Ionization Energies Of Atoms Research Articles

Simulation of Arc Discharge in an Argon/Methane Mixture, Taking into Account the Evaporation of Anode Material in Problems Related to the Synthesis of Functional Nanostructures.

In this work, within the framework of a self-consistent model of arc discharge, a simulation of plasma parameters in a mixture of argon and methane was carried out, taking into account the evaporation of the electrode material in the case of a refractory and non-refractory cathode. It is shown that in the case of a refractory tungsten cathode, almost the same methane conversion rate is observed, leading to similar values in the density of the main methane conversion products (C, C2, H) at different values of the discharge current density. However, with an increase in the current density, the evaporation rate of copper atoms from the anode increases, and a jump in the I-V characteristic is observed, caused by a change in the plasma-forming ion. This is due to the lower ionization energy of copper atoms compared to argon atoms. In this mode, an increase in metal-carbon nanoparticles is expected. It is shown that, in the case of a cathode made of non-refractory copper, the discharge characteristics and the component composition of the plasma depend on the field enhancement factor near the cathode surface. It is demonstrated that increasing the field enhancement factor leads to more efficient thermal field emission, lowering the cathode's surface temperature and the gas temperature in the discharge gap. This leads to the fact that, in the arc discharge mode with a cathode made of non-refractory copper, the dominant types of particles from which the synthesis of a nanostructure can begin are, in descending order, copper atoms (Cu), carbon clusters (C2), and carbon atoms (C).

Surface structure-based model to calculate thermal and optical properties in nanoscale and quantum dot semiconductors

Surface combination structure was used to design the construction of nano and quantum films, particles, and dots. The created model was applied to tetrahedral semiconductor nanoparticles and quantum dots with a successful performance. It works better than reported experimental data across the whole size range, from the bulk state to the critical size of quantum dots. The model helps to figure out the melting point that changes with the nanosize scale as applied on Si and Sn, which are simple tetrahedral semiconductors, and for CdS and CdSe, which are among II-VI group compounds. It was also used to calculate melting-related parameters such as cohesive energy, Debye temperature, vibrational entropy, and melting enthalpy. The nanosize dependence of the lattice volume and the atom's ionization energy describes the solid surface structure. From the model, an equation was obtained to calculate the energy gaps in Si, CdS, and CdSe particles that are nano- and quantum-dot-sized, and the results are compared to the experimental data that goes with these particles.

Examining the Electron Phase Transformation Theory in the Context of Atomic Structure

The shortcomings of the Rutherford atomic model can be eliminated by the suggested phase transformation of the electrons from point to non-revolving surface charge in the vicinity of the nucleus. The energy balance investigations of this atom model indicated that the stability of the surface charge valence electron shell is ensured by the one-dimensional Casimir effect. If this theoretical prediction is correct then the first ionization energies of the elements should correlate linearly to the inverse of atomic diameter. Classical physics approach, the electrostatic attraction of the nucleus and the repulsion of the surface charge electron shell result in an identical relationship. The problem with the classical physics approach is that it does not offer an adequate explanation for the photoelectric effect and the free electrons inside the metal. Therefore, classical electrostatics cannot be considered the right physical process responsible for the stability of the valence electron/s in neutral atoms. The derived theoretical relationship, between atomic diameter and ionization energy, was tested up to 86 elements of the periodic table. The correlation coefficient is 0.9187. The correlation is stronger for individual periods. The empirical relationship between the ionization energy and atomic radii is well known, resulting in the same correlation coefficients. However, the correlation to the atomic radii does not reproduce the theoretically derived constant multiplier, contrarily to the atomic diameter relationship. Thus, the first ionization energy is the function of the atomic diameter. The uncertainties in the reported atomic sizes are relatively high. Therefore, the correlation between theory and experiments should be considered as excellent. The theoretically derived relationship between the first ionization energy and atomic diameter is the consequence of the proposed phase transformation of the electron. Thus the detected strong correlation between theory and experiments adds further support to the proposed atomic structure.

All-electron basis sets for H to Xe specific for ZORA calculations: Applications in atoms and molecules

Abstract A segmented basis set of quadruple zeta valence quality plus polarization functions (QZP) for H through Xe was developed to be used in conjunction with the ZORA Hamiltonian. This set was augmented with diffuse functions to describe electrons farther away from the nuclei adequately. Using the ZORA-CCSD(T)/QZP-ZORA theoretical model, atomic ionization energies and bond lengths, harmonic vibrational frequencies, and atomization energies of some molecules were calculated. The addition of core-valence corrections has been shown to improve the agreement between theoretical and experimental results for molecular properties. For atomization energies, a similar observation emerges when considering spin-orbit couplings. With the augmented QZP-ZORA set, static mean dipole polarizabilities of a set of atoms were calculated and compared with previously published recommended and experimental values. Performance evaluations of the ZORA and Douglas–Kroll–Hess Hamiltonians were made for each property studied.

