Modification of charge transfer in a two-dimensional donor/acceptor framework by the insertion of another donor-type molecule into electronegative interlayer pockets.

Pyrene-intercalated layered compounds, [{Ru-2(O2CCF3)(4)}(2)-(TCNQR(x))] center dot 2(pyrene) (TCNQR(x) = 7,7,8,8-tetracyano-p-quinodimethane derivatives; R-x = H-4 and F-4), were synthesized. Pyrene prohibits intralayer electron transfer of [ Ru-2(II),(II)] -> TCNQR(x), even in the compound with R-x = F-4, from occurring.