Local Photochemical Nanoscopy of Hot-Carrier-Driven Catalytic Reactions Using Plasmonic Nanosystems
Status PubMed-not-MEDLINE Language English Country United States Media print-electronic
Document type Journal Article
- Keywords
- hot charge carriers, in situ nanoscopy, photocatalysis, plasmonics, scanning electrochemical microscopy,
- Publication type
- Journal Article MeSH
Nanoscale investigation of the reactivity of photocatalytic systems is crucial for their fundamental understanding and improving their design and applicability. Here, we present a photochemical nanoscopy technique that unlocks the local spatial detection of molecular products during plasmonic hot-carrier-driven photocatalytic reactions with nanometric precision. By applying the methodology to Au/TiO2 plasmonic photocatalysts, we experimentally and theoretically determined that smaller and denser Au nanoparticle arrays present lower optical contribution with quantum efficiency in hot-hole-driven photocatalysis closely related to the population heterogeneity. As expected, the highest quantum yield from a redox probe oxidation is achieved at the plasmon peak. Investigating a single plasmonic nanodiode, we unravel the areas where oxidation and reduction products are evolved with subwavelength resolution (∼200 nm), illustrating the bipolar behavior of such nanosystems. These results open the way to quantitative investigations at the nanoscale to evaluate the photocatalytic reactivity of low-dimensional materials in a variety of chemical reactions.
References provided by Crossref.org
Mass Transport Limitations in Plasmonic Photocatalysis
Interfacial States in Au/Reduced TiO2 Plasmonic Photocatalysts Quench Hot-Carrier Photoactivity
