Delay time dependence of wave packet motion and population transfer of four-level K₂ molecule in pump-pump-probe pulses

The effect of delay time on photoelectron spectra and state populations of a four-level ladder K₂ molecule is investigated by a pump1-pump2-probe pulse via the time-dependent wave packet approach. The periodical motion of the wave packet leads to the periodical change of the photoelectron spectra. The Autler-Townes triple splitting appears at zero delay time, double splitting appears at nonzero delay time between pump1 and pump2 pulses, and no splitting appears at nonzero delay time between pump2 and probe pulses. The periodical change of the state populations with the delay time may be due to the coupling effect between the two pulses. It is found that the selectivity of the state populations may be attained by regulating the delay time. The results can provide an important basis for realizing the optical control of molecules experimentally.