Long-range Coulomb Interaction Research Articles

Thermal melting of a quantum electron solid in the presence of strong disorder: Anderson localization versus the Wigner crystal

We consider the temperature-induced melting of a Wigner solid in one-dimensional (1D) and two-dimensional (2D) lattices of electrons interacting via the long-range Coulomb interaction in the presence of strong disorder arising from charged impurities in the system. The system simulates semiconductor-based 2D electron layers where Wigner crystallization is often claimed to be observed experimentally. Using exact diagonalization and utilizing the inverse participation ratio as well as conductance to distinguish between the localized insulating solid phase and the extended metallic liquid phase, we find that the effective melting temperature may be strongly enhanced by disorder since the disordered crystal typically could be in a localized glassy state incorporating the combined nonperturbative physics of both Anderson localization and Wigner crystallization. This disorder-induced enhancement of the melting temperature may explain why experiments often manage to observe insulating disorder-pinned Wigner solids in spite of the experimental temperature being decisively far above the theoretical melting temperature of the pristine Wigner crystal phase in many cases.

Galvani Offset Potential and Constant-pH Simulations of Membrane Proteins.

A central problem in computational biophysics is the treatment of titratable residues in molecular dynamics simulations of large biological macromolecular systems. Conventional simulation methods ascribe a fixed ionization state to titratable residues in accordance with their pKa and the pH of the system, assuming that an effective average model will be able to capture the predominant behavior of the system. While this assumption may be justifiable in many cases, it is certainly limited, and it is important to design alternative methodologies allowing a more realistic treatment. Constant-pH simulation methods provide powerful approaches to handle titratable residues more realistically by allowing the ionization state to vary statistically during the simulation. Extending the molecular mechanical (MM) potential energy function to a family of potential functions accounting for different ionization states, constant-pH simulations are designed to sample all accessible configurations and ionization states, properly weighted according to their Boltzmann factor. Because protonation and deprotonation events correspond to a change in the total charge, difficulties arise when the long-range Coulomb interaction is treated on the basis of an idealized infinite simulation model and periodic boundary conditions with particle-mesh Ewald lattice sums. Charging free-energy calculations performed under these conditions in aqueous solution depend on the Galvani potential of the bulk water phase. This has important implications for the equilibrium and nonequilibrium constant-pH simulation methods grounded in the relative free-energy difference corresponding to the protonated and unprotonated residues. Here, the effect of the Galvani potential is clarified, and a simple practical solution is introduced to address this issue in constant-pH simulations of the acid-sensing ion channel (ASIC).

Computing the Work of Solid-Liquid Adhesion in Systems with Damped Coulomb Interactions via Molecular Dynamics: Approaches and Insights.

Recently, the dry-surface method [Langmuir2016, 31, 8335−8345] has been developed to compute the work of adhesion of solid–liquid and other interfaces using molecular dynamics via thermodynamic integration. Unfortunately, when long-range Coulombic interactions are present in the interface, a special treatment is required, such as solving additional Poisson equations, which is usually not implemented in generic molecular dynamics software, or as fixing some groups of atoms in place, which is undesirable most of the time. In this work, we replace the long-range Coulombic interactions with damped Coulomb interactions, and explore several thermal integration paths. We demonstrate that regardless of the integration path, the same work of adhesion values are obtained as long as the path is reversible, but the numerical efficiency differs vastly. Simple scaling of the interactions is most efficient, requiring as little as 8 sampling points, followed by changing the Coulomb damping parameter, while modifying the Coulomb interaction cutoff length performs worst. We also demonstrate that switching long-range Coulombic interactions to damped ones results in a higher work of adhesion by about 10 mJ/m2 because of slightly different liquid molecule orientation at the solid–liquid interface, and this value is mostly unchanged for surfaces with substantially different Coulombic interactions at the solid–liquid interface. Finally, even though it is possible to split the work of adhesion into van der Waals and Coulomb components, it is known that the specific per-component values are highly dependent on the integration path. We obtain an extreme case, which demonstrates that caution should be taken even when restricting to qualitative comparison.

