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The field of attosecond science was first enabled by nonlinear compression ofintense laser pulses to a duration below two optical cycles. Twenty yearslater, creating such short pulses still requires state-of-the-art few-cyclelaser amplifiers to most efficiently exploit 'instantaneous' opticalnonlinearities in noble gases for spectral broadening and parametric frequencyconversion. Here, we show that nonlinear compression can in fact be much moreefficient when driven in molecular gases by pulses substantially longer than afew cycles, due to enhanced optical nonlinearity associated with rotationalalignment. We use 80-cycle pulses from an industrial-grade laser amplifier tosimultaneously drive molecular alignment and supercontinuum generation in agas-filled capillary, producing more than two octaves of coherent bandwidth andachieving >45-fold compression to a duration of 1.7 cycles. As the enhancednonlinearity is linked to rotational motion, the dynamics can be exploited forlong-wavelength frequency conversion and compressing picosecond lasers.

Multi-Octave Supercontinuum Generation and Frequency Conversion based on Rotational