Characterization of the second- and third-order nonlinear optical susceptibilities of monolayer MoS2 using multiphoton microscopy

R. I. Woodward, R. T. Murray, C. F. Phelan, R. E. P. de Oliveira, T. H. Runcorn, E. J. R. Kelleher, S. Li, E. C. de Oliveira, G. J. M. Fechine, G. Eda, C. J. S. de Matos

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Abstract

We report second- and third-harmonic generation in monolayer MoS2 as a tool for imaging and accurately characterizing the material's nonlinear optical properties under 1560 nm excitation. Using a surface nonlinear optics treatment, we derive expressions relating experimental measurements to second- and third-order nonlinear sheet susceptibility magnitudes, obtaining values of |χs(2)| = 2.0 × 10-20 m2 V-1 and, for the first time for monolayer MoS2, |χs(3)| = 1.7 × 10-28 m3 V-2. These sheet susceptibilities correspond to effective bulk nonlinear susceptibility values of |χb(2)| = 2.9 × 10-11 m V-1 and |χb(3)| = 2.4 × 10-19 m2 V-2, accounting for the sheet thickness. Experimental comparisons between MoS2 and graphene are also performed, demonstrating ∼3.4 times stronger third-order sheet nonlinearity in monolayer MoS2, highlighting the material's potential for nonlinear photonics in the telecommunications C band.

Original languageEnglish
Article number011006
Number of pages7
Journal2D Materials
Volume4
Issue number1
DOIs
Publication statusPublished - Mar 2017
Externally publishedYes

Keywords

  • MoS₂
  • two-dimensional (2D) materials
  • second-harmonic generation
  • third-harmonic generation
  • multiphoton microscopy

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