Numerical Simulations of femtosecond-laser-induced dynamic alignment of molecules in the high-frequency off-resonance regime

Abstract

The motion equation for ϑ between the molecular axis and laser polarization direction in a high-frequency off-resonance femtosecond laser field is deduced while simultaneously examining the effects of a permanent dipole moment and field-induced polarizability and hyperpolarizability to molecular rotation. Femtosecond-laser-induced dynamic alignment of CO, N₂, and Br₂ molecules are investigated by numerically solving the obtained rotation equation for the angle ϑ. The effects of the molecular permanent dipole moment and the field-induced polarizability and hyperpolarizability on the degree of alignment are presented at different intensities. Our computational results show that the dynamic alignment of molecules is primarily determined by field-induced polarizability and the second hyperpolarizability for the laser intensity range from 5 × 10¹⁴ to 5 × 10¹⁶ W/cm². The contributions of higher order correction terms to molecular alignment can usually be neglected. The polarizability-field interaction makes the angular distributions of a molecule have a maximum along the polarization axis and a minimum perpendicular to it. The role of the second hyperpolarizability keeps the molecular counts maximum along the laser polarization direction but minimum at an angle of 45° between the molecular axis and the polarization direction. There is also a second maximum of molecular counts perpendicular to the polarization axis. For CO, N₂, and Br₂ molecules, the dependences of laser-induced dynamic alignment on laser intensity exhibit completely different characteristics.