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Isolating the optical response of a MoS2 monolayer under extreme screening of a metal substrate

Tao Yang1,*, Stephan Sleziona1, Erik Pollmann1, Eckart Hasselbrink2, Peter Kratzer1, Marika Schleberger1, R. Kramer Campen1, and Yujin Tong1,†

  • 1Faculty of Physics, University of Duisburg-Essen, 47057 Duisburg, Germany
  • 2Faculty of Chemistry, University of Duisburg-Essen, 45117 Essen, Germany

  • *tao.yang@uni-due.de
  • †yujin.tong@uni-due.de

Phys. Rev. B 109, L161402 – Published 12 April, 2024

DOI: https://doi.org/10.1103/PhysRevB.109.L161402

Abstract

Transition metal dichalcogenides (TMDCs) monolayers, as two-dimensional (2D) direct bandgap semiconductors, hold promise for advanced optoelectronic and photocatalytic devices. Interaction with three-dimensional (3D) metals, like Au, profoundly affects their optical properties, posing challenges in characterizing the monolayer's optical responses within the semiconductor-metal junction. In this study, using precise polarization-controlled final-state sum frequency generation (FS-SFG), we successfully isolated the optical responses of a MoS2 monolayer from a MoS2/Au junction. The resulting SFG spectra exhibit a linear lineshape, devoid of A or B exciton features, attributed to the strong dielectric screening and substrate induced doping. The linear lineshape illustrates the expected constant density of states (DOS) at the band edge of the 2D semiconductor, a feature often obscured by excitonic interactions in weak-screening conditions such as in a free-standing monolayer. Extrapolation yields the onset of a direct quasiparticle bandgap of about 1.65±0.20eV, indicating a strong bandgap renormalization. This study not only enriches our understanding of the optical responses of a 2D semiconductor in extreme screening conditions but also provides a critical reference for advancing 2D semiconductor-based photocatalytic applications.

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