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Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons
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State-Specific Nonresonant and Resonant Plasmon-Driven Electron Transfer into Single Molecules.

Zhiwei Liu1,2, Jiayu Xu1,3, Xiang Zhu1,2

  • 1Hefei National Research Center for Physical Sciences at the Microscale, CAS Center for Excellence in Quantum Information and Quantum Physics, and New Cornerstone Science Laboratory, University of Science and Technology of China, Hefei, Anhui 230026, China.

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Researchers used scanning tunneling microscopy to distinguish between two plasmon-driven chemistry pathways. They identified how resonant charge transfer significantly accelerates C-H bond breaking in pentacene molecules.

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Published on: January 19, 2018

Area of Science:

  • Plasmonics
  • Photocatalysis
  • Surface Science
  • Molecular Optoelectronics

Background:

  • Plasmonic energy drives selective chemical transformations, crucial for photocatalysis and solar energy conversion.
  • Distinguishing between nonresonant hot electron transfer and resonant charge transfer pathways in plasmon-driven chemistry remains challenging, particularly in complex molecular systems.

Purpose of the Study:

  • To directly unveil and differentiate nonresonant and resonant plasmon-driven charge transfer channels with submolecular resolution.
  • To correlate plasmon-induced current with specific molecular orbitals.
  • To investigate the effect of different charge transfer pathways on chemical bond breaking.

Main Methods:

  • Utilized a scanning tunneling microscopy (STM) junction with a silver (Ag) tip and individual pentacene molecules on an Ag(110) surface to generate nanocavity plasmons.
  • Employed chopper-modulated laser excitation combined with lock-in detection for high-resolution plasmon-induced current mapping (0.3 nm resolution).
  • Tuned photon energy and bias voltage to selectively probe different electronic states and transfer mechanisms.

Main Results:

  • Successfully mapped plasmon-induced current with submolecular resolution, correlating it with the frontier molecular orbitals of pentacene.
  • Identified nonresonant hot-electron transfer occurring via the lowest unoccupied molecular orbital (LUMO).
  • Identified more efficient resonant charge transfer occurring via the LUMO + 1 state, which significantly accelerated C-H bond breaking.

Conclusions:

  • Directly demonstrated and distinguished between nonresonant and resonant charge transfer pathways in a model plasmonic system.
  • Established that resonant charge transfer via the LUMO + 1 orbital is a highly effective pathway for driving chemical reactions, specifically C-H bond activation.
  • Provides a high-resolution methodology for studying plasmon-driven chemistry at the molecular level, applicable to catalysis and optoelectronics.