Early dynamics of the emission of solvated electrons from nanodiamonds in water

Abstract

Solvated electrons are among the most reductive species in an aqueous environment. Diamond materials have been proposed as a promising source of solvated electrons, but the underlying emission process in water remains elusive so far. Here, we show spectroscopic evidence for the emission of solvated electrons from detonation nanodiamonds upon excitation with both deep ultraviolet (225 nm) and visible (400 nm) light using ultrafast transient absorption. The crucial role of surface termination in the emission process is evidenced by comparing hydrogenated, hydroxylated and carboxylated nanodiamonds. In particular, a transient response that we attribute to solvated electrons is observed on hydrogenated nanodiamonds upon visible light excitation, while it shows a sub-ps recombination due to trap states when excited with deep ultraviolet light. The essential role of surface reconstructions on the nanodiamonds in these processes is proposed based on density functional theory calculations. These results open new perspectives for solar-driven emission of solvated electrons in an aqueous phase using nanodiamonds.