A Note on the Binding Energy for Bosons in the Mean-Field Limit

We consider a gas of N weakly interacting bosons in the ground state. Such gases exhibit Bose–Einstein condensation. The binding energy is defined as the energy it takes to remove one particle from the gas. In this article, we prove an asymptotic expansion for the binding energy, and compute the first orders explicitly for the homogeneous gas. Our result addresses in particular a conjecture by Nam (Lett Math Phys 108(1):141–159, 2018), and provides an asymptotic expansion of the ionization energy of bosonic atoms.

Unveiling the physical mechanisms driving delafossite crystal (ABX2) formation through interpretable machine learning.

A method integrating machine learning with first-principles calculations is employed to forecast the formation energy of delafossite crystals, facilitating the rapid identification of stable crystals. This approach identifies several stable candidates and highlights the importance of atomic ionization energy and electron affinity in the formation of delafossite crystals.

Research on the mechanism of interactions between Li/Na/K atoms and electrode materials

As the demand for high-capacity battery materials continues to grow, the exploration of the interaction mechanisms between Li/Na/K atoms and electrode materials has gained tremendous attention. In this study, we introduce a descriptor (ɛɑ) aimed at efficiently identifying high-performance electrode materials, specifically from two-dimensional transition metal chalcogenides and C and N compounds (MXenes). Our density functional theory calculations disclose a robust linear relationship between this descriptor and the adsorption energy (Ead), represented as Ead = ɛɑ + b. The fitting parameters, ɛɑ and b, are individually linked to the inherent properties of the substrate and adsorbate. Explicitly, the descriptor ɛɑ represents the capacity of the electrode material to accommodate an extra electron, while the intercept b is determined by the ionization energy (EIP) of alkali atoms and the coupling energy (Ecp) between the cation to the negatively charged substrate. This finding serves as a practical guide for designing high-capacity battery materials and paves the way for future advancements in this field.

Heterogeneous N-heterocyclic carbenes supported single-atom catalysts for nitrogen fixation: A combined density functional theory and machine learning study

Electrocatalytic nitrogen reduction reaction (NRR) has emerged as a sustainable and eco-friendly alternative for ammonia production at ambient conditions. Exploring highly efficient and selective electrocatalysts for NRR continues to gain significant attention, but remains a challenge. In this work, we conducted a series of single-atom catalysts (SACs) by embedding 29 kinds of transition metal (TM) atoms on the two-dimensional heterogeneous N-heterocyclic carbene, and systematically investigated their catalytic performance for NRR using density functional theory, high-throughput screening, and machine learning. Two promising candidates (TM = Mn and Ta) with high catalytic activity and selectivity were identified, with limiting potentials of - 0.51 and - 0.53 V, respectively. Moreover, considering solvation effects, the limiting potential for Mn was further reduced to -0.43 V. Machinelearning(ML)analysis revealedthat the adsorption energy of N2 emerged as an efficient descriptor for NRR activity, and transition metal atomic Mendeleev number (Nm), the molar volume of TM atoms (Vm) and the 1st ionization energy of TM atoms (Im) were intrinsic to the difference in NRR performance of these SACs. Our findings demonstrate a novel class of efficient SACs based on heterogeneous N-heterocyclic carbene, offering valuable insights for further design of NRR electrocatalysts with exceptional catalytic performance.

Revisited relativistic Dirac-Hartree-Fock X-ray scattering factors. II. Chemically relevant cations and selected monovalent anions for atoms with Z = 3-112.

