Electron-electron Correlation Effects Research Articles

Electronic Nature and Thermoelectric Characteristics of Cubic LaPb3 LaIn3 and LaTl3 Compounds: B3PW91 Approach

In this paper the structural, electronic and transport properties of the strongly correlated intermetallics LaX3 (X=Pb, In and Tl) in the space group Pm-3m (221) have been investigated using B3PW91 hybrid functional within the framework of density functional theory. These compounds have 4f orbitals and hence strong electron-electron correlation effect is expected, therefore, the electronic properties are also calculated with the B3PW91 hybrid functional and the effect of B3PW91 hybrid functional on the density of states is discussed in details. The band structure and density of states, demonstrate the metallic nature of these compounds. Using the semi-empirical Boltzmann’s approach implemented in the BoltzTraP code, the transport parameters, such as the Seebeck coefficient, electrical conductivity, thermal conductivity and figure of merit as a function of the chemical potential are computed at a temperature gradient of 500 K. For all materials the thermal and electrical conductivities, and Seebeck coefficient has higher values for n-type doping in comparison with p-type doping. The moderate values of figure of merit obtained for these materials indicate that these materials have applicability where small values of thermoelectric efficiency are required and higher values can harm the process but need experimental verification. LaIn3 has the highest value of electrical conductivity per relaxation time and thermal conductivity per relaxation time are 9.43 x 1020 1/Ωms and 107.65 x 1014 W/mKs respectively. LaTl3 has the highest figure of merit among these materials.

Theoretical Studies of the Electronic and Thermoelectric Properties of PrIn3 and NdIn3 in Cubic Phase

The electronic and thermoelectric properties of AB3 (A =Pr, Nd and B=In) materials (crystallizing in the cubic structure) having space group Pm-3m (221) are studied using B3PW91 hybrid functional through the Full-Potential Linear Augmented Plane Wave (FP-LAPW) approach within the framework of Density Functional Theory (DFT). The calculated lattice parameters for PrIn3 and NdIn3 are 4.5668 Å and 4.5539 Å respectively. Electron-electron correlation effect is due to the 4f orbitals present in these materials and therefore, with the use of B3PW91 hybrid functional, band structure and density of states are calculated. When analyzing electron charge density, these materials showed a stronger ionic character. Band structure and density of state analysis confirms the metallic nature of the materials. Using the semi-empirical Boltzmann approach implemented in the BoltzTraP code, the thermoelectric parameters, such as Seebeck coefficient, figure of merit, electrical conductivity per relaxation time, and electronic thermal conductivity per relaxation time as a function of chemical potential, were computed at 500 K temperature gradient. PrIn3 showed highest Seebeck coefficient value, 50.68 μV/K among these compounds. The peak value of electrical conductivity per relaxation time and electronic thermal conductivity per relaxation time among these compounds is calculated for NdIn3 is 2.43 x 1020 1/Ωms and 22.50×1014 W/mKs.

Selective Electron-Phonon Coupling in Dimerized 1T-TaS2 Revealed by Resonance Raman Spectroscopy.

The layered transition-metal dichalcogenide material 1T-TaS2 possesses successive phase transitions upon cooling, resulting in strong electron-electron correlation effects and the formation of charge density waves (CDWs). Recently, a dimerized double-layer stacking configuration was shown to form a Peierls-like instability in the electronic structure. To date, no direct evidence for this double-layer stacking configuration using optical techniques has been reported, in particular through Raman spectroscopy. Here, we employ a multiple excitation and polarized Raman spectroscopy to resolve the behavior of phonons and electron-phonon interactions in the commensurate CDW lattice phase of dimerized 1T-TaS2. We observe a distinct behavior from what is predicted for a single layer and probe a richer number of phonon modes that are compatible with the formation of double-layer units (layer dimerization). The multiple-excitation results show a selective coupling of each Raman-active phonon with specific electronic transitions hidden in the optical spectra of 1T-TaS2, suggesting that selectivity in the electron-phonon coupling must also play a role in the CDW order of 1T-TaS2.

Ground state of superheavy elements with 120≤Z≤170 : Systematic study of the electron-correlation, Breit, and QED effects

For superheavy elements with atomic numbers $120\leq Z \leq 170$, the concept of the ground-state configuration is being reexamined. To this end, relativistic calculations of the electronic structure of the low-lying levels are carried out by means of the Dirac-Fock and configuration-interaction methods.The magnetic and retardation parts of the Breit interaction as well as the QED effects are taken into account. The influence of the relativistic, QED, and electron-electron correlation effects on the determination of the ground-state is analyzed.

