The adsorption behavior of diethyldisulfide (DEDS), CH(3)CH(2)S(2)CH(2)CH(3), on Au(111) was investigated using a combined system of high-resolution electron energy-loss spectroscopy (HREELS) and scanning tunneling microscopy (STM). At low exposure (0.5 L), all vibration modes of ethylthiolate on Au(lll) were observed by HREELS, and linear chains were recognized in STM images. At 100 L, some loss peaks decreased drastically in intensity and bright spots appeared in STM images. At low exposure, the ethylthiolate moiety reads to form a chain structure on Au(lll) with the terminal sulfur bonded to gold. The ethyl group is randomly oriented. At an exposure of 100 L, the orientation of the molecules is fixed, with the C-C bond of the ethyl group parallel to the surface due to the interaction between neighboring molecules. (C) 1999 Elsevier Science B.V. All rights reserved.