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Ultrafast dynamics of excited electronic states in nitrobenzene measured by ultrafast transient polarization spectroscopy

By Richard Thurston, Matthew M. Brister, Liang Z. Tan, Elio G. Champenois, Said Bakhti, Pavan Muddukrishna, Thorsten Weber, Ali Belkacem, Daniel S. Slaughter and Niranjan Shivaram

Abstract

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 page

Topics: Physics - Chemical Physics, Physics - Optics, Quantum Physics
Publisher: 'American Chemical Society (ACS)'
Year: 2019
DOI identifier: 10.1021/acs.jpca.0c01943
OAI identifier: oai:arXiv.org:1912.12902

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