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 ™ 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 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 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.

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