Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/s41467-017-00749-4
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Funding
- Academy of Finland [276376, 284548, 295777, 298297, 304666]
- TEKES (NP-Nano, OPEC)
- Royal Academy of Engineering (RAEng) Research Fellowships
- Fondazione Istituto Italiano di Tecnologia
- Graphene Flagship
- ERC grants Hetero2D
- Nokia Foundation
- EPSRC [EP/K01711X/1, EP/K017144/1, EP/L016087/1]
- AFOSR COMAS MURI [FA9550-10-1-0558]
- ONR NECom MURI
- CIAN NSF ERC [EEC-0812072]
- TRIF Photonics from the state of Arizona
- Micronova, Nanofabrication Centre of Aalto University
- EPSRC [EP/K01711X/1, EP/G042357/1, EP/K017144/1, EP/N010345/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/N010345/1, EP/G042357/1, EP/K017144/1, EP/K01711X/1] Funding Source: researchfish
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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 chi((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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