Lattice effects on the physical properties of half-doped perovskite ruthenates

We investigate the unusual phase transitions in SrRuO3 and Sr0.5Ca0.5RuCr x O3 (x = 0, 0.05 and 0.1) employing x-ray diffraction, resistivity, magnetic studies and x-ray photoemission spectroscopy. Our results show the compounds undergo a crossover from itinerant ferromagnetism to localized ferromagnetism. The combined studies suggest Ru and Cr be in the 4+ valence state. A Griffith phase and an enhancement in Curie temperature (T c ) from 38 K to 107 K are observed with Cr doping. A shift in the chemical potential towards the valence band is observed with Cr doping. In the metallic samples, interestingly, a direct link between the resistivity and orthorhombic strain is observed. We also observe a connection between orthorhombic strain and T c in all the samples. Detailed studies in this direction will be helpful to choose suitable substrate materials for thin-film/device fabrication and hence manoeuvre its properties. In the non-metallic samples, the resistivity is mainly governed due to disorder, electron-electron correlation effects and a reduction in the number of electrons at the Fermi level. The value of the resistivity for the 5% Cr doped sample suggests semi-metallic behaviour. Understanding its nature in detail using electron spectroscopic techniques could unravel the possibility of its utility in high-mobility transistors at room temperature and its combined property with ferromagnetism will be helpful in making spintronic devices.

Mottness in two-dimensional van der Waals Nb3X8 monolayers (X=Cl,Br,andI)

We investigate strong electron-electron correlation effects on two-dimensional van der Waals materials ${\mathrm{Nb}}_{3}{X}_{8} (X=\mathrm{Cl},\mathrm{Br},\phantom{\rule{0.28em}{0ex}}\text{and}\phantom{\rule{0.28em}{0ex}}\mathrm{I})$. We find that the monolayers ${\mathrm{Nb}}_{3}{X}_{8}$ are ideal systems close to the strong correlation limit. They can be described by a half-filled single band Hubbard model in which the ratio between the Hubbard, $U$, and the bandwidth, $W, U/W\ensuremath{\approx}5--10$. Both Mott and magnetic transitions of the material are calculated by the slave boson mean-field theory. Doping the Mott state, a ${d}_{{x}^{2}\ensuremath{-}{y}^{2}}+i{d}_{xy}$ superconducting pairing instability is found. We also construct a tunable bilayer Hubbard system for two sliding ${\mathrm{Nb}}_{3}{X}_{8}$ layers. The bilayer system displays a crossover between the band insulator and Mott insulator.

Production of autoionizing states by double-electron capture in intermediate-energy C4+ + He collisions

We have performed a kinematically complete experiment for state-selective double-electron capture occurring in 15-keV/u ${\mathrm{C}}^{4+}$ $+$ He collisions by means of cold-target recoil-ion momentum spectroscopy. It was shown that capture into ground and low excited states of the ${\mathrm{C}}^{2+}$ ions is overwhelmingly dominant. Besides, a small fraction of autoionization decays from doubly excited states of symmetric as well as asymmetric electron configurations following endothermic double-electron capture were clearly observed. Emphasis was given to the population mechanisms of the different electron configurations. Our analysis indicates that electron-electron correlation effects may play a major role in the double-electron capture process. In addition, the large transverse recoil-ion momentum of symmetric configurations as compared to asymmetric configurations for the doubly excited autoionizing states may be attributed to the different number of steps involved in the primary capture process, with the former likely produced by a two-step mechanism and the latter by a one-step mechanism.

Proton-helium collisions at intermediate energies: Singly differential ionization cross sections

We investigate the four-body proton-helium scattering problem using the two-center wave-packet convergent close-coupling approach. The approach uses a correlated two-electron wave function for the helium target. The continuum is discretized using wave-packet pseudostates. Calculations of ionization cross sections differential in the electron emission energy, in the emission angle, as well as in the scattered-projectile angle are performed in the intermediate energy region where coupling between various channels and electron-electron correlation effects are important. The results agree well with experimental data, where available. Moreover, our calculations reveal an interesting interplay between direct ionization and electron capture into the continuum. In particular, we demonstrate that the ionization cross section differential in the angle of the ejected electron is dominated by electron capture into the continuum for ejection into small angles, while ejection into large angles is purely due to direct ionization. It is concluded that the two-center wave-packet convergent close-coupling approach can provide accurate singly differential cross sections for ionization in proton-helium collisions. For comparison, a recently developed method that reduces the target to an effective single-electron system is also used. Somewhat unexpectedly, the results of the effective one-electron method exhibit a very good level of agreement with the full two-electron ones for all three singly differential cross sections. Therefore, we also conclude that, at least for the purpose of calculating the singly differential cross sections for single ionization of helium, an effective one-electron treatment of the target suffices.

