Leveraging Nanocavity Harmonics for Control of Optical Processes in 2D Semiconductors.

Akselrod, Gleb M; Ming, Tian; Argyropoulos, Christos; Hoang, Thang B; Lin, Yuxuan; Ling, Xi; Smith, David R; Kong, Jing et al. · Nano Lett · 2015

basic_science · Level V

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Abstract

Optical cavities with multiple tunable resonances have the potential to provide unique electromagnetic environments at two or more distinct wavelengths--critical for control of optical processes such as nonlinear generation, entangled photon generation, or photoluminescence (PL) enhancement. Here, we show a plasmonic nanocavity based on a nanopatch antenna design that has two tunable resonant modes in the visible spectrum separated by 350 nm and with line widths of ∼60 nm. The importance of utilizing two resonances simultaneously is demonstrated by integrating monolayer MoS2, a two-dimensional semiconductor, into the colloidally synthesized nanocavities. We observe a 2000-fold enhancement in the PL intensity of MoS2--which has intrinsically low absorption and small quantum yield--at room temperature, enabled by the combination of tailored absorption enhancement at the first harmonic and PL quantum-yield enhancement at the fundamental resonance.