Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 14, Issue 18, Pages 6200-6210Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2cp23649d
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Funding
- Core Research for Evolutional Science and Technology (CREST) of the Japan Science and Technology Agency (JST)
- National Science Council of the Republic of China, Taiwan [NSC 98-2112-M-009-001-MY3]
- Ministry of Education, Aiming for Top University (MOE ATU) at the National Chiao-Tung University (NCTU)
- Institute of Laser Engineering, Osaka University [A3-01]
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Time-resolved transient absorption spectroscopy with sub-9 fs ultrashort laser pulses in the deep-ultraviolet (DUV) region is reported for the first time. Single 8.7 fs DUV pulses with a spectral range of 255-290 nm are generated by a chirped-pulse four-wave mixing technique for use as pump and probe pulses. Electronic excited state and vibrational dynamics are simultaneously observed for an aqueous solution of thymine over the full spectral range using a 128-channel lock-in detector. Vibrational modes of the electronic ground state and excited states can be observed as well as the decay dynamics of the electronic excited state. Information on the initial phase of the vibrational modes is extracted from the measured difference absorbance trace, which contains oscillatory structures arising from the vibrational modes of the molecule. Along with other techniques such as time-resolved infrared spectroscopy, spectroscopy with sub-9 fs DUV pulses is expected to contribute to a detailed understanding of the photochemical dynamics of biologically significant molecules that absorb in the DUV region such as DNA and amino acids.
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