Chirped Pulse Control of Raman Coherence in Atoms and Molecules
- URL: http://arxiv.org/abs/2309.01232v1
- Date: Sun, 3 Sep 2023 17:40:20 GMT
- Title: Chirped Pulse Control of Raman Coherence in Atoms and Molecules
- Authors: Jabir Chathanathil and Svetlana A. Malinovskaya
- Abstract summary: A novel chirped pulse control scheme is presented based on Coherent Anti-Stokes Raman spectroscopy.
The robustness, spectral selectivity and adiabatic nature of C-CARS method may prove useful for sensing, imaging, and detection.
- Score: 0.0
- License: http://creativecommons.org/licenses/by/4.0/
- Abstract: A novel chirped pulse control scheme is presented based on Coherent
Anti-Stokes Raman Spectroscopy (C-CARS) aiming at maximizing the vibrational
coherence in atoms and molecules. The scheme utilizes chirping of the three
incoming pulses, the pump, the Stokes and the probe, in the four-wave mixing
process of C-CARS to fulfill the adiabatic passage conditions. The derivation
of the scheme is based on simplifying the four-level system into a
'super-effective' two level system via rotating wave approximation and
adiabatic elimination of the excited state manifold. The robustness, spectral
selectivity and adiabatic nature of C-CARS method may prove useful for sensing,
imaging, and detection. It is demonstrated that the selectivity in excitation
of vibrational degrees of freedom can be controlled by carefully choosing the
spectral chirp rate of the pulses. The C-CARS control scheme is applied to a
surrogate methanol molecule to generate an optimal anti-Stokes signal
backscattered from a cloud of molecules a kilometer away. The theory is based
on the solution of the coupled Maxwell-Liouville von Neumann equations and
focuses on the quantum effects induced in the target molecules by the control
pulse trains. The propagation effects of pulses through the medium are
evaluated and the buildup of the molecular-specific anti-Stokes signal is
demonstrated numerically. A deep learning technique, using Convolutional Neural
Networks (CNN), is implemented to characterize the control pulses and evaluate
time-dependent phase characteristics from them. The effects of decoherence
induced by spontaneous decay and collisional dephasing are also examined.
Additionally, we present the technique of Fractional Stimulated Raman Adiabatic
Passage (F-STIRAP) and demonstrate that it can be utilized for remote detection
in a multi-level system by creation of a maximally coherent superposition
state.
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