Non-Lorentzian atomic natural line-shape of core level multiplets: Access high energy x-ray photons in electron capture nuclear decay

TL;DR

This paper introduces a relativistic multi-reference configuration interaction method to calculate non-Lorentzian line shapes of atomic core level multiplets, revealing asymmetries and energy-dependent effects relevant for high-energy x-ray photon applications.

Contribution

It presents a novel computational approach to model energy-dependent atomic line shapes, accounting for deviations from Lorentzian profiles in core level spectra.

Findings

Atomic absorption lines exhibit asymmetry and high-energy spectral weight excess.

Energy-dependent fluorescence yield significantly increases ionizing radiation estimates.

Results align with previous data and suggest new experimental validation methods.

Abstract

We present a method to calculate the natural line width and energy dependent line shape due to fluorescence decay of core excited atoms within a full relativistic multi-reference configuration interaction theory. The atomic absorption lines show a deviation from a Lorentzian line-shape due to energy dependent matrix elements of the localized electronic state coupling to the photon field. This gives rise to spectral lines with small but visible asymmetry. One generally finds an excess of spectral weight at the high energy shoulder of the atomic absorption line. We present the example of nuclear decay of $^{55}$Fe by electron capture of an inner-shell core electron. We show that the amount of ionizing radiation in the energy window between 50 and 200 keV is around one order of magnitude larger due to the energy dependent fluorescence yield lifetime compared to the value one would obtain if one assumes a constant fluorescence decay rate. This yields a total change of energy deposited into ionizing radiation of about 1\textperthousand. Our calculations are in good agreement with previous calculations and experimental observations where data is available. Our results can be further validated by high precision measurements of electron capture nuclear decay spectra using recently developed experimental methods.