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Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
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Two-photon absorption arises from two-dimensional excitons.

Feng Zhou, Jing Han Kua, Shunbin Lu

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    |August 19, 2018
    PubMed
    Summary
    This summary is machine-generated.

    We developed a theoretical model for two-photon absorption in monolayer transition metal dichalcogenides (TMDCs). Selenium-based TMDCs show higher absorption than sulfur-based ones, with potential applications in nonlinear optics.

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    Area of Science:

    • Condensed Matter Physics
    • Materials Science
    • Quantum Optics

    Background:

    • Two-photon absorption (2PA) is a nonlinear optical process crucial for applications like 3D microfabrication and optical data storage.
    • Monolayer transition metal dichalcogenides (TMDCs) are promising 2D materials with unique excitonic properties.
    • Understanding 2PA in TMDCs is essential for harnessing their nonlinear optical potential.

    Purpose of the Study:

    • To develop a theoretical model for two-photon absorption (2PA) in monolayer transition metal dichalcogenides (TMDCs).
    • To investigate the influence of material composition (sulfur vs. selenium) on 2PA coefficients.
    • To compare theoretical predictions with experimental measurements.

    Main Methods:

    • Application of quantum perturbation theory.
    • Modeling of two-dimensional excitons in monolayer TMDCs.
    • Calculation of 2PA coefficients in the near-infrared spectral region.
    • Comparison with experimental data from Z-scans and nonlinear transmission measurements.

    Main Results:

    • A theoretical model for 2PA in monolayer TMDCs was successfully developed.
    • Calculated 2PA coefficients reached up to 50 cm/MW for a final excitonic state bandwidth of 0.15 eV.
    • Selenium-based monolayer TMDCs demonstrated significantly higher 2PA coefficients compared to sulfur-based counterparts.
    • The model showed good agreement with experimental data.

    Conclusions:

    • The developed theoretical model accurately predicts 2PA in monolayer TMDCs.
    • Monolayer TMDCs, particularly selenium-based ones, are highly efficient materials for nonlinear optical applications.
    • This work provides valuable insights for designing and optimizing optoelectronic devices utilizing 2PA in 2D materials.