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Ultra-strong nonlinear optical processes and trigonal warping in MoS2 layers

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  • Antti Säynätjoki

    (Department of Electronics and Nanoengineering, Aalto University
    Institute of Photonics, University of Eastern Finland)

  • Lasse Karvonen

    (Department of Electronics and Nanoengineering, Aalto University)

  • Habib Rostami

    (Istituto Italiano di Tecnologia, Graphene Labs)

  • Anton Autere

    (Department of Electronics and Nanoengineering, Aalto University)

  • Soroush Mehravar

    (College of Optical Sciences, University of Arizona)

  • Antonio Lombardo

    (University of Cambridge)

  • Robert A. Norwood

    (College of Optical Sciences, University of Arizona)

  • Tawfique Hasan

    (University of Cambridge)

  • Nasser Peyghambarian

    (Department of Electronics and Nanoengineering, Aalto University
    Institute of Photonics, University of Eastern Finland
    College of Optical Sciences, University of Arizona)

  • Harri Lipsanen

    (Department of Electronics and Nanoengineering, Aalto University)

  • Khanh Kieu

    (College of Optical Sciences, University of Arizona)

  • Andrea C. Ferrari

    (University of Cambridge)

  • Marco Polini

    (Istituto Italiano di Tecnologia, Graphene Labs)

  • Zhipei Sun

    (Department of Electronics and Nanoengineering, Aalto University)

Abstract

Nonlinear optical processes, such as harmonic generation, are of great interest for various applications, e.g., microscopy, therapy, and frequency conversion. However, high-order harmonic conversion is typically much less efficient than low-order, due to the weak intrinsic response of the higher-order nonlinear processes. Here we report ultra-strong optical nonlinearities in monolayer MoS2 (1L-MoS2): the third harmonic is 30 times stronger than the second, and the fourth is comparable to the second. The third harmonic generation efficiency for 1L-MoS2 is approximately three times higher than that for graphene, which was reported to have a large χ (3). We explain this by calculating the nonlinear response functions of 1L-MoS2 with a continuum-model Hamiltonian and quantum mechanical diagrammatic perturbation theory, highlighting the role of trigonal warping. A similar effect is expected in all other transition-metal dichalcogenides. Our results pave the way for efficient harmonic generation based on layered materials for applications such as microscopy and imaging.

Suggested Citation

  • Antti Säynätjoki & Lasse Karvonen & Habib Rostami & Anton Autere & Soroush Mehravar & Antonio Lombardo & Robert A. Norwood & Tawfique Hasan & Nasser Peyghambarian & Harri Lipsanen & Khanh Kieu & Andre, 2017. "Ultra-strong nonlinear optical processes and trigonal warping in MoS2 layers," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-00749-4
    DOI: 10.1038/s41467-017-00749-4
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