Dynamics of cooperative emissions in a cascade three-level molecular system driven by an ultrashort laser pulse

This paper investigates the dynamics of cooperative emissions in a cascade three-level system driven by an ultra, short 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.

级联三能级模型下超短脉冲激光与分子相互作用的动力学研究

通过求解麦克斯韦-布洛赫方程,研究了超短脉冲激光和一维对称π共轭分子材料(4,4′-二甲氨基二苯乙烯分子)的相互作用.该分子材料具有较强的非线性光学性质,其分子的电子结构和电偶极矩是在密度泛函理论水平上利用从头计算方法得到的.研究结果表明,慢变幅近似和旋波近似不能很好地描述超短脉冲在该分子介质中的传播.在单光子共振情况下,保持入射脉冲的脉冲宽度不变,当小面积脉冲在该分子介质中传播时,二能级模型可以较好地描述脉冲激光与该分子体系的相互作用过程.但对于大面积脉冲激光,由于较明显地产生了分子的二次激发,此时分子应采用三能级模型.当保持入射电场振幅不变时,第三个能级上的粒子数随着脉冲面积的增加而增多.

含时电离对分子动态双光子吸收截面的影响

通过采用时域有限差分法和预估矫正法数值求解麦克斯韦-布洛赫方程,研究了含时电离对分子材料4,4-二甲氨基二苯乙烯的动态双光子吸收截面的影响。研究结果表明,对周期量级的飞秒脉冲,介质发生的主要是一步共振双光子吸收,入射光强较高时出现双光子吸收饱和现象,入射光强小于双光子吸收饱和光强时介质的双光子吸收截面随入射光强的增大线性减小。在不同的传播距离处,分子的双光子吸收截而有较大的差别,因此,在对不同的实验条件下测得的双光子吸收截而数值进行比较时,需要考虑样品厚度对实验结果的影响。在同一传播距离处,随光电离截面取值的增大介质的双光子吸收截面减小。利用飞秒脉冲测量分子的双光子吸收截面时,通过数值模拟,讨论了已有解析结果的适用条件。