Preparations of alternate layer-by-layer self-assembled films of poly(diallyldimethyl ammonium chloride) (PDADMAC) and Direct Red 80 (DR80, azobenzene dye) and photo-induced surface relief gratings (SRGs) of the films have been investigated in situ using attenuated total reflection (ATR), that is, surface plasmon resonance spectroscopy (SPS) and quartz crystal microbalance (QCM) measurements. Gratings of the PDADMAC/DR80 films were fabricated by exposure to interference patterns of Ar+ laser light at 488 nm for 30 min. The formation of the gratings was observed using atomic force microscopy (AFM). The films were used for applications to liquid crystal (LC) display devices, and aligning properties of nematic liquid crystal molecules, 5CB, on the SRG in the films were also investigated in a hybrid LC cell configuration by monitoring birefringence properties of the LC cell in situ. It was estimated that the LC molecules in the cell did not align immediately after the photo-induced SRG was inscribed, but almost along the gratings after heat treatment at 40 degreesC for 1 min. (C) 2002 Elsevier Science B.V. All rights reserved.