Attosecond intra-valence band dynamics and resonant-photoemission delays in W(110)

Time-resolved photoelectron spectroscopy with attosecond precision provides new insights into the photoelectric effect and gives information about the timing of photoemission from different electronic states within the electronic band structure of solids. Electron transport, scattering phenomena and electron-electron correlation effects can be observed on attosecond time scales by timing photoemission from valence band states against that from core states. However, accessing intraband effects was so far particularly challenging due to the simultaneous requirements on energy, momentum and time resolution. Here we report on an experiment utilizing intracavity generated attosecond pulse trains to meet these demands at high flux and high photon energies to measure intraband delays between sp- and d-band states in the valence band photoemission from tungsten and investigate final-state effects in resonant photoemission.

Heisenberg and anisotropic exchange interactions in magnetic materials with correlated electronic structure and significant spin-orbit coupling

The Dzyaloshinskii-Moriya (DM) interaction, as well as symmetric anisotropic exchange, are important ingredients for stabilizing topologically non-trivial magnetic textures, such as, e.g., skyrmions, merons and hopfions. These types of textures are currently in focus from a fundamental science perspective and they are also discussed in the context of future spintronics information technology. While the theoretical understanding of the Heisenberg exchange interactions is well developed, it is still a challenge to access, from first principles theory, the DM interaction as well as the symmetric anisotropic exchange, which both require a fully-relativistic treatment of the electronic structure, in magnetic systems where substantial electron-electron correlations are present. Here, we present results of a theoretical framework which allows to compute these interactions in any given system and demonstrate its performance for several selected cases, for both bulk and low-dimensional systems. We address several representative cases, including the bulk systems CoPt and FePt, the B20 compounds MnSi and FeGe as well as the low-dimensional transition metal bilayers Co/Pt(111) and Mn/W(001). The effect of electron-electron correlations is analyzed using dynamical mean-field theory on the level of the spin-polarized $T$-matrix + fluctuating exchange (SPTF) approximation, as regards the strength and character of the isotropic (Heisenberg) and anisotropic (DM) interactions in relation to the underlying electronic structure. Our method can be combined with more advanced techniques for treating correlations, e.g., quantum Monte Carlo and exact diagonalization methods for the impurity solver of dynamical mean-field theory. We find that correlation-induced changes of the DM interaction can be rather significant, with up to five-fold modifications in the most distinctive case.

Abinitio Calculations of Energy Levels in Be-Like Xenon: Strong Interference between Electron-Correlation and QED Effects.

The strong mixing of close levels with two valence electrons in Be-like xenon greatly complicates abinitio QED calculations beyond the first-order approximation. Because of a strong interplay between the electron-electron correlation and QED effects, the standard single-level perturbative QED approach may fail, even if it takes into account the second-order screened QED diagrams. In the present Letter, the corresponding obstacles are overcome by working out the QED perturbation theory for quasidegenerate states. The contributions of all the Feynman diagrams up to the second order are taken into account. The many-electron QED effects are rigorously evaluated in the framework of the extended Furry picture to all orders in the nuclear-strength parameter αZ. The higher-order electron-correlation effects are considered within the Breit approximation. The nuclear recoil effect is accounted for as well. The developed approach is applied to high-precision QED calculations of the ground and singly excited energy levels in Be-like xenon. The most accurate theoretical predictions for the binding and excitation energies are obtained. These results deviate from the most precise experimental value by 3σ but perfectly agree with a more recent measurement.