Observation of giant quadrupole plasmon resonance in C60 in fast ion collisions

Strong perturbation caused due to the Coulomb interaction with fast highly charged ions has been used to probe the quadrupole plasmon excitation in ${\mathrm{C}}_{60}$ fullerene. The electron-emission spectrum arising from a free ${\mathrm{C}}_{60}$ molecule reveals a double-peak structure due to the decay of the giant plasmon resonance. Using a state-of-the-art theoretical approach describing the electron dynamics by time-dependent density functional theory, with an explicit ionic background these two peaks are unambiguously identified as arising from the dipole and quadrupole modes of the plasmon. Furthermore, the electron angular distribution clearly shows a double-well-type distribution which is well reproduced by quadrupole and plasmon resonances. The dipole and quadrupole excitations combined with a long-range postcollisional Coulomb interaction shows excellent agreement with the observed anisotropic angular distribution. The present paper serves as an independent confirmation of the presence of a substantial quadrupole plasmon contribution in molecular systems.

Two-dimensional Dirac nodal line state protected against spin-orbit coupling in MoTe monolayer

We theoretically study a kind of protected double-nodal line state in two-dimensional (2D) transition metal monochalcogenide MoTe by using symmetry analysis and first-principles calculation. Among this kind of materials, there are various intriguing electronic properties, such as the long-range Coulomb interaction. The 2D layer four-fold degeneracy nodal line material is susceptible to the perturbation of strong spin-orbit coupling (SOC). We find that the Dirac degeneracy of two low-energy bands around the S point of the Brillouin zone is robust against SOC in P21/m-MoTe. The degeneracy nodal lines are protected by nonsymmorphic screw-rotational crystal symmetry and time-reversal symmetry. Due to the protection of symmetries, the Dirac double node line states under SOC are different from the accidental band touching. Furthermore, several isolog structures of P21/m-MoTe are also discussed. We find that the fourfold degeneracy nodal line state of MoSe also is robust against SOC, similar to MoTe.

Theoretical investigation on two-dimensional conjugated aromatic polymer membranes for high-efficiency hydrogen separation: The effects of pore size and interaction

Based on two-dimensional conjugated aromatic polymer (2D-CAP), CAP-1S/CAP-1P monolayers were designed by substituting N with S/P atoms for H2 purification. By using MD and DFT approaches, the H2 purification performance and separation mechanisms of CAP-1S/CAP-1P membranes were investigated. Results showed that ultrahigh H2 permeances of 3.546 × 10−5 and 2.593 × 10−4 mol m−2 s−1 Pa−1 were obtained in CAP-1S/CAP-1P, which were almost 104–105 times larger than the industrially acceptable standard. The selectivities of H2 over CO2/CO/CH4/N2 ranged from 5.719 × 1018 to 3.683 × 1039 in CAP-1S and 4.554 × 1013 to 2.153 × 1033 in CAP-1P. From a statistic viewpoint, the CAP-1S/CAP-1P membranes exhibited complete selectivities of H2 over CO2/CO/CH4/N2. The cohesive energies confirmed the high stabilities of CAP-1S/CAP-1P membranes. The minimum energy pathways, energy profiles, electron density, and charge density difference were analyzed to illustrate the significant impact of precise pore size on the H2 separation performance. From a statistic mechanics view, the interaction between gases and CAP-1S/CAP-1P membranes indicated that the long-range Coulomb interactions dominated the gas diffusion processes. Results of this work highlighted CAP-1P as a promising H2 separation membrane and elucidated the promotion mechanism by fine-tunning pore size and interaction between gases and membranes to balance the H2 permeance and selectivity jointly.

