Intermolecular interaction was investigated by measuring the properties of self-assembled monolayers (SAMs) in the lateral direction. We formed SAMs of octadecyltrichlorosilane (OTS) and phenethyltrichlorosilane with Ag-or Au-patterned electrodes on mica surfaces and measured the conductance under various bias voltages. Using an atomic force microscope with a conductive cantilever, we could not detect current through the SAMs in the vicinity of the electrodes about 85 nm from the edge. The resistivity of the OTS film measured using the substrates with interdigitated (comb) electrodes was strongly dependent on the humidity. From the result in a dry N 2 atmosphere, the resistivity of a SAM of OTS in a lateral direction was estimated to be ∼ 9 × 10 10 Ω cm.Self-assembled monolayers (SAMs) are one of the promising candidates for sensors, ultra-thin passivating and insulating layers, resists for nanometer-scale lithography, and new devices, because their properties can be controlled by changing the species of constituent molecules. So far, a great number of studies have been made on the structure, formation process, physical properties, and so on. The study of the electrical properties has just started from both experimental and theoretical points of view. Most studies have been concerned with the electrical conduction along the molecular axis [1-4], but there have been few studies on the electrical conduction in the lateral direction, parallel to the surface of SAMs. Possible ways to measure the conductivity of SAMs are to make films on an insulating substrate with patterned electrodes (Fig. 1a), to form electrodes on the films (Fig. 1b), and to form films on the flat substrate with buried conductive regions (Figs. 1c,d).In this study, we formed SAMs on the metal-patterned substrates as shown in Fig. 1a and measured the electrical conductivity of SAMs in the lateral direction using atomic force microscopy (AFM) with a conductive cantilever as a counterelectrode. Generally, it is not easy to form SAMs on the patterned substrates, because their formation is quite sensitive to * Permanent address: Electrotechnical Laboratory, Tsukuba, Ibaraki 305. the nature of the substrate surfaces, e.g. its chemical properties, contaminations, and roughness. However, with a careful cleaning process, residuals in the process for forming electrodes were removed thoroughly, and we could form SAMs of the same quality as those on the pristine surface. Adding the electrode after the SAM formation (Fig. 1b) might cause some damage to the film. We also carried out macroscopic measurements of the conductivity of SAMs under controlled S A M electrode substrate (a) (b) conductive region (c) (d) conductive layer Fig. 1a-d. Schematic drawings for possible structures of SAMs on substrates with electrodes. a A SAM on the electrode-patterned substrate. b Electrode pattern on the substrate coated by a SAM c, d SAM on the flat substrate with a buried conductive region or layer. Substrates are insulative