Here, we expose planar and plasmonic Ag surfaces to a low-power O2/Ar plasma to form an ultrathin surface oxide layer. We study the chemical state and morphology of the plasma-treated Ag surfaces using X-ray photoelectron spectroscopy, scanning electron microscopy, and dark-field microscopy. We observe the formation of an ultrathin layer (< 10 nm) composed of both AgO x and Ag2CO3 for a plasma exposure time of 1 s by investigating shifts in the Ag3d, O1s, and C1s core level binding energies. For an exposure time of 1 s, the surface structure of the planar and plasmonic Ag surfaces remains unchanged. For exposure times of 5 - 30 s, the planar Ag surfaces become porous and exhibit increased surface roughness. We demonstrate that the plasma-treated planar and plasmonic Ag surfaces lead to improvements in the excited-state population of a polymer:fullerene coating through ultrafast pump-probe reflectometry. Copyright © Materials Research Society 2016.