journal article·2025-12-26Open access

Graphene Nanosheet-Gold Nanopatch Metasurfaces for Nonlinear Response at THz Frequencies

Anna Theodosi, Isaac Appiah Otoo, Anastasios D. Koulouklidis, Nikolaos Matthaiakakis, George Kakarantzas, Petri Mustonen, Harri Lipsanen, Georgy Fedorov, Ioannis Liontos, Stelios Tzortzakis, Polina Kuzhir, Maria Kafesaki, Odysseas Tsilipakos

ACS Applied Nano Materials· Volume 8· Issue 51

Abstract

High Resolution Image Download MS PowerPoint Slide Graphene’s exceptional nonlinear optical properties combined with resonant photonic structures offer a promising pathway for efficient nonlinear applications at terahertz (THz) frequencies. In this work, we propose and demonstrate a fabrication-friendly hybrid nonlinear metasurface composed of gold patches integrated with uniform graphene, circumventing the need for complex graphene patterning. The structure supports strong localized resonances that enhance nonlinear interactions. By exploiting resonant enhancement at both the fundamental and third harmonic frequencies, we predict via simulations third-harmonic generation efficiencies as high as −15 dB (3.2%) under continuous-wave excitation at modest intensities (0.1 MW/cm 2 ). The metasurface is fabricated via electron-beam lithography and experimentally characterized under pulsed excitation using THz time-domain spectroscopy. The broadband excitation spectrum prevents unambiguous isolation of a third-harmonic signal; however, we experimentally observe pronounced nonlinear frequency shifts up to 0.5 THz (12.5% fractional change), driven by self-phase modulation, consistent with simulation results. Our findings highlight the potential of tailored graphene-based metasurfaces for efficient nonlinear THz photonic devices.
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Research context

OpenAlex topics: Plasmonic and Surface Plasmon Research · Metamaterials and Metasurfaces Applications · Terahertz technology and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Electronic Structure and Laser

Foundation for Research and Technology Hellas

Department of Materials Science and Engineering

University of Crete

Department of Physics and Mathematics

University of Eastern Finland

Regensburg Center for Ultrafast Nanoscopy (RUN) and Department of Physics

University of Regensburg

Institute of Nanoscience and Nanotechnology

National Center for Scientific Research “Demokritos”

Theoretical and Physical Chemistry Institute

National Hellenic Research Foundation

Department of Electronics and Nanoengineering, Aalto University, Maarintie 8, 02150 Espoo, Finland

Funding

HORIZON EUROPE Marie Sklodowska-Curie Actions · Hellenic Foundation for Research and Innovation · Research Council of Finland

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