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Results for “electron correlation calculations for atoms and ions”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Nuclear charge radii of Na isotopes: Interplay of atomic and nuclear theory

The accuracy of atomic theory calculations limits the extraction of nuclear charge radii from isotope shift measurements of odd-proton nuclei. For Na isotopes, though precise spectroscopic measurements have existed for more than half a century, calculations by different methods offer a wide range of values. Here, we present accurate atomic calculations to reliably extract the Na charge radii. By combining experimental matter radii with nuclear coupled-cluster calculations based on nucleon-nucleon and three-nucleon forces, we constrain the parameters obtained from the atomic calculations. Furthermore, this study guides atomic theory and highlights the importance of using accurate atomic and nuclear computations in our understanding of the size of light nuclei.

20 ≤ A ≤ 38↗
DOE OSTI2023

Pump and ionizing-probe dynamics in a simultaneous treatment of electronic and nuclear motion in LiH

The dissociative single ionization of the LiH molecule using a two-color UV-UV pump-probe scheme is simulated in ab initio calculations demonstrating how the dynamics initiated on intermediate Rydberg states of diatomic molecules can be imaged by such experiments. The theoretical treatment combines nuclear motion with highly correlated descriptions of electronic continua and bound electronic states. Nuclear dynamics on Rydberg states are only weakly reflected by changes in photoelectron energies ejected by time-delayed ionizing pulses if the Rydberg potential curves parallel those of the ion states being produced. However, coincidence measurements guided by knowledge of the photoionization amplitudes as a function of internuclear distance can still reveal intermediate-state dynamics in pump-probe experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Evidence of Two-Source King Plot Nonlinearity in Spectroscopic Search for New Boson

Optical precision spectroscopy of isotope shifts can be used to test for new forces beyond the standard model, and to determine basic properties of atomic nuclei. We measure isotope shifts on the highly forbidden 2 S 1/2 → 2 F 7/2 octupole transition of trapped 168,170, 172, 174, 176 Yb ions. When combined with previous measurements in Yb + and very recent measurements in Yb, the data reveal a King plot nonlinearity of up to 240σ. Furthermore, the trends exhibited by experimental data are explained by nuclear density functional theory calculations with the Fayans functional. We also find, with 4.3σ confidence, that there is a second distinct source of nonlinearity, and discuss its possible origin.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Relativistic and correlation effects in the photoionization dynamics of oganesson ( Z = 118): Spin-orbit-interaction-activated interchannel coupling effects

High-Z atoms are excellent laboratories to study the combination of relativistic and many-electron correlation effects in electronic structure and dynamics. In the present work, the relativistic-random-phase approximation at different levels of truncation is employed to explore the final-state correlation effects in the photoelectron dynamics of the heaviest known element in the Periodic Table: oganesson (Og) with Z = 118. Here, the focus of this work is to illustrate the relativistic effects resulting from coupling different photoionization channels arising from spin-orbit split subshells, termed the spin-orbit-interaction-activated interchannel coupling effect. Comparison with the photoelectron dynamics of Rn on a qualitative level is also carried out, since Og is a homologue of Rn. The photoelectron dynamics of 7p, 7s, and 6d subshells are investigated and differences between Og and Rn, due to enhanced relativistic effects, are investigated.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Optical telecommunications-band clock based on neutral titanium atoms

Here, we propose an optical clock based on ultranarrow transitions in neutral titanium, which exhibit small blackbody radiation and quadratic Zeeman shifts and have wavelengths in the S-, C-, and L-telecommunications fiber bands, allowing for integration with robust laser technology. We calculate relevant properties using a high-precision relativistic hybrid method that combines configuration interaction and coupled-cluster approaches. To identify magic wavelengths, we have completed the largest-to-date direct dynamical polarizability calculations. Finally, we identify challenges that arise from magnetic dipole-dipole interactions and describe an approach to overcome them. A telecommunications-band atomic frequency standard will aid the deployment of optical clock networks and clock comparisons over long distances.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Using isotope shift for testing nuclear theory: The case of nobelium isotopes

