Plasmon-Mediated Electron Transport in Tip-Enhanced Raman Spectroscopic Junctions

Partha Pratim Pal, Nan Jiang, Matthew D. Sonntag, Naihao Chiang, Edward T. Foley, Mark C. Hersam, Richard P. Van Duyne*, Tamar Seideman

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

17 Scopus citations


We combine experiment, theory, and first-principles-based calculations to study the light-induced plasmon-mediated electron transport characteristics of a molecular-scale junction. The experimental data show a nonlinear increase in electronic current perturbation when the focus of a chopped laser beam moves laterally toward the tip-sample junction. To understand this behavior and generalize it, we apply a combined theory of the electronic nonequilibrium formed upon decoherence of an optically triggered plasmon and first-principles transport calculations. Our model illustrates that the current via an adsorbed molecular monolayer increases nonlinearly as more energy is pumped into the junction due to the increasing availability of virtual molecular orbital channels for transport with higher injection energies. Our results thus illustrate light-triggered, plasmon-enhanced tunneling current in the presence of a molecular linker.

Original languageEnglish (US)
Pages (from-to)4210-4218
Number of pages9
JournalJournal of Physical Chemistry Letters
Issue number21
StatePublished - Sep 22 2015


  • STM
  • electron
  • laser
  • molecular
  • nonthermal
  • plasmon

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry


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