Surface plasmon resonant nanoantennas can confine incident energy onto two-dimensional (2D) transition metal dichalcogenides (TMD) to enhance efficiency of harmonic conversion to higher energies, which is otherwise limited by the intrinsic Å-scale interaction length. Second harmonic generation (SHG) from nanoantenna-decorated 2D TMD was heuristically examined with hyper Rayleigh scattering (HRS), multi-photon microscopy, electron energy loss spectroscopy (EELS), and discrete dipole computation. HRS experimentally quantified the frequency dependence of the second-order nonlinear susceptibility, χ (2) , for liquid-exfoliated WS2. Measured χ(2) fell within 21% of independent density functional theory (DFT) calculations, overcoming the known 100-1000x overestimation of microscopy approaches. EELS supported design of nanoantennas for integration with TMD. Overall SHG conversion efficiencies from chemical vapor-deposited (CVD) 4×105 nm2 MoS2 crystals on silicon dioxide were enhanced up to 0.025 % W-1 in the presence of by single 150 nm Au nanoshell monomers and dimers, ostensibly due to augmented local plasmonic fields.
Gregory T. Forcherio, Luigi Bonacina, Jérémy Riporto, Yannick Mugnier, R. Le Dantec, Jeremy R. Dunklin, Mourad Benamara, and D. Keith Roper, "Integrating plasmonic metals and 2D transition metal dichalcogenides for enhanced nonlinear frequency conversion," Proc. SPIE 10724, Physical Chemistry of Semiconductor Materials and Interfaces XVII, 1072413 (Presented at SPIE Nanoscience + Engineering: August 23, 2018; Published: 7 September 2018); https://doi.org/10.1117/12.2321047.
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