We calculate field isotope shifts for nobelium atoms using nuclear charge distributions which come from different nuclear models.We demonstrate that comparing calculated isotope shifts with experiment can serve as a testing ground for nuclear theories. It also provides a way of extracting parameters of nuclear charge distribution beyond nuclear root mean square (rms) radius, e.g., parameter of quadrupole deformation β. The measurements of at least two atomic transitions is needed to disentangle the contributions of the changes in deformation and nuclear rms radius into field isotopic shift. We argue that a previous interpretation of the isotope measurements in terms of δ < r 2 > between 252,254 No isotopes should be amended when nuclear deformation is taken into account. As a result, we calculate isotope shifts for other known isotopes and for hypothetically metastable isotope 286 No for which the predictions of nuclear models differ substantially.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Stochastic and mixed density functional theory within the projector augmented wave formalism for simulation of warm dense matter

Stochastic density functional theory (DFT) and mixed stochastic-deterministic DFT are burgeoning approaches for the calculation of the equation of state and transport properties in materials under extreme conditions. In the intermediate warm dense matter regime, a state between correlated condensed matter and kinetic plasma, electrons can range from being highly localized around nuclei to delocalized over the whole simulation cell. The plane-wave basis pseudopotential approach is thus the typical tool of choice for modeling such systems at the DFT level. Unfortunately, stochastic DFT methods scale as the square of the maximum plane-wave energy in this basis. To reduce the effect of this scaling and improve the overall description of the electrons within the pseudopotential approximation, we present stochastic and mixed DFT approaches developed and implemented within the projector augmented wave formalism. In conclusion, we compare results between the different DFT approaches for both single-point and molecular dynamics trajectories and present calculations of self-diffusion coefficients of solid density carbon from 1 to 50 eV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Oscillate and renormalize: Fast phonons reshape the Kondo effect in flat-band systems

Here, we examine the interplay between electron correlations and phonons in an Anderson-Holstein impurity model with an Einstein phonon. When the phonons are slow compared to charge fluctuations (frequency 𝜔 0 ≪ 𝑈/2, the onsite Coulomb scale 𝑈/2), we demonstrate analytically that the expected phonon-mediated reduction of interactions is completely suppressed, even in the strong-coupling regime. This suppression arises from the oscillator's inability to respond to rapid charge fluctuations, manifested as a compensation effect between the polaronic cloud and the excited-state phonons associated with valence fluctuations. We identify a frozen mixed valence phase, above a threshold dimensionless electron-phonon coupling 𝛼* when the phonons are slow, where the static phonon cloud locks the impurity into specific valence configurations, potentially explaining the puzzling coexistence of mixed valence behavior and insulating properties in materials like rust. Conversely, when the phonon is fast (𝜔 0 ≳ 𝑈/2), the system exhibits conventional polaronic behavior with renormalized onsite interactions effectively 𝑈 eff due to phonon-mediated attraction, with additional satellite features in the local spectral function due to phonon excitations. Using numerical renormalization group calculations, a fully dynamic renormalization technique, we confirm these behaviors in both regimes. These findings have important implications for strongly correlated systems where phonon energy scales may be comparable to the Coulomb scale, such as in twisted bilayer graphene, necessitating careful consideration of interaction renormalizations in theoretical models.

Anderson impurity model↗
DOE OSTI2020

Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation

Here we present an experimental study on the photoionization dynamics of nonresonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3-eV photons produced via high harmonic generation and a three-dimensional momentum imaging spectrometer, we detect the photoelectrons and ions produced from nonresonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$- and $f$-partial-wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the vacuum ultraviolet polarization. The comparison between the present results and the two previous sets of theoretical calculations [Phys. Rev. A 44, 324 (1991), and J. Phys. B: At. Mol. Phys. 16, 2737 (1983)] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Temporal coherent control of resonant two-photon double ionization of the hydrogen molecule via doubly excited states

