Polycrystalline halogen-bonded assmblies fabricated by physical vapor deposition (PVD) exihibit controllable morphologies and microstructures. Although the solid-state packing may vary going from a solution crystal growth process (used for chromophore single-crystal determination) to a vapor-phase deposition process (used for PVD flim fabrication), the corresponding filim microstructure are independent of the substrate surface chemistry.