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Plasmon-Induced Direct Hot-Carrier Transfer at Metal-Acceptor Interfaces.

Priyank V Kumar1, Tuomas P Rossi2,3, Daniel Marti-Dafcik1

  • 1Optical Materials Engineering Laboratory , ETH Zurich , 8092 Zurich , Switzerland.

ACS Nano
|February 16, 2019
PubMed
Summary

This study quantifies direct plasmon-induced hot-carrier transfer at metal-acceptor interfaces using simulations. Direct hot-electron transfer and direct hot-hole transfer occur with similar probabilities, offering insights for efficient plasmonic devices.

Keywords:
direct transferhot electronshot holesplasmon decaytime-dependent density-functional theory

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Computational Physics

Background:

  • Plasmon-induced hot-carrier transfer is crucial for plasmonic devices.
  • Direct transfer is more efficient but poorly understood at the atomic level.
  • Experimental separation of direct and indirect transfer mechanisms is challenging due to femtosecond timescales.

Purpose of the Study:

  • To isolate and quantify the direct hot-carrier transfer process at a model metal-acceptor interface.
  • To elucidate the atomic-level mechanisms governing direct transfer.
  • To propose strategies for controlling direct hot-electron transfer (DHET) and direct hot-hole transfer (DHHT).

Main Methods:

  • Utilizing time-dependent density-functional theory (TD-DFT) simulations.
  • Modeling a silver-cadmium selenide (Ag147-Cd33Se33) interface.
  • Analyzing plasmon decay dynamics and carrier injection following laser excitation.

Main Results:

  • Simulations reveal plasmon decay within 10 fs upon excitation with a 10 fs laser pulse.
  • Direct transfer occurs with approximately 40% probability.
  • DHET and DHHT probabilities are found to be around 20% each.

Conclusions:

  • The study provides an atomic-level understanding of direct plasmon-induced hot-carrier transfer.
  • Identified DHET and DHHT as distinct processes with comparable probabilities.
  • Offers guidelines for designing metal-acceptor interfaces for enhanced plasmonic hot-carrier devices.