Plasmon Induced Delocalized Second-Harmonic Generation Towards Buried-Interface Spectroscopy

TL;DR

This paper demonstrates plasmon-mediated second-harmonic generation on gold surfaces, enabling wide-area interface spectroscopy with enhanced signals and potential applications in energy, catalysis, and sensing.

Contribution

It reports the first observation of delocalized, surface plasmon polariton-mediated second-harmonic generation at the microscale on gold surfaces, expanding interface probing capabilities.

Findings

Generated second-harmonic light up to 35 um from the excitation spot.

Observed signals from atomically flat surfaces without a local excitation beam.

Detected collimated second-harmonic emission perpendicular to the surface.

Abstract

Second-harmonic generation microscopy is a powerful technique capable of probing local crystal symmetries and electric fields at interfaces. However, it often suffers from weak signal strength and is difficult to understand in multilayer systems where many materials can give competing signal contributions. In this work we present direct observation of delocalized, surface plasmon polariton-mediated second-harmonic generation on gold monocrystalline surfaces and structures. We generate second-harmonic light up to 35 um from the excitation spot and, excitingly, we obtain signal from atomically flat surfaces without a fundamental excitation beam present in the same region. We reveal that this process arises from the interaction of two counter-propagating surface plasmon polaritons, which we believe to be the first observation of this process at the microscale. This signal has the same polarisation dependence as localised second-harmonic generation and is emitted in a collimated beam travelling perpendicular to the sample surface. In part due to local electric field enhancements, we were able to observe these signals on a CMOS camera with 1 s exposure and no gain using an industrial-grade pulsed laser. Our results enable wide area multilayer samples to be probed using a single excitation beam, with applications including in energy, catalysis and single particle surface sensing.