Gold-polymer hybrid metasurface for polarization-independent enhanced third harmonic generation in the ultraviolet

Abstract

We present a combined experimental and theoretical study of nonlinear light-matter interactions in a three-dimensional gold-polymer hybrid metasurface. In contrast to conventional two-dimensional designs, which by symmetry may support either transverse electric (TE) or transverse magnetic (TM) polarization, our volumetric architecture accepts both TE and TM modes simultaneously, reflecting the dimensionality and versatility required by the photonic devices. The metasurface comprises a periodic lattice of gold nanostructures embedded in a dielectric polymer matrix, creating complex metal–dielectric interfaces that sustain tightly confined plasmonic resonances. When driven by ultrafast near-infrared (NIR) pulses, these resonances concentrate optical energy at the nanoscale, enabling efficient third-harmonic generation and upconversion of visible light into the ultraviolet (UV) and deep-UV regimes with enhanced conversion efficiency. We perform spatial and temporal mapping of the nonlinear response under both TE and TM excitation. Our measurements reveal polarization-agnostic field enhancement and spectral tunability arising from the three-dimensional morphology-capabilities unattainable in planar metasurfaces, where two-dimensional symmetry inherently limits polarization flexibility and functional bandwidth. This quasi-3D platform provides a flexible design toolbox for polarization-independent UV and deep-UV light sources. Potential applications include high-resolution UV spectroscopy, optical multiplexing, data storage, and emerging quantum photonic architectures. By establishing fundamental insights into three-dimensional nonlinear metasurface behavior, our work paves the way for next-generation reconfigurable, multi-polarization nanophotonic devices.

SM, JT, and CC acknowledge the Spanish Agencia Estatal de Investigación from Ministerio de Ciencia, Investigación y Universidades (project PID2023-148620NB-I00 granted by MICIU/AEI/10.13039/501100011033 and FEDER, UE) and US Army Research Laboratory Cooperative Agreement N◦ W911NF-22-2-0236 issued by US ARMY ACC-APG-RTP. S. M. acknowledges predoctoral grant FPI-UPC 2022, funded by Universitat Politècnica de Catalunya (Government of Catalunya). M. A. V. thanks NATO SPS Grant no. G5984 - RESPONDER for financial support. This work has received funding from the Spanish Agencia Estatal de Investigación/ Spanish Ministry of Science and Innovation (AEI/MCIN) through grants PID2022-141956NB-I00 MCIN/AEI/10.13039/501100011033 (OUTLIGHT), and CEX2023-001263-S (MATRANS42, Spanish Severo Ochoa Centre of Excellence program) and from the Generalitat de Catalunya (2021-SGR-00444). A.C.R. acknowledges support from the postdoctoral fellowship program Beatriu de Pinós 2022 BP 00083, funded by the Secretary of Universities and Research (Government of Catalonia).

Peer Reviewed

Postprint (published version)