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Two-Dimensional Materials with Giant Optical Nonlinearities near the Theoretical Upper Limit.

Alireza Taghizadeh1,2,3, Kristian S Thygesen3,4, Thomas G Pedersen1,2

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Summary

Researchers discovered new 2D materials with exceptional nonlinear optical (NLO) properties. These materials show potential for advanced photonic devices, surpassing existing ones and offering tunable performance based on their bandgaps.

Keywords:
ab initio, high-throughput screeningdensity functional theorymaximum nonlinearitynonlinear opticsphotogalvanic effectsecond-harmonic generationtwo-dimensional materials

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Photonics

Background:

  • Nonlinear optical (NLO) phenomena are crucial for technologies like lasers and optical switches.
  • Two-dimensional (2D) materials exhibit unique and strong NLO properties, attracting significant research interest.

Purpose of the Study:

  • To develop an efficient computational workflow for calculating quadratic optical response.
  • To screen a large database of 2D materials for promising NLO properties.

Main Methods:

  • Utilized a first-principles computational approach to calculate NLO properties.
  • Applied the workflow to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB).
  • Analyzed the relationship between nonlinear coefficients and material bandgaps.

Main Results:

  • Identified an upper limit for nonresonant nonlinearities proportional to E_g^{-4}, explained by theoretical models.
  • Discovered numerous 2D materials with giant NLO properties and bandgaps from 0.4 to 5 eV.
  • Several candidates demonstrated NLO performance exceeding known materials and approaching theoretical limits.

Conclusions:

  • The study provides a comprehensive library of ab initio NLO spectra for 375 2D materials.
  • The findings highlight promising 2D materials for next-generation photonic and optoelectronic devices.
  • The developed workflow and database are valuable resources for the NLO materials research community.