A measurement system for resonant second harmonic(RSH) spectroscopy us
ing an optical arrangement of total internal reflection was developed
as an analytical method for investigating molecules adsorbed on substr
ate surfaces. RSH spectra were measured for the rhodamine B molecules
adsorbed on a fused quartz substrate with different coverages. It was
demonstrated for the first time by the polarization measurements that
aggregation of rhodamine B occurred on a fused quartz, and that both o
f the dimeric and monomeric species coexisted on the surface.