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Physical Review Letters

Manipulating Atomic Fragmentation Processes by Controlling the Projectile Coherence

Kisra Egodapitiya, Sachin Sharma, A. Hasan, Aaron C. LaForge, D. H. Madison, Robert Moshammer, Michael Schulz

Published Apr 14, 2011• 79 citations
Publisher

Abstract

We have measured the scattering angle dependence of cross sections for ionization in p+H2 collisions for a fixed projectile energy loss. Depending on the projectile coherence, interference due to indistinguishable diffraction of the projectile from the two atomic centers was either present or absent in the data. This shows that, due to the fundamentals of quantum mechanics, the preparation of the beam must be included in theoretical calculations. The results have far-reaching implications on formal atomic scattering theory because this critical aspect has been overlooked for several decades.

DOI
10.1103/physrevlett.106.153202

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We have measured the scattering angle dependence of cross sections for ionization in p+H2 collisions for a fixed projectile energy loss. Depending on the projectile coherence, interference due to indistinguishable diffraction of the projectile from the two atomic centers was either present or absent in the data. This shows that, due to the fundamentals of quantum mechanics, the preparation of the beam must be included in theoretical calculations. The results have far-reaching implications on formal atomic scattering theory because this critical aspect has been overlooked for several decades.
In the study of collision processes, a series of conditions is usually assumed. One of them is that the beam of projectiles is coherent in lengths greater than those of the targets against which it strikes. However, recent experimental results and theoretical analyzes have shown that this assumption can not only fail, but that it is possible to manipulate the coherence length experimentally to go from a coherent situation to an incoherent one. The most conspicuous and studied manifestation of such loss of coherence is the disappearance of interference effects. However, in the present work we show that a strong decrease can also occur in the magnitude of the cross section, not only differential but also total, due to an atomic concealment effect.
For the last 50 years, there has been considerable interest in the possibility of observing the equivalence of a Young's double-slit wave interference at the quantum level for diatomic molecules. For electron-impact ionization of diatomic molecules, indirect evidence for this type of interference has been found by changing the energy (wavelength) of the ejected electron while keeping the incident projectile scattering angle fixed. The present work represents an experimental and theoretical collaboration to better understand the physics of this type of interference. In addition to examining the effect of changing the ejected electron energy for a fixed scattered projectile angle, we have also examined the effect of keeping the ejected electron energy fixed while varying the projectile scattering angle. Model calculations are performed for three different types of possible two-center interference effects, and it is found that the most important one is diffraction of the projectile off two scattering centers.
The projectile beam coherence effects occurring in ion-atom collisions are analyzed on the basis of the recent theory of Karlovets et al. [Phys. Rev. A 92, 052703 (2015)] developed for the elastic scattering of wave packets of particles off a potential field. This theory is generalized to estimate the loss of coherence for inelastically scattered projectiles in ionizing collisions. The results obtained by the suggested model are compared with experimental data for the ionization of hydrogen atoms and molecules by 75-keV proton impact. Significantly improved agreement is observed between the theory and experiment.
We report the first observation of Young-type interference effects in a two-electron transfer process. These effects change strongly as the projectile velocity changes in fast (1.2 and 2.0 MeV) He(2+) + H(2) collisions as manifested in strong variations of the double-electron capture rates with the H(2) orientation. This is consistent with fully quantum mechanical calculations, which ignore sequential electron transfer, and a simple projectile de Broglie wave picture assuming that two-electron transfer probabilities are higher in collisions where the projectile passes close to either one of the H(2) nuclei.
The subtle and fundamental issue of indistinguishability and interference between independent pathways to the same target state is examined in the context of coherent control of atomic and molecular processes, with emphasis placed on possible "which-way" information due to quantum entanglement established in the quantum dynamics. Because quantum interference between independent pathways to the same target state occurs only when the independent pathways are indistinguishable, it is first shown that creating useful coherence between nondegenerate states of a molecule for subsequent quantum interference manipulation cannot be achieved by collisions between atoms or molecules that are prepared in momentum and energy eigenstates. Coherence can, however, be transferred from light fields to atoms or molecules. Using a particular coherent control scenario, it is shown that this coherence transfer and the subsequent coherent phase control can be readily realized by the most classical states of light, i.e., coherent states of light. It is further demonstrated that quantum states of light may suppress the extent of phase-sensitive coherent control by leaking out some which-way information while "incoherent interference control" scenarios proposed in the literature have automatically ensured the indistinguishability of multiple excitation pathways. The possibility of quantum coherence in photodissociation product states is also understood in terms of the disentanglement between photodissociation fragments. Results offer deeper insights into quantum coherence generation in atomic and molecular processes.