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Chinese journal of atomic and molecular physics

Resonant propagation of laser pulse in organic molecular material

Chuan‐Kui Wang

Published Jan 1, 2004• 0 citations
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Abstract

By use of Maxwell-Bloch coupled equations, we investigate the resonant propagation of laser pulse in 4,4′-bis(dimethylamino) stilbene organic molecular material. The spatial-temporal evolution of the laser pulse is numerically displayed. The damping effect resulted from inelastic or elastic collisions is considered.

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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.
Dynamics of multilevel molecules and pulse propagation is studied near the two-photon resonance. We have found a strict solution of this problem beyond the rotating wave approximation. Our analytical solution is in close agreement with the strict numerical solution for the $4,{4}^{\ensuremath{'}}$-bis(dimethylamino) stilbene molecule. The compensation of the dynamical Stark shift is studied for fixed-in-space molecules. It is shown that the orientational disorder does not allow complete compensation of the dynamical Stark shift.
Laser propagating through resonance media taking into account of spatial effect was discussed by simultaneously solving the Maxwell-Bloch equations with definite differential method. Results indicate that the propagation of a 2π pulse form would no longer be a soliton, its profile would expand, and the degree of distortion depends on the interaction intensity of laser and material: stronger interaction causes more distortion till the profile split. The interaction intensity was decided by such elements as the laser frequency, laser intensity, the dipole of material, detuning and the concentration of resonance particles．
This paper investigates the effect of Lorentz local field correction (LFC) on the propagation of ultrashort laser pulses in a para—nitroaniline molecular medium under resonant and nonresonant conditions by solving numerically the full-wave Maxwell—Bloch equations beyond slowly-varying envelope approximation and rotating-wave approximation. The effect of the LFC is considerably obvious when pulses with large areas propagate in the dense molecular medium. In the case of resonance, the group velocity of the sub-pulses split from the incident pulse along propagation is severely decreased by the LFC, especially for the latest sub-pulse. However, in the case of nonresonance, the influence of the LFC on the temporal evolution of the pulse is less obvious and lacks homogeneity with an increase in incident pulse area, propagation distance and molecular density.