Dynamics of two-photon absorption by molecules and solutions

被引:76
作者
Gel'mukhanov, F [1 ]
Baev, A [1 ]
Macák, P [1 ]
Luo, Y [1 ]
Ågren, H [1 ]
机构
[1] Royal Inst Technol, Dept Theoret Chem, S-10044 Stockholm, Sweden
关键词
D O I
10.1364/JOSAB.19.000937
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
A dynamic density-matrix based theory of two-photon absorption (TPA) of molecules and solutions is presented. The theory highlights the influence of pulse duration, dephasing, and resonant conditions on the final TPA cross section as well as that of saturation, including a hierarchy of saturation intensities. A breakdown of the conventional identification of TPA with coherent one-step TPA is predicted for the long-pulse regime in which incoherent two-step TPA can even dominate the coherent one-step TPA process. The major role of the solvent is to enhance the off-resonant contributions to TPA furnished by collisional dephasing. (C) 2002 Optical Society of America.
引用
收藏
页码:937 / 945
页数:9
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