Surface-enhanced coherent anti-Stokes Raman scattering (SECARS) measurements carried out on individual nanosphere dimer nantennas are presented. The ν-domain and t-domain CARS measurements in the few-molecule limit are contrasted as vibrational autocorrelation and cross-correlation, respectively. We show that in coherent Raman spectroscopies carried out with ultrashort pulses, the effect of surface enhancement is to saturate stimulated steps at very low incident intensities (100 fJ in 100 fs pulses), and the principal consideration in sensitivity is the effective quadratic enhancement of spontaneous emission cross sections, σ* = (E L /E o ) 2 σ. Through multicolor femtosecond SECARS measurements we show that beside enhancement factors, an effective plasmon mode matching consideration controls the interplay between coherent electronic Raman scattering on the nantenna and vibrational Raman scattering on its molecular load. Through extensive measurements on individual nantennas, we establish the tolerable average and peak intensities that can be used in ultrafast measurements at nanojunctions, and we highlight a variety of plasmon-driven chemical and physical channels of signal and sample degradation.
A comprehensive theoretical analysis of photo-induced forces in an illuminated nanojunction, formed between an atomic force microscopy tip and a sample, is presented. The formalism is valid within the dipolar approximation and includes multiple scattering effects between the tip, sample and a planar substrate through a dyadic Green's function approach. This physically intuitive description allows a detailed look at the quantitative contribution of multiple scattering effects to the measured photo-induced force, effects that are typically unaccounted for in simpler analytical models. Our findings show that the presence of the planar substrate and anisotropy of the tip have a substantial effect on the magnitude and the spectral response of the photo-induced force exerted on the tip. Unlike previous models, our calculations predict photo-induced forces that are within range of experimentally measured values in photo-induced force microscopy (PiFM) experiments.PACS numbers: May be entered using the \pacs{#1} command.
A new method is presented for visualizing the electric field distributions associated with propagating surface-plasmon-polariton (SPP) modes directly in the near-field. The method is based on detecting the photo-induced gradient force exerted by the evanescent field onto a sharp and polarizable tip. Using a photo-induced force microscope (PiFM), images of propagating SPPs are obtained on flat gold surfaces.
This work studies the effect of a plasmonic array structure coupled with thin film oxide substrate layers on optical surface enhancement using a finite element method. Previous results have shown that as the nanowire spacing increases in the sub-100 nm range, enhancement decreases; however, this work improves upon previous results by extending the range above 100 nm. It also averages optical enhancement across the entire device surface rather than localized regions, which gives a more practical estimate of the sensor response. A significant finding is that in higher ranges, optical enhancement does not always decrease but instead has additional plasmonic modes at greater nanowire and spacing dimensions resonant with the period of the structure and the incident light wavelength, making it possible to optimize enhancement in more accessibly fabricated nanowire array structures. This work also studies surface enhancement to optimize the geometries of plasmonic wires and oxide substrate thickness. Periodic oscillations of surface enhancement are observed at specific oxide thicknesses. These results will help improve future research by providing optimized geometries for SERS molecular sensors.
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