Here, we use time-delayed, counter-rotating, circularly polarized few-cycle attosecond nonoverlapping pulses to study the temporal coherent control of the resonant process of two-photon double ionization (TPDI) of hydrogen molecule via doubly excited states for pulse propagation direction along $\hat k$ either parallel or perpendicular to the molecular axis $\hat R$. For $\hat k$∥ $\hat R$ and a pulse carrier frequency of 36 eV resonantly populating the Q 2 1 Π$^+_u$ (1) doubly excited state as well as other 1 Π$^+_u$ doubly excited states, we find that the indirect ionization pathway through these doubly excited states changes the character of the kinematical vortex-shaped momentum distribution produced by the two direct ionization pathways from fourfold to twofold rotational symmetry. This result is similar to what found in TPDI of the He atom involving 1 P$^ o_ {±1}$ doubly excited states; however, angular distributions exhibiting a quantum beat effect between the ground state and a doubly excited state seen for the He atom are observed here for its molecular counterpart with an anomaly in shape and magnitude, not in frequency. The sixfold differential probability integrated over the azimuthal angle of the photoelectron pair shows that this anomaly is due to autoionization decays and quantum beats between doubly excited states. For $\hat k$⟂$\hat R$ and a broadband pulse carrier frequency of 30 eV populating the Q 1 1 Π$^+_u$(1), Q 1 1 Σ$^+_u$(1), Q 2 1 Π$^+_u$(1) , and Q 1 1 Σ$^+_u$ (2) doubly excited states, the momentum distribution is shown to exhibit dynamical electron vortices with four spiral arms, which originates from the interplay between the 1 Δ$^+_ g$ , 1 Π$^+_ g$, and 1 Σ$^+_ g$ dynamical ionization amplitudes. Our treatment within either the adiabatic-nuclei approximation or fixed-nuclei approximation shows that the latter provides a very good account for this correlated process.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Simple hydrogenic estimates for the exchange and correlation energies of atoms and atomic ions, with implications for density functional theory

Exact density functionals for the exchange and correlation energies are approximated in practical calculations for the ground-state electronic structure of a many-electron system. An important exact constraint for the construction of approximations is to recover the correct non-relativistic large-Z expansions for the corresponding energies of neutral atoms with atomic number Z and electron number N = Z, which are correct to leading order (–0.221 Z 5/3 and –0.021 Z ln Z respectively) even in the lowest-rung or local density approximation. We find that hydrogenic densities lead to E x (N,Z) ≈ –0.354 N 2/3 Z (as known before only for Z >> N >> 1) and E c ≈ –0.02 N ln N . These asymptotic estimates are most correct for atomic ions with large N and Z >> N, but we find that they are qualitatively and semi- quantitatively correct even for small N and for N ≈ Z. The large-N asymptotic behavior of the energy is pre-figured in small-N atoms and atomic ions, supporting the argument that widely-predictive approximate density functionals should be designed to recover the correct asymptotics. Here, it is shown that the exact Kohn-Sham correlation energy, when calculated from the pure ground-state wavefunction, should have no contribution proportional to Z in the Z → ∞ limit for any fixed N.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Recent advancements in atomic many-body methods for high-precision studies of isotope shifts

The development of atomic many-body methods, capable of incorporating electron correlation effects accurately, is required for isotope shift (IS) studies. In combination with precise measurements, such calculations help to extract nuclear charge radii differences, and to probe for signatures of physics beyond the Standard Model of particle physics. Here, we review here a few recently-developed methods in the relativistic many-body perturbation theory (RMBPT) and relativistic coupled-cluster (RCC) theory frameworks for calculations of IS factors in the highly charged ions (HCIs), and neutral or singly-charged ions, respectively. The results are presented for a wide range of atomic systems in order to demonstrate the interplay between quantum electrodynamics (QED) and electron correlation effects. In view of this, we start our discussions with the RMBPT calculations for a few HCIs by rigorously treating QED effects; then we outline methods to calculate IS factors in the one-valence atomic systems using two formulations of the RCC approach. Then we present calculations for two valence atomic systems, by employing the Fock-space RCC methods. For completeness, we briefly discuss theoretical input required for the upcoming experiments, their possibilities to probe nuclear properties and implications to fundamental physics studies.

