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The Philosophical Magazine A Journal of Theoretical Experimental and Applied Physics

Photoionization microscopy of Rydberg hydrogen atom near a dielectric surface

Qiang Chen, Dehua Wang

Published Oct 16, 2015• 2 citations
Publisher

Abstract

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.

DOI
10.1080/14786435.2015.1096026

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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.
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.
The detection of electrons from the surface interaction of Rydberg hydrogen atoms and molecules at a metal surface is investigated experimentally for the first time. The experimental detection of an electron signal in a time gate corresponding to when the Rydberg atoms or molecules are expected to collide with the surface provides evidence for the previously proposed backscattered electron loss (So et al 2009 Phys. Rev. A 79 012901) as a route of surface ionization under electron-extraction fields. Comparison of the ion- and electron-extraction results shows that the dynamics as the Rydberg states approach the surface are very different in the two cases, leading to the possible loss of control of the electronic polarization in the initially prepared Rydberg state from the traversal of level crossings during the Rydberg trajectory. The difference in the ionization dynamics observed for the Rydberg H and H2 cases also illustrates some of the fundamental differences between atomic and molecular, and hydrogenic and non-hydrogenic systems.
The present work has explained a long-standing discrepency between theory and experiment: the broadening of the distances at which Rydberg atoms ionize over a metallic surface. The uneven surface potential distribution on a template-stripped gold surface evaporated on mica is measured with Kelvin probe force microscopy. The stray fields generated by the surface potential are calculated. Simulation with C++ and Matlab predicts how stray fields affect the ionization of Rydberg state atoms near a gold surface. The predicted survival probabilities for different n levels and different incident angles provided by the simulations are then compared with experiments, which shows surprisingly good agreement. Although metallic surfaces are approximately ideal equipotentials in the macroscopic world, Rydberg atoms demonstrate the important role stray fields play in the microscopic world.
Photoionization of Rydberg atoms is considered in the framework of the quasiclassical (WKB) approach. Distribution of the photoelectron density in space and time is found and analyzed. This distribution is shown to consist of two main parts: the temporary population, which exists only as long as the light field is on; and the population corresponding to irreversible ionization. The irreversible-ionization wave packets are shown to experience the effect referred to as Coulomb narrowing. An origin of this effect and the conditions of its existence are discussed. In a strong field, rather simple analytical expressions are found for the partial probabilities of above-threshold ionization and for the total probability of ionization. In contrast to many earlier works, in the present theory neither the rotating-wave nor ``pole'' approximations are used, and the results are derived for an arbitrary pulse shape. Strong-field interference stabilization of Rydberg atoms is confirmed to occur at pulse durations shorter than the Kepler period. The arising regimes of interference stabilization are analyzed in comparison with the predictions of earlier works.
The charge transfer of Rydberg hydrogen atoms at a metal surface is investigated for the first time. The surface ionization of Stark states with various electron density distributions with respect to the surface is examined. Unlike the nonhydrogenic species studied previously, genuine control over the orientation of the electronic wave function in the surface-ionization process is demonstrated. A comparison of the results for a range of collisional velocities for the most redshifted Stark state with principal quantum numbers n=20-36 with the classical over-the-barrier approach shows a good agreement for the onset of the ion signal, but the shallow rise in signal is not accounted for. An excellent fit of the experimental results can be achieved using a simple semiempirical model.
This thesis reports the first controlled study of the interactions of Rydberg atoms with a metal surface. In these experiments, a collimated beam of potassium Rydberg atoms is directed at a plane surface at near grazing incidence. Positive ions formed by surface ionization are attracted to the surface by their image charge, which is counterbalanced by an external electric field applied perpendicular to the surface. The ions are detected by a position-sensitive detector (PSD). At some critical value of the external field, the ion trajectories just miss the surface, suggesting that analysis of the dependence of the ion signals on external electric field can be used to determine the distance from the surface at which ionization occurs. This distance, and thus the corresponding critical electric field, is expected to be n-dependent. Experimentally, however, it was observed that the ion signal had a sudden n-independent onset when only a small positive perpendicular electric field was applied at the surface. This observation requires, surprisingly, that the ions produced by surface ionization can readily escape from the surface. The data do, however, show that Rydberg atoms are efficiently ionized in collisions with the surface. This process may provide a useful new detection technique for Rydberg atoms.