Random Phase Approximation Research Articles

Effect of non-metal doping on the optoelectronic properties of ZrS2/ZrSe2 heterostructure under strain: a first-principles study.

In this paper, we systematically studied the effects of non-metallic element (B, C, N, O, F) doping and biaxial stretching on the photoelectric properties of ZrS2/ZrSe2 heterostructures by using the first-principles calculation method based on density functional theory. The results show that the p-type doping is realized by B, C, and N atom doping, and the n-type doping is realized by O and F atom doping. The doping of B and C atoms produces impurity energy levels in the band gap, which affects the conductivity of the heterostructure. The band gap of N and O atom-doped heterostructures increases under tensile strain, but it is still a direct band gap. The analysis of the optical properties of the heterostructures shows that the doping of non-metallic atoms can adjust the optical absorption rate and reflectivity of the heterostructures. Under the action of tensile strain, the optical properties of the doped heterostructures have changed significantly in the low-energy region. This article provides a theoretical basis for the future application of ZrS2/ZrSe2 heterostructures. This paper uses the first-principles calculation method based on density functional theory. The PBE exchange-correlation functional based on generalized gradient approximation (GGA) is selected for the specific calculation, and the crystal structure is geometrically optimized by the ultrasoft pseudopotential method. It is verified that when the cutoff energy of the ZrS2/ZrSe2 heterostructure is 500 eV, the K-point grid is selected to be 10 × 10 × 2 with the lowest energy, so the cutoff energy is selected to be 500 eV. The K-point grid is selected to be 10 × 10 × 2. The convergence limits for structural optimization are as follows: the maximum force between atoms is 0.01 eV/Å, the convergence threshold of the maximum energy change is set to 10-9 eV/atom, and the convergence threshold of the maximum displacement is 0.001 Å. In order to avoid the influence of atomic periodic motion between different atomic layers, a vacuum layer of 20 Å is added in the vertical direction. Considering the interaction of vdW between the interfaces, the DFT-D2 method is used to verify. The optical properties were calculated by the random phase approximation method, and the K-point grid was selected as 12 × 12 × 2.

Hartree–Fock Mean Field Calculations with Random Phase Approximation for 140Ce Nuclei Structure

Hartree–Fock Mean Field Calculations with Random Phase Approximation for 140Ce Nuclei Structure

Comparative studies of role of different structure factors in various physical properties of some simple liquid metals

In the current work, the comparison of the structure factors and pair correlation functions produced by using eight different theoretical models based on the Perckus-Yevick Hard Sphere (PYHS), Hard Sphere Yukawa (HSY), Mean Spherical Approximation (MSA), Generalized Mean Spherical Approximation (GMSA), Soft Sphere (SS), One-Component Plasma (OCP), Optimized Random Phase Approximation (ORPA) and Charged Hard Sphere (CHS) models for liquid metals viz. Li, Na, K, Rb, Cs, Mg, Zn, Ca, Al, Ga, In, Pb, Sn, Bi and Sb are carried out. Our own model potential is used with the Taylor (TY) screening function in the present computation. With this, certain physical properties such as electrical transport (electrical resistivity), vibrational property (phonon dispersion), dynamical property (velocity autocorrelation function (VACF)) and static (long wavelength of structure factor) properties has also been calculated. When the several theoretical models of the structure factors of the researched simple liquid metals are compared, it is discovered that the experimental data is consistent and in good agreement with the theoretical models.

Electric dipole polarizability of magic nuclei

The correlations between the electric dipole polarizability and neutron skin thickness are studied by the magic nuclei 40,48Ca, 68,78Ni, 132Sn, and 208Pb. The strength distribution of the E1 transitions is calculated within the random phase approximation model based on the Skyrme nuclear energy density functional. A comparison with the experimental data has allowed us to constrain the value of the nuclear symmetry energy J = 30–37 MeV.

