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Frontiers in Optics

Chirped Pulse Adiabatic Passage in CARS

Svetlana Malinovskaya

Published Jan 1, 2007• 0 citations
Publisher

Abstract

We use adiabatic passage control scheme implementing chirped femtosecond laser pulses to maximize coherence of Raman transitions in CARS. We investigate energy and phase relaxation as factors of quantum decoherence.
DOI
10.1364/fio.2007.jwc9

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We propose the adiabatic passage control scheme to maximize coherence in a predetermined molecular vibrational mode via two-photon Raman transitions. We investigate vibrational energy relaxation and collisional dephasing as factors of coherence loss, and demonstrate the possibility for sustaining high value of coherence in the presence of dephasing by two chirped pulse trains. The proposed method may be used to advance imaging techniques currently applied in the coherent anti-stokes Raman scattering (CARS) microscopy.
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Abstract A chirped-pulse quantum control scheme applicable to coherent anti-Stokes Raman scattering spectroscopy, named as C-CARS, is presented aimed at maximizing the vibrational coherence in molecules. It implies chirping of three incoming pulses in the four-wave mixing process of CARS, the pump, the Stokes and the probe, to fulfill the conditions of adiabatic passage. The scheme is derived in the framework of rotating wave approximation and adiabatic elimination of excited state manifold simplifying the four-level model system into a ‘super-effective’ two level system. We demonstrate that the selectivity of excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The robustness, spectral selectivity and adiabatic nature of this method are advantageous for improving the existing methods of CARS spectroscopy for sensing, imaging and detection.
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.