied magnetic field and Hubbard parameter strength in details.

Half-metallic ferromagnetism in double perovskites Pb2XX'O6 (X = V and Cr and X’ = Zr and Hf)

The structural, magnetic, and electronic properties of Pb-based double perovskite, Pb2XX'O6 (X = V and Cr and X’ = Zr and Hf), have been studied in this paper. This study uses the first-principal projector augmented wave (PAW) potential within the generalized gradient approximation (GGA) as well as considering the on-site Coulomb re-pulsive interaction (GGA+U). The structure of these Pb-based double perovskite is calculated with four magnetic states, antiferromagnetic (AFM), ferromagnetic (FM), ferrimagnetic (FiM), nonmagnetic (NM), and then we compare the energy of these states to find the most stable state. We quickly discovered that all these materials have a lower energy level at the ferromagnetic state, especially Pb2VZrO6 which has an energy difference between AFM and FM state of 120 meV. By analyzing the density of states (DOS) and its magnetic moment, we further discovered that all these materials are half-metallic ferromagnetic (HM-FM). They have an integer magnetic moment because all these materials have a band gap in the spin-down channel. Under GGA + U, the band gap still exists and enlarges, and the V series materials became more stable because of the larger differences between the state of AFM and FM, while the Cr series have the opposite. Lastly, we calculate the electron configuration of V, Cr, Zr, and Hf under GGA and GGA + U calculations in this paper. The HM characteristics of the band gap in one of its spin channels and its ferromagnetic nature mean that there are huge potential applications of these new compounds in spintronics.

Persistent current in a mesoscopic Holstein-Hubbard ring with Dresselhaus interaction

The effect of electron-phonon coupling, onsite repulsive Coulomb interaction and temperature on the persistent current in a quantum ring is studied in the presence of Dresselhaus spin-orbit interaction. The quantum ring threaded by the Aharonov-Bohm flux is modelled by the one-dimensional Holstein-Hubbard-Dresselhaus Hamiltonian. The electron-phonon interaction and Dresselhaus spin-orbit interaction are decoupled by employing the Lang-Firsov coherent transformation and a unitary transformation respectively. Thereafter, a self-consistent diagonalization technique is performed numerically at the Hartree-Fock level to obtain the effective electronic energy and current. It is shown that the intrinsic Dresselhaus spin-orbit interaction enhances the persistent charge and spin currents significantly. On the other hand, the persistent current is reduced by the onsite and nearest-neighbour electron-phonon interaction and Coulomb interaction. Also, the behaviour of the currents is modified by temperature. The spin-splitting of persistent spin current is enhanced considerably by Dresselhaus spin-orbit interaction and this splitting is tuneable in different regimes of magnetic flux, temperature, chemical potential and the interactions present in the system.

The Continuous Measure of Symmetry as a Dynamic Variable: A New Glance at the Three-Body Problem

The time evolution of the continuous measure of symmetry for a system built of three bodies interacting via the potential U(r)~1r is reported. Gravitational and electrostatic interactions between the point bodies were addressed. In the case of a pure gravitational interaction, the three-body-system deviated from its initial symmetrical location, described by the Lagrange equilateral triangle, comes eventually to collapse, accompanied by the growth of the continuous measure of symmetry. When three point bodies interact via the repulsive Coulomb interaction, the time evolution of the CMS is quite different. The CMS calculated for all of the studied initial configurations of the point charges, and all of their charge-to-mass ratios, always comes to its asymptotic value with time, evidencing the stabilization of the shape of the triangle, constituted by the interacting bodies. The influence of Stokes-like friction on the change in symmetry of three-body gravitating systems is elucidated; the Stokes-like friction slows the decrease in the CMS and increases the stability of the Lagrange triangle.

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.

Ion Mobility in Hydroxy-Functionalized Ionic Liquids Depends on Cationic Clustering: Tracking the Alkyl Chain Length Behavior with Deuteron NMR Relaxation.

Observing and quantifying the like-charge attraction in liquids and solutions is still challenging. However, we showed that elusive cation-cation hydrogen bonding may govern the structure and interaction in hydroxyl-functionalized ionic liquids. Therefore, cationic cluster formation depends on the shape, charge distribution, and functionality of the ions. We demonstrated by means of solid-state 2H NMR spectroscopy that cationic clusters change the structure and dynamics of ionic liquids. With increasing alkyl chain length, we observed two deuteron quadrupole coupling constants for the OD groups, differing by about 30 kHz. The lower value was assigned to the cation-cation interaction, indicating that the average (c-c) hydrogen bonds are stronger than the (c-a) hydrogen bonds between the cation and the anion despite the repulsive and attractive Coulomb interaction in the first and latter cases. Ion mobility could be studied by 2H NMR spectroscopy, although the deuterons in the hydrogen-bonded clusters underwent fast exchange. Our results also showed that simple relaxation models are not applicable anymore and that anisotropic motion must be considered.