The TDHF code Sky3D version 1.2

The Sky3D code has been widely used to describe nuclear ground states, collective vibrational excitations, and heavy-ion collisions. The approach is based on Skyrme forces or related energy density functionals. The static and dynamic equations are solved on a three-dimensional grid, and pairing is been implemented in the BCS approximation. This updated version of the code aims to facilitate the calculation of nuclear strength functions in the regime of linear response theory, while retaining all existing functionality and use cases. The strength functions are benchmarked against available RPA codes, and the user has the freedom of choice when selecting the nature of external excitation (from monopole to hexadecapole and more). Some utility programs are also provided that calculate the strength function from the time-dependent output of the dynamic calculations of the Sky3D code. New version program summaryProgram Title: Sky3DCPC Library link to program files:https://doi.org/10.17632/vzbrzvyrn4.2Developer's repository link:https://github.com/manybody/sky3dLicensing provisions: GPLv3Programming language: Fortran, with one post-processing utility in Python.Journal reference of previous version:: Schuetrumpf, B., Reinhard, P.G., Stevenson, P.D., Umar, A.S., and Maruhn, J.A. (2018). The TDHF code Sky3D version 1.1. Comput. Phys. Commun. 229 (2018) 211–213.Does the new version supersede the previous version?: Yes.Reasons for the new version: The capability of reproducing the nuclear strength function for a variety of newly-coded external boosts has been added.Nature of problem: Calculating nuclear multipole strength functions is a crucial probe that can help model the nuclear system and its structure properties. A variety of models exist for this task, such as QRPA (Quasiparticle Random Phase Approximation) and its variants, but such approaches are often limited due to symmetry constraints. Time-dependent Hartree Fock (TDHF) has been used to simulate nuclear vibrations and collisions between nuclei for low energies without assuming any symmetry in the system. This code extends the TDHF to calculate the multi-pole strength functions of atomic nuclei. We showcase its reliability by comparing it with the established RPA codes for the calculation of such strength functions.Solution method: We extended previous versions of the Sky3D code [1,2] to include an external boost of multipole type where the user can provide custom input that decides the nature of the multipole (monopole, quadrupole, octupole, and so on) boost. The principal aim is to calculate the multipole strength function, which is the Fourier transform of the time-dependent expectation value of the multipole operator, which has the same form as the external boost. The proper unit conversion is done so that one can extract the exact unit of the thus calculated strength function, which is comparable to the available literature in the field. The boundary conditions are chosen such that a Woods-Saxon-like function cuts off the external field, driving it to zero at the boundary.Summary of revisions: The ability to give a more general external field for excitation has been implemented, which can be of a chosen multipolarity and isospin nature. Then, as a function of time, moments for both isospins and for multipolarities up to L=5 are followed. A new analysis program is included to calculate strength functions and energy weighted sum rules. The ability to specify a mixing parameter in the pairing force is included. This allows a mixed surface-volume pairing to be selected in a way more compatable with QRPA codes for comparison. An updated Makefile is included which makes compilation on Apple silicon computers easier.

Nuclear structure properties and weak interaction rates of even-even Fe isotopes

Nuclear structure properties and weak interaction rates of neutron-rich even-even iron (Fe) isotopes (A = 50 – 70) are investigated using the Interacting Boson Model-1 (IBM-1) and the proton–neutron Quasiparticle Random Phase Approximation (pn-QRPA) model. The IBM-1 is used for the calculation of energy levels and the B(E2) values of neutron-rich Fe isotopes. Later their geometry was predicted within the potential energy formalism of the IBM-1 model. Weak interaction rates on neutron-rich nuclei are needed for the modeling and simulation of presupernova evolution of massive stars. In the current study, we investigate the possible effect of nuclear deformation on stellar rates of even-even Fe isotopes. The pn-QRPA model is applied to calculate the weak interaction rates of selected Fe isotopes using three different values of deformation parameter. It is noted that, in general, bigger deformation values led to smaller total strength and larger centroid values of the resulting Gamow-Teller distributions. This later translated to smaller computed weak interaction rates. The current finding warrants further investigation before it may be generalized. The reported stellar rates are up to 4 orders of magnitude smaller than previous calculations and may bear astrophysical significance.

Multireference Correlated Oscillator Strengths from Adiabatic Connection Approaches Based on Extended Random Phase Approximation.

We show that accurate oscillator strengths can be obtained from adiabatic connection (AC) approaches based on the extended random phase approximation (ERPA) combined with multireference (complete active space, CAS) wave functions. The oscillator strengths calculated using the perturbation-corrected ERPA transition density matrices, proposed in this work, and the excitation energies calculated with recently introduced AC correlation energy methods, AC0 and AC0D, compete with accuracy in the perturbational CASPT2 approach and require less computational effort. AC0 and AC0D methods scale more favorably with the number of active orbitals than multiconfigurational perturbation approaches like CASPT2 and NEVPT2 thanks to their dependence on reduced density matrices up to the order of 2. Importantly, the newly developed approach for computing correlated transition dipole moments does not entail any additional costs, as all intermediate quantities become available when AC0 energies are being computed. We also test the performance of the recently proposed AC method corrected for the negative-transition contributions to the correlation energy, AC0D, for triplet excitation energies. Similarly, as for the singlet excitations, the correction improves the performance of the AC0 method, particularly for the low-lying excited states.

