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Size Matters: d-Band Holes Drive Plasmonic Chemistry in Gold
1Vrije Universiteit Amsterdam, Department for Physics and Astronomy, De Boelelaan 1100, 1081HZ Amsterdam, The Netherlands.
Nano Letters
|September 22, 2025
Summary
Plasmonic gold nanoparticles (AuNPs) drive redox reactions via nonthermalized carriers. Their size dictates efficiency, with surface absorption being key for photocatalysis.
Area of Science:
- Materials Science
- Nanotechnology
- Photochemistry
Background:
- Plasmonic gold nanoparticles (AuNPs) are promising for photocatalysis due to light-induced nonthermalized electrons and holes.
- Characterizing these carriers and differentiating their effects from photothermal heating or field enhancement is difficult.
Purpose of the Study:
- To investigate the role of nonthermalized carriers in plasmonic gold photochemistry using a model reaction.
- To quantify the size-dependent internal quantum efficiencies (IQEs) of AuNPs.
Main Methods:
- Utilized light-driven silver shell synthesis around AuNPs as a model system.
- Coupled in situ extinction spectroscopy with Mie theory calculations.
- Analyzed the size dependence of IQEs for various AuNP diameters.
Main Results:
- The size dependence of IQE correlates with light absorption probability within 2-3 nm of the AuNP surface.
- Short-lived d-band holes, which recombine rapidly, are crucial for driving the observed chemistry.
- Demonstrated the importance of surface carrier dynamics in plasmonic photocatalysis.
Conclusions:
- The study highlights the critical role of short-lived d-band holes in AuNP-driven photocatalysis.
- Provides a framework for characterizing activation mechanisms and carrier dynamics in plasmonic photocatalysis.
- Emphasizes the significance of surface interactions and carrier lifetimes for photocatalytic efficiency.
