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Article: 4 pages, 3 figures; Supplementary information: 7 pages, 7 figuresA p-conjugated tetrathiafulvalene-fused perylenediimide (TTF-PDI) molecular dyad is successfully used as a solution-processed active material for light sensitive ambipolar field-effect transistors with balanced hole\udand electron mobilities. The photo-response of the TTF-PDI dyad resembles its absorption profile. Wavelength-dependent photoconductivity measurements reveal an important photo-response at an energy corresponding to a PDI-localized electronic p–p* transition and also a more moderate effect due to an intramolecular charge transfer from the HOMO localized on the TTF unit to the LUMO localized on the PDI moiety. This work clearly elucidates the interplay between intra- and intermolecular electronic processes in organic devices.The authors thank the EU Large Project ONE-P (FP7-NMP-2007-212311), ERC StG 2012-306826 e-GAMES, the Networking Research Center on Bioengineering, Biomaterials and Nanomedicine (CIBER-BBN), the DGI (Spain) with project\udPOMAS CTQ2010-19501/BQU and Generalitat de Catalunya 2009SGR516, as well as the Swiss National Science Foundation (grant no. 200020-130266/1). E.P. and G.B. acknowledge the support of the ESF Project GOSPEL (Ref. no: 09-Euro-GRAPHENE-FP-001). G.B. acknowledges the Slovenian Research Agency program P1-0055.Peer reviewe

Photo-induced intramolecular charge transfer in an ambipolar field-effect transistor based on a π-conjugated donor–acceptor dyad