Precise structure and energy of group 6 transition metal dichalcogenide homo- and heterobilayers in high-symmetry configurations

Two-dimensional group 6 transition metal dichalcogenide (2D TMDC) bilayers show various high-symmetry stacking configurations, which have also been observed in extended domains formed in their twisted homo- and heterobilayers. The interlayer energy varies for these stacking configurations, and the energy differences determine the relative size of the stacking domains. Therefore, the precise prediction of the composition- and stacking-dependent interlayer energy is crucial to model the domain structure of 2D TMDCs in their twisted bilayer homo- and heterostructures. For the validation of approximate methods that are necessary to tackle these systems encompassing thousands of atoms precise reference data is still lacking. Here, we employ the random phase approximation (RPA) on previously validated SCAN-rVV10 geometries to obtain interaction energies of state-of-the-art accuracy on the six high-symmetry stacking configurations ( Hhh , HhM , HhX , Rhh , RhM , and RhX ) of MX2 (M = Mo, W; X = S, Se) bilayers and compare them with the dispersion-corrected density-functional theory (DFT) functionals Perdew–Burke–Ernzerhof (PBE)+D3(BJ), PBE-rVV10L, and SCAN-rVV10. We identify SCAN-rVV10 as most reliable DFT variant with an average deviation of 1.2 meV/atom in relative energies from the RPA reference, and a root mean squared error of less than 2 meV/atom for interlayer interaction energies. We find interlayer distances obtained by PBE+D3(BJ) as being too short, with an impact on the electronic structure, resulting in the incorrect prediction of the band gap character in some cases. A further result of this work is the significant lowering of the interlayer energy and increasing of the interlayer distance in the high-energy stacking configurations. These stackings can be accessible via shear strain and promote exfoliation.

Combining mBJ exchange potential and bootstrap kernel of TDDFT to compute optical spectra of solids

One of the fundamental challenges in calculating the optical properties of crystalline materials is the accurate description of exciton effects so as to make it computationally viable for studying large systems. We combine the modified Becke-Johnson (mBJ) exchange potential and bootstrap kernel (BSK) of time-dependent density functional theory (TDDFT) to compute the imaginary part of the dielectric function of a variety of semiconductors and insulators (Si, GaAs, NiO, TiO2, LiF, LiCl, SrTiO3 and NaMgF3). The results are compared with the experimental data available in the literature. We also compute their dielectric functions using the random phase approximations (RPA) to verify the effect of the BSK method on the optical spectra of these compounds. We conclude that TDDFT+BSK+mBJ calculations can determine the optical spectra of the solids in good agreement with the experimental data (except for small-energy gap materials such as Si and GaAs) with low computational cost, and using a fully ab initio procedure.

Sensitivity of octant of θ23, CP violation and mass hierarchy in NOνA with multinucleon and detector effects

In this work, we investigate how multinucleon enhancement and RPA (Random Phase Approximation) suppression can affect the measurement of three unknown neutrino oscillation parameters — the CP-violating phase δCP, the octant of the atmospheric mixing angle θ23, and the determination of the mass hierarchy, in the appearance channel of the NOνA experiment. We include the presence of the detector effect as well in the analysis, which is crucial for capturing realistic experimental scenarios. We also conducted a comparison between the nuclear model Effective Spectral Function (calculated within the RFG model) with and without Transverse Enhancement in terms of sensitivity analysis. It is found that the analysis using our comprehensive model QE(+RPA)+2p2h along with Effective Spectral Function+Transverse Enhancement exhibits significantly enhanced sensitivity compared to the pure QE interaction process, in all the cases. Also, the higher octant of θ23, the lower half plane of δCP, and the normal mass hierarchy (HO-LHP-NH) exhibit improved sensitivity, enabling a more precise determination of the corresponding parameters. Furthermore, it is also noted that improving the performance of the detector also improves the results. Thus, including multinucleon effects and improving detector efficiency have the potential to enhance the capabilities of the NOνA (and other long baseline) experiment in conducting precise parameter studies.

