Ionization Energies of Ions in Hot and Dense Plasma: Beryllium-Like Ions for Z=26-36

Ionization energies of beryllium-like ions for Z = 26 - 36 in hot ana aense plasmas （ne=10^22 -10^24 cm^-3,kT= 500 - 2000 eV） are obtained by using an approach developed for electronic structure and transition property of ions in hot and dense plasmas based on the multi-configuration Dirac-Fock model. Influence of the plasma environment is considered by introducing a correction to the one-electron potential to account for the screening of the ionized electrons. This correction is calculated from the ionized electron micro-space distribution, which is obtained based on an ＂average atom model for the temperature and density-dependent average ionization of atoms in plasmas. Comparison between the present and the ion sphere models is made to display the significance of the ionized electron micro-space distribution.     

Accurate One-Centre Method for Hydrogen Molecule Ions in Strong Magnetic Field

An accurate one-centre method for the hydrogen molecule ion is tested. The slow convergence and singularities at the nuclear positions that are problems in the general one-centre method axe solved well by employing the optimal radial and angular B-spline basis. Therefore, the accuracy of the one-centre method is improved observably. For the ground state of the H2^＋ in the free field, 7 ×10^-8 accuracy is obtained, which rivals the best one-centre calculation before. As a test, the nuclear distances and the total energies of the 1σ g,u, 1πu, 1δ9,u and 2σg states of the H2^＋ for the magnetic field strength B = 1 a.u. are also obtained. Compared to other results, five-digit accuracy at least can be arrived even for the antibonding states 1σu and 1σu, whose equilibrium distances R is very large.     

Light-matter interactions within the Ehrenfest–Maxwell–Pauli–Kohn–Sham framework: fundamentals,implementation, and nano-optical applications

In recent years significant experimental advances in nano-scale fabrication techniques and in available light sources have opened the possibility to study a vast set of novel light-matter interaction scenarios, including strong coupling cases. In many situations nowadays, classical electromagnetic modeling is insufficient as quantum effects, both in matter and light, start to play an important role. Instead, a fully self-consistent and microscopic coupling of light and matter becomes necessary. We provide here a critical review of current approaches for electromagnetic modeling, highlighting their limitations. We show how to overcome these limitations by introducing the theoretical foundations and the implementation details of a density-functional approach for coupled photons, electrons, and effective nuclei in non-relativistic quantum electrodynamics. Starting point of the formalism is a generalization of the Pauli–Fierz field theory for which we establish a one-to-one correspondence between external fields and internal variables. Based on this correspondence, we introduce a Kohn-Sham construction which provides a computationally feasible approach for ab-initio light-matter interactions. In the mean-field limit, the formalism reduces to coupled Ehrenfest–Maxwell–Pauli–Kohn–Sham equations. We present an implementation of the approach in the real-space real-time code Octopus using the Riemann–Silberstein formulation of classical electrodynamics to rewrite Maxwell's equations in Schrödinger form. This allows us to use existing very efficient time-evolution algorithms developed for quantum-mechanical systems also for Maxwell's equations. We show how to couple the time-evolution of the electromagnetic fields self-consistently with the quantum time-evolution of the electrons and nuclei. This approach is ideally suited for applications in nano-optics, nano-plasmonics, (photo) electrocatalysis, light-matter coupling in 2D materials, cases where laser pulses carry orbital angular momentum, or light-tailored chemical reactions in optical cavities just to name but a few.     

Application of Complete Orthonormal Sets of Ψα-Exponential-Type Orbitals to Accurate Ground and Excited States Calculations of One-Electron Diatomic Molecules Using Single-Zeta Approximation

The applicability of the complete orthonormal sets of ψ^a-exponential-type orbitals introduced by one of the authors to the study of electronic structure of one electron diatomic molecules is demonstrated using single-zeta approximation. As an example of application, tile calculations have been performed for o, 7r and 5 states of one electron homo- and hetero-nucleac diatomic molecules H＋2 and Hell2＋, respectively. The calculation results are presented. The values for these molecules obtained in eight-digit accuracy ace close to the results of solution presented in literature.     

Molecules in clusters: The case of planar LiBeBCNOF built from a triangular form LiOB and a linear four-center species FBeCN

Krüger some years ago proposed a cluster LiBeBCNOF, now called periodane. His ground-state isomer proposal has recently been refined by Bera et al. using DFT. Here, we take the approach of molecules in such a cluster as starting point. We first study therefore the triangular molecule LiOB by coupled cluster theory (CCSD) and thereby specify accurately its equilibrium geometry in free space. The second fragment we consider is FBeCN, but treated now by restricted Hartree-Fock (RHF) theory. This four-center species is found to be linear, and the bond lengths are obtained from both RHF and CCSD calculations. Finally, we bring these two entities together and find that while LiOB remains largely intact, FBeCN becomes bent by the interaction with LiOB. Hartree-Fock and CCSD theories then predict precisely the same lowest isomer found by Bera et al. solely on the basis of DFT.     

