Dimensionality-driven optical and electronic evolution of naphthalenediimide-templated hybrid metal oxides

We generate hybrid molybdenum oxides featuring naphthalenediimide (NDI) derivatives, whose redox-activity enable emergent optoelectronic behavior that depends on inorganic dimensionality. We isolate an extended NDI-templated 2D molybdenum oxide-that features the largest-known interlayer spacing for any such hybrid oxide-and a 0D NDI-polyoxomolybdate, allowing us to directly compare molecular, cluster, and extended systems. Combined light absorption/emission and temperature-, light-, and power-dependent EPR studies suggest photogenerated NDI radical anions in molecular and cluster systems, with the latter featuring enhanced photoluminescence. In contrast, the extended structure stabilizes light-independent spins that couple strongly to the lattice. This work expands the physical and electronic boundaries of 2D hybrid molybdenum oxides and points toward addressable spin and charge states for quantum material applications.