Isolating the Nonlinear Optical Response of a MoS$_2$ Monolayer under Extreme Screening of a Metal Substrate

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Hauptverfasser: Yang, Tao, Sleziona, Stephan, Pollmann, Erik, Hasselbrink, Eckart, Kratzer, Peter, Schleberger, Marika, Campen, R. Kramer, Tong, Yujin
Format: Preprint
Veröffentlicht: 2023
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author Yang, Tao
Sleziona, Stephan
Pollmann, Erik
Hasselbrink, Eckart
Kratzer, Peter
Schleberger, Marika
Campen, R. Kramer
Tong, Yujin
author_facet Yang, Tao
Sleziona, Stephan
Pollmann, Erik
Hasselbrink, Eckart
Kratzer, Peter
Schleberger, Marika
Campen, R. Kramer
Tong, Yujin
contents 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 MoS$_2$ monolayer from a MoS$_2$/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 week-screening conditions such as in a free-standing monolayer. Extrapolation yields the onset of a direct quasiparticle bandgap of about $1.65\pm0.20$ eV, 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.
format Preprint
id arxiv_https___arxiv_org_abs_2310_19657
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Isolating the Nonlinear Optical Response of a MoS$_2$ Monolayer under Extreme Screening of a Metal Substrate
Yang, Tao
Sleziona, Stephan
Pollmann, Erik
Hasselbrink, Eckart
Kratzer, Peter
Schleberger, Marika
Campen, R. Kramer
Tong, Yujin
Mesoscale and Nanoscale Physics
Materials Science
Optics
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 MoS$_2$ monolayer from a MoS$_2$/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 week-screening conditions such as in a free-standing monolayer. Extrapolation yields the onset of a direct quasiparticle bandgap of about $1.65\pm0.20$ eV, 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.
title Isolating the Nonlinear Optical Response of a MoS$_2$ Monolayer under Extreme Screening of a Metal Substrate
topic Mesoscale and Nanoscale Physics
Materials Science
Optics
url https://arxiv.org/abs/2310.19657