Electronic structure and driving forces in α-cyclodextrin:butylparaben inclusion complexes

We investigate the geometry and electronic structure for complexes of α-cyclodextrin with butylparaben using DFT and Hartree-Fock calculations. The effect of solvent is explicitly taken into account. A Morokuma-Kiatura analysis of the bond energy is performed. We emphasize the role of the water, by pointing out the changes in the solvent's electronic structure for different docking geometries.     

Importance of Relativistic Effects for Intermediate-Z Elements： Photoionization Process of Excited Na

Using a modified R-matrix code, the fine-structure-resolved partial photoionization cross sections of excited Na （Z = 11） are calculated within the Breit-Pauli approximation. Our calculated energy levels of Na＋ and Na are in good agreement with the experimental values within 1% and the branching ratios of the J-resolved partial cross sections are consistent with the recent measurements within the experimental uncertainties. The agreements are impossible to be obtained without adequately taking into account the relativistic effects and the electron correlations together. Therefore, even for the intermediate-Z elements （e.g. Na with Z = 11）, the relativistic effects （mainly the spin-orbit interactions） should not be neglected.     

Optical properties of small silver clusters supported at MgO

We present structural and optical properties of silver clusters Ag_n (n=2, 4, 6, 8) at two model support sites of MgO, stoichiometric MgO(100) and F_S-center defect, based on density functional theory and embedded cluster model. Our results provide the mechanism responsible for the absorption and emission patterns due to the specific interaction between the excitations within the cluster and the support site which is strongly cluster size and structure dependent. We propose Ag₄ at stoichiometric site as well as Ag₂, Ag₄ and Ag₆ at F_S-center defects as good candidates for the emissive centers in the visible regime.     

Electron density and Fisher information of Dirac-Fock atoms

Numerical calculations on the gradient and Laplacian forms of the position space Fisher information measure are reported using the 1-normalised Dirac-Fock densities (shape function), σ(r), for atoms H-Lr. It is shown that the difference in effective electrostatic potentials, corresponding to the gradient and the Laplacian form of Fishers' information, is completely defined by the shape function (the density per particle) at the nucleus, σ(r=0). The influence of relativistic effects on the Fisher information is recovered for the first time.     

Electronic structure of Li3GaN2

First principles calculations, by means of the full-potential linearized augmented plane wave method within the local density approximation, were carried out for the electronic properties of Li₃GaN₂. The calculated lattice parameter is in good agreement with the measured one. The bandgap is direct at the Brillouin zone centre. The Li-N and Ga-N bonds are both ionic with a small covalent character of the latter one.     

Precision Calculations of Atomic Polarizabilities: A Relevant Physical Quantity in Modern Atomic Frequency Standard

Electric dipole polarizabilities of atoms are very important in many different physical applications, such as the precision atomic frequency standard. Calculations of these properties are very important and challenging. We propose a calculation strategy to calculate the frequency dependent dipole polarizabilities with high precision variationally by using a set of high quality orbital bases where the electron correlations can be taken into account adequately. The static polarizabilitiez of the ground state of Na are calculated accurately by such a method and can be compared with precision experiment measurement directly. The calculation result is in excellent agreement with the available experimental measurements within about 0.1~, which demonstrates the validity of our strategy. Our calculation strategy has a wide usage, not only in polarizibilies, but also in other fields such as theoretical treatment of electron-atom scattering processes. Using the same orbital bases, we carry out precision calculation of Na- affinities. Our calculated affinity is in excellent agreement with precision laser spectroscopy measurements within 0. 1%.     

Atomic Layer Deposition of Al2O3 on H-Passivated GeSi： Initial Surface Reaction Pathways with H/GeSi（100）-2 × 1

The reaction mechanisms of Al（CH3 ）3 （TMA） adsorption on H-passivated GeSi（100）-2 × 1 surface are investigated with density functional theory. The Si-Ge and Ge-Ge one-dimer cluster models are employed to represent the GeSi（100）-2 × 1 surface with different Ge compositions. For a Si-Ge dimer of a H-passivated SiGe surface, TMA adsorption on both Si-H^＊ and Ge-H^＊ sites is considered. The activation barrier of TMA with the Si-H^＊ site （1.2eV） is higher than that of TMA with the Ge-H^＊ site （0.91 eV）, which indicates that the reaction proceeds more slowly on the Si-H^＊ site than on the Ge-H^＊ site. In addition, adsorption of TMA is more energetically favorable on the Ge-Ge dimer than on the Si-Ge dimer of H-passivated SiGe.     

