Establishment of Molecular Light Modulation and its Application to Ultrashort Pulse Generation

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This project aimed realization of a novel ultrashort pulse laser by using a coherently-oscillating high-density molecular-ensemble as an ultrahigh-frequency light-modulator.We summarize the main points of the achievments for this three-years-project.1.Realization of ultrahigh frequency light-modulator at both 125THz (vibration) and 10THz (rotation) (This is equivalent to the realization of near-maximal coherence state such that all the molecules coherently oscillate.)2.Generation of ultrabroad Raman sidebands which extends from near vacuum ultraviolet to infrared with a frequency width of 〜70,000cm^<-1>(〜2,100 PHz)3.Generation of a train of 10-fs ultrashort pulses at ultrahigh repetition-rate of 10-THz with high stability as an actual light source by controlling the spectral phases of the broad Raman sidebands. This result is quantitatively evaluated based on a well-established pulse measurement technique, second-harmonic-generation autocorrelation.