QED effects↗
DOE OSTI2025

Photoelectron–residual-ion interaction in angle-resolved streaked shake-up ionization of helium

Streaked photoelectron emission spectra access the correlated dynamics of photoelectrons and residual target electrons with attosecond temporal resolution. Here, we calculated ab initio single-ionization spectra for photoemission from helium atoms by colinearly polarized ultrashort XUV and assisting few-femtosecond IR pulses. Distinguishing direct and shake-up ionization resulting in ground-state and excited (𝑛 = 2, 3) He + residual ions, respectively, we examined the effects of the correlated photoemission dynamics on the photoelectron phase accumulation as a function of the observable photoelectron detection direction and kinetic energy and XUV–IR pulse delay. We tracked the dynamical evolution of the residual ion in relative streaked photo- emission delays and found dominant contributions for shake-up emission from the residual-ion–photoelectron interaction. These are in very good and fair agreement, respectively, for 𝑛 = 2 and 𝑛 = 3 shake-up photoemission along the pulse-polarization directions, with previous experimental and theoretical investigations [Ossiander et al ., Nat. Phys. 13, 280 (2017)] and reveal a strong photoemission-direction dependence for shake-up ionization due to the coupling between the photoelectron and evolving residual-ion charge distribution in the IR-laser field.

Stark effect↗
DOE OSTI2021

Theoretical level energies, radiative lifetimes and transitions in W IX

The atomic states of the W IX (W{sup 8+}) tungsten ion lying below the W{sup 9+} ionisation threshold have been studied theoretically, employing the multiconfiguration Dirac–Hartree–Fock method with configuration interaction. The level electronic structures and their energies are presented. The electric dipole (E1), magnetic dipole (M1), electric quadrupole (E2), and magnetic quadrupole (M2) radiative transitions have been computed in order to calculate the radiative lifetimes of given states. Transition wavelengths, energies, and decay rates are also presented for selected high-intensity E1 transitions. The configuration interaction method was applied to estimate electron correlation effects. The aim of the present research was to fill a lack of atomic data for low-charged tungsten ions, which may be useful in low-temperature plasma diagnostics and may form the base for collisional–radiative modelling of spectra for low-charged tungsten ions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Negative Ion Formation in Complex Heavy Systems

The project’s primary objective is to gain a fundamental theoretical understanding of the near-threshold electron attachment mechanism in low energy electron elastic scattering from complex heavy systems through the calculation of integral and differential cross sections and extract reliable electron affinities (EAs). The complex angular momentum (CAM), also known as Regge-pole methodology wherein is fully embedded the crucial electron-electron correlations and the core polarization interaction, is used for the investigations. Regge trajectories allow us to probe electron attachment at the fundamental level near threshold, thereby uncovering new manifestations, including the mechanism of nanocatalysis, and determine reliable EAs. Low-energy electron elastic scattering total cross sections (TCSs) for the lanthanide and actinide atoms and the fullerene molecules are calculated. From the TCSs ground, metastable and excited states anionic binding energies (BEs) are extracted and compared with the available measured and/or calculated EAs. Significantly, our calculated ground state anionic BEs correspond to the theoretically challenging to calculate EAs and they are used to assess the reliability of existing EAs. Doubly charged negative ions of atoms and molecules are proposed as novel tunable catalysts and demonstrated in the oxidation of water into peroxide. Negatively charged fullerene molecules are used to catalyze water oxidation to peroxide and water synthesis from H 2 and O 2 as well. Violation of time-reversal and particle-hole symmetries in strongly correlated Fermi systems are reviewed with the collaboration involving the International Laboratory of Fermi Condensation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

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.

Felfli, Zineb↗