Tuning dimensionality in low-dimensional electronic materials

We demonstrate how dimensionality can be tuned in complex low-dimensional electronic materials via small perturbations in competing molecular forces. The delicate balance between molecular level forces on observed dimensionality in materials is illustrated by the 1-d to 3-d structural reorganization following deuteration of the ancillary ligands in the halogen-bridged transition-metal charge-transfer complex [Pt(en)2I2][Pt(en)2]I2 (PtI) where en denotes ethylenediamine. Specifically, the impact of competing forces on dimensionality is clearly demonstrated by the temperature-dependent phase transitions in perdeuterated PtI (D-PtI), where small changes in inter- and intra-sheet interactions drive mesoscopic structural changes.