Optical Rectification and Field Enhancement in a Plasmonic Nanogap

TL;DR

This study demonstrates optical rectification in a plasmonic nanogap, enabling direct measurement of electric field enhancement exceeding 1000 times, which is crucial for advancing nanophotonics and surface-enhanced spectroscopies.

Contribution

It introduces a method to measure optical field enhancement in nanogaps via nonlinear tunnelling conduction, providing experimental validation and insights into electromagnetic response at subnanometre scales.

Findings

Field enhancements exceed 1000 times

Optical rectification produces measurable DC photocurrent

Method enables direct probing of nanogap electric fields

Abstract

Metal nanostructures act as powerful optical antennas[1, 2] because collective modes of the electron fluid in the metal are excited when light strikes the surface of the nanostructure. These excitations, known as plasmons, can have evanescent electromagnetic fields that are orders of magnitude larger than the incident electromagnetic field. The largest field enhancements often occur in nanogaps between plasmonically active nanostructures[3, 4], but it is extremely challenging to measure the fields in such gaps directly. These enhanced fields have applications in surface-enhanced spectroscopies[5-7], nonlinear optics[1, 8-10], and nanophotonics[11-15]. Here we show that nonlinear tunnelling conduction between gold electrodes separated by a subnanometre gap leads to optical rectification, producing a DC photocurrent when the gap is illuminated. Comparing this photocurrent with low frequency conduction measurements, we determine the optical frequency voltage across the tunnelling region of the nanogap, and also the enhancement of the electric field in the tunnelling region, as a function of gap size. The measured field enhancements exceed 1000, consistent with estimates from surface-enhanced Raman measurements[16-18]. Our results highlight the need for more realistic theoretical approaches that are able to model the electromagnetic response of metal nanostructures on scales ranging from the free space wavelength, $\lambda$, down to $\sim \lambda/1000$, and for experiments with new materials, different wavelengths, and different incident polarizations.