Atoms, Volume 9, Issue 4 (December 2021) – 45 articles

The formation and decay of double-core-hole (DCH) states of the neon ion irradiated by an intense electromagnetic x-ray field are studied theoretically. In the present research DCH formation is the result of sequential absorption of two photons with the creation of an intermediate ion. Detailed calculations of the partial decays and probabilities of shake-ups at the atomic and ionic ionization stages are presented. The angular distribution of photoelectrons corresponding to various residual ionic states are calculated. Specifically, we predict the lack of any photoelectrons corresponding to the residual ionic state $1s^{1}2s^{2}2p^{n}m{p}^{n^{\prime }2S_f+1}D$ in the direction of the electric field polarization. Dynamical competition between single-core-hole state decay and excitation is analyzed and pulse parameters corresponding to various dynamical regimes are found. Full article

A detailed study of positron impact elastic scattering from methane and silane is carried out using a model potential consisting of static and polarization potentials. The static potential for the molecular target is obtained analytically by using accurate Gaussian molecular wavefunctions. The molecular orbitals are expressed as a linear combination of Gaussian atomic orbitals. Along with the analytically obtained static potential, a correlation polarization potential is also added to construct the model potential. Utilizing the model potential, the Schrödinger equation is solved using the partial wave phase shift analysis method, and the scattering amplitude is obtained in terms of the phase shifts. Thereafter, the differential, integrated and total cross sections are calculated. These cross-section results are compared with the previously reported measurements and theoretical calculations. Full article

Disorder is everywhere in nature and it has a fundamental impact on the behavior of many quantum systems. The presence of a small amount of disorder, in fact, can dramatically change the coherence and transport properties of a system. Despite the growing interest in this topic, a complete understanding of the issue is still missing. An open question, for example, is the description of the interplay of disorder and interactions, which has been predicted to give rise to exotic states of matter such as quantum glasses or many-body localization. In this review, we will present an overview of experimental observations with disordered quantum gases, focused on one-dimensional bosons, and we will connect them with theoretical predictions. Full article

The resonant profile of the rate coefficient for three-body recombination into a shallow dimer is investigated for mass-imbalanced systems. In the low-energy limit, three atoms collide with zero-range interactions, in a regime where the scattering lengths of the heavy–heavy and the heavy–light subsystems are positive and negative, respectively. For this physical system, the adiabatic hyperspherical representation is combined with a fully semi-classical method and we show that the shallow dimer recombination spectra display an asymmetric lineshape that originates from the coexistence of Efimov resonances with Stückelberg interference minima. These asymmetric lineshapes are quantified utilizing the Fano profile formula. In particular, a closed-form expression is derived that describes the width of the corresponding Efimov resonances and the Fano lineshape asymmetry parameter q. The profile of Efimov resonances exhibits a $q-$reversal effect as the inter- and intra-species scattering lengths vary. In the case of a diverging asymmetry parameter, i.e., $\left|q\right|\to \infty$, we show that the Efimov resonances possess zero width and are fully decoupled from the three-body and atom–dimer continua, and the corresponding Efimov metastable states behave as bound levels. Full article

The polarization dependence of the photoionization probability was analyzed in the case when a randomly oriented atom is irradiated by two crossing polarized monochromatic photon beams with the same frequency. It was found that the angular distributions of photoelectrons exhibit the effect of circular dichroism (CD), which consists of the dependence of the photoionization probability on the sign of the circular polarization degree of each beam. We demonstrate that the CD effect exists only for coherent crossing photon beams. It was shown that CD effects are strongly dependent on the phase difference between the electric field vectors of the photon beams and have a quite large magnitude. The possibilities of the experimental observation of CD effects are discussed. Full article

I met Oleg Zatsarinny in 2001, and he then worked with me at Western Michigan University for two years. From 2003 to 2013, we were coauthors of 15 papers on theoretical atomic physics, and maintained a friendly relationship over twenty years, meeting and socializing often at conferences. Further elaboration follows below. Full article

Recently it was shown that anyons on the two-sphere naturally arise from a system of molecular impurities exchanging angular momentum with a many-particle bath (Phys. Rev. Lett. 126, 015301 (2021)). Here we further advance this approach and rigorously demonstrate that in the experimentally realized regime the lowest spectrum of two linear molecules immersed in superfluid helium corresponds to the spectrum of two anyons on the sphere. We develop the formalism within the framework of the recently experimentally observed angulon quasiparticle. Full article

