). Below the scheme, photographs show 1a sandwiched between quartz plates before and after the reaction. in Fig. . The transformation proceeds through benzene ring dissociation from the cation, followed by coordination of three CN groups from the anion to form the tetranuclear complex. This coordination is evidenced by an IR spectral shift in the CN stretching vibration from 2201 cm -1 (uncoordinated) to 2227 cm -1 (metalcoordinated) (Fig. , ESI †). Furthermore, UV-vis spectrum shows increased absorption in the 300-450 nm region after photoirradiation, consistent with cyano-group coordination. Microscopic images of the sample revealed that photoirradiation produced a uniform microcrystalline film of 2a on the quartz plate (Fig. ). Partial volatilization of the released benzene occurred upon removing the top quartz plate. Despite containing alkyl chains, the product did not melt upon heating but decomposed at 273 °C (Fig. , ESI †), approximately 110 °C higher than 1a. This increased stability likely arises from the absence of a thermally labile arene ring and enhanced anion stabilization through metal coordination.