Abstract
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.
Highlights
To trace the dynamic processes in atoms and molecules, researchers have made big process in the development of the ultrashort laser pulse[1]
How do the higher-order harmonics code the electron dynamics of the excited state, which play a key role in the generation of ultrashort pulse1? Considering have adopted the pump-probe the fast scheme tdoispsroecpiaatrieoTn+2ofinHt2+heatseuxpceirtepdossittaitoenbsltuartreinogf some dynamic information, we the ground and excited states to further detect the electron dynamics of the excited state with the higher-order harmonics by solving the two-state time-dependent Schrödinger equation (TDSE) based on the non-Born-Oppenheimer (NBO) approximation
The spectral minimum can be observed at large tdel in the higher-order harmonic region, which can be viewed as a signature of the electron dynamics of the excited state
Summary
To trace the dynamic processes in atoms and molecules, researchers have made big process in the development of the ultrashort laser pulse[1]. Based on the pump-probe scheme[4, 5], Bandrauk et al have observed the attosecond electron motion between coherent electronic states by measuring the photoelectron signal and the photoelectron angular distribution as function of the pump-probe delay time (tdel)[6, 7]. In this scheme, the duration of the probe pulse is shorter than the electron oscillatory period. Classical kinetic energy map and ionization rate distribution are adopted to reveal the underlying physical mechanism
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