We demonstrated the efficient excitation of coherent molecular motion for the generation of high-order rotational Stokes and anti-Stokes Raman emissions using a femtosecond laser. Molecular phase modulation of a probe beam was efficiently induced by an optical beat of the pump beam emitting at two different frequencies, the separation of which corresponded to the multiplicative inverse of the period of molecular rotation. The spectral width of the probe pulse was expanded to 10 nm in the deep-ultraviolet region, suggesting the generation of a 10 fs pulse by Fourier synthesis of the emission lines.
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)