Radiative Contributions Dominate Plasmon Broadening for Post-Transition Metals in the Ultraviolet

We use classical electrodynamics calculations to investigate the plasmonic properties of the post-transition metals Al, Bi, Ga, In, and Sn active in the ultraviolet, focusing in particular on the material- and resonance-dependent origins of plasmon broadening. Analytic Mie theory, the modified-long wavelength approximation, and the quasistatic dipole approximation together show that radiative processes dominate plasmon dephasing and damping in small (5-25 nm radius) Al, Bi, Ga, In, and Sn spheres. For Al, Ga, In, and Sn, the radiative contribution (~0.1–0.2 eV) to the plasmon linewidth is 10-fold greater than the non-radiative contribution (0.001–0.02 eV) from the bulk dielectric function. This is significantly different than what is observed for Ag spheres, where non-radiative contributions (~0.1 eV) are the primary source of broadening up to a radius of 25 nm. Overall, these data suggest that the plasmonic properties, dephasing, and lifetimes for Al, Ga, In, and Sn —and to a lesser extent Bi— spheres are qualitatively similar. These observations have important implications for the use of these metals for ultraviolet plasmonics. The increased importance of radiative damping and dephasing processes for post-transition metals could influence the ability to harvest photons, generate hot carriers, and enhance spectroscopy in the ultraviolet while providing new opportunities for manipulating high-energy photons.