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Laser-Induced Alignment and Orientation Dynamics Beyond the Rigid-Rotor Approximation

  • Tamás SzidarovszkyEmail author
  • Kaoru Yamanouchi
Chapter
Part of the Springer Series in Chemical Physics book series (CHEMICAL, volume 118)

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.

Notes

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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Copyright information

© Springer Nature Switzerland AG 2018

Authors and Affiliations

  1. 1.Department of Chemistry, School of ScienceThe University of TokyoTokyoJapan
  2. 2.Laboratory of Molecular Structure and Dynamics, Institute of ChemistryEötvös Loránd University and MTA-ELTE Complex Chemical Systems Research GroupBudapestHungary

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