Optical detection of single sub-15 nm objects using elastic scattering strong coupling

Metallic nano-objects play crucial roles in diverse fields, including biomedical imaging, nanomedicine, spectroscopy, and photocatalysis. Nano-objects smaller than 15 nm exhibit extremely low scattering cross-sections, posing a significant challenge for optical detection. An approach to enhance optical detection is to exploit nonlinearity of strong coupling regime, especially for elastic scattering, which is universal to all objects. However, there is still no observation of the strong coupling of elastic light scattering from nano-objects. Here, we demonstrate the strong coupling of elastic light scattering in self-assembled plasmonic nanocavities formed between a gold nanoprobe and a gold film. We employ this technique to detect individual objects with diameters down to 1.8 nm. The resonant mode of the nano-object in the nanocavity environment strongly couples with the nanocavity mode, revealing anti-crossing scattering modes under dark-field spectroscopy. The experimental result agrees with numerical calculations, which we use to extend this technique to other metals. Furthermore, our results show that scattering cross-section ratio of the nano-object scales with the electric field to fourth power, similar to surface-enhanced Raman spectroscopy. This work establishes a new possibility of elastic strong coupling and demonstrates its applicability for observing small, non-fluorescent, Raman inactive sub-15 nm objects, complementary to existing microscopes.