The previously described approach for determination of the relativistic atomic X-ray scattering factors (XRSFs) at the Dirac-Hartree-Fock level [Olukayode et al. (2023). Acta Cryst. A79, 59-79] has been used to evaluate the XRSFs for a total of 318 species including all chemically relevant cations [Greenwood & Earnshaw (1997). Chemistry of the Elements], six monovalent anions (O-, F-, Cl-, Br-, I-, At-), the ns1np3 excited (valence) states of carbon and silicon, and several exotic cations (Db5+, Sg6+, Bh7+, Hs8+ and Cn2+) for which the chemical compounds have been recently identified, thus significantly extending the coverage relative to all the earlier studies. Unlike the data currently recommended by the International Union of Crystallography (IUCr) [Maslen et al. (2006). International Tables for Crystallography, Vol. C, Section 6.1.1, pp. 554-589], which originate from different levels of theory including the non-relativistic Hartree-Fock and correlated methods, as well as the relativistic Dirac-Slater calculations, the re-determined XRSFs come from a uniform treatment of all species within the same relativistic B-spline Dirac-Hartree-Fock approach [Zatsarinny & Froese Fischer (2016). Comput. Phys. Comm. 202, 287-303] that includes the Breit interaction correction and the Fermi nuclear charge density model. While it was not possible to compare the quality of the generated wavefunctions with that from the previous studies due to a lack (to the best of our knowledge) of such data in the literature, a careful comparison of the total electronic energies and the estimated atomic ionization energies with experimental and theoretical values from other studies instils confidence in the quality of the calculations. A combination of the B-spline approach and a fine radial grid allowed for a precise determination of the XRSFs for each species in the entire 0 ≤ sin θ/λ ≤ 6 Å-1 range, thus avoiding the necessity for extrapolation in the 2 ≤ sin θ/λ ≤ 6 Å-1 interval which, as was shown in the first study, may lead to inconsistencies. In contrast to the Rez et al. work [Acta Cryst. (1994), A50, 481-497], no additional approximations were introduced when calculating wavefunctions for the anions. The conventional and extended expansions were employed to produce interpolating functions for each species in both the 0 ≤ sin θ/λ ≤ 2 Å-1 and 2 ≤ sin θ/λ ≤ 6 Å-1 intervals, with the extended expansions offering a significantly better accuracy at a minimal computational overhead. The combined results of this and the previous study may be used to update the XRSFs for neutral atoms and ions listed in Vol. C of the 2006 edition of International Tables for Crystallography.

Defect physics in 2D monolayer I-VII semiconductor AgI

As a brand new two-dimensional (2D) material with promising electronic properties, monolayer I-VII silver iodide (AgI) has the potential for future 2D electronic devices. To advance the development of such devices, the exploration of n-type and p-type conductivities of AgI is indispensable. With first-principles calculations, we systematically investigate the properties of intrinsic defects and extrinsic dopants in monolayer AgI, including atomic structural pictures, formation energies, and ionization energies to offer carriers. Considering the divergence in energies of charged defects in 2D materials when the traditional jellium scheme is used, we adopt an extrapolation approach to overcome the problem. The Ag vacancy (VAg) and Be substitution on Ag site (BeAg) are found to be the most promising p-type and n-type doping candidates, respectively. They could provide bound carriers for transport through the defect-bound band edge states, although the ionization energies are still larger than thermal energy at room temperature. Furthermore, negative-U behaviors are demonstrated in I vacancy (VI), Zn substitution on Ag site (ZnAg), and Cd substitution on Ag site (CdAg). The present work, for the first time, offers a detailed study of the defect physics in 2D I-VII monolayer semiconductor, laying the foundation for subsequent physics and device explorations based on these brand new 2D materials.

Machine-learning-accelerated screening of single metal atoms anchored on MnPS3 monolayers as promising bifunctional oxygen electrocatalysts.

Searching for bifunctional oxygen electrocatalysts with good catalytic performance to promote the oxygen evolution/reduction reactions (OER/ORR) is of great significance to the development of sustainable and renewable clean energy. Herein, we performed density functional theory (DFT) and machine-learning (DFT-ML) hybrid computations to investigate the potential of a series of single transition metal atoms anchored on the experimentally available MnPS3 monolayer (TM/MnPS3) as the bifunctional electrocatalysts for the ORR/OER. The results revealed that the interactions of these metal atoms with MnPS3 are rather strong, thus guaranteeing their high stability for practical applications. Remarkably, the highly efficient ORR/OER can be achieved on Rh/MnPS3 and Ni/MnPS3 with lower overpotentials than those of metal benchmarks, which can be further rationalized by establishing the volcano and contour plots. Furthermore, the ML results showed that the bond length of TM atoms with the adsorbed O species (dTM-O), the number of d electrons (Ne), the d-center (εd), the radius (rTM) and the first ionization energy (Im) of the TM atoms are the primary descriptors featuring the adsorption behavior. Our findings not only suggest novel highly efficient bifunctional oxygen electrocatalysts, but also provide cost-effective opportunities for the design of single-atom catalysts using the DFT-ML hybrid method.

