Strongly coupled Raman scattering enhancement revealed by scattering-type scanning near-field optical microscopy.

Recent advances in near-field technology with an ultrahigh spatial resolution breaking optical diffraction limit, make it possible to further identify surface-enhanced Raman scattering (SERS) enhancement theories, and to monitor the SERS substrates. Here we verify the electromagnetic enhancement mechanism for SERS with a close-up view, using scattering-type scanning near-field optical microscopy. The array of metal-insulator-metal (MIM) subwavelength structures is studied, in which the field enhancement comes from the strong coupling between gap plasmon polariton and surface plasmon polariton modes. The near-field optical measurements reveal that SERS enhancement factor (EF) varies from one MIM subwavelength unit to another in a finite array. Besides the enhancement of isolated unit, the loss exchange phenomenon in strong coupling with a large Rabi splitting can give rise to an additional enhancement of more than 2 orders of magnitude in periodic arrays and close to 3 orders of magnitude in finite arrays. The SERS EF of the array composed of only 5 units is demonstrated to yield the best SERS performance. Our near-field optical measurements show evidence that finite-size structures embodied with strong coupling effect are a key way to develop practical high-performance SERS substrates.