Simultaneous optical and electrochemical recording of single nanoparticle electrochemistry

Abstract

Single nanoparticle collisions have become popular for studying the electrochemical activity of single nanoparticles by determining the transient current during stochastic collisions with the electrode surface. However, if only the electrochemical current is measured, it remains challenging to identify and characterize the individual particle that is responsible for a specific current peak in a collision event; this hampers the understanding of the structure–activity relationship. Herein, we report simultaneous optical and electrochemical recording of a single nanoparticle collision; the electrochemical signal corresponds with the activity of a single nanoparticle, and the optical signal reveals the size and location of the same nanoparticle. Consequently, the structure (optical signal)–activity (electrochemical signal) relationship can be elucidated at the single nanoparticle level; this has implications for various applications including batteries, electrocatalysts, and electrochemical sensors. In addition, our previous studies have suggested an optical-to-electrochemical conversion model to independently calculate the electron transfer rate of single nanoparticles from the optical signal. The simultaneous optical and electrochemical recording achieved in the present work enables direct and quantitative validation of the optical-to-electrochemical conversion model.