Rovibrational wave-packet manipulation using shaped midinfrared femtosecond pulses

Abstract

We have calculated the propagation of rovibrational wave-packet in the $^{1}\ensuremath{\Sigma}$ state of $\mathrm{CO}$ and the $^{2}\ensuremath{\Pi}$ state of $\mathrm{NO}$ manipulated by shaped midinfrared femtosecond laser pulses. The rotational states of the molecules were fully taken into account in the calculation and the effects of the rotational states in the vibrational wave-packet evolution were examined in detail. As a result, it is found that rotational excitations associated with the vibrational excitation affect the wave-packet propagation drastically, which suggests that the rotational states should not be ignored when vibrational states of molecules are used as the target state for coherent control and qubits for quantum computation. For the experimental detection of the amplitude and phase information on the rovibrational wave-packets, the time profiles of the transition intensities from the rovibrational wave-packet to an electronically excited state were calculated. It is shown that both ionization and laser induced fluorescence signals contain information necessary for the analysis of the phase and relative amplitude of the rovibrational wave-packets.