I will review the technique of Molecular Modulation and describe our recent results on efficient Raman generation in multi-level molecular systems, where excitations of adjacent transitions can interfere with each other. We use several (two or three) laser pulses at wavelengths such that their difference frequencies are tuned close to Raman resonances, so as to excite substantial molecular coherence. We use few-nanosecond pulses when we work with gasses, and sub-picosecond pulses when we work with Raman-active crystals. In both experiments we observe efficient generation of multiple mutually-coherent frequency sidebands that span infrared, visible, and ultraviolet spectral regions, opening possibilities for synthesis of subfemtosecond light waveforms, and for further studies of ultrafast molecular dynamics and molecular structure.