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  11. Nondegenerate Three-photon Absorption In Zinc-blende Semiconductors

Nondegenerate three-photon absorption in zinc-blende semiconductors

Matthew Reichert, Peng Zhao, David J Hagan

    Optics Express
    |June 14, 2025

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    View abstract on PubMed

    Summary
    This summary is machine-generated.

    This study presents a method for calculating the three-photon absorption spectrum in semiconductors. Significant enhancements were observed with non-degenerate photon energies, outperforming two-photon absorption.

    Area of Science:

    • Solid-state physics
    • Quantum optics
    • Materials science

    Background:

    • Three-photon absorption (3PA) is a nonlinear optical process relevant for advanced material applications.
    • Understanding 3PA spectra and their dependence on photon energy and polarization is crucial for material characterization.
    • Existing models may not fully capture the complexities of non-degenerate 3PA in various semiconductor structures.

    Purpose of the Study:

    • To develop a theoretical framework for predicting the non-degenerate three-photon absorption spectrum of zinc-blende semiconductors.
    • To investigate the potential for significant spectral enhancement using non-degenerate photon energies.
    • To explore the polarization dependence of 3PA for potential applications in excite-probe spectroscopy.

    Main Methods:

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  • Utilizing third-order perturbation theory and Kane's band structure model for theoretical calculations.
  • Calculating the non-degenerate three-photon absorption coefficient for arbitrary photon energies and polarizations.
  • Performing experimental measurements on zinc-blende (GaAs, ZnSe) and wurtzite (CdS) semiconductors.

    • Main Results:

    • Predicted enhancement of 3PA by over three orders of magnitude with non-degenerate photon energies, exceeding two-photon absorption.
    • Demonstrated significant polarization dependence (up to a factor of 10) in excite-probe measurements with spectral variations.
    • Experimental results for GaAs and ZnSe showed excellent agreement with theoretical predictions for spectral shape, enhancement, and polarization effects.
    • Observed large enhancement in wurtzite CdS compared to the degenerate case.

    Conclusions:

    • The presented theoretical prescription accurately determines the non-degenerate three-photon absorption spectrum of zinc-blende semiconductors.
    • Non-degenerate photon energies offer a substantial advantage for enhancing 3PA, with significant polarization sensitivity.
    • The findings provide a valuable tool for understanding and manipulating nonlinear optical properties in semiconductors for advanced applications.