Controlling molecular rotational population by wave-packet interference.

We propose a control scheme for selecting populations of molecular rotational states by wave-packet interference. A series of coherent rotational wave packets is created by nonadiabatic rotational excitation of molecules using two strong femtosecond laser pulses. By adjusting the time delay between the two laser pulses, constructive or destructive interference among these wave packets enables the population to be enhanced or suppressed for a specific rotational state. The evolution of the rotational wave packet with selected populations produces interference patterns with controlled spatial symmetries. This method provides an approach to prepare a molecular ensemble with selected quantum-state distributions and controlled spatial distributions under field-free condition.