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Supercontinuum second harmonic generation spectroscopy of atomically thin semiconductors.

Torsten Stiehm1, Robert Schneider1, Johannes Kern1

  • 1Institute of Physics and Center for Nanotechnology, University of Münster, 48149 Münster, Germany.

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Researchers developed a new spectroscopy method to precisely measure nonlinear optical properties of 2D semiconductors. This technique calibrates measurements, enabling detailed analysis of excitonic resonances in materials like MoS2 and WS2.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Optoelectronics

Background:

  • Two-dimensional (2D) semiconductors possess significant nonlinear optical properties.
  • These properties are crucial for applications in light sources, optical signal processing, and quantum light generation.
  • Second harmonic generation (SHG) spectroscopy is sensitive to crystal symmetry and material resonances, particularly excitonic effects.

Purpose of the Study:

  • To develop an ultrabroadband SHG spectroscopy technique for atomically thin semiconductors.
  • To accurately determine the frequency-dependent nonlinear susceptibility (χ(2)(ω)) by removing laser pulse artifacts.
  • To identify and characterize excitonic resonances in 2D materials.

Main Methods:

  • Utilized few-cycle femtosecond infrared laser pulses for ultrabroadband excitation.
  • Employed hexagonal boron nitride (hBN) as a reference material for SHG normalization, correcting for laser pulse characteristics.
  • Exploited the angular dependence of SHG to suppress interfering two-photon photoluminescence.

Main Results:

  • Successfully calibrated the frequency-dependent nonlinear susceptibility (χ(2)(ω)) for MoS2 and WS2 monolayers.
  • Identified prominent A and B exciton resonances and higher-lying excited exciton states.
  • Demonstrated a method to decouple material response from laser pulse properties.

Conclusions:

  • The developed SHG spectroscopy technique provides accurate, calibrated nonlinear optical characterization of 2D semiconductors.
  • This method allows for detailed investigation of excitonic properties, crucial for understanding and designing optoelectronic devices.
  • The approach is broadly applicable to other atomically thin materials for nonlinear optics research.