A nonperturbative analytic solution to the transient effective susceptibility tensor due to the presence of a rotational wave packet in nonrigid, symmetric-top molecules excited by intense, arbitrarily polarized laser pulses is presented. Calculations using the analytic model are carried out for the case of a linear and a symmetric-top molecule, including the effect of vibration–rotation coupling on the wave packet. We also compare the analytic results to a numeric solution of the Schrödinger equation for a linearly polarized pump pulse in order to assess the validity of the impulsive approximation.
© 2008 Optical Society of America
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