Wave functions, electronic localization, and bonding properties for correlated materials beyond the Kohn-Sham formalism

Many-body theories such as dynamical mean field theory (DMFT) have enabled the description of the electron-electron correlation effects that are missing in current density functional theory (DFT) calculations. However, there has been relatively little focus on the wave functions from these theories. We present the methodology of the newly developed elk-triqs interface and how to calculate the DFT with DMFT ($\mathrm{DFT}+\mathrm{DMFT}$) wave functions, which can be used to calculate $\mathrm{DFT}+\mathrm{DMFT}$ wave-function-dependent quantities. We illustrate this by calculating the electron localization function (ELF) in monolayer ${\mathrm{SrVO}}_{3}$ and ${\mathrm{CaFe}}_{2}{\mathrm{As}}_{2}$, which provides a means of visualizing their chemical bonds. Monolayer ${\mathrm{SrVO}}_{3}$ ELFs are sensitive to the charge redistribution between the DFT, one-shot $\mathrm{DFT}+\mathrm{DMFT}$, and fully charge self-consistent $\mathrm{DFT}+\mathrm{DMFT}$ calculations. In both tetragonal and collapsed tetragonal ${\mathrm{CaFe}}_{2}{\mathrm{As}}_{2}$ phases, the ELF changes weakly with correlation-induced charge redistribution of the hybridized As $p$ and Fe $d$ states. Nonetheless, the interlayer As-As bond in the collapsed tetragonal structure is robust to the changes at and around the Fermi level.

Photoionization cross section calculations of Ne-like Mo XXXIII

Within the framework of Breit Pauli R-matrix approach, a close-coupling calculation has been carried out for the process of photoionization of ground and excited states of Ne-like Mo XXXIII ion. The calculation includes 60 fine-structure levels and 15 parities for the target states. Level specific photoionization cross sections are computed for all levels at a fine energy mesh of 10−5 scaled Ryd, with 19500 energies for each Jπ = 0± - 6± symmetry, up to 2s22p43s (2S1/2) threshold at 212.33 Ryd above the first ionization threshold, 1s22s22p5 2Po3/2. In this article are presented cross sections for the photoionization of ground 1s22s22p6 1S0 and 1s22s22p5(2Po)3p 3P0, 1s22s22p5(2Po)3p 1S0, 1s22s2p63s 1S0, 1s22s22p53s(3Po2,1,0), 1s22s22p53s (1Po1) excited states. To explore the role of particle-hole, channels coupling and electron-electron correlation effects on the photoionization cross sections we have compared two calculation models, namely 8-target basic configurations and 5-target basic configurations, with and without 2s2p53l target states included into the model. Effects are highlighted in the photoionization cross section behavior of the excited of 2s2p63s of Mo XXXIII.We believe that this is the first such calculation for this ion to obtain the photoionization cross section and results are important for the modeling and diagnostics of laboratory and astrophysical plasmas.

Understanding Disorder in 2D Materials: The Case of Carbon Doping of Silicene.

We investigate the effect of lattice disorder and local correlation effects in finite and periodic silicene structures caused by carbon doping using first-principles calculations. For both finite and periodic silicene structures, the electronic properties of carbon-doped monolayers are dramatically changed by controlling the doping sites in the structures, which is related to the amount of disorder introduced in the lattice and electron-electron correlation effects. By changing the position of the carbon dopants, we found that a Mott-Anderson transition is achieved. Moreover, the band gap is determined by the level of lattice disorder and electronic correlation effects. Finally, these structures are ferromagnetic even under disorder which has potential applications in Si-based nanoelectronics, such as field-effect transistors (FETs).

Low-Energy Electron Elastic Total Cross Sections for Ho, Er, Tm, Yb, Lu, and Hf Atoms

The robust Regge-pole methodology wherein is fully embedded the essential electron-electron correlation effects and the vital core polarization interaction has been used to explore negative ion formation in the large lanthanide Ho, Er, Tm, Yb, Lu, and Hf atoms through the electron elastic total cross sections (TCSs) calculations. These TCSs are characterized generally by dramatically sharp resonances manifesting ground, metastable, and excited negative ion formation during the collisions, Ramsauer-Townsend minima, and shape resonances. The novelty and generality of the Regge-pole approach is in the extraction of the negative ion binding energies (BEs) of complex heavy systems from the calculated electron TCSs. The extracted anionic BEs from the ground state TCSs for Ho, Er, Tm, Yb, Lu, and Hf atoms are 3.51 eV, 3.53 eV, 3.36 eV, 3.49 eV, 4.09 eV and 1.68 eV, respectively. The TCSs are presented and the extracted from the ground; metastable and excited anionic states BEs are compared with the available measured and/or calculated electron affinities. We conclude with a remark on the existing inconsistencies in the meaning of the electron affinity among the various measurements and/or calculations in the investigated atoms and make a recommendation to resolve the ambiguity.

