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Ultrafast electronic relaxations from the S3 state of pyrene

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Abstract

The ultrafast relaxation occurring in pyrene upon excitation at 4.68 eV was studied in a supersonic gas-jet fs pump–probe experiment. Mass spectrometry and velocity map imaging of photoelectrons produced by probing via multiphoton ionisation at 800 nm reveal that the initially prepared wave packet exhibits a fast relaxation (<80 fs), followed by a slower one of 200 fs. By comparing the propensity rules of photoionisation observed at one color with ab initio calculations, we tentatively assign these two timescales to a first internal conversion to the dark bB3g state followed by a second one to the long lived aB2u first excited state. Vertical excitation energies determined using ab initio Multi-State Complete Active Space 2nd order Perturbation Theory (MS-CASPT2), as well as oscillator strengths between several electronic states, are reported.

Graphical abstract: Ultrafast electronic relaxations from the S3 state of pyrene

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Publication details

The article was received on 06 Nov 2018, accepted on 04 Feb 2019 and first published on 05 Feb 2019


Article type: Paper
DOI: 10.1039/C8CP06895J
Citation: Phys. Chem. Chem. Phys., 2019, Advance Article

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    Ultrafast electronic relaxations from the S3 state of pyrene

    J. A. Noble, C. Aupetit, D. Descamps, S. Petit, A. Simon, J. Mascetti, N. Ben Amor and V. Blanchet, Phys. Chem. Chem. Phys., 2019, Advance Article , DOI: 10.1039/C8CP06895J

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