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Optics Communications

Time–frequency analysis of ultrafast dynamics in cascade three-level system driven by hyper-Gaussian pulses

Ji‐Cai Liu, Fen-Fen Guo, Ya-Nan Zhao, Ye-Qi Zhang

Published Jan 11, 2019• 5 citations
Publisher
DOI
10.1016/j.optcom.2019.01.019

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Propagation of strong femtosecond hyper-Gaussian pulses in a cascade three-level molecular system is studied by solving numerically the Maxwell–Bloch equations by the iterative predictor-corrector finite-difference time-domain method. Optical power limiting behavior induced by strong nonlinear two-photon absorption is observed for different orders of the femtosecond hyper-Gaussian pulses. Pulses of a higher order temporal profile are found to have a wider power range of optical limiting but a larger output saturation intensity. Both the output saturation value and the damage threshold of optical power limiting decrease with pulse duration increasing. The decrease of the pulse area along the pulse propagation is much slower than that obtained from the two-photon area theorem due to invalidity of the slowly varying amplitude approximation and the monochromatic field hypothesis.
Propagation of strong femtosecond hyper-Gaussian pulses in an organic molecular medium is studied by solving numerically the Maxwell-Bloch equations using an iterative predictor-corrector finite-difference time-domain technique. The carrier-wave frequency of the field is tuned in two-photon resonance with the molecular system simplified by a cascade three-level model. Strong two-photon absorption induced optical power limiting behavior is observed for the hyper-Gaussian pulses of different orders. For the ultrashort hyper-Gaussian pulses, it is found that the ”two-photon area” is no further the deciding quantity of the two-photon induced dynamics, and pulses with different temporal profiles will induce different two-photon absorption dynamics and optical limiting processes. With the same pulse duration and field amplitude, pulses of a lower order is found to have a larger input ”two-photon area” but a smaller output area, and therefore show a better optical limiting behavior. The population distribution and the generation of new fields during pulse propagation also depend on the shape of the incident field.
Abstract When a two-level system is driven on resonance by a strong incident field, its emission spectrum is characterized by the well-known Mollow triplet. If the absorption from the excited state, in this continuously driven two-level system, to a third, higher energy level, is probed by a weak field, the resulting absorption spectrum features the Autler-Townes doublet with two peaks separated by the Rabi frequency of the strong driving field. It has been shown that when the two-level system is instead driven by a periodic pulse sequence, the emission spectrum obtained has similarities with the Mollow triplet even though the system is only driven during the short application time of the pulses and is allowed to evolve freely between pulses. Here, we evaluate the absorption spectrum of the three-level system in the ladder/cascade configuration when the bottom two levels are driven by a periodic pulse sequence while the transition between the middle and the highest level is probed by a weak field. The absorption spectrum displays similarities with the Autler-Townes doublet with frequency separation between the main peaks defined by the inter-pulse delay. In addition, this spectrum shows little dependence on the pulse carrier frequency. These results demonstrate the capacity to modulate the absorption spectrum of a three-level system with experimentally achievable pulse protocols.