Relativistic atomic structure calculations in support of spectroscopy

Abstract

Theory can provide important support at all the stages of spectroscopic experiments, from planning the measurements to the interpretation of the results. Such support is particularly valuable for the challenging experiments on heavy, unstable, and superheavy elements and for precision measurements aimed at testing the Standard Model of particle physics. To be reliable and useful in experimental context, theoretical predictions should be based on high-accuracy calculations. For heavy elements, such calculations must treat both relativistic effects and electron correlation on the highest possible level. Relativistic coupled cluster is considered one of the most powerful methods for accurate calculations on heavy many-electron atoms and molecules. This approach is highly accurate and versatile and can be used to obtain energies and a variety of atomic and molecular properties. Furthermore, its robust and transparent formulation allows for systematic improvement of the accuracy of the calculated results and for assigning uncertainties on theoretical values. The Fock-space coupled cluster (FSCC) variant of this method is particularly useful in the context of spectroscopic measurements as it provides access to atomic spectra and properties of the excited states. In this review, we present in detail the relativistic coupled cluster approach and its FSCC variant. We provide a description of the computational procedure used for accurate calculations and for assigning uncertainties. Outstanding recent examples of application to atomic properties, focusing on the experimental context are presented. Finally, we provide a brief discussion of the perspectives for future developments and applications of the CC approach.

References in corpus (110)

