Abstract
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.
Highlights
Many basic aromatic molecules absorb deep-ultraviolet (DUV) radiation and sometimes undergo photochemical reaction
Time-resolved ultrafast spectroscopy with sub-10-fs deep ultraviolet pulses was demonstrated for the first time
The electronic excited state and vibrational dynamics of an aqueous solution of a nucleobase, thymine were simultaneously probed with a sub10-fs time resolution
Summary
Many basic aromatic molecules absorb deep-ultraviolet (DUV) radiation and sometimes undergo photochemical reaction. In the visible spectral range, sub-10-fs optical pulses have been routinely obtained and applied in the transient absorption spectroscopy This allows one to probe the vibrational dynamics taking place simultaneously with the electronic-excited-state dynamics. Demonstration of this spectroscopy in the DUV wavelength range should lead to a powerful way to investigate the photochemical dynamics of biologically relevant molecules. The electronic excited state and vibrational dynamics of an aqueous solution of a nucleobase, thymine were simultaneously probed with a sub10-fs time resolution. This allows us to observe wavepackets corresponding to several vibrational modes in both the electronic excited states and ground state simultaneously.
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