Level sequence and splitting identification of closely-spaced energy levels by angle-resolved analysis of the fluorescence light

TL;DR

This paper investigates how the angular distribution and polarization of fluorescence light can reveal the sequence and splitting of closely spaced energy levels in atoms, using theoretical calculations for atomic sodium.

Contribution

It introduces a method to determine level sequence and splitting of overlapping resonances through analysis of fluorescence light properties, supported by detailed Dirac-Fock calculations.

Findings

Angular distribution and polarization depend strongly on level sequence and splitting.

The method can identify small energy splittings even when spectroscopic resolution is limited.

The approach is demonstrated with atomic sodium resonances.

Abstract

The angular distribution and linear polarization of the fluorescence light following the resonant photoexcitation is investigated within the framework of the density matrix and second-order perturbation theory. Emphasis has been placed on "signatures" for determining the level sequence and splitting of intermediate (partially) overlapping resonances, if analyzed as a function of the photon energy of the incident light. Detailed computations within the multiconfiguration Dirac-Fock method have been performed especially for the $1s^{2}2s^{2}2p^{6}3s\;\, J_{i}=1/2 \,+\, \gamma_{1} \:\rightarrow\: (1s^{2}2s2p^{6}3s)_{1}3p_{3/2}\;\, J=1/2, \, 3/2 \:\rightarrow\: 1s^{2}2s^{2}2p^{6}3s\;\, J_{f}=1/2 \,+\, \gamma_{2}$ photoexcitation and subsequent fluorescence emission of atomic sodium. A remarkably strong dependence of the angular distribution and linear polarization of the $\gamma_{2}$ fluorescence emission is found upon the level sequence and splitting of the intermediate $(1s^{2}2s2p^{6}3s)_{1}3p_{3/2}\;\, J=1/2, \, 3/2$ overlapping resonances owing to their finite lifetime (linewidth). We therefore suggest that accurate measurements of the angular distribution and linear polarization might help identify the sequence and small splittings of closely-spaced energy levels, even if they can not be spectroscopically resolved.