Citation for published item:furkh rdtD wF nd ted D eF nd xov kD wF nd i elD eF nd o¤ %t hovskyD uF nd tell iD pF nd rirs h D eF nd r likD wF @PHIHA 9gon ept of mole ul r h rge stor ge diele tri l yer for org ni thinE(lm memory tr nsistorsF9D edv n ed m teri lsFD PP @PQAF ppF PSPSEPSPVF Further information on publisher's website:httpXGGdxFdoiForgGIHFIHHPG dm FPHIHHHHQH Publisher's copyright statement: his is the epted version of the following rti leX furkh rdtD wF nd ted D eF nd xov kD wF nd i elD eF nd o¤ %t hovskyD uF nd tell iD pF nd rirs h D eF nd r likD wF @PHIHA 9gon ept of mole ul r h rge stor ge diele tri l yer for org ni thinE(lm memory tr nsistorsF9D edv n ed m teri lsFD PP @PQAF ppF PSPSEPSPVD whi h h s een pu lished in (n l form t httpXGGdxFdoiForgGIHFIHHPG dm FPHIHHHHQHF his rti le m y e used for nonE ommer i l purposes in ord n e ith ileyE gr erms nd gonditions for selfE r hivingFAdditional information:Use policyThe full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-pro t purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details. In this work we report on a novel concept of an electrically programmable selfassembled molecular gate dielectric layer for OTFTs (see figure 1a) that can be reversibly charged and discharged and retains these digital states even when the supply voltage is removed. Due to the small thickness of the dielectric stack (app. 5.7 nm), the memory transistors operate with very small program and erase voltages of ± 2 V. Despite the extremely small dielectric thickness, the retention time is already promising (~6 hours with a read voltage of -750 mV applied continuously). The dielectric is a mixed monolayer of aliphatic and C 60 -functionalized phosphonic acid molecules (app. 2.1 nm thickness) on a patterned and plasma-oxidized aluminum gate electrode on a glass substrate. The aluminum oxide (AlO x ) contributes with a thickness of 3.6 nm to the dielectric layer stack 6 . As the aliphatic component, n-octadecylphosphonic acid 1 was chosen, which has already shown excellent insulating characteristics as the gate dielectric 6 . As the charge storage component, the C 60 -derivative 2 was synthesized to take advantage of the strong acceptor properties and reversible redox behavior of C 60 (Figure 1b and Supplementary Information SI-1) and of the self-assembly properties induced by the C 18 -aliphatic tail with phosphonic acid anchor group.Mixed self-assembled monolayers of 1 and 2 were created by a simple "one pot" solution content) have a relatively small memory ratio of 2.5 (see Section I in Figure 3b), the devices