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Journal of Luminescence

Quantum coherence in nonlinear optical processes: theory and possible application to control of chemical reaction and quantum computation

Jianshu Cao

Published May 1, 2000• 3 citations
Publisher
DOI
10.1016/s0022-2313(99)00210-0

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Chemical reactions in a statistical ensemble are conventionally regarded as incoherent processes driven by thermodynamics. In the quantum degenerate regime, where atoms and molecules form coherent matter waves, reactions are theoretically described by nonlinear mixing of matter-wave fields. In this scenario, we expect phase matching between reactants and products, analogous to the mixing of photonic fields in nonlinear optics. Here we report on the observation of phase coherent reaction dynamics of Bose-condensed atoms and molecules near a Feshbach resonance. Using matter-wave diffraction with optical lattices, we verify spatial coherence of both atoms and molecules and observe phase doubling when atomic waves combine into molecular waves, the matter-wave analogue of optical frequency doubling. The diffraction patterns further reveal two-atom entanglement generated during the reaction. Our observations establish phase coherence and entanglement generation as two essential features of "quantum many-body chemistry". Moreover, our work opens a pathway to control of reaction dynamics by manipulation of matter-wave phases.
Entanglement is a crucial resource for achieving quantum advantages in quantum computation, quantum sensing, and quantum communication. As shown in this Letter, entanglement is also a valuable resource for the coherent control of the large class of bimolecular chemical reactions. We utilize an entanglement-enhanced coherent control scheme, in which the initial preparation of the superposition state is divided into two steps: the first entangles the reactants, and the second is responsible for coherent control. This approach can overcome the limitations of traditional coherent control of scattering caused by noninterfering pathways, known as satellite terms. By tuning the amount of entanglement between reactants, the visibility of coherent control in chemical reactions can be modulated and optimized. Significantly, there exists an optimal amount of entanglement, which ensures complete indistinguishability of the reaction pathways, maximizing the extent of control. This entanglement-enhanced coherent control scheme is computationally illustrated using the ultracold KRb + KRb reaction, where perfect control over the parity of the product rotational states is achieved.