Broadband-tunable LP₀₁ mode frequency shifting by Raman coherence waves in H₂-filled hollow-core PCF

When a laser pump beam of sufficient intensity is incident on a Raman-active medium such as hydrogen gas, a strong Stokes signal, red-shifted by the Raman transition frequency {\Omega}$_R$, is generated. This is accompanied by the creation of a "coherence wave" of synchronized molecular oscillations with wavevector {\Delta}{\beta} determined by the optical dispersion. Within its lifetime, this coherence wave can be used to shift by {\Omega}$_R$ the frequency of a third "mixing" signal, provided phase-matching is satisfied, i.e., {\Delta}{\beta} is matched. Conventionally this can be arranged using non-collinear beams or higher-order waveguide modes. Here we report collinear phase-matched frequency shifting of an arbitrary mixing signal using only the fundamental LP$_{01}$ modes of a hydrogen-filled hollow-core PCF. This is made possible by the S-shaped dispersion curve that occurs around the pressure-tunable zero dispersion point. Phase-matched frequency shifting by 125 THz is possible from the UV to the near-IR. Long interaction lengths and tight modal confinement reduce the peak intensities required, allowing conversion efficiencies in excess of 70%. The system is of great interest in coherent anti-Stokes Raman spectroscopy and for wavelength-conversion of broadband laser sources.