Long-lived modulation of plasmonic absorption by ballistic thermal injection

John A. Tomko, Evan L. Runnerstrom, Yi Siang Wang, Weibin Chu, Joshua R. Nolen, David H. Olson, Kyle P. Kelley, Angela Cleri, Josh Nordlander, Joshua D. Caldwell, Oleg V. Prezhdo, Jon Paul Maria, Patrick E. Hopkins

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Light–matter interactions that induce charge and energy transfer across interfaces form the foundation for photocatalysis1,2, energy harvesting3 and photodetection4, among other technologies. One of the most common mechanisms associated with these processes relies on carrier injection. However, the exact role of the energy transport associated with this hot-electron injection remains unclear. Plasmon-assisted photocatalytic efficiencies can improve when intermediate insulation layers are used to inhibit the charge transfer5,6 or when off-resonance excitations are employed7, which suggests that additional energy transport and thermal effects could play an explicit role even if the charge transfer is inhibited8. This provides an additional interfacial mechanism for the catalytic and plasmonic enhancement at interfaces that moves beyond the traditionally assumed physical charge injection9–12. In this work, we report on a series of ultrafast plasmonic measurements that provide a direct measure of electronic distributions, both spatially and temporally, after the optical excitation of a metal/semiconductor heterostructure. We explicitly demonstrate that in cases of strong non-equilibrium, a novel energy transduction mechanism arises at the metal/semiconductor interface. We find that hot electrons in the metal contact transfer their energy to pre-existing free electrons in the semiconductor, without an equivalent spatiotemporal transfer of charge. Further, we demonstrate that this ballistic thermal injection mechanism can be utilized as a unique means to modulate plasmonic interactions. These experimental results are well-supported by both rigorous multilayer optical modelling and first-principle ab initio calculations.

Original languageEnglish (US)
Pages (from-to)47-51
Number of pages5
JournalNature nanotechnology
Volume16
Issue number1
DOIs
StatePublished - Jan 2021

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Atomic and Molecular Physics, and Optics
  • Biomedical Engineering
  • Materials Science(all)
  • Condensed Matter Physics
  • Electrical and Electronic Engineering

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