Continuous-wave phase-matched molecular optical modulator

In optical modulation, the highest available modulation rate is basically limited to the GHz frequency range at best. This is because optical modulation is often performed using electro-optic or acousto-optic effects that require application of an external signal to solid-state nonlinear optical materials. Here we describe optical modulation of continuous-wave radiation at frequencies exceeding 10 THz based on ultrafast variation of molecule polarizability arising from coherent molecular motion. The optical modulation efficiency is extensively enhanced by fulfilling phase-matching conditions with the help of dispersion control of the optical cavity, generating sidebands with a highest ratio of 7.3 × 10(−3). These results will pave the way for development of versatile optical modulation-based techniques in a wide range of research fields in optical sciences, such as mode-locked lasers operating in the THz range.