Laser polarization as a critical factor in the SERS-based molecular sensing performance of nano-gapped Au nanowires.

Nowadays, Au dimer-based nanostructures are exhaustively studied due to their outstanding potential as plasmonic nanoantennas for future applications in high-sensitivity molecular sensing by Surface-Enhanced Raman Spectroscopy (SERS). In this work, we analyze nano-gapped Au nanowires (NWs) or Au-NW dimers for designing efficient nanoantennas, reporting an exhaustive study about dimer length and laser polarization orientation effects on their SERS-based molecular sensing performance. Arrays of nanoantennas with gaps of about 22 ± 4 nm, nominal square cross-sections of 60 nm × 60 nm, and different segment lengths from 300 nm up to 1200 nm were fabricated by Au evaporation and subsequent e-beam lithography. The SERS performance was studied by confocal Raman microscopy using a linearly-polarized 633 nm laser. A critical impact of the polarization alignment on the spectral resolution of the studied Raman marker imprint was observed. The results show that the Raman signal is maximized by aligning the polarization orientation with the nanowire long axis, it is reduced by increasing the relative angle, and it is abruptly minimized when both are perpendicular. These observations were consistent with numerical simulations carried out by the FDTD method, which predicts a similar dependence between the orientation of linearly-polarized light and electric-near field amplification in the nano-gap zone. Our results provide an interesting paradigm and relevant insights in determining the role of laser polarization in the Raman signal enhancement in nano-gapped Au nanowires, showing the key role of this measurement condition on the SERS-based molecular sensing efficiency of this kind of nanostructure.