Frequency-tunable multigigawatt sub-half-cycle light pulses from coupled-state dynamics of optical solitons and impulsively driven molecular vibrations.

Coupling ultrashort optical field waveforms to ultrafast molecular vibrations in an impulsively excited Raman medium is shown to enable the generation of frequency-tunable sub-half-cycle multigigawatt light pulses. In a gas-filled hollow waveguide, this coupled-state dynamics is strongly assisted by soliton effects, which help to suppress temporal stretching of subcycle optical pulses, providing efficient Raman-type impulsive excitation of ultrafast molecular vibrations over large propagation paths.