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Quantum-Coherence-Enhanced Hot-Electron Injection under Modal Strong Coupling.

Yen-En Liu1, Xu Shi2, Tomohiro Yokoyama3

  • 1Research Institute for Electronic Science, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan.

ACS Nano
|April 21, 2023
PubMed
Summary

Quantum coherence in plasmonic nanostructures boosts artificial photosynthesis efficiency by enhancing hot-electron injection. This study observed and quantified quantum coherence, paving the way for improved photochemical reactions.

Keywords:
Fabry−Pérot nanocavityhot-electron injectionlocalized surface plasmon resonancemodal strong couplingquantum coherence

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Area of Science:

  • Plasmonics
  • Quantum Optics
  • Materials Science
  • Photocatalysis

Background:

  • Artificial photosynthesis aims to improve quantum efficiency.
  • Localized surface plasmon resonance (LSPR) and Fabry-Pérot nanocavities are key optical structures.
  • Understanding hot-electron injection mechanisms is crucial for efficiency enhancement.

Purpose of the Study:

  • Investigate the mechanism of quantum efficiency enhancement in artificial photosynthesis.
  • Explore modal strong coupling between LSPR and nanocavities.
  • Determine the role of quantum coherence in hot-electron injection.

Main Methods:

  • Fabrication of Au nanodisk/titanium dioxide/Au film modal strong coupling structures.
  • Utilizing photoemission electron microscopy for near-field mapping.
  • Quantitative evaluation of coherence area via splitting energy and particle density analysis.
  • Theoretical modeling to support experimental findings.

Main Results:

  • Observed direct evidence of quantum coherence using photoemission electron microscopy.
  • Demonstrated that quantum coherence enhances apparent quantum efficiency of hot-electron injection.
  • Quantitatively evaluated the coherence area in the nanostructures.
  • Validated the quantum-coherence-enhanced hot-electron injection mechanism with a theoretical model.

Conclusions:

  • Quantum coherence plays a significant role in enhancing the quantum efficiency of artificial photosynthesis.
  • Modal strong coupling structures effectively facilitate quantum-coherence-enhanced hot-electron injection.
  • Applying quantum coherence principles can lead to significant improvements in photochemical reaction efficiencies.