Spacer-Mediated Gold Nanocube Arrays for Edge-Localized Excitonic Enhancement in Monolayer MoS2

Abstract

Plasmonic nanostructures offer an effective route for enhancing light-matter interaction in atomically thin semiconductors, whose optical response is intrinsically limited by their sub-nanometer active thickness. Here, we numerically investigate excitonic enhancement in monolayer (ML) Molybdenum Disulfide (MoS2) coupled to size-tuned gold (Au) nanocube arrays separated by thin aluminum oxide (Al2O3) and hexagonal boron nitride (h-BN) spacer layers. By varying the nanocube side length, the localized surface plasmon resonance is tuned across the visible spectral range to modulate the A- and B-excitonic transitions of monolayer MoS2. We show that the nanocube-size-dependent spectral redshift can be further controlled through the spacer material and thickness, enabling systematic tuning of the near-field distribution, carrier generation rate, quantum yield, and radiative decay enhancement. Localized plasmonic confinement yields excitation-rate enhancements of up to 4.35 at B-excitonic transition (605 nm) and 3.66 at A-excitonic transition (650 nm), while the radiative decay-rate enhancement exceeds 80, leading to 350-fold photoluminescence enhancement. Although both A- and B-excitonic channels are enhanced simultaneously, their relative contributions depend on nanocube size, spacer material, and spacer thickness, indicating wavelength-dependent excitonic modulation rather than strict exciton-selective switching. These findings establish Au nanocube arrays as a simple, scalable, and tunable plasmonic platform for enhancing excitonic carrier generation and emission in ML MoS2.