A rich catalog of C-C bonded species formed in CO reduction on a plasmonic photocatalyst.

The understanding and rational design of heterogeneous catalysts for complex reactions, such as CO reduction, requires knowledge of elementary steps and chemical species prevalent on the catalyst surface under operating conditions. Using in situ nanoscale surface-enhanced Raman scattering, we probe the surface of a Ag nanoparticle during plasmon-excitation-driven CO reduction in water. Enabled by the high spatiotemporal resolution and surface sensitivity of our method, we detect a rich array of C-C species formed on the photocatalytically active surface.

Control of Chemical Reaction Pathways by Light-Matter Coupling.

Because plasmonic metal nanostructures combine strong light absorption with catalytically active surfaces, they have become platforms for the light-assisted catalysis of chemical reactions. The enhancement of reaction rates by plasmonic excitation has been extensively discussed. This review focuses on a less discussed aspect: the induction of new reaction pathways by light excitation.

Nanoscale optical imaging in chemistry.

Single-molecule-level measurements are bringing about a revolution in our understanding of chemical and biochemical processes. Conventional measurements are performed on large ensembles of molecules. Such ensemble-averaged measurements mask molecular-level dynamics and static and dynamic fluctuations in reactivity, which are vital to a holistic understanding of chemical reactions.

Watching Visible Light-Driven CO Reduction on a Plasmonic Nanoparticle Catalyst.

Photocatalytic reduction of carbon dioxide (CO) by visible light has the potential to mimic plant photosynthesis and facilitate the renewable production of storable fuels. Accomplishing desirable efficiency and selectivity in artificial photosynthesis requires an understanding of light-driven pathways on photocatalyst surfaces. Here, we probe with single-nanoparticle spatial resolution the dynamics of a plasmonic silver (Ag) photocatalyst under conditions of visible light-driven CO reduction.