Second harmonic conversions of surface-plasmon-polariton-enhanced optical fields in nonlinear optics polymer/Ag/glass structures

摘要

Optical fields enhanced by surface plasmon polaritons (SPPs) on metal-dielectric interfaces are useful for increasing several light-matter interactions, and application to nonlinear optics (NLO) is one of the most important uses of this type of structure. Most previous studies on this subject took advantage of the nonlinear susceptibilities of metal surfaces. However, the limited NLO light-matter interaction lengths prevented the transfer of the technologies to practical use. In the present paper, we tried to overcome this problem by growing NLO polymer thin films on metal surfaces. The NLO responses of the system were characterized by second-harmonic generation (SHG) spectroscopy. Our experimental results suggested that SPP-enhanced optical fields induced not only surface nonlinearities in Ag but also bulk nonlinearities in NLO polymer. There was an optimal polymer thickness for the SHG conversions, and a greater thickness did not always result in higher conversion. The maximum conversion efficiency was approximately 40 times higher than that of the nonpolymer-coated bare Ag surface. The growth and propagation of the SHG waves were addressed with a numerical approach combining the transfer matrix method and Green's function analysis. The SHG conversion efficiencies were determined by three factors, the SPP-field enhancement factor, the nonlinear light-matter interaction length, and the degree of interference between the forward- and backward-propagating SHG waves. The latter two factors predominantly determined the optimal SHG conversion efficiencies. The proposed strategy of hybridizing NLO polymers brings us closer to practical uses for nonlinear plasmonics.