Tailoring Light–Matter Interactions in Overcoupled Resonator for Biomolecule Recognition and Detection

• Proposed a new paradigm for nanoantenna design using coupled-mode theory, enabling precise control of light–matter interactions. • Designed an OC-Hμ resonator with ultra-sensitive (7.25% nm−1) and ultra-broadband (3–10 μm) sensing performance, immune to asymmetric Fano lineshapes. • Demonstrated machine learning-assisted mixture classification, concentration prediction, and spectral reconstruction with up to 100% accuracy. • Showcased potential for SARS-CoV-2 detection, advancing SEIRA technology for biomolecule recognition and trace detection.