Abstract
Hollow-core photonic-crystal fibers are shown to offer the unique possibility of coherent excitation and probing of Raman-active vibrations in molecules by isolated air-guided modes of electromagnetic radiation. A $3\text{\ensuremath{-}}\mathrm{cm}$ section of a hollow photonic-crystal fiber is used to prepare isolated air-guided modes of pump and probe fields for a coherent excitation of $2331{\text{\ensuremath{-}}\mathrm{cm}}^{\ensuremath{-}1}$ $Q$-branch vibrations of molecular nitrogen in the gas filling the fiber core, enhancing coherent anti-Stokes Raman scattering through these vibrations by a factor of 15 relative to the regime of tight focusing.
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