Development of novel near-field microspectroscopy and imaging of local excitations and wave functions of nanomaterials

We have developed novel methods of near-field microspectroscopy by combining near-field optical microscopy with linear and non-linear optical techniques. The developed near-field microscope achieves high spatial resolution and high time resolution, and is applied to studies of local excitations and wave functions of single noble metal nanoparticles. We demonstrate that the plasmon wave functions and the optical fields in the vicinity of nanoparticles are visualized by the near-field methods. Based on these results, we clearly show that localized electromagnetic field enhancement in the vicinity of nanoparticles is one of the most important factors in surface-enhanced spectroscopies. We also extended the methods to ultrafast optical measurements, and show space-resolved ultrafast transient response of single gold nanorods. The characteristic spatio-temporal features observed in the nanorods are revealed to be arising from the changes of the plasmon-mode wave functions upon elevation of photo-induced electronic temperature of the nanorod.