Monitoring the electron dynamics of the excited state via higher-order spectral minimum

A pump-probe scheme for monitoring the electron dynamics of the excited state has been investigated by numerically solving the two-state time-dependent Schrödinger equation based on the non-Born-Oppenheimer approximation. By adjusting the delay time between a mid-infrared probe pulse and an ultra violet pump pulse, an obvious minimum can be seen in the higher-order harmonic region. With electron probability density distribution, ionization rate and classical simulation, the minimum can be ascribed to the electron localization around one nucleus at larger delay time and represents the electron dynamics of the excited state at the time of ionization. Moreover, the position of the minimum is much more sensitive to the nuclear motion.