Acoustic-phonon-mediated superconductivity in moiréless graphene multilayers

We investigate the competition between acoustic-phonon-mediated superconductivity and the long-range Coulomb interaction in moir\'eless graphene multilayers, specifically, Bernal bilayer graphene, rhombohedral trilayer graphene, and ABCA-stacked tetralayer graphene. In these graphene multilayers, the acoustic phonons can realize, through electron-phonon coupling, both spin-singlet and spin-triplet pairings, and the intra-sublattice pairings ($s$-wave spin-singlet and $f$-wave spin-triplet) are the dominant channels. Our theory naturally explains the distinct recent experimental findings in Bernal bilayer graphene and rhombohedral trilayer graphene, and we further predict existence of superconductivity in ABCA tetralayer graphene arising from electron-phonon interactions. In particular, we demonstrate that the acoustic-phonon-mediated superconductivity prevails over a wide range of doping in rhombohedral trilayer graphene and ABCA tetralayer graphene while superconductivity exists only in a narrow range of doping near the Van Hove singularity in Bernal bilayer graphene. Key features of our theory are the inclusion of realistic band structures with the appropriate Van Hove singularities and Coulomb repulsion effects (the so-called "$\mu^*$ effect") opposing the phonon-induced superconducting pairing. We also discuss how intervalley scatterings can suppress the spin-triplet spin-polarized superconductivity. Our work provides detailed prediction based on electron-acoustic-phonon-interaction-induced graphene superconductivity, which should be investigated in future experiments.

Impact of interfacial thickness on Raman intensity profiles and phonon anisotropy in short-period (AlSb)n/(GaSb)m superlattices

Comprehensive simulations of phonon dispersions ωj(q→SL) and atomic displacements are reported for short-period (AlSb)n/(GaSb)m superlattices (SLs) using a modified linear-chain model. A bond-polarizability methodology is employed for exploring the impact of meticulously included interfacial thickness Δ (≡1–3 monolayers) on the Raman intensity profiles of graded SLs in the optical phonon region. Results of ωj(q→SL) are also presented by exploiting a realistic rigid-ion-model (RIM) and considering short-range, long-range Coulomb interactions and SL symmetry. Besides the anisotropic behavior of optical phonons, the RIM provided evidence of the acoustic-mode anticrossing, minigap formation, confinement, and interface modes. Controlling the vibrational traits by altering a number of monolayers (n, m) in SLs can provide excellent opportunities for improving the electrical and thermal properties of Sb-based materials for engineering various electronic device structures.

Coherent polaron dynamics of electrons solvated in polar liquids.

An electron solvated in a polar liquid is an elementary quantum system with properties governed by electric interactions with a fluctuating molecular environment. In the prevailing single particle picture, the quantum ground and excited states are determined by a self-consistent potential, as defined by the particular local configuration of the solvation shell. This description neglects collective many-body excitations, which arise from the coupling of electronic degrees of freedom and nuclear motions of the environment. While recent experiments have demonstrated collective nonequilbrium electronic-nuclear motion, i.e. polaron excitations in liquid water, their relevance in the broader context of polar liquids has remained unexplored. Here, we study the nonequilibrium dielectric response of the, compared to water, less polar alcohols isopropanol, and ethylene glycol, that also display a different hydrogen bond pattern. We demonstrate that ultrafast relaxation of photogenerated electrons impulsively induces coherent charge oscillations, which persist for some 10ps. They emit electric waves in a frequency range from 0.1 to 2 THz, depending on electron concentration. Oscillation frequencies and line shapes are reproduced by a unified polaron picture for alcohols and water, which is based on a Clausius-Mossotti local field approach for the THz dielectric function. The analysis suggests a longitudinal character of many-body polaron excitations and a weak coupling to transverse excitations, supported by the underdamped character of charge oscillations. Polaron dynamics are governed by the long-range Coulomb interaction between an excess electron and several thousands of polar solvent molecules, while local electron solvation geometries play a minor role.

