Time-resolved ultrafast spectroscopy with sub-10-fs deep ultraviolet pulses was demonstrated for the first time. For the spectroscopy, the sub-10-fs pulses with smooth temporal and spectral profiles, which were suitable for spectroscopy, were prepared via the method of the broadband chirped-pulse four-wave mixing. The vibrational and electronically excited state dynamics in the aqueous solution of thymine were investigated with a sub-10-fs resolution. Vibrational wavepackets originating from the electronically excited state and ground state were observed simultaneously. Through this research, it was shown that the sub-10-fs pulses were successfully applied to the ultrafast spectroscopy, opening the door to the new research activity of ultrafast spectroscopy with a sub-10-fs time resolution in the deep ultraviolet.
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