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Plasmonic Photocatalysis with Nonthermalized Hot Carriers
Shengxiang Wu1, Yu Chen1, Shiwu Gao1
1Beijing Computational Science Research Center, Beijing, 100193, China.
Physical Review Letters
|September 2, 2022
Summary
Plasmonic hot carriers drive photocatalysis. This study reveals nonthermal electrons efficiently induce bond dissociation, especially in quantum regimes, advancing plasmon-enhanced energy transfer for catalysis.
Area of Science:
- Plasmonics
- Photocatalysis
- Surface Science
Background:
- Hot carriers from plasmon damping can enhance photocatalysis.
- The exact mechanisms of nonthermal hot carrier activation in energy transfer remain unclear.
Purpose of the Study:
- To develop a model describing vibrational excitation and bond dissociation by plasmonic hot carriers.
- To elucidate the role of nonthermal hot carriers in photocatalytic processes.
Main Methods:
- Utilized an Anderson-Newns model to simulate electron-molecule scattering.
- Incorporated nonthermal electron distributions alongside thermal carriers.
- Modeled vibrational excitation and bond dissociation dynamics.
Main Results:
- Nonthermal electrons, despite lower populations, are dominant in photodissociation, particularly at low temperatures and in quantum plasmon regimes.
- The model accurately predicts wavelength dependence and experimental enhancement factors for oxygen dissociation on silver nanoparticles.
- Demonstrated the efficiency of high-energy nonthermal electrons in driving chemical reactions.
Conclusions:
- Nonthermal hot carriers play a crucial, often dominant, role in plasmon-enhanced photocatalysis.
- The developed model provides insights into energy transfer mechanisms in the quantum plasmon regime.
- This work offers a pathway for utilizing nonthermal plasmonic energy for advanced photocatalytic applications.