A mathematical analysis of the adiabatic Dyson equation from time-dependent density functional theory

In this article, we analyse the Dyson equation for the density–density response function (DDRF) that plays a central role in linear response time-dependent density functional theory (LR-TDDFT). First, we present a functional analytic setting that allows for a unified treatment of the Dyson equation with general adiabatic approximations for discrete (finite and infinite) and continuum systems. In this setting, we derive a representation formula for the solution of the Dyson equation in terms of an operator version of the Casida matrix. While the Casida matrix is well-known in the physics literature, its general formulation as an (unbounded) operator in the N-body wavefunction space appears to be new. Moreover, we derive several consequences of the solution formula obtained here; in particular, we discuss the stability of the solution and characterise the maximal meromorphic extension of its Fourier transform. We then show that for adiabatic approximations satisfying a suitable compactness condition, the maximal domains of meromorphic continuation of the initial DDRF and the solution of the Dyson equation are the same. The results derived here apply to widely used adiabatic approximations such as (but not limited to) the random phase approximation and the adiabatic local density approximation. In particular, these results show that neither of these approximations can shift the ionisation threshold of the Kohn–Sham system.

Low-Scaling Algorithms for GW and Constrained Random Phase Approximation Using Symmetry-Adapted Interpolative Separable Density Fitting.

We present low-scaling algorithms for GW and constrained random phase approximation based on a symmetry-adapted interpolative separable density fitting (ISDF) procedure that incorporates the space-group symmetries of crystalline systems. The resulting formulations scale cubically, with respect to system size, and linearly with the number of k-points, regardless of the choice of single-particle basis and whether a quasiparticle approximation is employed. We validate these methods through comparisons with published literature and demonstrate their efficiency in treating large-scale systems through the construction of downfolded many-body Hamiltonians for carbon dimer defects embedded in hexagonal boron nitride supercells. Our work highlights the efficiency and general applicability of ISDF in the context of large-scale many-body calculations with k-point sampling beyond density functional theory.

Biomolecular phase separation through theoretical and computational microscope

AbstractBiomolecular phase separation is a vital mechanism for orchestrating biomolecules within living cells. This crucial role has spurred an intense pursuit to comprehend the molecular underpinnings governing and regulating these processes. Computational methodologies offer a unique perspective, augmenting experimental techniques by providing detailed information that cannot be obtained otherwise. In this review, we briefly overview the theoretical and computational approaches to investigate biomolecular phase separation. As a short primer, we explain the factors driving and affecting phase separation of biomolecules, and then we delve into analytical and simulation methods used to study phase separation. We explain how analytical methods like the Flory–Huggins theory, random phase approximation, and graph‐based methods have been used to study phase behaviors of various proteins. We also discuss principles and applications of all‐atom simulations, coarse‐grained simulations, and field‐theoretical approaches. Additionally, we explore the recent advances in machine learning approach to predict phase separation of biomolecules.

Refractory and thermoelectric properties of stabilized Tricalcium aluminate allotrope: A first-principles calculation approach

Tricalcium aluminate (Ca3Al2O6) is an indispensable component of Portland cement due to its high strength and reactivity. This study investigates the equilibrium lattice structure as well as the electronic and refractory properties of a newly discovered allotrope of Ca3Al2O6 using density functional theory and random phase approximation methods. Using density functional perturbation theory, we investigate the phonon dispersion of the refined structure’s experimental stability. In addition, the lattice thermal conductivity and thermoelectric figure of merit are computed by solving the Boltzmann Transport Equation with the modified Debye Callaway model and the Relaxation time Approximation methods. The computed Figure of merit, determined by the carrier concentration, indicates a substantial enhancement of 40 to 100-fold, leading to a superior figure of merit of 0.25 and 0.6 when appropriately doped. As a result, we anticipate that stable allotropes of Ca3Al2O6 in the Pm3̄m phase will be useful as energy-harvesting, convective cooling and infrared radiation shield-based cement materials in the cement and concrete industries.

Modeling of High-Harmonic Generation in the C60 Fullerene Using Ab Initio, DFT-Based, and Semiempirical Methods.

We report calculations of the high-harmonic generation spectra of the C60 fullerene molecule carried out by employing a diverse set of real-time time-dependent quantum chemical methods. All methodologies involve expanding the propagated electronic wave function in bases consisting of the ground and singly excited time-independent eigenstates obtained through the solution of the corresponding linear-response equations. We identify the correlation and exchange effect in the spectra by comparing the results from methods relying on the Hartree-Fock reference determinant with those obtained using approaches based on the density functional theory with different exchange-correlation functionals. The effect of the full random-phase approximation treatment of the excited electronic states is also analyzed and compared with the configuration interaction singles and the Tamm-Dancoff approximation. We also showcase the fact that the real-time extension of the semiempirical method INDO/S can be effectively applied for an approximate description of laser-driven dynamics in large systems.

