High-precision calculations of the energy levels of the superheavy elements E119 and E120+ are presented. Dominating correlation corrections beyond relativistic Hartree-Fock are included to all orders in the Coulomb interaction using the Feynman diagram technique and the correlation potential method. The Breit interaction and quantum electrodynamics radiative corrections are considered. Also, the volume isotope shift is determined. A similar treatment for Cs, Fr, Ba+ and Ra+ is used to gauge the accuracy of the calculations and to refine the ab initio results.
Theoretical study of electron structure of superheavy elements with an open $6d$-shell, Sg, Bh, Hs and Mt
我们用最近发展起来的有效的组态相互作用方法对超重元素Seaborgium（Sg，$Z=106$），Bohrium（Bh，$Z=107$），Hesium（Hs，$Z=108$）和Meitnerium（Mt，$Z=109$）的光谱进行了{\em ab initio}计算.计算了它们的能级、电离势、同位素位移和电偶极跃迁振幅。与较轻的类似物的比较揭示了超重元素中强相对论效应引起的显着差异。非常大的自旋-轨道相互作用区分了包含具有确定的总电子角动量$j$的轨道的子壳层。此效应取代了Hund规则对较轻元素的支持。
Optical spectroscopy constitutes the historical path to accumulate basic knowledge on the atom and its structure. Former work based on fluorescence and resonance ionization spectroscopy enabled identifying optical spectral lines up to element 102, nobelium. The new challenges faced in this research field are the refractory nature of the heavier elements and the decreasing production yields. A new concept of ion-mobility-assisted laser spectroscopy is proposed to overcome the sensitivity limits of atomic structure investigations persisting in the region of the superheavy elements. The concept o…
We employ a fully relativistic coupled-cluster theory to calculate the ground-state electric dipole polarizability and electron correlation energy of superheavy elements Cn, Nh$^+$ and Og. To assess the trend of electron correlation as function of $Z$, we also calculate the correlation energies for three lighter homologs--Zn, Cd and Hg; Ga$^+$, In$^+$ and Tl$^+$; Kr, Xe and Rn--for each superheavy elements. The relativistic effects and quantum electrodynamical corrections are included using the Dirac-Coulomb-Breit Hamiltonian with the corrections from the Uehling potential and the self-energy.…
Electronic structure calculation for superheavy elements Livermorium (Lv, Z=116) and Tennessine (Ts, Z=117) and their lighter analogs Te, I, Po, and At
The successive ionization potentials (IPs) and electron affinities (EAs) for superheavy elements with $111 \leq Z \leq 114$, namely, Rg, Cn, Nh, and Fl are reexamined using the relativistic Fock-space coupled-cluster method with nonperturbative single (S), double (D), and triple (T) cluster amplitudes (FS-CCSDT). For the most of considered quantities, the triple-amplitude contributions turn out to be important. The Breit and frequency-dependent Breit corrections are evaluated by means of the configuration-interaction method. The quantum-electrodynamics corrections to the IPs and EAs are taken …
We review the progress in atomic structure theory with a focus on superheavy elements and the aim to predict their ground state configuration and element's placement in the periodic table. To understand the electronic structure and correlations in the regime of large atomic numbers, it is important to correctly solve the Dirac equation in strong Coulomb fields, and also to take into account quantum electrodynamic effects. We specifically focus on the fundamental difficulties encountered when dealing with the many-particle Dirac equation. We further discuss the possibility for future many-elect…
The model-QED-operator approach [Phys. Rev. A 88, 012513 (2013)] to calculations of the radiative corrections to binding and transition energies in atomic systems is extended to the range of nuclear charges $110 \leqslant Z \leqslant 170$. The self-energy part of the model operator is represented by a nonlocal potential based on diagonal and off-diagonal matrix elements of the ab initio self-energy operator with the Dirac-Coulomb wave functions. The vacuum-polarization part consists of the Uehling contribution which is readily computed for an arbitrary nuclear-charge distribution and the Wichm…
Relativistic calculations of the electronic structure of the superheavy element of the eighth period $-$ eka-francium ($Z=119$) and its homologues, which form the group of alkali metals, are performed in the framework of the configuration-interaction method and many-body perturbation theory using the basis of the Dirac-Fock-Sturm orbitals (DFS). The obtained values of the ionization potentials, electron affinities, and root-mean-square radii are compared with the corresponding values calculated within the non-relativistic approximation. A comparison with the available experimental data and the…
Relativistic effective atomic configurations of superheavy elements Cn, Nh and Fl and their lighter homologues (Hg, Tl and Pb) in their simple compounds with fluorine and oxygen are determined using the analysis of local properties of molecular Kohn-Sham density matrices in the vicinity of heavy nuclei. The difference in populations of atomic spinors with the same orbital angular momentum and different total angular momenta is demonstrated to be essential for understanding the peculiarities of chemical bonding in superheavy element compounds. The results are fully compatible with those obtaine…
A new iterative version of population projection analysis is formulated and applied to determine relativistic effective atomic configurations of superheavy elements Cn and Fl and their lighter homologues (Hg and Pb) in the molecules of their fluorides and oxides. The dependence of the computed populations on the initial reference atomic spinors is completely avoided. The difference in population of atomic spinors with the same orbital angular momentum and different total angular momenta is demonstrated to be essential for understanding the peculiarities of chemical bonding in superheavy elemen…
