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Journal of Atomic and Molecular Physics

Dynamical behavior of two-color ultrashort laser pulses in a cascade three-level molecular system

Chuan‐Kui Wang

Published Jan 1, 2006• 0 citations
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Abstract

Using the finite-difference time domain technique(FDTD) for the fields and the predictor-corrector method for the material variables,we solve the Maxwell-Bloch equations beyond the slowly-varying envelope approximation and the rotating-wave approximation.4,4′-bis(dimethylamino) stilbene organic molecule is one type of one-dimensional symmetrical system and its electronic structure and parameters are calculated by density functional theory.The molecule can be simplified as a three-level system.By numerically simulating the propagation of two-color 2π ultrashort laser pulses in a cascade three-level organic molecule system,we analyze the temporal-spatial evolution properties of the ultrashort laser pulses and the population of each energy level under different resonant conditions.

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Using the finite-difference time domain technique(FDTD) for the fields and the predictor-corrector method for the material variables,we solve the Maxwell-Bloch equations beyond the slowly-varying envelope approximation and the rotating-wave approximation.4,4′-bis(dimethylamino) stilbene organic molecule is one type of one-dimensional symmetrical system and its electronic structure and parameters are calculated by density functional theory.The molecule can be simplified as a three-level system.By numerically simulating the propagation of two-color 2π ultrashort laser pulses in a cascade three-level organic molecule system,we analyze the temporal-spatial evolution properties of the ultrashort laser pulses and the population of each energy level under different resonant conditions.
We study the interaction between the ultra-short laser pulses and the one-dimensional symmetrical π conjugated molecular material (4,4′-bis (dimethylamino) stilbene) by solving Maxwell-Bloch equations. This kind of molecular material has strong nonlinear optical properties, and its electronic structures and dipole moments are calculated by use of density functional theory on ab initio level. The numerical results show that the slowly varying envelope approximation and the rotating wave approximation cannot accurately describe the propagation properties of the ultra-short pulse in the molecular medium. In the case of single photon resonance, the two-level model can well describe the interaction between the small area pulse and the molecular system. For large area pulse, due to the existence of strongly secondary excitation to the higher-lying levels, the three-level model should be used. When the amplitude of the incident electric field is kept constant, the third level's population increases with the increase of the pulse area.
This paper investigates the dynamics of cooperative emissions in a cascade three-level system driven by an ultrashort laser pulse by solving numerically the full-wave Maxwell–Bloch equations. The 4, 4'-bis(dimethylamino) stilbene molecule is used as the model molecule because of its strong two-photon absorption property. The two-colour cooperative emissions are studied as functions of molecular number density and dephasing rate of the dipole coherence. The propagation effects on the evolution of the cooperative radiations are also taken into account. The cooperative radiations are enhanced for large number density of the molecule, while the fast dephasing of the dipole coherence reduces the intensity of the cooperative radiations and delays the emission times or even inhibits the formation of the emissions. The delay time of the radiation decreases with the increase of the molecular number density and the propagation distance.
Propagation and amplification of an ultrashort laser pulse in a two-level medium is numerically investigated with the use of the finite-difference time-domain (FDTD) procedure simultaneously solving Maxwell and Schrodinger equations with no assumptions characteristic of slowly varying envelope approximation. Comparison of the results of FDTD numerical simulations with the predictions of the pulse area theorem has demonstrated that the developed numerical procedure provides an adequate description of pulse evolution in a two-level medium. Amplification of ultrashort light pulses in a two-level medium is analyzed. Two methods of improving the gain of ultrashort pulses in a two-level medium by modulating the spatial distribution of dipole moments of resonant transitions and using initially chirped frequency-detuned pulses are explored.
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.
In this paper the phase-dependent features of ultrashort laser pulse resonant propagation in a two-level dipolar molecule are demonstrated by solving full Maxwell–Bloch equations. The electronic properties of dipolar molecule 4-trans-[p-(N, N-Di-n-butylamino)-p -stilbenylvinyl] pyridine (DBASVP) molecule, one-dimensional asymmetric organic molecule, is calculated by density functional theory at ab initio level. The numerical results show that the carrier propagation and the spectrum evolution of the pulse are sensitive to its initial phase and the phase sensitivity is more obvious for larger area pulse. The phase-dependent feature is more evident in dipolar molecule because the permanent dipole moment makes the nonlinear effects stronger.