Semiclassical control theory of coherent anti-Stokes Raman scattering maximizing vibrational coherence for remote detection

J. Chathanathil, G. Liu, S. A. Malinovskaya

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Abstract

A semiclassical theory that describes the generation of a coherent anti-Stokes Raman scattering (CARS) signal is presented that maximizes vibrational coherence in a mode predetermined by the pump, the Stokes, and the probe chirped pulse trains and takes into account the field propagation effects in a cloud of molecules. The buildup of the anti-Stokes signal, which may be used as a molecular signature in the backward CARS signal, is demonstrated numerically. The theory is based on the solution of the coupled Maxwell's and Liouville-von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. A deep convolutional neural network technique is implemented to evaluate time-dependent phase characteristics of the control fields. The effect of decoherence induced by spontaneous decay and collisional dephasing is examined.

Original languageEnglish
Article number043701
JournalPhysical Review A
Volume104
Issue number4
DOIs
StatePublished - Oct 2021

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