We have studied the angular time delay in slow-electron elastic scattering by spherical targets as well as the average time delay of electrons in this process. It is demonstrated how the angular time delay is connected to the Eisenbud–Wigner–Smith (EWS) time delay. The specific features of both angular and energy dependencies of these time delays are discussed in detail. The potentialities of the derived general formulas are illustrated by the numerical calculations of the time delays of slow electrons in the potential fields of both absolutely hard-sphere and delta-shell potential well of the same radius. The conducted studies shed more light on the specific features of these time delays. Full article

Heavy atoms present challenges to atomic theory calculations due to the large number of electrons and their complicated interactions. Conventional approaches such as calculations based on Cowan’s code are limited and require a large number of parameters for energy agreement. One promising approach is relativistic configuration-interaction and many-body perturbation theory (CI-MBPT) methods. We present CI-MBPT results for various atomic systems where this approach can lead to reasonable agreement: La I, La II, Th I, Th II, U I, Pu II. Among atomic properties, energies, g-factors, electric dipole moments, lifetimes, hyperfine structure constants, and isotopic shifts are discussed. While in La I and La II accuracy for transitions is better than that obtained with other methods, more work is needed for actinides. Full article

Cross sections for electron scattering from atomic and molecular iodine are calculated based on the R-matrix (close-coupling) method. Elastic and electronic excitation cross sections are presented for both I and I${}_2$. The dissociative electron attachment and vibrational excitation cross sections of the iodine molecule are obtained using the local complex potential approximation. Ionization cross sections are also computed for I${}_2$ using the BEB model. Full article

Results of experimental and theoretical investigation of electron-impact excitation of the $6s^{2}6d\hspace{0.17em}D_2^{}\to 6s^{2}6p\hspace{0.17em}P_2^{}{}^{\mathrm{o}}$ spectral transitions from the ground $6s^{2}6p\hspace{0.17em}P_2^{}{}_{1/2}^{\mathrm{o}}$ level in the Pb⁺ ion are presented. The experimental excitation functions for the transitions, measured by a VUV spectroscopy method, using the crossed electron and ion beams technique, reveal a rather distinct resonance structure resulting mainly from the electron decay of both atomic and ionic autoionizing states. The absolute values of the emission cross-sections, obtained by normalizing the experimental data at the incident electron energy 100 eV by those calculated using the Flexible Atomic Code software package, were found to be (0.35 ± 0.17) × 10^–16 cm² for the $6s^{2}6d\hspace{0.17em}D_2^{}{}_{3/2}$ → $6s^{2}6p\hspace{0.17em}P_2^{}{}_{1/2}^{\mathrm{o}}$ (λ143.4 nm) transition and (0.19 ± 0.09) × 10^–16 cm² for the $6s^{2}6d\hspace{0.17em}D_2^{}{}_{5/2}$ → $6s^{2}6p\hspace{0.17em}P_2^{}{}_{3/2}^{\mathrm{o}}$ (λ182.2 nm) transition. Full article

Polar radioactive molecules have been suggested to be exceptionally sensitive systems in the search for signatures of symmetry-violating effects in their structure. Radium monofluoride (RaF) possesses an especially attractive electronic structure for such searches, as the diagonality of its Franck-Condon matrix enables the implementation of direct laser cooling for precision experiments. To maximize the sensitivity of experiments with short-lived RaF isotopologues, the molecular beam needs to be cooled to the rovibrational ground state. Due to the high kinetic energies and internal temperature of extracted beams at radioactive ion beam (RIB) facilities, in-flight rovibrational cooling would be restricted by a limited interaction timescale. Instead, cooling techniques implemented on ions trapped within a radiofrequency quadrupole cooler-buncher can be highly efficient due to the much longer interaction times (up to seconds). In this work, the feasibility of rovibrationally cooling trapped RaF${}^{+}$ and RaH${}^{+}$ cations with repeated laser excitation is investigated. Due to the highly diagonal nature between the ionic ground state and states in the neutral system, any reduction of the internal temperature of the molecular ions would largely persist through charge-exchange without requiring the use of cryogenic buffer gas cooling. Quasirelativistic X2C and scalar-relativistic ECP calculations were performed to calculate the transition energies to excited electronic states and to study the nature of chemical bonding for both RaF${}^{+}$ and RaH${}^{+}$. The results indicate that optical manipulation of the rovibrational distribution of trapped RaF${}^{+}$ and RaH${}^{+}$ is unfeasible due to the high electronic transition energies, which lie beyond the capabilities of modern laser technology. However, more detailed calculations of the structure of RaH${}^{+}$ might reveal possible laser-cooling pathways. Full article

