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The structures of three tetramethylammonium cyanocuprate(I) 3D networks [NMe 4 ] 2 [Cu(CN) 2 ] 2 •0.25H 2 O ( 1 ), [NMe 4 ][Cu 3 (CN) 4 ] ( 2 ), and [NMe 4 ][Cu 2 (CN) 3 ] ( 3 ), (Me 4 N = tetramethylammonium), and the photophysics of 1 and 2 are reported. These complexes are prepared by combining aqueous solutions of the simple salts tetramethylammonium chloride and potassium dicyanocuprate. Single-crystal X-ray diffraction analysis of complex 1 reveals {Cu 2 (CN) 2 ( μ  2 -CN) 4 } rhomboids crosslinked by cyano ligands and D 3h {Cu(CN) 3 } metal clusters into a 3D coordination polymer, while 2 features independent 2D layers of fused hexagonal {Cu 8 (CN) 8 } rings where two Cu(I) centers reside in a linear C ∞v coordination sphere. Metallophilic interactions are observed in 1 as close Cu⋯Cu distances, but are noticeably absent in 2 . Complex 3 is a simple honeycomb sheet composed of trigonal planar Cu(I) centers with no Cu … Cu interactions. Temperature and time-dependent luminescence of 1 and 2 have been performed between 298 K and 78 K and demonstrate that 1 is a dual singlet/triplet emitter at low temperatures while 2 is a triplet-only emitter. DFT and TD-DFT calculations were used to help interpret the experimental findings. Optical memory experiments show that 1 and 2 are both optical memory active. These complexes undergo a reduction of emission intensity upon laser irradiation at 255 nm although this loss is much faster in 2 . The loss of emission intensity is reversible in both cases by applying heat to the sample. We propose a light-induced electron transfer mechanism for the optical memory behavior observed.

Synthesis and Luminescence of Optical Memory Active Tetramethylammonium Cyanocuprate(I) 3D Networks