We report a combined experimental and theoretical study of the modulation of surface charge transfer on the tetrathiafulvalene (TTF)/Au(111) interface as a function of coverage in the submonolayer regime by combining low-temperature scanning tunneling microscopy, high-resolution photoemission spectroscopy using synchrotron radiation, and density functional theory (DFT) calculations. The modulation is induced by the competition between long-range repulsive Coulombic interactions and short-range attractive hydrogen-bonding interactions. The system shows the characteristic pattern evolution, from monomeric stripes at low coverages to two-dimensional islands, with the formation of labyrinths in the crossover. © 2011 American Chemical Society.

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