Iodine electron cyclotron resonance plasma source for electric propulsion

With the rapid development of commercial space in recent years, the low-power and low-cost propulsion systems are needed more and more urgently. Compared with conventional chemical propulsion, electric propulsion has a higher specific impulse. Compared with the conventional xenon propellant, iodine propellant that does not require high pressure storage, is cheap and close to the relative atomic mass and ionization energy of xenon. Electron cyclotron resonance source has the advantages of no internal electrode, low pressure ionization, high plasma density and compact structure, which is suitable for low power electric propulsion. Therefore, the study of low power iodine propellant electron cyclotron resonance plasma source is of great significance. In this study, a set of corrosion-resistant feed system with balanced and stable output of iodine vapor is designed. Then the iodine-corrosion-resistant electron cyclotron resonance thruster is designed completely. A corrosion-resistant coaxial cavity structure is used to feed the microwave to the thruster, and the channel magnetic field is changed into a cusped field to generate more electron cyclotron resonance (ECR) layers. Finally, the combined ignition experiment is successfully conducted, showing the first plasma source using electron cyclotron resonance to ionize iodine propellant that can be used for electric propulsion in the world. The analyses of experiments, static magnetic field, microwave electric field distribution show that the unstable plasma plume scintillation at low power and low flow is caused by the conversion between ordinary wave electron plasmon resonance heating mode and extraordinary wave electron cyclotron resonance heating mode. The decrease of ionization rate at a high flow rate is caused by electron loss, wall loss and electronegativity of iodine propellant. Based on this principle, an improvement scheme is proposed. The plasma source has no obvious damage after discharge, which indicates that it has the potential of long life. This work preliminarily proves that the low power electron cyclotron resonance electric propulsion scheme of low power iodine propellant is feasible.

Oxygen‐Chlorine Chemisorption Scaling for Seawater Electrolysis on Transition Metals: The Role of Redox

AbstractTo clarify what controls species oxidation selectivity in seawater electrolysis, density functional theory (DFT) is used to identify chemisorption enthalpy trends and scaling relations for the simplest relevant adsorbates (O, Cl, and H) on relevant surfaces of 3d transition metals, as well as Pd and Pt, in face‐centered‐cubic and, if different, their ground‐state crystal structures. Approximations are tested for electron exchange‐correlation (XC) and van der Waals interactions to assess their ability to reproduce experimental adsorption enthalpies of H and O on Pt(111). The vdW‐uncorrected generalized gradient approximation to XC of Perdew, Burke, and Ernzerhof (PBE) agrees most closely with experiments. Using DFT‐PBE thereafter, it is determined that the O chemisorption enthalpy on this wide range of transition‐metal surfaces is proportional to the sum of first and second atomic ionization energies, akin to a Born–Haber cycle for a redox reaction, indicating that metal redox activity controls O chemisorption strength. Then it is shown that the O and Cl chemisorption enthalpies are strongly correlated, suggesting that the transition metals considered will oxidize unselectively water and Cl–. This strong correlation appears also for crystal reduction potentials of binary oxides and chlorides, indicating a fundamental challenge for future seawater electrode materials design.

Two-dimensional axisymmetric radiation hydrodynamics model of moderate-intensity nanosecond laser-produced plasmas

A two-dimensional axisymmetric radiation hydrodynamics model has been proposed to simulate nanosecond laser ablation of a solid target in ambient argon, air and helium at different pressures. The heat conduction equation used to simulate the conduction of laser deposition energy in the target and gas dynamic equations to describe the interaction between laser and vapor plasma and the evolution of plasma are coupled through the Knudsen layer relations at the target-vapor interface. A collisional-radiative model including 12 atomic processes is used to calculate the population of atomic energy levels and fractional ion abundance. The internal energy and pressure of the plasma are expressed by the equations of state based on a real gas approximation, which divides the internal energy into the ionization energy, thermal energy, and excitation energy of atoms and ions. The distributions of the temperature, pressure, density and velocity of the target and plasma are calculated by using this model, and the results are analyzed. Experimental results of multiple diagnostic tools including fast photography, shadowgraphy images, spatio-temporally resolved optical emission spectroscopy and laser interferometry, are used to benchmark the simulation results, and satisfactory consistencies are obtained. The model provides a numerical tool to interpret experimental data of a moderate-intensity nanosecond laser ablated solid target when the temperature of the target surface does not reach the critical value.

Electronegativity: A continuing enigma

AbstractThere continues to be confusion concerning the concept of electronegativity. Pauling's original approach, focusing upon an atom in a molecule, continues to be widely invoked. There has also been a more recent tendency to view electronegativity as the negative of the chemical potential and to extend it to molecules. However, this leads to results that are incompatible with chemical experience. A more effective approach, which gives results in overall agreement with Pauling's values, is to relate electronegativity to the average valence electron ionization energies of atoms.