Rényi information of atoms

Position and momentum space Rényi information of order α has been studied within a Hartree-Fock framework for 103 neutral atoms, 54 singly charged cations and 43 anions in their ground state. The values of α?1 (α?1) stress the shell structure for position-space (momentum-space) Rényi information. The relationship between the complexity and Rényi information is also studied.     

Stability of asymmetric tetraquarks in the minimal-path linear potential

The linear potential binding a quark and an antiquark in mesons is generalized to baryons and multiquark configurations as the minimal length of flux tubes neutralizing the color, in units of the string tension. For tetraquark systems, i.e., two quarks and two antiquarks, this involves the two possible quark–antiquark pairings, and the Steiner tree linking the quarks to the antiquarks. A novel inequality for this potential demonstrates rigorously that within this model the tetraquark is stable in the limit of large quark-to-antiquark mass ratio.     

Theory of complete orthonormal sets of relativistic tensor wave functions and Slater tensor orbitals of particles with arbitrary spin in position, momentum and four-dimensional spaces

Using the complete orthonormal basis sets of nonrelativistic and quasirelativistic orbitals introduced by the author in previous papers for particles with arbitrary spin the new analytical relations for the 2(2s+1)-component relativistic tensor wave functions and Slater tensor orbitals in position, momentum and four-dimensional spaces are derived, where s=1/2,1,3/2,2,… . The relativistic tensor function sets are expressed through the corresponding nonrelativistic and quasirelativistic orbitals. The analytical formulas for overlap integrals over relativistic Slater tensor orbitals in position space are also derived.     

Molecular Dynamics Simulation of Bubble Nucleation in Explosive Boiling

Molecular dynamics （MD） simulation is carried out for the bubble nucleation of liquid nitrogen in explosive boiling. The heat is transferred into the simulation system by rescaling the velocity of the molecules. The results indicate that the initial equilibrium temperature of liquid and molecular cluster size affect the energy conversion in the process of bubble nucleation. The potential energy of the system violently varies at the beginning of the bubble nucleation, and then varies around a fixed value. At the end of bubble nucleation, the potential energy of the system slowly increases. In the bubble nucleation of explosive boiling, the lower the initial equilibrium temperature, the larger the size of the molecular cluster, and the more the heat transferred into the system of the simulation cell, causing the increase potential energy in a larger range.     

Theoretical investigation of the O2 adsorption effect in the electron transport of single Fe-porphyrin molecule

The effect of O₂ adsorption on the electron transport behavior of Fe-porphyrin molecule is investigated by the first-principles computational approach. The current-voltage characteristics of Fe-porphyrin and O₂ adsorbed Fe-porphyrin between gold electrodes are calculated. We find that the conductance of the Fe-porphyrin decreases dramatically upon the adsorption of O₂, which suggests that this system has potential application as a molecular sensor or a switch. This switching-behavior is analyzed from the evolutions of the transmission spectra and the molecular projected self-consistent Hamiltonian states of the molecular systems.     

Density functional theory investigation of S2 in KCl: evidence for the existence of a di-vacancy site

Electron paramagnetic resonance experiments have shown that, depending on the doping procedure, two different S₂⁻ centers may coexist in KCl. These centers have the ²B_2g and the ²B_3g ground state, respectively. As no experimental ligand hyperfine data are available, it could not be determined whether the S₂⁻ molecular ion replaces a single halide ion (mono-vacancy site) or two nearest neighbor halide ions (di-vacancy site). Also, other defect models could a priory be considered. In this work, cluster in vacuo density functional theory calculations of the g and ³³S hyperfine tensors show that the S₂⁻ ion at a mono-vacancy site has the ²B_2g ground state, whereas S₂⁻ in a di-vacancy exhibits a ²B_3g ground state. For the latter center, the possibility of charge compensation by a cation vacancy is also considered. The calculations indicate that a possible vacancy is not in the direct vicinity (nearest or next-nearest neighbor) of the S₂⁻ ion.     

Theoretical Study of Interesting Fine-Structure Splittings for 23P0, 1, 2 States along Helium Isoelectronic Sequence

Using the multi-configuration Dirac Fock method including the Breit interactions and QED corrections, we calculate the fine-structure energy levels of the 2^3 Po, 1,2 states along the helium isoelectronic sequence with atomic number up to Z = 36, where LS-coupling is appropriate. Our calculation results agree with the experimental results within about 1%. We elucidate the mechanism of the interesting fine-structure splittings for the 2^3Po,1,2 states along the helium isoelectronic sequence, i.e. the competitions between the spin-orbit interactions and the Breit interactions which represent the relativistic retardation effect of electromagnetic interactions.