Probing Temperature-Induced Plasmonic Nonlinearity: Unveiling Opto-Thermal Effects on Light Absorption and Near-Field Enhancement

Nano Lett. 2024 Mar 27;24(12):3598-3605. doi: 10.1021/acs.nanolett.3c04420. Epub 2024 Feb 26.

Abstract

Precise measurement and control of local heating in plasmonic nanostructures are vital for diverse nanophotonic devices. Despite significant efforts, challenges in understanding temperature-induced plasmonic nonlinearity persist, particularly in light absorption and near-field enhancement due to the absence of suitable measurement techniques. This study presents an approach allowing simultaneous measurements of light absorption and near-field enhancement through angle-resolved near-field scanning optical microscopy with iterative opto-thermal analysis. We revealed gold thin films exhibit sublinear nonlinearity in near-field enhancement due to nonlinear opto-thermal effects, while light absorption shows both sublinear and superlinear behaviors at varying thicknesses. These observations align with predictions from a simple harmonic oscillation model, in which changes in damping parameters affect light absorption and field enhancement differently. The sensitivity of our method was experimentally examined by measuring the opto-thermal responses of three-dimensional nanostructure arrays. Our findings have direct implications for advancing plasmonic applications, including photocatalysis, photovoltaics, photothermal effects, and surface-enhanced Raman spectroscopy.

Keywords: field enhancement; light absorption; near-field scanning optical microscopy; scanning probe microscopy; temperature-driven nonlinearity; thermoplasmonics.