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Chinese Physics B

Photoabsorption cross sections of the alkaline-earth-metal elements under strong interaction conditions

Mengmeng Liu, Xiao‐Guang Ma

Published Jun 1, 2011• 1 citation
Publisher

Abstract

The strong interatomic interaction effects on photoabsorption cross sections of a private atom have been interpreted by the contribution of both the real and imaginary parts of atomic polarizability in the present work. Some unresolved differences between the photoabsorption cross sections of isolated atoms and those of condensed atoms, especially near thresholds and resonances, probably could be interpreted by the competition between the imaginary and real parts of atomic frequency-dependent polarizabilities.

DOI
10.1088/1674-1056/20/6/067801

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The strong interatomic interaction effects on photoabsorption cross sections of a private atom have been interpreted by the contribution of both the real and imaginary parts of atomic polarizability in the present work. Some unresolved differences between the photoabsorption cross sections of isolated atoms and those of condensed atoms, especially near thresholds and resonances, probably could be interpreted by the competition between the imaginary and real parts of atomic frequency-dependent polarizabilities.
The influence of the local-field on the photoabsorption cross section of the atomic silver is studied in detail by using the Clausius–Mossotti (CM) model and the Onsager model separately. The variations of the photoabsorption cross section of atomic silver with number density and radius of the environmental interaction cavity are studied systematically by using more general expressions for the photoabsorption cross sections, proposed by Sun et al recently. It has proved to be reasonable to model the optical response properties of bulky material by coupling the property of isolated atom with the environmental effects in the present work.
The evolution of the photoabsorption cross sections of atomic xenon with number densities varying from ideal gas to condensed matter has been studied by an alternative view in the present work. The alternative expressions of the photoabsorption cross sections presented by Sun et al recently were used with the local field models that has proven to be generalized easily to multiatomic systems including molecules and condensed phase systems. The present results show that the variation of the photoabsorption cross sections of atomic xenon in the giant resonance region from the isolated to the condensed conditions is very small, which agrees well with the variation law of the solid and gas experiments.
Collisions of alkali-metal atoms in the ground state with the electron spin S = 1/2 are accompanied by exchange of electron coordinates between colliding particles, which leads to polarization transfer between them (i.e., to the well-known phenomenon of spin exchange). In addition, along with the polarization transfer from one partner to another, the magnetic resonance lines of colliding atoms are broadened and shifted in spin-exchange collisions. In particular the last two processes depend on the complex spin-exchange cross section. The real part of the cross section determines the so-called "spin-exchange cross section," which is responsible for the broadening of magnetic resonance lines, while the imaginary part determines the shift cross section, which governs the frequency shift of magnetic resonance. In order to describe the spin-exchange process one have to know complex spin-exchange cross sections. Complex spin-exchange cross sections are calculated on the basis of the data on the singlet (X 1 Σ + ) and triplet (a 3 Σ + ) potentials describing the interaction alkali-metal atoms in the ground state. Collisions of alkali-metal atoms Cs, Rb, K, Na in the ground state are considered in the energy interval of 10 −4 −10 −2 au.
Three mutually related problems concerning the interaction of an electron with an alkaline-earth atom are examined. (i) The scattering problem: the phaseshifts for p-electron scattering by Ca, Sr and Ba are calculated. (ii) The negative ion problem: the wavefunction and the binding energy are obtained for the outer electron in Ca - 4s 2 4p, Sr - 5s 2 5p and Ba - 6s 2 6p ions. (iii) The photodetachment problem: the photodetachment cross sections are calculated for the outer electron in each of these ions. The most intriguing feature of these problems is the strong correlational potential, attracting the electron to the atom due to the large dipole polarizabilities of Ca, Sr and Ba. The calculations are performed by means of the Dyson equation of the many-body theory.
We calculate near-threshold photodetachment cross sections for ${\mathrm{Rb}}^{\ensuremath{-}},$ ${\mathrm{Cs}}^{\ensuremath{-}},$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ using the Pauli equation method with a model potential describing the effective electron-atom interaction. Parameters of the model potential are fitted to reproduce ab initio scattering phase shifts obtained from Dirac R-matrix calculations. Special care is taken to formulate the boundary conditions near the atomic nucleus for solving the Pauli equation, based on the analytic solution of the Dirac equation for a Coulomb potential. We find a 3P1o{}^{3}{P}_{1}^{o}3P1o​ resonance contribution to the photodetachment cross section of ${\mathrm{Rb}}^{\ensuremath{-}},$ ${\mathrm{Cs}}^{\ensuremath{-}},$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ ions. Our calculated total photodetachment cross sections for Cs agree with experiments after tuning the resonance position by 2.4 meV. For ${\mathrm{Rb}}^{\ensuremath{-}}$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ the resonance contribution is much smaller than for Cs. We therefore also provide angle-differential cross sections and asymmetry parameters which are much more sensitive to the resonant contribution than total cross sections.
We have observed large oscillations in the photoabsorption cross sections of Ba and Na in the presence of an electric field. The two-step laser excitation technique allowed the use of various polarization combinations for studying the oscillations in the vicinity of the zero-field ionization limits. Thus, we could for the first time determine the relative contributions from two entirely different theoretical models: The quasibound m=0m=0m=0 states (strong-field-mixing resonances) on the one hand, and symmetry-induced oscillator-strength cancellations on the other. We found that the model of strong-field-mixing resonances alone is able to account for all our experimentally observed cross-section oscillations.