We investigated the influence of the orientation of individual gold nanorods on the polarization-dependent single-particle surface-enhanced Raman spectroscopy (SERS) of adenine. Higher-order laser beams (radial and azimuthal polarizations) have been used in combination with a parabolic mirror-assisted confocal optical microscope. Based on the photoluminescence (PL) patterns of the single gold nanorods and the simulated electric-field distribution in the focus, we distinguished between isolated gold rods and clusters as well as single nanorods with different orientations. We found that for single gold nanorods lying flat on the substrate, the longitudinal particle plasmon resonance (PPR) mode can be excited more efficiently with the in-plane field component in the focus of an azimuthally polarized laser beam, which enables the observation of stronger enhanced adenine Raman spectra from the single gold nanorods compared to the case of a radially polarized beam.
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