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This paper shows how oxygen plasma treatment affects the structural, localized surface plasmon resonance (LSPR) spectral, and spatial orientation changes in single gold nanorods coated with a mesoporous silica shell (AuNRs@SiO2) in comparison with bare AuNRs with the same aspect ratio (AR). Single AuNRs@SiO2 subjected to different plasma treatment times were characterized using scanning electron microscopy and total internal reflection scattering (TIRS) microscopy and spectroscopy. The AR of the single AuNRs without a silica shell was dec