The multipurpose nonlinear optical microscope was applied to elucidate the
structure of J-aggregate assembly (JA) of merocyanine dye (MD) in the monol
ayer. It was revealed that the two-dimensional cigar-shaped JA with noncent
ro-symmetric arrangement of MD along the assembly plane was formed, with th
e polar axis inclining by about 30 degrees from the long axis of the assemb
ly. The second harmonic generation (SHG) of the MD monolayer was first meas
ured as a function of the fundamental wavelength and the resonant SHG spect
rum was observed at the J-band.