Tailoring the Electron Pairing Process in a Pt–I Charge-Density-Wave Chain

The electron pairing process in strongly correlated solid-state materials governs a range of important phenomena, such as superconductivity, charge density wave (CDW) orders, and so on. The ability to manipulate the electron pairs and charge orders is of central importance. Herein, we report the construction of a one-dimensional molecular superlattice structure featuring alternating Pt-I and Pt-Pt-I-I double-chains. The interchain electrostatic interactions could fundamentally reconfigure the electron pairing process, shifting it from a conventional localized mechanism to a delocalized, multisite pathway. This transformation stabilizes the first iodide-bridged Pt(III) CDW chain. The delocalized electron pairing process within this CDW state elevates the material's bulk conductivity by roughly 3 orders of magnitude compared to the localized state. Our findings establish a versatile chemical strategy for manipulating electron correlations and charge orders at the molecular level, providing a new design principle for strongly correlated electronic materials.