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1.
J Phys Chem A ; 124(11): 2225-2230, 2020 Mar 19.
Article in English | MEDLINE | ID: mdl-32077290

ABSTRACT

We present a theoretical study of the time-dependent laser alignment of molecules taking into account the hyperfine coupling due to nuclear-quadrupole interactions. The coupling of nuclear spins to the overall angular momentum of molecules significantly influences their rotational dynamics. Here, we systematically analyze the impact of the nuclear-quadrupole coupling on the rotational dynamics of the linear and the asymmetric-top diiodobenzene molecule induced by external laser fields. We explore different regimes of pulse shapes and laser-pulse intensities and detail under which conditions the quadrupole coupling cannot be neglected in the description of the laser alignment of molecules.

2.
J Chem Phys ; 151(24): 244118, 2019 Dec 28.
Article in English | MEDLINE | ID: mdl-31893871

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 (Theoretical Ro-Vibrational Energies), which provides accurate rovibrational hyperfine energies and wavefunctions 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 postpulse molecular dynamics is negligible at early times, for the first several revivals; however, at longer time scales, 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.

3.
J Chem Phys ; 146(24): 244304, 2017 Jun 28.
Article in English | MEDLINE | ID: mdl-28668039

ABSTRACT

We present a theoretical study of the mixed-field orientation of molecules without rotational symmetry. The time-dependent one-dimensional and three-dimensional orientation of a thermal ensemble of 6-chloropyridazine-3-carbonitrile molecules in combined linearly or elliptically polarized laser fields and tilted dc electric fields is computed. The results are in good agreement with recent experimental results of one-dimensional orientation for weak dc electric fields [J. L. Hansen, J. Chem. Phys. 139, 234313 (2013)]. Moreover, they predict that using elliptically polarized laser fields or strong dc fields, three-dimensional orientation is obtained. The field-dressed dynamics of excited rotational states is characterized by highly non-adiabatic effects. We analyze the sources of these non-adiabatic effects and investigate their impact on the mixed-field orientation for different field configurations in mixed-field-orientation experiments.

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