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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Nonlinear Optics

Background:

  • Two-dimensional (2D) materials offer unique optical properties due to quantum confinement.
  • Second Harmonic Generation (SHG) is a key nonlinear optical phenomenon.
  • Characterizing nonlinear susceptibility in 2D materials is crucial for device applications.

Purpose of the Study:

  • To investigate and quantify the second-order nonlinear susceptibility of monolayer WS₂.
  • To develop a theoretical framework for modeling SHG in 2D materials.
  • To explore polarized SHG as a tool for probing 2D material symmetry and orientation.

Main Methods:

  • Experimental investigation of SHG in monolayer WS₂ on SiO₂/Si substrates and suspended samples.
  • Development of a Green's function formalism for modeling SHG with a 2D nonlinear sheet source.
  • Density Functional Theory (DFT) calculations to understand the origin of nonlinear susceptibility.

Main Results:

  • Monolayer WS₂ exhibits unusually large second-order nonlinear susceptibility (d(eff) ~ 4.5 nm/V), orders of magnitude higher than conventional nonlinear crystals.
  • Polarized SHG successfully probed structural symmetry and crystal orientation.
  • DFT calculations indicate resonance enhancement and large joint density of states as origins for the high nonlinear susceptibility, predicting d(eff) = 0.77 nm/V.

Conclusions:

  • Monolayer WS₂ possesses exceptionally high nonlinear optical properties, making it a promising material for nonlinear optics.
  • The developed theoretical formalism accurately models SHG in 2D materials.
  • Polarized SHG is a valuable technique for characterizing 2D materials, and WS₂'s large nonlinear susceptibility is attributed to electronic structure.