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Bulletin of the American Physical Society

Optimizing coherent anti-Stokes Raman scattering by genetic algorithm controlled pulse shaping

Wenlong Yang, Alexei V. Sokolov

Published Oct 22, 2010• 0 citations
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In this paper, we present a feasible method to realize and improve the selective excitation of femtosecond coherent anti-Stokes Raman scattering (CARS) in a mixture. We theoretically show that, by shaping both the pump and probe pulses with the pi phase step, the CARS signal from one quantum system can be enhanced and simultaneously that from the other quantum system is effectively suppressed. Comparing with only shaping the probe pulse [D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett., 88, 063004 (2002)], the selectivity of femtosecond CARS by shaping both pump and probe pulses can be greatly improved. Finally, we experimentally compare two shaping schemes by investigating the selective excitation of the femtosecond CARS in the mixture of dibromomethane (CH(2)Br(2)) and chloroform (CHCl(3)).

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We present a theoretical investigation of stimulated emission pumping to achieve sub-diffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. A pair of control light fields is used to prepopulate the Raman state involved in the CARS process prior to the CARS signal generation. Efficient prepopulation is achieved by employing a path via an electronic or vibrational state. Thereby, the buildup of a coherence between the ground and Raman state during irradiation by the light fields for CARS signal generation is prevented, resulting in the suppression of the CARS intensity by more than 99.8$%$. Two-dimensional spatial excitation profiles have been calculated using donut-shaped spatial profiles for the control light fields, thus, an intensity-dependent narrowing of the CARS excitation profiles below the diffraction limit. Using computer-generated test images we demonstrate a resolution beyond the diffraction limit for CARS microscopy, which is scalable by the control light field intensity, similar to stimulated emission depletion microscopy.

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We theoretically investigate a scheme in which backward coherent anti-Stokes Raman scattering (CARS) is significantly enhanced by using slow light. Specifically, we reduce the group velocity of the Stokes excitation pulse by introducing a coupling laser that causes electromagnetically induced transparency (EIT). When the Stokes pulse has a spatial length shorter than the CARS wavelength, the backward CARS emission is significantly enhanced. We also investigated the possibility of applying this scheme as a CARS lidar with O2 or N2 as the EIT medium. We found that if nanosecond laser with large pulse energy (>1 J) and a telescope with large aperture (~10 m) are equipped in the lidar system, a CARS lidar could become much more sensitive than a spontaneous Raman lidar.

arXiv:1701.00207•Jan 1, 2017•1 citation

Resonant coherent anti-Stokes Raman scattering

Brigitte Attal‐Trétout

•Sep 1, 1983•0 citations
In this paper, we present a feasible method to realize and improve the selective excitation of femtosecond coherent anti-Stokes Raman scattering (CARS) in a mixture. We theoretically show that, by shaping both the pump and probe pulses with the pi phase step, the CARS signal from one quantum system can be enhanced and simultaneously that from the other quantum system is effectively suppressed. Comparing with only shaping the probe pulse [D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, Phys. Rev. Lett., 88, 063004 (2002)], the selectivity of femtosecond CARS by shaping both pump and probe pulses can be greatly improved. Finally, we experimentally compare two shaping schemes by investigating the selective excitation of the femtosecond CARS in the mixture of dibromomethane (CH(2)Br(2)) and chloroform (CHCl(3)).
We present a theoretical investigation of stimulated emission pumping to achieve sub-diffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. A pair of control light fields is used to prepopulate the Raman state involved in the CARS process prior to the CARS signal generation. Efficient prepopulation is achieved by employing a path via an electronic or vibrational state. Thereby, the buildup of a coherence between the ground and Raman state during irradiation by the light fields for CARS signal generation is prevented, resulting in the suppression of the CARS intensity by more than 99.8%. Two-dimensional spatial excitation profiles have been calculated using donut-shaped spatial profiles for the control light fields, thus, an intensity-dependent narrowing of the CARS excitation profiles below the diffraction limit. Using computer-generated test images we demonstrate a resolution beyond the diffraction limit for CARS microscopy, which is scalable by the control light field intensity, similar to stimulated emission depletion microscopy.
We theoretically investigate a scheme in which backward coherent anti-Stokes Raman scattering (CARS) is significantly enhanced by using slow light. Specifically, we reduce the group velocity of the Stokes excitation pulse by introducing a coupling laser that causes electromagnetically induced transparency (EIT). When the Stokes pulse has a spatial length shorter than the CARS wavelength, the backward CARS emission is significantly enhanced. We also investigated the possibility of applying this scheme as a CARS lidar with O2 or N2 as the EIT medium. We found that if nanosecond laser with large pulse energy (>1 J) and a telescope with large aperture (~10 m) are equipped in the lidar system, a CARS lidar could become much more sensitive than a spontaneous Raman lidar.