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Quantum Information and Measurement (QIM)

Quantum Control in Ultrafast Coherent Bond Making

Zohar Amitay, Liat Levin, Daniel M. Reich, Ronnie Kosloff, Christiane P. Koch

Published Jan 1, 2019• 1 citation
Publisher

Abstract

Quantum control of ultrafast coherent bond making and subsequent molecular dynamics is experimentally demonstrated by controlling branching ratio into different target molecular states. This is a significant step toward realizing a new quantum coherent photochemistry.
DOI
10.1364/qim.2019.f5a.85

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Abstract Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg 2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg 2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.
Synopsis Coherent control of bond making (photoassociation) is crucial for the realization of a new photochemistry, where a laser field is actively photo-driving the irradiated system in a coherent way from the initial state of reactants to the final state of desired products. In a significant step forward, we experimentally demonstrate here coherent control over the photoassociation branching ratio to different target states of the generated molecule. The model process is strong-field multiphoton femtosecond photoassociation of thermally hot magnesium atoms into bound magnesium dimer molecules.
Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg2 molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg2 molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our joint experimental and theoretical study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.
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.
We review the principles and some recent advances in the theory of coherent control of molecular processes and discuss some of its experimental realizations. Amongst the topics discussed are: bichromatic and pump-dump control; the interference between N-photons and M-photon processes; the optical conversion of a mixture of left- and right-handed chiral molecules into an ensemble containing molecules of the handedness of choice; control of collisional processes; control over chaotic dynamics; effects of decoherence; the solution of the non-degenerate quantum control problem; and control over spontaneous emission and other decay processes.