Surface plasmon polaritons (SPPs) are responsible for exotic optical phenomena, including negative refraction, surface enhanced Raman scattering, and nanoscale focusing of light. Although many materials support SPPs, the choice of metal for most applications has been based on traditional plasmonic materials (Ag, Au) because there have been no side-by-side comparisons of the different materials on well-defined, nanostructured surfaces. Here, we report a platform that not only enabled rapid screening of a wide range of metals under different excitation conditions and dielectric environments, but also identified new and unexpected materials for biosensing applications. Nanopyramidal gratings were used to generate plasmon dispersion diagrams for Al, Ag, Au, Cu, and Pd. Surprisingly, the SPP coupling efficiencies of Cu and Al exceeded widely used plasmonic materials under certain excitation conditions. Furthermore, grazing angle excitation led to the highest refractive index sensitivities (figure of merit >85) reported at optical frequencies because of extremely narrow SPP resonances (full-width-at-half-minimum <6 nm or 7 meV). Finally, our screening process revealed that Ag, with the highest sensitivity, was not necessarily the preferred material for detecting molecules. We discovered that Au and even Pd, a weak plasmonic material, showed comparable index shifts on formation of a protein monolayer.nanophotonics ͉ surface plasmon polariton ͉ dispersion diagrams ͉ chemical and biological sensing S urface plasmon polaritons (SPPs) are collective excitations of free electrons trapped at a metal/dielectric interface (1). In the form of SPPs, light can be manipulated at length scales exceeding the diffraction limit (2, 3), which has the potential to transform chemical and biological sensing (4-7), imaging (8-10), and optoelectronics (11-13). To accelerate progress in any area; however, it is critical that rational design play an increasingly important role in developing standards so that applications based on SPP-supporting materials are not selected based on history or availability, but because of their optimal properties. For example, the grand challenge in SPP-based sensing is to achieve single (bio)molecule selectivity and sensitivity, but there are few reports on how to optimize the geometry of the nanostructures or their materials composition for a wide range of chemical environments. Recent reviews on different sensing modalities have also only explored a limited number of plasmonic materials and without seriously considering excitation conditions (14-16). Moreover, nontraditional plasmonic materials such as Cu and Al are desirable for electronic device applications, and catalytically active metals, including Pd (17) [and Cu (18)], are useful in monitoring surface reactions.The frequency range over which SPP resonances exist is dominated by intrinsic materials properties. Specifically, interband transitions of the metal play a large role in determining the relative electric permittivity ( m ), which sets an upper l...