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Jerusalem Symposia on Quantum Chemistry and Biochemistry

Quantum Interference and the Control of Molecular Processes

Paul W. Brumer, Moshe Shapiro

Published Jan 1, 1991• 5 citations
Publisher
DOI
10.1007/978-94-011-2642-7_22

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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.

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Interference is widely regarded as a foundational attribute of quantum mechanics. However, for a given experimental arrangement, interference can either contribute or not contribute to the outcome depending upon the basis in which it is measured. This observation is both foundational and particularly relevant to coherent control of molecular processes, an approach based upon quantum interference. Here, we address this issue and its relevance to controlling molecular processes via the "coherent control scattering (CCS) matrix," a formalism that allows for an analysis of modifications in an interference structure resulting from a change of basis. This analysis reveals that the change in the interference structure can be attributed to the non-commutativity of the transformation matrix with the CCS matrix and the non-orthogonality of the transformation. Additionally, minimal interference is shown to be associated with the CCS eigenbasis and that the Fourier transform of the eigenvectors of the CCS matrix provides the maximal interference and hence the best coherent control. The change of controllability through a change of basis is illustrated with an example of 85Rb+ 85Rb scattering. In addition, the developed formalism is applied to explain recent experimental results on He + D2 inelastic scattering demonstrating the presence or absence of interference depending on the basis.

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jan 5, 1994•0 citations
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.
Interference is widely regarded as a foundational attribute of quantum mechanics. However, for a given experimental arrangement, interference can either contribute or not contribute to the outcome depending upon the basis in which it is measured. This observation is both foundational and particularly relevant to coherent control of molecular processes, an approach based upon quantum interference. Here, we address this issue and its relevance to controlling molecular processes via the "coherent control scattering (CCS) matrix," a formalism that allows for an analysis of modifications in an interference structure resulting from a change of basis. This analysis reveals that the change in the interference structure can be attributed to the non-commutativity of the transformation matrix with the CCS matrix and the non-orthogonality of the transformation. Additionally, minimal interference is shown to be associated with the CCS eigenbasis and that the Fourier transform of the eigenvectors of the CCS matrix provides the maximal interference and hence the best coherent control. The change of controllability through a change of basis is illustrated with an example of 85Rb+ 85Rb scattering. In addition, the developed formalism is applied to explain recent experimental results on He + D2 inelastic scattering demonstrating the presence or absence of interference depending on the basis.