Three novel donor-acceptor systems have been characterised through their spectroscopic properties, magnetic susceptibility, conductivity and second harmonic generation. The magnetic properties of (H2DPE)xx+(DPE)^ x(TCNQ)gX and (H2DPA)xx+(DPA) 1 x(TCNQ)gX' where DPE = 1,2-di(4-pyridyl)ethylene, DPA = 1,2-di(4-pyridyl)ethane, TCNQ = tetracyanoquinodimethane and H2 signifies proton diquaternisation, have been found to depend upon the stoichiometry: For x > \ the magnetic susceptibility decreases with increasing x whereas for x ~ \ it is anomolously large, being ferromagnetically enhanced above the Curie Law value. A possible model involving spin dilution is proposed and its predictions are compared with the experimental results. Langmuir-Blodgett (LB) films of the long-chained analogues of the materials, (C^g)2DPE (TCNQ) 2 and (Cig^DPE^TCNQ)^" where (C16) 2 = bis(hexadecyl) were deposited and characterised. The conductivities of the LB films of the mixed valence system were found to be ~ 1000 times greater than those of the system lacking TCNQ^ molecules. Multiple layer LB films of trans-4-[4- (dimethylamino)styryl]-1- octadecylpyridinium iodide and trans-4-[4-(dimethylamino)styryl]-1- octadecylquinolinium iodide interleaved with 4,4'-dioctadecyl-3,5,3',5' -tetramethyldipyrrylmethene hydrobromide were deposited. The materials form an interlocking bilayer structure which renders their LB films exceptionally well-organised. The films’ second harmonic generation was investigated and one film was found to give the largest second harmonic signal yet seen from an LB structure.