Multioctave supercontinuum generation and frequency conversion based on rotational nonlinearity

The field of attosecond science was first enabled by nonlinear compression of intense laser pulses to a duration below two optical cycles. Twenty years later, creating such short pulses still requires state-of-the-art few-cycle laser amplifiers to most efficiently exploit "instantaneous" optical nonlinearities in noble gases for spectral broadening and parametric frequency conversion. Here, we show that nonlinear compression can be much more efficient when driven in molecular gases by pulses substantially longer than a few cycles because of enhanced optical nonlinearity associated with rotational alignment. We use 80-cycle pulses from an industrial-grade laser amplifier to simultaneously drive molecular alignment and supercontinuum generation in a gas-filled capillary, producing more than two octaves of coherent bandwidth and achieving >45-fold compression to a duration of 1.6 cycles. As the enhanced nonlinearity is linked to rotational motion, the dynamics can be exploited for long-wavelength frequency conversion and compressing picosecond lasers.