Optimizing Plasmonic Photocatalysis by Controlling the Temporal Distribution of Incident Photons
Of central interest in plasmonic photocatalysis is efficiency, defined as the ratio of the rate of chemical transformation to the power of the incident light. Efforts to enhance efficiency have focused largely on optimizing the photocatalyst structure and composition, reaction conditions, and reactor design. Here, we show that the temporal distribution of incident photons is another parameter that can be used to optimize efficiency. We illustrate the concept by varying the repetition rate of incident laser light pulses. By increasing the repetition rate from 13 to 78 MHz while keeping both the total photon flux and temperature constant, we observe a 7-fold increase in external quantum efficiency for ammonia decomposition. An increase of up to 20-fold in the reaction rate per pulse for pulses of identical energy but shorter time delay between pulses is also observed, revealing nonlinearities in the photocatalytic process. Our findings broaden the approaches for light delivery in photocatalysis, offering insight into how photocatalytic efficiency can be maximized for a fixed incident light energy and expanding current concepts for dynamic control in plasmon-driven chemistry.
Authors
- Peter Nordlander (ORCID: https://orcid.org/0000-0002-1633-2937)
- Margherita Maiuri (ORCID: https://orcid.org/0000-0001-9351-8551)
- Aaron Bayles (ORCID: https://orcid.org/0000-0001-7396-7800)
- Andrea Schirato (ORCID: https://orcid.org/0000-0001-8024-9778)
- Yigao Yuan (ORCID: https://orcid.org/0000-0003-1385-2395)
- Giuseppe Della Valle (ORCID: https://orcid.org/0000-0003-0117-2683)
- Simon Chung (ORCID: https://orcid.org/0000-0001-8087-8793)
- Alessandro Alabastri (ORCID: https://orcid.org/0000-0001-6180-8052)
- Naomi J. Halas (ORCID: https://orcid.org/0000-0002-8461-8494)
- Parmeet Dhindsa (ORCID: https://orcid.org/0000-0003-0711-4492)
- Henry O. Everitt (ORCID: https://orcid.org/0000-0002-8141-3768)
- Aliyu A. Ahmad (ORCID: https://orcid.org/0000-0002-3118-4872)
- Shan Deneen
- William Smith (ORCID: https://orcid.org/0009-0003-9779-0095)
- Catherine Fabiano
Institutions
- United States Department of the Army (US)
- DEVCOM Army Research Laboratory (US)
- Rice Research Institute (CN)
- Rice University (US)
- Politecnico di Milano (IT)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2026-04-24
- DOI
- https://doi.org/10.1021/acscatal.6c00415
- Primary Topic
- Gold and Silver Nanoparticles Synthesis and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Welch Foundation
- Air Force Office of Scientific Research
- HORIZON EUROPE Marie Sklodowska-Curie Actions
- NextGenerationEU