Ultrafast time-resolved pump-probe spectroscopy of PYP by a sub-8 fs pulse laser at 400 nm

Jun Liu, Atsushi Yabushita, Seiji Taniguchi, Haik Chosrowjan, Yasushi Imamoto, Keiichi Sueda, Noriaki Miyanaga, Takayoshi Kobayashi*

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    10 Scopus citations


    Impulsive excitation of molecular vibration is known to induce wave packets in both the ground state and excited state. Here, the ultrafast dynamics of PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser at 400 nm. The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal covering 360-440 nm. The dependence of the vibrational phase of the vibrational mode around 1155 cm-1 on the probe photon energy was observed for the first time to our knowledge. The vibrational mode coupled to the electronic transition observed in the probe spectral ranges of 2.95-3.05 and 3.15-3.35 eV was attributed to the wave packets in the ground state and the excited state, respectively. The frequencies in the ground state and excited state were determined to be 1155 ± 1 and 1149 ± 1 cm-1, respectively. The frequency difference is due to change after photoexcitation. This means a reduction of the bond strength associated with π-π* excitation, which is related to the molecular structure change associated with the primary isomerization process in the photocycle in PYP. Real-time vibrational modes at low frequency around 138, 179, 203, 260, and 317 cm -1 were also observed and compared with the Raman spectrum for the assignment of the vibrational wave packet.

    Original languageEnglish
    Pages (from-to)4818-4826
    Number of pages9
    JournalJournal of Physical Chemistry B
    Issue number17
    StatePublished - 2 May 2013


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