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.
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