| ATOMIC AND MOLECULAR PHYSICS |
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Two-Photon Excited State Dynamics of Dark Rydberg and Bright Valence States in Furan |
| Jin-You Long, Chun-Long Hu, Bing Zhang**, |
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071
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| Cite this article: |
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Jin-You Long, Chun-Long Hu, Bing Zhang 2017 Chin. Phys. Lett. 34 043101 |
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Abstract Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by one-photon absorption. Here we investigate ultrafast internal conversion (IC) dynamics of furan by using this strategy in combination with femtosecond time-resolved photoelectron imaging. The dark Rydberg $S_{1}$ and bright valence $S_{2}$ states are simultaneously excited by two photons of 405 nm, and then ionized by two photons of 800 nm. The IC from $S_{2}$ to $S_{1}$ is clearly observed and extracted from the time dependence of the higher photoelectron kinetic energy (PKE) component. More importantly, the internal conversions to hot $S_{0}$ from directly-prepared $S_{1}$ and secondarily-populated $S_{1}$ are unambiguously identified by the time-dependence of the lower PKE component. The average lifetime of the $S_{2}$ and $S_{1}$ states is measured to be 29 fs. The internal conversions of $S_{2}$ to $S_{1}$, $S_{1}$ to hot $S_{0 }$ occur on estimated timescales of 15.4 fs and 38 fs, respectively.
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Received: 29 November 2016
Published: 21 March 2017
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| PACS: |
31.70.Hq
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(Time-dependent phenomena: excitation and relaxation processes, and reaction rates)
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33.15.Vb
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(Correlation times in molecular dynamics)
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33.50.-j
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(Fluorescence and phosphorescence; radiationless transitions, quenching (intersystem crossing, internal conversion))
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| Fund: Supported by the National Natural Science Foundation of China under Grant Nos 21303255, 21273274 and 91121006. |
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