Citation: LIU Yu-Zhu, QIN Chao-Chao, ZHANG Song, WANG Yan-Mei, ZHANG Bing. Ultrafast Dynamics of the First Excited State of Chlorobenzene[J]. Acta Physico-Chimica Sinica, ;2011, 27(04): 965-970. doi: 10.3866/PKU.WHXB20110404 shu

Ultrafast Dynamics of the First Excited State of Chlorobenzene

1.
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China; Graduate University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Received Date: 16 December 2010
Available Online: 25 February 2011
Fund Project: 国家自然科学基金(20973194) (20973194)中国科学院创新基金(KJCX1-YW-N30)资助项目 (KJCX1-YW-N30)

Ultrafast dynamics of the first excited state (S₁) of chlorobenzene was studied using a combination of femtosecond time-resolved photoelectron imaging and time-resolved mass spectroscopy. One-photon absorption at 266.7 nm was used to populate the S₁ state of chlorobenzene. The time evolution of the parent ion signals consists of different biexponential decays. One is a fast component on a timescale of (152±3) fs and the other is a slow component with a timescale of (749±21) ps. Time- resolved electron kinetic energies (eKE) and time-resolved photoelectron angular distributions (PADs) were extracted from time-resolved photoelectron imaging and are discussed in detail. The ultrafast process with a time constant of (152±3) fs is a population transfer within the S₁ state, and only a vibrational energy transfer process with strong coupling is a reasonable explanation. This is attributed to an ultrafast process of dissipative intramolecular vibrational energy redistribution (IVR). The lifetime of the S₁ state was determined to be (749±21) ps, and its deactivation was due to slow internal conversion to the ground state. Additionally, nonadiabatic alignment and rotational dephasing of the S₁ state of chlorobenzene, as a typical asymmetric top molecule, were observed. The first C-type and J-type recurrences are expected at delay time of 205.8 and 359.3 ps, respectively.
- Photoelectron image,
- Ultrafast process,
- Vibrational energy redistribution,
- Chlorobenzene,
- Nonadiabatic alignment
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沈阳化工大学材料科学与工程学院沈阳 110142