Internal quantum efficiency enhancement of GaInN/GaN quantum-well structures using Ag nanoparticles AIP Advances 5, 097169 (2015)

We propose and demonstrate antenna-enhanced nonlinear infrared (IR) spectroscopy in reflection geometry. Our approach uses resonant metal nanoantennas to enhance near-fields and to amplify the interaction between molecular vibrations and IR light. We successfully obtain amplified nonlinear vibrational signals in backscattering light of nanoantennas using IR pump energy of 10 nJ, with local signal enhancement of more than 7 orders of magnitude. This ultrasensitive and reflection-type method is useful for characterizing the structure and dynamics of minute volumes of molecules, monolayer materials, and biomolecules in aqueous environments, with additional benefit of surface sensitivity.

We study spectral responses of localized surface plasmons (LSPs) in gold nanorods, which resonate at mid-infrared frequencies, by transmission spectroscopy and electromagnetic field analyses. The resonance linewidth is found to be linearly proportional to the resonance frequency, indicating that the dephasing due to Drude relaxation is suppressed and that the overall dephasing is dominated by radiative damping. Owing to the reduced radiative/non-radiative damping and large geometrical length of the nanorod, near-field intensity enhancement exceeds several hundred times. Nonetheless the resonance linewidth is comparable with or larger than the bandwidth of a 100-fs pulse, and therefore the enhanced near-field as short as 100-fs can be created upon pulsed excitation. The large enhancements with appropriate bandwidths make LSPs promising for enhanced nonlinear spectroscopies, coherent controls, and strong-field light-matter interactions in the mid-infrared range.