Abstract
We introduce theoretical methods we developed, with which the laser-induced alignment and/or orientation dynamics of polyatomic molecules can be investigated beyond the rigid rotor approximation. The time-dependent Schrödinger equation is solved by expanding the laser-induced wave packet in terms of the field-free rovibrational eigenstates of the system. We present the results of highly accurate numerical calculations on the laser-induced alignment dynamics of floppy and weakly-bound H2He + and rigid- and strongly-bound H2O , and investigate the effect of the vibrational excitations on the alignment dynamics. We show that one-photon vibrational excitations induce changes in the light-induced alignment and orientation dynamics through the changes in the molecular structure, leading to the breakdown of the rigid rotor approximation, and through the changes in the optical selections in the rotational excitation.
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Acknowledgements
The authors thank the support from the Grant-in-Aid (Tokubetsu Kenkyuin Shorei-hi) scientific research fund of JSPS (Japan Society for the Promotion of Science), project number 26-04333, the JSPS KAKENHI Grant No. 15H05696, and the NKFIH Grant No. PD124623.
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Szidarovszky, T., Yamanouchi, K. (2018). Laser-Induced Alignment and Orientation Dynamics Beyond the Rigid-Rotor Approximation. In: Yamanouchi, K., Martin, P., Sentis, M., Ruxin, L., Normand, D. (eds) Progress in Ultrafast Intense Laser Science XIV. Springer Series in Chemical Physics(), vol 118. Springer, Cham. https://doi.org/10.1007/978-3-030-03786-4_2
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