Rotational Dynamics of Quantum State-Selected Symmetric-Top Molecules in Nonresonant Femtosecond Laser Fields

Sizuo Luo; Wenhui Hu; Jiaqi Yu; Ruihan Zhu; Lanhai He; Xiaokai Li; Pan Ma; Chuncheng Wang; Fuchun Liu; Wim G Roeterdink; Steven Stolte; Dajun Ding

doi:10.1021/acs.jpca.6b11209

Rotational Dynamics of Quantum State-Selected Symmetric-Top Molecules in Nonresonant Femtosecond Laser Fields

J Phys Chem A. 2017 Feb 2;121(4):777-783. doi: 10.1021/acs.jpca.6b11209. Epub 2017 Jan 23.

Authors

Sizuo Luo^{1

2}, Wenhui Hu^{1

2}, Jiaqi Yu^{1

2}, Ruihan Zhu³, Lanhai He^{1

2}, Xiaokai Li^{1

2}, Pan Ma^{1

2}, Chuncheng Wang^{1

2}, Fuchun Liu^{1

2}, Wim G Roeterdink^{1

2}, Steven Stolte^{1

2}, Dajun Ding^{1

2}

Affiliations

¹ Institute of Atomic and Molecular Physics, Jilin University , Changchun 130012, China.
² Jilin Provincial Key Laboratory of Applied Atomic and Molecular Spectroscopy, Jilin University , Changchun 130012, China.
³ School of Science, Changchun University of Science and Technology , Changchun 130022, China.

PMID: 28067509
DOI: 10.1021/acs.jpca.6b11209

Abstract

Rotational dynamics of quantum state selected and unselected CH₃I 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.