Polarization control efficiency manipulation in resonance-mediated two-photon absorption by femtosecond spectral frequency modulation

The femtosecond laser polarization modulation is considered as a very simple and efficient method to control the multi-photon absorption process. In this work, we theoretically and experimentally show that the polarization control efficiency in the resonance-mediated two-photon absorption can be artificially manipulated by modulating the femtosecond spectral frequency components. We theoretically demonstrate that the on- and near-resonant parts in the resonance-mediated two-photon absorption process depend on the different femtosecond spectral frequency components, and therefore their contributions in the whole excitation process can be controlled by properly designing the femtosecond spectral frequency components. The near-resonant two-photon absorption is correlated with the femtosecond laser polarization while the on-resonant two-photon absorption is independent of it, and thus the polarization control efficiency in the resonance-mediated two-photon absorption can be manipulated by the femtosecond spectral frequency modulation. We experimentally verify these theoretical results by performing the laser polarization control experiment in the Dy³⁺-doped glass sample under the modulated femtosecond spectral frequency components, and the experimental results show that the polarization control efficiency can be increased when the central spectral frequency components are cut off, while it is decreased when both the low and high spectral frequency components are cut off, which is in good agreement with the theoretical predictions. Our works can provide a feasible pathway to understand and control the resonance-mediated multi-photon absorption process under the femtosecond laser field excitation, and also may open a new opportunity to the related application areas.