Superconductivity from a melted insulator in Josephson junction arrays.

Arrays of Josephson junctions are governed by a competition between superconductivity and repulsive Coulomb interactions, and are expected to exhibit diverging low-temperature resistance when interactions exceed a critical level. Here we report a study of the transport and microwave response of Josephson arrays with interactions exceeding this level. Contrary to expectations, we observe that the array resistance drops dramatically as the temperature is decreased-reminiscent of superconducting behaviour-and then saturates at low temperature. Applying a magnetic field, we eventually observe a transition to a highly resistive regime. These observations can be understood within a theoretical picture that accounts for the effect of thermal fluctuations on the insulating phase. On the basis of the agreement between experiment and theory, we suggest that apparent superconductivity in our Josephson arrays arises from melting the zero-temperature insulator.

MoS2 nanosheets based label-free colorimetric aptasensor for Escherichia coli O157: H7 detection

The aggregation behavior of large-scale two-dimensional molybdenum disulfide (MoS2) nanosheets prepared by sonication-assisted exfoliation in environmental friendly 45% ethanol/water mixture under different conditions (e.g., salt concentration, cation valence and nanosheets size) had been examined to make them more appropriate for biological sensing application. Adjustment of sonication time and centrifuging speed could be utilized to select MoS2 nanosheets with various concentrations and sizes. Higher concentrations of salt and cations with higher valence were more effective to aggregate MoS2 nanosheets and settle them than their counterparts, which could be attributed to the perturbation of attractive van der Waals forces and repulsive Coulombic interactions. Moreover, the ethanol in mixture was capable of assisting MoS2 nanosheets to resist this aggregation initiated by salt but it would disturb the stability of aptamer functionalized MoS2 nanosheets in salt solution. The interplay of Escherichia coli O157: H7 (E. coli O157:H7) aptamer functionalized MoS2 nanosheets and salt was then inspired to develop a high sensitive detection method of E. coli O157:H7. The introduction of target bacteria induced MoS2 nanosheets to be exposed to cations, and promoted the aggregation and sedimentation behavior of MoS2 nanosheets. The change in extinction of MoS2 nanosheets had a linear relationship with E. coli O157:H7 concentration in a range of 500–5000 CFU/mL with a detection limit of 116 CFU/mL. This proposed colorimetric sensor expands the application scope of MoS2 nanosheets and shows its promising potential as an alternative tool for bacteria detection in food and water quality monitoring.

Out-of-equilibrium dynamics of repulsive ranked diffusions: The expanding crystal.

We study the nonequilibrium Langevin dynamics of N particles in one dimension with Coulomb repulsive linear interactions. This is a dynamical version of the so-called jellium model (without confinement) also known as ranked diffusion. Using a mapping to the Lieb-Liniger model of quantum bosons, we obtain an exact formula for the joint distribution of the positions of the N particles at time t, all starting from the origin. A saddle-point analysis shows that the system converges at long time to a linearly expanding crystal. Properly rescaled, this dynamical state resembles the equilibrium crystal in a time-dependent effective quadratic potential. This analogy allows us to study the fluctuations around the perfect crystal, which, to leading order, are Gaussian. There are however deviations from this Gaussian behavior, which embody long-range correlations of purely dynamical origin, characterized by the higher-order cumulants of, e.g., the gaps between the particles, which we calculate exactly. We complement these results using a recent approach by one of us in terms of a noisy Burgers equation. In the large-N limit, the mean density of the gas can be obtained at any time from the solution of a deterministic viscous Burgers equation. This approach provides a quantitative description of the dense regime at shorter times. Our predictions are in good agreement with numerical simulations for finite and large N.

Incommensurate charge density wave in multiband intermetallic systems exhibiting competing orders

The appearance of an incommensurate charge density wave vector $\textbf{Q} = (Q_x,Q_y)$ on multiband intermetallic systems presenting commensurate charge density wave (CDW) and superconductivity (SC) orders is investigated. We consider a two-band model in a square lattice, where the bands have distinct effective masses. The incommensurate CDW (inCDW) and CDW phases arise from an interband Coulomb repulsive interaction, while the SC emerges due to a local intraband attractive interaction. For simplicity, all the interactions, the order parameters and hybridization between bands are considered $\textbf{k}$-independent. The multiband systems that we are interested are intermetallic systems with a $d$-band coexisting with a large $c$-band, for which a mean-field approach has proved suitable. We obtain the eigenvalues and eigenvectors of the Hamiltonian numerically and minimize the free energy density with respect to the diverse parameters of the model by means of the Hellmann-Feynman theorem. We investigate the system in real as well as momentum space and we find an inCDW phase with wave vector $\textbf{Q} = (\pi, Q_y) = (Q_x, \pi)$. Our numerical results show that the arising of an inCDW state depends on parameters, such as the magnitude of the inCDW and CDW interactions, band filling, hybridization and the relative depth of the bands. In general, inCDW tends to emerge at low temperatures, away from half-filling. We also show that, whether the CDW ordering is commensurate or incommensurate, large values of the relative depth between bands may suppress it. We discuss how each parameter of the model affects the emergence of an inCDW phase.

