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DOE OSTI · 1849506

Selective Enhancement of Spectroscopic Features by Quantum Optimal Control

Keefer, Daniel·Mukamel, Shaul
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Abstract

Tailored light can be used to steer atomic motions into selected quantum pathways. In optimal control theory (OCT), the target is usually expressed in terms of the molecular wave function, a quantity that is not directly observable in experiment. In this study, we present simulations using OCT that optimize the spectroscopic signal itself. By shaping the optical pump, the x-ray stimulated Raman signal, which occurs solely during the passage through conical intersections, is temporally controlled and amplified by up to 2 orders of magnitude. This enhancement can be crucial in order to bring small coherence-based signatures above the detectable threshold. Our approach is applicable to any signal that depends on the expectation value of a positive definite operator.

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74 ATOMIC AND MOLECULAR PHYSICScoherent controlultrafast phenomena

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BibTeXRIS

Keefer, Daniel, Mukamel, Shaul. 2021-04-19. Selective Enhancement of Spectroscopic Features by Quantum Optimal Control. https://doi.org/10.1103/physrevlett.126.163202

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