Novel Orientational Ordering and Reentrant Metallicity in KxC60 Monolayers for 3 <= x <= 5

We have performed local STM studies on potassium-doped C60 (KxC60) monolayers over a wide regime of the phase diagram. As K content increases from x = 3 to 5, KxC60 monolayers undergo metal-insulator-metal reentrant phase transitions and exhibit a variety of novel orientational orderings. The most striking new structure has a pinwheel-like 7-molecule unit cell in insulating K4+dC60. We propose that the driving mechanism for the orientational ordering in KxC60 is the lowering of electron kinetic energy through maximization of the overlap of neighboring molecular orbitals over the entire doping range x = 3 to 5. In the insulating and metallic phases this gives rise to orbital versions of the superexchange and double-exchange interactions respectively.