Surface plasmon polaritons (SPPs) are extremely sensitive to the surrounding refractive index and have found important applications in ultrasensitive label-free sensing. Reducing the linewidth of an SPP mode is an effective way to improve the figure of merit (FOM) and hence the sensitivity of the plasmonic mode. Many efforts have been devoted to achieving a narrow linewidth by mode coupling, which inevitably results in an asymmetrical lineshape compromising the performance. Instead, the SPP modes are directly narrowed by elaborately engineering periodic plasmonic structures with minimized feature sizes to effectively reduce the radiative losses. A narrow linewidth smaller than 8 nm is achieved over a wide wavelength ranging from 600 to 960 nm and a minimum full width at half maximum of 3 nm at 960 nm. Benefiting from the almost perfect Lorentzian lineshape and the extremely narrow linewidth, a record FOM value of 730 is obtained. The sensor is capable of detecting bovine serum albumin with an ultralow concentration of 10 m. The sensor has great potential for practical application for its ultrahigh FOM, broad working wavelength, and ease of high-throughput fabrication.

Plasmonic sensors are promising for ultrasensitive chemical and biological analysis. However, there are increasing experimental findings that cannot be well addressed by theoretical calculations, including the nonlinear dependence of the plasmonic peak wavelength on the refractive index (RI) and the ultrahigh sensitivity beyond the theoretical limit. The gap between experiments and theoretical calculations is that the bulk RI (BRI) used for calculation could be different from the interfacial RI (IRI) determining the electromagnetic response as a result of the interaction of molecules with the surface. But there is still no method to determine the IRI. Herein, we quantitatively determine the IRI by disentangling the surface RI (SRI) from the BRI. The obtained IRI can be directly applied in theoretical calculations to reliably reflect the experimental response and rigorously guide the design of plasmonic sensors. Moreover, it can be a fundamental dimensionless number to describe the light–matter interaction at the interface.

Delicate control of the surface plasmon resonance (SPR) line shapes is crucial for the development of nanoplasmonics with dedicated applications. In this paper, we develop a method to fabricate large-scale periodic structures with significantly different plasmonic properties by the holographic lithography method. We show that SPR line shapes can be controllably engineered from a broad superradiant line shape to an asymmetrical Fano-type resonance, as well as an ultranarrow subradiant mode, which are clearly correlated with the structural parameter (morphology) of the fabricated structures. The wavelength of the SPR band can be tuned from the visible to near-infrared region by changing the incident angle. The nanostructures fabricated by the present method show a clear correlation between the morphology of plasmonic structures and SPR line shapes, which can serve as an efficient platform for engineering SPR line shapes for specific applications. Most importantly, the capability to produce structures of large area further supports the unprecedented opportunity to push these plasmonic structures fabricated by holographic lithography toward real applications.