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Few-states models for three-photon absorption.

Peter Cronstrand1, Patrick Norman, Yi Luo

  • 1Theoretical Chemistry, Royal Institute of Technology, SCFAB, SE-106 91 Stockholm, Sweden.

The Journal of Chemical Physics
|July 21, 2004
PubMed
Summary
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Few-states models for three-photon absorption calculations are evaluated. These models, unlike those for two-photon absorption, do not quantitatively describe three-photon absorption, even for charge-transfer systems.

Area of Science:

  • Quantum Chemistry
  • Nonlinear Optics

Background:

  • Few-states models are approximations for calculating multiphoton absorption matrix elements.
  • Two-photon absorption models show good agreement with response theory for charge-transfer systems.

Purpose of the Study:

  • To derive and evaluate few-states models for three-photon absorption (3PA).
  • To compare the performance of 3PA models with response theory calculations.
  • To analyze factors influencing 3PA cross sections and model applicability.

Main Methods:

  • Derivation of few-states models for 3PA matrix elements.
  • Comparison with response theory calculations (sum-over-states).
  • Analysis of electronic structure properties (symmetry, charge transfer, conjugation).

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Main Results:

  • Few-states models fail to quantitatively describe 3PA, even for charge-transfer systems.
  • Model performance is poorer for 3PA than for two-photon absorption.
  • Electronic structure and generalized model considerations (dipolar directions, polarization) are crucial for 3PA.

Conclusions:

  • Few-states models have limitations in quantitatively predicting 3PA.
  • Despite quantitative shortcomings, these models can aid in interpreting 3PA phenomena.
  • Generalized few-states models are necessary for accurate 3PA cross-section analysis.