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Physical Review A

Erasing the traces of classical mechanics in ionization of H 2 by quantum interferences

O A Fojón, Carlos R. Stia, R D Rivarola

Published Sep 26, 2011• 5 citations
Publisher

Abstract

The single ionization of hydrogen molecules by fast electron impact is studied theoretically for transitions from the ground (gerade) state to final ground (gerade) and first-excited (ungerade) states of H${}_{2}^{+}$. It is shown that under definite conditions and for particular orientations of the molecule, the main physical features of the ionization reaction, which are the binary and recoil peaks usually associated with classical mechanisms, are completely erased by quantum interference effects that resemble the ones predicted previously for photoionization reactions. However, these new effects cannot be derived from photoionization results, as the electromagnetic field cannot transfer momentum. In addition, it is found that the emission spectra of transitions leading to the final gerade and ungerade states of the H${}_{2}^{+}$ residual target are analogous in certain cases to the patterns of two sources emitting waves in phase or antiphase, respectively. Finally, we show how an average of the emission from randomly oriented molecules produces a binary peak at the classical expected position, in agreement with experiments.

DOI
10.1103/physreva.84.032715

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The single ionization of hydrogen molecules by fast electron impact is studied theoretically for transitions from the ground (gerade) state to final ground (gerade) and first-excited (ungerade) states of H2+{}_{2}^{+}2+​. It is shown that under definite conditions and for particular orientations of the molecule, the main physical features of the ionization reaction, which are the binary and recoil peaks usually associated with classical mechanisms, are completely erased by quantum interference effects that resemble the ones predicted previously for photoionization reactions. However, these new effects cannot be derived from photoionization results, as the electromagnetic field cannot transfer momentum. In addition, it is found that the emission spectra of transitions leading to the final gerade and ungerade states of the H2+{}_{2}^{+}2+​ residual target are analogous in certain cases to the patterns of two sources emitting waves in phase or antiphase, respectively. Finally, we show how an average of the emission from randomly oriented molecules produces a binary peak at the classical expected position, in agreement with experiments.
We show that two-particle interferences can be used to probe the nuclear motion in a doubly excited hydrogen molecule. The dissociation of molecular hydrogen by electron impact involves several decay channels, associated with different molecular rotational states, which produce quantum interferences in the detection of the atomic fragments. Thanks to the correlations between the angular momentum and the vibrational states of the molecule, the fragments arising from each dissociation channel carry out a phase shift which is a signature of the molecule rotation. These phase shifts, which cannot be observed in a single-atom detection scheme, may be witnessed under realistic experimental conditions in a time-of-flight coincidence measurement. We analyze the interferences arising from the two lowest-energy rotational states of a parahydrogen molecule. Our result shows the relevance of two-fragment correlations to track the molecular rotation.
Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.
Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.
New experimental results are presented for short-pulse microwave ionization of highly excited hydrogen atoms. A comparison of these results with quantum numerical computations and analytical predictions provides for the first time experimentally grounded evidence of the localization phenomenon that leads to the suppression of the quantum version of the chaotic diffusion in action space occurring in the classical limit. The onset of chaotic motion in externally driven classical systems is a key problem in nonlinear dynamics that is now well understood in its essential aspects. In many physically interesting cases, as the perturbation strength increases beyond some critical value, the system starts absorbing energy in a diffusive way. The question whether “diffusive” excitation processes can take place also in externally driven quantum systems is then a very interesting one for the physics of atoms and molecules in external electromagnetic fields. This is a deep question involving the nature and the validity of the quasiclassical approximation when the underlying classical dynamics is chaotic. The question of “quantum diffusion” was first addressed in a simple model system, the kicked rotator. It was chosen because the features of classical chaos in it were relatively clean and well understood. Besides that, the numerical simulation of its quantum dynamics could be easily accomplished. The major indication of this model was that quantum mechanics suppresses the classical chaotic diffusion in action via a destructive interference effect similar to that responsible for the Anderson localization well known in condensed matter physics.