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Broadband Absorption Engineering to Enhance Light Absorption in Monolayer MoS2

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journal contribution
posted on 27.04.2016 by Shah Mohammad Bahauddin, Hossein Robatjazi, Isabell Thomann
Here we take a first step toward tackling the challenge of incomplete optical absorption in monolayers of transition metal dichalcogenides for conversion of photon energy, including solar, into other forms of energy. We present a monolayer MoS2-based photoelectrode architecture that exploits nanophotonic light management strategies to enhance absorption within the monolayer of MoS2, while simultaneously integrating an efficient charge carrier separation mechanism facilitated by a MoS2/NiOx heterojunction. Specifically, we demonstrate two extremely thin photoelectrode architectures for solar-fuel generation: (i) a planar optical cavity architecture, MoS2/NiOx/Al, that improves optical impedance matching and (ii) an architecture employing plasmonic silver nanoparticles (Ag NPs), MoS2/Ag NPs/NiOx/Al, that further improves light absorption within the monolayer. We used a combination of numerical simulations, analytical models, and experimental optical characterizations to gain insights into the contributions of optical impedance matching versus plasmonic near-field enhancement effects in our plasmonic photoelectrode structures. By performing three-dimensional electromagnetic simulations, we predict structures that can absorb 37% of the incident light integrated from 400 to 700 nm within a monolayer of MoS2, a 5.9× enhanced absorption compared to that of MoS2 on a sapphire (Al2O3) substrate. Experimentally, a 3.9× absorption enhancement is observed in the total structure compared to that of MoS2/Al2O3, and photoluminescence measurements suggest this enhancement largely arises from absorption enhancements within the MoS2 layer alone. The results of these measurements also confirm that our MoS2/NiOx/Al structures do indeed facilitate efficient charge separation, as required for a photoelectrode. To rapidly explore the parameter space of plasmonic photoelectrode architectures, we also developed an analytical model based on an effective medium model that is in excellent agreement with results from numerical FDTD simulations.