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Optics Express

Observation of CARS signal via maximal atomic coherence prepared by F-STIRAP in a three-level atomic system

Xiaoli Song, Lei Wang, Rui-Zhu Lin, Zhi‐Hui Kang, Xin Li, Yun Jiang, Jin-Yue Gao

Published Jan 1, 2007• 4 citations
Publisher

Abstract

We control the atomic coherence and the population transfer among Rb hyperfine atomic levels by the fractional stimulated Raman adiabatic passage (F-STIRAP) in a L-type configuration, and verify the theoretical predictions. Applying this technique, we are able to prepare the atoms with maximal coherence to enhance coherent anti-Stokes Raman scattering (CARS) signal. In our experiment by scanning the frequency of one laser from 794.9839 nm to 794.9844 nm with the 794.9698 nm laser frequency fixed to generate a maximum of the CARS signal we are able to obtain the energy level diagram of the sample.

DOI
10.1364/oe.15.007499

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We control the atomic coherence and the population transfer among Rb hyperfine atomic levels by the fractional stimulated Raman adiabatic passage (F-STIRAP) in a L-type configuration, and verify the theoretical predictions. Applying this technique, we are able to prepare the atoms with maximal coherence to enhance coherent anti-Stokes Raman scattering (CARS) signal. In our experiment by scanning the frequency of one laser from 794.9839 nm to 794.9844 nm with the 794.9698 nm laser frequency fixed to generate a maximum of the CARS signal we are able to obtain the energy level diagram of the sample.
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.
Robust control of atomic coherence and population transfer among Zeeman sublevels in the ground states of rubidium atom is investigated using adiabatic rapid passage in a nanosecond time scale, which is smaller than the lifetime of first excited Rb. It is shown that a slight change in the pump pulse time delay relative to the Stokes pulse leads to a significant modification of atomic coherence and population transfer, consequently having remarkable impacts on the generation of coherent anti-Stokes Raman scattering (CARS) signal and probe pulse absorption. This coherent control of quantum state and population is presented by numerical simulations based on self-consistent set of density matrix equations and Maxwell equations as well as experimental demonstration in rubidium atom with different atomic densities. Experimental observations are in good agreement with numerical calculations.
We have experimentally demonstrated the enhancement of coherent Raman scattering in Rb\mathrm{Rb}Rb atomic vapor by exciting maximal atomic coherence with fractional stimulated Raman adiabatic passage. Experimental results are in good agreement with numerical simulations. The results support the possibility of increasing the sensitivity of coherent anti-Stokes Raman spectroscopy by preparing maximal atomic or molecular coherence using short pulses.
We theoretically demonstrate the achievement of narrow-band coherent anti-Stokes Raman scattering (CARS) signal by manipulating broad-band probe spectrum. The narrowing of the CARS signal depends on the spectrum bandwidth of the probe beam, and thus high-resolution CARS signal for a complicated quantum system can be obtained by the simple spectrum manipulation. Furthermore, the energy-level diagram for the complicated quantum system can also be labelled by measuring the CARS signal at a given frequency.