• Search for New Physics with Atoms and Molecules
• Varying constants, Gravitation and Cosmology
• Single-Ion Atomic Clock with $3\times 10^{-18}$ Systematic Uncertainty
• The origin of the matter-antimatter asymmetry
• Frequency ratio of two optical clock transitions in ${}^{171}$Yb${}^{+}$ and constraints on the time-variation of fundamental constants
• Reduced Limit on the Permanent Electric Dipole Moment of ${}^{199}$Hg
• The DIRAC code for relativistic molecular calculations
• A new bound on the electron's electric dipole moment
• Highly charged ions: optical clocks and applications in fundamental physics
• Two-time Green function method in quantum electrodynamics of high-Z few-electron atoms
• Nuclear Equation of State from ground and collective excited state properties of nuclei
• BAGEL: Brilliantly Advanced General Electronic-structure Library
• The radiative potential method for calculations of QED radiative corrections to energy levels and electromagnetic amplitudes in many-electron atoms
• Lasercooled RaF as a promising candidate to measure molecular parity violation
• Model operator approach to the Lamb shift calculations in relativistic many-electron atoms
• Revisiting parity non-conservation in cesium
• Enhanced laboratory sensitivity to variation of the fine-structure constant using highly-charged ions
• Frequency ratio of the ${}^{229\mathrm{m}}$Th nuclear isomeric transition and the ${}^{87}$Sr atomic clock
• Basis set convergence of post-CCSD contributions to molecular atomization energies
• Development of a configuration-interaction + all-order method for atomic calculations
• Laser Spectroscopy for the Study of Exotic Nuclei
• Laser spectroscopic characterization of the nuclear clock isomer ${}^{229m}$Th
• Charge radii of exotic potassium isotopes challenge nuclear theory and the magic character of $N=32$
• Spectroscopy of short-lived radioactive molecules: A sensitive laboratory for new physics
• An Optical Atomic Clock Based on a Highly Charged Ion
• Highly-charged ions for atomic clocks, quantum information, and search for $\alpha$-variation
• E1 amplitudes, lifetimes, and polarizabilities of the low-lying levels of atomic ytterbium
• A proton density bubble in the doubly magic ${}^{34}$Si nucleus
• QED tests with highly-charged ions
• Electron and Nucleon Localization Functions of Oganesson: Approaching the Thomas-Fermi Limit
• QED and relativistic corrections in superheavy elements
• Equation-of-Motion Coupled-Cluster Theory based on the 4-component Dirac-Coulomb(-Gaunt) Hamiltonian. Energies for single electron detachment, attachment and electronically excited states
• Theoretical study of ThO for the electron electric dipole moment search
• The electron affinity of astatine
• Theoretical study of thorium monoxide for the electron electric dipole moment search, II: Electronic properties of $H^3{\Delta }_1$ in ThO
• High accuracy theoretical investigations of CaF, SrF, and BaF and implications for laser-cooling
• Highly charged ions with E1, M1, and E2 transitions within laser range
• AMBiT: A program for high-precision relativistic atomic structure calculations
• Ab initio calculation of the potential bubble nucleus ${}^{34}$Si
• Opportunities for Fundamental Physics Research with Radioactive Molecules
• Magnetic-dipole transitions in highly-charged ions as a basis of ultra-precise optical clocks
• Combined CI+MBPT calculations of energy levels and transition amplitudes in Be, Mg, Ca, and Sr
• Calculation of isotope shifts and relativistic shifts in CI, CII, CIII and CIV
• CeNTREX: A new search for time-reversal symmetry violation in the ${}^{205}$Tl nucleus
• Atomic many-body effects and Lamb shifts in alkali metals
• Generalized King linearity and new physics searches with isotope shifts
• Detection of the $5p-4f$ orbital crossing and its optical clock transition in Pr${}^{9+}$
• Analysis of the fine structure of Sn${}^{11+...14+}$ ions by optical spectroscopy in an electron beam ion trap
• Optical spectroscopy of complex open 4$d$-shell ions Sn${}^{7+}$-Sn${}^{10+}$
• 4-component relativistic Hamiltonian with effective QED potentials for molecular calculations
• Isotope Shifts of Radium Monofluoride Molecules
• Complete basis set extrapolation of electronic correlation energies using the Riemann zeta function
• Varying Constants
• Recent progress in laser spectroscopy of the actinides
• Implementation of relativistic coupled cluster theory for massively parallel GPU-accelerated computing architectures
• Nuclear magnetization distribution effect in molecules: Ra${}^{+}$ and RaF hyperfine structure
• Information content of the differences in the charge radii of mirror nuclei
• Systematic study of relativistic and chemical enhancements of $\mathcal{P},\mathcal{T}$-odd effects in polar diatomic radicals
• Approaching meV level for transition energies in the radium monofluoride molecule RaF and radium cation Ra${}^{+}$ by including quantum-electrodynamics effects
• Core-valence correlations for atoms with open shells
• Quantum electrodynamics corrections to energies, transition amplitudes and parity nonconservation in Rb, Cs, Ba${}^{+}$, Tl, Fr and Ra${}^{+}$
• Nuclear charge radii of silicon isotopes
• Testing Quantum Electrodynamics with Exotic Atoms
• Nuclear spin-dependent parity-violating effects in light polyatomic molecules
• Stringent tests of QED using highly charged ions
• Hyperfine structure constants on the relativistic coupled cluster level with associated uncertainties
• Systematic study and uncertainty evaluation of $P,T$-odd molecular enhancement factors in BaF
• A Partitioned Correlation Function Interaction approach for describing electron correlation in atoms
• Calculation of the parity and time reversal violating interaction in ^{225}RaO
• Testing atomic wave functions in the nuclear vicinity: the hyperfine structure with empirically-deduced nuclear and quantum electrodynamic effects
• Atomic structure calculations of super heavy noble element oganesson (Z=118)
• Actinide ions for testing the spatial $\alpha -$variation hypothesis
• Correlations between charge radii differences of mirror nuclei and stellar observables
• Electron affinity of oganesson
• Relativistic Fock space coupled cluster study of bismuth electronic structure to extract the Bi nuclear quadrupole moment
• A development of the CI + all-order method and application to the parity-nonconserving amplitude and other properties of Pb
• High-precision ab initio calculations of the spectrum of Lr${}^{+}$
• Benchmarking of the Fock space coupled cluster method and uncertainty estimation: Magnetic hyperfine interaction in the excited state of BaF
• A lower scaling four-component relativistic coupled cluster method based on natural spinors
• The theory of the Bohr-Weisskopf effect in the hyperfine structure
• MCDHF calculations of the electric dipole moment of radium induced by the nuclear Schiff moment
• Generalized relativistic small-core pseudopotentials accounting for quantum electrodynamic effects: construction and pilot applications
• Laser Resonance Chromatography of Superheavy Elements
• Laser-coolable AcOH${}^{+}$ ion for $\mathcal{C}\mathcal{P}$-violation searches
• The hyperfine anomaly in heavy atoms and its role in precision atomic searches for new physics
• Ab initio calculations of the spectrum of lawrencium
• Diagonal and off-diagonal hyperfine structure matrix elements in KCs within the relativistic Fock space coupled cluster theory
• When gold is not enough: platinum standard of quantum chemistry with $N^7$ cost
• Nuclear-spin dependent parity violation in diatomic molecular ions
• Nuclear Moments of Germanium Isotopes around $N$ = 40
• Implementation and Application of the Relativistic Equation of Motion Coupled-cluster Method for the Excited States of Closed-shell Atomic Systems
• Ground state of superheavy elements with $120\le Z\le 170$: systematic study of the electron-correlation, Breit, and QED effects
• $\mathcal{T},\mathcal{P}$-odd effects in the LuOH${}^{+}$ cation
• On three topical aspects of the N=28 isotonic chain
• Calculating the many-potential vacuum polarization density of the Dirac equation in the finite-basis approximation
• Bound-state relativistic quantum electrodynamics: a perspective for precision physics with atoms and molecules
• Accurate theoretical determination of the ionization potentials of CaF, SrF, and BaF
• Energy Level Structure of Sn${}^{3+}$ Ions
• High-order finite element method for atomic structure calculations
• Ab initio study and assignment of electronic states in molecular RaCl
• Cool molecular highly charged ions for precision tests of fundamental physics
• Electron correlation effects of the ThO and ThS molecules in the spinor basis. A relativistic coupled cluster study of ground and excited states properties
• Ab initio study of electronic states and radiative properties of the AcF molecule
• Global analysis of CP-violation in atoms, molecules and role of medium-heavy systems
• Relativistic coupled cluster calculations of the electron affinity and ionization potential of Nh(113)
• $(\mathcal{P},\mathcal{T})$-Odd Tensor-Pseudotensor Interactions in atomic {${}^{199}$Hg} and {${}^{225}$Ra}
• Refined theoretical values of field and mass isotope shifts in thallium to extract charge radii of Tl isotopes
• Estimating complete basis set extrapolation error through random walk
• State-specific ion mobilities of Lr^+ (Z = 103) in helium
• $\mathcal{C}\mathcal{P}$-violation sensitivity of closed-shell radium-containing polyatomic molecular ions

Cited by in corpus (1)

• Ab initio calculations of the electronic structure of Ac${}^{+}$