Synthesis, Characterization, and X‐Ray Crystal Structures of Bis[ N ‐(3,3‐diphenylallylidene)quinolin‐8‐amine‐ κN,κN 8 ]copper(1+) Tetraphenylborate(1−) ([Cu(dpa‐qa) 2 ]BPh 4 ) and Bis[ N,N ′‐bis(3,3‐diphenylallylidene)‐[1,1′‐biphenyl]‐2,2′‐diamine‐ κN,κN ′]copper(1+) Perchlorate ([Cu(bdpa‐bda) 2 ]ClO 4 ⋅ 3 H 2 O)

Two new ligands, N ‐(3,3‐diphenylallylidene)quinolin‐8‐amine (dpa‐qa; L 1 ) and N,N′ ‐bis‐(3,3‐diphenylallylidene)[1,1′‐biphenyl]‐2,2′‐diamine (bdpa‐bda; L 2 ), and their corresponding copper(I) complexes, [Cu(dpa‐qa) 2 ]BPh 4 ( 1 ) and [Cu(bdpa‐bda) 2 ]ClO 4  ⋅ 3 H 2 O ( 2 ), were synthesized and characterized by C,H,N analyses, 1 H‐ and 13 C‐NMR, IR, and UV/VIS spectroscopy. The crystal and molecular structures of 1 and 2 were determined by X‐ray crystallography from single‐crystal data. Complex 1 crystallizes in the orthorhombic space group Pbca , with a  = 14.391(3) Å, b  = 21.967(5) Å, c  = 35.463(8) Å, V  = 11211(4) Å 3 , and Z  = 8. Complex 2 crystallizes in the monoclinic space group C 2/ c , with a  = 30.746(10) Å, b  = 18.244(6) Å, c  = 27.835(9) Å, β  = 109.794(7)°, V  = 14691(8), and Z  = 8. The coordination polyhedron about the Cu I center in the two complexes is best described as a distorted tetrahedron. A quasireversible redox behavior is observed for complex 1 and 2 ( E 1/2  = 0.58 and 1.04 V).