Ultrafast dynamics of excited electronic states in nitrobenzene measured by ultrafast transient polarization spectroscopy
| Autor: | Thurston, Richard, Brister, Matthew M., Tan, Liang Z., Champenois, Elio G., Bakhti, Said, Muddukrishna, Pavan, Weber, Thorsten, Belkacem, Ali, Slaughter, Daniel S., Shivaram, Niranjan |
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| Rok vydání: | 2019 |
| Předmět: | |
| Druh dokumentu: | Working Paper |
| DOI: | 10.1021/acs.jpca.0c01943 |
| Popis: | We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using Ultrafast Transient Polarization Spectroscopy (UTPS), extending the well-known technique of Optical-Kerr Effect (OKE) spectroscopy to excited electronic states. The third-order non-linear response of the excited molecular ensemble is highly sensitive to details of excited state character and geometries and is measured using two femtosecond pulses following a third femtosecond pulse that populates the S1 excited state. By measuring this response as a function of time delays between the three pulses involved, we extract the dephasing time of the wave-packet on the excited state. The dephasing time measured as a function of time-delay after pump excitation shows oscillations indicating oscillatory wave-packet dynamics on the excited state. From the experimental measurements and supporting theoretical calculations, we deduce that the wave-packet completely leaves the S1 state surface after three traversals of the inter-system crossing between the singlet S1 and triplet T2 states. Comment: Manuscript 15 pages, 4 figures, 1 table. Supporting Information 5 pages |
| Databáze: | arXiv |
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