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The interest in monomolecular films as electric conductors arises from thesearch for innovative materials. The utility of non-covalently bonded films islimited because they are mechanically unstable and consist of poorly connecteddomains. Consequently, charge transfers in these films are limited to thedistances in the order of a micrometer. Here we show that a recently developedgas phase assembling method (Burtman, V., Zelichenok, A., Yitzchaik, S. (1999)Angewandte Chemie Inter. Ed. 38, 2041-2045.), which produces robust densemonolayers of NTCDI covalently attached to the surface of silicon, allows oneto overcome this scale limitation. These virtually insulating monolayers can bephoto-chemically populated with cation-radicals via ejection of electrons intothe semi-conducting base. The positive charges of cation-radicals can migrateas far as several millimeters within microseconds in a random walk fashion thusdemonstrating the macroscopic connectivity of the film. Since the charges existas cation-radicals, which are potent oxidants, their migration is coupled totransfer of the free energy of their reduction and is driven by the redoxpotential gradient. Reduction of cation-radicals by an anode converts this freeenergy into electromotive force. We show how these films can be implemented insolar energy conversion and basic time-resolved distance-controlled studies ofsequences of ultra-fast electron transfers.Comment: 18 pages, 4 figure

Free-Energy-Driven Transfer of Charge in Dense Electrochemically Active Monomolecular Films