We introduce two models for the computation of direct ionization cross sections by positron impact over a wide range of collision energies. The models are based on the binary-encounter-Bethe model and take into account an extension of the Wannier theory. The cross sections computed with these models show good agreement with experimental data. The extensions improve the agreement between theory and experiment for collision energies between the first ionization threshold and the peak of the cross section. The models are based on a small set of parameters, which can be computed with standard quantum chemistry program packages. Full article

Optical emission spectroscopy has been widely used in low-temperature argon plasma diagnostics. A coronal model is usually used to analyze the measured line ratios for diagnostics with a single temperature and density. However, many plasma processing conditions deviate from single temperature and density, optically thin conditions, or even coronal plasma conditions due to cascades from high-lying states. In this paper, we present a collisional-radiative model to investigate the validity of coronal approximations over a range of plasma conditions of T${}_e$ = 1–4 eV and N${}_e$ = 10${}^8$–10${}^{13}$ cm${}^{-3}$. The commonly used line ratios are found to change from a coronal limit where they are independent of N${}_e$ to a collisional-radiative regime where they are not. The effects of multiple-temperature plasma, radiation trapping, wall neutralization, and quenching on the line ratios are investigated to identify the plasma conditions under which these effects are significant. This study demonstrates the importance of the completeness of atomic datasets in applying a collisional-radiative model to low-temperature plasma diagnostics. Full article

The accuracy of the most recent recommended cross sections dataset for electron scattering from gaseous H₂O (J. Phys. Chem. Ref. Data 2021, 50, 023103) is probed in a joint experimental and computational study. Simulations of the magnetically confined electron transport through a gas cell containing H₂O for different beam energies (3, 10 and 70 eV) and pressures (2.5 to 20.0 mTorr) have been performed by using a specifically designed Monte Carlo code. The simulated results have been compared with the corresponding experimental data as well as with simulations performed with Geant4DNA. The comparison made between the experiment and simulation provides insight into possible improvement of the recommended dataset. Full article

More than one hundred years of experimental and theoretical investigations of electron scattering in gases delivered cross-sections in a wide energy range, from few meV to keV. An analogy in optics, characterizing different materials, comes under the name of the dispersion relation, i.e., of the dependence of the refraction index on the light wavelength. The dispersion relation for electron (and positron) scattering was hypothesized in the 1970s, but without clear results. Here, we review experimental, theoretical, and semi-empirical cross-sections for N${}_2$, CO${}_2$, CH${}_4$, and CF${}_4$ in search of any hint for such a relation—unfortunately, without satisfactory conclusions. Full article

Recently, there has been increased interest in developing advanced bright sources for lithography. Sn ions are particularly promising due to their bright emission spectrum in the required wavelength range. Cowan’s code has been used to model the emission; however, it has adjustable parameters, which limit its predictive power, and it has limited relativistic treatment. Here, we present calculations based on ab initio relativistic configuration-interaction many-body perturbation theory (CI-MBPT), with relativistic corrections included at the Dirac-Fock level and core-polarization effects with the second-order MBPT. As a proof of principle that the theory is generally applicable to other Sn ions with proper development, we focused on one ion where direct comparison with experimental observations is possible. The theory can also be used for ions of other elements to predict emissions for optimization of plasma-based bright sources. Full article

In this paper, the Accelerator Driven Subcritical Reactor (ADSR) was simulated based on the structure of the TRIGA-Mark II reactor by the MCNPX program. The proton beam interacts on the Pb-Bi molten target with various energy levels from 0.5 GeV to 2.0 GeV. The important neutron parameters to evaluate the operability of ADSR were calculated as: the neutron yields according to various thicknesses of the target and according to the energy of the incident proton beam; the effective neutron multiplication factor for various fuel mixtures, along with its stability for some fuel mixtures; the axial and radial distributions of the neutron flux along with the height and radius of the core. The obtained results had shown a good agreement in using Pb-Bi molten as the interaction target and coolant for ADSR. Full article

The Dirac B-spline R-matrix (DBSR) method is employed to treat low-energy electron collisions with thallium atoms. Special emphasis is placed on spin polarization phenomena that are investigated through calculations of the differential cross-section and the spin asymmetry function. Overall, good agreement between the present calculations and the available experimental measurements is found. The contributions of electron exchange to the spin asymmetry cannot be ignored at low impact energies, while the spin–orbit interaction plays an increasingly significant role as the impact energy rises. Full article

