ArticleNano letters2026
Electronically Forbidden Raman Pathways Create a New Contrast Mechanism in Single-Molecule TERS.
Article in Nano letters, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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3 authors.
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Abstract
Tip-enhanced Raman scattering (TERS) provides vibrational fingerprints with subnanometer resolution, yet resonant vibronic Raman pathways involving electronically forbidden (dark) intermediate states lack a validated, fully electrodynamic description. We develop a nonlocal quantum-electromagnetic framework based on transition-dipole densities that unifies Franck-Condon and Herzberg-Teller Raman amplitudes, including their interference, and treats the Stokes frequency near field self-consistently via dyadic Green functions evaluated with a discrete-dipole approximation for arbitrary lossy plasmonic geometries. The theory shows that dark intermediate resonances can make Herzberg-Teller-derived parity information and mode-dependent nodal patterns emerge in single-molecule TERS images, enabling clear discrimination of vibrational identity and parity even under strong resonance. It also predicts that neglecting Stokes frequency backaction/renormalization (prescribed near field) can alter apparent image symmetry.
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