Laser-induced dynamics of molecules with strong nuclear quadrupole coupling

Abstract

We present a general variational approach for computing the laser-induced rovibrational dynamics of molecules taking into account the hyperfine effects of the nuclear quadrupole coupling. The method combines the general variational approach TROVE, which provides accurate rovibrational hyperfine energies and wave functions for arbitrary molecules, with the variational method RichMol, designed for generalized simulations of the rovibrational dynamics in the presence of external electric fields. We investigate the effect of the nuclear quadrupole coupling on the short-pulse laser alignment of a prototypical molecule CFClBrI, which contains nuclei with large quadrupole constants. The influence of the nuclear quadrupole interactions on the post-pulse molecular dynamics is negligible at early times, first several revivals, however at longer timescales the effect is entirely detrimental and strongly depends on the laser intensity. This effect can be explained by dephasing in the laser-excited rotational wavepacket due to irregular spacings between the hyperfine-split nuclear spin states across different rotational hyperfine bands.

arXiv comment7 pages, 1 figure

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Cited by in corpus (7)

• Rotational coherence spectroscopy of molecules in helium nanodroplets: Reconciling the time and the frequency domains
• Calculation of Electric Quadrupole Linestrengths for Diatomic Molecules: Application to the H2, CO, HF and O2 Molecules
• First observation of electric-quadrupole infrared transitions in water vapour
• Electric quadrupole transitions in carbon dioxide
• The effect of nuclear-quadrupole coupling in the laser induced alignment of molecules
• The nuclear-spin-forbidden rovibrational transitions of water from first principles
• Controlling rotation in the molecular-frame with an optical centrifuge