Beam-foil EUV spectra of elements from Na through Cl are presented, partly in survey spectra and partly in detail spectra. The ionization stages of interest are medium to high, so that three to thirteen electrons remain. Research topics are outlined and the problems of the measurement technique discussed. Full article

In a mixture of two kinds of identical bosons, there are two types of pairs: identical bosons’ pairs, of either species, and pairs of distinguishable bosons. In the present work, the fragmentation of pairs in a trapped mixture of Bose–Einstein condensates is investigated using a solvable model, the symmetric harmonic-interaction model for mixtures. The natural geminals for pairs made of identical or distinguishable bosons are explicitly contracted by diagonalizing the intra-species and inter-species reduced two-particle density matrices, respectively. Properties of pairs’ fragmentation in the mixture are discussed, the role of the mixture’s center-of-mass and relative center-of-mass coordinates is elucidated, and a generalization to higher-order reduced density matrices is made. As a complementary result, the exact Schmidt decomposition of the wave function of the bosonic mixture is constructed. The entanglement between the two species is governed by the coupling of their individual center-of-mass coordinates, and it does not vanish at the limit of an infinite number of particles where any finite-order intra-species and inter-species reduced density matrix per particle is 100% condensed. Implications are briefly discussed. Full article

We report on an extensive semi-empirical analysis of scattering cross-sections for electron elastic collision with noble gases via the Markov Chain Monte Carlo-Modified Effective Range Theory (MCMC−MERT). In this approach, the contribution of the long-range polarization potential (∼$r^{-4}$) to the scattering phase shifts is precisely expressed, while the effect of the complex short-range interaction is modeled by simple quadratic expression (the so-called effective range expansion with several adjustable parameters). Additionally, we test a simple potential model of a rigid sphere combined with $r^{-4}$ interaction. Both models, the MERT and the rigid sphere are based on the analytical properties of Mathieu functions, i.e., the solutions of radial Schrödinger equation with pure polarization potential. However, in contrast to MERT, the rigid sphere model depends entirely upon one adjustable parameter—the radius of a hard-core. The model’s validity is assessed by a comparative study against numerous experimental cross-sections and theoretical phase shifts. We show that this simple approach can successfully describe the electron elastic collisions with helium and neon for energies below 1 eV. The purpose of the present analysis is to give insight into the relations between the parameters of both models (that translate into the cross-sections in the very low energy range) and some “macroscopic” features of atoms such as the polarizability and atomic “radii”. Full article

The paper presents an analysis of data on the cross sections of electron impact ionization of atoms of alkali metals, hydrogen, noble gases, some transition metals and Al, Fe, Ni, W, Au, Hg, U. For the selected sets of experimental and theoretical data, an optimal analytical formula is found and approximation coefficients are calculated. The obtained semi-empirical formula reproduces the values of the ionization cross sections in a wide range of energies with an accuracy of the order of error of the available theoretical and experimental data. Full article

We have explored the chemical space of BAl${}_4$Mg${}^{-/0/+}$ for the first time and theoretically characterized several isomers with interesting bonding patterns. We have used chemical intuition and a cluster building method based on the tabu-search algorithm implemented in the Python program for aggregation and reaction (PyAR) to obtain the maximum number of possible stationary points. The global minimum geometries for the anion (1a) and cation (1c) contain a planar tetracoordinate boron (ptB) atom, whereas the global minimum geometry for the neutral (1n) exhibits a planar pentacoordinate boron (ppB) atom. The low-lying isomers of the anion (2a) and cation (3c) also contain a ppB atom. The low-lying isomer of the neutral (2n) exhibits a ptB atom. Ab initio molecular dynamics simulations carried out at 298 K for 2000 fs suggest that all isomers are kinetically stable, except the cation 3c. Simulations carried out at low temperatures (100 and 200 K) for 2000 fs predict that even 3c is kinetically stable, which contains a ppB atom. Various bonding analyses (NBO, AdNDP, AIM, etc.) are carried out for these six different geometries of BAl${}_4$Mg${}^{-/0/+}$ to understand the bonding patterns. Based on these results, we conclude that ptB/ppB scenarios are prevalent in these systems. Compared to the carbon counter-part, CAl${}_4$Mg${}^{-}$, here the anion (BAl${}_4$Mg${}^{-}$) obeys the 18 valence electron rule, as B has one electron fewer than C. However, the neutral and cation species break the rule with 17 and 16 valence electrons, respectively. The electron affinity (EA) of BAl${}_4$Mg is slightly higher (2.15 eV) than the electron affinity of CAl${}_4$Mg (2.05 eV). Based on the EA value, it is believed that these molecules can be identified in the gas phase. All the ptB/ppB isomers exhibit $\pi$/$\sigma$ double aromaticity. Energy decomposition analysis predicts that the interaction between BAl${}_4^{-/0/+}$ and Mg is ionic in all these six systems. Full article

