Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 937-945 |
| Number of pages | 9 |
| Journal | Journal of the Optical Society of America B: Optical Physics |
| Volume | 19 |
| Issue number | 5 |
| DOIs | |
| State | Published - May 2002 |
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