Journal
CHEMPHYSCHEM
Volume 18, Issue 6, Pages 670-676Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201601295
Keywords
coumarin; Franck-Condon factors; Huang-Rhys factors; nuclear wave packets; time-resolved fluorescence
Funding
- Global Research Laboratory Program of the National Research Foundation of Korea (NRF) - Korean government (MSIP) [2009-00439]
- National Research Foundation of Korea [2009-00439, 2016K1A4A4A01922687] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Coherent nuclear wave packet motions in an electronic excited state of a molecule are measured directly by time-resolved spontaneous fluorescence spectroscopy with an unprecedented time resolution by using two-photon absorption excitation and fluorescence upconversion by noncollinear sum frequency generation. With an estimated time resolution of approximately 25fs, wave packet motions of vibrational modes up to 1600cm(-1) are recorded for coumarin153 in ethanol. Two-color transient absorption at 13fs time resolution are measured to confirm the result. Vibrational displacements between the ground and excited states and Huang-Rhys factors (HRFs) are calculated by quantum mechanical methods and are compared with the experimental results. HRFs calculated by density functional theory (DFT) and time-dependent DFT reproduce the experiment adequately. This fluorescence-based method provides a unique and direct way to obtain the vibrational spectrum of a molecule in an electronic excited state and the HRFs, as well as the dynamics of excited states, and it might provide information on the structure of an excited state through the HRFs.
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