Designing Special Nonmetallic Superalkalis Based on a Cage-like Adamanzane Complexant.

In this study, to examine the possibility of using cage-like complexants to design nonmetallic superalkalis, a series of X@36adz (X = H, B, C, N, O, F, and Si) complexes have been constructed and investigated by embedding nonmetallic atoms into the 36adamanzane (36adz) complexant. Although X atoms possess very high ionization energies, these resulting X@36adz complexes possess low adiabatic ionization energies (AIEs) of 0.78–5.28 eV. In particular, the adiabatic ionization energies (AIEs) of X@36adz (X = H, B, C, N, and Si) are even lower than the ionization energy (3.89 eV) of Cs atoms, and thus, can be classified as novel nonmetallic superalkalis. Moreover, due to the existence of diffuse excess electrons in B@36adz, this complex not only possesses pretty low AIE of 2.16 eV but also exhibits a remarkably large first hyperpolarizability (β 0) of 1.35 × 106 au, indicating that it can also be considered as a new kind of nonlinear optical molecule. As a result, this study provides an effective approach to achieve new metal-free species with an excellent reducing capability by utilizing the cage-like organic complexants as building blocks.

Near-exact non-relativistic ionization energies for many-electron atoms.

Electron–electron interactions and correlations form the basis of difficulties encountered in the theoretical solution of problems dealing with multi-electron systems. Accurate treatment of the electron–electron problem is likely to unravel some nice physical properties of matter embedded in the interaction. In an effort to tackle this many-body problem, a symmetry-dependent all-electron potential generalized for an n-electron atom is suggested in this study. The symmetry dependence in the proposed potential hinges on an empirically determined angular momentum-dependent partitioning fraction for the electron–electron interaction. With the potential, all atoms are treated in the same way regardless of whether they are open or closed shell using their system specific information. The non-relativistic ground-state ionization potentials for atoms with up to 103 electrons generated using the all-electron potential are in reasonable agreement with the existing experimental and theoretical data. The effects of higher-order non-relativistic interactions as well as the finite nuclear mass of the atoms are also analysed.

Exchange-Correlation Functional Comparison of Electronic Energies in Atoms Using a Grid Basis

Calculation of total energies of the electronic ground states of atoms forms the basis for the frozen-core pseudopotentials used in atomistic calculations of much larger scale. Reference values for these energies provide a benchmark for the validation of new software to calculate such potentials. In addition, basic atomic-scale electronic properties such as the (first) ionization energy provide a simple check on the approximation used in the calculation method. We present a comparison of the total energies and ionization energies of atoms Z = 1 - 92 calculated in density functional theory with several levels of exchange-correlation functional and the Hartree-Fock method, comparing ionization energies to experiment. We also investigate the role of relativistic treatment on these energies.

Calculation of radiation dose enhancement by gadolinium compounds for radiation therapy

In this study, we evaluate the features of dose enhancement with Gd contrast agent (Magnevist). Due to the increased relaxation time and high atomic number (z=64) Gd can be used in radiation therapy as a radiosensitizer. To perform a quantitative evaluation of the radiosensitization effect is determined a parameter called the dose enhancement factor - DEF. The DEF values were calculated based on the analysis of the mass absorption coefficients for gadolinium and biological tissue. An increase in DEF is observed when the radiation energy is higher than the K-shell ionization energy of Gd atoms. For the presence of 20315 ppm Gd contrast agent in biological tissue the dose enrichment factor is maximum DEF = 4.12 at photon irradiation energy 60 keV. Also, based on calculations for photon irradiation sources considered high degrees of dose enhancement occur for Am-241, Yb-196, and 100 kVp X-ray tube.

Influence of Gas Type on the Laser Produced Graphite Plasma

Plasma graphite creation by a pulsed Nd: YAG laser with a wavelength of 1064nm to a target in vacuum in two cases (Argon, Air) with varied gas pressures and the resulting spectrum was diagnosed using optical emission spectroscopy for the wavelength range 320-740nm electron temperature Te and electron density ne Debye lengthλD , and plasma frequency f p were calculated. The results showed that increasing the pulse laser energy causes all plasma parameters of both gases under study to increase, as well as a rise in the emission line intensity. The ionization energy of target atoms determines the presence of an element’s atomic and ionic emission lines in the emission spectrum, increase in pressure decreases the electron temperature, and Debye length, also plasma frequency and electron density increase, as it has been proven that the type of gas does not affect the properties of plasma.