Involvement of a low-lying Rydberg state in the ultrafast relaxation dynamics of ethylene
| Autor: | Elio G. Champenois, T. W. Wright, Chan-Shan Yang, Ali Belkacem, Niranjan Shivaram, James P. Cryan |
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| Rok vydání: | 2016 |
| Předmět: |
010304 chemical physics
Chemistry Wave packet General Physics and Astronomy Photoionization 010402 general chemistry Kinetic energy 01 natural sciences 0104 chemical sciences Photoexcitation Ab initio quantum chemistry methods Excited state 0103 physical sciences Physics::Atomic and Molecular Clusters Physics::Chemical Physics Physical and Theoretical Chemistry Rydberg state Atomic physics Excitation |
| Zdroj: | The Journal of chemical physics. 144(1) |
| ISSN: | 1089-7690 2808-2818 |
| Popis: | We present a measurement of the time-resolved photoelectron kinetic energy spectrum of ethylene using 156 nm and 260 nm laser pulses. The 156 nm pulse first excites ethylene to the (1)B1u (ππ(∗)) electronic state where 260 nm light photoionizes the system to probe the relaxation dynamics with sub-30 fs resolution. Recent ab initio calculations by Mori et al. [J. Phys. Chem. A 116, 2808-2818 (2012)] have predicted an ultrafast population transfer from the initially excited state to a low-lying Rydberg state during the relaxation of photoexcited ethylene. The measured photoelectron kinetic energy spectrum reveals wave packet motion on the valence state and shows indications that the low-lying π3s Rydberg state is indeed transiently populated via internal conversion following excitation to the ππ(∗) state, supporting the theoretical predictions. |
| Databáze: | OpenAIRE |
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