Optical harmonic generation in monolayer group-VI transition metal dichalcogenides

Research output: Contribution to journalArticleScientificpeer-review

Researchers

  • Anton Autere
  • Henri Jussila
  • Andrea Marini
  • J. R.M. Saavedra
  • Yunyun Dai

  • Antti Säynätjoki
  • Lasse Karvonen
  • He Yang
  • Babak Amirsolaimani
  • Robert A. Norwood
  • Nasser Peyghambarian
  • Harri Lipsanen

  • Khanh Kieu
  • F. Javier García De Abajo
  • Zhipei Sun

Research units

  • University of Eastern Finland
  • University of Arizona
  • ICREA
  • Barcelona Institute of Science and Technology
  • Aalto University

Abstract

Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS2 have indeed revealed very large second-order (χ(2)) and third-order (χ(3)) optical susceptibilities. However, third-harmonic generation results of other layered TMDs have not been reported. Furthermore, the reported χ(2) and χ(3) of MoS2 vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and three-photon photoluminescence in TMDs. Specifically, we present an experimental study of χ(2) and χ(3) of four common TMD materials (MoS2, MoSe2, WS2, and WSe2) by placing different TMD flakes in close proximity to each other on a common substrate, allowing their NLO properties to be accurately obtained from a single measurement. χ(2) and χ(3) of the four monolayer TMDs have been compared, indicating that they exhibit distinct NLO responses. We further present theoretical simulations of these susceptibilities in qualitative agreement with the measurements. Our comparative studies of the NLO responses of different two-dimensional layered materials allow us to select the best candidates for atomic-scale nonlinear photonic applications, such as frequency conversion and all-optical signal processing.

Details

Original languageEnglish
Article number115426
JournalPhysical Review B
Volume98
Issue number11
Publication statusPublished - 17 Sep 2018
MoE publication typeA1 Journal article-refereed

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