A simple second-harmonic microscope for in situ and real-time investig
ation of interfaces and ultrathin films is described. A spot on the in
terface is illuminated with a laser. The frequency-doubled light is us
ed for imaging. The technique is surface specific. A single laser puls
e is sufficient to create an image. Scanning of the sample with a shar
ply focused laser beam is not required. Harmonic imaging reveals more
information on surface order and symmetry than is possible with linear
optical microscopy experiments. Polarization microscopy with uncrosse
d polarizers is utilized as a linear optical technique. This simple me
thod provides superior resolution compared with Brewster angle microsc
opy.