Time-resolved Coulomb collision of single electrons.

A series of recent experiments have shown that collision of ballistic electrons in semiconductors can be used to probe the indistinguishability of single-electron wavepackets. Perhaps surprisingly, their Coulomb interaction has not been seen due to screening. Here we show Coulomb-dominated collision of high-energy single electrons in counter-propagating ballistic edge states, probed by measuring partition statistics while adjusting the collision timing. Although some experimental data suggest antibunching behaviour, we show that this is not due to quantum statistics but to strong repulsive Coulomb interactions. This prevents the wavepacket overlap needed for fermionic exchange statistics but suggests new ways to utilize Coulomb interactions: microscopically isolated and time-resolved interactions between ballistic electrons can enable the use of the Coulomb interaction for high-speed sensing or gate operations on flying electron qubits.

Accurate Host-Guest Binding Free Energies Using the AMOEBA Polarizable Force Field.

A grand challenge of computational biophysics is accurate prediction of interactions between molecules. Molecular dynamics (MD) simulations have recently gained much interest as a tool to directly compute rigorous intermolecular binding affinities. The choice of a fixed point-charge or polarizable multipole force field used in MD is a topic of ongoing discussion. To compare alternative methods, we participated in the SAMPL7 and SAMPL8 Gibb octaacid host-guest challenges to assess the Atomic Multipole Optimized Energetics for Biomolecular Applications (AMOEBA) polarizable multipole force field. Advantages of AMOEBA over fixed charge models include improved representation of molecular electrostatic potentials and better description of water occupying the unligated host cavity. Prospective predictions for 26 host-guest systems exhibit a mean unsigned error vs experiment of 0.848 kcal/mol across all absolute binding free energies, demonstrating excellent agreement between computational and experimental results. In addition, we explore two topics related to the inclusion of ions in MD simulations: use of a neutral co-alchemical protocol and the effect of salt concentration on binding affinity. Use of the co-alchemical method minimally affects computed energies, but salt concentration significantly perturbs our binding results. Higher salt concentration strengthens binding through classical charge screening. In particular, added Na+ ions screen negatively charged carboxylate groups near the binding cavity, thereby diminishing repulsive coulomb interactions with negatively charged guests. Overall, the AMOEBA results demonstrate the accuracy available through a force field providing a detailed energetic description of the four octaacid hosts and 13 charged organic guests. Use of the AMOEBA polarizable atomic multipole force field in conjunction with an alchemical free energy protocol can achieve chemical accuracy in application to realistic molecular systems.

Functional Renormalization Group Study of Superconductivity in Rhombohedral Trilayer Graphene.

We employ a functional renormalization group approach to ascertain the pairing mechanism and symmetry of the superconducting phase observed in rhombohedral trilayer graphene. Superconductivity in this system occurs in a regime of carrier density and displacement field with a weakly distorted annular Fermi sea. We find that repulsive Coulomb interactions can induce electron pairing on the Fermi surface by taking advantage of momentum-space structure associated with the finite width of the Fermi sea annulus. The degeneracy between spin-singlet and spin-triplet pairing is lifted by valley-exchange interactions that strengthen under the RG flow and develop nontrivial momentum-space structure. We find that the leading pairing instability is d-wave-like and spin singlet, and that the theoretical phase diagram versus carrier density and displacement field agrees qualitatively with experiment.

Multilayer graphenes as a platform for interaction-driven physics and topological superconductivity

Motivated by the recent discoveries of superconductivity in bilayer and trilayer graphene, we theoretically investigate superconductivity and other interaction-driven phases in multilayer graphene stacks. To this end, we study the density of states of multilayer graphene with up to four layers at the single-particle band structure level in the presence of a transverse electric field. Among the considered structures, tetralayer graphene with rhombohedral (ABCA) stacking reaches the highest density of states. We study the phases that can arise in ABCA graphene by tuning the carrier density and transverse electric field. For a broad region of the tuning parameters, the presence of strong Coulomb repulsion leads to a spontaneous spin and valley symmetry breaking via Stoner transitions. Using a model that incorporates the spontaneous spin and valley polarization, we explore the Kohn-Luttinger mechanism for superconductivity driven by repulsive Coulomb interactions. We find that the strongest superconducting instability is in the $p-$wave channel, and occurs in proximity to the onset of Stoner transitions. Interestingly, we find a range of densities and transverse electric fields where superconductivity develops out of a strongly corrugated, singly-connected Fermi surface in each valley, leading to a topologically non-trivial chiral $p+ip$ superconducting state with an even number of co-propagating chiral Majorana edge modes. Our work establishes ABCA stacked tetralayer graphene as a promising platform for observing strongly correlated physics and topological superconductivity.