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.

Using the spectral-interferometry method for the short pulse complete characterization, we demonstrate the nature and distinctive properties of the similariton generated in single-mode fiber without gain (passive fiber) due to the combined impacts of nonlinearity and dispersion. The nonlinear-spectronic character of such a similariton, with the key specificity of linear chirping, leads to its self-spectrotemporal imaging, important for applications to the signal analysis-synthesis problems in ultrafast optics.

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We demonstrate the use of a photonic crystal fiber (PCF) as a compact three-color fs laser system operating at 76 MHz, limited only by the repetition rate of the pump laser. The system is suitable for background-free time-resolved four-wave mixing measurements, which arguably reach fundamental limits in signal detectivity. We give a detailed characterization of the near transform-limited multi-color pulses that are extracted from the PCF, and prove the system through time-resolved coherent anti-Stokes Raman scattering measurements in bipyridyl ethylene and styrene.