Simulation of nonlinear Compton scattering from bound electrons

Recent investigations by Fuchs et al. [Nat. Phys. 11, 964 (2015)] revealed an anomalous frequency shift in non-linear Compton scattering of high-intensity X-rays by electrons in solid beryllium. This frequency shift was at least 800 eV to the red of the values predicted by analytical free-electron models for the same process. In this paper, we describe a method for simulating non-linear Compton scattering. The method is applied to the case of bound electrons in a local, spherical potential to explore the role of binding energy in the frequency shift of scattered X-rays for different scattered angles. The results of the calculation do not exhibit an additional redshift for the scattered X-rays beyond the non-linear Compton shift predicted by the free-electron model. However, it does reveal a small blue-shift relative to the free electron prediction for non-linear Compton scattering. The effect of electron-electron correlation effects is calculated and determined to be unlikely to be the source of the redshift. The case of linear Compton scattering from a photoionized electron followed by electron recapture is examined as a possible source of the redshift and ruled out.

Topological superconductivity in Ni-based transition metal trichalcogenides

Based on a two-orbital honeycomb lattice model and random phase approximation, we investigate the pairing symmetry of the Ni-based transition-metal trichalcogenide. We find that an I-wave (A2g) state and a chiral d-wave state are dominant and nearly degenerate for typical electron and hole dopings. These two states carry nontrivial topological properties, which are manifested by the presence of chiral edge states in the d+id-wave state and dispersionless Andreev bound state at zero energy in the I-wave state. Ni-based transition-metal trichalcogenides provide us a new platform to study the exotic phenomena emerged from electron-electron correlation effects.

QED calculation of electron-electron correlation effects in heliumlike ions

Fully relativistic approach to evaluate the correlation effects in highly charged ions is presented. The interelectronic-interaction contributions of first and second orders in $1/Z$ are treated rigorously within the framework of bound-state quantum electrodynamics, whereas the calculations of the third- and higher-order contributions are based on the Dirac-Coulomb-Breit Hamiltonian. The developed approach allows one to deal with single as well as degenerate or quasi-degenerate states. We apply this approach to the calculations of the correlation contributions to the $n=1$ and $n=2$ energy levels in heliumlike ions. The obtained contributions are combined with the one-electron and screened QED corrections, nuclear recoil and nuclear polarization corrections to get the total theoretical predictions for the ionization and transition energies in high-$Z$ heliumlike ions.

Revisiting the Fe xvii Line Emission Problem: Laboratory Measurements of the 3s–2p and 3d–2p Line-formation Channels

Abstract We determined relative X-ray photon emission cross sections in Fe xvii ions that were mono-energetically excited in an electron beam ion trap. Line formation for the 3s (3s−2p) and 3d (3d−2p) transitions of interest proceeds through dielectronic recombination (DR), direct electron-impact excitation (DE), resonant excitation (RE), and radiative cascades. By reducing the electron-energy spread to a sixth of that of previous works and increasing counting statistics by three orders of magnitude, we account for hitherto unresolved contributions from DR and the little-studied RE process to the 3d transitions, and also for cascade population of the 3s line manifold through forbidden states. We found good agreement with state-of-the-art many-body perturbation theory (MBPT) and the distorted-wave (DW) method for the 3s transition, while in the 3d transitions known discrepancies were confirmed. Our results show that DW calculations overestimate the 3d line emission due to DE by ∼20%. Inclusion of electron-electron correlation effects through the MBPT method in the DE cross-section calculations reduces this disagreement by ∼11%. The remaining ∼9% in 3d and ∼11% in 3s/3d discrepancies are consistent with those found in previous laboratory measurements, solar, and astrophysical observations. Meanwhile, spectral models of opacity, temperature, and turbulence velocity should be adjusted to these experimental cross sections to optimize the accuracy of plasma diagnostics based on these bright soft X-ray lines of Fe xvii.

Resonance strengths for KLL dielectronic recombination of highly charged mercury ions and improved empirical Z -scaling law

Theoretical and experimental resonance strengths for KLL dielectronic recombination (DR) into He-, Li-, Be-, and B-like mercury ions are presented, based on state-resolved DR x-ray spectra recorded at the Heidelberg electron beam ion trap. The DR resonance strengths were experimentally extracted by normalizing them to simultaneously recorded radiative recombination signals. The results are compared to state-of-the-art atomic calculations that include relativistic electron-electron correlation and configuration mixing effects. Combining the present data with other existing ones, we derive an improved semi-empirical $Z$-scaling law for DR resonance strength as a function of the atomic number, taking into account higher-order relativistic corrections, which are especially relevant for heavy highly charged ions.