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Physical Review Letters

Observation of interference between quadrupole and dipole transitions in low-energy (2-eV) photoionization from a sodium Rydberg state

Gerd Leuchs, Stephen J. Smith, S. N. Dixit, P. Lambropoulos

Published Feb 17, 1986• 14 citations
Publisher

Abstract

A measurement of the azimuthal dependence of the angular distribution of photoelectrons from ${13}^{3}$${\mathrm{D}}_{3/2}$-state sodium atoms aligned transversely to the direction of propagation of, and parallel to the direction of linear polarization of, 532-nm ionizing laser radiation, is described. The measured distribution is I(\ensuremath{\varphi})=1+0.026(6)cos\ensuremath{\varphi} where \ensuremath{\varphi}=0 is the direction of the laser beam. This departure from the symmetry I(\ensuremath{\varphi})=const predicted for a pure electric dipole transition is represented theoretically as due to a dipole-quadrupole interference term.

DOI
10.1103/physrevlett.56.708

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We have studied experimentally and theoretically two-step photoionization through the 3P state of sodium in an electric field of up to 3.90 kV/cm. The apparatus uses an atomic beam crossed by two pulsed laser beams, one at 589 nm for the first step, and the other swept through the zero field threshold Eo near 409 nm for the ionization. We observe broad undulations in the photocurrent above Eo that narrow with decreasing energy and eventually sharpen into well-defined but asymmetric transitions to Stark-shifted Rydberg states. We calculate the oscillator strength density for the appropriate transitions using modified hydrogenic wave functions and find excellent agreement for the position and relative strength of all the spectral features. We model the asymmetries as Fano-type interferences between quasi-discrete and continuum ionization channels. Using appropriate core potentials, and taking into account core-induced coupling of both discrete-to-continuum and continuum-to-continuum states, we obtain estimates of Fano's q and Ɖ that agree reasonably well with our measurements.
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A theoretical investigation has been carried out on the dependence of the photoelectron angular distributions on laser intensity for the case of two-photon-resonant three-photon ionization of sodium. Good overall agreement is obtained with the experimental anisotropy parameters for ionization via the 4D3/2{D}_{3/2}D3/2​ and 4D5/2{D}_{5/2}D5/2​ intermediate states. The comparison of the theoretical results with the experimental data also clearly shows that the hyperfine splitting of the ground state has to be taken into account at high laser intensities although the low-intensity angular distributions do not depend on the initial ground hyperfine state.