Plasmon-enhanced two photon excited emission from edges of one-dimensional plasmonic hotspots with continuous-wave laser excitation

J Chem Phys. 2024 Oct 28;161(16):164704. doi: 10.1063/5.0220026.

Abstract

One-dimensional junctions between parallelly and closely arranged multiple silver nanowires (NWs) exhibit a large electromagnetic (EM) enhancement factor (FR) owing to both localized and surface plasmon resonances. Such junctions are referred to as one-dimensional (1D) hotspots (HSs). This study found that two-photon excited emissions, such as hyper-Rayleigh, hyper-Raman, and two-photon fluorescence of dye molecules, are generated at the edge of 1D HSs of NW dimers with continuous-wave near-infrared (NIR) laser excitation and propagated through 1D HSs; however, they were not generated from the centers of 1D HSs. Numerical EM calculations showed that FR of the NIR region for the edges of 1D HSs was larger than that for the centers by ∼102 times, resulting in the observation of two-photon excited emissions only from the edge of 1D HSs. The analysis of the NW dimer gap distance dependence of FR revealed that the lowest surface plasmon (SP) mode, compressed and localized at the edges of 1D HSs, was the origin of the large FR in the NIR region. The propagation of two-photon-excited emissions was supported by the higher-order coupled SP mode.