Coexisting charge density wave and ferromagnetic instabilities in monolayer InSe

Recently fabricated InSe monolayers exhibit remarkable characteristics that indicate the potential of this material to host a number of many-body phenomena. In this work, we systematically describe collective electronic effects in hole-doped InSe monolayers using advanced many-body techniques. To this end, we derive a realistic electronic-structure model from first principles that takes into account the most important characteristics of this material, including a flat band with prominent van Hove singularities in the electronic spectrum, strong electron–phonon coupling, and weakly screened long-ranged Coulomb interactions. We calculate the temperature-dependent phase diagram as a function of band filling and observe that this system is in a regime with coexisting charge density wave and ferromagnetic instabilities that are driven by strong electronic Coulomb correlations. This regime can be achieved at realistic doping levels and high enough temperatures, and can be verified experimentally. We find that the electron–phonon interaction does not play a crucial role in these effects, effectively suppressing the local Coulomb interaction without changing the qualitative physical picture.

Theory and simulation of electrokinetic fluctuations in electrolyte solutions at the mesoscale

Electrolyte solutions play an important role in energy storage devices, whose performance relies heavily on the electrokinetic processes at sub-micron scales. Although fluctuations and stochastic features become more critical at small scales, the long-range Coulomb interactions pose a particular challenge for both theoretical analysis and simulation of fluid systems with fluctuating hydrodynamic and electrostatic interactions. Here, we present a theoretical framework based on the Landau–Lifshitz theory to derive closed-form expressions for fluctuation correlations in electrolyte solutions, indicating significantly different decorrelation processes of ionic concentration fluctuations from hydrodynamic fluctuations, which provides insights for understanding transport phenomena of coupled fluctuating hydrodynamics and electrokinetics. Furthermore, we simulate fluctuating electrokinetic systems using both molecular dynamics (MD) with explicit ions and mesoscopic charged dissipative particle dynamics (cDPD) with semi-implicit ions, from which we identify that the spatial probability density functions of local charge density follow a gamma distribution at sub-nanometre scale (i.e. $0.3\,{\rm nm}$ ) and converge to a Gaussian distribution above nanometre scales (i.e. $1.55\,{\rm nm}$ ), indicating the existence of a lower limit of length scale for mesoscale models using Gaussian fluctuations. The temporal correlation functions of both hydrodynamic and electrokinetic fluctuations are computed from all-atom MD and mesoscale cDPD simulations, showing good agreement with the theoretical predictions based on the linearized fluctuating hydrodynamics theory.

Dielectric response of electrons with strong local correlations and long-ranged Coulomb interactions

Motivated by recent experiments, we append long ranged Coulomb interactions to dominant strong local correlations and study the resulting t-J-VC model for the 2-dimensional cuprate materials. This model includes the effect of short ranged Hubbard–Gutzwiller–Kanamori type correlations and long ranged Coulomb interactions on tight binding electrons. We calculate the {q→,ω} dependent charge density fluctuations in this model using the extremely correlated Fermi liquid theory characterized by quasiparticles with very small weight Z. We develop a novel set of formulae to represent the dynamical charge susceptibility and the dielectric function, using a version of the charge-current continuity equation for a band system, valid for arbitrary q→. Combining these ingredients, we present results for the irreducible dynamical charge susceptibility χ˜ρρ(q→,ω), (longitudinal) dielectric function ɛ(q→,ω), current susceptibility χ˜JJ(q→,ω), conductivity σ(q→,ω), and the plasma frequency for any q→. We also present calculations for the first moment of the structure function and discuss a characteristic energy scale Ωp(q→) which locates a peak in Imχ˜ρρ(q→,ω).

