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

Antti Säynätjoki; Lasse Karvonen; Habib Rostami; Anton Autere; Soroush Mehravar; Antonio Lombardo; Robert A. Norwood; Tawfique Hasan; Nasser Peyghambarian; Harri Lipsanen; Khanh Kieu; Andrea C. Ferrari; Marco Polini; Zhipei Sun

doi:10.1038/s41467-017-00749-4

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

Antti Säynätjoki, Lasse Karvonen, Habib Rostami, Anton Autere, Soroush Mehravar, Antonio Lombardo, Robert A. Norwood, Tawfique Hasan, Nasser Peyghambarian, Harri Lipsanen, Khanh Kieu, Andrea C. Ferrari, Marco Polini, Zhipei Sun

Department of Physics

Research output: Contribution to journal › Article › peer-review

194 Citations (SciVal)

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.

Original language	English
Article number	893
Journal	Nature Communications
Volume	8
Issue number	1
DOIs	https://doi.org/10.1038/s41467-017-00749-4
Publication status	Published - 1 Dec 2017

Bibliographical note

Data availability
The data that support the findings of this study are available from the corresponding author on request.

Funding

We thank M.J. Huttunen and R.W. Boyd for useful discussions. We acknowledge funding from the Academy of Finland (Nos: 276376, 284548, 295777, 298297, and 304666), TEKES (NP-Nano, OPEC), Royal Academy of Engineering (RAEng) Research Fellowships, Fondazione Istituto Italiano di Tecnologia, the Graphene Flagship, ERC grants Hetero2D, Nokia Foundation, EPSRC Grants EP/K01711X/1, EP/K017144/1, EP/ L016087/1, AFOSR COMAS MURI (FA9550-10-1-0558), ONR NECom MURI, CIAN NSF ERC under Grant EEC-0812072, and TRIF Photonics funding from the state of Arizona and the Micronova, Nanofabrication Centre of Aalto University.

Funders	Funder number
AFOSR COMAS MURI	FA9550-10-1-0558
CIAN NSF ERC	EEC-0812072
ONR NECom MURI
TRIF
National Science Foundation	0812072
European Commission	298297
Engineering and Physical Sciences Research Council	EP/L016087/1, EP/K017144/1, EP/N010345/1, EP/G042357/1, EP/K01711X/1
Royal Academy Of Engineering
European Research Council	Hetero2D
Academy of Finland	276376, 284548, 295777, 304666
Aalto-Yliopisto
Tekes
Nokia Foundation
Italian Institute of Technology

ASJC Scopus subject areas

General Chemistry
General Biochemistry,Genetics and Molecular Biology
General Physics and Astronomy

Access to Document

10.1038/s41467-017-00749-4Licence: CC BY

Cite this

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title = "Ultra-strong nonlinear optical processes and trigonal warping in MoS2 layers",

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.",

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AU - Mehravar, Soroush

AU - Lombardo, Antonio

AU - Norwood, Robert A.

AU - Hasan, Tawfique

AU - Peyghambarian, Nasser

AU - Lipsanen, Harri

AU - Kieu, Khanh

AU - Ferrari, Andrea C.

AU - Polini, Marco

AU - Sun, Zhipei

N1 - Data availability The data that support the findings of this study are available from the corresponding author on request.

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