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Gas-phase surface-enhanced Raman scattering (SERS) remains challenging due to poor analyte affinity to SERS substrates. The reported use of capturing probes suffers from concurrent inconsistent signals and long response time due to the formation of multiple potential probe-analyte interaction orientations. Here, we demonstrate the use of multiple non-covalent interactions for ring complexation to boost the affinity of small gas molecules, SO2 and NO2 , to our SERS platform, achieving rapid capture and multiplex detection down to 100 ppm. Experimental and in-silico studies affirm stable ring complex formation, and kinetic investigations reveal a 4-fold faster response time compared to probes without stable ring complexation capability. By synergizing spectral concatenation and support vector machine regression, we achieve 91.7 % accuracy for multiplex quantification of SO2 and NO2 in excess CO2 , mimicking real-life exhausts. Our platform shows immense potential for on-site exhaust and air quality surveillance. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) Submitted/Accepted version This research is supported by Singapore National Research Foundation Central Gap Fund (NRF2020NRF-CG001-010) and A*STAR AME Individual Research Grant (A20E5c0082).

Harnessing large hotspot volumes is key for enhanced gas-phase surface-enhanced Raman scattering (SERS) sensing. Herein, we introduce versatile, air-stable 3D 'Plasmonic bubbles' with bi-directional sensing capabilities. Our Plasmonic bubbles are robust, afford strong and homogenous SERS signals, and can swiftly detect both encapsulated and surrounding 4-methylbenzenethiol vapors. Published version