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Physica Scripta

Photoionization Microscopy

Christian Bordas, F. L�pine, Céline Nicole, Marc J. J. Vrakking

Published Jan 1, 2004• 2 citations
Publisher

Abstract

Atomic photoionization provides an experimental situation where the outer electron is ejected to large distance without confinement condition. The application of an electric field during photoionization allows confining the electron flux along one coordinate. Therefore, photoionization in an electric field provides a unique opportunity where quantum properties of the wavefunction are projected into the macroscopic world, permitting a direct view of the square modulus of the electronic wavefunction. We present here the experimental observations of this effect, denominated photoionization microscopy. The analysis is carried out in the framework of the semiclassical model that allows a qualitative interpretation of the experimental results in terms of interferences among various classical trajectories.

DOI
10.1238/physica.topical.110a00068

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Atomic photoionization provides an experimental situation where the outer electron is ejected to large distance without confinement condition. The application of an electric field during photoionization allows confining the electron flux along one coordinate. Therefore, photoionization in an electric field provides a unique opportunity where quantum properties of the wavefunction are projected into the macroscopic world, permitting a direct view of the square modulus of the electronic wavefunction. We present here the experimental observations of this effect, denominated photoionization microscopy. The analysis is carried out in the framework of the semiclassical model that allows a qualitative interpretation of the experimental results in terms of interferences among various classical trajectories.
Photoionization of an atom in the presence of a uniform static electric field provides the unique opportunity to expand and visualize the atomic wave function at a macroscopic scale. In a number of seminal publications dating back to the 1980s, Fabrikant, Demkov, Kondratovich, and Ostrovsky showed that this goal could be achieved by projecting slow (meV) photoionized electrons onto a position-sensitive detector and underlined the distinction between continuum and resonant contributions. The uncovering of resonant signatures was achieved fairly recently in experiments on the nonhydrogenic lithium atoms [Cohen et al., Phys. Rev. Lett. 110, 183001 (2013)]. The purpose of the present article is the general description of these findings, with emphasis on the various manifestations of resonant character. From this point of view, lithium has been chosen as an illustrative example between the two limiting cases of hydrogen, where resonance effects are more easily identified, and heavy atoms like xenon, where resonant effects were not observed.
Synopsis Photoionization microscopy (PM) aims at imaging the flux of slow (meV) electrons released by atomic photoionization in the presence of a static electric field. We discuss the rotation of the linear light polari-zation with respect to the electric field direction. Two-photon ionization out of an m=0 initial state allows for the population of |m|=0,1,2 Stark states. The resulting |m|-beating effects in the PM images are demonstrated theoretically (in hydrogen atom) and experimentally (in Mg atom). Implications on the applicability of tomographic techniques for slow electrons are also discussed.
To describe the microscopic properties of matter, quantum mechanics uses wave functions, whose structure and time dependence is governed by the Schrödinger equation. In atoms the charge distributions described by the wave function are rarely observed. The hydrogen atom is unique, since it only has one electron and, in a dc electric field, the Stark Hamiltonian is exactly separable in terms of parabolic coordinates (η, ξ, φ). As a result, the microscopic wave function along the ξ coordinate that exists in the vicinity of the atom, and the projection of the continuum wave function measured at a macroscopic distance, share the same nodal structure. In this Letter, we report photoionization microscopy experiments where this nodal structure is directly observed. The experiments provide a validation of theoretical predictions that have been made over the last three decades.
Based on the semiclassical analysis of photoionization microscopy, we study the ionization of the Rydberg hydrogen atom near a dielectric surface. The radial electron probability density distributions on a given detector plane are calculated at different scaled energies and near different dielectric surfaces. We find due to the interference effect of different types of electron trajectories arriving at a given point on the detector plane, oscillatory structures appear in the electron probability density distributions. With the increase in the scaled energy, more types of electron ionization trajectories appear and the oscillatory structure in the electron probability density distributions becomes complex. Besides, the dielectric constant of the dielectric surface can also affect the electron probability density distributions. Since the photoionization microscopy interference pattern recorded on the detector plane reflects the distribution of the square modulus of the transverse component of the electronic wave function, with the recorded interference pattern, we can investigate the ionization dynamics of the Rydberg atom near surfaces clearly. This study provides some reference values for the future experiment research on the photoionization microscopy of the Rydberg atom near dielectric surfaces.
Electron microscopy and diffraction have long been used to study the structure of materials. A recent development is the achievement of ultrafast time resolution using high-repetition rate single electron sources and single-shot many-electron sources. Achieving large coherence lengths under these conditions is challenging due to intrinsic heating mechanisms including inter-particle Coulombic forces. Near-threshold, pulsed photoionization of atoms trapped and cooled with lasers is being investigated as a means to produce intense electron pulses with large intrinsic coherence length due to a low electron temperature. Photo-ionizaton sources are, of course, not an entirely new idea but recent implementations using trapped atoms offer new possibilities. Several properties of electron beams extracted from such ultracold sources have already been investigated, showing in particular that temperatures of a few Kelvin and emittances in the nanometer-radian range can be achieved with tens of thousands electrons per pulse for nanosecond pulse lengths. This can be combined with delicate shaping of the charge distribution to counteract emittance growth due to non-linear self fields. Using ultrafast lasers for the ionization step, shorter electron pulses can be achieved, but an interesting question is whether the concomitant spread in photon energy still allows for low electron temperature. Recent experiments have shown that few-Kelvin temperatures combined with picosecond pulse lengths are indeed possible. It turns out that this can be understood with a classical model for electron trajectories resulting from photoionization. In addition, experimentally observed polarization effects are in general agreement with model results. --------------------------------------------------------------------------------
Synopsis Photoionization microscopy (PM) is employed for imaging the flux of slow (meV) electrons ejected via atomic photoionization in the presence of a static electric field. Just above the ionization limit continuum and quasi-disrete states are degenerate. In hydrogen atom resonant excitation dominates over the continuum one, while the reverse holds for more complex atoms. We demonstrate theoretically that by using a bichromatic ω/2ω laser field and by applying phase sensitive coherent control techniques it is possible to unbury and isolate other-wise obscured resonant features in PM images.