Isoscalar giant quadrupole resonance of even-even 112-124Sn isotopes using BCS-QRPA

Using self-consistent Bardeen - Cooper - Schriffer + Hartree - Fock and quasiparticle random phase approximation, the isoscalar giant quadrupole resonance in the isotopes of 112,114,116,118,120,122,124Sn has been studied in this work. Five sets of Skyrme-type interactions of different values of the nuclear matter incompressibility coefficient KNM and effective mass m*/m are used in the calculations. Additionally, the impact of different types of pairing forces (i.e., volume, surface, and mixed) is examined. Comparisons are made between the computed strength distributions, centroid energies Ecen, scaled energies Es, and constrained energies Econ of the isoscalar giant quadrupole resonance and the available experimental data. Analysis is done on the relationships between KNM and m*/m, and the estimated properties.

Modulation Instability and Convergence of the Random-Phase Approximation for Stochastic Sea States

The nonlinear Schrödinger equation is widely used as an approximate model for the evolution in time of the water wave envelope. In the context of simulating ocean waves, initial conditions are typically generated from a measured power spectrum using the random-phase approximation, and periodized on an interval of length L. It is known that most realistic ocean waves power spectra do not exhibit modulation instability, but the most severe ones do; it is thus a natural question to ask whether the periodized random-phase approximation has the correct stability properties. In this work, we specify a random-phase approximation scaling, so that, in the limit of L→∞,\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$L\\rightarrow \\infty ,$$\\end{document} the stability properties of the periodized problem are identical to those of the continuous power spectrum on the infinite line. Moreover, it is seen through concrete examples that using a too short computational domain can completely suppress the modulation instability.

Dynamic polarization, quantum spectral function and effective mass for black phosphorous: Random phase approximation approach at finite temperature

In this work, the finite-temperature dynamic polarization function of black phosphorus is obtained using the random phase approximation (RPA) for the lower band of the corresponding effective Hamiltonian. The maximum temperature-dependent polarization of the orthorhombic honeycomb structure of black phosphorus is observed at ω=0.54eV for wavectors at the Fermi level. Several peaks are thus observed indicating that an overall Fermi-liquid behavior is present but with different kinds of quasiparticles. These quasiparticles appear due to the highly anisotropic energy dispersion. Experiments conducted on black phosphorous at a temperature of 10 K have a tremendous effect on the scattering mechanism. Subsequently, the quasiparticle behavior is studied through the spectral function and the effective mass, each resolved on the three components of the wave number. The resulting effective mass anisotropy causes the plasmon to disperse completely, leading to a lower resonant frequency when there is a larger mass along one of the axes. At large wavelengths, the RPA result is almost identical to that obtained from the classical plasmon dispersion.

Correlated ion stopping in dense plasmas with a temperature‐dependent plasmon pole approximation

AbstractThe plasmon pole approximation used for the stopping function in a dense electron plasma is given a temperature‐dependent cutoff wavenumber via the ion projectile thermal wavelength. Excepted for projectile inter‐ion distance smaller than the target electron screening length and small ion fragment velocities, featuring a attosecond interaction time with a maximum correlated ion stopping (CIS) in inertial confinement fusion and warm dense matter (WDM), the given procedure is shown to yield back accurately the CIS estimated within the standard random phase approximation framework at any temperature, provided the ion fragment distribution is taken Gaussian.

Structural phase transition, s±-wave pairing, and magnetic stripe order in bilayered superconductor La3Ni2O7 under pressure

Motivated by the recently discovered high-Tc superconductor La3Ni2O7, we comprehensively study this system using density functional theory and random phase approximation calculations. At low pressures, the Amam phase is stable, containing the Y2− mode distortion from the Fmmm phase, while the Fmmm phase is unstable. Because of small differences in enthalpy and a considerable Y2− mode amplitude, the two phases may coexist in the range between 10.6 and 14 GPa, beyond which the Fmmm phase dominates. In addition, the magnetic stripe-type spin order with wavevector (π, 0) was stable at the intermediate region. Pairing is induced in the s±-wave channel due to partial nesting between the M = (π, π) centered pockets and portions of the Fermi surface centered at the X = (π, 0) and Y = (0, π) points. This resembles results for iron-based superconductors but has a fundamental difference with iron pnictides and selenides. Moreover, our present efforts also suggest La3Ni2O7 is qualitatively different from infinite-layer nickelates and cuprate superconductors.