Many-body physics poses one of the greatest challenges to science in the 21st century. Still more daunting is the problem of accurately calculating the properties of quantum many-body systems in the strongly correlated regime. Cold atomic gases provide an excellent test ground, for both experimentalists and theorists, to study the exotic and sometimes counterintuitive behavior of quantum many-body problems. Of particular interest is the appearance of collective excitations in these systems, such as the famous Goldstone mode and the elusive Higgs mode. It is particularly important to assess the robustness of theoretical and computational techniques to study such excitations. We build on the unprecedented opportunity provided by the fact that, in some cases, exact numerical predictions can be obtained through quantum Monte Carlo. We use these predictions to assess the accuracy of the Random Phase Approximation, which is widely considered to be a method of choice for the study of the collective excitations in a cold atomic Fermi gas modeled with a Fermi–Hubbard Hamiltonian. We found good agreement between the two methodologies for the dynamic properties, particularly for the position of the Goldstone mode. We also explored the possibility of using a renormalized, effective potential in place of the physical potential. We determined that using a renormalized potential is likely too simplistic a method for improving the accuracy of generalized Random Phase Approximation and that a more sophisticated approach is needed. Full article

The approximate solution of the nonlinear Thomas–Fermi (TF) equation for ions is found by the Fermi method. The solution is based on the new asymptotic representation of the TF ion size valid for any ionization degree. The two universal functions and their derivatives, introduced by Fermi, are calculated by recent effective algorithms for the Emden–Fowler type equations with the accuracy sufficient for majority of applications. The comparison of our results with those obtained previously shows high accuracy and validity for arbitrary values of ionization degree. This study could potentially be of interest for the statistical TF method applications in physics and chemistry. Full article

Polarizabilities and hyperpolarizabilities, α₁, β₁, γ₁, α₂, β₂, γ₂, α₃, β₃, γ₃, δ and ε of hydrogenic systems have been calculated in the presence of a Debye–Huckel potential, using pseudostates for the S, P, D and F states. All of these converge very quickly as the number of terms in the pseudostates is increased and are essentially independent of the nonlinear parameters. All the results are in good agreement with the results obtained for hydrogenic systems obtained by Drachman. The effective potential seen by the outer electron is −α₁/x⁴ + (6β₁ − α₂)/x⁶ + higher-order terms, where x is the distance from the outer electron to the nucleus. The exchange and electron–electron correlations are unimportant because the outer electron is far away from the nucleus. This implies that the conventional variational calculations are not necessary. The results agree well with the results of Drachman for the screening parameter equal to zero in the Debye–Huckel potential. We can calculate the energies of Rydberg states by using the polarizabilities and hyperpolarizabilities in the presence of Debye potential seen by the outer electron when the atoms are embedded in a plasma. Most calculations are carried out in the absence of the Debye–Huckel potential. However, it is not possible to carry out experiments when there is a complete absence of plasma at a particular electron temperature and density. The present calculations of polarizabilities and hyperpolarizabilities will provide accurate results for Rydberg states when the measurements for such states are carried out. Full article

Gathering data on electron collisions in plasmas is a vital part of conducting plasma simulations. However, data on neutral radicals and neutrals formed in the plasma by reactions between different radicals are usually not readily available. While these cross-sections can be calculated numerically, this is a time-consuming process and it is not clear from the outset which additional cross-sections are needed for a given plasma process. Hence, identifying species for which additional cross-sections are needed in advance is highly advantageous. Here, we present a structured approach to do this. In this, a chemistry set using estimated data for unknown electron collisions is run in a global plasma model. The results are used to rank the species with regard to their influence on densities of important species such as electrons or neutrals inducing desired surface processes. For this, an algorithm based on graph theory is used. The species ranking helps to make an informed decision on which cross-sections need to be calculated to improve the chemistry set and which can be neglected to save time. The validity of this approach is demonstrated through an example in an SF${}_6$/O${}_2$ plasma. Full article