Luo Sizuo, Hu Wenhui, Yu Jiaqi, Zhu Ruihan, He Lanhai, Li Xiaokai, Ma Pan, Wang Chuncheng, Liu Fuchun, Roeterdink Wim G, Stolte Steven, Ding Dajun
Institute of Atomic and Molecular Physics, Jilin University , Changchun 130012, China.
Jilin Provincial Key Laboratory of Applied Atomic and Molecular Spectroscopy, Jilin University , Changchun 130012, China.
J Phys Chem A. 2017 Feb 2;121(4):777-783. doi: 10.1021/acs.jpca.6b11209. Epub 2017 Jan 23.
Rotational dynamics of quantum state selected and unselected CHI molecules in intense femtosecond laser fields has been studied. The orientation and alignment evolutions are derived from a pump-probe measurement and in good agreement with the numerical results from the time-dependent Schrödinger equation (TDSE) calculation. The different rotational transitions through nonresonant Raman process have been assigned from the Fourier analysis of the orientation and alignment revivals. These revivals are derived from a pump-probe measurement and in good agreement with the numerical results from the TDSE calculation. For the molecules in rotational state |1, ±1, ∓1⟩, the transitions can be assigned to ΔJ = ±1, ±2, while for thermally populated molecules, the transitions are ΔJ = ±2. Our results illustrate that the orientation and alignment revivals of the rotational quantum-state-selected molecules give a deep insight into the rotational excitation pathways for the transition of different rotational states of molecules in ultrafast laser fields.
研究了强飞秒激光场中量子态选择和未选择的CHI分子的转动动力学。取向和排列演化通过泵浦-探测测量得到，并且与含时薛定谔方程（TDSE）计算的数值结果吻合良好。通过对取向和排列复苏的傅里叶分析，确定了通过非共振拉曼过程的不同转动跃迁。这些复苏通过泵浦-探测测量得到，并且与TDSE计算的数值结果吻合良好。对于处于转动态|1, ±1, ∓1⟩的分子，跃迁可确定为ΔJ = ±1, ±2，而对于热分布的分子，跃迁为ΔJ = ±2。我们的结果表明，转动量子态选择分子的取向和排列复苏为深入了解超快激光场中分子不同转动态跃迁的转动激发途径提供了依据。