Pattern Formation and Aggregation in Ensembles of Solitons in Quasi One-Dimensional Electronic Systems

Broken symmetries of quasi one-dimensional electronic systems give rise to microscopic solitons taking roles of carriers of the charge or spin. The double degeneracy gives rise to solitons as kinks of the scalar order parameter A; the continuous degeneracy for the complex order parameter Aexp(iθ) gives rise to phase vortices, amplitudes solitons, and their combinations. These degrees of freedom can be controlled or accessed independently via either the spin polarization or the charge doping. The long-range ordering in dimensions above one imposes super-long-range confinement forces upon the solitons, leading to a sequence of phase transitions in their ensembles. The higher-temperature T transition enforces the confinement of solitons into topologically bound complexes: pairs of kinks or the amplitude solitons dressed by exotic half-integer vortices. At a second lower T transition, the solitons aggregate into rods of bi-kinks or into walls of amplitude solitons terminated by rings of half-integer vortices. With lowering T, the walls multiply, passing sequentially across the sample. Here, we summarize results of a numerical modeling for different symmetries, for charged and neutral soliton, in two and three dimensions. The efficient Monte Carlo algorithm, preserving the number of solitons, was employed which substantially facilitates the calculations, allowing to extend them to the three-dimensional case and to include the long-range Coulomb interactions.

Fermionic Monte Carlo Study of a Realistic Model of Twisted Bilayer Graphene

The rich phenomenology of twisted bilayer graphene (TBG) near the magic angle is believed to arise from electron correlations in topological flat bands. An unbiased approach to this problem is highly desirable, but also particularly challenging, given the multiple electron flavors, the topological obstruction to defining tight binding models and the long-ranged Coulomb interactions. While numerical simulations of realistic models have thus far been confined to zero temperature, typically excluding some spin or valley species, analytic progress has relied on fixed point models away from the realistic limit. Here we present for the first time unbiased Monte Carlo simulations of realistic models of magic angle TBG at charge-neutrality. We establish the absence of a sign problem for this model in a momentum space approach, and describe a computationally tractable formulation that applies even on breaking chiral symmetry and including band dispersion. Our results include (i) the emergence of an insulating Kramers inter-valley coherent ground state in competition with a correlated semi-metal phase, (ii) detailed temperature evolution of order parameters and electronic spectral functions which reveal a `pseudogap' regime, in which gap features are established at a higher temperature than the onset of order and (iii) predictions for electronic tunneling spectra and their evolution with temperature. Our results pave the way towards uncovering the physics of magic angle graphene through exact simulations of over a hundred electrons across a wide temperature range.

Dirac nodal-line semimetal zinc polynitride at high pressure

Topological semimetals exhibit novel quantum states and electronic structures with interesting Fermi surfaces. In contrast to Weyl and Dirac nodal points, nodal lines can have multiple topological configurations in momentum space that lead to new properties, such as long-range Coulomb interaction and flat Landau levels. Herein, we report the discovery of a Dirac nodal-line semimetal polynitride ${\mathrm{ZnN}}_{4}$, synthesized from the elements under high pressure via laser-heated diamond anvil cell technique. The crystal structure of ${\mathrm{ZnN}}_{4}$ has an $Ibam$ space group, and features infinite one-dimensional nitrogen chains in the pressure range of 14--130 GPa. The Dirac cone is observed midway between $S$ and $X$ points in the Brillouin zone and the Dirac nodal-line is found near the $T$ point. The measured electrical resistance of the ${\mathrm{ZnN}}_{4}$ sample shows an anomalous increase with pressure, which is attributed to the localization of valence electrons. The case of ${\mathrm{ZnN}}_{4}$ provides a unique example of Dirac nodal-line semimetal in nitrides.

Revisiting Anderson-Higgs mechanism: application of Lieb-Schultz-Mattis theorem

We consider an electron model of superconductivity on a three-dimensional lattice where there are on-site attractive Hubbard interaction and long-range repulsive Coulomb interaction. It is claimed that fully gapped s-wave superconductivity within this model, if present, exhibits spontaneous translation symmetry breaking possibly related to a charge order. Our discussions are based on an application of the Lieb-Schultz-Mattis theorem under some physical assumptions. The inconsistency between the proposed supersolid and experiments can impose some constraints on a reasonable choice of a theoretical model.

