Strong optical nonlinearity of CVD-grown MoS2 monolayer as probed by wavelength-dependent second-harmonic generation

D. J. Clark, V. Senthilkumar, C. T. Le, D. L. Weerawarne, B. Shim, J. I. Jang, J. H. Shim, J. Cho, Y. Sim, M. J. Seong, S. H. Rhim, Arthur J Freeman, K. H. Chung, Y. S. Kim

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Abstract

While noncentrosymmetric MoS2 monolayer is known to exhibit efficient second-harmonic generation (SHG), there is currently no agreement on its absolute nonlinear susceptibility χ(2), varying over three orders of magnitude according to recent experiments. In order to resolve this conflicting issue, we have studied the nonlinear optical properties of MoS2 monolayer grown by chemical vapor deposition. The polycrystalline nature of the monolayer was directly probed by the SHG polarization dependence across the grain boundaries using femtosecond pulses. Broadband wavelength-dependent SHG response (λ=1.1-2.0μm) using picosecond pulses was studied by comparing the relative SHG counts of MoS2 to quartz and incorporating the structural and optical characteristics of the monolayer. Significant nonlinear optical dispersion gives rise to χ(2)∼430 pm/V at 580 nm, where SHG is neither affected by any excitonic absorption/resonance nor by fundamental absorption. We also show that χ(2) must be derived from a thin bulk (sheet) optical nonlinearity and that the previous measurements are in fact all consistent, together with our measurements and first-principle calculations.

Original languageEnglish
Article number121409
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume90
Issue number12
DOIs
Publication statusPublished - Sep 29 2014

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Harmonic generation
Chemical vapor deposition
Monolayers
harmonic generations
nonlinearity
vapor deposition
Wavelength
wavelengths
Quartz
picosecond pulses
Ultrashort pulses
Grain boundaries
quartz
grain boundaries
Optical properties
Polarization
broadband
magnetic permeability
optical properties
polarization

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Electronic, Optical and Magnetic Materials

Cite this

Strong optical nonlinearity of CVD-grown MoS2 monolayer as probed by wavelength-dependent second-harmonic generation. / Clark, D. J.; Senthilkumar, V.; Le, C. T.; Weerawarne, D. L.; Shim, B.; Jang, J. I.; Shim, J. H.; Cho, J.; Sim, Y.; Seong, M. J.; Rhim, S. H.; Freeman, Arthur J; Chung, K. H.; Kim, Y. S.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 90, No. 12, 121409, 29.09.2014.

Research output: Contribution to journalArticle

Clark, DJ, Senthilkumar, V, Le, CT, Weerawarne, DL, Shim, B, Jang, JI, Shim, JH, Cho, J, Sim, Y, Seong, MJ, Rhim, SH, Freeman, AJ, Chung, KH & Kim, YS 2014, 'Strong optical nonlinearity of CVD-grown MoS2 monolayer as probed by wavelength-dependent second-harmonic generation', Physical Review B - Condensed Matter and Materials Physics, vol. 90, no. 12, 121409. https://doi.org/10.1103/PhysRevB.90.121409
Clark, D. J. ; Senthilkumar, V. ; Le, C. T. ; Weerawarne, D. L. ; Shim, B. ; Jang, J. I. ; Shim, J. H. ; Cho, J. ; Sim, Y. ; Seong, M. J. ; Rhim, S. H. ; Freeman, Arthur J ; Chung, K. H. ; Kim, Y. S. / Strong optical nonlinearity of CVD-grown MoS2 monolayer as probed by wavelength-dependent second-harmonic generation. In: Physical Review B - Condensed Matter and Materials Physics. 2014 ; Vol. 90, No. 12.
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