Single-molecule electronic components are potential building blocks for next-generation electronic devices. One architecture for such devices is quantum dot cellular automata (QCA), in which binary information is encoded in the charge configuration of a single cell and transferred by electric coupling between neighboring cells. A single mixed-valence molecule with two oxidationreduction centers can serve as a QCA cell, and ensemble measurements have shown that such molecules may have the desired electronic properties. Scanning tunneling microscopy (STM) is used to image dinuclear metal complexes, trans-[Cl-(dppe) 2 Ru(CtC) 6 Ru(dppe) 2 Cl] (Ru2) on Au(111) at 77 K. Oxidation to Ru2 þ [PF 6 ] -creates an unbalanced charge that localizes on one end group of the otherwise symmetric Ru2 molecule. This electronic asymmetry appears in STM images, which also resolve the associated [PF 6 ] -counterions. Comparison of Ru2 and Ru2 þ monolayers show that Coulomb interactions create long-range ordering of Ru2 þ electronic charge. This is a requirement for functionality in a QCA device.SECTION Surfaces, Interfaces, Catalysis S ingle-molecule electronic components have been investigated as the building blocks for next-generation electronic devices. 1-12 One proposed architecture for such devices is based upon quantum dot cellular automata (QCA), in which binary information is encoded in the charge configuration of a single cell and transferred by electric coupling between neighboring QCA cells. 13-17 Implementation of QCA at the molecular level requires mixed-valence molecules with two or more oxidation-reduction centers, and such molecules have been shown to have the desired electronic properties using ensemble measurement techniques. 18,19 For the fabrication of devices, it is imperative to understand the changes in charge configuration that result when an electron tunnels between redox sites in a single molecule on a surface. 20 In our work, we present the scanning tunneling microscopy (STM) studies of dinuclear metal complexes, trans-[Cl(dppe) 2 Ru(CtC) 6 Ru(dppe) 2 Cl] (abbreviated as Ru2, dppe = diphenylphosphinoethane) on Au(111) at cryogenic temperature. Close-packed Ru2 molecules form monolayers with ordered stripes on Au(111) at 77 K. Ru2 þ [PF 6 ] -, the oxidation product of Ru2, has an extra charge which can tunnel between two metal-centered end groups. Ru2 þ cations are imaged also as a pair of dots on Au(111) and form similar striped monolayers, except that the two dots appear to have different contrast in STM images due to the extra charge localized in one end group. [PF 6 ] -anions are observed as a small dot resting next to the positively charged ends of Ru2 þ cations.The dinuclear metal complex Ru2 is composed of two Ru-centered phenylphosphine groups connected by a linear hexa-alkyne-bond linker, as shown in Figure 1A. While Ru2 is a neutral dinuclear complex with both Ru metal atoms in the þ2 valence state, oxidation to Ru2 þ results in a mixed-valence þ2/þ3 molecule with an odd electron that can tunnel be...