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Laser Technology

Coherent control of population transfer of the excited double states based on pulse shaping

Zhenhao Wang, Yanghua Zhang, Quanjun Wang, Jingjie Ding, Zuoye Liu

Published Jan 1, 2016• 0 citations
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We investigated numerically and experimentally the enhancement of vibrational coherence and population transfer in solution using tailored pulses. The general control mechanism is based on the precise control of the absorption after excitation with multipulses. Transient absorption was used as an experimental method to quantify the enhancement after the excitation with a shaped pump pulse in the low-pulse energy regime. A density-matrix approach was used to investigate the effect of the shaped excitation of a four-level system (two ground-state vibrational levels + two excited-state vibrational levels). Density-matrix simulation results suggest similar wavelength dependence as observed in the transient absorption experiment. The results show that enhancement of population transfer and vibrational coherence depends crucially on the overlap between the excitation pulse spectrum and the molecular absorption band.
It is shown that, when two femtosecond chirped Gaussian pulses with equal pulse area and same size but opposite sign of the chirp coefficient, which will be simply called as double pulses, overlap and propagate in the three-level Λ-type atomic medium, both coherence between the double pulses and interaction between the double pulses and the atomic medium arise. Adjusting size of the chirp coefficient can change shape, i.e. field distribution, of the composite pulse of the double pulses, at the same time affect the interaction between the composite pulse field and atoms, and thereby control oscillation process and value of the atomic population. By selecting suitable size of the chirp coefficient, we can make the atoms at the lowest level exciting completely to the higher level; moreover the new population distribution is stationary. It is also show that, for the double pulses with any area, efficient and stable population transfer always can be realized by adjusting size of the chirp coefficient. And this conclusion doesn't vary with the pulse width or the medium density varying.