The refined determination of the ion pair lifetimes in ionic liquids

Assessing lifetimes of liquid’s local structures could bring impactful output. For example, the key transport properties of ionic liquids are governed by local structure dynamics to a large extent. Due to long-range Coulomb interactions, these systems show pronounced charge ordering. In this case, the local structure breaking rate could be described in terms of cation–anion pair lifetimes. Conventional pair lifetime analysis relies on geometrical criterion, defining the maximum distance from cation to anion in pair. In this study, we argue towards additional restriction to ensure pair stability. Based on vibrational properties, we introduce lower boundary for pair lifetime to exclude false pair recognition in the case of collision-like interaction. Also, we put forward a computational algorithm which allows obtaining both mean lifetime and lifetime distribution. The calculations of mean pair lifetimes in molten alkali halides support our reasoning.

Fermion dispersion renormalization in a two-dimensional semi-Dirac semimetal

We present a non-perturbative study of the quantum many-body effects caused by the long-range Coulomb interaction in a two-dimensional semi-Dirac semimetal. This kind of semimetal may be realized in deformed graphene and a class of other realistic materials. In the non-interacting limit, the dispersion of semi-Dirac fermion is linear in one direction and quadratic in the other direction. When the impact of Coulomb interaction is taken into account, such a dispersion can be significantly modified. To reveal the correlation effects, we first obtain the exact self-consistent Dyson-Schwinger equation of the full fermion propagator and then extract the momentum dependence of the renormalized fermion dispersion from the numerical solutions. Our results show that the fermion dispersion becomes linear in two directions. These results are compared to previous theoretical works on semi-Dirac semimetals.

Influence of Long-Range Forces on the Transition States and Dynamics of NaCl Ion-Pair Dissociation in Water.

We study NaCl ion-pair dissociation in a dilute aqueous solution using computer simulations both for the full system with long-range Coulomb interactions and for a well-chosen reference system with short-range intermolecular interactions. Analyzing results using concepts from Local Molecular Field (LMF) theory and the recently proposed AI-based analysis tool "State predictive information bottleneck" (SPIB), we show that the system with short-range interactions can accurately reproduce the transition rate for the dissociation process, the dynamics for moving between the underlying metastable states, and the transition state ensemble. Contributions from long-range interactions can be largely neglected for these processes because long-range forces from the direct interionic Coulomb interactions are almost completely canceled (>90%) by those from solvent interactions over the length scale where the transition takes place. Thus, for this important monovalent ion-pair system, short-range forces alone are able to capture detailed consequences of the collective solvent motion, allowing the use of physically suggestive and computationally efficient short-range models for the dissociation event. We believe that the framework here should be applicable to disentangling mechanisms for more complex processes such as multivalent ion disassociation, where previous work has suggested that long-range contributions may be more important.

Coherent effects in energy absorption in double quantum dot molecule – Metal nanoparticle hybrids

We theoretically study the optical properties of a hybrid structure consisting of a metal nanoparticle (MNP) and an asymmetric double semiconductor quantum dot (SQD) molecule, which are coupled together, via long-range Coulomb interaction. We derive and solve numerically the relevant density-matrix equations and use electromagnetic calculations to evaluate the energy absorption rate of the MNP and the asymmetric double SQD molecule, separately, as well as, the total absorption rate for the entire hybrid structure, as a function of the energy of an applied electromagnetic field , for two different applied field polarization directions. We also investigate the impact of the applied field intensity and the electron tunnelling coupling rate on the spectral profiles, for several values of the interparticle distance. The Autler-Townes splitting and double nonlinear Fano effects are obtained in the absorption spectra of the asymmetric double SQD molecule, the MNP and the total system.