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, [{Ru2(O2CCF3)4}2(TCNQRx)]·2(pyrene) (TCNQRx = 7,7,8,8-tetracyano-p-quinodimethane derivatives; Rx = H4 and F4), were synthesized. Pyrene prohibits intralayer electron transfer of [Ru2II,II] → TCNQRx, even in the compound with Rx = F4, from occurring.