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C60 fullerides are uniquely flexible molecular materials that exhibit a richvariety of behavior, including superconductivity and magnetism in bulkcompounds, novel electronic and orientational phases in thin films, and quantumtransport in a single-C60 transistor. The complexity of fulleride propertiesstems from the existence of many competing interactions, such aselectron-electron correlations, electron-vibration coupling, and intermolecularhopping. The exact role of each interaction is controversial due to thedifficulty of experimentally isolating the effects of a single interaction inthe intricate fulleride materials. Here we report a unique level of control ofthe material properties of KxC60 ultra-thin films through well-controlledatomic layer indexing and accurate doping concentrations. Using STM techniques,we observe a series of electronic and structural phase transitions as thefullerides evolve from two-dimensional monolayers to quasi-threedimensionalmultilayers in the early stages of layer-by-layer growth. These resultsdemonstrate the systematic evolution of fulleride electronic structure andmolecular ordering with variable KxC60 film layer index, and shed new light oncreating novel molecular structures and devices.

Tuning fulleride electronic structure and molecular ordering via variable layer index