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In this presentation, the effect of subtle difference in the molecular structures on the organization of the molecules in the self-assembly was described. Self-assembling and electrochemical techniques were employed to construct two-dimensional organic molecular adlayers on HOPG and various solid structure. Structural details of adlayers have been investigated by using STM and IR spectroscopy. Understanding the weak interactions controlling the organization of molecules on solid surface provides good opportunity to fabricate the sophisticated architectures. Finally, some future directions in the field are outlined.