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Minimizing Extrinsic Effects in High-Pressure Raman of Monolayer WSe2 through Substrate and Pressure-Transmitting

Jose Hugo Aguiar Sousa1, Ramon S Ferreira2, Alexandre Cavalheiro Dias3

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High pressure Raman spectra of monolayer tungsten diselenide (WSe2) reveal that strain, not electronic transitions, drives second-order mode intensification. Diamond substrates minimize artifacts, enabling accurate characterization of 2D materials.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Spectroscopy

Background:

  • Monolayer transition metal dichalcogenides (TMDs) like WSe2 exhibit unique electronic and optical properties.
  • High-pressure studies are crucial for understanding their behavior but are sensitive to experimental conditions.

Purpose of the Study:

  • To investigate the high-pressure Raman spectra of monolayer WSe2.
  • To elucidate the influence of substrates and pressure-transmitting media (PTMs) on vibrational responses.
  • To distinguish between strain-induced and electronic effects on Raman modes.

Main Methods:

  • High-pressure Raman spectroscopy up to 40 GPa.
  • Use of diamond as a low-strain substrate compared to Si/SiO2.
  • Density functional theory (DFT) calculations.

Main Results:

  • Substrate choice significantly impacts strain transfer; diamond minimizes it.
  • LA-related second-order modes intensify above 15 GPa, especially when PTM loses hydrostaticity.
  • Strain-induced disorder, not electronic band structure changes, is the primary driver for mode intensification.
  • Wrinkles formed upon decompression activate forbidden B2g modes.

Conclusions:

  • Diamond substrates offer superior isolation of intrinsic WSe2 response.
  • Non-hydrostatic pressure and strain-induced disorder are key factors in Raman spectral changes.
  • Findings provide guidelines for accurate high-pressure characterization of 2D materials, minimizing experimental artifacts.